Science.gov

Sample records for biogenic aerosol particles

  1. 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

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

    PubMed

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

    2010-10-14

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

  3. Characteristics of aerosolized ice forming marine biogenic particles

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.

    atomus and Emiliania huxleyi, cells and cell fragments efficiently nucleate ice in the deposition mode, however, only T. pseudonana and N. atomus form ice in the immersion mode, presumably due to different cell wall compositions. This further corroborates the role of phytoplanktonic species for aerosolization of marine biogenic cloud active particles. Experimental data are used to parameterize marine biogenic particle fluxes and heterogeneous ice nucleation as a function of biological activity. The atmospheric implications of the results and their implementation into cloud and climate models are discussed.

  4. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  6. Biogenic Potassium Salt Particles as Seeds for Secondary Organic Aerosol in the Amazon

    NASA Astrophysics Data System (ADS)

    Pöhlker, Christopher; Wiedemann, Kenia T.; Sinha, Bärbel; Shiraiwa, Manabu; Gunthe, Sachin S.; Smith, Mackenzie; Su, Hang; Artaxo, Paulo; Chen, Qi; Cheng, Yafang; Elbert, Wolfgang; Gilles, Mary K.; Kilcoyne, Arthur L. D.; Moffet, Ryan C.; Weigand, Markus; Martin, Scot T.; Pöschl, Ulrich; Andreae, Meinrat O.

    2012-08-01

    The fine particles serving as cloud condensation nuclei in pristine Amazonian rainforest air consist mostly of secondary organic aerosol. Their origin is enigmatic, however, because new particle formation in the atmosphere is not observed. Here, we show that the growth of organic aerosol particles can be initiated by potassium-salt-rich particles emitted by biota in the rainforest. These particles act as seeds for the condensation of low- or semi-volatile organic compounds from the atmospheric gas phase or multiphase oxidation of isoprene and terpenes. Our findings suggest that the primary emission of biogenic salt particles directly influences the number concentration of cloud condensation nuclei and affects the microphysics of cloud formation and precipitation over the rainforest.

  7. 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

    were enhanced with time compared with larger sizes. In contrast, all particle sizes were equally enhanced when frits were used. Aerosolized particles were hygroscopic, a finding with significance for warm cloud formation and potential liquid-to-ice phase transformations. Aqueous and dry aerosolized particles from biologically active mesocosm water were found to efficiently nucleate ice exposed to supersaturated water vapor. The majority of particles, including those nucleating ice, consisted of a sea salt core coated with organic material dominated by the carboxyl functional group, and corresponded to a particle type commonly found in marine air. Our results provide improved estimates of marine aerosol production, chemical composition, and hygroscopicity, as well as an accurate physical and chemical representation of ice nucleation by marine biogenic aerosol particles for use in cloud and climate models.

  8. Aerosols in Amazonia: Natural biogenic particles and large scale biomass burning impacts

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Barbosa, Henrique M. J.; Rizzo, Luciana V.; Brito, Joel F.; Sena, Elisa T.; Cirino, Glauber G.; Arana, Andrea

    2013-05-01

    The Large Scale Biosphere Atmosphere Experiment in Amazonia (LBA) is a long term (20 years) research effort aimed at the understanding of the functioning of the Amazonian ecosystem. In particular, the strong biosphere-atmosphere interaction is a key component looking at the exchange processes between vegetation and the atmosphere, focusing on aerosol particles. Two aerosol components are the most visible: The natural biogenic emissions of aerosols and VOCs, and the biomass burning emissions. A large effort was done to characterize natural biogenic aerosols that showed detailed organic characterization and optical properties. The biomass burning component in Amazonia is important in term of aerosol and trace gases emissions, with deforestation rates decreasing, from 27,000 Km2 in 2004 to about 5,000 Km2 in 2011. Biomass burning emissions in Amazonia increases concentrations of aerosol particles, CO, ozone and other species, and also change the surface radiation balance in a significant way. Long term monitoring of aerosols and trace gases were performed in two sites: a background site in Central Amazonia, 55 Km North of Manaus (called ZF2 ecological reservation) and a monitoring station in Porto Velho, Rondonia state, a site heavily impacted by biomass burning smoke. Several instruments were operated to measured aerosol size distribution, optical properties (absorption and scattering at several wavelengths), composition of organic (OC/EC) and inorganic components among other measurements. AERONET and MODIS measurements from 5 long term sites show a large year-to year variability due to climatic and socio-economic issues. Aerosol optical depths of more than 4 at 550nm was observed frequently over biomass burning areas. In the pristine Amazonian atmosphere, aerosol scattering coefficients ranged between 1 and 200 Mm-1 at 450 nm, while absorption ranged between 1 and 20 Mm-1 at 637 nm. A strong seasonal behavior was observed, with greater aerosol loadings during the

  9. Studies of aerosol at a coastal site using two aerosol mass spectrometry instruments and identification of biogenic particle types

    NASA Astrophysics Data System (ADS)

    Dall'Osto, M.; Harrison, R. M.; Furutani, H.; Prather, K. A.; Coe, H.; Allan, J. D.

    2005-10-01

    During August 2004 an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS Model 3800-100) and an Aerodyne Aerosol Mass Spectrometer (AMS) were deployed at Mace Head during the NAMBLEX campaign. Single particle data (size, positive and negative mass spectra) from the ATOFMS were imported into ART 2a, a neural network algorithm, which assigns individual particles to clusters on the basis of their mass spectral similarities. Results are very consistent with previous time consuming manual classifications (Dall'Osto et al., 2004). Three broad classes were found: sea-salt, dust and carbon-containing particles, with a number of sub-classes within each. The Aerodyne (AMS) instrument was also used during NAMBLEX, providing online, real time measurements of the mass of non-refractory components of aerosol particles as function of their size. The ATOFMS detected a type of particle not identified in our earlier analysis, with a strong signal at m/z 24, likely due to magnesium. This type of particle was detected during the same periods as pure unreacted sea salt particles and is thought to be biogenic, originating from the sea surface. AMS data are consistent with this interpretation, showing an additional organic peak in the corresponding size range at times when the Mg-rich particles are detected. The work shows the ATOFMS and AMS to be largely complementary, and to provide a powerful instrumental combination in studies of atmospheric chemistry.

  10. Impact of gas-to-particle partitioning approaches on the simulated radiative effects of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Scott, C. E.; Spracklen, D. V.; Pierce, J. R.; Riipinen, I.; D'Andrea, S. D.; Rap, A.; Carslaw, K. S.; Forster, P. M.; Kulmala, M.; Mann, G. W.; Pringle, K. J.

    2015-02-01

    The oxidation of biogenic volatile organic compounds (BVOCs) gives a range of products, from semi-volatile to extremely low-volatility compounds. To treat the interaction of these secondary organic vapours with the particle phase, global aerosol microphysics models generally use either a thermodynamic partitioning approach (assuming instant equilibrium between semi-volatile oxidation products and the particle phase) or a kinetic approach (accounting for the size-dependence of condensation). We show that model treatment of the partitioning of biogenic organic vapours into the particle phase, and consequent distribution of material across the size distribution, controls the magnitude of the first aerosol indirect effect (AIE) due to biogenic secondary organic aerosol (SOA). With a kinetic partitioning approach, SOA is distributed according to the existing condensation sink, enhancing the growth of the smallest particles, i.e., those in the nucleation mode. This process tends to increase cloud droplet number concentrations in the presence of biogenic SOA. By contrast, a thermodynamic approach distributes SOA according to pre-existing organic mass, restricting the growth of the smallest particles, limiting the number that are able to form cloud droplets. With an organically medicated new particle formation mechanism, applying a thermodynamic rather than a kinetic approach reduces our calculated global mean AIE due to biogenic SOA by 24%. Our results suggest that the mechanisms driving organic partitioning need to be fully understood in order to accurately describe the climatic effects of SOA.

  11. Impact of gas-to-particle partitioning approaches on the simulated radiative effects of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Scott, C. E.; Spracklen, D. V.; Pierce, J. R.; Riipinen, I.; D'Andrea, S. D.; Rap, A.; Carslaw, K. S.; Forster, P. M.; Artaxo, P.; Kulmala, M.; Rizzo, L. V.; Swietlicki, E.; Mann, G. W.; Pringle, K. J.

    2015-11-01

    The oxidation of biogenic volatile organic compounds (BVOCs) gives a range of products, from semi-volatile to extremely low-volatility compounds. To treat the interaction of these secondary organic vapours with the particle phase, global aerosol microphysics models generally use either a thermodynamic partitioning approach (assuming instant equilibrium between semi-volatile oxidation products and the particle phase) or a kinetic approach (accounting for the size dependence of condensation). We show that model treatment of the partitioning of biogenic organic vapours into the particle phase, and consequent distribution of material across the size distribution, controls the magnitude of the first aerosol indirect effect (AIE) due to biogenic secondary organic aerosol (SOA). With a kinetic partitioning approach, SOA is distributed according to the existing condensation sink, enhancing the growth of the smallest particles, i.e. those in the nucleation mode. This process tends to increase cloud droplet number concentrations in the presence of biogenic SOA. By contrast, an approach that distributes SOA according to pre-existing organic mass restricts the growth of the smallest particles, limiting the number that are able to form cloud droplets. With an organically mediated new particle formation mechanism, applying a mass-based rather than a kinetic approach to partitioning reduces our calculated global mean AIE due to biogenic SOA by 24 %. Our results suggest that the mechanisms driving organic partitioning need to be fully understood in order to accurately describe the climatic effects of SOA.

  12. Aerosol Measurements in the Atmospheric Surface Layer at L'Aquila, Italy: Focus on Biogenic Primary Particles

    NASA Astrophysics Data System (ADS)

    Pitari, Giovanni; Coppari, Eleonora; De Luca, Natalia; Di Carlo, Piero; Pace, Loretta

    2014-09-01

    Two year measurements of aerosol concentration and size distribution (0.25 μm < d < 30 μm) in the atmospheric surface layer, collected in L'Aquila (Italy) with an optical particle counter, are reported and analysed for the different modes of the particle size distribution. A different seasonal behaviour is shown for fine mode aerosols (largely produced by anthropogenic combustion), coarse mode and large-sized aerosols, whose abundance is regulated not only by anthropogenic local production, but also by remote natural sources (via large scale atmospheric transport) and by local sources of primary biogenic aerosols. The observed total abundance of large particles with diameter larger than 10 μm is compared with a statistical counting of primary biogenic particles, made with an independent technique. Results of these two observational approaches are analysed and compared to each other, with the help of a box model driven by observed meteorological parameters and validated with measurements of fine and coarse mode aerosols and of an atmospheric primary pollutant of anthropogenic origin (NOx). Except in winter months, primary biogenic particles in the L'Aquila measurement site are shown to dominate the atmospheric boundary layer population of large aerosol particles with diameter larger than 10 μm (about 80 % of the total during summer months), with a pronounced seasonal cycle, contrary to fine mode aerosols of anthropogenic origin. In order to explain these findings, the main mechanisms controlling the abundance and variability of particulate matter tracers in the atmospheric surface layer are analysed with the numerical box-model.

  13. The role of biogenic, biomass burning and urban pollution aerosol particles in controlling key atmospheric processes in Amazonia

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Ferreira De Brito, J.; Barbosa, H. M.; Rizzo, L. V.; Sena, E. T.; Cirino, G.; Arana, A.; Yanez-Serrano, A. M.

    2013-05-01

    As part of the LBA (The Large Scale Biosphere Atmosphere Experiment in Amazonia) experiment, a research program run in the last 10 years had help to understand critical atmospheric processes in Amazonia. The vegetation in Amazonia is a direct source of aerosol particles to the atmosphere as well as a source of biogenic trace gases that generates particles trough gas-to-particle conversion. Biomass burning is also a large source of particles and trace gases to the atmosphere. Over the last 10 years, the LBA experiment has unveiled several key processes that control Amazonian composition and influence regional climate. A significant fraction (60-80%) of airborne particles can act as Cloud Condensation Nuclei (CCN), influencing cloud formation and development. The radiation balance is strongly influenced by biomass burning particles, and surface radiative forcing up to -250 w/m2 is measured. A network of 8 sites with AERONET sunphotometers measures aerosol optical depth (AOD) and derive aerosol size distribution and optical properties. Aerosols are composed of more than 70% of organic material, with significant absorption characteristics. The aerosol radiative forcing during the biomass burning season can reach very high values, and the increase in diffuse radiation increases the carbon uptake by the forest for AOD values smaller than 1.2 at 500nm. For large AOD, the solar flux is strongly reduced making the carbon uptake approach zero for AOD larger than 3.0. The composition of aerosols is mostly organic, with contribution of K, Ca, Si, and other trace elements. The aerosol has high capability to serve as Cloud Condensation Nuclei (CCN), contributing with high water vapor amounts to the significant cloud cover over the region. In the last 20 years, an urbanization process took over for most of the Amazonian region, increasing urban pollution that interacts with forest emissions to produce a quite unique pattern of aerosols and pollutants around large urban areas such

  14. Biogenic oxidized organic functional groups in aerosol particles from a mountain forest site and their similarities to laboratory chamber products

    NASA Astrophysics Data System (ADS)

    Schwartz, R. E.; Russell, L. M.; Sjostedt, S. J.; Vlasenko, A.; Slowik, J. G.; Abbatt, J. P. D.; MacDonald, A. M.; Li, S. M.; Liggio, J.; Toom-Sauntry, D.; Leaitch, W. R.

    2010-06-01

    Submicron particles collected at Whistler, British Columbia, at 1020 m a.s.l. during May and June 2008 on Teflon filters were analyzed by Fourier transform infrared (FTIR) and X-ray fluorescence (XRF) techniques for organic functional groups (OFG) and elemental composition. Organic mass (OM) concentrations ranged from less than 0.5 to 3.1 μg m-3, with a project mean and standard deviation of 1.3±1.0 μg m-3 and 0.21±0.16 μg m-3 for OM and sulfate, respectively. On average, organic hydroxyl, alkane, and carboxylic acid groups represented 34%, 33%, and 23% of OM, respectively. Ketone, amine and organosulfate groups constituted 6%, 5%, and <1% of the average organic aerosol composition, respectively. Measurements of volatile organic compounds (VOC), including isoprene and monoterpenes from biogenic VOC (BVOC) emissions and their oxidation products (methyl-vinylketone / methacrolein, MVK/MACR), were made using co-located proton transfer reaction mass spectrometry (PTR-MS). We present chemically-specific evidence of OFG associated with BVOC emissions. Positive matrix factorization (PMF) analysis attributed 65% of the campaign OM to biogenic sources, based on the correlations of one factor to monoterpenes and MVK/MACR. The remaining fraction was attributed to anthropogenic sources based on a correlation to sulfate. The functional group composition of the biogenic factor (consisting of 32% alkane, 25% carboxylic acid, 21% organic hydroxyl, 16% ketone, and 6% amine groups) was similar to that of secondary organic aerosol (SOA) reported from the oxidation of BVOCs in laboratory chamber studies, providing evidence that the magnitude and chemical composition of biogenic SOA simulated in the laboratory is similar to that found in actual atmospheric conditions. The biogenic factor OM is also correlated to dust elements, indicating that dust may act as a non-acidic SOA sink. This role is supported by the organic functional group composition and morphology of single particles

  15. Biogenic oxidized organic functional groups in aerosol particles from a mountain forest site and their similarities to laboratory chamber products

    NASA Astrophysics Data System (ADS)

    Schwartz, R. E.; Russell, L. M.; Sjosted, S. J.; Vlasenko, A.; Slowik, J. G.; Abbatt, J. P. D.; MacDonald, A. M.; Li, S. M.; Liggio, J.; Toom-Sauntry, D.; Leaitch, W. R.

    2010-02-01

    Submicron particles collected at Whistler, British Columbia, at 1020 masl during May and June 2008 on Teflon filters were analyzed by Fourier transform infrared (FTIR) and X-ray fluorescence (XRF) techniques for organic functional groups (OFG) and elemental composition. Organic mass (OM) ranged from less than 0.5 to 3.1μg m-3, with a project mean and standard deviation of 1.3±1.0 μg m-3 and 0.21±0.16 μg m-3 for OM and sulfate, respectively. On average, organic hydroxyl, alkane, and carboxylic acid groups represented 34%, 33%, and 23% of OM, respectively. Ketone, amine and organosulfate groups constituted 6%, 5%, and <1% of the average organic aerosol composition, respectively. Measurements of volatile organic compounds (VOC), including isoprene and monoterpenes from biogenic VOC (BVOC) emissions and their oxidation products (methyl-vinylketone/methacrolein, MVK/MACR), were made using co-located proton transfer reaction mass spectrometry (PTR-MS). We present chemically-specific evidence of OFG associated with BVOC emissions. Positive matrix factorization (PMF) analysis attributed 65% of the campaign OM to biogenic sources, based on the correlations of one factor to monoterpenes and MVK/MACR. The remaining fraction was attributed to anthropogenic sources based on a correlation to sulfate. The functional group composition of the biogenic factor (consisting of 32% alkane, 25% carboxylic acid, 2% organic hydroxyl, 16% ketone, and 6% amine groups) was similar to that of secondary organic aerosol (SOA) reported from the oxidation of BVOCs in laboratory chamber studies, providing evidence that the magnitude and chemical composition of biogenic SOA simulated in the laboratory is similar to that found in actual atmospheric conditions. The biogenic factor OM is also correlated to dust elements, indicating that dust may act as a non-acidic SOA sink. This role is supported by the organic functional group composition and morphology of single particles, which were analyzed

  16. Marine aerosol formation from biogenic iodine emissions.

    PubMed

    O'Dowd, Colin D; Jimenez, Jose L; Bahreini, Roya; Flagan, Richard C; Seinfeld, John H; Hämeri, Kaarle; Pirjola, Liisa; Kulmala, Markku; Jennings, S Gerard; Hoffmann, Thorsten

    2002-06-01

    The formation of marine aerosols and cloud condensation nuclei--from which marine clouds originate--depends ultimately on the availability of new, nanometre-scale particles in the marine boundary layer. Because marine aerosols and clouds scatter incoming radiation and contribute a cooling effect to the Earth's radiation budget, new particle production is important in climate regulation. It has been suggested that sulphuric acid derived from the oxidation of dimethyl sulphide is responsible for the production of marine aerosols and cloud condensation nuclei. It was accordingly proposed that algae producing dimethyl sulphide play a role in climate regulation, but this has been difficult to prove and, consequently, the processes controlling marine particle formation remains largely undetermined. Here, using smog chamber experiments under coastal atmospheric conditions, we demonstrate that new particles can form from condensable iodine-containing vapours, which are the photolysis products of biogenic iodocarbons emitted from marine algae. Moreover, we illustrate, using aerosol formation models, that concentrations of condensable iodine-containing vapours over the open ocean are sufficient to influence marine particle formation. We suggest therefore that marine iodocarbon emissions have a potentially significant effect on global radiative forcing. PMID:12050661

  17. Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

    2013-11-01

    Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding these transformation processes has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a Southeast Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high-resolution aerosol mass spectrometry and Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyl tetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

  18. Linking biogenic hydrocarbons to biogenic aerosol in the Borneo rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, J. F.; Alfarra, M. R.; Robinson, N.; Ward, M. W.; Lewis, A. C.; McFiggans, G. B.; Coe, H.; Allan, J. D.

    2013-07-01

    Emissions of biogenic volatile organic compounds are though to contribute significantly to secondary organic aerosol formation in the tropics, but understanding the process of these transformations has proved difficult, due to the complexity of the chemistry involved and very low concentrations. Aerosols from above a South East Asian tropical rainforest in Borneo were characterised using liquid chromatography-ion trap mass spectrometry, high resolution aerosol mass spectrometry and fourier transform ion cyclotron resonance mass spectrometry (FTICRMS) techniques. Oxygenated compounds were identified in ambient organic aerosol that could be directly traced back to isoprene, monoterpenes and sesquiterpene emissions, by combining field data on chemical structures with mass spectral data generated from synthetically produced products created in a simulation chamber. Eighteen oxygenated species of biogenic origin were identified in the rainforest aerosol from the precursors isoprene, α-pinene, limonene, α-terpinene and β-caryophyllene. The observations provide the unambiguous field detection of monoterpene and sesquiterpene oxidation products in SOA above a pristine tropical rainforest. The presence of 2-methyltetrol organosulfates and an associated sulfated dimer provides direct evidence that isoprene in the presence of sulfate aerosol can make a contribution to biogenic organic aerosol above tropical forests. High-resolution mass spectrometry indicates that sulfur can also be incorporated into oxidation products arising from monoterpene precursors in tropical aerosol.

  19. Molecular genetics and diversity of primary biogenic aerosol particles in urban, rural, and high-alpine air

    NASA Astrophysics Data System (ADS)

    Després, V.; Nowoisky, J.; Klose, M.; Conrad, R.; Andreae, M. O.; Pöschl, U.

    2007-02-01

    This study explores the applicability of molecular methods for the characterization of primary biogenic aerosol (PBA) particles in the atmosphere. Samples of fine particulate matter (PM2.5) and total suspended particulates (TSP) have been collected on different types of filter materials at urban, rural, and high-alpine locations along an altitude transect in the south of Germany (Munich, Hohenpeissenberg, Mt. Zugspitze). From filter aliquots loaded with about one milligram of air particulate matter, DNA could be extracted and DNA sequences could be determined for bacteria, fungi, plants and animals. Sequence analyses were used to determine the identity of biological organisms, and terminal restriction length polymorphism analyses (T-RFLP) were applied to estimate diversities and relative abundances of bacteria. Investigations of blank and background samples showed that filter materials have to be decontaminated prior to use, and that the sampling and handling procedures have to be carefully controlled to avoid artifacts in the analyses. Mass fractions of DNA in PM2.5 were found to be around 0.05% in urban, rural, and high alpine aerosols. The average concentration of DNA determined for urban air was on the order of ~7 ng m-3, indicating that human adults may inhale about one microgram of DNA per day (corresponding to ~105 haploid human genomes). Most of the bacterial sequences found in PM2.5 were from Proteobacteria (42) and some from Actinobacteria (10) and Firmicutes (1). The fungal sequences were characteristic for Ascomycota (3) and Basidiomycetes (1), which are known to actively discharge spores into the atmosphere. The plant sequences could be attributed to green plants (2) and moss spores (2), while animal DNA was found only for one unicellular eukaryote (protist). Over 80% of the 53 bacterial sequences could be matched with about 40% of the 19 T-RF peaks (58 to 494 base pair length) found in the investigated PM2.5 samples. The results demonstrate that the T

  20. Aerosols-cloud-climate -interactions in the Norwegian Earth System Model (NorESM). Importance of biogenic particles for cloud properties and anthropogenic indirect effect.

    NASA Astrophysics Data System (ADS)

    Seland, Ø.; Iversen, T.; Kirkevâg, A.

    2012-04-01

    According to the 4th assessment report of IPCC, major sources of uncertainty in anthropogenic climate change projections are inaccurate model description and weak knowledge of aerosols and their interactions with radiation and clouds, as well as the cloud feedback to radiative forcing. One important aspect of the associated uncertainty is the natural atmosphere. Anthropogenic climate change is an increment caused by anthropogenic emissions relative to the properties of the climate system untouched by man. This is crucial for the direct and indirect effects of aerosols, since the amount, size and physical properties of natural background particles strongly influence the same properties of the anthropogenic aerosol components. In many climate models where CDNC is calculated explicitly, CDNC is constrained by prescribing a lower bound below which calculated values are not allowed. This is done in order to keep the aerosol in-direct effect within estimated values. The rationale for using such a lower bound is to keep the aerosol radiative forcing constrained by the forcing of green-house gases and 20th century climate.We hypothesize this lower bound can be removed or made less strict by including aerosols of biogenic origin. We will present results and sensitivity studies from simulations with the NorESM where we have added contributions from organic carbon of natural origin both from vegetation and oceanic sources. By including aerosols of biogenic origin we obtain close to the median indirect radiative forcing reported by IPCC AR4, as well as reproducing the temperature increase in the 20th century. NorESM is based on the Earth system model CCSM4.0 from NCAR, but is using CAM4-Oslo instead of CAM4 as atmosphere model and an updated version of MICOM from the Bergen Climate Model (BCM) instead of the ocean model POP2. The aerosol module includes sea-salt, dust, sulphate, black carbon (BC) and particulate organic matter (OM). Primary aerosol size-distributions are

  1. Characterization of submicron particles influenced by mixed biogenic and anthropogenic emissions using high-resolution aerosol mass spectrometry: results from CARES

    SciTech Connect

    Setyan, Ari; Zhang, Qi; Merkel, M.; Knighton, Walter B.; Sun, Y.; Song, Chen; Shilling, John E.; Onasch, Timothy B.; Herndon, Scott C.; Worsnop, Douglas R.; Fast, Jerome D.; Zaveri, Rahul A.; Berg, Larry K.; Wiedensohler, A.; Flowers, B. A.; Dubey, Manvendra K.; Subramanian, R.

    2012-09-11

    The Carbonaceous Aerosols and Radiative Effects Study (CARES) took place in the Sacramento Valley of California in summer 2010. We present results obtained at Cool, CA, the T1 site of the project ({approx}40 km downwind of urban emissions from Sacramento), where we deployed an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) in parallel with complementary instrumentation to characterize the sources and processes of submicron particles (PM1). Cool is located at the foothill of the Sierra Nevada Mountains, where intense biogenic emissions are periodically mixed with urban outflow transported by daytime southwesterly winds from the Sacramento metropolitan area. The particle mass loading was low (3.0 {micro}gm{sup -3} on average) and dominated by organics (80% of the PM1 mass) followed by sulfate (9.9 %). Organics and sulfate appeared to be externally mixed, as suggested by their different time series (r2 = 0.13) and size distributions. Sulfate showed a bimodal distribution with a droplet mode peaking at {approx}400nm in vacuum aerodynamic diameter (Dva), and a condensation mode at {approx}150 nm, while organics generally displayed a broad distribution in 60-600nm (Dva). New particle formation and growth events were observed almost every day, emphasizing the roles of organics and sulfate in new particle growth, especially that of organics. The organic aerosol (OA) had a nominal formula of C{sub 1}H{sub 1.38}N{sub 0.004}O{sub 0.44}, thus an average organic mass-to-carbon (OM/OC) ratio of 1.70. Two different oxygenated OA (OOA, 90% of total OA mass) and a hydrocarbon-like OA (HOA, 10 %) were identified by Positive matrix factorization (PMF) of the high resolution mass spectra. The more oxidized MO-OOA (O/C = 0.54) corresponded to secondary OA (SOA) primarily influenced by biogenic emissions, while the less oxidized LO-OOA (O/C = 0.42) corresponded to SOA associated with urban transport. The HOA factor corresponded to primary emissions mainly

  2. Assessment of biogenic secondary organic aerosol in the Himalayas

    NASA Astrophysics Data System (ADS)

    Stone, B. A.; Nguyen, T.; Pradhan, B.; Dangol, P.

    2012-12-01

    Biogenic contributions to secondary organic aerosol (SOA) in the Southeast Asian regional haze were assessed by measurement of particle-phase isoprene, monoterpene, and sesquiterpene photooxidation products in fine particles (PM2.5) at Godavari, Nepal, located in the Himalayas at an elevation of 1600 meters. Organic species were measured in solvent-extracts of filter samples using gas chromatography mass spectrometry (GCMS) and chemical derivatization. Molecular markers for primary aerosol sources—including motor vehicles, biomass burning, and detritus—and SOA tracers were measured. High concentrations of isoprene derivatives, particularly in the late summer months, point to biogenic SOA as a significant source of organic carbon in the Himalayan region. First-generation SOA products from alpha-pinene were detected in all samples, whereas multi-generation products were not, suggesting that monoterpenes were at an early stage of oxidation at Godavari. Biogenic SOA contributions to PM2.5 organic carbon in the 2005 monsoon and post-monsoon season ranged from 2-19% for isoprene, 1-5% for monoterpenes, and 1-4% for sesquiterpenes. Primary and secondary biogenic sources combined accounted for approximately half of observed organic aerosol, suggesting additional aerosol sources and/or precursors are significant in this region.

  3. Organosulfate Formation in Biogenic Secondary Organic Aerosol

    EPA Science Inventory

    Organosulfates of isoprene, α-pinene, and β-pinene have recently been identified in both laboratory-generated and ambient secondary organic aerosol (SOA). In this study, the mechanism and ubiquity of organosulfate formation in biogenic SOA is investigated by a comprehensive seri...

  4. The impact of port emissions and marine biogenics on the single-particle chemistry of marine aerosol measured on board the R/V Atlantis during the CalNEX 2010 field campaign

    NASA Astrophysics Data System (ADS)

    Gaston, C. J.; Quinn, P.; Bates, T. S.; Prather, K. A.

    2010-12-01

    Marine environments are characterized by low particle concentrations and, as such, are sensitive to changes in particle number concentration and chemistry induced by biogenic and anthropogenic influences. Measurements of both gas phase and particle phase emissions on board the R/V Atlantis during the CalNEX 2010 field campaign provided an opportunity to examine the impact of anthropogenic and marine biogenic emissions on particle chemistry along the California coast. Real-time, single-particle measurements made using an aerosol time-of-flight mass spectrometer (ATOFMS) revealed the single-particle mixing state of the sampled marine aerosols. Submicron particles (0.2-1.0 um) containing organic carbon, elemental carbon mixed with organic carbon, and unique V-containing particles previously detected in port regions were prevalent throughout the Southern California coast; most of these particles were also associated with sulfate. Measurements made in the deep water channel near Sacramento, CA revealed dramatically different particle chemistry that was characterized by organic carbon and amines. Particles measured further away from the continent toward the open ocean were influenced by marine biological activity due to a phytoplankton bloom that was occurring off the California coast. During this sampling period, unique ocean-derived particles containing internal mixtures of Mg and organic carbon were detected in addition to unique particles containing elemental S ions, which were only detected at night. An aerosol generator used to bubble seawater in order to characterize primary emissions from the ocean confirmed that the Mg-organic carbon and S-containing particles were indeed emitted from the ocean. These measurements reveal the strong impact of both port emissions as well as marine biogenic emissions on aerosol chemistry along the California coast.

  5. Biogenic amines in submicron marine aerosol (Invited)

    NASA Astrophysics Data System (ADS)

    Facchini, M.

    2010-12-01

    Ammonium salts of dimethyl and diethyl amine (DMA+ and DEA+) have been detected in size segregated marine samples collected in the North Atlantic over open ocean and at a coastal site. DMA+ and DEA+ peak in the accumulation mode range while very low concentration, close to detection limit, are observed in the coarse size fractions, as well as in sea spray aerosol artificially generated in the laboratory using sea water. These results indicate a secondary formation pathway. DMA+ and DEA+ represent up to 20% of secondary organic aerosol (SOA) in our samples , and to our knowledge they are the most abundant organic species besides MSA ever detected in clean marine aerosol . Maximum concentrations have been observed during spring and summer when the biological activity is high and in clean marine air masses, thus indicating biogenic sources. Total organic nitrogen (ON) concentration also peaks in the accumulation mode range and represents in our samples a fraction from 32 to 54 % of the total SOA. Ammonium salt formation from biogenic amines might be an important source of marine SOA and atmospheric nitrogen at the global scale with a seasonal variation connected to the oceanic biological productivity and an atmospheric cycle parallel to that of the organosulfur species.

  6. biogenic aerosol precursors: volatile amines from agriculture

    NASA Astrophysics Data System (ADS)

    Kuhn, Uwe; Sintermann, Jörg; Spirig, Christoph; Ammann, Christof; Neftel, Albrecht

    2010-05-01

    Information on the occurrence of volatile biogenic amines in the atmosphere is marginal. This group of N-bearing organic compounds are assumed to be a small, though significant component of the atmospheric N-cycle, but are not accounted for in global assessments due to the scarceness of available data. There is increasing evidence for an important role of biogenic amines in the formation of new particulate matter, as well as for aerosol secondary growth. Volatile amines are ubiquitously formed by biodegradation of organic matter, and agriculture is assumed to dominantly contribute to their atmospheric burden. Here we show that the mixing ratios of volatile amines within livestock buildings scale about 2 orders of magnitude lower than NH3, confirming the few literature data available (e.g., Schade and Crutzen, J. Atm. Chem. 22, 319-346, 1995). Flux measurements after manure application in the field, mixing ratios in the headspace of manure storage pools, and concentrations in distilled manure all indicate major depletion of amines relative to NH3 during manure processing. We conclude that the agricultural source distribution of NH3 and amines is not similar. While for NH3 the spreading of manure in the field dominates agricultural emissions, the direct release from livestock buildings dominates the budget of volatile biogenic amines.

  7. Cluster analysis on mass spectra of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Spindler, C.; Kiendler-Scharr, A.; Kleist, E.; Mensah, A.; Mentel, T.; Tillmann, R.; Wildt, J.

    2009-04-01

    Biogenic secondary organic aerosols (BSOA) are of high importance in the atmosphere. The formation of SOA from the volatile organic compound (VOC) emissions of selected trees was investigated in the JPAC (Jülich Plant Aerosol Chamber) facility. The VOC (mainly monoterpenes) were transferred into a reaction chamber where vapors were photo-chemically oxidized and formed BSOA. The aerosol was characterized by aerosol mass spectrometry (Aerodyne Quadrupol-AMS). Inside the AMS, flash-vaporization of the aerosol particles and electron impact ionization of the evaporated molecules cause a high fragmentation of the organic compounds. Here, we present a classification of the aerosol mass spectra via cluster analysis. Average mass spectra are produced by combination of related single mass spectra to so-called clusters. The mass spectra were similar due to the similarity of the precursor substances. However, we can show that there are differences in the BSOA mass spectra of different tree species. Furthermore we can distinguish the influence of the precursor chemistry and chemical aging. BSOA formed from plants exposed to stress can be distinguished from BSOA formed under non stressed conditions. Significance and limitations of the clustering method for very similar mass spectra will be demonstrated and discussed.

  8. The Radiative Forcing from Biogenic Secondary Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Scott, C. E.; Forster, P.; Spracklen, D. V.; Carslaw, K. S.; Arnold, S.; Rap, A.

    2012-12-01

    Vegetation emits biogenic volatile organic compounds (BVOCs), such as monoterpenes, isoprene and sesquiterpenes, into the atmosphere. Once emitted, BVOCs rapidly undergo reactions with the hydroxyl radical, ozone and the nitrate radical to yield a range of lower volatility oxidation products. These compounds are of sufficiently low volatility to partition into the aerosol phase, forming secondary organic aerosol (SOA). Increasingly, there are indications that organic compounds, specifically the oxidation products of terpenes, may contribute to the process of new particle formation as well as the growth of existing particles. The formation of SOA can influence the Earth's radiative balance by absorbing and scattering radiation (the direct effect) and by altering the properties of clouds (the indirect effect), via their action as cloud condensation nuclei (CCN). Biogenic SOA formed from the oxidation products of isoprene and monoterpenes has been shown to be CCN active under atmospherically relevant conditions, indicating that complex climate feedbacks may result from the emission of BVOCs. Using a global aerosol microphysics model (GLOMAP), and offline radiative transfer code, we simulate a present day aerosol indirect radiative forcing of between -0.07 and - 0.81 W.m-2, for the emission of BVOCs, due to a simulated increase in the number of particles able to act as CCN. The forcing obtained per emission is not spatially uniform, with monoterpenes in the southern hemisphere being most efficient at inducing a radiative change. We find a strong sensitivity to the treatment of concurrent anthropogenic emissions. In the present day, biogenic secondary organic material is more efficient at perturbing CCN number concentrations, but when anthropogenic emissions from 1750 are included in our simulations, the lower background aerosol concentration results in a more significant radiative response. The largest uncertainty in the forcing obtained however, comes from the

  9. Characterization of primary biogenic aerosol particles in urban, rural, and high-alpine air by DNA sequence and restriction fragment analysis of ribosomal RNA genes

    NASA Astrophysics Data System (ADS)

    Després, V. R.; Nowoisky, J. F.; Klose, M.; Conrad, R.; Andreae, M. O.; Pöschl, U.

    2007-12-01

    This study explores the applicability of DNA analyses for the characterization of primary biogenic aerosol (PBA) particles in the atmosphere. Samples of fine particulate matter (PM2.5) and total suspended particulates (TSP) have been collected on different types of filter materials at urban, rural, and high-alpine locations along an altitude transect in the south of Germany (Munich, Hohenpeissenberg, Mt. Zugspitze). From filter segments loaded with about one milligram of air particulate matter, DNA could be extracted and DNA sequences could be determined for bacteria, fungi, plants and animals. Sequence analyses were used to determine the identity of biological organisms, and terminal restriction fragment length polymorphism analyses (T-RFLP) were applied to estimate diversities and relative abundances of bacteria. Investigations of blank and background samples showed that filter materials have to be decontaminated prior to use, and that the sampling and handling procedures have to be carefully controlled to avoid artifacts in the analyses. Mass fractions of DNA in PM2.5 were found to be around 0.05% in urban, rural, and high-alpine aerosols. The average concentration of DNA determined for urban air was on the order of ~7 ng m-3, indicating that human adults may inhale about one microgram of DNA per day (corresponding to ~108 haploid bacterial genomes or ~105 haploid human genomes, respectively). Most of the bacterial sequences found in PM2.5 were from Proteobacteria (42) and some from Actinobacteria (10) and Firmicutes (1). The fungal sequences were characteristic for Ascomycota (3) and Basidiomycota (1), which are known to actively discharge spores into the atmosphere. The plant sequences could be attributed to green plants (2) and moss spores (2), while animal DNA was found only for one unicellular eukaryote (protist). Over 80% of the 53 bacterial sequences could be matched to one of the 19 T-RF peaks found in the PM2.5 samples, but only 40% of the T-RF peaks

  10. Biogenic, anthropogenic and sea salt sulfate size-segregated aerosols in the Arctic summer

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhad, Roghayeh; Norman, Ann-Lise; Abbatt, Jonathan P. D.; Levasseur, Maurice; Thomas, Jennie L.

    2016-04-01

    Size-segregated aerosol sulfate concentrations were measured on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic during July 2014. The objective of this study was to utilize the isotopic composition of sulfate to address the contribution of anthropogenic and biogenic sources of aerosols to the growth of the different aerosol size fractions in the Arctic atmosphere. Non-sea-salt sulfate is divided into biogenic and anthropogenic sulfate using stable isotope apportionment techniques. A considerable amount of the average sulfate concentration in the fine aerosols with a diameter < 0.49 µm was from biogenic sources (> 63 %), which is higher than in previous Arctic studies measuring above the ocean during fall (< 15 %) (Rempillo et al., 2011) and total aerosol sulfate at higher latitudes at Alert in summer (> 30 %) (Norman et al., 1999). The anthropogenic sulfate concentration was less than that of biogenic sulfate, with potential sources being long-range transport and, more locally, the Amundsen's emissions. Despite attempts to minimize the influence of ship stack emissions, evidence from larger-sized particles demonstrates a contribution from local pollution. A comparison of δ34S values for SO2 and fine aerosols was used to show that gas-to-particle conversion likely occurred during most sampling periods. δ34S values for SO2 and fine aerosols were similar, suggesting the same source for SO2 and aerosol sulfate, except for two samples with a relatively high anthropogenic fraction in particles < 0.49 µm in diameter (15-17 and 17-19 July). The high biogenic fraction of sulfate fine aerosol and similar isotope ratio values of these particles and SO2 emphasize the role of marine organisms (e.g., phytoplankton, algae, bacteria) in the formation of fine particles above the Arctic Ocean during the productive summer months.

  11. Biogenic Contributions to Summertime Arctic Aerosol: Observations of Aerosol Composition from the Netcare 2014 Aircraft Campaign

    NASA Astrophysics Data System (ADS)

    Willis, M. D.; Burkart, J.; Koellner, F.; Schneider, J.; Bozem, H.; Hoor, P. M.; Brauner, R.; Herber, A. B.; Leaitch, W. R.; Abbatt, J.

    2014-12-01

    The Arctic is a complex and poorly studied aerosol environment, impacted by strong anthropogenic contributions during winter months and by regional sources in cleaner summer months. In order to gain a predictive understanding of the changing climate in this region, it is necessary to understand the balance between these two aerosol sources to clarify how aerosol might be altered by or contribute to climate change. We present results of vertically resolved, submicron aerosol composition from an Aerodyne high-resolution aerosol mass spectrometer (AMS) during the NETCARE 2014 Polar6 aircraft campaign. The campaign was based in the high Arctic, at Resolute, NU (74°N), allowing measurements from 60 to 2900 meters over ice, open water and near the ice-edge. Concurrent measurements aboard the Polar6 included ultrafine and accumulation mode particle number and size, cloud condensation nuclei concentrations, trace gas concentrations and single particle composition. Aerosol vertical profiles measured by the AMS can be broadly characterized into two regimes corresponding to different meteorological conditions: the first with very low aerosol loading (<0.1 μg/m3) at low altitudes compared to that aloft and high numbers of nucleation mode particles, and the second with higher concentrations at lower levels. This second regime was associated with low concentrations of nucleation mode particles, and higher observable levels of methane sulphonic acid (MSA) from AMS measurements at low altitudes. MSA, produced during the oxidation of dimethyl sulphide, is a marker for the contribution of ocean-derived biogenic sulphur to particulate sulphur and could be identified and quantified using the high-resolution AMS. MSA to sulphate ratios were observed to increase towards lower altitudes, suggesting a contribution to aerosol loading from the ocean. In addition, we present measurements of aerosol neutralization and the characteristics of organic aerosol that relate to the growth of

  12. Rapid Detection and Identification of Biogenic Aerosol Releases and Sources

    NASA Astrophysics Data System (ADS)

    Wagner, J.; Macher, J.; Ghosal, S.; Ahmed, K.; Hemati, K.; Wall, S.; Kumagai, K.

    2011-12-01

    Biogenic aerosols can be important contributors to aerosol chemistry, cloud droplet and ice nucleation, absorption and scattering of radiation, human health and comfort, and plant, animal, and microbial ecology. Many types of bioaerosols, e.g., fungal spores, are released into the atmosphere in response to specific climatological and meteorological conditions. The rapid identification of bioaerosol releases is thus important for better characterization of the above phenomena, as well as enabling public officials to respond quickly and appropriately to releases of infectious agents or biological toxins. One approach to rapid and accurate bioaerosol detection is to employ sequential, automated samples that can be fed directly into an image acquisition and data analysis device. Raman spectroscopy-based identification of bioaerosols, automated analysis of microscopy images, and automated detection of near-monodisperse peaks in aerosol size-distribution data were investigated as complementary approaches to traditional, manual methods for the identification and counting of fungal and actinomycete spores. Manual light microscopy is a widely used analytical technique that is compatible with a number of air sample formats and requires minimal sample preparation. However, a major drawback is its dependence on a human analyst's ability to distinguish particles and accurately count, size, and identify them. Therefore, automated methods, such as those evaluated in this study, have the potential to provide cost-effective and rapid alternatives if demonstrated to be accurate and reliable. An exploratory examination of individual spores for several macro- and microfungi (those with and without large fruiting bodies) by Raman microspectroscopy found unique spectral features that were used to identify fungi to the genus level. Automated analyses of digital spore images accurately recognized and counted single fungal spores and clusters. An automated procedure to discriminate near

  13. Fungal spores overwhelm biogenic organic aerosols in a midlatitudinal forest

    NASA Astrophysics Data System (ADS)

    Zhu, Chunmao; Kawamura, Kimitaka; Fukuda, Yasuro; Mochida, Michihiro; Iwamoto, Yoko

    2016-06-01

    Both primary biological aerosol particles (PBAPs) and oxidation products of biogenic volatile organic compounds (BVOCs) contribute significantly to organic aerosols (OAs) in forested regions. However, little is known about their relative importance in diurnal timescales. Here, we report biomarkers of PBAP and secondary organic aerosols (SOAs) for their diurnal variability in a temperate coniferous forest in Wakayama, Japan. Tracers of fungal spores, trehalose, arabitol and mannitol, showed significantly higher levels in nighttime than daytime (p < 0.05), resulting from the nocturnal sporulation under near-saturated relative humidity. On the contrary, BVOC oxidation products showed higher levels in daytime than nighttime, indicating substantial photochemical SOA formation. Using tracer-based methods, we estimated that fungal spores account for 45 % of organic carbon (OC) in nighttime and 22 % in daytime, whereas BVOC oxidation products account for 15 and 19 %, respectively. To our knowledge, we present for the first time highly time-resolved results that fungal spores overwhelmed BVOC oxidation products in contributing to OA especially in nighttime. This study emphasizes the importance of both PBAPs and SOAs in forming forest organic aerosols.

  14. Sub-Antarctic marine aerosol: significant contributions from biogenic sources

    NASA Astrophysics Data System (ADS)

    Schmale, J.; Schneider, J.; Nemitz, E.; Tang, Y. S.; Dragosits, U.; Blackall, T. D.; Trathan, P. N.; Phillips, G. J.; Sutton, M.; Braban, C. F.

    2013-03-01

    Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea salt sulfate 2% nitrate, 7% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea salt signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acids/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 40%), a sea salt OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (C : N ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea salt aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated to sea

  15. Sub-Antarctic marine aerosol: dominant contributions from biogenic sources

    NASA Astrophysics Data System (ADS)

    Schmale, J.; Schneider, J.; Nemitz, E.; Tang, Y. S.; Dragosits, U.; Blackall, T. D.; Trathan, P. N.; Phillips, G. J.; Sutton, M.; Braban, C. F.

    2013-09-01

    Biogenic influences on the composition and characteristics of aerosol were investigated on Bird Island (54°00' S, 38°03' W) in the South Atlantic during November and December 2010. This remote marine environment is characterised by large seabird and seal colonies. The chemical composition of the submicron particles, measured by an aerosol mass spectrometer (AMS), was 21% non-sea-salt sulfate, 2% nitrate, 8% ammonium, 22% organics and 47% sea salt including sea salt sulfate. A new method to isolate the sea spray signature from the high-resolution AMS data was applied. Generally, the aerosol was found to be less acidic than in other marine environments due to the high availability of ammonia, from local fauna emissions. By positive matrix factorisation five different organic aerosol (OA) profiles could be isolated: an amino acid/amine factor (AA-OA, 18% of OA mass), a methanesulfonic acid OA factor (MSA-OA, 25%), a marine oxygenated OA factor (M-OOA, 41%), a sea spray OA fraction (SS-OA, 7%) and locally produced hydrocarbon-like OA (HOA, 9%). The AA-OA was dominant during the first two weeks of November and found to be related with the hatching of penguins in a nearby colony. This factor, rich in nitrogen (N : C ratio = 0.13), has implications for the biogeochemical cycling of nitrogen in the area as particulate matter is often transported over longer distances than gaseous N-rich compounds. The MSA-OA was mainly transported from more southerly latitudes where phytoplankton bloomed. The bloom was identified as one of three sources for particulate sulfate on Bird Island, next to sea salt sulfate and sulfate transported from South America. M-OOA was the dominant organic factor and found to be similar to marine OA observed at Mace Head, Ireland. An additional OA factor highly correlated with sea spray aerosol was identified (SS-OA). However, based on the available data the type of mixture, internal or external, could not be determined. Potassium was not associated

  16. Historical anthropogenic radiative forcing of changes in biogenic secondary aerosol

    NASA Astrophysics Data System (ADS)

    Acosta Navarro, Juan; D'Andrea, Stephen; Pierce, Jeffrey; Ekman, Annica; Struthers, Hamish; Zorita, Eduardo; Guenther, Alex; Arneth, Almut; Smolander, Sampo; Kaplan, Jed; Farina, Salvatore; Scott, Catherine; Rap, Alexandru; Farmer, Delphine; Spracklen, Domink; Riipinen, Ilona

    2016-04-01

    Human activities have lead to changes in the energy balance of the Earth and the global climate. Changes in atmospheric aerosols are the second largest contributor to climate change after greenhouse gases since 1750 A.D. Land-use practices and other environmental drivers have caused changes in the emission of biogenic volatile organic compounds (BVOCs) and secondary organic aerosol (SOA) well before 1750 A.D, possibly causing climate effects through aerosol-radiation and aerosol-cloud interactions. Two numerical emission models LPJ-GUESS and MEGAN were used to quantify the changes in aerosol forming BVOC emissions in the past millennium. A chemical transport model of the atmosphere (GEOS-Chem-TOMAS) was driven with those BVOC emissions to quantify the effects on radiation caused by millennial changes in SOA. We found that global isoprene emissions decreased after 1800 A.D. by about 12% - 15%. This decrease was dominated by losses of natural vegetation, whereas monoterpene and sesquiterpene emissions increased by about 2% - 10%, driven mostly by rising surface air temperatures. From 1000 A.D. to 1800 A.D, isoprene, monoterpene and sesquiterpene emissions decline by 3% - 8% driven by both, natural vegetation losses, and the moderate global cooling between the medieval climate anomaly and the little ice age. The millennial reduction in BVOC emissions lead to a 0.5% to 2% reduction in climatically relevant aerosol particles (> 80 nm) and cause a direct radiative forcing between +0.02 W/m² and +0.07 W/m², and an indirect radiative forcing between -0.02 W/m² and +0.02 W/m².

  17. Reversible and irreversible processing of biogenic olefins on acidic aerosols

    NASA Astrophysics Data System (ADS)

    Liggio, J.; Li, S.-M.

    2008-04-01

    Recent evidence has suggested that heterogeneous chemistry of oxygenated hydrocarbons, primarily carbonyls, plays a role in the formation of secondary organic aerosol (SOA); however, evidence is emerging that direct uptake of alkenes on acidic aerosols does occur and can contribute to SOA formation. In the present study, significant uptake of monoterpenes, oxygenated monoterpenes and sesquiterpenes to acidic sulfate aerosols is found under various conditions in a reaction chamber. Proton transfer mass spectrometry is used to quantify the organic gases, while an aerosol mass spectrometer is used to quantify the organic mass uptake and obtain structural information for heterogeneous products. Aerosol mass spectra are consistent with several mechanisms including acid catalyzed olefin hydration, cationic polymerization and organic ether formation, while measurable decreases in the sulfate mass on a per particle basis suggest that the formation of organosulfate compounds is also likely. A portion of the heterogeneous reactions appears to be reversible, consistent with reversible olefin hydration reactions. A slow increase in the organic mass after a fast initial uptake is attributed to irreversible reactions, consistent with polymerization and organosulfate formation. Uptake coefficients (γ) were estimated for a fast initial uptake governed by the mass accommodation coefficient (α) and ranged from 1×10-6-2.5×10-2. Uptake coefficients for a subsequent slower reactive uptake ranged from 1×10-7-1×10-4. These processes may potentially lead to a considerable amount of SOA from the various biogenic hydrocarbons under acidic conditions, which can be highly significant for freshly nucleated aerosols, particularly given the large array of atmospheric olefins.

  18. Characterization of Highly Oxidized Molecules in Fresh and Aged Biogenic Secondary Organic Aerosol.

    PubMed

    Tu, Peijun; Hall, Wiley A; Johnston, Murray V

    2016-04-19

    In this work, highly oxidized multifunctional molecules (HOMs) in fresh and aged secondary organic aerosol (SOA) derived from biogenic precursors are characterized with high-resolution mass spectrometry. Fresh SOA was generated by mixing ozone with a biogenic precursor (β-pinene, limonene, α-pinene) in a flow tube reactor. Aging was performed by passing the fresh SOA through a photochemical reactor where it reacted with hydroxyl radicals. Although these aerosols were as a whole not highly oxidized, molecular analysis identified a significant number of HOMs embedded within it. HOMs in fresh SOA consisted mostly of monomers and dimers, which is consistent with condensation of extremely low-volatility organic compounds (ELVOCs) that have been detected in the gas phase in previous studies and linked to SOA particle formation. Aging caused an increase in the average number of carbon atoms per molecule of the HOMs, which is consistent with particle phase oxidation of (less oxidized) oligomers already existing in fresh SOA. HOMs having different combinations of oxygen-to-carbon ratio, hydrogen-to-carbon ratio and average carbon oxidation state are discussed and compared to low volatility oxygenated organic aerosol (LVOOA), which has been identified in ambient aerosol based on average elemental composition but not fully understood at a molecular level. For the biogenic precursors and experimental conditions studied, HOMs in fresh biogenic SOA have molecular formulas more closely resembling LVOOA than HOMs in aged SOA, suggesting that aging of biogenic SOA is not a good surrogate for ambient LVOOA. PMID:27000653

  19. Reversible and irreversible processing of biogenic olefins on acidic aerosols

    NASA Astrophysics Data System (ADS)

    Liggio, J.; Li, S.-M.

    2007-08-01

    Recent evidence has suggested that heterogeneous chemistry of oxygenated hydrocarbons, primarily carbonyls, plays a role in the formation of secondary organic aerosol (SOA); however, evidence is emerging that direct uptake of alkenes on acidic aerosols does occur and can contribute to SOA formation. In the present study, significant uptake of monoterpenes, oxygenated monoterpenes and sesquiterpenes to acidic sulfate aerosols is found under various conditions in a reaction chamber. Proton transfer mass spectrometry is used to quantify the organic gases, while an aerosol mass spectrometer is used to quantify the organic mass uptake and obtain structural information for heterogeneous products. Aerosol mass spectra are consistent with several mechanisms including acid catalyzed olefin hydration, cationic polymerization and organic ester formation, while measurable decreases in the sulfate mass on a per particle basis suggest that the formation of organosulfate compounds is also likely. A portion of the heterogeneous reactions appears to be reversible, consistent with reversible olefin hydration reactions. A slow increase in the organic mass after a fast initial uptake is attributed to irreversible reactions, consistent with polymerization and organosulfate formation. Uptake coefficients (γ) were estimated for a fast initial uptake governed by the mass accommodation coefficient (α) and ranged from 1×10-6-2.5×10-2. Uptake coefficients for a subsequent slower reactive uptake ranged from 1×10-7-1×10-4. These processes are estimated to potentially produce greater than 2.5 μg m-3 of SOA from the various biogenic hydrocarbons under atmospheric conditions, which can be highly significant given the large array of atmospheric olefins.

  20. Ice Formation Potential of Field-Collected Marine Biogenic Particles

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

    Marine biogenic particles composed mainly of sea salt and organic material aerosolized from a mesocosm in laboratory experiments have recently been found to act as ice nuclei. How these particles relate to those collected from sea spray under ambient conditions in the field is unknown. This study reports on the heterogeneous ice nucleation potential of particles collected during the marine aerosol characterization experiment (MACE) on the south shore of Long Island, New York. Ambient aerosol size distributions were measured and particles were collected on hydrophobically coated substrates and subsequently used for ice nucleation experiments using an ice nucleation cell coupled to an optical microscope. This technique allows detection of ice formation for temperatures between 200 and 273 K and for relative humidity with respect to ice (RHice) from 100% up to water saturation. Individual ice nucleating particles were identified for subsequent chemical and physical characterization using both X-ray and electron micro-spectroscopic techniques. Concentrations of bacteria, viruses, and transparent exopolymer particles (TEP) in the bulk seawater, sea-surface microlayer (SML), and in sea spray were determined using established methods and related to airborne sea spray particles and their ice nucleation potential. Onshore aerosol size distribution measurements taken at 5 m height and 10 m away from the breaking waves, revealed a peak maximum at 100 nm and Ntot = 6.8 x 10^2 cm^-3. Bacterial, viral, and TEP were found to be enriched in the SML. Ambient particles collected during MACE were found to nucleate ice efficiently, e. g. at 215 K, ice nucleation occurred on average at 125% RHice. Results of aerosol size distributions and ice nucleation efficiencies are compared to laboratory bubble bursting experiments in which natural seawater was used. The goal of this study is to understand the connection between sea spray aerosolization and atmospheric ice cloud formation and to

  1. The influence of marine biogenic particles on ice phase initiation

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

    Aerosol particles vary in composition with many being biogenic and of terrestrial or marine origin. Efficient ice forming biogenic particles are typically thought to be of terrestrial origin; however, recent data demonstrate that marine biogenic particles can act as ice nuclei (IN) in both immersion and deposition modes, with and without association of NaCl. These results are significant given that ocean derived particles including phytoplankton, microorganisms, transparent exopolymers, and colloidal gels become aerosolized from the sea surface microlayer through wave breaking and bubble bursting. Such particles typically include sea salt, but in situ observations of air masses associated with phytoplankton blooms have identified organic compounds as significant mass contributors to aerosol loading. Here we present results from experiments with Thalassiosira pseudonana, Emiliania huxleyi, and Nanochloris atomus, phytoplankton with distinctly different cell walls: silica, calcite, and cellulose fibrils, respectively, as efficient IN in immersion and deposition modes at typical tropospheric conditions. In a separate set of experiments, submicron size particles with and without organics are generated through bubble bursting in a custom built seawater tank. Subsequently collected, these particles are observed using a coupled cooling stage/optical microscope, for their ice nucleation potential as a function of particle temperature (T), water activity (aw), relative humidity with respect to ice (RHice), droplet volume, and particle surface area. In the immersion mode, fragmented and intact cells of T. pseudonana and N. atomus enhance ice nucleation in aqueous NaCl solution droplets by ~10-30 K and 10-20 K above the homogeneous freezing limit, and for a range of aw of 1.0-0.8, while E. huxleyi do not enhance freezing temperatures. In the deposition mode, all three species nucleate ice for RHice as low as ~120%, however, for each, different nucleation modes occur at warmer

  2. Incremental Reactivity Effects of Anthropogenic and Biogenic Volatile Organic Compounds on Secondary Organic Aerosol Formation

    NASA Astrophysics Data System (ADS)

    Kacarab, M.; Li, L.; Carter, W. P. L.; Cocker, D. R., III

    2015-12-01

    Two surrogate reactive organic gas (ROG) mixtures were developed to create a controlled reactivity environment simulating different urban atmospheres with varying levels of anthropogenic (e.g. Los Angeles reactivity) and biogenic (e.g. Atlanta reactivity) influences. Traditional chamber experiments focus on the oxidation of one or two volatile organic compound (VOC) precursors, allowing the reactivity of the system to be dictated by those compounds. Surrogate ROG mixtures control the overall reactivity of the system, allowing for the incremental aerosol formation from an added VOC to be observed. The surrogate ROG mixtures were developed based on that used to determine maximum incremental reactivity (MIR) scales for O3 formation from VOC precursors in a Los Angeles smog environment. Environmental chamber experiments were designed to highlight the incremental aerosol formation in the simulated environment due to the addition of an added anthropogenic (aromatic) or biogenic (terpene) VOC. All experiments were conducted in the UC Riverside/CE-CERT dual 90m3 environmental chambers. It was found that the aerosol precursors behaved differently under the two altered reactivity conditions, with more incremental aerosol being formed in the anthropogenic ROG system than in the biogenic ROG system. Further, the biogenic reactivity condition inhibited the oxidation of added anthropogenic aerosol precursors, such as m-xylene. Data will be presented on aerosol properties (density, volatility, hygroscopicity) and bulk chemical composition in the gas and particle phases (from a SYFT Technologies selected ion flow tube mass spectrometer, SIFT-MS, and Aerodyne high resolution time of flight aerosol mass spectrometer, HR-ToF-AMS, respectively) comparing the two controlled reactivity systems and single precursor VOC/NOx studies. Incremental aerosol yield data at different controlled reactivities provide a novel and valuable insight in the attempt to extrapolate environmental chamber

  3. Modeling organic aerosols during MILAGRO: importance of biogenic secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Hodzic, A.; Jimenez, J. L.; Madronich, S.; Aiken, A. C.; Bessagnet, B.; Curci, G.; Fast, J.; Lamarque, J.-F.; Onasch, T. B.; Roux, G.; Schauer, J. J.; Stone, E. A.; Ulbrich, I. M.

    2009-09-01

    The meso-scale chemistry-transport model CHIMERE is used to assess our understanding of major sources and formation processes leading to a fairly large amount of organic aerosols - OA, including primary OA (POA) and secondary OA (SOA) - observed in Mexico City during the MILAGRO field project (March 2006). Chemical analyses of submicron aerosols from aerosol mass spectrometers (AMS) indicate that organic particles found in the Mexico City basin contain a large fraction of oxygenated organic species (OOA) which have strong correspondence with SOA, and that their production actively continues downwind of the city. The SOA formation is modeled here by the one-step oxidation of anthropogenic (i.e. aromatics, alkanes), biogenic (i.e. monoterpenes and isoprene), and biomass-burning SOA precursors and their partitioning into both organic and aqueous phases. Conservative assumptions are made for uncertain parameters to maximize the amount of SOA produced by the model. The near-surface model evaluation shows that predicted OA correlates reasonably well with measurements during the campaign, however it remains a factor of 2 lower than the measured total OA. Fairly good agreement is found between predicted and observed POA within the city suggesting that anthropogenic and biomass burning emissions are reasonably captured. Consistent with previous studies in Mexico City, large discrepancies are encountered for SOA, with a factor of 2-10 model underestimate. When only anthropogenic SOA precursors were considered, the model was able to reproduce within a factor of two the sharp increase in OOA concentrations during the late morning at both urban and near-urban locations but the discrepancy increases rapidly later in the day, consistent with previous results, and is especially obvious when the column-integrated SOA mass is considered instead of the surface concentration. The increase in the missing SOA mass in the afternoon coincides with the sharp drop in POA suggesting a

  4. Science Plan Biogenic Aerosols – Effects on Clouds and Climate (BAECC)

    SciTech Connect

    Petäjä, T

    2013-12-01

    Atmospheric aerosol particles impact human health in urban environments, while on regional and global scales they can affect climate patterns, the hydrological cycle, and the intensity of radiation that reaches the Earth’s surface. In spite of recent advances in the understanding of aerosol formation processes and the links between aerosol dynamics and biosphere-atmosphere-climate interactions, great challenges remain in the analysis of related processes on a global scale. Boreal forests, situated in a circumpolar belt in the northern latitudes throughout the United States, Canada, Russia and Scandinavia, are among the most active areas of atmospheric aerosol formation among all biomes. The formation of aerosol particles and their growth to the sizes of cloud condensation nuclei in these areas are associated with biogenic volatile organic emissions from vegetation and soil.

  5. BAECC Biogenic Aerosols - Effects on Clouds and Climate

    SciTech Connect

    Petäjä, Tuukka; Moisseev, Dmitri; Sinclair, Victoria; O'Connor, Ewan J.; Manninen, Antti J.; Levula, Janne; Väänänen, Riikka; Heikkinen, Liine; Äijälä, Mikko; Aalto, Juho; Bäck, Jaana

    2015-11-01

    Biogenic Aerosols - Effects on Clouds and Climate (BAECC)”, featured the U.S. Department of Energy’s Atmospheric Radiation Measurement (ARM) Program’s 2nd Mobile Facility (AMF2) in Hyytiälä, Finland. It operated for an 8-month intensive measurement campaign from February to September 2014. The main research goal was to understand the role of biogenic aerosols in cloud formation. One of the reasons to perform BAECC study in Hyytiälä was the fact that it hosts SMEAR-II (Station for Measuring Forest Ecosystem-Atmosphere Relations), which is one of the world’s most comprehensive surface in-situ observation sites in a boreal forest environment. The station has been measuring atmospheric aerosols, biogenic emissions and an extensive suite of parameters relevant to atmosphere-biosphere interactions continuously since 1996. The BAECC enables combining vertical profiles from AMF2 with surface-based in-situ SMEAR-II observations and allows the processes at the surface to be directly related to processes occurring throughout the entire tropospheric column. With the inclusion of extensive surface precipitation measurements, and intensive observation periods involving aircraft flights and novel radiosonde launches, the complementary observations of AMF2 and SMEAR-II provide a unique opportunity for investigating aerosol-cloud interactions, and cloud-to-precipitation processes. The BAECC dataset will initiate new opportunities for evaluating and improving models of aerosol sources and transport, cloud microphysical processes, and boundary-layer structures.

  6. Comparing Organic Aerosol Composition from Marine Biogenic Sources to Seawater and to Physical Sea Spray Models

    NASA Astrophysics Data System (ADS)

    Russell, L. M.; Frossard, A. A.; Sanchez, K.; Massoli, P.; Elliott, S.; Burrows, S. M.; Bates, T. S.; Quinn, P.

    2015-12-01

    In much of the marine atmosphere, organic components in aerosol particles have many sources other than sea spray that contribute organic constituents. For this reason, physical sea spray models provide an important technique for studying the organic composition of particles from marine biogenic sources. The organic composition of particles produced by two different physical sea spray models were measured in three open ocean seawater types: (i) Coastal California in the northeastern Pacific, which is influenced by wind-driven, large-scale upwelling leading to productive or eutrophic (nutrient-rich) seawater and high chl-a concentrations, (ii) George's Bank in the northwestern Atlantic, which is also influenced by nutrient upwelling and eutrophic seawater with phytoplankton productivity and high chl-a concentrations, and (iii) the Sargasso Sea in the subtropical western Atlantic, which is oligotrophic and nutrient-limited, reflected in low phytoplankton productivity and low chl-a concentrations. Fourier transform infrared spectroscopy provides information about the functional group composition that represents the marine organic fraction more completely than is possible with techniques that measure non-refractory mass (vaporizable at 650°C). After separating biogenic marine particles from those from other sources, the measured compositions of atmospheric marine aerosol particles from three ocean regions is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. The organic composition of atmospheric primary marine (ocean-derived) aerosol particles is nearly identical to model generated primary marine aerosol particles from bubbled seawater. Variability in productive and non-productive seawater may be caused by the presence of surfactants that can stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components without substantial changes in overall group composition

  7. Ion-induced nucleation of pure biogenic particles

    NASA Astrophysics Data System (ADS)

    Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Frege, Carla; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K.; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C.; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R.; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P.; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A. D.; Riipinen, Ilona; Rissanen, Matti P.; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E.; Seinfeld, John H.; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L.; Wagner, Andrea C.; Wagner, Paul E.; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M.; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M.; Worsnop, Douglas R.; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S.; Curtius, Joachim

    2016-05-01

    Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

  8. Ion-induced nucleation of pure biogenic particles.

    PubMed

    Kirkby, Jasper; Duplissy, Jonathan; Sengupta, Kamalika; Frege, Carla; Gordon, Hamish; Williamson, Christina; Heinritzi, Martin; Simon, Mario; Yan, Chao; Almeida, João; Tröstl, Jasmin; Nieminen, Tuomo; Ortega, Ismael K; Wagner, Robert; Adamov, Alexey; Amorim, Antonio; Bernhammer, Anne-Kathrin; Bianchi, Federico; Breitenlechner, Martin; Brilke, Sophia; Chen, Xuemeng; Craven, Jill; Dias, Antonio; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Fuchs, Claudia; Guida, Roberto; Hakala, Jani; Hoyle, Christopher R; Jokinen, Tuija; Junninen, Heikki; Kangasluoma, Juha; Kim, Jaeseok; Krapf, Manuel; Kürten, Andreas; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Molteni, Ugo; Onnela, Antti; Peräkylä, Otso; Piel, Felix; Petäjä, Tuukka; Praplan, Arnaud P; Pringle, Kirsty; Rap, Alexandru; Richards, Nigel A D; Riipinen, Ilona; Rissanen, Matti P; Rondo, Linda; Sarnela, Nina; Schobesberger, Siegfried; Scott, Catherine E; Seinfeld, John H; Sipilä, Mikko; Steiner, Gerhard; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Virtanen, Annele; Vogel, Alexander L; Wagner, Andrea C; Wagner, Paul E; Weingartner, Ernest; Wimmer, Daniela; Winkler, Paul M; Ye, Penglin; Zhang, Xuan; Hansel, Armin; Dommen, Josef; Donahue, Neil M; Worsnop, Douglas R; Baltensperger, Urs; Kulmala, Markku; Carslaw, Kenneth S; Curtius, Joachim

    2016-05-26

    Atmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere, and that ions have a relatively minor role. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution. PMID:27225125

  9. Organic aerosol formation from biogenic compounds over the Ponderosa pine forest in Colorado

    NASA Astrophysics Data System (ADS)

    Roux, Alma Hodzic; Lee-Taylor, Julia; Cui, Yuyan; Madronich, Sasha

    2013-05-01

    The secondary organic aerosol (SOA) formation and regional growth from biogenic precursors is of particular interest given their abundance in the atmosphere, and has been investigated during the Rocky Mountain Biogenic Aerosol field Study in 2011 in the pine forest canopy (dominated by terpene emissions) using both WRF/Chem 4km simulations and the GECKO-A explicit chemistry box-model runs. We have quantified the relative contribution of different biogenic precursors to SOA levels that were measured by the aerosol mass spectrometer at the site, and investigated the relative contribution of OH, O3 and NO3 chemistry to the formed SOA mass during day-and nighttime. Although, the local production and mass concentrations of submicron organic aerosols at the site seem relatively modest ˜1-2 ug/m3, we show that the optically active regional mass is increased as the SOA formation continues for several days in the background forest air. We investigate whether the simplified SOA parameterizations used in 3D models can capture this growth. In addition, preliminary comparisons of the number concentrations and the composition of ultrafine particles (8 - 30nm) from WRF/Chem simulations and TD-CIMS measurements are also discussed, and the contribution of organic aerosols to CCN formation is quantified.

  10. Molecular markers of biomass burning, fungal spores and biogenic SOA in the Taklimakan desert aerosols

    NASA Astrophysics Data System (ADS)

    Fu, Pingqing; Zhuang, Guoshun; Sun, Yele; Wang, Qiongzhen; Chen, Jing; Ren, Lujie; Yang, Fan; Wang, Zifa; Pan, Xiaole; Li, Xiangdong; Kawamura, Kimitaka

    2016-04-01

    Biogenic primary organic aerosols (POA) and secondary organic aerosols (SOA) are important organic constituents of atmospheric particulate matter (PM). In order to better understand the atmospheric abundances, molecular compositions and sources of the desert aerosols, biomass-burning tracers (e.g. levoglucosan), primary saccharides including fungal spore tracers, and SOA tracers from the oxidation of biogenic volatile organic compounds (e.g. isoprene, monoterpenes and sesquiterpene) have been studied in ambient aerosols from the Taklimakan desert, using gas chromatography-mass spectrometry. Results showed that the total concentrations of biomass-burning tracers at Hetian (177-359 ng m-3, mean 233 ng m-3 in PM2.5) in the south rim of the desert were much higher than those at Tazhong (1.9-8.8 ng m-3 in PM2.5 and 5.9-32 ng m-3 in TSP) in the central Taklimakan desert. Molecular markers of fungal spores were also detected in all the desert aerosols, highlighting the importance of primary bioaerosols in the Asian dust particles. A specific pattern of the dominance of 2-methylglyceric acid over 2-methyltetrols and C5-alkene triols was found in the Taklimakan desert aerosols, especially during the dust storm events, which is different from the 2-methyltetrols-dominated pattern in other ambient aerosols. Our results provide direct evidence on the biogenic POA and SOA tracers in the Taklimakan desert region, which help to better understand their impact on the aerosol chemistry in the down-wind regions.

  11. Atmospheric DMS and Biogenic Sulfur aerosol measurements in the Arctic

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhadgharelar, R.; Norman, A. L.; Wentworth, G.; Burkart, J.; Leaitch, W. R.; Abbatt, J.; Sharma, S.; Desiree, T. S.

    2014-12-01

    Dimethyl Sulfide (DMS) and its oxidation products were measured on the board of the Canadian Coast Guard Ship (CCGS) Amundsen and above melt ponds in the Arctic during July 2014 in the context of the NETCARE study which seeks to understand the effect of DMS and its oxidation products with respect to aerosol nucleation, as well as its effect on cloud and precipitation properties. The objective of this study is to quantify the role of DMS in aerosol growth and activation in the Arctic atmosphere. Atmospheric DMS samples were collected from different altitudes, from 200 to 9500 feet, aboard the POLAR6 aircraft expedition to determine variations in the DMS concentration and a comparison was made to shipboard DMS measurements and its effects on aerosol size fractions. The chemical and isotopic composition of sulfate aerosol size fractions was studied. Sulfur isotope ratios (34S/32S) offer a way to determine the oceanic DMS contribution to aerosol growth. The results are expected to address the contribution of anthropogenic as well as biogenic sources of aerosols to the growth of the different aerosol size fractions. In addition, aerosol sulfate concentrations were measured at the same time within precipitation and fogs to compare with the characteristics of aerosols in each size fraction with the characteristics of the sulfate in each medium. This measurement is expected to explain the contribution of DMS oxidation in aerosol activation in the Arctic summer. Preliminary results from the measurement campaign for DMS and its oxidation products in air, fog and precipitation will be presented.

  12. A biogenic source of oxalic acid in marine aerosol

    NASA Astrophysics Data System (ADS)

    Facchini, M.; Rinaldi, M.; Ceburnis, D.; O'Dowd, C.; Sciare, J.; Burrows, J. P.

    2010-12-01

    Oxalic acid has been often observed in marine aerosol, nevertheless, given the ubiquitous character and the high concentrations found in polluted environments, its origin has often been attributed to continental sources. In this work, we present the results of oxalic acid analyses, on aerosol samples collected at Mace Head (Ireland, 53°20’N, 9°54’W) and Amsterdam Island (Indian Ocean, 37°48’S, 77°34’E), supporting the existence of a biogenic source of oxalic acid over the oceans. Measurements cover the year 2006, at the Northern Hemisphere site, and the period 2003-2007, at the Southern Hemisphere one. Aerosol oxalic acid was detected in clean marine air masses in concentrations ranging from 2.7 to 39 ng m-3, at Mace Head, and from 0.31 to 17 ng m-3, at Amsterdam Island. In both hemispheres, oxalic acid concentration showed a clear seasonal trend, with maxima in spring-summer and minima in the fall-winter period, in analogy with other marine biogenic aerosol components (e.g., MSA and amines). Oxalic acid was distributed along the whole aerosol size spectrum, with the major contribution given by the 1.0-2.0 µm size range, and by the lower accumulation mode (0.25-0.5 µm). Given the observed size distributions, marine aerosol oxalic acid can be assumed as the result of the combination of different formation processes, among which in-cloud oxidation of gaseous precursors [1] and photochemical degradation of biogenic unsaturated fatty acids [2] are likely the most important. Among aerosol oxalic acid precursors, glyoxal is the most likely candidate in the marine boundary layer, as a source of glyoxal over the oceans has recently been discovered by satellite observations [3] and confirmed by in situ measurements [4]. In support of this hypothesis, SCIAMACHY satellite retrieved glyoxal column concentrations, over the two sampling sites, resulted characterized by a clear seasonal trend, resembling the aerosol oxalic acid one. [1] Warneck, Atmospheric

  13. A marine biogenic source of atmospheric ice-nucleating particles

    SciTech Connect

    Wilson, T. W.; Ladino, L. A.; Alpert, Peter A.; Breckels, M. N.; Brooks, I. M.; Browse, J.; Burrows, Susannah M.; Carslaw, K. S.; Huffman, J. A.; Judd, C.; Kilthau, W. P.; Mason, R. H.; McFiggans, Gordon; Miller, L. A.; Najera, J.; Polishchuk, E. A.; Rae, S.; Schiller, C. L.; Si, M.; Vergara Temprado, J.; Whale, Thomas; Wong, J P S; Wurl, O.; Yakobi-Hancock, J. D.; Abbatt, JPD; Aller, Josephine Y.; Bertram, Allan K.; Knopf, Daniel A.; Murray, Benjamin J.

    2015-09-09

    The formation of ice in clouds is facilitated by the presence of airborne ice nucleating particles1,2. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice3–11. Here we show that material in the sea surface microlayer, which is enriched in surface active organic material representative of that found in sub-micron sea- spray aerosol12–21, nucleates ice under conditions that occur in mixed-phase clouds and high-altitude ice clouds. The ice active material is likely biogenic and is less than ~0.2 ?m in size. We also show that organic material (exudate) released by a common marine diatom nucleates ice when separated from cells and propose that organic material associated with phytoplankton cell exudates are a candidate for the observed ice nucleating ability of the microlayer samples. By combining our measurements with global model simulations of marine organic aerosol, we show that ice nucleating particles of marine origin are dominant in remote marine environments, such as the Southern Ocean, the North Pacific and the North Atlantic.

  14. A marine biogenic source of atmospheric ice-nucleating particles.

    PubMed

    Wilson, Theodore W; Ladino, Luis A; Alpert, Peter A; Breckels, Mark N; Brooks, Ian M; Browse, Jo; Burrows, Susannah M; Carslaw, Kenneth S; Huffman, J Alex; Judd, Christopher; Kilthau, Wendy P; Mason, Ryan H; McFiggans, Gordon; Miller, Lisa A; Nájera, Juan J; Polishchuk, Elena; Rae, Stuart; Schiller, Corinne L; Si, Meng; Temprado, Jesús Vergara; Whale, Thomas F; Wong, Jenny P S; Wurl, Oliver; Yakobi-Hancock, Jacqueline D; Abbatt, Jonathan P D; Aller, Josephine Y; Bertram, Allan K; Knopf, Daniel A; Murray, Benjamin J

    2015-09-10

    The amount of ice present in clouds can affect cloud lifetime, precipitation and radiative properties. The formation of ice in clouds is facilitated by the presence of airborne ice-nucleating particles. Sea spray is one of the major global sources of atmospheric particles, but it is unclear to what extent these particles are capable of nucleating ice. Sea-spray aerosol contains large amounts of organic material that is ejected into the atmosphere during bubble bursting at the organically enriched sea-air interface or sea surface microlayer. Here we show that organic material in the sea surface microlayer nucleates ice under conditions relevant for mixed-phase cloud and high-altitude ice cloud formation. The ice-nucleating material is probably biogenic and less than approximately 0.2 micrometres in size. We find that exudates separated from cells of the marine diatom Thalassiosira pseudonana nucleate ice, and propose that organic material associated with phytoplankton cell exudates is a likely candidate for the observed ice-nucleating ability of the microlayer samples. Global model simulations of marine organic aerosol, in combination with our measurements, suggest that marine organic material may be an important source of ice-nucleating particles in remote marine environments such as the Southern Ocean, North Pacific Ocean and North Atlantic Ocean. PMID:26354482

  15. Formation of secondary organic aerosols from biogenic precursors: A case study over an Isoprene emitting forest.

    NASA Astrophysics Data System (ADS)

    Freney, Evelyn; Sellegri, Karine; Borbon, Agnès; Colomb, Aurelie; Delon, Claire; Jambert, Corinne; Durand, Pierre; Bourianne, Thierry; Gaimoz, Cecile; Feron, Anais; Triquette, Sylvain; Beekmann, Matthias; Sartelet, Karine; Dulcac, Francois

    2015-04-01

    Characterising the sources and formation patterns of atmospheric aerosols is fundamental to understanding the impact of anthropogenic emissions on the composition and physical properties of the atmosphere. Although, the contribution of urban anthropogenic aerosol particles is important (10 Tg C yr-1), the contribution of biogenic aerosols has been estimated to be as much as 90 Tg C yr-1 (Hallquist et al., 2009.). This large difference highlights the importance of understanding the formation mechanisms and sources of the biogenic aerosol in the atmosphere. An increasing number of studies have shown that the submicron aerosol mass concentration is dominated by organic aerosols in both rural and urban environments. In addition, there have been several studies showing that the combined emissions of both biogenic and anthropogenic VOC emissions can result in a higher yield of secondary organic aerosol (SOA) formation. Biogenic SOA is formed from the oxidation of biogenic volatile organic compounds that are emitted naturally from terrestrial vegetation. The most commonly emitted BVOCs include isoprene and monoterpenes (Kesslmeier and Staudt, 1999, Arneth et al., 2008). Despite their importance, the characterisation of BSOA from laboratory and field experiments is still poor and it is only recently that advances in measurement techniques providing more detailed analysis of these species is being provided. One of the reasons for the difficulty in characterising the abundance of these species, is their high temporal and spatial scales. As part of the ChArMEx (the Chemistry-Aerosol Mediterranean Experiment, http://charmex.lsce.ipsl.fr) experiment (SOP2a/SAFMED+) in July 2014, a number of research flights were performed over two forested areas in the south of France. These forested areas had different characteristics where one has mainly isoprene emitting vegetation, and the other is known to have more monoterpene emitting vegetation. The aims of these research flights were

  16. A marine biogenic source of atmospherically relevant ice nucleating particles

    NASA Astrophysics Data System (ADS)

    Wilson, Theodore W.; Ladino, Luis A.; Alpert, Peter A.; Chance, Rosie; Whale, Thomas F.; Vergara Temprado, Jesús; Burrows, Susannah M.; Breckels, Mark N.; Kilthau, Wendy P.; Browse, Jo; Bertram, Allan K.; Miller, Lisa A.; Carpenter, Lucy J.; Hamilton, Jacqui F.; Carslaw, Kenneth S.; Brooks, Ian M.; Abbatt, Jonathan P. D.; Aller, Josephine Y.; Knopf, Daniel A.; Murray, Benjamin J.

    2016-04-01

    There are limited observations describing marine sources of ice nucleating particles (INPs), despite sea spray aerosol being one of the dominant sources of atmospheric particles globally. Evidence indicates that some marine aerosol particles act as INPs, but the source of these particles is unclear. The sea surface microlayer is enriched in surface active organic material representative of that found in sub-micron sea-spray aerosol. We show that the sea surface microlayer is enriched in INPs that nucleate ice under conditions pertinent to both high-altitude ice clouds and low to mid-altitude mixed-phase clouds. The INPs pass through 0.2 μm pore filters, are heat sensitive and spectroscopic analysis indicates the presence of material consistent with phytoplankton exudates. Mass spectrometric analysis of solid phase extracted dissolved organic material from microlayer and sub-surface water samples showed that the relative abundance of certain ions correlated with microlayer ice nucleation activity. However, these ions were not themselves directly responsible for ice nucleation. We propose that material associated with phytoplankton exudates is a candidate for the observed activity of the microlayer samples. We show that laboratory produced exudate from a ubiquitous marine diatom contains INPs despite its separation from diatom cells. Finally we use a parameterisation of our field data to estimate the atmospheric INP contribution from primary marine organic emissions using a global model and test the model against existing INP measurements in the remote oceans. We find that biogenic marine INPs can be dominant in remote marine environments, such as the Southern Ocean.

  17. The Impact of Biogenic and Anthropogenic Atmospheric Aerosol on Climate in Egypt

    NASA Astrophysics Data System (ADS)

    Ibrahim, A. I.; Zakey, A.; Steiner, A. L.; Shokr, M. E.; El-Raey, M.; Ahmed, Y.; Al-Hadidi, A.; Zakey, A.

    2014-12-01

    Aerosols are indicators of air quality as they reduce visibility and adversely affect public health. Aerosol optical depth (AOD) is a measure of the radiation extinction due to interaction of radiation with aerosol particles in the atmosphere. Using this optical measure of atmospheric aerosols we explore the seasonal and annual patterns of aerosols from both anthropogenic and biogenic sources over Egypt. Here, we use an integrated environment-climate-aerosol model in conjunction with inversion technique to identify the aerosol particle size distribution over different locations in Egypt. The online-integrated Environment-Climate-Aerosol model (EnvClimA), which is based on the International Center for Theoretical Physics Regional Climate Model (ICTP-RegCM), is used to study the emission of different aerosols and their impact on climate parameters for a long-term base line simulation run over Egypt and North Africa. The global emission inventory is downscaled and remapping them over Egypt using local factors such as population, traffic and industrial activities to identify the sources of anthropogenic and biogenic emission from local emission over Egypt. The results indicated that the dominant natural aerosols over Egypt are dust emissions that frequently occur during the transitional seasons (Spring and Autumn). From the local observation we identify the number of dust and sand storm occurrences over Egypt. The Multiangle Imaging SpectroRadiometer (MISR) is used to identify the optical characterizations of different types of aerosols over Egypt. Modeled aerosol optical depth and MISR observed (at 555 nm) are compared from March 2000 through November 2013. The results identify that the MISR AOD captures the maximum peaks of AOD in March/April that coincide with the Khamasin dust storms. However, peaks in May are either due to photochemical reactions or anthropogenic activities. Note: This presentation is for a Partnerships for Enhanced Engagement in Research (PEER

  18. Observations of Terrestrial Biogenic and Biomass Burning Aerosol Impacts on Marine Stratocumulus off the Coast of California

    NASA Astrophysics Data System (ADS)

    Coggon, M. M.; Sorooshian, A.; Wang, Z.; Craven, J. S.; Metcalf, A. R.; Lin, J. J.; Nenes, A.; Jonsson, H.; Flagan, R. C.; Seinfeld, J.

    2014-12-01

    The nature of anthropogenic and marine aerosol interactions with stratocumulus clouds off the coast of California has been widely examined, yet limited studies have evaluated aerosol-cloud interactions resulting from terrestrial biogenic and biomass burning emissions. This study presents aircraft data from the 2011 Eastern Pacific Emitted Aerosol Cloud Experiment (E-PEACE) and 2013 Nucleation in California Experiment (NiCE). We investigate mechanisms by which biogenic and biomass burning aerosols originating from the Northwest United States are transported to the marine atmosphere. We present data showing the spatial extent to which these particles impact the free troposphere above marine stratocumulus and highlight their influence on cloud water composition and cloud condensation nuclei (CCN). Terrestrial biogenic and biomass burning particles had the greatest impact on marine aerosol and clouds north of San Francisco, CA due to synoptic-scale meteorology. These aerosols were observed to be CCN-active and led to elevated cloud water concentrations of species such as nitrate, acetate, formate, and oxalate.

  19. Water uptake is independent of the inferred composition of secondary aerosols derived from multiple biogenic VOCs

    NASA Astrophysics Data System (ADS)

    Alfarra, M. R.; Good, N.; Wyche, K. P.; Hamilton, J. F.; Monks, P. S.; Lewis, A. C.; McFiggans, G. B.

    2013-04-01

    We demonstrate that the water uptake properties derived from sub- and super-saturated measurements of chamber-generated biogenic secondary organic aerosol (SOA) particles are independent of their degree of oxidation determined using both online and offline methods. SOA particles are formed from the photooxidation of five structurally different biogenic VOCs representing a broad range of emitted species and their corresponding range of chemical reactivity: α-pinene, β-caryophyllene, limonene, myrcene and linalool. The fractional contribution of mass fragment 44 to the total organic signal (f44) is used to characterise the extent of oxidation of the formed SOA as measured online by an aerosol mass spectrometer. Results illustrate that the values of f44 are dependent on the precursor, the extent of photochemical ageing as well as on the initial experimental conditions. SOA generated from a single biogenic precursor should therefore not be used as a general proxy for biogenic SOA. Similarly, the generated SOA particles exhibit a range of hygroscopic properties depending on the precursor, its initial mixing ratio and photochemical ageing. The activation behaviour of the formed SOA particles show no temporal trends with photochemical ageing. The average κ values derived from the HTDMA and CCNc are generally found to cover the same range for each precursor under two different initial mixing ratio conditions. A positive correlation is observed between the hygroscopicity of particles of a single size and f44 for α-pinene, β-caryophyllene, linalool and myrcene, but not for limonene SOA. The investigation of the generality of this relationship reveal that α-pinene, limonene, linalool and myrcene are all able to generate particles with similar hygroscopicity (κHTDMA ~0.1) despite f44 exhibiting a relatively wide range of values (~4 to 11%). Similarly, κCCN is found to be independent of f44. The same findings are also true when sub- and super-saturated water uptake

  20. Water uptake is independent of the inferred composition of secondary aerosols derived from multiple biogenic VOCs

    NASA Astrophysics Data System (ADS)

    Alfarra, M. R.; Good, N.; Wyche, K. P.; Hamilton, J. F.; Monks, P. S.; Lewis, A. C.; McFiggans, G.

    2013-12-01

    We demonstrate that the water uptake properties derived from sub- and super-saturated measurements of chamber-generated biogenic secondary organic aerosol (SOA) particles are independent of their degree of oxidation, determined using both online and offline methods. SOA particles are formed from the photooxidation of five structurally different biogenic VOCs, representing a broad range of emitted species and their corresponding range of chemical reactivity: α-pinene, β-caryophyllene, limonene, myrcene and linalool. The fractional contribution of mass fragment 44 to the total organic signal (f44) is used to characterise the extent of oxidation of the formed SOA as measured online by an aerosol mass spectrometer. Results illustrate that the values of f44 are dependent on the precursor, the extent of photochemical ageing as well as on the initial experimental conditions. SOA generated from a single biogenic precursor should therefore not be used as a general proxy for biogenic SOA. Similarly, the generated SOA particles exhibit a range of hygroscopic properties, depending on the precursor, its initial mixing ratio and photochemical ageing. The activation behaviour of the formed SOA particles show no temporal trends with photochemical ageing. The average κ values derived from the HTDMA and CCNc are generally found to cover the same range for each precursor under two different initial mixing ratio conditions. A positive correlation is observed between the hygroscopicity of particles of a single size and f44 for α-pinene, β-caryophyllene, linalool and myrcene, but not for limonene SOA. The investigation of the generality of this relationship reveals that α-pinene, limonene, linalool and myrcene are all able to generate particles with similar hygroscopicity (κHTDMA ~0.1) despite f44 exhibiting a relatively wide range of values (~4 to 11%). Similarly, κCCN is found to be independent of f44. The same findings are also true when sub- and super-saturated water uptake

  1. The BOND project: Biogenic aerosols and air quality in Athens and Marseille greater areas

    NASA Astrophysics Data System (ADS)

    Sotiropoulou, R. E. P.; Tagaris, E.; Pilinis, C.; Andronopoulos, S.; Sfetsos, A.; Bartzis, J. G.

    2004-03-01

    The role of Secondary Biogenic Organic Aerosol in aerosol budget is examined using the Atmospheric Dispersion of Pollutants over Complex Terrain-Urban Airshed Model-Aerosols (ADREA-I/UAM-AERO) modeling system in two representative Mediterranean areas. The areas have been selected, because of their elevated biogenic emission levels and the sufficient degree of meteorological and land use diversity characterizing the locations. Comparison of the model results with and without biogenic emissions reveals the significant role biogenic emissions play in modulating ozone and aerosol concentrations. Biogenic emissions are predicted to affect the concentrations of organic aerosol constituents through the reactions of terpenes with O3, OH and NO3. The ozonolysis of terpenes is predicted to cause an increase in OH radical concentrations that ranges from 10% to 78% for Athens, and from 20% to 95% for Marseilles, depending on the location, compared to the predictions without biogenic emissions. The reactions of this extra hydroxyl radical with SO2 and NOx have as final products increased concentrations of sulfates and nitrates in the particulate phase. As a result, biogenic emissions are predicted to affect the concentrations not only of organic aerosols, but those of inorganic aerosols as well. Thus biogenic emissions should be taken into consideration when models for the prediction and enforcement of abatement strategies of atmospheric pollution are applied.

  2. A Classroom Demonstration of the Formation of Aerosols from Biogenic Hydrocarbons

    NASA Astrophysics Data System (ADS)

    Andino, Jean M.; Wallington, Timothy J.; Hurley, Michael D.; Wayne, Richard P.

    2000-12-01

    A demonstration that illustrates the formation of particulate matter from a biogenic source is described. Ozone is allowed to react with the terpenes present in an orange peel. Products formed from the ozone-terpene reaction condense to form aerosols that scatter light from a laser pointer source. This demonstration has been used for high school students as well as college-level students to explain the reactions of ozone in the troposphere, the formation of secondary particulate matter (gas-to-particle conversion mechanisms), and degradation of visibility.

  3. Aerosol size distribution and radiative forcing response to anthropogenically driven historical changes in biogenic secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    D'Andrea, S. D.; Acosta Navarro, J. C.; Farina, S. C.; Scott, C. E.; Rap, A.; Farmer, D. K.; Spracklen, D. V.; Riipinen, I.; Pierce, J. R.

    2015-03-01

    Emissions of biogenic volatile organic compounds (BVOCs) have changed in the past millennium due to changes in land use, temperature, and CO2 concentrations. Recent reconstructions of BVOC emissions have predicted that global isoprene emissions have decreased, while monoterpene and sesquiterpene emissions have increased; however, all three show regional variability due to competition between the various influencing factors. In this work, we use two modeled estimates of BVOC emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on secondary organic aerosol (SOA) formation, global aerosol size distributions, and radiative effects using the GEOS-Chem-TOMAS (Goddard Earth Observing System; TwO-Moment Aerosol Sectional) global aerosol microphysics model. With anthropogenic emissions (e.g., SO2, NOx, primary aerosols) turned off and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size Dp > 80 nm (N80) of > 25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000 which led to regional increases in the combined aerosol radiative effect (direct and indirect) of > 0.5 W m-2 in these regions. We test the sensitivity of our results to BVOC emissions inventory, SOA yields, and the presence of anthropogenic emissions; however, the qualitative response of the model to historic BVOC changes remains the same in all cases. Accounting for these uncertainties, we estimate millennial changes in BVOC emissions cause a global mean direct effect of between +0.022 and +0.163 W m-2 and the global mean cloud-albedo aerosol indirect effect of between -0.008 and -0.056 W m-2. This change in aerosols, and the associated radiative forcing, could be a largely overlooked and important anthropogenic aerosol effect on regional climates.

  4. Natural and Anthropogenically Perturbed Biogenic Aerosol over Tropical South East Asia

    NASA Astrophysics Data System (ADS)

    Coe, H.; Robinson, N.; Allan, J. D.; Hewitt, C. N.

    2014-12-01

    Tropical forested regions are of interest as sources of atmospheric aerosol since they cover very large areas of the tropics and are a source of a large amount of volatile organic compounds which act as precursors for particle formation. Natural forest regions offer the potential to study the background state of the tropics and so potentially gain some insight into the pre-perturbed atmosphere. However, over the last decade in South East Asia, a considerable fraction of the native tropical deciduous forest has been deforested and replanted with palm oil plantations. This changes the range of volatile organic compounds that are emitted and act as sources of secondary organic aerosol. A suite of intensive ground and airborne measurements were made over both tropical forest and oil palm plantations in Sabah, Malaysia as part of the "Oxidant and Particle Photochemical Processes above a South East Asian tropical rainforest (OP3) during 2008. These data will be used together with recent improvements in our understanding of aerosol formation from biogenic compounds to discuss aerosol formation in tropical regions and the influence of human influence through widespread palm oil agriculture.

  5. BIOGENIC CONTRIBUTION TO PM-2.5 AMBIENT AEROSOL FROM RADIOCARBON MEASUREMENTS

    EPA Science Inventory

    Knowledge of the relative contributions of biogenic versus anthropogenic sources to ambient aerosol is of great interest in the formulation of strategies to achieve nationally mandated air quality standards. Radiocarbon (Carbon-14) measurements provide a means to quantify the ...

  6. Seasonal variations of biogenic secondary organic aerosol tracers in ambient aerosols from Alaska

    NASA Astrophysics Data System (ADS)

    Haque, Md. Mozammel; Kawamura, Kimitaka; Kim, Yongwon

    2016-04-01

    We investigated total suspended particles (TSP) collected from central Alaska, USA for molecular compositions of secondary organic aerosol (SOA) derived from the oxidation of biogenic volatile organic compounds (BVOCs). Isoprene-, α-/β-pinene- and β-caryophyllene-SOA tracers were determined using gas chromatography-mass spectrometry. The concentration ranges of isoprene, α-/β-pinene and β-caryophyllene oxidation products were 0.02-18.6 ng m-3 (ave. 4.14 ng m-3), 0.42-8.24 ng m-3 (2.01 ng m-3) and 0.10-9 ng m-3 (1.53 ng m-3), respectively. Isoprene-SOA tracers showed higher concentrations in summer (ave. 8.77 ng m-3), whereas α-/β-pinene- and β-caryophyllene-SOA tracers exhibited highest levels in spring (3.55 ng m-3) and winter (4.04 ng m-3), respectively. β-Caryophyllinic acid and levoglucosan showed a positive correlation, indicating that biomass burning may be a major source for β-caryophyllene. We found that mean contributions of isoprene oxidation products to organic carbon (OC) and water-soluble organic (WSOC) (0.56% and 1.2%, respectively) were higher than those of α-/β-pinene (0.31% and 0.55%) and β-caryophyllene (0.08% and 0.13%). Using a tracer-based method, we estimated the concentrations of secondary organic carbon (SOC) produced from isoprene, α-/β-pinene and β-caryophyllene to be 0.66-718 ngC m-3 (ave. 159 ngC m-3), 7.4-143 ngC m-3 (35 ngC m-3) and 4.5-391 ngC m-3 (66.3 ngC m-3), respectively. Based on SOA tracers, this study suggests that isoprene is a more important precursor for the production of biogenic SOA than α-/β-pinene and β-caryophyllene in subarctic Alaska.

  7. Seasonal variations of biogenic secondary organic aerosol tracers in Cape Hedo, Okinawa

    NASA Astrophysics Data System (ADS)

    Zhu, Chunmao; Kawamura, Kimitaka; Fu, Pingqing

    2016-04-01

    Secondary organic aerosol (SOA) substantially contributes to particulate organic matter affecting the regional and global air quality and the climate. Total suspended particle (TSP) samples were collected in October 2009 to February 2012 on a weekly basis at Cape Hedo, Okinawa, Japan in the western North Pacific Rim, an outflow region of Asian aerosols and precursors. The TSP samples were analyzed for SOA tracers derived from biogenic volatile organic compounds (BVOCs). Total isoprene-SOA tracers showed a maximum in summer (2.12 ± 2.02 ng m-3) and minimum in winter (1.16 ± 0.92 ng m-3). This seasonality is mainly controlled by isoprene emission from the local subtropical forest, followed by regional scale emission of isoprene from the surrounding seas and long-range transported air masses. Total monoterpene-SOA tracers peaked in March (3.38 ± 2.03 ng m-3) followed by October (2.95 ± 1.62 ng m-3). In contrast, sesquiterpene-SOA tracer, β-caryophyllinic acid, showed winter maximum (1.63 ± 1.18 ng m-3) and summer minimum (0.20 ± 0.46 ng m-3). The variations of the monoterpene- and sesquiterpene-SOA tracers are likely related to the continental outflow of oxidation products of BVOC. Using a tracer-based method, we estimated the total biogenic SOC of 0.25-157 ng m-3 (mean 35.8 ng m-3) that accounts for 0.01-9.8% (mean 2.7%) of aerosol organic carbon. Our study suggests that SOA formation in the western North Pacific Rim is involved with not only local but also regional emissions followed by long-range atmospheric transport.

  8. Aerosol size distribution and radiative forcing response to anthropogenically driven historical changes in biogenic secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    D'Andrea, S. D.; Acosta Navarro, J. C.; Farina, S. C.; Scott, C. E.; Rap, A.; Farmer, D. K.; Spracklen, D. V.; Riipinen, I.; Pierce, J. R.

    2014-10-01

    Emissions of biogenic volatile organic compounds (BVOC) have changed in the past millennium due to changes in land use, temperature and CO2 concentrations. Recent model reconstructions of BVOC emissions over the past millennium predicted changes in dominant secondary organic aerosol (SOA) producing BVOC classes (isoprene, monoterpenes and sesquiterpenes). The reconstructions predicted that global isoprene emissions have decreased (land-use changes to crop/grazing land dominate the reduction), while monoterpene and sesquiterpene emissions have increased (temperature increases dominate the increases); however, all three show regional variability due to competition between the various influencing factors. These BVOC changes have largely been anthropogenic in nature, and land-use change was shown to have the most dramatic effect by decreasing isoprene emissions. In this work, we use two modeled estimates of BVOC emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on SOA formation, global aerosol size distributions, and radiative effects using the GEOS-Chem-TOMAS global aerosol microphysics model. With anthropogenic emissions (e.g. SO2, NOx, primary aerosols) held at present day values and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size Dp > 80 nm (N80) of >25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000 which led to regional increases in direct plus indirect aerosol radiative effect of >0.5 W m-2 in these regions. We test the sensitivity of our results to BVOC emissions inventory, SOA yields and the presence of anthropogenic emissions; however, the qualitative response of the model to historic BVOC changes remains the same in all cases. Accounting for these uncertainties, we estimate millennial changes in BVOC emissions cause a global mean direct effect of between +0.022 and +0.163 W m-2

  9. Modeling organic aerosols during MILAGRO: application of the CHIMERE model and importance of biogenic secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Hodzic, A.; Jimenez, J. L.; Madronich, S.; Aiken, A. C.; Bessagnet, B.; Curci, G.; Fast, J.; Lamarque, J. F.; Onasch, T. B.; Roux, G.; Ulbrich, I. M.

    2009-05-01

    The meso-scale chemistry-transport model CHIMERE is used to assess our understanding of major sources and formation processes leading to a fairly large amount of organic aerosols (OA, including primary OA (POA) and secondary OA (SOA)) observed in Mexico City during the MILAGRO field project (March 2006). Chemical analyses of submicron aerosols from aerosol mass spectrometers (AMS) indicate that organic particles found in the Mexico City basin contain a large fraction of oxygenated organic species (OOA) which have strong correspondence with SOA, and that their production actively continues downwind of the city. The SOA formation is modeled here by the one-step oxidation of anthropogenic (i.e. aromatics, alkanes), biogenic (i.e. monoterpenes and isoprene), and biomass-burning SOA precursors and their partitioning into both organic and aqueous phases. The near-surface model evaluation shows that predicted OA correlates reasonably well with measurements during the campaign, however it remains a factor of 2 lower than the measured total OA. Fairly good agreement is found between predicted and observed POA within the city suggesting that anthropogenic and biomass burning emissions are reasonably captured. Consistent with previous studies in Mexico City, large discrepancies are encountered for SOA, with a factor of 2-10 model underestimate. When only anthropogenic SOA precursors were considered, the model was able to reproduce within a factor of two the sharp increase in SOA concentrations during the late morning at both urban and near-urban locations but the discrepancy increases rapidly later in the day, consistent with previous results, and is especially obvious when the column-integrated SOA mass is considered instead of the surface concentration. The increase in the missing SOA mass in the afternoon coincides with the sharp drop in POA suggesting a tendency of the model to excessively evaporate the freshly formed SOA. Predicted SOA concentrations in our base case

  10. Biogenic and biomass burning organic aerosol in a boreal forest at Hyytiälä, Finland, during HUMPPA-COPEC 2010

    NASA Astrophysics Data System (ADS)

    Corrigan, A. L.; Russell, L. M.; Takahama, S.; Äijälä, M.; Ehn, M.; Junninen, H.; Rinne, J.; Petäjä, T.; Kulmala, M.; Vogel, A. L.; Hoffmann, T.; Ebben, C. J.; Geiger, F. M.; Chhabra, P.; Seinfeld, J. H.; Worsnop, D. R.; Song, W.; Auld, J.; Williams, J.

    2013-12-01

    Submicron aerosol particles were collected during July and August 2010 in Hyytiälä, Finland, to determine the composition and sources of aerosol at that boreal forest site. Submicron particles were collected on Teflon filters and analyzed by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFGs). Positive matrix factorization (PMF) was applied to aerosol mass spectrometry (AMS) measurements and FTIR spectra to identify summertime sources of submicron aerosol mass at the sampling site. The two largest sources of organic mass (OM) in particles identified at Hyytiälä were (1) biogenic aerosol from surrounding local forest and (2) biomass burning aerosol, transported 4-5 days from large wildfires burning near Moscow, Russia, and northern Ukraine. The robustness of this apportionment is supported by the agreement of two independent analytical methods for organic measurements with three statistical techniques. FTIR factor analysis was more sensitive to the chemical differences between biogenic and biomass burning organic components, while AMS factor analysis had a higher time resolution that more clearly linked the temporal behavior of separate OM factors to that of different source tracers even though their fragment mass spectrum were similar. The greater chemical sensitivity of the FTIR is attributed to the nondestructive preparation and the functional group specificity of spectroscopy. The FTIR spectra show strong similarities among biogenic and biomass burning factors from different regions as well as with reference OM (namely olive tree burning organic aerosol and α-pinene chamber secondary organic aerosol (SOA)). The biogenic factor correlated strongly with temperature and oxidation products of biogenic volatile organic compounds (BVOCs), included more than half of the oxygenated OFGs (carbonyl groups at 29% and carboxylic acid groups at 22%), and represented 35% of the submicron OM. Compared to previous studies at Hyytiälä, the

  11. Combined volatility and mass spectrometric measurements of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Emanuelsson, E.; Buchholz, A.; Hallquist, M.; Kiendler-Scharr, A.; Mentel, T.; Spindler, C.

    2009-04-01

    The volatility of secondary organic aerosol (SOA) from the oxidation of mixtures of biogenic Volatile Organic Compounds (VOC) has been investigated in the SAPHIR facility in Forschungszentrum Jülich, Germany, by using a Volatility Tandem Differential Mobility Analyser (VTDMA). The standard VTDMA setup comprises three main parts: 1) An initial DMA, where a nearly monodisperse size fraction of the aerosol particles is selected (typically 100 or 150 nm), 2) the oven unit, i.e. four ovens in parallel where each oven includes a heating and adsorption section where the evaporation and adsorption of the volatile fraction occurs and 3) a final SMPS (Scanning Mobility Particle Sizer) system where the residual particle number distribution is measured. For this measurement campaign the set-up also contained a Quadrupole Aerosol Mass Spectrometer (Aerodyne QAMS). The temperature of the ovens can be varied between 298 and well above 573 K. In parallel to the final SMPS the AMS was used for chemical composition and density measurements. When the system was dedicated for AMS measurements the initial DMA was bypassed to improve the aerosol concentration. However, the produced SOA has a narrow size distribution still making it possible to follow small changes in the aerosol peak diameter. A general feature of the thermo-denuder system is that a less volatile SOA gives a larger residual particle size distribution compared to more volatile SOA. The experiments conducted were based on photochemical oxidation of selected terpene mixtures. A reference boreal mixture of terpenes, consisting of α-pinene, β-pinene, limonene, ^-3-carene, and ocimene was used as base case. Secondary organic aerosol was formed from the precursor compounds by reaction with O3/H2O/OH in SAPHIR on the first day. The particles were kept in the chamber for up to two further days and were exposed to natural sunlight and OH radicals to initiate close to natural chemical ageing. The VTDMA results show that SOA

  12. Excitation-emission spectra and fluorescence quantum yields for fresh and aged biogenic secondary organic aerosols

    SciTech Connect

    Lee, Hyun Ji; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey A.

    2013-05-10

    Certain biogenic secondary organic aerosols (SOA) become absorbent and fluorescent when exposed to reduced nitrogen compounds such as ammonia, amines and their salts. Fluorescent SOA may potentially be mistaken for biological particles by detection methods relying on fluorescence. This work quantifies the spectral distribution and effective quantum yields of fluorescence of SOA generated from two monoterpenes, limonene and a-pinene, and two different oxidants, ozone (O3) and hydroxyl radical (OH). The SOA was generated in a smog chamber, collected on substrates, and aged by exposure to ~100 ppb ammonia vapor in air saturated with water vapor. Absorption and excitation-emission matrix (EEM) spectra of aqueous extracts of aged and control SOA samples were measured, and the effective absorption coefficients and fluorescence quantum yields (~0.005 for 349 nm excitation) were determined from the data. The strongest fluorescence for the limonene-derived SOA was observed for excitation = 420+- 50 nm and emission = 475 +- 38 nm. The window of the strongest fluorescence shifted to excitation = 320 +- 25 nm and emission = 425 +- 38 nm for the a-pinene-derived SOA. Both regions overlap with the excitation-emission matrix (EEM) spectra of some of the fluorophores found in primary biological aerosols. Our study suggests that, despite the low quantum yield, the aged SOA particles should have sufficient fluorescence intensities to interfere with the fluorescence detection of common bioaerosols.

  13. New Particle Formation and Secondary Organic Aerosol in Beijing

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  14. On-line characterization of organic aerosols formed from biogenic precursors using atmospheric pressure chemical ionization mass spectrometry.

    PubMed

    Kückelmann, U; Warscheid, B; Hoffmann, T

    2000-04-15

    A method to investigate the chemical composition of organic aerosols formed from biogenic hydrocarbon oxidation using atmospheric pressure chemical ionization mass spectrometry (APCI/MS) is described. The method involves the direct introduction of aerosol particles into the ion source of the mass spectrometer. Using this technique, reaction monitoring experiments of alpha-pinene ozonolysis show the formation of hetero- and homomolecular cluster anions (dimers) of the primary oxidation products (multifunctional carboxylic acids). Since the formation of dimers plays a profound role in new particle formation processes by homogeneous nucleation in the atmosphere and, at the same time, is an intrinsic feature of APCI, it is essential to differentiate between both processes when on-line APCI/MS is applied. In this paper, we compare the results from the investigations of organic aerosols and artificially generated dimer cluster ions of the same compounds using identical ionization conditions. The clusters and their formation processes are characterized by varying the analyte concentration, investigating the thermal stability of dimers, and studying collisional activation properties of both ion species. The investigations show a significant difference in ion stability: dimer anions measured on-line have an estimated stability that is 20 kJ mol(-1) higher than that of the corresponding artificially generated cluster ions. Hence, the technique provides the possibility to accurately characterize dimers as ionized reaction products from biogenic hydrocarbon oxidation and allows an insight into the process of new-particle formation by homogeneous nucleation. PMID:10784160

  15. Biogenic and biomass burning organic aerosol in a boreal forest at Hyytiälä, Finland, during HUMPPA-COPEC 2010

    NASA Astrophysics Data System (ADS)

    Corrigan, A. L.; Russell, L. M.; Takahama, S.; Äijälä, M.; Ehn, M.; Junninen, H.; Rinne, J.; Petäjä, T.; Kulmala, M.; Vogel, A. L.; Hoffmann, T.; Ebben, C. J.; Geiger, F. M.; Chhabra, P.; Seinfeld, J. H.; Worsnop, D. R.; Song, W.; Auld, J.; Williams, J.

    2013-06-01

    Submicron aerosol particles were collected during July and August 2010 in Hyytiälä, Finland, to determine the composition and sources of aerosol at that Boreal forest site. Submicron particles were collected on Teflon filters and analyzed by Fourier transform infrared (FTIR) spectroscopy for organic functional groups (OFG). Positive matrix factorization (PMF) was applied to aerosol mass spectrometry (AMS) measurements and FTIR spectra to identify summertime sources of submicron aerosol mass at the sampling site. The two largest sources of organic mass (OM) in particles identified at Hyytiälä were (1) biogenic aerosol from surrounding local forest and (2) biomass burning aerosol, transported 4-5 days from large wildfires burning near Moscow, Russia, and northern Ukraine. The robustness of this apportionment is supported by the agreement of two independent analytical methods for organic measurements with three statistical techniques. FTIR factor analysis was more sensitive to the chemical differences between biogenic and biomass burning organic components, while AMS factor analysis had a higher time resolution that more clearly linked the temporal behavior of separate OM factors to that of different source tracers even though their fragment mass spectrum were similar. The greater chemical sensitivity of the FTIR is attributed to the nondestructive preparation and the functional group specificity of spectroscopy. The FTIR spectra show strong similarities among biogenic and biomass burning factors from different regions as well as with reference OM (namely olive tree burning BBOA and α-pinene chamber secondary organic aerosol (SOA)). The biogenic factor correlated strongly with temperature and oxidation products of biogenic volatile organic compounds (BVOCs), included more than half oxygenated OFGs (carbonyl groups at 29% and carboxylic acid groups at 22%), and represented 35% of the submicron OM. Compared to previous studies at Hyytiälä, the summertime biogenic

  16. Simultaneous Factor Analysis of Coupled Aerosol and VOC Mass Spectra in Regions of Biogenic Influence

    NASA Astrophysics Data System (ADS)

    Slowik, Jay; Chang, Rachel; Hayden, Katherine; Li, Shao-Meng; Liggio, John; Sjostedt, Steven; Vlasenko, Alexander; Leaitch, Richard; Abbatt, Jonathan

    2010-05-01

    Recent studies suggest that the traditional binary treatments of atmospheric organics as either gases or particles may be inadequate, highlighting the need for analytical techniques capable of simultaneously considering particle and gas-phase species. Organic mass spectra of particles and volatile organic compounds (VOCs) were collected using an Aerodyne time-of-flight aerosol mass spectrometer (C-ToF-AMS), and a proton transfer reaction-mass spectrometer (PTR-MS), respectively. The particle and VOC mass spectra were combined into a single dataset, which was analyzed using the positive matrix factorization (PMF) receptor modeling technique. The relative weights of the AMS and PTR-MS data were balanced in the PMF analysis according to the criteria that the scaled residuals within a solution be independent of the measuring instrument. Instrument relative weight is controlled by the application of a scaling factor to the PTR-MS uncertainties. The AMS and PTR-MS instruments were deployed from mid-May to mid-June at two sites in Canada: (1) Egbert, ON (2007), a semirural site ~70 km north of Toronto, and (2) Whistler, BC (2008), a remote site ~120 km north of Vancouver. The Egbert site is influenced by anthropogenic emissions from Toronto and populated regions to the south, biogenic emissions from boreal forests to the north, and biomass burning emissions. The Whistler site is strongly influenced by boreal forest terpene emissions, with lesser contributions from long-range transport and anthropogenic emissions.

  17. Separation of biogenic and biomass burning submicron aerosol from a boreal forest in Hyytiälä, Finland during HUMPPA-COPEC 2010

    NASA Astrophysics Data System (ADS)

    Corrigan, A.; Russell, L.; Äijälä, M.; Petäjä, T.; Kulmala, M.; Song, W.; Williams, J.

    2012-04-01

    Forests play an important role in the emission of primary and secondary organic aerosol (POA, SOA). Biomass burning is believed to be the largest source of global primary organic carbon (POC), estimated to be 31-45 TgC yr-1 [1]. In addition, biogenic volatile organic compounds (BVOCs) produce a large portion of global SOA, as BVOC emissions are believed to be 10 times greater than anthropogenic VOC emissions [2]. The oxidation of BVOCs produces considerable amounts of SOA, 12-70 TgC yr-1 [3]. In addition, the influence of anthropogenic emissions (i.e. NOx) can substantially enhance biogenic SOA formation [4]. Due to large uncertainties in the role aerosols play in the climate sysyen, there is a need to better understand the chemical composition of organic aerosols derived from forest ecosystems. One approach to better understand the composition and contribution of biogenic derived organic aerosols is to apply Positive Matrix Facotrization (PMF) on a time series dataset [5]. Due to chemical similarity and multi-collinerarity, separation of biogenic and biomass burning aerosol in boreal forests has been problematic in previous work [6]. To investigate the composition and sources of atmospheric aerosol in a biogenically influenced site, submicron particles were collected from July 12 to August 12, 2010 at the boreal forest in Hyytiälä, Finland and analyzed using Fourier transform infrared (FTIR) spectroscopy and aerosol mass spectrometry (AMS). Campaign average organic functional groups from FTIR analysis of submicron aerosol includes alkane (37%), carboxylic acid (28%), organic hydroxyl (15%), non-carboxylic acid carbonyl (15%), and primary amine (5%), with traces of organonitrate and organosulphates. AMS analysis indicates that the aerosol composition was heavily dominated by organics (69%), followed by sulphate (21%), nitrate (6%), and ammonia (4%). Measurements of particle-phase organic functional groups and inorganic ions collected during the HUMPPA-COPEC10

  18. The role of anthropogenic species in Biogenic aerosol formation

    EPA Science Inventory

    Isoprene is a widely recognized source of organic aerosol in the southeastern United States. Models have traditionally represented isoprene-derived aerosol as semivolatile species formed from the initial isoprene + OH reaction. Recent laboratory and field studies indicate later g...

  19. Ozonolysis of a series of biogenic organic volatile compounds and secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Bernard, François; Quilgars, Alain; Cazaunau, Mathieu; Grosselin, Benoît.; Daele, Véronique; Mellouki, Abdelwahid; Winterhalter, Richard; Moortgat, Geert K.

    2010-05-01

    obtained will be compared with those from the literature when available and discussed in terms of their atmospheric impact. Berndt, T., O. Böge and F. Stratmann (2003). Gas-phase ozonolysis of a-pinene: gaseous products and particle formation. Atmospheric Environment, 37: 3933-3945. Bonn, B. and G.K. Moortgat (2003). Sesquiterpene ozonolysis: Origin of atmospheric new particle formation from biogenic hydrocarbons. Journal of Geophysical Research, 30(11). Kavouras, I. and E.G. Stephanou (2002). Direct evidence of atmospheric secondary organic aerosol formation in forest atmosphere through heteromolecular nucleation. Environmental Science and Technology, 36: 5083-5091. Koch, S., R. Winterhalter, E. Uherek, A. Kolloff, P. Neeb and G.K. Moortagt (2000). Formation of new particles in the gas-phase ozonolysis of monoterpenes. Atmospheric Environment, 34: 4031-4042. Kulmala, M., V.-M. Kerminen, T. Anttila, A. Laaksonen and C.D. O'Dowd (2004b). Organic aerosol formation via sulphate cluster activation. Journal of Geophysical Research, 109(D04205): 1-7. Kulmala, M., H. Vehkamäki, T. Petäjä, M. Dal Maso, A. Lauri, V.-M. Kerminen, W. Birmili and P.H. McMurry (2004a). Formation and growth rates of ultra-fine atmospheric particles: a review of observations. Journal of Aerosol Science, 35: 143-176. Lee, S. and R.M. Kamens (2005). Particle nucleation from the reaction of a-pinene and O3. Atmospheric Environment, 39: 6822-6832.

  20. Absorption of Visible and Long-wave Radiation by Primary and Secondary Biogenic Aerosols.

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

    Field results for the 14C content of carbonaceous aerosols are presented that indicate significant biogenic sources of both primary and secondary aerosols in urban and regional environments. Samples collected in Mexico City and downwind of the urban area during the MILAGRO field study are compared with results reported previously in the literature indicating a significant amount of biogenic aerosols from both biomass burning and secondary photochemical production (e.g. terpene oxidations) are contributing to the overall carbonaceous aerosols in the optically active region of 0.1 to 1.0 micron. Samples in this size range collected on quartz fiber filters were also examined using an integrating sphere and FTIR diffuse reflectance techniques to obtain absorption spectra from 280 to the mid-IR. These data clearly indicate that the biogenic derived primary aerosols from agricultural and trash-burning, as well as secondary organic aerosols from isoprene and terpene oxidations will produce both UV-Visible (short-wave) absorbing substances as well as IR (long-wave) absorbing compounds including humic-like-substances (HULIS). With the anticipated increases in growing seasons (i.e. earlier springs and longer summers) the likely hood of increased fires (forest and grassland) as well as the continuing growth in agricultural burning activities, these primary sources are expected to increase and may play a role in heating of the atmosphere. The compound effects of these primary and secondary biogenic sources of absorbing aerosols to the total aerosol loading and regional climate will be discussed. This work was supported by the Office of Science (BER), U.S. Department of Energy, Grant No. DE-FG02-07ER64328 as part of the Atmospheric Science Program.

  1. Incremental Reactivity Effects on Secondary Organic Aerosol Formation in Urban Atmospheres with and without Biogenic Influence

    NASA Astrophysics Data System (ADS)

    Kacarab, Mary; Li, Lijie; Carter, William P. L.; Cocker, David R., III

    2016-04-01

    Two different surrogate mixtures of anthropogenic and biogenic volatile organic compounds (VOCs) were developed to study secondary organic aerosol (SOA) formation at atmospheric reactivities similar to urban regions with varying biogenic influence levels. Environmental chamber simulations were designed to enable the study of the incremental aerosol formation from select anthropogenic (m‑Xylene, 1,2,4-Trimethylbenzene, and 1-Methylnaphthalene) and biogenic (α-pinene) precursors under the chemical reactivity set by the two different surrogate mixtures. The surrogate reactive organic gas (ROG) mixtures were based on that used to develop the maximum incremental reactivity (MIR) factors for evaluation of O3 forming potential. Multiple incremental aerosol formation experiments were performed in the University of California Riverside (UCR) College of Engineering Center for Environmental Research and Technology (CE-CERT) dual 90m3 environmental chambers. Incremental aerosol yields were determined for each of the VOCs studied and compared to yields found from single precursor studies. Aerosol physical properties of density, volatility, and hygroscopicity were monitored throughout experiments. Bulk elemental chemical composition from high-resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) data will also be presented. Incremental yields and SOA chemical and physical characteristics will be compared with data from previous single VOC studies conducted for these aerosol precursors following traditional VOC/NOx chamber experiments. Evaluation of the incremental effects of VOCs on SOA formation and properties are paramount in evaluating how to best extrapolate environmental chamber observations to the ambient atmosphere and provides useful insights into current SOA formation models. Further, the comparison of incremental SOA from VOCs in varying surrogate urban atmospheres (with and without strong biogenic influence) allows for a unique perspective on the impacts

  2. Atmospheric Aerosol Nucleation: Formation of Sub-3 nm Particles and Their Subsequent Growth

    NASA Astrophysics Data System (ADS)

    Lee, S.

    2012-12-01

    Aerosol nucleation is an important step in the chain reaction that lead to cloud formation but the nucleation mechanisms are poorly understand. Most of the previous aerosol nucleation studies were based on measurements of particles, typically larger than 3 nm, so it was unclear how gas phase molecules nucleate to form clusters and how they further grow to become aerosol particles. In this presentation, we will show recent results of aerosol nucleation based on direct measurements of sub-3 nm particles. We will show laboratory studies of multicomponent nucleation involving sulfuric acid, ammonia, and organic amines and atmospheric observations made in various atmospheric conditions (biogenic, marine, and less polluted continental atmosphere).

  3. Measurements of Biogenic and Anthropogenic Ozone and Aerosol Precursors during the SENEX (Southeast Nexus) Campaign 2013

    NASA Astrophysics Data System (ADS)

    Warneke, C.; Trainer, M.; De Gouw, J. A.

    2013-12-01

    Natural emissions of ozone and aerosol precursor gases such as isoprene and monoterpenes are the highest in the southeast of the U.S. and rival those found in tropical forests. In addition, anthropogenic emissions are significant in the Southeast and photochemistry is rapid. The southeast U.S. has not warmed like other parts of the U.S. in response to global climate change, and the temperature anomaly has been suggested to be related to aerosols derived from a combination of anthropogenic and biogenic precursors. The NOAA SENEX aircraft campaign took place in June-July 2013 in the southeast U.S. as part of the Southeast Atmosphere Study (SAS). The NOAA WP-3 aircraft conducted 20 research flights between May 27 and July 10, 2013 based out of Smyrna, TN. To investigate the combination of anthropogenic and biogenic emissions several flights were designed to follow the emissions of cities and power plants as they are transported over forested regions in the Southeast. For example, over-flights of Atlanta, Birmingham and Nashville were performed and the plumes were followed to the forested areas with high isoprene and monoterpene emissions. The same was done for several power plants such as EC Gaston, Scherer and Johnsonville. In the anthropogenic plumes, effects such as the modulation of the isoprene chemistry by high NOx and particle formation and growth were investigated. The same strategy was used for three nighttime flights over Atlanta, Birmingham and the New Madrid and White Bluff power plants. Flights over and downwind of St Lois and Indianapolis were used as a contrast in areas with smaller biogenic emissions. Other anthropogenic emissions sources that were investigated during SENEX included bio refineries, paper mills, coalmines, poultry and pork farming. Also biomass burning emissions were observed during one daytime and one nighttime flight. Another focus of the SENEX campaign was to determine the emissions of natural gas and oil production from the

  4. 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.

  5. Urban stress-induced biogenic VOC emissions impact secondary aerosol formation in Beijing

    NASA Astrophysics Data System (ADS)

    Ghirardo, A.; Xie, J.; Zheng, X.; Wang, Y.; Grote, R.; Block, K.; Wildt, J.; Mentel, T.; Kiendler-Scharr, A.; Hallquist, M.; Butterbach-Bahl, K.; Schnitzler, J.-P.

    2015-08-01

    Trees can significantly impact the urban air chemistry by the uptake and emission of reactive biogenic volatile organic compounds (BVOCs), which are involved in ozone and particle formation. Here we present the emission potentials of "constitutive" (cBVOCs) and "stress-induced" BVOCs (sBVOCs) from the dominant broadleaf woody plant species in the megacity of Beijing. Based on an inventory of BVOC emissions and the tree census, we assessed the potential impact of BVOCs on secondary particulate matter formation in 2005 and 2010, i.e., before and after realizing the large tree-planting program for the 2008 Olympic Games. We found that sBVOCs, such as fatty acid derivatives, benzenoids and sesquiterpenes, constituted a significant fraction (∼ 15 %) of the total annual BVOC emissions, and we estimated that the overall annual BVOC budget may have doubled from ∼ 3.6 × 109 g C year-1 in 2005 to ∼ 7.1 × 109 g C year-1 in 2010 due to the increase in urban greens, while at the same time, the emission of anthropogenic VOCs (AVOCs) could be lowered by 24 %. Based on our BVOC emission assessment, we estimated the biological impact on SOA mass formation in Beijing. Compared to AVOCs, the contribution of biogenic precursors (2-5 %) for secondary particulate matter in Beijing was low. However, sBVOCs can significantly contribute (∼ 40 %) to the formation of total secondary organic aerosol (SOA) from biogenic sources; apparently, their annual emission increased from 1.05 μg m-3 in 2005 to 2.05 μg m-3 in 2010. This study demonstrates that biogenic and, in particular, sBVOC emissions contribute to SOA formation in megacities. However, the main problems regarding air quality in Beijing still originate from anthropogenic activities. Nevertheless, the present survey suggests that in urban plantation programs, the selection of plant species with low cBVOC and sBVOC emission potentials have some possible beneficial effects on urban air quality.

  6. Investigation of formation and ageing of biogenic secondary aerosols by soft ionization aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Müller, Lars; Reinnig, Marc-Christopher; Vogel, Alexander; Mentel, Thomas; Tillmann, Ralf; Schlosser, E.; Wahner, Andreas; Donahue, Neil; Saathoff, Harald; Hoffmann, Thorsten

    2010-05-01

    The knowledge of the chemical composition of secondary organic aerosol is one essential key to understand the significance and fate of SOA in the atmosphere. However, the chemical evolution of SOA, from the very first condensing/nucleating molecules to the final oxidation products is still insufficiently understood and object of current research [1-3]. Consequently, the formation and photochemical ageing of secondary organic aerosol (SOA) was investigated in a series of reaction chamber experiments by applying on-line aerosol mass spectrometry (atmospheric pressure chemical ionization mass spectrometry (APCI/MS)) as well as off-line high performance liquid chromatography mass spectrometry (HPLC-MS). In a set of experiments, performed in the large outdoor reaction chamber SAPHIR (Jülich, Germany), SOA was generated from a boreal mixture of biogenic VOCs. During a two-day experiment the generated biogenic SOA was exposed to OH-radicals and the temporal evolution of the chemical composition was characterized. The applied on-line MS method not only provides highly time resolved chemical information (such as an AMS) but also allows molecular identification/quantification of specific marker compounds. Several first and higher generation BSOA products were identified. Among the higher generation products, especially a tricarboxylic acid (3-methyl-1,2,3-butanetricarboxylic acid) [2] was observed as an eye-catching oxidative processing marker. A more detailed investigation of hydroxyl radical induced SOA aging at the AIDA chamber facility in Karlsruhe, again using terpenes as SOA precursors, clearly showed that the formation of the tricarboxylic acid takes place in the gas phase by the reaction of semivolatile first generation products and hydroxyl radicals. Actually, there were no indications for OH induced oxidation of compounds in the condensed phase. The consequences of these results will be discussed in the contribution. 1. Rudich, Y., N.M. Donahue, and T.F. Mentel

  7. Chemistry of new particle growth in mixed urban and biogenic emissions - insights from CARES

    NASA Astrophysics Data System (ADS)

    Setyan, A.; Song, C.; Merkel, M.; Knighton, W. B.; Onasch, T. B.; Canagaratna, M. R.; Worsnop, D. R.; Wiedensohler, A.; Shilling, J. E.; Zhang, Q.

    2014-01-01

    Regional new particle formation and growth events (NPE) were observed on most days over the Sacramento and western Sierra Foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPE usually occurred in the morning with the appearance of an ultrafine mode centered at ~15 nm (in mobility diameter, Dm, measured by a scanning mobility particle sizer operating in the range 10-858 nm) followed by the growth of this mode to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h-1) than at T1 (6.2 ± 2.5 nm h-1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPE was very similar to that of anthropogenically-influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon, CO, NOx

  8. Chemistry of new particle growth in mixed urban and biogenic emissions - insights from CARES

    NASA Astrophysics Data System (ADS)

    Setyan, A.; Song, C.; Merkel, M.; Knighton, W. B.; Onasch, T. B.; Canagaratna, M. R.; Worsnop, D. R.; Wiedensohler, A.; Shilling, J. E.; Zhang, Q.

    2014-07-01

    Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range 10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1 ± 2.7 nm h-1) than at T1 (6.2 ± 2.5 nm h-1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+, C2H3N+, and C2H4N+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban plumes. In addition, the concentrations of species representative of urban emissions (e.g., black carbon

  9. Biogenic contribution to PM-2.5 ambient aerosol from radiocarbon measurements

    NASA Astrophysics Data System (ADS)

    Lewis, C.; Klouda, G.; Ellenson, W.

    2003-04-01

    Knowledge of the relative contributions of biogenic versus anthropogenic sources to ambient aerosol is of great interest in the formulation of strategies to achieve nationally mandated air quality standards. Radiocarbon (14C) measurements provide a means to quantify the biogenic fraction of any carbon-containing sample of ambient aerosol. In the absence of an impact from biomass burning (e.g., during summertime) such measurements can provide an estimate of the contribution of biogenic secondary organic aerosol, from biogenic volatile organic compound precursors. Radiocarbon results for 11.5-h PM-2.5 samples collected near Nashville, Tennessee, USA, during summer 1999 will be presented. On average the measured biogenic fraction was surprisingly large (more than half), with the average biogenic fraction for night samples being only slightly smaller than for day samples. Discussion will include (a) description of the radiocarbon methodology, (b) use of radiocarbon measurements on local vegetation and fuel samples as calibration data, (c) concurrent measurements of organic carbon and elemental carbon ambient concentrations, (d) assessment of organic aerosol sampling artifact through use of organic vapor denuders, variable face velocities, and filter extraction, and (e) comparison with published radiocarbon results obtained in Houston, Texas in a similar study. Disclaimer: This work has been funded wholly or in part by the United States Environmental Protection Agency under Interagency Agreement No. 13937923 to the National Institute of Standards and Technology, and Contract No. 68-D5-0049 to ManTech Environmental Tecnology, Inc. It has been subjected to Agency review and approved for publication.

  10. Understanding the anthropogenic influence on formation of biogenic secondary organic aerosols via analysis of organosulfates and related oxidation products

    NASA Astrophysics Data System (ADS)

    Nguyen, Q. T.; Christensen, M. K.; Cozzi, F.; Zare, A.; Hansen, A. M. K.; Kristensen, K.; Tulinius, T. E.; Madsen, H. H.; Christensen, J. H.; Brandt, J.; Massling, A.; Nøjgaard, J. K.; Glasius, M.

    2014-01-01

    Anthropogenic emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) may affect concentration levels and composition of biogenic secondary organic aerosols (BSOA) through photochemical reactions with biogenic organic precursors to form organosulfates and nitrooxy organosulfates. We investigated this influence in a field study from 19 May-22 June 2011 at two sampling sites in Denmark. Within the study, we identified a substantial number of organic acids, organosulfates and nitrooxy organosulfates in the ambient urban curbside and semi-rural background air. A high degree of correlation in concentrations was found among a group of specific organic acids, organosulfates and nitrooxy organosulfates, which may originate from various precursors, suggesting a common mechanism or factor affecting their concentration levels at the sites. It was proposed that the formation of those species most likely occurred on a larger spatial scale with the compounds being long-range transported to the sites on the days with highest concentrations. The origin of the long-range transported aerosols was investigated using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model in addition to modeled emissions of related precursors including isoprene and monoterpenes using the global Model of Emissions of Gases and Aerosols from Nature (MEGAN) and SO2 emissions using the European Monitoring and Evaluation Program (EMEP) database. The local impacts were also studied by examining the correlation between selected species which showed significantly enhanced concentrations at the urban curbside site and the local concentrations of various gases including SO2, ozone (O3), carbon monoxide (CO), NOx, aerosol acidity and other meteorological conditions. This investigation showed that an inter-play of the local parameters such as the aerosol acidity, NOx, relative humidity (RH), temperature and global radiation seemed to influence the concentration level of those species, via

  11. 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

  12. Dimethyl sulfide air-sea fluxes and biogenic sulfur as a source of new aerosols in the Arctic fall

    NASA Astrophysics Data System (ADS)

    Rempillo, Ofelia; Seguin, Alison Michelle; Norman, Ann-Lise; Scarratt, Michael; Michaud, Sonia; Chang, Rachel; Sjostedt, Steve; Abbatt, Jon; Else, Brent; Papakyriakou, Tim; Sharma, Sangeeta; Grasby, Steve; Levasseur, Maurice

    2011-09-01

    Dimethyl sulfide (DMS) and its oxidation products, which have been proposed to provide a climate feedback mechanism by affecting aerosol and cloud radiative properties, were measured on board the Canadian Coast Guard ship Amundsen in sampling campaigns in the Arctic in the fall of 2007 and 2008. DMS flux was calculated based on the surface water measurements and yielded 0.1-2.6 μmol m-2 d-1 along the Northwest Passage in 2007 and 0.2-1.3 μmol m-2 d-1 along Baffin Bay in 2008. DMS oxidation products, sulfur dioxide (SO2), methane sulfonic acid (MSA), and sulfate in aerosols were also measured. The amounts of biogenic SO2 and sulfate were approximated using stable isotope apportionment techniques. Calculating the threshold amount of SO2 needed for significant new particle formation from the formulation by Pirjola et al. (1999), the study suggests that instances of elevated biogenic SO2 concentrations (between 8 and 9 September 2008) derived using conservative assumptions may have been sufficient to form new aerosols in clean air conditions in the Arctic region.

  13. Size distribution studies in the SOA-particle formation during the ozonolysis of biogenic alkenes

    NASA Astrophysics Data System (ADS)

    Moortgat, G.; Bonn, B.; Winterhalter, R.

    2003-04-01

    It is established that secondary organic aerosols (SOA) are formed during the reaction of ozone with biogenic alkenes. Experiments of endocyclic (e.g. alpha-pinene, 3-carene) as well as exocyclic monoterpenes (e.g. beta-pinene, sabinene) with ozone have been performed with additional compounds such as water vapour, alcohols and carbonyl compounds, to examine their effect on the SOA particle size distribution in dependence of the alkene structure. This study was further used to describe the formation mechanism of nucleating species for both endo- and exocyclic terpene reactions. Experiments were performed in a spherical glass vessel of 570 L volume at atmospheric pressure. The particle size distribution was measured by a scanning mobility particle sizer, including a long DMA and an ultra-fine particle counter, with a time resolution of two minutes. Cyclohexane was present to prevent interfering reactions of the produced OH-radicals. The laboratory results seem to indicate that the homogeneous nucleation process during the ozonolysis of terpenes is controlled by the formation of large secondary ozonides and can be supressed by the addition of water vapour. These nucleating secondary ozonides are formed differently in endo-and exocyclic reactions: intramolecular in endocyclic and intermolecular in exocylic monoterpene ozonolyses. Such processes are known to be controlled by the stabilized Criegee Intermediates (CI), formed in the ozone reaction with biogenic terpenes. On the other hand, analysis of aerosol material from laboratory and some sparse field studies have identifed various multifunctional dicarboxylic, and keto-carboxylic acids (e.g. pinic and pinonic acid), whose current formation mechanism seems to involve excited CI. Due to their low volatility, these acids may act as nucleation precursors (new particle formation) or condense on preexisting particles (heterogeneous nucleation). The current dilemma, whether stabilized or excited CI are involved in the

  14. Potential Organic Aerosol Formation from Biogenic Compounds: Model and Measurement analysis of the BEACHON-RoMBAS 2011 field data

    NASA Astrophysics Data System (ADS)

    Hodzic, A.; Lee-Taylor, J.; Aumont, B.; Madronich, S.; Palm, B. B.; Campuzano Jost, P.; Day, D. A.; Jimenez, J. L.; Karl, T.; Apel, E. C.; Kaser, L.; Hansel, A.

    2012-12-01

    The scientific understanding of the formation of organic aerosols (OA) from biogenic precursors and their ageing, especially in the presence of anthropogenic pollution, is still limited. The Rocky Mountain Biogenic Aerosol field Study (RoMBAS) took place in summer 2011 at the Manitou Forest Observatory in the Colorado Front Range as part of the NCAR Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen (BEACHON) project with the specific objective of characterizing the formation and growth of biogenic particles in the forest canopy that is dominated by terpene and MBO biogenic emissions. Here we present the results of the box model Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A) that was applied at the measurement site to study local production of secondary OA (SOA), as well as the results of the 3D regional Weather Research and Forecasting model with chemistry (WRF/Chem) that was run at 4km horizontal resolution to simulate the regional transport and chemistry. First, we quantify the relative contribution of various biogenic and anthropogenic precursors to SOA levels that were measured by the Aerosol Mass Spectrometer (AMS). The GECKO-A model is initialized from measured VOC concentrations, and uses MEGAN biogenic emissions and WRF/Chem meteorological forcing. The predicted SOA daytime levels at the site of ~0.7-1.0 microg/m3 are consistent with the observations. The SOA production in GECKO from individual VOC precursors is estimated and compared with WRF/Chem predictions which are based on simplified two-product parameterizations as commonly used in regional models. The sensitivity of the SOA formation to the deposition of semi-volatile vapors, and to an increase in NOx and NO3 levels is also discussed for this site that is frequently influenced by advection of the anthropogenic plumes from Denver. Second, we examine how the organic vapors age after several days of atmospheric processing by

  15. Secondary Organic Aerosol from biogenic VOCs over West Africa during AMMA

    NASA Astrophysics Data System (ADS)

    Capes, G.; Murphy, J. G.; Reeves, C. E.; McQuaid, J. B.; Hamilton, J. F.; Hopkins, J. R.; Crosier, J.; Williams, P. I.; Coe, H.

    2009-01-01

    This paper presents measurements of organic aerosols above subtropical West Africa during the wet season using data from the UK Facility for Airborne Atmospheric Measurements (FAAM) aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment during July and August 2006 mainly above Benin, Nigeria and Niger. Data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show a median organic aerosol loading of 1.08 μg m-3 over tropical West Africa, which represents the first regionally averaged assessment of organic aerosol mass (OM) in this region during the wet season. This is in good agreement with predictions based on aerosol yields from isoprene and monoterpenes during chamber studies and model predictions based on partitioning schemes, contrasting markedly with the large under representations of OM in similar models when compared with data from mid latitudes.

  16. Organic nitrate aerosol formation via NO3 + biogenic volatile organic compounds in the southeastern United States

    NASA Astrophysics Data System (ADS)

    Ayres, B. R.; Allen, H. M.; Draper, D. C.; Brown, S. S.; Wild, R. J.; Jimenez, J. L.; Day, D. A.; Campuzano-Jost, P.; Hu, W.; de Gouw, J.; Koss, A.; Cohen, R. C.; Duffey, K. C.; Romer, P.; Baumann, K.; Edgerton, E.; Takahama, S.; Thornton, J. A.; Lee, B. H.; Lopez-Hilfiker, F. D.; Mohr, C.; Wennberg, P. O.; Nguyen, T. B.; Teng, A.; Goldstein, A. H.; Olson, K.; Fry, J. L.

    2015-12-01

    Gas- and aerosol-phase measurements of oxidants, biogenic volatile organic compounds (BVOCs) and organic nitrates made during the Southern Oxidant and Aerosol Study (SOAS campaign, Summer 2013) in central Alabama show that a nitrate radical (NO3) reaction with monoterpenes leads to significant secondary aerosol formation. Cumulative losses of NO3 to terpenes are correlated with increase in gas- and aerosol-organic nitrate concentrations made during the campaign. Correlation of NO3 radical consumption to organic nitrate aerosol formation as measured by aerosol mass spectrometry and thermal dissociation laser-induced fluorescence suggests a molar yield of aerosol-phase monoterpene nitrates of 23-44 %. Compounds observed via chemical ionization mass spectrometry (CIMS) are correlated to predicted nitrate loss to BVOCs and show C10H17NO5, likely a hydroperoxy nitrate, is a major nitrate-oxidized terpene product being incorporated into aerosols. The comparable isoprene product C5H9NO5 was observed to contribute less than 1 % of the total organic nitrate in the aerosol phase and correlations show that it is principally a gas-phase product from nitrate oxidation of isoprene. Organic nitrates comprise between 30 and 45 % of the NOy budget during SOAS. Inorganic nitrates were also monitored and showed that during incidents of increased coarse-mode mineral dust, HNO3 uptake produced nitrate aerosol mass loading at a rate comparable to that of organic nitrate produced via NO3 + BVOCs.

  17. Direct radiative feedback due to biogenic secondary organic aerosol estimated from boreal forest site observations

    NASA Astrophysics Data System (ADS)

    Lihavainen, Heikki; Asmi, Eija; Aaltonen, Veijo; Makkonen, Ulla; Kerminen, Veli-Matti

    2015-10-01

    We used more than five years of continuous aerosol measurements to estimate the direct radiative feedback parameter associated with the formation of biogenic secondary organic aerosol (BSOA) at a remote continental site at the edge of the boreal forest zone in Northern Finland. Our upper-limit estimate for this feedback parameter during the summer period (ambient temperatures above 10 °C) was -97 ± 66 mW m-2 K-1 (mean ± STD) when using measurements of the aerosol optical depth (fAOD) and -63 ± 40 mW m-2 K-1 when using measurements of the ‘dry’ aerosol scattering coefficient at the ground level (fσ). Here STD represents the variability in f caused by the observed variability in the quantities used to derive the value of f. Compared with our measurement site, the magnitude of the direct radiative feedback associated with BSOA is expected to be larger in warmer continental regions with more abundant biogenic emissions, and even larger in regions where biogenic emissions are mixed with anthropogenic pollution.

  18. 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

  19. 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.

  20. Ice Formation Potential of Laboratory Generated Biogenic and Anthropogenic-Biogenic SOA Particles

    NASA Astrophysics Data System (ADS)

    Knopf, D. A.; Alpert, P. A.; Charnawskas, J. C.; Lambe, A. T.; Massoli, P.; Onasch, T. B.; Davidovits, P.; Worsnop, D. R.

    2014-12-01

    Secondary organic aerosol (SOA) is ubiquitous in the atmosphere and may play an important role in cloud glaciation processes. We investigated several laboratory generated SOA particles systems for their initial water uptake and ice formation propensity as a function of temperature, T, relative humidity with respect to water, RH, relative humidity with respect to ice, RHice, and for different humidification rates, cRHice. This includes pure SOA particles formed from α-pinene, isoprene, and longifolene volatile organic compound precursors with and without the presence of sulfate seed particles as well as oxidized soot and soot-coated α-pinene and naphthalene SOA with varying O/C ratios and coating thicknesses. Micro-spectroscopic chemical imaging using scanning transmission X-ray microscopy with near edge X-ray absorption fine structure spectroscopy (STXM/NEXAFS) is used to characterize SOA, SOA-sulfate, SOA-soot particles generated in the Boston College potential aerosol mass (PAM) flow reactor in relation to their ice nucleation behavior. Water uptake is consistently observed on SOA particles at RH=75% and 95% for 262 and 228 K, respectively, followed by homogeneous ice nucleation applying atmospherically relevant cRHice=1 % min-1. When cRHice=25 % min-1, ice nucleation is delayed by about 30-40% RHice and cannot be explained by homogeneous ice nucleation. This implies diffusion limitation of water into these potentially glassy or semi-solid organic particles resulting in non-equilibrium between ambient RH and particle water activity. These data will aid in our understanding of the role of organic particle phase states in response to changes in T and RH which is crucial information for prediction of atmospheric ice nucleation.

  1. Aerosol Size Distribution Response to Anthropogenically Driven Historical Changes in Biogenic Secondary Organic Aerosol Formation

    NASA Astrophysics Data System (ADS)

    Pierce, J. R.; D'Andrea, S.; Acosta Navarro, J. C.; Farina, S.; Scott, C.; Farmer, D. K.; Spracklen, D. V.; Riipinen, I.

    2014-12-01

    Emissions of biological volatile organic compounds (BVOC) have changed in the past millennium due to changes in land use, temperature and CO2 concentrations. A recent model reconstruction of BVOC emissions over the past millennium predicted the changes in the three dominant secondary organic aerosol (SOA) producing BVOC classes (isoprene, monoterpenes and sesquiterpenes). The reconstruction predicted that in global averages isoprene emissions have decreased (land-use changes to crop/grazing land dominate the reduction), while monoterpene and sesquiterpene emissions have increased (temperature increases dominate the increases); however, all three show both increases and decreases in certain regions due to competition between the various influencing factors. These BVOC changes have largely been anthropogenic in nature, and land-use change was shown to have the most dramatic effect by decreasing isoprene emissions. We use these modeled estimates of these three dominant BVOC classes' emissions from the years 1000 to 2000 to test the effect of anthropogenic changes to BVOC emissions on SOA formation and global aerosol size distributions using the GEOS-Chem-TOMAS global aerosol microphysics model. With anthropogenic emissions (e.g. SO2, NOx, primary aerosols) held at present day values and BVOC emissions changed from year 1000 to year 2000 values, decreases in the number concentration of particles of size Dp > 80 nm (N80) of >25% in year 2000 relative to year 1000 were predicted in regions with extensive land-use changes since year 1000. This change in N80 was predominantly driven by a shift towards crop/grazing land that produces less BVOC than the natural vegetation. Similar sensitivities to year 1000 vs. year 2000 BVOC emissions exist when anthropogenic emissions are turned off. This large decrease in N80 could be a largely overlooked and important anthropogenic aerosol effect on regional climates.

  2. The effects of increasing atmospheric ozone on biogenic monoterpene profiles and the formation of secondary aerosols

    NASA Astrophysics Data System (ADS)

    Pinto, Delia M.; Tiiva, Päivi; Miettinen, Pasi; Joutsensaari, Jorma; Kokkola, Harri; Nerg, Anne-Marja; Laaksonen, Ari; Holopainen, Jarmo K.

    Monoterpenes are biogenic volatile organic compounds (BVOCs) which play an important role in plant adaptation to stresses, atmospheric chemistry, plant-plant and plant-insect interactions. In this study, we determined whether ozonolysis can influence the monoterpenes in the headspace of cabbage. The monoterpenes were mixed with an air-flow enriched with 100, 200 or 400 ppbv of ozone (O 3) in a Teflon chamber. The changes in the monoterpene and O 3 concentrations, and the formation of secondary organic aerosols (SOA) were determined during ozonolysis. Furthermore, the monoterpene reactions with O 3 and OH were modelled using reaction kinetics equations. The results showed that all of the monoterpenes were unequally affected: α-thujene, sabinene and D-limonene were affected to the greatest extend, whereas the 1,8-cineole concentration did not change. In addition, plant monoterpene emissions reduced the O 3 concentration by 12-24%. The SOA formation was dependent on O 3 concentration. At 100 ppbv of O 3, virtually no new particles were formed but clear SOA formation was observed at the higher ozone concentrations. The modelled results showed rather good agreements for α-pinene and 1,8-cineole, whereas the measured concentrations were clearly lower compared to modelled values for sabinene and limonene. In summary, O 3-quenching by monoterpenes occurs beyond the boundary layer of leaves and results in a decreased O 3 concentration, altered monoterpene profiles and SOA formation.

  3. Campholenic aldehyde ozonolysis: a mechanism leading to specific biogenic secondary organic aerosol constituents

    NASA Astrophysics Data System (ADS)

    Kahnt, A.; Iinuma, Y.; Mutzel, A.; Böge, O.; Claeys, M.; Herrmann, H.

    2014-01-01

    In the present study, campholenic aldehyde ozonolysis was performed to investigate pathways leading to specific biogenic secondary organic aerosol (SOA) marker compounds. Campholenic aldehyde, a known α-pinene oxidation product, is suggested to be a key intermediate in the formation of terpenylic acid upon α-pinene ozonolysis. It was reacted with ozone in the presence and absence of an OH radical scavenger, leading to SOA formation with a yield of 0.75 and 0.8, respectively. The resulting oxidation products in the gas and particle phases were investigated employing a denuder/filter sampling combination. Gas-phase oxidation products bearing a carbonyl group, which were collected by the denuder, were derivatised by 2,4-dinitrophenylhydrazine (DNPH) followed by liquid chromatography/negative ion electrospray ionisation time-of-flight mass spectrometry analysis and were compared to the gas-phase compounds detected by online proton-transfer-reaction mass spectrometry. Particle-phase products were also analysed, directly or after DNPH derivatisation, to derive information about specific compounds leading to SOA formation. Among the detected compounds, the aldehydic precursor of terpenylic acid was identified and its presence was confirmed in ambient aerosol samples from the DNPH derivatisation, accurate mass data, and additional mass spectrometry (MS2 and MS3 fragmentation studies). Furthermore, the present investigation sheds light on a reaction pathway leading to the formation of terpenylic acid, involving α-pinene, α-pinene oxide, campholenic aldehyde, and terpenylic aldehyde. Additionally, the formation of diaterpenylic acid acetate could be connected to campholenic aldehyde oxidation. The present study also provides insights into the source of other highly functionalised oxidation products (e.g. m / z 201, C9H14O5 and m / z 215, C10H16O5), which have been observed in ambient aerosol samples and smog chamber-generated monoterpene SOA. The m / z 201 and 215

  4. Dimers and organosulfates derived from biogenic oxidation products in aerosols during the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX) in California 2007 and 2009 (Invited)

    NASA Astrophysics Data System (ADS)

    Glasius, M.; Worton, D. R.; Kristensen, K.; Nguyen, Q.; Surratt, J.; Enggrob, K. L.; Bouvier-Brown, N. C.; Farmer, D.; Docherty, K. S.; Platt, S.; Bilde, M.; Nøjgaard, J. K.; Seinfeld, J.; Jimenez, J. L.; Goldstein, A.

    2010-12-01

    Oxidation products of biogenic volatile organic compounds, such as monoterpenes and isoprene, contribute to biogenic secondary organic aerosol (BSOA). The organosulfate derivatives of these compounds are formed through heterogeneous reactions involving sulphur compounds, with a considerable contribution from anthropogenic sources. Organosulfate derivatives of biogenic oxidation products thus belong to a new group of anthropogenic enhanced biogenic SOA (ABSOA). The Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX) during summers of 2007 and 2009 provided an excellent platform at Blodgett Forest, California (a ponderosa pine plantation) for studying ABSOA. Typically, polluted air masses were transported upslope from the California Central Valley during day, while night conditions were influenced by downslope transport of air masses, low local atmospheric mixing and formation of a shallow boundary layer. We collected particle samples (PM2.5) as one nighttime and two daytime samples per day. After extraction of filters in polar organic solvents (i.e. acetonitrile or methanol), organic aerosol constituents were analyzed by HPLC coupled through an electrospray inlet to a quadrupole time-of-flight mass spectrometer (qTOF-MS). Organosulfates and nitrooxy organosulfates derived from oxidation products of α-pinene, β-pinene, limonene and isoprene were identified based on their molecular mass and MS fragmentation patterns. Measurements by High Resolution Time of Flight Aerosol Mass Spectrometry (HR-ToF-AMS) show high mass loadings of nitrate in the night and morning samples with highest levels of the nitrooxy organosulfates with MW 295 and MW 297. This may indicate that elevated levels of nitrate and nitrooxy organosulfates are formed in the same polluted air mass, probably through nitrate radical reactions. Terpenylic acid, diterpenylic acid acetate, and methylbutane tricarboxylic acid were found at concentrations comparable to pinic acid. A dimer of

  5. Laboratory studies of the reactive uptake of biogenic species: Evidence for the direct polymerization of isoprene, terpenes and sesquiterpenes on acidic aerosols

    NASA Astrophysics Data System (ADS)

    Li, S.; Liggio, J.; Mihele, C.; Brook, J.

    2006-12-01

    Numerous studies on heterogeneous reactions have shown that polymerization of semi-volatile and volatile organic compounds occurs in aerosols. To date, most evidence suggests that gaseous hydrocarbon oxidation products containing carbonyl functionality are the prime candidates for these processes. Such processes involve primarily hydration, acetal formation, polymerization and aldol-condensation reactions, resulting in oligomer products of potential significance with respect to secondary organic aerosol formation (SOA). However, little information on the heterogeneous reactions of unsaturated hydrocarbons (olefins) is known. Given that biogenic species, many of them unsaturated, make up a considerable portion of hydrocarbons emitted globally, direct reactive uptake of these compounds on aerosols would also potentially be a major source of SOA. In the present study, individual biogenic hydrocarbons were exposed to pre-existing acidic sulfate aerosols within a 2 m3 Teflon reaction chamber under varying relative humidity conditions. An Aerosol Mass Spectrometer was used to quantify any subsequent increase in organic mass as a function of time, and to obtain information regarding the structure of products via aerosol mass spectra. A Proton Transfer Reaction Mass Spectrometer was used to measure the gas-phase concentrations of isoprene, terpenes (?-pinene, ?-pinene, limonene, and carene) and sesquiterpenes (?-caryophylene and humulene) in the reaction chamber. Results from these experiments show that a significant amount of these compounds are taken up by the acidic aerosols rapidly, in a polymerization process which was highly dependent on the particle acidity. This polymerization mechanism likely involves the oxygenation of the resulting polymers via acid catalyzed hydration. The uptake of the unsaturated hydrocarbons suggests that gas-phase oxidation of biogenics to condensable products is not the only route to SOA. Details of the polymerization and hydration

  6. Aerosol and precipitation chemistry measurements in a remote site in Central Amazonia: the role of biogenic contribution

    NASA Astrophysics Data System (ADS)

    Pauliquevis, T.; Lara, L. L.; Antunes, M. L.; Artaxo, P.

    2012-06-01

    In this analysis a 3.5 years data set of aerosol and precipitation chemistry, obtained in a remote site in Central Amazonia (Balbina, (1°55' S, 59°29' W, 174 m a.s.l.), about 200 km north of Manaus) is discussed. Aerosols were sampled using stacked filter units (SFU), which separate fine (d < 2.5 μm) and coarse mode (2.5 μm < d < 10.0 μm) aerosol particles. Filters were analyzed for particulate mass (PM), Equivalent Black Carbon (BCE) and elemental composition by Particle Induced X-Ray Emission (PIXE). Rainwater samples were collected using a wet-only sampler and samples were analyzed for pH and ionic composition, which was determined using ionic chromatography (IC). Natural sources dominated the aerosol mass during the wet season, when it was predominantly of natural biogenic origin mostly in the coarse mode, which comprised up to 81% of PM10. Biogenic aerosol from both primary emissions and secondary organic aerosol dominates the fine mode in the wet season, with very low concentrations (average 2.2 μg m-3). Soil dust was responsible for a minor fraction of the aerosol mass (less than 17%). Sudden increases in the concentration of elements as Al, Ti and Fe were also observed, both in fine and coarse mode (mostly during the April-may months), which we attribute to episodes of Saharan dust transport. During the dry periods, a significant contribution to the fine aerosols loading was observed, due to the large-scale transport of smoke from biomass burning in other portions of the Amazon basin. This contribution is associated with the enhancement of the concentration of S, K, Zn and BCE. Chlorine, which is commonly associated to sea salt and also to biomass burning emissions, presented higher concentration not only during the dry season but also for the April-June months, due to the establishment of more favorable meteorological conditions to the transport of Atlantic air masses to Central Amazonia. The chemical composition of rainwater was similar to those

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

    SciTech Connect

    Madronich, Sasha

    2015-12-09

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

  8. Formation of brown carbon via reactions of ammonia with secondary organic aerosols from biogenic and anthropogenic precursors

    NASA Astrophysics Data System (ADS)

    Updyke, Katelyn M.; Nguyen, Tran B.; Nizkorodov, Sergey A.

    2012-12-01

    Filter samples of secondary organic aerosols (SOA) generated from the ozone (O3)- and hydroxyl radical (OH)-initiated oxidation of various biogenic (isoprene, α-pinene, limonene, α-cedrene, α-humulene, farnesene, pine leaf essential oils, cedar leaf essential oils) and anthropogenic (tetradecane, 1,3,5-trimethylbenzene, naphthalene) precursors were exposed to humid air containing approximately 100 ppb of gaseous ammonia (NH3). Reactions of SOA compounds with NH3 resulted in production of light-absorbing "brown carbon" compounds, with the extent of browning ranging from no observable change (isoprene SOA) to visible change in color (limonene SOA). The aqueous phase reactions with dissolved ammonium (NH4+) salts, such as ammonium sulfate, were equally efficient in producing brown carbon. Wavelength-dependent mass absorption coefficients (MAC) of the aged SOA were quantified by extracting known amounts of SOA material in methanol and recording its UV/Vis absorption spectra. For a given precursor, the OH-generated SOA had systematically lower MAC compared to the O3-generated SOA. The highest MAC values, for brown carbon from SOA resulting from O3 oxidation of limonene and sesquiterpenes, were comparable to MAC values for biomass burning particles but considerably smaller than MAC values for black carbon aerosols. The NH3/NH4+ + SOA brown carbon aerosol may contribute to aerosol optical density in regions with elevated concentrations of NH3 or ammonium sulfate and high photochemical activity.

  9. 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.

  10. The impact of biogenic carbon emissions on aerosol absorption inMexico City

    SciTech Connect

    Marley, N; Gaffney, J; Tackett, M J; Sturchio, N; Hearty, L; Martinez, N; Hardy, K D; Machany-Rivera, A; Guilderson, T P; MacMillan, A; Steelman, K

    2009-02-24

    In order to determine the wavelength dependence of atmospheric aerosol absorption in the Mexico City area, the absorption angstrom exponents (AAEs) were calculated from aerosol absorption measurements at seven wavelengths obtained with a seven-channel aethalometer during two field campaigns, the Mexico City Metropolitan Area study in April 2003 (MCMA 2003) and the Megacity Initiative: Local and Global Research Observations in March 2006 (MILAGRO). The AAEs varied from 0.76 to 1.56 in 2003 and from 0.54 to 1.52 in 2006. The AAE values determined in the afternoon were consistently higher than the corresponding morning values, suggesting the photochemical formation of absorbing secondary organic aerosols (SOA) in the afternoon. The AAE values were compared to stable and radiocarbon isotopic measurements of aerosol samples collected at the same time to determine the sources of the aerosol carbon. The fraction of modern carbon (fM) in the aerosol samples, as determined from {sup 14}C analysis, showed that 70% of the carbonaceous aerosols in Mexico City were from modern sources, indicating a significant impact from biomass burning during both field campaigns. The {sup 13}C/{sup 12}C ratios of the aerosol samples illustrate the significant impact of Yucatan forest fires (C-3 plants) in 2003 and local grass fires (C-4 plants) at site T1 in 2006. A direct comparison of the fM values, stable carbon isotope ratios, and calculated aerosol AAEs suggested that the wavelength dependence of the aerosol absorption was controlled by the biogenically derived aerosol components.

  11. Abundance of Biogenic and Anthropogenic SOA Tracers Compounds in Fine Particles during the Nucleation in Forests Experiment (NIFTy)

    NASA Astrophysics Data System (ADS)

    Jobson, B. T.; Wallace, W.; Westberg, H.; Hamilton, H.; Pryor, S. C.; Barthelmie, R.

    2008-12-01

    The Nucleation in Forests field experiment was conducted in May 2008 at the Morgan-Monroe State forest in Indiana to observe the nature and occurrence of new particle formation. As part of this experiment filter samples were collected at mid-canopy height using a MOUDI-110. The MOUDI sampler collected 10 size fractions from 0.056 um to 5.6 um. The filter samples were collected for 24 hours and analyzed by gas chromatography ion trap mass spectrometry for several anthropogenic and biogenic secondary organic aerosol tracer compounds including 2-methyltetrols from isoprene oxidation. The objective of the size resolved PM sampling was to determine if the growth of small particles that occurs during nucleation events was driven by biogenic or anthropogenic VOC photooxidation products. Results from this analysis will be presented.

  12. Determination of the biogenic secondary organic aerosol fraction in the boreal forest by NMR spectroscopy

    NASA Astrophysics Data System (ADS)

    Finessi, E.; Decesari, S.; Paglione, M.; Giulianelli, L.; Carbone, C.; Gilardoni, S.; Fuzzi, S.; Saarikoski, S.; Raatikainen, T.; Hillamo, R.; Allan, J.; Mentel, Th. F.; Tiitta, P.; Laaksonen, A.; Petäjä, T.; Kulmala, M.; Worsnop, D. R.; Facchini, M. C.

    2012-01-01

    The study investigates the sources of fine organic aerosol (OA) in the boreal forest, based on measurements including both filter sampling (PM1) and online methods and carried out during a one-month campaign held in Hyytiälä, Finland, in spring 2007. Two aerosol mass spectrometers (Q-AMS, ToF-AMS) were employed to measure on-line concentrations of major non-refractory aerosol species, while the water extracts of the filter samples were analyzed by nuclear magnetic resonance (NMR) spectroscopy for organic functional group characterization of the polar organic fraction of the aerosol. AMS and NMR spectra were processed separately by non-negative factorization algorithms, in order to apportion the main components underlying the submicrometer organic aerosol composition and depict them in terms of both mass fragmentation patterns and functional group compositions. The NMR results supported the AMS speciation of oxidized organic aerosol (OOA) into two main fractions, which could be generally labelled as more and less oxidized organics. The more oxidized component was characterized by a mass spectrum dominated by the m/z 44 peak, and in parallel by a NMR spectrum showing aromatic and aliphatic backbones highly substituted with oxygenated functional groups (carbonyls/carboxyls and hydroxyls). Such component, contributing on average 50% of the OA mass throughout the observing period, was associated with pollution outbreaks from the Central Europe. The less oxidized component was enhanced in concomitance with air masses originating from the North-to-West sector, in agreement with previous investigations conducted at this site. NMR factor analysis was able to separate two distinct components under the less oxidized fraction of OA. One of these NMR-factors was associated with the formation of terrestrial biogenic secondary organic aerosol (BSOA), based on the comparison with spectral profiles obtained from laboratory experiments of terpenes photo-oxidation. The second NMR

  13. Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Mentel, Th. F.; Kleist, E.; Andres, S.; Dal Maso, M.; Hohaus, T.; Kiendler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2013-09-01

    Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Biogenic secondary organic aerosols (BSOAs) comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOCs) emitted by vegetation are the source of BSOAs. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed BSOAs, and possibly their climatic effects. This raises questions of whether stress-induced changes in BSOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on BSOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical BSOA formation for plants infested by aphids in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify BSOA formation and yield. Stress-induced emissions of sesquiterpenes, methyl salicylate, and C17-BVOCs increase BSOA yields. Mixtures including these compounds exhibit BSOA yields between 17 and 33%, significantly higher than mixtures containing mainly monoterpenes (4-6% yield). Green leaf volatiles suppress SOA formation, presumably by scavenging OH, similar to isoprene. By classifying emission types, stressors and BSOA formation potential, we discuss possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate-vegetation feedback mechanisms.

  14. Organic compounds in aerosols from selected European sites - Biogenic versus anthropogenic sources

    NASA Astrophysics Data System (ADS)

    Alves, Célia; Vicente, Ana; Pio, Casimiro; Kiss, Gyula; Hoffer, Andras; Decesari, Stefano; Prevôt, André S. H.; Minguillón, María Cruz; Querol, Xavier; Hillamo, Risto; Spindler, Gerald; Swietlicki, Erik

    2012-11-01

    Atmospheric aerosol samples from a boreal forest (Hyytiälä, April 2007), a rural site in Hungary (K-puszta, summer 2008), a polluted rural area in Italy (San Pietro Capofiume, Po Valley, April 2008), a moderately polluted rural site in Germany located on a meadow (Melpitz, May 2008), a natural park in Spain (Montseny, March 2009) and two urban background locations (Zurich, December 2008, and Barcelona, February/March 2009) were collected. Aliphatics, polycyclic aromatic hydrocarbons, carbonyls, sterols, n-alkanols, acids, phenolic compounds and anhydrosugars in aerosols were chemically characterised by gas chromatography-mass spectrometry, along with source attribution based on the carbon preference index (CPI), the ratios between the unresolved and the chromatographically resolved aliphatics, the contribution of wax n-alkanes, n-alkanols and n-alkanoic acids from plants, diagnostic ratios of individual target compounds and source-specific markers to organic carbon ratios. In spite of transboundary pollution episodes, Hyytiälä registered the lowest levels among all locations. CPI values close to 1 for the aliphatic fraction of the Montseny aerosol suggest that the anthropogenic input may be associated with the transport of aged air masses from the surrounding industrial/urban areas, which superimpose the locally originated hydrocarbons with biogenic origin. Aliphatic and aromatic hydrocarbons in samples from San Pietro Capofiume reveal that fossil fuel combustion is a major source influencing the diel pattern of concentrations. This source contributed to 25-45% of the ambient organic carbon (OC) at the Po Valley site. Aerosols from the German meadow presented variable contributions from both biogenic and anthropogenic sources. The highest levels of vegetation wax components and biogenic secondary organic aerosol (SOA) products were observed at K-puszta, while anthropogenic SOA compounds predominated in Barcelona. The primary vehicular emissions in the Spanish

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

    PubMed

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

    2013-12-27

    We present direct measurements of mixing between separately prepared organic aerosol populations in a smog chamber using single-particle mass spectra from the high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Docosane and docosane-d46 (22 carbon linear solid alkane) did not show any signs of mixing, but squalane and squalane-d62 (30 carbon branched liquid alkane) mixed on the time scale expected from a condensational-mixing model. Docosane and docosane-d46 were driven to mix when the chamber temperature was elevated above the melting point for docosane. Docosane vapors were shown to mix into squalane-d62, but not the other way around. These results are consistent with low diffusivity in the solid phase of docosane particles. We performed mixing experiments on secondary organic aerosol (SOA) surrogate systems finding that SOA derived from toluene-d8 (a surrogate for anthropogenic SOA (aSOA)) does not mix into squalane (a surrogate for hydrophobic primary organic aerosol (POA)) but does mix into SOA derived from α-pinene (biogenic SOA (bSOA) surrogate). For the aSOA/POA, the volatility of either aerosol does not limit gas-phase diffusion, indicating that the two particle populations do not mix simply because they are immiscible. In the aSOA/bSOA system, the presence of toluene-d8-derived SOA molecules in the α-pinene-derived SOA provides evidence that the diffusion coefficient in α-pinene-derived SOA is high enough for mixing on the time scale of 1 min. The observations from all of these mixing experiments are generally invisible to bulk aerosol composition measurements but are made possible with single-particle composition data. PMID:24131283

  16. Formation of anthropogenic secondary organic aerosol (SOA) and its influence on biogenic SOA properties

    NASA Astrophysics Data System (ADS)

    Emanuelsson, E. U.; Hallquist, M.; Kristensen, K.; Glasius, M.; Bohn, B.; Fuchs, H.; Kammer, B.; Kiendler-Scharr, A.; Nehr, S.; Rubach, F.; Tillmann, R.; Wahner, A.; Wu, H.-C.; Mentel, Th. F.

    2013-03-01

    Secondary organic aerosol (SOA) formation from mixed anthropogenic and biogenic precursors has been studied exposing reaction mixtures to natural sunlight in the SAPHIR chamber in Jülich, Germany. In this study aromatic compounds served as examples of anthropogenic volatile organic compound (VOC) and a mixture of α-pinene and limonene as an example for biogenic VOC. Several experiments with exclusively aromatic precursors were performed to establish a relationship between yield and organic aerosol mass loading for the atmospheric relevant range of aerosol loads of 0.01 to 10 μg m-3. The yields (0.5 to 9%) were comparable to previous data and further used for the detailed evaluation of the mixed biogenic and anthropogenic experiments. For the mixed experiments a number of different oxidation schemes were addressed. The reactivity, the sequence of addition, and the amount of the precursors influenced the SOA properties. Monoterpene oxidation products, including carboxylic acids and dimer esters were identified in the aged aerosol at levels comparable to ambient air. OH radicals were measured by Laser Induced Fluorescence, which allowed for establishing relations of aerosol properties and composition to the experimental OH dose. Furthermore, the OH measurements in combination with the derived yields for aromatic SOA enabled application of a simplified model to calculate the chemical turnover of the aromatic precursor and corresponding anthropogenic contribution to the mixed aerosol. The estimated anthropogenic contributions were ranging from small (≈8%) up to significant fraction (>50%) providing a suitable range to study the effect of aerosol composition on the aerosol volatility (volume fraction remaining (VFR) at 343 K: 0.86-0.94). The aromatic aerosol had higher oxygen to carbon ratio O/C and was less volatile than the biogenic fraction. However, in order to produce significant amount of aromatic SOA the reaction mixtures needed a higher OH dose that also

  17. Secondary Organic Aerosol from Biogenic VOCs over West Africa during AMMA

    NASA Astrophysics Data System (ADS)

    Capes, G. L.; Murphy, J. G.; Reeves, C. E.; McQuaid, J. B.; Hamilton, J. F.; Hopkins, J. R.; Coe, H.

    2008-12-01

    As part of the international AMMA (African Monsoon Multidisciplinary Analyses) project a large field experiment took place in West Africa during July and August 2006. This involved a number of ground-based facilities and 5 aircraft, including the UK Facility for Airborne Atmospheric Measurements (FAAM) BAe-146, which was based in Niamey, Niger and made 21 flights. The 146 was equipped with instruments measuring parameters relevant to dynamics, gas phase composition, radiation, aerosols and clouds. The flights made were designed to examine a range of multidisciplinary scientific questions. This paper presents measurements of organic aerosol above subtropical West Africa during the monsoon season using data from the FAAM aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during July and August 2006 mainly above Benin, Nigeria and Niger. In air masses characterised by high BVOC concentrations, data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show an organic aerosol loading of 0.58 μgm-3 over tropical West Africa. In contrast, organic aerosol mass (OM) concentrations were negligible when BVOC concentrations were low. This represents the first regionally averaged assessment of OM in this region during the wet season. This is in good agreement with predictions based on aerosol yields from isoprene and monoterpenes during chamber studies and model predictions based on partitioning schemes, contrasting markedly with the large under representations of OM in similar models when compared with data from mid latitudes.

  18. Chemistry of new particle growth in mixed urban and biogenic emissions – insights from CARES

    SciTech Connect

    Setyan, Ari; Song, Chen; Merkel, M.; Knighton, M.; Onasch, Timothy B.; Canagaratna, M. R.; Worsnop, Douglas R.; Wiedensohler, A.; Shilling, John E.; Zhang, Qi

    2014-07-01

    Regional new particle formation and growth events (NPEs) were observed on most days over the Sacramento and western Sierra foothills area of California in June 2010 during the Carbonaceous Aerosols and Radiative Effect Study (CARES). Simultaneous particle measurements at both the T0 (Sacramento, urban site) and the T1 (Cool, rural site located ~40 km northeast of Sacramento) sites of CARES indicate that the NPEs usually occurred in the morning with the appearance of an ultrafine mode at ~15 nm (in mobility diameter, Dm, measured by a mobility particle size spectrometer operating in the range10-858 nm) followed by the growth of this modal diameter to ~50 nm in the afternoon. These events were generally associated with southwesterly winds bringing urban plumes from Sacramento to the T1 site. The growth rate was on average higher at T0 (7.1±2.7 nm h-1) than at T1 (6.2±2.5 nm h-1), likely due to stronger anthropogenic influences at T0. Using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), we investigated the evolution of the size-resolved chemical composition of new particles at T1. Our results indicate that the growth of new particles was driven primarily by the condensation of oxygenated organic species and, to a lesser extent, ammonium sulfate. New particles appear to be fully neutralized during growth, consistent with high NH3 concentration in the region. Nitrogen-containing organic ions (i.e., CHN+, CH4N+,C2H3N+, and C2HN+) that are indicative of the presence of alkyl-amine species in submicrometer particles enhanced significantly during the NPE days, suggesting that amines might have played a role in these events. Our results also indicate that the bulk composition of the ultrafine mode organics during NPEs was very similar to that of anthropogenically influenced secondary organic aerosol (SOA) observed in transported urban

  19. Secondary organic aerosol from biogenic volatile organic compound mixtures

    NASA Astrophysics Data System (ADS)

    Hatfield, Meagan L.; Huff Hartz, Kara E.

    2011-04-01

    The secondary organic aerosol (SOA) yields from the ozonolysis of a Siberian fir needle oil (SFNO), a Canadian fir needle oil (CFNO), and several SOA precursor mixtures containing reactive and non-reactive volatile organic compounds (VOCs) were investigated. The use of precursor mixtures more completely describes the atmosphere where many VOCs exist. The addition of non-reactive VOCs such as bornyl acetate, camphene, and borneol had very little to no effect on SOA yields. The oxidation of VOC mixtures with VOC mass percentages similar to the SFNO produced SOA yields that became more similar to the SOA yield from SFNO as the complexity and concentration of VOCs within the mixture became more similar to overall SFNO composition. The SOA yield produced by the oxidation of CFNO was within the error of the SOA yield produced by the oxidation of SFNO at a similar VOC concentration. The SOA yields from SFNO were modeled using the volatility basis set (VBS), which predicts the SOA yields for a given mass concentration of mixtures containing similar VOCs.

  20. Nuclear microprobe analysis and source apportionment of individual atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Artaxo, Paulo; Rabello, Marta L. C.; Watt, Frank; Grime, Geoff; Swietlicki, Erik

    1993-04-01

    In atmospheric aerosol research, one key issue is to determine the sources of the airborne particles. Bulk PIXE analysis coupled with receptor modeling provides a useful, but limited view of the aerosol sources influencing one particular site or sample. The scanning nuclear microprobe (SNM) technique is a microanalytical technique that gives unique information on individual aerosol particles. In the SNM analyses a 1.0 μm size 2.4 MeV proton beam from the Oxford SNM was used. The trace elements with Z > 11 were measured by the particle induced X-ray emission (PIXE) method with detection limits in the 1-10 ppm range. Carbon, nitrogen and oxygen are measured simultaneously using Rutherford backscattering spectrometry (RBS). Atmospheric aerosol particles were collected at the Brazilian Antarctic Station and at biomass burning sites in the Amazon basin tropical rain forest in Brazil. In the Antarctic samples, the sea-salt aerosol particles were clearly predominating, with NaCl and CaSO 4 as major compounds with several trace elements as Al, Si, P, K, Mn, Fe, Ni, Cu, Zn, Br, Sr, and Pb. Factor analysis of the elemental data showed the presence of four components: 1) soil dust particles; 2) NaCl particles; 3) CaSO 4 with Sr; and 4) Br and Mg. Strontium, observed at 20-100 ppm levels, was always present in the CaSO 4 particles. The hierarchical cluster procedure gave results similar to the ones obtained through factor analysis. For the tropical rain forest biomass burning aerosol emissions, biogenic particles with a high organic content dominate the particle population, while K, P, Ca, Mg, Zn, and Si are the dominant elements. Zinc at 10-200 ppm is present in biogenic particles rich in P and K. The quantitative aspects and excellent detection limits make SNM analysis of individual aerosol particles a very powerful analytical tool.

  1. Evidence of aqueous secondary organic aerosol formation from biogenic emissions in the North American Sonoran Desert

    PubMed Central

    Youn, Jong-Sang; Wang, Zhen; Wonaschütz, Anna; Arellano, Avelino; Betterton, Eric A.; Sorooshian, Armin

    2013-01-01

    This study examines the role of aqueous secondary organic aerosol formation in the North American Sonoran Desert as a result of intense solar radiation, enhanced moisture, and biogenic volatile organic compounds (BVOCs). The ratio of water-soluble organic carbon (WSOC) to organic carbon (OC) nearly doubles during the monsoon season relative to other seasons of the year. When normalized by mixing height, the WSOC enhancement during monsoon months relative to preceding dry months (May–June) exceeds that of sulfate by nearly a factor of 10. WSOC:OC and WSOC are most strongly correlated with moisture parameters, temperature, and concentrations of O3 and BVOCs. No positive relationship was identified between WSOC or WSOC:OC and anthropogenic tracers such as CO over a full year. This study points at the need for further work to understand the effect of BVOCs and moisture in altering aerosol properties in understudied desert regions. PMID:24115805

  2. Microphysical processes affecting stratospheric aerosol particles

    NASA Technical Reports Server (NTRS)

    Hamill, P.; Toon, O. B.; Kiang, C. S.

    1977-01-01

    Physical processes which affect stratospheric aerosol particles include nucleation, condensation, evaporation, coagulation and sedimentation. Quantitative studies of these mechanisms to determine if they can account for some of the observed properties of the aerosol are carried out. It is shown that the altitude range in which nucleation of sulfuric acid-water solution droplets can take place corresponds to that region of the stratosphere where the aerosol is generally found. Since heterogeneous nucleation is the dominant nucleation mechanism, the stratospheric solution droplets are mainly formed on particles which have been mixed up from the troposphere or injected into the stratosphere by volcanoes or meteorites. Particle growth by heteromolecular condensation can account for the observed increase in mixing ratio of large particles in the stratosphere. Coagulation is important in reducing the number of particles smaller than 0.05 micron radius. Growth by condensation, applied to the mixed nature of the particles, shows that available information is consistent with ammonium sulfate being formed by liquid phase chemical reactions in the aerosol particles. The upper altitude limit of the aerosol layer is probably due to the evaporation of sulfuric acid aerosol particles, while the lower limit is due to mixing across the tropopause.

  3. The influence of temperature and aerosol acidity on biogenic secondary organic aerosol tracers: Observations at a rural site in the central Pearl River Delta region, South China

    NASA Astrophysics Data System (ADS)

    Ding, Xiang; Wang, Xin-Ming; Zheng, Mei

    2011-02-01

    At a rural site in the central Pearl River Delta (PRD) region in south China, fine particle (PM 2.5) samples were collected during fall-winter 2007 to measure biogenic secondary organic aerosol (SOA) tracers, including isoprene SOA tracers (3-methyl-2,3,4-trihydroxy-1-butene, 2-methylglyceric acid, 2-methylthreitol and 2-methylerythritol), α-pinene SOA tracers ( cis-pinonic acid, pinic acid, 3-methyl-1,2,3-butanetricarboxylic acid, 3-hydroxyglutaric acid and 3-hydroxy-4,4-dimethylglutaric acid) and a sesquiterpene SOA tracer (β-caryophyllinic acid). The isoprene-, α-pinene- and sesquiterpene-SOA tracers averaged 30.8 ± 15.9, 6.61 ± 4.39, and 0.54 ± 0.56 ng m -3, respectively; and 2-methyltetrols (sum of 2-methylthreitol and 2-methylerythritol, 27.6 ± 15.1 ng m -3) and cis-pinonic acid (3.60 ± 3.76 ng m -3) were the dominant isoprene- and α-pinene-SOA tracers, respectively. 2-Methyltetrols exhibited significantly positive correlations ( p < 0.05) with ambient temperature, probably resulting from the enhanced isoprene emission strength and tracer formation rate under higher temperature. The significantly positive correlation ( p < 0.05) between 2-methyltetrols and the estimated aerosol acidity with a slope of 59.4 ± 13.4 ng m -3 per μmol [H +] m -3 reflected the enhancement of isoprene SOA formation by aerosol acidity, and acid-catalyzed heterogeneous reaction was probably the major formation pathway for 2-methyltetrols in the PRD region. 2-Methylglyceric acid showed poor correlations with both temperature and aerosol acidity. The α-pinene SOA tracers showed poor correlations with temperature, probably due to the counteraction between temperature effects on the precursor emission/tracer formation and gas/particle partitioning. Among the α-pinene SOA tracers, only cis-pinonic acid and pinic acid exhibited significant correlations with aerosol acidity with slopes of -11.7 ± 3.7 and -2.2 ± 0.8 ng m -3 per μmol [H +] m -3, respectively. The negative

  4. Influence of Aerosol Acidity on the Formation of Secondary Organic Aerosol from Biogenic Precursor Hydrocarbons

    EPA Science Inventory

    Secondary organic aerosol (SOA) formation and dynamics may be important factors for the role of aerosols in adverse health effects, visibility and climate change. Formation of SOA occurs when a parent volatile organic compound is oxidized to create products that form in a conden...

  5. Anthropogenic and biogenic organic compounds in summertime fine aerosols (PM2.5) in Beijing, China

    NASA Astrophysics Data System (ADS)

    Yang, Fan; Kawamura, Kimitaka; Chen, Jing; Ho, Kinfai; Lee, Shuncheng; Gao, Yuan; Cui, Long; Wang, Tieguan; Fu, Pingqing

    2016-01-01

    Ambient fine aerosol samples (PM2.5) were collected at an urban site (PKU) in Beijing and its upwind suburban site (Yufa) during the CAREBEIJING-2007 field campaign. Organic molecular compositions of the PM2.5 samples were studied for seven organic compound classes (sugars, lignin/resin acids, hydroxy-/polyacids, aromatic acids, biogenic SOA tracers, fatty acids and phthalates) using capillary GC/MS to better understand the characteristics and sources of organic aerosol pollution in Beijing. More than 60 individual organic species were detected in PM2.5 and were grouped into different compound classes based on their functional groups. Concentrations of total quantified organics at Yufa (469-1410 ng m-3, average 1050 ng m-3) were slightly higher than those at PKU (523-1390 ng m-3, 900 ng m-3). At both sites, phthalates were found as the most abundant compound class. Using a tracer-based method, the contributions of the biogenic secondary organic carbon (SOC) to organic carbon (OC) were 3.1% at PKU and 5.5% at Yufa, among which isoprene-SOC was the dominant contributor. In addition, most of the measured organic compounds were higher at Yufa than those at PKU, indicating a more serious pollution in its upwind region than in urban Beijing.

  6. Molecular composition of biogenic secondary organic aerosols using ultrahigh resolution mass spectrometry: linking laboratory and field studies

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Fuller, Stephen; Aalto, Juho; Healy, Robert; Alfara, Rami; Ruuskanen, Taina; Wenger, John; McFiggans, Gordon; Kulmala, Markku; Kalberer, Markus

    2013-04-01

    Biogenic volatile organic compounds (BVOCs) play an important role in atmospheric chemistry and give rise to secondary organic aerosols (SOA), which have effects on climate and human health. Laboratory chamber experiments have been performed during several decades in an attempt to mimic atmospheric SOA formation. However, it is still unclear how close the aerosol particles generated in laboratory experiments resemble atmospheric SOA with respect to their detailed chemical composition. To date, most laboratory experiments have been performed using a single organic precursor (e.g., alpha- or beta-pinene, isoprene) while in the atmosphere a wide range of precursors contribute to SOA, which results most likely in a more complex SOA composition compared to the one-precursor laboratory systems. The objective of this work is to compare laboratory generated SOA from oxidation of BVOCs mixtures and remote ambient samples using ultrahigh-resolution mass spectrometry (UHR-MS) that allows detection of hundreds of individual SOA constituents. We examined aerosol samples from a boreal forest site, Hyytiälä, Finland and determined that a dominant fraction of the detected compounds are reaction products of a multi-component mixture of BVOCs. In the subsequent smog chamber experiments, SOA was generated from the ozonolysis and OH initiated reactions with BVOC mixtures containing species (alpha- and beta-pinene, delta-3-carene, and isoprene) that are most abundant in Hyytiälä's environment. The laboratory experiments were performed at conditions (e.g., RH, aerosol seed, and VOC ratios) that would resemble those at the boreal sampling site during the summer period. The elemental composition of the complex mixtures from laboratory generated SOA samples were compared with field samples using statistical data analysis methods.

  7. Secondary aerosol formation from stress-induced biogenic emissions and possible climate feedbacks

    NASA Astrophysics Data System (ADS)

    Mentel, Th. F.; Kleist, E.; Andres, S.; Maso, M. D.; Hohaus, T.; Kiendler-Scharr, A.; Rudich, Y.; Springer, M.; Tillmann, R.; Uerlings, R.; Wahner, A.; Wildt, J.

    2013-03-01

    Atmospheric aerosols impact climate by scattering and absorbing solar radiation and by acting as ice and cloud condensation nuclei. Secondary organic aerosols (SOA) comprise an important component of atmospheric aerosols. Biogenic volatile organic compounds (BVOC) emitted by vegetation are a major source of SOA. Pathogens and insect attacks, heat waves and droughts can induce stress to plants that may impact their BVOC emissions, and hence the yield and type of formed SOA, and possibly their climatic effects. This raises questions whether stress-induced changes in SOA formation may attenuate or amplify effects of climate change. In this study we assess the potential impact of stress-induced BVOC emissions on SOA formation for tree species typical for mixed deciduous and Boreal Eurasian forests. We studied the photochemical SOA formation for infested plants in a laboratory setup under well-controlled conditions and applied in addition heat and drought stress. The results indicate that stress conditions substantially modify SOA formation. While sesquiterpenes, methyl salicylate, and C17-BVOC increase SOA yield, green leaf volatiles suppress SOA formation. By classifying emission types, stressors and SOA formation potential, we propose possible climatic feedbacks regarding aerosol effects. We conclude that stress situations for plants due to climate change should be considered in climate-vegetation feedback mechanisms.

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

    NASA Astrophysics Data System (ADS)

    Tabazadeh, Azadeh

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

  9. Contribution of fungi to primary biogenic aerosols in the atmosphere: wet and dry discharged spores, carbohydrates, and inorganic ions

    NASA Astrophysics Data System (ADS)

    Elbert, W.; Taylor, P. E.; Andreae, M. O.; Pöschl, U.

    2007-09-01

    Biogenic aerosols play important roles in atmospheric chemistry physics, the biosphere, climate, and public health. Here, we show that fungi which actively discharge their spores with liquids into the air, in particular actively wet spore discharging Ascomycota (AAM) and actively wet spore discharging Basidiomycota (ABM), are a major source of primary biogenic aerosol particles and components. We present the first estimates for the global average emission rates of fungal spores. Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001) indicate that the spores of AAM and ABM may account for a large proportion of coarse particulate matter in tropical rainforest regions during the wet season (0.7-2.3 μg m-3). For the particle diameter range of 1-10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively wet discharged basidiospores (ABS). ABM emissions seem to account for most of the atmospheric abundance of mannitol (10-68 ng m-3), and can explain the observed diurnal cycle (higher abundance at night). ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter (7-49 ng m-3), but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night). AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season (17-43 ng m-3), and they can also explain the observed diurnal cycle (higher abundance at night). The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations. Based on the average abundance of mannitol reported for extratropical continental boundary layer air

  10. Secondary organic aerosol from biogenic VOCs over West Africa during AMMA

    NASA Astrophysics Data System (ADS)

    Capes, G.; Murphy, J. G.; Reeves, C. E.; McQuaid, J. B.; Hamilton, J. F.; Hopkins, J. R.; Crosier, J.; Williams, P. I.; Coe, H.

    2009-06-01

    This paper presents measurements of organic aerosols above subtropical West Africa during the wet season using data from the UK Facility for Airborne Atmospheric Measurements (FAAM) aircraft. Measurements of biogenic volatile organic compounds (BVOC) at low altitudes over these subtropical forests were made during the African Monsoon Multidisciplinary Analysis (AMMA) field experiment during July and August 2006 mainly above Benin, Nigeria and Niger. Data from an Aerodyne Quadrupole Aerosol Mass Spectrometer show a median organic aerosol loading of 1.07 μg m-3 over tropical West Africa, which represents the first regionally averaged assessment of organic aerosol mass (OM) in this region during the wet season. This is broadly in agreement with global model predictions based on partitioning schemes, although there are large uncertainties associated with such estimates. In contrast our own calculations based on aerosol yields from isoprene and monoterpenes during chamber studies under represent the OM measured in this region on a comparable scale to the under representations of OM by predictive models in the mid latitudes. As global models rely on similar yield calculations in their global estimates, as our calculations this points to further systematic differences between global model estimates and measurements of SOA, most likely caused by use of incorrect BVOC emission rates. The under predictions of OM by our calculations and those in the mid latitudes employ yields extrapolated from chamber data obtained at higher mass concentrations - more recent yield data for α-pinene obtained at ambient concentrations in a flow through chamber (Shilling et al., 2008) show considerably better agreement with our data.

  11. Biogenic secondary organic aerosol over the United States: Comparison of climatological simulations with observations

    NASA Astrophysics Data System (ADS)

    Liao, Hong; Henze, Daven K.; Seinfeld, John H.; Wu, Shiliang; Mickley, Loretta J.

    2007-03-01

    Understanding the effects of global climate change on regional air quality is central in future air quality planning. We report here on the use of the Goddard Institute for Space Studies (GISS) general circulation model (GCM) III to drive the GEOS-CHEM global atmospheric chemical transport model to simulate climatological present-day aerosol levels over the United States. Evaluation of model predictions using surface measurements from the Interagency Monitoring of Protected Visual Environments (IMPROVE) network indicates that the GISS GCM III/GEOS-CHEM model is a suitable tool for simulating aerosols over the United States in the present climate. The model reproduces fairly well the concentrations of sulfate (mean bias of -0.36 μg m-3, normalized mean bias (NMB) of -25.9%), black carbon (-0.004 μg m-3, -1.9%), organic carbon that comprises primary and secondary components (-0.56 μg m-3, -34.2%), and PM2.5 (-0.87 μg m-3, -20.4%). Nitrate concentrations are overpredicted in the western United States (west of 95°W) with a NMB of +75.6% and underestimated in the eastern United States with a NMB of -54.4%. Special attention is paid to biogenic secondary organic aerosol (SOA). The highest predicted seasonal mean SOA concentrations of 1-2 μg m-3 and 0.5-1.5 μg m-3 are predicted over the northwestern and southeastern United States, respectively, in the months of June-July-August. Isoprene is predicted to contribute 49.5% of the biogenic SOA burden over the United States, with the rest explained by the oxidation of terpenes. Predicted biogenic SOA concentrations are in reasonable agreement with inferred SOA levels from IMPROVE measurements. On an annual basis, SOA is predicted to contribute 10-20% of PM2.5 mass in the southeastern United States, as high as 38% in the northwest and about 5-15% in other regions, indicating the important role of SOA in understanding air quality and visibility over the United States.

  12. Secondary Organic Aerosol Formation and Organic Nitrate Yield from NO3 Oxidation of Biogenic Hydrocarbons

    PubMed Central

    2014-01-01

    The secondary organic aerosol (SOA) mass yields from NO3 oxidation of a series of biogenic volatile organic compounds (BVOCs), consisting of five monoterpenes and one sesquiterpene (α-pinene, β-pinene, Δ-3-carene, limonene, sabinene, and β-caryophyllene), were investigated in a series of continuous flow experiments in a 10 m3 indoor Teflon chamber. By making in situ measurements of the nitrate radical and employing a kinetics box model, we generate time-dependent yield curves as a function of reacted BVOC. SOA yields varied dramatically among the different BVOCs, from zero for α-pinene to 38–65% for Δ-3-carene and 86% for β-caryophyllene at mass loading of 10 μg m–3, suggesting that model mechanisms that treat all NO3 + monoterpene reactions equally will lead to errors in predicted SOA depending on each location’s mix of BVOC emissions. In most cases, organonitrate is a dominant component of the aerosol produced, but in the case of α-pinene, little organonitrate and no aerosol is formed. PMID:25229208

  13. Modelling Contribution of Biogenic VOCs to New Particle Formation in the Jülich Plant Atmosphere Chamber

    NASA Astrophysics Data System (ADS)

    Liao, L.; Boy, M.; Mogensen, D.; Mentel, T. F.; Kleist, E.; Kiendler-Scharr, A.; Tillman, R.; Kulmala, M. T.; Dal Maso, M.

    2012-12-01

    Biogenic VOCs are substantially emitted from vegetation to atmosphere. The oxidation of BVOCs by OH, O3, and NO3 in air generating less volatile compounds may lead to the formation and growth of secondary organic aerosol, and thus presents a link to the vegetation, aerosol, and climate interaction system (Kulmala et al, 2004). Studies including field observations, laboratory experiments and modelling have improved our understanding on the connection between BVOCs and new particle formation mechanism in some extent (see e.g. Tunved et al., 2006; Mentel et al., 2009). Nevertheless, the exact formation process still remains uncertain, especially from the perspective of BVOC contributions. The purpose of this work is using the MALTE aerosol dynamics and air chemistry box model to investigate aerosol formation from reactions of direct tree emitted VOCs in the presence of ozone, UV light and artificial solar light in an atmospheric simulation chamber. This model employs up to date air chemical reactions, especially the VOC chemistry, which may potentially allow us to estimate the contribution of BVOCs to secondary aerosol formation, and further to quantify the influence of terpenes to the formation rate of new particles. Experiments were conducted in the plant chamber facility at Forschungszentrum Jülich, Germany (Jülich Plant Aerosol Atmosphere Chamber, JPAC). The detail regarding to the chamber facility has been written elsewhere (Mentel et al., 2009). During the experiments, sulphuric acid was measured by CIMS. VOC mixing ratios were measured by two GC-MS systems and PTR-MS. An Airmodus Particle size magnifier coupled with a TSI CPC and a PH-CPC were used to count the total particle number concentrations with a detection limit close to the expected size of formation of fresh nanoCN. A SMPS measured the particle size distribution. Several other parameters including ozone, CO2, NO, Temperature, RH, and flow rates were also measured. MALTE is a modular model to predict

  14. Estimate of biogenic VOC emissions in Japan and their effects on photochemical formation of ambient ozone and secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Chatani, Satoru; Matsunaga, Sou N.; Nakatsuka, Seiji

    2015-11-01

    A new gridded database has been developed to estimate the amount of isoprene, monoterpene, and sesquiterpene emitted from all the broadleaf and coniferous trees in Japan with the Model of Emissions of Gases and Aerosols from Nature (MEGAN). This database reflects the vegetation specific to Japan more accurately than existing ones. It estimates much lower isoprene emitted from other vegetation than trees, and higher sesquiterpene emissions mainly emitted from Cryptomeria japonica, which is the most abundant plant type in Japan. Changes in biogenic emissions result in the decrease in ambient ozone and increase in organic aerosol simulated by the air quality simulation over the Tokyo Metropolitan Area in Japan. Although newly estimated biogenic emissions contribute to a better model performance on overestimated ozone and underestimated organic aerosol, they are not a single solution to solve problems associated with the air quality simulation.

  15. Seasonal variations and sources of ambient fossil and biogenic-derived carbonaceous aerosols based on 14C measurements in Lhasa, Tibet

    NASA Astrophysics Data System (ADS)

    Huang, Jie; Kang, Shichang; Shen, Chengde; Cong, Zhiyuan; Liu, Kexin; Wang, Wei; Liu, Lichao

    2010-06-01

    A total of 30 samples of total suspended particles were collected at an urban site in Lhasa, Tibet from August 2006 to July 2007 for investigating carbonaceous aerosol features. The fractions of contemporary carbon ( fc) in total carbon (TC) of ambient aerosols are presented using radiocarbon ( 14C) measurements. The value of fc represents the biogenic contribution to TC, as the biosphere releases organic compounds with the present 14C/ 12C level ( fc = 1), whereas 14C has become extinct in anthropogenic emissions of fossil carbon ( fc = 0). The fc values in Lhasa ranging from 0.357 to 0.702, are higher than Beijing and Tokyo, but clearly lower than the rural region of Launceston, which indicates a major biogenic influence in Lhasa. Seasonal variations of fc values corresponded well with variations of pollutants concentrations (e.g. NO 2). Higher fc values appeared in winter indicating carbonaceous aerosol is more dominated by wood burning and incineration of agricultural wastes within this season. The lower fc values in summer and autumn may be caused by increased diesel and petroleum emissions related to tourism in Lhasa. δ13C values ranged from - 26.40‰ to - 25.10‰, with relative higher values in spring and summer, reflecting the increment of fossil carbon emissions.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

    gas to particle partitioning and heterogeneous chemistry are discussed. [1] A. Virtanen et al. (2010): An amorphous solid state of biogenic secondary organic aerosol particles, Nature 467, 824-827. [2] B. Zobrist et al. (2011): Ultra-slow water diffusion in aqueous sucrose glasses, Phys. Chem. Chem. Phys. 13, 3514-3526. [3] D. L. Bones, J. P. Reid, D. M. Lienhard, and U. K. Krieger (2012): Comparing the mechanism of water condensation and evaporation in glassy aerosol, PNAS 109, 11613-11618. [4] O. Peña and U. Pal (2009): Scattering of electromagnetic radiation by a multilayered sphere, Comput. Phys. Commun. 180, 2348-2354.

  17. Standard aerosols for particle velocimeters

    NASA Technical Reports Server (NTRS)

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

    1976-01-01

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

  18. 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.

  19. Submicron Aerosol Particle Losses in Metalized Bags.

    NASA Astrophysics Data System (ADS)

    Lecinski, Alice

    1980-07-01

    Two new types of conducting bags were tested for aerosol particle storage and sampling, a 3M Company Velostat bag and a bag constructed from 3M Type 2100 Static Shielding Film. The half-lives of unipolar, unit-charged 0.025 m, 0.050 m and 0.090 m sized aerosol particles stored in the Velostat bag and the film bag were 130, 190 and 270 min and 40, 70 and 180 min, respectively. These results depend upon the history of bag filling. The values given here apply to bags which had not previously been filled on the day of experimentation. The lifetimes exhibited by the aerosol particles stored in the Velostat bag are the longest found to data.

  20. Phase state and humidity-induced phase transition studies of SOA particles from biogenic and anthropogenic precursors

    NASA Astrophysics Data System (ADS)

    Saukko, E.; Lambe, A. T.; Massoli, P.; Koop, T.; Wright, J. P.; Croasdale, D. R.; Pedernera, D. A.; Onasch, T. B.; Laaksonen, A.; Davidovits, P.; Worsnop, D. R.; Virtanen, A.

    2012-04-01

    There is mounting evidence showing that tropospheric secondary organic aerosol (SOA) may exist in a phase state other than liquid, namely semi-solid or solid amorphous. The solid or semi-solid, high viscosity material may have significantly higher lifetime in an oxidizing atmosphere than low viscosity liquid due to mass transfer limitations in the particle bulk. In this work we report a systematic study of the phase state of SOA particles produced by photo-oxidation of several volatile organic compound (VOC) precursors in a potential aerosol mass (PAM) flow tube reactor. The phase state of the particles was studied by their bounce behaviour upon impaction on a polished steel plate in a low pressure impactor. The SOA oxidation level (O/C) was determined by an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) The phase state for several types of SOA from different surrogate anthropogenic and biogenic precursors, produced at a wide range of oxidation conditions, were studied at a range of relative humidities. We report the solid or semi-solid phase state of SOA produced from cyclic and terpene precursors used in the study up to at least 50 % relative humidity. Furthermore, adding sulfur dioxide into the reaction chamber yielded liquefied particles, while particles formed from oxidation of pure organic precursor were solid or semi-solid. For a long-chain alkane precursor a liquid-like SOA at low oxidation level was produced, but upon increasing the oxidation level, the formed particles became more solid. While the bounce behaviour of the particles had no single explaining factor for all experiments, the precursor molar mass was seen to correlate with more solid phase at higher humidities in cases with cyclic or terpene precursor.

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  2. Black and Brown Carbon in Biogenic Settings with Different Levels of Anthropogenic Influence, and The Effect of Semivolatile Compounds on Aerosol Optical Properties

    NASA Astrophysics Data System (ADS)

    Tasoglou, A.; Ramachandran, S.; Khlystov, A.; Saha, P.; Grieshop, A. P.; Pandis, S. N.

    2015-12-01

    Secondary organic aerosol (SOA) is a major contributor to the global aerosol burden. Black carbon (BC) is a significant climate warming agent, while light-absorbing organic carbon (brown carbon, BrC), also impacts the atmospheric radiative balance. The optical properties of ambient aerosols can be affected by biogenic SOA through the lensing effect (coating of BC cores by semivolatile SOA), and by the potential formation of BrC from biogenic sources influenced by anthropogenic sources. To evaluate these effects, measurements of ambient aerosol optical properties and BC concentrations were made in rural Centreville, AL (a remote site with little anthropogenic influence) in summer 2013 and at Duke Forest in Chapel Hill, NC (a site close to high density vehicular traffic and industrial sources), during summer 2015. Photoacoustic extinctiometers (PAX, 405 nm and 532 nm) measured particulate light absorption and a single particle soot photometer (SP2) measured BC mass at both locations. A seven-wavelength Aethalometer and a three-wavelength nephelometer were also deployed at Duke Forest. A third PAX (870 nm) was deployed at Centreville. For absorption and BC measurements, the sample was cycled between a dry line and a dry/thermally-denuded line. Hourly samples were collected with a steam jet aerosol collector (SJAC) for online (2013) and offline (2015) chemical composition analysis. BC concentrations were generally higher at Duke Forest compared to the rural Centreville site. The Aethalometer readings at Duke Forest show greater absorption at the shorter wavelengths (370 nm and 470 nm) than expected from the absorption at 880 nm coupled with an inverse wavelength dependence, suggesting the presence of brown carbon. This presentation will examine the evidence for brown carbon at the two sites, as well as the effect of non-BC coatings on BC light absorption (the lensing effect.)

  3. Atmospheric aerosols in Amazonia and land use change: from natural biogenic to biomass burning conditions.

    PubMed

    Artaxo, Paulo; Rizzo, Luciana V; Brito, Joel F; Barbosa, Henrique M J; Arana, Andrea; Sena, Elisa T; Cirino, Glauber G; Bastos, Wanderlei; Martin, Scot T; Andreae, Meinrat O

    2013-01-01

    In the wet season, a large portion of the Amazon region constitutes one of the most pristine continental areas, with very low concentrations of atmospheric trace gases and aerosol particles. However, land use change modifies the biosphere-atmosphere interactions in such a way that key processes that maintain the functioning of Amazonia are substantially altered. This study presents a comparison between aerosol properties observed at a preserved forest site in Central Amazonia (TT34 North of Manaus) and at a heavily biomass burning impacted site in south-western Amazonia (PVH, close to Porto Velho). Amazonian aerosols were characterized in detail, including aerosol size distributions, aerosol light absorption and scattering, optical depth and aerosol inorganic and organic composition, among other properties. The central Amazonia site (TT34) showed low aerosol concentrations (PM2.5 of 1.3 +/- 0.7 microg m(-3) and 3.4 +/- 2.0 microg m(-3) in the wet and dry seasons, respectively), with a median particle number concentration of 220 cm(-3) in the wet season and 2200 cm(-3) in the dry season. At the impacted site (PVH), aerosol loadings were one order of magnitude higher (PM2.5 of 10.2 +/- 9.0 microg m(-3) and 33.0 +/- 36.0 microg m(-3) in the wet and dry seasons, respectively). The aerosol number concentration at the impacted site ranged from 680 cm(-3) in the wet season up to 20 000 cm(-3) in the dry season. An aerosol chemical speciation monitor (ACSM) was deployed in 2013 at both sites, and it shows that organic aerosol account to 81% to the non-refractory PM1 aerosol loading at TT34, while biomass burning aerosols at PVH shows a 93% content of organic particles. Three years of filter-based elemental composition measurements shows that sulphate at the impacted site decreases, on average, from 12% of PM2.5 mass during the wet season to 5% in the dry season. This result corroborates the ACSM finding that the biomass burning contributed overwhelmingly to the organic

  4. Photochemical Aging of Organic Aerosol Particles

    NASA Astrophysics Data System (ADS)

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

    2007-05-01

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

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

    SciTech Connect

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

    1999-06-07

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

  6. Holographic interferometry for aerosol particle characterization

    NASA Astrophysics Data System (ADS)

    Berg, Matthew J.; Subedi, Nava R.

    2015-01-01

    Using simulations based on Mie theory, this work shows how double-exposure digital holography can be used to measure the change in size of an expanding, or contracting, spherical particle. Here, a single particle is illuminated by a plane wave twice during its expansion: once when the particle is 27 λ in radius, and again when it is 47 λ. A hologram is formed from each illumination stage from the interference of the scattered and unscattered, i.e., incident, light. The two holograms are then superposed to form a double exposure. By applying the Fresnel-Kirchhoff diffraction theory to the double-exposed hologram, a silhouette-like image of the particle is computationally reconstructed that is superposed with interference fringes. These fringes are a direct result of the change in particle size occurring between the two illumination stages. The study finds that expansion on the scale of ~ 6 λ is readily discerned from the reconstructed particle image. This work could be important for improved characterization of single and multiple aerosol particles in situ. For example, by illuminating an aerosol particle with infrared light, it may be possible to measure photothermally induced particle expansion, thus providing insight into a particle's material properties simultaneous with an image of the particle.

  7. To What Extent Can Biogenic SOA Be Controlled?

    EPA Science Inventory

    Anthropogenic pollution facilitates transformation of naturally emitted volatile organic compounds (VOCs) to the particle phase, enhancing the ambient concentrations of material commonly referred to as biogenic secondary organic aerosol (SOA). It is therefore conceivable that som...

  8. 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. PMID:23216158

  9. SCAVENGING OF AEROSOL PARTICLES BY PRECIPITATION

    EPA Science Inventory

    Airborne measurements have been made of aerosol particle size distributions (>0.01 micrometer) in aged air masses, in the plumes from several coal power plants and a large Kraft paper mill, and in the emissions from a volcano, before and after rain or snow showers. These measurem...

  10. Aerosol particle analysis by Raman scattering technique

    SciTech Connect

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

    1992-10-01

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

  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. Mass Spectral Observations of Submicron Aerosol Particles and Production of Secondary Organic Aerosol at an Anthropogenically Influenced Site during the Wet Season of GoAmazon2014

    NASA Astrophysics Data System (ADS)

    de Sá, S. S.; Palm, B. B.; Campuzano Jost, P.; Day, D. A.; Hu, W.; Newburn, M. K.; Ferreira De Brito, J.; Artaxo, P.; Shilling, J. E.; Souza, R. A. F. D.; Manzi, A. O.; Alexander, M. L.; Jimenez, J. L.; Martin, S. T.

    2014-12-01

    As part of GoAmazon2014, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed to characterize the composition, size, and spectral markers present in submicron atmospheric aerosol particles at a site downwind of Manaus, Brazil, in the central Amazon basin. The focus was on the influence of biogenic-anthropogenic interactions on the measured aerosol particles, especially as related to the formation of secondary organic aerosol (SOA). Through a combination of meteorology, emissions, and chemistry, the research site was affected by biogenic emissions from the tropical rainforest that were periodically mixed with urban outflow from the Manaus metropolitan area. Results from the first intensive operation period, from 1 February to 31 March 2014, show that for the wet season the PM1 mass concentration had typical values on order of 1 to 2 μg/m3. The organic species were dominant, followed by sulfate. The mass-diameter distribution of the particle population had a prevailing mode between 300 and 400 nm (vacuum aerodynamic diameter, dva), and at times a smaller mode at finer size was also present. Highly oxidized organic material was frequently observed, characterized by a dominant peak at m/z 44. There was a diel trend in the elemental oxygen-to-carbon (O:C) ratio peaking in the afternoon. The analysis of the results aims at delineating the anthropogenic impact on the measurements. Multivariate statistical analysis by positive-matrix factorization (PMF) is applied to the time series of organic particle mass spectra. The factors and their loadings provide information on the relative and time-varying contributions of different sources and processes affecting the organic component of the aerosol particle phase. Relationships between AMS results and measurements from co-located instruments that provide information on anthropogenic and biogenic gas and particle tracers are investigated, toward the goal of improving the understanding of

  14. Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX

    NASA Astrophysics Data System (ADS)

    Brown, S. S.; Dubé, W. P.; Bahreini, R.; Middlebrook, A. M.; Brock, C. A.; Warneke, C.; de Gouw, J. A.; Washenfelder, R. A.; Atlas, E.; Peischl, J.; Ryerson, T. B.; Holloway, J. S.; Schwarz, J. P.; Spackman, R.; Trainer, M.; Parrish, D. D.; Fehshenfeld, F. C.; Ravishankara, A. R.

    2013-11-01

    Organic compounds are a large component of aerosol mass, but organic aerosol (OA) sources remain poorly characterized. Recent model studies have suggested nighttime oxidation of biogenic hydrocarbons as a potentially large OA source, but analysis of field measurements to test these predictions is sparse. We present nighttime vertical profiles of nitrogen oxides, ozone, VOCs and aerosol composition measured during low approaches of the NOAA P-3 aircraft to airfields in Houston, TX. This region has large emissions of both biogenic hydrocarbons and nitrogen oxides. The latter category serves as a source of the nitrate radical, NO3, a key nighttime oxidant. Biogenic VOCs (BVOC) and urban pollutants were concentrated within the nocturnal boundary layer (NBL), which varied in depth from 100-400 m. Despite concentrated NOx at low altitude, ozone was never titrated to zero, resulting in rapid NO3 radical production rates of 0.2-2.7 ppbv h-1 within the NBL. Monoterpenes and isoprene were frequently present within the NBL and underwent rapid oxidation (up to 1 ppbv h-1), mainly by NO3 and to a lesser extent O3. Concurrent enhancement in organic and nitrate aerosol on several profiles was consistent with primary emissions and with secondary production from nighttime BVOC oxidation, with the latter equivalent to or slightly larger than the former. Some profiles may have been influenced by biomass burning sources as well, making quantitative attribution of organic aerosol sources difficult. Ratios of organic aerosol to CO within the NBL ranged from 14 to 38 μg m-3 OA/ppmv CO. A box model simulation incorporating monoterpene emissions, oxidant formation rates and monoterpene SOA yields suggested overnight OA production of 0.5 to 9 μg m-3.

  15. Characterization of Halyomorpha halys (brown marmorated stink bug) biogenic volatile organic compound emissions and their role in secondary organic aerosol formation.

    PubMed

    Solomon, Danielle; Dutcher, Dabrina; Raymond, Timothy

    2013-11-01

    The formation of aerosols is a key component in understanding cloud formation in the context of radiative forcings and global climate modeling. Biogenic volatile organic compounds (BVOCs) are a significant source of aerosols, yet there is still much to be learned about their structures, sources, and interactions. The aims of this project were to identify the BVOCs found in the defense chemicals of the brown marmorated stink bug Halymorpha halys and quantify them using gas chromatography-mass spectrometry (GC/MS) and test whether oxidation of these compounds by ozone-promoted aerosol and cloud seed formation. The bugs were tested under two conditions: agitation by asphyxiation and direct glandular exposure. Tridecane, 2(5H)-furanone 5-ethyl, and (E)-2-decenal were identified as the three most abundant compounds. H. halys were also tested in the agitated condition in a smog chamber. It was found that in the presence of 100-180 ppm ozone, secondary aerosols do form. A scanning mobility particle sizer (SMPS) and a cloud condensation nuclei counter (CCNC) were used to characterize the secondary aerosols that formed. This reaction resulted in 0.23 microg/ bug of particulate mass. It was also found that these secondary organic aerosol particles could act as cloud condensation nuclei. At a supersaturation of 1%, we found a kappa value of 0.09. Once regional populations of these stink bugs stablilize and the populations estimates can be made, the additional impacts of their contribution to regional air quality can be calculated. PMID:24344570

  16. Absence of Biogenic New Particle Formation in the Southern U.S. during the 2013 SOAS Field Campaign

    NASA Astrophysics Data System (ADS)

    Uin, J.; You, Y.; Sierra-Hernández, M.; Guenther, A. B.; Brune, W. H.; Misztal, P. K.; Baumann, K.; Isaacman, G. A.; Goldstein, A. H.; Edgerton, E.; Lee, S.

    2013-12-01

    One of the main goals of the Southern Oxidant and Aerosol Study (SOAS) field campaign was to investigate the SOA formation mechanisms in the biogenic environment under anthropogenic influences. The SOAS campaign took place in a mixed deciduous forest near Centerville, Alabama between June 1 and July 15, 2013. To study the biogenic new particle formation (NPF) mechanism, Kent State University deployed two chemical ionization mass spectrometers (CIMS) to measure concentrations of gas phase sulfuric acid, amines and ammonia; additionally, two TSI SMPSs and an Airmodus particle size magnifier (PSM) were used to together measure the ambient aerosol size distributions in the range from 1-800 nm. Data were continuously collected during the 6 weeks of the campaign period, but only two clear particle growth events were observed. During both events, concentrations of sulfuric acid were high. When there were no NPF events, sulfuric acid concentrations were sometimes high (even during the night) and there were also sufficient amounts of ammonia and amines in the gas phase. These key nucleation precursors together with low condensation sinks should have provided a reasonable condition for NPF. The PTR-TOFMS (by NCAR and UC-Berkley) measurements showed that the ratio of isoprene to monoterpene carbon concentrations was consistently higher than 1 during the campaign period. The laser induced fluorescence (LIF by Penn State) measured-OH concentrations were at the high e5 and low e6 molecules per cubic centimeter range, which should have been sufficient for BVOCs oxidation to lead to NPF. These results are consistent with a previous study in the Michigan forest [Kanawade et al., 2011: Isoprene suppression of new particle formation in a mixed deciduous forest, ACP, 11, 6013], which showed that biogenic NPF was suppressed by high emissions of isoprene without OH depletion. But the chemical mechanisms behind the absence of NPF in mixed forests need to be further investigated. The PSM

  17. 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

  18. Determination of the biogenic secondary organic aerosol fraction in the boreal forest by AMS and NMR measurements

    NASA Astrophysics Data System (ADS)

    Finessi, E.; Decesari, S.; Paglione, M.; Giulianelli, L.; Carbone, C.; Gilardoni, S.; Fuzzi, S.; Saarikoski, S.; Raatikainen, T.; Hillamo, R.; Allan, J.; Mentel, Th. F.; Tiitta, P.; Laaksonen, A.; Petäjä, T.; Kulmala, M.; Worsnop, D. R.; Facchini, M. C.

    2011-08-01

    The study investigates the sources of fine organic aerosol (OA) in the boreal forest, based on measurements including both filter sampling (PM1) and online methods and carried out during a one-month campaign held in Hyytiälä, Finland, in spring 2007. Two aerosol mass spectrometers (Q-AMS, ToF-AMS) were employed to measure on-line air mass concentrations of major non-refractory aerosol species, while the water extracts of the filter samples were analyzed by nuclear magnetic resonance (NMR) spectroscopy for organic functional group characterization of the polar organic fraction of the aerosol. AMS and NMR spectra were processed separately by non-negative factorization algorithms, in order to apportion the main components underlying the submicrometer organic aerosol composition and depict them in terms of both mass fragmentation patterns and functional group compositions. The NMR results supported the AMS speciation of oxidized organic aerosol (OOA) into two main fractions, which could be generally labelled as more and less oxidized organics. The more oxidized component was characterized by a mass spectrum dominated by the m/z 44 peak, and in parallel by a NMR spectrum showing aromatic and aliphatic backbones highly substituted with oxygenated functional groups (carbonyls/carboxyls and hydroxyls). Such component, contributing on average 50 % of the OA mass throughout the observing period, was associated with pollution outbreaks from the Central Europe. The less oxidized component showed features consistent with less oxygenated aerosols and was enhanced in concomitance with air masses originating from the North-to-West sector, in agreement with previous investigations conducted at this site. NMR factor analysis was able to separate two distinct components under the less oxidized fraction of OA. One of these NMR-factors was associated to the formation of terrestrial biogenic secondary organic aerosol (BSOA), based on the comparison with spectral profiles obtained from

  19. Nature and evolution of ultrafine aerosol particles in the atmosphere

    NASA Astrophysics Data System (ADS)

    Smirnov, V. V.

    2006-12-01

    Results of experimental and theoretical studies of a poorly understood phenomenon, an intense emission of ultrafine (nanometer) aerosols (ENA), are reviewed. In the English-language literature, this phenomenon is commonly referred to as a nucleation burst. ENA events have been observed on all the continents and throughout the depth of the troposphere, with the number of corresponding publications growing steadily. Intense and long-lasting ENA events have been studied more or less comprehensively and in full detail for Northern Europe, with 60 to 70% of observations taken in a forest area in the presence of snow cover and 10 to 20% in coastal marine areas. Most often, ENA events occur during spring and fall, with 95% of cases in the daytime and under sunny calm conditions, typical of anticyclones. In ENA events, the concentration of nanoparticles initially grows rapidly to values of 103-105 cm-3. One or two hours later, the so-called nuclei fraction with diameters D = 3-15 nm is produced. The appearance of the Aitken fraction D = 20-80 nm and the enlargement of aerosol particles inside the accumulation fraction D = 80-200 nm may occur during the following 4-6 h. Thus, the cycle of formation and growth of atmospheric aerosol particles in the size range from a few to hundreds of nanometers is reproduced over 6-8 h. A specific synoptic feature of ENA events over land is that they occur when the polar air is transported to measuring sites and the temperature difference between day and light is large. During ENA periods, the formation rate of condensation nuclei with a diameter of 100 nm increases 10-to 100-fold. Important factors of ENA genesis are the “aerosol” and “electric” states of the atmosphere. More intense ENA events occur at low concentrations of background aerosols in the presence of atmospheric ions of medium mobility with D = 2-3 nm. The international experiments ACE 1 and 2, BIOFOR 1, 2, and 3, ESUP 2000, QUEST, etc., have not yet provided any

  20. Secondary organic aerosol origin in an urban environment: influence of biogenic and fuel combustion precursors.

    PubMed

    Minguillón, M C; Pérez, N; Marchand, N; Bertrand, A; Temime-Roussel, B; Agrios, K; Szidat, S; van Drooge, B; Sylvestre, A; Alastuey, A; Reche, C; Ripoll, A; Marco, E; Grimalt, J O; Querol, X

    2016-07-18

    Source contributions of organic aerosol (OA) are still not fully understood, especially in terms of quantitative distinction between secondary OA formed from anthropogenic precursors vs. that formed from natural precursors. In order to investigate the OA origin, a field campaign was carried out in Barcelona in summer 2013, including two periods characterized by low and high traffic conditions. Volatile organic compound (VOC) concentrations were higher during the second period, especially aromatic hydrocarbons related to traffic emissions, which showed a marked daily cycle peaking during traffic rush hours, similarly to black carbon (BC) concentrations. Biogenic VOC (BVOC) concentrations showed only minor changes from the low to the high traffic period, and their intra-day variability was related to temperature and solar radiation cycles, although a decrease was observed for monoterpenes during the day. The organic carbon (OC) concentrations increased from the first to the second period, and the fraction of non-fossil OC as determined by (14)C analysis increased from 43% to 54% of the total OC. The combination of (14)C analysis and Aerosol Chemical Speciation Monitor (ACSM) OA source apportionment showed that the fossil OC was mainly secondary (>70%) except for the last sample, when the fossil secondary OC only represented 51% of the total fossil OC. The fraction of non-fossil secondary OC increased from 37% of total secondary OC for the first sample to 60% for the last sample. This enhanced formation of non-fossil secondary OA (SOA) could be attributed to the reaction of BVOC precursors with NOx emitted from road traffic (or from its nocturnal derivative nitrate that enhances night-time semi-volatile oxygenated OA (SV-OOA)), since NO2 concentrations increased from 19 to 42 μg m(-3) from the first to the last sample. PMID:27119273

  1. Marine biogenic aerosol sources simulated from below the global ocean-atmosphere interface

    NASA Astrophysics Data System (ADS)

    Elliott, S.; Burrows, S. M.; Cameron-Smith, P. J.; Deal, C.; Maltrud, M. E.; Ogunro, O. O.; Russell, L. M.; Wang, S.; Wingenter, O. W.

    2015-12-01

    Full understanding of biogenic aerosol emissions may require modeling of production, interconversion, phase changes and other processes influencing precursor distributions below the ocean surface. We describe a bottom-up, chemical oceanographic approach to the representation of marine sources now under development for Earth System Models in the U.S. Department of Energy. The motivation is to move beyond indirect bulk indicators such as chlorophyll or total dissolved organics. Dynamic mechanistic capabilities are sought for the relevant mixed layer materials and flux fields. The resulting fidelity and predictive capabilities may prove crucial during the era of global change. Reactive transport calculations are outlined for organosulfur, the suite of biomacromolecules, their degradation products plus both interphase or interfacial transitions. Volatile and polymeric substances are controlled on a compound by compound basis, driven by results from a global ecodynamics model of multiple phytotaxa and trophic levels. Surfactant behavior is considered simultaneously at the global bubble and atmospheric interfaces, and such two dimensional chemistry is extended beyond Langmuir monolayers to electrostatically supported films. Colloidal and gel sweeping-impaction by the wind-driven bubble field are considered as alternate means of vertical transport. At the top of the ocean within the microlayer, effects on sea spray number flux are estimated. Moving beyond aerosol emissions, our methods can also provide insight into the uncertainties traditionally inherent to sea-air gas transfer, since they are connected to macromolecular viscoelastics in the laminar barrier layer. We find that resolution of all these subsurface processes is possible at the level of the biogeographic marine province, including specialized treatments for the ice domain, sea ice edge and coastal regime.

  2. Biogenic VOC oxidation and organic aerosol formation in an urban nocturnal boundary layer: aircraft vertical profiles in Houston, TX

    NASA Astrophysics Data System (ADS)

    Brown, S. S.; Dubé, W. P.; Bahreini, R.; Middlebrook, A. M.; Brock, C. A.; Warneke, C.; de Gouw, J. A.; Washenfelder, R. A.; Atlas, E.; Peischl, J.; Ryerson, T. B.; Holloway, J. S.; Schwarz, J. P.; Spackman, R.; Trainer, M.; Parrish, D. D.; Fehshenfeld, F. C.; Ravishankara, A. R.

    2013-05-01

    Organic compounds are a large component of aerosol mass, but organic aerosol (OA) sources remain poorly characterized. Recent model studies have suggested nighttime oxidation of biogenic hydrocarbons as a potentially large OA source, but analysis of field measurements to test these predictions is sparse. We present nighttime vertical profiles of nitrogen oxides, ozone, VOCs and aerosol composition measured during low approaches of the NOAA P-3 aircraft to airfields in Houston, TX. This region has large emissions of both biogenic hydrocarbons and nitrogen oxides. The latter serves as a source of the nitrate radical, NO3, a key nighttime oxidant. Biogenic VOCs (BVOC) and urban pollutants were concentrated within the nocturnal boundary layer (NBL), which varied in depth from 100-400 m. Despite concentrated NOx at low altitude, ozone was never titrated to zero, resulting in rapid NO3 radical production rates of 0.2-2.7ppbv h-1 within the NBL. Monoterpenes and isoprene were frequently present within the NBL and underwent rapid oxidation (up to 1ppbv h-1), mainly by NO3 and to a lesser extent O3. Concurrent enhancement in organic and nitrate aerosol on several profiles was consistent with primary emissions and with secondary production from nighttime BVOC oxidation, with the latter equivalent to or slightly larger than the former. Ratios of organic aerosol to CO within the NBL ranged from 14 to 38 μg m-3 OA/ppmv CO. A box model simulation incorporating monoterpene emissions, oxidant formation rates and monoterpene SOA yields suggested overnight OA production of 0.5 to 9 μg m-3.

  3. Characterization of fine primary biogenic organic aerosol in an urban area in the northeastern United States

    NASA Astrophysics Data System (ADS)

    Coz, Esther; Artíñano, Begoña; Clark, Lisa M.; Hernandez, Mark; Robinson, Allen L.; Casuccio, Gary S.; Lersch, Traci L.; Pandis, Spyros N.

    2010-10-01

    Scanning electron microscopy coupled to energy-dispersive x-ray spectroscopy (SEM/EDX) was used to quantify individual bioparticles in PM 2.5 samples collected during the Pittsburgh Air Quality Study. Microscopy-based estimates of primary biogenic organic aerosol (PBOA) mass were compared to carbohydrate mass associated with PM 2.5. Carbohydrates show substantial seasonal variations, with higher concentrations in the spring and the fall. During the summer, carbohydrates were about 30% of the estimated PBOA concentrations, but in the winter carbohydrate concentrations often greatly exceeded the PBOA mass estimate. Spores and insect detritus were the most abundant PBOA types in the summer samples, while winter samples were comprised predominantly of a mixture of microorganisms, insect and vegetative detritus. During the summer PBOA contributed on average 6.9 ± 5.4% by mass of the PM 2.5 versus 3.3 ± 1.4% of the PM 2.5 mass during the winter.

  4. 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

  5. Contribution from biogenic organic compounds to particle growth during the 2010 BEACHON-ROCS campaign in a Colorado temperate needleleaf forest

    DOE PAGESBeta

    Zhou, L.; Gierens, R.; Sogachev, A.; Mogensen, D.; Ortega, J.; Smith, J. N.; Harley, P. C.; Prenni, A. J.; Levin, E. J. T.; Turnipseed, A.; et al

    2015-08-06

    New particle formation (NPF) is an important atmospheric phenomenon. During an NPF event, particles first form by nucleation and then grow further in size. The growth step is crucial because it controls the number of particles that can become cloud condensation nuclei. Among various physical and chemical processes contributing to particle growth, condensation by organic vapors has been suggested as important. In order to better understand the influence of biogenic emissions on particle growth, we carried out modeling studies of NPF events during the BEACHON-ROCS (Bio–hydro–atmosphere interactions of Energy, Aerosol, Carbon, H2O, Organics & Nitrogen – Rocky Mountain Organic Carbonmore » Study) campaign at Manitou Experimental Forest Observatory in Colorado, USA. The site is representative of the semi-arid western USA. With the latest Criegee intermediate reaction rates implemented in the chemistry scheme, the model underestimates sulfuric acid concentration by 50 %, suggesting either missing sources of atmospheric sulfuric acid or an overestimated sink term. The results emphasize the contribution from biogenic volatile organic compound emissions to particle growth by demonstrating the effects of the oxidation products of monoterpenes and 2-Methyl-3-buten-2-ol (MBO). Monoterpene oxidation products are shown to influence the nighttime particle loadings significantly, while their concentrations are insufficient to grow the particles during the day. The growth of ultrafine particles in the daytime appears to be closely related to the OH oxidation products of MBO.« less

  6. Contribution from biogenic organic compounds to particle growth during the 2010 BEACHON-ROCS campaign in a Colorado temperate needleleaf forest

    SciTech Connect

    Zhou, L.; Gierens, R.; Sogachev, A.; Mogensen, D.; Ortega, J.; Smith, J. N.; Harley, P. C.; Prenni, A. J.; Levin, E. J. T.; Turnipseed, A.; Rusanen, A.; Smolander, S.; Guenther, A. B.; Kulmala, M.; Karl, T.; Boy, M.

    2015-08-06

    New particle formation (NPF) is an important atmospheric phenomenon. During an NPF event, particles first form by nucleation and then grow further in size. The growth step is crucial because it controls the number of particles that can become cloud condensation nuclei. Among various physical and chemical processes contributing to particle growth, condensation by organic vapors has been suggested as important. In order to better understand the influence of biogenic emissions on particle growth, we carried out modeling studies of NPF events during the BEACHON-ROCS (Bio–hydro–atmosphere interactions of Energy, Aerosol, Carbon, H2O, Organics & Nitrogen – Rocky Mountain Organic Carbon Study) campaign at Manitou Experimental Forest Observatory in Colorado, USA. The site is representative of the semi-arid western USA. With the latest Criegee intermediate reaction rates implemented in the chemistry scheme, the model underestimates sulfuric acid concentration by 50 %, suggesting either missing sources of atmospheric sulfuric acid or an overestimated sink term. The results emphasize the contribution from biogenic volatile organic compound emissions to particle growth by demonstrating the effects of the oxidation products of monoterpenes and 2-Methyl-3-buten-2-ol (MBO). Monoterpene oxidation products are shown to influence the nighttime particle loadings significantly, while their concentrations are insufficient to grow the particles during the day. The growth of ultrafine particles in the daytime appears to be closely related to the OH oxidation products of MBO.

  7. 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.

  8. Condensation on Aerosol Particles and its Inhibition.

    NASA Astrophysics Data System (ADS)

    Liu, Peter Shen King

    The atmospheric aerosol is of primary importance in the formation of precipitation. Except in the neighbourhood of large sources of pollution most of the atmospheric particles are of natural origin, but human contribution is increasing at such a rate that within a comparatively short time it may equal nature's. Such an increase in the atmospheric particulate load may have significant effects on the distribution and intensity of precipitation. There is a general perception that most of the atmospheric particulate load is soluble in water or has some soluble component and soluble particles condense water more readily than insoluble. In this work a study is made of the solubility of the atmospheric aerosol at various relative humidities. The results confirm that much of the atmospheric aerosol is indeed soluble, but that the soluble proportion is highly variable. This result has significant implications for studies of air pollution in which the respirable fraction of the atmospheric aerosol is deduced from the results of long term dichotomous sampling. Results are also presented of studies in which an attempt was made to inhibit the condensation of water on man-made and adventitious particles with a view to modifying their possible climatic effects. This work has demonstrated that certain agents, notably long chain amines, do indeed have an inhibiting effect on the condensation of water on particles which have been exposed to them, but that the effect of the agents so far tested is not sufficiently great to be of immediate practical importance. It is concluded that further advances must await more precise methods of producing small supersaturations reliably and reproducibly.

  9. Impact of regional transport on the anthropogenic and biogenic secondary organic aerosols in the Los Angeles Basin

    NASA Astrophysics Data System (ADS)

    Heo, Jongbae; de Foy, Benjamin; Olson, Michael R.; Pakbin, Payam; Sioutas, Constantinos; Schauer, James J.

    2015-02-01

    This manuscript explores the role of regional transport on anthropogenic and biogenic secondary organic carbon (SOC) concentrations in ambient fine particulate (PM2.5) organic carbon (OC) in the Los Angeles (LA) Basin. Daily organic molecular markers, water soluble organic carbon (WSOC), OC, and elemental carbon (EC) measurements from May 2009 through April 2010 at a central site in downtown LA, and results from a positive matrix factorization (PMF) analysis of these data, were used to understand the role of regional transport on SOC concentrations. A backward-trajectory analysis, coupled with the measurements and estimated source contributions, were used to evaluate the origins of SOC aerosols. Anthropogenic and biogenic SOC were identified in central LA over the study period, together contributing 40% of the annual average PM2.5 OC mass. There were distinct seasonal variations, with high contributions of anthropogenic SOC in summer, and high contributions of biogenic SOC in spring. The back-trajectory analysis, coupled with daily source contributions of SOC and organic compounds as indicators, allowed us to identify potential source locations and dominant meteorological conditions contributing to elevated SOC at the measurement site. The results show that air mass movements from the Pacific Ocean are associated with higher contributions of anthropogenic SOC to the PM2.5 OC in downtown LA, suggesting that the combination of local meteorological conditions and local anthropogenic emissions led to an increase in the anthropogenic SOC. In contrast, air masses passing over the Central Valley and forested areas where there are biogenic hydrocarbon emissions are closely associated with higher contributions of biogenic SOC in the region. The study emphasizes that higher anthropogenic SOC contributions are due to the combination of local emissions with humidity air from the ocean, and that higher biogenic SOC contributions are impacted by transport of pollutants from

  10. Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

    NASA Astrophysics Data System (ADS)

    Mochizuki, T.; Miyazaki, Y.; Ono, K.; Wada, R.; Takahashi, Y.; Saigusa, N.; Kawamura, K.; Tani, A.

    2015-04-01

    We conducted simultaneous measurements of concentrations and above-canopy fluxes of isoprene and α-pinene, along with their oxidation products in aerosols in a Larix kaempferi (Japanese larch) forest in summer 2012. Vertical profiles of isoprene showed the maximum concentration near the forest floor with a peak around noon, whereas oxidation products of isoprene, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higher concentrations near the canopy level of the forest. The vertical profile suggests large emissions of isoprene near the forest floor, likely due to Dryopteris crassirhizoma (a fern species), and the subsequent reaction within the canopy. The concentrations of α-pinene also showed highest values near the forest floor with maximums in the early morning and late afternoon. The vertical profiles of α-pinene suggest its large emissions from soil and litter in addition to emissions from L. kaempferi leaves at the forest site. Isoprene and its oxidation products in aerosols exhibited similar diurnal variations within the forest canopy, providing evidence for secondary organic aerosol (SOA) formation via oxidation of isoprene most likely emitted from the forest floor. Although high abundance of α-pinene was observed in the morning, its oxidation products in aerosols showed peaks in daytime, due to a time lag between the emission and atmospheric reactions of α-pinene to form SOA. Positive matrix factorization (PMF) analysis indicated that anthropogenic influence is the most important factor contributing to the elevated concentrations of molecular oxidation products of isoprene- (> 64%) and α-pinene-derived SOA (> 57%). The combination of the measured fluxes and vertical profiles of biogenic volatile organic compounds (BVOCs) suggests that the inflow of anthropogenic precursors/aerosols likely enhanced the formation of both isoprene- and α-pinene-SOA within the forest canopy even when the BVOC flux was relatively low. This study highlights

  11. 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.

  12. Understanding the anthropogenic influence on formation of biogenic secondary organic aerosols in Denmark via analysis of organosulfates and related oxidation products

    NASA Astrophysics Data System (ADS)

    Nguyen, Q. T.; Christensen, M. K.; Cozzi, F.; Zare, A.; Hansen, A. M. K.; Kristensen, K.; Tulinius, T. E.; Madsen, H. H.; Christensen, J. H.; Brandt, J.; Massling, A.; Nøjgaard, J. K.; Glasius, M.

    2014-09-01

    Anthropogenic emissions of sulfur dioxide (SO2) and nitrogen oxides (NOx) may affect concentration levels and composition of biogenic secondary organic aerosols (BSOA) through photochemical reactions with biogenic organic precursors to form organosulfates and nitrooxy organosulfates. We investigated this influence in a field study from 19 May to 22 June, 2011 at two sampling sites in Denmark. Within the study, we identified a substantial number of organic acids, organosulfates and nitrooxy organosulfates in the ambient urban curbside and semi-rural background air. A high degree of correlation in concentrations was found among a group of specific organic acids, organosulfates and nitrooxy organosulfates, which may originate from various precursors, suggesting a common mechanism or factor affecting their concentration levels at the sites. It was proposed that the formation of those species most likely occurred on a larger spatial scale, with the compounds being long-range transported to the sites on the days with the highest concentrations. The origin of the long-range transported aerosols was investigated using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model in addition to modeled emissions of related precursors, including isoprene and monoterpenes using the global Model of Emissions of Gases and Aerosols from Nature (MEGAN) and SO2 emissions using the European Monitoring and Evaluation Program (EMEP) database. The local impacts were also studied by examining the correlation between selected species, which showed significantly enhanced concentrations at the urban curbside site and the local concentrations of various gases, including SO2, ozone (O3), NOx, aerosol acidity and other meteorological conditions. This investigation showed that an inter-play of the local parameters such as the aerosol acidity, NOx, SO2, relative humidity (RH), temperature and global radiation seemed to affect the concentration level of those species, suggesting

  13. Crystallization by Particle Attachment in Synthetic, Biogenic, and Geologic Environments

    SciTech Connect

    De Yoreo, James J.; Gilbert, Pupa U.; Sommerdijk, Nico; Penn, R. Lee; Whitelam, Stephen B.; Joester, Derk; Zhang, Hengzhong; Rimer, Jeffrey D.; Navrotsky, Alexandra; Banfield, Jillian F.; Wallace, Adam F.; Michel, F. M.; Meldrum, Fiona C.; Colfen, Helmut; Dove, Patricia M.

    2015-07-31

    Field and laboratory observations show that crystals commonly form by the addition and attachment of particles that range from multi-ion complexes to fully formed nanoparticles. These non-classical pathways to crystallization are diverse, in contrast to classical models that consider the addition of monomeric chemical species. We review progress toward understanding crystal growth by particle attachment processes and show that multiple pathways result from the interplay of free energy landscapes and reaction dynamics. Much remains unknown about the fundamental aspects; particularly the relationships between solution structure, interfacial forces, and particle motion. Developing a predictive description that connects molecular details to ensemble behavior will require revisiting long-standing interpretations of crystal formation in synthetic systems and patterns of mineralization in natural environments.

  14. Characterization of biogenic elements in interplanetary dust particles

    NASA Technical Reports Server (NTRS)

    Bunch, T. E.

    1986-01-01

    Those particles that were designated cometary are aggregates of amorphous materials including carbon, iron-magnesium silicates, sulfides, metal and trace amounts of unusual phases. Most aggregates are carbon-rich with major and minor element abundances similar to a fine grained matrix of carbonaceous chondrites. Several particles were analyzed by a laser microprobe. The negative ionic species identified to date include carbon clusters, protonated carbon clusters, CN-, HCN-, CNO-, PO2-, PO3-, S-, S2- asnd OH-. These species are similar to those observed in cometary spectra and they support the assumption that organic materials are present. The occurance of phosphate ions suggests the presence of apatite or whitlockite. Cometary particle characteristics may indicate that the component grains represent primitive unaltered dust whose overall properties are extremely similar to altered primitive dust in carbonaceous chondrites.

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

    PubMed

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

    2015-06-24

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

  16. Simulated Transport and Mixing of Anthropogenic and Biogenic Aerosol and Their Entrainment into Clouds during the Goamazon Campaign

    NASA Astrophysics Data System (ADS)

    Fast, J. D.; Shrivastava, M. B.; Fan, J.; Berg, L. K.; Chand, D.; Fortner, E.; Mei, F.; Pekour, M. S.; Shilling, J. E.; Springston, S. R.; Tomlinson, J. M.; Wang, J.

    2014-12-01

    Several recent studies have suggested that anthropogenic emissions enhance the production of biogenic secondary organic aerosol (SOA). Because Manaus, Brazil is an isolated large city within the Amazon rainforest, measurements collected within and outside of the downwind urban plume during the 2014 Green Ocean Amazon (GoAmazon) campaign (supported by the U.S. Department of Energy's Atmospheric Radiation and Measurement program) will provide valuable information needed by regional and global models to evaluate parameterizations of SOA. The isolated urban plume should also provide distinct patterns of mixing with biogenic emissions and eliminate complications of multiple anthropogenic sources found in most other regions of the world. The objective of this study is to evaluate the performance of preliminary simulations of the transport, mixing, and chemical evolution of the Manaus urban plume from the chemistry version of the Weather Research and Forecasting model (WRF-Chem) using the available surface and aircraft measurements collected during the first intensive observation period (IOP) of GoAmazon. Simulations are performed using both a 10 km or 2 km grid spacing as well as a newly developed treatment that couples a sectional aerosol model and its parameterization of SOA using a volatility basis set approach with resolved clouds and a sub-grid scale cloud parameterization. Since the first IOP of GoAmazon was conducted during the wet season, shallow and deep convection were observed on most days and likely impacts the transport and vertical mixing of the Manaus plume. Therefore, we are using the available field campaign cloud measurements to evaluate the impact of sub-grid scale clouds on the horizontal and vertical distribution of aerosols. Satellite data is also used to assess the regional variability in simulated clouds and precipitation. Analyses of the simulations during the first IOP will be presented. Simulations with and without anthropogenic emissions will

  17. Cloud condensation nuclei activity, droplet growth kinetics, and hygroscopicity of biogenic and anthropogenic secondary organic aerosol (SOA)

    NASA Astrophysics Data System (ADS)

    Zhao, D. F.; Buchholz, A.; Kortner, B.; Schlag, P.; Rubach, F.; Fuchs, H.; Kiendler-Scharr, A.; Tillmann, R.; Wahner, A.; Watne, Å. K.; Hallquist, M.; Flores, J. M.; Rudich, Y.; Kristensen, K.; Hansen, A. M. K.; Glasius, M.; Kourtchev, I.; Kalberer, M.; Mentel, Th. F.

    2016-02-01

    Interaction of biogenic volatile organic compounds (VOCs) with Anthropogenic VOC (AVOC) affects the physicochemical properties of secondary organic aerosol (SOA). We investigated cloud droplet activation (CCN activity), droplet growth kinetics, and hygroscopicity of mixed anthropogenic and biogenic SOA (ABSOA) compared to pure biogenic SOA (BSOA) and pure anthropogenic SOA (ASOA). Selected monoterpenes and aromatics were used as representative precursors of BSOA and ASOA, respectively.

    We found that BSOA, ASOA, and ABSOA had similar CCN activity despite the higher oxygen to carbon ratio (O/C) of ASOA compared to BSOA and ABSOA. For individual reaction systems, CCN activity increased with the degree of oxidation. Yet, when considering all different types of SOA together, the hygroscopicity parameter, κCCN, did not correlate with O/C. Droplet growth kinetics of BSOA, ASOA, and ABSOA were comparable to that of (NH4)2SO4, which indicates that there was no delay in the water uptake for these SOA in supersaturated conditions.

    In contrast to CCN activity, the hygroscopicity parameter from a hygroscopic tandem differential mobility analyzer (HTDMA) measurement, κHTDMA, of ASOA was distinctively higher (0.09-0.10) than that of BSOA (0.03-0.06), which was attributed to the higher degree of oxidation of ASOA. The ASOA components in mixed ABSOA enhanced aerosol hygroscopicity. Changing the ASOA fraction by adding biogenic VOC (BVOC) to ASOA or vice versa (AVOC to BSOA) changed the hygroscopicity of aerosol, in line with the change in the degree of oxidation of aerosol. However, the hygroscopicity of ABSOA cannot be described by a simple linear combination of pure BSOA and ASOA systems. This indicates that additional processes, possibly oligomerization, affected the hygroscopicity.

    Closure analysis of CCN and HTDMA data showed κHTDMA was lower than κCCN by 30-70 %. Better closure was achieved for ASOA compared to BSOA. This

  18. Evidence for the presence of biogenic magnetic particles in the nocturnal migratory brown planthopper, Nilaparvata lugens

    PubMed Central

    Pan, Weidong; Wan, Guijun; Xu, Jingjing; Li, Xiaoming; Liu, Yuxin; Qi, Liping; Chen, Fajun

    2016-01-01

    Biogenic magnetic particles have been detected in some migratory insects, which implies the basis of magnetoreception mechanism for orientation and navigation. Here, the biogenic magnetic particles in the migratory brown planthopper (BPH), Nilaparvata lugens were qualitatively measured by SQUID magnetometry, and their characteristics were further determined by Prussian Blue staining, electron microscopy and energy dispersive x-ray spectroscopy. The results indicate that there were remarkable magnetic materials in the abdomens and not in the head or thorax of the 3rd–5th instar nymphs, and in macropterous and brachypterous female and male adults of BPH. The size of magnetic particles was shown to be between 50–450 nm with a shape factor estimate of between 0.8–1.0 for all the tested BPHs. Moreover, the amount of magnetic particles was associated with the developmental stage (the 3rd–5th instar), wing form (macropterous vs. brachypterous) and sex. The macropterous female adults had the largest amount of magnetic particles. Although the existence of magnetic particles in the abdomens of BPH provides sound basis for the assumption of magnetic orientation, further behavioral studies and complementary physical characterization experiments should be conducted to determine whether the orientation behavior of BPH is associated with the magnetic particles detected in this study. PMID:26727944

  19. Evidence for the presence of biogenic magnetic particles in the nocturnal migratory brown planthopper, Nilaparvata lugens.

    PubMed

    Pan, Weidong; Wan, Guijun; Xu, Jingjing; Li, Xiaoming; Liu, Yuxin; Qi, Liping; Chen, Fajun

    2016-01-01

    Biogenic magnetic particles have been detected in some migratory insects, which implies the basis of magnetoreception mechanism for orientation and navigation. Here, the biogenic magnetic particles in the migratory brown planthopper (BPH), Nilaparvata lugens were qualitatively measured by SQUID magnetometry, and their characteristics were further determined by Prussian Blue staining, electron microscopy and energy dispersive x-ray spectroscopy. The results indicate that there were remarkable magnetic materials in the abdomens and not in the head or thorax of the 3(rd)-5(th) instar nymphs, and in macropterous and brachypterous female and male adults of BPH. The size of magnetic particles was shown to be between 50-450 nm with a shape factor estimate of between 0.8-1.0 for all the tested BPHs. Moreover, the amount of magnetic particles was associated with the developmental stage (the 3(rd)-5(th) instar), wing form (macropterous vs. brachypterous) and sex. The macropterous female adults had the largest amount of magnetic particles. Although the existence of magnetic particles in the abdomens of BPH provides sound basis for the assumption of magnetic orientation, further behavioral studies and complementary physical characterization experiments should be conducted to determine whether the orientation behavior of BPH is associated with the magnetic particles detected in this study. PMID:26727944

  20. Oxodicarboxylic acids in atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Römpp, Andreas; Winterhalter, Richard; Moortgat, Geert K.

    Fine mode aerosol was collected on quartz fiber filters at several sites across Europe. These samples were analyzed for carboxylic acids by liquid chromatography coupled to a hybrid (quadrupole and time-of-flight) mass spectrometer (LC/MS/MS-TOF). A series of oxodicarboxylic acids (C 7-C 11) was detected. Oxodicarboxylic acids are linear dicarboxylic acids with an additional carbonyl group. Previous measurements of these acids are scarce and their sources are largely unknown. Several structural isomers (different positions of the carbonyl group within the molecule) could be identified and differentiated by the combination of laboratory experiments and high mass accuracy measurements. The homologs with 9-11 carbon atoms were identified for the first time in atmospheric aerosol particles. The concentrations of oxodicarboxylic acids in ambient aerosol samples frequently exceeded those of the corresponding unsubstituted dicarboxylic acids. Oxodicarboxylic acids have been shown to be products of the reaction of dicarboxylic acids with OH radicals in chamber experiments and a reaction mechanism is proposed. Good correlation of oxodicarboxylic acid and hydroxyl radical concentrations was found at two measurement sites (Finland and Crete) of different geographic location and meteorological conditions. The ratios of individual isomers from the field samples are comparable to those of the laboratory experiments. The results of this study imply that the reaction of OH radicals and dicarboxylic acids is an important pathway for the production of oxodicarboxylic acids in the atmosphere. Oxodicarboxylic acids seem to be important intermediates in atmospheric oxidation processes of organic compounds.

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

    PubMed Central

    2015-01-01

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

  2. Sources and composition of urban aerosol particles

    NASA Astrophysics Data System (ADS)

    Vogt, M.; Johansson, C.; Mårtensson, M.; Struthers, H.; Ahlm, L.; Nilsson, D.

    2011-09-01

    From May 2008 to March 2009 aerosol emissions were measured using the eddy covariance method covering the size range 0.25 to 2.5 μm diameter (Dp) from a 105 m tower, in central Stockholm, Sweden. Supporting chemical aerosol data were collected at roof and street level. Results show that the inorganic fraction of sulfate, nitrate, ammonium and sea salt accounts for approximately 15% of the total aerosol mass <1 μm Dp (PM1) with water soluble soil contributing 11% and water insoluble soil 47%. Carbonaceous compounds were at the most 27% of PM1 mass. It was found that heating the air from the tower to 200 °C resulted in the loss of approximately 60% of the aerosol volume at 0.25 μm Dp whereas only 40% of the aerosol volume was removed at 0.6 μm Dp. Further heating to 300 °C caused very little additional losses <0.6 μm Dp. The chemical analysis did not include carbonaceous compounds, but based on the difference between the total mass concentration and the sum of the analyzed non-carbonaceous materials, it can be assumed that the non-volatile particulate material (heated to 300 °C) consists mainly of carbonaceous compounds, including elemental carbon. Furthermore, it was found that the non-volatile particle fraction <0.6 μm Dp correlated (r2 = 0.4) with the BC concentration at roof level in the city, supporting the assumption that the non-volatile material consists of carbonaceous compounds. The average diurnal cycles of the BC emissions from road traffic (as inferred from the ratio of the incremental concentrations of nitrogen oxides (NOx) and BC measured on a densely trafficked street) and the fluxes of non-volatile material at tower level are in close agreement, suggesting a traffic source of BC. We have estimated the emission factors (EFs) for non-volatile particles <0.6 μm Dp to be 2.4±1.4 mg veh-1 km-1 based on either CO2 fluxes or traffic activity data. Light (LDV) and heavy duty vehicle (HDV) EFs were estimated using multiple linear regression and

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

    NASA Astrophysics Data System (ADS)

    Zuend, A.; Seinfeld, J.

    2011-12-01

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

  4. AEROSOL OPTICAL PROPERTIES AND BIOGENIC SOA: EFFECT ON HYGROSCOPIC PROPERTIES AND LIGHT ABSORPTION

    EPA Science Inventory

    This study will provide a comprehensive characterization of optical properties of biogenic SOA and their sensitivity to anthropogenic influence. Several parameters critical for climate modeling, such as absorption cross-section, single scattering albedo and sensitivity to R...

  5. Fast determination of biogenic amines in beverages by a core-shell particle column.

    PubMed

    Preti, Raffaella; Antonelli, Marta Letizia; Bernacchia, Roberta; Vinci, Giuliana

    2015-11-15

    A fast and reliable HPLC method for the determination of 11 biogenic amines in beverages has been performed. After pre-column derivatization with dansyl-chloride a Kinetex C18 core-shell particle column (100 mm × 4.6 mm, 2.6 μm particle size) has been employed and the biogenic amines were identified and quantified in a total run time of 13 min with ultraviolet (UV) or fluorescence detection (FLD). Chromatographic conditions such as column temperature (kept at 50 °C), gradient elution and flow rate have been optimized and the method has been tested on red wine and fruit nectar. The proposed method is enhanced in terms of reduced analysis time and eluent consumption with respect of classical HPLC method as to be comparable to UHPLC methods. Green and cost-effective, this method can be used as a quality-control tool for routine quantitative analysis of biogenic amines in beverages for the average laboratory. PMID:25977063

  6. 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

  7. Chemical characterisation of atmospheric aerosols during a 2007 summer field campaign at Brasschaat, Belgium: sources and source processes of biogenic secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Gómez-González, Y.; Wang, W.; Vermeylen, R.; Chi, X.; Neirynck, J.; Janssens, I. A.; Maenhaut, W.; Claeys, M.

    2012-01-01

    Measurements of organic marker compounds and inorganic species were performed on PM2.5 aerosols from a Belgian forest site that is severely impacted by urban pollution ("De Inslag", Brasschaat, Belgium) during a 2007 summer period within the framework of the "Formation mechanisms, marker compounds, and source apportionment for biogenic atmospheric aerosols (BIOSOL)" project. The measured organic species included (i) low-molecular weight (MW) dicarboxylic acids (LMW DCAs), (ii) methanesulfonate (MSA), (iii) terpenoic acids originating from the oxidation of α-pinene, β-pinene, d-limonene and Δ3-carene, and (iv) organosulfates related to secondary organic aerosol from the oxidation of isoprene and α-pinene. The organic tracers explained, on average, 5.3 % of the organic carbon (OC), of which 0.7 % was due to MSA, 3.4 % to LMW DCAs, 0.6 % to organosulfates, and 0.6 % to terpenoic acids. The highest atmospheric concentrations of most species were observed during the first five days of the campaign, which were characterised by maximum day-time temperatures >22 °C. Most of the terpenoic acids and the organosulfates peaked during day-time, consistent with their local photochemical origin. High concentrations of 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA) and low concentrations of cis-pinonic acid were noted during the first five days of the campaign, indicative of an aged biogenic aerosol. Several correlations between organic species were very high (r>0.85), high (0.70.7) and showed an Arrhenius-type relationship, consistent with their formation through OH radical chemistry.

  8. Transition metal associations with primary biological particles in sea spray aerosol generated in a wave channel.

    PubMed

    Guasco, Timothy L; Cuadra-Rodriguez, Luis A; Pedler, Byron E; Ault, Andrew P; Collins, Douglas B; Zhao, Defeng; Kim, Michelle J; Ruppel, Matthew J; Wilson, Scott C; Pomeroy, Robert S; Grassian, Vicki H; Azam, Farooq; Bertram, Timothy H; Prather, Kimberly A

    2014-01-21

    In the ocean, breaking waves generate air bubbles which burst at the surface and eject sea spray aerosol (SSA), consisting of sea salt, biogenic organic species, and primary biological aerosol particles (PBAP). Our overall understanding of atmospheric biological particles of marine origin remains poor. Here, we perform a control experiment, using an aerosol time-of-flight mass spectrometer to measure the mass spectral signatures of individual particles generated by bubbling a salt solution before and after addition of heterotrophic marine bacteria. Upon addition of bacteria, an immediate increase occurs in the fraction of individual particle mass spectra containing magnesium, organic nitrogen, and phosphate marker ions. These biological signatures are consistent with 21% of the supermicrometer SSA particles generated in a previous study using breaking waves in an ocean-atmosphere wave channel. Interestingly, the wave flume mass spectral signatures also contain metal ions including silver, iron, and chromium. The nascent SSA bioparticles produced in the wave channel are hypothesized to be as follows: (1) whole or fragmented bacterial cells which bioaccumulated metals and/or (2) bacteria-derived colloids or biofilms which adhered to the metals. This study highlights the potential for transition metals, in combination with specific biomarkers, to serve as unique indicators for the presence of marine PBAP, especially in metal-impacted coastal regions. PMID:24328130

  9. 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.

  10. Emissions of biogenic volatile organic compounds and subsequent formation of secondary organic aerosols in a Larix kaempferi forest

    NASA Astrophysics Data System (ADS)

    Mochizuki, T.; Miyazaki, Y.; Ono, K.; Wada, R.; Takahashi, Y.; Saigusa, N.; Kawamura, K.; Tani, A.

    2015-10-01

    We conducted simultaneous measurements of concentrations and above-canopy fluxes of isoprene and α-pinene, along with their oxidation products in aerosols in a Larix kaempferi (Japanese larch) forest in summer 2012. Vertical profiles of isoprene showed the maximum concentration near the forest floor with a peak around noon, whereas oxidation products of isoprene, i.e., methacrolein (MACR) and methyl vinyl ketone (MVK), showed higher concentrations near the canopy level of the forest. The vertical profile suggests large emissions of isoprene near the forest floor, likely due to Dryopteris crassirhizoma (a fern species), and the subsequent reaction within the canopy. The concentrations of α-pinene also showed highest values near the forest floor, with maximums in the early morning and late afternoon. The vertical profiles of α-pinene suggest its large emissions from soil and litter in addition to emissions from L. kaempferi leaves at the forest site. Isoprene and its oxidation products in aerosols exhibited similar diurnal variations within the forest canopy, providing evidence of secondary organic aerosol (SOA) formation via oxidation of isoprene most likely emitted from the forest floor. Although high abundance of α-pinene was observed in the morning, its oxidation products in aerosols showed peaks in daytime, due to a time lag between the emission and atmospheric reactions of α-pinene to form SOA. Positive matrix factorization (PMF) analysis indicated that anthropogenic influence is the most important factor contributing to the elevated concentrations of molecular oxidation products of isoprene- (> 64 %) and α-pinene-derived SOA (> 57 %). The combination of the measured fluxes and vertical profiles of biogenic volatile organic compounds (BVOCs) suggests that the inflow of anthropogenic precursors/aerosols likely enhanced the formation of both isoprene SOA and α-pinene SOA within the forest canopy even when the BVOC flux was relatively low. This study

  11. Field studies of biogenic sulfur aerosols in inland and coastal wetlands

    SciTech Connect

    Dill, J.A.

    1983-01-01

    Two separate field studies were conducted, each of which was designed to address a specific objective. One study was conducted around a known source of biogenic H/sub 2/S at an inland location in Monroe County, NY. The objective of the Monroe County Experiment was to determine whether or not biogenic H/sub 2/S emissions in that area contribute significantly to local atmospheric concentration levels of sulfur oxides such as SO/sub 2/ and sulfate. A second study was conducted in a coastal location at Wallops Island, Virginia, where biogenic H/sub 2/S emissions have been shown to contribute to local atmospheric concentrations of sulfur oxide species. The objective of the Wallops Island study was to investigate the properties and behavior of these biogenic sulfur gases and particulates in an attempt to ascertain which factors govern their formation. From the Monroe County field study, the properties and behavior of the collected species indicated that the sulfur oxide species were primarily of anthropogenic origin. Although it is possible that biogenic sulfur oxides could have been present in the immediate vicinity of one of the five sites, the spatial orientation of the other sites was not conducive to demonstrating that such was the case. From the Wallops Island field study, these measurements were not found to contain useful information with respect to achieving the goals of the Wallops Island Experiment. This negative result was attributed to two factors.

  12. 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.

  13. Oxidation products of biogenic emissions contribute to nucleation of atmospheric particles.

    PubMed

    Riccobono, Francesco; Schobesberger, Siegfried; Scott, Catherine E; Dommen, Josef; Ortega, Ismael K; Rondo, Linda; Almeida, João; Amorim, Antonio; Bianchi, Federico; Breitenlechner, Martin; David, André; Downard, Andrew; Dunne, Eimear M; Duplissy, Jonathan; Ehrhart, Sebastian; Flagan, Richard C; Franchin, Alessandro; Hansel, Armin; Junninen, Heikki; Kajos, Maija; Keskinen, Helmi; Kupc, Agnieszka; Kürten, Andreas; Kvashin, Alexander N; Laaksonen, Ari; Lehtipalo, Katrianne; Makhmutov, Vladimir; Mathot, Serge; Nieminen, Tuomo; Onnela, Antti; Petäjä, Tuukka; Praplan, Arnaud P; Santos, Filipe D; Schallhart, Simon; Seinfeld, John H; Sipilä, Mikko; Spracklen, Dominick V; Stozhkov, Yuri; Stratmann, Frank; Tomé, Antonio; Tsagkogeorgas, Georgios; Vaattovaara, Petri; Viisanen, Yrjö; Vrtala, Aron; Wagner, Paul E; Weingartner, Ernest; Wex, Heike; Wimmer, Daniela; Carslaw, Kenneth S; Curtius, Joachim; Donahue, Neil M; Kirkby, Jasper; Kulmala, Markku; Worsnop, Douglas R; Baltensperger, Urs

    2014-05-16

    Atmospheric new-particle formation affects climate and is one of the least understood atmospheric aerosol processes. The complexity and variability of the atmosphere has hindered elucidation of the fundamental mechanism of new-particle formation from gaseous precursors. We show, in experiments performed with the CLOUD (Cosmics Leaving Outdoor Droplets) chamber at CERN, that sulfuric acid and oxidized organic vapors at atmospheric concentrations reproduce particle nucleation rates observed in the lower atmosphere. The experiments reveal a nucleation mechanism involving the formation of clusters containing sulfuric acid and oxidized organic molecules from the very first step. Inclusion of this mechanism in a global aerosol model yields a photochemically and biologically driven seasonal cycle of particle concentrations in the continental boundary layer, in good agreement with observations. PMID:24833386

  14. Relationships linking primary production, sea ice melting, and biogenic aerosol in the Arctic

    NASA Astrophysics Data System (ADS)

    Becagli, S.; Lazzara, L.; Marchese, C.; Dayan, U.; Ascanius, S. E.; Cacciani, M.; Caiazzo, L.; Di Biagio, C.; Di Iorio, T.; di Sarra, A.; Eriksen, P.; Fani, F.; Giardi, F.; Meloni, D.; Muscari, G.; Pace, G.; Severi, M.; Traversi, R.; Udisti, R.

    2016-07-01

    This study examines the relationships linking methanesulfonic acid (MSA, arising from the atmospheric oxidation of the biogenic dimethylsulfide, DMS) in atmospheric aerosol, satellite-derived chlorophyll a (Chl-a), and oceanic primary production (PP), also as a function of sea ice melting (SIM) and extension of the ice free area in the marginal ice zone (IF-MIZ) in the Arctic. MSA was determined in PM10 samples collected over the period 2010-2012 at two Arctic sites, Ny Ålesund (78.9°N, 11.9°E), Svalbard islands, and Thule Air Base (76.5°N, 68.8°W), Greenland. PP is calculated by means of a bio-optical, physiologically based, semi-analytical model in the potential source areas located in the surrounding oceanic regions (Barents and Greenland Seas for Ny Ålesund, and Baffin Bay for Thule). Chl-a peaks in May in the Barents sea and in the Baffin Bay, and has maxima in June in the Greenland sea; PP follows the same seasonal pattern of Chl-a, although the differences in absolute values of PP in the three seas during the blooms are less marked than for Chl-a. MSA shows a better correlation with PP than with Chl-a, besides, the source intensity (expressed by PP) is able to explain more than 30% of the MSA variability at the two sites; the other factors explaining the MSA variability are taxonomic differences in the phytoplanktonic assemblages, and transport processes from the DMS source areas to the sampling sites. The taxonomic differences are also evident from the slopes of the correlation plots between MSA and PP: similar slopes (in the range 34.2-36.2 ng m-3of MSA/(gC m-2 d-1)) are found for the correlation between MSA at Ny Ålesund and PP in Barents Sea, and between MSA at Thule and PP in the Baffin Bay; conversely, the slope of the correlation between MSA at Ny Ålesund and PP in the Greenland Sea in summer is smaller (16.7 ng m-3of MSA/(gC m-2 d-1)). This is due to the fact that DMS emission from the Barents Sea and Baffin Bay is mainly related to the MIZ

  15. 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

  16. Probing the bulk viscosity of particles using aerosol optical tweezers

    NASA Astrophysics Data System (ADS)

    Power, Rory; Bones, David L.; Reid, Jonathan P.

    2012-10-01

    Holographic aerosol optical tweezers can be used to trap arrays of aerosol particles allowing detailed studies of particle properties and processes at the single particle level. Recent observations have suggested that secondary organic aerosol may exist as ultra-viscous liquids or glassy states at low relative humidity, potentially a significant factor in influencing their role in the atmosphere and their activation to form cloud droplets. A decrease in relative humidity surrounding a particle leads to an increased concentration of solute in the droplet as the droplet returns to equilibrium and, thus, an increase in the bulk viscosity. We demonstrate that the timescales for condensation and evaporation processes correlate with particle viscosity, showing significant inhibition in mass transfer kinetics using ternary sucrose/sodium chloride/water droplets as a proxy to atmospheric multi-component aerosol. We go on to study the fundamental process of aerosol coagulation in aerosol particle arrays, observing the relaxation of non-spherical composite particles formed on coalescence. We demonstrate the use of bright-field imaging and elastic light scattering to make measurements of the timescale for the process of binary coalescence contrasting the rheological properties of aqueous sucrose and sodium chloride aerosol over a range of relative humidities.

  17. Biogenic iodine emissions and identification of end-products in coastal ultrafine particles during nucleation bursts

    NASA Astrophysics Data System (ADS)

    MäKelä, J. M.; Hoffmann, T.; Holzke, C.; VäKevä, M.; Suni, T.; Mattila, T.; Aalto, P. P.; Tapper, U.; Kauppinen, E. I.; O'Dowd, C. D.

    2002-10-01

    Ultrafine particles sampled during new particle formation bursts observed in the coastal zone were studied with transmission electron microscopy (TEM) and elemental analysis using energy-dispersive X ray (EDX). It was observed that both iodine and sulphur were present in the new particles with diameter below 10 mn. Gaseous emissions of halogen compounds from seaweeds were also measured at the same location during low-tide particle nucleation episodes. Based on the presence of iodine in the particle phase during low-tide nucleation bursts, and the significant emission of iodine compounds from the seaweeds during these periods, it is apparent that part of the biogenic iodine species emitted from the seaweeds end up in the ultrafine particulate phase. It was not possible to quantitatively determine the iodine content in the particles; however, in most cases the relative contribution from iodine and sulphate was similar, while some cases indicated no sulphate. On larger sized particles the contribution of sulphate was significantly higher than iodine. It appears that the condensable species leading to the appearance of new particles in the coastal atmosphere is an iodine species. Whether or not this iodine species also participates in the nucleation of new stable clusters could not be completely verified.

  18. Complex refractive indices in the near-ultraviolet spectral region of biogenic secondary organic aerosol aged with ammonia

    SciTech Connect

    Flores, J. M.; Washenfelder, Rebecca; Adler, Gabriela; Lee, H-J; Segev, Lior; Laskin, Julia; Laskin, Alexander; Nizkorodov, Sergey; Brown, Steven; Rudich, Yinon

    2014-05-14

    Atmospheric absorption by brown carbon aerosol may play an important role in global radiative forcing. Brown carbon arises from both primary and secondary sources, but the mechanisms and reactions for the latter are highly uncertain. One proposed mechanism is the reaction of ammonia or amino acids with carbonyl products in secondary organic aerosol (SOA). We generated SOA in situ by reacting biogenic alkenes (α-pinene, limonene, and α-humulene) with excess ozone, humidifying the resulting aerosol, and reacting the humidified aerosol with gaseous ammonia. We determined the complex refractive indices (RI) in the 360 – 420 nm range for these aerosols using broadband cavity enhanced spectroscopy (BBCES). The average real part (n) of the measured spectral range of the NH3-aged α-pinene SOA increased from n = 1.50 (±0.01) for the unreacted SOA to n = 1.57 (± 0.01) after a 1.5h exposure to 1.9 ppm NH3; whereas,the imaginary component (k) remained below k < 0.001 (± 0.002). For the limonene and α-humulene SOA the real part did not change significantly, and we observed a small change in the imaginary component of the RI. The imaginary component increased from k = 0.0 to an average k= 0.029 (± 0.021) for α-humulene SOA, and from k < 0.001 (± 0.002) to an average k = 0.032 (±0.019) for limonene SOA after a 1.5 h exposure to 1.3 and 1.9 ppm of NH3, respectively. Collected filter samples of the aged and unreacted α-pinene SOA and limonene SOA were analyzed off-line with nanospray desorption electrospray ionization high resolution mass spectrometry (nano-DESI/HR-MS), and in-situ with a Time-of-Fligh Aerosol Mass Spectrometer, confirming that the SOA reacted and that various nitrogen-containing reaction products formed. If we assume that NH3 aging reactions scale linearly with time and concentration, then a 1.5 h reaction with 1 ppm NH3 in the laboratory is equivalent to 24 h reaction with 63 ppbv NH3, indicating that the observed aerosol absorption will be limited

  19. 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.

  20. High-time resolved measurements of biogenic and anthropogenic secondary organic aerosol precursors and products in urban air

    NASA Astrophysics Data System (ADS)

    Flores, Rosa M.; Doskey, Paul V.

    2016-04-01

    Volatile organic compounds (VOCs), which are present in the atmosphere entirely in the gas phase are directly emitted by biogenic (~1089 Tg yr-1) and anthropogenic sources (~185 Tg yr-1). However, the sources and molecular speciation of intermediate VOCs (IVOCs), which are for the most part also present almost entirely in the gas phase, are not well characterized. The VOCs and IVOCs participate in reactions that form ozone and semivolatile OC (SVOC) that partition into the aerosol phase. Formation and evolution of secondary organic aerosol (SOA) are part of a complex dynamic process that depends on the molecular speciation and concentration of VOCs, IVOCs, primary organic aerosol (POA), and the level of oxidants (NO3, OH, O3). The current lack of understanding of OA properties and their impact on radiative forcing, ecosystems, and human health is partly due to limitations of models to predict SOA production on local, regional, and global scales. More accurate forecasting of SOA production requires high-temporal resolution measurement and molecular characterization of SOA precursors and products. For the subject study, the IVOCs and aerosol-phase organic matter were collected using the high-volume sampling technique and were analyzed by multidimensional gas chromatography with time-of-flight mass spectrometry (GCxGC-ToFMS). The IVOCs included terpenes, terpenoids, n-alkanes, branched alkanes, isoprenoids, alkylbenzenes, cycloalkylbenzenes, PAH, alkyl PAH, and an unresolved complex mixture (UCM). Diurnal variations of OA species containing multiple oxygenated functionalities and selected SOA tracers of isorprene, α-pinene, toluene, cyclohexene, and n-dodecane oxidation were also quantified. The data for SOA precursor and oxidation products presented here will be useful for evaluating the ability of molecular-specific SOA models to forecast SOA production in and downwind of urban areas.

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

    SciTech Connect

    Davidovits, Paul

    2015-10-20

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

  2. Identifying organic aerosol sources by comparing functional group composition in chamber and atmospheric particles

    PubMed Central

    Russell, Lynn M.; Bahadur, Ranjit; Ziemann, Paul J.

    2011-01-01

    Measurements of submicron particles by Fourier transform infrared spectroscopy in 14 campaigns in North America, Asia, South America, and Europe were used to identify characteristic organic functional group compositions of fuel combustion, terrestrial vegetation, and ocean bubble bursting sources, each of which often accounts for more than a third of organic mass (OM), and some of which is secondary organic aerosol (SOA) from gas-phase precursors. The majority of the OM consists of alkane, carboxylic acid, hydroxyl, and carbonyl groups. The organic functional groups formed from combustion and vegetation emissions are similar to the secondary products identified in chamber studies. The near absence of carbonyl groups in the observed SOA associated with combustion is consistent with alkane rather than aromatic precursors, and the absence of organonitrate groups can be explained by their hydrolysis in humid ambient conditions. The remote forest observations have ratios of carboxylic acid, organic hydroxyl, and nonacid carbonyl groups similar to those observed for isoprene and monoterpene chamber studies, but in biogenic aerosols transported downwind of urban areas the formation of esters replaces the acid and hydroxyl groups and leaves only nonacid carbonyl groups. The carbonyl groups in SOA associated with vegetation emissions provides striking evidence for the mechanism of esterification as the pathway for possible oligomerization reactions in the atmosphere. Forest fires include biogenic emissions that produce SOA with organic components similar to isoprene and monoterpene chamber studies, also resulting in nonacid carbonyl groups in SOA. PMID:21317360

  3. Contribution of fungi to primary biogenic aerosols in the atmosphere: active discharge of spores, carbohydrates, and inorganic ions by Asco- and Basidiomycota

    NASA Astrophysics Data System (ADS)

    Elbert, W.; Taylor, P. E.; Andreae, M. O.; Pöschl, U.

    2006-11-01

    Spores and related chemical compounds from actively spore-discharging Ascomycota (AAM) and actively spore-discharging Basidiomycota (ABM) are primary biogenic components of air particulate matter (characteristic size range 1-10 μm). Measurement results and budget calculations based on investigations in Amazonia (Balbina, Brazil, July 2001) indicate that the forcible discharge of fungal spores may account for a large proportion of coarse air particulate matter in tropical rainforest regions during the wet season. For the particle diameter range of 1-10 μm, the estimated proportions are ~25% during day-time, ~45% at night, and ~35% on average. For the sugar alcohol, mannitol, the budget calculations indicate that it is suitable for use as a molecular tracer for actively discharged basidiospores (ABS), and that the literature-derived emission ratio of about 5 pg per ABS may be taken as a representative average. ABM emissions may account for most of the atmospheric abundance of mannitol, and can explain the observed diurnal cycle (higher abundance at night). ABM emissions of hexose carbohydrates might also account for a significant proportion of glucose and fructose in air particulate matter, but the literature-derived ratios are not consistent with the observed diurnal cycle (lower abundance at night). AAM emissions appear to account for a large proportion of potassium in air particulate matter over tropical rainforest regions during the wet season, and they can also explain the observed diurnal cycle (higher abundance at night). The results of our investigations and budget calculations for tropical rainforest aerosols are consistent with measurements performed at other locations. Based on the average abundance of mannitol in particulate matter, which is consistent with the above emission ratio and the observed abundance of ABS, we have also calculated a value of ~17 Tg yr-1 as a first estimate for the global average emission rate of ABS over land surfaces

  4. Dynamics of sinking particles in northern Japan trench in the western North Pacific: biogenic chemical components and fatty acids biomarkers

    NASA Astrophysics Data System (ADS)

    Shin, K. H.; Noriki, S.; Itou, M.; Tsunogai, S.

    Biogenic opal was predominant component, and had strongly positive correlation with organic carbon in both traps. The average atomic ratios of biogenic opal and calcium carbonate (CaCO 3) were also large (7.1 and 11 in the shallow and deep trap, respectively) and the highest ratio was found in May 1995, when the biogenic opal proportion (%) to the total particle flux and C org/C inorg ratio increased concomitantly. However, transient switching of the biogenic opal and CaCO 3 ratios (0.6 and 0.8) was observed in winter 1995, which seems to be related to a warm-core ring developed in the northwestern Pacific. Downward fluxes of fatty acids as molecular markers were determined and compared with major biogenic chemical components in sinking particles. As a diatom index of fatty acids, the 16:1(n-7)/16:0 ratio is positively related to biogenic opal contribution (%) to the sinking particles in the shallow and deep traps. 20:5(n-3) proportion (%) was also correlated with opal content (%) in sinking particles in the 1-km trap. In addition, a major source of sinking fatty acids in the western North Pacific might be characterized by algal fatty acids as a diatom marker (16:1(n-7)), comparing to a zooplankton fatty acid (18:1(n-9)) in the central North Pacific and fecal pellets and coccolithophores in the eastern North Pacific, respectively. Also, PUFA index (a measure of polyunsaturated fatty acids contribution to the total fatty acids) correlated well with Chl a inventory in surface 0-50 m water. These results suggest that undegraded diatomaceous fatty acids are present in sinking particles, and the composition of fatty acids is useful to understand the origin of sinking organic particles.

  5. Formation of Secondary Particulate Matter by Reactions of Gas Phase Hexanal with Sulfate Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Zhang, J.

    2003-12-01

    The formation of secondary particulate matter from the atmospheric oxidation of organic compounds can significantly contribute to the particulate burden, but the formation of organic secondary particulate matter is poorly understood. One way of producing organic secondary particulate matter is the oxidation of hydrocarbons with seven or more carbon atoms to get products with low vapor pressure. However, several recent reports suggest that relatively low molecular weight carbonyls can enter the particle phase by undergoing heterogeneous reactions. This may be a very important mechanism for the formation of organic secondary particulate matter. Atmospheric aldehydes are important carbonyls in the gas phase, which form via the oxidation of hydrocarbons emitted from anthropogenic and biogenic sources. In this poster, we report the results on particle growth by the heterogeneous reactions of hexanal. A 5 L Continuous Stirred Tank Reactor (CSTR) is set up to conduct the reactions in the presence of seed aerosol particles of deliquesced ammonia bisulfate. Hexanal is added into CSTR by syringe pump, meanwhile the concentrations of hexanal are monitored with High Pressure Liquid Chromatograph (HPLC 1050). A differential Mobility Analyzer (TSI 3071) set to an appropriate voltage is employed to obtain monodisperse aerosols, and another DMA associated with a Condensation Nuclear Counter (TSI 7610) is used to measure the secondary particle size distribution by the reaction in CSTR. This permits the sensitive determination of particle growth due to the heterogeneous reaction, very little growth occurs when hexanal added alone. Results for the simultaneous addition of hexanal and alcohols will also be presented.

  6. Inkjet aerosol generator as monodisperse particle number standard

    NASA Astrophysics Data System (ADS)

    Iida, Kenjiro; Sakurai, Hiromu; Ehara, Kensei

    2013-05-01

    Inkjet technology can be applied to generate highly monodisperse aerosol particles in micrometer range at a precisely controlled rate. AIST has been developing an inkjet aerosol generator (AIST-IAG), and the device will soon become the secondary measurement standard for aerosol particle number concentration in 0.35 μm to 10 μm range. The AIST-IAG can generate both solid and liquid particles consisting of water-soluble ionic compounds. We first report the characteristics of the particle sizes of the generated particles. The full width half maximum of the particle size distribution is about 2 percent, and the particle diameter of the IAG particles was calibrated as a function of the particle mass within 0.6-10 μm range using polystyrene latex sphere as reference material. Then we report the capability of the AIST-IAG as the particle number standard. The particle generation efficiency ηIAG was defined as the number of aerosol particles exiting from the AIST-IAG divided by the rate of the droplet generation, and the values of ηIAG within 0.35-10 μm is essentially 100%, and the 95% confidence interval of the values is less than 1%. The result strongly supports that the AISTIAG can be used to calibrate the counting efficiency of the optical particle counters in submicrometer to micrometer range.

  7. Characterization of primary and secondary organic aerosols in Melbourne airshed: The influence of biogenic emissions, wood smoke and bushfires

    NASA Astrophysics Data System (ADS)

    Iinuma, Yoshiteru; Keywood, Melita; Herrmann, Hartmut

    2016-04-01

    Detailed chemical characterisation was performed for wintertime and summertime PM10 samples collected in Melbourne, Australia. The samples were analysed for marker compounds of biomass burning and biogenic secondary organic aerosol (SOA). The chemical analysis showed that the site was significantly influenced by the emissions from wintertime domestic wood combustion and summertime bushfires. Monosaccharide anhydrides were major primary biomass burning marker compounds found in the samples with the average concentrations of 439, 191, 57 and 3630 ngm-3 for winter 2004, winter 2005, summer 2005 and summer 2006, respectively. The highest concentration was determined during the summer 2006 bushfire season with the concentration of 15,400 ngm-3. Biomass burning originating SOA compounds detected in the samples include substituted nitrophenols, mainly 4-nitrocatechol (Mr 155), methyl-nitrocatechols (Mr 169) and dimethyl-nitrocatechols (Mr 183) with the sum concentrations as high as 115 ngm-3 for the wintertime samples and 770 ngm-3 for the bushfire influenced samples. In addition to this, elevated levels of biogenic SOA marker compounds were determined in the summertime samples influence by bushfire smoke. These marker compounds can be categorised into carboxylic acid marker compounds and heteroatomic organic acids containing nitrogen and sulfur. Carboxylic acid marker compounds can be largely attributed to oxidation products originating from 1,8-cineole, α-pinene and β-pinene that are main constituents of eucalyptus VOC emissions. Among those, diaterpenylic acid, terpenylic acid and daterebic acid were found at elevated levels in the bushfire influenced samples. Heteroatomic monoterpene SOA marker compounds (Mr 295, C10H17NO7S) were detected during both winter and summer periods. Especially high levels of these compounds were determined in the severe bushfire samples from summer 2006. Based on the results obtained from the chemical analysis and a macro tracer method

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

    EPA Science Inventory

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

  9. Climate impacts of biogenic organic compounds

    NASA Astrophysics Data System (ADS)

    Sengupta, Kamalika; Gordon, Hamish; Almeida, Joao; Rap, Alex; Scott, Catherine; Pringle, Kirsty; Carslaw, Ken

    2016-04-01

    Currently the most uncertain driver of climate change, impact of anthropogenic aerosols on earth's radiative balance depends significantly on estimates of cloud condensation nuclei (CCN), representation of the pre-industrial atmosphere among others. Nearly 90% of aerosols in the tropics are organic in nature of which a major part comes from biogenic sources. About 45% of the CCN in the atmosphere are formed in-situ via nucleation. Understanding the role of biogenic organic compounds in particle formation and their subsequent growth is hence imperative in order to quantify the climate impact of aerosols. The CLOUD experiment at CERN, which measures particle formation and growth rates in a uniquely clean chamber under atmospherically relevant conditions, found evidence of a nucleation mechanism involving only biogenic organic compounds. This mechanism significantly changes our pre-industrial estimates. The experimental results have been parameterized and included in a global aerosol microphysics model, GLOMAP, to quantify the impact of pure biogenic nucleation on CCN formation and their climatic impact. Further the treatment of secondary organic compounds in GLOMAP has been improved and the sensitivity of our estimates of radiative forcing to the same has been evaluated.

  10. An increase in the biogenic aerosol concentration as a contributing factor to the recent wetting trend in Tibetan Plateau

    PubMed Central

    Fang, Keyan; Makkonen, Risto; Guo, Zhengtang; Zhao, Yan; Seppä, Heikki

    2015-01-01

    A significant wetting trend since the early 1980s in Tibetan Plateau (TP) is most conspicuous in central and eastern Asia as shown in the instrumental data and the long-term moisture sensitive tree rings. We found that anomalies in the large-scale oceanic and atmospheric circulations do not play a significant role on the wetting trend in TP. Meanwhile, the weak correlation between local temperature and precipitation suggests that the temperature-induced enhancement of the local water cycle cannot fully explain the wetting trend either. This may indicate the presence of nonlinear processes between local temperature and precipitation. We hypothesize that the current warming may enhance the emissions of the biogenic volatile organic compounds (BVOC) that can increase the secondary organic aerosols (SOA), contributing to the precipitation increase. The wetting trend can increase the vegetation cover and cause a positive feedback on the BVOC emissions. Our simulations indicate a significant contribution of increased BVOC emissions to the regional organic aerosol mass and the simulated increase in BVOC emissions is significantly correlated with the wetting trend in TP. PMID:26411261

  11. An increase in the biogenic aerosol concentration as a contributing factor to the recent wetting trend in Tibetan Plateau.

    PubMed

    Fang, Keyan; Makkonen, Risto; Guo, Zhengtang; Zhao, Yan; Seppä, Heikki

    2015-01-01

    A significant wetting trend since the early 1980s in Tibetan Plateau (TP) is most conspicuous in central and eastern Asia as shown in the instrumental data and the long-term moisture sensitive tree rings. We found that anomalies in the large-scale oceanic and atmospheric circulations do not play a significant role on the wetting trend in TP. Meanwhile, the weak correlation between local temperature and precipitation suggests that the temperature-induced enhancement of the local water cycle cannot fully explain the wetting trend either. This may indicate the presence of nonlinear processes between local temperature and precipitation. We hypothesize that the current warming may enhance the emissions of the biogenic volatile organic compounds (BVOC) that can increase the secondary organic aerosols (SOA), contributing to the precipitation increase. The wetting trend can increase the vegetation cover and cause a positive feedback on the BVOC emissions. Our simulations indicate a significant contribution of increased BVOC emissions to the regional organic aerosol mass and the simulated increase in BVOC emissions is significantly correlated with the wetting trend in TP. PMID:26411261

  12. 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.

  13. 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.

  14. Continuous air monitor for alpha-emitting aerosol particles

    SciTech Connect

    McFarland, A.R.; Ortiz, C.A. . Dept. of Mechanical Engineering); Rodgers, J.C.; Nelson, D.C. )

    1990-01-01

    A new alpha Continuous Air Monitor (CAM) sampler is being developed for use in detecting the presence of alpha-emitting aerosol particles. The effort involves design, fabrication and evaluation of systems for the collection of aerosol and for the processing of data to speciate and quantify the alpha emitters of interest. At the present time we have a prototype of the aerosol sampling system and we have performed wind tunnel tests to characterize the performance of the device for different particle sizes, wind speeds, flow rates and internal design parameters. The results presented herein deal with the aerosol sampling aspects of the new CAM sampler. Work on the data processing, display and alarm functions is being done in parallel with the particle sampling work and will be reported separately at a later date. 17 refs., 5 figs., 3 tabs.

  15. Seasonal Aerosol Distributions at Summit, Greenland: EC, OC, 14C and Individual Particle Analysis

    NASA Astrophysics Data System (ADS)

    Klouda, G. A.; Conny, J. M.; McNichol, A. P.; Dibb, J. E.

    2011-12-01

    Aerosol is known to affect the Earth's atmosphere and surface albedo thus having an influence on climate. In the case of carbonaceous aerosol, organic carbon (OC) tends to scatter sunlight while elemental (soot) carbon (EC) aerosol absorbs light. Considering the importance of these aerosols on snow and ice albedo (Hansen and Nazarenko, 2004), PM2.5, PM2.5-10 and snow-melt filters were collected weekly at Summit, Greenland from August 2000 to August 2002 to measure particulate EC, OC, and 14C of total carbon; the latter to quantify natural and anthropogenic source contributions. The pattern of PM2.5 shows a spring-summer maxima in EC (~10 ng m-3) and OC (~ 100 ng m-3); with levels consistent with summer 2006 measurements reported by Hagler et al. (2007). For a subset of filters over the two year period, the average biogenic contribution to PM2.5 OC was estimated to be 20 ng m-3 considering an average percent modern carbon of 46 % (SD=18 %; n=21) and an average total carbon concentration of 50 ng m-3. A summer maximum was observed in PM2.5-10 OC (~ 1000 ng m-3), while for the most part EC concentrations were below detection (< 300 ng m-3; limited primarily by the volume of air sampled). To provide insight into scattering and absorption properties of aerosols at Summit, we used scanning electron microscopy (SEM) to investigate the size, shape, and chemistry of particle populations as well as individual particles from selected filters. Particles were migrated from the filters to polished silicon or germanium wafers using an electrostatically-assisted centrifugation technique. Particle populations were studied by employing secondary electron imaging and energy dispersive x-ray spectroscopy (EDX) with automated SEM and associated particle analysis software. The size, shape, and composition of individual particles were studied with field-emission SEM employing secondary and backscatter electron imaging, bright-field and dark-field scanning transmission electron microscopy

  16. 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.

  17. 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.

  18. A portable optical particle counter system for measuring dust aerosols.

    PubMed

    Marple, V A; Rubow, K L

    1978-03-01

    A portable battery-operated optical particle counter/multichannel analyzer system has been developed for the numbers size distribution and number concentration measurement of light-absorbing irregular-shaped dust particles. An inertial impactor technique has been used to obtain calibration curves by relating the magnitude of the optical counter's signal to the particle's aerodynamic or Stokes' diameter. These calibrations have been made for aerosols of coal, potash, silica, rock (copper ore), and Arizona road dust particles. PMID:645547

  19. Secondary aerosol formation from the oxidation of biogenic hydrocarbons by chlorine atoms

    NASA Astrophysics Data System (ADS)

    Cai, Xuyi; Griffin, Robert J.

    2006-07-01

    The chlorine atom (Cl) is a potential oxidant of volatile organic compounds (VOCs) in the atmosphere and is hypothesized to lead to secondary organic aerosol (SOA) formation in coastal and industrialized areas. The purpose of this paper is to test this hypothesis and to quantify the SOA formation potentials of the common monoterpenes α-pinene, β-pinene, and d-limonene when oxidized by Cl in laboratory chamber experiments. Results indicate that the oxidation of these monoterpenes generates significant amounts of aerosol. The SOA yields of α-pinene, β-pinene, and d-limonene in this study are comparable to those when they are oxidized by ozone, by nitrate radical, and in photooxidation scenarios. For aerosol mass up to 30.0 μg m-3, their yields reach approximately 0.20, 0.20, and 0.30, respectively. For d-limonene, data indicate two yield curves that depend on the initial concentration ratio of Cl precursor to d-limonene. It is argued theoretically that multiple SOA yield curves may be common for VOCs, depending on the initial concentration ratio of oxidant to VOC. SOA formation from the three typical monoterpenes when oxidized by Cl in the marine boundary layer, coastal areas, and inland industrialized areas could be a source of organic aerosol in the early morning.

  20. Retrieval of particle size distribution from aerosol optical thickness using an improved particle swarm optimization algorithm

    NASA Astrophysics Data System (ADS)

    Mao, Jiandong; Li, Jinxuan

    2015-10-01

    Particle size distribution is essential for describing direct and indirect radiation of aerosols. Because the relationship between the aerosol size distribution and optical thickness (AOT) is an ill-posed Fredholm integral equation of the first type, the traditional techniques for determining such size distributions, such as the Phillips-Twomey regularization method, are often ambiguous. Here, we use an approach based on an improved particle swarm optimization algorithm (IPSO) to retrieve aerosol size distribution. Using AOT data measured by a CE318 sun photometer in Yinchuan, we compared the aerosol size distributions retrieved using a simple genetic algorithm, a basic particle swarm optimization algorithm and the IPSO. Aerosol size distributions for different weather conditions were analyzed, including sunny, dusty and hazy conditions. Our results show that the IPSO-based inversion method retrieved aerosol size distributions under all weather conditions, showing great potential for similar size distribution inversions.

  1. 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.

  2. Studying seasonal variations in carbonaceous aerosol particles in the atmosphere over central Siberia

    NASA Astrophysics Data System (ADS)

    Mikhailov, E. F.; Mironova, S. Yu.; Makarova, M. V.; Vlasenko, S. S.; Ryshkevich, T. I.; Panov, A. V.; Andreae, M. O.

    2015-07-01

    The results of 2-year (2010-2012) measurements of the concentrations of organic carbon (OC) and elemental carbon (EC), which were taken at the Zotino Tall Tower Observatory (ZOTTO) Siberian background station (61° N, 89° E), are given. Despite the fact that this station is located far from populated areas and industrial zones, the concentrations of OC and EC in the atmosphere over boreal forests in central Siberia significantly exceed their background values. In winter and fall, high concentrations of atmospheric carbonaceous aerosol particles are caused by the long-range transport (~1000 km) of air masses that accumulate pollutants from large cities located in both southern and southwestern regions of Siberia. In spring and summer, the pollution level is also high due to regional forest fires and agricultural burning in the steppe zone of western Siberia in the Russian-Kazakh border region. Background concentrations of carbonaceous aerosol particles were observed within relatively short time intervals whose total duration was no more than 20% of the entire observation period. In summer, variations in the background concentrations of OC closely correlated with air temperature, which implies that the biogenic sources of organic-particle formation are dominating.

  3. 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...

  4. 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.

  5. Short-term biogenic particle flux under late spring sea ice in the western Weddell Sea

    NASA Astrophysics Data System (ADS)

    Michels, Jan; Dieckmann, Gerhard S.; Thomas, David N.; Schnack-Schiel, Sigrid B.; Krell, Andreas; Assmy, Philipp; Kennedy, Hilary; Papadimitriou, Stathis; Cisewski, Boris

    2008-04-01

    In the framework of the "Ice Station POLarstern" (ISPOL) expedition in the western Weddell Sea, two sediment traps were deployed at 10 and 70 m water depth under a drifting ice floe in December 2004. The amount and composition of the vertical particle flux under sea ice were determined during a period of 30 days in order to investigate the influence of biological processes in sea ice and on its underside on the flux. The total mass flux was dominated by diatoms, faecal material, and aggregates, and ranged from 95.28 to 197.67 mg m -2 d -1 at 10 m depth and from 51.54 to 55.34 mg m -2 d -1 at 70 m depth. A strong increase with time of the flux of chlorophyll equivalents, biogenic silica, and faecal material was recorded during the observation period, coincident with the increase in the concentration of chlorophyll a in the bottom ice layer above the trap array. The latter suggests a concomitant increase in the amount of food available for grazers, such as krill, in the bottom ice layer and on the underside of the ice floe, resulting in an increased downward transport of ice-algal material into the water column. The sinking faecal material was dominated by krill faecal strings and contained large amounts of diatom frustule debris, as well as intact diatom frustules, mainly of the species Fragilariopsis curta and F. cylindrus. Single pronounced flux events of Phaeocystis antarctica and aggregates were also observed early in the study period. Low POC/PON and biogenic silica/POC ratios of the sinking particulate matter suggest that the material collected in the traps was relatively fresh.

  6. Hourly Measurement of the Concentration and Gas-Particle Partitioning of Oxygenated Organic Tracers in Ambient Aerosol: First Results from Berkeley, CA and Rural Alabama

    NASA Astrophysics Data System (ADS)

    Isaacman, G. A.; Kreisberg, N. M.; Yee, L.; Chan, A.; Worton, D. R.; Hering, S. V.; Goldstein, A. H.

    2013-12-01

    Hourly and bi-hourly time-resolved measurements of organic tracer compounds in ambient aerosols have been successfully used to elucidate sources and formation pathways of atmospheric particulate matter. Here we extend the Semi-Volatile Thermal desorption Aerosol Gas chromatograph (SVTAG), a custom in-situ instrument that collects, desorbs, and analyzes ambient aerosol and semi-volatile compounds with hourly time resolution, to include on-line derivatization and a second, parallel collection cell that provides simultaneous collection of both particle-phase and particle-plus-gas-phase organic compounds. By introducing a silylating agent upon desorption, SVTAG can measure highly oxygenated compounds that are not easily detected using traditional gas chromatography including most of the previously reported oxygenated tracers for biogenic and anthropogenic secondary organic aerosol. The use of a pair of matched collection cells with parallel sampling and serial analysis provides direct gas-particle partitioning information. One cell collects the total organic fraction of compounds with volatilities lower than a C13 hydrocarbon, while the other cell samples through an activated carbon denuder to selectively remove the gas-phase components. Taken together these provide a direct measurement of gas-particle partitioning to yield a check on classical absorption based partitioning theory while deviations from this theory provide constraints on other driving factors in aerosol formation chemistry, such as oligomerization, salt formation, and acidity. We present here the capabilities and utility of the dual cell SVTAG with derivatization, with chemical insights gained from initial tests on ambient Berkeley air and the first results from a rural site in Alabama obtained during the Southern Oxidant and Aerosol Study (SOAS). Tracers for varying isoprene oxidation pathways are used to explore the influence of anthropogenic emissions; concentrations of 2-methyltetrols and 2-methyl

  7. Secondary organic aerosols formed from oxidation of biogenic volatile organic compounds in the Sierra Nevada Mountains of California

    NASA Astrophysics Data System (ADS)

    Cahill, Thomas M.; Seaman, Vincent Y.; Charles, M. Judith; Holzinger, Rupert; Goldstein, Allen H.

    2006-08-01

    Biogenic volatile organic compound (BVOC) emissions, such as isoprene and terpenes, can be oxidized to form less volatile carbonyls, acids, and multifunctional oxygenated products that may condense to form secondary organic aerosols (SOA). This research was designed to assess the contribution of oxidized BVOC emissions to SOA in coniferous forests by collecting high-volume particulate samples for 6 days and 5 nights in the summer of 2003. The samples were analyzed for acids, carbonyls, polyols and alkanes to quantify oxidized BVOCs. Terpene and isoprene oxidation products were among the most abundant chemical species detected with the exception of hexadecanoic acid, octadecanoic acid and two butyl esters of unknown origin. The terpene oxidation products of pinonic acid, pinic acid, nopinone and pinonaldehyde showed clear diurnal cycles with concentrations two- to eight-fold higher at night. These cycles resulted from the diurnal cycles in gaseous terpene concentrations and lower temperatures that enhanced condensation of semivolatile chemicals onto aerosols. The terpene-derived compounds averaged 157 ± 118 ng/m3 of particulate organic matter while the isoprene oxidation compounds, namely the 2-methyltetrols and 2-methylglyceric acid, accounted for 53 ± 19 ng/m3. Together, the terpene and isoprene oxidation products represented 36.9% of the identified organic mass of 490 ± 95 ng/m3. PM10 organic matter loadings in the region were approximately 2.1 ± 1.2 μg/m3, so about 23% of the organic matter was identified and at least 8.6% was oxidized BVOCs. The BVOC oxidation products we measured were significant, but not dominant, contributors to the regional SOA only 75 km downwind of the Sacramento urban area.

  8. Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

    NASA Astrophysics Data System (ADS)

    Faiola, C. L.; Wen, M.; VanReken, T. M.

    2015-04-01

    The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- and post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.

  9. Chemical characterization of biogenic secondary organic aerosol generated from plant emissions under baseline and stressed conditions: inter- and intra-species variability for six coniferous species

    DOE PAGESBeta

    Faiola, C. L.; Wen, M.; VanReken, T. M.

    2015-04-01

    The largest global source of secondary organic aerosol (SOA) in the atmosphere is derived from the oxidation of biogenic emissions. Plant stressors associated with a changing environment can alter both the quantity and composition of the compounds that are emitted. Alterations to the biogenic volatile organic compound (BVOC) profile could impact the characteristics of the SOA formed from those emissions. This study investigated the impacts of one global change stressor, increased herbivory, on the composition of SOA derived from real plant emissions. Herbivory was simulated via application of methyl jasmonate (MeJA), a proxy compound. Experiments were repeated under pre- andmore » post-treatment conditions for six different coniferous plant types. Volatile organic compounds (VOCs) emitted from the plants were oxidized to form SOA via dark ozone-initiated chemistry. The SOA chemical composition was measured using a Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS). The aerosol mass spectra of pre-treatment biogenic SOA from all plant types tended to be similar with correlations usually greater than or equal to 0.90. The presence of a stressor produced characteristic differences in the SOA mass spectra. Specifically, the following m/z were identified as a possible biogenic stress AMS marker with the corresponding HR ion(s) shown in parentheses: m/z 31 (CH3O+), m/z 58 (C2H2O2+, C3H6O+), m/z 29 (C2H5+), m/z 57 (C3H5O+), m/z 59 (C2H3O2+, C3H7O+), m/z 71 (C3H3O2+, C4H7O+), and m/z 83 (C5H7O+). The first aerosol mass spectrum of SOA generated from the oxidation of the plant stress hormone, MeJA, is also presented. Elemental analysis results demonstrated an O : C range of baseline biogenic SOA between 0.3 and 0.47. The O : C of standard MeJA SOA was 0.52. Results presented here could be used to help identify a biogenic plant stress marker in ambient data sets collected in forest environments.« less

  10. 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.

  11. 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.

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

    SciTech Connect

    Fung, K.H.

    1999-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  14. Organosulfates and oxidation products from biogenic hydrocarbons in fine aerosols from a forest in North West Europe during spring

    NASA Astrophysics Data System (ADS)

    Kristensen, Kasper; Glasius, Marianne

    2011-09-01

    Organosulfates of monoterpenes and isoprene, as well as their oxidation products have been identified in biogenic secondary organic aerosols (BSOA) from both laboratory and field studies. Organosulfates provide an interesting coupling between air pollution and formation of low-volatility BSOA. HPLC quadrupole time-of-flight mass spectrometry was used to study polar acidic monoterpene and isoprene oxidation products including pinic acid, pinonic and terpenylic acid along with organosulfates and nitrooxy organosulfates in aerosols from ambient air. The method was first validated by analysis of spiked quartz filters, which showed acceptable recoveries >74% for pinic acid, pinonic acid, camphor sulphonic acid and adipic acid. Acetonitrile was identified as a better solvent than methanol for extraction and analysis of pinonic acid and adipic acid, due to improved analytical sensitivity and prevention of methyl ester formation during sample extraction. PM 1 (i.e, aerosols with an aerodynamic diameter ≤1 μm) were collected during spring 2008 in a forest in Denmark with mixed deciduous and coniferous trees. Average concentrations of the most abundant compounds were: pinic acid: 1.5 ng m -3, pinonic acid: 3.0 ng m -3, terpenylic acid: 0.8 ng m -3 and 3-methyl-1,2,3-butanetricarboxylic acid: 3.0 ng m -3. Organosulfates and nitrooxy organosulfates were identified in a majority of the daily samples and the highest levels were observed during a warm period in late spring. As a first approach, due to the lack of authentic standards, organosulfates and nitrooxy organosulfates were tentatively quantified based on the analytical response of camphor sulphonic acid. Generally the concentrations of organosulfates and nitrooxy organosulfates were lower than first generation oxidation products. The maximum concentration of a total of 10 organosulfates and nitrooxy organosulfates were found to be about three times lower than pinonic acid with a maximum concentration of 8 ng m -3. A

  15. Sugar markers in aerosol particles from an agro-industrial region in Brazil

    NASA Astrophysics Data System (ADS)

    Urban, R. C.; Alves, C. A.; Allen, A. G.; Cardoso, A. A.; Queiroz, M. E. C.; Campos, M. L. A. M.

    2014-06-01

    This work aimed to better understand how aerosol particles from sugar cane burning contribute to the chemical composition of the lower troposphere in an agro-industrial region of São Paulo State (Brazil) affected by sugar and ethanol fuel production. During a period of 21 months, we collected 105 samples and quantified 20 saccharides by GC-MS. The average concentrations of levoglucosan (L), mannosan (M), and galactosan (G) for 24-h sampling were 116, 16, and 11 ng m-3 respectively. The three anhydrosugars had higher and more variable concentrations in the nighttime and during the sugar cane harvest period, due to more intense biomass burning practices. The calculated L/M ratio, which may serve as a signature for sugar cane smoke particles, was 9 ± 5. Although the total concentrations of the anhydrosugars varied greatly among samples, the relative mass size distributions of the saccharides were reasonably constant. Emissions due to biomass burning were estimated to correspond to 69% (mass) of the sugars quantified in the harvest samples, whereas biogenic emissions corresponded to 10%. In the non-harvest period, these values were 44 and 27%, respectively, indicating that biomass burning is an important source of aerosol to the regional atmosphere during the whole year.

  16. 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.

  17. 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.

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

    DOE PAGESBeta

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

    2016-03-22

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

  19. 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

  20. Ergosterol, arabitol and mannitol as tracers for biogenic aerosols in the eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Burshtein, N.; Lang-Yona, N.; Rudich, Y.

    2011-01-01

    Aerosols containing biological components can have a significant effect on human health by causing primarily irritation, infection and allergies. Specifically, airborne fungi can cause a wide array of adverse responses in humans depending on the type and quantity present. In this study we used chemical biomarkers for analyzing fungi-containing aerosols in the eastern Mediterranean region during the year 2009 in order to quantify annual fungal abundances. The prime marker for fungi used in this study was ergosterol, and its concentrations were compared with those of mannitol and arabitol which were recently suggested to also correlate with fungal spores concentrations (Bauer et al., 2008a). Back trajectory analysis, inorganic ions, humidity and temperature were used in an attempt to identify sources as well as the dependence on seasonal and environmental conditions. We found that the ambient concentrations of ergosterol, arabitol and mannitol range between 0 and 2.73 ng m-3, 1.85 and 58.27 ng m-3, 5.57 and 138.03 ng m-3, respectively. The highest levels for all biomarkers were during the autumn, probably from local terrestrial sources, as deduced from the inorganic ions and back trajectory analysis. Significant correlations were observed between arabitol and mannitol during the entire year except for the winter months. Both sugars correlated with ergosterol only during the spring and autumn. We conclude that mannitol and arabitol might not be specific biomarkers for fungi and that the observed correlations during spring and autumn may be attributed to high levels of vegetation during spring blossoms and autumn decomposing.

  1. Ergosterol, arabitol and mannitol as tracers for biogenic aerosols in the Eastern Mediterranean

    NASA Astrophysics Data System (ADS)

    Burshtein, N.; Yona, N. Lang; Rudich, Y.

    2010-11-01

    Aerosols containing biological components can have a significant effect on human health by causing primarily irritation, infection and allergies. Specifically, airborne fungi can cause a wide array of adverse responses in humans depending on the type and quantity present. In this study we used chemical biomarkers for analyzing fungi-containing aerosols in the eastern Mediterranean region during the year 2009 in order to quantify annual fungal abundances. The prime marker for fungi used in this study was ergosterol, and its concentrations were compared with those of mannitol and arabitol, which were recently suggested to also correlate with fungal spores concentrations (Bauer et al., 2008a). Back trajectory analysis, inorganic ions, humidity and temperature were used in an attempt to identify sources as well as the dependence on seasonal and environmental conditions. We found that the ambient concentrations of ergosterol, arabitol and mannitol range between 0 and 2.73 ng m-3, 1.85 and 58.27 ng m-3, 5.57 and 138.03 ng m-3, respectively. The highest levels for all biomarkers were during the autumn, probably from local terrestrial sources, as deduced from the inorganic ions and back trajectory analysis. Significant correlations were observed between arabitol and mannitol during the entire year except for the winter months. Both sugars correlated with ergosterol only during the spring and autumn. We conclude that mannitol and arabitol might not be specific biomarkers for fungi and that the observed correlations during spring and autumn may be attributed to high levels of vegetation during spring blossoms and autumn decomposition.

  2. 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

  3. 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

    The stable carbon isotopes can be used to get information about sources and processing of carbonaceous aerosol. We will present results from source apportionment of carbonaceous aerosol as a function of particle size thermal refractiveness. Separate source apportionment for particles smaller than 200 nm and for different carbon volatility classes are rarely reported and give new insights into aerosol sources in the urban environment. Stable carbon isotope ratios were measured for the organic carbon (OC) fraction and total carbon (TC) of MOUDI impactor samples that were collected on a coastal site (Lithuania) during the winter 2012 and in the city of Vilnius (Lithuania) during the winter of 2009. The 11 impactor stages spanned a size range from 0.056 to 18 μm, but only the 6 stages in the submicron range were analysed. The δ13C values of bulk total carbon (δ13CTC) were determined with an elemental analyser (Flash EA 1112) coupled with an isotope ratio mass spectrometer (Thermo Finnigan Delta Plus Advantage) (EA - IRMS). Meanwhile δ13COC was measured using thermal-desorption isotope ratio mass spectrometry (IRMS) system. This allows a rough separation of the more volatile OC fraction (desorbed in the oven of IRMS up to 250 0C) from the more refractory fraction (desorbed up to 400 0C). In this study we investigated the composition of organic aerosol desorbed from filter samples at different temperatures using the thermal-desorption proton-transfer-reaction mass spectrometry (TD-PTR-MS) technique. During winter-time in Lithuania we expect photochemistry and biogenic emissions to be of minor importance. The main sources of aerosol carbon should be fossil fuel and biomass combustion. In both sites, the coastal and the urban site, δ13C measurements give a clear indication that the source contributions differ for small and large particles. Small particles < 200 nm are depleted in 13C with respect to larger particles by 1 - 2 ‰Ṫhis shows that OC in small particle

  4. Hygroscopic growth of aerosol particles in the Po Valley

    NASA Astrophysics Data System (ADS)

    Svenningsson, I. B.; Hansson, H.-C.; Wiedensohler, A.; Ogren, J. A.; Noone, K. J.; Hallberg, A.

    1992-11-01

    A Tandem Differential Mobility Analyser (TDMA) was used to study the hygroscopic growth of individual ambient aerosol particles in the Po Valley, Italy. The measurements were made during the GCE fog experiment in November 1989. During fog, the interstitial aerosol (Dp(at ambient relative humidity)<5µm) was sampled. Two modes of particles with different hygroscopic growth were found for 0.030µmparticles in the two modes were almost equal. The mean growth factor at 85% r.h. was 1.44±0.14 for the more-hygroscopic mode and 1.1±0.07 for the less-hygroscopic mode. The growth factors and the proportion of the particles that were less hygroscopic varied considerably from day to day, but no significant size dependence was seen. Comparison of growth factors for pure salt particles and the measured growth factors indicates that both hygroscopic modes contain a major insoluble part. The effect of the external mixing of hygroscopic properties on the activation of particles to fog droplets is discussed and the fraction of particles that were activated as a function of particle size is predicted. Comparison with the measured scavenging fraction as a function of particle size shows that the hygroscopic properties of the individual particle are as important as the particle size in determining if it will be activated in a fog.

  5. 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

  6. Molecular Formula Characterization of Biogenic Secondary Organic Aerosol: Descriptive Statistical Evaluation

    NASA Astrophysics Data System (ADS)

    Dalbec, M.; Zhao, Y.; Fisseha, R.; Putman, A.; Kundu, S.; Rahn, T. A.; Mazzoleni, L. R.

    2013-12-01

    The detailed molecular composition of approximately 20 laboratory generated terpene ozonolysis secondary organic aerosol (SOA) samples was studied using ultrahigh resolution Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry. Individual experiments were conducted with one of four terpene SOA precursors (α-pinene, β-pinene, limonene or β-caryophyllene), varied relative humidity (RH) conditions (0%, 4%, or 30%) and the presence or absence of cyclohexane (serving as a radical scavenger). In this work, we focus on the molecular composition of the SOA experiments conducted at 4% and 30% RH without cyclohexane. In each of the experimental SOA samples, the oxygen number and the DBE values increase with increasing carbon number and three or four distinct groups (aka oligomer groups) were observed in the mass spectra. The overall bulk properties, such as the elemental ratios and the average number of double bond equivalents (DBE), of the SOA were highly similar. Despite the high number of identified species (N ≥ 1000) in each SOA sample, compounds unique to the SOA formed at either 4% or 30% RH conditions were comparatively low (< 200). An exception to this was observed for the D-limonene ozonolysis SOA formed at 4% RH conditions where over 450 unique molecular formulas were observed. Due to the similarity in the bulk properties and composition of the SOA from the experiments, multivariate statistics were used to distinguish the experiments from each other. Hierarchical cluster analysis and principal component analysis was performed using the molecular formulas and their relative abundances for all of the identified species. Slight compositional differences between the experiments showed that experiments with the same terpene SOA precursor were most closely related regardless of the RH or the presence/absence of cyclohexane. Furthermore, SOA experiments with D-limonene and β-caryophyllene as precursors were clearly distinguished from β-pinene and

  7. OH-Radical initiated ageing of biogenic secondary organic aerosols - A detailed chemical analysis

    NASA Astrophysics Data System (ADS)

    Müller, L.; Reinnig, M.-C.; Mentel, Th. F.; Tillmann, R.; Schlosser, E.; Wahner, A.; Saathoff, H.; Donahue, N. M.; Hoffmann, T.

    2009-04-01

    The chemical ageing[1] of secondary organic aerosol (SOA) was investigated in two series of experiments using on-line mass spectrometry and off-line high performance liquid chromatography mass spectrometry (HPLC-MS). In a set of photochemical experiments, performed in the large outdoor reaction chamber SAPHIR (Jülich, Germany), SOA was generated from a boreal mixture including mono- and sesquiterpenes (α-pinene, β-pinene, Δ3-carene, limonene, caryophyllene). During a long time experiment (30h) the generated SOA was exposed to OH-radicals and the chemical composition was analyzed on-line using atmospheric pressure ionization mass spectrometry (API-MS). The on-line method provides highly time resolved chemical information and therefore a direct insight into the temporal changes of SOA-composition. In parallel, filter samples analysed by HPLC-MS allow the enrichment of trace compounds and finally an unambiguous identification of individual substances. In addition, filter samples allow a direct comparison to samples from field studies. The ageing experiments showed a clear change in SOA composition. The compounds observed can be divided into two groups: A group of first generation SOA-compounds, generated by the OH oxidation of the terpenes and a group of second generation compounds, generated by the reaction of OH with SOA compounds. Among the second generation products, especially a tricarboxylic acid (3-methyl-1,2,3-butanetricarboxylic acid, m/z 203)[2] was observed to be a good marker compound for BSOA ageing. A further set of experiments was carried out in another large aerosol chamber facility, the AIDA chamber of the Research Centre Karlsruhe. In this dark chamber, the experiments focused on the OH-induced ageing of α-pinene SOA and the influence of temperature. The results clearly show that the tricarboxylic acid is a distinctive marker for OH radical induced BSOA ageing and identify cis-pinonic acid as its precursor. To connect the results of the

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  10. Aerosol and bioaerosol particles in a dental office.

    PubMed

    Polednik, Bernard

    2014-10-01

    This study reports comprehensive aerosol and bioaerosol measurements in a dental office. The highest submicrometer particle concentrations were observed during dental grinding and they were on average 16 times higher than the indoor background. Certain metallic trace elements and total carbon concentrations were significantly elevated (>10 times) in the particles deposited in the operating room. Dental procedures also contributed to increased bacterial contamination that may pose a health risk both for dental personnel and patients. PMID:25218707

  11. Rocket-borne probes for charged mesospheric aerosol particles

    NASA Astrophysics Data System (ADS)

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

    We describe a series of rocket-borne probes for detecting charged solid particles in the ionosphere. The first type of probe is a flat charge-collecting surface on the skin of the rocket. Behind this surface is a permanent magnet that shields the probe from electrons. The current that is recorded is thus from heavier charged aerosol particles. This heavy charge carrier current is converted to a charge number density. A probe launched from White Sands in November 1998 detected a narrow layer at 86 km consistent with sporadic E layer of metallic ions. Two launches were made from the Andoya Rocket Range (Norway) during the MIDAS SOLSTICE campaign in the summer of 2001. Layers of positively and negatively charged aerosol particles were detected on both flights, but inadvertent positive ion collection complicated the analysis. Subsequent payloads included a second probe that supplemented the magnetic field with a positive bias voltage to improve positive ion rejection. Three launches were made from Andoya during the MIDAS MacWAVE campaign in July 2003 with this dual-probe package. Within PMSE, the probes measured an aerosol particle distribution, clearly resolving small positive, small negative, and large negative particles. A new mass-analyzing probe is being developed in which electric fields within the nosecone deflect charged aerosol particles admitted at the nosecone tip. This probe takes advantage of the reduced density behind the shock front to increase the mean free path within the instrument so that cryopumping is not required. The new probe has three pairs of collection surfaces with opposite polarities for collecting (1) electrons and light ions, (2) particles with mass 150-103 amu, and (3) particles with mass 103 -- 2 x 104 amu.

  12. Effective absorption cross sections and photolysis rates of anthropogenic and biogenic secondary organic aerosols

    NASA Astrophysics Data System (ADS)

    Romonosky, Dian E.; Ali, Nujhat N.; Saiduddin, Mariyah N.; Wu, Michael; Lee, Hyun Ji (Julie); Aiona, Paige K.; Nizkorodov, Sergey A.

    2016-04-01

    Mass absorption coefficient (MAC) values were measured for secondary organic aerosol (SOA) samples produced by flow tube ozonolysis and smog chamber photooxidation of a wide range of volatile organic compounds (VOC), specifically: α-pinene, β-pinene, β-myrcene, d-limonene, farnesene, guaiacol, imidazole, isoprene, linalool, ocimene, p-xylene, 1-methylpyrrole, and 2-methylpyrrole. Both low-NOx and high-NOx conditions were employed during the chamber photooxidation experiments. MAC values were converted into effective molecular absorption cross sections assuming an average molecular weight of 300 g/mol for SOA compounds. The upper limits for the effective photolysis rates of SOA compounds were calculated by assuming unity photolysis quantum yields and convoluting the absorption cross sections with a time-dependent solar spectral flux. A more realistic estimate for the photolysis rates relying on the quantum yield of acetone was also obtained. The results show that condensed-phase photolysis of SOA compounds can potentially occur with effective lifetimes ranging from minutes to days, suggesting that photolysis is an efficient and largely overlooked mechanism of SOA aging.

  13. 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

  14. 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.

  15. Ozone reactivity of biogenic volatile organic compound (BVOC) emissions during the Southeast Oxidant and Aerosol Study (SOAS)

    NASA Astrophysics Data System (ADS)

    Park, J.; Guenther, A. B.; Helmig, D.

    2013-12-01

    Recent studies on atmospheric chemistry in the forest environment showed that the total reactivity by biogenic volatile organic compound (BVOC) emission is still not well understood. During summer 2013, an intensive field campaign (Southeast Oxidant and Aerosol Study - SOAS) took place in Alabama, U.S.A. In this study, an ozone reactivity measurement system (ORMS) was deployed for the direct determination of the reactivity of foliage emissions. The ORMS is a newly developed measurement approach, in which a known amount of ozone is added to the ozone-free air sample stream, with the ORMS measuring ozone concentration difference between before and after a glass flask flow tube reaction vessel (2-3 minutes of residence time). Emissions were also collected onto adsorbent cartridges to investigate the discrepancy between total ozone reactivity observation and reactivity calculated from identified BVOC. Leaf and canopy level experiments were conducted by deploying branch enclosures on the three dominant tree species at the site (i.e. liquidambar, white oak, loblolly pine) and by sampling ambient air above the forest canopy. For the branch enclosure experiments, BVOC emissions were sampled from a 70 L Teflon bag enclosure, purged with air scrubbed for ozone, nitrogen oxides. Each branch experiment was performed for 3-5 days to collect at least two full diurnal cycle data. In addition, BVOCs were sampled using glass tube cartridges for 2 hours during daytime and 3 - 4 hours at night. During the last week of campaign, the inlet for the ORMS was installed on the top of scaffolding tower (~30m height). The ozone loss in the reactor showed distinct diurnal cycle for all three tree species investigated, and ozone reactivity followed patterns of temperature and light intensity.

  16. Single particle multichannel bio-aerosol fluorescence sensor.

    PubMed

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

    2005-05-16

    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 ~1mum 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. PMID:19495264

  17. 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.

  18. Specification of Biogenic VOC Emission Data in the Coupled System of Regional Climate and Atmospheric Chemistry/Aerosols Model

    NASA Astrophysics Data System (ADS)

    Zemankova, K.; Huszar, P.

    2009-12-01

    Coupling of regional climate model RegCM (Pal et al., 2007) and atmospheric chemistry/aerosols model CAMx (Environ, 2006) is being developed at our department under the CECILIA project (EC 6th FP) with the aim to study climate forcing due to atmospheric chemistry/aerosols on regional scale. Regional climate model RegCM with the resolution of 10 km drives transport, chemistry and dry/wet deposition of the CAMx model being operated on the Central and Eastern European domain and consequently the radiative active agents from the CAMx model enter the radiative transfer schemes for the calculation of heating rate changes in the regional climate model. In order to increase the accuracy of land cover data in this model system, a new input dataset has been prepared and used for the calculation of emissions of volatile organic compounds (VOCs) from natural sources. This dataset is mainly based on the single tree species database from the european project of JRC in Ispra - Agriculture, Forestry, and Other Land Uses in Europe (AFOLU) which covers most of the model domain. For the locations where AFOLU data were not available, i.e. basically non-EU areas, the USGS Eurasia land cover database has been used. Both databases are available in 1 km resolution. Emission factors for new land cover categories were obtained either from the laboratory measurements or from the literature. The Guenther et al. (1995) model algorithm has been used for the calculation of biogenic VOC (BVOC) emission fluxes. Effects of new land cover and BVOC emission data on the CAMx model simulations of low level ozone in the year 2000 have been studied. Improvement of model results when compared with the measured data may be seen, especially in the simulation of extreme values such as ozone summer maxima. References: - ENVIRON Corp., 2006. CAMx User’s Guide, version 4.40 - Guenther A., Hewitt N., Erickson D., Fall R., Geron Ch., Graedel T., Harley P., Klinger L., Lerdau M., McKay W. A., Pierce T., Scholes

  19. Timescales of water transport in viscous aerosol: measurements on sub-micron particles and dependence on conditioning history.

    PubMed

    Lu, Jessica W; Rickards, Andrew M J; Walker, Jim S; Knox, Kerry J; Miles, Rachael E H; Reid, Jonathan P; Signorell, Ruth

    2014-06-01

    Evaporation studies of single aqueous sucrose aerosol particles as a function of relative humidity (RH) are presented for coarse and fine mode particles down into the submicron size range (600 nm < r < 3.0 μm). These sucrose particles serve as a proxy for biogenic secondary organic aerosols that have been shown to exist, under ambient conditions, in an ultraviscous glassy state, which can affect the kinetics of water mass transport within the bulk phase and hinder particle response to changes in the gas phase water content. A counter-propagating Bessel beams (CPBBs) optical trapping setup is employed to monitor the real-time change in the particle radius with RH decreasing from 75% to 5%. The slow-down of the size change upon each RH step and the deviation from the theoretical equilibrium hygroscopic growth curve indicate the onset of glassy behavior in the RH range of 10-40%. Size-dependent effects were not observed within the uncertainty of the measurements. The influence of the drying time below the glass transition RH on the timescale of subsequent water condensation and re-equilibration for sucrose particles is explored by optical tweezers measurements of micron-sized particles (3 μm < r < 6 μm). The timescale for water condensation and re-equilibration is shown to increase with increasing drying time, i.e. the time over which a viscous particle is dried below 5% RH. These studies demonstrate the importance of the history of the particle conditioning on subsequent water condensation and re-equilibration dynamics of ultraviscous and glassy aerosol particles. PMID:24316593

  20. 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

  1. 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

  2. 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.

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

    PubMed Central

    Buesser, B.; Pratsinis, S.E.

    2013-01-01

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

  4. 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

  5. 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.

  6. 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.

  7. Towards an integrated optical single aerosol particle lab.

    PubMed

    Horstmann, Marcel; Probst, Karl; Fallnich, Carsten

    2012-01-21

    We present a manipulation and characterization system for single airborne particles which is integrated onto a microscope slide. Trapped particles are manipulated by means of radiation pressure and characterized by cavity enhanced Raman spectroscopy. Optical fibers are used to deliver the trapping laser light as well as to collect the Raman scattered light, allowing for a flexible usage of the device. The system features a sample chamber which is separated from an aerosol-flooded injection chamber by means of a light guiding glass-capillary. The coupling of this device with an aerosol optical tweezers setup to selectively load its trapping sites is demonstrated. Finally, a route towards chip-integrated handling and processing of multiple particles is shown and the first results are presented. PMID:22105700

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

    NASA Technical Reports Server (NTRS)

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

    2001-01-01

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

  9. 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

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

    PubMed

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

    2016-08-01

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

  11. The influence of meteoric smoke particles on stratospheric aerosol properties

    NASA Astrophysics Data System (ADS)

    Mann, Graham; Brooke, James; Dhomse, Sandip; Plane, John; Feng, Wuhu; Neely, Ryan; Bardeen, Chuck; Bellouin, Nicolas; Dalvi, Mohit; Johnson, Colin; Abraham, Luke

    2016-04-01

    The ablation of metors in the thermosphere and mesosphere introduces a signficant source of particulate matter into the polar upper stratosphere. These meteoric smoke particles (MSP) initially form at nanometre sizes but in the stratosphere have grown to larger sizes (tens of nanometres) following coagulation. The presence of these smoke particles may represent a significant mechanism for the nucleation of polar stratospheric clouds and are also known to influence the properties of the stratospheric aerosol or Junge layer. In this presentation we present findings from experiments to investigate the influence of the MSP on the Junge layer, carried out with the UM-UKCA composition-climate model. The UM-UKCA model is a high-top (up to 80km) version of the general circulation model with well-resolved stratospheric dynamics, includes the aerosol microphysics module GLOMAP and has interactive sulphur chemistry suitable for the stratosphere and troposphere (Dhomse et al., 2014). We have recently added to UM-UKCA a source of meteoric smoke particles, based on prescribing the variation of the smoke particles from previous simulations with the Whole Atmosphere Community Climate Model (WACCM). In UM-UKCA, the MSP particles are transported within the GLOMAP aerosol framework, alongside interactive stratospheric sulphuric acid aerosol. For the experiments presented here, we have activated the interaction between the MSP and the stratospheric sulphuric acid aerosol. The MSP provide an important sink term for the gas phase sulphuric acid simulated in the model, with subsequent effects on the formation, growth and temporal evolution of stratospheric sulphuric acid aerosol particles. By comparing simulations with and without the MSP-sulphur interactions we quantify the influence of the meteoric smoke on the properties of volcanically-quiescent Junge layer. We also investigate the extent to which the MSP may modulate the effects from SO2 injected into the stratosphere from volcanic

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2011-07-01

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

  14. 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

  15. Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

    NASA Astrophysics Data System (ADS)

    Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

    2014-12-01

    Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photo-oxidation under a range of controlled conditions (relative humidity or RH ~65-89%, volatile organic compound-to-NOx or VOC / NOx ~3-9 and NOx ~2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene but low isoprene emitter, and its emissions were observed to produce measurable amounts of secondary organic aerosol (SOA) via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e. in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photo-oxidation products of the minor volatile organic compounds (VOCs) co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally isoprene-emitting landscapes in Southeast

  16. 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...

  17. Zinc sorption to biogenic hexagonal-birnessite particles within a hydrated bacterial biofilm

    NASA Astrophysics Data System (ADS)

    Toner, Brandy; Manceau, Alain; Webb, Samuel M.; Sposito, Garrison

    2006-01-01

    Biofilm-embedded Mn oxides exert important controls on trace metal cycling in aquatic and soil environments. The speciation and mobility of Zn in particular has been linked to Mn oxides found in streams, wetlands, soils, and aquifers. We investigated the mechanisms of Zn sorption to a biogenic Mn oxide within a biofilm produced by model soil and freshwater Mn II-oxidizing bacteria Pseudomonas putida. The biogenic Mn oxide is a c-disordered birnessite with hexagonal layer symmetry. Zinc adsorption isotherm and Zn and Mn K-edge extended X-ray absorption fine structure (EXAFS) spectroscopy experiments were conducted at pH 6.9 to characterize Zn sorption to this biogenic Mn oxide, and to determine whether the bioorganic components of the biofilm affect metal sorption properties. The EXAFS data were analyzed by spectral fitting, principal component analysis, and linear least-squares fitting with reference spectra. Zinc speciation was found to change as Zn loading to the biosorbent [bacterial cells, extracellular polymeric substances (EPS), and biogenic Mn oxide] increased. At low Zn loading (0.13 ± 0.04 mol Zn kg -1 biosorbent), Zn was sorbed to crystallographically well-defined sites on the biogenic oxide layers in tetrahedral coordination to structural O atoms. The fit to the EXAFS spectrum was consistent with Zn sorption above and below the Mn IV vacancy sites of the oxide layers. As Zn loading increased to 0.72 ± 0.04 mol Zn kg -1 biosorbent, Zn was also detected in octahedral coordination to these sites. Overall, our results indicate that the biofilm did not intervene in Zn sorption by the Mn-oxide because sorption to the organic material was observed only after all Mn vacancy sites were capped by Zn. The organic functional groups present in the biofilm contributed significantly to Zn removal from solution when Zn concentrations exceeded the sorption capacity of the biooxide. At the highest Zn loading studied, 1.50 ± 0.36 mol Zn kg -1 biosorbent, the proportion

  18. Basic biogenic aerosol precursors: Agricultural source attribution of volatile amines revised

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Sintermann, J.; Spirig, C.; Jocher, M.; Ammann, C.; Neftel, A.

    2011-08-01

    Despite recent evidence on an important role of volatile amines in the nucleation of particulate matter, very scarce information is available on their atmospheric abundance and source distribution. Previous measurements in animal housings had identified livestock husbandry as the main amine source, with trimethylamine (TMA) being the key component. This has led to the assumption that the agricultural sources for amines are similar as for ammonia, emitted throughout the cascade of animal excretion, storage and application in the field. In this study, we present the first micrometeorological flux measurements as well as dynamic enclosure experiments showing that the amine source strength from stored slurry is negligible, implying significant consequences for the global amine emission inventory. In the case of cattle, amine production is attributed to the animal's rumination activity and exhalation is suggested to be an important emission pathway, similar to the greenhouse gas methane. Fodder like hay and silage also emits volatile amines, potentially assigning these alkaloid compounds a key function in enhancing particle formation in remote areas.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  20. 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

  1. Emissions of biogenic volatile organic compounds and subsequent photochemical production of secondary organic aerosol in mesocosm studies of temperate and tropical plant species

    NASA Astrophysics Data System (ADS)

    Wyche, K. P.; Ryan, A. C.; Hewitt, C. N.; Alfarra, M. R.; McFiggans, G.; Carr, T.; Monks, P. S.; Smallbone, K. L.; Capes, G.; Hamilton, J. F.; Pugh, T. A. M.; MacKenzie, A. R.

    2014-06-01

    Silver birch (Betula pendula) and three Southeast Asian tropical plant species (Ficus cyathistipula, Ficus benjamina and Caryota millis) from the pantropical fig and palm genera were grown in a purpose-built and environment-controlled whole-tree chamber. The volatile organic compounds emitted from these trees were characterised and fed into a linked photochemical reaction chamber where they underwent photooxidation under a range of controlled conditions (RH ∼65-89%, VOC/NOx ∼3-9 and NOx ∼2 ppbV). Both the gas phase and the aerosol phase of the reaction chamber were monitored in detail using a comprehensive suite of on-line and off-line, chemical and physical measurement techniques. Silver birch was found to be a high monoterpene and sesquiterpene, but low isoprene emitter, and its emissions were observed to produce measureable amounts of SOA via both nucleation and condensation onto pre-existing seed aerosol (YSOA 26-39%). In contrast, all three tropical species were found to be high isoprene emitters with trace emissions of monoterpenes and sesquiterpenes. In tropical plant experiments without seed aerosol there was no measurable SOA nucleation, but aerosol mass was shown to increase when seed aerosol was present. Although principally isoprene emitting, the aerosol mass produced from tropical fig was mostly consistent (i.e., in 78 out of 120 aerosol mass calculations using plausible parameter sets of various precursor specific yields) with condensation of photooxidation products of the minor VOCs co-emitted; no significant aerosol yield from condensation of isoprene oxidation products was required in the interpretations of the experimental results. This finding is in line with previous reports of organic aerosol loadings consistent with production from minor biogenic VOCs co-emitted with isoprene in principally-isoprene emitting landscapes in Southeast Asia. Moreover, in general the amount of aerosol mass produced from the emissions of the principally

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

    PubMed

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

    2016-08-21

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

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

    Energy Science and Technology Software Center (ESTSC)

    1999-07-14

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

  4. The vertical distribution of Martian aerosol particle size

    NASA Astrophysics Data System (ADS)

    Guzewich, Scott D.; Smith, Michael D.; Wolff, Michael J.

    2014-12-01

    Using approximately 410 limb-viewing observations from the Compact Reconnaissance Imaging Spectrometer for Mars (CRISM), we retrieve the vertical distribution of Martian dust and water ice aerosol particle sizes. We find that dust particles have an effective radius of 1.0 µm over much of the atmospheric column below 40 km throughout the Martian year. This includes the detached tropical dust layers detected in previous studies. Little to no variation with height is seen in dust particle size. Water ice clouds within the aphelion cloud belt exhibit a strong sorting of particle size with height, however, and the effective radii range from >3 µm below 20 km to near 1.0 µm at 40 km altitude. Conversely, water ice clouds in the seasonal polar hoods show a near-uniform particle size with an effective radius of approximately 1.5 µm throughout the atmospheric column.

  5. Organic peroxides gas-particle partitioning and rapid heterogeneous decomposition on secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Li, H.; Chen, Z. M.; Huang, L. B.; Huang, D.

    2015-10-01

    Organic peroxides, important species in the atmosphere, will promote secondary organic aerosols (SOA) aging, affect HOx radicals cycling, and cause adverse health effects. However, the formation, gas-particle partitioning, and evolution of organic peroxides are extremely complicated and still unclear. In this study, we investigate in the laboratory the production and gas-particle partitioning of peroxides from the ozonolysis of α-pinene, which is one of the major biogenic volatile organic compounds in the atmosphere and is an important precursor for SOA at a global scale. We have determined the molar yields of hydrogen peroxide (H2O2), hydroxymethyl hydroperoxide (HMHP), peroxyformic acid (PFA), peroxyacetic acid (PAA) and total peroxides (TPO, including unknown peroxides) and the fraction of peroxides in SOA. Comparing the gas-phase and particle-phase peroxides, we find that gas-particle partitioning coefficients of PFA and PAA are 104 times higher than theoretical prediction, indicating that organic peroxides play a more important role in the SOA formation than expected previously. Here, we give the partitioning coefficients of TPO as (2-3) × 10-4 m3μg-1. Even so, more than 80 % of the peroxides formed in the reaction remain in the gas phase. Water does not affect the total amount of peroxides in either the gas or particle phase, but can change the distribution of gaseous peroxides. About 18 % gaseous peroxides undergo rapid heterogeneous decomposition on SOA particles in the presence of water vapor, resulting in the additional production of H2O2. This process can partially interpret the unexpected high H2O2 yield under wet conditions. Transformation of organic peroxides to H2O2 also saves OH in the atmosphere, helping to improve the understanding of OH cycling.

  6. Organic peroxides' gas-particle partitioning and rapid heterogeneous decomposition on secondary organic aerosol

    NASA Astrophysics Data System (ADS)

    Li, Huan; Chen, Zhongming; Huang, Liubin; Huang, Dao

    2016-02-01

    Organic peroxides, important species in the atmosphere, promote secondary organic aerosol (SOA) aging, affect HOx radicals cycling, and cause adverse health effects. However, the formation, gas-particle partitioning, and evolution of organic peroxides are complicated and still unclear. In this study, we investigated in the laboratory the production and gas-particle partitioning of peroxides from the ozonolysis of α-pinene, which is one of the major biogenic volatile organic compounds in the atmosphere and an important precursor for SOA at a global scale. We have determined the molar yields of hydrogen peroxide (H2O2), hydromethyl hydroperoxide (HMHP), peroxyformic acid (PFA), peroxyacetic acid (PAA), and total peroxides (TPOs, including unknown peroxides) and the fraction of peroxides in α-pinene/O3 SOA. Comparing the gas-phase peroxides with the particle-phase peroxides, we find that gas-particle partitioning coefficients of PFA and PAA are 104 times higher than the values from the theoretical prediction, indicating that organic peroxides play a more important role in SOA formation than previously expected. Here, the partitioning coefficients of TPO were determined to be as high as (2-3) × 10-4 m3 µg-1. Even so, more than 80 % of the peroxides formed in the reaction remain in the gas phase. Water changes the distribution of gaseous peroxides, while it does not affect the total amount of peroxides in either the gas or the particle phase. Approx. 18 % of gaseous peroxides undergo rapid heterogeneous decomposition on SOA particles in the presence of water vapor, resulting in the additional production of H2O2. This process can partially explain the unexpectedly high H2O2 yields under wet conditions. Transformation of organic peroxides to H2O2 also preserves OH in the atmosphere, helping to improve the understanding of OH cycling.

  7. 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

  8. 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

  9. Secondary organic aerosol formation from fossil fuel sources contribute majority of summertime organic mass at Bakersfield

    EPA Science Inventory

    Secondary organic aerosols (SOA), known to form in the atmosphere from oxidation of volatile organic compounds (VOCs) emitted by anthropogenic and biogenic sources, are a poorly understood but substantial component of atmospheric particles. In this study, we examined the chemic...

  10. Particle size influences aerosol deposition in guinea pigs during bronchoconstriction

    SciTech Connect

    Praud, J.P.; Macquin-Mavier, I.; Wirquin, V.; Meignan, M.; Harf, A.

    1986-03-01

    The role of two factors determining the deposition of aerosols in the respiratory tract was investigated: the particle size and the nature of the airflow in the airways. An aerosol of Tc99 m-DTPA was generated, with a mass median aerodynamic diameter of either 3 ..mu..m (Bird nebulizer) or 0.5 ..mu..m (Jouan nebulizer). The vehicle was either saline (S) or histamine (H) at a concentration which was previously shown to induce a 50% decrease of specific airway conductance. Spontaneously breathing guinea pigs were exposed during 2 minutes to the aerosol, then killed and the radioactivity in the pharynx, the trachea, the large bronchi and the remaining parenchyma was measured. Results are evaluated as the percentage of total radioactivity in the respiratory tract (mean +/- SEM). Analysis of variance showed that there was a significant difference in the pattern of deposition for large particles (3 ..mu..m) during bronchoconstriction: the more proximal deposition can be ascribed to inertial impaction. Particle size should be clearly defined during histamine challenge in experimental animals.

  11. 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.

  12. The rate of equilibration of viscous aerosol particles

    NASA Astrophysics Data System (ADS)

    O'Meara, Simon; Topping, David O.; McFiggans, Gordon

    2016-04-01

    The proximity of atmospheric aerosol particles to equilibrium with their surrounding condensable vapours can substantially impact their transformations, fate and impacts and is the subject of vibrant research activity. In this study we first compare equilibration timescales estimated by three different models for diffusion through aerosol particles to assess any sensitivity to choice of model framework. Equilibration times for diffusion coefficients with varying dependencies on composition are compared for the first time. We show that even under large changes in the saturation ratio of a semi-volatile component (es) of 1-90 % predicted equilibration timescales are in agreement, including when diffusion coefficients vary with composition. For condensing water and a diffusion coefficient dependent on composition, a plasticising effect is observed, leading to a decreased estimated equilibration time with increasing final es. Above 60 % final es maximum equilibration times of around 1 s are estimated for comparatively large particles (10 µm) containing a relatively low diffusivity component (1 × 10-25 m2 s-1 in pure form). This, as well as other results here, questions whether particle-phase diffusion through water-soluble particles can limit hygroscopic growth in the ambient atmosphere. In the second part of this study, we explore sensitivities associated with the use of particle radius measurements to infer diffusion coefficient dependencies on composition using a diffusion model. Given quantified similarities between models used in this study, our results confirm considerations that must be taken into account when designing such experiments. Although quantitative agreement of equilibration timescales between models is found, further work is necessary to determine their suitability for assessing atmospheric impacts, such as their inclusion in polydisperse aerosol simulations.

  13. Volatility basis-set approach simulation of organic aerosol formation in East Asia: implications for anthropogenic-biogenic interaction and controllable amounts

    SciTech Connect

    Matsui, H.; Koike, Makoto; Kondo, Yutaka; Takami, A.; Fast, Jerome D.; Kanaya, Y.; Takigawa, M.

    2014-09-16

    Organic aerosol (OA) simulations using the volatility basis-set approach were made for East Asia and its outflow region. Model simulations were evaluated through comparisons with OA measured by aerosol mass spectrometers in and around Tokyo (at Komaba and Kisai in summer 2003 and 2004) and over the outflow region in East Asia (at Fukue and Hedo in spring 2009). The simulations with aging processes of organic vapors reasonably well reproduced mass concentrations, temporal variations, and formation efficiency of observed OA at all sites. As OA mass was severely underestimated in the simulations without the aging processes, the oxidations of organic vapors are essential for reasonable OA simulations over East Asia. By considering the aging processes, simulated OA concentrations considerably increased from 0.24 to 1.28 µg m-3 in the boundary layer over the whole of East Asia. OA formed from the interaction of anthropogenic and biogenic sources was also enhanced by the aging processes. The fraction of controllable OA was estimated to be 87 % of total OA over the whole of East Asia, showing that most of the OA in our simulations formed anthropogenically (controllable). A large portion of biogenic secondary OA (78 % of biogenic secondary OA) formed through the influence of anthropogenic sources. The high fraction of controllable OA in our simulations is likely because anthropogenic emissions are dominant over East Asia and OA formation is enhanced by anthropogenic sources and their aging processes. Both the amounts (from 0.18 to 1.12 µg m-3) and the fraction (from 75 % to 87 %) of controllable OA were increased by aging processes of organic vapors over East Asia.

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

    NASA Astrophysics Data System (ADS)

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

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

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

    NASA Technical Reports Server (NTRS)

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

    1980-01-01

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

  16. 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

  17. Physicochemical Characterization of Capstone Depleted Uranium Aerosols I: Uranium Concentration in Aerosols as a Function of Time and Particle Size

    SciTech Connect

    Parkhurst, MaryAnn; Cheng, Yung-Sung; Kenoyer, Judson L.; Traub, Richard J.

    2009-03-01

    During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium 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 the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.

  18. 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...

  19. 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.

  20. Rocket-borne probes for charged ionospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Smiley, B.; Sternovsky, Z.; Robertson, S.; Horanyi, M.

    2003-10-01

    A series of rocket-borne probes is described for detecting charged solid particles in the ionosphere. The probes are flat charge-collecting surfaces on the skin of the rocket that have behind them a permanent magnet that magnetically insulates the probe from electrons. Several probes have also had a small positive bias of several volts to reduce collection of light molecular ions. The current that is recorded is thus from heavier charged particles and this is converted to a charge number density. Several summer launches into the polar mesosphere have found charged aerosol layers at the altitudes of noctilucent clouds and polar summer mesospheric radar echoes. A new probe is being developed in which electric deflection is used to determine the mass of the particles. This probe takes advantage of the reduced density behind the shock front to increase the mean free path within the instrument, so that cryopumping is not required.

  1. Modelling the contribution of biogenic volatile organic compounds to new particle formation in the Jülich plant atmosphere chamber

    NASA Astrophysics Data System (ADS)

    Roldin, P.; Liao, L.; Mogensen, D.; Dal Maso, M.; Rusanen, A.; Kerminen, V.-M.; Mentel, T. F.; Wildt, J.; Kleist, E.; Kiendler-Scharr, A.; Tillmann, R.; Ehn, M.; Kulmala, M.; Boy, M.

    2015-09-01

    We used the Aerosol Dynamics gas- and particle-phase chemistry model for laboratory CHAMber studies (ADCHAM) to simulate the contribution of BVOC plant emissions to the observed new particle formation during photooxidation experiments performed in the Jülich Plant-Atmosphere Chamber and to evaluate how well smog chamber experiments can mimic the atmospheric conditions during new particle formation events. ADCHAM couples the detailed gas-phase chemistry from Master Chemical Mechanism with a novel aerosol dynamics and particle phase chemistry module. Our model simulations reveal that the observed particle growth may have either been controlled by the formation rate of semi- and low-volatility organic compounds in the gas phase or by acid catalysed heterogeneous reactions between semi-volatility organic compounds in the particle surface layer (e.g. peroxyhemiacetal dimer formation). The contribution of extremely low-volatility organic gas-phase compounds to the particle formation and growth was suppressed because of their rapid and irreversible wall losses, which decreased their contribution to the nano-CN formation and growth compared to the atmospheric situation. The best agreement between the modelled and measured total particle number concentration (R2 > 0.95) was achieved if the nano-CN was formed by kinetic nucleation involving both sulphuric acid and organic compounds formed from OH oxidation of BVOCs.

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

    PubMed

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

    2011-01-01

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

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

    PubMed Central

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

    2016-01-01

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

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

    PubMed

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

    2015-01-01

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

  7. Source apportionment of organic compounds in Berlin using positive matrix factorization - assessing the impact of biogenic aerosol and biomass burning on urban particulate matter.

    PubMed

    Wagener, Sandra; Langner, Marcel; Hansen, Ute; Moriske, Heinz-Jörn; Endlicher, Wilfried R

    2012-10-01

    Source apportionment of 13 organic compounds, elemental carbon and organic carbon of ambient PM(10) and PM(1) was performed with positive matrix factorization (PMF). Samples were collected at three sites characterized by different vegetation influences in Berlin, Germany in 2010. The aim was to determine organic, mainly biogenic sources and their impact on urban aerosol collected in a densely populated region. A 6-factor solution provided the best data fit for both PM-fractions, allowing the sources isoprene- and α-pinene-derived secondary organic aerosol (SOA), bio primary, primarily attributable to fungal spores, bio/urban primary including plant fragments in PM(10) and cooking and traffic emissions in PM(1), biomass burning and combustion fossil to be identified. With mean concentrations up to 2.6 μg Cm(-3), biomass burning dominated the organic fraction in cooler months. Concentrations for α-pinene-derived SOA exceeded isoprene-derived concentrations. Estimated secondary organic carbon contributions to total organic carbon (OC) were between 7% and 42% in PM(10) and between 11% and 60% in PM(1), which is slightly lower than observed for US- or Asian cities. Primary biogenic emissions reached up to 33% of OC in the PM(10)-fraction in the late summer and autumn months. Temperature-dependence was found for both SOA-factors, correlations with ozone and mix depth only for the α-pinene-derived SOA-factor. Latter indicated input of α-pinene from the borders, highlighting differences in the origin of the precursors of both factors. Most factors were regionally distributed. High regional distribution was found to be associated with stronger influence of ambient parameters and higher concentrations at the background station. A significant contribution of biogenic emissions and biomass burning to urban organic aerosol could be stated. This indicates a considerable impact on PM concentrations also in cities in a densely populated area, and should draw the attention

  8. Morphology and Optical Properties of Mixed Aerosol Particles

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

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

    PubMed Central

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

    2011-01-01

    Organic substances can adopt an amorphous solid or semisolid state, influencing the rate of heterogeneous reactions and multiphase processes in atmospheric aerosols. Here we demonstrate how molecular diffusion in the condensed phase affects the gas uptake and chemical transformation of semisolid organic particles. Flow tube experiments show that the ozone uptake and oxidative aging of amorphous protein is kinetically limited by bulk diffusion. The reactive gas uptake exhibits a pronounced increase with relative humidity, which can be explained by a decrease of viscosity and increase of diffusivity due to hygroscopic water uptake transforming the amorphous organic matrix from a glassy to a semisolid state (moisture-induced phase transition). The reaction rate depends on the condensed phase diffusion coefficients of both the oxidant and the organic reactant molecules, which can be described by a kinetic multilayer flux model but not by the traditional resistor model approach of multiphase chemistry. The chemical lifetime of reactive compounds in atmospheric particles can increase from seconds to days as the rate of diffusion in semisolid phases can decrease by multiple orders of magnitude in response to low temperature or low relative humidity. The findings demonstrate that the occurrence and properties of amorphous semisolid phases challenge traditional views and require advanced formalisms for the description of organic particle formation and transformation in atmospheric models of aerosol effects on air quality, public health, and climate. PMID:21690350

  10. Contributions of Biogenic and Anthropogenic Hydrocarbons to Secondary Organic Aerosol during 2006 in Research Triangle Park, NC

    EPA Science Inventory

    A recently developed, organic tracer-based method was used to estimate the secondary contributions of biogenic and anthropogenic precursor hydrocarbons to ambient organic carbon concentrations in PM2.5 during 2006 in Research Triangle Park, North Carolina, USA. Forty-s...

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

    DOEpatents

    Novick, Vincent J.

    1998-01-01

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

  12. 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.

  13. 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.

  14. Exploring Atmospheric Aerosol Chemistry with Advanced High-Resolution Mass Spectrometry and Particle Imaging Methods

    NASA Astrophysics Data System (ADS)

    Nizkorodov, S.

    2014-12-01

    Physical and chemical complexity of atmospheric aerosols presents significant challenges both to experimentalists working on aerosol characterization and to modelers trying to parameterize critical aerosol properties. Multi-modal approaches that combine state-of-the-art experimental, theoretical, and modeling methods are becoming increasingly important in aerosol research. This presentation will discuss recent applications of unique high-resolution mass spectrometry and particle imaging tools developed at two Department of Energy's user facilities, the Environmental Molecular Science Laboratory (EMSL) and Advanced Light Source (ALS), to studies of molecular composition, photochemical aging, and properties of laboratory-generated and field aerosols. Specifically, this presentation will attempt to address the following questions: (a) how do NO2, SO2, and NH3 affect molecular level composition of anthropogenic aerosols?; (b) what factors determine viscosity/surface tension of organic aerosol particles?; (c) how does photolysis affect molecular composition and optical properties of organic aerosols?

  15. 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.

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

    DOEpatents

    Novick, V.J.

    1998-10-06

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

  17. Real-time chemical analysis of aerosol particles

    SciTech Connect

    Yang, M.; Whitten, W.B.; Ramsey, J.M.

    1995-04-01

    An important aspect of environmental atmospheric monitoring requires the characterization of airborne microparticles and aerosols. Unfortunately, traditional sample collection and handling techniques are prone to contamination and interference effects that can render an analysis invalid. These problems can be avoided by using real-time atmospheric sampling techniques followed by immediate mass spectrometric analysis. The former is achieved in these experiments via a two state differential pumping scheme that is attached directly to a commercially available quadruple ion trap mass spectrometer. Particles produced by an external particle generator enter the apparatus and immediately pass through two cw laser/fiberoptic based detectors positioned two centimeters apart. Timing electronics measure the time between detection events, estimate the particles arrival in the center of the ion trap and control the firing of a YAG laser. Ions produced when the UV laser light ablates the particle`s surface are stored by the ion trap for mass analysis. Ion trap mass spectrometers have several advantages over conventional time-of-flight instruments. First, they are capable of MS/MS analysis by the collisional dissociation of a stored species, This permits complete chemical characterization of airborne samples. Second, ion traps are small and lend themselves to portable, field oriented applications.

  18. 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.

  19. On the Importance of Organic Oxygen for Understanding OrganicAerosol Particles

    SciTech Connect

    Pang, Y.; Turpin, B.J.; Gundel, L.A.

    2005-04-01

    This study shows how aerosol organic oxygen data could provide new information about organic aerosol mass, aqueous solubility of organic aerosols, formation of secondary organic aerosol (SOA) and the relative contributions of anthropogenic and biogenic sources. For more than two decades atmospheric aerosol organic mass (OM) concentration has been estimated by multiplying the measured carbon content by an assumed (OM)-to-organic carbon (OC) factor, usually 1.4. However, this factor can vary from 1.0 to 2.5 depending on location. This large uncertainty about aerosol organic mass limits our understanding of the influence of organic aerosol on climate, visibility and health. New examination of organic aerosol speciation data shows that the oxygen content is responsible for the observed range in the OM-to-OC factor. When organic oxygen content is excluded, the ratio of non-oxygen organic mass to carbon mass varies very little across different environments (1.12 to 1.14). The non-oxygen-OM-to-OC factor for all studied sites (urban and non-urban) averaged 1.13. The uncertainty becomes an order of magnitude smaller than the uncertainty in the best current estimates of organic mass to organic carbon ratios (1.6 {+-} 0.2 for urban and 2.1 {+-} 0.2 for non-urban areas). This analysis suggests that, when aerosol organic oxygen data become available, organic aerosol mass can be quite accurately estimated using just OC and organic oxygen (OO) without the need to know whether the aerosol is fresh or aged. In addition, aerosol organic oxygen data will aid prediction of water solubility since compounds with OO-to-OC higher than 0.4 have water solubilities higher than 1 g per 100 g water.

  20. 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

  1. 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.

  2. Secondary Organic Aerosol Formation from Glyoxal: Effects of Seed Aerosol on Particle Composition

    NASA Astrophysics Data System (ADS)

    Slowik, Jay; Waxman, Eleanor; Coburn, Sean; Klein, Felix; Koenig, Theodore; Krapf, Manuel; Kumar, Nivedita; Wang, Siyuan; Baltensperger, Urs; Dommen, Josef; Prévôt, Andre; Volkamer, Rainer

    2014-05-01

    Conventional models of secondary organic aerosol (SOA) production neglect aqueous-phase processing mechanisms, thereby excluding potentially important SOA formation pathways. These missing pathways may be an important factor in the inability of current models to fully explain SOA yields and oxidation states. Molecules identified as important precursors to SOA generated through aqueous-phase include glyoxal, which is an oxidation product of numerous organic gases. Glyoxal SOA formation experiments were conducted in the PSI smog chamber as a function of seed composition, relative humidity (RH, 60 to 85%), and the presence/absence of gaseous ammonia, affecting particle acidity. In a typical experiment, the chamber was filled with the selected seed aerosol (NaCl, (NH4)2SO4, NaNO3, or K2SO4), after which glyoxal was generated by the brief (i.e. a few minutes) exposure of acetylene to UV light. The experiment was then allowed to proceed undisturbed for several hours. Each experiment consisted of several UV exposures, followed by a dilution phase at constant RH to investigate the gas/particle partitioning behavior of the generated SOA. Gas-phase glyoxal was monitored by an LED-CE-DOAS system, while the particle composition was measured using online aerosol mass spectrometry (Aerodyne HR-ToF-AMS) and offline analysis of collected filter samples. SOA composition was observed to depend strongly on seed type, with increased imidazole formation evident during experiments with (NH4)2SO¬4 and K2SO4 seeds relative to those with NaCl and NaNO3. Additionally, experiments conducted in the presence of ammonia showed large enhancements in both imidazole content and total SOA yield. Analysis of mass spectral markers indicates reversible uptake of glyoxal but irreversible particle-phase production of the imidazole-containing SOA. Positive matrix factorization (PMF) using the Multilinear Engine (ME-2) was applied to the AMS mass spectral time series to quantify factors related to

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  4. Identification and quantification of individual chemical compounds in biogenic secondary organic aerosols using GCxGC-VUV/EI-HRTOFMS

    NASA Astrophysics Data System (ADS)

    Decker, M.; Worton, D. R.; Isaacman, G. A.; Chan, A. W.; Ruehl, C.; Zhao, Y.; Wilson, K. R.; Goldstein, A. H.

    2012-12-01

    Atmospheric aerosols have adverse effects on human health and air quality and affect radiative forcing and thus climate. While the organic fraction of aerosols is substantial, the sources and chemistry leading to the formation of secondary organic aerosols are very poorly understood. Characterizing individual compounds present in organic aerosol provides insights into the sources, formation mechanisms and oxidative transformations that have taken place. Fifteen aerosol samples collected over a 5 day period at the Blodgett Forest Research Station in the Sierra Nevada Mountains, part of the Biosphere Effects on Aerosols and Photochemistry Experiment (BEARPEX) in July 2009, were analyzed using comprehensive two dimensional gas chromatography with high resolution time of flight mass spectrometry (GCxGC-HRTOFMS). Approximately 600 compounds were observed in each sample as significant peaks in the chromatogram. Of these, around a third were identified by matching the unique electron ionization (EI) mass spectrum of each compound to the NIST library of characteristic fragmentation patterns. One filter sample was also analyzed using vacuum ultraviolet ionization (VUV) instead of EI. This 'soft' ionization technique results in much less fragmentation yielding the molecular ion of each compound, from which the exact mass was determined. If the formula of the EI library matched compound equaled the high mass resolution VUV molecular weight within a certain tolerance (< 30 ppm), then the library match was considered confirmed; 226 compounds were identified in this way. Using the VUV technique 234 additional compounds that were not in the EI mass spectral database were assigned chemical formulas based on the observed molecular weights. The chemical formulas in conjunction with the location of the compound in the GCxGC chromatogram were used to provide further classification of these compounds based on their likely functionalization. The broad array of observed oxygenated

  5. 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.

  6. Sources of Size Segregated Sulfate Aerosols in the Arctic Summer

    NASA Astrophysics Data System (ADS)

    Ghahremaninezhadgharelar, R.; Norman, A. L.; Abbatt, J.; Levasseur, M.

    2015-12-01

    Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor fitted to a high volume sampler was used for this study and was modified to permit collection of SO2 after aerosols were removed from the gas stream. The isotopic composition of sulfate aerosols and SO2 was measured and apportionment calculations have been performed to quantify the contribution of biogenic as well as anthropogenic sources to the growth of different aerosol size fractions in the atmosphere. The presence of sea salt sulfate aerosols was especially high in coarse mode aerosols as expected. The contribution of biogenic sulfate concentration in this study was higher than anthropogenic sulfate. Around 70% of fine aerosols (<0.49 μm) and 86% of SO2 were from biogenic sources. Concentrations of biogenic sulfate for fine aerosols, ranging from 18 to 625 ng/m3, were five times higher than total biogenic sulfate concentrations measured during Fall in the same region (Rempillo et al., 2011). A comparison of the isotope ratio for SO2 and fine aerosols offers a way to determine aerosol growth from local SO2 oxidation. For some samples, the values for SO2 and fine aerosols were close together suggesting the same source for SO2 and aerosol sulfur.Aerosols drive significant radiative forcing and affect Arctic climate. Despite the importance of these particles in Arctic climate change, there are some key uncertainties in the estimation of their effects and sources. Aerosols in six size fractions between <0.49 to 7.0 microns in diameter were collected on board the Canadian Coast Guard Ship (CCGS) Amundsen in the Arctic, during July 2014. A cascade impactor

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

    PubMed

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

    2013-12-17

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

  8. 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

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

    SciTech Connect

    Sheridan, P.J.

    1986-01-01

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

  10. Beyond single particle mass spectrometry: multidimensional characterisation of individual aerosol particles

    SciTech Connect

    Zelenyuk, Alla; Imre, D.

    2009-09-10

    The behavior of small aerosol particles depends on a number of their physical and chemical properties, many of which are strongly coupled. The size, internal composition, density, shape, morphology, hygroscopicity, index of refraction, activity as cloud condensation nuclei and ice nuclei, and other attributes of individual particles - all play a role in determining particle properties and their impacts. The traditional particle characterization approaches rely on separate parallel measurements that average over an ensemble of particles of different sizes and/or compositions and later attempt to draw correlations between them. As a result such studies overlook critical differences between particles and bulk and miss the fact that individual particles often exhibit major differences. Here we review the recently developed methods to simultaneously measure in-situ and in real time several of the attributes for individual particles using single particle mass spectrometer, SPLAT or its second generation SPLAT II. We also discuss novel approaches developed for classification, visualization and mining of large datasets produced by the multidimensional single particle characterization.

  11. Water uptake by organic aerosol and its influence on gas/particle partitioning of secondary organic aerosol in the United States

    NASA Astrophysics Data System (ADS)

    Jathar, Shantanu H.; Mahmud, Abdullah; Barsanti, Kelley C.; Asher, William E.; Pankow, James F.; Kleeman, Michael J.

    2016-03-01

    Organic aerosol (OA) is at least partly hygroscopic, i.e., water partitions into the organic phase to a degree determined by the relative humidity (RH), the organic chemical composition, and the particle size. This organic-phase water increases the aerosol mass and provides a larger absorbing matrix while decreasing its mean molecular weight, which can encourage additional condensation of semi-volatile organic compounds. Most regional and global atmospheric models account for water uptake by inorganic salts but do not explicitly account for organic-phase water and its subsequent impact on gas/particle partitioning of semi-volatile OA. In this work, we incorporated the organic-phase water model described by Pankow et al. (2015) into the UCD/CIT air quality model to simulate water uptake by OA and assessed its influence on total OA mass concentrations. The model was run for one summer month over two distinct regions: South Coast Air Basin (SoCAB) surrounding Los Angeles, California and the eastern United States (US). In SoCAB where the OA was dominated by non-hygroscopic primary OA (POA), there was very little organic-phase water uptake (0.1-0.2 μg m-3) and consequently very little enhancement (or growth) in total OA concentrations (OA + organic-phase water): a 3% increase in total OA mass was predicted for a 0.1 increase in relative humidity. In contrast, in the eastern US where secondary OA (SOA) from biogenic sources dominated the OA, substantial organic-phase water uptake and enhancement in total OA concentrations was predicted, even in urban locations. On average, the model predicted a 20% growth in total OA mass for a 0.1 increase in relative humidity; the growth was equivalent to a 250 nm particle with a hygroscopicity parameter (κ) of 0.15. Further, for the same relative humidity, the exact extent of organic-phase water uptake and total OA enhancement was found to be dependent on the particle mixing state. When the source-oriented mixing state of aerosols

  12. High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

    SciTech Connect

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

    2010-10-01

    This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities, types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.

  13. Detection and characterization of biological and other organic-carbon aerosol particles in atmosphere using fluorescence

    NASA Astrophysics Data System (ADS)

    Pan, Yong-Le

    2015-01-01

    This paper offers a brief review on the detection and characterization of biological and other organic-carbon (OC) aerosol particles in atmosphere using laser-induced-fluorescence (LIF) signatures. It focuses on single individual particles or aggregates in the micron and super-micron size range when they are successively drawn through the interrogation volume of a point detection system. Related technologies for these systems that have been developed in last two decades are also discussed. These results should provide a complementary view for studying atmospheric aerosol particles, particularly bioaerosol and OC aerosol particles from other analytical technologies.

  14. 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

  15. In situ Measurements of Gas- and Particle-Phase Organic Compounds: Insights for SOA Formation Mechanisms and Contributions of SOA to Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Zhao, Y.; Kreisberg, N. M.; Worton, D. R.; Isaacman, G. A.; Weber, R.; Liu, S.; Day, D. A.; Markovic, M. Z.; VandenBoer, T. C.; Russell, L. M.; Murphy, J. G.; Hering, S. V.; Goldstein, A. H.

    2011-12-01

    To investigate formation of secondary organic aerosol (SOA) and the contribution of SOA to organic aerosols, semi-volatile and intermediate-volatile organic compounds (SVOCs/IVOCs) in both gas and particle phases were measured using a modified Thermal Desorption Gas Chromatograph (TAG) instrument in Bakersfield, CA during the CALifornia at the NEXus between air quality and climate (CALNEX) campaign from 31 May through 27 June, 2010. More than 150 organic compounds were identified, spanning a wide range of volatility and functionality. Quantified compounds included organic tracers for primary and secondary organic sources, such as alkanes, PAHs, acids, hopanes and ketones. Hourly gas/particle partitioning was determined by a denuder difference method where the sample flow alternated every other sample through an active charcoal multi-channel denuder that efficiently removed gas-phase components. Gas/particle partitioning of three SOA tracers (phthalic acid, pinonaldehyde and 6, 10, 14-trimethyl-2-pentadecanone) was investigated to understand the formation mechanisms of SOA for different functional group classes in the ambient atmosphere. Comparison with Pankow gas/particle partitioning theory, observed particle-phase phthalic acid and pinonaldehyde, suggests formation by other mechanisms than gas-to-particle condensation. Source attribution is performed using Positive Matrix Factorization (PMF) analysis of speciated particle-phase TAG data along with total submicron organic aerosol (OA) measured by an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS). SOA accounts for a major component of OA and the contribution of biogenic SOA to total SOA is comparable to anthropogenic SOA during nights.

  16. AMS Measurements in National Parks of Aerosol Mass, Size and Composition, Comparison with Filter Samples and Correlation with Particle Hygroscopicity and Optical Extinction Properties

    NASA Astrophysics Data System (ADS)

    Alexander, M.; Taylor, N. F.; Collins, D. R.; Kumar, N.; Allen, J.; Newburn, M.; Lowenthal, D. H.; Zielinska, B.

    2011-12-01

    We report a comparison of results from aerosol studies at Great Smoky Mountain National Park (2006), Mt. Rainier National Park (2009) and Acadia National Park (2011), all class I visibility areas associated with IMPROVE (Interagency Monitoring of Protected Visual Environments) sites. This collaborative study was sponsored by the Electric Power Research Institute (EPRI) and was done with the cooperation of the National Park Service and the EPA. The atmospheric aerosol composition in these sites is influenced by a number of anthropogenic as well as biogenic sources, providing a rich environment for fundamental aerosol studies. The primary purpose of these studies was to add state-of-the-art aerosol instrumentation to the standard light extinction and aerosol measurements at the site, used to determine parameters for the IMPROVE light extinction reconstruction equation, adopted by the EPA to estimate light extinction from atmospheric aerosol concentrations and Rayleigh scattering. The combination of these diverse measurements also provides significant insight into fundamental aerosol properties such as aging and radiative forcing. New instrumentation included a quadrupole aerosol mass spectrometer (Aerodyne Q-AMS-Smoky Mountain Study), a high resolution aerosol time-of-flight mass spectrometer (Aerodyne HR-ToF-AMS - Mt. Rainier and Acadia studies) for real time measurements that directly address the relationship between sulfate, nitrate, and OC size and concentration, which is related to cloud and dry gas-to-particle conversion as air masses age during transport, the relationship between WSOC hygroscopic growth and oxygenated organic (OOA) composition, the OCM/OC ratio, and the chemical composition that determines the ambient hygroscopic state. The OCM/OC ratio and organic water uptake was addressed with high-volume and medium volume PM2.5 aerosol samples. Aerosols were collected daily on Teflon coated glass fiber filters (TGFF) in four high-volume PM2.5 samplers

  17. 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.

  18. Sizing of individual aerosol particles using TAOS (Two-dimensional Angular Optical Scattering) pattern total intensity

    NASA Astrophysics Data System (ADS)

    Zallie, J. T.; Aptowicz, K. B.; Martin, S.; Pan, Y.

    2015-12-01

    The morphology of single aerosol particles has been explored previously using the TAOS (Two-dimensional Angular Optical Scattering) technique, which captures angularly resolved scattering patterns. Particle size is known to strongly influence the light scattering properties of aerosols and therefore is a critical parameter to discern from the TAOS patterns. In this work, T-matrix simulation of light scattering from spherical and spheroidal particles is used to explore the possibility of sizing particles from the total light scattering signal detected using the TAOS technique. Scattering patterns were calculated for particles that span various particle sizes, spheroidal shapes, complex refractive indices and particles orientations representative of atmospheric aerosol distributions. A power law relationship between particle size and total scattering intensity was found that could crudely size particles but with significant error.

  19. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions

    NASA Astrophysics Data System (ADS)

    Guenther, A. B.; Jiang, X.; Heald, C. L.; Sakulyanontvittaya, T.; Duhl, T.; Emmons, L. K.; Wang, X.

    2012-06-01

    The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of 147 biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface models and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0 for isoprene emissions and MEGAN2.04, which estimates emissions of 138 compounds. Isoprene comprises about half of the estimated total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g). Another 10 compounds including methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the estimated emission. An additional 20 compounds (mostly terpenoids) are associated with another 17% of the total emission with the remaining 3% distributed among 125 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for 60% of terpenoid emissions and 48% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to landcover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from http://acd.ucar.edu/~guenther/MEGAN/MEGAN.htm and the version integrated into the Community Land Model version 4 (CLM4) can

  20. The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1): an extended and updated framework for modeling biogenic emissions

    NASA Astrophysics Data System (ADS)

    Guenther, A. B.; Jiang, X.; Heald, C. L.; Sakulyanontvittaya, T.; Duhl, T.; Emmons, L. K.; Wang, X.

    2012-11-01

    The Model of Emissions of Gases and Aerosols from Nature version 2.1 (MEGAN2.1) is a modeling framework for estimating fluxes of biogenic compounds between terrestrial ecosystems and the atmosphere using simple mechanistic algorithms to account for the major known processes controlling biogenic emissions. It is available as an offline code and has also been coupled into land surface and atmospheric chemistry models. MEGAN2.1 is an update from the previous versions including MEGAN2.0, which was described for isoprene emissions by Guenther et al. (2006) and MEGAN2.02, which was described for monoterpene and sesquiterpene emissions by Sakulyanontvittaya et al. (2008). Isoprene comprises about half of the total global biogenic volatile organic compound (BVOC) emission of 1 Pg (1000 Tg or 1015 g) estimated using MEGAN2.1. Methanol, ethanol, acetaldehyde, acetone, α-pinene, β-pinene, t-β-ocimene, limonene, ethene, and propene together contribute another 30% of the MEGAN2.1 estimated emission. An additional 20 compounds (mostly terpenoids) are associated with the MEGAN2.1 estimates of another 17% of the total emission with the remaining 3% distributed among >100 compounds. Emissions of 41 monoterpenes and 32 sesquiterpenes together comprise about 15% and 3%, respectively, of the estimated total global BVOC emission. Tropical trees cover about 18% of the global land surface and are estimated to be responsible for ~80% of terpenoid emissions and ~50% of other VOC emissions. Other trees cover about the same area but are estimated to contribute only about 10% of total emissions. The magnitude of the emissions estimated with MEGAN2.1 are within the range of estimates reported using other approaches and much of the differences between reported values can be attributed to land cover and meteorological driving variables. The offline version of MEGAN2.1 source code and driving variables is available from

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  2. 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...

  3. Modelling the contribution of biogenic VOCs to new particle formation in the Jülich plant atmosphere chamber

    NASA Astrophysics Data System (ADS)

    Liao, L.; Dal Maso, M.; Mogensen, D.; Roldin, P.; Rusanen, A.; Kerminen, V.-M.; Mentel, T. F.; Wildt, J.; Kleist, E.; Kiendler-Scharr, A.; Tillmann, R.; Ehn, M.; Kulmala, M.; Boy, M.

    2014-11-01

    We used the MALTE-BOX model including near-explicit air chemistry and detailed aerosol dynamics to study the mechanisms of observed new particle formation events in the Jülich Plant Atmosphere Chamber. The modelled and measured H2SO4 (sulfuric acid) concentrations agreed within a factor of two. The modelled total monoterpene concentration was in line with PTR-MS observations, and we provided the distributions of individual isomers of terpenes, when no measurements were available. The aerosol dynamic results supported the hypothesis that H2SO4 is one of the critical compounds in the nucleation process. However, compared to kinetic H2SO4 nucleation, nucleation involving OH oxidation products of monoterpenes showed a better agreement with the measurements, with R2 up to 0.97 between modelled and measured total particle number concentrations. The nucleation coefficient for kinetic H2SO4 nucleation was 2.1 × 10-11 cm3 s-1, while the organic nucleation coefficient was 9.0 × 10-14 cm3 s-1. We classified the VOC oxidation products into two sub-groups including extremely low-volatility organic compounds (ELVOCs) and semi-volatile organic compounds (SVOCs). These ELVOCs and SVOCs contributed approximately equally to the particle volume production, whereas only ELVOCs made the smallest particles to grow in size. The model simulations revealed that the chamber walls constitute a major net sink of SVOCs on the first experiment day. However, the net wall SVOC uptake was gradually reduced because of SVOC desorption during the following days. Thus, in order to capture the observed temporal evolution of the particle number size distribution, the model needs to consider reversible gas-wall partitioning.

  4. Reactive uptake of HOCl to laboratory generated sea salt particles and nascent sea-spray aerosol

    NASA Astrophysics Data System (ADS)

    Campbell, N. R.; Ryder, O. S.; Bertram, T. H.

    2013-12-01

    Field observations suggest that the reactive uptake of HOCl on marine aerosol particles is an important source of chlorine radicals, particularly under low NOx conditions. However to date, laboratory measurements disagree on the magnitude of the reactive uptake coefficient for HOCl by a factor of 5 (γ(HOCl) ranges between 0.0004 and 0.0018), and there are no measurements of γ(HOCl) on nascent sea-spray aerosol. Here, we present measurements of the reactive uptake of HOCl to laboratory generated sodium chloride and sea-spray aerosol particles generated in a novel Marine Aerosol Reference Tank (MART), coupled to an entrained aerosol flow reactor and Chemical Ionization Mass Spectrometer (CIMS). Measurements of γ(HOCl) retrieved here are compared against those in the literature, and the role of organic coatings on nascent sea-spray aerosol is explored.

  5. CRYSTAL GROWTH. Crystallization by particle attachment in synthetic, biogenic, and geologic environments.

    PubMed

    De Yoreo, James J; Gilbert, Pupa U P A; Sommerdijk, Nico A J M; Penn, R Lee; Whitelam, Stephen; Joester, Derk; Zhang, Hengzhong; Rimer, Jeffrey D; Navrotsky, Alexandra; Banfield, Jillian F; Wallace, Adam F; Michel, F Marc; Meldrum, Fiona C; Cölfen, Helmut; Dove, Patricia M

    2015-07-31

    Field and laboratory observations show that crystals commonly form by the addition and attachment of particles that range from multi-ion complexes to fully formed nanoparticles. The particles involved in these nonclassical pathways to crystallization are diverse, in contrast to classical models that consider only the addition of monomeric chemical species. We review progress toward understanding crystal growth by particle-attachment processes and show that multiple pathways result from the interplay of free-energy landscapes and reaction dynamics. Much remains unknown about the fundamental aspects, particularly the relationships between solution structure, interfacial forces, and particle motion. Developing a predictive description that connects molecular details to ensemble behavior will require revisiting long-standing interpretations of crystal formation in synthetic systems, biominerals, and patterns of mineralization in natural environments. PMID:26228157

  6. 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.

  7. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  9. 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.

  10. X-RAY FLUORESCENCE ANALYSIS OF FILTER-COLLECTED AEROSOL PARTICLES

    EPA Science Inventory

    X-ray fluorescence (XRF) has become an effective technique for determining the elemental content of aerosol samples. For quantitative analysis, the aerosol particles must be collected as uniform deposits on the surface of Teflon membrane filters. An energy dispersive XRF spectrom...

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

    PubMed

    Xie, Mike; Waring, Michael T

    2015-08-01

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

  12. TIME-OF-FLIGHT AEROSOL BEAM SPECTROMETER FOR PARTICLE SIZE MEASUREMENTS

    EPA Science Inventory

    A time-of-flight aerosol beam spectrometer (TOFABS) is described. The instrument has been designed and constructed to perform in situ real time measurements of the aerodynamic size of individual aerosol particles in the range 0.3 to 10 micrometers diameter. The measurement method...

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

    PubMed Central

    Zhang, Chao; Zhu, Rong; Yang, Wenming

    2016-01-01

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

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

    PubMed

    Zhang, Chao; Zhu, Rong; Yang, Wenming

    2016-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2012-01-01

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

  16. Carbon in southeastern U.S. aerosol particles: Empirical estimates of secondary organic aerosol formation

    NASA Astrophysics Data System (ADS)

    Blanchard, Charles L.; Hidy, George M.; Tanenbaum, Shelley; Edgerton, Eric; Hartsell, Benjamin; Jansen, John

    Fine particles in the southeastern United States are rich in carbon: Southeastern Aerosol Research and Characterization (SEARCH) network measurements from 2001 through 2004 indicate that fine particles less than 2.5 μm aerodynamic diameter (PM 2.5) at two inland urban sites, Atlanta, GA and Birmingham, AL, contain 9 and 11% black carbon (BC) by mass, respectively, on average. For neighboring rural or urban Gulf Coast sites, the range is 4-7% BC. Organic carbon (OC) ranges from 25 to 27% in the inland cities, and 19-24% at the rural or Gulf Coast locations. Evidence in the literature suggests that a substantial fraction of the OC found in the Southeast is produced by atmospheric chemical reactions of volatile organic compounds (VOCs). Estimation of the fraction of OC from primary and secondary sources is difficult from first principles, because the chemistry is complex and incompletely understood, and the emission sources are both anthropogenic and natural. As an alternative, measurement-based models can be used to estimate empirically the primary and secondary source contributions. Three complementary empirical models are described and applied using the SEARCH database. The methods include (a) a multiple regression model employing markers for primary and secondary carbon using gas and particle data, (b) a carbon mass balance using carbon and CO data, along with certain assumptions about the OC/CO ratios in primary emissions for different urban and rural conditions, and (c) exploitation of isotopic measurements of carbon along with the BC and OC data. Secondary organic carbon (SOC) represents ˜20-60% of mean OC, depending upon location and season. The results are sensitive to estimates of emissions of primary OC and BC.

  17. Effect of Hydrophobic Primary Organic Aerosols on Secondary Organic Aerosol Formation from Ozonolysis of α-Pinene

    SciTech Connect

    Song, Chen; Zaveri, Rahul A.; Alexander, M. Lizabeth; Thornton, Joel A.; Madronich, Sasha; Ortega, John V.; Zelenyuk, Alla; Yu, Xiao-Ying; Laskin, Alexander; Maughan, A. D.

    2007-10-16

    Semi-empirical secondary organic aerosol (SOA) models typically assume a well-mixed organic aerosol phase even in the presence of hydrophobic primary organic aerosols (POA). This assumption significantly enhances the modeled SOA yields as additional organic mass is made available to absorb greater amounts of oxidized secondary organic gases than otherwise. We investigate the applicability of this critical assumption by measuring SOA yields from ozonolysis of α-pinene (a major biogenic SOA precursor) in a smog chamber in the absence and in the presence of dioctyl phthalate (DOP) and lubricating oil seed aerosol. These particles serve as surrogates for urban hydrophobic POA. The results show that these POA did not enhance the SOA yields. If these results are found to apply to other biogenic SOA precursors, then the semi-empirical models used in many global models would predict significantly less biogenic SOA mass and display reduced sensitivity to anthropogenic POA emissions than previously thought.

  18. A Year-round Observation of Size Distribution of Aerosol Particles at the Cape Ochiishi, Japan

    NASA Astrophysics Data System (ADS)

    Miura, K.; Mukai, H.; Hashimoto, S.; Uematsu, M.

    2010-12-01

    New particle formation by nucleation of gas-phase compounds emitted from marine biogenic sources is very important for climate change. To clarify the mechanism of the formation, size distributions of submicron aerosols have been measured at the Cape Ochiishi, facing the North Western Pacific Ocean where primary productivity is high. A test observation was done from 22nd May to 18th June 2008 and a year-round observation has been performed from 16th October 2009 to 7th September 2010. The size distribution from 10 nm to 487 nm in diameter was measured with a scanning mobility particle sizer (SMPS, TSI 3034). Sample air was dried to lower than 40%. Transport of sulfate, organic carbon (OC), and black carbon (BC) was estimated with Chemical weather FORecasting System (CFORS), developed by Prof. Uno, Kyushu University, Japan. Existence of inversion layer was estimated with temperature profile measured at surface, 10m, 30m, and 50m in altitude. The burst of the particles smaller than 20nm in diameter continuing longer than 3 hrs was observed ten times until 3rd November 2009. Two were observed in early summer and the other was in autumn. Banana shape was faintly observed five times. Transport of sulfate, OC, and BC was observed 3, 8, 9 times, respectively. Source of air mass was estimated with these elements, weather map, and wind direction. Five air masses were estimated to continental. Clearly nucleation related to marine sources was not observed. The size distribution of burst evens of maritime and continental air mass showed the shift of mode to larger diameter. Strong inversion of temperature was observed once. The value of size distribution did not show high. Minimum value of size distribution was observed in the strong rain on 27th October. Acknowledgments This study was partly supported by the Grant-in-Aids for Scientific Research on Priority Areas from the Ministry of Education, Culture, Sports, Science and Technology, Japan (18067005). The observation was

  19. Sources markers in aerosols, oceanic particles and sediments

    NASA Astrophysics Data System (ADS)

    Saliot, A.

    2009-02-01

    This review presents some diagnostic criteria used for identifying and quantifying terrestrial organic matter inputs to the ocean. Coupled to the isotopic composition of total organic carbon, the analysis of stable biomarkers permits to trace higher plant contributions in aerosols, dusts, sedimenting particles and dissolved phase in the water column and ultimately in recent and ancient sediments and soils. Some applications are presented, based on the analysis of n-alkyl compounds by a combination of gas chromatography and mass spectrometry (n-alkanes, n-alkanols, n-alkanoic acids and wax esters). Another approach has been developed using the analysis of macromolecular compounds present in higher plants. Abundances of the phenolic compounds from lignin, benzene carboxylic acids obtained during cupric oxide oxidation, Curie pyrolysis are used to characterise terrestrial organic matter sources and inputs. Finally due to the importance of biomass burning in continent-ocean transfers, biomarkers are presented in the polycyclic aromatic hydrocarbon class and for monosaccharide derivatives from the breakdown of cellulose.

  20. How biogenic terpenes govern the correlation between sulfuric acid concentrations and new particle formation

    NASA Astrophysics Data System (ADS)

    Bonn, B.; Kulmala, M.; Riipinen, I.; Sihto, S.-L.; Ruuskanen, T. M.

    2008-06-01

    New particle formation has been observed to take place all around the world. However, because of the inability to determine the chemical composition of the smallest clusters or particles, indirect tools such as the correlation between nucleation rate and measured sulfuric acid concentrations have been used to infer the nucleation mechanism. In this study we describe the observed correlation with gaseous sulfuric acid concentrations by interactions of sesquiterpene oxidation products with sulfuric acid. Two formation pathways of nucleation initiating molecules are considered. The interaction of sulfuric acid with organic sulfates, which are formed from stabilized Criegee intermediates (sCIs, formed from sesquiterpenes), can be used to explain the observed squared relationship between particle formation rate and ambient sulfuric acid concentrations. The corresponding linear dependence is explained with the participation of secondary ozonides, which are formed from sCIs and aldehydes. Both pathways are negatively affected by increasing water vapor concentration as observed in recent studies. In order to check the assumptions made we apply the derived nucleation coefficients to measurements of the BACCI/QUEST IV campaign made during spring 2005 in Hyytiälä, Finland. A reasonable agreement between the measurement data and the predicted nucleation rates is found, giving support for the presented nucleation description.

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

  3. Measurement of internal and external mixtures of test aerosols with a new Single Particle Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Wonaschütz, Anna; Hitzenberger, Regina

    2015-04-01

    The mixing state of atmospheric aerosol particles is a very important property affecting processes such as CCN activation and scattering and absorption of light by the particles, but is challenging to determine. A new Single Particle Aerosol Mass Spectrometer (LAAPTOF, AeroMegt GmbH) was tested with regards to its capability of measuring internal and external mixture of aerosols using laboratory generated particles. To create the external mixture, solutions of three different salts in deionized water, and a suspension of carbon black (Cabot Corporation) in a mixture of isopropanol and water were nebulized and individually dried, before being passed into a small mixing chamber. To create the internal mixture, equal parts of each solution/suspension were mixed, fed into a single nebulizer, nebulized and dried. The LAAPTOF sampled from the mixing chamber and recorded mass spectra of individual particles. The analysis shows a heterogeneous ensemble of single particle spectra for the external mixture, and a homogeneous ensemble of spectra for the internal mixture. The ability of a fuzzy clustering algorithm to resolve the difference between the two mixing states was also tested.

  4. Interactions Between Biogenic Silica (BSiO2) and Organic Carbon (POC) During the Recycling of Sinking Particles

    NASA Astrophysics Data System (ADS)

    Moriceau, B.; Goutx, M.; Guigue, C.; Tamburini, C.; Lee, C.; Armstrong, R. A.; Duflos, M.; Charriere, B.; Ragueneau, O.

    2006-12-01

    Despite recent progress in understanding the ocean's role in the global carbon cycle, we are not yet able to predict the response of ecosystems to climate change and feedbacks of the ocean onto atmospheric CO2. In particular, particle flux dynamics must be represented more faithfully in ocean models. We know that particulate organic carbon (POC) flux is associated with ballast minerals (BSiO2, CaCO3), but the processes controlling the interactions between carbon and ballast minerals during decomposition must be explored further. The present study aims to provide a better understanding of interactions between carbon and BSiO2 during mineralization of sinking particles. Previous studies have provided evidence that the degradation of the external membrane by bacteria increase the BSiO2 dissolution rate. Alternatively, it has been hypothesized that biogenic silica could protect carbon from degradation. To test this hypothesis, an in-vitro batch experiment using the diatom Skeletonema costatum was conducted. In this experiment, carbon degradation, bacterial growth, and BSiO2 dissolution were followed simultaneously. To identify the processes involved and the types of carbon that eventually interact with BSiO2 during mineralization, the concentrations of different lipids and amino acids were also measured. A strong increase of the degradation rate constant of the POC and PON was observed after dissolution of 40 % of initial BSiO2. This increase is associated to a peak of glycine in total amino acids and a switch between free and attached bacteria. These results suggest that carbon degradation is increased when enough of the frustule is dissolved to uncover the glycine contain inside the frustule, this amino acid may trigger an increase in the concentration of attached bacteria, which may in turn increase the degradation rate constant of organic carbon.

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

    PubMed

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

    2015-05-14

    Understanding the interactions of water with atmospheric aerosols is crucial for determining the size, physical state, reactivity, and climate impacts of this important component of the Earth's atmosphere. Here we show that water uptake and hygroscopic growth of multicomponent, atmospherically relevant particles can be size dependent when comparing 100 nm versus ca. 6 μm sized particles. It was determined that particles composed of ammonium sulfate with succinic acid and of a mixture of chlorides typical of the marine environment show size-dependent hygroscopic behavior. Microscopic analysis of the distribution of components within the aerosol particles show that the size dependence is due to differences in the mixing state, that is, whether particles are homogeneously mixed or phase separated, for different sized particles. This morphology-dependent hygroscopicity has consequences for heterogeneous atmospheric chemistry as well as aerosol interactions with electromagnetic radiation and clouds. PMID:25521409

  6. 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.

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

    NASA Astrophysics Data System (ADS)

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

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

  8. Comparison between CARIBIC Aerosol Samples Analysed by Accelerator-Based Methods and Optical Particle Counter Measurements

    NASA Astrophysics Data System (ADS)

    Martinsson, B. G.; Friberg, J.; Andersson, S. M.; Weigelt, A.; Hermann, M.; Assmann, D.; Voigtländer, J.; Brenninkmeijer, C. A. M.; van Velthoven, P. J. F.; Zahn, A.

    2014-08-01

    Inter-comparison of results from two kinds of aerosol systems in the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on a Instrument Container) passenger aircraft based observatory, operating during intercontinental flights at 9-12 km altitude, is presented. Aerosol from the lowermost stratosphere (LMS), the extra-tropical upper troposphere (UT) and the tropical mid troposphere (MT) were investigated. Aerosol particle volume concentration measured with an optical particle counter (OPC) is compared with analytical results of the sum of masses of all major and several minor constituents from aerosol samples collected with an impactor. Analyses were undertaken with the following accelerator-based methods: particle-induced X-ray emission (PIXE) and particle elastic scattering analysis (PESA). Data from 48 flights during 1 year are used, leading to a total of 106 individual comparisons. The ratios of the particle volume from the OPC and the total mass from the analyses were in 84% within a relatively narrow interval. Data points outside this interval are connected with inlet-related effects in clouds, large variability in aerosol composition, particle size distribution effects and some cases of non-ideal sampling. Overall, the comparison of these two CARIBIC measurements based on vastly different methods show good agreement, implying that the chemical and size information can be combined in studies of the MT/UT/LMS aerosol.

  9. Comparison between CARIBIC aerosol samples analysed by accelerator-based methods and optical particle counter measurements

    NASA Astrophysics Data System (ADS)

    Martinsson, B. G.; Friberg, J.; Andersson, S. M.; Weigelt, A.; Hermann, M.; Assmann, D.; Voigtländer, J.; Brenninkmeijer, C. A. M.; van Velthoven, P. J. F.; Zahn, A.

    2014-04-01

    Inter-comparison of results from two kinds of aerosol systems in the CARIBIC (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container) passenger aircraft based observatory, operating during intercontinental flights at 9-12 km altitude, is presented. Aerosol from the lowermost stratosphere (LMS), the extra-tropical upper troposphere (UT) and the tropical mid troposphere (MT) were investigated. Aerosol particle volume concentration measured with an optical particle counter (OPC) is compared with analytical results of the sum of masses of all major and several minor constituents from aerosol samples collected with an impactor. Analyses were undertaken with accelerator-based methods particle-induced X-ray emission (PIXE) and particle elastic scattering analysis (PESA). Data from 48 flights during one year are used, leading to a total of 106 individual comparisons. The ratios of the particle volume from the OPC and the total mass from the analyses were in 84% within a relatively narrow interval. Data points outside this interval are connected with inlet-related effects in clouds, large variability in aerosol composition, particle size distribution effects and some cases of non-ideal sampling. Overall, the comparison of these two CARIBIC measurements based on vastly different methods show good agreement, implying that the chemical and size information can be combined in studies of the MT/UT/LMS aerosol.

  10. Observations of aerosol light scattering, absorption, and particle morphology changes as a function of relative humidity

    NASA Astrophysics Data System (ADS)

    Arnott, W. P.; Lewis, K.; Paredes-Miranda, G.; Winter, S.; Day, D.; Chakrabarty, R.; Moosmuller, H.; Jimenez, J. L.; Ulbrich, I.; Huffman, A.; Onasch, T.; Trimborn, A.; Kreidenweis, S.; Carrico, C.; Wold, C.; Lincoln, E.; Freeborn, P.; Hao, W.; McMeeking, G.

    2006-12-01

    A very interesting case of smoke aerosol with very low single scattering albedo, yet very large hygroscopic growth for scattering is presented. Several samples of chamise (Adenostoma fasciculatum), a common and often dominant species in California chaparral, were recently burned at the USFS Fire Science Laboratory in Missoula Montana, and aerosol optics and chemistry were observed, along with humidity-dependent light scattering, absorption, and particle morphology. Photoacoustic measurements of light absorption by two instruments at 870 nm, one on the dry channel, one on the humidified channel, showed strong reduction of aerosol light absorption with RH above 65 percent, and yet a strong increase in light scattering was observed both at 870 nm and 550 nm with nephelometers. Multispectral measurements of aerosol light absorption indicated an Angstrom coefficient for absorption near unity for the aerosols from chamise combustion. It is argued that the hygroscopic growth of scattering is due to uptake of water by the sulfur bearing aerosol. Furthermore, the reduction of aerosol light absorption is argued to be due to the collapse of chain aggregate aerosol as the RH increases wherein the interior of aerosol does no longer contribute to absorption. Implications for biomass burning in general are that humidity processing of aerosols from this source and others like it tends to substantially increase its single scattering albedo, probably in a non-reversible manner. The chemical pathway to hygroscopicity will be addressed.

  11. 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

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

    SciTech Connect

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

    2011-02-15

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

  13. Inside versus Outside: Ion Redistribution in Nitric Acid Reacted Sea Spray Aerosol Particles as Determined by Single Particle Analysis (Invited)

    NASA Astrophysics Data System (ADS)

    Ault, A. P.; Guasco, T.; Ryder, O. S.; Baltrusaitis, J.; Cuadra-Rodriguez, L. A.; Collins, D. B.; Ruppel, M. J.; Bertram, T. H.; Prather, K. A.; Grassian, V. H.

    2013-12-01

    Sea spray aerosol (SSA) particles were generated under real-world conditions using natural seawater and a unique ocean-atmosphere facility equipped with actual breaking waves or a marine aerosol reference tank (MART) that replicates those conditions. The SSA particles were exposed to nitric acid in situ in a flow tube and the well-known chloride displacement and nitrate formation reaction was observed. However, as discussed here, little is known about how this anion displacement reaction affects the distribution of cations and other chemical constituents within and phase state of individual SSA particles. Single particle analysis of individual SSA particles shows that cations (Na+, K+, Mg2+ and Ca2+) within individual particles undergo a spatial redistribution after heterogeneous reaction with nitric acid, along with a more concentrated layer of organic matter at the surface of the particle. These data suggest that specific ion and aerosol pH effects play an important role in aerosol particle structure in ways that have not been previously recognized. The ordering of organic coatings can impact trace gas uptake, and subsequently impact trace gas budgets of O3 and NOx.

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

    NASA Astrophysics Data System (ADS)

    Li, Weijun; Shao, Longyi

    2009-05-01

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

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

    PubMed

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

    2016-07-18

    Organic aerosols provide a measure of complexity in the urban atmosphere. This is because the aerosols start as an external mixture, with many populations from varied local sources, that all interact with each other, with background aerosols, and with condensing vapors from secondary organic aerosol formation. The externally mixed particle populations start to evolve immediately after emission because the organic molecules constituting the particles also form thermodynamic mixtures - solutions - in which a large fraction of the constituents are semi-volatile. The external mixtures are thus well out of thermodynamic equilibrium, with very different activities for many constituents, and yet also have the capacity to relax toward equilibrium via gas-phase exchange of semi-volatile vapors. Here we describe experiments employing quantitative single-particle mass spectrometry designed to explore the extent to which various primary organic aerosol particle populations can interact with each other or with secondary organic aerosols representative of background aerosol populations. These methods allow us to determine when these populations will and when they will not mix with each other, and then to constrain the timescales for that mixing. PMID:27092377

  16. 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.

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

    PubMed Central

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

    2013-01-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2012-01-01

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

  19. 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

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

    PubMed

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

    2009-03-01

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

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

    SciTech Connect

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

    2014-09-01

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

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

    SciTech Connect

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

    2005-04-25

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

  4. 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

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

    NASA Astrophysics Data System (ADS)

    Kaloshin, Gennady

    2013-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2005-10-01

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

  7. Prospects of real-time single-particle biological aerosol analysis: A comparison between laser-induced breakdown spectroscopy and aerosol time-of-flight mass spectrometry

    NASA Astrophysics Data System (ADS)

    Beddows, D. C. S.; Telle, H. H.

    2005-08-01

    In this paper we discuss the prospects of real-time, in situ laser-induced breakdown spectroscopy applied for the identification and classification of bio-aerosols (including species of potential bio-hazard) within common urban aerosol mixtures. In particular, we address the issues associated with the picking out of bio-aerosols against common background aerosol particles, comparing laser-induced breakdown spectroscopy measurements with data from a mobile single-particle aerosol mass spectrometer (ATOFMS). The data from the latter provide statistical data over an extended period of time, highlighting the variation of the background composition. While single-particle bio-aerosols are detectable in principle, potential problems with small (˜ 1 μm size) bio-aerosols have been identified; constituents of the air mass other than background aerosols, e.g. gaseous CO 2 in conjunction with common background aerosols, may prevent unique recognition of the bio-particles. We discuss whether it is likely that laser-induced breakdown spectroscopy on its own can provide reliable, real-time identification of bio-aerosol in an urban environment, and it is suggested that more than one technique should be or would have to be used. A case for using a combination of laser-induced breakdown spectroscopy and Raman (and/or) laser-induced fluorescence spectroscopy is made.

  8. 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.

  9. Direct observation of aerosol particles in aged agricultural biomass burning plumes impacting urban atmospheres

    NASA Astrophysics Data System (ADS)

    Li, W. Y.; Shao, L. Y.

    2010-04-01

    Emissions from agricultural biomass burning (ABB) in northern China have a significant impact on the regional and the global climate. According to the Giovanni's Aerosol optical depth (AOD) map, the monthly average AOD at 550 nm in northern China in 2007 shows a maximum value of 0.7 in June, suggesting that episodes of severe aerosol pollution occurred in this region. Aerosol particles were collected in urban Beijing during regional brown hazes from 12 to 30 June, 2007. Transmission electron microscopy with energy-dispersive X-ray spectrometry characterized the morphology, composition, and mixing state of aerosol particles. Potassium salts (K2SO4 and KNO3), ammonium sulfate, soot, and organic particles predominated in fine particles (diameter <1 μm) collected from 12 to 20 June, 2007. In contrast, from 21 to 30 June, 2007, ammonium sulfate, soot, and organic particles were dominant. Potassium-dominant particles as a tracer of biomass burning, together with wildfire maps, show that intensive regional ABB in northern China from 10 to 20 June, 2007 contributed significantly to the regional haze. After long-range transport, ABB particles exhibited marked changes in their morphology, elemental composition, and mixing state. Heterogeneous reactions completely converted KCl particles from ABB into K2SO4 and KNO3. Soot particles were generally mixed with potassium salts, ammonium salts, and organic particles. In addition, the abundant aged organic particles and soluble salts emitted by ABB become more hygroscopic and increase their size during long-range transport, becoming in effect additional cloud condensation nuclei. The high AOD (average value at 2.2) during 12 to 20 June, 2007, in Beijing is partly explained by the hygroscopic growth of aged fine aerosol particles and by the strong absorption of internally mixed soot particles, both coming from regional ABB emissions.

  10. Heterogeneous nucleation of ice particles on glassy aerosols modifies TTL cirrus

    NASA Astrophysics Data System (ADS)

    Wilson, T. W.; Murray, B. J.; Dobbie, S.; Al-Jumur, S. M.; Cui, Z.; Wagner, R.; Moehler, O.; Schnaiter, M.; Benz, S.; Niemand, M.; Saathoff, H.; Skrotzki, J.; Ebert, V.; Wagner, S.; Karcher, B.

    2010-12-01

    Experiments at the AIDA chamber, Karlsruhe Institute of Technology, have shown that glassy aqueous citric acid aerosol can nucleate ice at temperatures relevant to the tropical tropopause layer (TTL)(1). Modelling suggests this new route to the formation of TTL cirrus can provide an explanation for the very low ice particle number density observed in cirrus clouds in this region and may lead to high in-cloud supersaturations(1). Nucleation of ice on glassy aerosol is consistent with the absence of traditional ice nuclei in sampled TTL cirrus residue(2). In addition, we will present new data from experiments performed in July 2010 at the AIDA chamber using glassy aerosols composed of other atmospherically relevant compounds (levoglucosan, raffinose) and an internal mixture of five dicarboxylic acids and ammonium sulphate (raffinose/M5AS)(3). All four systems tested nucleate ice when in a glassy state. This indicates that heterogeneous ice nucleation is a general property of glassy aerosols and that natural aerosols which are composed of similar molecules will also nucleate ice if glassy. Glassy aqueous levoglucosan and raffinose/M5AS aerosol nucleated ice at temperatures similar to those found for glassy aqueous citric acid aerosol (<202 K). Whereas raffinose, which forms a glass at much higher temperatures, nucleated ice heterogeneously at up to ~220 K. This activity at higher temperatures suggests that ice nucleation by glassy aerosol may also play a role in the formation of warmer ice clouds. (1)B. J. Murray et al., Heterogeneous nucleation of ice particles on glassy aerosols under cirrus conditions, Nature Geosci, 2010, 3, 233-237. (2)K. D. Froyd et al., Aerosols that form subvisible cirrus at the tropical tropopause, Atmos. Chem. Phys., 2010, 10, 209-218. (3)B. Zobrist et al., Do atmospheric aerosols form glasses?, Atmos. Chem. Phys., 2008, 8, 5221-5244.

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

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2010-06-01

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

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

    PubMed

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

    2015-06-01

    The hygroscopic properties of submicron aerosol particles have significant effects on spectral distribution, CCN activation, climate forcing, human health and so on. A Hygroscopic Tandem Differential Mobility Analyzer (HTDMA) was utilized to analyze the hygroscopic properties of aerosol particles in the northern suburb of Nanjing during 16 April to 21 May, 2014. At relative humidity (RH) of 90%, for particles with dry diameters 30-230 nm, the probability distribution of GF (GF-PDF) shows a distinct bimodal pattern, with a dominant more-hygroscopic group and a smaller less-hygroscopic group. A contrast analysis between day and night suggests that, aerosol particles during day time have a stronger hygroscopicity and a higher number fraction of more-hygroscopic group than that at night overall. Aerosol particles during night have a higher degree of externally mixed state. Backward trajectory analysis using HYSPLIT mode reveals that, the sampling site is mainly affected by three air masses. For aitken nuclei, northwest continental air masses experience a longer aging process and have a stronger hygroscopicity. For condensation nuclei, east air masses have a stronger hygroscopicity and have a higher number fraction of more-hygroscopic group. Aerosol particles in local air masses have a high number fraction of more-hygroscopic group in the whole diameter range. PMID:26387289

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

    SciTech Connect

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

    2008-05-15

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

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

    PubMed

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

    2016-02-01

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

  16. 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.

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

    PubMed Central

    Ku, Bon Ki; Evans, Douglas E.

    2015-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  19. Atmospheric science: marine aerosols and iodine emissions.

    PubMed

    McFiggans, Gordon

    2005-02-10

    O'Dowd et al. describe the formation of marine aerosols from biogenic iodine and the growth of these aerosols into cloud-condensation nuclei (CCN). Based on chamber and modelling results, the authors suggest that biogenic organic iodine compounds emitted from macroalgae may be responsible for coastal particle bursts and that production of these compounds in the open ocean could increase CCN there too. It has since been shown that coastal particles are more likely to be produced from the photooxidation of molecular iodine. Moreover, I contend that open-ocean particle production and cloud enhancement do not result from emissions of organic iodine at atmospheric levels. For iodine particles to affect cloud properties over the remote ocean, an additional source of iodine is necessary as organic precursors cannot be responsible. PMID:15703706

  20. IN-SITU AERODYNAMIC SIZING OF AEROSOL PARTICLES WITH THE SPART ANALYZER

    EPA Science Inventory

    A single particle aerodynamic relaxation time (SPART) analyzer has been developed to measure the aerodynamic size distribution of aerosol particulates in the range 0.1 to 10.0 micrometer in diameter. The analyzer sizes and counts individual suspended particles and droplets from s...

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

    EPA Science Inventory

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

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

    NASA Astrophysics Data System (ADS)

    Eversole, Jay D.

    2011-03-01

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

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

    PubMed

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

    2007-08-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2007-08-01

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

  5. [Size distributions of aerosol particles and the impact on visibility in winter of Nanjing].

    PubMed

    Shang, Qian; Li, Zi-Hua; Yang, Jun; Pu, Mei-Juan

    2011-09-01

    High resolution instruments were used to investigate the relationship between aerosol size distribution characteristics and meteorological factors, and its possible influence on visibility in urban Nanjing from November to December 2009. Results show that the size distribution of aerosol number concentration showed a bimodal shape with the main peak value concentrating at particle sizes of 0.04-0.1 microm. Mass concentration distribution presented a bimodal shape with the two peak values concentrating at particle sizes of 0.5-0.7 microm and 2.7 microm, and the surface area concentration distribution presented two peaks from 0.1 to 0.5 microm and from 0.5 to 0.9 microm. It is found that the diurnal and interdiurnal variations of particle concentrations are obvious. Human activities and variation of atmospheric stability had great effect on daily variation of particle concentrations, while meteorological conditions such as precipitation, wind, relative humidity and so on had strong influence on interdiurnal variation. The aerosol size distribution was significantly affected by relative humidity. When RH was lower than 54%, number concentration of aerosol particles less than 1 microm in diameter increased gradually as RH increased, and concentration of particles with diameter larger than 1 microm almost had no change. When RH was higher than 54%, number concentration of aerosol particles ranging from 0.01 to 0.2 microm and from 2.7 to 10 microm decreased with the increase of RH, in contrast, concentration of aerosol particles between 0.5 and 1.5 microm in diameter increased. In addition, the particle number size distributions were different in rainy, foggy, sunny and haze weather conditions. Compared to sunny day, concentration of particles with different sizes all decreased in rainy day. In foggy weather, The number concentration of aerosol particles ranging from 0.01 to 0.3 microm and from 2.7 to 10 microm decreased, and aerosol particles between 0.3 and 2.7 microm

  6. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  8. The Humidity Dependence of N2O5 Uptake to Citric Acid Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Grzinic, G.; Bartels-Rausch, T.; Tuerler, A.; Ammann, M.

    2013-12-01

    Dinitrogen pentoxide is a significant reactive intermediate in the night time chemistry of nitrogen oxides. Depending on atmospheric conditions it can act either as a NO3 radical reservoir or as a major NOx sink by heterogeneous hydrolysis on aerosol surfaces. As such, it can influence tropospheric ozone production and therefore the oxidative capacity of the atmosphere. The heterogeneous loss of N2O5 to aerosol particles has remained uncertain, and reconciling lab and field data has demonstrated some gaps in our understanding of the detailed mechanism. We used the short-lived radioactive tracer 13N to study N2O5 uptake kinetics on aerosol particles in an aerosol flow reactor at ambient pressure, temperature and relative humidity. Citric acid, representing strongly oxidized polyfunctional organic compounds in atmospheric aerosols, has been chosen as a proxy due to its well established physical properties. Aerosol uptake measurements were performed with citric acid aerosols in a humidity range of 15-75 % RH, within which the uptake coefficient varies between about 0.001 and about 0.02. Taking into account the well established hygroscopic properties of citric acid, we interpret uptake in terms of disproportionation of N2O5 into nitrate ion and nitronium ion and reaction of the latter with liquid water.

  9. A rocket-borne mass analyzer for charged aerosol particles in the mesosphere

    SciTech Connect

    Knappmiller, Scott; Robertson, Scott; Sternovsky, Zoltan; Friedrich, Martin

    2008-10-15

    An electrostatic mass spectrometer for nanometer-sized charged aerosol particles in the mesosphere has been developed and tested. The analyzer is mounted on the forward end of a rocket and has a slit opening for admitting a continuous sample of air that is exhausted through ports at the sides. Within the instrument housing are two sets of four collection plates that are biased with positive and negative voltages for the collection of negative and positive aerosol particles, respectively. Each collection plate spans about an order of magnitude in mass which corresponds to a factor of 2 in radius. The number density of the charge is calculated from the current collected by the plates. The mean free path for molecular collisions in the mesosphere is comparable to the size of the instrument opening; thus, the analyzer performance is modeled by a Monte Carlo computer code that finds the aerosol particles trajectories within the instrument including both the electrostatic force and the forces from collisions of the aerosol particles with air molecules. Mass sensitivity curves obtained using the computer models are near to those obtain