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Sample records for aerosol particle composition

  1. Chemistry and Composition of Atmospheric Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Kolb, Charles E.; Worsnop, Douglas R.

    2012-05-01

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

  2. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2001-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2012-04-01

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

  6. Composition and Particle Size Retrievals for Homogeneous Binary Aerosols

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  7. 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

  8. 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.

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

    PubMed

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

    2010-01-01

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

  10. 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.

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

  13. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    NASA Astrophysics Data System (ADS)

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

    2011-03-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in Southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources were reflected through three factors: two biomass burning factors and a highly chemically processed long range transport factor. The biomass burning factors were separated by PMF due to differences in chemical processing which were caused in part by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range

  14. Elucidating determinants of aerosol composition through particle-type-based receptor modeling

    NASA Astrophysics Data System (ADS)

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

    2011-08-01

    An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique

  15. The Composition of Individual Aerosol Particles over the North Slope of Alaska during ISDAC

    NASA Astrophysics Data System (ADS)

    Zelenyuk, A.; Imre, D.; Liu, P.; MacDonald, A.; Leaitch, R.

    2008-12-01

    During the month of April 2008 a single particle mass spectrometer, SPLAT II, was deployed on board the Canadian National Research Council Convair 580 aircraft for participation in the Indirect and Semi-Direct Aerosol Campaign (ISDAC). ISDAC's main scientific objective was to improve our understanding of the relationship between the properties of aerosol particles over the North Pole and their impact on the regional climate. During ISDAC SPLAT II participated in all 27 flights that lasted slightly over 100 hrs. It measured the size of more than 10 million particles and characterized the composition of over 3 million of them. When sampling in clear air SPLAT II measured a wide range of particle compositions, including sulfates mixed with organics, nitrates mixed with organic, processed and freshly emitted sea-salt, a few dust particles, and a significant number of biomass burning particles. Many of these particle types appeared in aerosol layers that had horizontal and vertical filamentous structures. Biomass burning particles, many of which were transported from Asia, were rather prevalent over the North Slope of Alaska during the campaign. Since one of the main goals of this campaign was to characterize cloud properties, large fraction of the data was collected through the CVI inlet. The ice-clouds sampled in ISDAC had typically very low ice crystal concentrations; correspondingly, when sampled through the CVI inlet the number of characterized particles drops precipitously. Despite the low number concentrations SPLAT was able to measure the size and composition of thousands of ice-nuclei. Since the CVI inlet transmits, in addition to ice crystals, liquid droplets, SPLAT was able to characterize a large number of particles that served as cloud condensation nuclei as well. We will present a preliminary analysis of the single particle data collected during this campaign.

  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

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

  17. Chemical composition of individual aerosol particles from working areas in a nickel refinery.

    PubMed

    Höflich, B L; Wentzel, M; Ortner, H M; Weinbruch, S; Skogstad, A; Hetland, S; Thomassen, Y; Chaschin, V P; Nieboer, E

    2000-06-01

    Individual aerosol particles (n = 1170) collected at work stations in a nickel refinery were analyzed by wavelength-dispersive electron-probe microanalysis. By placing arbitrary restrictions on the contents of sulfur and silicon, the particles could be divided into four main groups. Scanning electron images indicated that most of the particles examined were relatively small (< or = 2 microm, equivalent projected area diameter), and that their morphology suggested formation from a melt. There was an absence of well-defined phases and simple stoichiometries, indicating that exposures to pure substances such as nickel subsulfide or specific oxides appeared not to occur. Although the elemental composition of particles varied greatly, a rough association was evident with the known elemental content of the refinery intermediates. The implications of the findings for aerosol speciation measurements, toxicological studies and interpretation of adverse health effects are explored. PMID:11256701

  18. 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

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  1. [Chemical Composition of the Single Particle Aerosol in Winter in Nanning Using SPAMS].

    PubMed

    Liu, Hui-lin; Song, Hong-jun; Chen, Zhi-ming; Huang, Jiong-li; Yang, Jun-chao; Mao, Jing-ying; Li, Hong; Liang, Gui-yun; Mo, Zhao-yu

    2016-02-15

    Single Particle Aerosol Mass Spectrometry (SPAMS) was performed to characterize the PM2.5 in Nanning from 15 to 24 February 2015. The correlation (R2) between the PM2.5 number concentration and the mass concentration of PM2.5 obtained using SPAMS was 0.76. The particle number concentration could reflect the atmospheric pollution situation to some degree. The Art-2a classification method was used to classify the chemical composition of PM2.5. The results showed that the principal chemical constituents were elemental carbon, organic elements carbon hybrid particles, organic carbon, rich potassium particles, mineral substance, rich sodium particles, second inorganic particles, levoglucosan and other heavy metals. Among them, the composition of elemental carbon was the highest, followed by organic carbon and rich potassium particles. The particle size of 80% of PM2.5 was mainly concentrated in the range of 0.2 microm to 1.0 microm with a peak value occurring at 0. 62 microm. The particle size distribution characteristics of different chemical components were similar. The number concentration of the chemical components in PM2.5 had the same variation tread with the mass concentration of PM2.5 over time. To a certain extent, the change in chemical composition could reflect the instantaneous pollution source.

  2. [Chemical Composition of the Single Particle Aerosol in Winter in Nanning Using SPAMS].

    PubMed

    Liu, Hui-lin; Song, Hong-jun; Chen, Zhi-ming; Huang, Jiong-li; Yang, Jun-chao; Mao, Jing-ying; Li, Hong; Liang, Gui-yun; Mo, Zhao-yu

    2016-02-15

    Single Particle Aerosol Mass Spectrometry (SPAMS) was performed to characterize the PM2.5 in Nanning from 15 to 24 February 2015. The correlation (R2) between the PM2.5 number concentration and the mass concentration of PM2.5 obtained using SPAMS was 0.76. The particle number concentration could reflect the atmospheric pollution situation to some degree. The Art-2a classification method was used to classify the chemical composition of PM2.5. The results showed that the principal chemical constituents were elemental carbon, organic elements carbon hybrid particles, organic carbon, rich potassium particles, mineral substance, rich sodium particles, second inorganic particles, levoglucosan and other heavy metals. Among them, the composition of elemental carbon was the highest, followed by organic carbon and rich potassium particles. The particle size of 80% of PM2.5 was mainly concentrated in the range of 0.2 microm to 1.0 microm with a peak value occurring at 0. 62 microm. The particle size distribution characteristics of different chemical components were similar. The number concentration of the chemical components in PM2.5 had the same variation tread with the mass concentration of PM2.5 over time. To a certain extent, the change in chemical composition could reflect the instantaneous pollution source. PMID:27363128

  3. Origin and impact of particle-to-particle variations in composition measurements with the nano-aerosol mass spectrometer.

    PubMed

    Klems, Joseph P; Johnston, Murray V

    2013-09-01

    In the nano-aerosol mass spectrometer, individual particles in the 10-30 nm size range are trapped and irradiated with a high pulse energy laser beam. The laser pulse generates a plasma that disintegrates the particle into atomic ions, from which the elemental composition is determined. Particle-to-particle variations among the mass spectra are shown to arise from plasma energetics: Low ionization energy species are enhanced in some spectra while high ionization energy species are enhanced in others. These variations also limit the accuracy and precision of elemental analysis, with higher deviations generally observed when low ionization energy species are dominant in the mass spectrum. For standard datasets generated from nominally identical particles, it is shown that that the error associated with composition measurement is random and that averaging the spectra from a few tens of particles is sufficient for measuring the mole fractions of common elements to within about 10% of the expected value. Averaging a greater number of particles offers limited improvement of the measurement precision but has the deleterious effect of degrading the measurement time-resolution, which is given by the time needed to obtain the required number of particle spectra for averaging. An internally mixed ambient particle dataset was found to give a similar result to the standard datasets, that is, the measured elemental composition converged to the average value after a few tens of particles were averaged.

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

    NASA Technical Reports Server (NTRS)

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

    2003-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

  6. Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

    PubMed

    Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

    2015-05-14

    Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores

  7. Chemical compositions of black carbon particle cores and coatings via soot particle aerosol mass spectrometry with photoionization and electron ionization.

    PubMed

    Canagaratna, Manjula R; Massoli, Paola; Browne, Eleanor C; Franklin, Jonathan P; Wilson, Kevin R; Onasch, Timothy B; Kirchstetter, Thomas W; Fortner, Edward C; Kolb, Charles E; Jayne, John T; Kroll, Jesse H; Worsnop, Douglas R

    2015-05-14

    Black carbon is an important constituent of atmospheric aerosol particle matter (PM) with significant effects on the global radiation budget and on human health. The soot particle aerosol mass spectrometer (SP-AMS) has been developed and deployed for real-time ambient measurements of refractory carbon particles. In the SP-AMS, black carbon or metallic particles are vaporized through absorption of 1064 nm light from a CW Nd:YAG laser. This scheme allows for continuous "soft" vaporization of both core and coating materials. The main focus of this work is to characterize the extent to which this vaporization scheme provides enhanced chemical composition information about aerosol particles. This information is difficult to extract from standard SP-AMS mass spectra because they are complicated by extensive fragmentation from the harsh 70 eV EI ionization scheme that is typically used in these instruments. Thus, in this work synchotron-generated vacuum ultraviolet (VUV) light in the 8-14 eV range is used to measure VUV-SP-AMS spectra with minimal fragmentation. VUV-SP-AMS spectra of commercially available carbon black, fullerene black, and laboratory generated flame soots were obtained. Small carbon cluster cations (C(+)-C5(+)) were found to dominate the VUV-SP-AMS spectra of all the samples, indicating that the corresponding neutral clusters are key products of the SP vaporization process. Intercomparisons of carbon cluster ratios observed in VUV-SP-AMS and SP-AMS spectra are used to confirm spectral features that could be used to distinguish between different types of refractory carbon particles. VUV-SP-AMS spectra of oxidized organic species adsorbed on absorbing cores are also examined and found to display less thermally induced decomposition and fragmentation than spectra obtained with thermal vaporization at 200 °C (the minimum temperature needed to quantitatively vaporize ambient oxidized organic aerosol with a continuously heated surface). The particle cores

  8. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry.

  9. Real-Time Characterization of Aerosol Particle Composition above the Urban Canopy in Beijing: Insights into the Interactions between the Atmospheric Boundary Layer and Aerosol Chemistry.

    PubMed

    Sun, Yele; Du, Wei; Wang, Qingqing; Zhang, Qi; Chen, Chen; Chen, Yong; Chen, Zhenyi; Fu, Pingqing; Wang, Zifa; Gao, Zhiqiu; Worsnop, Douglas R

    2015-10-01

    Despite extensive efforts into the characterization of air pollution during the past decade, real-time characterization of aerosol particle composition above the urban canopy in the megacity Beijing has never been performed to date. Here we conducted the first simultaneous real-time measurements of aerosol composition at two different heights at the same location in urban Beijing from December 19, 2013 to January 2, 2014. The nonrefractory submicron aerosol (NR-PM1) species were measured in situ by a high-resolution aerosol mass spectrometer at near-ground level and an aerosol chemical speciation monitor at 260 m on a 325 m meteorological tower in Beijing. Secondary aerosol showed similar temporal variations between ground level and 260 m, whereas much weaker correlations were found for the primary aerosol. The diurnal evolution of the ratios and correlations of aerosol species between 260 m and the ground level further illustrated a complex interaction between vertical mixing processes and local source emissions on aerosol chemistry in the atmospheric boundary layer. As a result, the aerosol compositions at the two heights were substantially different. Organic aerosol (OA), mainly composed of primary OA (62%), at the ground level showed a higher contribution to NR-PM1 (65%) than at 260 m (54%), whereas a higher concentration and contribution (15%) of nitrate was observed at 260 m, probably due to the favorable gas-particle partitioning under lower temperature conditions. In addition, two different boundary layer structures were observed, each interacting differently with the evolution processes of aerosol chemistry. PMID:26348650

  10. 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

  11. Sources and composition of submicron organic mass in marine aerosol particles

    SciTech Connect

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemical reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group peak

  12. Sources and composition of submicron organic mass in marine aerosol particles

    DOE PAGES

    Frossard, Amanda A.; Russell, Lynn M.; Burrows, Susannah M.; Elliott, Scott M.; Bates, Timothy S.; Quinn, Patricia K.

    2014-11-27

    Recent studies have proposed a variety of interpretations of the sources and composition of atmospheric marine aerosol particles (aMA) based on a range of physical and chemical measurements collected during open-ocean research cruises. To investigate the processes that affect marine organic particles, this study uses the characteristic functional group composition (from Fourier transform infrared (FTIR) spectroscopy) of aMAP from five ocean regions to show that: (i) The organic functional group composition of aMAP that can be identified as atmospheric primary marine (ocean-derived) aerosol (aPMA) is 65±12% hydroxyl, 21±9% alkane, 6±6% amine, and 7±8% carboxylic acid functional groups. Contributions from photochemicalmore » reactions add carboxylic acid groups (15%-25%), shipping effluent in seawater and ship emissions add additional alkane groups (up to 70%), and coastal emissions mix in alkane and carboxylic acid groups from coastal pollution sources. (ii) The organic composition of aPMA is nearly identical to model generated primary marine aerosol particles (gPMA) from bubbled seawater (55% hydroxyl, 32% alkane, and 13% amine functional groups), indicating that its overall functional group composition is the direct consequence of the organic constituents of the seawater source. (iii) While the seawater organic functional group composition was nearly invariant across all three ocean regions studied, the gPMA alkane group fraction increased with chlorophyll-a concentrations (r = 0.79). gPMA from productive seawater had a larger fraction of alkane functional groups (35%) compared to gPMA from non-productive seawater (16%), likely due to the presence of surfactants in productive seawater that stabilize the bubble film and lead to preferential drainage of the more soluble (lower alkane group fraction) organic components. gPMA has a hydroxyl group absorption peak location characteristic of monosaccharides and disaccharides, where the seawater OM hydroxyl group

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2010-05-01

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

  16. Estimation of aerosol particle composition using ground-based sun-sky radiometer measurements at typical sites in China

    NASA Astrophysics Data System (ADS)

    Li, Z.; Gu, X.; Wang, L.; Li, D.; Xing, X.; Gai, J.; Wang, Q.; Li, K.; Li, L.; Zhang, Y.

    2011-12-01

    Atmospheric aerosol affects climate and environment through radiative and health effects determined by its physical and chemical properties. In this study, we modeled aerosol by an internal mixture of different components like water, sulfate and black carbon following Maxwell-Garnett effective medium approximation theory. In order to deal with complex aerosol mixing situation in China, we considered extra mineral dust component in case of large particles. Remote sensing data obtained from ground-based CE318 sun-sky radiometers in typical China sites are used to derive the aerosol mixture model. Measurements are firstly calibrated by using intercomparison and vicarious calibration methods and then retrieved by using AErosol RObotic NETwork (AERONET) inversion algorithm to obtain refractive indices of the mixture, which are then used to yield aerosol component fraction. Results at typical China regions like megacity, industrial, arid, oceanic and background sites show considerable difference between their aerosol particle compositions and agree with a priori information like regional aerosol sources and formation processes.

  17. The 2005 Study of Organic Aerosols at Riverside (SOAR-1): instrumental intercomparisons and fine particle composition

    NASA Astrophysics Data System (ADS)

    Docherty, K. S.; Aiken, A. C.; Huffman, J. A.; Ulbrich, I. M.; Decarlo, P. F.; Sueper, D.; Worsnop, D. R.; Snyder, D. C.; Grover, B. D.; Eatough, D. J.; Goldstein, A. H.; Ziemann, P. J.; Jimenez, J. L.

    2011-02-01

    Multiple state-of-the-art instruments sampled ambient aerosol in Riverside, California during the 2005 Study of Organic Aerosols at Riverside (SOAR) to investigate sources and chemical composition of fine particles (PMf) in the inland region of Southern California. This paper briefly summarizes the spatial, meteorological and gas-phase conditions during SOAR-1 (15 July-15 August) and provides detailed intercomparisons of complementary measurements and average PMf composition during this period. Daily meteorology and gas-phase species concentrations were highly repetitive with meteorological and gas-phase species concentrations displaying clear diurnal cycles and weekday/weekend contrast, with organic aerosol (OA) being the single largest component contributing approximately one-third of PMf mass. In contrast with historical characterizations of OA in the region, several independent source apportionment efforts attributed the vast majority (~80%) of OA mass during SOAR-1 to secondary organic aerosol (SOA). Given the collocation of complementary aerosol measurements combined with a dominance of SOA during SOAR-1, this paper presents new results on intercomparisons among several complementary measurements and on PMf composition during this period. Total non-refractory submicron (NR-PM1) measurements from a high-resolution aerosol mass spectrometer (HR-AMS) are compared with measurements by tapered element oscillating microbalances (TEOM) including a filter dynamics measurement system (TEOMFDMS). NR-PM1 is highly correlated with PM2.5 TEOMFDMS measurements and accounts for the bulk of PM2.5 mass with the remainder contributed primarily by refractory material. In contrast, measurements from a heated TEOM show substantial losses of semi-volatile material, including ammonium nitrate and semi-volatile organic material. Speciated HR-AMS measurements are also consistent and highly correlated with several complementary measurements, including those of a collocated compact AMS

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

    PubMed

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

    2011-03-01

    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.

  19. 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

  20. Chemical composition of aerosol particles and light extinction apportionment before and during the heating season in Beijing, China

    NASA Astrophysics Data System (ADS)

    Wang, Qingqing; Sun, Yele; Jiang, Qi; Du, Wei; Sun, Chengzhu; Fu, Pingqing; Wang, Zifa

    2015-12-01

    Despite extensive efforts into characterization of the sources and formation mechanisms of severe haze pollution in the megacity of Beijing, the response of aerosol composition and optical properties to coal combustion emissions in the heating season remain poorly understood. Here we conducted a 3 month real-time measurement of submicron aerosol (PM1) composition by an Aerosol Chemical Speciation Monitor and particle light extinction by a Cavity Attenuated Phase Shift extinction monitor in Beijing, China, from 1 October to 31 December 2012. The average (±σ) PM1 concentration was 82.4 (±73.1) µg/m3 during the heating period (HP, 15 November to 31 December), which was nearly 50% higher than that before HP (1 October to 14 November). While nitrate and secondary organic aerosol (SOA) showed relatively small changes, organics, sulfate, and chloride were observed to have significant increases during HP, indicating the dominant impacts of coal combustion sources on these three species. The relative humidity-dependent composition further illustrated an important role of aqueous-phase processing for the sulfate enhancement during HP. We also observed great increases of hydrocarbon-like OA (HOA) and coal combustion OA (CCOA) during HP, which was attributed to higher emissions at lower temperatures and coal combustion emissions, respectively. The relationship between light extinction and chemical composition was investigated using a multiple linear regression model. Our results showed that the largest contributors to particle extinction were ammonium nitrate (32%) and ammonium sulfate (28%) before and during HP, respectively. In addition, the contributions of SOA and primary OA to particle light extinction were quantified. The results showed that the OA extinction was mainly caused by SOA before HP and by SOA and CCOA during HP, yet with small contributions from HOA and cooking aerosol for the entire study period. Our results elucidate substantial changes of aerosol

  1. On the composition of ammonia-sulfuric-acid ion clusters during aerosol particle formation

    NASA Astrophysics Data System (ADS)

    Schobesberger, S.; Franchin, A.; Bianchi, F.; Rondo, L.; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; Schnitzhofer, R.; Almeida, J.; Amorim, A.; Dommen, J.; Dunne, E. M.; Ehn, M.; Gagné, S.; Ickes, L.; Junninen, H.; Hansel, A.; Kerminen, V.-M.; Kirkby, J.; Kupc, A.; Laaksonen, A.; Lehtipalo, K.; Mathot, S.; Onnela, A.; Petäjä, T.; Riccobono, F.; Santos, F. D.; Sipilä, M.; Tomé, A.; Tsagkogeorgas, G.; Viisanen, Y.; Wagner, P. E.; Wimmer, D.; Curtius, J.; Donahue, N. M.; Baltensperger, U.; Kulmala, M.; Worsnop, D. R.

    2015-01-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new-particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from < 2 to 1400 pptv, [H2SO4] from 3.3 × 106 to 1.4 × 109 cm-3 (0.1 to 56 pptv), and a temperature range from -25 to +20 °C. Negatively and positively charged clusters were directly measured by an atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometer, as they initially formed from gas-phase NH3 and H2SO4, and then grew to larger clusters containing more than 50 molecules of NH3 and H2SO4, corresponding to mobility-equivalent diameters greater than 2 nm. Water molecules evaporate from these clusters during sampling and are not observed. We found that the composition of the NH3-H2SO4 clusters is primarily determined by the ratio of gas-phase concentrations [NH3] / [H2SO4], as well as by temperature. Pure binary H2O-H2SO4 clusters (observed as clusters of only H2SO4) only form at [NH3] / [H2SO4] < 0.1 to 1. For larger values of [NH3] / [H2SO4], the composition of NH3-H2SO4 clusters was characterized by the number of NH3 molecules m added for each added H2SO4 molecule n (Δm/Δ n), where n is in the range 4-18 (negatively charged clusters) or 1-17 (positively charged clusters). For negatively charged clusters, Δ m/Δn saturated between 1 and 1.4 for [NH3] / [H2SO4] > 10. Positively

  2. On the composition of ammonia-sulfuric acid clusters during aerosol particle formation

    NASA Astrophysics Data System (ADS)

    Schobesberger, S.; Franchin, A.; Bianchi, F.; Rondo, L.; Duplissy, J.; Kürten, A.; Ortega, I. K.; Metzger, A.; Schnitzhofer, R.; Almeida, J.; Amorim, A.; Dommen, J.; Dunne, E. M.; Ehn, M.; Gagné, S.; Ickes, L.; Junninen, H.; Hansel, A.; Kerminen, V.-M.; Kirkby, J.; Kupc, A.; Laaksonen, A.; Lehtipalo, K.; Mathot, S.; Onnela, A.; Petäjä, T.; Riccobono, F.; Santos, F. D.; Sipilä, M.; Tomé, A.; Tsagkogeorgas, G.; Viisanen, Y.; Wagner, P. E.; Wimmer, D.; Curtius, J.; Donahue, N. M.; Baltensperger, U.; Kulmala, M.; Worsnop, D. R.

    2014-05-01

    The formation of particles from precursor vapors is an important source of atmospheric aerosol. Research at the Cosmics Leaving OUtdoor Droplets (CLOUD) facility at CERN tries to elucidate which vapors are responsible for this new particle formation, and how in detail it proceeds. Initial measurement campaigns at the CLOUD stainless-steel aerosol chamber focused on investigating particle formation from ammonia (NH3) and sulfuric acid (H2SO4). Experiments were conducted in the presence of water, ozone and sulfur dioxide. Contaminant trace gases were suppressed at the technological limit. For this study, we mapped out the compositions of small NH3-H2SO4 clusters over a wide range of atmospherically relevant environmental conditions. We covered [NH3] in the range from <2 to 1400 pptv, [H2SO4] from 3.3 × 106 to 1.4 × 109 cm-3, and a temperature range from -25 to +20 °C. Negatively and positively charged clusters were directly measured by an atmospheric pressure interface time-of-flight (APi-TOF) mass spectrometer, as they initially formed from gas-phase NH3 and H2SO4, and then grew to larger clusters containing more than 50 molecules of NH3 and H2SO4, corresponding to mobility-equivalent diameters greater than 2 nm. Water molecules evaporate from these clusters during sampling and are not observed. We found that the composition of the NH3-H2SO4 clusters is primarily determined by the ratio of gas-phase concentrations [NH3] / [H2SO4], as well as by temperature. Pure binary H2O-H2SO4 clusters (observed as clusters of only H2SO4) only form at [NH3] / [H2SO4]<0.1 to 1. For larger values of [NH3] / [H2SO4], the composition of NH3-H2SO4 clusters was characterized by the number of NH3 molecules m added for each added H2SO4 molecule n (Δm / Δn), where n is in the range 4-18 (negatively charged clusters) or 1-17 (positively charged clusters). For negatively charged clusters, Δm / Δn saturated between 1 and 1.4 for [NH3] / [H2SO4]>10. Positively charged clusters grew on

  3. Organic aerosol molecular composition and gas-particle partitioning coefficients at a Mediterranean site (Corsica).

    PubMed

    Rossignol, Stéphanie; Couvidat, Florian; Rio, Caroline; Fable, Sébastien; Grignion, Guillaume; Savelli; Pailly, Olivier; Leoz-Garziandia, Eva; Doussin, Jean-Francois; Chiappini, Laura

    2016-02-01

    Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica (June 2011). Aimed at assessing the performance on the field of newly developed analytical protocols, this work focuses on the molecular composition of both gas and particulate phases and provides an insight into partitioning behavior of the semi-volatile oxygenated fraction. Limonene ozonolysis tracers were specifically searched for, according to gas chromatography-mass spectrometry (GC-MS) data previously recorded for smog chamber experiments. A screening of other oxygenated species present in the field atmosphere was also performed. About sixty polar molecules were positively or tentatively identified in gas and/or particle phases. These molecules comprise a wide range of branched and linear, mono and di-carbonyls (C3-C7), mono and di-carboxylic acids (C3-C18), and compounds bearing up to three functionalities. Among these compounds, some can be specifically attributed to limonene oxidation and others can be related to α- or β-pinene oxidation. This provides an original snapshot of the organic matter composition at a Mediterranean site in summer. Furthermore, for compounds identified and quantified in both gaseous and particulate phases, an experimental gas/particle partitioning coefficient was determined. Several volatile products, which are not expected in the particulate phase assuming thermodynamic equilibrium, were nonetheless present in significant concentrations. Hypotheses are proposed to explain these observations, such as the possible aerosol viscosity that could hinder the theoretical equilibrium to be rapidly reached.

  4. Organic aerosol molecular composition and gas-particle partitioning coefficients at a Mediterranean site (Corsica).

    PubMed

    Rossignol, Stéphanie; Couvidat, Florian; Rio, Caroline; Fable, Sébastien; Grignion, Guillaume; Savelli; Pailly, Olivier; Leoz-Garziandia, Eva; Doussin, Jean-Francois; Chiappini, Laura

    2016-02-01

    Molecular speciation of atmospheric organic matter was investigated during a short summer field campaign performed in a citrus fruit field in northern Corsica (June 2011). Aimed at assessing the performance on the field of newly developed analytical protocols, this work focuses on the molecular composition of both gas and particulate phases and provides an insight into partitioning behavior of the semi-volatile oxygenated fraction. Limonene ozonolysis tracers were specifically searched for, according to gas chromatography-mass spectrometry (GC-MS) data previously recorded for smog chamber experiments. A screening of other oxygenated species present in the field atmosphere was also performed. About sixty polar molecules were positively or tentatively identified in gas and/or particle phases. These molecules comprise a wide range of branched and linear, mono and di-carbonyls (C3-C7), mono and di-carboxylic acids (C3-C18), and compounds bearing up to three functionalities. Among these compounds, some can be specifically attributed to limonene oxidation and others can be related to α- or β-pinene oxidation. This provides an original snapshot of the organic matter composition at a Mediterranean site in summer. Furthermore, for compounds identified and quantified in both gaseous and particulate phases, an experimental gas/particle partitioning coefficient was determined. Several volatile products, which are not expected in the particulate phase assuming thermodynamic equilibrium, were nonetheless present in significant concentrations. Hypotheses are proposed to explain these observations, such as the possible aerosol viscosity that could hinder the theoretical equilibrium to be rapidly reached. PMID:26969549

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

    NASA Astrophysics Data System (ADS)

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

    2012-07-01

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

  6. Long-term aerosol measurements in Gran Canaria, Canary Islands: Particle concentration, sources and elemental composition

    NASA Astrophysics Data System (ADS)

    Gelado-Caballero, MaríA. D.; López-GarcíA, Patricia; Prieto, Sandra; Patey, Matthew D.; Collado, Cayetano; HéRnáNdez-Brito, José J.

    2012-02-01

    There are very few sets of long-term measurements of aerosol concentrations over the North Atlantic Ocean, yet such data is invaluable in quantifying atmospheric dust inputs to this ocean region. We present an 8-year record of total suspended particles (TSP) collected at three stations on Gran Canaria Island, Spain (Taliarte at sea level, Tafira 269 m above sea level (a.s.l.) and Pico de la Gorra 1930 m a.s.l.). Using wet and dry deposition measurements, the mean dust flux was calculated at 42.3 mg m-2 d-1. Air mass back trajectories (HYSPLIT, NOAA) suggested that the Sahara desert is the major source of African dust (dominant during 32-50% of days), while the Sahel desert was the major source only 2-10% of the time (maximum in summer). Elemental composition ratios of African samples indicate that, despite the homogeneity of the dust in collected samples, some signatures of the bedrocks can still be detected. Differences were found for the Sahel, Central Sahara and North of Sahara regions in Ti/Al, Mg/Al and Ca/Al ratios, respectively. Elements often associated with pollution (Pb, Cd, Ni, Zn) appeared to share a common origin, while Cu may have a predominantly local source, as suggested by a decrease in the enrichment factor (EF) of Cu during dust events. The inter-annual variability of dust concentrations is investigated in this work. During winter, African dust concentration measurements at the Pico de la Gorra station were found to correlate with the North Atlantic Oscillation (NAO) index.

  7. Size-segregated compositional analysis of aerosol particles collected in the European Arctic during the ACCACIA campaign

    NASA Astrophysics Data System (ADS)

    Young, G.; Jones, H. M.; Darbyshire, E.; Baustian, K. J.; McQuaid, J. B.; Bower, K. N.; Connolly, P. J.; Gallagher, M. W.; Choularton, T. W.

    2016-03-01

    Single-particle compositional analysis of filter samples collected on board the Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 aircraft is presented for six flights during the springtime Aerosol-Cloud Coupling and Climate Interactions in the Arctic (ACCACIA) campaign (March-April 2013). Scanning electron microscopy was utilised to derive size-segregated particle compositions and size distributions, and these were compared to corresponding data from wing-mounted optical particle counters. Reasonable agreement between the calculated number size distributions was found. Significant variability in composition was observed, with differing external and internal mixing identified, between air mass trajectory cases based on HYbrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) analyses. Dominant particle classes were silicate-based dusts and sea salts, with particles notably rich in K and Ca detected in one case. Source regions varied from the Arctic Ocean and Greenland through to northern Russia and the European continent. Good agreement between the back trajectories was mirrored by comparable compositional trends between samples. Silicate dusts were identified in all cases, and the elemental composition of the dust was consistent for all samples except one. It is hypothesised that long-range, high-altitude transport was primarily responsible for this dust, with likely sources including the Asian arid regions.

  8. Monitoring aerosol elemental composition in particle size fractions of long-range transport

    NASA Astrophysics Data System (ADS)

    Metternich, P.; Georgii, H.-W.; Groeneveld, K. O.

    1983-04-01

    Collection of atmospheric samples was performed at Malta, a semi-remote environment in the Mediterranean, in case of long-range transport studies of pollutants and natural substances. Using PIXE as a non-destructive trace-element analytical tool, the elemental composition of these samples was determined. Atmospheric concentrations obtained in this study were of one magnitude higher than those observed over the open North Alantic in purely marine air. For most of the anomalously enriched elements in the Mediterranean aerosol, the high concentrations can be explained by long-range transport.

  9. Changes in background aerosol composition in Finland during polluted and clean periods studied by TEM/EDX individual particle analysis

    NASA Astrophysics Data System (ADS)

    Niemi, J. V.; Saarikoski, S.; Tervahattu, H.; Mäkelä, T.; Hillamo, R.; Vehkamäki, H.; Sogacheva, L.; Kulmala, M.

    2006-11-01

    Aerosol samples were collected at a rural background site in southern Finland in May 2004 during pollution episode (PM1~16 µg m-3, backward air mass trajectories from south-east), intermediate period (PM1~5 µg m-3, backtrajectories from north-east) and clean period (PM1~2 µg m-3, backtrajectories from north-west/north). The elemental composition, morphology and mixing state of individual aerosol particles in three size fractions were studied using transmission electron microscopy (TEM) coupled with energy dispersive X-ray (EDX) microanalyses. The TEM/EDX results were complemented with the size-segregated bulk chemical measurements of selected ions and organic and elemental carbon. Many of the particles in PM0.2-1 and PM1-3.3 size fractions were strongly internally mixed with S, C and/or N. The major particle types in PM0.2-1 samples were 1) soot and 2) (ammonium)sulphates and their mixtures with variable amounts of C, K, soot and/or other inclusions. Number proportions of those two particle groups in PM0.2-1 samples were 0-12% and 83-97%, respectively. During the pollution episode, the proportion of Ca-rich particles was very high (26-48%) in the PM1-3.3 and PM3.3-11 samples, while the PM0.2-1 and PM1-3.3 samples contained elevated proportions of silicates (22-33%), metal oxides/hydroxides (1-9%) and tar balls (1-4%). These aerosols originated mainly from polluted areas of Eastern Europe, and some open biomass burning smoke was also brought by long-range transport. During the clean period, when air masses arrived from the Arctic Ocean, PM1-3.3 samples contained mainly sea salt particles (67-89%) with a variable rate of Cl substitution (mainly by NO3-). During the intermediate period, the PM1-3.3 sample contained porous (sponge-like) Na-rich particles (35%) with abundant S, K and O. They might originate from the burning of wood pulp wastes of paper industry. The proportion of biological particles and C-rich fragments (probably also biological origin) were highest

  10. Sulfur speciation in individual aerosol particles

    NASA Astrophysics Data System (ADS)

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

    1996-08-01

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

  11. Time-resolved mass concentration, composition and sources of aerosol particles in a metropolitan underground railway station

    NASA Astrophysics Data System (ADS)

    Salma, Imre; Weidinger, Tamás; Maenhaut, Willy

    Aerosol samples were collected using a stacked filter unit (SFU) for PM10-2.0 and PM2.0 size fractions on the platform of a metropolitan underground railway station in downtown Budapest. Temporal variations in the PM10 mass concentration and wind speed and direction were determined with time resolutions of 30 and 4 s using a tapered-element oscillating microbalance (TEOM) and a wind monitor, respectively. Sample analysis involved gravimetry for particulate mass, and particle-induced X-ray emission spectrometry (PIXE) for elemental composition. Diurnal variation of the PM10 mass concentration exhibited two peaks, one at approximately 07:00 h and the other at approximately 17:00 h. The mean±SD PM10 mass concentration for working hours was 155±55 μg m -3. Iron, Mn, Ni, Cu, and Cr concentrations were higher than in outdoor air by factors between 5 and 20, showing substantial enrichment compared to both the average crustal rock composition and the average outdoor aerosol composition. Iron accounted for 40% and 46% of the PM10-2.0 and PM2.0 masses, respectively, and 72% of the PM10 mass was associated with the PM10-2.0 size fraction. The aerosol composition in the metro station (in particular the abundance of the metals mentioned above) is quite different from the average outdoor downtown composition. Mechanical wear and friction of electric conducting rails and bow sliding collectors, ordinary rails and wheels, as well as resuspension, were identified as the primary sources. Possible health implications based on comparison to various limit values and to data available for other underground railways are discussed.

  12. Composition-dependent freezing nucleation rates for HNO3/H2O aerosols resembling gravity-wave-perturbed stratospheric particles

    NASA Astrophysics Data System (ADS)

    Prenni, Anthony J.; Onasch, Timothy B.; Tisdale, Robert T.; Siefert, Ronald L.; Tolbert, Margaret A.

    1998-11-01

    Laboratory measurements are presented for the freezing kinetics of H2O/HNO3 aerosols over the temperature range of 188-204 K. For 2:1 H2O:HNO3 aerosols crystallizing to NAD we observed a maximum nucleation rate of J = 9.3×109 cm-3 s-1 at 194 K. This temperature is between the glass point of 161 K [Ji et al., 1993] and the melting point of 235.5 K [Ji et al., 1996]. This can be compared to a previous measurement of J = 6.7×109 cm-3 s-1 at 193 K [Disselkamp et al., 1996] and lower temperature measurements of J ≈ 1010-1012 cm-3 s-1 at 178.8 - 175.8 K [Bertram and Sloan, 1998a]. Measured nucleation rates decrease as the aerosol becomes dilute, but NAD formation is still observable for 2.5:1 H2O:HNO3 at temperatures near 195 K. In contrast, freezing of 3:1 H2O:HNO3 aerosol was not observed for constant temperature experiments throughout this temperature range, yielding an upper limit of J<1.5×109 cm-3 s-1. This is the lowest experimental value determined for 3:1 H2O:HNO3 freezing rates at these temperatures. From the measured freezing rates and knowledge of the free energy of diffusion the average interfacial free energy for NAD in a 2:1 H2O:HNO3 solution was determined to be σ = 25.2 ergs cm-2. A limit for the interfacial free energy was placed on 3:1 H2O:HNO3 particles, for which freezing was not observed. These data imply that if aerosols reach compositions more concentrated than 3:1 H2O:HNO3 in the atmosphere, NAD may play a role in polar stratospheric cloud formation.

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

    NASA Astrophysics Data System (ADS)

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

    2003-04-01

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

  14. Optical properties and chemical composition of aerosol particles at an urban location: An estimation of the aerosol mass scattering and absorption efficiencies

    NASA Astrophysics Data System (ADS)

    Titos, G.; Foyo-Moreno, I.; Lyamani, H.; Querol, X.; Alastuey, A.; Alados-Arboledas, L.

    2012-02-01

    We investigated aerosol optical properties, mass concentration and chemical composition over a 1 year period (from March 2006 to February 2007) at an urban site in Southern Spain (Granada, 37.18°N, 3.58°W, 680 m above sea level). Light-scattering and absorption measurements were performed using an integrating nephelometer and a MultiAngle Absorption Photometer (MAAP), respectively, with no aerosol size cut-off and without any conditioning of the sampled air. PM10 and PM1 (ambient air levels of atmospheric particulate matter finer than 10 and 1 microns) were collected with two high volume samplers, and the chemical composition was investigated for all samples. Relative humidity (RH) within the nephelometer was below 50% and the weighting of the filters was also at RH of 50%. PM10 and PM1 mass concentrations showed a mean value of 44 ± 19 μg/m3 and 15 ± 7 μg/m3, respectively. The mineral matter was the major constituent of the PM10-1 fraction (contributing more than 58%) whereas organic matter and elemental carbon (OM+EC) contributed the most to the PM1 fraction (around 43%). The absorption coefficient at 550 nm showed a mean value of 24 ± 9 Mm-1 and the scattering coefficient at 550 nm presented a mean value of 61 ± 25 Mm-1, typical of urban areas. Both the scattering and the absorption coefficients exhibited the highest values during winter and the lowest during summer, due to the increase in the anthropogenic contribution and the lower development of the convective mixing layer during winter. A very low mean value of the single scattering albedo of 0.71 ± 0.07 at 550 nm was calculated, suggesting that urban aerosols in this site contain a large fraction of absorbing material. Mass scattering and absorption efficiencies of PM10 particles exhibited larger values during winter and lower during summer, showing a similar trend to PM1 and opposite to PM10-1. This seasonality is therefore influenced by the variations on PM composition. In addition, the mass

  15. Liquid-liquid phase separation in aerosol particles: Dependence on O:C, organic functionalities, and compositional complexity

    NASA Astrophysics Data System (ADS)

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

    2012-10-01

    Atmospheric aerosol particles may undergo liquid-liquid phase separation (LLPS) when exposed to varying relative humidity. In this study we investigated the occurrence of LLPS for mixtures consisting of up to ten organic compounds, ammonium sulfate, and water in relationship with the organic oxygen-to-carbon (O:C) ratio. LLPS always occurred for O:C < 0.56, never occurred for O:C > 0.80, and depended on the specific types and compositions of organic functional groups in the regime 0.56 < O:C < 0.80. In the intermediate regime, mixtures with a high share of aromatic compounds shifted the limit of occurrence of LLPS to lower O:C ratios. The number of mixture components and the spread of the O:C range did not notably influence the conditions for LLPS to occur. Since in ambient aerosols O:C range typically between 0.2 and 1.0, LLPS is expected to be a common feature of tropospheric aerosols.

  16. Sulfur Isotopic Compositions of Individual Aerosol Particles from Below and Within Stratocumulus Clouds over the Southeast Pacific Ocean During VOCALS

    NASA Astrophysics Data System (ADS)

    Bose, M.; Anderson, J. R.; Twohy, C. H.; Williams, P.

    2012-12-01

    The VAMOS Ocean-Cloud-Atmosphere-Land Study Regional Experiment (VOCALS-Rex) was a large multi-national field experiment that collected data and samples from a region of the southeast Pacific with the world's largest stratocumulus cloud systems. Samples examined here are residues of cloud droplets and ambient particles from below the clouds collected during flights of the NCAR C-130 off the coast of Chile. Selected samples were studied using scanning electron microscopy (SEM) and secondary ion mass spectrometry (SIMS) in order to contribute to the understanding of the source of non-sea-salt sulfate in this region. Particles in the size range from 0.2 to 1μm diameter on holey and lacey carbon were characterized by SEM combined with energy dispersive spectrometry (EDS), thus identifying sulfur-containing particles. Subsequently, sulfur ion imaging of identified sea salt, ammonium sulfate and sodium sulfate particles was done with the Cameca Ametek NanoSIMS 50L at Arizona State University. A <1pA Cs+ beam was rastered over 5×5μm2 or 10×10μm2 areas while secondary ions (12C-, 16O-, 32S-, 34S-, 35Cl-) and secondary electrons were collected simultaneously at high mass resolution (m/Δm>10000). Each measurement typically consists of 5 to 8 frames (~5.4 min/frame). NIST barium sulfate and ammonium sulfate particles were used as isotopic standards. Preliminary analyses on a small pool of VOCALS individual particles show a wide range in sulfur isotopic compositions (δ34S = -56 to +41‰). In addition, the in-cloud particles are enriched in 32S, while the ambient particles exhibit 34S excesses. Isotopic data on a large inventory of particles is being currently acquired, which will be presented at the meeting. Data will be used to investigate sulfur sources (marine vs. continental) and the processing of aerosols through sulfate formation.

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

    SciTech Connect

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

    1995-06-01

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

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

    DOE PAGES

    Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; Brune, W. H.; Hunter, J. F.; Kroll, J. H.; Cummings, M. J.; Brogan, J. F.; Parmar, Y.; Worsnop, D. R.; et al

    2015-03-18

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

  19. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

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

    2003-01-01

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

  20. Apparatus for rapid measurement of aerosol bulk chemical composition

    DOEpatents

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

    2006-04-18

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

  1. Time- and size-resolved chemical composition of submicron particles in Pittsburgh: Implications for aerosol sources and processes

    NASA Astrophysics Data System (ADS)

    Zhang, Qi; Canagaratna, Manjula R.; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis

    2005-04-01

    An Aerodyne aerosol mass spectrometer (AMS) was deployed at the Pittsburgh Environmental Protection Agency Supersite from 7 to 22 September 2002 as part of the Pittsburgh Air Quality Study (PAQS). The main objectives of this deployment were to characterize the concentrations, size distributions, and temporal variations of nonrefractory (NR) chemical species in submicron particles (approximately PM1) and to further develop and evaluate the AMS. Reasonably good agreement was observed on particle concentrations, composition, and size distributions between the AMS data and measurements from collocated instruments (given the difference between the PM1 and PM2.5 size cuts), including TEOM, semicontinuous sulfate, 2-hour- and 24-hour-averaged organic carbon, SMPS, 4-hour-averaged ammonium, and micro-orifice uniform deposit impactor. Total NR-PM1 mass concentration in Pittsburgh accumulates over periods of several days punctuated with rapid cleaning due to rain or air mass changes. Sulfate and organics are the major NR-PM1 components while the concentrations of nitrate and chloride are generally low. Significant amounts of ammonium, which most of the time are consistent with sulfate present as ammonium sulfate, are also present in particles. However, there are periods when the aerosols are relatively acidic and more than 50% of sulfate is estimated to be in the form of ammonium bisulfate. No major enhancement of the organic concentration is observed during these acidic periods, which suggests that acid-catalyzed SOA formation was not an important process during this study. Size distributions of particulate sulfate, ammonium, organics, and nitrate vary on timescales of hours to days, showing unimodal, bimodal and even trimodal characteristics. The accumulation mode (peaking around 350-600 nm in vacuum aerodynamic diameter for the mass distributions) and the ultrafine mode (<100 nm) are observed most frequently. The accumulation mode is dominated by sulfate that appears to

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

    PubMed

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

    2015-06-24

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

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

    PubMed

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

    2015-06-24

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

  4. Seasonality of new particle formation in Vienna, Austria - Influence of air mass origin and aerosol chemical composition

    NASA Astrophysics Data System (ADS)

    Wonaschütz, Anna; Demattio, Anselm; Wagner, Robert; Burkart, Julia; Zíková, Naděžda; Vodička, Petr; Ludwig, Wolfgang; Steiner, Gerhard; Schwarz, Jaroslav; Hitzenberger, Regina

    2015-10-01

    The impact of air mass origin and season on aerosol chemical composition and new particle formation and growth events (NPF events) in Vienna, Austria, is investigated using impactor samples from short-term campaigns and two long-term number size distribution datasets. The results suggest that air mass origin is most important for bulk PM concentrations, chemical composition of the coarse fraction (>1.5 μm) and the mass size distribution, and less important for chemical composition of the fine fraction (<1.5 μm). Continental air masses (crustal elements) were distinguished from air masses of marine origin (traces of sea salt). NPF events were most frequent in summer (22% of measurement days), and least frequent in winter (3% of measurement days). They were associated with above-average solar radiation and ozone concentrations, but were largely independent of PM2.5. Air mass origin was a secondary influence on NPF, largely through its association with meteorological conditions. Neither a strong dependence on the PM2.5 loading of the air masses, nor indications of a source area for NPF precursors outside the city were found.

  5. Ice nucleation, shape, and composition of aerosol particles in one of the most polluted cities in the world: Ulaanbaatar, Mongolia

    NASA Astrophysics Data System (ADS)

    Hasenkopf, Christa A.; Veghte, Daniel P.; Schill, Gregory P.; Lodoysamba, Sereeter; Freedman, Miriam Arak; Tolbert, Margaret A.

    2016-08-01

    Air pollution is attributable to 7 million deaths per year, or one out of every eight deaths globally. In particular, high concentrations of particulate matter (PM), a major air pollutant, have significant impacts on health and regional climate in urban centers. Many of the most polluted places, largely in developing countries, go severely understudied. Additionally, high particulate matter levels can have an impact on the microphysical properties of clouds, impacting precipitation and regional climate. Semi-arid regions can be especially affected by small changes in precipitation. Here we characterize the physical and chemical properties of PM in one of the most PM-polluted cities in the world: Ulaanbaatar, Mongolia, a semi-arid region in central Asia. Twice monthly aerosol samples were collected over 10 months from a central location and analyzed for composition and ice nucleation activity. Almost all particles collected were inhalable, consisting primarily of mineral dust, soot, and sulfate-organic. In winter, all classes of PM increase in concentration, with increased sulfur concentrations, and the particles are less active towards heterogeneous ice nucleation. In addition, concurrent monthly average PM10, SO2, NOx, and O3 levels and meteorological data at a nearby location are reported and made publicly available. These measurements provide an unprecedented seasonal characterization of the size, shape, chemical structure, and ice nucleating activity of PM data from Ulaanbaatar. This 10-month field study, exploring a variety of aerosol properties in Ulaanbaatar, Mongolia, is one of very few such studies conducted in the region or in such a highly polluted environment. The results of this study may inform work done in other similarly situated and polluted cities in Asia and elsewhere.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  7. 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

  8. Measuring the temporal evolution of aerosol composition in a remote marine environment influenced by Saharan dust outflow using a new single particle mass spectrometer.

    NASA Astrophysics Data System (ADS)

    Marsden, Nicholas; Williams, Paul; Flynn, Michael; Taylor, Jonathan; Liu, Dantong; Allan, James; Coe, Hugh

    2016-04-01

    Refractory material constitutes a significant fraction of the atmospheric aerosol burden and has a strong influence on climate through the direct radiative effect and aerosol-cloud interactions, particularly in cold and mixed phase clouds. Composition of refractory aerosols is traditionally measured using off-line analytical techniques such as filter analyses. However, when using off-line techniques the temporal evolution of the data set is lost, meaning the measurements are difficult to relate to atmospheric processes. Recently, single particle mass spectrometry (SPMS) has proven a useful tool for the on-line study of refractory aerosols with the ability to probe size resolved chemical composition with high temporal resolution on a particle by particle basis. A new Laser Ablation Aerosol Time-of-Flight (LAAP-TOF) SPMS instrument with a modified optical detection system was deployed for ground based measurements at Praia, Cape Verde during the Ice in Cloud - Dust (ICE-D) multi-platform campaign in August 2015. A primary aim of the project was to evaluate the impact of Saharan dust on ice nucleation in mixed phase clouds. The instrument was operated over a 16 day period in which several hundred thousand single particle mass spectra were obtained from air masses with back trajectories traversing the Mid-Atlantic, Sahara Desert and West Africa. The data presented indicate external mixtures of sea salt and silicate mineral dust internally mixed with secondary species that are consistent with long range transport to a remote marine environment. The composition and size distributions measured with the LAAP-TOF are compared with measurements from an aerodynamic particle sizer (APS), Single Particle Soot Photometer (SP2), and data from SEM-EDX analysis of filter samples. The particle number fraction identified as silicate mineral from the mass spectra correlates with a fraction of the incandescent particles measured with the SP2. We discuss the suitability of the modified

  9. Particle size dependent response of aerosol counters

    NASA Astrophysics Data System (ADS)

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

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-06-01

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

  11. Laser-Assisted Analysis of Aerosol Particles

    NASA Technical Reports Server (NTRS)

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

    1985-01-01

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

  12. Mixing state, composition, and sources of fine aerosol particles in the Qinghai-Tibetan Plateau and the influence of agricultural biomass burning

    NASA Astrophysics Data System (ADS)

    Li, W. J.; Chen, S. R.; Xu, Y. S.; Guo, X. C.; Sun, Y. L.; Yang, X. Y.; Wang, Z. F.; Zhao, X. D.; Chen, J. M.; Wang, W. X.

    2015-09-01

    Transmission electron microscopy (TEM) was employed to obtain morphology, size, composition, and mixing state of background fine particles with diameter less than 1 μm in the Qinghai-Tibetan Plateau (QTP) during 15 September to 15 October 2013. Individual aerosol particles mainly contained secondary inorganic aerosols (SIA-sulfate and nitrate) and organics during clean periods (PM2.5: particles less than 2.5 μg m-3). The presence of KCl-NaCl associated with organics and an increase of soot particles suggest that an intense biomass burning event caused the highest PM2.5 concentrations (> 30 μg m-3) during the study. A large number fraction of the fly ash-containing particles (21.73 %) suggests that coal combustion emissions in the QTP significantly contributed to air pollutants at the median pollution level (PM2.5: 10-30 μg m-3). We concluded that emissions from biomass burning and from coal combustion both constantly contribute to anthropogenic particles in the QTP atmosphere. Based on size distributions of individual particles in different pollution levels, we found that gas condensation on existing particles is an important chemical process for the formation of SIA with organic coating. TEM observations show that refractory aerosols (e.g., soot, fly ash, and visible organic particles) likely adhere to the surface of SIA particles larger than 200 nm due to coagulation. Organic coating and soot on surface of the aged particles likely influence their hygroscopic and optical properties in the QTP, respectively. To our knowledge, this study reports the first microscopic analysis of fine particles in the background QTP air.

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

    NASA Astrophysics Data System (ADS)

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

    2013-01-01

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

  14. Wind reduction by aerosol particles

    NASA Astrophysics Data System (ADS)

    Jacobson, Mark Z.; Kaufman, Yoram J.

    2006-12-01

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

  15. 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.

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

    NASA Astrophysics Data System (ADS)

    Gao, Yuan; Anderson, James R.

    2001-08-01

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

  17. 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.

  18. Ion composition of coarse and fine particles in Iasi, north-eastern Romania: Implications for aerosols chemistry in the area

    NASA Astrophysics Data System (ADS)

    Arsene, Cecilia; Olariu, Romeo Iulian; Zarmpas, Pavlos; Kanakidou, Maria; Mihalopoulos, Nikolaos

    2011-02-01

    Atmospheric loadings of the aerosols coarse (particles of AED > 1.5 μm) and fine fractions (particles of AED < 1.5 μm) were determined in Iasi, north-eastern Romania from January 2007 to March 2008. Concentrations of water soluble ions (SO 42-, NO 3-, Cl -, C 2O 42-, NH 4+, K +, Na +, Ca 2+ and Mg 2+) were measured using ion chromatography (IC). In the coarse particles, calcium and carbonate are the main ionic constituents (˜65%), whereas in the fine particles SO 42-, NO 3-, Cl - and NH 4+ are the most abundant. Temperature and relative humidity (RH) associated with increased concentrations of specific ions might be the main factors controlling the aerosol chemistry at the investigated site. From August 2007 to March 2008 high RH (as high as 80% for about 82% of the investigated period) was prevailing in Iasi and the collected particles were expected to have deliquesced and form an internal mixture. We found that in fine particles ammonium nitrate (NH 4NO 3) is important especially under conditions of NH 4+/SO 42- ratio higher than 1.5 and high RH (RH above deliquescence of NH 4Cl, NH 4NO 3 and (NH 4) 2SO 4). At the investigated site large ammonium artifacts may occur due to inter-particle interaction especially under favorable meteorological conditions. A methodology for estimating the artifact free ambient ammonium concentration is proposed for filter pack sampling data of deliquesced particles. Nitrate and sulfate ions in coarse particles are probably formed via reactions of nitric and sulfuric acid with calcium carbonate and sodium chloride which during specific seasons are abundant at the investigated site. In the fine mode sulfate concentration maximized during summer (due to enhanced photochemistry) and winter (due to high concentration of SO 2 emitted from coal burning). Natural contributions, dust or sea-salt related, prevail mainly in the coarse particles. From May 2007 to August 2007, when air masses originated mainly from Black Sea, in the coarse

  19. 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

  20. 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.

  1. Rapid Measurements of Aerosol Ionic Composition and 3-10 nm Particle Size Distributions On The NASA P3 To Better Quantify Processes Affecting Aerosols Advected From East Asia

    NASA Technical Reports Server (NTRS)

    Weber, Rodney J.

    2004-01-01

    The Particle Into Liquid Sample (PILS) was deployed on the NASA P3 for airborne measurements of fine particle ionic chemical composition. The data have been quality assured and reside in the NASA data archive. We have analyzed our data to characterize the sources and atmospheric processing of fine aerosol particles advected from the region during the experiments. Fine particle water-soluble potassium was found to serve as a useful aerosol tracer for biomass smoke. Ratios of PILS potassium to sulfate are used as a means of estimating the percent contribution of biomass burning to fine particle mass in mixed plumes advecting from Asia. The high correlations between K+ and NO3(sup -) and NH4(sup +)' indicated that biomass burning was a significant source of these aerosol compounds in the region. It is noteworthy that the air mass containing the highest concentrations of fine particles recorded in all of ACE-Asia and TRACE-P appeared to be advecting from the Bejing/Tientsin urban region and also had the highest K(+), NO3(sup -) and NH4(sup +) concentrations of both studies. Based on K+/SO4(sup 2-) ratio's, we estimated that the plume was composed of approx. 60% biomass burning emissions, possibly from the use of bio-fuels in the urban regions.

  2. Phase transitions and morphologies of aerosol particles

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

  3. Optical properties of mineral dust aerosol including analysis of particle size, composition, and shape effects, and the impact of physical and chemical processing

    NASA Astrophysics Data System (ADS)

    Alexander, Jennifer Mary

    Atmospheric mineral dust has a large impact on the earth's radiation balance and climate. The radiative effects of mineral dust depend on factors including, particle size, shape, and composition which can all be extremely complex. Mineral dust particles are typically irregular in shape and can include sharp edges, voids, and fine scale surface roughness. Particle shape can also depend on the type of mineral and can vary as a function of particle size. In addition, atmospheric mineral dust is a complex mixture of different minerals as well as other, possibly organic, components that have been mixed in while these particles are suspended in the atmosphere. Aerosol optical properties are investigated in this work, including studies of the effect of particle size, shape, and composition on the infrared (IR) extinction and visible scattering properties in order to achieve more accurate modeling methods. Studies of particle shape effects on dust optical properties for single component mineral samples of silicate clay and diatomaceous earth are carried out here first. Experimental measurements are modeled using T-matrix theory in a uniform spheroid approximation. Previous efforts to simulate the measured optical properties of silicate clay, using models that assumed particle shape was independent of particle size, have achieved only limited success. However, a model which accounts for a correlation between particle size and shape for the silicate clays offers a large improvement over earlier modeling approaches. Diatomaceous earth is also studied as an example of a single component mineral dust aerosol with extreme particle shapes. A particle shape distribution, determined by fitting the experimental IR extinction data, used as a basis for modeling the visible light scattering properties. While the visible simulations show only modestly good agreement with the scattering data, the fits are generally better than those obtained using more commonly invoked particle shape

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

    NASA Astrophysics Data System (ADS)

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

    2014-06-01

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

  5. 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.

  6. Subarctic atmospheric aerosol composition: 1. Ambient aerosol characterization

    SciTech Connect

    Friedman, Beth; Herich, Hanna; Kammermann, Lukas; Gross, Deborah S.; Ameth, Almut; Holst, Thomas; Lohmann, U.; Cziczo, Daniel J.

    2009-07-10

    Sub-Arctic aerosol was sampled during July 2007 at the Abisko Research Station Stordalen field site operated by the Royal Swedish Academy of Sciences. Located in northern Sweden at 68º latitude and 385 meters above sea level (msl), this site is classified as a semi-continuous permafrost mire. Number density, size distribution, cloud condensation nucleus properties, and chemical composition of the ambient aerosol were determined. Backtrajectories showed that three distinct airmasses were present over Stordalen during the sampling period. Aerosol properties changed and correlated with airmass origin to the south, northeast, or west. We observe that Arctic aerosol is not compositionally unlike that found in the free troposphere at mid-latitudes. Internal mixtures of sulfates and organics, many on insoluble biomass burning and/or elemental carbon cores, dominate the number density of particles from ~200 to 2000 nm aerodynamic diameter. Mineral dust which had taken up gas phase species was observed in all airmasses. Sea salt, and the extent to which it had lost volatile components, was the aerosol type that most varied with airmass.

  7. Sources and transformations of atmospheric aerosol particles

    NASA Astrophysics Data System (ADS)

    Cross, Eben Spencer

    transported towards Europe. In this study, particles were highly processed prior to sampling, with residence times of a few days in the atmosphere. The MILAGRO campaign focused on the evolution of the Mexico City plume as it was transported north. During this study, regional and locally emitted particles were measured with residence times varying from minutes to days in the atmosphere. In both studies, the light scattering - AMS system provided detailed information about the density and composition of single particles, leading to important insights into how atmospheric processing transforms the particle properties. In Mexico City, the light scattering-AMS system was used for the first time as a true single particle mass spectrometer and revealed specific details about the atmospheric processing of primary particles from combustion sources. To quantify the radiative effects of the particles on climate, the processing and ultimate fate of primary emissions (often containing black carbon or soot) must be understood. To provide a solid basis for the interpretation of the data obtained during the field studies, experiments were conducted with a well characterized soot generation-sampling system developed by the Boston College research group. The laboratory soot source was combined with the light scattering - AMS system and a Cloud Condensation Nuclei Counter (CCNC) to measure the change in cloud-forming activity of soot particles as they are processed in the atmosphere. Because of the importance of black carbon in the atmosphere, several instruments have been developed to measure black carbon. In July of 2008, an intercomparison study of 18 instruments was conducted in the Boston College laboratory, with soot particles produced and processed to mimic a wide range of atmospherically-relevant conditions. Transformations in the physical, chemical, and optical properties of soot particles were monitored with the combined suite of aerosol instrumentation. Results from the

  8. Test-Aerosol Generator For Calibrating Particle Counters

    NASA Technical Reports Server (NTRS)

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

    1996-01-01

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

  9. Long-term real-time measurements of aerosol particle composition in Beijing, China: seasonal variations, meteorological effects, and source analysis

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Wang, Z. F.; Du, W.; Zhang, Q.; Wang, Q. Q.; Fu, P. Q.; Pan, X. L.; Li, J.; Jayne, J.; Worsnop, D. R.

    2015-09-01

    High concentrations of fine particles (PM2.5) are frequently observed during all seasons in Beijing, China, leading to severe air pollution and human health problems in this megacity. In this study, we conducted real-time measurements of non-refractory submicron aerosol (NR-PM1) species (sulfate, nitrate, ammonium, chloride, and organics) in Beijing using an Aerodyne Aerosol Chemical Speciation Monitor for 1 year, from July 2011 to June 2012. This is the first long-term, highly time-resolved (~ 15 min) measurement of fine particle composition in China. The seasonal average (±1σ) mass concentration of NR-PM1 ranged from 52 (±49) μg m-3 in the spring season to 62 (±49) μg m-3 in the summer season, with organics being the major fraction (40-51 %), followed by nitrate (17-25 %) and sulfate (12-17 %). Organics and chloride showed pronounced seasonal variations, with much higher concentrations in winter than in the other seasons, due to enhanced coal combustion emissions. Although the seasonal variations of secondary inorganic aerosol (SIA, i.e., sulfate + nitrate + ammonium) concentrations were not significant, higher contributions of SIA were observed in summer (57-61 %) than in winter (43-46 %), indicating that secondary aerosol production is a more important process than primary emissions in summer. Organics presented pronounced diurnal cycles that were similar among all seasons, whereas the diurnal variations of nitrate were mainly due to the competition between photochemical production and gas-particle partitioning. Our data also indicate that high concentrations of NR-PM1 (> 60 μg m-3) are usually associated with high ambient relative humidity (RH) (> 50 %) and that severe particulate pollution is characterized by different aerosol composition in different seasons. All NR-PM1 species showed evident concentration gradients as a function of wind direction, generally with higher values associated with wind from the south, southeast or east. This was consistent

  10. Composite powder particles

    NASA Technical Reports Server (NTRS)

    Parker, Donald S. (Inventor); MacDowell, Louis G. (Inventor)

    2009-01-01

    A liquid coating composition including a coating vehicle and composite powder particles disposed within the coating vehicle. Each composite powder particle may include a magnesium component, a zinc component, and an indium component.

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

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

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

    DOE PAGES

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

    2015-03-16

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-08-01

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

  14. Glassy aerosols heterogeneously nucleate cirrus ice particles

    NASA Astrophysics Data System (ADS)

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

    2010-05-01

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

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

    SciTech Connect

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

    2010-09-11

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

  16. 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.

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

    NASA Astrophysics Data System (ADS)

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

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

  18. Equilibrium absorptive partitioning theory between multiple aerosol particle modes

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

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

    SciTech Connect

    Davidovits, Paul

    2015-10-20

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

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

    PubMed

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

    2015-07-15

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

  1. Characteristics of aerosolized ice forming marine biogenic particles

    NASA Astrophysics Data System (ADS)

    Alpert, Peter A.

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

  2. Airborne Measurements of Coarse Mode Aerosol Composition and Abundance

    NASA Astrophysics Data System (ADS)

    Froyd, K. D.; Murphy, D. M.; Brock, C. A.; Ziemba, L. D.; Anderson, B. E.; Wilson, J. C.

    2015-12-01

    Coarse aerosol particles impact the earth's radiative balance by direct scattering and absorption of light and by promoting cloud formation. Modeling studies suggest that coarse mode mineral dust and sea salt aerosol are the dominant contributors to aerosol optical depth throughout much of the globe. Lab and field studies indicate that larger aerosol particles tend to be more efficient ice nuclei, and recent airborne measurements confirm the dominant role of mineral dust on cirrus cloud formation. However, our ability to simulate coarse mode particle abundance in large scale models is limited by a lack of validating measurements above the earth's surface. We present airborne measurements of coarse mode aerosol abundance and composition over several mid-latitude, sub-tropical, and tropical regions from the boundary layer to the stratosphere. In the free troposphere the coarse mode constitutes 10-50% of the total particulate mass over a wide range of environments. Above North America mineral dust typically dominates the coarse mode, but biomass burning particles and sea salt also contribute. In remote environments coarse mode aerosol mainly consists of internally mixed sulfate-organic particles. Both continental and marine convection can enhance coarse aerosol mass through direct lofting of primary particles and by secondary accumulation of aerosol material through cloud processing.

  3. Mexico City Aerosol Analysis during MILAGRO using High Resolution Aerosol Mass Spectrometry at the Urban Supersite (T0). Part 1: Fine Particle Composition and Organic Source Apportionment

    SciTech Connect

    Aiken, Allison; Salcedo, D.; Cubison, Michael J.; Huffman, J.; DeCarlo, Peter; Ulbrich, Ingrid M.; Docherty, Kenneth S.; Sueper, D. T.; Kimmel, Joel; Worsnop, Douglas R.; Trimborn, Achim; Northway, Megan; Stone, Elizabeth A.; Schauer, James J.; Volkamer, Rainer M.; Fortner, Edward; de Foy, B.; Wang, Jian; Laskin, Alexander; Shutthanandan, V.; Zheng, Junsheng; Zhang, Renyi; Gaffney, Jeffrey S.; Marley, Nancy A.; Paredes-Miranda, Guadalupe L.; Arnott, W. P.; Molina, Luisa T.; Sosa, G.; Jimenez, Jose L.

    2009-09-11

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identifies three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning.

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

    NASA Astrophysics Data System (ADS)

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

    2016-10-01

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

  5. Aerosol particles collected on aircraft flights over the northwestern Pacific region during the ACE-Asia campaign: Composition and major sources of the organic compounds

    NASA Astrophysics Data System (ADS)

    Simoneit, Bernd R. T.; Kobayashi, Minoru; Mochida, Michihiro; Kawamura, Kimitaka; Huebert, Barry J.

    2004-10-01

    Atmospheric particulate matter, collected over the polluted east Asia/Pacific region in spring 2001 during research flights with the National Center for Atmospheric Research (NCAR) C-130 aircraft, was analyzed for different types of organic compounds using capillary gas chromatography-mass spectrometry. More than 70 organic species were detected in the aerosols and grouped into different compound classes on the basis of functional groups, including n-alkanes, polycyclic aromatic hydrocarbons, fatty acids, dehydroabietic acid, alkanols, water-soluble sugars (including glucose, sucrose, mycose, and levoglucosan), monocarboxylic and dicarboxylic acids, urea, and phthalates. Interestingly, the water-soluble compounds (72-133 ng m-3) were found to account for 16-50% (average 34%) of the total identified compound mass (TCM). Organic compounds were further categorized into several groups to suggest their sources. Fossil fuel combustion was recognized as the most significant source for the TCM (contributing 33-80% of TCM, average 50%), followed by soil resuspension (5-25%, average 19%) and secondary oxidation products (4-15%, average 9%). In contrast, the contribution of natural sources such as terrestrial plant wax and marine lipids (fatty acids and alkanols) was relatively small (3.4% and 9.4% on average, respectively). Biomass burning was suggested to contribute only a minor portion to the TCM of the Asian aerosols during the spring season (1.4% on average based on levoglucosan). However, levoglucosan may have been hydrolyzed and/or oxidized in part during long-range transport, and therefore this value represents a lower limit. The organic compound compositions of these samples are very different from those reported for aerosol particles of the Atlantic Ocean and from the earlier data for the mid-Pacific in terms of the abundant presence of water-soluble compounds consisting of saccharides, anhydrosaccharides, and the secondary dicarboxylic acids. This study

  6. Direct shortwave forcing of climate by anthropogenic sulfate aerosol: Sensitivity to particle size, composition, and relative humidity

    SciTech Connect

    Nemesure, S.; Wagener, R.; Schwartz, S.E.

    1996-04-01

    Recent estimates of global or hemispheric average forcing of climate by anthropogenic sulfate aerosol due to scattering of shortwave radiation are uncertain by more than a factor of 2. This paper examines the sensitivity of forcing to these microphysical properties for the purposes of obtaining a better understanding of the properties required to reduce the uncertainty in the forcing.

  7. 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.

  8. 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

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

    NASA Astrophysics Data System (ADS)

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

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

  10. Aerosol chemical composition in cloud events by high resolution time-of-flight aerosol mass spectrometry.

    PubMed

    Hao, Liqing; Romakkaniemi, Sami; Kortelainen, Aki; Jaatinen, Antti; Portin, Harri; Miettinen, Pasi; Komppula, Mika; Leskinen, Ari; Virtanen, Annele; Smith, James N; Sueper, Donna; Worsnop, Douglas R; Lehtinen, Kari E J; Laaksonen, Ari

    2013-03-19

    This study presents results of direct observations of aerosol chemical composition in clouds. A high-resolution time-of-flight aerosol mass spectrometer was used to make measurements of cloud interstitial particles (INT) and mixed cloud interstitial and droplet residual particles (TOT). The differences between these two are the cloud droplet residuals (RES). Positive matrix factorization analysis of high-resolution mass spectral data sets and theoretical calculations were performed to yield distributions of chemical composition of the INT and RES particles. We observed that less oxidized hydrocarbon-like organic aerosols (HOA) were mainly distributed into the INT particles, whereas more oxidized low-volatile oxygenated OA (LVOOA) mainly in the RES particles. Nitrates existed as organic nitrate and in chemical form of NH(4)NO(3). Organic nitrates accounted for 45% of total nitrates in the INT particles, in clear contrast to 26% in the RES particles. Meanwhile, sulfates coexist in forms of acidic NH(4)HSO(4) and neutralized (NH(4))(2)SO(4). Acidic sulfate made up 64.8% of total sulfates in the INT particles, much higher than 10.7% in the RES particles. The results indicate a possible joint effect of activation ability of aerosol particles, cloud processing, and particle size effects on cloud formation.

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

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

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

  12. Predicting the Mineral Composition of Dust Aerosols

    NASA Astrophysics Data System (ADS)

    Perlwitz, J. P.; Perez, C.; Miller, R. L.; Rodriguez, S.

    2012-12-01

    Models of the soil (''mineral'') dust aerosol cycle, embedded in climate and Earth system models, are essential tools for understanding the causal relationships and feedbacks between dust and climate. Many soil dust schemes in Earth system models use a simplified representation of soil dust aerosols, where the soil dust is distinguished by size bins or size distribution modes, with a globally uniform representation of the mineralogical composition of the particles. Although models with such a simplified assumption about the properties of soil dust particles have already significantly contributed to the understanding of the role of soil dust aerosols in climate, this is a limitation for a number of reasons: 1. The response of clouds and the large-scale circulation depends on the radiative properties like the single scattering albedo, which should vary with the mineral composition of the source region; 2. Chemical processes at the surface of the soil dust particles that form sulfate and nitrate coatings depend on the dust mineral composition; 3. The availability of soil dust minerals as cloud condensation nuclei depends on their hygroscopicity, which in turn depends on the mineral composition; 4. Fertilization of phytoplankton with soluble iron, a process that influences ocean carbon uptake, depends upon mineral types. We present a new version of the soil dust scheme in the NASA GISS Earth System ModelE, which takes into account the mineral composition of the soil dust particles. Soil dust aerosols are represented as a mixture of externally and internally mixed minerals, such as Illite, Kaolinite, Smectite, Calcite, Iron(hydr)oxide, Quartz, Feldspar, and Gypsum, as well as aggregates between Iron(hydr)oxide and each of the minerals. We test two approaches to constrain the mineral composition of the soil dust particles against data from measurements published in literature as well as measurements from Izaña (Tenerife). The comparison between modeled and measured data

  13. Mexico City aerosol analysis during MILAGRO using high resolution aerosol mass spectrometry at the urban supersite (T0) - Part 1: Fine particle composition and organic source apportionment

    SciTech Connect

    Aiken, A.C.; Wang, J.; Salcedo, D.; Cubison, M. J.; Huffman, J. A.; DeCarlo, P. F.; Ulbrich, I. M.; Docherty, K. S.; Sueper, D.; Kimmel, J. R.; Worsnop, D. R.; Trimborn, A.; Northway, M.; Stone, E. A.; Schauer, J. J.; Volkamer, R. M.; Fortner, E.; de Foy, B.; Laskin, A.; Shutthanandan, V.; Zheng, J.; Zhang, R.; Gaffney, J.; Marley, N. A.; Paredes-Miranda, G.; Arnott, W. P.; Molina, L. T.; Sosa, G.; Jimenez, J. L.

    2009-09-01

    Submicron aerosol was analyzed during the MILAGRO field campaign in March 2006 at the T0 urban supersite in Mexico City with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and complementary instrumentation. Mass concentrations, diurnal cycles, and size distributions of inorganic and organic species are similar to results from the CENICA supersite in April 2003 with organic aerosol (OA) comprising about half of the fine PM mass. Positive Matrix Factorization (PMF) analysis of the high resolution OA spectra identified three major components: chemically-reduced urban primary emissions (hydrocarbon-like OA, HOA), oxygenated OA (OOA, mostly secondary OA or SOA), and biomass burning OA (BBOA) that correlates with levoglucosan and acetonitrile. BBOA includes several very large plumes from regional fires and likely also some refuse burning. A fourth OA component is a small local nitrogen-containing reduced OA component (LOA) which accounts for 9% of the OA mass but one third of the organic nitrogen, likely as amines. OOA accounts for almost half of the OA on average, consistent with previous observations. OA apportionment results from PMF-AMS are compared to the PM{sub 2.5} chemical mass balance of organic molecular markers (CMB-OMM, from GC/MS analysis of filters). Results from both methods are overall consistent. Both assign the major components of OA to primary urban, biomass burning/woodsmoke, and secondary sources at similar magnitudes. The 2006 Mexico City emissions inventory underestimates the urban primary PM{sub 2.5} emissions by a factor of {approx}4, and it is {approx}16 times lower than afternoon concentrations when secondary species are included. Additionally, the forest fire contribution is at least an order-of-magnitude larger than in the inventory.

  14. 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.

  15. Comparison of secondary organic aerosol formed with an aerosol flow reactor and environmental reaction chambers: effect of oxidant concentration, exposure time and seed particles on chemical composition and yield

    DOE PAGES

    Lambe, A. T.; Chhabra, P. S.; Onasch, T. B.; Brune, W. H.; Hunter, J. F.; Kroll, J. H.; Cummings, M. J.; Brogan, J. F.; Parmar, Y.; Worsnop, D. R.; et al

    2014-12-02

    We performed a systematic intercomparison study of the chemistry and yields of SOA generated from OH oxidation of a common set of gas-phase precursors in a Potential Aerosol Mass (PAM) continuous flow reactor and several environmental chambers. In the flow reactor, SOA precursors were oxidized using OH concentrations ranging from 2.0×108 to 2.2×1010 molec cm-3 over exposure times of 100 s. In the environmental chambers, precursors were oxidized using OH concentrations ranging from 2×106 to 2×107 molec cm-3 over exposure times of several hours. The OH concentration in the chamber experiments is close to that found in the atmosphere, butmore » the integrated OH exposure in the flow reactor can simulate atmospheric exposure times of multiple days compared to chamber exposure times of only a day or so. A linear correlation analysis of the mass spectra (m=0.91–0.92, r2=0.93–0.94) and carbon oxidation state (m=1.1, r2=0.58) of SOA produced in the flow reactor and environmental chambers for OH exposures of approximately 1011 molec cm-3 s suggests that the composition of SOA produced in the flow reactor and chambers is the same within experimental accuracy as measured with an aerosol mass spectrometer. This similarity in turn suggests that both in the flow reactor and in chambers, SOA chemical composition at low OH exposure is governed primarily by gas-phase OH oxidation of the precursors, rather than heterogeneous oxidation of the condensed particles. In general, SOA yields measured in the flow reactor are lower than measured in chambers for the range of equivalent OH exposures that can be measured in both the flow reactor and chambers. The influence of sulfate seed particles on isoprene SOA yield measurements was examined in the flow reactor. The studies show that seed particles increase the yield of SOA produced in flow reactors by a factor of 3 to 5 and may also account in part for higher SOA yields obtained in the chambers, where seed particles are

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

    SciTech Connect

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

    2015-03-16

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

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

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

  17. The Hohenpeissenberg aerosol characterization experiment (HAZE2002): Aerosol composition derived from mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hock, N.; Berresheim, H.; Borrmann, S.; Poeschl, U.; Roempp, A.; Schneider, J.

    2003-04-01

    The HAZE Experiment was conducted between 17.05.2002 and 31.05.2002, at the meteorological observatory of the Deutsche Wetterdienst (DWD) at Hohenpeissenberg (47^o48'N,11^o02'E, 985m). The objective was to make essential progress in understanding of the physical and chemical properties of the atmospheric aerosol, in particular relating to the Gas-To-Particle-Conversion and the interaction with meteorological processes. The measurements included online mass spectrometric analysis using the Aerosol Mass Spectrometer (AMS), filter samples with GC analyses of organic compounds, particle size distribution (Electrical Low Pressure Impactor (ELPI), SMPS, OPC), as well as the total particle concentration (CPC). Additionally, several gas-phase substances were measured (e.g. Benzene, Acetone). The measurements obtained with the AMS show a strong variability of the aerosol composition. The non-refractory aerosol composition was dominated by nitrate, sulphate, and organics, whereas ammonium was surprisingly low. High number concentration of up to 14000 particles/cm^3 were observed. These particles mostly had diameters between 200 nm and 400 nm and were mainly composed of ammonium sulphate and ammonium nitrate. Various meteorological conditions allowed to study their influence on the aerosol. For example, on rainy days the concentrations of ammonium sulphate particles decreased, whereas the concentrations of ammonium nitrate particles increased.

  18. 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.

  19. Supercritical Fluid Extraction and Analysis of Tropospheric Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Hansen, Kristen J.

    An integrated sampling and supercritical fluid extraction (SFE) cell has been designed for whole-sample analysis of organic compounds on tropospheric aerosol particles. The low-volume extraction cell has been interfaced with a sampling manifold for aerosol particle collection in the field. After sample collection, the entire SFE cell was coupled to a gas chromatograph; after on-line extraction, the cryogenically -focused sample was separated and the volatile compounds detected with either a mass spectrometer or a flame ionization detector. A 20-minute extraction at 450 atm and 90 ^circC with pure supercritical CO _2 is sufficient for quantitative extraction of most volatile compounds in aerosol particle samples. A comparison between SFE and thermal desorption, the traditional whole-sample technique for analyses of this type, was performed using ambient aerosol particle samples, as well as samples containing known amounts of standard analytes. The results of these studies indicate that SFE of atmospheric aerosol particles provides quantitative measurement of several classes of organic compounds. SFE provides information that is complementary to that gained by the thermal desorption analysis. The results also indicate that SFE with CO _2 can be validated as an alternative to thermal desorption for quantitative recovery of several organic compounds. In 1989, the organic constituents of atmospheric aerosol particles collected at Niwot Ridge, Colorado, along with various physical and meteorological data, were measured during a collaborative field study. Temporal changes in the composition of samples collected during summertime at the rural site were studied. Thermal desorption-GC/FID was used to quantify selected compounds in samples collected during the field study. The statistical analysis of the 1989 Niwot Ridge data set is presented in this work. Principal component analysis was performed on thirty-one variables selected from the data set in order to ascertain

  20. The Role of Aerosol Composition in Arctic Cloud Formation

    NASA Astrophysics Data System (ADS)

    Brooks, S. D.; Hiranuma, N.; Moffet, R.; Laskin, A.; Gilles, M. K.; Glen, A.

    2010-12-01

    While it has been shown that aerosol size has a direct correlation with its ability to act as an ice nucleus, the role of the composition of freshly emitted and evolving aerosol in nucleation is poorly understood. Here we use combined measurements of ice nucleation and high resolution single particle composition to provide insight on the connection between aerosol composition in ice nucleation. These measurements were collected during the Indirect and Semidirect Aerosols Campaign (ISDAC) over Barrow, AK in the springtime of 2008. In-situ ice nucleation measurements were conducted using the Texas Continuous Flow Diffusion Chamber (CFDC). The composition of ambient particles as well as residuals of cloud droplets and ice crystals were studied on a particle by particle basis using computer controlled scanning electron microscopy with energy dispersive X-ray analysis (CCSEM/EDX) and scanning transmission X-Ray microscopy coupled with near edge X-ray absorption spectroscopy (STXM/NEXAFAS). Observed IN concentrations varied from frequent values of 0.01 per liter to more than 10 per liters, depending on conditions and the availability of ice-nucleating aerosols. Ice crystals residuals collected in a fully glaciated cloud demonstrate that both particle chemistry and size requirement must be met for a particle to be an efficient ice nucleus. According to the STXM/NEXAFAS spectral maps, ice crystals residuals are characterized by insoluble cores of either large brown or black carbon (BBC) or carbonates coated by water soluble organics. In contrast, in ambient air samples collected from a biomass burning plume, many organic particles were also observed, but these were smaller and did not have insoluble cores. In-situ ice nucleation measurements show that these biomass particles have inferior ice nuclei ability, relative to those collected in the glaciated cloud. Taken together our measurements suggest that two key elements, a critical size (provided by BBC and/or carbonate

  1. 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.

  2. 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.

  3. 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.

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

    PubMed

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

    2016-09-20

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

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

    PubMed

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

    2016-09-20

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

  6. 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.

  7. Measurements of aerosol chemical composition in boreal forest summer conditions

    NASA Astrophysics Data System (ADS)

    ńijälä, M.; Junninen, H.; Ehn, M.; Petäjä, T.; Vogel, A.; Hoffmann, T.; Corrigan, A.; Russell, L.; Makkonen, U.; Virkkula, A.; Mäntykenttä, J.; Kulmala, M.; Worsnop, D.

    2012-04-01

    Boreal forests are an important biome, covering vast areas of the northern hemisphere and affecting the global climate change via various feedbacks [1]. Despite having relatively few anthropogenic primary aerosol sources, they always contain a non-negligible aerosol population [2]. This study describes aerosol chemical composition measurements using Aerodyne Aerosol Mass Spectrometer (C-ToF AMS, [3]), carried out at a boreal forest area in Hyytiälä, Southern Finland. The site, Helsinki University SMEAR II measurement station [4], is situated at a homogeneous Scots pine (Pinus sylvestris) forest stand. In addition to the station's permanent aerosol, gas phase and meteorological instruments, during the HUMPPA (Hyytiälä United Measurements of Photochemistry and Particles in Air) campaign in July 2010, a very comprehensive set of atmospheric chemistry measurement instrumentation was provided by the Max Planck Institute for chemistry, Johannes Gutenberg-University, University of California and the Finnish Meteorological institute. In this study aerosol chemical composition measurements from the campaign are presented. The dominant aerosol chemical species during the campaign were the organics, although periods with elevated amounts of particulate sulfates were also seen. The overall AMS measured particle mass concentrations varied from near zero to 27 μg/m observed during a forest fire smoke episode. The AMS measured aerosol mass loadings were found to agree well with DMPS derived mass concentrations (r2=0.998). The AMS data was also compared with three other aerosol instruments. The Marga instrument [5] was used to provide a quantitative semi-online measurement of inorganic chemical compounds in particle phase. Fourier Transform Infrared Spectroscopy (FTIR) analysis was performed on daily filter samples, enabling the identification and quantification of organic aerosol subspecies. Finally an Atmospheric Pressure Chemical Ionization Ion Trap Mass Spectrometer (APCI

  8. Mixing properties of individual submicrometer aerosol particles in Vienna

    NASA Astrophysics Data System (ADS)

    Okada, Kikuo; Hitzenberger, Regina M.

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

  9. 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.

  10. 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

  11. 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

  12. 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

  13. 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

  14. Sulfur speciation of single aerosol particles

    SciTech Connect

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

    1995-12-31

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

  15. Morphologies of aerosol particles consisting of two liquid phases

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  16. Size-Segregated Aerosol Composition and Mass Loading of Atmospheric Particles as Part of the Pacific Northwest 2001(PNW2001) Air Quality Study In Puget Sound

    NASA Astrophysics Data System (ADS)

    Disselkamp, R. S.; Barrie, L. A.; Shutthanadan, S.; Cliff, S.; Cahill, T.

    2001-12-01

    In mid-August, 2001, an aircraft-based air-quality study was performed in the Puget Sound, WA, area entitled PNW2001 (http://www.pnl.gov/pnw2001). The objectives of this field campaign were the following: 1. reveal information about the 3-dimensional distribution of ozone, its gaseous precursors and fine particulate matter during weather conditions favoring air pollution; 2. derive information about the accuracy of urban and biogenic emissions inventories that are used to drive the air quality forecast models; and 3. examine the accuracy of modeled ozone concentration with that observed. In support of these efforts, we collected time-averaged ( { ~}10 minute averages), size-segregated, aerosol composition and mass-loading information using ex post facto analysis techniques of synchrotron x-ray fluorescence (s-XRF), proton induced x-ray emissions(PIXE), proton elastic scattering (PESA), and scanning transmission ion microscopy (STIM). This is the first time these analysis techniques have been used together on samples collected from aircraft using an optimized 3-stage rotating drum impactor. In our presentation, we will discuss the aerosol components in three aerosol size fractions as identified by statistical analysis of multielemental data (including total mass, H, Na, Mg, Al, Si, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Pb) and relate variations in these components to physical aerosol properties, other gaseous trace constituents and to air mass origin.

  17. Characterization of aerosols and fibers emitted from composite materials combustion.

    PubMed

    Chivas-Joly, C; Gaie-Levrel, F; Motzkus, C; Ducourtieux, S; Delvallée, A; De Lagos, F; Nevé, S Le; Gutierrez, J; Lopez-Cuesta, J-M

    2016-01-15

    This work investigates the aerosols emitted during combustion of aircraft and naval structural composite materials (epoxy resin/carbon fibers and vinyl ester/glass fibers and carbon nanotubes). Combustion tests were performed at lab-scale using a modified cone calorimeter. The aerosols emitted have been characterized using various metrological devices devoted to the analysis of aerosols. The influence of the nature of polymer matrices, the incorporation of fibers and carbon nanotubes as well as glass reinforcements on the number concentration and the size distribution of airborne particles produced, was studied in the 5 nm-10 μm range. Incorporation of carbon fibers into epoxy resin significantly reduced the total particle number concentration. In addition, the interlaced orientation of carbon fibers limited the particles production compared to the composites with unidirectional one. The carbon nanotubes loading in vinyl ester resin composites influenced the total particles production during the flaming combustion with changes during kinetics emission. Predominant populations of airborne particles generated during combustion of all tested composites were characterized by a PN50 following by PN(100-500). PMID:26348148

  18. Particle size distribution of indoor aerosol sources

    SciTech Connect

    Shah, K.B.

    1990-10-24

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

  19. 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

    goes through a pumped counterflow virtual impactor (PCVI), which rejects aerosol particles and transmits larger particles that are either droplet residuals or coagulated particles. The larger particles are sent to 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 from 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 present the collection efficiency data of a suite of dust particles with well-defined types, sizes and concentrations under atmospherically relevant temperatures and relative humidity conditions.

  20. Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

    NASA Astrophysics Data System (ADS)

    Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

    2015-06-01

    Aerosol particles were characterized by an Aerodyne aerosol chemical speciation monitor along with various collocated instruments in Beijing, China, to investigate the role of fireworks (FW) and secondary aerosol in particulate pollution during the Chinese Spring Festival of 2013. Three FW events, exerting significant and short-term impacts on fine particles (PM2.5), were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW were shown to have a large impact on non-refractory potassium, chloride, sulfate, and organics in submicron aerosol (PM1), of which FW organics appeared to be emitted mainly in secondary, with its mass spectrum resembling that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated the total PM1 mass on average, accounting for 63-82% during nine PEs in this study. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impact of reduced anthropogenic emissions on aerosol chemistry in the city. Primary species showed ubiquitous reductions during the holiday period with the largest reduction being in cooking organic aerosol (OA; 69%), in nitrogen monoxide (54%), and in coal combustion OA (28%). Secondary sulfate, however, remained only slightly changed, and the SOA and the total PM2.5 even slightly increased. Our results have significant implications for controlling local primary source emissions during PEs, e.g., cooking and traffic activities. Controlling these factors might have a limited effect on improving air quality in the megacity of Beijing, due to the dominance of SPM from regional transport in aerosol particle composition.

  1. 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

  2. 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

  3. Studies of Ambient and Chamber Aerosol Composition using the Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Craven, Jill Suzanne

    This thesis presents composition measurements for atmospherically relevant inorganic and organic aerosol from laboratory and ambient measurements using the Aerodyne aerosol mass spectrometer. Studies include the oxidation of dodecane in the Caltech environmental chambers, and several aircraft- and ground-based field studies, which include the quantification of wildfire emissions off the coast of California, and Los Angeles urban emissions. The oxidation of dodecane by OH under low NO conditions and the formation of secondary organic aerosol (SOA) was explored using a gas-phase chemical model, gas-phase CIMS measurements, and high molecular weight ion traces from particlephase HR-TOF-AMS mass spectra. The combination of these measurements support the hypothesis that particle-phase chemistry leading to peroxyhemiacetal formation is important. Positive matrix factorization (PMF) was applied to the AMS mass spectra which revealed three factors representing a combination of gas-particle partitioning, chemical conversion in the aerosol, and wall deposition. Airborne measurements of biomass burning emissions from a chaparral fire on the central Californian coast were carried out in November 2009. Physical and chemical changes were reported for smoke ages 0--4 h old. CO 2 normalized ammonium, nitrate, and sulfate increased, whereas the normalized OA decreased sharply in the first 1.5--2 h, and then slowly increased for the remaining 2 h (net decrease in normalized OA). Comparison to wildfire samples from the Yucatan revealed that factors such as relative humidity, incident UV radiation, age of smoke, and concentration of emissions are important for wildfire evolution. Ground-based aerosol composition is reported for Pasadena, CA during the sumix mer of 2009. The OA component, which dominated the submicron aerosol mass, was deconvolved into hydrocarbon-like organic aerosol (HOA), semi-volatile oxidized organic aerosol (SVOOA), and low-volatility oxidized organic aerosol

  4. Individual Aerosol Particle Types Produced by Savanna Burning

    NASA Astrophysics Data System (ADS)

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

    2001-12-01

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

  5. Using Brittle Fragmentation Theory to represent Aerosol Mineral Composition

    NASA Astrophysics Data System (ADS)

    Pérez García-Pando, C.; Miller, R. L.; Perlwitz, J. P.

    2014-12-01

    Improved estimates of dust aerosol effects upon climate require the characterization of dust mineral and chemical composition. Regional variations in soil mineral composition lead to variations in dust aerosol composition. Yet, deriving aerosol mineral content also requires knowledge of the parent soil size distribution along with the fragmentation of soil particles and aggregates during the emission process. These processes modify the size distribution and mineral abundance of the emitted aerosols compared to the parent soil. An additional challenge for modeling is that global atlases of soil texture and composition are based on wet sieving, a technique that breaks the aggregates, particularly phyllosilicates, that are encountered in natural soils, drastically altering the original size distribution of the soil that is subject to wind erosion. We propose both a semi-empirical and theoretical method to constrain the size-resolved mineral composition of emitted dust aerosols based on global atlases of soil texture and composition. Our semi-empirical method re-aggregates clay phyllosilicate minerals into larger soil particle sizes and constrains the size distribution of each emitted mineral based on observed mineral distributions at the source. Our theoretical method extends Kok's brittle fragmentation theory to individual minerals. To this end we reconstruct the undisturbed size distribution for each mineral as a function of soil texture and soil type and calculate the emitted size distribution applying brittle fragmentation and assuming homogeneous fragmentation properties among the mineral aggregates. These approaches were tested within the NASA GISS Earth System ModelE. We discuss the improvements achieved and suggest future developments.

  6. 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

  7. 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

  8. Aerosol composition and sources during the Chinese Spring Festival: fireworks, secondary aerosol, and holiday effects

    NASA Astrophysics Data System (ADS)

    Jiang, Q.; Sun, Y. L.; Wang, Z.; Yin, Y.

    2014-08-01

    Aerosol particles were characterized by an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) along with various collocated instruments in Beijing, China to investigate the aerosol composition and sources during the Chinese Spring Festival, 2013. Three fireworks (FW) events exerting significant and short-term impacts on fine particles (PM2.5) were observed on the days of Lunar New Year, Lunar Fifth Day, and Lantern Festival. The FW showed major impacts on non-refractory potassium, chloride, sulfate, and organics in PM1, of which the FW organics appeared to be mainly secondary with its mass spectrum resembling to that of secondary organic aerosol (SOA). Pollution events (PEs) and clean periods (CPs) alternated routinely throughout the study. Secondary particulate matter (SPM = SOA + sulfate + nitrate + ammonium) dominated PM1 accounting for 63-82% during the nine PEs observed. The elevated contributions of secondary species during PEs resulted in a higher mass extinction efficiency of PM1 (6.4 m2 g-1) than that during CPs (4.4 m2 g-1). The Chinese Spring Festival also provides a unique opportunity to study the impacts of reduced anthropogenic emissions on aerosol chemistry in the city. The primary species showed ubiquitous reductions during the holiday period with the largest reduction for cooking OA (69%), nitrogen monoxide (54%), and coal combustion OA (28%). The secondary sulfate, however, remained minor change, and the SOA and the total PM2.5 even slightly increased. These results have significant implications that controlling local primary source emissions, e.g., cooking and traffic activities, might have limited effects on improving air quality during PEs when SPM that is formed over regional scales dominates aerosol particle composition.

  9. 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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

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

    PubMed

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

    2010-07-01

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

  12. 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

  13. A study on major inorganic ion composition of atmospheric aerosols.

    PubMed

    Salve, P R; Krupadam, R J; Wate, S R

    2007-04-01

    Atmospheric aerosol samples were collected from Akola and Buldana region covering around 40 sqkm area during October-November 2002 and were analyzed for ten major inorganic ions namely F-, Cl-, NO3-, SO4(2-), PO4(2-), Na+, K+, Ca2+, Mg2+ and NH4+ using ion chromatographic technique. The average mass of aerosols was found to be 225.81 microg/m3 with standard deviation of 31.29 and average total water soluble load of total cations and anions was found to be 4.32 microg/m3. The concentration of ions in samples showed a general pattern as SO4(2-) > NO3- > Cl- > PO4(2-) > F- for anions and Na+ > Ca2+ > NH4+ > Mg2+ > K+ for cations. The overall composition of the aerosols was taken into account to identify the sources. The trend showed higher concentration of sodium followed by calcium, sulfate, nitrate, phosphate and ammoinum and found to be influenced by terrestrial sources. The presence of SO4(2-) and NO3- in aerosols may be due to re-suspension of soil particles. Ca2+, Mg2+ and Cl- are to be derived from soil materials. The presence of NH4+ may be attributed to the reaction of NH3 vapors with acidic gases may react or condense on an acidic particle surface of anthropogenic origin. The atmospheric aerosol is slightly acidic due to neutralization of basicity by SO2 and NO(x).

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

    DOE PAGES

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

    2015-09-25

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

  16. 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

  17. 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

  18. Spectroscopic studies of the size and composition of single aerosol droplets

    NASA Astrophysics Data System (ADS)

    Reid, Jonathan P.; Meresman, Helena; Mitchem, Laura; Symes, Rachel

    The characterization of aerosol properties and processes, non-intrusively and directly, poses a severe analytical challenge. In order to understand the role of aerosols in often complex environments, it is necessary to probe the particles in situ and without perturbation. Sampling followed by end-of-line analysis can lead to perturbations in particle composition, morphology and size, particularly when analysing liquid aerosol droplets containing volatile components. Optical spectroscopy can provide a strategy for the direct assessment of particle size, composition and phase. We review here the application of linear and non-linear Raman spectroscopies in the characterization of liquid aerosol droplets. Spontaneous Raman scattering can allow the unambiguous identification of chemical components and the determination of droplet composition. Stimulated Raman spectroscopy can allow the determination of droplet size with nanometre accuracy and can allow the characterization of near-surface composition. When combined, the mixing state and homogeneity in droplet composition can be investigated. We highlight some applications of these spectroscopic techniques in studies of the kinetics of particle transformation, the equilibrium composition of aqueous aerosol droplets, and the coagulation and mixing state of organic and aqueous aerosol components. Specifically, we examine the heat and mass transfer accompanying the evaporation of volatile components from liquid droplets, the equilibrium size of aqueous/sodium chloride droplets with varying relative humidity, and the mixing of the immiscible decane and water components during droplet coagulation. We conclude by considering the potential of these techniques for improving our understanding of aerosol properties and processes.

  19. Single particle characterization using a light scattering module coupled to a time-of-flight aerosol mass spectrometer

    SciTech Connect

    Cross, E.; Onasch, Timothy B.; Canagaratna, Manjula; Jayne, J. T.; Kimmel, Joel; Yu, Xiao-Ying; Alexander, M. L.; Worsnop, Douglas R.; Davidovits, Paul

    2009-10-01

    To accurately model the radiative forcing of aerosol particles, one must measure in real-time the size, shape, density, chemical composition, and mixing state of ambient particles. This is a formidable challenge because the chemical and physical properties of the aerosol particles are highly complex, dependent on the emission sources, the geography and meteorology of the surroundings, and the gas phase composition of the regional atmosphere.

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

    NASA Astrophysics Data System (ADS)

    Ro, C.

    2008-12-01

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

  1. Retrieval of aerosol composition using ground-based remote sensing measurements

    NASA Astrophysics Data System (ADS)

    Xie, Yisong; Li, Zhengqiang; Zhang, Ying; Li, Donghui; Li, Kaitao

    2016-04-01

    states of aerosol particles on aerosol composition retrieval.

  2. Retrieval of aerosol composition using ground-based remote sensing measurements

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

    The chemical composition and mixing status of ambient aerosol are the main factors deciding aerosol microphysical and optical properties, and thus have significant impacts on regional or global climate change and air quality. Traditional approaches to detect atmospheric aerosol composition include sampling with laboratory analysis and in-situ measurement. They can accurately acquire aerosol components, however, the sampling or air exhausting could change the status of aerosol or have some mass loss. Additionally, aerosol is usually sampled at the surface level so that it is difficult to detect the columnar aerosol properties. Remote sensing technology, however, can overcome these problems because it investigate aerosol information by optical and microphysical properties without destructing the natural status of ambient aerosol. This paper introduce a method to acquire aerosol composition by the remote sensing measurements of CIMEL CE318 ground-based sun-sky radiometer. A six component aerosol model is used in this study, including one strong absorbing component Black Carbon (BC), two partly absorbing components Brown Carbon (BrC) and Mineral Dust (MD), two scattering components Ammonia Sulfate-like (AS) and Sea Salt (SS), and Aerosol Water uptake (AW). Sensitivity analysis are performed to find the most sensitive parameters to each component and retrieval method for each component is accordingly developed. The residual minimization method is used by comparing remote sensing measurements and simulation outputs to find the optimization of aerosol composition (including volume fraction and mass concentration of each component). This method is applied to real measurements obtained from Beijing site under different weather conditions, including polluted haze, dust storm and clean days, to investigate the impacts of mixing states of aerosol particles on aerosol composition retrieval.

  3. Identification of key aerosol populations through their size and composition resolved spectral scattering and absorption

    NASA Astrophysics Data System (ADS)

    Costabile, F.; Barnaba, F.; Angelini, F.; Gobbi, G. P.

    2013-03-01

    Characterizing chemical and physical aerosol properties is important to understand their sources, effects, and feedback mechanisms in the atmosphere. This study proposes a scheme to classify aerosol populations based on their spectral optical properties (absorption and scattering). The scheme is obtained thanks to the outstanding set of information on particle size and composition these properties contain. The spectral variability of the aerosol single scattering albedo (dSSA), and the extinction, scattering and absorption Angstrom exponents (EAE, SAE and AAE, respectively) were observed on the basis of two-year measurements of aerosol optical properties (scattering and absorption coefficients at blue, green and red wavelengths) performed in the suburbs of Rome (Italy). Optical measurements of various aerosol types were coupled to measurements of particle number size distributions and relevant optical properties simulations (Mie theory). These latter allowed the investigation of the role of the particle size and composition in the bulk aerosol properties observed. The combination of simulations and measurements suggested a general "paradigm" built on dSSA, SAE and AAE to optically classify aerosols. The paradigm proved suitable to identify the presence of key aerosol populations, including soot, biomass burning, organics, dust and marine particles. The work highlights that (i) aerosol populations show distinctive combinations of SAE and dSSA times AAE, these variables being linked by a linear inverse relation varying with varying SSA; (ii) fine particles show EAE > 1.5, whilst EAE < 2 is found for both coarse particles and ultrafine soot-rich aerosols; (iii) fine and coarse particles both show SSA > 0.8, whilst ultrafine urban Aitken mode and soot particles show SSA < 0.8. The proposed paradigm agrees with aerosol observations performed during past major field campaigns, this indicating that relations concerning the paradigm have a general validity.

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

    SciTech Connect

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

    2013-12-09

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

  5. 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.

  6. Elemental Composition of Primary Aerosols Emitted from Burning of 21 Biomass Fuels Measured by Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Desyaterik, Y.; Mack, L.; Lee, T.; Kreidenweis, S. M.; Collett, J. L.; Jimenez, J. L.; Worsnop, D. R.

    2010-12-01

    Biomass burning emissions are an important contributor to regional aerosol loading and have a large impact of on air quality, visibility, and radiative forcing. However, the detailed chemical composition of the aerosols emitted during biomass burning is largely unknown. In order to gain a better understanding of the chemical and physical properties of these emissions, 92 burns were undertaken in the combustion chamber of the USDA/FS Fire Sciences Laboratory in Missoula, Montana, in well-defined laboratory conditions. A set of 21 different fuels was tested that represents biomass burned annually in the western and southeastern U.S. The chemical composition of the resulting biomass smoke aerosols was analyzed with a high-resolution aerosol mass spectrometer (Aerodyne HR-ToF-AMS). Simultaneous measurements of CO2 and CO concentrations allowed flaming and smoldering fire regimes to be distinguished. The elemental composition of the organic portion of the aerosols was extracted from the AMS measurements. Here we present the variation of O/C, H/C and organic mass to organic carbon ratios (OM/OC) versus fire regime and fuel type. We also discuss the influence on the organic aerosol chemical composition of various factors such as fuel moisture content and total aerosol loading, as well as the approach used to account for water vapor ions derived from water originally present in sampled particles versus water vapor ions produced by electron impact fragmentation of organic molecules.

  7. Composition of the Martian aerosols through near-IR spectroscopy

    NASA Technical Reports Server (NTRS)

    Erard, Stephane; Cerroni, Priscilla; Coradini, Angioletta

    1993-01-01

    Near-infrared spectroscopy is a powerful technique to study the composition of planetary surfaces, as the main minerals exhibit absorption bands in this spectral range. It gave important information on the mineralogy and petrology of Mars in the past twenty years although in this case it is well known that a large fraction of light is scattered by the airborne particles before reaching the surface. The measured signal is thus the sum of two different contributions that should be studied separately: One from the surface and one from the aerosols that depends on their density, size distribution and composition. Data from the ISM imaging spectrometer are used here to derive the aerosols spectrum. They consist in sets of spectra (from 0.76 to 3.16 microns) of approximately 3000 pixels approximately 25x25 sq km in size. The resulting spectrum exhibits both water-ice and clay mineral features superimposed on a scattering continuum.

  8. Direct Observations of the Composition of Sub-20 Nanometer Ambient Aerosol

    NASA Astrophysics Data System (ADS)

    Moore, K. F.; Smith, J. N.; Eisele, F. L.; McMurry, P. H.

    2002-12-01

    Understanding new particle formation in the atmosphere depends upon many factors including detailed knowledge of their chemical composition. The chemical composition of sub-20 nanometer ambient aerosol particles, however, is typically inferred from observations of the aerosol behavior when subjected to varying conditions during sampling. Direct observations of aerosol chemical composition are usually limited to or dominated by larger particles of higher mass. Recently a new instrument has been developed - the Thermal Desorption Chemical Ionization Mass Spectrometer (TDCIMS) - which can directly measure the chemical composition of sub-20 nanometer aerosol particles. Briefly, the front end of the TDCIMS functions as an electrostatic precipitator using a strong electric field to collect charged aerosol particles onto a sample wire. After volatilization by heating, the component species of the collected particles are subjected to chemical ionization prior to introduction into the mass spectrometer for analysis. Detection limits on the order of picograms permit sample collection periods as small as five minutes for ambient aerosol concentrations providing near "real-time" resolution. For selected periods from April through June 2002, we used the TDCIMS to measure the chemical composition of ambient aerosol for the first time. We investigated both the positive and negative ion spectrums produced by sub-20 nanometer ambient aerosol particles at the National Center for Atmospheric Research in Boulder, Colorado. Principal species identified include ammonium, sulfate and nitrate although additional peaks consistent with particle-phase origin were readily observed. Diurnal concentration profiles appear to be present and the relative proportion of sulfate and nitrate to each other can vary appreciably over several hours and between days. Validation of the TDCIMS' performance and the interpretation of its results will also be discussed.

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

    PubMed Central

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

    1982-01-01

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

  10. 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

  11. Heterogeneous Reactivity of Nitric Acid with Nascent Sea Spray Aerosol: Large Differences Observed between and within Individual Particles.

    PubMed

    Ault, Andrew P; Guasco, Timothy L; Baltrusaitis, Jonas; Ryder, Olivia S; Trueblood, Jonathan V; Collins, Douglas B; Ruppel, Matthew J; Cuadra-Rodriguez, Luis A; Prather, Kimberly A; Grassian, Vicki H

    2014-08-01

    Current climate and atmospheric chemistry models assume that all sea spray particles react as if they are pure NaCl. However, recent studies of sea spray aerosol particles have shown that distinct particle types exist (including sea salt, organic carbon, and biological particles) as well as mixtures of these and, within each particle type, there is a range of single-particle chemical compositions. Because of these differences, individual particles should display a range of reactivities with trace atmospheric gases. Herein, to address this, we study the composition of individual sea spray aerosol particles after heterogeneous reaction with nitric acid. As expected, a replacement reaction of chloride with nitrate is observed; however, there is a large range of reactivities spanning from no reaction to complete reaction between and within individual sea spray aerosol particles. These data clearly support the need for laboratory studies of individual, environmentally relevant particles to improve our fundamental understanding as to the properties that determine reactivity.

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  13. 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.

  14. Fatty acids on continental sulfate aerosol particles

    NASA Astrophysics Data System (ADS)

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

    2005-03-01

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

  15. 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.

  16. Volatility and composition of aerosols in tropical stratosphere and TTL over Biak, Indonesia

    NASA Astrophysics Data System (ADS)

    Hayashi, M.; Shibata, T.; Hara, K.; Hasebe, F.

    2014-12-01

    Number concentration and volatility of aerosols in the Tropical Tropopause Layer (TTL) over Biak (1.2 oS, 136.1 oE) were observed using balloon-borne dual optical particle counters (OPC) in January 2011, 2012, and 2013. One OPC observed number concentration of ambient aerosols and another OPC had an inlet with a thermo denuder, whose temperature were set at 100 to 300 oC, in order to observe volatility. The results suggest that major composition of aerosol change with altitude, from sulfate in upper troposphere to sulfuric acid in stratosphere through TTL region. The ratios of number concentrations of un-volatile aerosol, to those of ambient aerosol in sub-micrometer size range are few percent in stratosphere and several percent in TTL. In addition, un-volatile aerosol concentrations were similar to the concentration of ice particle in sub-visible cirrus.

  17. Morphology and Optical Properties of Mixed Aerosol Particles

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    LLPS in accumulation-sized particles and the change in their absorption using a cavity ring down aerosol spectrometer. If LLPS alters the absorptive properties of the suggested model aerosols significantly, absorption measurements of accumulation mode particles of the same composition would allow proving that LLPS indeed occurs in particles of accumulation mode size. Up to now LLPS has not been studied for particles in this size range. References: 1. Bertram, et al. Atmos. Chem & Phys, 11(21), 10995-11006, 2011.
 2. Krieger, et al. Chemical Society Reviews, 41(19), 6631-6662, 2012 
3. Song, M. et al. Geophys Res Lett, 39(19), 2012b 4. Smith et al. Atmos Chem & Phys, 12(20), 9613- 9628, 2012.
 5. You, Y. et al. Proceedings of the National Academy of Sciences, 109(33), 13188-13193, 2012.

  18. 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.

  19. 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.

  20. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  3. 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...

  4. 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.

  5. 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.

  6. Identification of aerosol composition from multi-wavelength lidar measurements

    NASA Technical Reports Server (NTRS)

    Wood, S. A.

    1984-01-01

    This paper seeks to develop the potential of lidar for the identification of the chemical composition of atmospheric aerosols. Available numerical computations suggest that aerosols can be identified by the wavelength dependence of aerosol optical properties. Since lidar can derive the volume backscatter coefficient as a function of wavelength, a multi-wavelength lidar system may be able to provide valuable information on the composition of aerosols. This research theoretically investigates the volume backscatter coefficients for the aerosol classes, sea-salts, and sulfates, as a function of wavelength. The results show that these aerosol compositions can be characterized and identified by their backscatter wavelength dependence. A method to utilize multi-wavelength lidar measurements to discriminate between compositionally different thin aerosol layers is discussed.

  7. Photocatalytic/Magnetic Composite Particles

    NASA Technical Reports Server (NTRS)

    Wu, Chang-Yu; Goswami, Yogi; Garretson, Charles; Andino, Jean; Mazyck, David

    2007-01-01

    Photocatalytic/magnetic composite particles have been invented as improved means of exploiting established methods of photocatalysis for removal of chemical and biological pollutants from air and water. The photocatalytic components of the composite particles are formulated for high levels of photocatalytic activity, while the magnetic components make it possible to control the movements of the particles through the application of magnetic fields. The combination of photocatalytic and magnetic properties can be exploited in designing improved air- and water treatment reactors.

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

    SciTech Connect

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

    2009-05-05

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

  9. Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

    SciTech Connect

    Baustian, Kelly J.; Cziczo, Daniel J.; Wise, M. A.; Pratt, Kerri; Kulkarni, Gourihar R.; Hallar, Anna G.; Tolbert, Margaret A.

    2012-03-30

    In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single-particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse-mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine-mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic-containing particles serve as efficient ice nuclei while others do not. For coarse-mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

  10. Importance of aerosol composition, mixing state, and morphology for heterogeneous ice nucleation: A combined field and laboratory approach

    NASA Astrophysics Data System (ADS)

    Baustian, Kelly J.; Cziczo, Daniel J.; Wise, Matthew E.; Pratt, Kerri A.; Kulkarni, Gourihar; Hallar, A. Gannet; Tolbert, Margaret A.

    2012-03-01

    In this study chemical compositions of background aerosol and ice nuclei were examined through laboratory investigations using Raman spectroscopy and field measurements by single-particle mass spectrometry. Aerosol sampling took place at Storm Peak Laboratory in Steamboat Springs, Colorado (elevation of 3210 m). A cascade impactor was used to collect coarse-mode aerosol particles for laboratory analysis by Raman spectroscopy; the composition, mixing state, and heterogeneous ice nucleation activity of individual particles were examined. For in situ analysis of fine-mode aerosol, ice nucleation on ambient particles was observed using a compact ice nucleation chamber. Ice crystals were separated from unactivated aerosol using a pumped counterflow virtual impactor, and ice nuclei were analyzed using particle analysis by laser mass spectrometry. For both fine and coarse modes, the ice nucleating particle fractions were enriched in minerals and depleted in sulfates and nitrates, compared to the background aerosol sampled. The vast majority of particles in both the ambient and ice active aerosol fractions contained a detectable amount of organic material. Raman spectroscopy showed that organic material is sometimes present in the form of a coating on the surface of inorganic particles. We find that some organic-containing particles serve as efficient ice nuclei while others do not. For coarse-mode aerosol, organic particles were only observed to initiate ice formation when oxygen signatures were also present in their spectra.

  11. REAL-TIME MEASUREMENTS OF THE CHEMICAL COMPOSITION OF SIZE-RESOLVED PARTICLES DURING A SANTA ANA WIND EPISODE, CALIFORNIA USA. (R826240)

    EPA Science Inventory

    Size-resolved particle composition, mass and number concentrations, aerosol scattering coefficients, and prevailing meteorological conditions were measured at the Ellen Browning Scripps Memorial Pier located in La Jolla, California on 15 December 1998. Aerosol particles were s...

  12. Chemical Composition of Laboratory Generated Seafoam Particles

    NASA Astrophysics Data System (ADS)

    Tyree, C. A.; Alexandrova, O. A.; Allen, J. O.

    2005-12-01

    Remote marine aerosols include a significant number of sea-salt particles that may be effective cloud condensation nuclei. For example, O`Dowd and Smith (1993) found that remote marine aerosols in the particle size range 0.1-3.0 μm were dominated by sea-salt particles in the case of moderate-to-high wind speeds. Measurements of the flux of sub-micron sea-salt particles for the same wind speed vary by orders of magnitude, which indicate that other parameters, for example, may have a role in their production (Reid et al., 2001). Previous laboratory experiments using artificial seawater have shown that organic content (Garrett, 1968) and salinity (Mortensson et al., 2003) affect sea-salt particle production. We present laboratory measurements of sea-salt particles generated from seawater foams and compare them to measurements of remote marine particles. Foam droplets were generated by bubbling air through a fine pore diffuser into aqueous media in a precleaned glass column. The effect of salinity was studied by varying the salinity of artificial seawater over the range 0-3.5%. The effect of organic content was also studied by diluting filtered seawater with artificial seawater. Size distributions of dried seafoam droplets were measured using a scanning mobility particle sizer. Seafoam particles were also size segregated and collected using a Micro-Orifice Uniform Deposit Impactor. Collected material was analyzed for sodium, chloride, sulfate, and dissolved organic carbon (DOC). Sub-micron particle size distributions were unimodal with a mean diameter of ~100 nm in agreement with recent seafoam laboratory experiments (Martensson et al., 2003). This mode is comparable to the "accumulation" mode particles typical of the remote marine environment and known to contain significant amounts of sea-salt (Bates et al., 1998). The size and number of seafoam particles were dependent on salinity; mean droplet size and total number concentration increased with salinity

  13. 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.

  14. 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.

  15. 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

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

    SciTech Connect

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

    2015-09-25

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

  17. 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

  18. 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.

  19. Characterizing the impact of urban emissions on regional aerosol particles; airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouch, N.; Pichon, J.-M.; Prévôt, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2013-09-01

    The MEGAPOLI experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS) giving detailed information of the non-refractory submicron aerosol species. The mass concentration of BC, measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), black carbon and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy). Plotting the equivalent ratios for the Positive Matrix Factorization (PMF) resolved species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA). Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in Mexico city, Mexico and in New England, USA. Using the measured VOCs species together with recent organic aerosol formation yields we predicted ~ 50% of the measured organics. These airborne measurements during the MEGAPOLI experiment show that urban emissions contribute to the formation of OA

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

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

    SciTech Connect

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

    1992-05-01

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

  2. 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

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

    PubMed

    Weber; Schweiger

    1999-02-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  5. 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.

  6. Gas-particle partitioning of semivolatile organic compounds (SOCs) on mixtures of aerosols in a smog chamber.

    PubMed

    Chandramouli, Bharadwaj; Jang, Myoseon; Kamens, Richard M

    2003-09-15

    The partitioning behavior of a set of diverse SOCs on two and three component mixtures of aerosols from different sources was studied using smog chamber experimental data. A set of SOCs of different compound types was introduced into a system containing a mixture of aerosols from two or more sources. Gas and particle samples were taken using a filter-filter-denuder sampling system, and a partitioning coefficient Kp was estimated using Kp = Cp/(CgTSP). Particle size distributions were measured using a differential mobility analyzer and a light scattering detector. Gas and particle samples were analyzed using GCMS. The aerosol composition in the chamber was tracked chemically using a combination of signature compounds and the organic matter mass fraction (f(om)) of the individual aerosol sources. The physical nature of the aerosol mixture in the chamber was determined using particle size distributions, and an aggregate Kp was estimated from theoretically calculated Kp on the individual sources. Model fits for Kp showed that when the mixture involved primary sources of aerosol, the aggregate Kp of the mixture could be successfully modeled as an external mixture of the Kp on the individual aerosols. There were significant differences observed for some SOCs between modeling the system as an external and as an internal mixture. However, when one of the aerosol sources was secondary, the aggregate model Kp required incorporation of the secondary aerosol products on the preexisting aerosol for adequate model fits. Modeling such a system as an external mixture grossly overpredicted the Kp of alkanes in the mixture. Indirect evidence of heterogeneous, acid-catalyzed reactions in the particle phase was also seen, leading to a significant increase in the polarity of the resulting aerosol mix and a resulting decrease in the observed Kp of alkanes in the chamber. The model was partly consistent with this decrease but could not completely explain the reduction in Kp because of

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

    SciTech Connect

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

    2003-02-16

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

  8. 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...

  9. Chemical composition of Eastern Black Sea aerosol--preliminary results.

    PubMed

    Balcılar, Ilker; Zararsız, Abdullah; Kalaycı, Yakup; Doğan, Güray; Tuncel, Gürdal

    2014-08-01

    Trace element composition of atmospheric particles collected at a high altitude site on the Eastern Black Sea coast of Turkey was investigated to understand atmospheric transport of pollutants to this semi-closed basin. Aerosol samples were collected at a timber-storage area, which is operated by the General Directorate of Forestry. The site is situated at a rural area and is approximately 50 km to the Black Sea coast and 200 km to the Georgia border of Turkey. Coarse (PM2.5-10) and fine (PM2.5) aerosol samples were collected between 2011 and 2013 using a "stacked filter unit". Collected samples were shipped to the Middle East Technical University in Ankara, where Na, Mg, Al, Si, S, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Ba, Pb were measured by Energy dispersive x-ray fluorescence technique (EDXRF). Comparison of measured concentrations of elements with corresponding data generated at other parts of Turkey demonstrated that concentrations of pollution derived elements are higher at Eastern Black Sea than their corresponding concentrations measured at other parts of Turkey, which is attributed to frequent transport of pollutants from north wind sector. Positive matric factorization revealed four factors including three anthropogenic and a crustal factor. Southeastern parts of Turkey, Georgia and Black Sea coast of Ukraine were identified as source regions affecting composition of particles at our site, using trajectory statistics, namely "potential source contribution function" (PSCF). PMID:24373640

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

  12. Stable Carbon Fractionation In Size Segregated Aerosol Particles Produced By Controlled Biomass Burning

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

    Biomass burning is the largest source of primary fine fraction carbonaceous particles and the second largest source of trace gases in the global atmosphere with a strong effect not only on the regional scale but also in areas distant from the source . Many studies have often assumed no significant carbon isotope fractionation occurring between black carbon and the original vegetation during combustion. However, other studies suggested that stable carbon isotope ratios of char or BC may not reliably reflect carbon isotopic signatures of the source vegetation. Overall, the apparently conflicting results throughout the literature regarding the observed fractionation suggest that combustion conditions may be responsible for the observed effects. The purpose of the present study was to gather more quantitative information on carbonaceous aerosols produced in controlled biomass burning, thereby having a potential impact on interpreting ambient atmospheric observations. Seven different biomass fuel types were burned under controlled conditions to determine the effect of the biomass type on the emitted particulate matter mass and stable carbon isotope composition of bulk and size segregated particles. Size segregated aerosol particles were collected using the total suspended particle (TSP) sampler and a micro-orifice uniform deposit impactor (MOUDI). The results demonstrated that particle emissions were dominated by the submicron particles in all biomass types. However, significant differences in emissions of submicron particles and their dominant sizes were found between different biomass fuels. The largest negative fractionation was obtained for the wood pellet fuel type while the largest positive isotopic fractionation was observed during the buckwheat shells combustion. The carbon isotope composition of MOUDI samples compared very well with isotope composition of TSP samples indicating consistency of the results. The measurements of the stable carbon isotope ratio in

  13. Ozone, Iodine, and MSA - Case studies in Antarctic aerosol composition from the 2ODIAC Campaign

    NASA Astrophysics Data System (ADS)

    Giordano, M.; Kalnajs, L.; Deshler, T.; Davis, S. M.; Johnson, A.; Slater, A. G.; Goetz, J. D.; Mukherjee, A. D.; DeCarlo, P. F.

    2015-12-01

    Aerosol generation and transport over the Polar Regions, and especially Antarctica, remains a source of uncertainty for geophysical scientists. A characterization of aerosol sources, production, and lifecycle processes in the Polar Regions is required to better understand the polar atmosphere. In an attempt to better characterize Antarctic aerosol and trace gas interactions, the Two-Season, Ozone Depletion and Interaction with Aerosols Campaign (2ODIAC) was launched over the Austral Spring/Summer of 2014 and Austral Winter of 2015. One highlight of the campaign is the first ever deployment of a high-resolution aerosol mass spectrometer to Antarctica. In conjunction with trace gas, meteorology, and aerosol sizing measurements, this presentation will focus on case studies from the campaign relevant to the atmospheric science community. Questions about the role of iodine, MSA, and ozone depletion events in regards to aerosol composition will be examined. Specific attention will be paid to aerosol compositional changes before, during, and after particle bursts especially where changes in aerosol sulfate oxidation occurred (SO2 -> SO4)

  14. 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.

  15. Total-Reflection X-ray fluorescence analysis of elements in size-fractionated particulate matter sampled on polycarbonate filters — Composition and sources of aerosol particles in Göteborg, Sweden

    NASA Astrophysics Data System (ADS)

    Wagner, Annemarie; Mages, Margarete

    2010-06-01

    This is the first study applying the technique of cold plasma ashing on polycarbonate filters as a preparative step for subsequent elemental analysis of aerosol particles by Total-Reflection X-ray fluorescence. The procedure has been validated by analyzing blanks of the filter material, chemicals used as additives as well as certified standard reference material. The results showed that cold plasma ashing is superior to conventional digestion methods with regard to the ease of sample preparation and contamination. A PIXE cascade impactor was used to collect size-fractionated aerosol particles in 9 size classes ranging from 16 to 0.06 µm aerodynamic diameter at an urban and a suburban site in Göteborg, Sweden. Filter segments loaded with the aerosol particles were cut out and fixed on Quartz carriers. After adding 10 ng of Ga as internal standard the samples were dried, digested by cold plasma ashing and analyzed by Total-Reflection X-ray fluorescence. The analysis of aerosol particles showed that elemental concentrations at both the urban and the suburban site in Göteborg were low compared to central Europe. More and concurrent sampling of size-fractionated particles is required to identify local sources of trace elements in the urban area of Göteborg.

  16. Characterizing the impact of urban emissions on regional aerosol particles: airborne measurements during the MEGAPOLI experiment

    NASA Astrophysics Data System (ADS)

    Freney, E. J.; Sellegri, K.; Canonaco, F.; Colomb, A.; Borbon, A.; Michoud, V.; Doussin, J.-F.; Crumeyrolle, S.; Amarouche, N.; Pichon, J.-M.; Bourianne, T.; Gomes, L.; Prevot, A. S. H.; Beekmann, M.; Schwarzenböeck, A.

    2014-02-01

    The MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) experiment took place in July 2009. The aim of this campaign was to study the aging and reactions of aerosol and gas-phase emissions in the city of Paris. Three ground-based measurement sites and several mobile platforms including instrument equipped vehicles and the ATR-42 aircraft were involved. We present here the variations in particle- and gas-phase species over the city of Paris, using a combination of high-time resolution measurements aboard the ATR-42 aircraft. Particle chemical composition was measured using a compact time-of-flight aerosol mass spectrometer (C-ToF-AMS), giving detailed information on the non-refractory submicron aerosol species. The mass concentration of black carbon (BC), measured by a particle absorption soot photometer (PSAP), was used as a marker to identify the urban pollution plume boundaries. Aerosol mass concentrations and composition were affected by air-mass history, with air masses that spent longest time over land having highest fractions of organic aerosol and higher total mass concentrations. The Paris plume is mainly composed of organic aerosol (OA), BC, and nitrate aerosol, as well as high concentrations of anthropogenic gas-phase species such as toluene, benzene, and NOx. Using BC and CO as tracers for air-mass dilution, we observe the ratio of ΔOA / ΔBC and ΔOA / ΔCO increase with increasing photochemical age (-log(NOx / NOy)). Plotting the equivalent ratios of different organic aerosol species (LV-OOA, SV-OOA, and HOA) illustrate that the increase in OA is a result of secondary organic aerosol (SOA) formation. Within Paris the changes in the ΔOA / ΔCO are similar to those observed during other studies in London, Mexico City, and in New England, USA. Using the measured SOA volatile organic compounds (VOCs) species together with organic aerosol formation

  17. 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.

  18. Mass spectrometric airborne measurements of submicron aerosol and cloud residual composition in tropic deep convection during ACRIDICON-CHUVA

    NASA Astrophysics Data System (ADS)

    Schulz, Christiane; Schneider, Johannes; Mertes, Stephan; Kästner, Udo; Weinzierl, Bernadett; Sauer, Daniel; Fütterer, Daniel; Walser, Adrian; Borrmann, Stephan

    2015-04-01

    Airborne measurements of submicron aerosol and cloud particles were conducted in the region of Manaus (Amazonas, Brazil) during the ACRIDICON-CHUVA campaign in September 2014. ACRIDICON-CHUVA aimed at the investigation of convective cloud systems in order to get a better understanding and quantification of aerosol-cloud-interactions and radiative effects of convective clouds. For that, data from airborne measurements within convective cloud systems are combined with satellite and ground-based data. We used a C-ToF-AMS (Compact-Time-of-Flight-Aerosol-Mass-Spectrometer) to obtain information on aerosol composition and vertical profiles of different aerosol species, like organics, sulphate, nitrate, ammonium and chloride. The instrument was operated behind two different inlets: The HASI (HALO Aerosol Submicrometer Inlet) samples aerosol particles, whereas the CVI (Counterflow Virtual Impactor) samples cloud droplets and ice particles during in-cloud measurements, such that cloud residual particles can be analyzed. Differences in aerosol composition inside and outside of clouds and cloud properties over forested or deforested region were investigated. Additionally, the in- and outflow of convective clouds was sampled on dedicated cloud missions in order to study the evolution of the clouds and the processing of aerosol particles. First results show high organic aerosol mass concentrations (typically 15 μg/m3 and during one flight up to 25 μg/m3). Although high amounts of organic aerosol in tropic air over rainforest regions were expected, such high mass concentrations were not anticipated. Next to that, high sulphate aerosol mass concentrations (about 4 μg/m3) were measured at low altitudes (up to 5 km). During some flights organic and nitrate aerosol was observed with higher mass concentrations at high altitudes (10-12 km) than at lower altitudes, indicating redistribution of boundary layer particles by convection. The cloud residuals measured during in

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

    SciTech Connect

    Meskhidze, Nicholas

    2013-10-21

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

  20. A preliminary analysis of the surface chemistry of atmospheric aerosol particles in a typical urban area of Beijing.

    PubMed

    Zhang, Zhengzheng; Li, Hong; Liu, Hongyan; Ni, Runxiang; Li, Jinjuan; Deng, Liqun; Lu, Defeng; Cheng, Xueli; Duan, Pengli; Li, Wenjun

    2016-09-01

    Atmospheric aerosol particle samples were collected using an Ambient Eight Stage (Non-Viable) Cascade Impactor Sampler in a typical urban area of Beijing from 27th Sep. to 5th Oct., 2009. The surface chemistry of these aerosol particles was analyzed using Static Time of Flight-Secondary Ion Mass Spectrometry (Static TOF-SIMS). The factors influencing surface compositions were evaluated in conjunction with the air pollution levels, meteorological factors, and air mass transport for the sampling period. The results show that a variety of organic ion groups and inorganic ions/ion groups were accumulated on the surfaces of aerosol particles in urban areas of Beijing; and hydrophobic organic compounds with short- or middle-chain alkyl as well as hydrophilic secondary inorganic compounds were observed. All these compounds have the potential to affect the atmospheric behavior of urban aerosol particles. PM1.1-2.1 and PM3.3-4.7 had similar elements on their surfaces, but some molecules and ionic groups demonstrated differences in Time of Flight-Secondary Ion Mass Spectrometry spectra. This suggests that the quantities of elements varied between PM1.1-2.1 and PM3.3-4.7. In particular, more intense research efforts into fluoride pollution are required, because the fluorides on aerosol surfaces have the potential to harm human health. The levels of air pollution had the most significant influence on the surface compositions of aerosol particles in our study. Hence, heavier air pollution was associated with more complex surface compositions on aerosol particles. In addition, wind, rainfall, and air masses from the south also greatly influenced the surface compositions of these urban aerosol particles.

  1. A preliminary analysis of the surface chemistry of atmospheric aerosol particles in a typical urban area of Beijing.

    PubMed

    Zhang, Zhengzheng; Li, Hong; Liu, Hongyan; Ni, Runxiang; Li, Jinjuan; Deng, Liqun; Lu, Defeng; Cheng, Xueli; Duan, Pengli; Li, Wenjun

    2016-09-01

    Atmospheric aerosol particle samples were collected using an Ambient Eight Stage (Non-Viable) Cascade Impactor Sampler in a typical urban area of Beijing from 27th Sep. to 5th Oct., 2009. The surface chemistry of these aerosol particles was analyzed using Static Time of Flight-Secondary Ion Mass Spectrometry (Static TOF-SIMS). The factors influencing surface compositions were evaluated in conjunction with the air pollution levels, meteorological factors, and air mass transport for the sampling period. The results show that a variety of organic ion groups and inorganic ions/ion groups were accumulated on the surfaces of aerosol particles in urban areas of Beijing; and hydrophobic organic compounds with short- or middle-chain alkyl as well as hydrophilic secondary inorganic compounds were observed. All these compounds have the potential to affect the atmospheric behavior of urban aerosol particles. PM1.1-2.1 and PM3.3-4.7 had similar elements on their surfaces, but some molecules and ionic groups demonstrated differences in Time of Flight-Secondary Ion Mass Spectrometry spectra. This suggests that the quantities of elements varied between PM1.1-2.1 and PM3.3-4.7. In particular, more intense research efforts into fluoride pollution are required, because the fluorides on aerosol surfaces have the potential to harm human health. The levels of air pollution had the most significant influence on the surface compositions of aerosol particles in our study. Hence, heavier air pollution was associated with more complex surface compositions on aerosol particles. In addition, wind, rainfall, and air masses from the south also greatly influenced the surface compositions of these urban aerosol particles. PMID:27593274

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

    PubMed

    Quenzel, H

    1969-01-01

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

  3. The impact of relative humidity on aerosol composition and evolution processes during wintertime in Beijing, China

    NASA Astrophysics Data System (ADS)

    Sun, Yele; Wang, Zifa; Fu, Pingqing; Jiang, Qi; Yang, Ting; Li, Jie; Ge, Xinlei

    2013-10-01

    Non-refractory submicron aerosol (NR-PM1) species measured by an Aerodyne Aerosol Chemical Speciation Monitor (ACSM) along with collocated gaseous species are used to investigate the impacts of relative humidity (RH) on aerosol composition and evolution processes during wintertime in Beijing, China. Aerosol species exhibit strong, yet different RH dependence between low and high RH levels. At low RH levels (<50%), all aerosol species increase linearly as a function of RH, among which organics present the largest mass increase rate at 11.4 μg m-3/10% RH. Because the particle liquid water predicted by E-AIM model is very low and the temperature is relatively constant, the enhancement of aerosol species is primarily due to the decrease of wind speed. While the rates of increase for most aerosol species are reduced at high RH levels (>50%), sulfate presents an even faster increasing rate, indicating the significant impact of liquid water on sulfate production. The RH dependence of organic aerosol (OA) components is also quite different. Among OA components, coal combustion OA (CCOA) presents the largest enhancement in both mass concentration and contribution as a function of RH. Our results elucidate the important roles of liquid water in aerosol processing at elevated RH levels, in particular affecting sulfate and CCOA via aqueous-phase reaction and gas-particle partitioning associated with water uptake, respectively. It is estimated that aqueous-phase processing can contribute more than 50% of secondary inorganic species production along with an increase of aerosol particle acidity during the fog periods. However, it appears not to significantly enhance secondary organic aerosol (SOA) formation and the oxidation degree of OA.

  4. Chemical composition and characteristics of ambient aerosols and rainwater residues during Indian summer monsoon: Insight from aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Gupta, Tarun; Tripathi, Sachchida N.

    2016-07-01

    Real time composition of non-refractory submicron aerosol (NR-PM1) is measured via Aerosol mass spectrometer (AMS) for the first time during Indian summer monsoon at Kanpur, a polluted urban location located at the heart of Indo Gangetic Plain (IGP). Submicron aerosols are found to be dominated by organics followed by nitrate. Source apportionment of organic aerosols (OA) via positive matrix factorization (PMF) revealed several types of secondary/oxidized and primary organic aerosols. On average, OA are completely dominated by oxidized OA with a very little contribution from biomass burning OA. During rain events, PM1 concentration is decreased almost by 60%, but its composition remains nearly the same. Oxidized OA showed slightly more decrease than primary OAs, probably due to their higher hygroscopicity. The presence of organo nitrates (ON) is also detected in ambient aerosols. Apart from real-time sampling, collected fog and rainwater samples were also analyzed via AMS in offline mode and in the ICP-OES (Inductively coupled plasma - Optical emission spectrometry) for elements. The presence of sea salt, organo nitrates and sulfates has been observed. Rainwater residues are also dominated by organics but their O/C ratios are 15-20% lower than the observed values for ambient OA. Alkali metals such as Ca, Na, K are found to be most abundant in the rainwater followed by Zn. Rainwater residues are also found to be much less oxidized than the aerosols present inside the fog water, indicating presence of less oxidized organics. These findings indicate that rain can act as an effective scavenger of different types of pollutants even for submicron particle range. Rainwater residues also contain organo sulfates which indicate that some portion of the dissolved aerosols has undergone aqueous processing, possibly inside the cloud. Highly oxidized and possibly hygroscopic OA during monsoon period compared to other seasons (winter, post monsoon), indicates that they can act

  5. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

    , extending over more than twelve years of MISR data, aid in the assessment. Comparisons with the limited available AERONET aerosol type data are also made and evaluated as appropriate. Seasons and regions that regularly show poorly constrained aerosol type results are identified, as are times and places where particle property information can be used with confidence. This work is performed in part at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration and in part at the NASA Goddard Space Flight Center.

  8. Preliminary Results of Aerosol Chemical Composition Measurements in the Gulf of Maine with an Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Middlebrook, A. M.; Canagaratna, M. R.; Worsnop, D. R.

    2002-12-01

    The New England Air Quality Study is a multi-institutional research project to improve understanding of the atmospheric processes that control the production and distribution of air pollutants in the New England region. During July-August, 2002 a large, collaborative, intensive period of atmospheric measurement and model comparisons took place. As part of this study, an Aerosol Mass Spectrometer (AMS) was deployed aboard the NOAA ship RONALD H. BROWN in the Gulf of Maine. The AMS measures semi-volatile components of aerosol particles with aerodynamic diameters between roughly 40 and 1500 nm. During this study, the AMS collected 2-minute averaged particle mass spectra as well as speciated organic, sulfate, and nitrate size distributions. Sodium chloride, sodium sulfate, and sodium nitrate components of the aerosol, which are relatively non-volatile at the AMS heater temperature, were not detected with the AMS. A wide variety of air masses were sampled during the intensive period, including clean marine, clean continental, and polluted continental air masses. In general, the volatile particle composition was mostly organic and sulfate with lesser amounts of nitrate. Furthermore, particle mass loadings typically peaked around 400-600 nm in aerodynamic diameter. Several events with high aerosol organic, sulfate, and/or nitrate mass loadings were observed and the atmospheric processes that cause them will be discussed.

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

    NASA Astrophysics Data System (ADS)

    Xu, Lingling; Chen, Jinsheng

    2016-04-01

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

  10. Cloud Nucleating Properties of Aerosols During TexAQS - GoMACCS 2006: Influence of Aerosol Sources, Composition, and Size

    NASA Astrophysics Data System (ADS)

    Quinn, P. K.; Bates, T. S.; Coffman, D. J.; Covert, D. S.; Onasch, T. B.; Alllan, J. D.; Worsnop, D.

    2006-12-01

    TexAQS - GoMACCS 2006 was conducted from July to September 2006 in the Gulf of Mexico and Houston Ship Channel to investigate sources and processing of gas and particulate phase species and to determine their impact on regional air quality and climate. As part of the experiment, the NOAA R.V. Ronald H. Brown transited from Charleston, S.C. to the study region. The ship was equipped with a full compliment of gas and aerosol instruments. To determine the cloud nucleating properties of aerosols, measurements were made of the aerosol number size distribution, aerosol chemical composition, and cloud condensation nuclei (CCN) concentration at five supersaturations. During the transit and over the course of the experiment, a wide range of aerosol sources and types was encountered. These included urban and industrial emissions from the S.E. U.S. as the ship left Charleston, a mixture of Saharan dust and marine aerosol during the transit around Florida and across the Gulf of Mexico, urban emissions from Houston, and emissions from the petrochemical industries, oil platforms, and marine vessels in the Gulf coast region. Highest activation ratios (ratio of CCN to total particle number concentration at 0.4 percent supersaturation) were measured in anthropogenic air masses when the aerosol was composed primarily of ammonium sulfate salts and in marine air masses with an aerosol composed of sulfate and sea salt. A strong gradient in activation ratio was measured as the ship moved from the Gulf of Mexico to the end of the Houston Ship Channel (values decreasing from about 0.8 to less than 0.1) and the aerosol changed from marine to industrial. The activation ratio under these different regimes in addition to downwind of marine vessels and oil platforms will be discussed in the context of the aerosol size distribution and chemical composition. The discussion of composition will include the organic mass fraction of the aerosol, the degree of oxidation of the organics, and the water

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

    DOE PAGES

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

    2016-03-22

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

  12. 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

  13. Single particle atmospheric aerosol analysis using digital holographic microscopy

    NASA Astrophysics Data System (ADS)

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

    2011-06-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  15. Biogenic Aerosols Over the Amazon Basin: Optical Properties and Relationship With Elemental and Ionic Composition

    NASA Astrophysics Data System (ADS)

    Artaxo, P.; Martin, S. T.; Andreae, M. O.; Godoy, J. M.; Godoy, M. L.; Rizzo, L. V.; Paixao, M.

    2008-12-01

    We investigated the optical properties of natural biogenic aerosol particles over the central Amazon Basin near Manaus during the wet season in February and March 2008. The measurements were conducted as part of the AMAZE-08 (Amazonian Aerosol Characterization Experiment) sampling campaign. Light absorption was determined with the use of an Aethalometer and an MAAP (Multi Angle Absorption Photometer). Light scattering was measured with a 3 wavelength TSI nephelometer and an Ecotech nephelometer. The elemental composition was measured trough PIXE and IC. Single scattering albedo shows relatively low values varying from 0.86 to 0.95. Very low fine mode aerosol mass was measured, and coarse mode particles are responsible for a significant fraction of scattering and absorption. Sulfur was observed in very low concentrations, and most of the aerosol mass was organic. Long range transport of soil dust from Sahara were observed and reflected in the light scattering coefficient. Wavelength dependence of absorption indicates the strong influence of coarse mode aerosol. Aerosol optical thickness shows low values, but with significant single scattering albedo values, showing strong absorption properties of these biogenic aerosols. Size distribution measurements shows consistence with the scattering coefficients measured, if the coarse mode particles are taken into account.

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

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Volkamer, R.

    2010-09-01

    possibly catalytic role of aerosol water in SOA formation. However, the reversible nature of uptake under dark conditions is not captured by keffupt, and can be parameterized by an effective Henry's law constant including an equilibrium constant Kolig = 1000 (in ammonium sulfate solution). Such reversible glyoxal oligomerization contributes <1% to total predicted SOA masses at any time. Sensitivity tests reveal five parameters that strongly affect the predicted SOA mass from glyoxal: (1) time scales to reach equilibrium states (as opposed to assuming instantaneous equilibrium), (2) particle pH, (3) chemical composition of the bulk aerosol, (4) particle surface composition, and (5) particle liquid water content that is mostly determined by the amount and hygroscopicity of aerosol mass and to a lesser extent by the ambient relative humidity. Glyoxal serves as an example molecule, and the conclusions about SOA formation in aqueous particles can serve for comparative studies of other molecules that form SOA as the result of multiphase chemical processing in aerosol water. This SOA source is currently underrepresented in atmospheric models; if included it is likely to bring SOA predictions (mass and O/C ratio) into better agreement with field observations.

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

    NASA Astrophysics Data System (ADS)

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

    2014-07-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-08-01

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

  20. 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

  1. 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.

  2. Light Absorption of Biogenic Aerosol Particles in Amazonia

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  3. 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

  4. 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

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  6. Single particle multichannel bio-aerosol fluorescence sensor

    NASA Astrophysics Data System (ADS)

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

    2005-05-01

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

  7. Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

    NASA Astrophysics Data System (ADS)

    Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

    2015-10-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

  8. Predicting the Mineral Composition of Dust Aerosols. Part 1; Representing Key Processes

    NASA Technical Reports Server (NTRS)

    Perlwitz, J. P.; Garcia-Pando, C. Perez; Miller, R. L.

    2015-01-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wetsieved soil and the emitted aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent at these diameters in a soil whose aggregates are dispersed by wet sieving. We calculate the emitted mass of each mineral with respect to size by accounting for the disintegration of soil aggregates during wet sieving. These aggregates are emitted during mobilization and fragmentation of the original undispersed soil that is subject to wind erosion. The emitted aggregates are carried far downwind from their parent soil. The soil mineral fractions used to calculate the aggregates also include larger particles that are suspended only in the vicinity of the source. We calculate the emitted size distribution of these particles using a normalized distribution derived from aerosol measurements. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to

  9. Elemental composition of aerosols in fourteen experiments of the Cloud Condensation Nuclei Workshop

    NASA Technical Reports Server (NTRS)

    Mach, W. H.; Hucek, R. R.

    1981-01-01

    Aeosols were collected with two Ci impactors and analyzed with proton induced X-ray emission (PIXE) for chemical composition and to detect if contamination was present. One of the impactors sampled the generated aerosols; the other impactor sampled droplets from a diffusion cloud chamber. The purpose of the experiments was to test the feasibility of a study of the transfer of chemical elements from the fine particle sizes to the coarse particle sizes, after CCN are activated and cloud droplets are formed. The data indicated that sulfur-containing aerosols did exhibit the expected transfer.

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

    PubMed

    Dette, Hans P; Koop, Thomas

    2015-05-14

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

  11. Measurement of Fluorescence Spectra from Ambient Aerosol Particles Using Laser-induced Fluorescence Technique

    NASA Astrophysics Data System (ADS)

    Taketani, F.; Kanaya, Y.; Nakamura, T.; Moteki, N.; Takegawa, N.

    2011-12-01

    To obtain the information of composition of organic aerosol particles in atmosphere, we developed an instrument using laser-induced fluorescence (LIF) technique. To measure the fluorescence from a particle, we employed two lasers. Scattering light signal derived from a single particle upon crossing the 635nm-CW laser triggers the 266nm-pulsed laser to excite the particle. Fluorescence from the particle in the wavelength range 300-600nm is spectrally dispersed by a grating spectrometer and then detected by a 32-Ch photo-multiplier tube(PMT). The aerosol stream is surrounded by a coaxial sheath air flow and delivered to the optical chamber at atmospheric pressure. Using PSL particles with known sizes, we made a calibration curve to estimate particle size from scattering light intensity. With the current setup of the instrument we are able to detect both scattering and fluorescence from particles whose diameters are larger than 0.5um. Our system was able to differentiate particles composed of mono-aromatic species (e.g. Tryptophan) from those of Riboflavin, by their different fluorescence wavelengths. Also, measurements of fluorescence spectra of ambient particles were demonstrated in our campus in Yokosuka city, facing Tokyo bay in Japan. We obtained several types of florescence spectra in the 8 hours. Classification of the measured fluorescence spectra will be discussed in the presentation.

  12. 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.

  13. 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

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

    SciTech Connect

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

    2012-10-01

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

  15. 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.

  16. Coagulation of monodisperse aerosol particles by isotropic turbulence

    NASA Astrophysics Data System (ADS)

    Chun, J.; Koch, D. L.

    2005-02-01

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

  17. 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

  18. 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

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

    NASA Astrophysics Data System (ADS)

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

    2013-12-01

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

  20. Revisiting methods to predict the rate of equilibration of viscous aerosol particles

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    Recent attention on aerosol particle phase state has motivated questions about methods to model diffusion through them. At the single particle level, some methods have already been used to: prescribe general equilibration timescales; infer relative importance of processes in SOA formation; derive diffusion coefficients in mixtures and even assess effects on cloud dynamics. Modelling diffusion is a well-established discipline. It is important to assess models that attempt to predict or infer the effects of diffusion limitations in order to report findings with confidence. In this study, we compare equilibration timescales estimated by three different models. Particles were subject to varying saturation ratio changes of a semi-volatile component in the gas phase, with the diffusion coefficient both dependent and independent of composition. We show that introducing a composition dependant diffusion coefficient significantly alters the perceived importance of kinetic mass transfer limitations in viscous aerosol, relative to a constant diffusion coefficient. In a fickian framework, simplified approximations to the partial differential form of Ficks second law can be used for all studied scenarios, although computational expense of previously available models may be an important factor to consider. We demonstrate the ability to capture the behaviour of simulations with compositional dependant diffusion coefficients in a box model framework, enabling potential effects on the microphysics of aerosol populations to be assessed.

  1. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight.

    PubMed

    Loh, N D; Hampton, C Y; Martin, A V; Starodub, D; Sierra, R G; Barty, A; Aquila, A; Schulz, J; Lomb, L; Steinbrener, J; Shoeman, R L; Kassemeyer, S; Bostedt, C; Bozek, J; Epp, S W; Erk, B; Hartmann, R; Rolles, D; Rudenko, A; Rudek, B; Foucar, L; Kimmel, N; Weidenspointner, G; Hauser, G; Holl, P; Pedersoli, E; Liang, M; Hunter, M S; Hunter, M M; Gumprecht, L; Coppola, N; Wunderer, C; Graafsma, H; Maia, F R N C; Ekeberg, T; Hantke, M; Fleckenstein, H; Hirsemann, H; Nass, K; White, T A; Tobias, H J; Farquar, G R; Benner, W H; Hau-Riege, S P; Reich, C; Hartmann, A; Soltau, H; Marchesini, S; Bajt, S; Barthelmess, M; Bucksbaum, P; Hodgson, K O; Strüder, L; Ullrich, J; Frank, M; Schlichting, I; Chapman, H N; Bogan, M J

    2012-06-28

    The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis.

  2. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight.

    PubMed

    Loh, N D; Hampton, C Y; Martin, A V; Starodub, D; Sierra, R G; Barty, A; Aquila, A; Schulz, J; Lomb, L; Steinbrener, J; Shoeman, R L; Kassemeyer, S; Bostedt, C; Bozek, J; Epp, S W; Erk, B; Hartmann, R; Rolles, D; Rudenko, A; Rudek, B; Foucar, L; Kimmel, N; Weidenspointner, G; Hauser, G; Holl, P; Pedersoli, E; Liang, M; Hunter, M S; Hunter, M M; Gumprecht, L; Coppola, N; Wunderer, C; Graafsma, H; Maia, F R N C; Ekeberg, T; Hantke, M; Fleckenstein, H; Hirsemann, H; Nass, K; White, T A; Tobias, H J; Farquar, G R; Benner, W H; Hau-Riege, S P; Reich, C; Hartmann, A; Soltau, H; Marchesini, S; Bajt, S; Barthelmess, M; Bucksbaum, P; Hodgson, K O; Strüder, L; Ullrich, J; Frank, M; Schlichting, I; Chapman, H N; Bogan, M J

    2012-06-28

    The morphology of micrometre-size particulate matter is of critical importance in fields ranging from toxicology to climate science, yet these properties are surprisingly difficult to measure in the particles' native environment. Electron microscopy requires collection of particles on a substrate; visible light scattering provides insufficient resolution; and X-ray synchrotron studies have been limited to ensembles of particles. Here we demonstrate an in situ method for imaging individual sub-micrometre particles to nanometre resolution in their native environment, using intense, coherent X-ray pulses from the Linac Coherent Light Source free-electron laser. We introduced individual aerosol particles into the pulsed X-ray beam, which is sufficiently intense that diffraction from individual particles can be measured for morphological analysis. At the same time, ion fragments ejected from the beam were analysed using mass spectrometry, to determine the composition of single aerosol particles. Our results show the extent of internal dilation symmetry of individual soot particles subject to non-equilibrium aggregation, and the surprisingly large variability in their fractal dimensions. More broadly, our methods can be extended to resolve both static and dynamic morphology of general ensembles of disordered particles. Such general morphology has implications in topics such as solvent accessibilities in proteins, vibrational energy transfer by the hydrodynamic interaction of amino acids, and large-scale production of nanoscale structures by flame synthesis. PMID:22739316

  3. Visibility-reducing organic aerosols in the vicinity of Grand Canyon National Park: 2. Molecular composition

    SciTech Connect

    Mazurek, M.A.; Newman, L.; Daum, P.H.

    1995-12-31

    In this study we examine the molecular organic constituents (C8 to C40 lipid compounds) collected as aerosol from two sites located in Grand Canyon National Park during summer ambient conditions. Of special interest are molecular species which serve as tracers for possible sources of the observed aerosol organic matter. Ambient samples were collected from Hopi Point (rim site) and from Indian Gardens (in-canyon site) as fine (dp< 2.1 =B5m) and total particle samples. The samples were grouped into fine particle and total particle monthly composites to provide sufficient material for molecular marker analysis then analyzed by capillary gas chromatography/mass spectrometry (GUMS), The molecular constituents of each aerosol composite were screened for key tracer compounds using a computerized data reduction method that was based on molecular ion fragment identification. Comparisons were made to a reference database that included molecular information obtained from authentic sources of primary organic aerosol emissions. Emission sources studied included vehicular exhaust, as well as local sources at the Grand Canyon which included soil dust, wood smoke, and particles from vegetation indigenous to the two Grand Canyon sampling sites. Our results show that summertime ambient aerosols contain many organic molecular compounds which can be related directly to the local vegetation. Another major component found in all samples consists of highly oxidized organic species which are not emitted directly from local primary organic aerosol source types. These oxidized species are thought to be secondary organic aerosols that originate from photochemical transformations involving either locally emitted primary organic compounds or transported aged emissions from source regions upwind of the Grand Canyon.

  4. Contact nucleation of ice induced by biological aerosol particles

    NASA Astrophysics Data System (ADS)

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

    2014-05-01

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

  5. 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...

  6. Aerosols in Santiago de Chile: A study using receptor modeling with X-ray fluorescence and single particle analysis

    NASA Astrophysics Data System (ADS)

    Rojas, Carlos M.; Artaxo, Paulo; Van Grieken, René

    Between 15 January and 26 February 1987, 51 fine and coarse mode aerosol samples were collected at the Universidad de Santiago de Chile Planetarium using a dichotomous sampler. The samples were analyzed by X-ray fluorescence for up to 17 elements (Mg, Al, Si, P, S, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Br and Pb). Aerosol particles were individually studied by Electron Probe Microanalysis (EPMA) and Laser Microprobe Mass Analysis (LAMMA). The data set consisting of aerosol elemental concentrations and meteorological variables was subjected to Principal Factor Analysis (PFA), allowing the identification of six fine mode particle source classes (soil, industrial, sulfate particles, traffic, residual oil, wood-burnings), and five coarse mode particle source classes (soil, industrial, traffic, residual oil, sulfate particles). Both PFA solutions explained about 81 and 90% of the total variance in the data set, respectively. The regression of elemental mass concentrations on the Absolute Principal Factor Scores allowed the estimation of the contribution of the different source classes to the Santiago aerosol. Within the fine fraction, secondary SO 42- particles were responsible for about 49% of the fine mode aerosol mass concentration, while 26, 13, 6.4 and 5.6% were attributed to wood-burning/car exhausts, residual oil combustion, soil dust/metallurgical, and soil dust/wood-burning releases, respectively. The coarse fraction source apportionment was mainly dominated by soil dust, accounting for 74% of the coarse mode aerosol mass concentration. A composite of soil dust and industrial release accounted for 13%; a composite of secondary sulfates contributed with 9%; a composite of soil dust and automotive emissions, and secondary sulfates were responsible for 4 and 0.03% of the coarse aerosol mass concentration, respectively. EPMA results are in satisfactory agreement with those from the bulk analysis and allowed the identification of eight particle types in both fine

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  8. Microscopy and Spectroscopy Techniques to Guide Parameters for Modeling Mineral Dust Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Veghte, D. P.; Moore, J. E.; Jensen, L.; Freedman, M. A.

    2013-12-01

    Mineral dust aerosol particles are the second largest emission by mass into the atmosphere and contribute to the largest uncertainty in radiative forcing. Due to the variation in size, composition, and shape, caused by physical and chemical processing, uncertainty exists as to whether mineral dust causes a net warming or cooling effect. We have used Cavity Ring-Down Aerosol Extinction Spectroscopy (CRD-AES), Scanning Electron Microscopy (SEM), and Transmission Electron Microscopy (TEM) to measure extinction cross sections and morphologies of size-selected, non-absorbing and absorbing mineral dust aerosol particles. We have found that microscopy is essential for characterizing the polydispersity of the size selection of non-spherical particles. Through the combined use of CRD-AES, microscopy, and computation (Mie theory and Discreet Dipole Approximation), we have determined the effect of shape on the optical properties of additional species including clay minerals, quartz, and hematite in the sub-micron regime. Our results have shown that calcite can be treated as polydisperse spheres while quartz and hematite need additional modeling parameters to account for their irregularity. Size selection of clay minerals cannot be performed due to their irregular shape, but microscopy techniques can be used to better quantify the particle aspect ratio. Our results demonstrate a new method that can be used to extend cavity ring-down spectroscopy for the measurement of the optical properties of non-spherical particles. This characterization will lead to better aerosol extinction parameters for modeling aerosol optical properties in climate models and satellite retrieval algorithms.

  9. Organic Composition and Morphology of Sea Spray Aerosols as a Function of Biological Life during IMPACTS

    NASA Astrophysics Data System (ADS)

    Pham, D.; Moffet, R.; Fraund, M. W.; O'Brien, R.; Laskina, O.; Prather, K. A.; Grassian, V. H.; Beall, C.; Wang, X.; Forestieri, S.; Cappa, C. D.

    2015-12-01

    Aerosols influence climate by directly reflecting or absorbing sunlight, or indirectly by affecting clouds. A major source of aerosols is from oceanic wave breaking. Due to their complexity, the effects of marine aerosol on climate are uncertain. To provide more detailed measurements of the chemical composition of marine aerosols, Scanning Transmission X-Ray Microscopy coupled with Near Edge X-Ray Absorption Fine Structure (SXTM-NEXAFS) was used to give spatially resolved molecular information for carbon and oxygen. Application of STXM/NEXAFS to particles collected during a mesocosm study using a unique wave channel facility to generate aerosols shows that the organic volume fraction of aerosols at the aerodynamic diameter size range of 0.18-0.32 μm are a direct function of the biological activity in the sea water. Aerosol organic volume fraction increased from 0.32 for particles generated from seawater containing low biolife to 0.49 and 0.40 for particles produced during phytoplankton blooms. However, the organic volume fraction of aerosols at the aerodynamic diameter size range of 0.56-1 μm did not change with biological activity. Measurements also show that different types of organics can concentrate into aerosols depending on the enzyme activity expressed at the time. Enhanced spectral signatures for aliphatic hydrocarbons were observed during the first phytoplankton bloom compared to a second phytoplankton bloom occurring directly thereafter. The decreased signature of aliphatic organics in the second phytoplankton bloom was correlated with increased lipase activity from heterobacteria. Organic aggregates having similar morphology also differ in composition from their carbon spectra from the two blooms. For July 17, organic aggregates were much richer in hydrocarbons, which showed a remarkably intense C-H absorbance and a broad C-C absorbance. Organic aggregates observed for July 26-27, did not have the C-H and C-C signatures, but contained more polar

  10. Kinetics and Products of Heterogeneous Oxidation of Erythritol and Levoglucosan in Aerosol Particles

    NASA Astrophysics Data System (ADS)

    Kessler, S. H.; Kroll, J. H.; Wilson, K. R.; Smith, J. D.

    2009-12-01

    Although organic aerosols in the atmosphere have been implicated in concerns related to both human health and global radiative forcing, they remain collectively a significant source of uncertainty in long-term predictions, in part because of the inherent chemical complexity of possible oxidation products formed from a given compound during its atmospheric lifetime. Here we study the heterogeneous oxidation of model compounds used as surrogates for biomass burning aerosol and secondary organic aerosol (SOA): levoglucosan, a frequently used tracer for biomass burning, and erythritol ((2R,3S)-butane-1,2,3,4-tetraol) an analog of the methyltetrols found in isoprene oxidation SOA. The present experiments are aimed at examining the kinetics and products of further oxidation of both compounds, in order both to explore how each compound contributes to atmospheric aerosol formation and to examine model single-component systems to determine how structural and compositional differences between compounds affect the relative paths of oxidative degradation. Particles are sent through a flow tube reactor where they are exposed to high concentrations (~1013 molecule1 s1 cm-3) of hydroxyl radicals (OH), after which the aerosols are sized and their composition analyzed using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) with both electron impact (EI) and vacuum-ultraviolet (VUV) ionization techniques. Although erythritol and levoglucosan have similar second-order degradation rate constants (2.03 ± 0.20 × 10-13 and 4.7 ± 0.5 × 10-13 cm3 molecule-1 s-1, respectively), the differences between the loss of particle mass upon an equivalent amount of oxidation (80% vs 30% respectively) are much more pronounced.

  11. A role of aerosol particles in forming urban skyglow and skyglow from distant cities

    NASA Astrophysics Data System (ADS)

    Kocifaj, Miroslav; Kómar, Ladislav

    2016-05-01

    Aerosol particles may represent the largest uncertainty about skyglow change in many locations under clear-sky conditions. This is because aerosols are ubiquitous in the atmosphere and influence the ground-reaching radiation in different ways depending on their concentrations, origins, shapes, sizes, and compositions. Large particles tend to scatter in Fraunhofer diffraction regime, while small particles can be treated in terms of Rayleigh formalism. However, the role of particle microphysics in forming the skyglow still remains poorly quantified. We have shown in this paper that the chemistry is somehow important for backscattering from large particles that otherwise work as efficient attenuators of light pollution if composed of absorbing materials. The contribution of large particles to the urban skyglow diminishes as they become more spherical in shape. The intensity of backscattering from non-absorbing particles is more-or-less linearly decreasing function of particle radius even if number size distribution is inversely proportional to the fourth power of particle radius. This is due to single particle backscattering that generally increases steeply as the particle radius approaches large values. Forward scattering depends on the particle shape but is independent of the material composition, thus allowing for a simplistic analytical model of skyglow from distant cities. The model we have developed is based on mean value theorem for integrals and incorporates the parametrizable Garstang's emission pattern, intensity decay along optical beam path, and near-forward scattering in an atmospheric environment. Such model can be used by modellers and experimentalists for rapid estimation of skyglow from distant light sources.

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

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

    SciTech Connect

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

    2009-03-01

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

  14. Neural networks for aerosol particles characterization

    NASA Astrophysics Data System (ADS)

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

    2016-11-01

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

  15. Real time analysis of lead-containing atmospheric particles in Beijing during springtime by single particle aerosol mass spectrometry.

    PubMed

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

    2016-07-01

    Using a single particle aerosol mass spectrometer (SPAMS), the chemical composition and size distributions of lead (Pb)-containing particles with diameter from 0.1 μm to 2.0 μm in Beijing were analyzed in the spring of 2011 during clear, hazy, and dusty days. Based on mass spectral features of particles, cluster analysis was applied to Pb-containing particles, and six major classes were acquired consisting of K-rich, carboneous, Fe-rich, dust, Pb-rich, and Cl-rich particles. Pb-containing particles accounted for 4.2-5.3%, 21.8-22.7%, and 3.2% of total particle number during clear, hazy and dusty days, respectively. K-rich particles are a major contribution to Pb-containing particles, varying from 30.8% to 82.1% of total number of Pb-containing particles, lowest during dusty days and highest during hazy days. The results reflect that the chemical composition and amount of Pb-containing particles has been affected by meteorological conditions as well as the emissions of natural and anthropogenic sources. K-rich particles and carbonaceous particles could be mainly assigned to the emissions of coal combustion. Other classes of Pb-containing particles may be associated with metallurgical processes, coal combustion, dust, and waste incineration etc. In addition, Pb-containing particles during dusty days were first time studied by SPAMS. This method could provide a powerful tool for monitoring and controlling of Pb pollution in real time.

  16. 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

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

    NASA Astrophysics Data System (ADS)

    van Pinxteren, Manuela; Herrmann, Hartmut

    2014-05-01

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

  18. Extractive Electrospray Ionization Mass Spectrometry of Heterogeneous Particles: Implications for Applications to Complex Atmospheric Aerosol

    NASA Astrophysics Data System (ADS)

    Longin, T.; Waring-Kidd, C.; Wingen, L. M.; Lyster, K.; Anderson, C.; Kumbhani, S.; Finlayson-Pitts, B. J.

    2015-12-01

    Extractive electrospray ionization mass spectrometry (EESI-MS) is a direct, real time technique for obtaining mass spectra of gases, liquid droplets, solid particles, and aerosols with little sample processing. EESI-MS involves the interaction of charged electrospray droplets with a separate spray containing the analyte of interest, but the exact mechanism by which the solvent droplets extract analyte from the sample is unclear. Possible mechanisms include complete coalescence of the sample particle with the solvent droplet in which all of the analyte is incorporated into the solvent or a more temporary interaction such that only some of the analyte is transferred to the solvent. Previous studies of the mechanism of EESI-MS on homogeneous particles indicate that both mechanisms are possible. We studied the behavior of EESI-MS toward heterogeneous particles created by coating NaCl particles with various thicknesses of organic diacids. Our results indicate that the signal strength depends on the solubility of the organic acid in the electrospray solvent, in agreement with previous studies, and also that the outer 10-15 nm of the particles are most susceptible to extraction into the electrospray droplets. Our results combined with those of previous studies suggest that the mass spectra obtained with EESI will not necessarily reflect the overall particle composition, especially for particles that are spatially inhomogeneous, and hence caution in interpretation of the data is advised for application to complex atmospheric aerosol.

  19. Measurements of the chemical, physical, and optical properties of single aerosol particles

    NASA Astrophysics Data System (ADS)

    Moffet, Ryan Christopher

    Knowledge of aerosol physical, chemical, optical properties is essential for judging the effect that particulates have on human health, climate and visibility. The aerosol time-of-flight mass spectrometer (ATOFMS) is capable of measuring, in real-time, the size and chemical composition of atmospheric aerosols. This was exemplified by the recent deployments of the ATOFMS to Mexico City and Riverside. The ATOFMS provided rapid information about the major particle types present in the atmosphere. Industrial sources of particles, such as fine mode particles containing lead, zinc and chloride were detected in Mexico City. The rapid time response of the ATOFMS was also exploited to characterize a coarse particle concentrator used in human health effects studies. The ATOFMS showed the ability to detect changes in particle composition with a time resolution of 15 min during short 2 hour human exposure studies. As a major component of this work, an optical measurement has been added to the ATOFMS. The scattered light intensity was acquired for each sized and chemically analyzed particle. This scattering information together with the particle aerodynamic diameter, enabled the refractive index and density of the aerosol to be retrieved. This method was validated in the laboratory using different test particles such as oils, aqueous salt solutions and black carbon particles. It was found that the nozzle-type inlet does not evaporate aqueous salt particles as has been observed for aerodynamic lens inlets. These new optical and microphysical measurements were integrated into the ATOFMS for field deployment in Riverside and Mexico City. For both cities, the different mixing states were found to have unique refractive indexes and densities. A fraction of the strongly absorbing elemental carbon particles were observed to have a spherical morphology due to heavy mixing with secondary species. In addition to the quantitative refractive index and effective density measurements

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

    SciTech Connect

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

    2015-04-21

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

  1. 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

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

    1999-07-14

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

  3. 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.

  4. 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

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

    PubMed

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

    2010-10-14

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  7. Predicting the mineral composition of dust aerosols - Part 1: Representing key processes

    NASA Astrophysics Data System (ADS)

    Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

    2015-02-01

    Soil dust aerosols created by wind erosion are typically assigned globally uniform physical and chemical properties within Earth system models, despite known regional variations in the mineral content of the parent soil. Mineral composition of the aerosol particles is important to their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, coating by heterogeneous uptake of sulfates and nitrates, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Here, aerosol mineral composition is derived by extending a method that provides the composition of a wet-sieved soil. The extension accounts for measurements showing significant differences between the mineral fractions of the wet-sieved soil and the resulting aerosol concentration. For example, some phyllosilicate aerosols are more prevalent at silt sizes, even though they are nearly absent in a soil whose aggregates are dispersed by wet sieving during analysis. We reconstruct the undispersed size distribution of the original soil that is subject to wind erosion. An empirical constraint upon the relative emission of clay and silt is applied that further differentiates the soil and aerosol mineral composition. In addition, a method is proposed for mixing minerals with small impurities composed of iron oxides. These mixtures are important for transporting iron far from the dust source, because pure iron oxides are more dense and vulnerable to gravitational removal than most minerals comprising dust aerosols. A limited comparison to measurements from North Africa shows that the extension brings the model into better agreement, consistent with a more extensive comparison to global observations as well as measurements of elemental composition downwind of the Sahara, as described in companion articles.

  8. The Effect of Particle Size on Iron Solubility in Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Marcotte, A. R.; Majestic, B. J.; Anbar, A. D.; Herckes, P.

    2012-12-01

    The long range transport of mineral dust aerosols, which contain approximately 3% iron by mass, results in an estimated 14-16 Tg of iron deposited into the oceans annually; however, only a small percentage of the deposited iron is soluble. In high-nutrient, low chlorophyll ocean regions iron solubility may limit phytoplankton primary productivity. Although the atmospheric transport processes of mineral dust aerosols have been well studied, the role of particle size has been given little attention. In this work, the effect of particle size on iron solubility in atmospheric aerosols is examined. Iron-containing minerals (illite, kaolinite, magnetite, goethite, red hematite, black hematite, and quartz) were separated into five size fractions (10-2.5, 2.5-1, 1-0.5, 0.5-0.25, and <0.25μm) and extracted into buffer solutions simulating environments in the transport of aerosol particles for 150 minutes. Particle size was confirmed by scanning electron microscopy (SEM). Soluble iron content of the extracted mineral solutions was determined by inductively coupled plasma-mass spectrometry (ICP-MS). Extracted mineral solutions were also analyzed for Fe(II) and Fe(III) content using a ferrozine/UV-VIS method. Preliminary results show that differences in solution composition are more important than differences in size. When extracted into acetate and cloudwater buffers (pH 4.25-4.3), < 0.3% of the Fe in iron oxides (hematite, magnetite, and goethite) is transferred to solution as compared to ~0.1-35% for clays (kaolinite and illite). When extracted into a marine aerosol solution (pH 1.7), the percentage of Fe of the iron oxides and clays transferred to solution increases to approximately 0.5-3% and 5-70%, respectively. However, there is a trend of increased %Fe in the minerals transferred to solution in the largest and smallest size fractions (~0.01-0.3% and ~0.5-35% for iron oxides and clays, respectively), and decreased %Fe in the minerals transferred to solution in the mid

  9. Virtual Impactor for Sub-micron Aerosol Particles

    NASA Astrophysics Data System (ADS)

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

    2005-12-01

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

  10. Combined effects of organic aerosol loading and fog processing on organic aerosols oxidation and composition

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Tripathi, Sachchida; Gupta, Tarun

    2016-04-01

    Fog is a natural meteorological phenomenon that occurs throughout the world, it contains substantial quantity of liquid water and generally seen as a natural cleansing agent but it also has the potential to form highly oxidized secondary organic aerosols (SOA) via aqueous processing of ambient aerosols. On the other hand higher organic aerosols (OA) loading tend to decrease the overall oxidation level (O/C) of the particle phase organics, due to enhanced partitioning of less oxidized organics from gas to particle phase. However, combined impact of these two parameters; aqueous oxidation and OA loading, on the overall oxidation ratio (O/C) of ambient OA has never been studied. To assess this, real time ambient sampling using HR-ToF-AMS was carried out at Kanpur, India from 15 December 2014 - 10 February 2015. In first 3 weeks of this campaign, very high OA loading is (134 ± 42 μg/m3) observed (termed as high loading or HL period) while loading is substantially reduced from 2nd January, 2016 (56 ± 20 μg/m3, termed as low loading or LL period) . However, both the loading period was affected by several fog episodes (10 in HL and 7 in LL), thus providing the opportunity of studying the combined effects of fog and OA loading on OA oxidation. It is found that O/C ratio is very strongly anti-correlated with OA loading in both the loading period, however, slope of this ant-correlation is much steep during HL period than in LL period. Source apportionment of OA revealed that there is drastic change in the types of OA from HL to LL period, clearly indicating difference in OA composition from HL to LL period. During foggy night continuous oxidation of OA is observed from early evening to early morning with 15-20% enhancement in O/C ratio, while the same is absent during non-foggy period, clearly indicating the efficient fog processing of ambient OA. It is also found that night time fog aqueous oxidation can be as effective as daytime photo chemistry in oxidation of OA. Fog

  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. Morphology, composition, and atmospheric processing of soot particles

    NASA Astrophysics Data System (ADS)

    Slowik, Jay G.

    Combustion-generated soot aerosols play an important role in climate forcing due to their strong light-absorbing properties. Quantitative measurement of BC is challenging because BC often occurs in highly non-spherical soot particles of complex morphology. The task is further complicated because of the lack of an unambiguous chemical definition of the material. Here we present the development and application of a new technique for determining particle morphology and composition. Simultaneous measurements of mobility diameter, vacuum aerodynamic diameter, and non-refractory composition were used to determine the particle mass, volume, density, composition, dynamic shape factor, and fractal dimension. Under certain conditions, particle surface area and the number and size of the primary spherules composing the soot fractal aggregates were also determined. The particle characterization technique described above was applied to the following four studies: (1) Characterization of flame-generated soot particles. Depending on flame conditions, either fractal or near-spherical particles were generated and their properties interpreted in terms of the mechanism for soot formation. (2) Coating and denuding experiments were performed on soot particles. The results yielded information about morphology changes to the entire soot particle and to the internal black carbon structure due to atmospheric processing. The denuding experiments also provided particle surface area, which was used to determine the atmospheric lifetime of fractal soot particles relative to spheres. (3) An inter-comparison study of instruments measuring the black carbon content of soot particles was conducted. The detailed characterization of soot particles enabled a number of assumptions about the operation of the selected instruments to be tested. (4) Ambient particles were sampled in Mexico City. In the early morning, ambient particles were detected with a fractal morphology similar to that of diesel

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

    NASA Astrophysics Data System (ADS)

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

    2007-12-01

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

  14. Influence of Heterogeneous OH Oxidation on the Evaporation Behavior and Composition of a Model Organic Aerosol

    NASA Astrophysics Data System (ADS)

    Kolesar, K. R.; Cappa, C. D.; Wilson, K. R.

    2011-12-01

    Heterogeneously oxidized squalane particles are used here as a model system to investigate the interplay between chemical composition and particle volatility. Reaction of squalane particles by OH radicals leads to the production of oxygenated products. Here we use the vacuum ultra-violet Aerosol Mass Spectrometer (VUV-AMS) at beamline 9.0.2 at the Advanced Light Source to monitor the evolution of specific oxidation products that result from increasing OH exposures, and how the composition changes as the oxidized particles evaporate. The soft ionization in the VUV-AMS allows us to uniquely track the parent squalane molecule and the various oxidation products over multiple generations of oxidation. Compositional changes of the oxidized particles resulting from evaporation have been measured in three sets of laboratory experiments. In the first set, a thermodenuder at varying temperatures was used to induce evaporation of particles at a fixed OH exposure. Second, the OH exposure was varied along with temperature to create a cross-sectional observation of particle composition at 50% mass fraction remaining for ten different oxidation levels. The combination of these two experiments provides information as to the compositional changes that occur during evaporation due to heating. In the third set of experiments, VUV-AMS spectra of oxidized squalane particles following dilution-induced evaporation were measured for comparison with the thermodenuder experiments. These experiments provide insights into the relationships between particle oxidation, composition and evaporation kinetics.

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

    NASA Astrophysics Data System (ADS)

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

    2014-02-01

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

  16. Impact of aerosol composition and foliage characteristics on forest canopy deposition rates: A laboratory study

    NASA Astrophysics Data System (ADS)

    Hornsby, K. E.; Pryor, S. C.

    2013-12-01

    Forests are a major sink for atmospheric aerosols. Hence it has been suggested that (i) increased tree planting in urban areas might lead to a reduction in aerosol particle concentrations and thus a reduction in respiratory conditions and heart complications, and (ii) forests may be responsible for removing a disproportionately large fraction of potentially climate-relevant fine and ultra-fine aerosol particles from the atmosphere. However, larger uncertainties remain with respect to controls on uptake rates for forests. E.g. the deposition flux partitioning between foliage and non-foliage elements, the influence of particle size and composition, the role of leaf surface morphology and stomatal aperture in surface uptake. Improved understanding of the relative importance of these factors and the variability across different tree species should help determine how much of a sink naturally occurring and planted forests can provide downstream of fine particle production. In this study, a sample of trees native to southern Indiana were exposed to ultra-fine aerosol particle populations in a 1.5 m x 1.5 m x 1.5 m Teflon chamber. Stable particle size distributions (PSD) with geometric mean diameters (GMD) ranging from 40 to 80 nm were generated from sodium chloride, ammonium nitrate, ammonium sulfate and sodium sulfite solutions using a TSI model 3940 Aerosol Generation System (AGS). The aerosol stream was diluted using scrubbed and dried zero air to allow a variation of total number concentration across two orders of magnitude. PSD in the chamber are continuously measured using a TSI Scanning Mobility Particle Spectrometer (SMPS) comprising an Electrostatic Classifier (EC model 3080) attached to a Long DMA (LDMA model 3081) and a TSI model 3025A Butanol Condensation Particle Counter (CPC) operated with both the internal diffusion loss and multiple charge corrections turned on. The composition of the chamber air was also monitored for carbon dioxide (CO2) and water vapor

  17. Size effects in aerosol particle interactions: the van der Waals potential and collision rates

    SciTech Connect

    Marlow, W H

    1980-01-01

    Three effects which are explicitly dependent on aerosol particle size are identified and discussed. They are focussed about the particle collision rate and how it relates to the properties of the gas, the particle, and the particle's interaction potential energy which play roles in particle-particle collision rates. By incorporating the conduction electronic free path effect for conductors into the frequency-dependent dielectric constants of silver and graphite, particle size effects in the Lifshitz-van der Waals potentials for identical pairs of 1 nm and 100 nm particles are evaluated. Water and tetradecane particle interaction potentials for the same size particles are also calculated to illustrate size effects due to the retardation of the interaction. These potentials are then used to calculate the enhancement of the particle collision rates above their values in the absence of any potential at various gas pressures. The roles of the interaction potential in collision among identical pairs of particles of differing compositions is also briefly discussed.

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

    NASA Astrophysics Data System (ADS)

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

    2012-12-01

    The MISR instrument aboard the NASA Earth Observing System's Terra satellite has the unique capability to retrieve aerosol properties under favorable conditions. General aerosol type retrieval quality guidelines are provided in the MISR Data Quality Statement and related publications. Here we report on the steps we are taking to provide an aerosol-type data quality flag, to be provided with each individual retrieval result. Some factors affecting retrieval quality that can be assessed pre-retrieval are the number of cameras available, the range of scattering angles and surface conditions such as shallow water or seasonal coastal runoff. Factors that must be assessed post-retrieval include low values of retrieved optical depth and the number and type of mixtures successfully passing the MISR algorithm acceptance criteria. Regional monthly plots with MISR measurements binned at 0.5 degree resolution with color-coded stratification of one or more parameters is the main method for identifying locations and times where particle properties are retrieved. Individual MISR values such as mid-visible AOD, number and type of mixtures passing, number of cameras used, the range and maximum scattering angles are plotted individually or as joint distributions. Initially, thresholds and conditions are determined for each MISR parameter separately. Finally, MISR parameters are combined for a given month and region, with their thresholds, to show the overall quality of the retrieval for determining particle properties. Multi-month summaries for more than twelve years of MISR data will aid in assessing quality. Seasons and regions that regularly show poorly constrained aerosol type results are identified, as are times and places where particle property information can be used with confidence. This work is performed in part at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration and in part at the NASA

  19. Liquid-liquid phase separation in aerosol particles: imaging at the nanometer scale.

    PubMed

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

    2015-04-21

    Atmospheric aerosols can undergo phase transitions including liquid-liquid phase separation (LLPS) while responding to changes in the ambient relative humidity (RH). Here, we report results of chemical imaging experiments using environmental scanning electron microscopy (ESEM) and scanning transmission X-ray microscopy (STXM) to investigate the LLPS of micrometer-sized particles undergoing a full hydration-dehydration cycle. Internally mixed particles composed of ammonium sulfate (AS) and either: limonene secondary organic carbon (LSOC), α, 4-dihydroxy-3-methoxybenzeneaceticacid (HMMA), or polyethylene glycol (PEG-400) were studied. Events of LLPS were observed for all samples with both techniques. Chemical imaging with STXM showed that both LSOC/AS and HMMA/AS particles were never homogeneously mixed for all measured RH's above the deliquescence point and that the majority of the organic component was located in the outer phase. The outer phase composition was estimated as 65:35 organic: inorganic in LSOC/AS and as 50:50 organic: inorganic for HMMA/AS. PEG-400/AS particles showed fully homogeneous mixtures at high RH and phase separated below 89-92% RH with an estimated 70:30% organic to inorganic mix in the outer phase. These two chemical imaging techniques are well suited for in situ analysis of the hygroscopic behavior, phase separation, and surface composition of collected ambient aerosol particles.

  20. [Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer (SPAMS)].

    PubMed

    Mu, Ying-Ying; Lou, Sheng-Rong; Chen, Chang-Hong; Zhou, Min; Wang, Hong-Li; Zhou, Zhen; Qiao, Li-Ping; Huang, Cheng; Li, Mei; Li, Li; Wang, Qian; Huang, Hai-Ying; Zou, Lan-Jun

    2013-06-01

    A single particle aerosol mass spectrometer (SPAMS) was applied to characterize the size distribution (200 nm-2.0 microm) and chemical compositions of ambient particles during a polluted event from 11th to 18th, November 2011. OCEC, METAL, EC, SECONDARY and K-Na types of particulates were the dominant groups observed in hazy day period, which were 27.4%, 3.4%, 7.3% , 45.6% and 5.4% of the overall measured particles, respectively. The observed five types of particles contained the secondary composition such as 18NH4(+), 80SO3(-), 96SO4(-), 97HSO4(-), 46NO2(-), 62NO3(-) and 125H (NO3) -, showing that they probably went through different aging processes, and the increasing of the SECONDARY particles during the event clearly indicated a secondary aerosol pollution. Heterogeneous reactions of SO2 and particles could be the reason of strong 97HSO4(-) signals in the mass spectrums of OCEC type particles while the existence of organic compounds might have an important influence on the aerosol formation with the gas-phase sulfuric acid. Fresh EC particles in the environment tended to be aging with above-mentioned secondary ions by the analysis of particle size distribution and eventually lead to a particle type conversion from EC to SECONDARY. Organic amine in marine environment was brought to the land by the warm, moist marine air mass that dramatically removed atmospheric SECONDARY and OCEC particles from the air with a heavy rain and leading to the observation of amine particles in the clean day period. PMID:23947016

  1. [Aging and mixing state of particulate matter during aerosol pollution episode in autumn Shanghai using a single particle aerosol mass spectrometer (SPAMS)].

    PubMed

    Mu, Ying-Ying; Lou, Sheng-Rong; Chen, Chang-Hong; Zhou, Min; Wang, Hong-Li; Zhou, Zhen; Qiao, Li-Ping; Huang, Cheng; Li, Mei; Li, Li; Wang, Qian; Huang, Hai-Ying; Zou, Lan-Jun

    2013-06-01

    A single particle aerosol mass spectrometer (SPAMS) was applied to characterize the size distribution (200 nm-2.0 microm) and chemical compositions of ambient particles during a polluted event from 11th to 18th, November 2011. OCEC, METAL, EC, SECONDARY and K-Na types of particulates were the dominant groups observed in hazy day period, which were 27.4%, 3.4%, 7.3% , 45.6% and 5.4% of the overall measured particles, respectively. The observed five types of particles contained the secondary composition such as 18NH4(+), 80SO3(-), 96SO4(-), 97HSO4(-), 46NO2(-), 62NO3(-) and 125H (NO3) -, showing that they probably went through different aging processes, and the increasing of the SECONDARY particles during the event clearly indicated a secondary aerosol pollution. Heterogeneous reactions of SO2 and particles could be the reason of strong 97HSO4(-) signals in the mass spectrums of OCEC type particles while the existence of organic compounds might have an important influence on the aerosol formation with the gas-phase sulfuric acid. Fresh EC particles in the environment tended to be aging with above-mentioned secondary ions by the analysis of particle size distribution and eventually lead to a particle type conversion from EC to SECONDARY. Organic amine in marine environment was brought to the land by the warm, moist marine air mass that dramatically removed atmospheric SECONDARY and OCEC particles from the air with a heavy rain and leading to the observation of amine particles in the clean day period.

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  3. Microphysical aerosol parameters of spheroidal particles via regularized inversion of lidar data

    NASA Astrophysics Data System (ADS)

    Samaras, Stefanos; Böckmann, Christine

    2015-04-01

    One of the main topics in understanding the aerosol impact on climate requires the investigation of the spatial and temporal variability of microphysical properties of particles, e.g., the complex refractive index, the effective radius, the volume and surface-area concentration, and the single-scattering albedo. Remote sensing is a technique used to monitor aerosols in global coverage and fill in the observational gap. This research topic involves using multi-wavelength Raman lidar systems to extract the microphysical properties of aerosol particles, along with depolarization signals to account for the non-sphericity of the latter. Given, the optical parameters (measured by a lidar), the kernel functions, which summarize the size, shape and composition of particles, we solve for the size distribution of the particles modeled by a Fredholm integral system and further calculate the refractive index. This model works well for spherical particles (e.g. smoke); the kernel functions are derived from relatively simplified formulas (Mie scattering theory) and research has led to successful retrievals for particles which at least resemble a spherical geometry (small depolarization ratio). Obviously, more complicated atmospheric structures (e.g dust) require employment of non-spherical kernels and/or more complicated models which are investigated in this paper. The new model is now a two-dimensional one including the aspect ratio of spheroidal particles. The spheroidal kernel functions are able to be calculated via T-Matrix; a technique used for computing electromagnetic scattering by single, homogeneous, arbitrarily shaped particles. In order to speed up the process and massively perform simulation tests, we created a software interface using different regularization methods and parameter choice rules. The following methods have been used: Truncated singular value decomposition and Pade iteration with the discrepancy principle, and Tikhonov regularization with the L

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

    SciTech Connect

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

    2015-09-28

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

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

    NASA Technical Reports Server (NTRS)

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

    2000-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  9. Using microchip electrophoresis for real-time aerosol composition measurements: Field study results from San Gorgonio Wilderness, California

    NASA Astrophysics Data System (ADS)

    Evanoski-Cole, A. R.; Hecobian, A.; Lewis, G. S.; Hering, S. V.; Henry, C. S.; Collett, J. L.

    2012-12-01

    The detrimental impacts of atmospheric aerosol on human and ecosystem health, visibility and climate change have been studied extensively. However, the role of aerosol composition in these issues still needs further investigation due to the variability of aerosol particles over both time and space. The need for better temporal and spatial resolution of aerosol composition measurements is addressed in the development of a real-time instrument using microchip capillary electrophoresis. Termed Aerosol microChip Electrophoresis (ACE), this lab-on-a-chip instrument is inexpensive to manufacture, portable and provides sensitive real-time and semi-continuous aerosol composition measurements. A water condensation growth tube is used to enlarge water soluble aerosol particles with an aerodynamic diameter less than 2.5 μm. The aqueous sample is continuously collected by impaction into a sample reservoir on a custom designed microchip. A rapid separation of select aerosol components is achieved using microchip capillary electrophoresis coupled with conductivity detection. Here we present data from a recent field campaign in the San Gorgonio Wilderness in south western California. This unique high elevation wilderness site located to the east of the heavily populated cities of San Bernardino and Los Angeles provides a contrast of both clean background and aged urban aerosol as dictated by the meteorological conditions at the site. Ambient aerosol particles were continuously collected at a flow rate of 0.7 L/min into a liquid sample with a volume of 16.7 μL and then analyzed for sulfate, nitrate, chloride and oxalate every 48 seconds. When comparing the ambient concentrations with the meteorological conditions, the most notable trend was high nitrate and sulfate concentrations in ambient aerosol during upslope wind events, with values reaching as high as 34 and 5 μg/m3, respectively. Comparison aerosol composition measurements from filter samples and a particle

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

    NASA Technical Reports Server (NTRS)

    Buseck, Peter R.

    2004-01-01

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

  11. Exploration of the seasonal variation of organic aerosol composition using an explicit modeling approach

    NASA Astrophysics Data System (ADS)

    Ouzebidour, Farida; Camredon, Marie; Stéphanie La, Yuyi; Madronich, Sasha; Taylor, Julia Lee; Hodzic, Alma; Beekmann, Matthias; Siour, Guillaume; Aumont, Bernard

    2014-05-01

    Organic compounds account for a major fraction of fine aerosols in the atmosphere. This organic fraction is dominated by secondary organic aerosol (SOA). Processes leading to SOA formation are however still uncertain and SOA composition is far from being fully characterized. The goals of this study are to evaluate our current understanding of SOA formation and explore its composition. For this purpose, a box-model that describes explicitly processes involved in SOA formation has been developed. This model includes the emission of 183 gaseous and particulate organic compounds. The oxidation of these emitted organic compounds is described using the Generator of Explicit Chemistry and Kinetics of Organics in the Atmosphere (GECKO-A). Gas/particle partitioning has been implemented considering an ideal homogeneous condensed phase. The generated chemical scheme contains 500,000 species and the gas/particle partitioning is performed for 90,000 of them. Simulations have been performed for summer and winter scenarios representative of continental and urban conditions. NOx and ozone simulated concentrations reproduce the expected winter and summer diurnal evolutions. The predicted organic aerosol composition is a mixture of primary and secondary organic aerosols during the winter and is largely dominated by SOA during the summer.

  12. The Influence of Aerosol Composition on Photolysis Rates Based on Airborne Observations

    NASA Astrophysics Data System (ADS)

    Corr, C.; Barrick, J. D. W.; Beyersdorf, A. J.; Chen, G.; Crawford, J. H.; Jordan, C. E.; Moore, R.; Shook, M.; Thornhill, K. L., II; Winstead, E.; Ziemba, L. D.; Madronich, S.; Anderson, B. E.

    2015-12-01

    The potential variability in modeled photolysis rates introduced by aerosol optical properties measured at visible wavelengths is presented here. Aerosol scattering and absorption were measured aboard the NASA P-3B aircraft during the Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) using a TSI Nephelometer and a Radiance Research Particle Soot Absorption Photometer (PSAP), respectively. To isolate the effect of aerosols on photolysis rates, cloud-free case studies were identified using aircraft videos for the four DISCOVER-AQ deployments: Baltimore, MD-Washington, D.C. in July 2011, the California Central Valley in January/February 2013, Houston, TX in September 2013, and Denver, CO in July 2014. For these case studies, absorption measurements at 470 and 532 nm were extrapolated to the Nephelometer wavelengths (450 and 550nm) using the 470-532nm absorption Angstrom exponent (AAE470-532) to calculate aerosol extinction and SSAs at these wavelengths. Photolysis rates were modeled using the Tropospheric Ultraviolet model version 5.2 (TUV 5.2) for three scenarios: 1) an aerosol-free case, 2) using a spectrally-flat SSA at 550nm and 3) using a spectrally-dependent SSA derived from scattering and absorption measurements. Modeled photolysis rates were compared to those measured aboard the P-3B during DISCOVER-AQ. The relationship between airborne measurements of water soluble organic carbon (WSOC) made by a Particle-Into-Liquid-Sampler (PILS), AAE470-532 and model/measurement discrepancies were explored to assess the influence of aerosol composition on photolysis rates. Additional comparisons between photolysis rates modeled with vertically-resolved aerosol optical properties and those modeled using column-average values were performed to assess the influence of aerosol vertical distribution on photolysis rates.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

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

  16. Characteristics of fine and coarse particles of natural and urban aerosols of Brazil

    NASA Astrophysics Data System (ADS)

    Orsini, C. Q.; Tabacniks, M. H.; Artaxo, P.; Andrade, M. F.; Kerr, A. S.

    Fine and coarse particles have been sampled from 1982 to 1985 in one natural forest seacoast site (Juréia) and five urban-industrial cities (Vitória, Salvador, Porto Alegre, São Paulo and Belo Horizonte). The time variations of concentrations in air and the relative elemental compositions of fine and coarse particle fractions, sampled by Nuclepore stacked filter units (SFU), have been determined gravimetrically and by PIXE analysis, respectively. Enrichment factors and correlation coefficients of the trace elements measured led to unambiguous characterization of soil dust and sea salt, both major aerosol sources that emit coarse particles, and soil dust is also a significant source of fine particles.

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

    The tropics emit a huge amount of volatile organic compounds (VOCs) into the Earth's atmosphere. The processes by which these gases are oxidised to form secondary organic aerosol (SOA) are currently not well understood or quantified. Intensive field measurements were carried out as part of the Oxidant and Particle Photochemical Processes (OP3) and the Aerosol Coupling in the Earth System (ACES) projects around pristine rainforest in Malaysian Borneo. This is the first campaign of its type in a South East Asian rainforest. We present detailed organic aerosol composition measurements made using an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) at Bukit Atur, a Global Atmosphere Watch site located in the Danum Valley Conservation Area. This is a state-of-the-art field deployable instrument that can provide real time composition, mass loading and aerodynamic particle sizing information. In addition, the mass spectral resolution is sufficient to perform an analysis of the elemental composition of the organic species present. Other tools such as positive matrix factorisation (PMF) have been used to help assess the relative source contributions to the organic aerosol. A suite of supporting aerosol and gas phase measurements were made, including size resolved number concentration measurements with Differential Mobility Particle Sizer (DMPS), as well as absorption measurements made with a Multi-Angle Absorption Photometer (MAAP). The ground site data are compared with Aerodyne Compact Time of Flight Aerosol Mass Spectrometer (C-ToF-AMS) measurements made on the UK Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft. Airborne measurements were made above pristine rainforest surrounding the Danum Valley site, as well as nearby oil palm agricultural sites and palm oil rendering plants. Airborne hygroscopicity was measured using a Droplet Measurement Technology Cloud Condensation Nuclei counter (DMT CCN counter) in

  18. 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.

  19. Sea Spray Aerosol Structure and Composition Using Cryogenic Transmission Electron Microscopy

    PubMed Central

    2016-01-01

    The composition and surface properties of atmospheric aerosol particles largely control their impact on climate by affecting their ability to uptake water, react heterogeneously, and nucleate ice in clouds. However, in the vacuum of a conventional electron microscope, the native surface and internal structure often undergo physicochemical rearrangement resulting in surfaces that are quite different from their atmospheric configurations. Herein, we report the development of cryogenic transmission electron microscopy where laboratory generated sea spray aerosol particles are flash frozen in their native state with iterative and controlled thermal and/or pressure exposures and then probed by electron microscopy. This unique approach allows for the detection of not only mixed salts, but also soft materials including whole hydrated bacteria, diatoms, virus particles, marine vesicles, as well as gel networks within hydrated salt droplets—all of which will have distinct biological, chemical, and physical processes. We anticipate this method will open up a new avenue of analysis for aerosol particles, not only for ocean-derived aerosols, but for those produced from other sources where there is interest in the transfer of organic or biological species from the biosphere to the atmosphere. PMID:26878061

  20. 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...

  1. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2012-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2011-10-01

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

  4. 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.

  5. 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

  6. Lidar determination of the composition of atmosphere aerosols

    NASA Technical Reports Server (NTRS)

    Wright, M. L.

    1980-01-01

    Theoretical and experimental studies of the feasibility of using DIfferential SCatter (DISC) lidar to measure the composition of atmospheric aerosols are described. This technique involves multiwavelength measurements of the backscatter cross section of aerosols in the middle infrared, where a number of materials display strong restrahlen features that significantly modulate the backscatter spectrum. The theoretical work indicates that a number of materials of interest, including sulfuric acid, ammonium sulfate, and silicates, can be discriminated among with a CO2 lidar. An initial evaluation of this procedure was performed in which cirrus clouds and lower altitude tropospheric aerosols were developed. The observed ratio spectrum of the two types of aerosol displays structure that is in crude accord with theoretical expectations.

  7. Predicting the Mineral and Chemical Composition of Dust Aerosols: Evaluation and Implications

    NASA Astrophysics Data System (ADS)

    Perlwitz, J. P.; Pérez García-Pando, C.; Miller, R. L.

    2014-12-01

    Soil dust aerosols in Earth system models are typically assumed to have globally uniform properties. However, important climate processes related to dust depend on the aerosol mineral and chemical composition, which varies regionally. Such processes include aerosol radiative forcing, transport of bioavailable iron that catalyzes marine photosynthesis, heterogeneous chemistry, ice nucleation, and cloud condensation.We have implemented a new version of the soil dust aerosol scheme in the NASA GISS Earth System ModelE that takes into account the mineral composition of the dust particles. Dust aerosols are represented as an external mixture of minerals such as illite, kaolinite, smectite, carbonates, quartz, feldspar and gypsum, as well as iron oxides and accretions of iron oxides with each of the these minerals.We present a new publically available compilation of measurements of mineral fractions derived from ca. 50 references from the literature. This compilation is used to evaluate our new model of mineral and elemental composition within ModelE. We discuss the challenges of comparing simulated mineral fractions to measurements, which often come from field campaigns and ship cruises of limited duration. Despite uncertainties of the measurements, we show the importance of estimating the undisturbed size distribution of the parent soil prior to wet sieving, along with the modification of this size distribution during emission. In particular, our new model reproduces measurements showing greater amount of aerosols at silt sizes (whose diameters exceed 2 μm) including significant amounts of clay mineral aerosols (like illite) at silt sizes. Our model also reduces the systematic overestimation of quartz, while allowing iron to be transported farther from its source as impurities than in its pure, crystalline form.

  8. 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

  9. 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

  10. The mixing state of carbonaceous aerosol particles in northern and southern California measured during CARES and CalNex 2010

    SciTech Connect

    Cahill, John F.; Suski, Kaitlyn; Seinfeld, John H.; Zaveri, Rahul A.; Prather, Kimberly A.

    2012-11-21

    Carbonaceous aerosols impact climate directly by scattering and absorbing radiation, and hence play a major, although highly uncertain, role in global radiative forcing. Commonly, ambient carbonaceous aerosols are internally mixed with secondary species such as nitrate, sulfate, and ammonium, which influence their climate impacts through optical properties, hygroscopicity, and atmospheric lifetime. Aircraft-aerosol time-of-flight mass spectrometry (A-ATOFMS), which measures single-particle mixing state, was used to determine the fraction of organic and soot aerosols that were internally mixed and the variability of their mixing state in California during the Carbonaceous Aerosol and Radiative Effects Study (CARES) and the Research at the Nexus of Air Quality and Climate Change (CalNex) field campaigns in the late spring and early summer of 2010. Nearly 88% of all A-ATOFMS measured particles (100-1000 nm in diameter) were internally mixed with secondary species, with 96% and 75% of particles internally mixed with nitrate and/or sulfate in southern and northern California, respectively. Even though atmospheric particle composition in both regions was primarily influenced by urban sources, the mixing state was found to vary greatly, with nitrate and soot being the dominant species in southern California, and sulfate and organic carbon in northern California. Furthermore, mixing state varied temporally in northern California, with soot becoming the prevalent particle type towards the end of the study as regional pollution levels increased. The results from these studies demonstrate that the majority of ambient carbonaceous particles are internally mixed and are heavily influenced by secondary species that are most predominant in each region. Based on these findings, considerations of regionally dominant sources and secondary species, as well as temporal variations of aerosol physical and optical properties, will be required to obtain more accurate predictions of the

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

    PubMed

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

    2011-07-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-03-01

    there. Thus, larger scale forcings that impact cloud macrophysical properties, as well as enhanced aerosol particles, are important in determining cloud droplet size and cloud albedo. Differences in the size distribution of droplet residual particles and ambient aerosol particles were observed. By progressively excluding small droplets from the CVI sample, we were able to show that the larger drops, some of which may initiate drizzle, contain the largest aerosol particles. Geometric mean diameters of droplet residual particles were larger than those of the below-cloud and above cloud distributions. However, a wide range of particle sizes can act as droplet nuclei in these stratocumulus clouds. A detailed LES microphysical model was used to show that this can occur without invoking differences in chemical composition of cloud-nucleating particles.

  13. Seasonal differences of urban organic aerosol composition - an ultra-high resolution mass spectrometry study

    NASA Astrophysics Data System (ADS)

    Rincon, A. G.; Calvo, A. I.; Dietzel, M.; Kalberer, M.

    2012-04-01

    The understanding of the chemical composition of atmospheric aerosols, their properties and reactivity are important for assessing aerosol effects upon both global climate change and human health. The composition of organic aerosols is poorly understood mainly due to their highly complex chemical composition with several thousand compounds. In the present study the water-soluble organic fraction of ambient particles collected at an urban site in Cambridge, UK, during different seasons were analysed with ultra-high resolution mass spectrometry. For several thousand peaks in the mass specta (between 3000-6000) an elemental composition could be assigned and summer samples generally contained more components than winter samples. Up to 80% of the peaks in the mass spectra contain nitrogen and/or sulphur functional groups and only about 20% of the compounds contain only C, H and O atoms. In summer the fraction of compounds with oxidized nitrogen and sulphur groups increases compared to winter indicating a photo-chemical formation route of these multifunctional compounds. In addition to oxidized nitrogen compounds a large number of highly unsaturated reduced nitrogen-containing compounds were detected, corresponding likely to cyclic amines. A significant number of oxidized PAHs have been detected in summer samples, which were not present in winter, indicating again photo-chemical aging processes. Both, amines and long-chain aliphatic acids (also frequently observed in these urban samples) are likely signatures of biomass burning and primary biological sources. Potential biomass burning markers are discussed. Particle-phase oligomerisation reactions have only been observed to a very limited degree. Compounds larger than m/z 350 almost exclusively contained N and/or S functional groups indicating that the high molecular weight compounds in these organic aerosol extracts might be mainly due to particle-phase heterogeneous reactions of organic compounds with inorganic

  14. Laboratory studies of collection efficiency of sub-micrometer aerosol particles by cloud droplets on a single droplet basis

    NASA Astrophysics Data System (ADS)

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

    2015-03-01

    An experimental setup has been constructed to measure the Collection Efficiency (CE) of sub-micrometer aerosol particles by cloud droplets. Water droplets of a dilute aqueous ammonium sulfate solution with a radius of ~20 μm fall freely into a chamber and collide with sub-micrometer Polystyrene Latex Sphere (PSL) particles of variable size and concentrations. Two RH conditions, ~15 and ~88%, hereafter termed "Low" and "High", respectively, were varied with different particles size and concentrations. After passing through the chamber, the droplets and aerosol particles were sent to the Particle Analysis by Laser Mass Spectrometry (PALMS) instrument to determine chemical compositions on a single particle basis. Coagulated droplets had mass spectra that contain signatures from both an aerosol particle and a droplet residual. CE values range from 5.7 × 10-3 to 4.6 × 10-2 for the Low RH and from 6.4 × 10-3 to 2.2 × 10-2 for the High RH cases. CE values were, within experimental uncertainty, independent of the aerosol concentrations. CE values in this work were found to be in agreement with previous experimental and theoretical studies. To our knowledge, this is the first coagulation experiment performed on a single droplet basis.

  15. Determination of particle nucleation and growth rates from measured aerosol size distributions

    NASA Astrophysics Data System (ADS)

    Verheggen, B.; Mozurkewich, M.

    2003-04-01

    The effects of aerosols on atmospheric chemistry, health and climate are dependent on particle size and composition, and therefore on particle nucleation and growth. An analytical model has been developed to determine nucleation and growth rates from measurements of consecutive aerosol size distributions. The evolution of an aerosol population in time is described by the General Dynamic Equation (GDE). Wall loss, coagulation loss and coagulation production are determined, based on the measured aerosol size distributions. Taking their contributions into account, a non-linear regression analysis of the GDE is performed for each time interval to find the value of the growth rate, that gives best agreement between the measured and calculated change in the size distribution. Other parameters can also be verified and/or optimized by regression analysis. Knowing the growth rate as a function of time (and size) from the regression analysis, each measured cohort of particles is tracked backwards in time to their time of formation, where the radius of the critical cluster is assumed to be 0.5 nm. The number density of each cohort has decreased since their formation, due to wall losses and coagulation processes. Perturbation theory is used to approximate the contribution of within mode coagulation in decreasing the number density. Wall losses and coagulation scavenging are well characterized for each time interval. The integrated losses, from time of formation to time of measurement, are used to obtain the number of nucleated particles, and ultimately the -empirically determined- nucleation rate. The analysis is applied to measurements made in Calspan's 590 m3 smog chamber, following SO2 nucleation.

  16. 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.

  17. All year round chemical composition of aerosol reaching the inner Antarctic Plateau (Dome C - East Antarctica)

    NASA Astrophysics Data System (ADS)

    Udisti, R.; Becagli, S.; Castellano, E.; Cerri, O.; Marino, F.; Morganti, A.; Nava, S.; Rugi, F.; Severi, M.; Traversi, R.

    2009-04-01

    Since 2005, continuous, all-year-round aerosol sampling was carried out at Dome C (Central East Antarctica, 3233 m a.s.l., about 1100 km far from the coast-line), in the framework of Station Concordia project. Size-segregated aerosol samples were collected in summer and winter period by using different low- and medium-volume systems, including pre-selected cut-off samplers (with PM10, PM2.5 and PM1 heads) and multi-stage (Andersen 8-stage and Dekati 4-stage) impactors. Sampling resolution and volume range from 1 day to 1 month and from 2.3 to 12 m3/h respectively. Aerosol study at Dome C aims to improve our knowledge on present day source intensity, transport efficiency and pathways (including stratosphere-to-troposphere interchanges) of particles reaching internal sites of Antarctica and to understand size- and chemical-fractionation effects occurring during the transport (by comparison with coastal aerosol composition). Besides, more information on atmosphere-snow interaction, including depositional and post depositional processes, as well as the effect of sublimation/condensation processes on snow surface, improves the reconstruction of past atmosphere composition from EPICA-DC deep ice core, drilled in the same site. Here we report some results of the chemical composition of the Antarctic background aerosol reaching Dome C, pointing out the seasonal pattern and the temporal trend of some ionic components used as tracers of sea spray, marine biogenic and crustal emissions. The atmospheric load in the summer is more than one order of magnitude lower than that measured in coastal sites and chemical composition is dominated by secondary aerosol, mainly originated by biological marine activity (S-cycle), and distributed in the finest aerosol fractions. H2SO4 from oxidation of biogenic DMS is the main component, while the contribution of HNO3 to the ionic budget is difficult to evaluate because of the re-emission into the atmosphere from the filter surface (acidic

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

    PubMed

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

    1989-06-20

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

  19. 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.

  20. Size-specific composition of aerosols in the El Chichon volcanic cloud

    NASA Technical Reports Server (NTRS)

    Woods, D. C.; Chuan, R. L.

    1983-01-01

    A NASA U-2 research aircraft flew sampling missions in April, May, July, November, and December 1982 aimed at obtaining in situ data in the stratospheric cloud produced from the March-April 1982 El Chichon eruptions. Post flight analyses provided information on the aerosol composition and morphology. The particles ranged in size from smaller than 0.05 m to larger than 20 m diameter and were quite complex in composition. In the April, May, and July samples the aerosol mass was dominated by magmatic and lithic particles larger than about 3 m. The submicron particles consisted largely of sulfuric acid. Halite particles, believed to be related to a salt dome beneath El Chichon, were collected in the stratosphere in April and May. On the July 23 flight, copper-zinc oxide particles were collected. In July, November, and December, in addition to the volcanic ash and acid particles, carbon-rich particles smaller than about 0.1 m aerodynamic diameter were abundant.

  1. Characterization of the physical, chemical, and optical properties of atmospheric aerosol particles in New Hampshire

    NASA Astrophysics Data System (ADS)

    Slater, John Frederick

    Tropospheric aerosol particles directly affect the radiative budget of the Earth, and degrade visibility, by scattering and absorbing short-wavelength solar radiation. However, the radiative effect of aerosols is highly uncertain due to the non-uniform spatial distribution of the particles over Earth, their heterogeneous chemical composition, and their variable size. This dissertation quantifies some of the physical, chemical, and optical (radiative) properties of aerosols at different locations within New Hampshire (NH) from spring 2000 to fall 2001. During spring 2000, a 1-month study conducted at a mountaintop location adjacent to the White Mountain National Forest in northern NH showed that synoptic-scale air mass transport heavily influenced aerosol properties, and hence regional visibility. During W/SW flow, aerosol parameters and haziness were generally twice as high as times of N/NE flow. Similar transport dependent results were observed in October 2000 during a regional pollution event. Pollutants built-up in concentration during 22--28 October, culminated on 28 October, and then dropped 10-fold to background levels within a 6-hour period. Synoptic weather conditions during the transition from high to low pollutant levels indicated that an intense frontal boundary traversed the region, serving as a divide between a warm, humid, and polluted air mass from the W/SW, and a cold, dry, and clean air mass advancing out of Canada. Further work connecting air mass transport and aerosol variability in southern NH revealed that maximum aerosol optical depth (AOD) occurred in summer and was primarily associated with W/SW flow. Minimum AOD occurred in winter and was generally associated with N/NE flow. Mass scattering and absorption efficiencies of PM2.5 did not vary significantly between times of transport from different source regions and were very close to theoretical values. Maximum positive values of aerosol direct radiative forcing occurred in winter and maximum

  2. Lake spray aerosol generation: a method for producing representative particles from freshwater wave breaking

    NASA Astrophysics Data System (ADS)

    May, Nathaniel W.; Axson, Jessica L.; Watson, Alexa; Pratt, Kerri A.; Ault, Andrew P.

    2016-09-01

    Wave-breaking action in bodies of freshwater produces atmospheric aerosols via a similar mechanism to sea spray aerosol (SSA) from seawater. The term lake spray aerosol (LSA) is proposed to describe particles formed by this mechanism, which have been observed over the Laurentian Great Lakes. Though LSA has been identified from size distribution measurements during a single measurement campaign, no measurements of LSA composition or relationship to bubble-bursting dynamics have been conducted. An LSA generator utilizing a plunging jet, similar to many SSA generators, was constructed for the generation of aerosol from freshwater samples and model salt solutions. To evaluate this new generator, bubble and aerosol number size distributions were measured for salt solutions representative of freshwater (CaCO3) and seawater (NaCl) at concentrations ranging from that of freshwater to seawater (0.05-35 g kg-1), synthetic seawater (inorganic), synthetic freshwater (inorganic), and a freshwater sample from Lake Michigan. Following validation of the bubble and aerosol size distributions using synthetic seawater, a range of salt concentrations were investigated. The systematic studies of the model salts, synthetic freshwater, and Lake Michigan sample indicate that LSA is characterized by a larger number size distribution mode diameter of 300 nm (lognormal), compared to seawater at 110 nm. Decreasing salt concentrations from seawater to freshwater led to greater bubble coalescence and formation of larger bubbles, which generated larger particles and lower aerosol number concentrations. This resulted in a bimodal number size distribution with a primary mode (180 ± 20 nm) larger than that of SSA, as well as a secondary mode (46 ± 6 nm) smaller than that of SSA. This new method for studying LSA under isolated conditions is needed as models, at present, utilize SSA parameterizations for freshwater systems, which do not accurately predict the different size distributions observed

  3. Aerosol composition, chemistry, and source characterization during the 2008 VOCALS Experiment

    SciTech Connect

    Lee, Y.; Springston, S.; Jayne, J.; Wang, J.; Senum, G.; Hubbe, J.; Alexander, L.; Brioude, J.; Spak, S.; Mena-Carrasco, M.; Kleinman, L.; Daum, P.

    2010-03-15

    Chemical composition of fine aerosol particles over the northern Chilean coastal waters was determined onboard the U.S. DOE G-1 aircraft during the VOCALS (VAMOS Ocean-Cloud-Atmosphere-Land Study) field campaign between October 16 and November 15, 2008. SO42-, NO3-, NH4+, and total organics (Org) were determined using an Aerodyne Aerosol Mass Spectrometer, and SO42-, NO3-, NH4+, Na+, Cl-, CH3SO3-, Mg2+, Ca2+, and K+ were determined using a particle-into-liquid sampler-ion chromatography technique. The results show the marine boundary layer (MBL) aerosol mass was dominated by non- sea-salt SO42- followed by Na+, Cl-, Org, NO3-, and NH4+, in decreasing importance; CH3SO3-, Ca2+, and K+ rarely exceeded their respective limits of detection. The SO42- aerosols were strongly acidic as the equivalent NH4+ to SO42- ratio was only {approx}0.25 on average. NaCl particles, presumably of sea-salt origin, showed chloride deficits but retained Cl- typically more than half the equivalency of Na+, and are externally mixed with the acidic sulfate aerosols. Nitrate was observed only on sea-salt particles, consistent with adsorption of HNO3 on sea-salt aerosols, responsible for the Cl- deficit. Dust particles appeared to play a minor role, judging from the small volume differences between that derived from the observed mass concentrations and that calculated based on particle size distributions. Because SO42- concentrations were substantial ({approx}0.5 - {approx}3 {micro}g/m3) with a strong gradient (highest near the shore), and the ocean-emitted dimethylsulfide and its unique oxidation product, CH3SO3-, were very low (i.e., {le} 40 parts per trillion and <0.05 {micro}g/m3, respectively), the observed SO42- aerosols are believed to be primarily of terrestrial origin. Back trajectory calculations indicate sulfur emissions from smelters and power plants along coastal regions of Peru and Chile are the main sources of these SO4- aerosols. However, compared to observations, model

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

    NASA Astrophysics Data System (ADS)

    Mochida, Michihiro; Kawamura, Kimitaka

    2004-11-01

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

  5. Composition and major sources of organic compounds in urban aerosols

    NASA Astrophysics Data System (ADS)

    Bi, Xinhui; Simoneit, Bernd R. T.; Sheng, Guoying; Ma, Shexia; Fu, Jiamo

    Total suspended particles (TSP), collected during June 2002 to July 2003 in Guangzhou, a typical economically developed city in South China, were analyzed for the organic compound compositions using gas chromatography-mass spectrometry (GC/MS). Over 140 organic compounds were detected in the aerosols and grouped into different classes including n-alkanes, hopanoids, polycyclic aromatic hydrocarbons, alkanols, fatty acids, dicarboxylic acids excluding oxalic acid, polyols/polyacids, lignin products, phytosterols, phthalates and water-soluble sugars. The total amounts of the identified organic compounds including unresolved complex mixture (UCM) ranged from 3112 ng/m 3 in spring to 5116 ng/m 3 in winter, comprising on seasonal average 2.8% of TSP. Primary organic compounds peaked in winter although there are no heating systems burning fuels in Guangzhou. The highest saccharide levels occurred in fall due to agricultural activities. This study demonstrated that utilization of fossil fuels, biomass burning, soil resuspension and plastic/refuse burning are the major contributors to the identified organic compounds in the urban atmosphere of South China.

  6. Characteristics and Composition of Atmospheric Aerosols in Phimai, Central Thailand During BASE-ASIA

    NASA Technical Reports Server (NTRS)

    Li, Can; Tsay, Si-Chee; Hsu, N. Christina; Kim, Jin Young; Howell, Steven G.; Huebert, Barry J.; Ji, Qiang; Jeong, Myeong-Jae; Wang, Sheng-Hsiang; Hansell, Richard A.; Bell, Shaun W.

    2012-01-01

    +/- 8 Mm(exp -1); PM(sub 10) concentration: 33 +/- 17 miro-g/ cubic m and dominated by submicron particles. Major aerosol compounds included carbonaceous (OC: 9.5 +/- 3.6miro-g/ cubic m; EC: 2.0 2.3 miro-g/ cubic m and secondary species (SO4(2-): 6.4 +/- 3.7 miro-g/ cubic m, NH4(+): 2.2 +/- 1.3 miro-g/ cubic m). While the site was seldom under the direct influence of large forest fires to its north, agricultural fires were ubiquitous during the experiment, as suggested by the substantial concentration of K+ (0.56 +/- 0.33 micro-g/ cubic m). Besides biomass burning, aerosols in Phimai during the experiment were also strongly influenced by industrial and vehicular emissions from the Bangkok metropolitan region and long-range transport from southern China. High humidity played an important role in determining the aerosol composition and properties in the region. Sulfate was primarily formed via aqueous phase reactions, and hygroscopic growth could enhance the aerosol light scattering by up to 60%, at the typical morning RH level of 85%. The aerosol single scattering albedo demonstrated distinct diurnal variation, ranging from 0.86 +/- 0.04 in the evening to 0.92 +/- 0.02 in the morning. This experiment marks the first time such comprehensive characterization of aerosols was made for rural central Thailand. Our results indicate that aerosol pollution has developed into a regional problem for northern Indochina, and may become more severe as the region's population and economy continue to grow.

  7. Automated Measurements of Ambient Aerosol Chemical Composition and its Dry and Wet Size Distributions at Pittsburgh Supersite

    NASA Astrophysics Data System (ADS)

    Khlystov, A. Y.; Stanier, C.; Chun, W.; Vayenas, D.; Mandiro, M.; Pandis, S. N.

    2001-12-01

    Ambient aerosol particles change size with changes in ambient relative humidity. The magnitude of the size change depends on the hygroscopic properties of the particles, which is determined by their chemical composition. Hygroscopic properties of particles influence many environmentally important aerosol qualities, such as light scattering and partitioning between the gas and particle phases of semivolitile compounds. Studying the hygroscopic growth of ambient particles is thus of paramount importance. The highroscopic growth of ambient particles and their chemical composition are measured continuously within the Pittsburgh Air Quality Study (EPA supersite program). The hygroscopic size changes are measured using an automated system built for this study. The system consists of two Scanning Mobility Particle Sizers (SMPS, TSI Inc.) and an Aerodynamic Particle Sizer (APS, TSI Inc.). The three instruments measure aerosol size distribution between 5 nanometers and 10 micrometers in diameter. The inlets of the instruments and the sheath air lines of the SMPS systems are equipped with computer controlled valves that direct air through Nafion dryers (PermaPure Inc.) or bypass them. The Nafion dryers are drying the air stream below 40% RH at which point ambient particles are expected to lose most or all water and thus be virtually dry. To avoid changes in relative humidity and evaporation of volatile particles due to temperature differences the system is kept at ambient temperature. The system measures alternatively dry (below 40% RH) and wet (actual ambient RH) aerosol size distributions every 6 minutes. The hygroscopic growth observed with the size-spectrometer system is compared with theoretic predictions based on the chemical composition of aerosol particles. A modified semi-continuous Steam-Jet Aerosol Collector provides the total available budget (particles and gas) of water-soluble species, which is used as an input to the thermodynamic model. The model calculates

  8. 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.

  9. Enabling in-situ observation of organic aerosol speciated composition: Advances in TAG instrumentation (Invited)

    NASA Astrophysics Data System (ADS)

    Goldstein, A. H.; Worton, D. R.; Zhao, Y.; Kreisberg, N. M.; Teng, A. P.; Hering, S. V.; Gorecki, T.; Ranjan, M.; Hennigan, C. J.; Lambe, A.; Nguyen, N.; Donahue, N. M.; Robinson, A. L.; Jayne, J. T.; Williams, B. J.; Worsnop, D. R.

    2009-12-01

    The complex chemical composition of atmospheric aerosols, particularly the organic carbon portion, presents unique measurement challenges. We developed the Thermal Desorption Aerosol Gas chromatograph (TAG) system for hourly in-situ speciation of a wide range of primary and secondary organic compounds in aerosols. This instrument combines an impactor particle collector with thermal desorption followed by gas chromatography and mass spectrometric detection to provide separation, identification, and quantification of organic constituents at the molecular level. Observed compounds include alkanes, aldehydes, ketones, PAHs, monocarboxylic acids, and many more. The hourly time resolution measurements provided by TAG capture dynamic and frequent changes in aerosol composition that would not be resolved using traditional filter collection. TAG measurements also provide a much larger data set, facilitating the use of statistical approaches such as positive matrix factorization to identify source categories and their contributions to the total observed aerosol. Because TAG identifies organic compounds at the molecular level, it can build on the extensive work obtained by traditional GC/MS analysis of filter samples on source emission profiles and secondary organic aerosol formation. We report here continued developments in the capabilities of our TAG system. Most recently, we have incorporated a two-dimensional chromatography (GC×GC) capability into TAG, and now have that instrument operating with a time of flight (TOF) MS detector. Two-dimensional chromatography provides two types of compound separation, most typically by volatility and polarity. It uses two columns with different stationary phases connected in series separated by a modulator. The modulator periodically traps analytes eluting from the first column, and injects fractions of this effluent onto the second column in the form of narrow pulses providing additional separation for co-eluting peaks. The approach

  10. Modeling global impacts of heterogeneous loss of HO2 on cloud droplets, ice particles and aerosols

    NASA Astrophysics Data System (ADS)

    Huijnen, V.; Williams, J. E.; Flemming, J.

    2014-03-01

    The abundance and spatial variability of the hydroperoxyl radical (HO2) in the troposphere strongly affects atmospheric composition through tropospheric ozone production and associated HOx chemistry. One of the largest uncertainties in the chemical HO2 budget is its heterogeneous loss on the surface of cloud droplets, ice particles and aerosols. We quantify the importance of the heterogeneous HO2 loss at global scale using the latest recommendations on the scavenging efficiency on various surfaces. For this we included the simultaneous loss on cloud droplets and ice particles as well as aerosol in the Composition-Integrated Forecast System (C-IFS). We show that cloud surface area density (SAD) is typically an order of magnitude larger than aerosol SAD, using assimilated satellite retrievals to constrain both meteorology and global aerosol distributions. Depending on the assumed uptake coefficients, loss on liquid water droplets and ice particles accounts for ∼53-70% of the total heterogeneous loss of HO2, due to the ubiquitous presence of cloud droplets. This indicates that HO2 uptake on cloud should be included in chemistry transport models that already include uptake on aerosol. Our simulations suggest that the zonal mean mixing ratios of HO2 are reduced by ∼25% in the tropics and up to ∼50% elsewhere. The subsequent decrease in oxidative capacity leads to a global increase of the tropospheric carbon monoxide (CO) burden of up to 7%, and an increase in the ozone tropospheric lifetime of ∼6%. This increase results in an improvement in the global distribution when compared against CO surface observations over the Northern Hemisphere, although it does not fully resolve the wintertime bias in the C-IFS. There is a simultaneous increase in the high bias in C-IFS for tropospheric CO over the Southern Hemisphere, which constrains on the assumptions regarding HO2 uptake on a global scale. We show that enhanced HO2 uptake on aerosol types associated with

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

    PubMed

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

    2012-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  14. A seasonal time history of the size resolved composition of fine aerosol in Manchester UK

    NASA Astrophysics Data System (ADS)

    Choularton, Thomas; Martin, Claire; Allan, James; Coe, Hugh; Bower, Keith; Gallagher, Martin

    2010-05-01

    Numerous studies have been conducted in urban centres now using sophisticated instruments that measure aerosol properties needed to determine their effects on human health, air quality and climate change) showing that a significant fraction of urban aerosols (mainly from automotive sources) are composed of organic compounds with implications for human health. In this project we have produced the first seasonal aerosol composition and emission database for the City of Manchester in the UK Several recent projects have been conducted by SEAES looking at fundamental properties of urban atmospheric aerosol to understand their influence on climate. This work is now expanding through collaboration with the School of Geography & Centre for Occupational & Environmental Health to investigate urban aerosol emission impacts on human health In this paper we present a compendium of data from field campaigns in Manchester city centre over the past decade. The data are from six different campaigns, between 2001 - 2007, each campaign was between 2 weeks and 2 months long predominantly from January and June periods . The data analysis includes air parcel trajectory examination and comparisons with external data, including PM10, CO and NOx data from AURN fixed monitoring sites Six Manchester fine aerosol datasets from the past decade have been quality controlled and analysed regarding averages of the size distributions of Organic, NO3, NH4 and SO4 mass loadings. It was found that: Organic material is the largest single component of the aerosol with primary aliphatic material dominating the smallest sizes, but with oxygenated secondary organic material being important in the accumulation mode. In the accumulation mode the organic material seems to be internally mixed with sulphate and nitrate. The accumulation mode particles were effective as cloud condensation nuclei. Seasonal effects surrounding atmospheric stability and photochemistry were found to play an important role in the

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  17. 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.

  18. 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.

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

    NASA Astrophysics Data System (ADS)

    Slade, Jonathan H.; Knopf, Daniel A.

    2014-07-01

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

  20. Water nucleation properties of chaparral fire aerosol particles

    SciTech Connect

    Hudson, J.G.; Rogers, C.F.; Hallett, J.

    1989-05-01

    In December, 1986, planned and prescribed forest management burns took place at Lodi Canyon, on the north side of the Los Angeles Basin, California. These fires involved a mixture of species of small trees and shrubs, including scrub oak, chamise, and mountain mahogany, known collectively as ''chaparral'' in the Western US. Over a period of about two weeks, about 200 hectares of chaparral were consumed. This prescribed burn presented an opportunity for three days of airborne measurements of aerosol properties including total particle or condensation nuclei (CN) concentrations and cloud condensation nuclei (CCN) concentrations. This study is in coordination with other efforts conducted simultaneously; here the emphasis will be on the airborne CN and CCN measurements and on related studies conducted on a laboratory scale. In this study, we distinguish between CCN and the total aerosol particle population as gauged by the CN count. CCN and CN concentrations and CCN/CN ratios will be presented for the airborne measurements and for laboratory measurements employing a similar fuel. Ancillary ion chromatography (IC) and scanning electron microscopy (SEM) information will also be presented for the laboratory-scale chaparral burn. 11 refs., 4 figs., 4 tabs.

  1. 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.

  2. Aerosol composition and properties variation at the ground and over the column under different air masses advection in South Italy.

    PubMed

    Pavese, G; Lettino, A; Calvello, M; Esposito, F; Fiore, S

    2016-04-01

    Aerosol composition and properties variation under the advection of different air masses were investigated, as case studies, by contemporary measurements over the atmospheric column and at the ground in a semi-rural site in South Italy. The absence of local strong sources in this area allowed to characterize background aerosol and to compare particle mixing effects under various atmospheric circulation conditions. Aerosol optical depth (AOD) and Ǻngström parameters from radiometric measurements allowed the detection and identification of polluted, dust, and volcanic atmospheric conditions. AODs were the input for a suitable model to evaluate the columnar aerosol composition, according to six main atmospheric components (water-soluble, soot, sea salt accumulation, sea salt coarse, mineral dus,t and biological). Scanning electron microscope (SEM) analysis of particulate sampled with a 13-stage impactor at the ground showed not only fingerprints typical of the different air masses but also the effects of transport and aging on atmospheric particles, suggesting processes that changed their chemical and optical properties. Background columnar aerosol was characterized by 72% of water-soluble and soot, in agreement with ground-based findings that highlighted 60% of contribution from anthropogenic carbonate particles and soot. In general, a good agreement between ground-based and columnar results was observed. Under the advection of trans-boundary air masses, water-soluble and soot were always present in columnar aerosol, whereas, in variable percentages, sea salt and mineral particles characterized both dust and volcanic conditions. At the ground, sulfates characterized the amorphous matrix produced in finer stages by the evaporation of solutions of organic and inorganic aerosols. Sulfates were also one of the key players involved in heterogeneous chemical reactions, producing complex secondary aerosol, as such clay-sulfate internally mixed particle externally mixed

  3. Composition of energetic particles from solar flares.

    PubMed

    Garrard, T L; Stone, E C

    1994-10-01

    We present a model for composition of heavy ions in the solar energetic particles (SEP). The SEP composition in a typical large solar particle event reflects the composition of the Sun, with adjustments due to fractionation effects which depend on the first ionization potential (FIP) of the ion and on the ratio of ionic charge to mass (Q/M). Flare-to-flare variations in composition are represented by parameters describing these fractionation effects and the distributions of these parameters are presented.

  4. Quantitative ED-EPMA combined with morphological information for the characterization of individual aerosol particles collected in Incheon, Korea

    NASA Astrophysics Data System (ADS)

    Kang, SuJin; Hwang, HeeJin; Kang, Sunni; Park, YooMyung; Kim, HyeKyeong; Ro, Chul-Un

    A quantitative single-particle analytical technique, called low- Z particle electron probe X-ray microanalysis, combined with the utilization of their morphological information on individual particles, was applied to characterize six aerosol samples collected in one Korean city, Incheon, during March 9-15, 2006. The collected supermicron aerosol particles were classified based on their chemical species and morphology on a single-particle basis. Many different particle types were identified and their emission source, transport, and reactivity in the air were elucidated. In the samples, particles in the "soil-derived particles" group were the most abundant, followed by "reacted sea-salts", "reacted CaCO 3-containing particles", "genuine sea-salts", "reacted sea-salts + others", "Fe-containing particles", "anthropogenic organics", (NH 4) 2SO 4, "K-containing particles", and "fly ash". The application of this single-particle analysis, fully utilizing their chemical compositional and morphological data of individual particles, clearly revealed the different characteristics of the six aerosol samples. For samples S3 and S5, which were sampled during two Asian dust storm events, almost all particles were of soil origin that had not experienced chemical modification and that did not entrain sea-salts during their long-range transport. For sample S1, collected at an episodic period of high PM 10 concentration and haze, anthropogenic, secondary, and soil-derived particles emitted from local sources were predominant. For samples S2, S4, and S6, which were collected on average spring days with respect to their PM 10 concentrations, marine originated particles were the most abundant. Sample S2 seems to have been strongly influenced by emissions from the Yellow Sea and Korean peninsula, sample S4 had the minimum anthropogenic influence among the four samples collected in the absence of any Asian dust storm event, and sample S6 seems to have entrained air pollutants that had been

  5. 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

  6. 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

  7. Vertical distribution of non-volatile species of upper tropospheric and lower stratospheric aerosol observed by balloon-borne optical particle counter above Ny-Aalesund, Norway in the winter of 2015

    NASA Astrophysics Data System (ADS)

    Shiraishi, K.; Hayashi, M.; Shibata, T.; Neuber, R.; Ruhe, W.

    2015-12-01

    The polar lower stratosphere is the sink area of stratospheric global circulation. The composition, concentration and size distribution of aerosol in the polar stratosphere are considered to be strongly influenced by the transportations from mid-latitude to polar region and exchange of stratosphere to troposphere. In order to study the aerosol composition and size distribution in the Arctic stratosphere and the relationship between their aerosol microphysical properties and transport process, we carried out balloon-borne measurement of aerosol volatility above Ny-Aalesund, Norway in the winter of 2015. In our observation, two optical particle counters and a thermo denuder were suspended by one rubber balloon. A particle counter measured the heated aerosol size distribution (after heating at the temperature of 300 degree by the thermo denuder) and the other measured the ambient aerosol size distribution during the observation. The observation was carried out on 15 January, 2015. Balloon arrived at the height of 30km and detailed information of aerosol size distributions in upper troposphere and lower stratosphere for both heated aerosol and ambient aerosol were obtained. As a Result, the number ratio of non-volatile particles to ambient aerosol particles in lower stratosphere (11-15km) showed different feature in particle size range of fine mode (0.3particles to ambient aerosol particles were 1-3% in fine mode range and 7-20% in coarse mode range. They suggested that fine particles are composed dominantly of volatile species (probably sulfuric acid), and coarse particles are composed of non-volatile species such as minerals, sea-salts. In our presentation, we show the obtained aerosol size distribution and discuss the aerosol compositions and their transport process.

  8. Single-particle speciation of alkylamines in ambient aerosol at five European sites.

    PubMed

    Healy, Robert M; Evans, Greg J; Murphy, Michael; Sierau, Berko; Arndt, Jovanna; McGillicuddy, Eoin; O'Connor, Ian P; Sodeau, John R; Wenger, John C

    2015-08-01

    Alkylamines are associated with both natural and anthropogenic sources and have been detected in ambient aerosol in a variety of environments. However, little is known about the ubiquity or relative abundance of these species in Europe. In this work, ambient single-particle mass spectra collected at five sampling sites across Europe have been analysed for their alkylamine content. The aerosol time-of-flight mass spectrometer (ATOFMS) data used were collected in Ireland (Cork), France (Paris, Dunkirk and Corsica) and Switzerland (Zurich) between 2008 and 2013. Each dataset was queried for mass spectral marker ions associated with the following ambient alkylamines: dimethylamine (DMA), trimethylamine (TMA), diethylamine (DEA), triethylamine (TEA), dipropylamine (DPA) and tripropylamine (TPA). The fraction of ambient particles that contained detectable alkylamines ranged from 1 to 17 % depending on location, with the highest fractions observed in Paris and Zurich in the winter months. The lowest fractions were observed at coastal sites, where the influence of animal husbandry-related alkylamine emissions is also expected to be lowest. TMA was the most ubiquitous particle phase alkylamine detected and was observed at all locations. Alkylamines were found to be internally mixed with both sulphate and nitrate for each dataset, suggesting that aminium salt formation may be important at all sites investigated. Interestingly, in Corsica, all alkylamine particles detected were also found to be internally mixed with methanesulphonic acid (MSA), indicating that aminium methanesulphonate salts may represent a component of marine ambient aerosol in the summer months. Internal mixing of alkylamines with sea salt was not observed, however. Alkylamine-containing particle composition was found to be reasonably homogeneous at each location, with the exception of the Corsica and Dunkirk sites, where two and four distinct mixing states were observed, respectively.

  9. Aging of Secondary Organic Aerosol from β-Pinene: Changes in Chemical Composition, Density and Morphology

    NASA Astrophysics Data System (ADS)

    Sarrafzadeh, M.; Hastie, D. R.

    2013-12-01

    Biogenic volatile organic compounds (VOC) are emitted in large quantities into the atmosphere. These VOC, which includes β-pinene, can react to produce secondary organic aerosols (SOA), which contribute to a substantial fraction of ambient organic aerosols and are known to adversely affect visibility, climate and health. Despite this, the current knowledge regarding the SOA composition, their physical properties and the chemical aging processes they undergo in the atmosphere is limited. In this study, chemical aging of SOA generated from the photooxidation of β-pinene was investigated in the York University smog chamber. The formation and aging of both gas and particle phase products were analyzed using an atmospheric pressure chemical ionization triple quadrupole mass spectrometer. The density of secondary organic matter was also simultaneously measured over the course of the aging experiments, allowing us to improve our understanding in changes in particle composition that may occur. In addition, particle phase and shape was investigated for generated particles from β-pinene oxidation by scanning electron microscope (SEM). Results of this work, including particle density and morphology will be presented as well as comparisons of gas and particle phase products time profiles during aging.

  10. Systematic Relationships Between Lidar Observables And Sizes And Mineral Composition Of Dust Aerosols

    NASA Astrophysics Data System (ADS)

    van Diedenhoven, B.; Perlwitz, J. P.; Fridlind, A. M.; Chowdhary, J.; Cairns, B.; Stangl, A. J.

    2015-12-01

    The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

  11. Systematic Relationships Between Lidar Observables and Sizes And Mineral Composition Of Dust Aerosols

    NASA Technical Reports Server (NTRS)

    Van Diedenhoven, Bastiaan; Stangl, Alexander; Perlwitz, Jan; Fridlind, Ann M.; Chowdhary, Jacek; Cairns, Brian

    2015-01-01

    The physical and chemical properties of soil dust aerosol particles fundamentally affect their interaction with climate, including shortwave absorption and radiative forcing, nucleation of cloud droplets and ice crystals, heterogeneous formation of sulfates and nitrates on the surface of dust particles, and atmospheric processing of iron into bioavailable forms that increase the productivity of marine phytoplankton. Lidar measurements, such as extinction-to-backscatter, color and depolarization ratios, are frequently used to distinguish between aerosol types with different physical and chemical properties. The chemical composition of aerosol particles determines their complex refractive index, hence affecting their backscattering properties. Here we present a study on how dust aerosol backscattering and depolarization properties at wavelengths of 355, 532 and 1064 nm are related to size and complex refractive index, which varies with the mineral composition of the dust. Dust aerosols are represented by collections of spheroids with a range of prolate and oblate aspect ratios and their optical properties are obtained using T-matrix calculations. We find simple, systematic relationships between lidar observables and the dust size and complex refractive index that may aid the use of space-based or airborne lidars for direct retrieval of dust properties or for the evaluation of chemical transport models using forward simulated lidar variables. In addition, we present first results on the spatial variation of forward-simulated lidar variables based on a dust model that accounts for the atmospheric cycle of eight different mineral types plus internal mixtures of seven mineral types with iron oxides, which was recently implemented in the NASA GISS Earth System ModelE2.

  12. Phosphorus-bearing Aerosol Particles From Volcanic Plumes

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

  13. A strategy for characterizing the mixing state of immiscible aerosol components and the formation of multiphase aerosol particles through coagulation.

    PubMed

    Mitchem, Laura; Buajarern, Jariya; Ward, Andrew D; Reid, Jonathan P

    2006-07-20

    We demonstrate that the coagulation of two aerosol droplets of different chemical composition can be studied directly through the unique combination of optical tweezers and Raman spectroscopy. Multiple optical traps can be established, allowing the manipulation of multiple aerosol droplets. Spontaneous Raman scattering allows the characterization of droplet composition and mixing state, permitting the phase segregation of immiscible components in multiphase aerosol to be investigated with spatial resolution. Stimulated Raman scattering allows the integrity of the droplet and uniformity of refractive index to be probed. The combination of these spectroscopic probes with optical tweezers is shown to yield unprecedented detail in studies of the coagulation of decane and water droplets.

  14. Evaluation of the particle measurement programme (PMP) protocol to remove the vehicles' exhaust aerosol volatile phase.

    PubMed

    Giechaskiel, B; Chirico, R; Decarlo, P F; Clairotte, M; Adam, T; Martini, G; Heringa, M F; Richter, R; Prevot, A S H; Baltensperger, U; Astorga, C

    2010-10-01

    European regulation for Euro 5/6 light duty emissions introduced the measurement of non-volatile particles with diameter >23 nm. The volatile phase is removed by using a heated dilution stage (150 degrees C) and a heated tube (at 300-400 degrees C). We investigated experimentally the removal efficiency for volatile species of the specific protocol by conducting measurements with two Euro 3 diesel light duty vehicles, a Euro 2 moped, and a Euro III heavy duty vehicle with the system's heaters on and off. The particle number distributions were measured with a Scanning Mobility Particle Sizer (SMPS) and a Fast Mobility Particle Sizer (FMPS). An Aerosol Mass Spectrometer (AMS) was used to identify the non-refractory chemical composition of the particles. A Multi-Angle Absorption Photometer (MAAP) was used to measure the black carbon concentration. The results showed that the condensed material in the accumulation mode (defined here as particles in the diameter range of approximately 50-500 nm) was removed with an efficiency of 50-90%. The (volatile) nucleation mode was also completely evaporated or was decreased to sizes <23 nm; thus these particles wouldn't be counted from the particle counter, indicating the robustness of the protocol.

  15. Evaluation of the particle measurement programme (PMP) protocol to remove the vehicles' exhaust aerosol volatile phase.

    PubMed

    Giechaskiel, B; Chirico, R; Decarlo, P F; Clairotte, M; Adam, T; Martini, G; Heringa, M F; Richter, R; Prevot, A S H; Baltensperger, U; Astorga, C

    2010-10-01

    European regulation for Euro 5/6 light duty emissions introduced the measurement of non-volatile particles with diameter >23 nm. The volatile phase is removed by using a heated dilution stage (150 degrees C) and a heated tube (at 300-400 degrees C). We investigated experimentally the removal efficiency for volatile species of the specific protocol by conducting measurements with two Euro 3 diesel light duty vehicles, a Euro 2 moped, and a Euro III heavy duty vehicle with the system's heaters on and off. The particle number distributions were measured with a Scanning Mobility Particle Sizer (SMPS) and a Fast Mobility Particle Sizer (FMPS). An Aerosol Mass Spectrometer (AMS) was used to identify the non-refractory chemical composition of the particles. A Multi-Angle Absorption Photometer (MAAP) was used to measure the black carbon concentration. The results showed that the condensed material in the accumulation mode (defined here as particles in the diameter range of approximately 50-500 nm) was removed with an efficiency of 50-90%. The (volatile) nucleation mode was also completely evaporated or was decreased to sizes <23 nm; thus these particles wouldn't be counted from the particle counter, indicating the robustness of the protocol. PMID:20692024

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

    SciTech Connect

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

    2015-09-25

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

  17. Aerosol particle properties in a South American megacity

    NASA Astrophysics Data System (ADS)

    Ulke, Ana; Torres-Brizuela, Marcela; Raga, Graciela; Baumgardner, Darrel; Cancelada, Marcela

    2015-04-01

    The subtropical city of Buenos Aires is located on the western shore of Río de la Plata, on the southeastern coast of Argentina. It is the second largest metropolitan area in South America, with a population density of around 14 thousand people per km2. When all 24 counties of the Great Buenos Aires Metropolitan Area are included it is the third-largest conurbation in Latin America, with a population of around fifteen million inhabitants. The generalized worldwide trend to concentrate human activities in urban regions that continue to expand in area, threatens the local and regional environment. Air pollution in the Buenos Aires airshed is due to local sources (mainly the mobile sources, followed by the electric power plants and some industries) and to distant sources (like biomass burning, dust, marine aerosols and occasionally volcanic ash) whose products arrive in the city area due to the regional transport patterns. Previous research suggests that ambient aerosol particle concentrations should be considered an air quality problem. A field campaign was conducted in Buenos Aires in 2011 in order to characterize some aerosol particles properties measured for the first time in the city. Measurements began in mid- April and continued until December. The field observations were done in a collaborative effort between the Universities of Mexico (UNAM) and Buenos Aires (UBA). A suite of instruments was installed on the roof of an UBA laboratory and classroom buildings (34.54° S, 58.44° W) at an altitude of approximately 30 m above sea level. The measurements included the number concentration of condensation nuclei (CN) larger than approximately 50 nm, the mass concentration of particle-bound polycyclic aromatic hydrocarbons (PPAH), the scattering (Bscat) and absorption (Babs) coefficients at 550 nm and the vertical profiles of backscattered light from aerosols at a wavelength of 910 nm using a ceilometer. In addition, a weather station recorded the meteorological

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

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

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

    SciTech Connect

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

    2009-01-01

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

  1. On the role of particle inorganic mixing state in the reactive uptake of N2O5 to ambient aerosol particles.

    PubMed

    Ryder, Olivia S; Ault, Andrew P; Cahill, John F; Guasco, Timothy L; Riedel, Theran P; Cuadra-Rodriguez, Luis A; Gaston, Cassandra J; Fitzgerald, Elizabeth; Lee, Christopher; Prather, Kimberly A; Bertram, Timothy H

    2014-01-01

    The rates of heterogeneous reactions of trace gases with aerosol particles are complex functions of particle chemical composition, morphology, and phase state. Currently, the majority of model parametrizations of heterogeneous reaction kinetics focus on the population average of aerosol particle mass, assuming that individual particles have the same chemical composition as the average state. Here we assess the impact of particle mixing state on heterogeneous reaction kinetics using the N2O5 reactive uptake coefficient, γ(N2O5), and dependence on the particulate chloride-to-nitrate ratio (nCl(-)/nNO3(-)). We describe the first simultaneous ambient observations of single particle chemical composition and in situ determinations of γ(N2O5). When accounting for particulate nCl(-)/nNO3(-) mixing state, model parametrizations of γ(N2O5) continue to overpredict γ(N2O5) by more than a factor of 2 in polluted coastal regions, suggesting that chemical composition and physical phase state of particulate organics likely control γ(N2O5) in these air masses. In contrast, direct measurement of γ(N2O5) in air masses of marine origin are well captured by model parametrizations and reveal limited suppression of γ(N2O5), indicating that the organic mass fraction of fresh sea spray aerosol at this location does not suppress γ(N2O5). We provide an observation-based framework for assessing the impact of particle mixing state on gas-particle interactions.

  2. 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

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

    PubMed

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

    2014-04-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

  5. Suppression of Fermi acceleration in composite particles

    NASA Astrophysics Data System (ADS)

    Siqueira, Kellen Manoela; de Aguiar, Marcus Aloizio Martinez

    2016-09-01

    We study the motion of a composite particle in a one-dimensional billiard with a moving wall. The particle is modeled by two point masses coupled by a harmonic spring. We show that the energy gained by the composite particle is greatly reduced with respect to a single point particle. We show that the amount of energy transferred to the system at each collision with the walls is independent of the spring constant. However, the presence of the spring is responsible for the energy suppression because it diminishes the number of collisions by storing part of the system's energy and reducing the velocity of the particle's center of mass.

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  7. Molecular composition of atmospheric aerosols from Halley Bay, Antarctica, using ultra-high resolution mass spectrometry

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Brough, Neil; Rincon, Angela; Jones, Anna; Kalberer, Markus

    2016-04-01

    Antarctica is one of the few pristine places to study natural processes of atmospheric aerosols and anthropogenic impacts on the clean remote atmosphere. Although stratospheric aerosol in Antarctica has now been explored in some detail because of the ozone depletion phenomenon, tropospheric aerosol particles in Antarctica remain very little studied. The main goal of this work is to identify in detail the organic chemical composition of aerosol from Halley Bay station, which is located on the Brunt Ice Shelf floating on the Weddell Sea in Antarctica. In this study we characterise the molecular composition of aerosols from three seasons (summer, autumn and winter in 2012) using ultra-high resolution mass spectrometry (UHRMS). The technique provides high accuracy and high mass resolving power that allows determining unambiguous number of organic compounds present in complex organic mixtures (Noziere et al., 2015). The molecular composition interpretation was facilitated using visualisation methods (e.g. double bond equivalent, Van Krevelen diagrams, Kendrick mass analysis, and carbon oxidation state), which allowed to identify patterns, such as differences between sampling times and atmospheric processes. The majority of the identified compounds were attributed to nitrogen and sulphur containing species which exhibited very strong seasonal trends. Relatively large fraction (up to 30% of the total number of molecules) of these species contained very low hydrogen to carbon ratios (below 1) indicating that the site is impacted by anthropogenic emissions. Influences of the meteorological parameters and air mass trajectories on the molecular composition are discussed. Nozière et al., The Molecular Identification of Organic Compounds in the Atmosphere: State of the Art and Challenges, Chem. Rev., 115, 3920-3983, 2015.

  8. Investigation of the detailed chemical composition of organic aerosol in a South East Asian Rainforest

    NASA Astrophysics Data System (ADS)

    Hamilton, Jacqueline; Ward, Martyn; Rami Alfarra, M.; Lewis, Alastair; McFiggans, Gordon; Robinson, Niall

    2010-05-01

    The formation of secondary organic aerosol (SOA) in tropical regions is a key uncertainty in quantifying the effect of man made emissions on the climate. Large quantities of volatile organic compounds are emitted from natural biogenic sources in the tropics, including isoprene, monoterpenes and sequiterpenes. There are very few studies of the detailed chemical composition of organic aerosols in tropical rainforest regions, but these would provide information on the importance of primary versus secondary organic aerosols, the key VOC precursors, oxidation state and volatility. Particle samples were collected in a tropical rainforest at Danum Valley in Borneo as part of the OP3 field campaign in 2008. Twenty four hour filter samples were collected at the Global Atmospheric Watch station at a height of around 10 m and shipped back to the laboratory (below -4 °C) for offline analysis. The OA composition was studied using multiple high resolution chromatographic techniques including comprehensive two dimensional gas chromatography coupled to time of flight mass spectrometry (GCXGC-TOFMS) and liquid chromatography coupled to ion trap mass spectrometry (LC-MSn). The composition was directly compared to chamber generated SOA (as part of the Aerosol Coupling in the Earths System , ACES, experiment) to determine SOA tracers. A biogenic SOA tracer MS fragmentation library was constructed and a number of SOA components from limonene, linalool and -pinene were identified in the rainforest OA. Very high resolution mass spectrometry (Fourier Transform Ion Cyclotron Resonance FTICR-MS) allowed the O:C and H:C ratios to be determined and these will be compared to those obtained by aerosol mass spectrometry (AMS). In addition, the OA composition from the rainforest will be compared to other locations.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2008-03-01

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

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

    PubMed

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

    2016-01-01

    The present article presents an experimental protocol to investigate particle aerosolization of a product under abrasion and under environmental weathering, which is a fundamental element to the approach of nanosafety-by-design of nanostructured products for their durable development. This approach is basically a preemptive one in which the focus is put on minimizing the emission of engineered nanomaterials' aerosols during the usage phase of the product's life cycle. This can be attained by altering its material properties during its design phase without compromising with any of its added benefits. In this article, an experimental protocol is presented to investigate the nanosafety-by-design of three commercial nanostructured products with respect to their mechanical solicitation and environmental weathering. The means chosen for applying the mechanical solicitation is an abrasion process and for the environmental weathering, it is an accelerated UV exposure in the presence of humidity and heat. The eventual emission of engineered nanomaterials is studied in terms of their number concentration, size distribution, morphology and chemical composition. The purpose of the protocol is to study the emission for test samples and experimental conditions which are corresponding to real life situations. It was found that the application of the mechanical stresses alone emits the engineered nanomaterials' aerosols in which the engineered nanomaterial is always embedded inside the product matrix, thus, a representative product element. In such a case, the emitted aerosols comprise of both nanoparticles as well as microparticles. But if the mechanical stresses are coupled with the environmental weathering, the experimental protocol reveals then the eventual deterioration of the product, after a certain weathering duration, may lead to the emission of the free engineered nanomaterial aerosols too. PMID:27684430

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

    PubMed

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

    2016-09-16

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

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

  14. Extending the Capabilities of Single Particle Mass Spectrometry: II. Measurements of Aerosol Particle Density without D