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Sample records for aerosol mass concentration

  1. 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

  2. Direct gravimetric determination of aerosol mass concentration in central antarctica.

    PubMed

    Annibaldi, Anna; Truzzi, Cristina; Illuminati, Silvia; Scarponi, Giuseppe

    2011-01-01

    In Antarctica, experimental difficulties due to extreme conditions have meant that aerosol mass has rarely been measured directly by gravimetry, and only in coastal areas where concentrations were in the range of 1-7 μg m(-3). The present work reports on a careful differential weighing methodology carried out for the first time on the plateau of central Antarctica (Dome C, East Antarctica). To solve problems of accurate aerosol mass measurements, a climatic room was used for conditioning and weighing filters. Measurements were carried out in long stages of several hours of readings with automatic recording of temperature/humidity and mass. This experimental scheme allowed us to sample from all the measurements (up to 2000) carried out before and after exposure, those which were recorded under the most stable humidity conditions and, even more importantly, as close to each other as possible. The automatic reading of the mass allowed us in any case to obtain hundreds of measurements from which to calculate average values with uncertainties sufficiently low to meet the requirements of the differential weighing procedure (±0.2 mg in filter weighing, between ±7% and ±16% both in aerosol mass and concentration measurements). The results show that the average summer aerosol mass concentration (aerodynamic size ≤10 μm) in central Antarctica is about 0.1 μg m(-3), i.e., about 1/10 of that of coastal Antarctic areas. The concentration increases by about 4-5 times at a site very close to the station. PMID:21141836

  3. Characterization of aerosol composition, concentrations, and sources at Baengnyeong Island, Korea using an aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Lee, Taehyoung; Choi, Jinsoo; Lee, Gangwoong; Ahn, Junyoung; Park, Jin Soo; Atwood, Samuel A.; Schurman, Misha; Choi, Yongjoo; Chung, Yoomi; Collett, Jeffrey L.

    2015-11-01

    To improve understanding of the sources and chemical properties of particulate pollutants on the western side of the Korean Peninsula, an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) measured non-refractory fine (PM1) particles from May to November, 2011 at Baengnyeong Island, South Korea. Organic matter and sulfate were generally the most abundant species and exhibited maximum concentrations of 36 μg/m3 and 39 μg/m3, respectively. Nitrate concentrations peaked at 32 μg/m3 but were typically much lower than sulfate and organic matter concentrations. May, September, October, and November featured the highest monthly average concentrations, with lower concentrations typically observed from June through August. Potential source contribution function (PSCF) analysis and individual case studies revealed that transport from eastern China, an area with high SO2 emissions, was associated with high particulate sulfate concentrations at the measurement site. Observed sulfate aerosol sometimes was fully neutralized by ammonium but often was acidic; the average ammonium to sulfate molar ratio was 1.49. Measured species size distributions revealed a range of sulfate particle size distributions with modes between 100 and 600 nm. Organic aerosol source regions were widespread, including contributions from eastern China and South Korea. Positive matrix factorization (PMF) analysis indicated three "factors," or types of organic aerosol, comprising one primary, hydrocarbon-like organic aerosol (HOA) and two oxidized organic aerosol (OOA) components, including a more oxidized (MO-OOA) and a less oxidized (LO-OOA) oxidized organic aerosol. On average, HOA and OOA contributed 21% and 79% of the organic mass (OM), respectively, with the MO-OOA fraction nearly three times as abundant as the LO-OOA fraction. Biomass burning contributions to observed OM were low during the late spring/early summer agricultural burning season in eastern China, since

  4. Aerosol chemical elemental mass concentration at lower free troposphere

    NASA Astrophysics Data System (ADS)

    do Carmo Freitas, Maria; Dionísio, Isabel; Fialho, Paulo; Barata, Filipe

    2007-08-01

    This paper shows the use of Instrumental neutron activation analysis (INAA) technique to determine elemental masses collected by a seven-wavelength Aethalometer instrument at the summit of Pico mountain in the Azorean archipelago, situated in the Central North Atlantic Ocean. Each sample corresponds to air particulate matter measured continuously for periods of approximately 24 h taken from 14th July 2001 through 14th July 2002. The statistical analysis of the coefficients of correlation between all the elements identified, permitted to establish six groups that could potentially be associated with the type of source responsible for the aerosol sampled in the lower free troposphere at the Azorean archipelago. Calculation of the synoptic back trajectories helped to corroborate the use of the iron/cesium relation as a tracer for the Saharan dust aerosol. It was demonstrated that INAA constituted an important tool to identify these events.

  5. A CLOSURE STUDY OF AEROSOL MASS CONCENTRATION MEASUREMENTS: COMPARISON OF VALUES OBTAINED WITH FILTERS AND BY DIRECT MEASUREMENTS OF MASS DISTRIBUTIONS. (R826372)

    EPA Science Inventory

    We compare measurements of aerosol mass concentrations obtained gravimetrically using Teflon coated glass fiber filters and by integrating mass distributions measured with the differential mobility analyzer–aerosol particle mass analyzer (DMA–APM) technique (Aero...

  6. Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

    NASA Astrophysics Data System (ADS)

    Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

    2013-11-01

    Multi-wavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentration profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analysed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical in distinguishing between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

  7. Assessment of aerosol's mass concentrations from measured linear particle depolarization ratio (vertically resolved) and simulations

    NASA Astrophysics Data System (ADS)

    Nemuc, A.; Vasilescu, J.; Talianu, C.; Belegante, L.; Nicolae, D.

    2013-06-01

    Multiwavelength depolarization Raman lidar measurements from Magurele, Romania are used in this study along with simulated mass-extinction efficiencies to calculate the mass concentrations profiles of different atmospheric components, due to their different depolarization contribution to the 532 nm backscatter coefficient. Linear particle depolarization ratio (δpart) was computed using the relative amplification factor and the system-dependent molecular depolarization. The low depolarizing component was considered as urban/smoke, with a mean δpart of 3%, while for the high depolarizing component (mineral dust) a mean δpart of 35% was assumed. For this study 11 months of lidar measurements were analyzed. Two study cases are presented in details: one for a typical Saharan dust aerosol intrusion, 10 June 2012 and one for 12 July 2012 when a lofted layer consisting of biomass burning smoke extended from 3 to 4.5 km height. Optical Properties of Aerosols and Clouds software package (OPAC) classification and conversion factors were used to calculate mass concentrations. We found that calibrated depolarization measurements are critical to distinguish between smoke-reach aerosol during the winter and dust-reach aerosol during the summer, as well as between elevated aerosol layers having different origins. Good agreement was found between lidar retrievals and DREAM- Dust REgional Atmospheric Model forecasts in cases of Saharan dust. Our method was also compared against LIRIC (The Lidar/Radiometer Inversion Code) and very small differences were observed.

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

    PubMed Central

    Ku, Bon Ki; Evans, Douglas E.

    2015-01-01

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

  9. Mass concentration and mineralogical characteristics of aerosol particles collected at Dunhuang during ACE-Asia

    NASA Astrophysics Data System (ADS)

    Shen, Z. X.; Cao, J. J.; Li, X. X.; Okuda, T.; Wang, Y. Q.; Zhang, X. Y.

    2006-03-01

    Measurements were performed in spring 2001 and 2002 to determine the characteristics of soil dust in the Chinese desert region of Dunhuang, one of the ground sites of the Asia-Pacific Regional Aerosol Characterization Experiment (ACE-Asia). The mean mass concentrations of total suspended particle matter during the spring of 2001 and 2002 were 317 mu g m(-3) and 307 mu g m(-3) respectively. Eleven dust storm events were observed with a mean aerosol concentration of 1095 mu g m(-3), while the non-dusty days with calm or weak wind speed had a background aerosol loading of 196 mu g m(-3) on average in the springtime. The main minerals detected in the aerosol samples by X-ray diffraction were illite, kaolinite, chlorite, quartz, feldspar, calcite and dolomite. Gypsum, halite and amphibole were also detected in a few samples. The mineralogical data also show that Asian dust is characterized by a kaolinite to chlorite (K/C) ratio lower than 1 whereas Saharan dust exhibits a K/C ratio larger than 2. Air mass back- trajectory analysis show that three families of pathways are associated with the aerosol particle transport to Dunhuang, but these have similar K/C ratios, which further demonstrates that the mineralogical characteristics of Asian dust are different from African dust.

  10. Comparison of two methods for obtaining quantitative mass concentrations from aerosol time-of-flight mass spectrometry measurements.

    PubMed

    Qin, Xueying; Bhave, Prakash V; Prather, Kimberly A

    2006-09-01

    Aerosol time-of-flight mass spectrometry (ATOFMS) measurements provide continuous information on the aerodynamic size and chemical composition of individual particles. In this work, we compare two approaches for converting unscaled ATOFMS measurements into quantitative particle mass concentrations using (1) reference mass concentrations from a co-located micro-orifice uniform deposit impactor (MOUDI) with an accurate estimate of instrument busy time and (2) reference number concentrations from a co-located aerodynamic particle sizer (APS). Aerodynamic-diameter-dependent scaling factors are used for both methods to account for particle transmission efficiencies through the ATOFMS inlet. Scaling with APS data retains the high-resolution characteristics of the ambient aerosol because the scaling functions are specific for each hourly time period and account for a maximum in the ATOFMS transmission efficiency curve for larger-sized particles. Scaled mass concentrations obtained from both methods are compared with co-located PM(2.5) measurements for evaluation purposes. When compared against mass concentrations from a beta attenuation monitor (BAM), the MOUDI-scaled ATOFMS mass concentrations show correlations of 0.79 at Fresno, and the APS-scaled results show correlations of 0.91 at Angiola. Applying composition-dependent density corrections leads to a slope of nearly 1 with 0 intercept between the APS-scaled absolute mass concentration values and BAM mass measurements. This paper provides details on the methodologies used to convert ATOFMS data into continuous, quantitative, and size-resolved mass concentrations that will ultimately be used to provide a quantitative estimate of the number and mass concentrations of particles from different sources. PMID:16944899

  11. Fire and biofuel contributions to annual mean aerosol mass concentrations in the United States

    NASA Astrophysics Data System (ADS)

    Park, Rokjin J.; Jacob, Daniel J.; Logan, Jennifer A.

    We estimate the contributions from biomass burning (summer wildfires, other fires, residential biofuel, and industrial biofuel) to seasonal and annual aerosol concentrations in the United States. Our approach is to use total carbonaceous (TC) and non-soil potassium (ns-K) aerosol mass concentrations for 2001-2004 from the nationwide IMPROVE network of surface sites, together with satellite fire data. We find that summer wildfires largely drive the observed interannual variability of TC aerosol concentrations in the United States. TC/ns-K mass enhancement ratios from fires range from 10 for grassland and shrub fires in the south to 130 for forest fires in the north. The resulting summer wildfire contributions to annual TC aerosol concentrations for 2001-2004 are 0.26 μg C m -3 in the west and 0.14 μg C m -3 in the east; Canadian fires are a major contributor in the east. Non-summer wildfires and prescribed burns contribute on an annual mean basis 0.27 and 0.31 μg C m -3 in the west and the east, highest in the southeast because of prescribed burning. Residential biofuel is a large contributor in the northeast with annual mean concentration of up to 2.2 μg C m -3 in Maine. Industrial biofuel (mainly paper and pulp mills) contributes up to 0.3 μg C m -3 in the southeast. Total annual mean fine aerosol concentrations from biomass burning average 1.2 and 1.6 μg m -3 in the west and east, respectively, contributing about 50% of observed annual mean TC concentrations in both regions and accounting for 30% (west) and 20% (east) of total observed fine aerosol concentrations. Our analysis supports bottom-up source estimates for the contiguous United States of 0.7-0.9 Tg C yr -1 from open fires (climatological) and 0.4 Tg C yr -1 from biofuel use. Biomass burning is thus an important contributor to US air quality degradation, which is likely to grow in the future.

  12. The Aerosol Research and Inhalation Epidemiology Study (ARIES): PM2.5 mass and aerosol component concentrations and sampler intercomparisons.

    PubMed

    Van Loy, M; Bahadori, T; Wyzga, R; Hartsell, B; Edgerton, E

    2000-08-01

    The Aerosol Research and Inhalation Epidemiology Study (ARIES) was designed to provide high-quality measurements of PM2.5, its components, and co-varying pollutants for an air pollution epidemiology study in Atlanta, GA. Air pollution epidemiology studies have typically relied on available data on particle mass often collected using filter-based methods. Filter-based PM2.5 sampling is susceptible to both positive and negative errors in the measurement of aerosol mass and particle-phase component concentrations in the undisturbed atmosphere. These biases are introduced by collection of gas-phase aerosol components on the filter media or by volatilization of particle phase components from collected particles. As part of the ARIES, we collected daily 24-hr PM2.5 mass and speciation samples and continuous PM2.5 data at a mixed residential-light industrial site in Atlanta. These data facilitate analysis of the effects of a wide variety of factors on sampler performance. We assess the relative importance of PM2.5 components and consider associations and potential mechanistic linkages of PM2.5 mass concentrations with several PM2.5 components. For the 12 months of validated data collected to date (August 1, 1998-July 31, 1999), the monthly average Federal Reference Method (FRM) PM2.5 mass always exceeded the proposed annual average standard (12-month average = 20.3 +/- 9.5 micrograms/m3). The particulate SO4(2-) fraction (as (NH4)2SO4) was largest in the summer and exceeded 50% of the FRM mass. The contribution of (NH4)2SO4 to FRM PM2.5 mass dropped to less than 30% in winter. Particulate NO3- collected on a denuded nylon filter averaged 1.1 +/- 0.9 micrograms/m3. Particle-phase organic compounds (as organic carbon x 1.4) measured on a denuded quartz filter sampler averaged 6.4 +/- 3.1 micrograms/m3 (32% of FRM PM2.5 mass) with less seasonal variability than SO4(2-). PMID:11002607

  13. A Miniature System for Separating Aerosol Particles and Measuring Mass Concentrations

    PubMed Central

    Liang, Dao; Shih, Wen-Pin; Chen, Chuin-Shan; Dai, Chi-An

    2010-01-01

    We designed and fabricated a new sensing system which consists of two virtual impactors and two quartz-crystal microbalance (QCM) sensors for measuring particle mass concentration and size distribution. The virtual impactors utilized different inertial forces of particles in air flow to classify different particle sizes. They were designed to classify particle diameter, d, into three different ranges: d < 2.28 μm, 2.28 μm ≤ d ≤ 3.20 μm, d > 3.20 μm. The QCM sensors were coated with a hydrogel, which was found to be a reliable adhesive for capturing aerosol particles. The QCM sensor coated with hydrogel was used to measure the mass loading of particles by utilizing its characteristic of resonant frequency shift. An integrated system has been demonstrated. PMID:22319317

  14. THE TAPERED ELEMENT OSCILLATING MICROBALANCE: A MONITOR FOR SHORT-TERM MEASUREMENT OF FINE AEROSOL MASS CONCENTRATION

    EPA Science Inventory

    A new instrument for short-term monitoring of ambient aerosol fine mass concentration has been developed based on a unique device called a Tapered Element Oscillating Microbalance (TEOM). The detector consists of a tapered hollow tube fixed at the wide end and holding an exchange...

  15. The potential of LIRIC to validate the vertical profiles of the aerosol mass concentration estimated by an air quality model

    NASA Astrophysics Data System (ADS)

    Siomos, Nikolaos; Filoglou, Maria; Poupkou, Anastasia; Liora, Natalia; Dimopoulos, Spyros; Melas, Dimitris; Chaikovsky, Anatoli; Balis, Dimitris

    2015-04-01

    Vertical profiles of the aerosol mass concentration derived by a retrieval algorithm that uses combined sunphotometer and LIDAR data (LIRIC) were used in order to validate the mass concentration profiles estimated by the air quality model CAMx. LIDAR and CIMEL measurements of the Laboratory of Atmospheric Physics of the Aristotle University of Thessaloniki were used for this validation.The aerosol mass concentration profiles of the fine and coarse mode derived by CAMx were compared with the respective profiles derived by the retrieval algorithm. For the coarse mode particles, forecasts of the Saharan dust transportation model BSC-DREAM8bV2 were also taken into account. Each of the retrieval algorithm's profiles were matched to the models' profile with the best agreement within a time window of four hours before and after the central measurement. OPAC, a software than can provide optical properties of aerosol mixtures, was also employed in order to calculate the angstrom exponent and the lidar ratio values for 355nm and 532nm for each of the model's profiles aiming in a comparison with the angstrom exponent and the lidar ratio values derived by the retrieval algorithm for each measurement. The comparisons between the fine mode aerosol concentration profiles resulted in a good agreement between CAMx and the retrieval algorithm, with the vertical mean bias error never exceeding 7 μgr/m3. Concerning the aerosol coarse mode concentration profiles both CAMx and BSC-DREAM8bV2 values are severely underestimated, although, in cases of Saharan dust transportation events there is an agreement between the profiles of BSC-DREAM8bV2 model and the retrieval algorithm.

  16. 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.

  17. LIDAR technique: a central puzzle piece to build an integrated observation - modeling approach for air mass aerosols concentration evaluation

    NASA Astrophysics Data System (ADS)

    Tudose, Ovidiu-Gelu

    2013-04-01

    This paper presents a study of the temporal and vertical variation of mixed aerosol mass concentration near Bucharest during a dedicated observation campaign performed in summer 2012. To obtain the vertical mass concentrations profiles a combination of measured (mainly based on LIDAR technique) and modeled data was used. This method is based on the hypothesis that any mixture in the atmosphere can be described as a combination of low-depolarizing and high-depolarizing particles of a particular type. It uses the method proposed by Tesche et al. (2009), combined with forward simulations (i.e. OPAC). Based on supplementary information (e.g. preliminary assessment of aerosol source from forecast models and back trajectories) and several optical indicators (Angstrom exponent, LIDAR ratio, particle depolarization, AOD we built an approach to 2 cases of aerosol mixture, and validate the results using other information sources: sun photometry, forecasts, back trajectories. The first case was proved to be a smoke predominant layer, the second a Saharan dust predominant layer. Information from various data sources (DREAM, HYSPLIT, AERONET, MODIS) was consistent with our retrievals.

  18. The Potential of The Synergy of Sunphotometer and Lidar Data to Validate Vertical Profiles of The Aerosol Mass Concentration Estimated by An Air Quality Model

    NASA Astrophysics Data System (ADS)

    Siomos, N.; Filioglou, M.; Poupkou, A.; Liora, N.; Dimopoulos, S.; Melas, D.; Chaikovsky, A.; Balis, D. S.

    2016-06-01

    Vertical profiles of the aerosol mass concentration derived by the Lidar/Radiometer Inversion Code (LIRIC), that uses combined sunphotometer and lidar data, were used in order to validate the aerosol mass concentration profiles estimated by the air quality model CAMx. Lidar and CIMEL measurements performed at the Laboratory of Atmospheric Physics of the Aristotle University of Thessaloniki, Greece (40.5N, 22.9E) from the period 2013-2014 were used in this study.

  19. A new method for assessing the contribution of Primary Biological Atmospheric Particles to the mass concentration of the atmospheric aerosol.

    PubMed

    Perrino, Cinzia; Marcovecchio, Francesca

    2016-02-01

    Primary Biologic Atmospheric Particles (PBAPs) constitute an interesting and poorly investigated component of the atmospheric aerosol. We have developed and validated a method for evaluating the contribution of overall PBAPs to the mass concentration of atmospheric particulate matter (PM). The method is based on PM sampling on polycarbonate filters, staining of the collected particles with propidium iodide, observation at epifluorescence microscope and calculation of the bioaerosol mass using a digital image analysis software. The method has been also adapted to the observation and quantification of size-segregated aerosol samples collected by multi-stage impactors. Each step of the procedure has been individually validated. The relative repeatability of the method, calculated on 10 pairs of atmospheric PM samples collected side-by-side, was 16%. The method has been applied to real atmospheric samples collected in the vicinity of Rome, Italy. Size distribution measurements revealed that PBAPs was mainly in the coarse fraction of PM, with maxima in the range 5.6-10 μm. 24-h samples collected during different period of the year have shown that the concentration of bioaerosol was in the range 0.18-5.3 μg m(-3) (N=20), with a contribution to the organic matter in PM10 in the range 0.5-31% and to the total mass concentration of PM10 in the range 0.3-18%. The possibility to determine the concentration of total PBAPs in PM opens up interesting perspectives in terms of studying the health effects of these components and of increasing our knowledge about the composition of the organic fraction of the atmospheric aerosol. PMID:26680730

  20. Changes in ground-level PM mass concentration and column aerosol optical depth over East Asia during 2004-2014

    NASA Astrophysics Data System (ADS)

    Nam, J.; Kim, S. W.; Park, R.; Yoon, S. C.; Sugimoto, N.; Park, J. S.; Hong, J.

    2015-12-01

    Multi-year records of moderate resolution imaging spectroradiometer (MODIS), ground-level particulate matter (PM) mass concentration, cloud-aerosol lidar with orthogonal polarization (CALIOP), and ground-level lidar were analyzed to investigate seasonal and annual changes of aerosol optical depth (AOD) and PM mass concentration over East Asia. Least mean square fit method is applied to detect the trends and their magnitudes for each selected regions and stations. Eleven-year MODIS measurements show generally increasing trends in both AOD (1.18 % yr-1) and Ångström exponent (0.98 % yr-1), especially over the east coastal industrialized region in China. Monthly variation of AOD show maximum value at April-July, which were related to the progress of summer monsoon rain band and stationary continental air mass on the northeast of Asia. Increasing trends of AOD were found for eight cites in China (0.80 % yr-1) and Seoul site, Korea (0.40 % yr-1), whereas no significant change were shown in Gosan background site (0.04 % yr-1) and decreasing trend at five background sites in Japan (-0.42 % yr-1). Contrasting to AOD trend, all fifteen sites in China (-1.28 % yr-1), Korea (-2.77 % yr-1), and Japan (-2.03 % yr-1) showed decreasing trend of PM10 mass concentration. Also, PM2.5 mass concentration at Beijing, Seoul, Rishiri, and Oki show significant decreasing trend of -1.16 % yr-1. To further discuss the opposite trend of surface PM mass concentration and column AOD, we investigate vertical aerosol profile from lidar measurements. AOD estimated for planetary boundary layer (surface~1.5 km altitude; AODPBL) from CALIOP measurements over East China show decreasing trend of -1.71 % yr-1 over the period of 2007-2014, wherever AOD estimated for free troposphere (1.5 km~5 km altitude; AODFT) show increasing trend of 2.92 % yr-1. In addition, ground-level lidar measurements in Seoul show decreasing AODPBL trend of -2.57 % yr-1, whereas, AODFT show no significant change (-0.44 % yr

  1. In Situ Measurements of Aerosol Mass Concentration and Spectral Absorption at Three Location in and Around Mexico City

    NASA Astrophysics Data System (ADS)

    Chaudhry, Z.; Martins, V.; Li, Z.

    2006-12-01

    As a result of population growth and increasing industrialization, air pollution in heavily populated urban areas is one of the central environmental problems of the century. As a part of the MILAGRO (Megacity Initiative: Local and Global Research Observations) study, Nuclepore filters were collected in two size ranges (PM10 and PM2.5) at 12 hour intervals at three location in Mexico during March, 2006. Sampling stations were located at the Instituto Mexicano del Petroleo (T0), at the Rancho La Bisnago in the State of Hidalgo (T2) and along the Gulf Coast in Tampico (Tam). Each filter was analyzed for mass concentration, aerosol scattering and absorption efficiencies. Mass concentrations at T0 ranged from 47 to 179 μg/m3 for PM10 with an average concentration of 96 μg/m3, and from 20 to 93 μg/m3 for PM2.5 with an average concentration of 41 μg/m3. Mass concentrations at T2 ranged from 12 to 154 μg/m3 for PM10 with an average concentration of 51 μg/m3, and from 7 to 50 μg/m3 for PM2.5 with an average concentration of 25 μg/m3. Mass concentrations at Tam ranged from 34 to 80 μg/m3 for PM10 with an average concentration of 52 μg/m3, and from 8 to 23 μg/m3 for PM2.5 with an average concentration of 13 μg/m3. While some of the extreme values are likely linked to local emissions, regional air pollution episodes also played important roles. Each of the sampling stations experienced a unique atmospheric condition. The site at T0 was influenced by urban air pollution and dust storms, the site at T2 was significantly less affected by air pollution but more affected by regional dust storms and local dust devils while Tam was influenced by air pollution, dust storms and the natural marine environment. The spectral mass absorption efficiency was measured from 350 to 2500 nm and shows large differences between the absorption properties of soil dust, black carbon, and organic aerosols. The strong spectral differences observed can be related to differences in

  2. 40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size...

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 5 2011-07-01 2011-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval...

  3. 40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized “Typical” Coarse Aerosol Size...

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 6 2014-07-01 2014-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM 2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval...

  4. 40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size...

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 6 2012-07-01 2012-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval...

  5. 40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized “Typical” Coarse Aerosol Size...

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 6 2013-07-01 2013-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM 2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval...

  6. 40 CFR Table F-5 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size...

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 5 2010-07-01 2010-07-01 false Estimated Mass Concentration... 53—Estimated Mass Concentration Measurement of PM2.5 for Idealized “Typical” Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval...

  7. A method for segregating the optical absorption properties and the mass concentration of winter time urban aerosol

    NASA Astrophysics Data System (ADS)

    Ajtai, T.; Utry, N.; Pintér, M.; Major, B.; Bozóki, Z.; Szabó, G.

    2015-12-01

    A novel in-situ, real time method for the determination of inherent absorption properties of light absorbing carbonaceous particulate matter and its possible application for source apportionment are introduced here. The method is deduced from a two-week campaign under wintry urban conditions during which strong correlation was found between aerosol number size distribution and wavelength dependent optical absorption coefficient (AOC(λ)), measured by a Single Mobility Particle Sizer (SMPS) and a multi-wavelength photoacoustic absorption spectrometer, respectively, while wood burning and traffic (i.e. fossil fuel burning) activity were identified to be the dominant sources of carbonaceous particulate. Indeed, during the whole campaign, regardless of the actual emission strength of the aerosol sources, the measured number size distributions were always dominated by two unimodal modes with Count Mean Diameter (CMD) of 20 and 100 nm, which could be correlated to traffic and wood burning activities, respectively. AAEff, AAEwb (i.e. the Aerosol Angström Exponent of traffic and wood burning aerosol, respectively), σff(266 nm), σff(1064 nm), σwb(266 nm) and σff(1064 nm) (i.e. the segregated mass specific optical absorption coefficients at two of the measurement wavelengths) were found to be 1.17 ± 0.18, 2.6 ± 0.14, 7.3 ± 0.3 m2g-1, 1.7 ± 0.1 m2g-1 3.4 ± 0.3 m2g-1 and 0.31 ± 0.08 m2g-1, respectively. Furthermore the introduced methodology can also disentangle and quantify the temporal variation of both the segregated optical absorptions and the segregated mass concentrations of traffic and wood burning aerosol. Accordingly, the contribution of wood burning to optical absorption of PM was found to be negligible at 1064 nm but increased gradually towards the shorter wavelengths and became commensurable with the optical absorption of traffic at 266 nm during the whole measurement period. Furthermore, the contribution of wood burning mass to CM (mass of carbonaceous

  8. Evolution of size-segregated aerosol mass concentration during the Antarctic summer at Northern Foothills, Victoria Land

    NASA Astrophysics Data System (ADS)

    Illuminati, Silvia; Bau, Sébastien; Annibaldi, Anna; Mantini, Caterina; Libani, Giulia; Truzzi, Cristina; Scarponi, Giuseppe

    2016-01-01

    Within the framework of the Italian National Programm for Antarctic Research (PNRA), the first direct gravimetric measurements of size-segregated aerosol fractions were carried out at Faraglione Camp, ˜3-km far from the Italian station "M. Zucchelli" (Terra Nova Bay, Ross Sea), during the 2014-2015 austral summer. A six-stage high-volume cascade impactor with size classes between 10 μm and 0.49 μm, and, in parallel, for comparison purposes, a PM10 high-volume sampler (50% cut-off aerodynamic diameter of 10 μm) were used. A 10-day sampling strategy was adopted. Aerosol mass measurements were carried out before and after exposure by using a microbalance specifically designed for the filter weight and placed inside a glove bag in order to maintain stable temperature and humidity conditions during weighing sessions. Measured atmospheric concentrations (referred to the "actual air conditions" of mean temperature of 268 K and mean pressure of 975 hPa) of size-segregated aerosol fractions showed the following values, given as size range, means (interquartile range): Dp < 0.49 μm, 0.33 (0.26-0.34) μg m-3; 0.49-0.95 μm, 0.20 (0.19-0.24) μg m-3; 0.95-1.5 μm, 0.16 (0.13-0.21) μg m-3; 1.5-3.0 μm 0.075 (0.05-0.11) μg m-3; 3.0-7.2 μm 0.12 (0.02-0.19) μg m-3; 7.2-10 μm 0.06 (0.01-0.03) μg m-3. The average mass concentration of the total PM10 at Faraglione Camp for the entire sampling period was 0.92 (0.67-1.1) μg m-3. Although a great variability, the aerosol mass concentration showed a tri-modal distribution, with an accumulation mode (in the range 0.1-1.0 μm) and two coarse modes (CM1 in the range 1.0-3.0 μm, and CM2 in the range 3.0-10 μm). From 50% to 90% of the PM10 mass comes from particles of a size smaller than 1.0 μm. The two coarse modes represented from ˜5% to ˜35% of the PM10, showing opposite seasonal trends (CM1 decreased while CM2 increased). During summer, PM10 mass concentration increased to a maximum of ˜1.6 μg m-3 at mid-December, while

  9. Tropopsheric Aerosol Chemistry via Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Worsnop, Douglas

    2008-03-01

    A broad overview of size resolved aerosol chemistry in urban, rural and remote regions is evolving from deployment of aerosol mass spectrometers (AMS) throughout the northern hemisphere. Using thermal vaporization and electron impact ionization as universal detector of non-refractory inorganic and organic composition, the accumulation of AMS results represent a library of mass spectral signatures of aerosol chemistry. For organics in particular, mass spectral factor analysis provides a procedure for classifying (and simplifying) complex mixtures composed of the hundreds or thousands of individual compounds. Correlations with parallel gas and aerosol measurements (e.g. GC/MS, HNMR, FTIR) supply additional chemical information needed to interpret mass spectra. The challenge is to separate primary and secondary; anthropogenic, biogenic and biomass burning sources - and subsequent - transformations of aerosol chemistry and microphysics.

  10. Size segregated mass concentration and size distribution of near surface aerosols over a tropical Indian semi-arid station, Anantapur: Impact of long range transport.

    PubMed

    Raghavendra Kumar, K; Narasimhulu, K; Balakrishnaiah, G; Suresh Kumar Reddy, B; Rama Gopal, K; Reddy, R R; Moorthy, K Krishna; Suresh Babu, S

    2009-10-15

    Regular measurements of size segregated as well as total mass concentration and size distribution of near surface composite aerosols, made using a ten-channel Quartz Crystal Microbalance (QCM) cascade impactor during the period of September 2007-May 2008 are used to study the aerosol characteristics in association with the synoptic meteorology. The total mass concentration varied from 59.70+/-1.48 to 41.40+/-1.72 microg m(-3), out of which accumulation mode dominated by approximately 50%. On a synoptic scale, aerosol mass concentration in the accumulation (submicron) mode gradually increased from an average low value of approximately 26.92+/-1.53 microg m(-3) during the post monsoon season (September-November) to approximately 34.95+/-1.32 microg m(-3) during winter (December-February) and reaching a peak value of approximately 43.56+/-1.42 microg m(-3) during the summer season (March-May). On the contrary, mass concentration of aerosols in the coarse (supermicron) mode increased from approximately 9.23+/-1.25 microg m(-3)during post monsoon season to reach a comparatively high value of approximately 25.89+/-1.95 microg m(-3) during dry winter months and a low value of approximately 8.07+/-0.76 microg m(-3) during the summer season. Effective radius, a parameter important in determining optical (scattering) properties of aerosol size distribution, varied between 0.104+/-0.08 microm and 0.167+/-0.06 microm with a mean value of 0.143+/-0.01 microm. The fine mode is highly reduced during the post monsoon period and the large and coarse modes continue to remain high (replenished) so that their relative dominance increases. It can be seen that among the two parameters measured, correlation of total mass concentration with air temperature is positive (R(2)=0.82) compared with relative humidity (RH) (R(2)=0.75). PMID:19640569

  11. Long-Term Observations on Aerosol Elemental Carbon and Mass Concentrations in Winter-Time in New Delhi: Implications for Local Source Changes

    NASA Astrophysics Data System (ADS)

    Aggarwal, S. G.; Singh, K.; Singh, N.; Gupta, P. K.

    2009-12-01

    Fossil-fuel and bio-fuel burning are the two major sources identified for high carbonaceous aerosol loadings in several mega cities in India. In the last decade, according to a report from the Central Pollution Control Board (CPCB, 1999), the vehicular emission (mostly diesel-powered engines) was contributed to ~67% of the total air pollution load in New Delhi. Therefore, a policy decision was taken by the government, and most of the diesel-powered engines were converted to compressed natural gas (CNG) -powered engines by 2003. To better understand the effect of these changes on air quality, we collected high volume aerosol samples (total suspended particles, TSP) mostly for a day basis at our institute building in New Delhi almost everyday during winter season (November to January) from 2002 to 2008. We found very high mean aerosol loading, i.e., 488±47 μg m-3 in 2002 winter, which dropped significantly to 280±73 μg m-3 in 2003 winter. Thereafter, a steadily increased trend of aerosol mass loadings was observed, i.e., 339±112, 339±120, 412±107 and 444±55 μg m-3 in 2004, 2005, 2006 and 2007 winters, respectively. Similar trend was also observed for elemental carbon (EC) concentration in TSP, which was peaked in 2002 (47±11 μg m-3) and minimized in 2003 (32±6 μg m-3), and then gradually increased to 41±8 μg m-3 in 2007 winter. These decline trends of aerosol mass and EC concentrations in 2003 can be explained well, because of the conversion of diesel engine to CNG engines of public transport facilities. However, again increase in aerosol mass and EC concentrations possibly because of a high increase in road traffic in recent years. According to the economic survey of New Delhi 2008-09, the number of vehicles (which includes all types of engines, i.e., petrol, diesel and CNG) has grown from ~3.3 millions in 1997-98 to ~5.6 millions in 2007-08. The influence of engine types and vehicle population on aerosol loading can also be explained well by SO2 and

  12. Characterization of Florida red tide aerosol and the temporal profile of aerosol concentration

    PubMed Central

    Cheng, Yung Sung; Zhou, Yue; Pierce, Richard H.; Henry, Mike; Baden, Daniel G.

    2009-01-01

    Red tide aerosols containing aerosolized brevetoxins are produced during the red tide bloom and transported by wind to coastal areas of Florida. This study reports the characterization of Florida red tide aerosols in human volunteer studies, in which an asthma cohort spent 1 h on Siesta Beach (Sarasota, Florida) during aerosolized red tide events and non-exposure periods. Aerosol concentrations, brevetoxin levels, and particle size distribution were measured. Hourly filter samples were taken and analyzed for brevetoxin and NaCl concentrations. In addition, the aerosol mass concentration was monitored in real time. The results indicated that during a non-exposure period in October 2004, no brevetoxin was detected in the water, resulting in non-detectable levels of brevetoxin in the aerosol. In March 2005, the time-averaged concentrations of brevetoxins in water samples were moderate, in the range of 5–10 μg/L, and the corresponding brevetoxin level of Florida red tide aerosol ranged between 21 and 39 ng/m3. The temporal profiles of red tide aerosol concentration in terms of mass, NaCl, and brevetoxin were in good agreement, indicating that NaCl and brevetoxins are components of the red tide aerosol. By continuously monitoring the marine aerosol and wind direction at Siesta Beach, we observed that the marine aerosol concentration varied as the wind direction changed. The temporal profile of the Florida red tide aerosol during a sampling period could be explained generally with the variation of wind direction. PMID:19879288

  13. Long-term comparative study of columnar and surface mass concentration aerosol properties in a background environment

    NASA Astrophysics Data System (ADS)

    Bennouna, Y. S.; Cachorro, V. E.; Mateos, D.; Burgos, M. A.; Toledano, C.; Torres, B.; de Frutos, A. M.

    2016-09-01

    The relationship between columnar and surface aerosol properties is not a straightforward problem. The Aerosol Optical Depth (AOD), Ångström exponent (AE), and ground-level Particulate Matter (PMX, x = 10 or 2.5 μm) data have been studied from a climatological point of view. Despite the different meanings of AOD and PMx both are key and complementary quantities that quantify aerosol load in the atmosphere and many studies intend to find specific relationships between them. Related parameters such as AE and PM ratio (PR = PM2.5/PM10), giving information about the predominant particle size, are included in this study on the relationships between columnar and surface aerosol parameters. This study is based on long measurement records (2003-2014) obtained at two nearby background sites from the AERONET and EMEP networks in the north-central area of Spain. The climatological annual cycle of PMx shows two maxima along the year (one in late-winter/early-spring and another in summer), but this cycle is not followed by the AOD which shows only a summer maximum and a nearly bell shape. However, the annual means of both data sets show strong correlation (R = 0.89) and similar decreasing trends of 40% (PM10) and 38% (AOD) for the 12-year record. PM10 and AOD daily data are moderately correlated (R = 0.58), whereas correlation increases for monthly (R = 0.74) and yearly (R = 0.89) means. Scatter plots of AE vs. AOD and PR vs. PM10 have been used to characterize aerosols over the region. The PR vs. AE scatterplot of daily data shows no correlation due to the prevalence of intermediate-sized particles. As day-to-day correlation is low (especially for high turbidity events), a binned analysis was also carried out to establish consistent relationships between columnar and surface quantities, which is considered to be an appropriate approach for environmental and climate studies. In this way the link between surface concentrations and columnar remote sensing data is shown to

  14. Analysis of spatial and seasonal distributions of MODIS aerosol optical properties and ground-based measurements of mass concentrations in the Yellow Sea region in 2009.

    PubMed

    Kim, Hak-Sung; Chung, Yong-Seung; Lee, Sun-Gu

    2013-01-01

    Satellite-retrieved data on aerosol optical depth (AOD) and Ångström exponent (AE) using a moderate resolution imaging spectrometer (MODIS) were used to analyze large-scale distributions of atmospheric aerosols in East Asia. AOD was relatively high in March (0.44 ± 0.25) and low in September (0.24 ± 0.21) in the East Asian region in 2009. Sandstorms originating from the deserts and dry areas in northern China and Mongolia were transported on a massive scale during the springtime, thus contributing to the high AOD in East Asia. However, whereas PM10 with diameters ≤10 μm was the highest in February at Anmyon, Cheongwon, and Ulleung, located leeward about halfway through the Korean Peninsula, AOD rose to its highest in May. The growth of hygroscopic aerosols attendant on increases in relative humidity prior to the Asian monsoon season contributed to a high AOD level in May. AE typically appears at high levels (1.30 ± 0.37) in August due to anthropogenic aerosols originating from the industrial areas in eastern China, while AOD stays low in summer due to the removal process caused by rainfall. The linear correlation coefficients of the MODIS AOD and ground-based mass concentrations of PM10 at Anmyon, Cheongwon, and Ulleung were measured at 0.4~0.6. Four cases (6 days) of mineral dustfall from sandstorms and six cases (12 days) of anthropogenically polluted particles were observed in the central area of the Korean Peninsula in 2009. PM10 mass concentrations increased at both Anmyon and Cheongwon in the cases of mineral dustfall and anthropogenically polluted particles. Cases of dustfall from sandstorms and anthropogenic polluted particles, with increasing PM10 mass concentrations, showed higher AOD values in the Yellow Sea region. PMID:22362557

  15. Intercomparison of methods to measure the mass concentration of the atmospheric aerosol during INTERCOMP2000—influence of instrumentation and size cuts

    NASA Astrophysics Data System (ADS)

    Hitzenberger, R.; Berner, A.; Galambos, Z.; Maenhaut, W.; Cafmeyer, J.; Schwarz, J.; Müller, K.; Spindler, G.; Wieprecht, W.; Acker, K.; Hillamo, R.; Mäkelä, T.

    Within the EUROTRAC-2 subproject AEROSOL, the intensive field campaign INTERCOMP2000 was conducted to compare aerosol samplers and methods to measure various aerosol properties. Here a comparison of mass concentrations measured with different PM2.5 and PM10 samplers as well as cascade impactors is described. Different filter types were used. In general, the PM2.5 and PM10 mass concentrations obtained on filters agree well. The data agree within 18.1% (PM2.5, all data). If data obtained with the TEOM (18% low) and on Whatman QM-A quartz fibre filters (low face velocity, 38% high) are excluded, PM2.5 data agree within 8.1%. For PM10, the agreement is within 6.6% (again excluding the Whatman QM-A quartz fibre filters, 22% high) or 12.1% (all data). For the impactor samples, the data agreed within 6.3% (excluding the ELPI, which was 92% high) and 8.7% for PM2.5 and PM10.

  16. Online atmospheric pressure chemical ionization ion trap mass spectrometry (APCI-IT-MSn) for measuring organic acids in concentrated bulk aerosol - a laboratory and field study

    NASA Astrophysics Data System (ADS)

    Vogel, A. L.; Äijälä, M.; Brüggemann, M.; Ehn, M.; Junninen, H.; Petäjä, T.; Worsnop, D. R.; Kulmala, M.; Williams, J.; Hoffmann, T.

    2012-08-01

    The field application of an aerosol concentrator in conjunction with an atmospheric pressure chemical ionization ion trap mass spectrometer (APCI-IT-MS) at the boreal forest station SMEAR II at Hyytiälä, Finland, is demonstrated in this study. APCI is a soft ionization technique allowing online measurements of organic acids in the gas and particle phase. The detection limit for the acid species in the particle phase was increased by a factor of 7.5 to 11 (e.g. ~40 ng m-3 for pinonic acid) by using the miniature Versatile Aerosol Concentration Enrichment System (mVACES) upstream of the mass spectrometer. The APCI-IT-MS was calibrated in the negative ion mode with two biogenic organic acid standards - pinic acid and pinonic acid. Pinic acid was used as a surrogate for the quantification of the total amount of organic acids in the ambient aerosol based on the total signal intensities in the negative ion mode. The results were compared with the total organic signal of a C-ToF-AMS during the HUMPPA-COPEC 2010 field campaign. The campaign average contribution of organic acids measured by APCI-IT-MS to the total sub-micron organic aerosol mass was estimated to be about 60%. Very good correlation between APCI-IT-MS and C-ToF-AMS (Pearson's R = 0.94) demonstrates soft ionization mass spectrometry as a complimentary technique to AMS with electron impact ionization. MS2 studies of specific m/z ratios recorded during the HUMPPA-COPEC 2010 field campaign were compared to MS2 studies of selected monoterpene oxidation products formed in simulation chamber experiments. The comparison of the resulting fragments shows that oxidation products of the main VOCs emitted at Hyytiälä (α-pinene and Δ3-carene) cannot account for all of the measured fragments, which illustrates the complexity of ambient aerosol and possibly indicates unidentified or underestimated biogenic SOA precursor in the boreal forest.

  17. Online atmospheric pressure chemical ionization ion trap mass spectrometry (APCI-IT-MSn) for measuring organic acids in concentrated bulk aerosol - a laboratory and field study

    NASA Astrophysics Data System (ADS)

    Vogel, A. L.; Äijälä, M.; Brüggemann, M.; Ehn, M.; Junninen, H.; Petäjä, T.; Worsnop, D. R.; Kulmala, M.; Williams, J.; Hoffmann, T.

    2013-02-01

    The field application of an aerosol concentrator in conjunction with an atmospheric pressure chemical ionization ion trap mass spectrometer (APCI-IT-MS) at the boreal forest station SMEAR II at Hyytiälä, Finland, is demonstrated in this study. APCI is a soft-ionization technique allowing online measurements of organic acids in the gas and particle phase. The detection limit for the acid species in the particle phase was improved by a factor of 7.5 to 11 (e.g. ∼40 ng m3 for pinonic acid) by using the miniature versatile aerosol concentration enrichment system (mVACES) upstream of the mass spectrometer. The APCI-IT-MS was calibrated in the negative ion mode with two biogenic organic acid standards - pinic acid and pinonic acid. Pinic acid was used as a surrogate for the quantification of the total amount of organic acids in the ambient aerosol based on the total signal intensities in the negative ion mode. The results were compared with the total organic signal of a C-ToF-AMS during the HUMPPA-COPEC 2010 field campaign. The campaign average contribution of organic acids measured by APCI-IT-MS to the total submicron organic aerosol mass was estimated to be about 60%, based on the response of pinic acid. Very good correlation between APCI-IT-MS and C-ToF-AMS (Pearson's R = 0.94) demonstrates soft-ionization mass spectrometry as a complimentary technique to AMS with electron impact ionization. MS2 studies of specific m/z ratios recorded during the HUMPPA-COPEC 2010 field campaign were compared to MS2 studies of selected monoterpene oxidation products formed in simulation chamber experiments. The comparison of the resulting fragments shows that oxidation products of the main VOCs emitted at Hyytiälä (α-pinene and Δ3-carene) cannot account for all of the measured fragments. Possible explanations for those unaccounted fragments are the presence of unidentified or underestimated biogenic SOA precursors, or that different products are formed by a different oxidant

  18. Boundary layer aerosol size distribution, mass concentration and mineralogical composition in Morocco and at Cape Verde Islands during SAMUM I-II

    NASA Astrophysics Data System (ADS)

    Kandler, K.; Lieke, K.

    2009-04-01

    The Saharan Mineral Dust Experiment (SAMUM) is dedicated to the understanding of the radiative effects of mineral dust. Two major field experiments were performed: A first joint field campaign took place at Ouarzazate and near Zagora, southern Morocco, from May 13 to June 7, 2006. Aircraft and ground based measurements of aerosol physical and chemical properties were carried out to collect a data set of surface and atmospheric columnar information within a major dust source. This data set combined with satellite data provides the base of the first thorough columnar radiative closure tests in Saharan dust. A second field experiment was conducted during January-February 2008, in the Cape Verde Islands region, where about 300 Tg of mineral dust are transported annually from Western Africa across the Atlantic towards the Caribbean Sea and the Amazon basin. Along its transport path, the mineral dust is expected to influence significantly the radiation budget - by direct and indirect effects - of the subtropical North Atlantic. We are lacking a radiative closure in the Saharan air plume. One focus of the investigation within the trade wind region is the spatial distribution of mixed dust/biomass/sea salt aerosol and their physical and chemical properties, especially with regard to radiative effects. We report on measurements of size distributions, mass concentrations and mineralogical composition conducted at the Zagora (Morocco) and Praia (Cape Verde islands) ground stations. The aerosol size distribution was measured from 20 nm to 500

  19. Three years of aerosol mass, black carbon and particle number concentrations at Montsec (southern Pyrenees, 1570 m a.s.l.)

    NASA Astrophysics Data System (ADS)

    Ripoll, A.; Pey, J.; Minguillón, M. C.; Pérez, N.; Pandolfi, M.; Querol, X.; Alastuey, A.

    2014-04-01

    Time variation of mass particulate matter (PM1 and PM1&minus10), black carbon (BC) and number of particles (N3: number of particles with an aerodynamic diameter higher than 3 nm, and N10: higher than 10 nm) concentrations at the high-altitude site of Montsec (MSC) in the southern Pyrenees was interpreted for the period 2010-2012. At MSC, PM10 (12 μg m-3) and N7 (2140 # cm-3) three-year arithmetic average concentrations were higher than those measured at other high-altitude sites in central Europe during the same period (PM10: 3-9 μg m-3 and N: 634-2070 # cm-3). By contrast, BC concentrations at MSC (0.2 μg m-3) were equal to or even lower than those measured at these European sites (0.2-0.4 μg m-3). These differences were attributed to the higher relevance of Saharan dust transport and to the higher importance of the biogenic precursor emissions and new particle formation (NPF) processes, and to the lower influence of anthropogenic emissions at MSC. The different time variation of PM and BC concentrations compared with that of N suggests that these aerosol parameters were governed by diverse factors at MSC. Both PM and BC concentrations showed marked differences for different meteorological scenarios, with enhanced concentrations under North African air outbreaks (PM1&minus10: 13 μg m-3, PM1: 8 μg m-3 and BC: 0.3 μg m-3) and low concentrations when Atlantic advections occurred (PM1-10: 5 μg m-3, PM1: 4 μg m-3 and BC: 0.1 μg m-3). PM and BC concentrations increased in summer, with a secondary maximum in early spring, and were at their lowest in winter, due to the contrasting origin of the air masses in the warmer seasons (spring and summer) and in the colder seasons (autumn and winter). The maximum in the warmer seasons was attributed to long-range transport processes that mask the breezes and regional transport breaking the daily cycles of these pollutants. By contrast, PM and BC concentrations showed clear diurnal cycles, with maxima at midday in the

  20. Three years of aerosol mass, black carbon and particle number concentrations at Montsec (southern~Pyrenees, 1570 m a.s.l.)

    NASA Astrophysics Data System (ADS)

    Ripoll, A.; Pey, J.; Minguillón, M. C.; Pérez, N.; Pandolfi, M.; Querol, X.; Alastuey, A.

    2013-10-01

    Time variation of mass particulate matter (PM1 and PM1-10), black carbon (BC) and particle number (N) concentrations at the high altitude site of Montsec (MSC) in the southern Pyrenees was interpreted for the period 2010-2012. The MSC site registered higher PM10 (12 μg m-3) and N > 7 nm (2209 # cm-3) concentrations than those measured at other high altitude sites in central Europe (PM10: 3-9 μg m-3 and N: 634-2070 # cm-3). By contrast, BC concentrations at MSC (0.2 μg m-3) were equal or even lower than those measured at these European sites (0.2-0.4 μg m-3). These differences were attributed to the lower influence of anthropogenic emissions and to the higher relevance of Saharan dust transport and new particle formation (NPF) processes at MSC. The different time variation of PM and BC concentrations compared with that of N suggests that these aerosol parameters were governed by diverse factors at MSC. Both PM and BC concentrations showed marked differences for different meteorological scenarios, with enhanced concentrations under North African outbreaks (PM1-10: 13 μg m-3, PM1: 8 μg m-3 and BC: 0.3 μg m-3) and low concentrations when Atlantic advections occurred (PM1-10: 5 μg m-3, PM1: 4 μg m-3 and BC: 0.1 μg m-3). Because of the contrasting origin of the air masses in the warmer seasons (spring and summer) and in the colder seasons (autumn and winter), PM and BC concentrations showed a marked increase in summer, with a secondary maximum in early spring, and were at their lowest during winter. The maximum in the warmer seasons was attributed to long-range transport processes which mask the breezes and regional transport breaking the daily cycles of these pollutants. By contrast, PM and BC concentrations showed clear diurnal cycles with maxima at midday in the colder seasons. A statistically significant weekly variation was also obtained for the BC concentrations, displaying a progressive increase from Tuesday to Saturday, followed by a significant

  1. Non-Refractory Submicron Aerosol Mass Loadings during NEAQS

    NASA Astrophysics Data System (ADS)

    Middlebrook, A. M.; Matthew, B. M.; Canagaratna, M. R.; Worsnop, D. R.; Quinn, P. K.; Degouw, J. A.; Warneke, C.; Goldan, P. D.; Kuster, W. C.; Williams, E. J.; McKeen, S. A.

    2003-12-01

    During the New England Air Quality Study (NEAQS) in July-August 2002, an Aerosol Mass Spectrometer (AMS) was deployed aboard the NOAA ship RONALD H. BROWN and collected 2-minute averaged data. The AMS, which measures non-refractory components of aerosol particles with aerodynamic diameters between roughly 40 and 1500 nm, produced particle mass spectra as well as aerosol organic, sulfate, ammonium, and nitrate mass distributions. A wide variety of air masses were sampled, 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 ammonium and nitrate and the mass loadings typically peaked around 400-600 nm in vacuum aerodynamic diameter. Although the AMS sulfate and ammonium concentrations were highly correlated with the sulfate and ammonium concentrations from the Particle into Liquid (PILS) instrument also deployed on the ship, the AMS and PILS nitrate concentrations were not correlated and at times anti-correlated. In contrast, the AMS nitrate and organic concentrations as well as the AMS nitrate and gas phase alkyl nitrate concentrations were highly correlated. These results suggest that organic nitrate was present in the submicron aerosol phase. The AMS organic concentrations were generally higher than the AMS sulfate concentrations, consistent with other shipboard measurements. Whenever the sulfate concentration increased, the organic concentration also increased, indicating that sulfate and organic aerosol growth are influenced by the same processes or that sulfate may play a role in organic aerosol growth. The exception to this pattern occurred during a sea fog event where the sulfate concentration increased and the organic concentration decreased, probably due to rapid aqueous phase sulfur oxidation and relatively less oxidation of organic compounds. Furthermore, the organic concentration often increased without concurrent increases in

  2. Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea ice

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

    2016-02-01

    Better characterisation of aerosol processes in pristine, natural environments, such as Antarctica, have recently been shown to lead to the largest reduction in uncertainties in our understanding of radiative forcing. Our understanding of aerosols in the Antarctic region is currently based on measurements that are often limited to boundary layer air masses at spatially sparse coastal and continental research stations, with only a handful of studies in the vast sea-ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the icebreaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the polar front, with mean polar cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low-pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air masses quickly from the free troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea-ice boundary layer air masses travelled equatorward into the low-albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei which, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and their transport pathways described here, could help reduce the discrepancy currently present between simulations and observations of

  3. Spatio-temporal variations of optical properties of aerosols in East Asia measured by MODIS and relation to the ground-based mass concentrations observed in central Korea during 2001˜2010

    NASA Astrophysics Data System (ADS)

    Kim, Hak-Sung; Chung, Yong-Seung; Kim, Joon-Tae

    2014-02-01

    Long-term variations and trends of atmospheric aerosols in the East Asian region were analyzed by using aerosol optical depth (AOD or τ), and ångström exponent (AE or α) obtained from the Moderate Resolution Imaging Spectroradiometer (MODIS) from 2001 to 2010. The increased emission of anthropogenic fine aerosols in east China resulted in the high AOD in this region during summer. The steady increasing emission of anthropogenic fine aerosols caused an increasing trend of AOD in east China, and the large-scale transport of sandstorms and smoke plume caused by forest fires affected intense inter-annual variations of AOD in the East Asian region. While in the central part of South Korea, located in the lee side of the East Asian continent, AE tended to rise to a level higher than in east China, the ground-based mass concentrations continued to decline. A noticeable decrease of PM10 mass concentration in spring and winter in central Korea is most likely attributable to decreases in sandstorms in the source region of East Asia. However, the ratio of PM2.5 mass concentration to PM10 increases overall with a high level in summer. Aerosol types were classified into dust, smoke plume, and sulphate by using satellite data over Cheongwon in central Korea. The columnar AOD, with different aerosol types, was compared with the ground-based mass concentrations at Cheongwon, and the relatively high level of the correlations presented between PM2.5 and AOD produced in sulphate. Growth and increases of fine hygroscopic aerosols generated as gas-to-particle conversion particularly in summer contribute to increases of columnar AOD in the East Asian region.

  4. Intercomparison between a single particle soot photometer and evolved gas analysis in an industrial area in Japan: Implications for the consistency of soot aerosol mass concentration measurements

    NASA Astrophysics Data System (ADS)

    Miyakawa, T.; Kanaya, Y.; Komazaki, Y.; Taketani, F.; Pan, X.; Irwin, M.; Symonds, J.

    2016-02-01

    Mass concentrations of soot (typically comprising black and elemental carbon; BC and EC, respectively) aerosols, were measured at Yokosuka city, an industrial region in Japan in the early summer of 2014. The results of laser-induced incandescence (LII) and evolved gas analysis (EGA) techniques were compared using a single particle soot photometer (SP2) and semi-continuous elemental/organic carbon analyzer (EC/OC analyzer), respectively. We revisited the procedure of SP2 calibration with a focus on investigating the relationship between LII intensity (SLII) and refractory BC (rBC) mass per particle (mPP) for some BC-proxies in the laboratory, as well as for ambient rBC particles in order to discuss the uncertainty of the SP2. It was found that the mPP-SLII for the fullerene soot and carbon black particles agreed well within 3% and 10%, respectively, with that for ambient rBC particles. This is the first time to suggest the use of carbon black as a reference material. We also found that the mPP-SLII for the aqueous deflocculated Acheson graphite particles with the correction factor given by Baumgardner et al. (2012) was still biased by around +20% to that for ambient rBC particles. EC quantified by the semi-continuous EC/OC analyzer using a thermal-protocol similar to that of Interagency Monitoring of Protected Visual Environments (IMPROVE-like), systematically showed higher concentrations than rBC measured by the SP2. The uncertainties related to SP2 cannot fully account for this difference. This result was likely caused by the contribution of charred organic materials to EC, which can be affected significantly by thermal-protocols for the EGA. The consistency and differences between rBC and EC are discussed with regard to comparing their respective mass concentrations.

  5. An explicit study of aerosol mass conversion and its parameterization in warm rain formation of cumulus clouds

    NASA Astrophysics Data System (ADS)

    Sun, J.; Fen, J.; Ungar, R. K.

    2013-10-01

    The life time of atmospheric aerosols is highly affected by in-cloud scavenging processes. Aerosol mass conversion from aerosols embedded in cloud droplets into aerosols embedded in raindrops is a pivotal pathway for wet removal of aerosols in clouds. The aerosol mass conversion rate in the bulk microphysics parameterizations is always assumed to be linearly related to the precipitation production rate, which includes the cloud water autoconversion rate and the cloud water accretion rate. The ratio of the aerosol mass concentration conversion rate to the cloud aerosol mass concentration has typically been considered to be the same as the ratio of the precipitation production rate to the cloud droplet mass concentration. However, the mass of an aerosol embedded in a cloud droplet is not linearly proportional to the mass of the cloud droplet. A simple linear relationship cannot be drawn between the precipitation production rate and the aerosol mass concentration conversion rate. In this paper, we studied the evolution of aerosol mass concentration conversion rates in a warm rain formation process with a 1.5-dimensional non-hydrostatic convective cloud and aerosol interaction model in the bin microphysics. We found that the ratio of the aerosol mass conversion rate to the cloud aerosol mass concentration can be statistically expressed by the ratio of the precipitation production rate to the cloud droplet mass concentration with an exponential function. We further gave some regression equations to determine aerosol conversions in the warm rain formation under different threshold radii of raindrops and different aerosol size distributions.

  6. Spatial and Temporal Variability of Outdoor Coarse Particulate Matter Mass Concentrations Measured with a New Coarse Particulate Sampler during the Detroit Exposure and Aerosol Research Study

    EPA Science Inventory

    The Detroit Exposure and Aerosol Research Study (DEARS) provided data to compare outdoor residential coarse particulate matter (PM10-2.5) concentrations in six different areas of Detroit with data from a central monitoring site. Daily and seasonal influences on the spa...

  7. Contribution of methane to aerosol carbon mass

    NASA Astrophysics Data System (ADS)

    Bianchi, F.; Barmet, P.; Stirnweis, L.; El Haddad, I.; Platt, S. M.; Saurer, M.; Lötscher, C.; Siegwolf, R.; Bigi, A.; Hoyle, C. R.; DeCarlo, P. F.; Slowik, J. G.; Prévôt, A. S. H.; Baltensperger, U.; Dommen, J.

    2016-09-01

    Small volatile organic compounds (VOC) such as methane (CH4) have long been considered non-relevant to aerosol formation due to the high volatility of their oxidation products. However, even low aerosol yields from CH4, the most abundant VOC in the atmosphere, would contribute significantly to the total particulate carbon budget. In this study, organic aerosol (OA) mass yields from CH4 oxidation were evaluated at the Paul Scherrer Institute (PSI) smog chamber in the presence of inorganic and organic seed aerosols. Using labeled 13C methane, we could detect its oxidation products in the aerosol phase, with yields up to 0.09

  8. 40 CFR Table F-6 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Fine Aerosol Size Distribution

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 5 2011-07-01 2011-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-6 Table F-6 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  9. 40 CFR Table F-4 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Coarse Aerosol Size Distribution

    Code of Federal Regulations, 2011 CFR

    2011-07-01

    ... 40 Protection of Environment 5 2011-07-01 2011-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-4 Table F-4 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  10. 40 CFR Table F-6 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized Fine Aerosol Size Distribution

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 6 2014-07-01 2014-07-01 false Estimated Mass Concentration... Equivalent Methods for PM 2.5 Pt. 53, Subpt. F, Table F-6 Table F-6 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  11. 40 CFR Table F-4 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized Coarse Aerosol Size Distribution

    Code of Federal Regulations, 2014 CFR

    2014-07-01

    ... 40 Protection of Environment 6 2014-07-01 2014-07-01 false Estimated Mass Concentration... Equivalent Methods for PM 2.5 Pt. 53, Subpt. F, Table F-4 Table F-4 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  12. 40 CFR Table F-4 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized Coarse Aerosol Size Distribution

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 6 2013-07-01 2013-07-01 false Estimated Mass Concentration... Equivalent Methods for PM 2.5 Pt. 53, Subpt. F, Table F-4 Table F-4 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m 3)...

  13. 40 CFR Table F-6 to Subpart F of... - Estimated Mass Concentration Measurement of PM 2.5 for Idealized Fine Aerosol Size Distribution

    Code of Federal Regulations, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 6 2013-07-01 2013-07-01 false Estimated Mass Concentration... Equivalent Methods for PM 2.5 Pt. 53, Subpt. F, Table F-6 Table F-6 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m 3)...

  14. 40 CFR Table F-6 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Fine Aerosol Size Distribution

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 6 2012-07-01 2012-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-6 Table F-6 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  15. 40 CFR Table F-4 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Coarse Aerosol Size Distribution

    Code of Federal Regulations, 2012 CFR

    2012-07-01

    ... 40 Protection of Environment 6 2012-07-01 2012-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-4 Table F-4 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  16. 40 CFR Table F-4 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Coarse Aerosol Size Distribution

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 5 2010-07-01 2010-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-4 Table F-4 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  17. 40 CFR Table F-6 to Subpart F of... - Estimated Mass Concentration Measurement of PM2.5 for Idealized Fine Aerosol Size Distribution

    Code of Federal Regulations, 2010 CFR

    2010-07-01

    ... 40 Protection of Environment 5 2010-07-01 2010-07-01 false Estimated Mass Concentration... Equivalent Methods for PM2.5 Pt. 53, Subpt. F, Table F-6 Table F-6 to Subpart F of Part 53—Estimated Mass... (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  18. INDOOR CONCENTRATION MODELING OF AEROSOL STRONG ACIDITY

    EPA Science Inventory

    A model for estimating indoor concentrations of acid aerosol was applied to data collected during the summer of 1989, in a densely populated location in New Jersey. he model, from a study of a semi-rural community in Pennsylvania, was used to estimate indoor concentrations of aer...

  19. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Croft, B.; Lohmann, U.; Martin, R. V.; Stier, P.; Wurzler, S.; Feichter, J.; Hoose, C.; Heikkilä, U.; van Donkelaar, A.; Ferrachat, S.

    2009-10-01

    A diagnostic nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. Sensitivity studies are presented, which compare aerosol concentrations, and deposition between a variety of in-cloud scavenging approaches, including prescribed fractions, several diagnostic schemes, and a prognostic aerosol cloud processing treatment that passes aerosol in-droplet and in-ice crystal concentrations between model time steps. For one sensitivity study, assuming 100% of the in-cloud aerosol is scavenged into the cloud droplets and ice crystals, the annual global mean accumulation mode number burden is decreased by 65%, relative to a simulation with prognostic aerosol cloud processing. Diagnosing separate nucleation scavenging ratios for aerosol number and mass distributions, as opposed to equating the aerosol mass scavenging to the number scavenging ratios, reduces the annual global mean sulfate burden by near to 10%. The annual global mean sea salt burden is 30% lower for the diagnostic approach, which does not carry aerosol in-droplet and in-crystal concentrations between model time-steps as compared to the prognostic scheme. Implementation of in-cloud impaction scavenging reduced the annual, global mean black carbon burden by 30% for the prognostic aerosol cloud processing scheme. Better agreement with observations of black carbon profiles from aircraft (changes near to one order of magnitude for mixed phase clouds), 210Pb surface layer concentrations and wet deposition, and the geographic distribution of aerosol optical depth are found for the new diagnostic scavenging as compared to prescribed ratio scavenging scheme of the standard ECHAM

  20. Investigating Types and Sources of Organic Aerosol in Rocky Mountain National Park Using Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L.

    2011-12-01

    The Rocky Mountain Atmospheric Nitrogen and Sulfur Study (RoMANS) focuses on identifying pathways and sources of nitrogen deposition in Rocky Mountain National Park (RMNP). Past work has combined measurements from a range of instrumentation such as annular denuders, PILS-IC, Hi-Vol samplers, and trace gas analyzers. Limited information from early RoMANS campaigns is available regarding organic aerosol. While prior measurements have produced a measure of total organic carbon mass, high time resolution measures of organic aerosol concentration and speciation are lacking. One area of particular interest is characterizing the types, sources, and amounts of organic nitrogen aerosol. Organic nitrogen measurements in RMNP wet deposition reveal a substantial contribution to the total reactive nitrogen deposition budget. In this study an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed in summer 2010 at RMNP to investigate organic aerosol composition and its temporal variability. The species timeline and diurnal species variations are combined with meteorological data to investigate local transport events and chemistry; transport from the Colorado Front Range urban corridor appears to be more significant for inorganic species than for the overall organic aerosol mass. Considerable variation in organic aerosol concentration is observed (0.5 to 20 μg/m3), with high concentration episodes lasting between hours and two days. High resolution AMS data are analyzed for organic aerosol, including organic nitrogen species that might be expected from local biogenic emissions, agricultural activities, and secondary reaction products of combustion emissions. Positive matrix factorization reveals that semi-volatile oxidized OA, low-volatility oxidized OA, and biomass burning OA comprise most organic mass; the diurnal profile of biomass burning OA peaks at four and nine pm and may arise from local camp fires, while constant concentrations of

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

    PubMed

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

    2009-03-01

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

  2. Relating Aerosol Mass and Optical Depth in the Summertime Continental Boundary Layer

    NASA Astrophysics Data System (ADS)

    Brock, C. A.; Wagner, N.; Middlebrook, A. M.; Attwood, A. R.; Washenfelder, R. A.; Brown, S. S.; McComiskey, A. C.; Gordon, T. D.; Welti, A.; Carlton, A. G.; Murphy, D. M.

    2014-12-01

    Aerosol optical depth (AOD), the column-integrated ambient aerosol light extinction, is determined from satellite and ground-based remote sensing measurements. AOD is the parameter most often used to validate earth system model simulations of aerosol mass. Relating aerosol mass to AOD, however, is problematic due to issues including aerosol water uptake as a function of relative humidity (RH) and the complicated relationship between aerosol physicochemical properties and light extinction. Measurements of aerosol microphysical, chemical, and optical properties help to constrain the relationship between aerosol mass and optical depth because aerosol extinction at ambient RH is a function of the abundance, composition and size distribution of the aerosol. We use vertical profiles of humidity and dry aerosol extinction observed in the southeastern United States (U.S.) to examine the relationship between submicron aerosol mass concentration and extinction at ambient RH. We show that the κ-Köhler parameterization directly, and without additional Mie calculations, describes the change in extinction with varying RH as a function of composition for both aged aerosols typical of the polluted summertime continental boundary layer and the biomass burning aerosols we encountered. We calculate how AOD and the direct radiative effect in the eastern U.S. have likely changed due to trends in aerosol composition in recent decades. We also examine the sensitivity of AOD to the RH profile and to aerosol composition, size distribution and abundance.

  3. Intercomparison of aerosol instruments: number concentration

    SciTech Connect

    Knutson, E O; Sinclair, D; Tu, K W; Hinchliffe, L; Franklin, H

    1982-05-01

    An intercomparison of aerosol instruments conducted February 23-27, 1981, at the Environmental Measurements Laboratory (EML) focused on five instruments: the Pollak and TSI condensation nucleus counters; the Active Scattering Aerosol Spectrometer (ASAS-X); and two aerosol electrometers. Test aerosols of sodium chloride and ammonium fluorescein generated by nebulization/electrostatic classification were used to obtain 195 lines of comparison data. Concentrations measured by the ASAS-X and the TSI aerosol electrometer averaged respectively 1.388 and 1.581 times that measured by the Pollak. These ratios were very stable during the week and there was little effect of particle size or material. Most other comparisons were equally stable. However, a review of past work at EML and elsewhere led to the disturbing conclusion that these ratios may change from year to year, or from season to season. A filter sample was taken from microscopy, concurrent with readings from the ASAS-X and the TSI condensation nucleus counters. In this sample, the two instruments differed by 20%. Within its 20% uncertainty, the filter result matched both the TSI and ASAS-X readings.

  4. A new method for estimating aerosol mass flux in the urban surface layer using LAS technology

    NASA Astrophysics Data System (ADS)

    Yuan, Renmin; Luo, Tao; Sun, Jianning; Liu, Hao; Fu, Yunfei; Wang, Zhien

    2016-04-01

    Atmospheric aerosol greatly influences human health and the natural environment, as well as the weather and climate system. Therefore, atmospheric aerosol has attracted significant attention from society. Despite consistent research efforts, there are still uncertainties in understanding its effects due to poor knowledge about aerosol vertical transport caused by the limited measurement capabilities of aerosol mass vertical transport flux. In this paper, a new method for measuring atmospheric aerosol vertical transport flux is developed based on the similarity theory of surface layer, the theory of light propagation in a turbulent atmosphere, and the observations and studies of the atmospheric equivalent refractive index (AERI). The results show that aerosol mass flux can be linked to the real and imaginary parts of the atmospheric equivalent refractive index structure parameter (AERISP) and the ratio of aerosol mass concentration to the imaginary part of the AERI. The real and imaginary parts of the AERISP can be measured based on the light-propagation theory. The ratio of the aerosol mass concentration to the imaginary part of the AERI can be measured based on the measurements of aerosol mass concentration and visibility. The observational results show that aerosol vertical transport flux varies diurnally and is related to the aerosol spatial distribution. The maximum aerosol flux during the experimental period in Hefei City was 0.017 mg m-2 s-1, and the mean value was 0.004 mg m-2 s-1. The new method offers an effective way to study aerosol vertical transport in complex environments.

  5. Indoor concentration modeling of aerosol strong acidity

    SciTech Connect

    Zelenka, M.; Waldman, J.; Suh, H.; Koutrakis, P.

    1993-01-01

    A model for estimating indoor concentrations of acid aerosol was applied to data collected during the summer of 1989, in a densely populated location in New Jersey. The model, from a study of a semi-rural community in Pennsylvania, was used to estimate indoor concentrations of aerosol strong acidity (H+) at an elderly care residence in suburban New Jersey. The purpose of the present work is to assess the applicability of the model for predicting H+ exposures in a suburban environment and to evaluate the models performance for daytime and nighttime periods. Indoor and outdoor samples were taken at an elderly care home between June 20 and July 30, 1989. The indoor and outdoor monitoring schedule collected two 12-h samples per day. Samples were taken with the Indoor Denuder Sampler (IDS). Samples were analyzed for indoor and outdoor concentrations of aerosol strong acidity (H+), ammonia (NH3), and anion determination. The model generally underestimated the indoor H+ concentration. Slight improvement was seen in the model estimate of H+ for the nighttime period (7:00 pm to 7:00 am, local time). The model applied to the site in New Jersey did not predict the indoor H+ concentrations as well as it did for the experiment from which it was developed.

  6. Ambient aerosol analysis using aerosol-time-of-flight mass spectrometry

    SciTech Connect

    Prather, K.A.; Noble, C.A.; Liu, D.Y.; Silva, P.J.; Fergenson, D.F.

    1996-10-01

    We have recently developed a technique, Aerosol-Time-of-Flight Mass Spectrometry (ATOFMS), which is capable of real-time determination of the aerodynamic size and chemical composition of individual aerosol particles. In order to obtain such information, the techniques of aerodynamic particle sizing and time-of-flight mass spectrometry are combined in a single instrument. ATOFMS is being used for the direct analysis of ambient aerosols with the goal of establishing correlations between particle size and chemical composition. Currently, measurements are being made to establish potential links between the presence of particular types of particles with such factors as the time of day, weather conditions, and concentration levels of gaseous smog components such as NO{sub x} and ozone. This data will be used to help establish a better understanding of tropospheric gas-aerosol processes. This talk will discuss the operating principles of ATOFMS as well as present the results of ambient analysis studies performed in our laboratory.

  7. Characterization of urban aerosol using aerosol mass spectrometry and proton nuclear magnetic resonance spectroscopy

    NASA Astrophysics Data System (ADS)

    Cleveland, M. J.; Ziemba, L. D.; Griffin, R. J.; Dibb, J. E.; Anderson, C. H.; Lefer, B.; Rappenglück, B.

    2012-07-01

    Particulate matter was measured during August and September of 2006 in Houston as part of the Texas Air Quality Study II Radical and Aerosol Measurement Project. Aerosol size and composition were determined using an Aerodyne quadrupole aerosol mass spectrometer. Aerosol was dominated by sulfate (4.1 ± 2.6 μg m-3) and organic material (5.5 ± 4.0 μg m-3), with contributions of organic material from both primary (˜32%) and secondary (˜68%) sources. Secondary organic aerosol appears to be formed locally. In addition, 29 aerosol filter samples were analyzed using proton nuclear magnetic resonance (1H NMR) spectroscopy to determine relative concentrations of organic functional groups. Houston aerosols are less oxidized than those observed elsewhere, with smaller relative contributions of carbon-oxygen double bonds. These particles do not fit 1H NMR source apportionment fingerprints for identification of secondary, marine, and biomass burning organic aerosol, suggesting that a new fingerprint for highly urbanized and industrially influenced locations be established.

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

    SciTech Connect

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

    2009-03-01

    During the Capstone Depleted Uranium (DU) Aerosol Study, aerosols containing depleted uranium were produced inside unventilated armored vehicles (i.e., Abrams tanks and Bradley Fighting Vehicles) by perforation with large-caliber DU penetrators. These aerosols were collected and characterized, and the data were subsequently used to assess human health risks to personnel exposed to DU aerosols. The DU content of each aerosol sample was first quantified by radioanalytical methods, and selected samples, primarily those from the cyclone separator grit chambers, were analyzed radiochemically. Deposition occurred inside the vehicles as particles settled on interior surfaces. Settling rates of uranium from the aerosols were evaluated using filter cassette samples that collected aerosol as total mass over eight sequential time intervals. A moving filter was used to collect aerosol samples over time particularly within the first minute after the shot. The results demonstrate that the peak uranium concentration in the aerosol occurred in the first 10 s, and the concentration decreased in the Abrams tank shots to about 50% within 1 min and to less than 2% 30 min after perforation. In the Bradley vehicle, the initial (and maximum) uranium concentration was lower than those observed in the Abrams tank and decreased more slowly. Uranium mass concentrations in the aerosols as a function of particle size were evaluated using samples collected in the cyclone samplers, which collected aerosol continuously for 2 h post perforation. The percentages of uranium mass in the cyclone separator stages from the Abrams tank tests ranged from 38% to 72% and, in most cases, varied with particle size, typically with less uranium associated with the smaller particle sizes. Results with the Bradley vehicle ranged from 18% to 29% and were not specifically correlated with particle size.

  9. Atmospheric pressure flow reactor / aerosol mass spectrometer studies of tropospheric aerosol nucleat and growth kinetics. Final report, June, 2001

    SciTech Connect

    Worsnop, Douglas R.

    2001-06-01

    The objective of this program was to determine the mechanisms and rates of growth and transformation and growth processes that control secondary aerosol particles in both the clear and polluted troposphere. The experimental plan coupled an aerosol mass spectrometer (AMS) with a chemical ionization mass spectrometer to provide simultaneous measurement of condensed and particle phases. The first task investigated the kinetics of tropospheric particle growth and transformation by measuring vapor accretion to particles (uptake coefficients, including mass accommodation coefficients and heterogeneous reaction rate coefficients). Other work initiated investigation of aerosol nucleation processes by monitoring the appearance of submicron particles with the AMS as a function of precursor gas concentrations. Three projects were investigated during the program: (1) Ozonolysis of oleic acid aerosols as model of chemical reactivity of secondary organic aerosol; (2) Activation of soot particles by measurement deliquescence in the presence of sulfuric acid and water vapor; (3) Controlled nucleation and growth of sulfuric acid aerosols.

  10. Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic-Mediterranean 2008 Scholar Ship cruise (Part I): Particle mass concentrations, size ratios, and main chemical components

    NASA Astrophysics Data System (ADS)

    Pérez, Noemí; Moreno, Teresa; Querol, Xavier; Alastuey, Andrés; Bhatia, Ravinder; Spiro, Baruch; Hanvey, Melanie

    2010-07-01

    We report on ambient atmospheric aerosols present at sea during the Atlantic-Mediterranean voyage of Oceanic II (The Scholar Ship) in spring 2008. A record was obtained of hourly PM 10, PM 2.5, and PM 1 particle size fraction concentrations and 24-h filter samples for chemical analysis which allowed for comparison between levels of crustal particles, sea spray, total carbon, and secondary inorganic aerosols. On-board monitoring was continuous from the equatorial Atlantic to the Straits of Gibraltar, across the Mediterranean to Istanbul, and back via Lisbon to the English Channel. Initially clean air in the open Atlantic registered PM 10 levels <10 μg m -3 but became progressively polluted by increasingly coarse PM as the ship approached land. Away from major port cities, the main sources of atmospheric contamination identified were dust intrusions from North Africa (NAF), smoke plumes from biomass burning in sub-Saharan Africa and Russia, industrial sulphate clouds and other regional pollution sources transported from Europe, sea spray during rough seas, and plumes emanating from islands. Under dry NAF intrusions PM 10 daily mean levels averaged 40-60 μg m -3 (30-40 μg m -3 PM 2.5; c. 20 μg m -3 PM 1), peaking briefly to >120 μg m -3 (hourly mean) when the ship passed through curtains of higher dust concentrations amassed at the frontal edge of the dust cloud. PM 1/PM 10 ratios ranged from very low during desert dust intrusions (0.3-0.4) to very high during anthropogenic pollution plume events (0.8-1).

  11. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGESBeta

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-03-02

    We used an electrostatic size classification technique to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Moreover, we counted size-segregated particles with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized bymore » the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10-5 to 10-11. Free molecular heat and mass transfer theory was

  12. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-05-01

    An electrostatic size classification technique was used to segregate particles of known composition prior to being injected into an inductively coupled plasma mass spectrometer (ICP-MS). Size-segregated particles were counted with a condensation nuclei counter as well as sampled with an ICP-MS. By injecting particles of known size, composition, and aerosol concentration into the ICP-MS, efficiencies of the order of magnitude aerosol detection were calculated, and the particle size dependencies for volatile and refractory species were quantified. Similar to laser ablation ICP-MS, aerosol detection efficiency was defined as the rate at which atoms were detected in the ICP-MS normalized by the rate at which atoms were injected in the form of particles. This method adds valuable insight into the development of technologies like laser ablation ICP-MS where aerosol particles (of relatively unknown size and gas concentration) are generated during ablation and then transported into the plasma of an ICP-MS. In this study, we characterized aerosol detection efficiencies of volatile species gold and silver along with refractory species aluminum oxide, cerium oxide, and yttrium oxide. Aerosols were generated with electrical mobility diameters ranging from 100 to 1000 nm. In general, it was observed that refractory species had lower aerosol detection efficiencies than volatile species, and there were strong dependencies on particle size and plasma torch residence time. Volatile species showed a distinct transition point at which aerosol detection efficiency began decreasing with increasing particle size. This critical diameter indicated the largest particle size for which complete particle detection should be expected and agreed with theories published in other works. Aerosol detection efficiencies also displayed power law dependencies on particle size. Aerosol detection efficiencies ranged from 10- 5 to 10- 11. Free molecular heat and mass transfer theory was applied, but

  13. Aerosol and cloud droplet number concentrations observed in marine stratocumulus

    SciTech Connect

    Vong, R.J.; Covert, D.S.

    1995-12-01

    The relationship between measurements of cloud droplet number concentration and cloud condensation nuclei (CCN) concentration, as inferred from aerosol size spectra, was investigated at a {open_quote}clean air{close_quote}, marine site (Cheeka Peak) located near the coast of the Olympic Peninsula in Washington State. Preliminary results demonstrated that cloud droplet number increased and droplet diameter decreased as aerosol number concentration (CCN) increased. These results support predictions of a climate cooling due to any future increases in marine aerosol concentrations.

  14. Influences of in-cloud aerosol scavenging parameterizations on aerosol concentrations and wet deposition in ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Croft, B.; Lohmann, U.; Martin, R. V.; Stier, P.; Wurzler, S.; Feichter, J.; Hoose, C.; Heikkilä, U.; van Donkelaar, A.; Ferrachat, S.

    2010-02-01

    A diagnostic cloud nucleation scavenging scheme, which determines stratiform cloud scavenging ratios for both aerosol mass and number distributions, based on cloud droplet, and ice crystal number concentrations, is introduced into the ECHAM5-HAM global climate model. This scheme is coupled with a size-dependent in-cloud impaction scavenging parameterization for both cloud droplet-aerosol, and ice crystal-aerosol collisions. The aerosol mass scavenged in stratiform clouds is found to be primarily (>90%) scavenged by cloud nucleation processes for all aerosol species, except for dust (50%). The aerosol number scavenged is primarily (>90%) attributed to impaction. 99% of this impaction scavenging occurs in clouds with temperatures less than 273 K. Sensitivity studies are presented, which compare aerosol concentrations, burdens, and deposition for a variety of in-cloud scavenging approaches: prescribed fractions, a more computationally expensive prognostic aerosol cloud processing treatment, and the new diagnostic scheme, also with modified assumptions about in-cloud impaction and nucleation scavenging. Our results show that while uncertainties in the representation of in-cloud scavenging processes can lead to differences in the range of 20-30% for the predicted annual, global mean aerosol mass burdens, and near to 50% for accumulation mode aerosol number burden, the differences in predicted aerosol mass concentrations can be up to one order of magnitude, particularly for regions of the middle troposphere with temperatures below 273 K where mixed and ice phase clouds exist. Different parameterizations for impaction scavenging changed the predicted global, annual mean number removal attributed to ice clouds by seven-fold, and the global, annual dust mass removal attributed to impaction by two orders of magnitude. Closer agreement with observations of black carbon profiles from aircraft (increases near to one order of magnitude for mixed phase clouds), mid

  15. Secondary Ion Mass Spectrometry of Environmental Aerosols

    SciTech Connect

    Gaspar, Daniel J.; Cliff, John B.

    2010-08-01

    Atmospheric particles influence many aspects of climate, air quality and human health. Understanding the composition, chemistry and behavior of atmospheric aerosols is a key remaining challenge in improving climate models. Furthermore, particles may be traced back to a particular source based on composition, stable isotope ratios, or the presence of particular surface chemistries. Finally, the characterization of atmospheric particles in the workplace plays an important role in understanding the potential for exposure and environmental and human health effects to engineered and natural nanoscale particles. Secondary ion mass spectrometry (SIMS) is a useful tool in determining any of several aspects of the structure, composition and chemistry of these particles. Often used in conjunction with other surface analysis and electron microscopy methods, SIMS has been used to determine or confirm reactions on and in particles, the presence of particular organic species on the surface of atmospheric aerosols and several other interesting and relevant findings. Various versions of SIMS instruments – dynamic SIMS, time of flight secondary ion mass spectrometry or TOF-SIMS, nanoSIMS – have been used to determine specific aspects of aerosol structure and chemistry. This article describes the strengths of each type of SIMS instrument in the characterization of aerosols, along with guidance on sample preparation, specific characterization specific to the particular information sought in the analysis. Examples and guidance are given for each type of SIMS analysis.

  16. Anthropogenic sulfate and organic aerosols, CCN, and cloud project concentration at a marine site

    SciTech Connect

    Novakao, T.; Rivera-Carpio, C.; Penner, J.E.; Rogers, C.F.

    1993-10-01

    The need to establish the relationships between the number concentration of cloud droplets, cloud condensation nuclei (CCN), and the mass concentrations of major aerosol species has been heightened by the results of recent modeling studies suggesting that anthropogenic sulfate and biomass smoke aerosols may cause a globally averaged climate forcing comparable in magnitude but opposite in sign to the forcing due to ``greenhouse`` gases. In this paper we present the results of measurements of nonseasalt (nss) sulfate and organic carbon mass concentrations and mass size distributions, CCN, and cloud droplet number concentrations obtained in 1991 and 1992 on El Yunque peak, Puerto Rico . This peak (18{degree}19N, 65{degree}45W; elevation 1000 m) is located the eastern end of the island, directly exposed to the ocean winds and frequently covered with clouds. Our results show that although CCN number concentrations (measured at 0.5% supersaturation) and nss sulfate mass concentrations are significantly correlated at this site, estimates based on measured mass size distributions of organic and sulfate aerosols indicate that the organic aerosols may account for the majority of CCN number concentrations. Droplet concentrations in the cumulus clouds do not show a discernible trend with nss sulfate mass concentrations. In stratocumulus clouds a small increase in droplet concentrations with nss sulfate mass concentrations was observed.

  17. Estimation of aerosol mass scattering efficiencies under high mass loading: case study for the megacity of Shanghai, China.

    PubMed

    Cheng, Zhen; Jiang, Jingkun; Chen, Changhong; Gao, Jian; Wang, Shuxiao; Watson, John G; Wang, Hongli; Deng, Jianguo; Wang, Buying; Zhou, Min; Chow, Judith C; Pitchford, Marc L; Hao, Jiming

    2015-01-20

    Aerosol mass scattering efficiency (MSE), used for the scattering coefficient apportionment of aerosol species, is often studied under the condition of low aerosol mass loading in developed countries. Severe pollution episodes with high particle concentration frequently happened in eastern urban China in recent years. Based on synchronous measurement of aerosol physical, chemical, and optical properties at the megacity of Shanghai for two months during autumn 2012, we studied MSE characteristics at high aerosol mass loading. Their relationships with mass concentrations and size distributions were examined. It was found that MSE values from the original US IMPROVE algorithm could not represent the actual aerosol characteristics in eastern China. It results in an underestimation of the measured ambient scattering coefficient by 36%. MSE values in Shanghai were estimated to be 3.5 ± 0.55 m(2)/g for ammonia sulfate, 4.3 ± 0.63 m(2)/g for ammonia nitrate, and 4.5 ± 0.73 m(2)/g for organic matter, respectively. MSEs for three components increased rapidly with increasing mass concentration in low aerosol mass loading, then kept at a stable level after a threshold mass concentration of 12–24 μg/m(3). During severe pollution episodes, particle growth from an initial peak diameter of 200–300 nm to a peak diameter of 500–600 nm accounts for the rapid increase in MSEs at high aerosol mass loading, that is, particle diameter becomes closer to the wavelength of visible lights. This study provides insights of aerosol scattering properties at high aerosol concentrations and implies the necessity of MSE localization for extinction apportionment, especially for the polluted regions. PMID:25495050

  18. Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice

    NASA Astrophysics Data System (ADS)

    Humphries, R. S.; Klekociuk, A. R.; Schofield, R.; Keywood, M.; Ward, J.; Wilson, S. R.

    2015-10-01

    The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3) concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm-3 - higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol concentrations and

  19. ACTRIS ACSM intercomparison - Part I: Reproducibility of concentration and fragment results from 13 individual Quadrupole Aerosol Chemical Speciation Monitors (Q-ACSM) and consistency with Time-of-Flight ACSM (ToF-ACSM), High Resolution ToF Aerosol Mass Spectrometer (HR-ToF-AMS) and other co-located instruments

    NASA Astrophysics Data System (ADS)

    Crenn, V.; Sciare, J.; Croteau, P. L.; Verlhac, S.; Fröhlich, R.; Belis, C. A.; Aas, W.; Äijälä, M.; Alastuey, A.; Artiñano, B.; Baisnée, D.; Bonnaire, N.; Bressi, M.; Canagaratna, M.; Canonaco, F.; Carbone, C.; Cavalli, F.; Coz, E.; Cubison, M. J.; Esser-Gietl, J. K.; Green, D. C.; Gros, V.; Heikkinen, L.; Herrmann, H.; Lunder, C.; Minguillón, M. C.; Močnik, G.; O'Dowd, C. D.; Ovadnevaite, J.; Petit, J.-E.; Petralia, E.; Poulain, L.; Priestman, M.; Riffault, V.; Ripoll, A.; Sarda-Estève, R.; Slowik, J. G.; Setyan, A.; Wiedensohler, A.; Baltensperger, U.; Prévôt, A. S. H.; Jayne, J. T.; Favez, O.

    2015-07-01

    As part of the European ACTRIS project, the first large Quadrupole Aerosol Chemical Speciation Monitor (Q-ACSM) intercomparison study was conducted in the region of Paris for three weeks during the late fall-early winter period (November-December 2013). The first week was dedicated to tuning and calibration of each instrument whereas the second and third were dedicated to side-by-side comparison in ambient conditions with co-located instruments providing independent information on submicron aerosol optical, physical and chemical properties. Near real-time measurements of the major chemical species (organic matter, sulfate, nitrate, ammonium and chloride) in the non-refractory submicron aerosols (NR-PM1) were obtained here from 13 Q-ACSM. The results show that these instruments can produce highly comparable and robust measurements of the NR-PM1 total mass and its major components. Taking the median of the 13 Q-ACSM as a reference for this study, strong correlations (r2 > 0.9) were observed systematically for each individual ACSM across all chemical families except for chloride for which three ACSMs showing weak correlations partly due to the very low concentrations during the study. Reproducibility expanded uncertainties of Q-ACSM concentration measurements were determined using appropriate methodologies defined by the International Standard Organization (ISO 17025) and were found to be of 9, 15, 19, 28 and 36 % for NR-PM1, nitrate, organic matter, sulfate and ammonium respectively. However, discrepancies were observed in the relative concentrations of the constituent mass fragments for each chemical component. In particular, significant differences were observed for the organic fragment at mass-to-charge ratio 44, which is a key parameter describing the oxidation state of organic aerosol. Following this first major intercomparison exercise of a large number of ACSMs, detailed intercomparison results are presented as well as a discussion of some recommendations

  20. Organic Aerosols in Rural and Remote Atmospheric Environments: Insights from Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Zhang, Q.; Jimenez, J.; Ulbrich, I.; Dunlea, E.; Decarlo, P.; Huffman, A.; Allan, J.; Coe, H.; Alfarra, R.; Canagaratna, M.; Onasch, T.; Jayne, J.; Worsnop, D.; Takami, A.; Miyoshi, T.; Shimono, A.; Hatakeyama, S.; Weimer, S.; Demerjian, K.; Drewnick, F.; Schneider, J.; Middlebrook, A.; Bahreini, R.; Cotrell, L.; Griffin, R.; Leaitch, R.; Li, S.; Hayden, K.; Rautiainen, J.

    2006-12-01

    Organic matter usually accounts for a large fraction of the fine particle mass in rural and remote atmospheres. However, little is known about the sources and properties of this material. Here we report findings on the characteristics and the major types of organic aerosols (OA) in urban downwind, high elevation, forested, and marine atmospheres based on analyses of more than 20 highly time resolved AMS datasets sampled from various locations in the mid-latitude Northern Hemisphere. Organic aerosol components are extracted from these datasets using a custom multiple component mass spectral analysis technique and the Positive Matrix Factorization (PMF) method. These components are evaluated according to their extracted mass spectra and correlations to aerosol species, such as sulfate, nitrate, and elemental carbon, and gas-phase tracer compounds, such as CO and NOx. We have identified a hydrocarbon-like organic aerosol (HOA) component similar in mass spectra to the hydrocarbon substances observed at urban locations. We have also identified several oxygenated OA (OOA) components that show different fragmentation patterns and oxygen to carbon ratios in their mass spectra. Two OOA components a highly oxygenated that has mass spectrum resembling that of fulvic acid (a model compound representative for highly processed/oxidized organics in the environment) and a less oxygenated OOA component, whose spectrum is dominated with ions that are mainly associated with carbonyls and alcohols, are very frequently observed at various rural/remote sites. The oxygenated OOA component is more prevalent at downwind sites influenced by urban transport and the less oxygenated shows correlation to biogenic chamber OA at some locations. Compared to the total OOA concentration, HOA is generally very small and accounts for < 10% of the total OA mass at rural/remote sites. The comparisons between the concentrations of HOA and primary OA (POA) that would be predicted according to inert

  1. DESIGN AND PERFORMANCE OF AN AEROSOL MASS DISTRIBUTION MONITOR

    EPA Science Inventory

    An aerosol mass monitor has been built to measure the masses of non-volatile aerosols in the range of 0.05 to 5 micrometers aerodynamic particle diameter. The instrument consists of a newly designed spiral duct aerosol centrifuge equipped with highly sensitive quartz sensors for ...

  2. Effects of aerosol organics on cloud condensation nucleus (CCN) concentration and first indirect aerosol effect

    SciTech Connect

    Wang, J. X.; Lee, Y.- N.; Daum, Peter H.; Jayne, John T.; Alexander, M. L.

    2008-11-03

    Abstract. Aerosol microphysics, chemical composition, and CCN properties were measured on the Department of Energy Gulfstream-1 aircraft during the Marine Stratus/ Stratocumulus Experiment (MASE) conducted over the coastal waters between Point Reyes National Seashore and Monterey Bay, California, in July 2005. Aerosols measured during MASE included free tropospheric aerosols, marine boundary layer aerosols, and aerosols with high organic concentration within a thin layer above the cloud. Closure analysis was carried out for all three types of aerosols by comparing the measured CCN concentrations at 0.2% supersaturation to those predicted based on size distribution and chemical composition using K¨ohler theory. The effect of aerosol organic species on predicted CCN concentration was examined using a single hygroscopicity parameterization.

  3. Laboratory and field measurements of organic aerosols with the photoionization aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Dreyfus, Matthew A.

    Analytical methods developed to sample and characterize ambient organic aerosols often face the trade-off between long sampling times and the loss of detailed information regarding specific chemical species present. The soft, universal ionization scheme of the Photoionization Aerosol Mass Spectrometer (PIAMS) allows for identification of various chemical compounds by a signature ion, often the molecular ion. The goal of this thesis work is to apply PIAMS to both laboratory and field experiments to answer questions regarding the formation, composition, and behavior of organic aerosols. To achieve this goal, a variety of hardware and software upgrades were administered to PIAMS to optimize the instrument. Data collection and processing software were either refined or built from the ground up to simplify difficult or monotonous tasks. Additional components were added to PIAMS with the intent to automate the instrument, enhance the results, and make the instrument more rugged and user-friendly. These changes, combined with the application of an external particle concentration system (mini-Versatile Aerosol Concentration Enrichment System, m-VACES), allowed PIAMS to be suitable for field measurements of organic aerosols. Two such field campaigns were completed, both at the State of Delaware Air Quality Monitoring Site in Wilmington, Delaware: a one week period in June, 2006, and an 18 day period in October and November of 2007. A sampling method developed was capable of collecting sufficient ambient organic aerosol and analyzing it with a time resolution of 3.5 minutes. Because of this method, short term concentration changes of individual species can be tracked. Combined with meteorological data, the behavior of these species can be analyzed as a function of time or wind direction. Many compounds are found at enhanced levels during the evening/night-time hours; potentially due to the combined effects of temperature inversion, and fresh emissions in a cooler environment

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

    NASA Astrophysics Data System (ADS)

    Hearn, John D.; Smith, Geoffrey D.

    2006-12-01

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

  5. Mass size distributions of elemental aerosols in industrial area

    PubMed Central

    Moustafa, Mona; Mohamed, Amer; Ahmed, Abdel-Rahman; Nazmy, Hyam

    2014-01-01

    Outdoor aerosol particles were characterized in industrial area of Samalut city (El-minia/Egypt) using low pressure Berner cascade impactor as an aerosol sampler. The impactor operates at 1.7 m3/h flow rate. Seven elements were investigated including Ca, Ba, Fe, K, Cu, Mn and Pb using atomic absorption technique. The mean mass concentrations of the elements ranged from 0.42 ng/m3 (for Ba) to 89.62 ng/m3 (for Fe). The mass size distributions of the investigated elements were bi-modal log normal distribution corresponding to the accumulation and coarse modes. The enrichment factors of elements indicate that Ca, Ba, Fe, K, Cu and Mn are mainly emitted into the atmosphere from soil sources while Pb is mostly due to anthropogenic sources. PMID:26644919

  6. Derivation of Aerosol Columnar Mass from MODIS Optical Depth

    NASA Technical Reports Server (NTRS)

    Gasso, Santiago; Hegg, Dean A.

    2003-01-01

    In order to verify performance, aerosol transport models (ATM) compare aerosol columnar mass (ACM) with those derived from satellite measurements. The comparison is inherently indirect since satellites derive optical depths and they use a proportionality constant to derive the ACM. Analogously, ATMs output a four dimensional ACM distribution and the optical depth is linearly derived. In both cases, the proportionality constant requires a direct intervention of the user by prescribing the aerosol composition and size distribution. This study introduces a method that minimizes the direct user intervention by making use of the new aerosol products of MODIS. A parameterization is introduced for the derivation of columnar aerosol mass (AMC) and CCN concentration (CCNC) and comparisons between sunphotometer, MODIS Airborne Simulator (MAS) and in-measurements are shown. The method still relies on the scaling between AMC and optical depth but the proportionality constant is dependent on the MODIS derived r$_{eff}$,\\eta (contribution of the accumulation mode radiance to the total radiance), ambient RH and an assumed constant aerosol composition. The CCNC is derived fkom a recent parameterization of CCNC as a function of the retrieved aerosol volume. By comparing with in-situ data (ACE-2 and TARFOX campaigns), it is shown that retrievals in dry ambient conditions (dust) are improved when using a proportionality constant dependent on r$ {eff}$ and \\eta derived in the same pixel. In high humidity environments, the improvement inthe new method is inconclusive because of the difficulty in accounting for the uneven vertical distribution of relative humidity. Additionally, two detailed comparisons of AMC and CCNC retrieved by the MAS algorithm and the new method are shown. The new method and MAS retrievals of AMC are within the same order of magnitude with respect to the in-situ measurements of aerosol mass. However, the proposed method is closer to the in-situ measurements than

  7. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2015-01-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9% and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/z 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ~10 years of meteorological, particle composition, and fire data.

  8. Investigating types and sources of organic aerosol in Rocky Mountain National Park using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Schurman, M. I.; Lee, T.; Sun, Y.; Schichtel, B. A.; Kreidenweis, S. M.; Collett, J. L., Jr.

    2014-07-01

    The environmental impacts of atmospheric particles are highlighted in remote areas where visibility and ecosystem health can be degraded by even relatively low particle concentrations. Submicron particle size, composition, and source apportionment were explored at Rocky Mountain National Park using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer. This summer campaign found low average, but variable, particulate mass (PM) concentrations (max = 93.1 μg m-3, avg. = 5.13 ± 2.72 μg m-3) of which 75.2 ± 11.1% is organic. Low-volatility oxidized organic aerosol (LV-OOA, 39.3% of PM1 on average) identified using Positive Matrix Factorization appears to be mixed with ammonium sulfate (3.9 and 16.6% of mass, respectively), while semi-volatile OOA (27.6%) is correlated with ammonium nitrate (nitrate: 4.3%); concentrations of these mixtures are enhanced with upslope (SE) surface winds from the densely populated Front Range area, indicating the importance of transport. A local biomass burning organic aerosol (BBOA, 8.4%) source is suggested by mass spectral cellulose combustion markers (m/zs 60 and 73) limited to brief, high-concentration, polydisperse events (suggesting fresh combustion), a diurnal maximum at 22:00 local standard time (LST) when campfires were set at adjacent summer camps, and association with surface winds consistent with local campfire locations. The particle characteristics determined here represent typical summertime conditions at the Rocky Mountain site based on comparison to ∼10 years of meteorological, particle composition, and fire data.

  9. The effect of anthropogenic sulfate aerosols on marine cloud droplet concentrations

    NASA Astrophysics Data System (ADS)

    Novakov, T.; Rivera-Carpio, C.; Penner, J. E.; Rogers, C. F.

    1994-04-01

    Nonseasalt sulfate (nss SO42-) mass concentrations, cloud condensation nuclei (CCN) number concentrations, and cloud droplet concentrations in warm cumulus and stratocumulus clouds were simultaneously measured in situ in marine air masses on El Yunque peak in Puerto Rico. Our results show that CNN number concentrations (measured at 0.5% supersaturation) and nss SO42- mass concentrations (in the range of ˜ 400 1700ng m-342- mass concentrations (in the range of ˜ 300 1400ng m-3). In stratocumulus clouds, a small increase in droplet concentration with nss SO42- mass concentrations in the range of ˜ 300 1100ng m-3 was observed. We attribute the low sensitivities of the droplet number concentrations to nss SO42- mass concentrations to the entrainment/mixing processes in these clouds. The magnitudes of the empirically derived sensitivities are considerably lower than those assumed in recent assessments of the effect of anthropogenic sulfate aerosols on cloud albedo.

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

    SciTech Connect

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

    2011-02-15

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

  11. Aerosol chemical components in Alaska air masses: 1. Aged pollution

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    1991-12-01

    A 4-year Alaska chemical data set of aerosols or "dust" in the air clearly reveals a mixture of distinct aerosol components with different and interesting chemical composition, one or two being ascribed to pollution imported to Alaska by winds all the way from other continents. Of particular note is a strong chemical contrast between what we imagine to be highly scavenged, orographically lifted, northern Pacific air (Pacific marine air mass) and stagnant Arctic air (polar air mass), the latter containing seasonal average concentrations of between 2-4 times the concentration of the former, at least for pollution markers noncrustal vanadium, noncrustal manganese, arsenic, selenium, bromine, and antimony. The findings concur our old discovery that Arctic air is persistently polluted (Arctic haze), but Pacific air is relatively clean, in spite of the fact that Alaska is downwind of major pollution sources in the Orient. This is remarkable. In this the first of a two-part paper, we concentrate on the pollution component found primarily during incursion of Arctic polar air. Two major occurrences of visual haze with optical depths of approximately 0.2 and elevated aerosol concentration lasting about a month (spring 1985 and 1986) were affiliated with strong incoming transport of polar air, temperatures ranging from 10° to 20°C below normal (polar air) and air trajectory hindcasts leading back to industrial pollution sources in Eurasia. These long-range transport pollution events brought metal-rich aerosol of removal-resistant submicron particles. The size, chemistry, and meteorology all strongly suggest the presence of a well-aged (10-100 day) polluted air mass. An important implication is that in spring a large fraction of the Arctic polar air mass becomes charged with by-products of industrial pollution. In this multiyear chemical data set one finds a notable summer-winter contrast, changing by factors of 2 to 4 for pollution markers As, Se, Sb, and noncrustal

  12. 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.

  13. Aerosol Composition in the Los Angeles Basin Studied by High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Hayes, P. L.; Ortega, A. M.; Cubison, M.; Hu, W.; Toohey, D. W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Alvarez, S. L.; Rappenglueck, B.; Allan, J. D.; Taylor, J.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; De Gouw, J. A.; Massoli, P.; Zhang, X.; Weber, R.; Zhao, Y.; Cliff, S. S.; Wexler, A. S.; Isaacman, G. A.; Worton, D. R.; Kreisberg, N. M.; Hering, S. V.; Goldstein, A. H.; Jimenez, J. L.

    2011-12-01

    Atmospheric aerosols impact climate and health, but their sources and composition are poorly understood. To address this knowledge gap, a high-resolution aerosol mass spectrometer (AMS) and complementary instrumentation were deployed during the 2010 CalNex campaign to characterize aerosol composition in the Los Angeles (LA) area. Total mass concentrations as well as the species concentrations measured by the AMS compare well with most other instruments. Nitrate dominates in the mornings, but its concentration is reduced in the afternoon when organic aerosols (OA) increase and dominate. The diurnal variations in concentrations are strongly influenced by emission transport from the source-rich western basin. The average OA to enhanced CO ratio increases with photochemical age from 25 to 80 μg m-3 ppm-1, which indicates significant secondary OA (SOA) production and that a large majority of OA is secondary in aged air. The ratio values are similar to those from Mexico City as well as New England and the Mid-Atlantic States. Positive matrix factorization (PMF) is used to assess the concentrations of different OA components. The major OA classes are oxygenated OA (OOA, a surrogate for total SOA), and hydrocarbon-like OA (HOA, a surrogate for primary combustion OA). Several subclasses of OA are identified as well including diesel-influenced HOA (DI-HOA) and non-diesel HOA. DI-HOA exhibits low concentrations on Sundays consistent with the well-known weekday/weekend effect in LA. PMF analysis finds that OOA is 67% of the total OA concentration. A strong correlation between OOA and Ox (O3 + NO2) concentrations is observed with a slope of 0.15 that suggests the production of fresh SOA in Pasadena. Plotting the OA elemental ratios in a Van Krevelen diagram (H:C vs. O:C) yields a slope of -0.6, which is less steep than that observed in Riverside during the SOAR-2005 campaign. The difference in slopes may be attributed to the highly oxidized HOA present in Pasadena that is

  14. Process evaluation of sea salt aerosol concentrations at remote marine locations

    NASA Astrophysics Data System (ADS)

    Struthers, H.; Ekman, A. M.; Nilsson, E. D.

    2011-12-01

    Sea salt, an important natural aerosol, is generated by bubbles bursting at the surface of the ocean. Sea salt aerosol contributes significantly to the global aerosol burden and radiative budget and are a significant source of cloud condensation nuclei in remote marine areas (Monahan et al., 1986). Consequently, changes in marine aerosol abundance is expected to impact on climate forcing. Estimates of the atmospheric burden of sea salt aerosol mass derived from chemical transport and global climate models vary greatly both in the global total and the spatial distribution (Texor et al. 2006). This large uncertainty in the sea salt aerosol distribution in turn contributes to the large uncertainty in the current estimates of anthropogenic aerosol climate forcing (IPCC, 2007). To correctly attribute anthropogenic climate change and to veraciously project future climate, natural aerosols including sea salt must be understood and accurately modelled. In addition, the physical processes that determine the sea salt aerosol concentration are susceptible to modification due to climate change (Carslaw et al., 2010) which means there is the potential for feedbacks within the climate/aerosol system. Given the large uncertainties in sea salt aerosol modelling, there is an urgent need to evaluate the process description of sea salt aerosols in global models. An extremely valuable source of data for model evaluation is the long term measurements of PM10 sea salt aerosol mass available from a number of remote marine observation sites around the globe (including the GAW network). Sea salt aerosol concentrations at remote marine locations depend strongly on the surface exchange (emission and deposition) as well as entrainment or detrainment to the free troposphere. This suggests that the key parameters to consider in any analysis include the sea surface water temperature, wind speed, precipitation rate and the atmospheric stability. In this study, the sea salt aerosol observations

  15. Aerosol and CCN Concentrations under Extremely High DMS Levels over the North Atlantic Ocean

    NASA Astrophysics Data System (ADS)

    Deng, C.; Brooks, S. D.; Thornton, D. C.; Bell, T. G.; Saltzman, E. S.; De Bruyn, W. J.

    2013-12-01

    Despite numerous studies since the CLAW hypothesis was first suggested in 1987, the extent to which marine phytoplankton derived dimethyl sulfide (CH3SCH3, DMS) contributes to marine atmospheric aerosol populations and the ability of those aerosols to act as cloud condensation nuclei (CCN) remains unclear, especially over oceanic areas obviously influenced by continental sources. Here, we present data from a cruise aboard the R/V Knorr over the North Atlantic during June-July 2011which passed through areas of both high and low phytoplankton biomasses, as well as intermediate primary production bloom regions where extremely high DMS concentrations (over 1800 pptv) were observed. Continuous ambient measurements of aerosol concentration, cloud condensation nuclei (CCN) concentration, aerosol particle size distributions, and surface seawater and atmospheric dimethyl sulfide (DMS) concentrations were performed simultaneously during the three-week-cruise. Throughout the cruise, CCN concentrations were measured at a series of five supersaturation levels and used to derive the critical supersaturation required for aerosols to activate as CCN. Air masses have been classified into three different categories based on the 48-hr back trajectories, i.e., air mass influenced by continents, coasts and the open ocean. Aerosol concentrations have noticeably different patterns depending on the air mass paths. Continually high CCN and aerosol concentrations had been found to coincide with high DMS concentration over the open ocean, which may be explained by the nucleation and condensational growth in marine boundary layer (MBL) resulting from the oxidation products of DMS or primary aerosols from the sea surface. Calculation of DMS oxidation rates based on the variation of DMS in the lower atmosphere and sea-to-air flux measurement during the whole cruise verified that the influence of continental sources on marine atmosphere is significant during the majority of sample times

  16. Concentrations and sources of metals in the Antarctic Peninsula aerosol

    SciTech Connect

    Dick, A.L. )

    1991-07-01

    Aerosol samples were collected at a remote site near the east coast of the Antarctic Peninsula during the austral summer of 1984/85. Filter samples were analyzed for Al (as a crustal reference element), marine cations (Na, K, and Ca), heavy metals (Cd, Cu, Pb, and Zn), and sulfate using atomic absorption spectrometry, isotope dilution mass spectrometry, neutron activation analysis, and ion chromatography. Ultraclean sample collection and analysis procedures used to avoid sample contamination are described in detail here. Mean concentrations of heavy metals were found to be: Cd, 0.06 pg m{sup {minus}3}; Cu, 1.0 pg m{sup {minus}3}; Pb, 4.7 pg m{sup {minus}3}; and Zn, 6.1 pg m{sup {minus}3}. These are the lowest concentrations yet determined in the troposphere, but for Pb and Zn they still indicate a significant enrichment over expected crustal concentrations. For these elements, estimated marine and volcanic contributions cannot account for this excess and suggest pollution as the dominant source even at this remote location. For Cd and Cu a dominant anthropogenic source cannot be ruled out, although current estimated of crustal, marine, a volcanic emissions could account for levels determined.

  17. Unraveling the Complexity of Atmospheric Aerosol: Insights from Ultrahigh Resolution Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Mazzoleni, Lynn R.; Zhao, Yunzhu; Samburova, Vera; Gannet Hallar, A.; Lowenthal, Douglas

    2016-04-01

    Atmospheric aerosol organic matter (AOM) is a complex mixture of thousands of organic compounds, which may have significant influence on the climate-relevant properties of atmospheric aerosols. An improved understanding of the molecular composition of AOM is needed to evaluate the effect of aerosol composition upon aerosol physical properties. Products of gas, aqueous and particle phase reactions contribute to the aerosol organic mass. Thus, ambient aerosols carry a complex array of AOM components with variable chemical signatures depending upon its origin and aerosol life-cycle processes. In this work, ultrahigh-resolution Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS) was used to characterize ambient aerosol AOM collected at the Storm Peak Laboratory (3210 m a.s.l.) near Steamboat Springs, CO. Thousands of molecular formulas were assigned in the mass range of m/z 100-800 after negative-ion electrospray ionization. Using multivariate statistical analysis, correlations between the site meteorological conditions and specific molecular compositions were identified. For example, days with strong UV radiation and high temperature were found to contain large numbers of biogenic SOA molecular formulas. Similarly, days with high relative humidity and high sulfate concentrations were found to contain many sulfur-containing compounds, suggesting their aqueous phase formation.

  18. Calculating Capstone depleted uranium aerosol concentrations from beta activity measurements.

    PubMed

    Szrom, Frances; Falo, Gerald A; Parkhurst, Mary Ann; Whicker, Jeffrey J; Alberth, David P

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the DU source term for the subsequent Human Health Risk Assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short-lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Values for the equilibrium fraction ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92. This paper describes the process used and adjustments necessary to calculate uranium mass from proportional counting measurements. PMID:19204483

  19. 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

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  1. Contributions of Acid-Catalysed Processes to Secondary Organic Aerosol Mass - A Modelling pproach

    NASA Astrophysics Data System (ADS)

    Ervens, B.; Feingold, G.; Kreidenweis, S. M.

    2005-12-01

    A significant fraction of secondary organic aerosol (SOA) mass is formed by chemical and/or physical processes. However, the amount of organic material found in ambient organic aerosols cannot be explained with current models. Recently, several laboratory studies have been published which suggest that also acid-catalyzed processes that occur either in particles or at their surfaces (heterogeneous) might contribute significantly to mass formation. However, to date there is no general conclusion about the efficiency of such processes due to the great diversity of species and experimental conditions. We present a compilation of literature data (thermodynamic and kinetic) of these processes. The aerosol yields of (i) additional species which are thought previously not contribute to SOA formation (e.g. isoprene, aliphatic aldehydes) and (ii) species which form apparently higher SOA masses on acidic seed aerosols are reported and compared to input data of previous SOA models. Available kinetic data clearly exclude aldol condensation as a significant process for SOA formation on a time scale of typical aerosol life times. Using aerosol size distributions and gas phase concentrations measured during NEAQS2002 as model input data, we show that (even under assumption of equilibrium conditions) these additional processes only contribute a minor fraction to the organic aerosol mass.

  2. Characterization of organic aerosols in Beijing using an aerodyne high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, Junke; Wang, Yuesi; Huang, Xiaojuan; Liu, Zirui; Ji, Dongsheng; Sun, Yang

    2015-06-01

    Fine particle of organic aerosol (OA), mostly arising from pollution, are abundant in Beijing. To achieve a better understanding of the difference in OA in summer and autumn, a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS, Aerodyne Research Inc., USA) was deployed in urban Beijing in August and October 2012. The mean OA mass concentration in autumn was 30±30 μg m-3, which was higher than in summer (13±6.9 μg m-3). The elemental analysis found that OA was more aged in summer (oxygen-to-carbon (O/C) ratios were 0.41 and 0.32 for summer and autumn, respectively). Positive matrix factorization (PMF) analysis identified three and five components in summer and autumn, respectively. In summer, an oxygenated OA (OOA), a cooking-emission-related OA (COA), and a hydrocarbon-like OA (HOA) were indentified. Meanwhile, the OOA was separated into LV-OOA (low-volatility OOA) and SV-OOA (semi-volatile OOA); and in autumn, a nitrogen-containing OA (NOA) was also found. The SOA (secondary OA) was always the most important OA component, accounting for 55% of the OA in the two seasons. Back trajectory clustering analysis found that the origin of the air masses was more complex in summer. Southerly air masses in both seasons were associated with the highest OA loading, while northerly air masses were associated with the lowest OA loading. A preliminary study of OA components, especially the POA (primary OA), in different periods found that the HOA and COA all decreased during the National Day holiday period, and HOA decreased at weekends compared with weekdays.

  3. MCS precipitation and downburst intensity response to increased aerosol concentrations

    NASA Astrophysics Data System (ADS)

    Clavner, M.; Cotton, W. R.; van den Heever, S. C.

    2015-12-01

    Mesoscale convective systems (MCSs) are important contributors to rainfall in the High Plains of the United States as well as producers of severe weather such as hail, tornados and straight-line wind events known as derechos. Past studies have shown that changes in aerosol concentrations serving as cloud condensation nuclei (CCN) alter the MCS hydrometeor characteristics which in turn modify precipitation yield, downdraft velocity, cold-pool strength, storm propagation and the potential for severe weather to occur. In this study, the sensitivity of MCS precipitation characteristics and convective downburst velocities associated with a derecho to changes in CCN concentrations were examined by simulating a case study using the Regional Atmospheric Modeling System (RAMS). The case study of the 8 May 2009 "Super-Derecho" MCS was chosen since it produced a swath of widespread wind damage in association with an embedded large-scale bow echo, over a broad region from the High Plains of western Kansas to the foothills of the Appalachians. The sensitivity of the storm to changes in CCN concentrations was examined by conducting a set of three simulations which differed in the initial aerosol concentration based on output from the 3D chemical transport model, GEOS-Chem. Results from this study indicate that while increasing CCN concentrations led to an increase in precipitation rates, the changes to the derecho strength were not linear. A moderate increase in aerosol concentration reduced the derecho strength, while the simulation with the highest aerosol concentrations increased the derecho intensity. These changes are attributed to the impact of enhanced CCN concentration on the production of convective downbursts. An analysis of aerosol loading impacts on these MCS features will be presented.

  4. Calculating Capstone Depleted Uranium Aerosol Concentrations from Beta Activity Measurements

    SciTech Connect

    Szrom, Fran; Falo, Gerald A.; Parkhurst, MaryAnn; Whicker, Jeffrey J.; Alberth, David P.

    2009-03-01

    Beta activity measurements were used as surrogate measurements of uranium mass in aerosol samples collected during the field testing phase of the Capstone Depleted Uranium (DU) Aerosol Study. These aerosol samples generated by the perforation of armored combat vehicles were used to characterize the depleted uranium (DU) source term for the subsequent human health risk assessment (HHRA) of Capstone aerosols. Establishing a calibration curve between beta activity measurements and uranium mass measurements is straightforward if the uranium isotopes are in equilibrium with their immediate short-lived, beta-emitting progeny. For DU samples collected during the Capstone study, it was determined that the equilibrium between the uranium isotopes and their immediate short lived, beta-emitting progeny had been disrupted when penetrators had perforated target vehicles. Adjustments were made to account for the disrupted equilibrium and for wall losses in the aerosol samplers. Correction factors for the disrupted equilibrium ranged from 0.16 to 1, and the wall loss correction factors ranged from 1 to 1.92.

  5. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-01-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the Southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8±8.4 μg m-3 and 13.5±8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva)~200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  6. Characterization and source apportionment of submicron aerosol with aerosol mass spectrometer during the PRIDE-PRD 2006 campaign

    NASA Astrophysics Data System (ADS)

    Xiao, R.; Takegawa, N.; Zheng, M.; Kondo, Y.; Miyazaki, Y.; Miyakawa, T.; Hu, M.; Shao, M.; Zeng, L.; Gong, Y.; Lu, K.; Deng, Z.; Zhao, Y.; Zhang, Y. H.

    2011-07-01

    Size-resolved chemical compositions of non-refractory submicron aerosol were measured using an Aerodyne quadrupole aerosol mass spectrometer (Q-AMS) at the rural site Back Garden (BG), located ~50 km northwest of Guangzhou in July 2006. This paper characterized the submicron aerosol particles of regional air pollution in Pearl River Delta (PRD) in the southern China. Organics and sulfate dominated the submicron aerosol compositions, with average mass concentrations of 11.8 ± 8.4 μg m-3 and 13.5 ± 8.7 μg m-3, respectively. Unlike other air masses, the air masses originated from Southeast-South and passing through the PRD urban areas exhibited distinct bimodal size distribution characteristics for both organics and sulfate: the first mode peaked at vacuum aerodynamic diameters (Dva) ∼200 nm and the second mode occurred at Dva from 300-700 nm. With the information from AMS, it was found from this study that the first mode of organics in PRD regional air masses was contributed by both secondary organic aerosol formation and combustion-related emissions, which is different from most findings in other urban areas (first mode of organics primarily from combustion-related emissions). The analysis of AMS mass spectra data by positive matrix factorization (PMF) model identified three sources of submicron organic aerosol including hydrocarbon-like organic aerosol (HOA), low volatility oxygenated organic aerosol (LV-OOA) and semi-volatile oxygenated organic aerosol (SV-OOA). The strong correlation between HOA and EC indicated primary combustion emissions as the major source of HOA while a close correlation between SV-OOA and semi-volatile secondary species nitrate as well as between LV-OOA and nonvolatile secondary species sulfate suggested secondary aerosol formation as the major source of SV-OOA and LV-OOA at the BG site. However, LV-OOA was more aged than SV-OOA as its spectra was highly correlated with the reference spectra of fulvic acid, an indicator of aged and

  7. Influence of air mass origin on aerosol properties at a remote Michigan forest site

    NASA Astrophysics Data System (ADS)

    VanReken, T. M.; Mwaniki, G. R.; Wallace, H. W.; Pressley, S. N.; Erickson, M. H.; Jobson, B. T.; Lamb, B. K.

    2015-04-01

    The northern Great Lakes region of North America is a large, relatively pristine area. To date, there has only been limited study of the atmospheric aerosol in this region. During summer 2009, a detailed characterization of the atmospheric aerosol was conducted at the University of Michigan Biological Station (UMBS) as part of the Community Atmosphere-Biosphere Interactions Experiment (CABINEX). Measurements included particle size distribution, water-soluble composition, and CCN activity. Aerosol properties were strongly dependent on the origin of the air masses reaching the site. For ∼60% of the study period, air was transported from sparsely populated regions to the northwest. During these times aerosol loadings were low, with mean number and volume concentrations of 1630 cm-3 and 1.91 μm3 cm-3, respectively. The aerosol during clean periods was dominated by organics, and exhibited low hygroscopicities (mean κ = 0.18 at s = 0.3%). When air was from more populated regions to the east and south (∼29% of the time), aerosol properties reflected a stronger anthropogenic influence, with 85% greater particle number concentrations, 2.5 times greater aerosol volume, six times more sulfate mass, and increased hygroscopicity (mean k = 0.24 at s = 0.3%). These trends are have the potential to influence forest-atmosphere interactions and should be targeted for future study.

  8. Submicron aerosol mass balance at urban and semirural sites in the Milan area (Italy)

    NASA Astrophysics Data System (ADS)

    Putaud, J. P.; van Dingenen, Rita; Raes, Frank

    2002-11-01

    During the Pianura Padana Produzione di Ozono (PIPAPO) field campaign (May-June 1998), aerosol measurements were performed at an urban site and a semirural site to determine the particulate matter chemical composition in the Milan area. Aerosol samples were collected on filters for subsequent chemical analysis using virtual impactors. Possible sampling artifacts for semivolatile particulate species were addressed. Our NH4NO3 measurements were successfully compared with artifact free wet denuder-wet aerosol collector sampler data. Positive sampling artifacts for organic species were corrected using the back-to-back filter technique, allowing us to assess the lower limit for particulate organic carbon (POC) concentrations. Aerosol size distributions were measured on-line with differential mobility analyzers (DMA). The variations in the submicron aerosol mass concentration estimated from chemical analyses compared well with the variations in the submicron particle volume calculated from number size distributions. At both sites, 70% of the PM10 mass was found in the submicron fraction. The mean submicron aerosol mass concentrations were 28 μg m-3 and 20 μg m-3 at the urban site and the semirural site, respectively. The correlations between NH4+ and NO3- + 2SO4= indicate that strong acids were fully neutralized at both sites. At the urban site the submicron concentrations of NH4NO3, (NH4)2SO4, and POC were 8.1 μg m-3, 6.3 μg m-3, and 6.4 μgC m-3, respectively. At the semi-rural site, these concentrations were 4.9 μg m-3, 4.0 μg m-3, and 5.6 μgC m-3, respectively. These results show that sulfate and nitrate contribute about the same amount to submicron aerosol mass concentration, and that particulate organic matter (POM) could be the major component of the aerosol submicron mass in the Milan region, especially in semirural areas. The correlation between normalized concentrations of POM and O3 observed at the semirural site suggests that POM results at least

  9. 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

  10. Secondary Aerosol Formation in the planetary boundary layer observed by aerosol mass spectrometry on a Zeppelin NT

    NASA Astrophysics Data System (ADS)

    Rubach, Florian; Trimborn, Achim; Mentel, Thomas; Wahner, Andreas; Zeppelin Pegasos-Team 2012

    2014-05-01

    The airship Zeppelin NT is an airborne platform capable of flying at low speed throughout the entire planetary boundary layer (PBL). In combination with the high scientific payload of more than 1 ton, the Zeppelin is an ideal platform to study regional processes in the lowest layers of the atmosphere with high spatial resolution. Atmospheric aerosol as a medium long lived tracer substance is of particular interest due to its influence on the global radiation budget. Due its lifetime of up to several days secondaray aerosol at a certain location can result from local production or from transport processes. For aerosol measurements on a Zeppelin, a High-Resolution Time-of-Flight Aerosol Mass spectrometer (DeCarlo et al, 2006) was adapted to the requirements posed by an airborne platform. A weight reduction of over 20 % compared to the commercial instrument was achieved, while space occupation and footprint were each reduced by over 25 %. Within the PEGASOS project, the instrument was part of 10 measurement flight days over the course of seven weeks. Three flights were starting from Rotterdam, NL, seven flights were starting from Ozzano in the Po Valley, IT. Flight patterns included vertical profiles to study the dynamics of the PBL and cross sections through regions of interest to shed light on local production and transport processes. Analysis of data from transects between the Apennin and San Pietro Capofiume in terms of "residence time of air masses in the Po valley" indicates that aerosol nitrate has only local sources while aerosol sulfate is dominated by transport. The organic aerosol component has significant contributions of both processes. The local prodcution yields are commensurable with imultaneously observed precursor concentrations and oxidant levels. The PEGASOS project is funded by the European Commission under the Framework Programme 7 (FP7-ENV-2010-265148). DeCarlo, P.F. et al (2006), Anal. Chem., 78, 8281-8289.

  11. ON THE PROPORTIONALITY OF FINE MASS CONCENTRATION AND EXTINCTION COEFFICIENT FOR BIMODAL SIZE DISTRIBUTIONS

    EPA Science Inventory

    For a bimodal size distribution of ambient aerosol, an upper limit in particle size can be chosen for the fine aerosol fraction so that the extinction coefficient for light scattering and absorption is directly proportional to the fine mass concentration, with no dependence on th...

  12. Determination of organic compounds from wood combustion aerosol nanoparticles by different gas chromatographic systems and by aerosol mass spectrometry.

    PubMed

    Laitinen, Totti; Martín, Sara Herrero; Parshintsev, Jevgeni; Hyötyläinen, Tuulia; Hartonen, Kari; Riekkola, Marja-Liisa; Kulmala, Markku; Pavón, José Luis Pérez

    2010-01-01

    Organic compounds in atmospheric nanoparticles have an effect on human health and the climate. The determination of these particles is challenged by the difficulty of sampling, the complexity of sample composition, and the trace-level concentrations of the compounds. Meeting the challenge requires the development of sophisticated sampling systems for size-resolved particles and the optimization of sensitive, accurate and simple analytical techniques and methods. A new sampling system is proposed where particles are charged with a bipolar charger and size-segregated with a differential mobility analyzer. This system was successfully used to sample particles from wood pyrolysis with particle sizes 30-100nm. Particles were analyzed by four techniques: comprehensive two-dimensional gas chromatography-time-of-flight mass spectrometry, gas chromatography-time-of-flight mass spectrometry, gas chromatography-quadrupole mass spectrometry, and aerosol mass spectrometry (aerosol MS). In the chromatographic techniques, particles were collected on a filter and analyzed off-line after sample preparation, whereas in the aerosol MS, particle analysis was performed directly from the particle source. Target compounds of the samples were polyaromatic hydrocarbons and n-alkanes. The analytical techniques were compared and their advantages and disadvantages were evaluated. The sampling system operated well and target compounds were identified in low concentrations. PMID:19945113

  13. Overview of submicron aerosol characterization in China using an Aerodyne high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Huang, X.; He, L.; Gong, Z.; Hu, M.; Zhang, Y.

    2011-12-01

    China is one of the most rapidly developing countries in the world, but in the meantime it is suffering from severe air pollution due to heavy industrial/metropolitan emissions. Most previous aerosol studies in China were based on filter sampling followed by laboratory analysis, which provided datasets at a coarse time resolution like a day. The coarse time resolution of the aerosol datasets cannot match the actual faster variation of aerosol properties in the real atmosphere, which strongly favors highly time-resolved on-line measurement techniques. In recent years, our group deployed an Aerodyne high-resolution aerosol mass spectrometer (AMS) in different ambient atmospheres in China, including Beijing (urban), Shanghai (urban), Shenzhen (urban), Jiaxing (suburban), and Kaiping (rural). In this presentation, we will overview these on-line AMS measurement results to characterize the properties of submicron particles in China atmosphere, such as chemical composition, size distribution, diurnal variation, elemental composition, primary and secondary organic aerosol constitution, etc. The newly-developed AMS-PMF modeling techniques were utilized to quantitatively differentiate the contributions from fossil fuel combustion, cooking emissions, biomass burning, as well as secondary organic aerosol to ambient organic aerosol loadings in China. These AMS results have provided new outlook of the formation mechanisms of high aerosol pollution in China.

  14. Aerosol formation by ozonolysis of α- and β-pinene with initial concentrations below 1 ppb

    NASA Astrophysics Data System (ADS)

    Saathoff, Harald; Naumann, Karl-Heinz; Möhler, Ottmar

    2014-05-01

    Secondary organic aerosols (SOA) from the oxidation of biogenic volatile organic compounds (BVOC) are a large fraction of the tropospheric aerosol especially over tropical continental regions. The dominant SOA forming compounds are monoterpenes of which pinene is the most abundant. The reactions of monoterpenes with OH radicals, NO3 radicals, and ozone yield secondary organic aerosol mass in highly variable yields. Despite the various studies on SOA formation the influence of temperature and precursor concentrations on SOA yields are still major uncertainties in tropospheric aerosol models. In previous studies we observed a negative temperature dependence of SOA yields for SOA from ozonolysis α-pinene and limonene (Saathoff et al., 2009). However, this study as well as most of the literature data for measured SOA yields is limited to terpene concentrations of several ppb and higher (e.g. Bernard et al., 2012), hence about an order of magnitude higher than terpene concentrations even near their sources. Monoterpene concentrations in and above tropical or boral forests reach values up to a few tenth of a ppb during daytime decreasing rapidly with altitude in the boundary layer (Kesselmeier et al. 2000; Boy et al., 2004). Therefore we investigated the yield of SOA material from the ozonolysis of α- and β-pinene under simulated tropospheric conditions in the large aerosol chamber AIDA on time scales of several hours and for terpene concentrations between 0.1 and 1 ppb. The temperatures investigated were 243, 274, and 296 K with relative humidities ranging from 25% to 41%. The organic aerosol was generated by controlled oxidation with an excess of ozone (220-930 ppb) and the aerosol yield is calculated from size distributions measured with differential mobility analysers (SMPS, TSI, 3071 & 3080N) in the size range between 2 and 820 nm. On the basis of the measured initial particle size distribution, particle number concentration (CPC, TSI, 3775, 3776, 3022), and

  15. Ambient aerosol concentrations of sugars and sugar-alcohols at four different sites in Norway

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Dye, C.; Kiss, G.

    2007-04-01

    Sugars and sugar-alcohols are demonstrated to be important constituents of the ambient aerosol water-soluble organic carbon fraction (WSOC), and to be tracers for primary biological aerosol particles (PBAP). In the present study, levels of four sugars (fructose, glucose, sucrose, trehalose) and three sugar-alcohols (arabitol, inositol, mannitol) in ambient aerosols have been quantified using a novel HPLC/HRMS-TOF (High Performance Liquid Chromatography in combination with High Resolution Mass Spectrometry - Time of Flight) method to assess the contribution of PBAP to PM10 and PM2.5. Samples were collected at four sites in Norway at different times of the year in order to reflect the various contributing sources and the spatial and seasonal variation of the selected compounds. Sugars and sugar-alcohols were present at all sites investigated, underlining the ubiquity of these highly polar organic compounds. The highest concentrations were reported for sucrose, reaching a maximum concentration of 320 ng m-3 in PM10 and 55 ng m-3 in PM2.5. The mean concentration of sucrose was up to 10 times higher than fructose, glucose and trehalose. The mean concentrations of the sugar-alcohols were typically lower, or equal, to that of the monomeric sugars and trehalose. Peak concentrations of arabitol and mannitol did not exceed 30 ng m-3 in PM10, and for PM2.5 all concentrations were below 6 ng m-3. Sugars and sugar-alcohols were associated primarily with coarse aerosols except during wintertime at the suburban site in Elverum, where a shift towards sub micron aerosols was observed. It is proposed that this shift was due to the intensive use of wood burning for residential heating at this site during winter, confirmed by high concurrent concentrations of levoglucosan. Elevated concentrations of sugars in PM2.5 were observed during spring and early summer at the rural background site Birkenes. It is hypothesized that this was due to ruptured pollen.

  16. Concentrations and size distributions of Antarctic stratospheric aerosols

    NASA Technical Reports Server (NTRS)

    Ferry, G. V.; Pueschel, R. F.; Neish, E.; Schultz, M.

    1989-01-01

    Particle Measuring Systems laser particle spectrometer (ASAS-X and FSSP) probes were used to measure aerosol particle concentrations and size distributions during 11 ER-2 flights between Punta Arenas (53 deg S) and Antarctica (up to 72 deg S) from August 17 to September 22, 1987. The time resolution was 10 s, corresponding to a spatial resolution of 2 km. The data were divided into two size classes (0.05-0.25 and 0.53-5.5 micron radius) to separate the small particle from the coarse particle populations. Results show that the small-particle concentrations are typical for a background aerosol during volcanic quiescence. This concentration is generally constant along a flight track; in only one instance a depletion of small particles during a polar stratospheric cloud (PSC) encounter was measured, suggesting a nucleation of type I PSC particles on background aerosols. Temporary increases of the coarse particle concentrations indicated the presence of tenuous polar stratospheric clouds that were encountered most frequently at the southernmost portion of a flight track and when the aircraft descended to lower altitudes. During 'particle events', particle modes were found at 0.6-micron radius, corresponding to type I PSCs, and occasionally, at 2.0-micron radius corresponding to type II PSCs.

  17. Aerosol chemical mass closure during the EUROTRAC-2 AEROSOL Intercomparison 2000

    NASA Astrophysics Data System (ADS)

    Maenhaut, Willy; Schwarz, Jaroslav; Cafmeyer, Jan; Chi, Xuguang

    2002-04-01

    The field work for the AEROSOL Intercomparison 2000 took place from 4 to 14 April 2000 at Melpitz, Germany. One objective was to assess to which extent aerosol chemical mass closure could be obtained for the site. For this purpose, we operated four filter samplers in parallel (mostly using 12-h collections): two Gent PM10 stacked filter unit (SFU) samplers (one with coarse and fine Nuclepore polycarbonate filters, the other with a Gelman Teflo filter as fine filter) and two single filter holders (one with PM2.5 inlet, the other with PM10 inlet) with Whatman QM-A quartz fibre filters. All samples were analysed for the particulate mass (PM) by weighing; the samples from the first SFU were analysed for 42 elements by a combination of particle-induced X-ray emission spectroscopy and instrumental neutron activation analysis, those from the other SFU for major anions and cations by ion chromatography. All quartz filters were analysed for organic carbon and elemental carbon by a thermal-optical transmission technique. Aerosol chemical mass closure calculations were done for the separate fine (PM2) and coarse (2-10 μm) size fractions. As gravimetric PM data we used the averages from the parallel SFU collections. For reconstituting this PM, nine aerosol types (or components) were considered. Crustal matter, organic aerosol and nitrate were the major aerosol types in the coarse size fraction; the dominant aerosol types in the fine fraction were organic aerosol, nitrate and sulphate. The included components explained 116% and 86% of the gravimetric PM in the coarse and fine size fractions, respectively.

  18. Characterization of near-highway submicron aerosols in New York City with a high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Lin, Y.-C.; Ng, N. L.; Jayne, J.; Massoli, P.; Williams, L. R.; Demerjian, K. L.

    2012-02-01

    Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML), equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE) - a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1) species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz) of gaseous pollutants (e.g. HCHO, NO2, NO, O3, and CO2, etc.), black carbon (BC), and particle number concentrations and size distributions. Particulate organics varied dramatically during periods with high traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA), a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate) and oxygenated OA (OOA) showed much smoother variations indicating minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60%) with HOA accounting for a major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ∼120 nm and 500 nm (vacuum aerodynamic diameter, Dva), respectively. OOA and inorganic species appear to be

  19. Sensitivity of warm-frontal processes to cloud-nucleating aerosol concentrations

    NASA Technical Reports Server (NTRS)

    Igel, Adele L.; Van Den Heever, Susan C.; Naud, Catherine M.; Saleeby, Stephen M.; Posselt, Derek J.

    2013-01-01

    An extratropical cyclone that crossed the United States on 9-11 April 2009 was successfully simulated at high resolution (3-km horizontal grid spacing) using the Colorado State University Regional Atmospheric Modeling System. The sensitivity of the associated warm front to increasing pollution levels was then explored by conducting the same experiment with three different background profiles of cloud-nucleating aerosol concentration. To the authors' knowledge, no study has examined the indirect effects of aerosols on warm fronts. The budgets of ice, cloud water, and rain in the simulation with the lowest aerosol concentrations were examined. The ice mass was found to be produced in equal amounts through vapor deposition and riming, and the melting of ice produced approximately 75% of the total rain. Conversion of cloud water to rain accounted for the other 25%. When cloud-nucleating aerosol concentrations were increased, significant changes were seen in the budget terms, but total precipitation remained relatively constant. Vapor deposition onto ice increased, but riming of cloud water decreased such that there was only a small change in the total ice production and hence there was no significant change in melting. These responses can be understood in terms of a buffering effect in which smaller cloud droplets in the mixed-phase region lead to both an enhanced vapor deposition and decreased riming efficiency with increasing aerosol concentrations. Overall, while large changes were seen in the microphysical structure of the frontal cloud, cloud-nucleating aerosols had little impact on the precipitation production of the warm front.

  20. Effects of diesel exhaust aftertreatment devices on concentrations and size distribution of aerosols in underground mine air.

    PubMed

    Bugarski, Aleksandar D; Schnakenberg, George H; Hummer, Ion A; Cauda, Emanuele; Janisko, Samuel I; Patts, Larry D

    2009-09-01

    Three types of uncatalyzed diesel particulate filter (DPF) systems, three types of high-temperature disposable filter elements (DFEs), and one diesel oxidation catalytic converter (DOC) were evaluated in underground mine conditions for their effects on the concentrations and size distributions of diesel aerosols. Those effects were compared with the effects of a standard muffler. The experimental work was conducted directly in an underground environment using a unique diesel laboratory developed in an underground experimental mine. The DPF systems reduced total mass of aerosols in the mine air approximately 10-fold for light-load and 20-fold or more for high-load test conditions. The DFEs offered similar reductions in aerosol mass concentrations. The efficiency of the new DFEs significantly increased with accumulation of operating time and buildup of diesel particulate matter in the porous structure of the filter elements. A single laundering process did not exhibit substantial effects on performance of the filter element The effectiveness of DPFs and DFEs in removing aerosols by number was strongly influenced by engine operating mode. The concentrations of nucleation mode aerosols in the mine air were found to be substantially higher for both DPFs and DFEs when the engine was operated at high-load modes than at low-load modes. The effects of the DOC on mass and number concentrations of aerosols in mine air were relatively minor when compared to those of the DPF and DFE systems. PMID:19764243

  1. Precipitation effects on aerosol concentration in the background EMEP station of Zarra (Valencia), Spain

    NASA Astrophysics Data System (ADS)

    Calvo, Ana Isabel; San Martín, Isabel; Castro, Amaya; Alonso-Blanco, Elisabeth; Alves, Célia; Duarte, Márcio; Fernández-González, Sergio; Fraile, Roberto

    2014-05-01

    Aerosols and precipitation are closely related, presenting a bidirectional influence and constituting an important source of uncertainties on climate change studies. However, they are usually studied independently and in general are only linked to one another for the development or validation of cloud models. The primary and secondary pollutants may be removed by wet and dry deposition. Wet deposition, including in-cloud and below-cloud scavenging processes, can efficiently remove atmospheric aerosols and it is considered a critical process for determining aerosol concentrations in the atmosphere. In this study, aerosols and precipitation data from a background Spanish EMEP (Cooperative Programme for the Monitoring and Evaluation of Long Range Transmission of Air Pollutants in Europe) station located in Zarra, Valencia (Spain) were analyzed (1° 06' W and 39° 05' N, 885 m asl). The effect of precipitation on aerosol concentration was studied and the correlation between the intensity of precipitation and scavenging effect was investigated. In order to evaluate the effects of precipitation on different aerosol size ranges three different aerosol fractions were studied: PM10, PM10-2.5 and PM2.5. In order to eliminate the influence of the air mass changes, only the days in which the air mass of the precipitation day and the previous day had the same origin were considered. Thus, from a total of 3586 rainy days registered from March 2001 to December 2010, 34 precipitation days satisfied this condition and were analyzed. During the period of study, daily precipitation ranged between 0.2 and 28.8 mm, with a mean value of 4 mm. Regarding the origin of the air masses, those from west were dominant at the three height levels investigated (500, 1500 and 3000 m). In order to obtain additional information, aerosol and precipitation chemical composition were also studied in relation to the days of precipitation and the previous days. Furthermore, in order to identify the type

  2. Theoretical Basis for Convective Invigoration due to Increased Aerosol Concentration

    NASA Astrophysics Data System (ADS)

    Lebo, Z. J.; Chen, Y.; Seinfeld, J.

    2010-12-01

    Recent reports using a one-dimensional parcel model suggest that increases in aerosol number concentration may invigorate deep convection by mitigating the autoconversion process until air parcels reach the freezing level. This would lead to an increase in ice water aloft and the potential for enhanced upward heat transport due to phase changes, hence leading to invigorated convection. Other studies have proposed that an increase in aerosol loading may act to increase cloud top height, increasing the liquid water content, which ultimately increases the cumulative precipitation. Here we study the effect of aerosol perturbations on deep convection by employing the Weather Research and Forecasting model as a three-dimensional CRM with a two-moment, six-class bulk microphysics scheme. These results are corroborated using a newly developed bin microphysics scheme. The bulk microphysics scheme is augmented with a state-of-the-art activation scheme based on Köhler Theory and Population Splitting to analyze the effect of CCN perturbations on cloud development. Moreover, we include a physically-based parameterization for homogeneous and heterogeneous freezing to determine the effects of changes in IN number concentration on deep convective cloud development. We perform idealized simulations of deep convection over a wide range of CCN concentrations (i.e., 102 to 103 cm-3), which encompasses clean maritime conditions to polluted continental conditions, respectively. The detailed model calculations reveal that the CCN effect on precipitation in deep convective clouds depends strongly on the ambient water vapor mixing ratio profile. Our simulations suggest that under relatively dry conditions, an increase in aerosol number concentration leads to a decrease in precipitation (-4.2%), while under moist conditions, an increase in aerosol number concentration leads to an increase in precipitation (8.1%). However, when the water vapor in the mid- to upper-troposphere is depleted

  3. Can anthropogenic aerosol concentrations effect the snowfall rate?

    NASA Astrophysics Data System (ADS)

    Lohmann, U.; Zhang, J.; Pi, J.

    2003-04-01

    The mesoscale model GESIMA is used to simulate microphysical properties of Arctic clouds and their effect on radiation. Different case studies during the FIRE.ACE/SHEBA project show that GESIMA is able to simulate the cloud boundaries, ice and liquid water content and effective radii in good agreement with observations. For two different aerosol scenarios, the simulation results show that the anthropogenic aerosol can alter microphysical properties of Arctic clouds, and consequently modify surface precipitation. Borys et al. (2000) proposed that anthropogenically-induced decreases in cloud droplet size inhibit the riming process. On the contrary, we find that the accretion of snow crystals with cloud droplets is increased in the polluted cloud due to its higher cloud droplet number concentration. Instead the autoconversion rate of cloud droplets and accretion of drizzle by snow decreases caused by the shut-down of the collision-coalescence process in the polluted cloud. The amount of precipitation reaching the surface as snow depends crucially on the crystal shape. If aggregates are assumed, then a 10-fold increase in aerosol concentration leads to an increase in accumulated snow by 40% after 7 hours of simulation whereas the snow amount decreases by 30% when planar crystals are assumed because of the larger accretion efficiency of snow crystals with cloud droplets in case of aggregates. We will also perform climate model simulations to estimate the importance of this effect globally.

  4. Characterization of ambient aerosols at the San Francisco International Airport using BioAerosol Mass Spectrometry

    SciTech Connect

    Steele, P T; McJimpsey, E L; Coffee, K R; Fergenson, D P; Riot, V J; Tobias, H J; Woods, B W; Gard, E E; Frank, M

    2006-03-16

    The BioAerosol Mass Spectrometry (BAMS) system is a rapidly fieldable, fully autonomous instrument that can perform correlated measurements of multiple orthogonal properties of individual aerosol particles. The BAMS front end uses optical techniques to nondestructively measure a particle's aerodynamic diameter and fluorescence properties. Fluorescence can be excited at 266nm or 355nm and is detected in two broad wavelength bands. Individual particles with appropriate size and fluorescence properties can then be analyzed more thoroughly in a dual-polarity time-of-flight mass spectrometer. Over the course of two deployments to the San Francisco International Airport, more than 6.5 million individual aerosol particles were fully analyzed by the system. Analysis of the resulting data has provided a number of important insights relevant to rapid bioaerosol detection, which are described here.

  5. The impact of residential combustion emission on Arctic aerosol concentrations

    NASA Astrophysics Data System (ADS)

    Eckhardt, Sabine; Stohl, Andreas; Olivie, Dirk J. L.; Grini, Alf

    2016-04-01

    Arctic haze is a seasonal phenomenon with high concentrations of accumulation-mode aerosols occurring in the Arctic in winter and early spring. It has been challenging to reproduced this cylce and concentration levels with atmospheric transport and climate models. However, simulations have been improving recently and it has been shown, that a better scavenging parametrization as well as more realistic emissions are important to obtain better results. In this study we focus on the emission from residential heating, which depend on air temperature, as heating demand is higher on cold days. Varying this emission shows a clear effect on modeled Arctic concentrations. Arctic-mean and annual-mean concentrations of black carbon from Arctic domestic combustion emissions due to heating requirements, are nearly 70% higher when accounting for diurnal emission variability relative to constant emissions (Stohl et al., 2013). Emissions are high when ambient temperatures are low and cold air is transported to the Arctic. In order to capture this systematic effect, we created an interactive emission module for NorESM, a climate model, using the heating degree-day concept. Domestic combustion emissions of BC and other species are scaled interactively with the modeled ambient air temperatures, while securing that levels of annual total emissions from emission scenarios are reproduced. We compare the modeled aerosol concentration in the Arctic to observations and show the level of improvements achieved by using varying emission.

  6. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

    NASA Astrophysics Data System (ADS)

    Dron, J.; El Haddad, I.; Temime-Roussel, B.; Jaffrezo, J.-L.; Wortham, H.; Marchand, N.

    2010-04-01

    The functional group composition of various organic aerosols (OA) is being investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS). The determinations of the three functional groups' contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups) and precursor ion (nitro groups) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photo-oxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounted for 1.7% (vehicular) to 13.5% (o-xylene photo-oxidation) of the organic carbon. The diagnostic functional group ratios are then used to tentatively differentiate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to distinguish the sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assesses a wood burning organic carbon contribution of about 60%. Finally, examples of functional group mass spectra of all

  7. Urban increments of gaseous and aerosol pollutants and their sources using mobile aerosol mass spectrometry measurements

    NASA Astrophysics Data System (ADS)

    Elser, Miriam; Bozzetti, Carlo; El-Haddad, Imad; Maasikmets, Marek; Teinemaa, Erik; Richter, Rene; Wolf, Robert; Slowik, Jay G.; Baltensperger, Urs; Prévôt, André S. H.

    2016-06-01

    Air pollution is one of the main environmental concerns in urban areas, where anthropogenic emissions strongly affect air quality. This work presents the first spatially resolved detailed characterization of PM2.5 (particulate matter with aerodynamic equivalent diameter daero ≤ 2.5 µm) in two major Estonian cities, Tallinn and Tartu. The measurements were performed in March 2014 using a mobile platform. In both cities, the non-refractory (NR)-PM2.5 was characterized by a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) using a recently developed lens which increases the transmission of super-micron particles. Equivalent black carbon (eBC) and several trace gases including carbon monoxide (CO), carbon dioxide (CO2), and methane (CH4) were also measured. The chemical composition of PM2.5 was found to be very similar in the two cities. Organic aerosol (OA) constituted the largest fraction, explaining on average about 52 to 60 % of the PM2.5 mass. Four sources of OA were identified using positive matrix factorization (PMF): hydrocarbon-like OA (HOA, from traffic emissions), biomass burning OA (BBOA, from biomass combustion), residential influenced OA (RIOA, probably mostly from cooking processes with possible contributions from waste and coal burning), and oxygenated OA (OOA, related to secondary aerosol formation). OOA was the major OA source during nighttime, explaining on average half of the OA mass, while during daytime mobile measurements the OA was affected by point sources and dominated by the primary fraction. A strong increase in the secondary organic and inorganic components was observed during periods with transport of air masses from northern Germany, while the primary local emissions accumulated during periods with temperature inversions. Mobile measurements offered the identification of different source regions within the urban areas and the assessment of the extent to which pollutants concentrations exceeded regional background

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

    EPA Science Inventory

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

  9. THE MASS ACCOMMODATION COEFFICIENT OF AMMONIUM NITRATE AEROSOL. (R823514)

    EPA Science Inventory

    The mass transfer rate of pure ammonium nitrate between the aerosol and gas phases was
    quantified experimentally by the use of the tandem differential mobility analyzer/scanning mobility
    particle sizer (TDMA/SMPS) technique. Ammonium nitrate particles 80-220 nm in diameter<...

  10. ANALYSIS OF ATMOSPHERIC ORGANIC AEROSOLS BY MASS SPECTROSCOPY

    EPA Science Inventory

    High resolution mass spectroscopy has been found to be a useful means of characterizing the organic fraction of urban aerosols. Quantitative accuracy, however, was limited, particularly for compounds of low abundance. Some ambiguities were found in the assignment of origins of io...

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

    SciTech Connect

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

    2007-01-01

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

  12. Aerosol mass spectrometry systems and methods

    SciTech Connect

    Fergenson, David P.; Gard, Eric E.

    2013-08-20

    A system according to one embodiment includes a particle accelerator that directs a succession of polydisperse aerosol particles along a predetermined particle path; multiple tracking lasers for generating beams of light across the particle path; an optical detector positioned adjacent the particle path for detecting impingement of the beams of light on individual particles; a desorption laser for generating a beam of desorbing light across the particle path about coaxial with a beam of light produced by one of the tracking lasers; and a controller, responsive to detection of a signal produced by the optical detector, that controls the desorption laser to generate the beam of desorbing light. Additional systems and methods are also disclosed.

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

    NASA Astrophysics Data System (ADS)

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

    2015-04-01

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

  14. Black Carbon Concentration from Worldwide Aerosol Robotic Network (AERONET)

    NASA Technical Reports Server (NTRS)

    Schuster, Greg; Dubovik, Oleg; Holben, Brent; Clothiaux, Eugene

    2008-01-01

    Worldwide black carbon concentration measurements are needed to assess the efficacy of the carbon emissions inventory and transport model output. This requires long-term measurements in many regions, as model success in one region or season does not apply to all regions and seasons. AERONET is an automated network of more than 180 surface radiometers located throughout the world. The sky radiance measurements obtained by AERONET are inverted to provide column-averaged aerosol refractive indices and size distributions for the AERONET database, which we use to derive column-averaged black carbon concentrations and specific absorptions that are constrained by the measured radiation field. This provides a link between AERONET sky radiance measurements and the elemental carbon concentration of transport models without the need for an optics module in the transport model. Knowledge of both the black carbon concentration and aerosol absorption optical depth (i.e., input and output of the optics module) will enable improvements to the transport model optics module.

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

    PubMed

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

    2014-09-01

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

  16. Time-resolved measurements of aerosol elemental concentrations in indoor working environments

    NASA Astrophysics Data System (ADS)

    Žitnik, M.; Kastelic, A.; Rupnik, Z.; Pelicon, P.; Vaupetič, P.; Bučar, K.; Novak, S.; Samardžija, Z.; Matsuyama, S.; Catella, G.; Ishii, K.

    2010-12-01

    We have measured the elemental concentrations in aerosols with a 2-h time resolution in two different types of working environment: a chemistry laboratory dealing with the processing of advanced nanoparticulate materials and a medium-sized machine workshop. Non-stop 10-day and 12-day samplings were performed at each location in order to determine the concentration trends during the non-working/working and weekday/weekend periods. Supplementary measurements of PM10 aerosols with a 2-day sample collection time were performed with a standard Gent PM10 sampler to compare the elemental concentrations with the time-averaged concentrations detected by the 2D step-sampler. The concentrations were determined a posteriori by analyzing the x-ray spectra of aerosol samples emitted after 3-MeV proton bombardment. The PM10 samples collected in the chemistry laboratory were additionally inspected by scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX) to determine the chemical compositions of the individual particles. In the workshop, a total PM10 mass sampling was performed simultaneously with a minute resolution to compare the signal with typical outdoor PM10 concentration levels. A factor analysis of the time-resolved dataset points to six and eight factors in the chemistry laboratory and the machine workshop, respectively. These factors describe most of the data variance, and their composition in terms of different elements can be related to specific indoor activities and conditions. We were able to demonstrate that the elemental concentration sampling with hourly resolution is an excellent tool for studying the indoor air pollution. While sampling the total PM10 mass concentration with a minute resolution may lack the potential to identify the emission sources in a "noisy" environment, the time averaging on a day time scale is too coarse to cope with the working dynamics, even if elemental sensitivity is an option.

  17. Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

    NASA Technical Reports Server (NTRS)

    DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins,D. R.; Knapp, D.; Weinheimer, A. J.; Montzka,D. D.; Campos,T.; Jimenez, J. L.

    2007-01-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM(sub l)) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM(sub l) mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 microg/cubic m (STP) ppm(exp -1). This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2008). The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city

  18. Mass spectroscopy of single aerosols from field measurements

    SciTech Connect

    Thomson, D.S.; Murphy, D.M.

    1995-12-31

    We are developing an aircraft instrument for the chemical analysis of individual ambient aerosols in real time. In order to test the laboratory version of this instrument, we participated in a field campaign near the continental divide in Colorado in September, 1993. During this campaign, over 5000 mass spectra of ambient aerosols were collected. Analysis of the negative ion spectra shows that sulfate was the most commonly seen component of smaller particles, while nitrate was more common in larger particles. Organic compounds are present in most particles, and we believe we can distinguish inorganic carbon in some particles. Although numerous distinct classes of particles were observed, indicating external mixtures, almost all of these particle types were themselves mixtures of several compounds. Finally, we note that although the field site experienced distinct polluted and unpolluted episodes, aerosol composition did not correlate with gas phase chemistry.

  19. Continuous emission monitoring of metal aerosol concentrations in atmospheric air

    NASA Astrophysics Data System (ADS)

    Gomes, Anne-Marie; Sarrette, Jean-Philippe; Madon, Lydie; Almi, Abdenbi

    1996-11-01

    Improvements of an apparatus for continuous emission monitoring (CEM) by inductively coupled plasma atomic emission spectrometry (ICP-AES) of metal aerosols in air are described. The method simultaneously offers low operating costs, large volume of tested air for valuable sampling and avoids supplementary contamination or keeping of the air pollutant concentrations. Questions related to detection and calibration are discussed. The detection limits (DL) obtained for the eight pollutants studied are lower than the recommended threshold limit values (TLV) and as satisfactory as the results obtained with other CEM methods involving air-argon plasmas.

  20. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-06-01

    An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed along with a Scanning Mobility Particle Sizer (SMPS) and a Multi Angle Absorption Photometers (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1) in Lanzhou, northwest China, during 12 July-7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution mass spectra of organic aerosols (OA) identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns both with peak at ~07:00-11:00 (BJT: UTC +8) corresponding to the morning rush hours, while cooking OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00-15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00-13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity with that of

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

    PubMed

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

    2013-12-27

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

  2. Determination of minimum mass and spatial location of initiator for detonation of propylene oxide aerosols

    NASA Astrophysics Data System (ADS)

    Apparao, A.; Saji, J.; Balaji, M.; Devangan, A. K.; Rao, C. R.

    2016-06-01

    The mishandling of liquid fuels during production, processing or transportation can lead to the formation of combustible two-phase mixtures. These mixtures, with the availability of a suitable energy source, may be ignited generating a deflagration, or even a detonation wave. For military applications, unconfined fuel aerosols are created and detonated with the help of a strong shock generated by a powerful energy source. The minimum energy requirement is expressed in terms of the shock strength, or mass of the high-explosive-based initiator. In this study, the detonability of unconfined aerosols of 4.3 kg propylene oxide was studied by positioning different quantities of cylindrical-shaped initiators of RDX/wax (95/5) at a fixed spatial location in the aerosol cloud, and the minimum mass of the initiator required for detonation initiation was determined. The effect of spatial location and the requirement of initiator mass, especially at farther locations where the fuel concentration is likely to be lower and closer to the lower explosive limit, was also investigated. The experimental findings help identify the detonable zone in unconfined propylene oxide aerosol clouds for different combinations of spatial location and mass of initiator.

  3. Capstone depleted uranium aerosol biokinetics, concentrations, and doses.

    PubMed

    Guilmette, Raymond A; Miller, Guthrie; Parkhurst, Mary Ann

    2009-03-01

    One of the principal goals of the Capstone Depleted Uranium (DU) Aerosol Study was to quantify and characterize DU aerosols generated inside armored vehicles by perforation with a DU penetrator. This study consequently produced a database in which the DU aerosol source terms were specified both physically and chemically for a variety of penetrator-impact geometries and conditions. These source terms were used to calculate radiation doses and uranium concentrations for various scenarios as part of the Capstone Human Health Risk Assessment (HHRA). This paper describes the scenario-related biokinetics of uranium, and summarizes intakes, chemical concentrations to the organs, and E(50) and HT(50) for organs and tissues based on exposure scenarios for personnel in vehicles at the time of perforation as well as for first responders. For a given exposure scenario (duration time and breathing rates), the range of DU intakes among the target vehicles and shots was not large, about a factor of 10, with the lowest being for a ventilated operational Abrams tank and the highest being for an unventilated Abrams with DU penetrator perforating DU armor. The ranges of committed effective doses were more scenario-dependent than were intakes. For example, the largest range, a factor of 20, was shown for scenario A, a 1 min exposure, whereas, the range was only a factor of two for the first-responder scenario (E). In general, the committed effective doses were found to be in the tens of mSv. The risks ascribed to these doses are discussed separately. PMID:19204489

  4. The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

    NASA Astrophysics Data System (ADS)

    Pfaffenberger, L.; Barmet, P.; Slowik, J. G.; Praplan, A. P.; Dommen, J.; Prévôt, A. S. H.; Baltensperger, U.

    2012-09-01

    A series of smog chamber (SC) experiments was conducted to identify driving factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of organic mass measured at m/z 44 (f44), a surrogate for carboxylic/organic acids as well as the atomic oxygen-to-carbon ratio (O : C), vs. f43, a surrogate for aldehydes, alcohols and ketones. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. On average, an OH exposure of 2.9 ± 1.3 × 107 cm-3 h is needed to increase f44 by 1% during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.5 and 15 μg m-3 at an OH exposure of 4 × 107 cm-3 h, corresponding to about two days oxidation time in the atmosphere, based on a global mean OH concentration of ∼1 × 106 cm-3. Not only is the α-pinene SOA more oxygenated at low organic mass loadings, but the functional dependence of oxygenation on mass loading is enhanced at atmospherically-relevant precursor concentrations. Since the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near

  5. Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Yang, T.; Ng, N. L.; Demerjian, K. L.

    2012-09-01

    Positive matrix factorization (PMF) was applied to the merged high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS) measurements to investigate the sources and evolution processes of submicron aerosols in New York City in summer 2009. This new approach is able to study the distribution of organic and inorganic species in different types of aerosols, the acidity of organic aerosol (OA) factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrix resolved 8 factors. The hydrocarbon-like OA (HOA) and cooking OA (COA) factors contain negligible amounts of inorganic species. The two factors that are primarily ammonium sulfate (SO4-OA) and ammonium nitrate (NO3-OA), respectively, are overall neutralized. Among all OA factors the organic fraction of SO4-OA shows the highest degree of oxidation (O/C = 0.69). Two semi-volatile oxygenated OA (OOA) factors, i.e., a less oxidized (LO-OOA) and a more oxidized (MO-OOA), were also identified. MO-OOA represents local photochemical products with a diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO) and Ox(= O3 + NO2). The NO+/NO2+ ion ratio in MO-OOA is much higher than that in NO3-OA and in pure ammonium nitrate, indicating the formation of organic nitrates. The nitrogen-enriched OA (NOA) factor contains ~25% of acidic inorganic salts, suggesting the formation of secondary OA via acid-base reactions of amines. The size distributions of OA factors derived from the size-resolved mass spectra show distinct diurnal evolving behaviors but overall a progressing evolution from smaller to larger particle mode as the oxidation degree of OA increases. Our results demonstrate that PMF analysis of the unified aerosol mass spectral matrix which contains both inorganic and organic aerosol signals may enable the deconvolution of more OA factors and gain more insights into the

  6. 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.

  7. A qualitative comparison of secondary organic aerosol yields and composition from ozonolysis of monoterpenes at varying concentrations of NO2

    NASA Astrophysics Data System (ADS)

    Draper, D. C.; Farmer, D. K.; Desyaterik, Y.; Fry, J. L.

    2015-11-01

    The effect of NO2 on secondary organic aerosol (SOA) formation from ozonolysis of α-pinene, β-pinene, Δ3-carene, and limonene was investigated using a dark flow-through reaction chamber. SOA mass yields were calculated for each monoterpene from ozonolysis with varying NO2 concentrations. Kinetics modeling of the first-generation gas-phase chemistry suggests that differences in observed aerosol yields for different NO2 concentrations are consistent with NO3 formation and subsequent competition between O3 and NO3 to oxidize each monoterpene. α-Pinene was the only monoterpene studied that showed a systematic decrease in both aerosol number concentration and mass concentration with increasing [NO2]. β-Pinene and Δ3-carene produced fewer particles at higher [NO2], but both retained moderate mass yields. Limonene exhibited both higher number concentrations and greater mass concentrations at higher [NO2]. SOA from each experiment was collected and analyzed by HPLC-ESI-MS, enabling comparisons between product distributions for each system. In general, the systems influenced by NO3 oxidation contained more high molecular weight products (MW > 400 amu), suggesting the importance of oligomerization mechanisms in NO3-initiated SOA formation. α-Pinene, which showed anomalously low aerosol mass yields in the presence of NO2, showed no increase in these oligomer peaks, suggesting that lack of oligomer formation is a likely cause of α-pinene's near 0 % yields with NO3. Through direct comparisons of mixed-oxidant systems, this work suggests that NO3 is likely to dominate nighttime oxidation pathways in most regions with both biogenic and anthropogenic influences. Therefore, accurately constraining SOA yields from NO3 oxidation, which vary substantially with the volatile organic compound precursor, is essential in predicting nighttime aerosol production.

  8. A comparison of secondary organic aerosol (SOA) yields and composition from ozonolysis of monoterpenes at varying concentrations of NO2

    NASA Astrophysics Data System (ADS)

    Draper, D. C.; Farmer, D. K.; Desyaterik, Y.; Fry, J. L.

    2015-05-01

    The effect of NO2 on secondary organic aerosol (SOA) formation from ozonolysis of α-pinene, β-pinene, Δ3-carene, and limonene was investigated using a dark flow-through reaction chamber. SOA mass yields were calculated for each monoterpene from ozonolysis with varying NO2 concentrations. Kinetics modeling of the first generation gas-phase chemistry suggests that differences in observed aerosol yields for different NO2 concentrations are consistent with NO3 formation and subsequent competition between O3 and NO3 to oxidize each monoterpene. α-pinene was the only monoterpene studied that showed a systematic decrease in both aerosol number concentration and mass concentration with increasing [NO2]. β-pinene and Δ3-carene produced fewer particles at higher [NO2], but both retained moderate mass yields. Limonene exhibited both higher number concentrations and greater mass concentrations at higher [NO2]. SOA from each experiment was collected and analyzed by HPLC-ESI-MS, enabling comparisons between product distributions for each system. In general, the systems influenced by NO3 oxidation contained more high molecular weight products (MW >400 amu), suggesting the importance of oligomerization mechanisms in NO3-initiated SOA formation. α-pinene, which showed anomalously low aerosol mass yields in the presence of NO2, showed no increase in these oligomer peaks, suggesting that lack of oligomer formation is a likely cause of α-pinene's near 0% yields with NO3. Through direct comparisons of mixed-oxidant systems, this work suggests that NO3 is likely to dominate nighttime oxidation pathways in most regions with both biogenic and anthropogenic influences. Therefore, accurately constraining SOA yields from NO3 oxidation, which vary substantially with the VOC precursor, is essential in predicting nighttime aerosol production.

  9. Effect of aerosol concentration and absorbing aerosol on the radiation fog life cycle

    NASA Astrophysics Data System (ADS)

    Maalick, Z.; Kühn, T.; Korhonen, H.; Kokkola, H.; Laaksonen, A.; Romakkaniemi, S.

    2016-05-01

    Analogous to cloud formation, the formation and life cycle of fogs is largely influenced by aerosol particles. The objective of this work is to analyze how changes in aerosol properties affect the fog life cycle, with special emphasis on how droplet concentrations change with cloud condensation nuclei (CCN) concentrations and on the effect that absorbing black carbon (BC) particles have on fog dissipation. For our simulation case study, we chose a typical fall time radiation fog at mid-latitudes (45° north) in fairly highly polluted conditions. Our results show that CCN concentrations have a strong influence on the fog lifetime. This is because the immediate effect of CCN on cloud droplet number concentrations (CDNC) is enhanced through two positive feedback loops: (1) Higher CDNC leads to more radiative cooling at the fog top, which leads to even stronger activation and (2) if CDNC is higher, the average droplet size is smaller, which slows down droplet removal through sedimentation. The effect that radiation fogs have on solar surface irradiation is large - the daily mean can change by 50% if CCN concentrations are doubled or halved (considering a reference CCN mixing ratio of 800 #/mg). With the same changes in CCN, the total fog lifetime increases 160 min or decreases 65 min, respectively. Although BC has a noticeable effect on fog height and dissipation time, its relative effect compared to CCN is small, even if BC concentrations are high. The fog formation is very sensitive to initial meteorological conditions which may be altered considerably if fog was present the previous day. This effect was neglected here, and future simulations, which span several days, may thus be a valuable extension of this study.

  10. Ambient aerosol concentrations of sugars and sugar-alcohols at four different sites in Norway

    NASA Astrophysics Data System (ADS)

    Yttri, K. E.; Dye, C.; Kiss, G.

    2007-08-01

    Sugars and sugar-alcohols are demonstrated to be important constituents of the ambient aerosol water-soluble organic carbon fraction, and to be tracers for primary biological aerosol particles (PBAP). In the present study, levels of four sugars (fructose, glucose, sucrose, trehalose) and three sugar-alcohols (arabitol, inositol, mannitol) in ambient aerosols have been quantified using a novel HPLC/HRMS-TOF (High Performance Liquid Chromatography in combination with High Resolution Mass Spectrometry - Time of Flight) method to assess the contribution of PBAP to PM>sub>10 and PM2.5. Samples were collected at four sites in Norway at different times of the year in order to reflect the various contributing sources and the spatial and seasonal variation of the selected compounds. Sugars and sugar-alcohols were present at all sites investigated, underlining the ubiquity of these highly polar organic compounds. The highest concentrations were reported for sucrose, reaching a maximum concentration of 320 ng m-3 in PM10 and 55 ng m-3 in PM2.5. The mean concentration of sucrose was up to 10 times higher than fructose, glucose and the dimeric sugar trehalose. The mean concentrations of the sugar-alcohols were typically lower, or equal, to that of the monomeric sugars and trehalose. Peak concentrations of arabitol and mannitol did not exceed 30 ng m-3 in PM10, and for PM2.5 all concentrations were below 6 ng m-3. Sugars and sugar-alcohols were associated primarily with coarse aerosols except during wintertime at the suburban site in Elverum, where a shift towards sub micron aerosols was observed. It is proposed that this shift was due to the intensive use of wood burning for residential heating at this site during winter, confirmed by high concurrent concentrations of levoglucosan. Elevated concentrations of sugars in PM2.5 were observed during spring and early summer at the rural background site Birkenes. It is hypothesized that this was due to ruptured pollen.

  11. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2015-02-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Qomolangma (Mt. Everest) Station for Atmospheric and Environmental Observation and Research (QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The average concentrations of organic carbon (OC), elemental carbon (EC) and water-soluble organic carbon were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high-elevation sites on the southern slopes of the Himalayas (Langtang and Nepal Climate Observatory at Pyramid, or NCO-P), but 3 to 6 times lower than those at Manora Peak, India, and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. OC, EC and other ionic species (NH4+, K+, NO3- and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season, being similar to the seasonal trends of aerosol composition reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they mainly originated from biomass burning. The fire spots observed by MODIS and backward air-mass trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. Moreover, the CALIOP observations confirmed that air-pollution plumes crossed the Himalayas during this period. The highly coherent variation of daily aerosol optical depth (500 nm) between QOMS and NCO-P indicates that both slopes of the Himalayas share a common atmospheric environment

  12. On the Interpretation of Oxygenated Organic Aerosols (and their Subtypes) Arising from Factor Analysis of Aerosol Mass Spectrometer Data

    NASA Astrophysics Data System (ADS)

    Jimenez, J. L.; Zhang, Q.; Canagaratna, M. R.; Ulbrich, I. M.; Ng, N. L.; Aiken, A. C.; Decarlo, P. F.; Kroll, J.; Mohr, C.; Allan, J. D.; Worsnop, D. R.

    2008-12-01

    Zhang et al. (ES&T 2005; ACP 2005) first performed factor analysis (FA) of Aerodyne Aerosol Mass Spectrometer (AMS) complete organic aerosol (OA) mass spectra. This study showed that an oxygenated organic aerosol (OOA) factor accounted for 2/3 of the OA mass at an urban site in Pittsburgh and strongly linked OOA to secondary organic aerosols (SOA). Many subsequent studies and the application of more powerful solution algorithms such as Positive Matrix Factorization (PMF) to the same FA problem have demonstrated the importance of OOA at most locations (e.g. Volkamer et al., GRL, 2006; Zhang et al., GRL, 2007; Lanz et al., ACP, 2007 and ES&T, 2008; Ulbrich et al., ACPD, 2008). Multiple studies have also identified several subtypes of OOA (e.g. OOA-1 and OOA-2). This type of analysis offers new insights because it provides some chemical resolution on the total OA mass with high time and size resolution, and bypasses the limitations of techniques that only analyze tracers and which may favor more reduced species. However the chemical resolution is limited and careful interpretation of the FA output is required, including the use of database spectra, time series of external tracers, tracer ratios, back-trajectory analyses, size- distribution analyses, etc. This presentation will address the interpretation of total OOA and its subfactors across a large range of locations in urban, suburban, rural, remote, and forested areas, and will compare with the results of other source apportionment techniques. Based on data from multiple datasets we conclude that (1) anthropogenic SOA in and downwind of urban areas is an important source of OOA; (2) motor vehicles, meat cooking, and trash burning are unlikely to be sources of primary OOA; (3) SOA from biogenic and biomass burning precursors are also clear sources of OOA; (4) primary biomass burning OA (P-BBOA) typically shows significant differences with ambient OOA factors; (5) heterogeneous oxidation of urban POA may give rise to

  13. Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

    NASA Astrophysics Data System (ADS)

    Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

    2008-12-01

    The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

  14. Fungal Spore Concentrations and Ergosterol Content in Aerosol Samples in the Caribbean During African Dust Events

    NASA Astrophysics Data System (ADS)

    Santos-Figueroa, G.; Bolaños-Rosero, B.; Mayol-Bracero, O. L.

    2015-12-01

    Fungal spores are a major component of primary biogenic aerosol particles that are emitted to the atmosphere, are ubiquitous, and play an important role in the chemistry and physics of the atmosphere, climate, and public health. Every year, during summer months, African dust (AD) particles are transported to the Caribbean region causing an increase in the concentrations of particulate matter in the atmosphere. AD is one of the most important natural sources of mineral particulate matter at the global scale, and many investigations suggest that it has the ability to transport dust-associated biological particles through long distances. The relationship between AD incursions and the concentration of fungal spores in the Caribbean region is poorly understood. In order to investigate the effects of AD incursions on fungal spore's emissions, fungal spore concentrations were monitored using a Burkard spore trap at the tropical montane cloud forest of Pico del Este at El Yunque National Forest, Puerto Rico. The presence of AD was supported with satellite images of aerosol optical thickness, and with the results from the air masses backward trajectories calculated with the NOAA HYSPLIT model. Basidiospores and Ascospores comprised the major components of the total spore's concentrations, up to a maximum of 98%, during both AD incursions and background days. A considerably decrease in the concentration of fungal spores during AD events was observed. Ergosterol, biomarker for measuring fungal biomass, concentrations were determined in aerosols that were sampled at a marine site, Cabezas de San Juan Nature Reserve, in Fajardo Puerto Rico, and at an urban site, Facundo Bueso building at the University of Puerto Rico. Additional efforts to understand the relationship between the arrival of AD to the Caribbean and a decrease in spore's concentrations are needed in order to investigate changes in local spore's vs the contribution of long-range spores transported within the AD.

  15. Surface ozone concentration and its behaviour with aerosols in the northwestern Himalaya, India

    NASA Astrophysics Data System (ADS)

    Sharma, Priyanka; Kuniyal, Jagdish Chandra; Chand, Kesar; Guleria, Raj Paul; Dhyani, Pitamber Prasad; Chauhan, Chetan

    2013-06-01

    Surface ozone (O3), black carbon (BC) concentration and their relationship were established with PM10 and PM2.5 mass concentration at Mohal (31.9°N, 77.12°E, 1154 m amsl), a semi-urban site, in the Kullu valley of the northwestern part of the Indian Himalaya during January to December, 2010. O3 showed highest diurnal variation (84 ppb) during daytime and lowest (10 ppb) during late evening as well as early morning hours. The maximum concentration of O3 during summer was influenced by meteorological parameters, high insolation and backward airmass trajectories with transported pollutants. Rate of increase of O3 was observed as high as 2.92 ppb h-1 in October, followed by 2.73 ppb h-1 in March and 2.71 ppb h-1 in May. However, it was low 1.89 ppb h-1 in February. Monthly average concentration of O3 showed distinct seasonal variations with maximum in summer (55.9 ± 9.3 ppb in May) and minimum in winter (30.0 ± 6.2 ppb in January). Most of the O3 episodes were observed in summer during fair weather conditions like high solar flux (480-500 W m-2), relatively high temperature (22-24 °C) and negligible rainfall. By applying backward trajectory Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model, the origin of the airmasses contributing to the background O3 concentration was investigated. O3 showed negative correlation with BC (r = -0.42). BC contributed 10-20% and 14-42% to the total aerosol mass concentration of PM10 and PM2.5 respectively which showed positive correlation (r = 0.65) with PM10 as well as PM2.5 aerosol mass concentration.

  16. A single-particle characterization of a mobile Versatile Aerosol Concentration Enrichment System for exposure studies

    PubMed Central

    Freney, Evelyn J; Heal, Mathew R; Donovan, Robert J; Mills, Nicholas L; Donaldson, Kenneth; Newby, David E; Fokkens, Paul HB; Cassee, Flemming R

    2006-01-01

    Background An Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) was used to investigate the size and chemical composition of fine concentrated ambient particles (CAPs) in the size range 0.2–2.6 μm produced by a Versatile Aerosol Concentration Enrichment System (VACES) contained within the Mobile Ambient Particle Concentrator Exposure Laboratory (MAPCEL). The data were collected during a study of human exposure to CAPs, in Edinburgh (UK), in February-March 2004. The air flow prior to, and post, concentration in the VACES was sampled in turn into the ATOFMS, which provides simultaneous size and positive and negative mass spectral data on individual fine particles. Results The particle size distribution was unaltered by the concentrator over the size range 0.2–2.6 μm, with an average enrichment factor during this study of ~5 (after dilution of the final air stream). The mass spectra from single particles were objectively grouped into 20 clusters using the multivariate K-means algorithm and then further grouped manually, according to similarity in composition and time sequence, into 8 main clusters. The particle ensemble was dominated by pure and reacted sea salt and other coarse inorganic dusts (as a consequence of the prevailing maritime-source climatology during the study), with relatively minor contributions from carbonaceous and secondary material. Very minor variations in particle composition were noted pre- and post-particle concentration, but overall there was no evidence of any significant change in particle composition. Conclusion These results confirm, via single particle analysis, the preservation of the size distribution and chemical composition of fine ambient PM in the size range 0.2–2.6 μm after passage through the VACES concentration instrumentation. PMID:16723024

  17. Quantitative determination of carbonaceous particle mixing state in Paris using single particle mass spectrometer and aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

    2013-04-01

    Single particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been estimated using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulphate and potassium were compared with concurrent measurements from an Aerodyne high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal/optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and ten discrete mixing states for carbonaceous particles were identified and quantified. Potassium content was used to identify particles associated with biomass combustion. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorization, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulphate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA/EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidized OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the heterogeneity of primary and

  18. Quantitative determination of carbonaceous particle mixing state in Paris using single-particle mass spectrometer and aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Healy, R. M.; Sciare, J.; Poulain, L.; Crippa, M.; Wiedensohler, A.; Prévôt, A. S. H.; Baltensperger, U.; Sarda-Estève, R.; McGuire, M. L.; Jeong, C.-H.; McGillicuddy, E.; O'Connor, I. P.; Sodeau, J. R.; Evans, G. J.; Wenger, J. C.

    2013-09-01

    Single-particle mixing state information can be a powerful tool for assessing the relative impact of local and regional sources of ambient particulate matter in urban environments. However, quantitative mixing state data are challenging to obtain using single-particle mass spectrometers. In this study, the quantitative chemical composition of carbonaceous single particles has been determined using an aerosol time-of-flight mass spectrometer (ATOFMS) as part of the MEGAPOLI 2010 winter campaign in Paris, France. Relative peak areas of marker ions for elemental carbon (EC), organic aerosol (OA), ammonium, nitrate, sulfate and potassium were compared with concurrent measurements from an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), a thermal-optical OCEC analyser and a particle into liquid sampler coupled with ion chromatography (PILS-IC). ATOFMS-derived estimated mass concentrations reproduced the variability of these species well (R2 = 0.67-0.78), and 10 discrete mixing states for carbonaceous particles were identified and quantified. The chemical mixing state of HR-ToF-AMS organic aerosol factors, resolved using positive matrix factorisation, was also investigated through comparison with the ATOFMS dataset. The results indicate that hydrocarbon-like OA (HOA) detected in Paris is associated with two EC-rich mixing states which differ in their relative sulfate content, while fresh biomass burning OA (BBOA) is associated with two mixing states which differ significantly in their OA / EC ratios. Aged biomass burning OA (OOA2-BBOA) was found to be significantly internally mixed with nitrate, while secondary, oxidised OA (OOA) was associated with five particle mixing states, each exhibiting different relative secondary inorganic ion content. Externally mixed secondary organic aerosol was not observed. These findings demonstrate the range of primary and secondary organic aerosol mixing states in Paris. Examination of the temporal

  19. The link between organic aerosol mass loading and degree of oxygenation: an α-pinene photooxidation study

    NASA Astrophysics Data System (ADS)

    Pfaffenberger, L.; Barmet, P.; Slowik, J. G.; Praplan, A. P.; Dommen, J.; Prévôt, A. S. H.; Baltensperger, U.

    2013-07-01

    A series of smog chamber (SC) experiments was conducted to identify factors responsible for the discrepancy between ambient and SC aerosol degree of oxygenation. An Aerodyne high-resolution time-of-flight aerosol mass spectrometer is used to compare mass spectra from α-pinene photooxidation with ambient aerosol. Composition is compared in terms of the fraction of particulate CO2+, a surrogate for carboxylic acids, vs. the fraction of C2H3O+, a surrogate for aldehydes, alcohols and ketones, as well as in the Van Krevelen space, where the evolution of the atomic hydrogen-to-carbon ratio (H : C) vs. the atomic oxygen-to-carbon ratio (O : C) is investigated. Low (near-ambient) organic mass concentrations were found to be necessary to obtain oxygenation levels similar to those of low-volatility oxygenated organic aerosol (LV-OOA) commonly identified in ambient measurements. The effects of organic mass loading and OH (hydroxyl radical) exposure were decoupled by inter-experiment comparisons at the same integrated OH concentration. An OH exposure between 3 and 25 × 107 cm-3 h is needed to increase O : C by 0.05 during aerosol aging. For the first time, LV-OOA-like aerosol from the abundant biogenic precursor α-pinene was produced in a smog chamber by oxidation at typical atmospheric OH concentrations. Significant correlation between measured secondary organic aerosol (SOA) and reference LV-OOA mass spectra is shown by Pearson's R2 values larger than 0.90 for experiments with low organic mass concentrations between 1.2 and 18 μg m-3 at an OH exposure of 4 × 107 cm-3 h, corresponding to about two days of oxidation time in the atmosphere, based on a global mean OH concentration of ~ 1 × 106 cm-3. α-Pinene SOA is more oxygenated at low organic mass loadings. Because the degree of oxygenation influences the chemical, volatility and hygroscopic properties of ambient aerosol, smog chamber studies must be performed at near-ambient concentrations to accurately simulate

  20. Aerosol characterization over the southeastern United States using high resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition, sources, and organic nitrates

    NASA Astrophysics Data System (ADS)

    Xu, L.; Suresh, S.; Guo, H.; Weber, R. J.; Ng, N. L.

    2015-04-01

    We deployed a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) to characterize the chemical composition of submicron non-refractory particles (NR-PM1) in the southeastern US. Measurements were performed in both rural and urban sites in the greater Atlanta area, GA and Centreville, AL for approximately one year, as part of Southeastern Center of Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR1 mass concentration regardless of sampling sites and seasons. Positive matrix factorization (PMF) analysis of HR-ToF-AMS measurements identified various OA sources, depending on location and season. Hydrocarbon-like OA (HOA) and cooking OA (COA) have important but not dominant contributions to total OA in urban sites. Biomass burning OA (BBOA) concentration shows a distinct seasonal variation with a larger enhancement in winter than summer. We find a good correlation between BBOA and brown carbon, indicating biomass burning is an important source for brown carbon, although an additional, unidentified brown carbon source is likely present at the rural Yorkville site. Isoprene-derived OA (Isoprene-OA) is only deconvolved in warmer months and contributes 18-36% of total OA. The presence of Isoprene-OA factor in urban sites is more likely from local production in the presence of NOx than transport from rural sites. More-oxidized and less-oxidized oxygenated organic aerosol (MO-OOA and LO-OOA, respectively) are dominant fractions (47-79%) of OA in all sites. MO-OOA correlates well with ozone in summer, but not in winter, indicating MO-OOA sources may vary with seasons. LO-OOA, which reaches a daily maximum at night, correlates better with estimated nitrate functionality from organic nitrates than total nitrates. Based on the HR-ToF-AMS measurements, we estimate that the nitrate functionality from organic nitrates

  1. Changes in organic aerosol composition with aging inferred from aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

    2011-03-01

    Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C). Heald et al. (2010) suggested that the bulk composition of OA line up in the Van Krevelen diagram with a slope ~ -1; such slope can potentially arise from the physical mixing of HOA and OOA, and/or from chemical aging of these components. In this study, we find that the OOA components from all sites occupy an area in the Van Krevelen space, with the evolution of OOA following a shallower slope of ~ -0.5, consistent with the additions of both acid and alcohol functional groups without fragmentation, and/or the addition of acid groups with C-C bond breakage. The importance of acid formation in OOA evolution is consistent with increasing f44 in the triangle plot with photochemical age. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

  2. Spatial and temporal distributions of aerosol concentrations and depositions in Asia during the year 2010.

    PubMed

    Park, Soon-Ung; Lee, In-Hye; Joo, Seung Jin

    2016-01-15

    Aerosol Modeling System (AMS) that is consisted of the Asian Dust Aerosol Model2 (ADAM2) and the Community Multi-scale Air Quality (CMAQ) modeling system has been employed to document the spatial distributions of the monthly and the annual averaged concentration of both the Asian dust (AD) aerosol and the anthropogenic aerosol (AA), and their total depositions in the Asian region for the year 2010. It is found that the annual mean surface aerosol (PM10) concentrations in the Asian region affect in a wide region as a complex mixture of AA and AD aerosols; they are predominated by the AD aerosol in the AD source region of northern China and Mongolia with a maximum concentration exceeding 300 μg m(-3); AAs are predominated in the high pollutant emission regions of southern and eastern China and northern India with a maximum concentration exceeding 110 μg m(-3); while the mixture of AA and AD aerosols is dominated in the downwind regions extending from the Yellow Sea to the Northwest Pacific Ocean. It is also found that the annual total deposition of aerosols in the model domain is found to be 485 Tg (372 Tg by AD aerosol and 113 Tg by AA), of which 66% (319 Tg) is contributed by the dry deposition (305 Tg by AD aerosol and 14 Tg by AA) and 34% (166 Tg) by the wet deposition (66 Tg by AD aerosol and 100 Tg by AA), suggesting about 77% of the annual total deposition being contributed by the AD aerosol mainly through the dry deposition process and 24% of it by AA through the wet deposition process. The monthly mean aerosol concentration and the monthly total deposition show a significant seasonal variation with high in winter and spring, and low in summer. PMID:26520259

  3. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; Prévôt, A. S. H.; El Haddad, I.

    2015-08-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make impractical its deployment at sufficient sites to determine regional characteristics. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, PM10) collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g. AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 μg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon, oxygen containing and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g. filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially-resolved long-term datasets.

  4. Characterization and source apportionment of organic aerosol using offline aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Daellenbach, K. R.; Bozzetti, C.; Křepelová, A.; Canonaco, F.; Wolf, R.; Zotter, P.; Fermo, P.; Crippa, M.; Slowik, J. G.; Sosedova, Y.; Zhang, Y.; Huang, R.-J.; Poulain, L.; Szidat, S.; Baltensperger, U.; El Haddad, I.; Prévôt, A. S. H.

    2016-01-01

    Field deployments of the Aerodyne Aerosol Mass Spectrometer (AMS) have significantly advanced real-time measurements and source apportionment of non-refractory particulate matter. However, the cost and complex maintenance requirements of the AMS make its deployment at sufficient sites to determine regional characteristics impractical. Furthermore, the negligible transmission efficiency of the AMS inlet for supermicron particles significantly limits the characterization of their chemical nature and contributing sources. In this study, we utilize the AMS to characterize the water-soluble organic fingerprint of ambient particles collected onto conventional quartz filters, which are routinely sampled at many air quality sites. The method was applied to 256 particulate matter (PM) filter samples (PM1, PM2.5, and PM10, i.e., PM with aerodynamic diameters smaller than 1, 2.5, and 10 µm, respectively), collected at 16 urban and rural sites during summer and winter. We show that the results obtained by the present technique compare well with those from co-located online measurements, e.g., AMS or Aerosol Chemical Speciation Monitor (ACSM). The bulk recoveries of organic aerosol (60-91 %) achieved using this technique, together with low detection limits (0.8 µg of organic aerosol on the analyzed filter fraction) allow its application to environmental samples. We will discuss the recovery variability of individual hydrocarbon ions, ions containing oxygen, and other ions. The performance of such data in source apportionment is assessed in comparison to ACSM data. Recoveries of organic components related to different sources as traffic, wood burning, and secondary organic aerosol are presented. This technique, while subjected to the limitations inherent to filter-based measurements (e.g., filter artifacts and limited time resolution) may be used to enhance the AMS capabilities in measuring size-fractionated, spatially resolved long-term data sets.

  5. Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Yang, T.; Ng, N. L.; Demerjian, K. L.

    2012-05-01

    The high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS) measurements were first combined into positive matrix factorization (PMF) analysis to investigate the sources and evolution processes of atmospheric aerosols. The new approach is able to study the mixing of organic aerosols (OA) and inorganic species, the acidity of OA factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrices resolved 8 factors for the submicron aerosols measured at Queens College in New York City in summer 2009. The hydrocarbon-like OA (HOA) and cooking OA (COA) contain very minor inorganic species, indicating the different sources and mixing characteristics between primary OA and secondary species. The two factors that are primarily ammonium sulfate (SO4-OA) and ammonium nitrate (NO3-OA), respectively, are overall neutralized, of which the OA in SO4-OA shows the highest oxidation state (O/C = 0.69) among OA factors. The semi-volatile oxygenated OA comprises two components, i.e., a less oxidized (LO-OOA) and a more oxidized (MO-OOA). The MO-OOA represents a local photochemical product with the diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO) and Ox (= O3+NO2). The much higher NO+/NO2+ fragment ion ratio in MO-OOA than that from ammonium nitrate alone provides evidence for the formation of organic nitrates. The amine-related nitrogen-enriched OA (NOA) contains ~25% of acidic inorganic salts, elucidating the formation of secondary OA from amines in acidic environments. The size distributions derived from 3-dimensional size-resolved mass spectra show distinct diurnal evolving behaviors for different OA factors, but overall a progressing evolution from smaller to larger particle mode as a function of oxidation states. Our results demonstrate that PMF analysis by incorporating inorganic aerosols is of importance for

  6. Mass Spectrometry of Atmospheric Aerosol: 1 nanometer to 1 micron

    NASA Astrophysics Data System (ADS)

    Worsnop, D. R.; Ehn, M.; Junninen, H.; Kulmala, M. T.

    2010-12-01

    The role of aerosol particles remains the largest uncertainty in quantitatively assessing past, current and future climate change. The principal reason for that uncertainty arises from the need to characterize and model composition and size dependent aerosol processes, ranging from nanometer to micron scales. Aerosol mass spectrometry results have shown that about half the sub-micron aerosol composition is composed of highly oxygenated organics that are not well understood in terms of photochemical reaction mechanisms (Jimenez et al, 2009). This work has included application of high resolution time-of-flight mass spectrometry (ToFMS) in order to determine elemental and functional group composition of complex organic components. Recently, we have applied similar ToFMS to determine the composition of ambient ions, molecules and clusters, potentially involved in formation and growth of nano-particles (Junninen et al, 2010). Observed organic anions (molecular weight range 200-500 Th) have similar chemical composition as the least volatile secondary organics observed in fine particles; while organic cations are dominated by amines and pyridines. During nucleation events, anions are dominated by sulphuric acid cluster ions (Ehn et al, 2010). In both nanometer and micrometer size ranges, the goal to elucidate the roles of inorganic and organic species, particularly how particle evolution and physical properties depend on mixed compositions. Recent results will be discussed, including ambient and experimental chamber observations. Ehn et al, Atmos. Chem. Phys. Discuss., 10, 14897-14946, 2010 Jimenez et al, Science, 326, 1525-1529, 2009 Junninen et al, Atmos. Meas. Tech., 3, 1039-1053, 2010

  7. Characterization of aerosol composition and sources in the greater Atlanta area by aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Ng, N. L.; Xu, L.; Suresh, S.; Weber, R. J. J.; Baumann, K.; Edgerton, E. S.

    2014-12-01

    An important and uncertain aspect of biogenic secondary organic aerosol (SOA) formation is that it is often associated with anthropogenic pollution tracers. Prior studies in Atlanta suggested that 70-80% of the carbon in water-soluble organic carbon (WSOC) is modern, yet it is well-correlated with the anthropogenic CO. In this study, we deployed a High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) and an Aerosol Chemical Speciation Monitor (ACSM) at multiple sites in different seasons (May 2012-February 2013) to characterize the sources and chemical composition of aerosols in the greater Atlanta area. This area in the SE US is ideal to investigate anthropogenic-biogenic interactions due to high natural and anthropogenic emissions. These extensive field studies are part of the Southeastern Center for Air Pollution and Epidemiology study (SCAPE). The HR-ToF-AMS is deployed at four sites (~ 3 weeks each) in rotation: Jefferson Street (urban), Yorkville (rural), roadside site (near Highway 75/85), and Georgia Tech site (campus), with the urban and rural sites being part of the SEARCH network. We obtained seven HR-ToF-AMS datasets in total. During the entire measurement period, the ACSM is stationary at the GIT site and samples continuously. We perform positive matrix factorization (PMF) analysis on the HR-ToF-AMS and ACSM data to deconvolve the OA into different components. While the diurnal cycle of the total OA is flat as what have been previously observed, the OA factors resolved by PMF analysis show distinctively different diurnal trends. We find that the "more-oxidized oxygenated OA" (MO-OOA) constitutes a major fraction of OA at all sites. In summer, OA is dominated by SOA, e.g., isoprene-OA and OOA with different degrees of oxidation. In contrary, biomass burning OA is more prominent in winter data. By comparing HR-ToF-AMS and ACSM data during the same sampling periods, we find that the aerosol time series are highly correlated, indicating the

  8. Contributions of the pollutant emission in South Korea to the aerosol concentrations and depositions in Asia

    NASA Astrophysics Data System (ADS)

    Park, Soon-Ung; Lee, In-Hye; Choe, Anna; Joo, Seung Jin

    2015-05-01

    The spatial distributions of annual mean concentrations and the annual total depositions of the Asian dust (AD) aerosol and the anthropogenic aerosol (AA) in 2010 are investigated with pollutant emissions over the whole model domain of Asia and without the pollutant emission from South Korea using the Aerosol Modeling System (AMS) that is modified from the Asian Dust Aerosol Model2 (ADAM2) and the Community Multi-Scale Air Quality (CMAQ) modeling System. The annual mean surface aerosol concentrations in Asia are found to affect a wide region as a complex mixture of AA and AD aerosols. However, the contribution of the pollutant emission from South Korea is found to be limited to the neighboring regions. The annual total aerosol deposition in Asia is 485.2 Tg. However, the contribution due to the pollutant emission from South Korea is about 1.9 Tg, suggesting of no significant contribution to the environment.

  9. Carbonaceous aerosols on the south edge of the Tibetan Plateau: concentrations, seasonality and sources

    NASA Astrophysics Data System (ADS)

    Cong, Z.; Kang, S.; Kawamura, K.; Liu, B.; Wan, X.; Wang, Z.; Gao, S.; Fu, P.

    2014-10-01

    To quantitatively evaluate the effect of carbonaceous aerosols on the south edge of the Tibetan Plateau, aerosol samples were collected weekly from August 2009 to July 2010 at Mt. Everest (Qomolangma Station for Atmospheric and Environmental Observation and Research, briefly QOMS, 28.36° N, 86.95° E, 4276 m a.s.l.). The samples were analyzed for organic carbon (OC), elemental carbon (EC), water-soluble organic carbon (WSOC) and major ions. The average concentrations of OC, EC and WSOC were 1.43, 0.25 and 0.77 μg m-3, respectively. The concentration levels of OC and EC at QOMS are comparable to those at high elevation sites on the southern slopes of the Himalayas (Langtang and NCO-P), but three to six times lower than those at Manora Peak, India and Godavari, Nepal. Sulfate was the most abundant anion species followed by nitrate, accounting for 25 and 12% of total ionic mass, respectively. Ca2+ was the most abundant cation species (annual average of 0.88 μg m-3). The various aerosol compositions showed distinctive seasonality. The dust loading, represented by Ca2+ concentration, was relatively constant throughout the year. While OC, EC and other ionic species (NH4+, K+, NO3-, and SO42-) exhibited a pronounced peak in the pre-monsoon period and a minimum in the monsoon season. Similar seasonal trends of aerosol composition were also reported previously from the southern slope of the Himalayas, such as Langtang and NCO-P. This phenomenon indicates that both slopes of Himalayas share a common atmospheric environment regime. The strong correlation of OC and EC in QOMS aerosols with K+ and levoglucosan indicates that they were mainly originated from biomass burning. The active fire spots observed by MODIS and their backward trajectories further demonstrate that in pre-monsoon season, agricultural and forest fires in the northern India and Nepal were most likely sources of carbonaceous aerosol at QOMS. In addition to large-scale atmospheric circulation, the unique

  10. Changes in organic aerosol composition with aging inferred from aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Ng, N. L.; Canagaratna, M. R.; Jimenez, J. L.; Chhabra, P. S.; Seinfeld, J. H.; Worsnop, D. R.

    2011-07-01

    Organic aerosols (OA) can be separated with factor analysis of aerosol mass spectrometer (AMS) data into hydrocarbon-like OA (HOA) and oxygenated OA (OOA). We develop a new method to parameterize H:C of OOA in terms of f43 (ratio of m/z 43, mostly C2H3O+, to total signal in the component mass spectrum). Such parameterization allows for the transformation of large database of ambient OOA components from the f44 (mostly CO2+, likely from acid groups) vs. f43 space ("triangle plot") (Ng et al., 2010) into the Van Krevelen diagram (H:C vs. O:C) (Van Krevelen, 1950). Heald et al. (2010) examined the evolution of total OA in the Van Krevelen diagram. In this work total OA is deconvolved into components that correspond to primary (HOA and others) and secondary (OOA) organic aerosols. By deconvolving total OA into different components, we remove physical mixing effects between secondary and primary aerosols which allows for examination of the evolution of OOA components alone in the Van Krevelen space. This provides a unique means of following ambient secondary OA evolution that is analogous to and can be compared with trends observed in chamber studies of secondary organic aerosol formation. The triangle plot in Ng et al. (2010) indicates that f44 of OOA components increases with photochemical age, suggesting the importance of acid formation in OOA evolution. Once they are transformed with the new parameterization, the triangle plot of the OOA components from all sites occupy an area in Van Krevelen space which follows a ΔH:C/ΔO:C slope of ~ -0.5. This slope suggests that ambient OOA aging results in net changes in chemical composition that are equivalent to the addition of both acid and alcohol/peroxide functional groups without fragmentation (i.e. C-C bond breakage), and/or the addition of acid groups with fragmentation. These results provide a framework for linking the bulk aerosol chemical composition evolution to molecular-level studies.

  11. Aerosols in polluted versus nonpolluted air masses Long-range transport and effects on clouds

    NASA Technical Reports Server (NTRS)

    Pueschel, R. F.; Van Valin, C. C.; Castillo, R. C.; Kadlecek, J. A.; Ganor, E.

    1986-01-01

    To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United States, aerosol and cloud-drop size distributions, elemental composition of aerosols as a function of size, and ionic content of cloud water were measured on Whiteface Mountain, NY, during the summers of 1981 and 1982. In several case studies, the data were cross-correlated with different air mass types - background continental, polluted continental, and maritime - that were advected to the sampling site. The results are the following: (1) Anthropogenic sources hundreds of kilometers upwind cause the small-particle (accumulation) mode number to increase from hundreds of thousands per cubic centimeter and the mass loading to increase from a few to several tens of micrograms per cubic meter, mostly in the form of sulfur aerosols. (2) A significant fraction of anthropogenic sulfur appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (3) Clouds in Atlantic maritime air masses have cloud drop spectra that are markedly different from those measured in continental clouds. The drop concentration is significantly lower, and the drop size spectra are heavily skewed toward large drops. (4) Effects of anthropogenic pollutants on cloud water ionic composition are an increase of nitrate by a factor of 50, an increase of sulfate by more than one order of magnitude, and an increase of ammonium ion by a factor of 7. The net effect of the changes in ionic concentrations is an increase in cloud water acidity. An anion deficit even in maritime clouds suggests an unknown, possibly biogenic, source that could be responsible for a pH below neutral, which is frequently observed in nonpolluted clouds.

  12. Evaluation of a Low-Cost Aerosol Sensor to Assess Dust Concentrations in a Swine Building.

    PubMed

    Jones, Samuel; Anthony, T Renée; Sousan, Sinan; Altmaier, Ralph; Park, Jae Hong; Peters, Thomas M

    2016-06-01

    Exposure to dust is a known occupational hazard in the swine industry, although efforts to measure exposures are labor intensive and costly. In this study, we evaluated a Dylos DC1100 as a low-cost (~$200) alternative to assess respirable dust concentrations in a swine building in winter. Dust concentrations were measured with collocated monitors (Dylos DC1100; an aerosol photometer, the pDR-1200; and a respirable sampler analyzed gravimetrically) placed in two locations within a swine farrowing building in winter for 18-24-h periods. The particle number concentrations measured with the DC1100 were converted to mass concentration using two methods: Physical Property Method and Regression Method. Raw number concentrations from the DC1100 were highly correlated to mass concentrations measured with the pDR-1200 with a coefficient of determination (R (2)) of 0.85, indicating that the two monitors respond similarly to respirable dust in this environment. Both methods of converting DC1100 number concentrations to mass concentrations yielded strong linear relationships relative to that measured with the pDR-1200 (Physical Property Method: slope = 1.03, R (2) = 0.72; Regression Method: slope = 0.72, R (2) = 0.73) and relative to that measured gravimetrically (Physical Property Method: slope = 1.08, R (2) = 0.64; Regression Method: slope = 0.75, R (2) = 0.62). The DC1100 can be used as a reasonable indicator of respirable mass concentrations within a CAFO and may have broader applicability to other agricultural and industrial settings. PMID:26944922

  13. Functional group composition of ambient and source organic aerosols determined by tandem mass spectrometry

    NASA Astrophysics Data System (ADS)

    Dron, J.; El Haddad, I.; Temime-Roussel, B.; Jaffrezo, J.-L.; Wortham, H.; Marchand, N.

    2010-08-01

    The functional group composition of various organic aerosols (OA) is investigated using a recently developed analytical approach based on atmospheric pressure chemical ionisation-tandem mass spectrometry (APCI-MS/MS). The determinations of three functional groups contents are performed quantitatively by neutral loss (carboxylic and carbonyl groups, R-COOH and R-CO-Ŕ respectively) and precursor ion (nitro groups, R-NO2) scanning modes of a tandem mass spectrometer. Major organic aerosol sources are studied: vehicular emission and wood combustion for primary aerosol sources; and a secondary organic aerosol (SOA) produced through photooxidation of o-xylene. The results reveal significant differences in the functional group contents of these source aerosols. The laboratory generated SOA is dominated by carbonyls while carboxylics are preponderate in the wood combustion particles. On the other hand, vehicular emissions are characterised by a strong nitro content. The total amount of the three functional groups accounts for 1.7% (vehicular) to 13.5% (o-xylene photooxidation) of the organic carbon. Diagnostic functional group ratios are then used to tentatively discriminate sources of particles collected in an urban background environment located in an Alpine valley (Chamonix, France) during a strong winter pollution event. The three functional groups under study account for a total functionalisation rate of 2.2 to 3.8% of the organic carbon in this ambient aerosol, which is also dominated by carboxylic moieties. In this particular case study of a deep alpine valley during winter, we show that the nitro- and carbonyl-to-carboxylic diagnostic ratios can be a useful tool to discriminate sources. In these conditions, the total OA concentrations are highly dominated by wood combustion OA. This result is confirmed by an organic markers source apportionment approach which assess a wood burning organic carbon contribution of about 60%. Finally, examples of functional group mass

  14. Organosulfates and organic acids in Arctic aerosols: speciation, annual variation and concentration levels

    NASA Astrophysics Data System (ADS)

    Hansen, A. M. K.; Kristensen, K.; Nguyen, Q. T.; Zare, A.; Cozzi, F.; Nøjgaard, J. K.; Skov, H.; Brandt, J.; Christensen, J. H.; Ström, J.; Tunved, P.; Krejci, R.; Glasius, M.

    2014-02-01

    Sources, composition and occurrence of secondary organic aerosols (SOA) in the Arctic were investigated at Zeppelin Mountain, Svalbard, and Station Nord, northeast Greenland, during the full annual cycle of 2008 and 2010 respectively. We focused on the speciation of three types of SOA tracers: organic acids, organosulfates and nitrooxy organosulfates from both anthropogenic and biogenic precursors, here presenting organosulfate concentrations and compositions during a full annual cycle and chemical speciation of organosulfates in Arctic aerosols for the first time. Aerosol samples were analysed using High Performance Liquid Chromatography coupled to a quadrupole Time-of-Flight mass spectrometer (HPLC-q-TOF-MS). A total of 11 organic acids (terpenylic acid, benzoic acid, phthalic acid, pinic acid, suberic acid, azelaic acid, adipic acid, pimelic acid, pinonic acid, diaterpenylic acid acetate (DTAA) and 3-methyl-1,2,3-butanetricarboxylic acid (MBTCA)), 12 organosulfates and one nitrooxy organosulfate were identified at the two sites. Six out of the 12 organosulfates are reported for the first time. Concentrations of organosulfates follow a distinct annual pattern at Station Nord, where high concentration were observed in late winter and early spring, with a mean total concentration of 47 (±14) ng m-3, accounting for 7 (±2)% of total organic matter, contrary to a considerably lower organosulfate mean concentration of 2 (±3) ng m-3 (accounting for 1 (±1)% of total organic matter) observed during the rest of the year. The organic acids followed the same temporal trend as the organosulfates at Station Nord; however the variations in organic acid concentrations were less pronounced, with a total mean organic acid concentration of 11.5 (±4) ng m-3 (accounting for 1.7 (±0.6)% of total organic matter) in late winter and early spring, and 2.2 (±1) ng m-3 (accounting for 0.9 (±0.4)% of total organic matter) during the rest of the year. At Zeppelin Mountain

  15. In situ vertical profiles of aerosol extinction, mass, and composition over the SEUS during the SENEX and SEAC4RS studies

    NASA Astrophysics Data System (ADS)

    Wagner, N. L.; Brock, C. A.; Day, D. A.; Diskin, G. S.; Gordon, T. D.; Graus, M.; Holloway, J. S.; Huey, L. G.; Jimenez, J. L.; Lack, D.; Liao, J.; Liu, X.; Markovic, M. Z.; Middlebrook, A. M.; Perring, A. E.; Richardson, M.; Schwarz, J. P.; Warneke, C.; Welti, A.; Wisthaler, A.; Ziemba, L. D.; Murphy, D. M.; Campuzano Jost, P.

    2014-12-01

    Shallow cumulus convection enhances vertical transport of trace gases and aerosol and creates a cloudy transition layer on top of the sub-cloud mixed layer. Two recent studies have proposed that an elevated layer of enhanced organic aerosol over the southeastern United States (SEUS) could explain the discrepancy in the summertime enhancement of aerosol optical depth (AOD) and summertime enhancement of surface measurements of aerosol mass. We investigate the vertical profile of aerosol over the SEUS during the summertime using in situ aircraft-based measurements of aerosol from the SENEX and SEAC4RS studies. During shallow cumulus convection over the SEUS, we found that aerosol and trace gas concentration in the transition layer are diluted by cleaner air from the free troposphere, and the absolute aerosol loading decreases with altitude in the transition layer. However, after normalizing the vertical profiles to the CO boundary layer enhancement to correct for the dilution, the aerosol mass, volume, and extinction relative to the boundary layer CO enhancement is ~20% greater in the transition layer than in the mixed layer. The enhancement of aerosol loading suggests production of aerosol mass in the transition layer, although biomass burning could also be the source of the enhancement. The median composition of the aerosol in the mixed layer is ~70% organics and ~18% sulfate, while it is 65% organics and 23% sulfate in the transition layer. The composition of the aerosol enhancement in the transition layer is roughly equal parts sulfate and organics by mass. The enhancement of aerosol extinction in the transition layer is not sufficient to explain the summertime enhancement of AOD over SEUS.

  16. Contrasting trends of mass and optical properties of aerosols over the Northern Hemisphere from 1992 to 2011

    NASA Astrophysics Data System (ADS)

    Wang, K.; Dickinson, R. E.; Su, L.; Trenberth, K. E.

    2012-07-01

    Atmospheric aerosols impact both human health and climate. PMX is the mass concentration of aerosol particles that have aerodynamic diameters less than X μm, PM10 was initially selected to measure the environmental impact of aerosols. Recently, it was realized that fine particles are more hazardous than larger ones and should be measured. Consequently, observational data for PM2.5 have been obtained but only for a much shorter period than that of PM10. Optical extinction of aerosols, the inverse of meteorological visibility, is sensitive to particles less than 1.0 μm. These fine particles only account for a small part of total mass of aerosols although they are very efficient in light extinction. Comparisons are made between PM10 and PM2.5 over the period when the latter is available and with visibility data for a longer period. PM10 has decreased by 44% in Europe from 1992 to 2009, 33% in the US from 1993 to 2010, 10% in Canada from 1994 to 2009, and 26% in China from 2000 to 2010. However, in contrast, aerosol optical extinction increased 7% in the US, 10% in Canada, and 18% in China during the above study periods. The reduction of optical extinction over Europe of 5% is also much less than the 44% reduction in PM10. Over its short period of record PM2.5 decreased less than PM10. Hence, PM10 is neither a good measure of changes in smaller particles or of their long-term trends, a result that has important implications for both climate impact and human health effects. The increased fraction of anthropogenic aerosol emission, such as vehicle exhaust, to total atmospheric aerosols partly explains this contrasting trend of optical and mass properties of aerosols.

  17. Contrasting trends of mass and optical properties of aerosols over the Northern Hemisphere from 1992 to 2011

    NASA Astrophysics Data System (ADS)

    Wang, K. C.; Dickinson, R. E.; Su, L.; Trenberth, K. E.

    2012-10-01

    Atmospheric aerosols affect both human health and climate. PMX is the mass concentration of aerosol particles that have aerodynamic diameters less than X μm, PM10 was initially selected to measure the environmental impact of aerosols. Recently, it was realized that fine particles are more hazardous than larger ones and should be measured. Consequently, observational data for PM2.5 have been obtained but only for a much shorter period than that of PM10. Optical extinction of aerosols, the inverse of meteorological visibility, is sensitive to particles less than 1.0 μm. These fine particles only account for a small part of total mass of aerosols although they are very efficient in light extinction. Comparisons are made between PM10 and PM2.5 over the period when the latter is available and with visibility data for a longer period. PM10 has decreased by 44% in Europe from 1992 to 2009, 33% in the US from 1993 to 2010, 10% in Canada from 1994 to 2009, and 26% in China from 2000 to 2011. However, in contrast, aerosol optical extinction has increased 7% in the US, 10% in Canada, and 18% in China during the above study periods. The reduction of optical extinction over Europe of 5% is also much less than the 44% reduction in PM10. Over its short period of record PM2.5 decreased less than PM10. Hence, PM10 is neither a good measure of changes in smaller particles nor of their long-term trends, a result that has important implications for both climate impact and human health effects. The increased fraction of anthropogenic aerosol emission, such as from vehicle exhaust, to total atmospheric aerosols partly explains this contrasting trend of optical and mass properties of aerosols.

  18. Aerosol formation from high-velocity uranium drops: Comparison of number and mass distributions. Final report

    SciTech Connect

    Rader, D.J.; Benson, D.A.

    1995-05-01

    This report presents the results of an experimental study of the aerosol produced by the combustion of high-velocity molten-uranium droplets produced by the simultaneous heating and electromagnetic launch of uranium wires. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. As reported earlier, the resulting aerosol consists mainly of web-like chain agglomerates. A condensation nucleus counter was used to investigate the decay of the total particle concentration due to coagulation and losses. Number size distributions based on mobility equivalent diameter obtained soon after launch with a Differential Mobility Particle Sizer showed lognormal distributions with an initial count median diameter (CMD) of 0.3 {mu}m and a geometric standard deviation, {sigma}{sub g} of about 2; the CMD was found to increase and {sigma}{sub g} decrease with time due to coagulation. Mass size distributions based on aerodynamic diameter were obtained for the first time with a Microorifice Uniform Deposit Impactor, which showed lognormal distributions with mass median aerodynamic diameters of about 0.5 {mu}m and an aerodynamic geometric standard deviation of about 2. Approximate methods for converting between number and mass distributions and between mobility and aerodynamic equivalent diameters are presented.

  19. Spatial variation of the aerosol concentration and deposition over the Mediterranean coastal zone

    NASA Astrophysics Data System (ADS)

    Piazzola, J.; Tedeschi, G.; Blot, R.

    2010-07-01

    A model for the spatial variation of aerosol concentrations and deposition along the coastal zone is of great interest for studies on air and water quality. In coastal areas, sea-spray aerosols generated at the sea surface by the interaction between wind and waves add to a continental contribution emitted from natural and/or anthropogenic sources. To include coastal effects in the model for the prediction of aerosol concentrations, Piazzola et al. (2003) developed the coastal Mediterranean aerosol model. The present paper deals with an extension of the Mediterranean coastal aerosol to a regional scale applied to the prediction of the sea surface flux deposition. This was achieved by the development of an automatic coupling process between the aerosol model and a regional meso-scale meteorological model which allows accounting for the details of the orography of the coast. The results show a non-homogeneous spatial coverage of aerosol concentrations over the northwestern Mediterranean. The simulations were then validated using aerosol size distributions recorded on board the ship "Atalante" for two kinds of meteorological conditions. Error calculations show a good performance of the coupling process since it predicts the aerosol concentration to within a maximum factor of 3 for particle radii between 0.1 to 10 µm. This process was then used to provide the spatial distribution of the particle deposition fluxes over the study area.

  20. Bio-Aerosol Detection Using Mass Spectrometry: Public Health Applications

    SciTech Connect

    Ludvigson, L D

    2004-03-05

    I recently spent a summer as an intern at the Lawrence Livermore National Laboratory. I worked on a project involving the real-time, reagentless, single cell detection of aerosolized pathogens using a novel mass spectrometry approach called Bio-Aerosol Mass Spectrometry (BAMS). Based upon preliminary results showing the differentiation capabilities of BAMS, I would like to explore the development and use of this novel detection system in the context of both environmental and clinical sample pathogen detection. I would also like to explore the broader public health applications that a system such as BAMS might have in terms of infectious disease prevention and control. In order to appreciate the potential of this instrument, I will demonstrate the need for better pathogen detection methods, and outline the instrumentation, data analysis and preliminary results that lead me toward a desire to explore this technology further. I will also discuss potential experiments for the future along with possible problems that may be encountered along the way.

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  2. Mass-based hygroscopicity parameter interaction model and measurement of atmospheric aerosol water uptake

    NASA Astrophysics Data System (ADS)

    Mikhailov, E.; Vlasenko, S.; Rose, D.; Pöschl, U.

    2013-01-01

    In this study we derive and apply a mass-based hygroscopicity parameter interaction model for efficient description of concentration-dependent water uptake by atmospheric aerosol particles with complex chemical composition. The model approach builds on the single hygroscopicity parameter model of Petters and Kreidenweis (2007). We introduce an observable mass-based hygroscopicity parameter κm which can be deconvoluted into a dilute hygroscopicity parameter (κm0) and additional self- and cross-interaction parameters describing non-ideal solution behavior and concentration dependencies of single- and multi-component systems. For reference aerosol samples of sodium chloride and ammonium sulfate, the κm-interaction model (KIM) captures the experimentally observed concentration and humidity dependence of the hygroscopicity parameter and is in good agreement with an accurate reference model based on the Pitzer ion-interaction approach (Aerosol Inorganic Model, AIM). Experimental results for pure organic particles (malonic acid, levoglucosan) and for mixed organic-inorganic particles (malonic acid - ammonium sulfate) are also well reproduced by KIM, taking into account apparent or equilibrium solubilities for stepwise or gradual deliquescence and efflorescence transitions. The mixed organic-inorganic particles as well as atmospheric aerosol samples exhibit three distinctly different regimes of hygroscopicity: (I) a quasi-eutonic deliquescence & efflorescence regime at low-humidity where substances are just partly dissolved and exist also in a non-dissolved phase, (II) a gradual deliquescence & efflorescence regime at intermediate humidity where different solutes undergo gradual dissolution or solidification in the aqueous phase; and (III) a dilute regime at high humidity where the solutes are fully dissolved approaching their dilute hygroscopicity. For atmospheric aerosol samples collected from boreal rural air and from pristine tropical rainforest air (secondary

  3. Number size distribution of aerosols at Mt. Huang and Nanjing in the Yangtze River Delta, China: Effects of air masses and characteristics of new particle formation

    NASA Astrophysics Data System (ADS)

    Wang, Honglei; Zhu, Bin; Shen, Lijuan; An, Junlin; Yin, Yan; Kang, Hanqing

    2014-12-01

    Aerosol number spectra in the range of 10 nm-10 μm were observed at Mt. Huang (Aug. 15-Sep. 15) and Nanjing (Oct. 13-Nov. 15) by a wide-range particle spectrometer (WPS) in 2011. Based on the backward trajectories obtained using the HYSPLIT model, the transport pathways of observed air masses during the study periods were classified into the following four groups: maritime air mass, continental air mass, marine-continental mixed air mass and local air mass. The variations in the aerosol number spectrum and the new particle formation (NPF) events for various types of air masses were discussed, along with meteorological data. The results showed that the average number concentration was 12,540 cm- 3 at Nanjing and only 2791 cm- 3 at Mt. Huang. The aerosol number concentration in Nanjing was 3-7 times higher than that in Mt. Huang; the large discrepancy was in the range of 10-100 nm. Different types of air masses had different effects on number concentration distribution. The number concentration of aerosols was higher in marine air masses, continental air masses and continental-marine mixed air masses at 10-50 nm, 100-500 nm and 50-200 nm, respectively. Under the four types of air masses, the aerosol size spectra had bimodal distributions in Nanjing and unimodal distributions in Mt. Huang (except under continental air masses: HT1). The effects of the diverse air masses on aerosol size segments of the concentration peak in Mt. Huang were stronger than those in Nanjing. The local air masses were dominant at these two sites and accounted for 44% of the total air masses. However, the aerosol number concentration was the lowest in Mt. Huang and the highest in Nanjing when local air masses were present. The number concentrations for foreign air masses increased at Mt. Huang and decreased at Nanjing. Different types of air masses had greater effects on the aerosol spectrum distribution at Mt. Huang than at Nanjing. During the NPF events, the particle growth rates at Mt

  4. Seasonal differences in aerosol water may reconcile AOT and surface mass measurements in the Southeast U.S.

    NASA Astrophysics Data System (ADS)

    Nguyen, T. K. V.; Ghate, V. P.; Carlton, A. M. G.

    2015-12-01

    Summertime aerosol optical thickness (AOT) in the Southeast U.S. is high and sharply enhanced (2-3 times) compared to wintertime AOT. This seasonal pattern is unique to the Southeast U.S. and is of particular interest because temperatures there have not warmed over the past 100 years, contrasting with trends in other U.S. regions. Some investigators hypothesize the Southeast temperature trend is due to secondary organic aerosols (SOA) formed from interactions of biogenic volatile organic compounds (BVOCs) and anthropogenic emissions that create a cooling haze. However, aerosol measurements made at the surface do not exhibit strong seasonal differences in mass or organic fraction to support this hypothesis. In this work, we attempt to reconcile the spatial and temporal distribution of AOT over the U.S. with surface mass measurements by examining trends in particle-phase liquid water, an aerosol constituent that effectively scatters radiation and is removed from aerosols in mass measurements at routine surface monitoring sites. We employ the thermodynamic model ISORROPIA (v2.1) to estimate surface and aloft aerosol water mass concentrations at locations of Interagency Monitoring of Protected Visual Environments (IMPROVE) sites using measured speciated ion mass concentrations and NCEP North American Regional Reanalysis (NARR) meteorological data. Results demonstrate strong seasonal differences in aerosol water in the eastern compared to the western part of the U.S., consistent with geographic patterns in AOT. The highest mean regional seasonal difference from 2000 to 2007 is 5.5 μg m-3 and occurs the Southeast, while the lowest is 0.44 μg m-3 and occurs in the dry Mountain West. Our findings suggest 1) similarity between spatial trends in aerosol water in the U.S. and previously published AOT data from the MODIS-TERRA instrument and 2) similar interannual trends in mean aerosol water and previously published interannual AOT trends from MISR, MODIS-TERRA, MODIS

  5. Dry Deposition of Fine Aerosol Nitrogen to an Agricultural Field Measured by Eddy-Correlation Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Gonzales, D. A.; Allen, J. O.

    2005-12-01

    In urban areas high emissions of reactive nitrogen species cause an increase in atmospheric aerosol nitrogen formation and deposition. This nitrogen is eventually removed from the atmosphere by wet or dry deposition, with dry deposition often accounting for more than half of the total deposition of particulate nitrate. Total N deposition is not adequately characterized, in part because dry deposition is difficult to measure or model. For example measured fine particle deposition to a forest canopy differs from predicted values by an order of magnitude. The eddy-correlation technique is a micrometeorological method used to directly measure fluxes from measurements made above the surface. Eddy-correlation mass spectrometry (ECMS) has been developed to directly measure aerosol particle deposition velocities from fast response aerosol concentration and wind velocity measurements. Using an Aerodyne Aerosol Mass Spectrometer (AMS), the size and composition of ambient aerosols were measured at 10~Hz. The AMS signal is proportional to non-refractory PM1.0 mass. Aerosol deposition fluxes for a given averaging period are then calculated directly as the covariance of the vertical wind velocity with the AMS signal (F = -\\overline{w'S'}). A field study was conducted to measure aerosol nitrogen dry deposition to an agricultural field immediately downwind of the Phoenix metropolitan area using eddy-correlation mass spectrometry. The study was supplemented with aerosol composition measurements including bulk deposition collectors and filter bank samplers. Here we compare the results of the flux estimates from bulk collection with inferential measurements (filter samples and modeled deposition velocities) and direct micrometeorological measurements (ECMS) in order to improve nitrogen deposition estimates.

  6. Dry Deposition of Fine Aerosol Nitrogen to an Agricultural Field Measured by Eddy-Correlation Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Gonzales, D. A.; Allen, J. O.; Smith, K. A.; Hope, D.

    2004-12-01

    In urban areas high emissions of reactive nitrogen species cause an increase in atmospheric aerosol nitrogen formation and deposition. This nitrogen is eventually removed from the atmosphere by wet or dry deposition, with dry deposition often accounting for more than half of the total deposition of particulate nitrate (Lovett, 1994). Total N deposition is not adequately characterized, in part because dry deposition is difficult to measure or model. For example measured fine particle deposition to a forest canopy differs from predicted values by an order of magnitude (Gallagher et al., 1997). The eddy-correlation technique is a micrometeorological method used to directly measure fluxes from measurements made above the surface (Wesely and Hicks, 2000). Eddy-correlation mass spectrometry (ECMS) has been developed to directly measure aerosol particle deposition velocities from fast response aerosol concentration and wind velocity measurements. Using an Aerodyne Aerosol Mass Spectrometer (AMS) (Jayne et al., 2000), the size and composition of ambient aerosols is measured at a high frequency. The AMS signal is proportional to non-refractory PM1.0 mass. Aerosol deposition fluxes for a given averaging period are then calculated directly as the covariance of the vertical wind velocity with the AMS signal (F = -/line{w'S'}). A field study was conducted to measure aerosol nitrogen dry deposition to an agricultural field immediately downwind of the Phoenix metropolitan area using eddy-correlation mass spectrometry. The study was supplemented with aerosol composition measurements including bulk deposition collectors and filter bank samplers. Bulk deposition samples and 24-hour filter samples were analyzed for ammonia and nitrogen. Here we compare the results of the flux estimates from bulk collection with inferential measurements (filter samples and modeled deposition velocities) and direct micrometeorological measurements (ECMS) in order to improve N deposition estimates.

  7. Response of an aerosol mass spectrometer to organonitrates and organosulfates and implications for atmospheric chemistry.

    PubMed

    Farmer, D K; Matsunaga, A; Docherty, K S; Surratt, J D; Seinfeld, J H; Ziemann, P J; Jimenez, J L

    2010-04-13

    Organonitrates (ON) are important products of gas-phase oxidation of volatile organic compounds in the troposphere; some models predict, and laboratory studies show, the formation of large, multifunctional ON with vapor pressures low enough to partition to the particle phase. Organosulfates (OS) have also been recently detected in secondary organic aerosol. Despite their potential importance, ON and OS remain a nearly unexplored aspect of atmospheric chemistry because few studies have quantified particulate ON or OS in ambient air. We report the response of a high-resolution time-of-flight aerosol mass spectrometer (AMS) to aerosol ON and OS standards and mixtures. We quantify the potentially substantial underestimation of organic aerosol O/C, commonly used as a metric for aging, and N/C. Most of the ON-nitrogen appears as NO(x)+ ions in the AMS, which are typically dominated by inorganic nitrate. Minor organonitrogen ions are observed although their identity and intensity vary between standards. We evaluate the potential for using NO(x)+ fragment ratios, organonitrogen ions, HNO(3)+ ions, the ammonium balance of the nominally inorganic ions, and comparison to ion-chromatography instruments to constrain the concentrations of ON for ambient datasets, and apply these techniques to a field study in Riverside, CA. OS manifests as separate organic and sulfate components in the AMS with minimal organosulfur fragments and little difference in fragmentation from inorganic sulfate. The low thermal stability of ON and OS likely causes similar detection difficulties for other aerosol mass spectrometers using vaporization and/or ionization techniques with similar or larger energy, which has likely led to an underappreciation of these species. PMID:20194777

  8. Profiling the PM2.5 mass concentration vertical distribution in the boundary layer

    NASA Astrophysics Data System (ADS)

    Tao, Z.; Wang, Z.; Yang, S.; Shan, H.; Ma, X.; Zhang, H.; Zhao, S.; Liu, D.; Xie, C.; Wang, Y.

    2015-12-01

    Fine particle (PM2.5) affects human life and activities directly; the detection of PM2.5 mass concentration profile is very essential due to its practical and scientific meanings (such as, quantifying of air quality and its variability, and improving air quality forecast and assessment). But so far, it is difficult to detect PM2.5 mass concentration profile. The proposed methodology to study the relationship between aerosol extinction coefficient and PM2.5 mass concentration is described, which indicates that the PM2.5 mass concentration profile could be retrieved by combining a charge-coupled device (CCD) side-scatter lidar and a PM2.5 sampling detector. When the relative humidity is less than 70 %, PM2.5 mass concentration is proportional to aerosol extinction coefficient, and then the specific coefficient can be calculated. Using this specific coefficient, aerosol extinction profile is converted to PM2.5 mass concentration profile. Three cases of clean night (on 21 September 2014), pollutant night (on 17 March 2014), and heavy pollutant night (on 13 February 2015) are studied. The characteristic of PM2.5 mass concentration profile in near-ground during these three nights' cases in the western suburb of Hefei city was discussed. The PM2.5 air pollutant concentration is comparatively large in close surface varying with time and altitude. The experiment results show that the CCD side-scatter lidar combined with a PM2.5 detector is an effective and new method to explore pollutant mass concentration profile in near-ground.

  9. Profiling the PM2.5 mass concentration vertical distribution in the boundary layer

    NASA Astrophysics Data System (ADS)

    Tao, Zongming; Wang, Zhenzhu; Yang, Shijun; Shan, Huihui; Ma, Xiaomin; Zhang, Hui; Zhao, Sugui; Liu, Dong; Xie, Chenbo; Wang, Yingjian

    2016-04-01

    Fine particles (PM2.5) affect human life and activities directly; the detection of PM2.5 mass concentration profile is very essential due to its practical and scientific significance (such as the quantification of air quality and its variability as well as the assessment of improving air quality forecast). But so far, it has been difficult to detect PM2.5 mass concentration profile. The proposed methodology to study the relationship between aerosol extinction coefficient and PM2.5 mass concentration is described, which indicates that the PM2.5 mass concentration profile could be retrieved by combining a charge-coupled device (CCD) side-scatter lidar with a PM2.5 sampling detector. When the relative humidity is less than 70 %, PM2.5, mass concentration is proportional to the aerosol extinction coefficient, and then the specific coefficient can be calculated. Through this specific coefficient, aerosol extinction profile is converted to PM2.5 mass concentration profile. Three cases of clean night (on 21 September 2014), pollutant night (on 17 March 2014), and heavy pollutant night (on 13 February 2015) are studied. The characteristics of PM2.5 mass concentration profile at the near-ground level during the cases of these 3 nights in the western suburb of Hefei city were discussed. The PM2.5 air pollutant concentration is comparatively large close to the surface and varies with time and altitude. The experiment results show that the CCD side-scatter lidar combined with a PM2.5 detector is an effective and new method to explore pollutant mass concentration profile at the near-ground level.

  10. Ultrasensitive detection of inhaled organic aerosol particles by accelerator mass spectrometry.

    PubMed

    Parkhomchuk, E V; Gulevich, D G; Taratayko, A I; Baklanov, A M; Selivanova, A V; Trubitsyna, T A; Voronova, I V; Kalinkin, P N; Okunev, A G; Rastigeev, S A; Reznikov, V A; Semeykina, V S; Sashkina, K A; Parkhomchuk, V V

    2016-09-01

    Accelerator mass spectrometry (AMS) was shown to be applicable for studying the penetration of organic aerosols, inhaled by laboratory mice at ultra-low concentration ca. 10(3) cm(-3). We synthesized polystyrene (PS) beads, composed of radiocarbon-labeled styrene, for testing them as model organic aerosols. As a source of radiocarbon we used methyl alcohol with radioactivity. Radiolabeled polystyrene beads were obtained by emulsifier-free emulsion polymerization of synthesized (14)C-styrene initiated by K2S2O8 in aqueous media. Aerosol particles were produced by pneumatic spraying of diluted (14)C-PS latex. Mice inhaled (14)C-PS aerosol consisting of the mix of 10(3) 225-nm particles per 1 cm(3) and 5·10(3) 25-nm particles per 1 cm(3) for 30 min every day during five days. Several millions of 225-nm particles deposited in the lungs and slowly excreted from them during two weeks of postexposure. Penetration of particles matter was also observed for liver, kidneys and brain, but not for a heart. PMID:27281540

  11. Concentration Effects and Ion Properties Controlling the Fractionation of Halides during Aerosol Formation

    NASA Technical Reports Server (NTRS)

    Guzman, Marcelo I.; Athalye, Richa R.; Rodriguez, Jose M.

    2012-01-01

    During the aerosolization process at the sea surface, halides are incorporated into aerosol droplets, where they may play an important role in tropospheric ozone chemistry. Although this process may significantly contribute to the formation of reactive gas phase molecular halogens, little is known about the environmental factors that control how halides selectively accumulate at the air-water interface. In this study, the production of sea spray aerosol is simulated using electrospray ionization (ESI) of 100 nM equimolar solutions of NaCl, NaBr, NaI, NaNO2, NaNO3, NaClO4, and NaIO4. The microdroplets generated are analyzed by mass spectrometry to study the comparative enrichment of anions (f (Isub x-)) and their correlation with ion properties. Although no correlation exists between f (sub x-) and the limiting equivalent ionic conductivity, the correlation coefficient of the linear fit with the size of the anions R(sub x-), dehydration free-energy ?Gdehyd, and polarizability alpha, follows the order: (R(sub x-)(exp -2)) > (R(sub x-)(exp -1)) >(R(sub x-) > delta G(sub dehyd) > alpha. The same pure physical process is observed in H2O and D2O. The factor f (sub x-) does not change with pH (6.8-8.6), counterion (Li+, Na+, K+, and Cs+) substitution effects, or solvent polarity changes in methanol - and ethanol-water mixtures (0 <= xH2O <= 1). Sodium polysorbate 20 surfactant is used to modify the structure of the interface. Despite the observed enrichment of I- on the air-water interface of equimolar solutions, our results of seawater mimic samples agree with a model in which the interfacial composition is increasingly enriched in I- < Br- < Cl- over the oceanic boundary layer due to concentration effects in sea spray aerosol formation.

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

    NASA Astrophysics Data System (ADS)

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

    2011-07-01

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

  13. In situ vertical profiles of aerosol extinction, mass, and composition over the southeast United States during SENEX and SEAC4RS: observations of a modest aerosol enhancement aloft

    NASA Astrophysics Data System (ADS)

    Wagner, N. L.; Brock, C. A.; Angevine, W. M.; Beyersdorf, A.; Campuzano-Jost, P.; Day, D. A.; de Gouw, J. A.; Diskin, G. S.; Gordon, T. D.; Graus, M. G.; Huey, G.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Liu, X.; Markovic, M. Z.; Middlebrook, A. M.; Mikoviny, T.; Peischl, J.; Perring, A. E.; Richardson, M. S.; Ryerson, T. B.; Schwarz, J. P.; Warneke, C.; Welti, A.; Wisthaler, A.; Ziemba, L. D.; Murphy, D. M.

    2015-02-01

    Vertical profiles of submicron aerosol over the southeastern United States (SEUS) during the summertime from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10% larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10% to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary organic aerosol (SOA) aloft to explain the summertime enhancement of AOD (2-3 times greater than winter) over the southeastern United States. In contrast to this hypothesis, the modest enhancement we observed in the transition layer was not dominated by OA and was not a large fraction of the summertime AOD.

  14. Analytical determination of the aerosol organic mass-to-organic carbon ratio.

    PubMed

    El-Zanan, Hazem S; Zielinska, Barbara; Mazzoleni, Lynn R; Hansen, D Alan

    2009-01-01

    Particulate matter (PM) with an aerodynamic diameter < or = 2.5 microm (PM2.5) was collected daily (mid-July 1998 to the end of December 1999) over a 24-hr sampling period in a mixed light industrial-residential area in Atlanta, GA, to provide a subset of data for the Aerosol Research and Inhalation Epidemiology Study (ARIES). This study included the measurement of organic carbon (OC), elemental carbon (EC), and individual organic compounds. OC and EC average mean concentrations were 4.50 +/- 0.33 and 2.08 +/- 0.19 microg/m3, respectively. The ratio of organic matter mass (OM) to OC in PM2.5 aerosols in Atlanta was measured using three different approaches: (1) solvent extract residue gravimetric masses to individual OC concentrations of sequential apolar to polar solvent extracts (dichloromethane, acetone, and water); (2) mass balance of the PM2.5 measured gravimetric mass minus the mass concentrations of the inorganic/elemental constituents to the total OC concentration; and (3) polar organic compound speciation with the concentration weighted ratio to the total OC concentration. We found very good agreement between approach 1 and 2. The average OM/OC ratio calculated from the extract residue mass was 2.14 +/- 0.17. The average OM/OC ratio determined by mass balance was 2.16 +/- 0.43 for the whole period. The concentration weighted ratio calculated from the concentrations of polar organic compounds ranged between 1.55 and 1.72, which was likely a lower limit for the ratio because of the limited number of the polar organic compounds that can be quantified using gas chromatographic methods. We found seasonal differences with an OM/OC range of 1.77 in December 1999 to 2.39 in July 1999. These results suggest that the previously accepted value of 1.4 for the OM/OC ratio was too low even for urban locations during the winter months. Molecular-level speciation of the PM2.5-associated organic compounds showed that the concentrations of the molecular markers for wood

  15. Ambient Observations of Organic Nitrogen Compounds in Submicrometer Aerosols in New York Using High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Zhou, S.; Ge, X.; Xu, J.; Sun, Y.; Zhang, Q.

    2015-12-01

    Organic nitrogen (ON) compounds, which include amines, nitriles, organic nitrates, amides, and N-containing aromatic heterocycles, are an important class of compounds ubiquitously detected in atmospheric particles and fog and cloud droplets. Previous studies indicate that these compounds can make up a significant fraction (20-80%) of the total nitrogen (N) content in atmospheric condensed phases and play important roles in new particle formation and growth and affecting the optical and hygroscopicity of aerosols. In this study, we report the observation of ON compounds in submicrometer particles (PM1) at two locations in New York based on measurements using Aerodyne high-resolution time-of-flight mass spectrometer (HR-ToF-AMS). One study was conducted as part of the US Department of Energy funded Aerosol Lifecyle - Intensive Operation Period (ALC-IOP) campaign at Brookhaven National Lab (BNL, 40.871˚N, 72.89˚W) in summer, 2011 and the other was conducted at the Queen's College (QC) in New York City (NYC) in summer, 2009. We observed a notable amount of N-containing organic fragment ions, CxHyNp+ and CxHyOzNp+, in the AMS spectra of organic aerosols at both locations and found that they were mainly associated with amino functional groups. Compared with results from lab experiments, the C3H8N+ at m/z = 58 was primarily attributed to trimethylamine. In addition, a significant amount of organonitrates was observed at BNL. Positive matrix factorization (PMF) analysis of the high resolution mass spectra (HRMS) of organic aerosols identified a unique nitrogen-enriched OA (NOA) factor with elevated nitrogen-to-carbon (N/C) at both BNL and QC. Analysis of the size distributions, volatility profiles, and correlations with external tracer indicates that acid-base reactions of amino compounds with sulfate and acidic gas were mainly responsible for the formation of amine salts. Photochemical production was also observed to play a role in the formation of NOA. Bivariate polar

  16. Effect of Organic Sea Spray Aerosol on Global and Regional Cloud Condensation Nuclei Concentrations

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Nenes, A.; Moore, R.; Adams, P. J.

    2009-12-01

    Physical processes on the ocean surface (bubble bursting) result in formation of sea spray aerosol. It is now recognized that this aerosol source includes a significant amount of organic matter (O’Dowd et al. 2004). Higher amounts of aerosol lead to higher cloud condensation nuclei (CCN) concentrations, which perturb climate by brightening clouds in what is known as the aerosol indirect effect (Twomey 1977). This work quantifies the marine organic aerosol global emission source as well the effect of the aerosol on CCN by implementing an organic sea spray source function into a series of global aerosol simulations. The new organic sea spray source function correlates satellite retrieved chlorophyll concentrations to fraction of organic matter in sea spray aerosol (O’Dowd et al. 2008). Using this source function, a global marine organic aerosol emission rate of 17.2 Tg C yr-1 is estimated. Effect on CCN concentrations (0.2% supersaturation) is modeled using the Two-Moment Aerosol Sectional (TOMAS) microphysics algorithm coupled to a general circulation model (Adams and Seinfeld 2002). Upon including organic sea spray aerosol in global simulations, changes in CCN concentrations are induced by the changed aerosol composition as well as the ability of the organic matter to serve as surfactants. To explore surfactant effects, surface tension depression data from seawater samples taken near the Georgia coast were applied as a function of carbon concentrations (Moore et al. 2008). Preliminary findings suggest that organic sea spray aerosol exerts a localized influence on CCN(0.2%) concentrations. Surfactant effects appear to be the most important impact of marine organic aerosol on CCN(0.2%), as changes in aerosol composition alone have a weak influence, even in regions of high organic sea spray emissions. 1. O’Dowd, C.D., Facchini, M.C. et al., Nature, 431, (2004) 2. Twomey, S., J. Atmos. Sci., 34, (1977) 3. O’Dowd C.D et al. Geophys. Res. Let., 35, (2008) 4

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

    NASA Astrophysics Data System (ADS)

    Nizkorodov, S.

    2014-12-01

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

  18. Constraining Aerosol Optical Models Using Ground-Based, Collocated Particle Size and Mass Measurements in Variable Air Mass Regimes During the 7-SEAS/Dongsha Experiment

    NASA Technical Reports Server (NTRS)

    Bell, Shaun W.; Hansell, Richard A.; Chow, Judith C.; Tsay, Si-Chee; Wang, Sheng-Hsiang; Ji, Qiang; Li, Can; Watson, John G.; Khlystov, Andrey

    2012-01-01

    During the spring of 2010, NASA Goddard's COMMIT ground-based mobile laboratory was stationed on Dongsha Island off the southwest coast of Taiwan, in preparation for the upcoming 2012 7-SEAS field campaign. The measurement period offered a unique opportunity for conducting detailed investigations of the optical properties of aerosols associated with different air mass regimes including background maritime and those contaminated by anthropogenic air pollution and mineral dust. What appears to be the first time for this region, a shortwave optical closure experiment for both scattering and absorption was attempted over a 12-day period during which aerosols exhibited the most change. Constraints to the optical model included combined SMPS and APS number concentration data for a continuum of fine and coarse-mode particle sizes up to PM2.5. We also take advantage of an IMPROVE chemical sampler to help constrain aerosol composition and mass partitioning of key elemental species including sea-salt, particulate organic matter, soil, non sea-salt sulphate, nitrate, and elemental carbon. Our results demonstrate that the observed aerosol scattering and absorption for these diverse air masses are reasonably captured by the model, where peak aerosol events and transitions between key aerosols types are evident. Signatures of heavy polluted aerosol composed mostly of ammonium and non sea-salt sulphate mixed with some dust with transitions to background sea-salt conditions are apparent in the absorption data, which is particularly reassuring owing to the large variability in the imaginary component of the refractive indices. Extinctive features at significantly smaller time scales than the one-day sample period of IMPROVE are more difficult to reproduce, as this requires further knowledge concerning the source apportionment of major chemical components in the model. Consistency between the measured and modeled optical parameters serves as an important link for advancing remote

  19. Intrinsic and observed concentration-mass relation

    NASA Astrophysics Data System (ADS)

    Rasia, Elena; Meneghetti, M.; Borgani, S.; Ettori, S.

    2012-05-01

    The concentration-mass relation represents a valuable tool to constrain cosmological parameters such as matter density and \\sigma_8. In the last few years, samples of optical and X-ray data led to the conclusion that the observed relation has a higher normalization and slope than predicted by dark-matter only simulations. In this work, we explore whether this disagreement is real and, if so, why it exists. To this purpose, we consider 30 clusters simulated by progressively increasing the simulation complexity: (i) dark-matter only, (ii) non-radiative hydrodynamics, (iii) adding cooling, star-formation and feedback by Supernovae, (iv) further adding feedback by AGN. We produced X-ray and optical synthetic catalogues to derive the concentration-mass relation following an observational approach. We find that even if cooling has the effect of steepening the concentration-mass relation with respect to the DM-only simulations, the introduction of AGN makes this difference small (5-10%). A larger variation is expected when reducing the radial range over which density profiles are fitted to a NFW profile. In particular if the external radius is about half $R_{500}$ the slope can double its value. Therefore, observations, suffering from background contamination, are more inclined to detect a steeper c-M relations. Finally, the strong lensing analysis of the synthetic catalogues shows a bias leading to an over-estimate the concentration of small objects. We acknowledge financial contribution from contracts ASI-INAF I/023/05/0, ASI-INAF I/088/06/0, PRIN-INAF-2009 Grant "Towards an Italian Network for Computational Cosmology", INFN PD51, the Michigan Society of Fellow, and the Michigan Center for Theoretical Physics.

  20. Compositional and Optical Properties of Titan Haze Analogs Using Aerosol Mass Spectrometry, Photoacoustic Spectroscopy and Cavity Ring-Down Spectroscopy

    NASA Astrophysics Data System (ADS)

    Ugelow, M.; Zarzana, K. J.; Tolbert, M. A.

    2015-12-01

    The organic haze that surrounds Saturn's moon Titan is formed through the photolysis and electron initiated dissociation of methane and nitrogen. The chemical pathways leading to haze formation and the resulting haze optical properties are still highly uncertain. Here we examine the compositional and optical properties of Titan haze aerosol analogs. By studying these properties together, the impact of haze on Titan's radiative balance can be better understood. The aerosol analogs studied are produced from different initial methane concentrations (0.1, 2 and 10% CH4) using spark discharge excitation. To determine the complex refractive index of the aerosol, we combine two spectroscopic techniques, one that measures absorption and one that measures extinction: photoacoustic spectroscopy coupled with cavity ring-down spectroscopy (PASCaRD). This technique provides the benefit of a high precision determination of the imaginary component of the refractive index (k), along with the highly sensitive determination of the real component of the refractive index (n). The refractive indices are retrieved at two wavelengths, 405 and 532 nm, using the PASCaRD system. To yield aerosol composition, quadrupole aerosol mass spectrometry is used. Compositional information is obtained from a technique that uses isotopically labeled and unlabeled methane gas. I will present preliminary data on the complex refractive indices of Titan aerosol analogs at both wavelengths, in conjunction with the aerosol composition as a percent by weight of carbon, nitrogen and hydrogen. The correlation of optical and chemical properties should be useful for remote sensing instruments probing Titan haze.

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

    NASA Astrophysics Data System (ADS)

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

    2010-05-01

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

  2. Concentrations and sources of organic carbon aerosols in the free troposphere over North America

    NASA Astrophysics Data System (ADS)

    Heald, Colette L.; Jacob, Daniel J.; Turquety, SolèNe; Hudman, Rynda C.; Weber, Rodney J.; Sullivan, Amy P.; Peltier, Richard E.; Atlas, Eliot L.; de Gouw, Joost A.; Warneke, Carsten; Holloway, John S.; Neuman, J. Andrew; Flocke, Frank M.; Seinfeld, John H.

    2006-12-01

    Aircraft measurements of water-soluble organic carbon (WSOC) aerosol over NE North America during summer 2004 (ITCT-2K4) are simulated with a global chemical transport model (GEOS-Chem) to test our understanding of the sources of organic carbon (OC) aerosol in the free troposphere (FT). Elevated concentrations were observed in plumes from boreal fires in Alaska and Canada. WSOC aerosol concentrations outside of these plumes average 0.9 ± 0.9 μg C m-3 in the FT (2-6 km). The corresponding model value is 0.7 ± 0.6 μg C m-3, including 42% from biomass burning, 36% from biogenic secondary organic aerosol (SOA), and 22% from anthropogenic emissions. Previous OC aerosol observations over the NW Pacific in spring 2001 (ACE-Asia) averaged 3.3 ± 2.8 μg C m-3 in the FT, compared to a model value of 0.3 ± 0.3 μg C m-3. WSOC aerosol concentrations in the boundary layer (BL) during ITCT-2K4 are consistent with OC aerosol observed at the IMPROVE surface network. The model is low in the boundary layer by 30%, which we attribute to secondary formation at a rate comparable to primary anthropogenic emission. Observed WSOC aerosol concentrations decrease by a factor of 2 from the BL to the FT, as compared to a factor of 10 decrease for sulfate, indicating that most of the WSOC aerosol in the FT originates in situ. Despite reproducing mean observed WSOC concentrations in the FT to within 25%, the model cannot account for the variance in the observations (R = 0.21). Covariance analysis of FT WSOC aerosol with other measured chemical variables suggests an aqueous-phase mechanism for SOA generation involving biogenic precursors.

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

  4. A balloon-borne aerosol spectrometer for high altitude low aerosol concentration measurements

    SciTech Connect

    Brown, G.S. ); Weiss, R.E. )

    1990-08-01

    Funded by Air Force Wright Aeronautical Laboratory, a new balloon-borne high altitude aerosol spectrometer, for the measurement of cirrus cloud ice crystals, has been developed and successfully flown by Sandia National Laboratories and Radiance Research. This report (1) details the aerosol spectrometer design and construction, (2) discusses data transmission and decoding, (3) presents data collected on three Florida flights in tables and plots. 2 refs., 11 figs., 3 tabs.

  5. Characteristics of aerosols and mass closure study at two WMO GAW regional background stations in eastern China

    NASA Astrophysics Data System (ADS)

    Yan, Peng; Zhang, Renjian; Huan, Ning; Zhou, Xiuji; Zhang, Yangmei; Zhou, Huaigang; Zhang, Leiming

    2012-12-01

    In the summer and winter of 2004 and 2005, size-segregated atmospheric aerosols were sampled with modified Andersen KA200 Multi-stage impactor at two regional background stations in the eastern China, the Shangdianzi station (SDZ) in the suburb of Beijing and the Lin'An station (LA) in the Yangtze river delta region, both are WMO Global Atmospheric Watch station, which represent the regional background of air pollutions of the two rapid developing economical zone of China, the Yangtze River Delta region (YRD) and Beijing-Tianjin region. The aerosol mass size distributions, ionic compositions, organic and elemental carbon (OC and EC), and elemental components were analyzed. The mass concentrations for TSP (total suspend particle), PM11 (aerodynamic diameter less than 11 μm), and PM2.1 (aerodynamic diameter less than 2.1 μm) at both sites showed obviously different between the winter and summer, with higher mass concentrations measured in the winter time. All seasonal mean mass concentrations of PM2.1 accounted for over 50% of PM11 at both sites. The aerosol mass closure study indicated that the total mass concentration reconstructed from the aerosol chemical composition agreed well with the measured gravimetric mass at the two stations. The fine aerosol particles at the two stations were composed mainly of sulfate and organic matter. In the summer, more than half of the PM2.1 mass was sulfate, suggesting a dominant contribution of secondary aerosol to the fine particles in these two regions. In the winter, the contribution of nitrate to the fine particles increased significantly due to the lower volatile losses under the cold weather. The proportions of soil type components in the PM2.1 showed similar magnitude in the winter and summer at Lin'An station but significant seasonal differences with higher fractions in the winter at Shangdianzi station. On average EC accounted for about 2%-6% of the fine particle mass (PM2.1) at both sites with proportionally lower EC

  6. Pattern of aerosol mass loading and chemical composition over the atmospheric environment of an urban coastal station

    NASA Astrophysics Data System (ADS)

    Bindu, G.; Nair, Prabha R.; Aryasree, S.; Hegde, Prashant; Jacob, Salu

    2016-02-01

    Aerosol sampling was carried out at four locations in and around Cochin (9°58‧ N, 76°17‧ E), an urban area, located on the southwest coast of India. The gravimetric estimates of aerosol mass loading showed wide range from 78 μg m-3 to >450 μg m-3, occasionally reaching values >500 μg m-3, associated with regional source characteristics. Most of the values were above the air quality standard. Both boundary layer and synoptic scale airflow pattern play role in the temporal features in aerosol mass loading and chemical composition. Chemical analysis of the aerosol samples were done for anionic species viz; F-, Cl-, Br-, NO2-,   NO3-,   PO43-,   SO42- and metallic/cationic species viz; Na, Ca, K, Mg, NH4+, Fe, Al, Cu, Mg, Pb, etc using Ion Chromatography, Atomic Absorption Spectroscopy (AAS) and Inductively Coupled Plasma- Atomic Emission Spectroscopy (ICP-AES). At all the locations, extremely high mass concentration of SO42- was observed with the mean value of 13±6.4 μg m-3 indicating the strong anthropogenic influence. Statistical analysis of the chemical composition data was carried out and the principal factors presented. Seasonal variation of these chemical species along with their percentage contributions and regional variations were also examined. Increase in level of Na in aerosol samples indicated the influence of monsoonal activity. Most of the species showed mass concentrations well above those measured over another coastal site Thiruvananthapuram (8°29‧ N, 76°57‧ E) situated ~220 km south of Cochin revealing the highly localized aerosol features.

  7. Field-deployable, high-resolution, time-of-flight aerosol mass spectrometer.

    PubMed

    DeCarlo, Peter F; Kimmel, Joel R; Trimborn, Achim; Northway, Megan J; Jayne, John T; Aiken, Allison C; Gonin, Marc; Fuhrer, Katrin; Horvath, Thomas; Docherty, Kenneth S; Worsnop, Doug R; Jimenez, Jose L

    2006-12-15

    The development of a new high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is reported. The high-resolution capabilities of this instrument allow the direct separation of most ions from inorganic and organic species at the same nominal m/z, the quantification of several types of organic fragments (CxHy, CxHyOz, CxHyNp, CxHyOzNp), and the direct identification of organic nitrogen and organosulfur content. This real-time instrument is field-deployable, and its high time resolution (0.5 Hz has been demonstrated) makes it well-suited for studies in which time resolution is critical, such as aircraft studies. The instrument has two ion optical modes: a single-reflection configuration offers higher sensitivity and lower resolving power (up to approximately 2100 at m/z 200), and a two-reflectron configuration yields higher resolving power (up to approximately 4300 at m/z 200) with lower sensitivity. The instrument also allows the determination of the size distributions of all ions. One-minute detection limits for submicrometer aerosol are <0.04 microg m(-3) for all species in the high-sensitivity mode and <0.4 microg m(-3) in the high-resolution mode. Examples of ambient aerosol data are presented from the SOAR-1 study in Riverside, CA, in which the spectra of ambient organic species are dominated by CxHy and CxHyOz fragments, and different organic and inorganic fragments at the same nominal m/z show different size distributions. Data are also presented from the MIRAGE C-130 aircraft study near Mexico City, showing high correlation with independent measurements of surrogate aerosol mass concentration. PMID:17165817

  8. Factors affecting the indoor concentrations of carbonaceous aerosols of outdoor origin

    SciTech Connect

    Lunden, Melissa M.; Kirchstetter, Thomas W.; Thatcher, Tracy L.; Hering, Susanne V.; Brown, Nancy J.

    2007-06-25

    A field study was conducted in an unoccupied single story residence in Clovis, California to provide data to address issues important to assess the indoor exposure to particles of outdoor origin. Measurements of black and organic carbonaceous aerosols were performed using a variety of methods, resulting in both near real-time measurements as well as integrated filter based measurements. Comparisons of the different measurement methods show that it is crucial to account for gas phase adsorption artifacts when measuring organic carbon (OC). Measured concentrations affected by the emissions of organic compounds sorbed to indoor surfaces imply a higher degree of infiltration of outdoor organic carbon aerosols into the indoor environment for our unoccupied house. Analysis of the indoor and outdoor data for black carbon (BC) aerosols show that, on average, the indoor concentration of black carbon aerosols behaves in a similar manner to sulfate aerosols. In contrast, organic carbon aerosols are subject to chemical transformations indoors that, for our unoccupied home, resulted in lower indoor OC concentrations than would be expected by physical loss mechanisms alone. These results show that gas to particle partitioning of organic compounds, as well as gas to surface interactions within the residence, are an important process governing the indoor concentration to OC aerosols of outdoor origin.

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  10. Atmospheric aerosols: increased concentrations during the last decade.

    PubMed

    Peterson, J T; Bryson, R A

    1968-10-01

    Atmospheric turbidity values calculated each month from solar radiation observations at MaunaLoa Observatory, Hawaii, show an increase of aerosols from 1958 through the present. These data indicate that either the effects of the Mount Agung eruption are still being observed or a longer-term trend of increasing turbidity is in evidence. PMID:4877369

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

    NASA Astrophysics Data System (ADS)

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

    2005-10-01

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

  12. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2001-11-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-07-01

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

  15. Mass analysis of charged aerosol particles in NLC and PMSE during the ECOMA/MASS campaign

    NASA Astrophysics Data System (ADS)

    Robertson, S.; Horányi, M.; Knappmiller, S.; Sternovsky, Z.; Holzworth, R.; Shimogawa, M.; Friedrich, M.; Torkar, K.; Gumbel, J.; Megner, L.; Baumgarten, G.; Latteck, R.; Rapp, M.; Hoppe, U.-P.; Hervig, M. E.

    2009-03-01

    MASS (Mesospheric Aerosol Sampling Spectrometer) is a multichannel mass spectrometer for charged aerosol particles, which was flown from the Andøya Rocket Range, Norway, through NLC and PMSE on 3 August 2007 and through PMSE on 6 August 2007. The eight-channel analyzers provided for the first time simultaneous measurements of the charge density residing on aerosol particles in four mass ranges, corresponding to ice particles with radii <0.5 nm (including ions), 0.5-1 nm, 1-2 nm, and >3 nm (approximately). Positive and negative particles were recorded on separate channels. Faraday rotation measurements provided electron density and a means of checking charge density measurements made by the spectrometer. Additional complementary measurements were made by rocket-borne dust impact detectors, electric field booms, a photometer and ground-based radar and lidar. The MASS data from the first flight showed negative charge number densities of 1500-3000 cm-3 for particles with radii >3 nm from 83-88 km approximately coincident with PMSE observed by the ALWIN radar and NLC observed by the ALOMAR lidar. For particles in the 1-2 nm range, number densities of positive and negative charge were similar in magnitude (~2000 cm-3) and for smaller particles, 0.5-1 nm in radius, positive charge was dominant. The occurrence of positive charge on the aerosol particles of the smallest size and predominately negative charge on the particles of largest size suggests that nucleation occurs on positive condensation nuclei and is followed by collection of negative charge during subsequent growth to larger size. Faraday rotation measurements show a bite-out in electron density that increases the time for positive aerosol particles to be neutralized and charged negatively. The larger particles (>3 nm) are observed throughout the NLC region, 83-88 km, and the smaller particles are observed primarily at the high end of the range, 86-88 km. The second flight into PMSE alone at 84-88 km, found only

  16. Direct measurements of mass-specific optical cross sections of single-component aerosol mixtures.

    PubMed

    Radney, James G; Ma, Xiaofei; Gillis, Keith A; Zachariah, Michael R; Hodges, Joseph T; Zangmeister, Christopher D

    2013-09-01

    The optical properties of atmospheric aerosols vary widely, being dependent upon particle composition, morphology, and mixing state. This diversity and complexity of aerosols motivates measurement techniques that can discriminate and quantify a variety of single- and multicomponent aerosols that are both internally and externally mixed. Here, we present a new combination of techniques to directly measure the mass-specific extinction and absorption cross sections of laboratory-generated aerosols that are relevant to atmospheric studies. Our approach employs a tandem differential mobility analyzer, an aerosol particle mass analyzer, cavity ring-down and photoacoustic spectrometers, and a condensation particle counter. This suite of instruments enables measurement of aerosol particle size, mass, extinction and absorption coefficients, and aerosol number density, respectively. Taken together, these observables yield the mass-specific extinction and absorption cross sections without the need to model particle morphology or account for sample collection artifacts. Here we demonstrate the technique in a set of case studies which involve complete separation of aerosol by charge, separation of an external mixture by mass, and discrimination between particle types by effective density and single-scattering albedo. PMID:23875772

  17. Contribution of isoprene-derived organosulfates to free tropospheric aerosol mass.

    PubMed

    Froyd, K D; Murphy, S M; Murphy, D M; de Gouw, J A; Eddingsaas, N C; Wennberg, P O

    2010-12-14

    Recent laboratory studies have demonstrated that isoprene oxidation products can partition to atmospheric aerosols by reacting with condensed phase sulfuric acid, forming low-volatility organosulfate compounds. We have identified organosulfate compounds in free tropospheric aerosols by single particle mass spectrometry during several airborne field campaigns. One of these organosulfates is identified as the sulfate ester of IEPOX, a second generation oxidation product of isoprene. The patterns of IEPOX sulfate ester in ambient data generally followed the aerosol acidity and NO(x) dependence established by laboratory studies. Detection of the IEPOX sulfate ester was most sensitive using reduced ionization laser power, when it was observed in up to 80% of particles in the tropical free troposphere. Based on laboratory mass calibrations, IEPOX added > 0.4% to tropospheric aerosol mass in the remote tropics and up to 20% in regions downwind of isoprene sources. In the southeastern United States, when acidic aerosol was exposed to fresh isoprene emissions, accumulation of IEPOX increased aerosol mass by up to 3%. The IEPOX sulfate ester is therefore one of the most abundant single organic compounds measured in atmospheric aerosol. Our data show that acidity-dependent IEPOX uptake is a mechanism by which anthropogenic SO(2) and marine dimethyl sulfide emissions generate secondary biogenic aerosol mass throughout the troposphere. PMID:21098310

  18. Characterization of ice-nucleating bacteria using on-line electron impact ionization aerosol mass spectrometry.

    PubMed

    Wolf, R; Slowik, J G; Schaupp, C; Amato, P; Saathoff, H; Möhler, O; Prévôt, A S H; Baltensperger, U

    2015-04-01

    The mass spectral signatures of airborne bacteria were measured and analyzed in cloud simulation experiments at the AIDA (Aerosol Interaction and Dynamics in the Atmosphere) facility. Suspensions of cultured cells in pure water were sprayed into the aerosol and cloud chambers forming an aerosol which consisted of intact cells, cell fragments and residual particles from the agar medium in which the bacteria were cultured. The aerosol particles were analyzed with a high-resolution time-of-flight aerosol mass spectrometer equipped with a newly developed PM2.5 aerodynamic lens. Positive matrix factorization (PMF) using the multilinear engine (ME-2) source apportionment was applied to deconvolve the bacteria and agar mass spectral signatures. The bacteria mass fraction contributed between 75 and 95% depending on the aerosol generation, with the remaining mass attributed to agar. We present mass spectra of Pseudomonas syringae and Pseudomonas fluorescens bacteria typical for ice-nucleation active bacteria in the atmosphere to facilitate the distinction of airborne bacteria from other constituents in ambient aerosol, e.g. by PMF/ME-2 source apportionment analyses. Nitrogen-containing ions were the most salient feature of the bacteria mass spectra, and a combination of C4 H8 N(+) (m/z 70) and C5 H12 N(+) (m/z 86) may be used as marker ions. PMID:26149110

  19. Relationships among particle number, surface area, and respirable mass concentrations in automotive engine manufacturing.

    PubMed

    Heitbrink, William A; Evans, Douglas E; Ku, Bon Ki; Maynard, Andrew D; Slavin, Thomas J; Peters, Thomas M

    2009-01-01

    This study investigated the relationships between particle number, surface area, and respirable mass concentration measured simultaneously in a foundry and an automotive engine machining and assembly center. Aerosol concentrations were measured throughout each plant with a condensation particle counter for number concentration, a diffusion charger for active surface area concentration, and an optical particle counter for respirable mass concentration. At selected locations, particle size distributions were characterized with the optical particle counter and an electrical low pressure impactor. Statistical analyses showed that active surface area concentration was correlated with ultrafine particle number concentration and weakly correlated with respirable mass concentration. Correlation between number and active surface area concentration was stronger during winter (R2 = 0.6 for both plants) than in the summer (R2 = 0.38 and 0.36 for the foundry and engine plant respectively). The stronger correlation in winter was attributed to use of direct-fire gas fired heaters that produced substantial numbers of ultrafine particles with a modal diameter between 0.007 and 0.023 mu m. These correlations support findings obtained through theoretical analysis. Such analysis predicts that active surface area increasingly underestimates geometric surface area with increasing particle size, particularly for particles larger than 100 nm. Thus, a stronger correlation between particle number concentration and active surface area concentration is expected in the presence of high concentrations of ultrafine particles. In general, active surface area concentration may be a concentration metric that is distinct from particle number concentration and respirable mass concentration. For future health effects or toxicological studies involving nano-materials or ultrafine aerosols, this finding needs to be considered, as exposure metrics may influence data interpretation. PMID:18982535

  20. Potential source identification for aerosol concentrations over a site in Northwestern India

    NASA Astrophysics Data System (ADS)

    Payra, Swagata; Kumar, Pramod; Verma, Sunita; Prakash, Divya; Soni, Manish

    2016-03-01

    The collocated measurements of aerosols size distribution (ASD) and aerosol optical thickness (AOT) are analyzed simultaneously using Grimm aerosol spectrometer and MICROTOP II Sunphotometer over Jaipur, capital of Rajasthan in India. The contrast temperature characteristics during winter and summer seasons of year 2011 are investigated in the present study. The total aerosol number concentration (TANC, 0.3-20 μm) during winter season was observed higher than in summer time and it was dominated by fine aerosol number concentration (FANC < 2 μm). Particles smaller than 0.8 μm (at aerodynamic size) constitute ~ 99% of all particles in winter and ~ 90% of particles in summer season. However, particles greater than 2 μm contribute ~ 3% and ~ 0.2% in summer and winter seasons respectively. The aerosols optical thickness shows nearly similar AOT values during summer and winter but corresponding low Angstrom Exponent (AE) values during summer than winter, respectively. In this work, Potential Source Contribution Function (PSCF) analysis is applied to identify locations of sources that influenced concentrations of aerosols over study area in two different seasons. PSCF analysis shows that the dust particles from Thar Desert contribute significantly to the coarse aerosol number concentration (CANC). Higher values of the PSCF in north from Jaipur showed the industrial areas in northern India to be the likely sources of fine particles. The variation in size distribution of aerosols during two seasons is clearly reflected in the log normal size distribution curves. The log normal size distribution curves reveals that the particle size less than 0.8 μm is the key contributor in winter for higher ANC.

  1. [Characteristics of Number Concentration Size Distributions of Aerosols Under Processes in Beijing].

    PubMed

    Su, Jie; Zhao, Pu-sheng; Chen, Yi-na

    2016-04-15

    The aerosol number concentration size distributions were measured by a Wide-Range Particle Spectrometer (WPS-1000XP) at an urban site of Beijing from 2012 to 2014; and the characteristics of the size distributions in different seasons and weather conditions were discussed. The results showed that the daily average number concentration of Aitken mode aerosols was highest in the spring and lowest in the autumn; the daily average number concentration of accumulation mode aerosols was bigher in the spring and winter, while lowest in summer; and the average concentration of coarse mode was highest during the winter. The Aitken mode particles had the most significant diurnal variations resulted from the traffic sources and the summer photochemical reactions. In the spring, autumn and winter, the number concentrations of accumulation mode of the nighttime was higher than that of the daytime. The coarse mode particles did not have obvious diurnal variation. During the heavy pollution process, the accumulation mode aerosols played a decisive role in PM₂.₅ concentrations and was usually removed by the north wind. The precipitation could effectively eliminate the coarse mode particles, but it bad no obvious effect on the accumulation mode particles under small speed wind and zero speed wind. During the dust process, the concentrations of coarse mode particles increased significantly, while the accumulation mode aerosol concentration was obviously decreased. PMID:27548939

  2. High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years

    NASA Astrophysics Data System (ADS)

    Weber, Rodney J.; Guo, Hongyu; Russell, Armistead G.; Nenes, Athanasios

    2016-04-01

    Particle acidity affects aerosol concentrations, chemical composition and toxicity. Sulfate is often the main acid component of aerosols, and largely determines the acidity of fine particles under 2.5 μm in diameter, PM2.5. Over the past 15 years, atmospheric sulfate concentrations in the southeastern United States have decreased by 70%, whereas ammonia concentrations have been steady. Similar trends are occurring in many regions globally. Aerosol ammonium nitrate concentrations were assumed to increase to compensate for decreasing sulfate, which would result from increasing neutrality. Here we use observed gas and aerosol composition, humidity, and temperature data collected at a rural southeastern US site in June and July 2013 (ref. ), and a thermodynamic model that predicts pH and the gas-particle equilibrium concentrations of inorganic species from the observations to show that PM2.5 at the site is acidic. pH buffering by partitioning of ammonia between the gas and particle phases produced a relatively constant particle pH of 0-2 throughout the 15 years of decreasing atmospheric sulfate concentrations, and little change in particle ammonium nitrate concentrations. We conclude that the reductions in aerosol acidity widely anticipated from sulfur reductions, and expected acidity-related health and climate benefits, are unlikely to occur until atmospheric sulfate concentrations reach near pre-anthropogenic levels.

  3. Detection of brake wear aerosols by aerosol time-of-flight mass spectrometry

    NASA Astrophysics Data System (ADS)

    Beddows, D. C. S.; Dall'Osto, M.; Olatunbosun, O. A.; Harrison, Roy M.

    2016-03-01

    Brake dust particles were characterised using an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) operated using two inlet configurations, namely the aerodynamic lens (AFL) inlet and countersunk nozzle inlet. Laboratory studies show that dust particles are characterised by mass spectra containing ions deriving from Fe and Ba and although highly correlated to each other, the Fe and Ba signals were mostly detected using the nozzle inlet with relatively high laser desorption energies. When using the AFL, only [56Fe] and [-88FeO2] ions were observed in brake dust spectra generated using lower laser desorption pulse energies, and only above 0.75 mJ was the [138Ba] ion detected. When used with the preferred nozzle inlet configuration, the [-88FeO2] peak was considered to be the more reliable tracer peak, because it is not present in other types of dust (mineral, tyre, Saharan etc). As shown by the comparison with ambient data from a number of locations, the aerodynamic lens is not as efficient in detecting brake wear particles, with less than 1% of sampled particles attributed to brake wear. Five field campaigns within Birmingham (background, roadside (3) and road tunnel) used the nozzle inlet and showed that dust particles (crustal and road) accounted for between 3.1 and 65.9% of the particles detected, with the remaining particles being made up from varying percentages of other constituents.

  4. Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site

    NASA Astrophysics Data System (ADS)

    Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

    2012-08-01

    Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban Environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter <2.5 μm) resolved Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie FP7-EU framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the unique approach used is the simultaneous PIXE measurements at two monitoring sites: urban background (UB) and a street canyon traffic road site (RS). Elements related to primary non exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (secondary sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non exhaust brake dust (Fe-Cu) - 7%), and three types industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%). The validity of the PMF solution of the PIXE data is supported by strong correlations with external single particle mass spectrometry measurements. Beside apportioning the aerosol sources, some important air quality related conclusions can be drawn about the PM2.5 fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both monitoring sites at similar concentrations regardless their different ventilation conditions; (2) by contrast, local industrial

  5. New approach using lidar measurements to characterize spatiotemporal aerosol mass distribution in an underground railway station in Paris

    NASA Astrophysics Data System (ADS)

    Raut, J.-C.; Chazette, P.; Fortain, A.

    For the first time eye safe lidar measurements were performed at 355 nm simultaneously to in situ measurements in an underground station so as to test the potential interest of active remote sensing measurements to follow the spatiotemporal evolution of aerosol content inside such a confined microenvironment. The purpose of this paper is to describe different methods enabling the conversion of lidar-derived aerosol extinction coefficient into aerosol mass concentrations (PM 2.5 and PM 10). A theoretical method based on a well marked linear regression between mass concentrations simulated from the size distribution and extinction coefficients retrieved from Mie calculations provides averaged mass to optics' relations over the campaign for traffic (6.47 × 10 5 μg m -2) or no traffic conditions (3.73 × 10 5 μg m -2). Two empirical methods enable to significantly reduce CPU time. The first one is based upon the knowledge of size distribution measurements and scattering coefficients from nephelometer and allows retrieving mass to optics' relations for well determined periods or particular traffic conditions, like week-ends, with a good accuracy. The second method, that is more direct, is simply based on the ratio between TEOM concentrations and extinction coefficients obtained from nephelometer. This method is easy to set up but is not suitable for nocturnal measurements where PM stabilization time is short. Lidar signals thus converted into PM concentrations from those approaches with a fine accuracy (30%) provide a spatiotemporal distribution of concentrations in the station. This highlights aerosol accumulation in one side of the station, which can be explained by air displacement from the tunnel entrance. Those results allow expecting a more general use of lidar measurement to survey indoor air quality.

  6. Characterization of submicron aerosols during a serious pollution month in Beijing (2013) using an aerodyne high-resolution aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Zhang, J. K.; Sun, Y.; Liu, Z. R.; Ji, D. S.; Hu, B.; Liu, Q.; Wang, Y. S.

    2013-07-01

    In January 2013, Beijing experienced several serious haze events. To achieve a better understanding of the characteristics, sources and processes of aerosols during this month, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at an urban site between 1 January and 1 February 2013 to obtain the size-resolved chemical composition of non-refractory submicron particles (NR-PM1). During this period, the mean measured NR-PM1 mass concentration was 87.4 μg m-3 and was composed of organics (49.8%), sulfate (21.4%), nitrate (14.6%), ammonium (10.4%), and chloride (3.8%). Moreover, inorganic matter, such as sulfate and nitrate comprised an increasing fraction of the NR-PM1 load as NR-PM1 loading increased, denoting their key roles in particulate pollution during this month. The average size distributions of the species were all dominated by an accumulation mode peaking at approximately 600 nm in vacuum aerodynamic diameter and organics characterized by an additional smaller size (∼200 nm). Elemental analyses showed that the average O/C, H/C, and N/C (molar ratio) of organic matter were 0.34, 1.44 and 0.015, respectively, corresponding to an OM/OC ratio (mass ratio of organic matter to organic carbon) of 1.60. Positive matrix factorization (PMF) analyses of the high-resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., oxygenated organic aerosols (OOA), cooking-related (COA), nitrogen-containing (NOA) and hydrocarbon-like (HOA), which on average accounted for 40.0, 23.4, 18.1 and 18.5% of the total organic mass, respectively. Back trajectory clustering analyses indicated that the WNW air masses were associated with the highest NR-PM1 pollution during the campaign. Aerosol particles in southern air masses were especially rich in inorganic and oxidized organic species, whereas northern air masses contained a large fraction of primary species.

  7. In situ vertical profiles of aerosol extinction, mass, and composition over the southeast United States during SENEX and SEAC4RS: observations of a modest aerosol enhancement aloft

    NASA Astrophysics Data System (ADS)

    Wagner, N. L.; Brock, C. A.; Angevine, W. M.; Beyersdorf, A.; Campuzano-Jost, P.; Day, D.; de Gouw, J. A.; Diskin, G. S.; Gordon, T. D.; Graus, M. G.; Holloway, J. S.; Huey, G.; Jimenez, J. L.; Lack, D. A.; Liao, J.; Liu, X.; Markovic, M. Z.; Middlebrook, A. M.; Mikoviny, T.; Peischl, J.; Perring, A. E.; Richardson, M. S.; Ryerson, T. B.; Schwarz, J. P.; Warneke, C.; Welti, A.; Wisthaler, A.; Ziemba, L. D.; Murphy, D. M.

    2015-06-01

    Vertical profiles of submicron aerosol from in situ aircraft-based measurements were used to construct aggregate profiles of chemical, microphysical, and optical properties. These vertical profiles were collected over the southeastern United States (SEUS) during the summer of 2013 as part of two separate field studies: the Southeast Nexus (SENEX) study and the Study of Emissions and Atmospheric Composition, Clouds, and Climate Coupling by Regional Surveys (SEAC4RS). Shallow cumulus convection was observed during many profiles. These conditions enhance vertical transport of trace gases and aerosol and create a cloudy transition layer on top of the sub-cloud mixed layer. The trace gas and aerosol concentrations in the transition layer were modeled as a mixture with contributions from the mixed layer below and the free troposphere above. The amount of vertical mixing, or entrainment of air from the free troposphere, was quantified using the observed mixing ratio of carbon monoxide (CO). Although the median aerosol mass, extinction, and volume decreased with altitude in the transition layer, they were ~10 % larger than expected from vertical mixing alone. This enhancement was likely due to secondary aerosol formation in the transition layer. Although the transition layer enhancements of the particulate sulfate and organic aerosol (OA) were both similar in magnitude, only the enhancement of sulfate was statistically significant. The column integrated extinction, or aerosol optical depth (AOD), was calculated for each individual profile, and the transition layer enhancement of extinction typically contributed less than 10 % to the total AOD. Our measurements and analysis were motivated by two recent studies that have hypothesized an enhanced layer of secondary aerosol aloft to explain the summertime enhancement of AOD (2-3 times greater than winter) over the southeastern United States. The first study attributes the layer aloft to secondary organic aerosol (SOA) while

  8. Using Raman-lidar-based regularized microphysical retrievals and Aerosol Mass Spectrometer measurements for the characterization of biomass burning aerosols

    NASA Astrophysics Data System (ADS)

    Samaras, Stefanos; Nicolae, Doina; Böckmann, Christine; Vasilescu, Jeni; Binietoglou, Ioannis; Labzovskii, Lev; Toanca, Florica; Papayannis, Alexandros

    2015-10-01

    In this work we extract the microphysical properties of aerosols for a collection of measurement cases with low volume depolarization ratio originating from fire sources captured by the Raman lidar located at the National Institute of Optoelectronics (INOE) in Bucharest. Our algorithm was tested not only for pure smoke but also for mixed smoke and urban aerosols of variable age and growth. Applying a sensitivity analysis on initial parameter settings of our retrieval code was proved vital for producing semi-automatized retrievals with a hybrid regularization method developed at the Institute of Mathematics of Potsdam University. A direct quantitative comparison of the retrieved microphysical properties with measurements from a Compact Time of Flight Aerosol Mass Spectrometer (CToF-AMS) is used to validate our algorithm. Microphysical retrievals performed with sun photometer data are also used to explore our results. Focusing on the fine mode we observed remarkable similarities between the retrieved size distribution and the one measured by the AMS. More complicated atmospheric structures and the factor of absorption appear to depend more on particle radius being subject to variation. A good correlation was found between the aerosol effective radius and particle age, using the ratio of lidar ratios (LR: aerosol extinction to backscatter ratios) as an indicator for the latter. Finally, the dependence on relative humidity of aerosol effective radii measured on the ground and within the layers aloft show similar patterns.

  9. MULTIWAVELENGTH TRANSMISSOMETER FOR MEASURING MASS CONCENTRATION OF PARTICULATE EMISSIONS

    EPA Science Inventory

    A multiwavelength transmissometer potentially capable of making near-real-time measurements of particulate mass concentration in industrial stacks was developed. A computer program is employed to interpret the transmissometer data and translate the results into mass concentration...

  10. The importance of aerosol composition and mixing state on predicted CCN concentration and the variation of the importance with atmospheric processing of aerosol

    SciTech Connect

    Wang, J.; Cubison, M.; Aiken, A.; Jimenez, J.; Collins, D.; Gaffney, J.; Marley, N.

    2010-03-15

    The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols are complex and heterogeneous mixtures of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition and mixing state are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban super-site in Mexico City during MILAGRO are analyzed. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The biases associated with these simplifications are compared for different supersaturations, and the variation of the biases is examined as a function of aerosol age. The results show that the simplification of internally mixed, size

  11. The Role of Atmospheric Aerosol Concentration on Deep Convective Precipitation: Cloud-resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, W.-K.; Li, X.; Khain, A.; Mastsui, T.; Lang, S.; Simpson, J.

    2007-01-01

    Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 20011. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds NRC [2001]." The aerosol effect on clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path and the "semi-direct" effect on cloud coverage. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect, is even more complex, especially for mixed-phase convective clouds. ln this paper, a cloud-resolving model (CRM) with detailed spectral-bin microphysics was used to examine the effect of aerosols on three different deep convective cloud systems that developed in different geographic locations: South Florida, Oklahoma and the Central Pacific. In all three cases, rain reaches the ground earlier for the low CCN (clean) case. Rain suppression is also evident in all three cases with high CCN (dirty) case. However, this suppression only occurs during the first hour of the simulations. During the mature stages of the simulations, the effects of increasing aerosol concentration range from rain suppression in the Oklahoma case, to almost no effect in the Florida case, to rain enhancement in the Pacific case. These results show the complexity of aerosol interactions with convection.

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

    PubMed

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

    2016-02-01

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

  13. Mass size distributions of soluble sulfate, nitrate and ammonium in the Madrid urban aerosol

    NASA Astrophysics Data System (ADS)

    Plaza, J.; Pujadas, M.; Gómez-Moreno, F. J.; Sánchez, M.; Artíñano, B.

    2011-09-01

    This paper analyzes the mass size distribution of some inorganic species present in the atmospheric aerosol from a field campaign carried out in Madrid throughout a complete year (February 2007-February 2008). Samplings were performed by means of a micro-orifice uniform deposit impactor (MOUDI). Ambient air was sampled during consecutive nocturnal and diurnal periods, and diurnal/nocturnal behaviors were compared for the twenty night-day sampling pairs that were gathered. Annual and seasonal averages were obtained, and some case studies under specific atmospheric conditions are discussed in the paper. Results have shown that the sulfate and ammonium mass was concentrated in the accumulation mode, between 0.18 and 0.56 μm, so that gas-phase and condensation processes for secondary aerosol formation prevailed during the sampling periods in this area. An exception to this behavior was found during a fog event when distributions for these two species were centered in the 0.56-1 and 1-1.8 μm size stages, corresponding to the droplet mode. In most of the samples, the ammonium mass measured in these size ranges was enough or almost enough to neutralize inorganic acidity by formation of ammonium sulfate and nitrate. However, a significant sulfate mass not neutralized by ammonium was found in the impactor backup quartz filter (aerodynamic diameter < 0.056 μm). The concentration of this sulfate and its contribution to the ultrafine fraction mass was higher under good dispersive conditions, prevailing in summer, when particle growth processes are not so favored due to the higher atmospheric dilution factors. The origin of this ultrafine sulfate has been attributed to direct emissions from traffic, associated to the nucleation mode. Regarding the nitrate concentration, it was found higher in the coarse mode than in the accumulation mode on an annual basis. The highest concentrations were measured in winter episodic situations. The marked seasonal variability shown in the

  14. Fractal morphology, imaging and mass spectrometry of single aerosol particles in flight (CXIDB ID 16)

    DOE Data Explorer

    Loh, N. Duane

    2012-06-20

    This deposition includes the aerosol diffraction images used for phasing, fractal morphology, and time-of-flight mass spectrometry. Files in this deposition are ordered in subdirectories that reflect the specifics.

  15. Dependence of Heterogeneous OH Kinetics with Biomass Burning Aerosol Proxies on Oxidant Concentration and Relative Humidity

    NASA Astrophysics Data System (ADS)

    Slade, J. H.; Knopf, D. A.

    2013-12-01

    Chemical transformations of aerosol particles by heterogeneous reactions with trace gases such as OH radicals can influence particle physicochemical properties and lifetime, affect cloud formation, light scattering, and human health. Furthermore, OH oxidation can result in degradation of particle mass by volatilization reactions, altering the budget of volatile organic compounds (VOCs). However, the reactive uptake coefficient (γ) and particle oxidation degree can vary depending on several factors including oxidant concentration and relative humidity (RH). While RH can influence the extent of dissociation/ionization, it can also affect particle phase and thus oxidant diffusivity. Only one study so far has investigated the effect of RH on the rate of OH uptake to organic surfaces; however, the underlying processes affecting OH reactivity with organic aerosol under humidified conditions still remains elusive. Here, we determine the effect of RH on OH reactivity with laboratory-generated biomass burning aerosol (BBA) surrogate particles: levoglucosan and 4-methyl-5-nitrocatechol. The effect of OH concentration on γ for three common BBA molecular markers (levoglucosan, abietic acid, and nitroguaiacol) under dry conditions was investigated from [OH]≈107-1011 molecule cm-3, covering both [OH] in biomass burning plumes and [OH] commonly used in particle aging studies. Furthermore, key VOC reaction products and their production pathways resulting from BBA volatilization by OH were identified. OH radicals are produced using a microwave induced plasma (MIP) of H2 in He or Ar followed by reaction with O2, or by photolysis of O3 in the presence of H2O. A cylindrical rotating wall flow-tube reactor and fast-flow aerosol flow reactor are used for conducting kinetic studies. OH is detected using a Chemical Ionization Mass Spectrometer (CIMS) and a Proton Transfer Reaction Time-of-Flight Mass Spectrometer (PTR-ToF-MS) is employed for VOC analysis. γ decreases from 0.2-0.5 at

  16. Emission Controls Versus Meteorological Conditions in Determining Aerosol Concentrations in Beijing during the 2008 Olympic Games

    SciTech Connect

    Gao, Yi; Liu, Xiaohong; Zhao, Chun; Zhang, Meigen

    2011-12-12

    A series of emission control measures were undertaken in Beijing and the adjacent provinces in China during the 2008 Beijing Olympic Games on August 8th-24th, 2008. This provides a unique opportunity for investigating the effectiveness of emission controls on air pollution in Beijing. We conducted a series of numerical experiments over East Asia for the period of July to September 2008 using a coupled meteorology-chemistry model (WRF-Chem). Model can generally reproduce the observed variation of aerosol concentrations. Consistent with observations, modeled concentrations of aerosol species (sulfate, nitrate, ammonium, black carbon, organic carbon, total particulate matter) in Beijing were decreased by 30-50% during the Olympic period compared to the other periods in July and August in 2008 and the same period in 2007. Model results indicate that emission controls were effective in reducing the aerosol concentrations by comparing simulations with and without emission controls. However, our analysis suggests that meteorological conditions (e.g., wind direction and precipitation) are at least as important as emission controls in producing the low aerosol concentrations appearing during the Olympic period. Transport from the regions surrounding Beijing determines the temporal variation of aerosol concentrations in Beijing. Based on the budget analysis, we suggest that emission control strategy should focus on the regional scale instead of the local scale to improve the air quality over Beijing.

  17. Emission controls versus meteorological conditions in determining aerosol concentrations in Beijing during the 2008 Olympic Games

    NASA Astrophysics Data System (ADS)

    Gao, Y.; Liu, X.; Zhao, C.; Zhang, M.

    2011-12-01

    A series of emission control measures were undertaken in Beijing and the adjacent provinces in China during the 2008 Beijing Olympic Games on 8-24 August 2008. This provides a unique opportunity for investigating the effectiveness of emission controls on air pollution in Beijing. We conducted a series of numerical experiments over East Asia for the period of July to September 2008 using a coupled meteorology-chemistry model (WRF-Chem). Model can generally reproduce the observed variation of aerosol concentrations. Consistent with observations, modeled concentrations of aerosol species (sulfate, nitrate, ammonium, black carbon, organic carbon, total particulate matter) in Beijing were decreased by 30-50% during the Olympic period compared to the other periods in July and August in 2008 and the same period in 2007. Model results indicate that emission controls were effective in reducing the aerosol concentrations by comparing simulations with and without emission controls. In addition to emission controls, our analysis suggests that meteorological conditions (e.g. wind direction and precipitation) were also important in producing the low aerosol concentrations appearing during the Olympic period. Transport from the regions surrounding Beijing determined the daily variation of aerosol concentrations in Beijing. Based on the budget analysis, we suggest that to improve the air quality over Beijing, emission control strategy should focus on the regional scale instead of the local scale.

  18. AGRICULTURAL AMMONIA EMISSIONS AND AMMONIUM CONCENTRATIONS ASSOCIATED WITH AEROSOLS AND PRECIPITATION IN THE SOUTHEAST UNITED STATES

    EPA Science Inventory

    Temporal and spatial variations in ammonia (NH3) emissions and ammonium (NH4+) concentrations associated with aerosols and volume-weighted NH4+ concentration in precipitation are investigated over the period 1990-1998 in the southeast United States (Alabama, Florida, Georgia, Ken...

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

    NASA Astrophysics Data System (ADS)

    Hariyama, Tatsuo; Takaya, Yasuhiro; Miyoshi, Takashi

    2005-11-01

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

  20. Chemical composition, sources, and processes of urban aerosols during summertime in northwest China: insights from high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-12-01

    An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with a scanning mobility particle sizer (SMPS) and a multi-angle absorption photometer (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of submicron particulate matter (PM1) in Lanzhou, northwest China, during 11 July-7 August 2012. The average (PM1 mass concentration including non-refractory (PM1 (NR-(PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105 μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. Organic aerosol (OA) on average consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution organic mass spectra identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns, both with peak at ~ 07:00-11:00 (BJT: UTC +8), corresponding to the morning rush hours, while cooking-emission related OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ~ 07:00 and 15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak between ~ 08:00-13:00. The later morning and early afternoon maximum in the diurnal profiles of secondary aerosol species was likely caused by downward mixing of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during nighttime. The mass spectrum of SV-OOA was

  1. Combining AOT, Angstrom Exponent and PM concentration data, with PSCF model, to distinguish fine and coarse aerosol intrusions in Southern France

    NASA Astrophysics Data System (ADS)

    Dimitriou, Konstantinos; Kassomenos, Pavlos

    2016-05-01

    In this paper, a cluster analysis of backward air mass trajectories, arriving in Avignon (Southern France), was combined with a Potential Source Contribution Function (PSCF) model on a 0.5° × 0.5° resolution grid, in order to indicate possible aerosol intrusions. A strict triple criterion was constructed from Aerosol Optical Thickness (AOT), Angstrom Exponent (AE), and PM (PM10 and PM2.5) concentration measurements, aiming to distinguish more effectively Episodes of Fine, Coarse and Overall Aerosols (FAE, CAE and OAE respectively). Large fractions of FAE (60.0%) and CAE (40.6%) were strongly attributed to the prevalence of Eastern and South-Southwest (S-SW) airflows respectively, whereas these distinct trajectory clusters also gathered large fractions of OAE (90.2% cumulatively). According to PSCF results, FAE events were strongly associated with the influence of air masses traveling over North Italy and Southern Germany, hence the impact of urban and industrial combustion was emerged. Main sources of coarse aerosols were principally isolated over the Mediterranean, thus the import of sea spray and dust from the Sahara desert is presumed. Satellite AOT observations were used for a more detailed identification of an intense 5-day intrusion of coarse aerosols. Short range slow moving air mass trajectories, were proven to be a clear marker of atmospheric stagnation, based on a wind speed analysis, triggering the accumulation of locally emitted anthropogenic aerosols (mainly PM2.5) and lack of city ventilation.

  2. Impacts of interannual variation of the East Asian winter monsoon on aerosol concentrations over eastern China

    NASA Astrophysics Data System (ADS)

    Zhu, J.; Liao, H.; Li, J.; Feng, J.

    2012-04-01

    China has been experiencing increased concentrations of aerosols, commonly attributed to the large increases in emissions associated with the rapid economic development. We apply a global three-dimensional Goddard Earth Observing System chemical transport model (GEOS-Chem) driven by the NASA/GEOS-4 assimilated meteorological data to quantify the impacts of East Asian winter monsoon (EAWM) on the aerosol concentrations over eastern China. We found that the simulated aerosol concentrations over eastern China have strong interannual variation and negative correlations with the strength of EAWM. Model results show that, accounting for sulfate, nitrate, ammonium, black carbon, and organic carbon aerosols, the winter surface layer PM2.5 concentration averaged over eastern China (110°-125°E, 20°-45°N) can be 17.97% (4.78 µg m-3) higher in the weak monsoon years than that in the strong monsoon years. Regionally, the weakening of EAWM is shown to be able to increase PM2.5 concentration in the middle and lower reach of the Yellow River by 12 µg m-3. This point indicates that climate change associated with variation of EAWM has an essential influence on worsening air quality over eastern China. The possible causes of higher aerosol concentrations in the weak monsoon years may be attributed to the changing in wind fields and planetary boundary layer height between the weak and strong monsoon years. Sensitivity studies are performed to identify the role of chemical reaction associated with temperature and humidity on the higher aerosol concentrations in the weak monsoon years over eastern China.

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

    NASA Astrophysics Data System (ADS)

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

    2005-10-01

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

  4. Size and mass distributions of ground-level sub-micrometer biomass burning aerosol from small wildfires

    NASA Astrophysics Data System (ADS)

    Okoshi, Rintaro; Rasheed, Abdur; Chen Reddy, Greeshma; McCrowey, Clinton J.; Curtis, Daniel B.

    2014-06-01

    Biomass burning emits large amounts of aerosol particles globally, influencing human health and climate, but the number and size of the particles is highly variable depending on fuel type, burning and meteorological conditions, and secondary reactions in the atmosphere. Ambient measurements of aerosol during wildfire events can therefore improve our understanding of particulate matter produced from biomass burning. In this study, time-resolved sub-micrometer ambient aerosol size and mass distributions of freshly emitted aerosol were measured for three biomass burning wildfire events near Northridge, California, located in the highly populated San Fernando Valley area of Los Angeles. One fire (Marek) was observed during the dry Santa Ana conditions that are typically present during large Southern California wildfires, but two smaller fires (Getty and Camarillo) were observed during the more predominant non-Santa Ana weather conditions. Although the fires were generally small and extinguished quickly, they produced particle number concentrations as high as 50,000 cm-3 and mass concentrations as large as 150 μg cm-3, well above background measurements and among the highest values observed for fires in Southern California. Therefore, small wildfires can have a large impact on air quality if they occur near urban areas. Particle number distributions were lognormal, with peak diameters in the accumulation mode at approximately 100 nm. However, significant Aitken mode and nucleation mode particles were observed in bimodal distributions for one fire. Significant variations in the median diameter were observed over time, as particles generally became smaller as the fires were contained. The results indicate that it is likely that performing mass measurements alone could systematically miss detection of the smaller particles and size measurements may be better suited for studies of ambient biomass burning events. Parameters of representative unimodal and bimodal lognormal

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  6. Mass Independent Isotopic Compositions of Aerosol Sulfate and Nitrates

    NASA Astrophysics Data System (ADS)

    Thiemens, M. H.

    2001-12-01

    For nearly a half-century stable isotope ratio measurements have been utilized as a tool to understand sources, fates, and transformation mechanisms of atmospheric molecules. Carbon and oxygen (δ 13C and δ 18O) measurements of CO2 have been instrumental in providing specific details of the carbon cycle. Without these measurements, understanding of the carbon cycle and transfer rates between reservoirs would be considerably diminished. Deuterium and oxygen isotopic measurements of atmospheric water has similarly enhanced the ability to model the atmospheric and geochemical recycling of the hydrologic cycle. Other molecules investigated include, for example, CO, CH4, N2O, SO4, NH, and Cl. The ability to interpret these high precision isotope ratio measurements relies upon a fundamental understanding of the basic physical-chemical processes which produce the alteration of the stable isotope ratio. Such processes typically include thermodynamics (viz a viz isotope exchange), kinetics, and evaporation-condensation. Though the mechanism by which these alterations occur, they all depend in some fashion upon mass differences in the isotopically substituted atoms. In 1983, Thiemens and Heidenreich (1) demonstrated that a chemical process is capable of producing an alteration of stable isotopes which was independent of mass. Subsequent to that time, it has been shown that measurements of mass independent isotopic compositions provide a new view of atmospheric process which may not be derived from single isotope ratio measurements (reviews by (2), (3)). In the past few years, mass independent isotopic compositions have been utilized to understand ancient atmospheres on both Earth and Mars (review by (4)). It has been known for decades that atmospheric sulfate is an extraordinary species. It participates in climate change in its capacity as a cloud condensation nuclei and it is a human and environmental health hazard. By the same token, aerosol nitrate is an environmental

  7. Vertical Resolved Dust Mass Concentration and Backscatter Coefficient Retrieval of Asian Dust Plume Using Quartz Raman Channel in Lidar Measurements

    NASA Astrophysics Data System (ADS)

    Noh, Young M.; Mueller, Detlef; Shin, Sungkyun

    2016-06-01

    In this work, we present a method for estimating vertical resolved mass concentration of dust immersed in Asian dust plume using Raman scattering of quartz (silicon dioxide, silica). During the Asian dust period of March 15, 16, and 21 in 2010, Raman lidar measurements detected the presence of quartz, and successfully showed the vertical profiles of the quartz backscatter coefficient. Since the Raman backscatter coefficient was connected with the Raman backscatter differential cross section and the number density of quartz molecules, the mass concentration of quartz in the atmosphere can be estimated from the quartz backscatter coefficient. The weight percentage from 40 to 70 % for quartz in the Asian dust was estimated from references. The vertical resolved mass concentration of dust was estimated by quartz mass concentration and weight percentage. We also present a retrieval method to obtain dust backscatter coefficient from the mixed Asian dust and pollutant layer. OPAC (Optical Properties of Aerosol and Clouds) simulations were conducted to calculate dust backscatter coefficient. The retrieved dust mass concentration was used as an input parameter for the OPAC calculations. These approaches in the study will be useful for characterizing the quartz dominated in the atmospheric aerosols and estimating vertical resolved mass concentration of dust. It will be especially applicable for optically distinguishing the dust and non-dust aerosols in studies on the mixing state of Asian dust plume. Additionally, the presented method combined with satellite observations is enable qualitative and quantitative monitoring for Asian dust.

  8. [Concentration distribution of metal elements in atmospheric aerosol under different weather conditions in Qingdao Coastal Region].

    PubMed

    Chen, Xiao-Jing; Qi, Jian-Hua; Liu, Ning; Zhang, Xiang-Yu; Shen, Heng-Qing; Liu, Ming-Xu

    2014-10-01

    To know the influence of different weather conditions on the concentration of metal elements in aerosols in the coastal region, total suspended particles (TSP) samples were collected from April to May 2012, and August 2012 to March 2013 in the Qingdao coastal region, and common trace metals were analyzed by using Inductively Coupled Plasma-Mass Spectrometry (ICP-MS) and Inductively Coupled Plasma-Atomic Emission Spectrometry (ICP-AES). The results showed that Al, Ca, Fe, Na, K and Mg were the dominant metal elements in TSP, and the sum of the six elements accounted for 94.2% of the sum of all metals. TSP and metal elements had significant monthly variations, Fe, Al, K, Ca, Mg, Zn, Ba, Mn, Ti, Sr and Li had the highest concentration in November and January, while Be, Sc, Co, Ni and Cr showed the highest value in January. Na had the highest concentration in August, November and February, and the lowest in December. Pb had the highest concentration in January and February, and the lowest in August and December. Enrichment factors indicated that Be, Co, Al, Ca, Fe, K, Mg, Mn, Sr and Ti were mainly affected by natural sources; Li, Cr, Ni, Zn, Ba and Na were affected by natural sources and part of anthropogenic sources; Pb was mainly from anthropogenic sources. Different weather conditions had great impact on TSP and metal elements concentrations, all the measured metals had the highest concentrations in smog except Ti. Compared with the sunny day, the concentration of atmospheric particulate Ti decreased, while the other elements increased by 1 to 4 times in smog. Li, Be, Cr, Ni, Al, Fe, Mg and Mn had little variation in concentration in foggy day, and the concentration of Pb and Na increased considerably. The concentration of Co, Ca and Ti reduced obviously in fog. Except for Cr, Co and Ti, the other elements increased by 1 to 3 times in haze. Most of the elements had the minimal enrichment factors in sunny day, while the other had the maximal enrichment factor in

  9. Effect of Vaporizer Temperature on Ambient Non-Refractory Submicron Aerosol Composition and Mass Spectra Measured by the Aerosol Mass Spectrometer

    EPA Science Inventory

    Aerodyne Aerosol Mass Spectrometers (AMS) are routinely operated with a constant vaporizer temperature (Tvap) of 600oC in order to facilitate quantitative detection of non-refractory submicron (NR-PM1) species. By analogy with other thermal desorption instrument...

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

    SciTech Connect

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

    2012-06-29

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

  11. Determination of aromatic tracer compounds for environmental tobacco smoke aerosol by two step laser mass spectrometry

    NASA Astrophysics Data System (ADS)

    Morrical, Brad D.; Zenobi, Renato

    Cigarette smoking is a major cause of indoor aerosol pollution. Determination of exposure to environmental tobacco smoke (ETS) aerosol is critical to understanding health effects. Sizing studies have shown that ETS has a size distribution that is efficiently deposited into the lungs and can therefore provide effective delivery of carcinogenic compounds into the human body. Two-step laser mass spectrometry is used to analyze aromatic compounds on aerosols collected from a smoking lobby. The determination and suitability of ETS tracers on aerosols is examined. Additionally, the transport of aerosol from the smoking lobby is examined to determine what effect deposition and dilution have on the mass spectrum observed. Results from the analysis of ETS, both from lobby samples and direct cigarette sampling, show that several unique peaks are present in the mass spectrum when compared to other combustion sources, such as automobiles and diesel trucks. In particular, ions at m/ z 118, 132, 146, and 160 are consistently present and are not found in other combustion sources. For the indoor environment, where chemical transformation is much less rapid than in the outdoor environment, these ions were found to be present as soon as the first smokers appeared and persisted over the course of the day. Aerosol samples taken in the morning prior to the presence of smokers in the lobby reveal the presence of skeletal PAHs, indicative of outdoor urban traffic aerosol penetration into the building.

  12. An Examination of Carbon Monoxide and Organic Aerosol Mass Sources in the Southeastern United States during the SENEX Project

    NASA Astrophysics Data System (ADS)

    Middlebrook, A. M.; Angevine, W. M.; Brioude, J. F.; Brock, C. A.; De Gouw, J. A.; Gilman, J.; Graus, M.; Hanisco, T. F.; Holloway, J. S.; Horowitz, L. W.; Kaiser, J.; Keutsch, F. N.; Lerner, B. M.; Liao, J.; Mao, J.; Trainer, M.; Warneke, C.; Welti, A.; Wolfe, G. M., Jr.

    2014-12-01

    The NOAA Southeast Nexus (SENEX) project occurred during the summer of 2013 over the southeastern United States and involved studying the interactions between natural and anthropogenic emissions at the nexus of climate change and air quality. As part of the project, a suite of instruments for aerosol and gas-phase species was deployed on the NOAA WP-3D aircraft and models were used to calculate trace gas and aerosol species in the region and along the aircraft flight tracks. Throughout the study, the measured non-refractory submicron aerosol mass was dominated by organic material (58% +/- 9%) with smaller contributions from sulfate (27% +/- 8%), ammonium (10% +/- 3%), nitrate (3% +/- 1%), and chloride (0.1% +/- 0.1%). Here we examine the influence of urban emissions on the organic aerosol (OA) mass in regions characterized by higher and lower biogenic emissions. For the air around and downwind of urban areas, OA mass is highly correlated with carbon monoxide (CO), a tracer of anthropogenic emissions as well as an oxidation product of isoprene, a biogenic species. The slope of this correlation is roughly 0.15 micrograms per standard cubic meter per ppbv, which is significantly higher than observed in prior studies downwind of urban areas. The enhancement in OA mass relative to the enhancement in CO is independent of the concentration of biogenic species. In contrast, formaldehyde enhancements are clearly higher in the presence of biogenic species in agreement with the NOAA GFDL AM3 model. Downwind from the urban areas, CO and OA mass were not strongly enhanced relatively to a region-wide enhancement in these species that can only be explained from the accumulation of emissions in the eastern U.S. for several days. Back-trajectories of air parcels with emissions from biogenic and anthropogenic sources will be examined to elucidate the impact of both sources on CO and OA mass.

  13. Real-time analysis of ambient organic aerosols using aerosol flowing atmospheric-pressure afterglow mass spectrometry (AeroFAPA-MS)

    NASA Astrophysics Data System (ADS)

    Brüggemann, Martin; Karu, Einar; Stelzer, Torsten; Hoffmann, Thorsten

    2015-04-01

    Organic aerosol accounts for a major fraction of atmospheric aerosols and has implications on the earth's climate and human health. However, due to the chemical complexity its measurement remains a major challenge for analytical instrumentation.1 Here, we present the development, characterization and application of a new soft ionization technique that allows mass spectrometric real-time detection of organic compounds in ambient aerosols. The aerosol flowing atmospheric-pressure afterglow (AeroFAPA) ion source utilizes a helium glow discharge plasma to produce excited helium species and primary reagent ions. Ionization of the analytes occurs in the afterglow region after thermal desorption and results mainly in intact molecular ions, facilitating the interpretation of the acquired mass spectra. In the past, similar approaches were used to detect pesticides, explosives or illicit drugs on a variety of surfaces.2,3 In contrast, the AeroFAPA source operates 'online' and allows the detection of organic compounds in aerosols without a prior precipitation or sampling step. To our knowledge, this is the first application of an atmospheric-pressure glow discharge ionization technique to ambient aerosol samples. We illustrate that changes in aerosol composition and concentration are detected on the time scale of seconds and in the ng-m-3 range. Additionally, the successful application of AeroFAPA-MS during a field study in a mixed forest region in Central Europe is presented. Several oxidation products of monoterpenes were clearly identified using the possibility to perform tandem MS experiments. The acquired data are in agreement with previous studies and demonstrate that AeroFAPA-MS is a suitable tool for organic aerosol analysis. Furthermore, these results reveal the potential of this technique to enable new insights into aerosol formation, growth and transformation in the atmosphere. References: 1) IPCC, 2013: Summary for Policymakers. In: Climate Change 2013: The

  14. Progress Toward a Global, EOS-Era Aerosol Air Mass Type Climatology

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2012-01-01

    The MISR and MODIS instruments aboard the NASA Earth Observing System's Terra Satellite have been collecting data containing information about the state of Earth's atmosphere and surface for over eleven years. Data from these instruments have been used to develop a global, monthly climatology of aerosol amount that is widely used as a constraint on climate models, including those used for the 2007 IPCC assessment report. The next frontier in assessing aerosol radiative forcing of climate is aerosol type, and in particular, the absorption properties of major aerosol air masses. This presentation will focus on the prospects for constraining aerosol type globally, and the steps we are taking to apply a combination of satellite and suborbital data to this challenge.

  15. Diurnal and elevational variations in ozone and aerosol concentrations in New Hampshire`s Class-I Airsheds

    SciTech Connect

    Hill, L.B.; Allen, G.A.

    1994-12-31

    Ozone and fine mass aerosol concentrations on New Hampshire`s Mount Washington, situated adjacent to both the Presidential/Dry River and Great Gulf Wilderness Class-I Airsheds, exhibit distinct diurnal and elevational patterns. These patterns are attributed to regional pollutant transport dynamics, nocturnal atmospheric stratification, mountain meteorological phenomena and scavenging. A well-defined planetary boundary layer (PBL) forms at about 1 km elevation at night as demonstrated by nocturnal ozone monitoring along the Mount Washington Auto Road. The PBL provides an effective elevational barrier at night, isolating the valleys from the regionally transported air pollutants present above the mixing layer. During the daytime, the PBL breaks up due to convective processes and katabatic winds resulting from solar heating in the valley. This process creates a diurnal mixing cycle with ozone maxima recorded near mid-day in the adjacent valley. In contrast, fine mass concentrations are higher at the valley site, attributed to local source inputs, and the lack of strong nocturnal scavenging processes, compared with ozone. How aerosol concentrations are related to the PBL and how they are affected by diurnal mixing remains unclear largely due to current sampling methods. Exposure to ozone is generally greater above the treeline in the two airsheds.

  16. Submicron aerosol size distributions and cloud condensation nuclei concentrations measured at Gosan, Korea, during the Atmospheric Brown Clouds-East Asian Regional Experiment 2005

    NASA Astrophysics Data System (ADS)

    Yum, Seong Soo; Roberts, Greg; Kim, Jong Hwan; Song, Keunyong; Kim, Dohyeong

    2007-11-01

    Submicron aerosol size distributions, CN and CCN concentrations at a constant supersaturation of 0.6% were measured at a relatively remote coastal site at Gosan in Jeju Island, Korea, during the ABC-EAREX from 11 March to 8 April 2005. The average CN concentrations were 6088 ± 3988, 5231 ± 2454 and 3513 ± 1790 cm-3, respectively, for the three major air mass types classified by their origins. The corresponding CCN concentrations were 2393 ± 1156, 2897 ± 1226 and 1843 ± 585 cm-3. The type III air mass was the closest to maritime origins, but these lowest concentrations at Gosan were an order of magnitude higher than those of clean marine boundary layer, indicating that regardless of air mass designation springtime submicron aerosols at Gosan were under steady continental influences. Distinct new particle formation and growth events occurred on 6 d, when clear sky weather conditions prevailed that brought air from northern China, Mongolia or Russia by anticyclonic circulations. Simultaneous occurrence of these events at a western coastal site in the Korean Peninsula 350 km north of Gosan suggests that these events were not local but at least regional-scale events. CCN concentrations were predicted with the aerosol size distributions and the assumption of particles being composed of (NH4)2SO4. The predicted to measured CCN concentration ratio was 1.27 ± 0.29 and the r2 was 0.77 for the whole measurement period. The type I air mass that has the most continental influences showed a slight tendency to overpredict CCN concentrations but the good agreement overall suggests that springtime Gosan aerosols act almost like ammonium sulfate as far as CCN activity is concerned, almost regardless of air mass origin.

  17. Detection response of elemental species in single particles using aerosol time-of-flight mass spectrometry

    SciTech Connect

    Silva, P.J.; Gross, D.S.; Gaelli, M.E.; Prather, K.A.

    1998-12-31

    The introduction of real-time particle mass spectrometry(RTSPMS) techniques creates a powerful tool for the study of particulate pollution on the single particle level. One such technique, aerosol time-of-flight mass spectrometry (ATOFMS) provides the aerodynamic size and chemical composition of individual particles. By combining data on size and composition, identification of individual particle classes in ambient outdoor samples is possible. Chemical composition is obtained by performing laser desorption ionization of individual particles using a Nd:YAG laser with a wavelength of 266 nm. The power of RTSPMS techniques is due to the ability to analyze the chemical composition of a single particle. The application of these techniques to analysis of ambient data has been limited however, because few studies have been performed to assess the ability of RTSPMS techniques to detect a wide range of compounds present in the atmosphere on a quantitative rather than qualitative level. It is known that various elemental species will respond differently to laser desorption mass spectrometric detection due to characteristic absorption cross-section and ionization potentials. In order to determine the capability and biases of RTSPMS techniques for detection of elemental species, a series of in-laboratory and ambient experiments has been performed using controlled conditions. Particles of known concentration have been produced from solution using an aerosol generator and analyzed using ATOFMS to determine responses of individual elements on a single particle level. In addition, side-by-side analyses with traditional sampling methods such as MOUDI impactors provide data to show how ATOFMS measurements correlate with federal reference methods.

  18. Identification of aerosol types over an urban site based on air-mass trajectory classification

    NASA Astrophysics Data System (ADS)

    Pawar, G. V.; Devara, P. C. S.; Aher, G. R.

    2015-10-01

    Columnar aerosol properties retrieved from MICROTOPS II Sun Photometer measurements during 2010-2013 over Pune (18°32‧N; 73°49‧E, 559 m amsl), a tropical urban station in India, are analyzed to identify aerosol types in the atmospheric column. Identification/classification is carried out on the basis of dominant airflow patterns, and the method of discrimination of aerosol types on the basis of relation between aerosol optical depth (AOD500 nm) and Ångström exponent (AE, α). Five potential advection pathways viz., NW/N, SW/S, N, SE/E and L have been identified over the observing site by employing the NOAA-HYSPLIT air mass back trajectory analysis. Based on AE against AOD500 nm scatter plot and advection pathways followed five major aerosol types viz., continental average (CA), marine continental average (MCA), urban/industrial and biomass burning (UB), desert dust (DD) and indeterminate or mixed type (MT) have been identified. In winter, sector SE/E, a representative of air masses traversed over Bay of Bengal and Eastern continental Indian region has relatively small AOD (τpλ = 0.43 ± 0.13) and high AE (α = 1.19 ± 0.15). These values imply the presence of accumulation/sub-micron size anthropogenic aerosols. During pre-monsoon, aerosols from the NW/N sector have high AOD (τpλ = 0.61 ± 0.21), and low AE (α = 0.54 ± 0.14) indicating an increase in the loading of coarse-mode particles over Pune. Dominance of UB type in winter season for all the years (i.e. 2010-2013) may be attributed to both local/transported aerosols. During pre-monsoon seasons, MT is the dominant aerosol type followed by UB and DD, while the background aerosols are insignificant.

  19. Calculations of relative optical air masses for various aerosol types and minor gases in Arctic and Antarctic atmospheres

    NASA Astrophysics Data System (ADS)

    Tomasi, Claudio; Petkov, Boyan H.

    2014-02-01

    The dependence functions of relative optical air mass on apparent solar zenith angle θ have been calculated over the θ < 87° range for the vertical profiles of wet-air molecular number density in the Arctic and Antarctic atmospheres, extinction coefficients of different aerosol types, and molecular number density of water vapor, ozone, nitrogen dioxide, and oxygen dimer. The calculations were made using as weight functions the seasonal average vertical profiles of (i) pressure and temperature derived from multiyear sets of radiosounding measurements performed at Ny-Ålesund, Alert, Mario Zucchelli, and Neumayer stations; (ii) volume extinction coefficients of background summer aerosol, Arctic haze, and Kasatochi and Pinatubo volcanic aerosol measured with lidars or balloon-borne samplings; and (iii) molecular number concentrations of the above minor gases, derived from radiosonde, ozonesonde, and satellite-based observations. The air mass values were determined using a formula based on a realistic atmospheric air-refraction model. They were systematically checked by comparing their mutual differences with the uncertainties arising from the seasonal and daily variations in pressure and temperature conditions within the various ranges, where aerosol and gases attenuate the solar radiation most efficiently. The results provide evidence that secant-approximated and midlatitude air mass values are inappropriate for analyzing the Sun photometer measurements performed at polar sites. They indicate that the present evaluations can be reliably used to estimate the aerosol optical depth from the Arctic and Antarctic measurements of total optical depth, after appropriate corrections for the Rayleigh scattering and gaseous absorption optical depths.

  20. Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

    NASA Astrophysics Data System (ADS)

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

    2011-03-01

    Vacuum Ultraviolet (VUV) photoionization mass spectrometry has been used to measure the evolution of chemical composition for two distinct organic aerosol types as they are passed through a thermodenuder at different temperatures. The two organic aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the α-pinene + O3 reaction (αP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct changes with temperature in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In contrast, the αP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in agreement with expectations from absorptive partitioning theory whereas the αP spectra suggest that the evaporation of αP derived aerosol appears to not be governed by partitioning theory. We postulate that this difference arises from diffusivity within the αP particles being sufficiently slow that they do not exhibit the expected liquid-like behavior and perhaps exist in a glassy state. To reconcile these observations with decades of aerosol growth measurements, which indicate that OA formation is described by equilibrium partitioning, we present a conceptual model wherein the secondary OA is formed and then rapidly converted from an absorbing form to a non-absorbing form. The results suggest that, although OA growth may be describable by equilibrium partitioning theory, the properties of organic aerosol once formed may differ significantly from the properties determined in the equilibrium framework.

  1. Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

    NASA Astrophysics Data System (ADS)

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

    2010-11-01

    Vacuum Ultraviolet (VUV) photoionization mass spectrometry has been used to measure the evolution of chemical composition for two distinct organic aerosol types as they are passed through a thermodenuder at different temperatures. The two organic aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the α-pinene + O3 reaction (αP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct changes with temperature in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In contrast, the αP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in agreement with expectations from absorptive partitioning theory whereas the αP spectra suggest that the evaporation of αP derived aerosol appears to not be governed by partitioning theory. We postulate that this difference arises from the αP particles existing as in a glassy state instead of having the expected liquid-like behavior. To reconcile these observations with decades of aerosol growth measurements, which indicate that OA formation is described by equilibrium partitioning, we present a conceptual model wherein the secondary OA is formed and then rapidly converted from an absorbing form to a non-absorbing form. The results suggest that although OA growth may be describable by equilibrium partitioning theory, the properties of organic aerosol once formed may differ significantly from the properties determined in the equilibrium framework.

  2. Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

    SciTech Connect

    UC Davis; Cappa, Christopher D.; Wilson, Kevin R.

    2010-10-28

    Vacuum Ultraviolet (VUV) photoionization mass spectrometry has been used to measure the evolution of chemical composition for two distinct organic aerosol types as they are passed through a thermodenuder at different temperatures. The two organic aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the alpha-pinene + O3 reaction (alphaP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct changes with temperature in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In contrast, the alphaP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in agreement with expectations from absorptive partitioning theory whereas the alphaP spectra suggest that the evaporation of alphaP derived aerosol appears to not be governed by partitioning theory. We postulate that this difference arises from the alphaP particles existing as in a glassy state instead of having the expected liquid-like behavior. To reconcile these observations with decades of aerosol growth measurements, which indicate that OA formation is described by equilibrium partitioning, we present a conceptual model wherein the secondary OA is formed and then rapidly converted from an absorbing form to a non-absorbing form. The results suggest that although OA growth may be describable by equilibrium partitioning theory, the properties of organic aerosol once formed may differ significantly from the properties determined in the equilibrium framework.

  3. Estimation of multiple-aerosol concentration and backscatter using multi-wavelength range-resolved lidar

    NASA Astrophysics Data System (ADS)

    Warren, Russell E.; Vanderbeek, Richard G.

    2007-09-01

    Previous work by the authors has produced statistically based methods for detecting, estimating and classifying aerosol materials in the atmosphere using multiple-wavelength range-resolved CO2 lidar. This work has thus far been limited to the presence of a single aerosol material at a given time within the lidar line-of-sight. Practical implementation requires the ability to detect and discriminate multiple aerosol materials present simultaneously such as smoke and dust in addition to hazardous materials. Treating mixtures of materials necessitates fundamentally different approaches from the single-material case since neither the aerosol backscatter wavelength-dependence nor the concentrations as a function of range are known. Because of this, linear processing cannot resolve the mixture data into its components unambiguously, and non-linear methods must be considered. In this paper we describe an empirical Bayes (EB) approach for resolving mixtures of aerosol into their components. The basic idea of EB is to use the same data to estimate the prior distribution of a set of parameters as that used to estimate the parameters themselves. In our case the concentration and backscatter are the parameters that are estimated with the help of a prior distribution of the backscatter. We implement the EB estimator through the EM (Expectation Maximization) algorithm. The resulting processor is applied to injections of interferent dust into data sets collected by ECBC during JBSDS testing at Dugway Proving Ground, UT in 2006.

  4. Preferential concentration of certain elements in smaller aerosols emitted from aircraft engines

    NASA Technical Reports Server (NTRS)

    Jolly, R. K.; Gupta, S. K.; Randers-Pehrson, G.; Buckle, D. C.; Thornton, W. B.; Aceto, H., Jr.; Singh, J. J.; Woods, D. C.

    1975-01-01

    Aerosols from aircraft engines were collected with an eight-stage cascade sampler for a period of 24 h. The aerosol samples from each stage were analyzed for their elemental composition using the proton-induced X-ray emission (PIXE) technique. Seventeen elements (Si, P, S, Cl, K, Ca, Ti, V, Fe, Ni, Cu, Zn, Br, Sr, Nb, Sn, and Pb) were positively identified and quantitated at each stage. Six elements (S, Ca, Fe, Zn, Sn, and Pb) showed a fractional concentration increase with decreasing aerosol size. Similar, but less well-defined, trends were also observed for V and Ni. Silicon and chlorine, on the other hand, showed an opposite trend. Neutron-activation analysis of bulk aerosol samples collected every 2 h over the same period showed a correlation between concentration of Si, Ca, V, Ti, Zn, Br, and Sn and the density of air traffic at the airport. Analysis of the aviation-fuel samples by PIXE indicates that major fractions of Pb, Sn, Br, Zn, Ni, Fe, V, Ca, and S observed in these aerosol studies come from the aircraft engine exhaust.

  5. Separating refractory and non-refractory particulate chloride and estimating chloride depletion by aerosol mass spectrometry in a marine environment

    NASA Astrophysics Data System (ADS)

    Nuaaman, I.; Li, S.-M.; Hayden, K. L.; Onasch, T. B.; Massoli, P.; Sueper, D.; Worsnop, D. R.; Bates, T. S.; Quinn, P. K.; McLaren, R.

    2015-01-01

    Aerosol composition and concentration measurements along the coast of California were obtained using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) onboard the research vessel Atlantis during the CalNex study in 2010. This paper focuses on the measurement of aerosol chloride using the HR-AMS that can be ambiguous in regions with significant quantities of sea salt aerosols. This ambiguity arises due to large differences in the sensitivity of the HR-AMS to refractory chloride species (i.e., NaCl) and non refractory chloride species (i.e., NH4Cl, HCl, etc.). Using the HR-AMS, the aerosol chloride signal is typically quantified using ion signals for 35Cl+, H35Cl+, 37Cl+ and H37Cl+ (HxCl+). During this study, the highest aerosol chloride signal was observed during sea sweep experiments when the source of the aerosol chloride was NaCl present in artificially generated sea salt aerosols even though the HR-AMS has significantly lower sensitivity to such refractory species. Other prominent ion signals that arise from NaCl salt were also observed at m/z 22.99 for Na+ and m/z 57.96 for Na35Cl+ during both sea sweep experiments and during periods of ambient measurements. Thus, refractory NaCl contributes significantly to the HxCl+ signal, interfering with attempts to quantify non sea salt chloride (nssCl). It was found that during ambient aerosol measurements, the interference in the HxCl+ signal from sea salt chloride (ssCl) was as high as 89%, but with a study wide average of 10%. The Na35Cl+ ion signal was found to be a good tracer for NaCl. We outline a method to establish nssCl in the ambient aerosols by subtracting the sea salt chloride (ssCl) signal from the HxCl+ signal. The ssCl signal is derived from the Na35Cl+ ion tracer signal and the HxCl+ to Na35Cl+ ratio established from the sea sweep experiments. Ambient submicron concentrations of ssCl were also established using the Na35Cl

  6. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  8. Characterizing an extractive electrospray ionization (EESI) source for the online mass spectrometry analysis of organic aerosols.

    PubMed

    Gallimore, Peter J; Kalberer, Markus

    2013-07-01

    Organic compounds comprise a major fraction of tropospheric aerosol and understanding their chemical complexity is a key factor for determining their climate and health effects. We present and characterize here a new online technique for measuring the detailed chemical composition of organic aerosols, namely extractive electrospray ionization mass spectrometry (EESI-MS). Aerosol particles composed of soluble organic compounds were extracted into and ionized by a solvent electrospray, producing molecular ions from the aerosol with minimal fragmentation. We demonstrate here that the technique has a time resolution of seconds and is capable of making stable measurements over several hours. The ion signal in the MS was linearly correlated with the mass of aerosol delivered to the EESI source over the range tested (3-600 μg/m(3)) and was independent of particle size and liquid water content, suggesting that the entire particle bulk is extracted for analysis. Tandem MS measurements enabled detection of known analytes in the sub-μg/m(3) range. Proof-of-principle measurements of the ozonolysis of oleic acid aerosol (20 μg/m(3)) revealed the formation of a variety of oxidation products in good agreement with previous offline studies. This demonstrates the technique's potential for studying the product-resolved kinetics of aerosol-phase chemistry at a molecular level with high sensitivity and time resolution. PMID:23710930

  9. 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.

  10. Validation of a gas chromatography/mass spectrometry method for the quantification of aerosolized Jet Propellant 8.

    PubMed

    Dietzel, Katherine D; Campbell, Jerry L; Bartlett, Michael G; Witten, Mark L; Fisher, Jeffrey W

    2005-11-01

    Jet Propellant 8 (JP-8) jet fuel is a kerosene-based fuel containing hundreds of hydrocarbons used by the military in NATO countries. Previous rodent inhalation studies carried out with aerosolized JP-8 never evaluated the exposure chamber atmosphere. For this reason, our laboratory developed an analytical method, with an accuracy of better than 80% and precision of better than 20%, for JP-8 aerosol and vapor samples using gas chromatography/mass spectrometry (GC/MS). A method was developed for quantification of selected individual components of JP-8 and for the total amount of JP-8 in aerosolized fuel. A 34 component surrogate hydrocarbon mixture (SHM) was developed and used for simultaneous analysis of the individual components. Three separate runs containing a standard curve and five replicates each at the selected concentrations were analyzed for both the SHM and neat JP-8. The resulting interday accuracy (100-percent relative error) and precision (relative standard deviation) values for the SHM were 86.5% or better and 8.0% or better, respectively. The intraday accuracy and precision values ranged from 99.29% to 84.50% and 0.97% to 12.4%, respectively. For the total amount of JP-8 in aerosol and vapor, the interday accuracy was 83.7% or better and interday precision was 7.0% or better. The intraday accuracy and precision values ranged from 94.8% to 80.4% and 2.4% to 10.5%, respectively. We then used this method to analyze samples collected from an inhalation chamber. From the data obtained, we are able to account for approximately 40-44% of the mass of the aerosol portion and 68-70% of the mass of the vapor portion. The aerosol represented 6-10% of the total mass of the aerosolized JP-8 fuel with the remaining portion being the vapor. From these experiments individual components were identified for further in vivo and in vitro toxicological testing. PMID:16233866

  11. AEROSOL CONCENTRATIONS DURING THE 1999 FRESNO EXPOSURE STUDIES AS FUNCTIONS OF SIZE, SEASON, AND METEOROLOGY

    EPA Science Inventory

    The 1999 Fresno exposure studies took place in February (winter season) and April/May (spring season) for two periods of four weeks. During that time, nearly-continuous measurements of outdoor aerosol concentrations were made with a scanning mobility spectrometer (TSI SNIPS) an...

  12. Concentrations of iodine isotopes ((129)I and (127)I) and their isotopic ratios in aerosol samples from Northern Germany.

    PubMed

    Daraoui, A; Riebe, B; Walther, C; Wershofen, H; Schlosser, C; Vockenhuber, C; Synal, H-A

    2016-04-01

    New data about (129)I, (127)I concentrations and their isotopic ratios in aerosol samples from the trace survey station of the Physikalisch-Technische Bundesanstalt (PTB) in Braunschweig, Northern Germany, are presented and discussed in this paper. The investigated samples were collected on a weekly basis during the years 2011 to 2013. Iodine was extracted from aerosol filters using a strong basic solution and was separated from the matrix elements with chloroform and was analysed by accelerator mass spectrometry (AMS) for (129)I and by inductively coupled plasma mass spectrometry (ICP-MS) for (127)I. The concentrations of (127)I and (129)I in aerosol filters ranged from 0.31 to 3.71 ng m(-3) and from 0.06 to 0.75 fg m(-3), respectively. The results of (129)I/(127)I isotopic ratios were in the order 10(-8) to 10(-7). The (129)I originated directly from gaseous emissions and indirectly from liquid emissions (via sea spray) from the reprocessing plants in Sellafield and La Hague. In comparison with the results of (131)I after the Fukushima accident, no contribution of (129)I from this accident was detectable in Central Europe due to the high background originating from the (129)I releases of the European reprocessing plants. (129)I atmospheric activity concentrations were compared with those of an anthropogenic radionuclide ((85)Kr). We did not find any correlation between (129)I and (85)Kr, both having nuclear reprocessing plant as the main source. PMID:26867099

  13. Ultrahigh resolution mass spectrometric characterization of organic aerosol from European and Chinese cities

    NASA Astrophysics Data System (ADS)

    Wang, Kai; Huang, Ru-Jin; Hoffmann, Thorsten

    2016-04-01

    Organic aerosol constitutes a substantial fraction (20-90%) of submicrometer aerosol mass, playing an important role in air quality and human health. Over the past few years, ultra-high resolution mass spectrometry (UHRMS) has been applied to elucidate the chemical composition of ambient aerosols. However, most of the UHRMS studies used direct infusion without prior separation by liquid chromatography, which may cause the loss of individual compound information and interference problems. In the present study, urban ambient aerosol with particle diameter < 2.5 μm was collected in Mainz, Germany and Beijing, China, respectively. Two pretreatment procedures were applied to extract the organic compounds from the filter samples: One method uses a mixture of acetonitrile and water, the other uses pure water and prepared for the extraction of humic-like substances. The extracts were analyzed by ultra-high-performance liquid chromatography coupled with an Orbitrap mass spectrometer in both negative and the positive modes. The effects of pretreatment procedures on the characterization of organic aerosol and the city-wise difference in chemical composition of organic aerosol will be discussed in detail.

  14. Prospects of real-time single-particle biological aerosol analysis: A comparison between laser-induced breakdown spectroscopy and aerosol time-of-flight mass spectrometry

    NASA Astrophysics Data System (ADS)

    Beddows, D. C. S.; Telle, H. H.

    2005-08-01

    In this paper we discuss the prospects of real-time, in situ laser-induced breakdown spectroscopy applied for the identification and classification of bio-aerosols (including species of potential bio-hazard) within common urban aerosol mixtures. In particular, we address the issues associated with the picking out of bio-aerosols against common background aerosol particles, comparing laser-induced breakdown spectroscopy measurements with data from a mobile single-particle aerosol mass spectrometer (ATOFMS). The data from the latter provide statistical data over an extended period of time, highlighting the variation of the background composition. While single-particle bio-aerosols are detectable in principle, potential problems with small (˜ 1 μm size) bio-aerosols have been identified; constituents of the air mass other than background aerosols, e.g. gaseous CO 2 in conjunction with common background aerosols, may prevent unique recognition of the bio-particles. We discuss whether it is likely that laser-induced breakdown spectroscopy on its own can provide reliable, real-time identification of bio-aerosol in an urban environment, and it is suggested that more than one technique should be or would have to be used. A case for using a combination of laser-induced breakdown spectroscopy and Raman (and/or) laser-induced fluorescence spectroscopy is made.

  15. Criteria for significance of simultaneous presence of both condensible vapors and aerosol particles on mass transfer (deposition) rates

    NASA Technical Reports Server (NTRS)

    Gokoglu, S. A.

    1986-01-01

    The simultaneous presence of aerosol particles and condensible vapors in a saturated boundary layer which may affect deposition rates to subcooled surfaces because of vapor-particle interactions is discussed. Scavenging of condensible vapors by aerosol particles may lead to increased particle size and decreased vapor mass fraction, which alters both vapor and particle deposition rates. Particles, if sufficiently concentrated, may also coagulate. Criteria are provided to assess the significance of such phenomena when particles are already present in the mainstream and are not created inside the boundary layer via homogeneous nucleation. It is determined that there is direct proportionality with: (1) the mass concentration of both condensible vapors and aerosol particles; and (2) the square of the boundary layer thickness to particle diameter ratio (delta d sub p) square. Inverse proportionality was found for mainstream to surface temperature difference if thermophoresis dominates particle transport. It is concluded that the square of the boundary layer thickness to particle diameter ratio is the most critical factor to consider in deciding when to neglect vapor-particle interactions.

  16. The Role of Atmospheric Aerosol Concentration on Deep Convective Precipitation: Cloud-Resolving Model Simulations

    NASA Technical Reports Server (NTRS)

    Tao, Wei-Kuo; Li, Xiaowen; Khain, Alexander; Matsui, Toshihisa; Lang, Stephen; Simpson, Joanne

    2010-01-01

    Aerosols and especially their effect on clouds are one of the key components of the climate system and the hydrological cycle [Ramanathan et al., 2001]. Yet, the aerosol effect on clouds remains largely unknown and the processes involved not well understood. A recent report published by the National Academy of Science states "The greatest uncertainty about the aerosol climate forcing - indeed, the largest of all the uncertainties about global climate forcing - is probably the indirect effect of aerosols on clouds NRC [2001]." The aerosol effect on Clouds is often categorized into the traditional "first indirect (i.e., Twomey)" effect on the cloud droplet sizes for a constant liquid water path and the "semi-direct" effect on cloud coverage. The aerosol effect on precipitation processes, also known as the second type of aerosol indirect effect, is even more complex, especially for mixed-phase convective clouds. In this paper, a cloud-resolving model (CRM) with detailed spectral-bin microphysics was used to examine the effect of aerosols on three different deep convective cloud systems that developed in different geographic locations: South Florida, Oklahoma and the Central Pacific, In all three cases, rain reaches the ground earlier for the low CCN (clean) case. Rain suppression is also evident in all three cases with high CCN (dirty) case. However, this suppression only occurs during the first hour of the simulations. During the mature stages of the simulations, the effects of increasing aerosol concentration range from rain suppression in the Oklahoma case, to almost no effect in the Florida case, to rain enhancement in the Pacific case. These results show the complexity of aerosol interactions with convection. The model results suggest that evaporative cooling is a key process in determining whether high CCN reduces or enhances precipitation. Stronger evaporative cooling can produce a stronger cold pool and thus stronger low-level convergence through interactions

  17. Characterization of near-highway submicron aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y. L.; Zhang, Q.; Schwab, J. J.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Lin, Y.-C.; Ng, N. L.; Jayne, J.; Massoli, P.; Williams, L. R.; Demerjian, K. L.

    2011-11-01

    Knowledge of the variations of mass concentration, chemical composition and size distributions of submicron aerosols near roadways is of importance for reducing exposure assessment uncertainties in health effects studies. The goal of this study is to deploy and evaluate an Atmospheric Sciences Research Center-Mobile Laboratory (ASRC-ML), equipped with a suite of rapid response instruments for characterization of traffic plumes, adjacent to the Long Island Expressway (LIE) - a high-traffic highway in the New York City Metropolitan Area. In total, four measurement periods, two in the morning and two in the evening were conducted at a location approximately 30 m south of the LIE. The mass concentrations and size distributions of non-refractory submicron aerosol (NR-PM1) species were measured in situ at a time resolution of 1 min by an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer, along with rapid measurements (down to 1 Hz) of gaseous pollutants (e.g., HCHO, NO2, NO, O3, and CO2, etc.), black carbon (BC), and particle number concentrations and size distributions. The particulate organics varied dramatically during periods with highest traffic influences from the nearby roadway. The variations were mainly observed in the hydrocarbon-like organic aerosol (HOA), a surrogate for primary OA from vehicle emissions. The inorganic species (sulfate, ammonium, and nitrate) and oxygenated OA (OOA) showed much smoother variations - with minor impacts from traffic emissions. The concentration and chemical composition of NR-PM1 also varied differently on different days depending on meteorology, traffic intensity and vehicle types. Overall, organics dominated the traffic-related NR-PM1 composition (>60%) with HOA being the major fraction of OA. The traffic-influenced organics showed two distinct modes in mass-weighted size distributions, peaking at ~120 nm and 500 nm (vacuum aerodynamic diameter, Dva), respectively. OOA and inorganic species appear to be

  18. CCN Study at Urban Supersite (T0) During MILAGRO: the Essential Information for Prediction of Aerosol CCN Concentrations

    NASA Astrophysics Data System (ADS)

    Wang, J.; Cubison, M.; Aiken, A. C.; Jimenez, J. L.; Collins, D. R.

    2009-12-01

    The influences of atmospheric aerosols on cloud properties (i.e., aerosol indirect effects) strongly depend on the aerosol CCN concentrations, which can be effectively predicted from detailed aerosol size distribution, mixing state, and chemical composition using Köhler theory. However, atmospheric aerosols often consist of a large number of species that cannot be individually simulated in global or regional models due to computational constraints. Furthermore, the thermodynamic properties or even the molecular identities of many organic species present in ambient aerosols are often not known to predict their cloud-activation behavior using Köhler theory. As a result, simplified presentations of aerosol composition are necessary for large-scale models. In this study, aerosol microphysics, CCN concentrations, and chemical composition measured at the T0 urban supersite in Mexico City during MILAGRO are analyzed and the degree of closure is evaluated. During the campaign in March 2006, aerosol size distribution and composition often showed strong diurnal variation as a result of both primary emissions and aging of aerosols through coagulation and local photochemical production of secondary aerosol species. The submicron aerosol composition was ~1/2 organic species. Closure analysis is first carried out by comparing CCN concentrations calculated from the measured aerosol size distribution, mixing state, and chemical composition using extended Köhler theory to concurrent CCN measurements at five supersaturations ranging from 0.11% to 0.35%. The closure agreement and its diurnal variation are studied. CCN concentrations are also derived using various simplifications of the measured aerosol mixing state and chemical composition. The uncertainties associated with these simplifications are compared for different supersaturations and the variation of the uncertainties is examined as a function of aerosol age. The results show that the simplification of internally mixed

  19. Time-of-flight aerosol mass spectrometry: Measuring gaseous iodine species after selective uptake in lab-generated aerosols

    NASA Astrophysics Data System (ADS)

    Kundel, Michael; Ries, Marco; Schott, Mathias; Hoffmann, Thorsten

    2010-05-01

    Reactive iodine species play an important role in the marine atmospheric chemistry. Recent studies show that iodine containing compounds (e.g. I2 and ICl) are involved in the tropospheric ozone depletion, the enrichment of iodine in marine aerosols and the formation of new particles in the marine boundary layer (MBL). Various laboratory and field measurements report that molecular iodine (I2) and organoiodine compounds (e.g. CH3I, CH2I2) are the most important precursors for reactive iodine in the MBL[1],[2]. However, the identification and quantification of reactive iodine containing compounds are still analytical challenges. Here, we present a new application of the time-of-flight aerosol mass spectrometer (ToF-AMS) for the quantification of gaseous I2 and ICl in real-time. Time-of-flight aerosol mass spectrometry enables the real-time analysis of the particle size, the particle mass and the chemical composition of non-refractory aerosols[3]. The aerosol enters the ToF-AMS through a critical orifice of 100 μm inner diameter. An aerodynamic lens system focuses the particles in a size range of 50-600 nm as a narrow beam into the vacuum system. While most of the air is removed by a skimmer, the particle beam is transmitted into the particle-sizing chamber. After passing the particle-sizing chamber, the non-refractory particles are flash-vaporized on a heated tungsten surface (500-600 °C) and then ionized by electron impact. The generated ions are extracted by an orthogonal extractor into the time-of-flight mass spectrometer, where the time resolved particle mass detection is performed. Since gaseous compounds are removed inside the ToF-AMS, a direct measurement of gaseous iodine species is not possible. Therefore gaseous iodine species have to be transferred from the gas phase to the particle phase before entering the ToF-AMS. For this purpose α-cyclodextrin (α-CD) particles were used as selective sampling probes for I2 and 1,3,5-trimethoxybenzene (1,3,5-TMB

  20. Vapor-phase concentrations of PAHs and their derivatives determined in a large city: correlations with their atmospheric aerosol concentrations.

    PubMed

    Barrado, Ana Isabel; García, Susana; Sevillano, Marisa Luisa; Rodríguez, Jose Antonio; Barrado, Enrique

    2013-11-01

    Thirteen PAHs, five nitro-PAHs and two hydroxy-PAHs were determined in 55 vapor-phase samples collected in a suburban area of a large city (Madrid, Spain), from January 2008 to February 2009. The data obtained revealed correlations between the concentrations of these compounds and a series of meteorological factors (e.g., temperature, atmospheric pressure) and physical-chemical factors (e.g., nitrogen and sulfur oxides). As a consequence, seasonal trends were observed in the atmospheric pollutants. A "mean sample" for the 14-month period would contain a total PAH concentration of 13835±1625 pg m(-3) and 122±17 pg m(-3) of nitro-PAHs. When the data were stratified by season, it emerged that a representative sample of the coldest months would contain 18900±2140 pg m(-3) of PAHs and 150±97 pg m(-3) of nitro-PAHs, while in an average sample collected in the warmest months, these values drop to 9293±1178 pg m(-3) for the PAHs and to 97±13 pg m(-3) for the nitro-PAHs. Total vapor phase concentrations of PAHs were one order of magnitude higher than concentrations detected in atmospheric aerosol samples collected on the same dates. Total nitro-PAH concentrations were comparable to their aerosol concentrations whereas vapor phase OH-PAHs were below their limits of the detection, indicating these were trapped in airborne particles. PMID:23816454

  1. Estimating the backscatter spectral dependence and relative concentration for multiple aerosol materials from lidar data

    NASA Astrophysics Data System (ADS)

    Warren, Russell E.; Vanderbeek, Richard G.

    2004-08-01

    Detection and estimation of materials in the atmosphere by lidar has heretofore required that the spectral dependence of the relevant cross section coefficients -- backscatter in the case of aerosols and absorptivity for vapors -- be known in advance. While this typically is a reasonable assumption in the case of vapor, the aerosol backscatter coefficients are complicated functions of particle size, shape, and refractive index, and are therefore usually not well characterized a priori. Using incorrect parameters will give biased concentration estimates and impair discrimination ability. This paper describes an approach for estimating both the spectral dependence of the aerosol backscatter and relative concentration range-dependence of a set of materials using multi-wavelength lidar. The approach is based on state-space filtering that applies a Kalman filter in range for concentration, and updates the backscatter spectral estimates through a sequential least-squares algorithm at each time step. The method is illustrated on aerosol-release data of the bio-simulant ovalbumin collected by ECBC during field tests in 2002, as well as synthetic data sets.

  2. Black Carbon Concentration from Worldwide Aerosol Robotic Network (AERONET) Measurements

    NASA Technical Reports Server (NTRS)

    Schuster, Gregory L.; Dubovik, Oleg; Holben, Brent N.; Clothiaux, Eugene E.

    2006-01-01

    The carbon emissions inventories used to initialize transport models and general circulation models are highly parameterized, and created on the basis of multiple sparse datasets (such as fuel use inventories and emission factors). The resulting inventories are uncertain by at least a factor of 2, and this uncertainty is carried forward to the model output. [Bond et al., 1998, Bond et al., 2004, Cooke et al., 1999, Streets et al., 2001] Worldwide black carbon concentration measurements are needed to assess the efficacy of the carbon emissions inventory and transport model output on a continuous basis.

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

    NASA Astrophysics Data System (ADS)

    Wonaschütz, Anna; Hitzenberger, Regina

    2015-04-01

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

  4. Submicron aerosol analysis and organic source apportionment in an urban atmosphere in Pearl River Delta of China using high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    He, Ling-Yan; Huang, Xiao-Feng; Xue, Lian; Hu, Min; Lin, Yun; Zheng, Jun; Zhang, Renyi; Zhang, Yuan-Hang

    2011-06-01

    The Pearl River Delta (PRD) region in South China is one of the most economically developed regions in China while also noted for its severe air pollution, especially in the urban environments. In order to understand in depth the aerosol chemistry and the emission sources in PRD, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site in the Hong Kong-Shenzhen metropolitan area between 25 October and 2 December 2009. Ten minute-resolved measurement data were analyzed, and an average mass concentration of 44.5 ± 34.0 μg m-3 was calculated for the entire campaign. On average, organic matter was the most abundant PM1 component accounting for 39.7% of the total mass, followed by sulfate (24.5%), black carbon (measured by aethalometer, 14.0%), ammonium (10.2%), nitrate (10.0%), and chloride (1.6%). Moreover, organic matter comprised an increasing fraction of the PM1 loading as the PM1 loading increased, denoting its key role in particulate pollution in this region. Calculations of organic elemental composition based on the high-resolution organic mass spectra obtained indicated that C, H, O, and N on average contributed 33.8%, 55.1%, 10.2%, and 0.9%, respectively, to the total atomic numbers of organic aerosol (OA), which corresponded to an OM/OC ratio (the ratio of organic matter mass/organic carbon mass) of 1.57 ± 0.08. Positive matrix factorization analysis was then conducted on the high-resolution organic mass spectral data set. Four OA components were identified, including a hydrocarbon-like (HOA), a biomass burning (BBOA), and two oxygenated (LV-OOA and SV-OOA) components, which on average accounted for 29.5%, 24.1%, 18.8%, and 27.6%, respectively, of the total organic mass. The HOA was found to have contributions from both fossil fuel combustion and cooking emissions, while the BBOA was well correlated with acetonitrile, a known biomass burning marker. The LV-OOA and SV-OOA corresponded to more aged and

  5. A High Performance Liquid Chromatography Method for Determination of Levoglucosan Concentrations in Atmospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Dixon, R. W.; Baltzell, G.

    2002-12-01

    Levoglucosan (1,6-anhydro-β-D-glucopyranose) recently has been measured in atmospheric aerosols where it is a major organic compound originating from biomass combustion. Past analysis methods have used gas chromatography with and without derivitization. We have developed a method for analyzing levoglucosan in atmospheric aerosols using high peformance liquid chromatography (HPLC) with a new detection method called aerosol charge detection. In aerosol charge detection, the column effluent is converted to an aerosol that is charged by passage near a corona discharge region and detected by charge collection. A column specific for carbohydrate compounds, which separates compounds by ligand-exchange and by partitioning based on polarity, was used for the separation using a 100% water eluent at 60°C. Under these conditions, aerosol filter samples extracted in methanol and water gave peaks with the same retention time as a levoglucosan standard. The detection limit was estimated to be about 0.1 μg mL-1 for extracts or 5 to 10 ng m-3 for air sample volumes employed. Samples collected at locations in central New Mexico and central California were found to contain concentrations of levoglucosan from the detection limit to 270 ng m-3, with higher concentrations observed under colder conditions when more fireplaces would tend to be in use. Mannosan (1,6-anhydro-β-D-mannopyranose), another monosaccharide anhydride, also was observed in one sample. The presence of other organic compounds, which have not yet been identified, was inferred by other observed peaks and by an increased baseline in sample chromatograms.

  6. Chemical composition of Titan's aerosols analogues characterized with a systematic pyrolysis-gas chromatography-mass spectrometry characterization

    NASA Astrophysics Data System (ADS)

    Szopa, Cyril; Raulin, Francois; Coll, Patrice; Cabane, Michel; GCMS Team

    2014-05-01

    The in situ chemical characterization of Titan's atmosphere was achieved in 2005 with two instruments present onboard the Huygens atmospheric probe : the Aerosol Collector and Pyrolyzer (ACP) devoted to collect and pyrolyse Titan's aerosols ; the Gas Chromatograph-Mass Spectrometer (GCMS) experiment devoted to analyze gases collected in the atmosphere or coming from the aerosols pyrolysis. The GCMS was developed by Hasso Niemann in the filiation of the quadrupole mass spectrometers he built for several former space missions. The main objectives were to : determine the concentration profile of the most abundant chemical species; seek for minor atmospheric organic species not detected with remote observations ; give a first view of the organic aerosols structure; characterize the condensed volatiles present at the surface (e.g. lakes) in case of survival of the probe to the landing impact. Taking into account for the potential complexity of the gaseous samples to be analyzed, it was decided to couple to the MS analyzer a gas chromatograph capable to separate volatile species from light inorganic molecules and noble gases, to organic compounds including aromatics. This was the first GCMS analyzer that worked in an extraterrestrial environment since the Viking missions on Mars. Even if the GCMS coupling mode did not provide any result of interest, it has been demonstrated to be functional during the Huygens descent. But, the direct MS analysis of the atmosphere, and the pyrolysis-MS analysis of aerosols allowed to make great discoveries which are still of primary importance to describe the Titan's lower atmosphere composition. This contribution aims at presenting this instrument that worked in the Titan's atmosphere, and summarizing the most important discoveries it allowed.

  7. A rocket-borne mass analyzer for charged aerosol particles in the mesosphere

    SciTech Connect

    Knappmiller, Scott; Robertson, Scott; Sternovsky, Zoltan; Friedrich, Martin

    2008-10-15

    An electrostatic mass spectrometer for nanometer-sized charged aerosol particles in the mesosphere has been developed and tested. The analyzer is mounted on the forward end of a rocket and has a slit opening for admitting a continuous sample of air that is exhausted through ports at the sides. Within the instrument housing are two sets of four collection plates that are biased with positive and negative voltages for the collection of negative and positive aerosol particles, respectively. Each collection plate spans about an order of magnitude in mass which corresponds to a factor of 2 in radius. The number density of the charge is calculated from the current collected by the plates. The mean free path for molecular collisions in the mesosphere is comparable to the size of the instrument opening; thus, the analyzer performance is modeled by a Monte Carlo computer code that finds the aerosol particles trajectories within the instrument including both the electrostatic force and the forces from collisions of the aerosol particles with air molecules. Mass sensitivity curves obtained using the computer models are near to those obtained in the laboratory using an ion source. The first two flights of the instrument returned data showing the charge number densities of both positive and negative aerosol particles in four mass ranges.

  8. Aerosol particle and organic vapor concentrations at industrial work sites in Malaysia.

    PubMed

    Armstrong, R W; Rood, M J; Sani, S; Mohamed, M; Rashid, M; Jab, A T; Landsberger, S

    2001-01-01

    The objective of this study was to establish baseline data about air pollutants potentially related to nasopharyngeal carcinoma (NPC) in the Federal Territory and Selangor, Malaysia. During 1991-1993, ambient air quality was monitored at 42 work sites representing ten industrial sectors: adhesive manufacturing, foundries, latex processing, metalworking, plywood/veneer milling, ricemilling, rubber tire manufacturing, sawmilling, shoemaking, and textile related industries. At each work site, aerosol particle size distributions and concentrations of formaldehyde, benzene, toluene, isopropyl alcohol, and furfural were measured. Mean aerosol particle concentrations ranged from 61 micrograms/m3 in foundries to 5,578 micrograms/m3 in ricemills, with five industries (adhesives, metalworking, ricemilling, sawmilling, and shoemaking) exceeding the US EPA 24-hr ambient air standard for PM-10. Formaldehyde concentrations exceeded the threshold limit value (TLV) in adhesives factories. Other vapours and elements measured were well below TLVs. PMID:12109256

  9. Comparison of GOES and MODIS aerosol optical depth (AOD) to aerosol robotic network (AERONET) AOD and IMPROVE PM2.5 mass at Bondville, Illinois.

    PubMed

    Green, Mark; Kondragunta, Shobha; Ciren, Pubu; Xu, Chuanyu

    2009-09-01

    Collocated Interagency Monitoring of Protected Visual Environments (IMPROVE) particulate matter (PM) less than 2.5 microm in aerodynamic diameter (PM2.5) chemically speciated data, mass of PM less than 10 microm in aerodynamic diameter (PM10), and Aerosol Robotic Network (AERONET) aerosol optical depth (AOD) and size distribution at Bondville, IL, were compared with satellite-derived AOD. This was done to evaluate the quality of the Geostationary Operational Environmental Satellite (GOES) and Moderate Resolution Imaging Spectroradiometer (MODIS) AOD data and their potential to predict surface PM2.5 concentrations. MODIS AOD correlated better to AERONET AOD (r = 0.835) than did GOES AOD (r = 0.523). MODIS and GOES AOD compared better to AERONET AOD when the particle size distribution was dominated by fine mode. For all three AOD methods, correlation between AOD and PM2.5 concentration was highest in autumn and lowest in winter. The AERONET AOD-PM2.5 relationship was strongest with moderate relative humidity (RH). At low RH, AOD attributable to coarse mass degrades the relationship; at high RH, added AOD from water growth appears to mask the relationship. For locations such as many in the central and western United States with substantial coarse mass, coarse mass contributions to AOD may make predictions of PM2.5 from AOD data problematic. Seasonal and diurnal variations in particle size distributions, RH, and seasonal changes in boundary layer height need to be accounted for to use satellite AOD to predict surface PM2.5. PMID:19785275

  10. Laboratory investigation of photochemical oxidation of organic aerosol from wood fires Part 2: Analysis of aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Grieshop, A. P.; Donahue, N. M.; Robinson, A. L.

    2008-09-01

    Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA) in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit mass resolution quadrupole Aerosol Mass Spectrometer (AMS). The results highlight how photochemical processing can lead to considerable evolution of the mass, the volatility and the level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the primary contribution after a few hours of aging under typical summertime conditions. Aging decreased the OA volatility of the total OA as measured with a thermodenuder; it also made the OA progressively more oxygenated in every experiment. With explicit knowledge of the condensed-phase mass spectrum (MS) of the primary emissions from each fire, each MS can be decomposed into primary and residual spectra throughout the experiment. The residual spectra provide an estimate of the composition of the photochemically produced OA. These spectra are also very similar to those of the oxygenated OA that dominates ambient AMS datasets. In addition, aged wood smoke spectra are shown to be similar to those from OA created by photo-oxidized dilute diesel exhaust and aged biomass-burning OA measured in urban and remote locations. This demonstrates that the oxygenated OA observed in the atmosphere can be produced by photochemical aging of dilute emissions from combustion of fuels containing both modern and fossil carbon.

  11. Simulations of organic aerosol concentrations during springtime in the Guanzhong Basin, China

    NASA Astrophysics Data System (ADS)

    Feng, Tian; Li, Guohui; Cao, Junji; Bei, Naifang; Shen, Zhenxing; Zhou, Weijian; Liu, Suixin; Zhang, Ting; Wang, Yichen; Huang, Ru-jin; Tie, Xuexi; Molina, Luisa T.

    2016-08-01

    The organic aerosol (OA) concentration is simulated in the Guanzhong Basin, China from 23 to 25 April 2013 utilizing the WRF-CHEM model. Two approaches are used to predict OA concentrations: (1) a traditional secondary organic aerosol (SOA) module; (2) a non-traditional SOA module including the volatility basis-set modeling method in which primary organic aerosol (POA) is assumed to be semivolatile and photochemically reactive. Generally, the spatial patterns and temporal variations of the calculated hourly near-surface ozone and fine particle matters agree well with the observations in Xi'an and surrounding areas. The model also yields reasonable distributions of daily PM2.5 and elemental carbon (EC) compared to the filter measurements at 29 sites in the basin. Filter-measured organic carbon (OC) and EC are used to evaluate OA, POA, and SOA using the OC / EC ratio approach. Compared with the traditional SOA module, the non-traditional module significantly improves SOA simulations and explains about 88 % of the observed SOA concentration. Oxidation and partitioning of POA treated as semivolatile constitute the most important pathway for the SOA formation, contributing more than 75 % of the SOA concentrations in the basin. Residential emissions are the dominant anthropogenic OA source, constituting about 50 % of OA concentrations in urban and rural areas and 30 % in the background area. The OA contribution from transportation emissions decreases from 25 % in urban areas to 20 % in the background area, and the industry emission OA contribution is less than 6 %.

  12. Primary and secondary organic aerosols in urban air masses intercepted at a rural site

    NASA Astrophysics Data System (ADS)

    Liggio, John; Li, Shao-Meng; Vlasenko, Alexander; Sjostedt, Steve; Chang, Rachel; Shantz, Nicole; Abbatt, Jonathan; Slowik, J. G.; Bottenheim, J. W.; Brickell, P. C.; Stroud, C.; Leaitch, W. Richard

    2010-11-01

    Measurements made at a rural site in central Ontario during May-June 2007 are used to investigate the composition of organic aerosol (OA) downwind of an urban region. Observations of aerosol organic carbon and oxygen containing fragments from a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) are combined with toluene to benzene ratios to estimate the relative importance of secondary organic aerosol (SOA) and primary organic aerosol (POA) to the total OA at the site during periods of significant urban influence. We estimate that SOA formed within 1-2 days of the anthropogenic source regions was 40-50% of the measured OA and that POA was 5-16% of the OA. The remaining 35-45% of the OA is assumed to have been present in the aerosol upwind of the source regions prior to entering the study domain as defined by trajectories and estimates of the potential photochemical aging time. The apportionment results were also compared to that of positive matrix factorization analysis. In addition, the measurements of the molar oxygen to carbon ratio (O/C) in the OA demonstrates that SOA becomes progressively more oxygenated with increasing photochemical age and at low total OA mass.

  13. Mass distributions and morphological and chemical characterization of urban aerosols in the continental Balkan area (Belgrade).

    PubMed

    Đorđević, D; Buha, J; Stortini, A M; Mihajlidi-Zelić, A; Relić, D; Barbante, C; Gambaro, A

    2016-01-01

    This work presents characteristics of atmospheric aerosols of urban central Balkans area, using a size-segregated aerosol sampling method, calculation of mass distributions, SEM/EDX characterization, and ICP/MS analysis. Three types of mass distributions were observed: distribution with a pronounced domination of coarse mode, bimodal distribution, and distribution with minimum at 1 μm describing the urban aerosol. SEM/EDX analyses have shown morphological difference and variation in the content of elements in samples. EDX spectra demonstrate that particles generally contain the following elements: Al, Ca, K, Fe, Mg, Ni, K, Si, S. Additionally, the presence of As, Br, Sn, and Zn found in air masses from southeast segment points out the anthropogenic activities most probably from mining activities in southeastern part of Serbia. The ratio Al/Si equivalent to the ratio of desert dust was associated with air masses coming from southeastern and southwestern segments, pointing to influences from North Africa and Middle East desert areas whereas the Al/Si ratio in other samples is significantly lower. In several samples, we found high values of aluminum in the nucleation mode. Samples with low share of crustal elements in the coarse mode are collected when Mediterranean air masses prevailed, while high share in the coarse mode was associated with continental air masses that could be one of the approaches for identification of the aerosol origin. Graphical abstract ᅟ. PMID:26347417

  14. Anthropogenic sources of aerosol particles in a football stadium: Real-time characterization of emissions from cigarette smoking, cooking, hand flares, and color smoke bombs by high-resolution aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Faber, Peter; Drewnick, Frank; Veres, Patrick R.; Williams, Jonathan; Borrmann, Stephan

    2013-10-01

    Aerosol particles from several anthropogenic sources associated with football stadia including cooking, cigarette smoking, burning of color smoke bombs and hand flares were analyzed by high-resolution aerosol mass spectrometry. The physical and chemical characteristics of these different aerosols, in particular the organic fraction, were explored in laboratory studies to obtain robust references. These data were compared with field campaign results from a Bundesliga (German football league) match in the Coface Arena (Mainz, Germany) on 20th April 2012. The field measurement revealed a strongly elevated mass concentration of organic aerosols (OA) compared to background levels showing a temporal structure clearly related to the match. PMF analysis established that during the football match event cigarette smoke was the predominant component of submicron organic aerosol (67% of total OA). Cooking emissions from food outlets within the stadium correlated well with the sales figures of the catering stations and were also found to be of relevance (24% of total OA) especially in the period before kickoff. Pyrotechnics were not observed during this football match and no signatures of these sources were found in the mass spectra from the stadium measurements. All species that were elevated during the football match returned to their initial background levels within one hour after the match had finished. This demonstrates a good ventilation capacity of the open-topped Coface Arena.

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

    DOE PAGESBeta

    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

  16. Vertical distribution of aerosol number concentration in the troposphere over Siberia derived from airborne in-situ measurements

    NASA Astrophysics Data System (ADS)

    Arshinov, Mikhail Yu.; Belan, Boris D.; Paris, Jean-Daniel; Machida, Toshinobu; Kozlov, Alexandr; Malyskin, Sergei; Simonenkov, Denis; Davydov, Denis; Fofonov, Alexandr

    2016-04-01

    Knowledge of the vertical distribution of aerosols particles is very important when estimating aerosol radiative effects. To date there are a lot of research programs aimed to study aerosol vertical distribution, but only a few ones exist in such insufficiently explored region as Siberia. Monthly research flights and several extensive airborne campaigns carried out in recent years in Siberian troposphere allowed the vertical distribution of aerosol number concentration to be summarized. In-situ aerosol measurements were performed in a wide range of particle sizes by means of improved version of the Novosibirsk-type diffusional particle sizer and GRIMM aerosol spectrometer Model 1.109. The data on aerosol vertical distribution enabled input parameters for the empirical equation of Jaenicke (1993) to be derived for Siberian troposphere up to 7 km. Vertical distributions of aerosol number concentration in different size ranges averaged for the main seasons of the year will be presented. This work was supported by Interdisciplinary integration projects of the Siberian Branch of the Russian Academy of Science No. 35, No. 70 and No. 131; the Branch of Geology, Geophysics and Mining Sciences of RAS (Program No. 5); and Russian Foundation for Basic Research (grant No. 14-05-00526). Jaenicke R. Tropospheric aerosols, in Aerosol-Cloud-Climate Interactions, edited by P.V. Hobs. -Academic Press, San Diego, CA, 1993.- P. 1-31.

  17. Aerosol-Radiation Feedback and PM10 Air Concentrations Over Poland

    NASA Astrophysics Data System (ADS)

    Werner, Małgorzata; Kryza, Maciej; Skjøth, Carsten Ambelas; Wałaszek, Kinga; Dore, Anthony J.; Ojrzyńska, Hanna; Kapłon, Jan

    2016-03-01

    We have implemented the WRF-Chem model version 3.5 over Poland to quantify the direct and indirect feedback effects of aerosols on simulated meteorology and aerosol concentrations. Observations were compared with results from three simulations at high spatial resolutions of 5 × 5 km: (1) BASE—without any aerosol feedback effects; (2) DIR—with direct aerosol-radiative effects (3) INDIR—with direct and indirect aerosol-radiative effects. We study the overall effect during January 2011 as well as selected episodes of the highest differences in PM10 concentrations between the three simulations. For the DIR simulation, the decrease in monthly mean incoming solar radiation (SWDOWN) appears for the entire study area. It changes geographically, from about -8.0 to -2.0 W m-2, respectively for the southern and northern parts of the country. The highest changes do not correspond to the highest PM10 concentration. Due to the solar radiation changes, the surface mean monthly temperature (T2) decreases for 96 % of the area of Poland, but not more than 1.0 °C. Monthly mean PBLH changes by more than ±5 m for 53 % of the domain. Locally the differences in PBLH between the DIR and BASE are higher than ± 20 m. Due to the direct effect, for 84 % of the domain, the mean monthly PM10 concentrations increase by up to 1.9 µg m-3. For the INDIR simulation the spatial distribution of changes in incoming solar radiation as well as air temperature is similar to the DIR simulation. The decrease of SWDOWN is noticed for the entire domain and for 23 % of the domain is higher than -5.0 W m-2. The absolute differences of PBLH are slightly higher for INDIR than DIR but similarly distributed spatially. For daily episodes, the differences between the simulations are higher, both for meteorology and PM10 concentrations, and the pattern of changes is usually more complex. The results indicate the potential importance of the aerosol feedback effects on modelled meteorology and PM10

  18. Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Slowik, J. G.; Richter, R.; Reche, C.; Alastuey, A.; Querol, X.; Seco, R.; Peñuelas, J.; Jiménez, J. L.; Crippa, M.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.

    2011-10-01

    PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O/C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O/C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the organic mass fragments at m/z 55, 57, and 44 is developed here and

  19. Characterization of Organic Nitrogen in the Atmosphere Using High Resolution Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Ge, X.; Sun, Y.; Chen, M.; Zhang, Q.

    2015-12-01

    Despite extensive efforts on characterizing organic nitrogen (ON) compounds in atmospheric aerosols and aqueous droplets, knowledge of ON chemistry is still limited, mainly due to its chemical complexity and lack of highly time-resolved measurements. This work is aimed at optimizing the method of using Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) to characterize ON compounds in atmospheric aerosols. Seventy-five pure nitrogen-containing organic compounds covering a variety of functional groups were analyzed with the HR-AMS. Our results show that ON compounds commonly produce NHx+, NOx+, which are usually attributed to inorganic N species such as ammonium and nitrate, and CH2N+ at m/z = 28, which is rarely quantified in ambient aerosol due to large interference from N2+ in the air signal. As a result, using the nitrogen-to-carbon (N/C) calibration factor proposed by Aiken et al. (2008) on average leads to ~ 20% underestimation of N/C in ambient organic aerosol. A new calibration factor of 0.79 is proposed for determining the average N/C in organics. The relative ionization efficiencies (RIEs) of different ON species, on average, are found to be consistent with the default RIE value (1.4) for the total organics. The AMS mass spectral features of various types of ON species (amines, amides, amino acids, etc.) are examined and used for characterizing ON composition in ambient aerosols. Our results indicate that submicron organic aerosol measured during wintertime in Fresno, CA contains significant amounts of amino-compounds whereas more diversified ON species, including N-containing aromatic heterocycle (e.g., imidazoles), are observed in fog waters collected simultaneously. Our findings have important implications for understanding atmospheric ON behaviors via the widespread HR-AMS measurements of ambient aerosols and droplets.

  20. Analysis of secondary organic aerosols from ozonolysis of isoprene by proton transfer reaction mass spectrometry

    NASA Astrophysics Data System (ADS)

    Inomata, Satoshi; Sato, Kei; Hirokawa, Jun; Sakamoto, Yosuke; Tanimoto, Hiroshi; Okumura, Motonori; Tohno, Susumu; Imamura, Takashi

    2014-11-01

    To understand the mechanism of formation of the secondary organic aerosols (SOAs) produced by the ozonolysis of isoprene, proton transfer reaction mass spectrometry (PTR-MS) was used to identify the semi-volatile organic compounds (SVOCs) produced in both the gaseous and the aerosol phases and to estimate the gas-aerosol partitioning of each SVOC in chamber experiments. To aid in the identification of the SVOCs, the products were also studied with negative ion-chemical ionization mass spectrometry (NI-CIMS), which can selectively detect carboxylic acids and hydroperoxides. The gaseous products were observed by on-line PTR-MS and NI-CIMS, whereas the SVOCs in SOAs collected on a filter were vaporized by heating the filter and were then analysed by off-line PTR-MS and NI-CIMS. The formation of oligomeric hydroperoxides involving a Criegee intermediate as a chain unit was observed in both the gaseous and the aerosol phases by NI-CIMS. PTR-MS also detected oligomeric hydroperoxides as protonated molecules from which a H2O molecule was eliminated, [M-OH]+. In the aerosol phase, oligomers involving formaldehyde and methacrolein as chain units were observed by PTR-MS in addition to oligomeric hydroperoxides. The gas-aerosol partitioning of each component was calculated from the ion signals in the gaseous and aerosol phases measured by PTR-MS. From the gas-aerosol partitioning, the saturated vapour pressures of the oligomeric hydroperoxides were estimated. Measurements by a fast-mobility-particle-sizer spectrometer revealed that the increase of the number density of the particles was complete within a few hundred seconds from the start of the reaction.

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

    NASA Astrophysics Data System (ADS)

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

    2014-11-01

    The sources and composition of atmospheric marine aerosol particles (aMA) have been investigated with a range of physical and chemical measurements from open-ocean research cruises. This study uses the characteristic functional group composition (from Fourier transform infrared spectroscopy) of aMA from five ocean regions to show the following: (i) The organic functional group composition of aMA that can be identified as mainly atmospheric primary marine (ocean derived) aerosol particles (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 or continental emissions mix in alkane and carboxylic acid groups. (ii) The organic composition of aPMA is nearly identical to model-generated primary marine aerosol particles from bubbled seawater (gPMA, which has 55 ± 14% hydroxyl, 32 ± 14% alkane, and 13 ± 3% 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 and the ratio of organic carbon to sodium (OC/Na+) in the gPMA remained nearly constant over a broad range of chlorophyll a concentrations, the gPMA alkane group fraction appeared to increase with chlorophyll a concentrations (r = 0.66). gPMA from productive seawater had a larger fraction of alkane functional groups (42 ± 9%) compared to gPMA from nonproductive seawater (22 ± 10%), perhaps 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

  2. Detailed mass size distributions of elements and species, and aerosol chemical mass closure during fall 1999 at Gent, Belgium

    NASA Astrophysics Data System (ADS)

    Maenhaut, Willy; Cafmeyer, Jan; Dubtsov, Sergei; Chi, Xuguang

    2002-04-01

    A 10-stage microorifice uniform deposit impactor (MOUDI) and a 12-stage small deposit area low pressure impactor (SDI) were operated at Gent from 6 September to 30 October 1999. Thirty-four parallel samples (of typically 24 h) were collected. The MOUDI samples were analysed for the particulate mass (PM) by weighing, and for organic carbon (OC) and elemental carbon (EC) by a thermal-optical transmission technique. The SDI samples were analysed for 27 elements by PIXE. PM and OC exhibited typically a rather similar bimodal size distribution, with most of their mass in the submicrometer size range. EC was predominantly associated with fine particles, with maximum typically at around 0.2 μm equivalent aerodynamic diameter (EAD). Sulphur was also mainly in the fine size range, but with maximum at 0.5 μm EAD. Other elements with mainly a fine mode were V, Ni, As, Se and Pb. The crustal elements (Al, Si, Ti, Fe, Zr) exhibited mostly a unimodal coarse mode size distribution, with maximum at about 4 μm EAD. Other elements with mainly a coarse mode were Na, Mg, P, Ca, Cr, Mn, Cu, Ga and Sr. The elements K, Zn and Rb were generally bimodal. Aerosol chemical mass closure calculations indicated that organic aerosol and crustal matter were the major aerosol types in the supermicrometer size range, and that the dominant aerosol types in the submicrometer fraction were organic aerosol and sulphate. On average, 74% of the gravimetric PM was accounted for by the aerosol types considered.

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

    SciTech Connect

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

    2009-11-27

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

  4. Evolution of organic aerosol mass spectra upon heating: implications for OA phase and partitioning behavior

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

    VUV mass spectra for two distinct aerosol types as they are passed through a thermodenuder at different temperatures have been measured. The two aerosol types considered are primary lubricating oil (LO) aerosol and secondary aerosol from the α-pinene + O3 reaction (αP). The evolution of the VUV mass spectra for the two aerosol types with temperature are observed to differ dramatically. For LO particles, the spectra exhibit distinct, T-dependent changes in which the lower m/z peaks, corresponding to compounds with higher vapor pressures, disappear more rapidly than the high m/z peaks. In stark contrast, the αP aerosol spectrum is essentially unchanged by temperature even though the particles experience significant mass loss due to evaporation. The variations in the LO spectra are found to be quantitatively in good agreement with expectations from absorptive partitioning theory whereas the αP spectra suggest that the evaporation of αP particles is not governed by partitioning theory. We postulate that this difference arises from the αP particles existing as a glass instead of having the expected liquid-like behavior. To reconcile these observations with decades of aerosol growth experiments, which indicate that OA formation is describable through equilibrium partitioning, we put forward a sequential partitioning model wherein secondary OA is rapidly converted from an absorbing form to a non-absorbing form. The results suggest that although OA growth may be describable through equilibrium partitioning theory, the thermodynamic properties of formed OA particles may differ significantly from the properties determined in the equilibrium framework.

  5. New characteristics of submicron aerosols and factor analysis of combined organic and inorganic aerosol mass spectra during winter in Beijing

    NASA Astrophysics Data System (ADS)

    Zhang, J. K.; Ji, D. S.; Liu, Z. R.; Hu, B.; Wang, L. L.; Huang, X. J.; Wang, Y. S.

    2015-07-01

    In recent years, an increasing amount of attention has been paid to heavy haze pollution in Beijing, China. In addition to Beijing's population of approximately 20 million and its 5 million vehicles, nearby cities and provinces are host to hundreds of heavily polluting industries. In this study, a comparison between observations in January 2013 and January 2014 showed that non-refractory PM1 (NR-PM1) pollution was weaker in January 2014, which was primarily caused by variations in meteorological conditions. For the first time, positive matrix factorization (PMF) was applied to the merged high-resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer measurements in Beijing, and the sources and evolution of NR-PM1 in January 2014 were investigated. The two factors, NO3-OA1 and NO3-OA2, were primarily composed of ammonium nitrate, and each showed a different degree of oxidation and diurnal variation. The organic fraction of SO4-OA showed the highest degree of oxidation of all PMF factors. The hydrocarbon-like organic aerosol (OA) and cooking OA factors contained negligible amounts of inorganic species. The coal combustion OA factor contained a high contribution from chloride in its mass spectrum. The NR-PM1 composition showed significant variations in January 2014, in which the contribution of nitrate clearly increased during heavy pollution events. The most effective way to control fine particle pollution in Beijing is through joint prevention and control measures at the regional level, rather than a focus on an individual city, especially for severe haze events.

  6. Laboratory investigation of photochemical oxidation of organic aerosol from wood fires 2: analysis of aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Grieshop, A. P.; Donahue, N. M.; Robinson, A. L.

    2009-03-01

    Experiments were conducted to investigate the effects of photo-oxidation on organic aerosol (OA) in dilute wood smoke by exposing emissions from soft- and hard-wood fires to UV light in a smog chamber. This paper focuses on changes in OA composition measured using a unit-mass-resolution quadrupole Aerosol Mass Spectrometer (AMS). The results highlight how photochemical processing can lead to considerable evolution of the mass, volatility and level of oxygenation of biomass-burning OA. Photochemical oxidation produced substantial new OA, more than doubling the OA mass after a few hours of aging under typical summertime conditions. Aging also decreased the volatility of the OA and made it progressively more oxygenated. The results also illustrate strengths of, and challenges with, using AMS data for source apportionment analysis. For example, the mass spectra of fresh and aged BBOA are distinct from fresh motor-vehicle emissions. The mass spectra of the secondary OA produced from aging wood smoke are very similar to those of the oxygenated OA (OOA) that dominates ambient AMS datasets, further reinforcing the connection between OOA and OA formed from photo-chemistry. In addition, aged wood smoke spectra are similar to those from OA created by photo-oxidizing dilute diesel exhaust. This demonstrates that the OOA observed in the atmosphere can be produced by photochemical aging of dilute emissions from different types of combustion systems operating on fuels with modern or fossil carbon. Since OOA is frequently the dominant component of ambient OA, the similarity of spectra of aged emissions from different sources represents an important challenge for AMS-based source apportionment studies.

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

    PubMed

    Kückelmann, U; Warscheid, B; Hoffmann, T

    2000-04-15

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

  8. Identification and quantification of organic aerosol from cooking and other sources in Barcelona using aerosol mass spectrometer data

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Decarlo, P. F.; Heringa, M. F.; Chirico, R.; Slowik, J. G.; Richter, R.; Reche, C.; Alastuey, A.; Querol, X.; Seco, R.; Peñuelas, J.; Jiménez, J. L.; Crippa, M.; Zimmermann, R.; Baltensperger, U.; Prévôt, A. S. H.

    2012-02-01

    PM1 (particulate matter with an aerodynamic diameter <1 μm) non-refractory components and black carbon were measured continuously together with additional air quality and atmospheric parameters at an urban background site in Barcelona, Spain, during March 2009 (campaign DAURE, Determination of the sources of atmospheric Aerosols in Urban and Rural Environments in the western Mediterranean). Positive matrix factorization (PMF) was conducted on the organic aerosol (OA) data matrix measured by an aerosol mass spectrometer, on both unit mass (UMR) and high resolution (HR) data. Five factors or sources could be identified: LV-OOA (low-volatility oxygenated OA), related to regional, aged secondary OA; SV-OOA (semi-volatile oxygenated OA), a fresher oxygenated OA; HOA (hydrocarbon-like OA, related to traffic emissions); BBOA (biomass burning OA) from domestic heating or agricultural biomass burning activities; and COA (cooking OA). LV-OOA contributed 28% to OA, SV-OOA 27%, COA 17%, HOA 16%, and BBOA 11%. The COA HR spectrum contained substantial signal from oxygenated ions (O:C: 0.21) whereas the HR HOA spectrum had almost exclusively contributions from chemically reduced ions (O:C: 0.03). If we assume that the carbon in HOA is fossil while that in COA and BBOA is modern, primary OA in Barcelona contains a surprisingly high fraction (59%) of non-fossil carbon. This paper presents a method for estimating cooking organic aerosol in ambient datasets based on the fractions of organic mass fragments at m/z 55 and 57: their data points fall into a V-shape in a scatter plot, with strongly influenced HOA data aligned to the right arm and strongly influenced COA data points aligned to the left arm. HR data show that this differentiation is mainly driven by the oxygen-containing ions C3H3O+ and C3H5O+, even though their contributions to m/z 55 and 57 are low compared to the reduced ions C4H7+ and C4H9+. A simple estimation method based on the markers m/z 55, 57, and 44 is

  9. Hillslope soil erosion estimated from aerosol concentrations, North Halawa Valley, Oahu, Hawaii

    USGS Publications Warehouse

    Hill, B.R.; Fuller, C.C.; DeCarlo, E.H.

    1997-01-01

    Concentrations of aerosolic quartz and 137Cs were used to estimate rates of hillslope soil erosion during 1990-91 in the North Halawa Valley on the island of Oahu, Hawaii. Fluvial transport of quartz was estimated to be 6.1 Mg in 1990 and 14.9 Mg in 1991. Fluvial transport of 137Cs from North Halawa Valley was estimated to be 1.29 ?? 109 pCi in 1991. Results were used with quartz contents, 137Cs activities, and bulk densities of hillslope soils to compute rates of basinwide hillslope soil erosion ranging from 0.1 to 0.3 mm yr-1. These rates are within the range of previous estimates of denudation computed for drainage basins on Oahu. The aerosol-concentration approach, therefore, is a useful method for assessing basinwide soil erosion.

  10. The Influence of High Aerosol Concentration on Atmospheric Boundary Layer Temperature Stratification

    SciTech Connect

    Khaykin, M.N.; Kadygrove, E.N.; Golitsyn, G.S.

    2005-03-18

    Investigations of the changing in the atmospheric boundary layer (ABL) radiation balance as cased by natural and anthropogenic reasons is an important topic of the U.S. Department of Energy's Atmospheric Radiation Measurement (ARM) program. The influence of aerosol on temperature stratification of ABL while its concentration was extremely high within a long period of time was studied experimentally. The case was observed in Moscow region (Russia) with the transport of combustion products from peat-bog and forest fires in July-September, 2002. At this time the visibility was some times at about 100-300 m. Aerosol concentration measured by Moscow University Observatory and A.M. Obukhov Institute of Atmospheric Physics field station in Zvenigorod (55.7 N; 36.6 E) for several days was in 50-100 times more than background one (Gorchakov at al 2003). The high aerosol concentration can change the radiation balance at ABL, and so to change thermal stratification in ABL above the mega lopolis. For the analysis the data were used of synchronous measurements by MTP-5 (Microwave Temperature Profiler operating at wavelength 5 mm) in two locations, namely: downtown Moscow and country-side which is 50 km apart to the West (Zvenigorod station). (Kadygrov and Pick 1998; Westwater at al 1999; Kadygrov at al 2002). Zvenigorod station is located in strongly continental climate zone which is in between of the climates of ARM sites (NSANorth Slope of Alaska and SGP-Southern Great Plains). The town of Zvenigorod has little industry, small traffic volume and topography conductive to a good air ventilation of the town. For these reasons Zvenigorod can be considered as an undisturbed rural site. For the analysis some days were chosen with close meteorological parameters (average temperature, humidity, wind, pressure and cloud form) but strongly differing in aerosol concentration level.

  11. Mammographic mass detection based on extended concentric morphology model

    NASA Astrophysics Data System (ADS)

    Li, Yanfeng; Chen, Houjin

    2014-01-01

    Breast cancer occurs with high frequency among women. In most cases, the main early signs appear as mass and calcification. Distinguishing masses from normal tissues is still a challenging work as mass varies with shapes, margins and sizes. In this paper, a novel method for mass detection in mammograms was presented. First, morphology operators are employed to locate mass candidates. Then anisotropic diffusion was applied to make mass region display better multiple concentric layers (MCL). Finally an extended concentric morphology model (ECMM) criterion combining MCL criterion and template matching was proposed to detect masses. This method was examined on 170 images from Digital Database for Screening Mammography (DDSM) database. The detection rate is 93.92% at 1.88 false positives per image (FPs/I), demonstrating the effectiveness of the proposed method.

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

    NASA Astrophysics Data System (ADS)

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

    2015-09-01

    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

  13. Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.; McKinney, K.; Martin, S. T.; Hu, M.; Budisulistiorini, S. H.; Riva, M.; Surratt, J. D.; St. Clair, J. M.; Isaacman-Van Wertz, G.; Yee, L. D.; Goldstein, A. H.; Carbone, S.; Brito, J.; Artaxo, P.; de Gouw, J. A.; Koss, A.; Wisthaler, A.; Mikoviny, T.; Karl, T.; Kaser, L.; Jud, W.; Hansel, A.; Docherty, K. S.; Alexander, M. L.; Robinson, N. H.; Coe, H.; Allan, J. D.; Canagaratna, M. R.; Paulot, F.; Jimenez, J. L.

    2015-10-01

    Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12-40 ‰) but varies substantially between locations, which is shown to reflect

  14. Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    DOE PAGESBeta

    Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; et al

    2015-10-23

    Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accountedmore » by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O (fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown

  15. Influence of a high aerosol concentration on the thermal structure of the atmospheric boundary layer

    NASA Astrophysics Data System (ADS)

    Khaikin, M. N.; Kuznetsova, I. N.; Kadygrov, E. N.

    2006-12-01

    The influence of increased concentrations of submicron aerosol produced by forest fires on thermal characteristics of the atmospheric boundary layer (ABL) in Moscow and its remote vicinity (the town of Zvenigorod) are analyzed on the basis of regular remote measurements of the ABL temperature profile with the use of MTP-5 profilers. In the air basin of a large city, additional aerosol and accompanying pollutants in early morning hours (at small heights of the Sun) most frequently did not cause substantial changes in the ABL thermal structure. In the locality remote from the megalopolis (Zvenigorod), the atmospheric pollution by aerosol led to noticeable changes in the ABL thermal characteristics. Especially strong changes were observed in the daytime, during the maximum supply of solar radiation. In morning hours, the heating rate of the lower 100-m layer of the polluted air exceeded the heating rate of a relatively pure air by more than one degree. In higher layers, the differences between the rates of temperature changes in a relatively clean atmosphere and in an atmosphere polluted by aerosol (in the suburb) were insignificant.

  16. The contribution of secondary organic aerosol to PM2.5 concentrations in Pittsburgh

    NASA Astrophysics Data System (ADS)

    Cabada, J. C.; Pandis, S. N.; Robinson, A. L.; Subramanian, R.; Polidori, A.; Turpin, B.

    2002-12-01

    A major component of PM2.5 in the Eastern US is carbonaceous material. This organic particulate matter results from both direct emissions from sources such as automobiles, trucks and industries (primary), and from the oxidation of organic gases (secondary). Data from the Pittsburgh Air Quality Study are used to examine the contribution of secondary organic aerosol to the total organic aerosol loading measured in the city during 2001 and 2002. The contribution of secondary organic aerosol is estimated by using elemental carbon as a tracer for primary emissions of organic particulate matter (OC to EC ratio approach). A systematic method for the determination of the primary ratio has been developed based on the correlation of measurements of OC and EC to gaseous tracers of photochemical activity (O3) and primary emissions (CO, NOx). This method is applied to different sets of organic aerosols measurements (using an undenuded sampler, a denuded sampler and an in-situ carbon analyzer) for carbonaceous concentrations. Consistent results for the SOA fraction are obtained when the method is applied to the different sets of measurements for OC and EC. This approach indicates that between 20 and 40% of the organic particulate matter in Pittsburgh during the summer and fall of 2001 is secondary in origin while negligible contributions of SOA are estimated for the winter of 2001 and the spring of 2002.

  17. Online Aerosol Mass Spectrometry of Single Micrometer-Sized Particles Containing Poly(ethylene glycol)

    SciTech Connect

    Bogan, M J; Patton, E; Srivastava, A; Martin, S; Fergenson, D; Steele, P; Tobias, H; Gard, E; Frank, M

    2006-10-25

    Analysis of poly(ethylene glycol)(PEG)-containing particles by online single particle aerosol mass spectrometers equipped with laser desorption ionization (LDI) is reported. We demonstrate that PEG-containing particles are useful in the development of aerosol mass spectrometers because of their ease of preparation, low cost, and inherently recognizable mass spectra. Solutions containing millimolar quantities of PEGs were nebulized and, after drying, the resultant micrometer-sized PEG containing particles were sampled. LDI (266 nm) of particles containing NaCl and PEG molecules of average molecular weight <500 generated mass spectra reminiscent of mass spectra of PEG collected by other MS schemes including the characteristic distribution of positive ions (Na{sup +} adducts) separated by the 44 Da of the ethylene oxide units separating each degree of polymerization. PEGs of average molecular weight >500 were detected from particles that also contained t the tripeptide tyrosine-tyrosine-tyrosine or 2,5-dihydroxybenzoic acid, which were added to nebulized solutions to act as matrices to assist LDI using pulsed 266 nm and 355 nm lasers, respectively. Experiments were performed on two aerosol mass spectrometers, one reflectron and one linear, that each utilize two time-of-flight mass analyzers to detect positive and negative ions created from a single particle. PEG-containing particles are currently being employed in the optimization of our bioaerosol mass spectrometers for the application of measurements of complex biological samples, including human effluents, and we recommend that the same strategies will be of great utility to the development of any online aerosol LDI mass spectrometer platform.

  18. Concentrations and composition of aerosols and particulate matter in surface waters along the transatlantic section

    NASA Astrophysics Data System (ADS)

    Nemirovskaya, I. A.; Lisitzin, A. P.; Novigatsky, A. N.; Redzhepova, Z. U.; Dara, O. M.

    2016-07-01

    Along the transatlantic section from Ushuaia to Gdańsk (March 26-May 7, 2015; cruise 47 of R/V Akademik Ioffe), data were obtained on the concentrations of aerosols in the near-water layer of the atmosphere and of particulate matter in surface waters, as well as of organic compounds within the considered matter (Corg, chlorophyll a, lipids, and hydrocarbons). The concentrations of aerosols amounted to 1237-111 739 particles/L for the fraction of 0.3-1 μm and to 0.02-34.4 μg/m2/day for the matter collected by means of the network procedure. The distribution of aerosols is affected by circumcontinental zoning and by the fluxes from arid areas of African deserts. The maximum concentration of the treated compounds were found in the river-sea frontal area (the runoff of the Colorado River, Argentina), as well as when nearing the coasts, especially in the English Channel.

  19. Determination of particulate lead during MILAGRO/MCMA-2006 using Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

    2010-02-01

    We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s) and ~75% exhibiting slow evaporation (τ~2.4 min) at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at T0 (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the compounds generating Pb

  20. Determination of particulate lead using aerosol mass spectrometry: MILAGRO/MCMA-2006 observations

    NASA Astrophysics Data System (ADS)

    Salcedo, D.; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

    2010-06-01

    We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO)/Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600 °C. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ<0.1 s) and ~75% exhibiting slow evaporation (τ~2.4 min) at the T0 urban supersite and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 min with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the

  1. Determination of particulate lead during MILAGRO / MCMA-2006 using Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Salcedo, Dara; Onasch, T. B.; Aiken, A. C.; Williams, L. R.; de Foy, B.; Cubison, M. J.; Worsnop, D. R.; Molina, L. T.; Jimenez, J. L.

    2010-05-01

    We report the first measurements of particulate lead (Pb) from Aerodyne Aerosol Mass Spectrometers, which were deployed in and around Mexico City during the Megacity Initiative: Local and Global Research Observations (MILAGRO) / Mexico City Metropolitan Area 2006 (MCMA-2006) field campaigns. The high resolution mass spectrometer of one of the AMS instruments (HR-AMS) and the measured isotopic ratios unequivocally prove the detection of Pb in ambient particles. A substantial fraction of the lead evaporated slowly from the vaporizer of the instruments, which is indicative of species with low volatility at 600oC. A model was developed in order to estimate the ambient particulate Pb entering the AMS from the signals in the "open" and the "closed" (or "background") mass spectrum modes of the AMS. The model suggests the presence of at least two lead fractions with ~25% of the Pb signal exhibiting rapid evaporation (1/e decay constant, τ < 0.1 s) and ~75% exhibiting slow evaporation (τ ~2.4 min) at T0 and a different fraction (70% prompt and 30% slow evaporation) at a site northwest from the metropolitan area (PEMEX32 site). From laboratory experiments with pure Pb(NO3)2 particles, we estimated that the Pb ionization efficiency relative to nitrate (RIEPb) is 0.5. Comparison of time series of AMS Pb with other measurements carried out at the T0 urban supersite during MILAGRO (using Proton Induced X-ray Emission (PIXE), Inductively-Coupled Plasma Mass Spectrometry (ICP-MS) and single-particle counts from an Aerosol Time-of-Fight Mass Spectrometer (ATOFMS)) shows similar levels (for PIXE and ICP-MS) and substantial correlation. During part of the campaign, sampling at T0 was alternated every 10 minutes with an Aerosol Concentrator, which enabled the detection of signals for PbCl+ and PbS+ ions. PbS+ displays the signature of a slowly evaporating species, while PbCl+ appears to arise only from fast evaporation, which is likely due to the higher vapor pressure of the

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

    EPA Science Inventory

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

  3. Submicron particle mass concentrations and sources in the Amazonian wet season (AMAZE-08)

    SciTech Connect

    Chen, Q.; Farmer, D. K.; Rizzo, L. V.; Pauliqueivis, T.; Kuwata, Mikinori; Karl, Thomas G.; Guenther, Alex B.; Allan, James D.; Coe, H.; Andreae, M. O.; Poeschl, U.; Jiminez, J. L.; Artaxo, Paulo; Martin, Scot T.

    2015-01-01

    Real-time mass spectra of non-refractory component of submicron aerosol particles were recorded in a tropical rainforest in the central Amazon basin during the wet season of 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic components accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. Ammonium was present in sufficient quantities to halfway neutralize sulfate. In this acidic, isoprene-dominated, low-NOx environment the high-resolution mass spectra as well as mass closures with ion chromatography measurements did not provide evidence for significant contributions of organosulfate species, at least at concentrations above uncertainty levels. Positive-matrix factorization of the time series of particle mass spectra identified four statistical factors to account for the variance of the signal intensities of the organic constituents: a factor HOA having a hydrocarbon-like signature and identified as regional emissions of primary organic material, a factor OOA-1 associated with fresh production of secondary organic material by a mechanism of BVOC oxidation followed by gas-to-particle conversion, a factor OOA-2 consistent with reactive uptake of isoprene oxidation products, especially epoxydiols by acidic particles, and a factor OOA-3 associated with long range transport and atmospheric aging. The OOA-1, -2, and -3 factors had progressively more oxidized signatures. Diameter-resolved mass spectral markers also suggested enhanced reactive uptake of isoprene oxidation products to the accumulation mode for the OOA-2 factor, and such size partitioning can be indicative of in-cloud process. The campaign-average factor loadings were in a ratio of 1.1:1.0 for the OOA-1 compared to the OOA-2 pathway, suggesting the comparable importance of gas-phase compared to particle-phase (including cloud waters) production pathways of secondary organic material during

  4. Aerosol Charge Model Consistent with Flight Data from the ECOMA/MASS Rocket Campaign

    NASA Astrophysics Data System (ADS)

    Knappmiller, S.; Robertson, S. H.; Rapp, M.; Gumbel, J.; Horanyi, M.; Sternovsky, Z.; Friedrich, M.; Baumgarten, G.; Latteck, R.

    2009-12-01

    In August of 2007 two sounding rockets were launched from the Andoya Rocket Range, Norway carrying the MASS instrument (Mesospheric Aerosol Sampling Spectrometer). The instrument detects charged aerosols in four different mass ranges on four pairs of biased collector plates, one set for positive particles and one set for negative particles. The first sounding rocket was launched into PMSE and NLC on 3 August. The solar zenith angle was 93 degrees and NLC were seen in the previous hour at 83 km by the ALOMAR RMR lidar. NLC were also detected at the same altitude by rocket-borne photometer measurements. The data from the MASS instrument shows a negatively charged population with radii >3 nm in the 83-89 km altitude range, which is collocated with PMSE detected by the ALWIN radar. Smaller particles, 1-2 nm in radius with both positive and negative polarity were detected between 86-88 km. Positively charged particles <1 nm in radius were detected at the same altitude. A charging model is developed to investigate the coexistence of positively and negatively charged aerosols in the NLC environment. Natanson’s rate equations are used for the attachment of free electrons and ions and the model includes charging by photo-electron emission and photo-detachment. Although the MASS flight occurred during night time conditions, the solar flux was still significant to affect the charge state of the aerosols. The calculations are done assuming three types of particles with different photo-electron charging properties: 1) Icy NLC particles, 2) Hematite particles of meteoric origin as condensation nuclei, and 3) Hematite particles coated with ice. The charge model results are consistent with the MASS rocket data, displaying both positively and negatively charged aerosols for small radii and only negatively charged particles for large radii.

  5. Hourly elemental concentrations in PM2.5 aerosols sampled simultaneously at urban background and road site during SAPUSS - diurnal variations and PMF receptor modelling

    NASA Astrophysics Data System (ADS)

    Dall'Osto, M.; Querol, X.; Amato, F.; Karanasiou, A.; Lucarelli, F.; Nava, S.; Calzolai, G.; Chiari, M.

    2013-04-01

    Hourly-resolved aerosol chemical speciation data can be a highly powerful tool to determine the source origin of atmospheric pollutants in urban environments. Aerosol mass concentrations of seventeen elements (Na, Mg, Al, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Sr and Pb) were obtained by time (1 h) and size (PM2.5 particulate matter < 2.5 μm) resolved aerosol samples analysed by Particle Induced X-ray Emission (PIXE) measurements. In the Marie Curie European Union framework of SAPUSS (Solving Aerosol Problems by Using Synergistic Strategies), the approach used is the simultaneous sampling at two monitoring sites in Barcelona (Spain) during September-October 2010: an urban background site (UB) and a street canyon traffic road site (RS). Elements related to primary non-exhaust traffic emission (Fe, Cu), dust resuspension (Ca) and anthropogenic Cl were found enhanced at the RS, whereas industrial related trace metals (Zn, Pb, Mn) were found at higher concentrations at the more ventilated UB site. When receptor modelling was performed with positive matrix factorization (PMF), nine different aerosol sources were identified at both sites: three types of regional aerosols (regional sulphate (S) - 27%, biomass burning (K) - 5%, sea salt (Na-Mg) - 17%), three types of dust aerosols (soil dust (Al-Ti) - 17%, urban crustal dust (Ca) - 6%, and primary traffic non-exhaust brake dust (Fe-Cu) - 7%), and three types of industrial aerosol plumes-like events (shipping oil combustion (V-Ni) - 17%, industrial smelters (Zn-Mn) - 3%, and industrial combustion (Pb-Cl) - 5%, percentages presented are average source contributions to the total elemental mass measured). The validity of the PMF solution of the PIXE data is supported by very good correlations with external single particle mass spectrometry measurements. Some important conclusions can be drawn about the PM2.5 mass fraction simultaneously measured at the UB and RS sites: (1) the regional aerosol sources impact both

  6. MODELING THE EFFECT OF CHLORINE EMISSIONS ON ATMOSPHERIC OZONE AND SECONDARY ORGANIC AEROSOL CONCENTRATIONS ACROSS THE UNITED STATES

    EPA Science Inventory

    This paper presents the modeled effects of natural and anthropogenic chlorine emissions on the atmospheric concentrations of ozone and secondary organic aerosol across the United States. The model calculations include anthropogenic molecular chlorine emissions, anthropogenic hypo...

  7. Future Projections of Aerosol Optical Depth, Radiative Forcing, and Climate Response Due to Declining Aerosol Emissions in the Representative Concentration Pathways

    NASA Astrophysics Data System (ADS)

    Westervelt, D. M.; Mauzerall, D. L.; Horowitz, L. W.; Naik, V.

    2014-12-01

    It is widely expected that global emissions of atmospheric aerosols and their precursors will decrease strongly throughout the remainder of the 21st century, due to emission reduction policies enacted based on human health concerns. However, the resulting decrease in atmospheric aerosol burden will have unintended climate consequences. Since aerosols generally exert a net cooling influence on the climate, their removal will lead to an unmasking of global warming as well as other changes to the climate system. Aerosol and precursor global emissions decrease by as much as 80% by the year 2100, according to projections in four Representative Concentration Pathway (RCP) scenarios. We use the Geophysical Fluid Dynamics Laboratory Climate Model version 3 (GFDL CM3) to simulate future climate over the 21st century with and without aerosol emission changes projected by the RCPs in order to isolate the radiative forcing and climate response due to the aerosol reductions. We find that up to 1 W m-2 of radiative forcing may be unmasked globally by 2100 due to reductions in aerosol and precursor emissions, leading to average global temperature increases up to 1 K and global precipitation rate increases up to 0.09 mm d-1 (3%). Regionally and locally, climate impacts are much larger, as RCP8.5 projects a 2.1 K warming over China, Japan, and Korea due to reduced aerosol emissions. Our results highlight the importance of crafting emissions control policies with both climate and air pollution benefits in mind. The expected unmasking of additional global warming from aerosol reductions highlights the importance of robust greenhouse gas mitigation policies and may require more aggressive policies than anticipated.

  8. Outdoor and indoor aerosol size, number, mass and compositional dynamics at an urban background site during warm season

    NASA Astrophysics Data System (ADS)

    Talbot, N.; Kubelova, L.; Makes, O.; Cusack, M.; Ondracek, J.; Vodička, P.; Schwarz, J.; Zdimal, V.

    2016-04-01

    This paper describes the use of a unique valve switching system that allowed for high temporal resolution indoor and outdoor data to be collected concurrently from online C-ToF-AMS, SMPS and OC/EC, and offline BLPI measurements. The results reveal near real-time dynamic aerosol behaviour along a migration path from an outdoor to indoor environment. An outdoor reduction in NR-PM1 mass concentration occurred daily from AM (06:00-12:00) to PM (12:00-18:00). SO4 (26%-37%) [AM/PM] increased proportionally during afternoons at the expense of NO3 (18%-7%). The influences of mixing height, temperature and solar radiation were considered against the mean mass concentration loss for each species. Losses were then calculated according to species via a basic input/output model. NO3 lost the most mass during afternoon periods, which we attribute to the accelerated dissociation of NH4NO3 through increasing temperature and decreasing relative humidity. Indoor/outdoor (I/O) ratios varied from 0.46 for <40 nm to 0.65 for >100 nm. These ratios were calculated using average SMPS PNC measurements over the full campaign and corroborated using a novel technique of calculating I/O penetration ratios through the indoor migration of particles during a new particle formation event. This ratio was then used to observe changes in indoor composition relative to those outdoors. Indoor sampling was carried out in an undisturbed room with no known sources. Indoor concentrations were found to be proportional to those outdoors, with organic matter [2.7 μg/m3] and SO4 [1.7 μg/m3] being the most prominent species. These results are indicative of fairly rapid aerosol penetration, a source-free indoor environment and small afternoon I/O temperature gradients. Fine fraction NO3 was observed indoors in both real-time AMS PM1 and off-line BLPI measurements. Greater mass concentration losses were observed from filter measurements, highlighting an important time dependency factor when investigating semi

  9. Vibration analysis of rotor blades with an attached concentrated mass

    NASA Technical Reports Server (NTRS)

    Murthy, V. R.; Barna, P. S.

    1977-01-01

    The effect of an attached concentrated mass on the dynamics of helicopter rotor blades is determined. The point transmission matrix method was used to define, through three completely automated computer programs, the natural vibrational characteristics (natural frequencies and mode shapes) of rotor blades. The problems of coupled flapwise bending, chordwise bending, and torsional vibration of a twisted nonuniform blade and its special subcase pure torsional vibration are discussed. The orthogonality relations that exist between the natural modes of rotor blades with an attached concentrated mass are derived. The effect of pitch, rotation, and point mass parameters on the collective, cyclic, scissor, and pure torsional modes of a seesaw rotor blade is determined.

  10. 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.

  11. Using MAIAC Aerosol Products to Estimate PM10 Concentrations in the Southeastern U.S

    NASA Astrophysics Data System (ADS)

    Jinnagara Puttaswamy, S.; Hu, X.; Lyapustin, A.; Wang, Y.; Liu, Y.

    2012-12-01

    Acute and chronic exposure to particulate matter has been linked to various adverse health effects. High PM levels including inhalable particles (PM10) and fine particles (PM2.5) are commonly found in large urban centers in the developing world. Unlike PM2.5 whose routine ground monitoring is very sparse, PM10 is regularly measured in many large cities in developing countries. In this analysis, we evaluate the potential for satellite aerosol remote sensing product to estimate PM10 levels. We chose AOD values in 2003 retrieved by the Multiangle Implementation of Atmospheric Correction (MAIAC) algorithm based on MODIS measurements, which has a high spatial resolution of 1 km. Our study area is a 600 km x 600 km region centered in Atlanta, GA. Linear mixed effect (LME) models were developed with MAIAC AOD as the primary predictor variable, meteorology, PM10 emission locations and land use variables as secondary predictor variables. Daily PM10 concentrations measured at ~70 EPA air quality monitoring stations were used as the dependent variable. Model day of year was used as the grouping factor for the random effect of MAIAC AOD. We aggregated AOD and other covariates on 1 km, 3km, 5km and 10km resolution grids and similar LME models were developed for each spatial resolution to compare their abilities to capture the spatial patterns of PM10 mass concentrations at various scales. Our models show that MAIAC AOD, temperature, wind speed and PM 10 emissions source locations are statistically significant predictors of PM 10 at all the spatial scales. Model fitting R2 ranges from 0.35 in winter to 0.56 in the summer. Model performances show a slight decline as the grid resolution decreases. Although the performances of PM10 exposure models are not as good as those of PM2.5 models reported in the literature, these models can still provide spatially resolved PM10 levels at urban scale, which would enable preliminary PM10-related public health research in developing countries.

  12. Is It Possible to Distinguish Between Dust and Salt Aerosol Over Waters with Unknown Chlorophyll Concentrations Using Spectral Remote Sensing?

    NASA Technical Reports Server (NTRS)

    Levy, R. C.; Kaufman, Y. J.

    1999-01-01

    Atmospheric aerosol has uncertain impacts on the global climate system, as well as on atmospheric and bio-geo-chemical processes of regional and local scales. EOS-MODIS is one example of a satellite sensor designed to improve understanding of the aerosols' type, size and distribution at all temporal and spatial scales. Ocean scientists also plan to use data from EOS-MODIS to assess the temporal and spatial coverage of in-water chlorophyll. MODIS is the first sensor planned to observe the combined ocean-atmosphere system with a wide spectral range (from 410 to 2200 nm). Dust aerosol and salt aerosol have similar spectral signals for wavelengths longer than 550 nm, but because dust selectively absorbs blue light, they have divergent signals in the blue wavelength regions (412 to 490 nm). Chlorophyll also selectively absorbs blue radiation, so that varying chlorophyll concentrations produces a highly varying signal in the blue regions, but less variability in the green, and almost no signal in the red to mid-infrared regions. Thus, theoretically, it may be difficult to differentiate dust and salt in the presence of unknown chlorophyll in the ocean. This study attempts to address the cases in which aerosol and chlorophyll signals can and cannot be separated. For the aerosol spectra, we use the aerosol lookup table from the operational MODIS aerosol-over-ocean algorithm, and for chlorophyll spectra, we use the SeaBAM data set (created for SeaWiFS). We compare the signals using Principal Component Analysis and attempt to retrieve both chlorophyll and aerosol properties using a variant of the operational MODIS aerosol-over-ocean algorithm. Results show that for small optical depths, less than 0.5, it is not possible to differentiate between dust and salt and to determine the chlorophyll concentration at the same time. For larger aerosol optical depths, the chlorophyll signals are comparatively insignificant, and we can hope to distinguish between dust and salt.

  13. SAGE and SAM II measurements of global stratospheric aerosol optical depth and mass loading

    NASA Technical Reports Server (NTRS)

    Kent, G. S.; Mccormick, M. P.

    1984-01-01

    Several volcanic eruptions between November 1979 and April 1981 have injected material into the stratosphere. The SAGE and SAM II satellite systems have measured, with global coverage, the 1-micron extinction produced by this material, and examples of the data product are shown in the form of global maps of stratospheric optical depth and altitude-latitude plots of zonal mean extinction. These data, and that for the volcanically quiet period in early 1979, have been used to determine the changes in the total stratospheric mass loading. Estimates have also been made of the contribution to the total aerosol mass from each eruption. It has been found that between 1979 and mid-1981, the total stratospheric aerosol mass increased from a background level of approximately 570,000 metric tons to a peak of approximately 1,300,000 metric tons.

  14. On the Aerosol Particle Size Distribution Spectrum in Alaskan Air Mass Systems: Arctic Haze and Non-Haze Episodes.

    NASA Astrophysics Data System (ADS)

    Shaw, Glenn E.

    1983-05-01

    Aerosols in central Alaskan winter air mass system were classified according to size by diffusive separation and light-scattering spectrometry. Particles entering central Alaska from the Pacific Marine environment had number concentrations ranging from 300 to 2000 cm3 (geometric mean 685 cm3) and unimodal size spectra, with maximum in number concentration near 1 × 106 cm radius.Air masses entering Alaska from the Eurasian Arctic possessed a factor of two smaller aerosol number concentrations than Pacific Marine systems (e.g., 150-700 cm3; geometric mean 386 cm3) but contained a factor of two greater particle volume loading within the fine particle radius range 5 × 107 < r < 1 × 105 cm. The particles in Eurasian Arctic air masses were bimodally distributed, with maxima in the particle size spectra near r = 3 × 107 and 5 × 106 cm. Sulfur was the predominant element in all cases studied.A particle depleted region was present in the size spectra obtained for Eurasian Arctic air masses. The deficiency of particles in the 106 cm radius range is interpreted as being the result of thermal coagulation taking place between sulfur-rich nuclei (produced at a rate of 1020 to 1018 g cm3 s1 and in sizes r < 106 cm) and `large' (r 105 cm) imported primary particles. The primary particles are in the removal-resistant Greenfield Gap (r 105 cm) and seem to originate in the central Eurasian region.

  15. Photochemistry of limonene secondary organic aerosol studied with chemical ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

    Pan, Xiang

    Limonene is one of the most abundant monoterpenes in the atmosphere. Limonene easily reacts with gas-phase oxidants in air such as NO3, ozone and OH. Secondary organic aerosol (SOA) is formed when low vapor pressure products condense into particles. Chemicals in SOA particles can undergo further reactions with oxidants and with solar radiation that significantly change SOA composition over the course of several days. The goal of this work was to characterize radiation induced reaction in SOA. To perform experiments, we have designed and constructed an Atmospheric Pressure Chemical Ionization Mass Spectrometer (APCIMS) coupled to a photochemical cell containing SOA samples. In APCIMS, (H2O)nH 3O+ clusters are generated in a 63Ni source and react with gaseous organic analytes. Most organic chemicals are not fragmented by the ionization process. We have focused our attention on limonene SOA prepared in two different ways. The first type of SOA is produced by oxidation of limonene by ozone; and the second type of SOA is formed by the NO3-induced oxidation of limonene. They model the SOA formed under daytime and nighttime conditions, respectively. Ozone initiated oxidation is the most important chemical sink for limonene both indoors, where it is used for cleaning purposes, and outdoors. Terpenes are primarily oxidized by reactions with NO3 at night time. We generated limonene SOA under different ozone and limonene concentrations. The resulting SOA samples were exposed to wavelength-tunable radiation in the UV-Visible range between 270 nm and 630 nm. The results show that the photodegradation rates strongly depend on radiation wavelengths. Gas phase photodegradation products such as acetone, formaldehyde, acetaldehyde, and acetic acid were shown to have different production rates for SOA formed in different concentration conditions. Even for SOA prepared under the lowest concentrations, the SOA photodegradation was efficient. The conclusion is that exposure of SOA to

  16. Dust and Pollution Aerosol Air Mass Mapping from Satellite Multi-angle Imaging

    NASA Astrophysics Data System (ADS)

    Kahn, R. A.; Nelson, D. L.; Yau, K. S.; Martonchik, J.; Diner, D. J.; Gaitley, B. J.; Russell, P.; Livingston, J.; Redemann, J.; Quinn, P. R.; Clarke, A. R.; Howell, S.; McNaughton, C.; Reid, J.; Holben, B.; Wendisch, M.; Petzold, A.

    2006-12-01

    One objective of the NASA Earth Observing System's Multi-angle Imaging SpectroRadiometer (MISR) is to map aerosol air mass types, based on retrieved column-average particle microphysical properties. Early results demonstrated the ability to distinguish three-to-five bins over the 0.1 to 2.5 micron aerosol size range, about two-to-four groupings of single-scattering albedo, and to separate spherical from randomly oriented non- spherical particles, under good but not ideal viewing conditions. These results relied heavily on the MISR Research Aerosol Retrieval algorithm, which allows flexibility in choosing retrieval patch size and location, component aerosol properties and mixtures, and mixture acceptance criteria, compared to early versions of the MISR Standard algorithm, designed to routinely process the entire global data set. Early mid-visible column aerosol optical depth results were validated against surface-based sun photometer measurements. The corresponding particle property results appeared qualitatively promising, but formal validation requires quantitative constraints on component particle properties and mixtures in a range of natural settings, available mainly from the combination of height-resolved and total column data collected by surface and airborne instruments during field campaigns. This presentation will highlight the latest detailed, multi-platform case studies, as well as MISR regional mapping, of smoke, Saharan dust, and mixtures of pollution aerosol and desert dust collected during the INTEX, SAMUM, and UAE-2 campaigns, respectively. The broader implications of these results for global, and especially regional, aerosol climate and air quality studies will also be discussed. This work is performed at the Jet Propulsion Laboratory, California Institute of Technology, under contract with the National Aeronautics and Space Administration.

  17. Organic Mass to Organic Carbon ratio in Atmospheric Aerosols: Observations and Global Simulations

    NASA Astrophysics Data System (ADS)

    Tsigaridis, K.; Kanakidou, M.; Daskalakis, N.

    2012-12-01

    Organic compounds play an important role in atmospheric chemistry and affect Earth's climate through their impact on oxidants and aerosol formation (e.g. O3 and organic aerosols (OA)). Due to the complexity of the mixture of organics in the atmosphere, the organic-mass-to-organic-carbon ratio (OM/OC) is often used to characterize the organic component in atmospheric aerosols. This ratio varies dependant on the aerosol origin and the chemical processing in the atmosphere. Atmospheric observations have shown that as OA and its precursor gases age in the atmosphere, it leads to the formation of more oxidized (O:C atomic ratio 0.6 to 0.8), less volatile and less hydrophobic compounds (particle growth factor at 95% relative humidity of 0.16 to 0.20) that have more similar properties than fresh aerosols. While reported OM:OC ratios observed over USA range between 1.29 and 1.95, indicating significant contribution of local pollution sources to the OC in that region, high O/C ratio associated with a high OM/OC ratio of 2.2 has been also observed for the summertime East Mediterranean aged aerosol. In global models, the OM/OC ratio is either calculated for specific compounds or estimated for compound groups. In the present study, we review OM/OC observations and compare them with simulations from a variety of models that contributed to the AEROCOM exercise. We evaluate the chemical processing level of atmospheric aerosols simulated by the models. A total of 32 global chemistry transport models are considered in this study with variable complexity of the representation of OM/OC ratio in the OA. The analysis provides an integrated view of the OM/OC ratio in the global atmosphere and of the accuracy of its representation in the global models. Implications for atmospheric chemistry and climate simulations are discussed.

  18. Relating Aerosol Profile and Column Measurements to Surface Concentrations: What Have We Learned from Discover-AQ?

    NASA Astrophysics Data System (ADS)

    Hoff, R. M.

    2014-12-01

    One research goal of the Deriving Information on Surface Conditions from COlumn and VERtically Resolved Observations Relevant to Air Quality (DISCOVER-AQ) mission was to determine sufficient column profile measurements to relate column integrated quantities such as Aerosol Optical Depth to surface concentrations. I will review the relationship between AOD and PM2.5 at the surface. DISCOVER-AQ in Baltimore, the San Joaquin Valley, Houston and Denver revealed quite different conditions for determining this relationship. In each case, the surface reflectivity made determination of aerosol optical depth challenging, but upward looking columns of aerosol optical depth from sunphotometers provided confirmation of the AOD results from space. In Baltimore, AOD fields reflected PM2.5 concentrations well. In California, however, the low boundary layer heights and dominance of nitrate and organic aerosols made the AOD fields less predictive of PM2.5. In California and Colorado, hydration of the aerosol varied dramatically with aerosol type (especially smoke and dust) and revealed that without an understanding of the degree of aerosol hydration with aerosol composition, the relationship between AOD and PM2.5 will continue to be a challenge. Model predictions in the Baltimore-Washington study are relatively disappointing in helping define the needed physics between the optical and microphysical properties. An overview of the measurements from DISCOVER-AQ which will help define the needed information in a more general case in the future will be given.

  19. Performance of the chemical mass balance model with simulated local-scale aerosols

    NASA Astrophysics Data System (ADS)

    Javitz, H. S.; Watson, J. G.; Robinson, N.

    A general methodology for performing simulations of the Chemical Mass Balance (CMB) model is developed and applied to simple and complex local scale scenarios. The simple scenario consists of crustal, coal-fired power plant, motor vehicle and vegetative burning sources; the complex scenario adds oil-fired power plant, ocean, steel mill, lead smelter, municipal incinerator and background aerosol sources. Daily receptor filter concentrations of the most commonly measured elements in the primary emissions are simulated. These simulations incorporate daily fluctuations in source strengths, daily fluctuations in source profiles (as parameterized by a coefficient of variation, or CV, of temporal source profiles) and measurement error at the receptor (as parameterized by a CV of measurement error). The CMB is applied to each daily measurement using a source library containing all sources and their long-term profiles (which, though correct on average, are incorrect on any particular day). The extent of agreement of the actual and CMBestimated primary emission source strengths is measured as an average absolute error (AAE, the absolute difference between the daily actual and estimated primary emission source strengths averaged over 100 simulated days). These moderately realistic simulations provide an encouraging picture of CMB accuracy and precision. The CMB yields acceptable accuracy and precision (an AAE of 50% or less) even when the CV of temporal source profiles is 25% and the CV of measurement error is 10%.

  20. Sensitivity of aerosol concentrations and cloud properties to nucleation and secondary organic distribution in ECHAM5-HAM global circulation model

    NASA Astrophysics Data System (ADS)

    Makkonen, R.; Asmi, A.; Korhonen, H.; Kokkola, H.; Järvenoja, S.; Räisänen, P.; Lehtinen, K. E. J.; Laaksonen, A.; Kerminen, V.-M.; Järvinen, H.; Lohmann, U.; Bennartz, R.; Feichter, J.; Kulmala, M.

    2009-03-01

    The global aerosol-climate model ECHAM5-HAM was modified to improve the representation of new particle formation in the boundary layer. Activation-type nucleation mechanism was introduced to produce observed nucleation rates in the lower troposphere. A simple and computationally efficient model for biogenic secondary organic aerosol (BSOA) formation was implemented. Here we study the sensitivity of the aerosol and cloud droplet number concentrations (CDNC) to these additions. Activation-type nucleation significantly increases aerosol number concentrations in the boundary layer. Increased particle number concentrations have a significant effect also on cloud droplet number concentrations and therefore on cloud properties. We performed calculations with activation nucleation coefficient values of 2×10-7s-1, 2×10-6s-1 and 2×10-5s-1 to evaluate the sensitivity to this parameter. For BSOA we have used yields of 0.025, 0.07 and 0.15 to estimate the amount of monoterpene oxidation products available for condensation. The hybrid BSOA formation scheme induces large regional changes to size distribution of organic carbon, and therefore affects particle optical properties and cloud droplet number concentrations locally. Although activation-type nucleation improves modeled aerosol number concentrations in the boundary layer, the use of a global activation coefficient generally leads to overestimation of aerosol number. Overestimation can also arise from underestimation of primary emissions.

  1. 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...

  2. Characteristics of dimethylsulfide, ozone, aerosols, and cloud condensation nuclei in air masses over the northwestern Pacific Ocean

    NASA Astrophysics Data System (ADS)

    Nagao, Ippei; Matsumoto, Kiyoshi; Tanaka, Hiroshi

    1999-05-01

    Long-term measurements of several trace gases and aerosols were carried out from December 1994 to October 1996 at Ogasawara Hahajima Island over the northwestern Pacific Ocean. The continental impact on the concentrations of sulfur compounds, ozone (O3), and cloud condensation nuclei (CCN) was estimated on the basis of the classification of air mass into seven types by isentropic trajectory analysis. From May to October, the air mass originating from the central North Pacific Ocean is predominant and regarded as the clean marine air for the concentrations of sulfur compounds and CCN. From the results of the molar ratio of methane sulfonic acid to non-sea-salt sulfate (NSS) and the positive correlation between dimethylsulfide (DMS) and CCN in this air mass it can be concluded that DMS largely contributes to the production of NSS and CCN. On the other hand, continental and anthropogenic substances are preferably transported to the northwestern Pacific Ocean by the predominant continental air mass from November to March. The enhancement of concentrations by the outflow from the Asian continent are estimated by a factor of 2.8 for O3, 3.9 for SO2, 3.5 for CCN activated at 0.5% supersaturation (0.5% CCN), 4.7 for 1.0% CCN, and 5.5 for NSS. Moreover, the CCN supersaturation spectra are also affected by the continental substances resulting in factor 2 of enhancement of cloud droplet number concentration. The diurnal variations of DMS and O3 for each air mass show a pattern of daytime minimum and nighttime maximum, which are typically found in remote ocean, even though those amplitudes are different for each air mass. Consequently, it can be concluded that the influence of nitric oxides (NOx) for the daytime O3 production and nitrate (NO3) radical for the nighttime oxidation of DMS are small even in the continental air mass.

  3. Study of node and mass sensitivity of resonant mode based cantilevers with concentrated mass loading

    SciTech Connect

    Zhang, Kewei Chai, Yuesheng; Fu, Jiahui

    2015-12-15

    Resonant-mode based cantilevers are an important type of acoustic wave based mass-sensing devices. In this work, the governing vibration equation of a bi-layer resonant-mode based cantilever attached with concentrated mass is established by using a modal analysis method. The effects of resonance modes and mass loading conditions on nodes and mass sensitivity of the cantilever were theoretically studied. The results suggested that the node did not shift when concentrated mass was loaded on a specific position. Mass sensitivity of the cantilever was linearly proportional to the square of the point displacement at the mass loading position for all the resonance modes. For the first resonance mode, when mass loading position x{sub c} satisfied 0 < x{sub c} < ∼ 0.3l (l is the cantilever beam length and 0 represents the rigid end), mass sensitivity decreased as the mass increasing while the opposite trend was obtained when mass loading satisfied ∼0.3l ≤ x{sub c} ≤ l. Mass sensitivity did not change when concentrated mass was loaded at the rigid end. This work can provide scientific guidance to optimize the mass sensitivity of a resonant-mode based cantilever.

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

    PubMed

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

    2016-01-01

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

  5. 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

  6. Heterogeneous processing of {sup 13}NO{sub 2} at zero concentration by monodisperse carbon aerosols

    SciTech Connect

    Tabor, K.; Kalberer, M.; Parrat, Y.

    1995-12-31

    The heterogeneous chemical processing of atmospheric cases by both natural and anthropogenic aerosols plays a key role in the regional as well as global environment. The oxides of nitrogen in the presence of soot present a particularly interesting and relevant topic covering a wide range of such diverse phenomena as acid rain and stratospheric ozone depletion. Detailed investigations of such systems is difficult due to low aerosol and gas species concentrations and, to date, most studies have investigated the chemistry using bulk samples. Nitrogen dioxide is known to be the most important reactive species in this system proceeding as, NO{sub 2} + (C) {r_arrow} (NO{sub 2}{lg_bullet} C){r_arrow} NO + (O {lg_bullet} C). In our current study, we have used {sup 13}N(T{sub 1/2} = 9.96 min) radioisotope labeling techniques to investigate the uptake and chemical conversion of NO{sub 2} in the presence of monodisperse carbon aerosols under real atmospheric conditions, which represents a significant improvement over earlier studies in our lab. {sup 13}N was produced using 14 MeV protons from the PSI Philips cyclotron and a gas target of 2% O{sub 2} in He for the reaction {sup 16}O(p,{alpha}) {sup 13}N. The resulting {sup 13}NO{sub y} were reduced to {sup 13}NO over molybdenum and subsequently oxidized to {sup 13}NO{sub 2} over CrO{sub 3}. Carbon aerosol was generated by spark discharge between graphite rods in argon. Mono-disperse size cuts were selected with a differential mobility analyzer operated with synthetic air. The NO{sub 2} and aerosol streams were admixed and passed through a reaction volume for a reaction time of 10s. A series of selective traps and one filter were used to separate products and reactants: (1) triethanolamine (TEA) denuder to remove unreacted gas phase NO{sub 2}, (2) TEA impregnated class fiber filter to remove aerosol fraction and NO{sub 2} released after uptake, and (3) Co{sub x}O{sub y} trap to remove all residual NO{sub x}.

  7. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    SciTech Connect

    Kleinman L. I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek III, A. J.; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2012-01-04

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a boundary layer (BL) contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (D{sub p} > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25 % of aerosol with D{sub p} > 100 nm are interstitial (not activated). A direct comparison of pre-cloud and in-cloud aerosol yields a higher estimate. Artifacts in the measurement of interstitial aerosol due to droplet shatter and evaporation are discussed. Within each of 102 constant altitude cloud transects, CDNC and interstitial aerosol were anti-correlated. An examination of one cloud as a case study shows that the

  8. Preliminary Observations of organic gas-particle partitioning from biomass combustion smoke using an aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Lee, T.; Kreidenweis, S. M.; Collett, J. L.; Sullivan, A. P.; Carrico, C. M.; Jimenez, J. L.; Cubison, M.; Saarikoski, S.; Worsnop, D. R.; Onasch, T. B.; Fortner, E.; Malm, W. C.; Lincoln, E.; Wold, C. E.; Hao, W.

    2010-12-01

    Aerosols play important roles in adverse health effects, indirect and direct forcing of Earth’s climate, and visibility degradation. Biomass burning emissions from wild and prescribed fires can make a significant contribution to ambient aerosol mass in many locations and seasons. In order to better understand the chemical properties of particles produced by combustion of wild land fuels, an experiment was conducted in 2009 at the U.S. Forest Service/United States Department of Agriculture (USFS/USDA) Fire Science Laboratory (FSL) located in Missoula, Montana, to measure volatility of open biomass burning emissions for a variety of fuel types. Both isothermal and temperature-dependent volatilization were studied, using an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) coupled with thermal denuder. Small quantities (200-800g) of various fuel types, primarily from the U.S., were burned in a large combustion chamber and diluted in two stages in continuous-flow residence chambers. The partitioning of particulate organic mass concentrations by the HR-ToF-AMS was evaluated for each fuel type using nominal dilution ratios characterized both by measuring flow rates in continuous-flow residence chambers and from the concentrations of several conserved tracers. The volatility of biomass burning smoke was found to vary across fuel types. Up to ~60% volatile loss of organic matter was observed as a result of dilution for some smoke samples (e.g., Lodgepole pine and Ponderosa pine). We will investigate relationships between volatility and several parameters such as the absolute mass concentration and chemical composition. We will also examine the behavior of biomass burning tracers, such as AMS m/z 60, under dilution conditions. Previous studies (e.g. Lee et al., AS&T 2010 and Aiken et al., ACP 2009) have observed a strong relationship between OA and AMS m/z 60 in fresh biomass burning smoke. We will examine whether this relationship is altered

  9. Potential Aerosol Mass (PAM) flow reactor measurements of SOA formation in a Ponderosa Pine forest in the southern Rocky Mountains during BEACHON-RoMBAS

    NASA Astrophysics Data System (ADS)

    Palm, B. B.; Ortega, A. M.; Campuzano Jost, P.; Day, D. A.; Kaser, L.; Karl, T.; Jud, W.; Hansel, A.; Fry, J.; Brown, S. S.; Zarzana, K. J.; Dube, W. P.; Wagner, N.; Draper, D.; Brune, W. H.; Jimenez, J. L.

    2012-12-01

    A Potential Aerosol Mass (PAM) photooxidation flow reactor was used in combination with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer to characterize biogenic secondary organic aerosol (SOA) formation in a terpene-dominated forest during the July-August 2011 Bio-hydro-atmosphere interactions of Energy, Aerosols, Carbon, H2O, Organics & Nitrogen - Rocky Mountain Biogenic Aerosol Study (BEACHON-RoMBAS) field campaign at the U.S. Forest Service Manitou Forest Observatory, Colorado, as well as in corresponding laboratory experiments. In the PAM reactor, a chosen oxidant (OH, O3, or NO3) was generated and controlled over a range of values up to 10,000 times ambient levels. High oxidant concentrations accelerated the gas-phase, heterogeneous, and possibly aqueous oxidative aging of volatile organic compounds (VOCs), inorganic gases, and existing aerosol, which led to repartitioning into the aerosol phase. PAM oxidative processing represented from a few hours up to ~20 days of equivalent atmospheric aging during the ~3 minute reactor residence time. During BEACHON-RoMBAS, PAM photooxidation enhanced SOA at intermediate OH exposure (1-10 equivalent days) but resulted in net loss of OA at long OH exposure (10-20 equivalent days), demonstrating the competing effects of functionalization vs. fragmentation (and possibly photolysis) as aging increased. PAM oxidation also resulted in f44 vs. f43 and Van Krevelen diagram (H/C vs. O/C) slopes similar to ambient oxidation, suggesting the PAM reactor employs oxidation pathways similar to ambient air. Single precursor aerosol yields were measured using the PAM reactor in the laboratory as a function of organic aerosol concentration and reacted hydrocarbon amounts. When applying the laboratory PAM yields with complete consumption of the most abundant VOCs measured at the forest site (monoterpenes, sesquiterpenes, MBO, and toluene), a simple model underpredicted the amount of SOA formed in the PAM reactor in the

  10. Variability of aerosol particle number concentrations observed over the western Pacific in the spring of 2009

    NASA Astrophysics Data System (ADS)

    Takegawa, N.; Moteki, N.; Oshima, N.; Koike, M.; Kita, K.; Shimizu, A.; Sugimoto, N.; Kondo, Y.

    2014-12-01

    Airborne measurements of aerosols were conducted over the western Pacific in the spring of 2009 during the Aerosol Radiative Forcing in East Asia (A-FORCE) aircraft campaign. The A-FORCE flights intensively covered an important vertical-latitudinal range in the outflow region of East Asia (0-9 km altitude; 27°N-38°N). This paper presents the variability of aerosol particle number concentrations obtained by condensation particle counters and a Single-Particle Soot Photometer (SP2), with the focus on those in the free troposphere. The number concentration data include total condensation nuclei with particle diameters (dp) larger than 10 nm (total CN10), PM0.17-CN10 (dp ~10-130 nm), and SP2 black carbon (NBC; dp ~75-850 nm). Large increases in total CN10 that were not associated with NBC were observed in the free troposphere, suggesting influences from new particle formation (NPF). Statistical characteristics of total CN10, PM0.17-CN10, and NBC in the lower troposphere (LT; 0-3 km), middle troposphere (MT; 3-6 km), and upper troposphere (UT; 6-9 km) are investigated. The correlation between total CN10 and NBC, along with the ratio of PM0.17 to total CN10 and carbon monoxide mixing ratio (CO), is used to interpret the observed variability. The median concentrations of total CN10 and PM0.17-CN10 in the UT were higher than those in the MT by a factor of ~1.4 and ~1.6, respectively. We attribute the enhancements of CN10 in the UT to NPF. Possible mechanisms affecting NPF in the free troposphere are discussed.

  11. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

    2012-02-01

    Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25-0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate

  12. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    NASA Astrophysics Data System (ADS)

    Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

    2011-10-01

    Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm) mass. Secondary organic aerosol (SOA) is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra in the m/z range 12-250 showing Pearson's r values >0.94 for the correlations between the different SOA types after 5 h of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxidized OA (SV-OOA) observed in the ambient aerosol. The atomic O : C ratios were found to be in the range of 0.25-0.55 with no major increase during the first 5 h of aging. On average, the diesel SOA showed the lowest O : C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions based on their carbon number revealed that the SOA source with the highest O : C ratio had the largest fraction of small ions. Fragment ions containing up to 3 carbon atoms accounted for 66%, 68%, 72% and 76% of the organic spectrum of the SOA produced by the diesel car, wood burner, α-pinene and

  13. Investigation of the seasonal variations of aerosol physicochemical properties and their impact on cloud condensation nuclei number concentration

    NASA Astrophysics Data System (ADS)

    Logan, Timothy S.

    Aerosols are among the most complex yet widely studied components of the atmosphere not only due to the seasonal variability of their physical and chemical properties but also their effects on climate change. The three main aerosol types that are known to affect the physics and chemistry of the atmosphere are: mineral dust, anthropogenic pollution, and biomass burning aerosols. In order to understand how these aerosols affect the atmosphere, this dissertation addresses the following three scientific questions through a combination of surface and satellite observations: SQ1: What are the seasonal and regional variations of aerosol physico-chemical properties at four selected Asian sites? SQ2: How do these aerosol properties change during transpacific and intra-continental long range transport? SQ3: What are the impacts of aerosol properties on marine boundary layer cloud condensation nuclei number concentration? This dissertation uses an innovative approach to classify aerosol properties by region and season to address SQ1. This is useful because this method provides an additional dimension when investigating the physico-chemical properties of aerosols by linking a regional and seasonal dependence to both the aerosol direct and indirect effects. This method involves isolating the aerosol physico-chemical properties into four separate regions using AERONET retrieved Angstrom exponent (AEAOD) and single scattering co-albedo (o oabs) to denote aerosol size and absorptive properties. The aerosols events are then clustered by season. The method is first applied to four AERONET sites representing single mode aerosol dominant regions: weakly absorbing pollution (NASA Goddard), strongly absorbing pollution (Mexico City), mineral dust (Solar Village), and biomass burning smoke (Alta Floresta). The method is then applied to four Asian sites that represent complicated aerosol components. There are strong regional and seasonal influences of the four aerosol types over the

  14. Characterization of ambient aerosols during the Southern Oxidant and Aerosol Study (SOAS) in Centreville, AL with a high-resolution time-of-flight aerosol mass spectrometer Basak Karakurt Cevik1, Yu Jun Leong1, Carlos Hernandez1, Robert Griffin1 1 Rice University, CEE Department, 6100 Main St., Houston, TX 77005, USA

    NASA Astrophysics Data System (ADS)

    Karakurt Cevik, B.; Leong, Y.; Hernandez, C.; Griffin, R. J.

    2013-12-01

    An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a Brechtel Manufacturing, Inc. particle-into-liquid sampler (PILS) were deployed at a rural location in Centreville, AL, from 1 June to 15 July 2013 as a part of the Southern Oxidant and Aerosol Study (SOAS). PILS samples were analyzed with Dionex ion chromatographs. The data will allow us to characterize the temporal characteristics of the concentrations and size distributions of non-refractory (NR) chemical species in the ambient submicron particles. Preliminary analysis of the data indicates that the sub-micron particulate matter is highly dominated by organic matter with a relatively high state of oxidation and it is followed by smaller contributions from sulfate and ammonium. In order to investigate the processes and sources that lead to observed aerosol concentrations at the site, the time series will be analyzed in conjunction with additional trace gas, aerosol, and meteorological measurements. The region is known to have high biogenic volatile organic compounds (VOCs) emissions and many of these biogenic VOCs (BVOCs) are important secondary organic aerosol (SOA) precursors. Preliminary data from the HR-ToF-AMS indicates the importance of oxidized organic aerosol during SOAS. The study will also focus on the importance of the SOA in the total organic fraction and the effect of atmospheric processing on the chemical composition of the organic fraction.

  15. Toward new techniques to measure heterogeneous oxidation of aerosol: Electrodynamic Balance-Mass Spectrometry (EDB-MS) and Aerosol X-ray Photoelectron Spectroscopy

    NASA Astrophysics Data System (ADS)

    Jacobs, M. I.; Heine, N.; Xu, B.; Davies, J. F.; Kirk, B. B.; Kostko, O.; Alayoglu, S.; Wilson, K. R.; Ahmed, M.

    2015-12-01

    The chemical composition and physical properties of aerosol can be changed via heterogeneous oxidation with the OH radical. However, the physical state of the aerosol influences the kinetics of this reaction; liquid particles with a high diffusion coefficient are expected to be well mixed and homogenously oxidized, while oxidation of solid, diffusion-limited aerosol is expected to occur primarily on the surface, creating steep chemical gradients within the particle. We are working to develop several new techniques to study the heterogeneous oxidation of different types of aerosol. We are developing a "modular" electrodynamic balance (EDB) that will enable us to study heterogeneous oxidation at aqueous interfaces using a mass-spectrometer (and potentially other detection techniques). Using a direct analysis in real time (DART) interface, preliminary droplet train measurements have demonstrated single-droplet mass spectrometry to be possible. With long reaction times in our EDB, we will be able to study heterogeneous oxidation of a wide variety of organic species in aqueous droplets. Additionally, we are working to use aerosol photoemission and velocity map imaging (VMI) to study the surface of aerosol particles as they undergo heterogeneous oxidation. With VMI, we're able to collect electrons with a 4π collection efficiency over conventional electron energy analyzers. Preliminary results looking at the ozonolysis of squalene using ultraviolet photoelectron spectroscopy (UPS) show that heterogeneous oxidation kinetic data can be extracted from photoelectron spectra. By moving to X-ray photoemission spectroscopy (XPS), we will determine elemental and chemical composition of the aerosol surface. Thus, aerosol XPS will provide information on the steep chemical gradients that form as diffusion-limited aerosol undergo heterogeneous oxidation.

  16. Influence of methane concentration on the optical indices of Titan’s aerosols analogues

    NASA Astrophysics Data System (ADS)

    Mahjoub, A.; Carrasco, N.; Dahoo, P.-R.; Gautier, T.; Szopa, C.; Cernogora, G.

    2012-11-01

    This work deals with the optical constant characterization of Titan aerosol analogues or “tholins” produced with the PAMPRE experimental setup and deposited as thin films onto a silicon substrate. Tholins were produced in different N2-CH4 gaseous mixtures to study the effect of the initial methane concentration on their optical constants. The real (n) and imaginary (k) parts of the complex refractive index were determined using the spectroscopic ellipsometry technique in the 370-1000 nm wavelength range. We found that optical constants depend strongly on the methane concentrations of the gas phase in which tholins are produced: imaginary optical index (k) decreases with initial CH4 concentration from 2.3 × 10-2 down to 2.7 × 10-3 at 1000 nm wavelength, while the real optical index (n) increases from 1.48 up to 1.58 at 1000 nm wavelength. The larger absorption in the visible range of tholins produced at lower methane percentage is explained by an increase of the secondary and primary amines signature in the mid-IR absorption. Comparison with results of other tholins and data from Titan observations are presented. We found an agreement between our values obtained with 10% methane concentration, and Imanaka et al. (Imanaka, H., Khare, B.N., Elsila, J.E., Bakes, E.L.O., McKay, C.P., Cruikshank, D.P., Sugita, S., Matsui, T., Zare, R.N. [2004]. Icarus, 168, 344-366) values, in spite of the difference in the analytical method. This confirms a reliability of the optical properties of tholins prepared with various setups but with similar plasma conditions. Our comparison with Titan’s observations also raises a possible inconsistency between the mid-IR aerosol signature by VIMS and CIRS Cassini instruments and the visible Huygens-DISR derived data. The mid-IR VIMS and CIRS signatures are in agreement with an aerosol dominated by an aliphatic carbon content, whereas the important visible absorption derived from the DISR measurement seems to be incompatible with such

  17. Fine-mode organic mass concentrations and sources in the Amazonian wet season (AMAZE-08)

    NASA Astrophysics Data System (ADS)

    Chen, Q.; Farmer, D. K.; Rizzo, L. V.; Pauliquevis, T.; Kuwata, M.; Karl, T. G.; Guenther, A.; Allan, J. D.; Coe, H.; Andreae, M. O.; Pöschl, U.; Jimenez, J. L.; Artaxo, P.; Martin, S. T.

    2014-06-01

    Real-time mass spectra of non-refractory species in submicron aerosol particles were recorded in a tropical rainforest in the central Amazon Basin during the wet season from February to March 2008, as a part of the Amazonian Aerosol Characterization Experiment (AMAZE-08). Organic material accounted on average for more than 80% of the non-refractory submicron particle mass concentrations during the period of measurements. Ammonium was present in sufficient quantities to partially neutralize sulfate. In this acidic, isoprene-rich, HO2-dominant environment positive-matrix factorization (PMF) of the time series of particle mass spectra identified four statistical factors to account for the 99% variance of the signal intensities of the organic constituents: an HOA factor having a hydrocarbon-like signature and identified as regional and local pollution, an OOA-1 factor associated with long-range transport, an OOA-2 factor implicated as associated with the reactive uptake of isoprene oxidation products, especially of epoxydiols to acidic haze, fog or cloud droplets, and an OOA-3 factor consistent with the fresh production of secondary organic material (SOM) by a mechanism of gas-phase oxidation of biogenic volatile organic compounds (BVOC) followed by gas-to-particle conversion of the oxidation products. The OOA-1, -2, and -3 factors had progressively less oxidized signatures. Aqueous-phase oxidation of water-soluble products of gas-phase photochemistry might have been also involved in the formation of the OOA-2 factor. The campaign-average mass concentrations were in a ratio of 7 : 5 for the OOA-2 compared to the OOA-3 pathway, suggesting the comparable importance of particle-phase compared to gas-phase pathways for the production of SOM during the study period.

  18. High Resolution Mass Spectrometry of Seasonal Aerosol Samples From an Urban Location in the Italian Po Valley

    NASA Astrophysics Data System (ADS)

    Mahon, Brendan; Giorio, Chiara; Gallimore, Peter J.; Zielinski, Arthur T.; Tapparo, Andrea; Kalberer, Markus

    2016-04-01

    The Po Valley in Northern Italy represents one of the most polluted environments in Europe, with PM2.5 and ozone concentrations regularly exceeding 100μg/m3 and 50ppb respectively. Particularly during winter, prolonged inversion conditions together with biomass burning and anthropogenic emissions regularly lead to severe air pollution events. Over the course of several months in 2013-14, we carried out a sampling program at a city-centre site in Padova, Italy, collecting 24-hour high-volume aerosol filter samples, 18 in winter (mid December - mid March) and 20 in summer (late May - late July). Utilising high-resolution Orbitrap mass spectrometry techniques, we have characterised these sample sets to examine the long-term variation in aerosol composition over the sampling campaign and to determine the effect of anthropogenic gaseous pollutants such as NOx and SO2 on the composition of organic particle components. The results showed that between ca. 450-700 ions were measured in each sample in both the summer and winter sample sets, however the majority (90%) of ions in the winter samples were below 300m/z and below 380m/z in the summer samples. A much higher percentage of CHO-only ions were found in winter (ca. 27%) compared to the summer samples (ca. 6%), indicating a higher degree of photochemical reactions taking place involving pollutants such as NOx and SO2 in summer. Our results represent the first long term data set of high-resolution measurements of aerosol composition and demonstrate that this technique is an important tool in evaluating the composition of aerosol particles in complex polluted urban areas.

  19. Real-time measurement of sodium chloride in individual aerosol particles by mass spectrometry

    NASA Technical Reports Server (NTRS)

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

    1985-01-01

    The method of particle analysis by mass spectrometry has been applied to the quantitative measurement of sodium chloride in individual particles on a real-time basis. Particles of known masses are individually introduced, in the form of a beam, into a miniature Knudsen cell oven (1600 K). The oven is fabricated from rhenium metal sheet (0.018 mm thick) and is situated in the ion source of a quadrupole mass spectrometer. A particle once inside the oven is trapped and completely volatilized; this overcomes the problem of partial volatilization due to particles bouncing from the filament surface. Individual particles are thermally volatilized and ionized inside the rhenium oven, and produce discrete sodium ion pulses whose intensities are measured with the quadrupole mass spectrometer. An ion pulse width of several milliseconds (4-12 ms) is found for particles in the mass range 1.3 x 10 to the -13th to 5.4 x 10 to the -11th g. The sodium ion intensity is found to be proportional to the particle mass to the 0.86-power. The intensity distribution for monodisperse aerosol particles possesses a geometric standard deviation of 1.09, showing that the method can be used for the determination of the mass distribution function with good resolution in a polydisperse aerosol.

  20. Sudden changes in aerosol and gas concentrations in the central Arctic marine boundary layer: Causes and consequences

    NASA Astrophysics Data System (ADS)

    Bigg, E. Keith; Leck, Caroline; Nilsson, E. Douglas

    2001-12-01

    Measurements of aerosol number size distributions and concentrations of the precursor gases dimethyl sulfide, sulfur dioxide and ammonia were made within the pack ice region of the central Arctic Ocean during July and August 1996 from the icebreaker Oden. Changes in concentration, sometimes exceeding the entire seasonal variation, often occurred within an hour and attempts to find the reasons for them are described. Vertical profiles of aerosol concentration in Aitken and accumulation mode particles obtained on helicopter flights revealed intense concentration gradients in the lowest 1000 m. Those below 100 m were common. Concentrations of accumulation mode particles were usually greater near the surface than at 100 m. Four representative case studies for which vertical aerosol profiles were obtained are presented. Observations of rapid large changes in near-surface concentration of aerosols in different size ranges are compared with the vertical profiles, meteorological information, and acoustic or optical remote sensing to infer processes causing the changes. Comparison of simultaneous variations in aerosols and precursor gas concentrations are used to define the vertical profiles of the gases. It was found that dimethyl sulfide and ammonia concentrations usually must have been strongly depleted near the surface relative to concentrations at about 100 m. Sulfur dioxide profiles appeared to be more complex. Turbulence or vertical air motions initiated by atmospheric wave motions trapped within the stable boundary layer appeared to be directly responsible for many of the sudden concentration changes, through interaction with concentration gradients close to the surface. The presence of low-level jets also had direct or indirect influences on mixing in the lowest few hundred meters. The extent to which aerosols measured near the surface can determine the microphysics of central Arctic marine boundary layer clouds is examined.

  1. Size-resolved aerosol chemical concentrations at rural and urban sites in Central California, USA

    NASA Astrophysics Data System (ADS)

    Chow, Judith C.; Watson, John G.; Lowenthal, Douglas H.; Magliano, Karen L.

    2008-11-01

    Aerosol size distributions were measured with Micro Orifice Uniform Deposit Impactor (MOUDI) cascade impactors at the rural Angiola and urban Fresno Supersites in California's San Joaquin Valley during the California Regional PM 10/PM 2.5 Air Quality Study (CRPAQS) winter campaign from December 15, 2000 to February 3, 2001. PM 2.5 filter samples were collected concurrently at both sites with Sequential Filter Samplers (SFS). MOUDI nitrate (NO 3-) concentrations reached 66 μg/m 3 on January 6, 2001 during the 1000-1600 PST (GMT-8) period. Pair-wise comparisons between PM 2.5 MOUDI and SFS concentrations revealed high correlations at the Angiola site ( r > 0.93) but more variability ( r < 0.85) at the Fresno site for NO 3-, sulfate (SO 4=), and ammonium (NH 4+). Correlations were higher at Fresno ( r > 0.87) than at Angiola ( r < 0.7) for organic carbon (OC), elemental carbon (EC), and total carbon (TC). NO 3- and SO 4= size distributions in Fresno were multi-modal and wider than the uni-modal distributions observed at Angiola. Geometric mean diameters (GMD) were smaller for OC and EC than for NO 3- and SO 4= at both sites. OC and EC were more concentrated on the lowest MOUDI stage (0.056 µm) at Angiola than at Fresno. The NO 3- GMD increased from 0.97 to 1.02 µm as the NO 3- concentration at Angiola increased from 43 to 66 µg m - 3 during a PM 2.5 episode from January 4-7, 2001. There was a direct relationship between GMD and NO 3- and SO 4= concentrations at Angiola but no such relationships for OC or EC. This demonstrates that secondary aerosol formation increases both concentration and particle size for the rural California environment.

  2. Molecular Characterization of Nitrogen Containing Organic Compounds in Biomass Burning Aerosols Using High Resolution Mass Spectrometry

    SciTech Connect

    Laskin, Alexander; Smith, Jeffrey S.; Laskin, Julia

    2009-05-13

    Although nitrogen-containing organic compounds (NOC) are important components of atmospheric aerosols, little is known about their chemical compositions. Here we present detailed characterization of the NOC constituents of biomass burning aerosol (BBA) samples using high resolution electrospray ionization mass spectrometry (ESI/MS). Accurate mass measurements combined with MS/MS fragmentation experiments of selected ions were used to assign molecular structures to individual NOC species. Our results indicate that N-heterocyclic alkaloid compounds - species naturally produced by plants and living organisms - comprise a substantial fraction of NOC in BBA samples collected from test burns of five biomass fuels. High abundance of alkaloids in test burns of ponderosa pine - a widespread tree in the western U.S. areas frequently affected by large scale fires - suggests that N-heterocyclic alkaloids in BBA can play a significant role in dry and wet deposition of fixed nitrogen in this region.

  3. Investigation of the time evolved spatial distribution of urban PM2.5 concentrations and aerosol composition during episodic high PM events in Yuma, AZ

    NASA Astrophysics Data System (ADS)

    Holmes, Heather A.; Pardyjak, Eric R.; Tyler, Bonnie J.; Peterson, Richard E.

    An interdisciplinary field study designed to investigate the spatial and temporal variability of atmospheric aerosols during high particulate matter ( PM) events along the US-Mexico border near Yuma, AZ was run during the week of March 18, 2007. The experiments were designed to quantify chemical composition and physical phenomena governing the transport of aerosols generated from episodic high PM events. The field study included two micrometeorological monitoring sites; one rural and one urban, equipped with sonic anemometers, continuous particulate concentration monitors and ambient aerosol collection equipment. In addition to the two main monitoring sites, five additional locations were equipped with optical particle counters to allow for the investigation of the spatial and temporal distribution of PM2.5 in the urban environment. In this paper, the meteorological and turbulence parameters governing the distribution and concentration of PM2.5 in the urban environment for two high-wind erosion events and one burning event are compared. The interaction between local atmospheric conditions and the particulate distribution is investigated. Results indicate that a single point measurement in the urban area of Yuma may not be sufficient for determining the ambient PM concentrations that the local population experiences; all three high PM events indicated PM2.5 varied considerably with maximum urban concentrations 5-10 times greater than the measured minima. A comparison of inorganic and carbonaceous content of the aerosols for the three high PM events is presented. The comparison shows an increase in silicon during crustal dust events and an increase in elemental and organic carbon during the burn event. Additional surface chemistry analysis, using time-of-flight secondary ion mass spectrometry (ToF-SIMS), for aerosols collected at the urban and rural sites during the burn event are discussed. The surface chemistry analysis provides positive ion mass spectra of organic

  4. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    SciTech Connect

    Kleinman, L.I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek III, A. J.; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2011-06-21

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O{sub 3} and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO{sub 2} from Cu smelters and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of {approx}150 cm{sup -3}, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that {approx}25% of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50% of aerosol with D{sub p} > 110 nm were not activated, the difference between the two

  5. Aerosol concentration and size distribution measured below, in, and above cloud from the DOE G-1 during VOCALS-REx

    NASA Astrophysics Data System (ADS)

    Kleinman, L. I.; Daum, P. H.; Lee, Y.-N.; Lewis, E. R.; Sedlacek, A. J., III; Senum, G. I.; Springston, S. R.; Wang, J.; Hubbe, J.; Jayne, J.; Min, Q.; Yum, S. S.; Allen, G.

    2011-06-01

    During the VOCALS Regional Experiment, the DOE G-1 aircraft was used to sample a varying aerosol environment pertinent to properties of stratocumulus clouds over a longitude band extending 800 km west from the Chilean coast at Arica. Trace gas and aerosol measurements are presented as a function of longitude, altitude, and dew point in this study. Spatial distributions are consistent with an upper atmospheric source for O3 and South American coastal sources for marine boundary layer (MBL) CO and aerosol, most of which is acidic sulfate in agreement with the dominant pollution source being SO2 from Cu smelters and power plants. Pollutant layers in the free troposphere (FT) can be a result of emissions to the north in Peru or long range transport from the west. At a given altitude in the FT (up to 3 km), dew point varies by 40 °C with dry air descending from the upper atmospheric and moist air having a BL contribution. Ascent of BL air to a cold high altitude results in the condensation and precipitation removal of all but a few percent of BL water along with aerosol that served as CCN. Thus, aerosol volume decreases with dew point in the FT. Aerosol size spectra have a bimodal structure in the MBL and an intermediate diameter unimodal distribution in the FT. Comparing cloud droplet number concentration (CDNC) and pre-cloud aerosol (Dp > 100 nm) gives a linear relation up to a number concentration of ~150 cm-3, followed by a less than proportional increase in CDNC at higher aerosol number concentration. A number balance between below cloud aerosol and cloud droplets indicates that ~25 % of aerosol in the PCASP size range are interstitial (not activated). One hundred and two constant altitude cloud transects were identified and used to determine properties of interstitial aerosol. One transect is examined in detail as a case study. Approximately 25 to 50 % of aerosol with Dp > 110 nm were not activated, the difference between the two approaches possibly representing

  6. Effect of variable power levels on the yield of total aerosol mass and formation of aldehydes in e-cigarette aerosols.

    PubMed

    Gillman, I G; Kistler, K A; Stewart, E W; Paolantonio, A R

    2016-03-01

    The study objective was to determine the effect of variable power applied to the atomizer of refillable tank based e-cigarette (EC) devices. Five different devices were evaluated, each at four power levels. Aerosol yield results are reported for each set of 25 EC puffs, as mass/puff, and normalized for the power applied to the coil, in mass/watt. The range of aerosol produced on a per puff basis ranged from 1.5 to 28 mg, and, normalized for power applied to the coil, ranged from 0.27 to 1.1 mg/watt. Aerosol samples were also analyzed for the production of formaldehyde, acetaldehyde, and acrolein, as DNPH derivatives, at each power level. When reported on mass basis, three of the devices showed an increase in total aldehyde yield with increasing power applied to the coil, while two of the devices showed the opposite trend. The mass of formaldehyde, acetaldehyde, and acrolein produced per gram of total aerosol produced ranged from 0.01 to 7.3 mg/g, 0.006 to 5.8 mg/g, and <0.003 to 0.78 mg/g, respectively. These results were used to estimate daily exposure to formaldehyde, acetaldehyde, and acrolein from EC aerosols from specific devices, and were compared to estimated exposure from consumption of cigarettes, to occupational and workplace limits, and to previously reported results from other researchers. PMID:26743740

  7. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-03-01

    China is experiencing severe carbonaceous aerosol pollution driven mainly by large emissions resulting from intensive use of solid fuels. To gain a better understanding of the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations at the national scale, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal, spatial, and size distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols, and propose possible improvements in emission estimation for the future. The national OC emissions are estimated to have increased 29% from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37% (from 1356 to 1857 Gg). The residential, industrial, and transportation sectors contributed an estimated 76 ± 2, 19 ± 2 and 5 ± 1% of the total emissions of OC, respectively, and 52 ± 3, 32 ± 2 and 16 ± 2% of EC. Updated emission factors based on the most recent local field measurements, particularly for biofuel stoves, lead to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while larger OC/EC and SOC/OC ratios are found in southern cities, due to the joint effects of primary emissions and meteorology. Higher SOC/OC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, higher concentrations of OC, EC, and SOC are observed in colder seasons, while SOC/OC is reduced, particularly at rural and

  8. Patterns in atmospheric carbonaceous aerosols in China: emission estimates and observed concentrations

    NASA Astrophysics Data System (ADS)

    Cui, H.; Mao, P.; Zhao, Y.; Nielsen, C. P.; Zhang, J.

    2015-08-01

    China is experiencing severe carbonaceous aerosol pollution driven mainly by large emissions resulting from intensive use of solid fuels. To gain a better understanding of the levels and trends of carbonaceous aerosol emissions and the resulting ambient concentrations at the national scale, we update an emission inventory of anthropogenic organic carbon (OC) and elemental carbon (EC) and employ existing observational studies to analyze characteristics of these aerosols including temporal, spatial, and size distributions, and the levels and shares of secondary organic carbon (SOC) in total OC. We further use ground observations to test the levels and inter-annual trends of the calculated national and provincial emissions of carbonaceous aerosols, and propose possible improvements in emission estimation for the future. The national OC emissions are estimated to have increased 29 % from 2000 (2127 Gg) to 2012 (2749 Gg) and EC by 37 % (from 1356 to 1857 Gg). The residential, industrial, and transportation sectors contributed an estimated 74-78, 17-21, and 4-6 % of the total emissions of OC, respectively, and 49-55, 30-34, and 14-18 % of EC. Updated emission factors (EFs) based on the most recent local field measurements, particularly for biofuel stoves, led to considerably lower emissions of OC compared to previous inventories. Compiling observational data across the country, higher concentrations of OC and EC are found in northern and inland cities, while higher OC / EC ratios are found in southern sites, due to the joint effects of primary emissions and meteorology. Higher OC / EC ratios are estimated at rural and remote sites compared to urban ones, attributed to more emissions of OC from biofuel use, more biogenic emissions of volatile organic compound (VOC) precursors to SOC, and/or transport of aged aerosols. For most sites, higher concentrations of OC, EC, and SOC are observed in colder seasons, while SOC / OC is reduced, particularly at rural and remote sites

  9. Black Carbon Mass Concentration in California Mountain Snow

    NASA Astrophysics Data System (ADS)

    Hadley, O. L.; Corrigan, C.; Kirchstetter, T. W.; Cliff, S. S.; Ramanathan, V.

    2007-12-01

    Recent modeling studies have shown that deposition of black carbon (BC) to snow and ice lowers the albedo of snow and exerts a positive forcing on the climate. This effect is also a likely contributor to the observed ice and snow retreat in glaciers, ice sheets, and mountain snow pack. Observational data of actual BC concentrations in snow, which would help to constrain and validate these results, are scarce. This study presents the concentration of BC in fresh snow measured at two mountain locations in Northern California (Lassen Volcano Natl. Park and Donner Summit), as well as that in coastal rainfall at Trinidad Head, CA. These measurements are the first of this kind made in California. Average BC concentration at Lassen Natl. Park and Donner summit were respectively 6.8 and 9.7 ng per gram of snow. When placed in context with the modeled effect of BC on fresh snow albedo, these concentrations indicate a lowering of the snow albedo by 0.5 to 0.8%. As the snow pack ages, models predict that this effect will be increasingly amplified. Measurements of ambient aerosols during the rain events, as well as HySPLIT back-trajectories, provide additional information regarding possible sources of BC in California mountain snow packs. For the samples collected in this study, most of the soot in the snow appears to be of local origin. The average BC concentration in the coastal rain was 6.0 ng per gram of water, with the highest concentrations (12 ng/g) corresponding to the only back-trajectories clearly indicative of long-range trans-Pacific transport.

  10. 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.

  11. An online method for the analysis of volatile organic compounds in electronic cigarette aerosol based on proton transfer reaction mass spectrometry

    PubMed Central

    Breiev, Kostiantyn; Burseg, Kerstin M. M.; O'Connell, Grant; Hartungen, Eugen; Biel, Stefan S.; Cahours, Xavier; Colard, Stéphane; Märk, Tilmann D.

    2016-01-01

    Rationale Due to the recent rapid increase in electronic cigarette (e‐cigarette) use worldwide, there is a strong scientific but also practical interest in analyzing e‐cigarette aerosols. Most studies to date have used standardized but time‐consuming offline technologies. Here a proof‐of‐concept for a fast online quantification setup based on proton transfer reaction mass spectrometry (PTR‐MS) is presented. Methods The combination of a novel sampling interface with a time‐of‐flight PTR‐MS instrument specially designed for three scenarios is introduced: (i) mainstream aerosol analysis (aerosol that the user inhales prior to exhalation), and analysis of exhaled breath following (ii) mouth‐hold (no inhalation) and (iii) inhalation of e‐cigarette aerosols. A double‐stage dilution setup allows the various concentration ranges in these scenarios to be accessed. Results First, the instrument is calibrated for the three principal constituents of the e‐cigarettes' liquids, namely propylene glycol, vegetable glycerol and nicotine. With the double‐stage dilution the instrument's dynamic range was easily adapted to cover the concentration ranges obtained in the three scenarios: 20–1100 ppmv for the mainstream aerosol characterisation; 4–300 ppmv for the mouth‐hold; and 2 ppbv to 20 ppmv for the inhalation experiment. Conclusions It is demonstrated that the novel setup enables fast, high time resolution e‐cigarette studies with online quantification. This enables the analysis and understanding of any puff‐by‐puff variations in e‐cigarette aerosols. Large‐scale studies involving a high number of volunteers will benefit from considerably higher sample throughput and shorter data processing times. © 2016 The Authors. Rapid Communications in Mass Spectrometry Published by John Wiley & Sons Ltd. PMID:26864521

  12. Analysis of charged aerosols in the mesosphere during the MASS/ECOMA rocket campaign

    NASA Astrophysics Data System (ADS)

    Knappmiller, Scott Robert

    In the polar summer mesosphere ice particles grow sufficiently large to scatter sunlight, giving rise to visible cloud displays called Noctilucent Clouds (NLC). In August of 2007, two sounding rockets were launched from the Andoya Rocket Range, Norway carrying the newly developed MASS instrument (Mesospheric Aerosol Sampling Spectrometer) to study NLC. The instrument detects charged aerosols in four different mass ranges on four pairs of biased collector plates, one set for positive particles and one set for negative particles. The first sounding rocket was launched into a Polar Mesospheric Summer echo (PMSE) and into a NLC on 3 August. The solar zenith angle was 93 degrees and NLC were seen in the previous hour at 83 km by the ALOMAR RMR lidar. NLC were also detected at the same altitude by rocket-borne photometer measurements. The data from the MASS instrument shows a negatively charged population with radii >3 nm in the 83--89 km altitude range, which is collocated with PMSE detected by the ALWIN radar. Smaller particles, 1--2 nm in radius with both positive and negative polarity were detected between 86--88 km. Positively charged particles <1 nm in radius were detected at the same altitude. This is the first time the charge number densities of positive and negative NLC particles have been measured simultaneously. A charging model is developed to investigate the coexistence of positively and negatively charged aerosols in the NLC environment as measured by the MASS instrument. Natanson's rate equations are used for the attachment of free electrons and ions and the model includes charging by photo-electron emission and photo-detachment. Although the MASS flight occurred during twilight conditions, the solar UV flux was still sufficient to affect the charge state of the aerosols. The calculations are done assuming three types of particles with different photo-electron charging properties: (1) Icy NLC particles, (2) Hematite particles of meteoric origin as

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

    DOE PAGESBeta

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

    2014-12-12

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

  14. Detection of biological particles in ambient air using bio-aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    McJimpsey, Erica L.; Steele, Paul T.; Coffee, Keith R.; Fergenson, David P.; Riot, Vincent J.; Woods, Bruce W.; Gard, Eric E.; Frank, Matthias; Tobias, Herbert J.; Lebrilla, Carlito

    2006-05-01

    The Bio-Aerosol Mass Spectrometry (BAMS) system is an instrument used for the real time detection and identification of biological aerosols. Particles are drawn from the atmosphere directly into vacuum and tracked as they scatter light from several continuous wave lasers. After tracking, the fluorescence of individual particles is excited by a pulsed 266nm or 355nm laser. Molecules from those particles with appropriate fluorescence properties are subsequently desorbed and ionized using a pulsed 266nm laser. Resulting ions are analyzed in a dual polarity mass spectrometer. During two field deployments at the San Francisco International Airport, millions of ambient particles were analyzed and a small but significant fraction were found to have fluorescent properties similar to Bacillus spores and vegetative cells. Further separation of non-biological background particles from potential biological particles was accomplished using laser desorption/ionization mass spectrometry. This has been shown to enable some level of species differentiation in specific cases, but the creation and observation of higher mass ions is needed to enable a higher level of specificity across more species. A soft ionization technique, matrix-assisted laser desorption/ionization (MALDI) is being investigated for this purpose. MALDI is particularly well suited for mass analysis of biomolecules since it allows for the generation of molecular ions from large mass compounds that would fragment under normal irradiation. Some of the initial results from a modified BAMS system utilizing this technique are described.

  15. Detection of biological particles in ambient air using Bio-Aerosol Mass Spectrometry

    SciTech Connect

    McJimpsey, E L; Steele, P T; Coffee, K R; Fergenson, D P; Riot, V J; Woods, B W; Gard, E E; Frank, M; Tobias, H J; Lebrilla, C

    2006-03-16

    The Bio-Aerosol Mass Spectrometry (BAMS) system is an instrument used for the real time detection and identification of biological aerosols. Particles are drawn from the atmosphere directly into vacuum and tracked as they scatter light from several continuous wave lasers. After tracking, the fluorescence of individual particles is excited by a pulsed 266nm or 355nm laser. Molecules from those particles with appropriate fluorescence properties are subsequently desorbed and ionized using a pulsed 266nm laser. Resulting ions are analyzed in a dual polarity mass spectrometer. During two field deployments at the San Francisco International Airport, millions of ambient particles were analyzed and a small but significant fraction were found to have fluorescent properties similar to Bacillus spores and vegetative cells. Further separation of non-biological background particles from potential biological particles was accomplished using laser desorption/ionization mass spectrometry. This has been shown to enable some level of species differentiation in specific cases, but the creation and observation of higher mass ions is needed to enable a higher level of specificity across more species. A soft ionization technique, matrix-assisted laser desorption/ionization (MALDI) is being investigated for this purpose. MALDI is particularly well suited for mass analysis of biomolecules since it allows for the generation of molecular ions from large mass compounds that would fragment under normal irradiation. Some of the initial results from a modified BAMS system utilizing this technique are described.

  16. Characterization of a real-time tracer for Isoprene Epoxydiols-derived Secondary Organic Aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    NASA Astrophysics Data System (ADS)

    Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; de Sá, S. S.; Martin, S. T.; Hu, M.; Budisulistiorini, S. H.; Riva, M.; Surratt, J. D.; St. Clair, J. M.; Isaacman-Van Wertz, G.; Yee, L. D.; Goldstein, A. H.; Carbone, S.; Artaxo, P.; de Gouw, J. A.; Koss, A.; Wisthaler, A.; Mikoviny, T.; Karl, T.; Kaser, L.; Jud, W.; Hansel, A.; Docherty, K. S.; Robinson, N. H.; Coe, H.; Allan, J. D.; Canagaratna, M. R.; Paulot, F.; Jimenez, J. L.

    2015-04-01

    Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene low-NO oxidation pathways, was quantified by applying Positive Matrix Factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of OA in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the SOAS study, 78% of IEPOX-SOA is accounted for the measured molecular tracers, making it the highest level of molecular identification of an ambient SOA component to our knowledge. Enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O ( fC5H6O = C5H6O+/OA) across multiple field, chamber and source datasets. A background of ~ 1.7 ± 0.1‰ is observed in studies strongly influenced by urban, biomass-burning and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.8‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7‰). Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12-40‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3‰) observed in non IEPOX-derived isoprene-SOA indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from

  17. Characterization of a real-time tracer for Isoprene Epoxydiols-derived Secondary Organic Aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    DOE PAGESBeta

    Hu, W. W.; Campuzano-Jost, P.; Palm, B. B.; Day, D. A.; Ortega, A. M.; Hayes, P. L.; Krechmer, J. E.; Chen, Q.; Kuwata, M.; Liu, Y. J.; et al

    2015-04-16

    Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene low-NO oxidation pathways, was quantified by applying Positive Matrix Factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of OA in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the SOAS study, 78% of IEPOX-SOA is accounted for the measured molecular tracers, making itmore » the highest level of molecular identification of an ambient SOA component to our knowledge. Enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O ( fC5H6O = C5H6O+/OA) across multiple field, chamber and source datasets. A background of ~ 1.7 ± 0.1‰ is observed in studies strongly influenced by urban, biomass-burning and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.8‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7‰). Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3‰) observed in non IEPOX-derived isoprene-SOA indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA

  18. Evaluation of the tropospheric aerosol number concentrations simulated by two versions of the global model ECHAM5-HAM

    NASA Astrophysics Data System (ADS)

    Zhang, K.; Kazil, J.; Feichter, J.

    2009-04-01

    Since its first version developed by Stier et al. (2005), the global aerosol-climate model ECHAM5-HAM has gone through further development and updates. The changes in the model include (1) a new time integration scheme for the condensation of the sulfuric acid gas on existing particles, (2) a new aerosol nucleation scheme that takes into account the charged nucleation caused by cosmic rays, and (3) a parameterization scheme explicitly describing the conversion of aerosol particles to cloud nuclei. In this work, simulations performed with the old and new model versions are evaluated against some measurements reported in recent years. The focus is on the aerosol size distribution in the troposphere. Results show that modifications in the parameterizations have led to significant changes in the simulated aerosol concentrations. Vertical profiles of the total particle number concentration (diameter > 3nm) compiled by Clarke et al. (2002) suggest that, over the Pacific in the upper free troposphere, the tropics are associated with much higher concentrations than the mid-latitude regions. This feature is more reasonably reproduced by the new model version, mainly due to the improved results of the nucleation mode aerosols. In the lower levels (2-5 km above the Earth's surface), the number concentrations of the Aitken mode particles are overestimated compared to both the Pacific data given in Clarke et al. (2002) and the vertical profiles over Europe reported by Petzold et al. (2007). The physical and chemical processes that have led to these changes are identified by sensitivity tests. References: Clarke and Kapustin: A Pacific aerosol survey - part 1: a decade of data on production, transport, evolution and mixing in the troposphere, J. Atmos. Sci., 59, 363-382, 2002. Petzold et al.: Perturbation of the European free troposphere aerosol by North American forest fire plumes during the ICARTT-ITOP experiment in summer 2004, Atmos. Chem. Phys., 7, 5105-5127, 2007

  19. Determination of the chemical composition of titan4s aerosols analogues using pyrolysis gas chromatography mass spectrometry

    NASA Astrophysics Data System (ADS)

    He, J.; Buch, A.; Szopa, C.; Carrasco, N.

    2013-12-01

    The in situ chemical characterization of Titan's aerosols with the ACP-GCMS (Aerosol Collector and Pyrolyze-Gas Chromatograph and Mass Spectrometer) experiments onboard the Cassini-Huygens mission showed that the aerosols heated at 600°C were releasing two main gaseous compounds: NH3 and HCN. To better understand the process of production of these species at high temperature, and their relationship to the solid aerosol composition, it is possible to mimic in laboratory the Titan's atmosphere chemistry to produce analogues of Titan's aerosols (tholins), chemical and physical properties of which can be studied with laboratory instrumentation. In the present work, we studied the thermal decomposition of tholins produced with the PAMPRE cold plasma experiment[1]. For this study, pyrolysis at various temperatures, coupled to gas chromatography mass spectrometry (Pyr-GCMS), has been used in order to understand the origin and formation mechanism of the NH3 and HCN compounds. With this aim, two samples were produced using different initial CH4/N2 gaseous mixtures with different concentration ratios: (5:95) and (10:90). Pyr-GCMS was applied to characterize their chemical composition and molecule structure. In order to study the evolution of chemical compounds released as a function of temperature, the final pyrolysis temperature has been set from 100°C to 900°C with a 100°C step increment. The results show that the major compounds released are similar for the two different studied samples. They include hydrocarbon compounds, nitriles, ammonia, hydrogen cyanide, and some pyrrole isomers. Moreover, whatever the final temperature is, acetonitrile is the most abundant compound released by the samples. At 100°C only water contribution can be detected. Then the number of compounds released increases with the temperature up to 600°C. With the temperature increase the nature of the gaseous species detected does not change significantly. Pyrrole was not detected until the

  20. CHEMICAL ANALYSIS METHODS FOR ATMOSPHERIC AEROSOL COMPONENTS

    EPA Science Inventory

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

  1. Control of aerosol contaminants in indoor air: combining the particle concentration reduction with microbial inactivation.

    PubMed

    Grinshpun, Sergey A; Adhikari, Atin; Honda, Takeshi; Kim, Ki Youn; Toivola, Mika; Rao, K S Ramchander; Reponen, Tiina

    2007-01-15

    An indoor air purification technique, which combines unipolar ion emission and photocatalytic oxidation (promoted by a specially designed RCI cell), was investigated in two test chambers, 2.75 m3 and 24.3 m3, using nonbiological and biological challenge aerosols. The reduction in particle concentration was measured size selectively in real-time, and the Air Cleaning Factor and the Clean Air Delivery Rate (CADR) were determined. While testing with virions and bacteria, bioaerosol samples were collected and analyzed, and the microorganism survival rate was determined as a function of exposure time. We observed that the aerosol concentration decreased approximately 10 to approximately 100 times more rapidly when the purifier operated as compared to the natural decay. The data suggest that the tested portable unit operating in approximately 25 m3 non-ventilated room is capable to provide CADR-values more than twice as great than the conventional closed-loop HVAC system with a rating 8 filter. The particle removal occurred due to unipolar ion emission, while the inactivation of viable airborne microorganisms was associated with photocatalytic oxidation. Approximately 90% of initially viable MS2 viruses were inactivated resulting from 10 to 60 min exposure to the photocatalytic oxidation. Approximately 75% of viable B. subtilis spores were inactivated in 10 min, and about 90% or greater after 30 min. The biological and chemical mechanisms that led to the inactivation of stress-resistant airborne viruses and bacterial spores were reviewed. PMID:17310729

  2. 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.

  3. Fluorescent biological aerosol particle concentrations and size distributions measured with an ultraviolet aerodynamic particle sizer (UV-APS) in Central Europe

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Treutlein, B.; Pöschl, U.

    2009-08-01

    Primary biological aerosol particles (PBAPs), including bacteria, spores and pollen, are essential for the spread of organisms and disease in the biosphere, and numerous studies have suggested that they may be important for atmospheric processes, including the formation of clouds and precipitation. The atmospheric abundance and size distribution of PBAPs, however, are largely unknown. At a semi-urban site in Mainz, Germany, we used an ultraviolet aerodynamic particle sizer (UV-APS) to measure fluorescent biological aerosol particles (FBAPs), which can be regarded as viable bioaerosol particles representing a lower limit for the actual abundance of PBAPs. Fluorescence of non-biological aerosol components are likely to influence the measurement results obtained for fine particles (<1 μm), but not for coarse particles (1-20 μm). Averaged over the four-month measurement period (August-December 2006), the mean number concentration of coarse FBAPs was ~3×10-2 cm-3, corresponding to ~4% of total coarse particle number. The mean mass concentration of FBAPs was ~1 μg m-3, corresponding to ~20% of total coarse particle mass. The FBAP number size distributions exhibited alternating patterns with peaks at various diameters. A pronounced peak at ~3 μm was essentially always observed and can be described by the following campaign-average lognormal fit parameters: geometric mean diameter 3.2 μm, geometric standard deviation 1.3, number concentration 1.6×10-2 cm-3. This peak is likely due to fungal spores or agglomerated bacteria, and it exhibited a pronounced diel cycle with maximum intensity during early/mid-morning. FBAP peaks around ~1.5 μm, ~5 μm, and ~13 μm were also observed, but less pronounced and less frequent. These may be explained by single bacterial cells, larger fungal spores, and pollen grains, respectively. The observed number concentrations and characteristic sizes of FBAPs are consistent with microscopic, biological and chemical analyses of PBAPs in

  4. Fluorescent Biological Aerosol Particle Concentrations and Size Distributions Measured with an Ultraviolet Aerodynamic Particle Sizer (UV-APS) in Central Europe

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Treutlein, B.; Pöschl, U.

    2009-12-01

    Primary biological aerosol particles (PBAPs), including bacteria, spores and pollen, are essential for the spread of organisms and disease in the biosphere, and numerous studies have suggested that they may be important for atmospheric processes, including the formation of clouds and precipitation. The atmospheric abundance and size distribution of PBAPs, however, are largely unknown. At a semi-urban site in Mainz, Germany, we used an ultraviolet aerodynamic particle sizer (UV-APS) to measure fluorescent biological aerosol particles (FBAPs), which can be regarded as viable bioaerosol particles representing a lower limit for the actual abundance of PBAPs. Fluorescence of non-biological aerosol components are likely to influence the measurement results obtained for fine particles (< 1 µm), but not for coarse particles (1 - 20 µm). Averaged over the four-month measurement period (August - December 2006), the mean number concentration of coarse FBAPs was ~3x10-2 cm-3, corresponding to ~4% of total coarse particle number [1]. The mean mass concentration of FBAPs was ~1 µg m-3, corresponding to ~20% of total coarse particle mass. The FBAP number size distributions exhibited alternating patterns with peaks at various diameters. A pronounced peak at ~3 µm was essentially always observed and can be described by the following campaign-average lognormal fit parameters: geometric mean diameter 3.2 µm, geometric standard deviation 1.3, number concentration 1.6 x 10-2 cm-3. This peak is likely due to fungal spores or agglomerated bacteria, and it exhibited a pronounced diel cycle with maximum intensity during early/mid-morning. FBAP peaks around ~1.5 µm, ~5 µm, and ~13 µm were also observed, but less pronounced and less frequent. These may be explained by single bacterial cells, larger fungal spores, and pollen grains, respectively. The observed number concentrations and characteristic sizes of FBAPs are consistent with microscopic, biological and chemical analyses of

  5. Fluorescent biological aerosol particle concentrations and size distributions measured with an Ultraviolet Aerodynamic Particle Sizer (UV-APS) in Central Europe

    NASA Astrophysics Data System (ADS)

    Huffman, J. A.; Treutlein, B.; Pöschl, U.

    2010-04-01

    Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen, are essential for the spread of organisms and disease in the biosphere, and numerous studies have suggested that they may be important for atmospheric processes, including the formation of clouds and precipitation. The atmospheric abundance and size distribution of PBAPs, however, are largely unknown. At a semi-urban site in Mainz, Germany we used an Ultraviolet Aerodynamic Particle Sizer (UV-APS) to measure Fluorescent Biological Aerosol Particles (FBAPs), which provide an estimate of viable bioaerosol particles and can be regarded as an approximate lower limit for the actual abundance of PBAPs. Fluorescence of non-biological aerosol components are likely to influence the measurement results obtained for fine particles (<1 μm), but not for coarse particles (1-20 μm). Averaged over the four-month measurement period (August-December 2006), the mean number concentration of coarse FBAPs was ~3×10-2 cm-3, corresponding to ~4% of total coarse particle number. The mean mass concentration of FBAPs was ~1μg m-3, corresponding to ~20% of total coarse particle mass. The FBAP number size distributions exhibited alternating patterns with peaks at various diameters. A pronounced peak at ~3 μm was essentially always observed and can be described by the following campaign-average lognormal fit parameters: geometric mean diameter 3.2 μm, geometric standard deviation 1.3, number concentration 1.6×10-2 cm-3. This peak is likely due to fungal spores or agglomerated bacteria, and it exhibited a pronounced diel cycle (24-h) with maximum intensity during early/mid-morning. FBAP peaks around ~1.5 μm, ~5 μm, and ~13 μm were also observed, but less pronounced and less frequent. These may be single bacterial cells, larger fungal spores, and pollen grains, respectively. The observed number concentrations and characteristic sizes of FBAPs are consistent with microscopic, biological and chemical

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

    NASA Astrophysics Data System (ADS)

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

    2014-09-01

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

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

    PubMed

    Mihara, Toshiyuki; Mochida, Michihiro

    2011-11-01

    To characterize atmospheric particulate organics with respect to polarity, aerosol samples collected on filters in the urban area of Nagoya, Japan, in 2009 were extracted using water, methanol, and ethyl acetate. The extracts were atomized and analyzed using a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) and a hygroscopicity tandem differential mobility analyzer. The atmospheric concentrations of the extracted organics were determined using phthalic acid as a reference material. Comparison of the organic carbon concentrations measured using a carbon analyzer and the HR-ToF-AMS suggests that organics extracted with water (WSOM) and ethyl acetate (EASOM) or those extracted with methanol (MSOM) comprise the greater part of total organics. The oxygen-carbon ratios (O/C) of the extracted organics varied: 0.51-0.75 (WSOM), 0.37-0.48 (MSOM), and 0.27-0.33 (EASOM). In the ion-group analysis, WSOM, MSOM, and EASOM were clearly characterized by the different fractions of the CH and CO(2) groups. On the basis of the hygroscopic growth measurements of the extracts, κ of organics at 90% relative humidity (κ(org)) were estimated. Positive correlation of κ(org) with O/C (r 0.70) was found for MSOM and EASOM, but no clear correlation was found for WSOM. PMID:21877700

  8. Parametric uncertainties in global model simulations of black carbon column mass concentration

    NASA Astrophysics Data System (ADS)

    Pearce, Hana; Lee, Lindsay; Reddington, Carly; Carslaw, Ken; Mann, Graham

    2016-04-01

    Previous studies have deduced that the annual mean direct radiative forcing from black carbon (BC) aerosol may regionally be up to 5 W m‑2 larger than expected due to underestimation of global atmospheric BC absorption in models. We have identified the magnitude and important sources of parametric uncertainty in simulations of BC column mass concentration from a global aerosol microphysics model (GLOMAP-Mode). A variance-based uncertainty analysis of 28 parameters has been performed, based on statistical emulators trained on model output from GLOMAP-Mode. This is the largest number of uncertain model parameters to be considered in a BC uncertainty analysis to date and covers primary aerosol emissions, microphysical processes and structural parameters related to the aerosol size distribution. We will present several recommendations for further research to improve the fidelity of simulated BC. In brief, we find that the standard deviation around the simulated mean annual BC column mass concentration varies globally between 2.5 x 10‑9 g cm‑2 in remote marine regions and 1.25 x 10‑6 g cm‑2 near emission sources due to parameter uncertainty Between 60 and 90% of the variance over source regions is due to uncertainty associated with primary BC emission fluxes, including biomass burning, fossil fuel and biofuel emissions. While the contributions to BC column uncertainty from microphysical processes, for example those related to dry and wet deposition, are increased over remote regions, we find that emissions still make an important contribution in these areas. It is likely, however, that the importance of structural model error, i.e. differences between models, is greater than parametric uncertainty. We have extended our analysis to emulate vertical BC profiles at several locations in the mid-Pacific Ocean and identify the parameters contributing to uncertainty in the vertical distribution of black carbon at these locations. We will present preliminary

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

    SciTech Connect

    Timothy B. Onasch

    2011-10-20

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

  10. Worldwide impact of aerosol's time scale on the predicted long-term concentrating solar power potential.

    PubMed

    Ruiz-Arias, Jose A; Gueymard, Christian A; Santos-Alamillos, Francisco J; Pozo-Vázquez, David

    2016-01-01

    Concentrating solar technologies, which are fuelled by the direct normal component of solar irradiance (DNI), are among the most promising solar technologies. Currently, the state-of the-art methods for DNI evaluation use datasets of aerosol optical depth (AOD) with only coarse (typically monthly) temporal resolution. Using daily AOD data from both site-specific observations at ground stations as well as gridded model estimates, a methodology is developed to evaluate how the calculated long-term DNI resource is affected by using AOD data averaged over periods from 1 to 30 days. It is demonstrated here that the use of monthly representations of AOD leads to systematic underestimations of the predicted long-term DNI up to 10% in some areas with high solar resource, which may result in detrimental consequences for the bankability of concentrating solar power projects. Recommendations for the use of either daily or monthly AOD data are provided on a geographical basis. PMID:27507711

  11. 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

  12. Chemical Nature Of Titan’s Organic Aerosols Constrained from Spectroscopic and Mass Spectrometric Observations

    NASA Astrophysics Data System (ADS)

    Imanaka, Hiroshi; Cruikshank, D. P.

    2012-10-01

    The Cassini-Huygens observations greately extend our knowledge about Titan’s organic aerosols. The Cassini INMS and CAPS observations clearly demonstrate the formation of large organic molecules in the ionosphere [1, 2]. The VIMS and CIRS instruments have revealed spectral features of the haze covering the mid-IR and far-IR wavelengths [3, 4, 5, 6]. This study attempts to speculate the possible chemical nature of Titan’s aerosols by comparing the currently available observations with our laboratory study. We have conducted a series of cold plasma experiment to investigate the mass spectrometric and spectroscopic properties of laboratory aerosol analogs [7, 8]. Titan tholins and C2H2 plasma polymer are generated with cold plasma irradiations of N2/CH4 and C2H2, respectively. Laser desorption mass spectrum of the C2H2 plasma polymer shows a reasonable match with the CAPS positive ion mass spectrum. Furthermore, spectroscopic features of the the C2H2 plasma polymer in mid-IR and far-IR wavelegths qualitatively show reasonable match with the VIMS and CIRS observations. These results support that the C2H2 plasma polymer is a good candidate material for Titan’s aerosol particles at the altitudes sampled by the observations. We acknowledge funding supports from the NASA Cassini Data Analysis Program, NNX10AF08G, and from the NASA Exobiology Program, NNX09AM95G, and the Cassini Project. [1] Waite et al. (2007) Science 316, 870-875. [2] Crary et al. (2009) Planet. Space Sci. 57, 1847-1856. [3] Bellucci et al. (2009) Icarus 201, 198-216. [4] Anderson and Samuelson (2011) Icarus 212, 762-778. [5] Vinatier et al. (2010) Icarus 210, 852-866. [6] Vinatier et al. (2012) Icarus 219, 5-12. [7] Imanaka et al. (2004) Icarus 168, 344-366. [8] Imanaka et al. (2012) Icarus 218, 247-261.

  13. Characterizing particulate matter emissions from vehicles: chassis-dynamometer tests using a High-Resolution Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Collier, S.; Zhang, Q.; Forestieri, S.; Kleeman, M.; Cappa, C. D.; Kuwayama, T.

    2012-12-01

    During September of 2011 a suite of real-time instruments was used to sample vehicle emissions at the California Air Resources Board Haagen-Schmidt facility in El Monte, CA. A representative fleet of 8 spark ignition gasoline vehicles, a diesel passenger vehicle, a gasoline direct-injection vehicle and an ultra-low emissions vehicle were tested on a chassis dynamometer. The emissions were sampled into the facility's standard CVS tunnel and diluted to atmospherically relevant levels (5-30 μg/m3) while controlling other factors such as relative humidity or background black carbon particulate loading concentrations. An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-MS) was among the real-time instruments used and sampled vehicle emissions at 10 second time resolution in order to characterize the non-refractory organic and inorganic particulate matter (PM). PM composition and concentration were tracked throughout the cold start driving cycle which included periods of fast acceleration and high velocity cruise control, meant to recreate typical commuter driving behavior. Variations in inorganic and organic PM composition for a given vehicle throughout the driving cycle as well as for various vehicles with differing emissions loading were characterized. Differences in PM composition for a given vehicle whose emissions are being exposed to differing experimental conditions such as varying relative humidity will also be reported. In conjunction with measurements from a Multi Wavelength Photoacoustic Black Carbon Spectrometer (MWPA-BC) and real-time gas measurements from the CARB facility, we determine the real-time emission ratios of primary organic aerosols (POA) with respect to BC and common combustion gas phase pollutants and compared to different vehicle driving conditions. The results of these tests offer the vehicle emissions community a first time glimpse at the real-time behavior of vehicle PM emissions for a variety of conditions and

  14. Analysis of tear glucose concentration with electrospray ionization mass spectrometry.

    PubMed

    Taormina, Christopher R; Baca, Justin T; Asher, Sanford A; Grabowski, Joseph J; Finegold, David N

    2007-02-01

    We have developed a mass spectrometry-based method that allows one to accurately determine the glucose concentration of tear fluid. We used a 1 microL micro-capillary to collect tear fluid from the tear meniscus with minimal irritation of the eye. We analyzed the 1 muL volume of collected tear fluid with liquid-chromatography electrospray ionization mass spectrometry with the use of D-glucose-6,6-d2 as an internal standard. Repeated measurements and a recovery experiment on pooled, onion-induced tears showed that the analysis of the glucose in tears was precise (4% relative standard deviation) and provided 100% recovery. We found the tear glucose concentration of one fasting nondiabetic subject to be 13 to 51 microM while the onion-induced tear glucose concentration of a different nondiabetic subject to be 211 to 256 microM. PMID:17084090

  15. Analysis of Tear Glucose Concentration with Electrospray Ionization Mass Spectrometry

    PubMed Central

    Taormina, Christopher R.; Baca, Justin T.; Finegold, David N.; Asher, Sanford A.; Grabowski, Joseph J.

    2007-01-01

    We have developed a mass spectrometry-based method which allows one to accurately determine the glucose concentration of tear fluid. We used a 1 μL micro-capillary to collect tear fluid from the tear meniscus with minimal irritation of the eye. We analyzed the 1 μL volume of collected tear fluid with liquid-chromatography electrospray ionization mass spectrometry with the use of D-glucose-6,6-d2 as an internal standard. Repeated measurements and a recovery experiment on pooled, onion-induced tears showed that the analysis of the glucose in tears was precise (4% relative standard deviation) and provided 100% recovery. We found the tear glucose concentration of one fasting non-diabetic subject to be 13 to 51 μM while the onion-induced tear glucose concentration of a different non-diabetic subject to be 211 to 256 μM. PMID:17084090

  16. Source apportionment of elevated BaP concentrations in PM10 aerosols in an alpine valley in Austria

    NASA Astrophysics Data System (ADS)

    Bauer, Heidi; Puxbaum, Hans; Jankowski, Nicole; Sampaio Cordeiro Wagner, Lylian

    2010-05-01

    INTRODUCTION: In a village situated at 1215 m a.s.l. in a natural preserve in an Austrian alpine valley elevated BaP concentrations have been measured in the last years. A highly frequented highway leading from Italy to Germany passes near the village. Monthly means of particulate BaP concentrations show a clear seasonal trend with values below 1 ng/m³ during the warmer months and with concentrations up to 9 ng/m³ in the cold season. Annual averages in the years 2000 - 2005 ranged between 1.4 and 2.8 ng/m³ - much higher than the EU target value of 1 ng/m³. We used a macrotracer model developed at the Vienna University of Technology to determine the contributions of the sources for BaP emissions, which were mainly space heating with wood and traffic from the highway. EXPERIMENTAL: The macrotracer concept is a nine component model to derive source contribution and explains 80-100% of PM10 aerosols in Austria. The amount of traffic exhaust is derived by using EC as tracer, whereas EC produced by wood burning is subtracted, the amount of wood smoke is derived by the anhydro-sugar levoglucosan and the ratio between the anhydro-sugars levoglucosan and mannosan. For the source apportionment of BaP the applied factors reflect on the one hand the composition of the automotive fleet in Austria and on the other hand the composition of the fire wood in the region. Filter samples collected with a high volume sampler in winter were analyzed for PM10 aerosol mass, total, organic, elemental and carbonate carbon, HULIS, anhydro-sugars, polyols and ions (major ions and organic acids) and PAHs. In the same way emission samples taken at a motor test stand and at a test stand for wood combustion were analyzed (Schmidl et al. 2008). The saccharides were determined using high pH anion exchange and pulsed amperometry (HPAE-PAD). Details of the analytical method are given in Iinuma et al., 2009. Elemental and organic carbon were determined with a thermal-optical instrument (Sunset lab

  17. BioAerosol Mass Spectrometry: Reagentless Detection of Individual Airborne Spores and Other Bioagent Particles Based on Laser Desorption/Ionization Mass Spectrometry

    SciTech Connect

    Steele, P T

    2004-07-20

    Better devices are needed for the detection of aerosolized biological warfare agents. Advances in the ongoing development of one such device, the BioAerosol Mass Spectrometry (BAMS) system, are described here in detail. The system samples individual, micrometer-sized particles directly from the air and analyzes them in real-time without sample preparation or use of reagents. At the core of the BAMS system is a dual-polarity, single-particle mass spectrometer with a laser based desorption and ionization (DI) system. The mass spectra produced by early proof-of-concept instruments were highly variable and contained limited information to differentiate certain types of similar biological particles. The investigation of this variability and subsequent changes to the DI laser system are described. The modifications have reduced the observed variability and thereby increased the usable information content in the spectra. These improvements would have little value without software to analyze and identify the mass spectra. Important improvements have been made to the algorithms that initially processed and analyzed the data. Single particles can be identified with an impressive level of accuracy, but to obtain significant reductions in the overall false alarm rate of the BAMS instrument, alarm decisions must be made dynamically on the basis of multiple analyzed particles. A statistical model has been developed to make these decisions and the resulting performance of a hypothetical BAMS system is quantitatively predicted. The predictions indicate that a BAMS system, with reasonably attainable characteristics, can operate with a very low false alarm rate (orders of magnitude lower than some currently fielded biodetectors) while still being sensitive to small concentrations of biological particles in a large range of environments. Proof-of-concept instruments, incorporating some of the modifications described here, have already performed well in independent testing.

  18. Ozone and aerosol tropospheric concentrations variability analyzed using the ADRIMED measurements and the WRF and CHIMERE models

    NASA Astrophysics Data System (ADS)

    Menut, L.; Mailler, S.; Siour, G.; Bessagnet, B.; Turquety, S.; Rea, G.; Briant, R.; Mallet, M.; Sciare, J.; Formenti, P.; Meleux, F.

    2015-06-01

    During the months of June and July 2013, over the Euro-Mediterranean area, the ADRIMED (Aerosol Direct Radiative Impact on the regional climate in the MEDiterranean region) project was dedicated to characterize the ozone and aerosol concentrations in the troposphere. It is first shown that this period was not highly polluted compared to previous summers in this region, with a moderate ozone production, no significant vegetation fire events and several precipitation periods scavenging the aerosol. The period is modeled with the WRF (Weather Research and Forecasting) and CHIMERE models, and their ability to quantify the observed pollution transport events is presented. The CHIMERE model simulating all kinds of sources (anthropogenic, biogenic, mineral dust, vegetation fires); the aerosol speciation, not available with the measurements, is presented: during the whole period, the aerosol was mainly constituted by mineral dust, sea salt and sulfates close to the surface and mainly by mineral dust in the troposphere. Compared to the AERONET (Aerosol Robotic Network) size distribution, it is shown that the model underestimates the coarse mode near mineral dust sources and overestimates the fine mode in the Mediterranean area, highlighting the need to improve the model representation of the aerosol size distribution both during emissions, long-range transport and deposition.

  19. Comparison of three techniques for analysis of data from an Aerosol Time-of-Flight Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Giorio, Chiara; Tapparo, Andrea; Dall'Osto, Manuel; Harrison, Roy M.; Beddows, David C. S.; Di Marco, Chiara; Nemitz, Eiko

    2012-12-01

    The Aerosol Time-of-Flight Mass Spectrometer (ATOFMS) is one of few instruments able to measure the size and mass spectra of individual airborne particles with high temporal resolution. Data analysis is challenging and in the present study, we apply three different techniques (PMF, ART-2a and K-means) to a regional ATOFMS dataset collected at Harwell, UK. For the first time, Positive Matrix Factorization (PMF) was directly applied to single particle mass spectra as opposed to clusters already generated by the other methods. The analysis was performed on a total of 56,898 single particle mass