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Sample records for aerosol mass loadings

  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. 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.

  3. 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.

  4. Increased cloud activation potential of secondary organic aerosol for atmospheric mass loadings

    NASA Astrophysics Data System (ADS)

    King, S. M.; Rosenoern, T.; Shilling, J. E.; Chen, Q.; Martin, S. T.

    2009-05-01

    The effect of organic particle mass loading from 1 to ≥100 μg m-3 on the cloud condensation nuclei (CCN) properties of mixed organic-sulfate particles was investigated in the Harvard Environmental Chamber. Mixed particles were produced by the condensation of organic molecules onto ammonium sulfate particles during the dark ozonolysis of α-pinene. A continuous-flow mode of the chamber provided stable conditions over long time periods, allowing for signal integration and hence increased measurement precision at low organic mass loadings representative of atmospheric conditions. CCN activity was measured at eight mass loadings for 80- and 100-nm particles grown on 50-nm sulfate seeds. A two-component (organic/sulfate) Köhler model, which included the particle heterogeneity arising from DMA size selection and from organic volume fraction for the selected 80- and 100-nm particles, was used to predict CCN activity. For organic mass loadings of 2.9 μg m-3 and greater, the observed activation curves were well predicted using a single set of physicochemical parameters for the organic component. For mass loadings of 1.74 μg m-3 and less, the observed CCN activity increased beyond predicted values using the same parameters, implying changed physicochemical properties of the organic component. A sensitivity analysis suggests that a drop in surface tension must be invoked to explain quantitatively the CCN observations at low SOA particle mass loadings. Other factors, such as decreased molecular weight, increased density, or increased van't Hoff factor, can contribute to the explanation but are quantitatively insufficient as the full explanation.

  5. Increased Cloud Activation Potential of Secondary Organic Aerosol for Atmospheric Mass Loadings

    SciTech Connect

    King, Stephanie M.; Rosenoern, Thomas; Shilling, John E.; Chen, Qi; Martin, Scot T.

    2009-05-01

    The effect of organic particle mass loading from 1 to ≥100 μg m-3 on the cloud condensation nuclei (CCN) properties of mixed organic-sulfate particles was investigated in the Harvard Environmental Chamber. Mixed particles were produced by the condensation of organic molecules onto ammonium sulfate particles during the dark ozonolysis of α-pinene. A continuous-flow mode of the chamber provided stable conditions over long time periods, allowing for signal integration and hence increased measurement precision at low organic mass loadings representative of atmospheric conditions. CCN activity was measured at eight mass loadings for 80- and 100-nm particles grown on 50-nm sulfate seeds. A two-component (organic/sulfate) Köhler model, which included the particle heterogeneity arising from DMA size selection and from organic volume fraction for the selected 80- and 100-nm particles, was used to predict CCN activity. For organic mass loadings of 2.9 μg m-3 and greater, the observed activation curves were well predicted using a single set of physicochemical parameters for the organic component. For mass loadings of 1.74 μg m-3 and less, the observed CCN activity increased beyond predicted values using the same parameters, implying changed physicochemical properties of the organic component. Of possible changes in surface tension, effective molecular weight, and effective density, a sensitivity analysis implicated a decrease of up to 10% in surface tension at low mass loadings as the plausible dominant mechanism for the observed increase in CCN activity.

  6. Comparison of the impact of volcanic eruptions and aircraft emissions on the aerosol mass loading and sulfur budget in the stratosphere

    NASA Technical Reports Server (NTRS)

    Yue, Glenn K.; Poole, Lamont R.

    1992-01-01

    Data obtained by the Stratospheric Aerosol and Gas Experiment (SAGE) 1 and 2 were used to study the temporal variation of aerosol optical properties and to assess the mass loading of stratospheric aerosols from the eruption of volcanos Ruiz and Kelut. It was found that the yearly global average of optical depth at 1.0 micron for stratospheric background aerosols in 1979 was 1.16 x 10(exp -3) and in 1989 was 1.66 x 10(exp -3). The eruptions of volcanos Ruiz and Kelut ejected at least 5.6 x 10(exp 5) and 1.8 x 10(exp 5) tons of materials into the stratosphere, respectively. The amount of sulfur emitted per year from the projected subsonic and supersonic fleet is comparable to that contained in the background aerosol particles in midlatitudes from 35 deg N to 55 deg N.

  7. 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.

  8. The global atmospheric loading of dust aerosols

    NASA Astrophysics Data System (ADS)

    Kok, J. F.; Ridley, D. A.; Haustein, K.; Miller, R. L.; Zhao, C.

    2015-12-01

    Mineral dust is one of the most ubiquitous aerosols in the atmosphere, with important effects on human health and the climate system. But despite its importance, the global atmospheric loading of dust has remained uncertain, with model results spanning about a factor of five. Here we constrain the particle size-resolved atmospheric dust loading and global emission rate, using a novel theoretical framework that uses experimental constraints on the optical properties and size distribution of dust to eliminate climate model errors due to assumed dust properties. We find that most climate models underestimate the global atmospheric loading and emission rate of dust aerosols.

  9. Mass loading of size-segregated atmospheric aerosols in the ambient air during fireworks episodes in eastern Central India.

    PubMed

    Nirmalkar, Jayant; Deb, Manas K; Deshmukh, Dhananjay K; Verma, Santosh K

    2013-04-01

    The effects of combustion of the fire crackers on the air quality in eastern Central India were studied for the first time during Diwali festival. This case study analyzes the size distribution and temporal variation of aerosols collected in the rural area of eastern Central India during pre-diwali, Diwali and post-diwali period for the year of 2011. Fifteen aerosol samples were collected during the special case study of Diwali period using Andersen sampler. The mean concentrations of PM10 (respirable particulate matter) were found to be 212.8 ± 4.2, 555.5 ± 20.2 and 284.4 ± 5.8 during pre-diwali, Diwali and post-diwali period, respectively. During Diwali festival PM10 concentration was about 2.6 and 1.9 times higher than pre-diwali and post-diwali period, respectively. PM2.5 (fine) and PM1 (submicron) concentrations during Diwali festival were more than 2 times higher than pre-diwali and post-diwali.

  10. 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

  11. Mass loading and episodic variation of molecular markers in PM2.5 aerosols over a rural area in eastern central India

    NASA Astrophysics Data System (ADS)

    Nirmalkar, Jayant; Deshmukh, Dhananjay K.; Deb, Manas K.; Tsai, Ying I.; Sopajaree, Khajornsak

    2015-09-01

    The impact of biomass burning in atmospheric aerosols load is poorly known. We investigated the impact of biomass burning through molecular markers on the concentration of PM2.5 aerosol samples collected from a rural site in eastern central India during three episodic periods from October to November 2011. The collected PM2.5 samples were chemically quantified for potassium as well as sugars and dicarboxylic acids using ion chromatography. Levoglucosan and glucose were found as the most abundant sugar compounds and sugar-alcohols showed the predominance of mannitol whereas oxalic acid was the most abundant diacid followed by maleic acid in PM2.5 aerosols. Substantially enhanced concentrations of K+ as well as levoglucosan and glucose were observed in eastern central India. Analysis of the source specific molecular markers and ratios of sugars and diacids infer that combustion of biomass was the major emission sources of organic compounds associated with PM2.5 aerosols over eastern central India. We applied Spearman correlation analysis and principal component analysis to further investigate the sources of measured sugars and diacids. The concentrations of K+ and levoglucosan were significantly correlated with sugars and diacids that verifying their common sources from biomass burning emission. This study demonstrates that biomass burning for domestic heating and cooking purposes and agricultural activities significantly influence the air quality of eastern central India during the investigation period. The obtained data in this research is helpful for the global scientific community to assessments and remedial of air quality parameters in rural areas of developing countries under similar atmospheric circumstances.

  12. Genesis of elevated aerosol loading over the Indian region

    NASA Astrophysics Data System (ADS)

    Prijith, S. S.; Rao, P. V. N.; Mohan, Mannil

    2016-05-01

    Elevated aerosols assume importance as the diabatic heating due to aerosol absorption is more intense at higher altitudes where the atmosphere becomes thinner. Indian region, especially its central and northern latitudes, experiences significant loading of elevated aerosols during pre-monsoon and summer months. Genesis of elevated aerosol loading over Indian region is investigated in the present study, using multi-year satellite observations from Cloud Aerosol Lidar with Orthogonal Polarization (CALIOP) and Moderate Resolution Imaging Spectroradiometer (MODIS) along with reanalysis winds from MERRA. Central India is observed to have prominent aerosols loading at higher altitudes during pre-monsoon season, whereas it is during summer months over north-west India. Further analysis reveals that the elevated aerosols over Indian region in pre-monsoon and summer months are significantly contributed by transported mineral dust from the arid continental regions at west. In addition to the mineral dust advection, aerosols at higher altitudes over Indian region are enriched by strong convection and associated vertical transport of surface level aerosols. Vertical transport of aerosols observed over Indian region during pre-monsoon and summer months is aided by intense convergence at the surface level and divergence at the upper level. Moreover, aerosol source/sink strength estimated using aerosol flux continuity equation show significant aerosol production over central India during pre-monsoon. Strong vertical transport prevails during pre-monsoon uplifts the locally produced aerosols, with considerable anthropogenic fraction, to higher altitudes where their impacts would be more intense.

  13. Aerosol Properties and Radiative Forcing over Kanpur during Severe Aerosol Loading Conditions

    SciTech Connect

    Kaskaoutis, D. G.; Sinha, P. R.; Vinoj, V.; Kosmopoulos, P. G.; Tripathi, S. N.; Misra, Amit; Sharma, M.; Singh, R. P.

    2013-11-01

    Atmospheric aerosols over India exhibit large spatio-temporal fluctuation driven by the local monsoon system, emission rates and seasonally-changed air masses. The northern part of India is well-known for its high aerosol loading throughout the year due to anthropogenic emissions, dust influence and biomass burning. On certain circumstances and, under favorable weather conditions, the aerosol load can be severe, causing significant health concerns and climate implications. The present work analyzes the aerosol episode (AE) days and examines the modification in aerosol properties and radiative forcing during the period 2001-2010 based on Kanpur-AERONET sun photometer data. As AEs are considered the days having daily-mean aerosol optical depth (AOD) above the decadal mean + 1 STD (standard deviation); the threshold value is defined at 0.928. The results identify 277 out of 2095 days (13.2%) of AEs over Kanpur, which are most frequently observed during post-monsoon (78 cases, 18.6%) and monsoon (76, 14.7%) seasons due to biomass-burning episodes and dust influence, respectively. On the other hand, the AEs in winter and pre-monsoon are lower in both absolute and percentage values (65, 12.5% and 58, 9.1%, respectively). The modification in aerosol properties on the AE days is strongly related to season. Thus, in post-monsoon and winter the AEs are associated with enhanced presence of fine-mode aerosols and Black Carbon from anthropogenic pollution and any kind of burning, while in pre-monsoon and monsoon seasons they are mostly associated with transported dust. Aerosol radiative forcing (ARF) calculated using SBDART shows much more surface (~-69 to -97 Wm-2) and Top of Atmosphere cooling (-20 to -30 Wm-2) as well as atmospheric heating (~43 to 71 Wm-2) during the AE days compared to seasonal means. These forcing values are mainly controlled by the higher AODs and the modified aerosol characteristics (Angstrom α, SSA) during the AE days in each season and may cause

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

    PubMed

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

    2015-07-15

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

  15. Mass Loading Characteristics of Crystal Clock Oscillators

    NASA Technical Reports Server (NTRS)

    Cobb, Janel; Morris, V. R.; Thorpe, A. N.

    1997-01-01

    The 10-MHz piezoelectric quartz-crystal microbalance (QCM) has been used extensively for stratospheric aerosol sampling. We have undertaken laboratory studies of the QCM response to mass loading by trace gases. However, this device requires dual oscillator circuitry and the mass sensitivity can often be affected by the electronics. The coatings on the quartz crystals are sometimes difficult to remove after they have reacted with a particular gas and a disposable crystal system would be desirable. The cost of the dual oscillator-based QCM makes this a prohibitive option. Since our goal is to develop a cost-effective microbalance system with stable electronics we have begun testing of crystal clock oscillators, which are assembled with their own circuitry. We have been using chemically specific coatings for ozone to determine if the sensitivity and mass-frequency ratios are comparable to that of the 10-MHz QCM.

  16. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    DOE PAGES

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-03-02

    applied, but evaporative phenomena were not sufficient to explain the dependence of aerosol detection on particle diameter. Additional work is needed to correlate experimental data with theory for metal-oxides where thermodynamic property data are sparse relative to pure elements. Finally, when matrix effects and the diffusion of ions inside the plasma were considered, mass loading was concluded to have had an effect on the dependence of detection efficiency on particle diameter.« less

  17. Aerosol detection efficiency in inductively coupled plasma mass spectrometry

    NASA Astrophysics Data System (ADS)

    Hubbard, Joshua A.; Zigmond, Joseph A.

    2016-05-01

    evaporative phenomena were not sufficient to explain the dependence of aerosol detection on particle diameter. Additional work is needed to correlate experimental data with theory for metal-oxides where thermodynamic property data are sparse relative to pure elements. Lastly, when matrix effects and the diffusion of ions inside the plasma were considered, mass loading was concluded to have had an effect on the dependence of detection efficiency on particle diameter.

  18. SAGE measurements of the stratospheric aerosol dispersion and loading from the Soufriere Volcano

    NASA Technical Reports Server (NTRS)

    Mccormick, M. P.; Kent, G. S.; Yue, G. K.; Cunnold, D. M.

    1981-01-01

    Explosions of the Soufriere volcano on the Caribbean Island of St. Vincent reduced two major stratospheric plumes which the stratospheric aerosol and gas experiment (SAGE) satellite tracked to West Africa and the North Atlantic Ocean. The total mass of the stratospheric ejecta measured is less than 0.5% of the global stratospheric aerosol burden. No significant temperature or climate perturbation is expected. It is found that the movement and dispersion of the plumes agree with those deduced from high altitude meteorological data and dispersion theory. The stratospheric aerosol dispersion and loading from the Soufrier volcano was measured.

  19. 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.

  20. The impacts of aerosol loading, composition, and water uptake on aerosol extinction variability in the Baltimore-Washington, D.C. region

    NASA Astrophysics Data System (ADS)

    Beyersdorf, A. J.; Ziemba, L. D.; Chen, G.; Corr, C. A.; Crawford, J. H.; Diskin, G. S.; Moore, R. H.; Thornhill, K. L.; Winstead, E. L.; Anderson, B. E.

    2016-01-01

    In order to utilize satellite-based aerosol measurements for the determination of air quality, the relationship between aerosol optical properties (wavelength-dependent, column-integrated extinction measured by satellites) and mass measurements of aerosol loading (PM2.5 used for air quality monitoring) must be understood. This connection varies with many factors including those specific to the aerosol type - such as composition, size, and hygroscopicity - and to the surrounding atmosphere, such as temperature, relative humidity (RH), and altitude, all of which can vary spatially and temporally. During the DISCOVER-AQ (Deriving Information on Surface conditions from Column and Vertically Resolved Observations Relevant to Air Quality) project, extensive in situ atmospheric profiling in the Baltimore, MD-Washington, D.C. region was performed during 14 flights in July 2011. Identical flight plans and profile locations throughout the project provide meaningful statistics for determining the variability in and correlations between aerosol loading, composition, optical properties, and meteorological conditions. Measured water-soluble aerosol mass was composed primarily of ammonium sulfate (campaign average of 32 %) and organics (57 %). A distinct difference in composition was observed, with high-loading days having a proportionally larger percentage of sulfate due to transport from the Ohio River Valley. This composition shift caused a change in the aerosol water-uptake potential (hygroscopicity) such that higher relative contributions of inorganics increased the bulk aerosol hygroscopicity. These days also tended to have higher relative humidity, causing an increase in the water content of the aerosol. Conversely, low-aerosol-loading days had lower sulfate and higher black carbon contributions, causing lower single-scattering albedos (SSAs). The average black carbon concentrations were 240 ng m-3 in the lowest 1 km, decreasing to 35 ng m-3 in the free troposphere (above

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

    NASA Astrophysics Data System (ADS)

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

    2010-12-01

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

  2. Road traffic impact on urban atmospheric aerosol loading at Oporto, Portugal

    NASA Astrophysics Data System (ADS)

    Oliveira, César; Pio, Casimiro; Caseiro, Alexandre; Santos, Patrícia; Nunes, Teresa; Mao, Hongjun; Luahana, Lakhumal; Sokhi, Ranjeet

    2010-08-01

    At urban areas in south Europe atmospheric aerosol levels are frequently above legislation limits as a result of road traffic and favourable climatic conditions for photochemical formation and dust suspension. Strategies for urban particulate pollution control have to take into account specific regional characteristics and need correct information concerning the sources of the aerosol. With these objectives, the ionic and elemental composition of the fine (PM 2.5) and coarse (PM 2.5-10) aerosol was measured at two contrasting sites in the centre of the city of Oporto, roadside (R) and urban background (UB), during two campaigns, in winter and summer. Application of Spatial Variability Factors, in association with Principal Component/Multilinear Regression/Inter-site Mass Balance Analysis, to aerosol data permitted to identify and quantify 5 main groups of sources, namely direct car emissions, industry, photochemical production, dust suspension and sea salt transport. Traffic strongly influenced PM mass and composition. Direct car emissions and road dust resuspension contributed with 44-66% to the fine aerosol and with 12 to 55% to the coarse particles mass at both sites, showing typically highest loads at roadside. In fine particles secondary origin was also quite important in aerosol loading, principally during summer, with 28-48% mass contribution, at R and UB sites respectively. Sea spray has an important contribution of 18-28% to coarse aerosol mass in the studied area, with a highest relative contribution at UB site. Application of Spatial Variability/Mass Balance Analysis permitted the estimation of traffic contribution to soil dust in both size ranges, across sites and seasons, demonstrating that as much as 80% of present dust can result from road traffic resuspension.

  3. 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.

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

    PubMed

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

    2007-08-01

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

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

    PubMed

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

    2007-08-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2007-08-01

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

  7. Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

    SciTech Connect

    Gerstl, S.A.W.; Zardecki, A.

    1981-08-01

    The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10/sup 1/ g is sufficient to reduce photosynthesis to 10/sup -3/ of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated.

  8. Sulfur mass loading of the atmosphere from volcanic eruptions: Calibration of the ice core record on basis of sulfate aerosol deposition in polar regions from the 1982 El Chichon eruption

    NASA Technical Reports Server (NTRS)

    Sigurdsson, Haraldur; Laj, Paolo

    1990-01-01

    Major volcanic eruptions disperse large quantities of sulfur compound throughout the Earth's atmosphere. The sulfuric acid aerosols resulting from such eruptions are scavenged by snow within the polar regions and appear in polar ice cores as elevated acidity layers. Glacio-chemical studies of ice cores can, thus, provide a record of past volcanism, as well as the means for understanding the fate of volcanic sulfur in the atmosphere. The primary objectives of this project are to study the chemistry and physical properties of volcanic fallout in a Greenland Ice Core in order to evaluate the impact of the volcanic gases on the atmospheric chemistry and the total atmospheric mass of volcanic aerosols emitted by major volcanic eruptions. We propose to compare the ice core record to other atmospheric records performed during the last 10 years to investigate transport and deposition of volcanic materials.

  9. 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.

  10. 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

  11. 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

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

    NASA Astrophysics Data System (ADS)

    Chakraborty, Abhishek; Tripathi, Sachchida; Gupta, Tarun

    2016-04-01

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

  13. Predicting mass loading as a function of pressure difference across prefilter/HEPA filter systems

    SciTech Connect

    Novick, V.J.; Klassen, J.F. ); Monson, P.R. )

    1992-01-01

    The purpose of this work is to develop a methodology for predicting the mass loading and pressure drop effects on a prefilter/ HEPA filter system. The methodology relies on the use of empirical equations for the specific resistance of the aerosol loaded filter as a function of the particle diameter. These correlations relate the pressure difference across a filter to the mass loading on the filter and accounts for aerosol particle density effects. These predictions are necessary for the efficient design of new filtration systems and for risk assessment studies of existing filter systems. This work specifically addresses the prefilter/HEPA filter Airborne Activity Confinement Systems (AACS) at the Savannah River Plant. In order to determine the mass loading on the system, it is necessary to establish the efficiency characteristics for the prefilter, the mass loading characteristics of the prefilter measured as a function of pressure difference across the prefilter, and the mass loading characteristics of the HEPA filter as a function of pressure difference across the filter. Furthermore, the efficiency and mass loading characteristics need to be determined as a function of the aerosol particle diameter. A review of the literature revealed that no previous work had been performed to characterize the prefilter material of interest. In order to complete the foundation of information necessary to predict total mass loadings on prefilter/HEPA filter systems, it was necessary to determine the prefilter efficiency and mass loading characteristics. The measured prefilter characteristics combined with the previously determined HEPA filter characteristics allowed the resulting pressure difference across both filters to be predicted as a function of total particle mass for a given particle distribution. These predictions compare favorably to experimental measurements ({plus minus}25%).

  14. Aerosol Analysis via Electrostatic Precipitation-Electrospray Ionization Mass Spectrometry.

    PubMed

    He, Siqin; Li, Lin; Duan, Hongxu; Naqwi, Amir; Hogan, Christopher J

    2015-07-01

    Electrospray ionization (ESI) is the preferred mode of ion generation for mass analysis of many organic species, as alternative ionization techniques can lead to appreciable analyte fragmentation. For this reason, ESI is an ideal method for the analysis of species within aerosol particles. However, because of their low concentrations (∼10 μg/m(3)) in most environments, ESI has been applied sparingly in aerosol particle analysis; aerosol mass spectrometers typically employ analyte volatilization followed by electron ionization or chemical ionization, which can lead to a considerable degree of analyte fragmentation. Here, we describe an approach to apply ESI to submicrometer and nanometer scale aerosol particles, which utilizes unipolar ionization to charge particles, electrostatic precipitation to collect particles on the tip of a Tungsten rod, and subsequently, by flowing liquid over the rod, ESI and mass analysis of the species composing collected particles. This technique, which we term electrostatic precipitation-ESI-MS (EP-ESI-MS), is shown to enable analysis of nanogram quantities of collected particles (from aerosol phase concentrations as low as 10(2) ng m(-3)) composed of cesium iodide, levoglucosan, and levoglucosan within a carbon nanoparticle matrix. With EP-ESI-MS, the integrated mass spectrometric signals are found to be a monotonic function of the mass concentration of analyte in the aerosol phase. We additionally show that EP-ESI-MS has a dynamic range of close to 5 orders of magnitude in mass, making it suitable for molecular analysis of aerosol particles in laboratory settings with upstream particle size classification, as well as analysis of PM 2.5 particles in ambient air. PMID:26024017

  15. 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.

  16. 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.

  17. 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

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

    NASA Astrophysics Data System (ADS)

    Craven, Jill Suzanne

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

  19. Development of a continuous aerosol mass concentration measurement device.

    PubMed

    Bémer, D; Thomas, D; Contal, P; Subra, I

    2003-08-01

    A dynamic aerosol mass concentration measurement device has been developed for personal sampling. Its principle consists in sampling the aerosol on a filter and monitoring the change of pressure drop over time (Delta P). Ensuring that the linearity of the Delta P = f(mass of particles per unit area of filter) relationship has been well established, the change of concentration can be deduced. The response of the system was validated in the laboratory with a 3.5 microm alumina aerosol (mass median diameter) generated inside a 1-m(3) ventilated enclosure. As the theory predicted that the mass sensitivity of the system would vary inversely with the square of the particle diameter, only sufficiently fine aerosols were able to be measured. The system was tested in the field in a mechanical workshop in the vicinity of an arc-welding station. The aerosol produced by welding is indeed particularly well-adapted due to the sub-micronic size of the particles. The device developed, despite this limitation, has numerous advantages over other techniques: robustness, compactness, reliability of calibration, and ease of use.

  20. Aerosol propellant interference with clinical mass spectrometers.

    PubMed

    Kharasch, E D; Sivarajan, M

    1991-04-01

    Metered dose inhalers containing halogenated propellants may interfere with mass spectrometer quantitation of halogenated inhalation anesthetics. We identify the propellant(s) in a commercially available metered dose inhaler that caused erroneous mass spectrometer readings. In addition, we identify the causes of different types of interference in different mass spectrometers. PMID:2072131

  1. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-10-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks.

  2. Enhanced Volatile Organic Compounds emissions and organic aerosol mass increase the oligomer content of atmospheric aerosols

    PubMed Central

    Kourtchev, Ivan; Giorio, Chiara; Manninen, Antti; Wilson, Eoin; Mahon, Brendan; Aalto, Juho; Kajos, Maija; Venables, Dean; Ruuskanen, Taina; Levula, Janne; Loponen, Matti; Connors, Sarah; Harris, Neil; Zhao, Defeng; Kiendler-Scharr, Astrid; Mentel, Thomas; Rudich, Yinon; Hallquist, Mattias; Doussin, Jean-Francois; Maenhaut, Willy; Bäck, Jaana; Petäjä, Tuukka; Wenger, John; Kulmala, Markku; Kalberer, Markus

    2016-01-01

    Secondary organic aerosol (SOA) accounts for a dominant fraction of the submicron atmospheric particle mass, but knowledge of the formation, composition and climate effects of SOA is incomplete and limits our understanding of overall aerosol effects in the atmosphere. Organic oligomers were discovered as dominant components in SOA over a decade ago in laboratory experiments and have since been proposed to play a dominant role in many aerosol processes. However, it remains unclear whether oligomers are relevant under ambient atmospheric conditions because they are often not clearly observed in field samples. Here we resolve this long-standing discrepancy by showing that elevated SOA mass is one of the key drivers of oligomer formation in the ambient atmosphere and laboratory experiments. We show for the first time that a specific organic compound class in aerosols, oligomers, is strongly correlated with cloud condensation nuclei (CCN) activities of SOA particles. These findings might have important implications for future climate scenarios where increased temperatures cause higher biogenic volatile organic compound (VOC) emissions, which in turn lead to higher SOA mass formation and significant changes in SOA composition. Such processes would need to be considered in climate models for a realistic representation of future aerosol-climate-biosphere feedbacks. PMID:27733773

  3. 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.

  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. MASS SPECTROMETRY OF INDIVIDUAL AEROSOL PARTICLES. (R823980)

    EPA Science Inventory

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

  6. 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<...

  7. Aerosol mass spectrometry systems and methods

    DOEpatents

    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.

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

    NASA Astrophysics Data System (ADS)

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

    2003-04-01

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

  9. 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

  10. 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.

  11. Measurement and analysis of aerosol and black carbon in the southwestern United States and Panama and their dependence on air mass origin

    NASA Astrophysics Data System (ADS)

    Junker, C.; Sheahan, J. N.; Jennings, S. G.; O'Brien, P.; Hinds, B. D.; Martinez-Twary, E.; Hansen, A. D. A.; White, C.; Garvey, D. M.; Pinnick, R. G.

    2004-07-01

    Total aerosol mass loading, aerosol absorption, and black carbon (BC) content were determined from aerosol collected on 598 quartz fiber filters at a remote, semiarid site near Orogrande, New Mexico from December 1989 to October 1995. Aerosol mass was determined by weighing filters before and after exposure, and aerosol absorption was determined by measuring the visible light transmitted through loaded filter samples and converting these measurements to aerosol absorption. BC content was determined by measuring visible light transmitted through filter samples before and after firing and converting the absorption to BC mass, assuming a BC absorption cross section of 19 m2/g in the fiber filter medium. Two analyses were then performed on each of the logged variables: an autoregressive integrating moving average (ARIMA) analysis and a decomposition analysis using an autoregressive model to accommodate first-order autocorrelation. The two analyses reveal that BC mass has no statistically significant seasonal dependence at the 5% level of significance but only random fluctuations varying around an average annual value that has a long-term decreasing trend (from 0.16 to 0.11 μg/m3 during 1990-1995). Aerosol absorption, which is dominated by BC, also displays random fluctuations about an average value, and decreases from 1.9 Mm-1 to 1.3 Mm-1 during the same period. Unlike BC, aerosol mass at the Orogrande site displays distinctly different character. The analyses reveal a pronounced seasonal dependence, but no long-term trend for aerosol mass. The seasonal indices resulting from the autoregression analysis have a minimum in January (-0.78) and maximum in June (+0.58). The geometric mean value over the 1990-1995 period for aerosol mass is 16.0 μg/m3. Since BC aerosol at the Orogrande site is a product of long-range atmospheric transport, a back trajectory analysis of air masses was conducted. Back trajectory analyses indicate that air masses traversing high population

  12. 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

  13. 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.

  14. 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.

  15. 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.

  16. 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

  17. 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.

  18. 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

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

    SciTech Connect

    Prather, K.A.; Noble, C.; Salt, K.; Nordmeyer, T.; Fergenson, D.; Morrical, B.

    1995-12-31

    Particulate pollution is an area of growing concern in light of recent studies which suggest a link between high concentrations of ambient PM{sub 10} (particles with diameters equal to or less than 10 {mu}m) and adverse health effects ranging from respiratory ailments to premature death. However, analytical chemistry techniques aimed at sampling and analysis of atmospheric aerosols are extremely limited in comparison to the number of methods that exist for studying gas phase smog components. As a result, current government regulations for levels of ambient particulates are necessarily general, lacking any chemical specificity. The authors have recently developed a technique, Aerosol-Time-of-Flight Mass Spectrometry (ATOFMS), which is capable of real-time determination of the size and chemical composition of individual aerosol particles. In order to obtain such information, the techniques of aerodynamic particle sizing and time-of-flight spectrometry are combined in a single instrument. In one of the aerosol studies performed in this laboratory, this instrument is being used for the direct analysis of ambient aerosols with the goal of establishing correlations between particle size and chemical composition. To date, the authors have observed very distinct size/composition correlations for organic and inorganic particles.

  20. Aerosol Lidar and MODIS Satellite Comparisons for Future Aerosol Loading Forecast

    NASA Technical Reports Server (NTRS)

    DeYoung, Russell; Szykman, James; Severance, Kurt; Chu, D. Allen; Rosen, Rebecca; Al-Saadi, Jassim

    2006-01-01

    Knowledge of the concentration and distribution of atmospheric aerosols using both airborne lidar and satellite instruments is a field of active research. An aircraft based aerosol lidar has been used to study the distribution of atmospheric aerosols in the California Central Valley and eastern US coast. Concurrently, satellite aerosol retrievals, from the MODIS (Moderate Resolution Imaging Spectroradiometer) instrument aboard the Terra and Aqua satellites, were take over the Central Valley. The MODIS Level 2 aerosol data product provides retrieved ambient aerosol optical properties (e.g., optical depth (AOD) and size distribution) globally over ocean and land at a spatial resolution of 10 km. The Central Valley topography was overlaid with MODIS AOD (5x5 sq km resolution) and the aerosol scattering vertical profiles from a lidar flight. Backward air parcel trajectories for the lidar data show that air from the Pacific and northern part of the Central Valley converge confining the aerosols to the lower valley region and below the mixed layer. Below an altitude of 1 km, the lidar aerosol and MODIS AOD exhibit good agreement. Both data sets indicate a high presence of aerosols near Bakersfield and the Tehachapi Mountains. These and other results to be presented indicate that the majority of the aerosols are below the mixed layer such that the MODIS AOD should correspond well with surface measurements. Lidar measurements will help interpret satellite AOD retrievals so that one day they can be used on a routine basis for prediction of boundary layer aerosol pollution events.

  1. 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.

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

    PubMed

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

    2013-03-19

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

  3. 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

  4. Comparison of Aerosol Mass Spectrometer and Aerosol Chemical Speciation Monitor Measurements of Secondary Organic Aerosol Formation in Smog Chamber Studies

    NASA Astrophysics Data System (ADS)

    Croteau, P. L.; Hunter, J. F.; Daumit, K. E.; Carrasquillo, A. J.; Cross, E. S.; Canagaratna, M.; Jayne, J.; Worsnop, D. R.; Kroll, J. H.

    2012-12-01

    Thermal vaporization-electron impact ionization (TV-EI) mass spectrometry is a powerful tool for understanding the chemistry of secondary organic aerosol (SOA) formation and atmospheric aging. The Aerodyne Aerosol Mass Spectrometer (AMS) and recently developed Aerosol Chemical Speciation Monitor (ACSM) are two instruments that utilize the same TV-EI technique. The ACSM trades the particle sizing capability, sensitivity, speed, and resolution of the AMS for simplicity, affordability, and ease of operation - enabling stand-alone continuous sampling for extended periods of time. Here we present results of an intercomparison between a high-resolution AMS and an ACSM. Three well-studied SOA formation chamber experiments were conducted: isoprene photooxidation under high NOx conditions, m-xylene photooxidation under high NOx conditions, and α-pinene ozonolysis under low NOx conditions. Comparisons between time-series and mass spectra from these experiments, along with positive matrix factorization analysis results demonstrate that the ACSM, while it does not provide the same level of detail as an AMS, is a suitable tool for exploring the chemistry of SOA formation in chamber studies.

  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. Aerosols in Polluted versus Nonpolluted Air Masses: Long-Range Transport and Effects on Clouds.

    NASA Astrophysics Data System (ADS)

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

    1986-12-01

    To assess the influence of anthropogenic aerosols on the physics and chemistry of clouds in the northeastern United State, 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, New York, 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 to 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. (ii) A significant fraction of anthropogenic sulfur aerosols appears to act as cloud condensation nuclei (CCN) to affect the cloud drop concentration. (iii) 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. (iv) 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.

  7. 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

  8. 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

  9. 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.

  10. Effects on stratospheric ozone from high-speed civil transport: Sensitivity to stratospheric aerosol loading

    NASA Technical Reports Server (NTRS)

    Weisenstein, Debra K.; Ko, Malcolm K. W.; Rodriguez, Jose M.; Sze, Nien-Dak

    1993-01-01

    The potential impact of high-speed civil transport (HSCT) aircraft emissions on stratospheric ozone and the sensitivity of these results to changes in aerosol loading are examined with a two-dimensional model. With aerosols fixed at background levels, calculated ozone changes due to HSCT aircraft emissions range from negligible up to 4-6% depletions in column zone at northern high latitudes. The magnitude of the ozone change depends mainly on the NO(x) increase due to aircraft emissions, which depends on fleet size, cruise altitude, and engine design. The partitioning of the odd nitrogen species in the lower stratosphere among NO, NO2, N2O5, is strongly dependent on the concentration of sulfuric acid aerosol particles, and thus the sensitivity of O3 to NO(x) emissions changes when the stratospheric aerosol loading changes. Aerosol concentrations 4 times greater than background levels have not been unusual in the last 2 decades. Our model results show that a factor of 4 increase in aerosol loading would significantly reduce the calculated ozone depletion due to HSCT emissions. Because of the neutral variabiltiy of stratospheric aerosols, the possible impact of HSCT emissions on ozone must be viewed as a range of possible results.

  11. 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.

  12. 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.

  13. 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

  14. 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

  15. 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.

  16. 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.

  17. Quantification of re-evaporated mass from loaded fibre-mist eliminators.

    PubMed

    Riss, B; Wahlmüller, E; Höflinger, W

    1999-08-01

    Airborne lubricant emissions are a serious health hazard for employees in the metal working industry. The basic components of lubricants are oils and additives for adapting the properties to achieve the process demands. The oils used in lubricants are either mineral, synthetic or of biological origin. The lubricants are used as water-emulsions and also as straight oils. Extreme process conditions cause considerable amounts of aerosol and vapour emissions of lubricants into the working environment. Fibre filters are used in industrial demisters for pollution control and also for sampling purposes. Re-evaporation of separated lubricants from loaded fibre filters causes increased vapour emissions. Quantification of lubricant vapour emission was the subject of this research. An apparatus and an appropriate procedure for measuring the dynamic behaviour of evaporative losses from fibre filters were developed. The test piece of a loaded fibre filter was fixed in a sampling probe according to VDI 2066. The vapour concentration of organic compounds in downstream air was measured in real-time by using a photo-ionisation detector (PID). The PID was checked by sampling the vapour on an oleophilic adsorbent resin, solvent extraction and quantitative IR analysis and also gravimetrically. The two basic processes of filtering volatile aerosols are, on the one hand, collecting droplets on the fibres and, on the other hand, the evaporation of collected liquid. These two processes had to be separated in order to measure the increase of the vapour concentration caused by the tested fibre filter. The experiments were carried out using pure dodecane and hexadecane in order to avoid difficulties due to the unknown chemical composition of lubricant vapour. The variation of the air flow and the initial liquid mass on the filter covered the relevant range for industrial fibre demisters and for sampling methods based on collecting aerosols on fibre filters. It was found that the downstream

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

    NASA Astrophysics Data System (ADS)

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

    2003-12-01

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

  19. 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...

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

    SciTech Connect

    Ludvigson, Laura D.

    2004-01-01

    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. 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

  2. Investigation of the relative fine and coarse mode aerosol loadings and properties in the Southern Arabian Gulf region

    NASA Astrophysics Data System (ADS)

    Kaku, Kathleen C.; Reid, Jeffrey S.; Reid, Elizabeth A.; Ross-Langerman, Kristy; Piketh, Stuart; Cliff, Steven; Al Mandoos, Abdulla; Broccardo, Stephen; Zhao, Yongjing; Zhang, Jianglong; Perry, Kevin D.

    2016-03-01

    The aerosol chemistry environment of the Arabian Gulf region is extraordinarily complex, with high concentrations of dust aerosols from surrounding deserts mixed with anthropogenic aerosols originating from a large petrochemical industry and pockets of highly urbanized areas. Despite the high levels of aerosols experienced by this region, little research has been done to explore the chemical composition of both the anthropogenic and mineral dust portion of the aerosol burden. The intensive portion of the United Arab Emirates Unified Aerosol Experiment (UAE2), conducted during August and September 2004 was designed in part to resolve the aerosol chemistry through the use of multiple size-segregated aerosol samplers. The coarse mode mass (derived by subtracting the PM2.5 aerosol mass from the PM10 mass) is largely dust at 76% ± 7% of the total coarse mode mass, but is significantly impacted by anthropogenic pollution, primarily sulfate and nitrate. The PM2.5 aerosol mass also contains a large dust burden, at 38% ± 26%, but the anthropogenic component dominates. The total aerosol burden has significant impact not only on the atmosphere, but also the local population, as the air quality levels for both the PM10 and PM2.5 aerosol masses reached unhealthy levels for 24% of the days sampled.

  3. The Dependence of Cloud Particle Size on Non-Aerosol-Loading Related Variables

    SciTech Connect

    Shao, H.; Liu, G.

    2005-03-18

    An enhanced concentration of aerosol may increase the number of cloud drops by providing more cloud condensation nuclei (CCN), which in turn results in a higher cloud albedo at a constant cloud liquid water path. This process is often referred to as the aerosol indirect effect (AIE). Many in situ and remote sensing observations support this hypothesis (Ramanathan et al. 2001). However, satellite observed relations between aerosol concentration and cloud drop size are not always in agreement with the AIE. Based on global analysis of cloud effective radius (r{sub e}) and aerosol number concentration (N{sub a}) derived from satellite data, Sekiguchi et al. (2003) found that the correlations between the two variables can be either negative, or positive, or none, depending on the location of the clouds. They discovered that significantly negative r{sub e} - N{sub a} correlation can only be identified along coastal regions of the continents where abundant continental aerosols inflow from land, whereas Feingold et al. (2001) found that the response of r{sub e} to aerosol loading is the greatest in the region where aerosol optical depth ({tau}{sub a}) is the smallest. The reason for the discrepancy is likely due to the variations in cloud macroscopic properties such as geometrical thickness (Brenguier et al. 2003). Since r{sub e} is modified not only by aerosol but also by cloud geometrical thickness (H), the correlation between re and {tau}{sub a} actually reflects both the aerosol indirect effect and dependence of H. Therefore, discussing AIE based on the r{sub e}-{tau}{sub a} correlation without taking into account variations in cloud geometrical thickness may be misleading. This paper is motivated to extract aerosols' effect from overall effects using the independent measurements of cloud geometrical thickness, {tau}{sub a} and r{sub e}.

  4. 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

  5. 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

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

    NASA Astrophysics Data System (ADS)

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

    2008-12-01

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

  7. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-01-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  8. Study of the effect of humidity, particle hygroscopicity and size on the mass loading capacity of HEPA filters

    SciTech Connect

    Gupta, A.

    1992-09-01

    The effect of humidity, particle hygroscopicity and size on the mass loading capacity of glass fiber HEPA filters has been studied. At humidifies above the deliquescent point, the pressure drop across the HEPA filter increased non-linearly with the areal loading density (mass collected/filtration area) of NaCl aerosol, thus significantly reducing the mass loading capacity of the filter compared to dry hygroscopic or non-hygroscopic particle mass loadings. The specific cake resistance, K{sub 2}, has been computed for different test conditions and used as a measure of the mass loading capacity. K. was found to decrease with increasing humidity for the non-hygroscopic aluminum oxide particles and the hygroscopic NaCl particles (at humidities below the deliquescent point). It is postulated that an increase in humidity leads to the formation of a more open particulate cake which lowers the pressure drop for a given mass loading. A formula for predicting K{sub 2} for lognormally distributed aerosols (parameters obtained from impactor data) is derived. The resistance factor, R, calculated using this formula was compared to the theoretical R calculated using the Rudnick-Happel expression. For the non-hygroscopic aluminum oxide the agreement was good but for the hygroscopic sodium chloride, due to large variation in the cake porosity estimates, the agreement was poor.

  9. Secondary organic aerosol formation from in-use motor vehicle emissions using a potential aerosol mass reactor.

    PubMed

    Tkacik, Daniel S; Lambe, Andrew T; Jathar, Shantanu; Li, Xiang; Presto, Albert A; Zhao, Yunliang; Blake, Donald; Meinardi, Simone; Jayne, John T; Croteau, Philip L; Robinson, Allen L

    2014-10-01

    Secondary organic aerosol (SOA) formation from in-use vehicle emissions was investigated using a potential aerosol mass (PAM) flow reactor deployed in a highway tunnel in Pittsburgh, Pennsylvania. Experiments consisted of passing exhaust-dominated tunnel air through a PAM reactor over integrated hydroxyl radical (OH) exposures ranging from ∼ 0.3 to 9.3 days of equivalent atmospheric oxidation. Experiments were performed during heavy traffic periods when the fleet was at least 80% light-duty gasoline vehicles on a fuel-consumption basis. The peak SOA production occurred after 2-3 days of equivalent atmospheric oxidation. Additional OH exposure decreased the SOA production presumably due to a shift from functionalization to fragmentation dominated reaction mechanisms. Photo-oxidation also produced substantial ammonium nitrate, often exceeding the mass of SOA. Analysis with an SOA model highlight that unspeciated organics (i.e., unresolved complex mixture) are a very important class of precursors and that multigenerational processing of both gases and particles is important at longer time scales. The chemical evolution of the organic aerosol inside the PAM reactor appears to be similar to that observed in the atmosphere. The mass spectrum of the unoxidized primary organic aerosol closely resembles ambient hydrocarbon-like organic aerosol (HOA). After aging the exhaust equivalent to a few hours of atmospheric oxidation, the organic aerosol most closely resembles semivolatile oxygenated organic aerosol (SV-OOA) and then low-volatility organic aerosol (LV-OOA) at higher OH exposures. Scaling the data suggests that mobile sources contribute ∼ 2.9 ± 1.6 Tg SOA yr(-1) in the United States, which is a factor of 6 greater than all mobile source particulate matter emissions reported by the National Emissions Inventory. This highlights the important contribution of SOA formation from vehicle exhaust to ambient particulate matter concentrations in urban areas.

  10. MISR Aerosol Air Mass Type Mapping over Mega-City: Validation and Applications

    NASA Astrophysics Data System (ADS)

    Patadia, F.; Kahn, R. A.

    2010-12-01

    Most aerosol air-quality monitoring in mega-city environments is done from scattered ground stations having detailed chemical and optical sampling capabilities. Satellite instruments such as the Multi-angle Imaging SpectroRadiometer (MISR) can retrieve total-column Aerosol Optical Depth (AOD), along with some information about particle microphysical properties. Although the particle property information from MISR is much less detailed than that obtained from the ground sampling stations, the coverage is extensive, making it possible to put individual surface observations into the context of regional aerosol air mass types. This paper presents an analysis of MISR aerosol observations made coincident with aircraft and ground-based instruments during the INTEX-B field campaign. These detailed comparisons of satellite aerosol property retrievals against dedicated field measurements provide the opportunity to validate the retrievals quantitatively at a regional level, and help to improve aerosol representation in retrieval algorithms. Validation of MISR retrieved AOD and other aerosol properties over the INTEX-B study region in and around Mexico City will be presented. MISR’s ability to distinguish among aerosol air mass types will be discussed. The goal of this effort is to use the MISR aerosol property retrievals for mapping both aerosol air mass type and AOD gradients in mega-city environments over the decade-plus that MISR has made global observations.

  11. Fullerene Soot in Eastern China Air: Results from Soot Particle-Aerosol Mass Spectrometer

    NASA Astrophysics Data System (ADS)

    Wang, J.; Ge, X.; Chen, M.; Zhang, Q.; Yu, H.; Sun, Y.; Worsnop, D. R.; Collier, S.

    2015-12-01

    In this work, we present for the first time, the observation and quantification of fullerenes in ambient airborne particulate using an Aerodyne Soot Particle - Aerosol Mass Spectrometer (SP-AMS) deployed during 2015 winter in suburban Nanjing, a megacity in eastern China. The laser desorption and electron impact ionization techniques employed by the SP-AMS allow us to differentiate various fullerenes from other aerosol components. Mass spectrum of the identified fullerene soot is consisted by a series of high molecular weight carbon clusters (up to m/z of 2000 in this study), almost identical to the spectral features of commercially available fullerene soot, both with C70 and C60 clusters as the first and second most abundant species. This type of soot was observed throughout the entire study period, with an average mass loading of 0.18 μg/m3, accounting for 6.4% of the black carbon mass, 1.2% of the total organic mass. Temporal variation and diurnal pattern of fullerene soot are overall similar to those of black carbon, but are clearly different in some periods. Combining the positive matrix factorization, back-trajectory and analyses of the meteorological parameters, we identified the petrochemical industrial plants situating upwind from the sampling site, as the major source of fullerene soot. In this regard, our findings imply the ubiquitous presence of fullerene soot in ambient air of industry-influenced area, especially the oil and gas production regions. This study also offers new insights into the characterization of fullerenes from other environmental samples via the advanced SP-AMS technique.

  12. Mass-loading and the formation of the Venus tail

    NASA Technical Reports Server (NTRS)

    Russell, C. T.; Luhmann, J. G.; Saunders, M. A.

    1985-01-01

    Despite its lack of intrinsic magnetic field Venus has a well defined magnetotail, containing about 3 megawebers of magnetic flux in a tail about 4 Venus radii across with perhaps a slightly elliptical cross section. This tail arises through the mass-loading of magnetic flux tubes passing by the planet. Mass-loading can occur due to charge exchange and photoionization as well as from the diffusion of magnetic field into the ionosphere. Various evidence exists for the mass-loading process, including the direct observation of the picked up ions with both the Venera and Pioneer Venus plasma analyzers.

  13. 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

  14. 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

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

    PubMed Central

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

    2010-01-01

    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 NOx 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 SO2 and marine dimethyl sulfide emissions generate secondary biogenic aerosol mass throughout the troposphere. PMID:21098310

  16. 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

  17. 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.

  18. Aerosol and trace gas vehicle emission factors measured in a tunnel using an Aerosol Mass Spectrometer and other on-line instrumentation

    NASA Astrophysics Data System (ADS)

    Chirico, Roberto; Prevot, Andre S. H.; DeCarlo, Peter F.; Heringa, Maarten F.; Richter, Rene; Weingartner, Ernest; Baltensperger, Urs

    2011-04-01

    In this study we present measurements of gas and aerosol phase composition for a mixed vehicle fleet in the Gubrist tunnel (Switzerland) in June 2008. PM 1 composition measurements were made with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (AMS) and a Multi Angle Absorption Photometer (MAAP). Gas-phase measurements of CO, CO 2, NO x and total hydrocarbons (THC) were performed with standard instrumentation. Weekdays had a characteristic diurnal pattern with 2 peaks in concentrations for all traffic related species corresponding to high vehicle density (˜300 ± 30 vehicles per 5 min) in the morning rush hour between 06:00 and 09:00 and in the afternoon rush hours from approximately 15:30 to 18:30. The emission factors (EF) of OA were heavily influenced by the OA mass loading. To exclude this partitioning effect, only organic aerosol mass concentrations from 60 μg m -3 to 90 μg m -3 were considered and for these conditions the EF(OA) value for HDV was 33.7 ± 2.3 mg km -1 for a temperature inside the tunnel of 20-25 °C. This value is not directly applicable to ambient conditions because it is derived from OA mass concentrations that are roughly a factor of 10 higher than typical ambient concentrations. An even higher EF(OA) HDV value of 47.4 ± 1.6 mg km -1 was obtained when the linear fit was applied to all data points including OA concentrations up to 120 μg m -3. Similar to the increasing EF, the OA/BC ratio in the tunnel was also affected by the organic loading and it increased by a factor of ˜3 over the OA range 10-120 μg m -3. This means that also the OA emission factors at ambient concentrations of around 5-10 μg m -3 would be 2-3 times lower than the emission factor given above. For OA concentrations lower than 40 μg m -3 the OA/BC mass ratio was below 1, while at an OA concentration of 100-120 μg m -3 the OA/BC ratio was ˜1.5. The AMS mass spectra (MS) acquired in the tunnel were highly correlated with the primary organic aerosol

  19. Mass spectrometry investigation of Titan aerosols analogs formed with traces of aromatic compounds

    NASA Astrophysics Data System (ADS)

    Gautier, Thomas; Trainer, Melissa; Sebree, Joshua; Li, Xiang; Pinnick, Veronica; Getty, Stephanie; Brinckerhoff, Will

    2016-06-01

    The detection of benzene at ppm levels in Titan's atmosphere [1] by Cassini's Ion and Neutral Mass Spectrometer (INMS) supports the idea that aromatic and heteroaromatic reaction pathways may play an important role in Titan's aerosols formation. In laboratory studies it has been shown that these aromatic molecules are easily dissociated by ultraviolet radiation and can therefore contribute significantly to aerosol formation [2] and be used to dope the production of aerosol analogs [3]. In this work we investigate the effect on the aerosol composition and growth pattern of the chemical nature of the aromatic reactant used to produce aerosol. Analysis are performed using Laser Desorption-Time of Flight mass spectrometry (LD-TOF) and Fourier Transform Infrared Spectroscopy (FTIR) Infrared analysis of our samples shows that inclusion of aromatic compounds as trace precursors allows to better fit laboratory data to Titan aerosol spectra observed by Cassini [3,4]. The improvement is especially visible on the far infrared (˜200 cm‑1) bands observed by CIRS [5]. LDMS results show that the aerosol growth patterns depend both on the number of rings and on the nitrogen content of the trace precursor used. We also perform MS/MS analysis on some prominent peaks of aerosol mass spectra. This MS/MS approach allows us to identify some of the key compounds in the aerosol growth processes.

  20. Mass spectrometry investigation of Titan aerosols analogs formed with traces of aromatic compounds

    NASA Astrophysics Data System (ADS)

    Gautier, Thomas; Trainer, Melissa; Sebree, Joshua; Li, Xiang; Pinnick, Veronica; Getty, Stephanie; Brinckerhoff, Will

    2016-06-01

    The detection of benzene at ppm levels in Titan's atmosphere [1] by Cassini's Ion and Neutral Mass Spectrometer (INMS) supports the idea that aromatic and heteroaromatic reaction pathways may play an important role in Titan's aerosols formation. In laboratory studies it has been shown that these aromatic molecules are easily dissociated by ultraviolet radiation and can therefore contribute significantly to aerosol formation [2] and be used to dope the production of aerosol analogs [3]. In this work we investigate the effect on the aerosol composition and growth pattern of the chemical nature of the aromatic reactant used to produce aerosol. Analysis are performed using Laser Desorption-Time of Flight mass spectrometry (LD-TOF) and Fourier Transform Infrared Spectroscopy (FTIR) Infrared analysis of our samples shows that inclusion of aromatic compounds as trace precursors allows to better fit laboratory data to Titan aerosol spectra observed by Cassini [3,4]. The improvement is especially visible on the far infrared (˜200 cm-1) bands observed by CIRS [5]. LDMS results show that the aerosol growth patterns depend both on the number of rings and on the nitrogen content of the trace precursor used. We also perform MS/MS analysis on some prominent peaks of aerosol mass spectra. This MS/MS approach allows us to identify some of the key compounds in the aerosol growth processes.

  1. Study of node and mass sensitivity of resonant mode based cantilevers with concentrated mass loading

    NASA Astrophysics Data System (ADS)

    Zhang, Kewei; Chai, Yuesheng; Fu, Jiahui

    2015-12-01

    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 xc satisfied 0 < xc < ˜ 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 ≤ xc ≤ 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.

  2. 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.

  3. Aerosol matrix-assisted laser desorption ionization for liquid chromatography/time-of-flight mass spectrometry

    SciTech Connect

    Murray, K.K.; Lewis, T.M.; Beeson, M.D.; Russell, D.H. )

    1994-05-15

    We report the application of aerosol matrix-assisted laser desorption ionization (MALDI) to liquid chromatography/mass spectrometry (LC/MS). The aerosol MALDI experiment uses aerosol liquid introduction in conjunction with pulsed UV laser ionization to form ions from large biomolecules in solution. Mass analysis is achieved in a time-of-flight mass spectrometer. In the LC/MALDI-MS experiment, the matrix solution is combined with the column effluent in a mixing tee, LC/MALDI-MS is demonstrated for the separation of bradykinin, gramicidin S, and myoglobin. 32 refs., 8 figs., 1 tab.

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

    NASA Astrophysics Data System (ADS)

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

    2011-07-01

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

  5. Columnar and surface aerosol load over the Iberian Peninsula establishing annual cycles, trends, and relationships in five geographical sectors.

    PubMed

    Mateos, D; Cachorro, V E; Toledano, C; Burgos, M A; Bennouna, Y; Torres, B; Fuertes, D; González, R; Guirado, C; Calle, A; de Frutos, A M

    2015-06-15

    The study of atmospheric aerosol load over the Iberian Peninsula (IP) under a climatological perspective is accomplished by means of PM10 and AOD440 nm measurements from EMEP and AERONET networks, respectively, in the period 2000-2013. The PM10 annual cycles in five Iberian sectors show a main maximum in summer and a secondary maximum in spring, which is only observed in the southern area for the AOD climatology. The characteristics of PM10-AOD annual cycles of each geographical sector are explained by the different climatology of the air mass origins and their apportioning. The two magnitudes are correlated with a factor ranging between 20 and 90 depending on the sector. The temporal evolution of the aerosol load has shown a notable decrease in the IP since the 1980s. Statistically significant trends are obtained in the Northeastern sector with a reduction of 26% (period 1985-2000) for the total suspended particles, which continues for the PM10 data with a value of 35% per decade (2001-2013), and also in the whole column, 61% per decade in the AOD440 nm (2004-2013).

  6. Columnar and surface aerosol load over the Iberian Peninsula establishing annual cycles, trends, and relationships in five geographical sectors.

    PubMed

    Mateos, D; Cachorro, V E; Toledano, C; Burgos, M A; Bennouna, Y; Torres, B; Fuertes, D; González, R; Guirado, C; Calle, A; de Frutos, A M

    2015-06-15

    The study of atmospheric aerosol load over the Iberian Peninsula (IP) under a climatological perspective is accomplished by means of PM10 and AOD440 nm measurements from EMEP and AERONET networks, respectively, in the period 2000-2013. The PM10 annual cycles in five Iberian sectors show a main maximum in summer and a secondary maximum in spring, which is only observed in the southern area for the AOD climatology. The characteristics of PM10-AOD annual cycles of each geographical sector are explained by the different climatology of the air mass origins and their apportioning. The two magnitudes are correlated with a factor ranging between 20 and 90 depending on the sector. The temporal evolution of the aerosol load has shown a notable decrease in the IP since the 1980s. Statistically significant trends are obtained in the Northeastern sector with a reduction of 26% (period 1985-2000) for the total suspended particles, which continues for the PM10 data with a value of 35% per decade (2001-2013), and also in the whole column, 61% per decade in the AOD440 nm (2004-2013). PMID:25770951

  7. 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

  8. 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.

  9. 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

  10. Long-term visibility variation in Athens (1931-2013): a proxy for local and regional atmospheric aerosol loads

    NASA Astrophysics Data System (ADS)

    Founda, Dimitra; Kazadzis, Stelios; Mihalopoulos, Nikolaos; Gerasopoulos, Evangelos; Lianou, Maria; Raptis, Panagiotis I.

    2016-09-01

    This study explores the interdecadal variability and trends of surface horizontal visibility at the urban area of Athens from 1931 to 2013, using the historical archives of the National Observatory of Athens (NOA). A prominent deterioration of visibility in the city was detected, with the long-term linear trend amounting to -2.8 km decade-1 (p < 0.001), over the entire study period. This was not accompanied by any significant trend in relative humidity or precipitation over the same period. A slight recovery of visibility levels seems to be established in the recent decade (2004-2013). It was found that very good visibility (> 20 km) occurred at a frequency of 34 % before the 1950s, while this percentage drops to just 2 % during the decade 2004-2013. The rapid impairment of the visual air quality in Athens around the 1950s points to the increased levels of air pollution on a local and/or regional scale, related to high urbanization rates and/or increased anthropogenic emissions on a global scale at that period. Visibility was found to be negatively/positively correlated with relative humidity/wind speed, the correlation being statistically valid at certain periods. Wind regime and mainly wind direction and corresponding air mass origin were found to highly control visibility levels in Athens. The comparison of visibility variation in Athens and at a non-urban reference site on Crete island revealed similar negative trends over the common period of observations. This suggests that apart local sources, visibility in Athens is highly determined by aerosol load of regional origin. AVHRR and MODIS satellite-derived aerosol optical depth (AOD) retrievals over Athens and surface measurements of PM10 confirmed the relation of visibility to aerosol load.

  11. 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.

  12. Aerosol speciation and mass prediction from toluene oxidation under high NO x conditions

    NASA Astrophysics Data System (ADS)

    Kelly, Janya L.; Michelangeli, Diane V.; Makar, Paul A.; Hastie, Donald R.; Mozurkewich, Michael; Auld, Janeen

    2010-01-01

    A kinetically based gas-particle partitioning box model is used to highlight the importance of parameter representation in the prediction of secondary organic aerosol (SOA) formation following the photo-oxidation of toluene. The model is initialized using experimental data from York University's indoor smog chamber and provides a prediction of the total aerosol yield and speciation. A series of model sensitivity experiments were performed to study the aerosol speciation and mass prediction under high NO x conditions (VOC/NO x = 0.2). Sensitivity experiments indicate vapour pressure estimation to be a large area of weakness in predicting aerosol mass, creating an average total error range of 70 μg m -3 (range of 5-145 μg m -3), using two different estimation methods. Aerosol speciation proved relatively insensitive to changes in vapour pressure. One species, 3-methyl-6-nitro-catechol, dominated the aerosol phase regardless of the vapour pressure parameterization used and comprised 73-88% of the aerosol by mass. The dominance is associated with the large concentration of 3-methyl-6-nitro-catechol in the gas-phase. The high NO x initial conditions of this study suggests that the predominance of 3-methyl-6-nitro-catechol likely results from the cresol-forming branch in the Master Chemical Mechanism taking a significant role in secondary organic aerosol formation under high NO x conditions. Further research into the yields and speciation leading to this reaction product is recommended.

  13. 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.

  14. Mass loading of soil particles on plant surfaces

    SciTech Connect

    Pinder, J.E. III; McLeod, K.W. )

    1989-12-01

    Radionuclide-bearing soil particles on plant surfaces can be ingested and contribute to human dose, but evaluating the potential dose is limited by the relatively few data available on the masses of soil particles present on plant surfaces. This report summarizes mass loading data (i.e., mass of soil per unit of vegetation) for crops in the southeastern United States and compares these data to (1) those from other regions and (2) the mass loadings used in radionuclide transfer models to predict soil contamination of plant surfaces. Mass loadings were estimated using the 238Pu content of crops as an indicator of soil on plant surfaces. Crops were grown in two soils: a sandy clay loam soil and a loamy sand soil. Concentrations of soil on southeastern crops (i.e., mg soil g-1 plant) differed by more than a factor of 100 due to differences in crop growth form and biomass. Mean concentrations ranged from 1.7 mg g-1 for corn to 260 mg g-1 for lettuce. Differences in mass loadings between soils were less than those among crops. Concentrations differed by less than a factor of two between the two soil types. Because of (1) the differences among crops and (2) the limited data available from other systems, it is difficult to draw conclusions regarding regional or climatic variation in mass loadings. There is, however, little evidence to suggest large differences among regions. The mass loadings used to predict soil contamination in current radionuclide transfer models appear to be less than those observed for most crops.

  15. Heavy aerosol loading over the Bohai Bay as revealed by ground and satellite remote sensing

    NASA Astrophysics Data System (ADS)

    Zhang, Jinqiang; Chen, Jing; Xia, Xiangao; Che, Huizheng; Fan, Xuehua; Xie, Yiyang; Han, Zhiwei; Chen, Hongbin; Lu, Daren

    2016-01-01

    Heavy aerosol loading over the Bohai Bay, the innermost gulf of the Yellow Sea, was often recorded by the satellite observations. In order to understand aerosol optical properties and potential causes for the high aerosol loading there, a Cimel sunphotometer station (BH) was established on an offshore platform over the Bay for the first time in June 2012. The aerosol optical properties between July 2012 and July 2013 were employed to validate the satellite retrievals and to characterize temporal variability of aerosol optical properties. In particular, aerosol optical properties at BH were compared with those at Beijing (BJ), an urban station of the North China Plain (NCP), to discuss their potential difference during the same months of the same years. Mean aerosol optical depth at 550 nm (AOD) retrieved from the Moderate Resolution Imaging Spectroradiometer (MODIS) measurements over the Bohai Bay was 0.79 ± 0.68 during 2004-2013, that even exceeded value over the NCP (0.50 ± 0.57). This fact was supported by the comparison of ground-based remote sensing AODs at BH and BJ. The annual mean Cimel AOD at BH was 0.76 ± 0.62, which was larger than that at BJ (0.64 ± 0.52). The MODIS AOD difference between the Bohai Bay and the NCP was 0.29, being more than two times larger than the Cimel AOD difference between BH and BJ (0.12). This strongly implied that the MODIS retrievals had significant biases over the Bohai Bay that was likely due to sediment in the water and also sea ice in winter. A distinct seasonal variation of AOD was revealed over ocean. The maxima Cimel AOD was observed in summer (1.02 ± 0.75), which was followed by spring (0.86 ± 0.61), autumn (0.54 ± 0.41), and winter (0.39 ± 0.24); this was in good agreement with that over the NCP. High AOD over the Bohai Bay was associated with the heavy exhaust emissions from the ships across the Bay and transport of aerosols from the NCP. Furthermore, a much strong hygroscopic growth of fine mode aerosols over

  16. Buildup of Aerosol Loading over the Indian Ocean during the Monsoon Transition

    NASA Astrophysics Data System (ADS)

    Corrigan, C.; Ramanathan, V.; Schauer, J. J.; Carmichael, G.

    2005-12-01

    In recent years, black carbon has been recognized to significantly affect radiative forcing and global climate change. The Atmospheric Brown Cloud project (ABC-Asia) has focused on measuring the anthropogenic influence of aerosols, including black carbon, to determine the extent of sunlight dimming and radiative forcing over the Asian region. The first station in the ABC network is located in the Republic of Maldives, which is located in the Indian Ocean near the southern tip of India. The presence of black carbon over the Indian Ocean varies with the cyclic nature of the Asian-Australian Monsoon. Every 6 months, the winds change directions. From May to October, the wet season brings clean air into the region from the southern hemisphere. Conversely, the dry season brings polluted air from the Indian subcontinent and South East Asia from November thru April. As a result, the region becomes charged with black carbon and other anthropogenic pollutants during the dry season. During 2004, the transition between the clean and polluted seasons resulted in nearly a 10 fold increase of scattering and absorbing aerosols. The change occurred very abruptly over a period of a few days as air from India and South East Asia arrived in the Maldives at the surface level. The new, polluted aerosol was characteristically darker since the black carbon increased more substantially than the overall aerosol scattering. As a result, the single scatter albedo was reduced from an average of 0.98 to 0.92. In addition, aerosol particles were collected using filter samplers and the aerosol composition and mass were obtained. Observed results have been compared to the CFORS regional model and show good agreement for trends and concentrations.

  17. 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

  18. 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...

  19. Evidence for mass-loading of the Venus magnetosheath

    NASA Technical Reports Server (NTRS)

    Luhmann, J. G.; Russell, C. T.; Spreiter, J. R.; Stahara, S. S.

    1985-01-01

    The observed magnetic field configuration in the Venus magnetosheath contains information about the solar wind mass-loading processes occurring as a result of the extension of the neutral atmosphere into the magnetosheath. In this paper, magnetic field signatures of various mass-loading processes are discussed and experimental results from the Pioneer Venus Orbiter magnetometer experiment are examined for evidence of these signatures. The data suggest that the -V(bar)XB(bar) acceleration process, stochastic pickup of ionospheric ions, and J(bar)XB(bar) force 'scavenging' at the ionopause all occur at various times.

  20. Evidence for mass-loading of the Venus magnetosheath

    SciTech Connect

    Luhmann, J.G.; Russell, C.T.; Spreiter, J.R.; Stahara, S.S.

    1985-01-01

    The observed magnetic field configuration in the Venus magnetosheath contains information about the solar wind mass-loading processes occurring as a result of the extension of the neutral atmosphere into the magnetosheath. In this paper, magnetic field signatures of various mass-loading processes are discussed and experimental results from the Pioneer Venus Orbiter magnetometer experiment are examined for evidence of these signatures. The data suggest that the -V(bar)XB(bar) acceleration process, stochastic pickup of ionospheric ions, and J(bar)XB(bar) force scavenging at the ionopause all occur at various times. 16 references.

  1. 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.

  2. Mass Measurements of Saharan Dust Aerosols in Puerto Rico

    NASA Astrophysics Data System (ADS)

    Armstrong, R. A.; Jimenez, B.; Detres, Y.

    2003-12-01

    During the summer months, Saharan dust aerosols reach maximum values throughout the Caribbean Region. The respirable fraction of this dust, measured as PM 2.5, has the potential to induce regional health impacts, such as asthma and allergic reactions in sensitive individuals. Surface measurements of dust aerosols were obtained at Fajardo, on the northeastern corner of Puerto Rico, since November 2000. The PM 2.5 and PM 10 size fractions from the filter samples were related to satellite and sunphotometer measurements of aerosol optical depth before, during, and after Saharan dust events. In 2002, PM 2.5 ranged from 2.5 to 18.4 ug/m-3 while PM 10 ranged from 11 to 60 ug/m-3. The PM 2.5 fraction was approximately 25% of the PM 10. Saharan dust aerosols are also responsible for substantial heavy metal deposition in the tropical western Atlantic. In 2001, Iron increase from less than 4 mg/g during the first four months of the year, to a maximum of 24 mg/g in June, with relatively high values from May through September. An AVHRR 4-year climatology of aerosol optical depth for northeastern Puerto Rico shows a well-defined maximum peak during the last week of June and first week of July.

  3. OMI tropospheric NO2 air mass factors over South America: effects of biomass burning aerosols

    NASA Astrophysics Data System (ADS)

    Castellanos, P.; Boersma, K. F.; Torres, O.; de Haan, J. F.

    2015-03-01

    Biomass burning is an important and uncertain source of aerosols and NOx (NO + NO2) to the atmosphere. OMI observations of tropospheric NO2 are essential for characterizing this emissions source, but inaccuracies in the retrieval of NO2 tropospheric columns due to the radiative effects of aerosols, especially light-absorbing carbonaceous aerosols, are not well understood. It has been shown that the O2-O2 effective cloud fraction and pressure retrieval is sensitive to aerosol optical and physical properties, including aerosol optical depth (AOD). Aerosols implicitly influence the tropospheric air mass factor (AMF) calculations used in the NO2 retrieval through the effective cloud parameters used in the independent pixel approximation. In this work, we explicitly account for the effects of biomass burning aerosols in the tropospheric NO2 AMF calculation by including collocated aerosol extinction vertical profile observations from the CALIOP instrument, and aerosol optical depth (AOD) and single scattering albedo (SSA) retrieved by the OMI near-UV aerosol algorithm (OMAERUV) in the DISAMAR radiative transfer model for cloud-free scenes. Tropospheric AMFs calculated with DISAMAR were benchmarked against AMFs reported in the Dutch OMI NO2 (DOMINO) retrieval; the mean and standard deviation (SD) of the difference was 0.6 ± 8%. Averaged over three successive South American biomass burning seasons (2006-2008), the spatial correlation in the 500 nm AOD retrieved by OMI and the 532 nm AOD retrieved by CALIOP was 0.6, and 72% of the daily OMAERUV AOD observations were within 0.3 of the CALIOP observations. Overall, tropospheric AMFs calculated with observed aerosol parameters were on average 10% higher than AMFs calculated with effective cloud parameters. For effective cloud radiance fractions less than 30%, or effective cloud pressures greater than 800 hPa, the difference between tropospheric AMFs based on implicit and explicit aerosol parameters is on average 6 and 3

  4. The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation

    NASA Astrophysics Data System (ADS)

    Drinovec, L.; Močnik, G.; Zotter, P.; Prévôt, A. S. H.; Ruckstuhl, C.; Coz, E.; Rupakheti, M.; Sciare, J.; Müller, T.; Wiedensohler, A.; Hansen, A. D. A.

    2014-09-01

    Aerosol black carbon is a unique primary tracer for combustion emissions. It affects the optical properties of the atmosphere and is recognized as the second most important anthropogenic forcing agent for climate change. It is the primary tracer for adverse health effects caused by air pollution. For the accurate determination of mass equivalent black carbon concentrations in the air and for source apportionment of the concentrations, optical measurements by filter-based absorption photometers must take into account the "filter loading effect". We present a new real-time loading effect compensation algorithm based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer model AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier Aethalometer models, and other filter-based absorption photometers. The real-time loading effect compensation algorithm provides the high-quality data necessary for real-time source apportionment, and for determination of the temporal variation of the compensation parameter k.

  5. The "dual-spot" Aethalometer: an improved measurement of aerosol black carbon with real-time loading compensation

    NASA Astrophysics Data System (ADS)

    Drinovec, L.; Močnik, G.; Zotter, P.; Prévôt, A. S. H.; Ruckstuhl, C.; Coz, E.; Rupakheti, M.; Sciare, J.; Müller, T.; Wiedensohler, A.; Hansen, A. D. A.

    2015-05-01

    Aerosol black carbon is a unique primary tracer for combustion emissions. It affects the optical properties of the atmosphere and is recognized as the second most important anthropogenic forcing agent for climate change. It is the primary tracer for adverse health effects caused by air pollution. For the accurate determination of mass equivalent black carbon concentrations in the air and for source apportionment of the concentrations, optical measurements by filter-based absorption photometers must take into account the "filter loading effect". We present a new real-time loading effect compensation algorithm based on a two parallel spot measurement of optical absorption. This algorithm has been incorporated into the new Aethalometer model AE33. Intercomparison studies show excellent reproducibility of the AE33 measurements and very good agreement with post-processed data obtained using earlier Aethalometer models and other filter-based absorption photometers. The real-time loading effect compensation algorithm provides the high-quality data necessary for real-time source apportionment and for determination of the temporal variation of the compensation parameter k.

  6. 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.

  7. 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

  8. 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.

  9. Aerosol Organic Matter-Trace Metal Relationships Revealed by Ultra-High Resolution Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Wozniak, A. S.; Sleighter, R. L.; Morton, P. L.; Landing, W. M.; Shelley, R. U.; Hatcher, P. G.

    2011-12-01

    Atmospheric delivery of aerosols is important for the biogeochemical cycling of organic matter (OM) and trace elements in marine environments. Aerosols over marine environments can be derived from marine sources or transported from continental regions of variable vegetative cover and anthropogenic influence. These different sources are key determinants of aerosol OM composition, as well as trace metal amounts and characteristics. Dust-influenced aerosols typically contain higher amounts of Fe than anthropogenic-influenced aerosols but have lesser % of soluble Fe (%FeS), believed to be the bioavailable form of Fe for marine phytoplankton. Four samples from the 2008 GEOTRACES intercalibration experiments (Miami, FL, USA) were analyzed by electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and related to both air mass back trajectories and %FeS. Three samples showed aerosol sources from the east consistent with Saharan dust inputs, while the fourth sample was derived in part from air masses to the north, influenced by the North American continent. This North American-influenced sample was collected following the 3 day period with the highest %FeS (1.3-1.7%) of the 11 day intercalibration experiment (mean = 0.4-1.1%). FT-ICR mass spectra showed 795 peaks common to the dust-influenced samples but absent from the North American-influenced sample. These peaks were assigned molecular formulas characterized by CHO and CHON compounds with lower H/C and O/C ratios than the 1257 formulas common to all 4 samples, suggesting that the dust-influenced aerosols carry OM that is less oxygenated and more condensed in structure along with Fe of lesser solubility. Air mass trajectory analyses revealed samples collected during a 2010 cruise in the North Atlantic Ocean to be characterized by European-influenced (anthropogenic), African-influenced (dust), and primarily marine air masses, making them ideal for further exploration of the

  10. Size-resolved aerosol chemistry on Whistler Mountain, Canada with a High-Resolution Aerosol Mass Spectrometer during INTEX-B

    NASA Astrophysics Data System (ADS)

    Sun, Y.; Zhang, Q.; MacDonald, A. M.; Hayden, K.; Li, S. M.; Liggio, J.; Liu, P. S. K.; Anlauf, K. G.; Leaitch, W. R.; Cubison, M.; Worsnop, D.; van Donkelaar, A.; Martin, R. V.

    2008-12-01

    An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed at the peak of Whistler Mountain (elevation 2182 m-MSL), British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1) species (i.e., sulfate, nitrate, ammonium, chloride, and organics) were measured in situ every 5 min. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m-3) is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed a~large accumulation mode peaking around 500-600 nm in Dva while those of organic aerosol (OA) and nitrate peaked at ~300 nm. The size differences suggest that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC) of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C) of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral contents, the composition and characteristics of NR-PM1 were significantly different between them. One trans-Pacific event

  11. 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.

  12. 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

  13. Skeletal mass change as a function of gravitational loading

    NASA Technical Reports Server (NTRS)

    Pace, N.; Smith, A. H.; Rahlmann, D. F.

    1985-01-01

    The hypothesis that increased loading on an animal by chronic centrifugation results in an increase in skeletal mass was tested, using metabolically mature hamsters, rats, guinea pigs, Dutch rabbits and New Zealand rabbits representing a body mass range from 0.15 to 3.8 kg. Groups of 12 male animals of each species were subjeted to 2.0 g for 6 weeks on a 2.74 radius centrifuge with one degree of freedom. Subsequently, six of the animals were killed to measure whole body composition, while the rest comprised the control group, recovering for four weeks at 1.0 g prior to composition analysis. Results show a significant increase in bone mineral mass at 2.0 g. These centrifuge experiment results were then compared with the results of the USSR Cosmos Biosatellite experiment, whereby five rats experienced osteoporosis after 18.5 days of weightlessness. The opposing nature of effects that occurred at 0 g and 2.0 g is indicated schematically of particular interest is the fact that the bone mineral mass of the Cosmos 1129 flight rats was 17 pct less than that of the 1.0 g controls; whereas the bone mineral mass of the centrifuge rats was 18 pct greater than that of their 1.0 g controls. It is concluded that the bone mineral mass of the rat is directly proportional to gravitational loading over the range of 0 g to 2.0 g.

  14. 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

  15. Significant contributions of fungal spores to the organic carbon and to the aerosol mass balance of the urban atmospheric aerosol

    NASA Astrophysics Data System (ADS)

    Bauer, Heidi; Schueller, Elisabeth; Weinke, Gert; Berger, Anna; Hitzenberger, Regina; Marr, Iain L.; Puxbaum, Hans

    Fungal spores are ubiquitous components of atmospheric aerosols and are therefore also contributors to the organic carbon (OC) component and to the mass of PM 10 (PM—particulate matter) aerosols. In this study we use spore counts and an experimentally derived factor of 13 pg C and of 33 pg fresh weight per spore for assessing quantitatively the contribution to OC and PM 10. The concentrations of airborne fungal spores were determined at a suburban (Schafberg) and a traffic-dominated urban site (Rinnböckstrasse) in Vienna, Austria, during spring and summer. Fungal spores OC ranged from 22 to 677 ng m -3 with a summer mean value of around 350 ng m -3 at the suburban site and 300 ng m -3 at the urban traffic site. At the suburban site fungal spores contributed on average 6% in spring and 14% in summer to aerosol OC mass concentration. At the traffic-dominated site fungal spores accounted for 2% of OC in spring and for 8% in summer. The fungal contribution to PM 10 was also notable and amounted to 3% and 7% at the suburban and to 1% and 4% at the urban site in spring and summer, respectively. Impactor measurements of OC at the suburban site showed that in summer fungal spores were predominant contributors to the coarse aerosol OC, and accounted on average for 60% of the OC in the PM 2-10 fraction. Fungal spores thus can be regarded as main components to PM 10, total OC and, most importantly, coarse OC even in urban areas.

  16. Mass spectrometry of atmospheric aerosols--recent developments and applications. Part II: On-line mass spectrometry techniques.

    PubMed

    Pratt, Kerri A; Prather, Kimberly A

    2012-01-01

    Many of the significant advances in our understanding of atmospheric particles can be attributed to the application of mass spectrometry. Mass spectrometry provides high sensitivity with fast response time to probe chemically complex particles. This review focuses on recent developments and applications in the field of mass spectrometry of atmospheric aerosols. In Part II of this two-part review, we concentrate on real-time mass spectrometry techniques, which provide high time resolution for insight into brief events and diurnal changes while eliminating the potential artifacts acquired during long-term filter sampling. In particular, real-time mass spectrometry has been shown recently to provide the ability to probe the chemical composition of ambient individual particles <30 nm in diameter to further our understanding of how particles are formed through nucleation in the atmosphere. Further, transportable real-time mass spectrometry techniques are now used frequently on ground-, ship-, and aircraft-based studies around the globe to further our understanding of the spatial distribution of atmospheric aerosols. In addition, coupling aerosol mass spectrometry techniques with other measurements in series has allowed the in situ determination of chemically resolved particle effective density, refractive index, volatility, and cloud activation properties.

  17. The Io mass-loading disk: Model calculations

    NASA Astrophysics Data System (ADS)

    Wang, Yongli; Russell, Christopher T.; Raeder, Joachim

    2001-11-01

    The observations of ion cyclotron waves up to 0.5 RJ beyond the orbit of Io are best explained by the presence of a thin disk of fast neutrals whose ionization and pickup provide the free energy for the waves. We extend the model of Wilson and Schneider [1999] in order to explain the observed properties of this mass-loading region, especially the most recent Galileo observations near Io. In the extended model, some of the molecules of sulfur compounds in Io's exobase are first ionized by photoionization, impact ionization, and charge exchange. These charged particles are accelerated in the corotation electric field associated with the motion of the magnetized Io torus plasma that is moving through its exosphere. After a period of acceleration the heavy ions are neutralized by charge exchange with other exospheric neutral particles or combined with local electrons. These newly neutralized particles continue with high velocities similar to those of their former charged state, moving only under the influence of the gravity fields of Jupiter and Io, not affected by the electric and magnetic field. If they do not impact Io or its atmosphere, these neutral particles can propagate large distances across the magnetic field before they are reionized. Eventually, the reionized particles are lost by dissociation. Characteristic Io mass-loading particle distributions, such as high torus plasma density outside Io's orbit and the lower density inside, and the directional feature of the mass-loading neutral cloud, are qualitatively reproduced in the model. Meanwhile, the configuration of the mass-loading region, in which the ion cyclotron waves are observed, is obtained, and the results are consistent with Galileo wave observations. Three parameters are found to control the structure of the neutral and ion loading disks: the characteristic lifetimes of the initially created ions, of the neutral molecules, and of the ions generated by neutral particle reionization. In addition

  18. Rifapentine-loaded PLGA microparticles for tuberculosis inhaled therapy: Preparation and in vitro aerosol characterization.

    PubMed

    Parumasivam, Thaigarajan; Leung, Sharon S Y; Quan, Diana Huynh; Triccas, Jamie A; Britton, Warwick J; Chan, Hak-Kim

    2016-06-10

    Inhaled delivery of drugs incorporated into poly (lactic-co-glycolic acid) (PLGA) microparticles allows a sustained lung concentration and encourages phagocytosis by alveolar macrophages that harboring Mycobacterium tuberculosis. However, limited data are available on the effects of physicochemical properties of PLGA, including the monomer ratio (lactide:glycide) and molecular weight (MW) on the aerosol performance, macrophage uptake, and toxicity profile. The present study aims to address this knowledge gap, using PLGAs with monomer ratios of 50:50, 75:25 and 85:15, MW ranged 24 - 240kDa and an anti-tuberculosis (TB) drug, rifapentine. The PLGA-rifapentine powders were produced through a solution spray drying technique. The particles were spherical with a smooth surface and a volume median diameter around 2μm (span ~2). When the powders were dispersed using an Osmohaler(®) at 100L/min for 2.4s, the fine particle fraction (FPFtotal, wt.% particles in aerosol <5μm relative to the total recovered drug mass) was ranged between 52 and 57%, with no significant difference between the formulations. This result suggests that the monomer ratio and MW are not crucial parameters for the aerosol performance of PLGA. The phagocytosis analysis was performed using Thp-1 monocyte-derived macrophages. The highest rate of uptake was observed in PLGA 85:15 followed by 75:25 and 50:50 with about 90%, 80% and 70%, respectively phagocytosis over 4h of exposure. Furthermore, the cytotoxicity analysis on Thp-1 and human lung adenocarcinoma epithelial cells demonstrated that PLGA concentration up to 1.5mg/mL, regardless of the monomer composition and MW, were non-toxic. In conclusion, the monomer ratio and MW are not crucial in determining the aerosol performance and cytotoxicity profile of PLGA however, the particles with high lactide composition have a superior tendency for macrophage uptake. PMID:27049049

  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. 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

  1. In Situ Measurements of Aerosol Mass Concentration and Spectral Absorption in Xianghe, SE of Beijing, China

    NASA Astrophysics Data System (ADS)

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

    2005-12-01

    China's rapid industrialization over the last few decades has affected air quality in many regions of China, and even the regional climate. As a part of the EAST-AIRE (East Asian Study of Tropospheric Aerosols: an International Regional Experiment) study, Nuclepore filters were collected in two size ranges (PM10 and PM2.5) at 12 hour intervals since January 2005 at Xianghe, about 70 km southeast of Beijing. Each filter was analyzed for mass concentration, aerosol scattering and absorption efficiencies. Mass concentrations during the winter months (January-March) ranged from 9 to 459 μg/m3 in the coarse mode with an average concentration of 122 μg/m3, and from 11 to 203 μg/m3 in the fine mode with an average concentration of 45 μg/m3. While some of the extreme values are likely linked to local emissions, regional air pollution episodes also played important roles. Absorption efficiency measurements at 550 nm show very high values compared to measurements performed in the United States during the CLAMS experiment. 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 refractive indices from the several collected species and particle size effects. The absorption properties from aerosols measured in China show large absorption efficiencies, compared to aerosols measured in the US, possibly linked to different technology practices used in these countries. For organic plus black carbon aerosols, where the refractive index seems to be relatively constant, the absorption efficiency spectral dependence for fine mode aerosols falls between 1/λ and 1/λ2. The coarse mode absorption shows much less spectral dependence.

  2. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2015-10-01

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

  4. Organic compounds present in the natural Amazonian aerosol: Characterization by gas chromatography-mass spectrometry

    NASA Astrophysics Data System (ADS)

    Graham, Bim; Guyon, Pascal; Taylor, Philip E.; Artaxo, Paulo; Maenhaut, Willy; Glovsky, M. Michael; Flagan, Richard C.; Andreae, Meinrat O.

    2003-12-01

    As part of the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA)-Cooperative LBA Airborne Regional Experiment (CLAIRE) 2001 campaign in July 2001, separate day and nighttime aerosol samples were collected at a ground-based site in Amazonia, Brazil, in order to examine the composition and temporal variability of the natural "background" aerosol. We used a high-volume sampler to separate the aerosol into fine (aerodynamic diameter, AD < 2.5 μm) and coarse (AD > 2.5 μm) size fractions and quantified a range of organic compounds in methanolic extracts of the samples by a gas chromatographic-mass spectrometric technique. The carbon fraction of the compounds could account for an average of 7% of the organic carbon (OC) in both the fine and coarse aerosol fractions. We observed the highest concentrations of sugars, sugar alcohols, and fatty acids in the coarse aerosol samples, which suggests that these compounds are associated with primary biological aerosol particles (PBAP) observed in the forest atmosphere. Of these, trehalose, mannitol, arabitol, and the fatty acids were found to be more prevalent at night, coinciding with a nocturnal increase in PBAP in the 2-10 μm size range (predominantly yeasts and other small fungal spores). In contrast, glucose, fructose, and sucrose showed persistently higher daytime concentrations, coinciding with a daytime increase in large fungal spores, fern spores, pollen grains, and, to a lesser extent, plant fragments (generally >20 μm in diameter), probably driven by lowered relative humidity and enhanced wind speeds/convective activity during the day. For the fine aerosol samples a series of dicarboxylic and hydroxyacids were detected with persistently higher daytime concentrations, suggesting that photochemical production of a secondary organic aerosol from biogenic volatile organic compounds may have made a significant contribution to the fine aerosol. Anhydrosugars (levoglucosan, mannosan, galactosan), which are

  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.

    2015-09-01

    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

  6. 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

  7. Measurements of skylight polarization: a case study in urban region with high-loading aerosol.

    PubMed

    Wu, Lianghai; Gao, Jun; Fan, Zhiguo; Zhang, Jun

    2015-02-01

    We investigate skylight polarization patterns in an urban region using our developed full-Stokes imaging polarimeter. A detailed description of our imaging polarimeter and its calibration are given, then, we measure skylight polarization patterns at wavelength λ=488  nm and at solar elevation between -05°10' and +35°42' in the city of Hefei, China. We show that in an urban region with high-loading aerosols: (1) the measured degree of linear polarization reaches the maximum near sunset, and large areas of unpolarized sky exist in the forward sunlight direction close to the Sun; (2) the position of neural points shifts from the local meridian plane and, if compared with a clear sky, alters the symmetrical characteristics of celestial polarization pattern; and (3) the observed circular polarization component is negligible. PMID:25967834

  8. Stratifying Tropical Fires by Land Cover: Insights into Amazonian Fires, Aerosol Loading, and Regional Deforestation

    NASA Technical Reports Server (NTRS)

    TenHoeve, J. E.; Remer, L. A.; Jacobson, M. Z.

    2010-01-01

    This study analyzes changes in the number of fires detected on forest, grass, and transition lands during the 2002-2009 biomass burning seasons using fire detection data and co-located land cover classifications from the Moderate Resolution Imaging Spectroradiometer (MODIS). We find that the total number of detected fires correlates well with MODIS mean aerosol optical depth (AOD) from year to year, in accord with other studies. However, we also show that the ratio of forest to savanna fires varies substantially from year to year. Forest fires have trended downward, on average, since the beginning of 2006 despite a modest increase in 2007. Our study suggests that high particulate matter loading detected in 2007 was likely due to a large number of savanna/agricultural fires that year. Finally, we illustrate that the correlation between annual Brazilian deforestation estimates and MODIS fires is considerably higher when fires are stratified by MODIS-derived land cover classifications.

  9. Development and characterization of an aircraft aerosol time-of-flight mass spectrometer.

    PubMed

    Pratt, Kerri A; Mayer, Joseph E; Holecek, John C; Moffet, Ryan C; Sanchez, Rene O; Rebotier, Thomas P; Furutani, Hiroshi; Gonin, Marc; Fuhrer, Katrin; Su, Yongxuan; Guazzotti, Sergio; Prather, Kimberly A

    2009-03-01

    Vertical and horizontal profiles of atmospheric aerosols are necessary for understanding the impact of air pollution on regional and global climate. To gain further insight into the size-resolved chemistry of individual atmospheric particles, a smaller aerosol time-of-flight mass spectrometer (ATOFMS) with increased data acquisition capabilities was developed for aircraft-based studies. Compared to previous ATOFMS systems, the new instrument has a faster data acquisition rate with improved ion transmission and mass resolution, as well as reduced physical size and power consumption, all required advances for use in aircraft studies. In addition, real-time source apportionment software allows the immediate identification and classification of individual particles to guide sampling decisions while in the field. The aircraft (A)-ATOFMS was field-tested on the ground during the Study of Organic Aerosols in Riverside, CA (SOAR) and aboard an aircraft during the Ice in Clouds Experiment-Layer Clouds (ICE-L). Initial results from ICE-L represent the first reported aircraft-based single-particle dual-polarity mass spectrometry measurements and provide an increased understanding of particle mixing state as a function of altitude. Improved ion transmission allows for the first single-particle detection of species out to approximately m/z 2000, an important mass range for the detection of biological aerosols and oligomeric species. In addition, high time resolution measurements of single-particle mixing state are demonstrated and shown to be important for airborne studies where particle concentrations and chemistry vary rapidly.

  10. 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...

  11. 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.

  12. 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

  13. 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.

  14. 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

  15. OMI tropospheric NO2 air mass factors over South America: effects of biomass burning aerosols

    NASA Astrophysics Data System (ADS)

    Castellanos, P.; Boersma, K. F.; Torres, O.; de Haan, J. F.

    2015-09-01

    Biomass burning is an important and uncertain source of aerosols and NOx (NO + NO2) to the atmosphere. Satellite observations of tropospheric NO2 are essential for characterizing this emissions source, but inaccuracies in the retrieval of NO2 tropospheric columns due to the radiative effects of aerosols, especially light-absorbing carbonaceous aerosols, are not well understood. It has been shown that the O2-O2 effective cloud fraction and pressure retrieval is sensitive to aerosol optical and physical properties, including aerosol optical depth (AOD). Aerosols implicitly influence the tropospheric air mass factor (AMF) calculations used in the NO2 retrieval through the effective cloud parameters used in the independent pixel approximation. In this work, we explicitly account for the effects of biomass burning aerosols in the Ozone Monitoring Instrument (OMI) tropospheric NO2 AMF calculation for cloud-free scenes. We do so by including collocated aerosol extinction vertical profile observations from the CALIOP instrument, and aerosol optical depth (AOD) and single scattering albedo (SSA) retrieved by the OMI near-UV aerosol algorithm (OMAERUV) in the DISAMAR radiative transfer model. Tropospheric AMFs calculated with DISAMAR were benchmarked against AMFs reported in the Dutch OMI NO2 (DOMINO) retrieval; the mean and standard deviation of the difference was 0.6 ± 8 %. Averaged over three successive South American biomass burning seasons (2006-2008), the spatial correlation in the 500 nm AOD retrieved by OMI and the 532 nm AOD retrieved by CALIOP was 0.6, and 68 % of the daily OMAERUV AOD observations were within 30 % of the CALIOP observations. Overall, tropospheric AMFs calculated with observed aerosol parameters were on average 10 % higher than AMFs calculated with effective cloud parameters. For effective cloud radiance fractions less than 30 %, or effective cloud pressures greater than 800 hPa, the difference between tropospheric AMFs based on implicit and

  16. Mass Loading at the Magnetopause through the Plasmaspheric Plume

    NASA Astrophysics Data System (ADS)

    Wang, Y.; Tu, J.; Song, P.

    2015-12-01

    An investigation of the transport of the plasmaspheric plasma to the dayside magnetopause through plasmaspheric plumes under disturbed geomagnetic conditions is conducted by numerical simulations using the Dynamic Fluid-Kinetic (DyFK) model. The simulation calculates the field-aligned density distributions of multiple ion species (H+/He+/O+) in a plasmaspheric flux tube that corotates while convecting toward the dayside magnetopause. When the convection is enhanced, a plasmaspheric plume is formed and plasmaspheric plasma mass loads to the dayside magnetopause. The effect of wave-particle interactions on the density distributions is also studied.

  17. 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

  18. 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.

  19. 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.

  20. Estimating nutrient loadings using chemical mass balance approach.

    PubMed

    Jain, C K; Singhal, D C; Sharma, M K

    2007-11-01

    The river Hindon is one of the important tributaries of river Yamuna in western Uttar Pradesh (India) and carries pollution loads from various municipal and industrial units and surrounding agricultural areas. The main sources of pollution in the river include municipal wastes from Saharanpur, Muzaffarnagar and Ghaziabad urban areas and industrial effluents of sugar, pulp and paper, distilleries and other miscellaneous industries through tributaries as well as direct inputs. In this paper, chemical mass balance approach has been used to assess the contribution from non-point sources of pollution to the river. The river system has been divided into three stretches depending on the land use pattern. The contribution of point sources in the upper and lower stretches are 95 and 81% respectively of the total flow of the river while there is no point source input in the middle stretch. Mass balance calculations indicate that contribution of nitrate and phosphate from non-point sources amounts to 15.5 and 6.9% in the upper stretch and 13.1 and 16.6% in the lower stretch respectively. Observed differences in the load along the river may be attributed to uncharacterized sources of pollution due to agricultural activities, remobilization from or entrainment of contaminated bottom sediments, ground water contribution or a combination of these sources. PMID:17616829

  1. Estimating nutrient loadings using chemical mass balance approach.

    PubMed

    Jain, C K; Singhal, D C; Sharma, M K

    2007-11-01

    The river Hindon is one of the important tributaries of river Yamuna in western Uttar Pradesh (India) and carries pollution loads from various municipal and industrial units and surrounding agricultural areas. The main sources of pollution in the river include municipal wastes from Saharanpur, Muzaffarnagar and Ghaziabad urban areas and industrial effluents of sugar, pulp and paper, distilleries and other miscellaneous industries through tributaries as well as direct inputs. In this paper, chemical mass balance approach has been used to assess the contribution from non-point sources of pollution to the river. The river system has been divided into three stretches depending on the land use pattern. The contribution of point sources in the upper and lower stretches are 95 and 81% respectively of the total flow of the river while there is no point source input in the middle stretch. Mass balance calculations indicate that contribution of nitrate and phosphate from non-point sources amounts to 15.5 and 6.9% in the upper stretch and 13.1 and 16.6% in the lower stretch respectively. Observed differences in the load along the river may be attributed to uncharacterized sources of pollution due to agricultural activities, remobilization from or entrainment of contaminated bottom sediments, ground water contribution or a combination of these sources.

  2. Characterization of events by aerosol mass size distributions.

    PubMed

    Nicolás, José; Yubero, Eduardo; Galindo, Nuria; Giménez, Joaquín; Castañer, Ramón; Carratalá, Adoración; Crespo, Javier; Pastor, Carlos

    2009-02-01

    Continuous measurements of particle mass size distributions were carried out in summer 2004 at an urban location in the western Mediterranean using an optical particle counter. In this work we propose a simple methodology to identify PM episodes and determine their influence on mass size distributions. During the study period three types of event produced a significant increase in TSP daily levels: Saharan dust intrusions, firework displays and strong winds, modifying size distributions in different ways. As well, a traffic-related mass size spectrum was obtained showing road dust particles injected into the atmosphere by vehicle-induced resuspension having mainly aerodynamic diameters between 5 and 15 microm. This was confirmed by principal component and conditional probability function analyses.

  3. Aerosolized Antimicrobial Agents Based on Degradable Dextran Nanoparticles Loaded with Silver Carbene Complexes

    PubMed Central

    Ornelas-Megiatto, Cátia; Shah, Parth N.; Wich, Peter R.; Cohen, Jessica L.; Tagaev, Jasur A.; Smolen, Justin A.; Wright, Brian D.; Panzner, Matthew J.; Youngs, Wiley J.; Fréchet, Jean M. J.; Cannon, Carolyn L.

    2012-01-01

    Degradable acetalated dextran (Ac-DEX) nanoparticles were prepared and loaded with a hydrophobic silver carbene complex (SCC) by a single-emulsion process. The resulting particles were characterized for morphology and size distribution using scanning electron microscopy (SEM), transmission electron microscopy (TEM), and dynamic light scattering (DLS). The average particle size and particle size distribution were found to be a function of the ratio of the organic phase to the surfactant containing aqueous phase with a 1:5 volume ratio of Ac-DEX CH2Cl2 (organic): PBS (aqueous) being optimal for the formulation of nanoparticles with an average size of 100 ± 40 nm and a low polydispersity. The SCC loading was found to increase with an increase in the SCC quantity in the initial feed used during particle formulation up to 30% (w/w); however, the encapsulation efficiency was observed to be the best at a feed ratio of 20% (w/w). In vitro efficacy testing of the SCC loaded Ac-DEX nanoparticles demonstrated their activity against both Gram-negative and Gram-positive bacteria; the nanoparticles inhibited the growth of every bacterial species tested. As expected, a higher concentration of drug was required to inhibit bacterial growth when the drug was encapsulated within the nanoparticle formulations compared with the free drug illustrating the desired depot release. Compared with free drug, the Ac-DEX nanoparticles were much more readily suspended in an aqueous phase and subsequently aerosolized, thus providing an effective method of pulmonary drug delivery. PMID:23025592

  4. Three-dimensional factorization of size-resolved organic aerosol mass spectra from Mexico City

    NASA Astrophysics Data System (ADS)

    Ulbrich, I. M.; Canagaratna, M. R.; Cubison, M. J.; Zhang, Q.; Ng, N. L.; Aiken, A. C.; Jimenez, J. L.

    2011-07-01

    A size-resolved submicron organic aerosol composition dataset from a high-resolution time-of-flight mass spectrometer (HR-ToF-AMS) collected in Mexico City during the MILAGRO campaign in March 2006 is analyzed using 3-dimensional (3-D) factorization models. A method for estimating the precision of the size-resolved composition data for use with the factorization models is presented here for the first time. Two 3-D models are applied to the dataset. One model is a 3-vector decomposition (PARAFAC model), which assumes that each chemical component has a constant size distribution over all time steps. The second model is a vector-matrix decomposition (Tucker 1 model) that allows a chemical component to have a size distribution that varies in time. To our knowledge, this is the first report of an application of 3-D factorization models to data from fast aerosol instrumentation; it is also the first application of this vector-matrix model to any ambient aerosol dataset. A larger number of degrees of freedom in the vector-matrix model enable fitting real variations in factor size distributions, but also make the model susceptible to fitting noise in the dataset, giving some unphysical results. For this dataset and model, more physical results were obtained by partially constraining the factor mass spectra using a priori information and a new regularization method. We find four factors with each model: hydrocarbon-like organic aerosol (HOA), biomass-burning organic aerosol (BBOA), oxidized organic aerosol (OOA), and a locally occurring organic aerosol (LOA). These four factors have previously been reported from 2-dimensional factor analysis of the high-resolution mass spectral dataset from this study. The size distributions of these four factors are consistent with previous reports for these particle types. Both 3-D models produce useful results, but the vector-matrix model captures real variability in the size distributions that cannot be captured by the 3-vector model. A

  5. Three-dimensional factorization of size-resolved organic aerosol mass spectra from Mexico City

    NASA Astrophysics Data System (ADS)

    Ulbrich, I. M.; Canagaratna, M. R.; Cubison, M. J.; Zhang, Q.; Ng, N. L.; Aiken, A. C.; Jimenez, J. L.

    2012-01-01

    A size-resolved submicron organic aerosol composition dataset from a high-resolution time-of-flight mass spectrometer (HR-ToF-AMS) collected in Mexico City during the MILAGRO campaign in March 2006 is analyzed using 3-dimensional (3-D) factorization models. A method for estimating the precision of the size-resolved composition data for use with the factorization models is presented here for the first time. Two 3-D models are applied to the dataset. One model is a 3-vector decomposition (PARAFAC model), which assumes that each chemical component has a constant size distribution over all time steps. The second model is a vector-matrix decomposition (Tucker 1 model) that allows a chemical component to have a size distribution that varies in time. To our knowledge, this is the first report of an application of 3-D factorization models to data from fast aerosol instrumentation, and the first application of this vector-matrix model to any ambient aerosol dataset. A larger number of degrees of freedom in the vector-matrix model enable fitting real variations in factor size distributions, but also make the model susceptible to fitting noise in the dataset, giving some unphysical results. For this dataset and model, more physically meaningful results were obtained by partially constraining the factor mass spectra using a priori information and a new regularization method. We find four factors with each model: hydrocarbon-like organic aerosol (HOA), biomass-burning organic aerosol (BBOA), oxidized organic aerosol (OOA), and a locally occurring organic aerosol (LOA). These four factors have previously been reported from 2-dimensional factor analysis of the high-resolution mass spectral dataset from this study. The size distributions of these four factors are consistent with previous reports for these particle types. Both 3-D models produce useful results, but the vector-matrix model captures real variability in the size distributions that cannot be captured by the 3-vector

  6. 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

  7. Mass spectra deconvolution of low, medium, and high volatility biogenic secondary organic aerosol.

    PubMed

    Kostenidou, Evangelia; Lee, Byong-Hyoek; Engelhart, Gabriella J; Pierce, Jeffrey R; Pandis, Spyros N

    2009-07-01

    Secondary organic aerosol (SOA) consists of compounds with a wide range of volatilities and its ambient concentration is sensitive to this volatility distribution. Recent field studies have shown that the typical mass spectrum of ambient oxygenated organic aerosol (OOA) as measured by the Aerodyne Aerosol Mass Spectrometer (AMS) is quite different from the SOA mass spectra reported in smog chamber experiments. Part of this discrepancy is due to the dependence of SOA composition on the organic aerosol concentration. High precursor concentrations lead to higher concentrations of the more volatile species in the produced SOA while at lower concentrations the less volatile compounds dominate the SOA composition. alpha-Pinene, beta-pinene, d-limonene, and beta-caryophyllene ozonolysis experiments were performed at moderate concentration levels. Using a thermodenuder the more volatile SOA species were removed achieving even lower SOA concentration. The less volatile fraction was then chemically characterized by an AMS. The signal fraction of m/z44, and thus the concentration of C02+, is significantly higher for the less volatile SOA. High NO(x) conditions result in less oxidized SOA than low NO(x) conditions, while increasing relative humidity levels results in more oxidized products for limonene but has little effect on alpha-and beta-pinene SOA. Combining a smog chamber with a thermodenuder model employing the volatility basis-set framework, the AMS SOA mass spectrum for each experiment and for each precursor is deconvoluted into low, medium, and high volatility component mass spectra. The spectrum of the surrogate component with the lower volatility is quite similar to that of ambient OOA.

  8. 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

  9. 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

  10. 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.

  11. Extremely large anthropogenic-aerosol contribution to total aerosol load over the Bay of Bengal during winter season

    NASA Astrophysics Data System (ADS)

    Kaskaoutis, D. G.; Kharol, S. Kumar; Sinha, P. R.; Singh, R. P.; Kambezidis, H. D.; Rani Sharma, A.; Badarinath, K. V. S.

    2011-07-01

    Ship-borne observations of spectral aerosol optical depth (AOD) have been carried out over the entire Bay of Bengal (BoB) as part of the W-ICARB cruise campaign during the period 27 December 2008-30 January 2009. The results reveal a pronounced temporal and spatial variability in the optical characteristics of aerosols mainly due to anthropogenic emissions and their dispersion controlled by local meteorology. The highest aerosol amount, with mean AOD500>0.4, being even above 1.0 on specific days, is found close to the coastal regions in the western and northern parts of BoB. In these regions the Ångström exponent is also found to be high (~1.2-1.25) indicating transport of strong anthropogenic emissions from continental regions, while very high AOD500 (0.39±0.07) and α380-870 values (1.27±0.09) are found over the eastern BoB. Except from the large α380-870 values, an indication of strong fine-mode dominance is also observed from the AOD curvature, which is negative in the vast majority of the cases, suggesting dominance of an anthropogenic-pollution aerosol type. On the other hand, clean maritime conditions are rather rare over the region, while the aerosol types are further examined through a classification scheme based on the relationship between α and dα. It was found that even for the same α values the fine-mode dominance is larger for higher AODs showing the strong continental influence over the marine environment of BoB. Furthermore, there is also an evidence of aerosol-size growth under more turbid conditions indicative of coagulation and/or humidification over specific BoB regions. The results obtained using OPAC model show significant fraction of soot aerosols (~6 %-8 %) over the eastern and northwestern BoB, while coarse-mode sea salt particles are found to dominate in the southern parts of BoB.

  12. 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.

  13. 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.

  14. The Development of Electrostatic Precipitation-Electrospray Ionization Mass Spectrometry (EP-ESI-MS) for Atmospheric Aerosol Analysis

    NASA Astrophysics Data System (ADS)

    He, S.; Hogan, C. J., Jr.; Naqwi, A.; Gross, D. S.; Li, L.; Duan, H.; Jiang, L.; Flowers, J.; Grubb, E.; Au, L.

    2015-12-01

    Chemical composition analysis of atmospheric aerosols is of considerable interest and has been facilitated by mass spectrometry. Electrospray ionization (ESI) is a suitable mode of ion generation of many organic species comprising aerosol particles, as it leads to minimal analyte fragmentation. However, particles exist in the atmosphere at mass concentrations of the order 10 μg/m3 or less in many environments and are highly heterogeneous; low concentrations and chemical complexity have limited ESI application in aerosol analysis. In this presentation, the development of an approach to apply ESI to molecules within submicrometer and nanometer scale aerosol particles is discussed. The technique, which we term electrostatic precipitation-ESI-MS (EP-ESI-MS), utilizes unipolar ionization to charge particles, electrostatic precipitation to collect particles on the tip of a tungsten rod, and subsequently, by flowing liquid over the rod, ESI and mass analysis of dissolved species originating from the collected particles. EP-ESI-MS is shown to enable analysis of nanogram quantities of collected inorganic and organic components. Furthermore, it is coupled with a tandem mass spectrometry and challenged with oxidation products of α-pinene to investigate its capability of enabling structure analysis of complex organic compounds in aerosol particles. With EP-ESI-MS, the identification of chemical components in aerosol particles is realized and the integrated mass spectrometric signals are found to be a monotonic function of the analyte mass concentration in the aerosol phase. Additionally, it is shown to have a dynamic range of 5 orders of magnitude in mass, making it suitable for molecular analysis of aerosol particles in laboratory settings, as well as analysis of atmospheric aerosols in ambient air.

  15. 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.

  16. Submicron particles at Thompson Farm during ICARTT measured using aerosol mass spectrometry

    NASA Astrophysics Data System (ADS)

    Cottrell, Laura D.; Griffin, Robert J.; Jimenez, Jose L.; Zhang, Qi; Ulbrich, Ingrid; Ziemba, Luke D.; Beckman, Pieter J.; Sive, Barkley C.; Talbot, Robert W.

    2008-04-01

    The composition and size of aerosols were measured using an Aerodyne quadrupole aerosol mass spectrometer at Thompson Farm in Durham, NH, during the International Consortium for Atmospheric Research on Transport and Transformation campaign during summer 2004. Submicron, non-refractory aerosol was dominated by organic matter and sulfate (averages of 5.7 μg m-3 and 3.6 μg m-3, respectively), with smaller contributions from nitrate and ammonium (averages of 0.3 μg m-3 and 1.02 μg m-3, respectively). Organic aerosol (OA) mass correlates well with anthropogenic tracers such as carbon monoxide (CO, R2 = 0.58) and black carbon (R2 = 0.59), but multiple analyses indicate possible contributions from primary, secondary, anthropogenic, and biogenic OA. Multivariate statistical analysis of the OA mass spectra indicates the presence of two types of oxygenated OA (OOA) and a hydrocarbon-like OA (HOA) component that also contains contributions from biomass burning OA (BBOA). On average, the HOA/BBOA component accounts for 21% of the total OA mass while the two OOA components account for 24% and 55%, respectively, of the OA burden. Observed nitrate correlates well with OA (R2 = 0.67), suggesting interference, the presence of organic nitrates, processing/uptake of nitric acid by OA, or other temporally coincident processes because of the ammonia-poor environment with respect to sulfate. The relative increase of OA with respect to background compared to that of CO (average of 72.7 μg m-3 ppmv-1) indicates values that are higher than those based on previous measurements in New England.

  17. In situ measurements of aerosol mass concentration and radiative properties in Xianghe, southeast of Beijing

    NASA Astrophysics Data System (ADS)

    Chaudhry, Zahra; Martins, J. Vanderlei; Li, Zhanqing; Tsay, Si-Chee; Chen, Hongbin; Wang, Pucai; Wen, Tianxue; Li, Can; Dickerson, Russell R.

    2007-12-01

    As a part of the EAST-AIRE study, Nuclepore filters were collected in two size ranges (coarse, 2.5 μm < d < 10 μm, and fine, d < 2.5 μm) from January to May 2005 in Xianghe, about 70 km southeast of Beijing, and analyzed for aerosol mass concentration, spectral absorption efficiency and absorption coefficient. Twelve-hour aerosol mass concentration measurements showed an average concentration of 120 μg/m3 in the coarse mode and an average concentration of 25 μg/m3 in the fine mode. To determine how representative ground-based measurements are of the total column, the mass concentration data was compared with AERONET AOT at 500 nm and AERONET size distribution data. The vertical distribution of the aerosols were studied with a micropulse lidar and in the cases where the vertical column was found to be fairly homogenous, the comparisons of the filter results with AERONET agreed favorably, while in the cases of inhomogeneity, the comparisons have larger disagreement. For fine mode aerosols, the average spectral absorption efficiency equates well to a λ-1 model, while the coarse mode shows a much flatter spectral dependence, consistent with large particle models. The coarse mode absorption efficiency was compatible with that of the fine mode in the NIR region, indicating the much stronger absorption of the coarse mode due to its composition and sizable mass. Single scattering albedo results are presented from a combination between absorption coefficients derived from the filter measurements, from a PSAP and from a three-wavelength Nephelometer.

  18. 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.

  19. 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.

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

    NASA Astrophysics Data System (ADS)

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

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

  1. 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.

  2. 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.

  3. 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

  4. 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).

  5. 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

  6. 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.

  7. Measuring Bipolar Charge and Mass Distributions of Powder Aerosols by a Novel Tool (BOLAR).

    PubMed

    Wong, Jennifer; Lin, Yu-Wei; Kwok, Philip Chi Lip; Niemelä, Ville; Crapper, John; Chan, Hak-Kim

    2015-09-01

    The Bipolar Charge Analyzer (BOLAR) was evaluated for measuring bipolar electrostatic charge and mass distributions of powder aerosols generated from a dry powder inhaler. Mannitol powder (5, 10, and 20 mg) was dispersed using an Osmohaler inhaler into the BOLAR at air flow rates of 30 or 60 L/min. As the aerosol sample was drawn through the BOLAR, the air flow was divided into six equal fractions. Five of them entered individual detection tubes with a defined cutoff diameter in the range of 0.95 to 16.36 μm (depending on the flow rate) and the remaining (i.e., the sixth) fraction passed through a reference chamber. The aerosols that entered the detection tubes were separated according to the particle charge polarity (positive, negative, or neutral) and charge was measured by separate electrometers. The deposited powder of a single actuation from the inhaler was chemically assayed using high performance liquid chromatography. Additionally, the aerosol measurements were conducted on a modified Classic Electrical Low Pressure Impactor (ELPI) for comparison of the net specific charge per size fraction. Spray-dried mannitol carried significantly different positively and negatively charged particles in each of the five defined particle size fractions. The charge-to-mass ratio (q/m) of positively charged particles ranged from +1.11 to +32.57 pC/μg and negatively charged particles ranged from -1.39 to -9.25 pC/μg, resulting in a net q/m of -3.08 to +13.34 pC/μg. The net q/m values obtained on the modified ELPI ranged from -5.18 to +4.81 pC/μg, which were comparable to the BOLAR measurements. This is the first full report to utilize the BOLAR to measure bipolar charge and mass distributions of a powder aerosol. Positively and negatively charged particles were observed within each size fraction, and their corresponding q/m profiles were successfully characterized. Despite some potential drawbacks, the BOLAR has provided a new platform for investigating bipolar charge

  8. Mass balance of organic carbon fractions in atmospheric aerosols

    NASA Astrophysics Data System (ADS)

    Alves, CéLia; Carvalho, Abel; Pio, Casimiro

    2002-11-01

    Total suspended particulate matter was collected in two Portuguese urban areas (Lisbon and Aveiro) and in a Finnish forested site. Samples were sequentially extracted with dichloromethane and water. The solvent extract was separated by flash chromatography into aliphatics, aromatics, carbonyls, alcohols, and an acidic fraction, and analyzed by gas chromatography-mass spectrometry. An organic/black carbon analyzer was used to evaluate the carbonaceous matter in filters, the water-soluble fraction, solvent extractable material, and the content of different organic classes. Results showed that the common simple extraction with dichloromethane is able to dissolve less than 50% of the particulate organic material. The successive extraction with water removes an important quantity of the leftover organic polar compounds. The sum of both extractions recovers between 70% and 90% of the organic carbon present. The amount of oxygenated compounds is frequently more than 70% of the extracted material, with a large predominance of organic acids and alcohols, especially for particles with diameters less than 0.49 μm. The organic compounds identified in the extractable atmospheric particulate matter are represented by primary compounds with both anthropogenic and biogenic origin, which mainly derive from vegetation waxes and from petrogenic sources. Secondary products resulting from the oxidation of volatile organic compounds were also detected. The water-soluble fraction contains essentially oxocarboxylic and dicarboxylic acids, and cellulosic constituents. In accordance with the anthropogenic characteristics of the sampling sites, nonpolar fractions constitute up to 24% of the extracted organic carbon in Lisbon and present high levels of petroleum markers, while in the forested station these compounds represent 8%. The oxygenated organic compounds account for 76-92% of the extracted carbon in samples from Aveiro and Finland. Owing to favorable photochemical conditions during

  9. Evolution of aerosol loading in Santiago de Chile between 1997 and 2014

    NASA Astrophysics Data System (ADS)

    Pistone, Kristina; Gallardo, Laura

    2015-04-01

    While aerosols produced by major cities are a significant component of anthropogenic climate forcing as well as an important factor in public health, many South American cities have not been a major focus of aerosol studies due in part to relatively few long-term observations in the region. Here we present a synthesis of the available data for the emerging megacity of Santiago, Chile. We report new results from a recent NASA AERONET (AErosol RObotic NETwork) site in the Santiago basin, combining these with previous AERONET observations in Santiago as well as with a new assessment of the 11-station air quality monitoring network currently administered by the Chilean Environment Ministry (MMA, Ministerio del Medio Ambiente) to assess changes in aerosol composition since 1997. While the average surface concentration of pollution components (specifically PM2.5 and PM10) has decreased, no significant change in total aerosol optical depth was observed. However, changes in aerosol size and composition are suggested by the proxy measurements. Previous studies have revealed limitations in purely satellite-based studies over Santiago due to biases from high surface reflection in the region, particularly in summer months (e.g. Escribano et al 2014). To overcome this difficulty and certain limitations in the air quality data, we next incorporate analysis of aerosol products from the Multi-angle Imaging SpectroRadiometer (MISR) instrument along with those from the Moderate Resolution Imaging Spectroradiometer (MODIS) instrument, both on NASA's Terra satellite, to better quantify the high bias of MODIS. Thus incorporating these complementary datasets, we characterize the aerosol over Santiago over the period 1997 to 2014, including the evolution of aerosol properties over time and seasonal dependencies in the observed trends. References: Escribano et al (2014), "Satellite Retrievals of Aerosol Optical Depth over a Subtropical Urban Area: The Role of Stratification and Surface

  10. Molecular composition of organic aerosols in central Amazonia: an ultra-high-resolution mass spectrometry study

    NASA Astrophysics Data System (ADS)

    Kourtchev, Ivan; Godoi, Ricardo H. M.; Connors, Sarah; Levine, James G.; Archibald, Alex T.; Godoi, Ana F. L.; Paralovo, Sarah L.; Barbosa, Cybelli G. G.; Souza, Rodrigo A. F.; Manzi, Antonio O.; Seco, Roger; Sjostedt, Steve; Park, Jeong-Hoo; Guenther, Alex; Kim, Saewung; Smith, James; Martin, Scot T.; Kalberer, Markus

    2016-09-01

    The Amazon Basin plays key role in atmospheric chemistry, biodiversity and climate change. In this study we applied nanoelectrospray (nanoESI) ultra-high-resolution mass spectrometry (UHRMS) for the analysis of the organic fraction of PM2.5 aerosol samples collected during dry and wet seasons at a site in central Amazonia receiving background air masses, biomass burning and urban pollution. Comprehensive mass spectral data evaluation methods (e.g. Kendrick mass defect, Van Krevelen diagrams, carbon oxidation state and aromaticity equivalent) were used to identify compound classes and mass distributions of the detected species. Nitrogen- and/or sulfur-containing organic species contributed up to 60 % of the total identified number of formulae. A large number of molecular formulae in organic aerosol (OA) were attributed to later-generation nitrogen- and sulfur-containing oxidation products, suggesting that OA composition is affected by biomass burning and other, potentially anthropogenic, sources. Isoprene-derived organosulfate (IEPOX-OS) was found to be the most dominant ion in most of the analysed samples and strongly followed the concentration trends of the gas-phase anthropogenic tracers confirming its mixed anthropogenic-biogenic origin. The presence of oxidised aromatic and nitro-aromatic compounds in the samples suggested a strong influence from biomass burning especially during the dry period. Aerosol samples from the dry period and under enhanced biomass burning conditions contained a large number of molecules with high carbon oxidation state and an increased number of aromatic compounds compared to that from the wet period. The results of this work demonstrate that the studied site is influenced not only by biogenic emissions from the forest but also by biomass burning and potentially other anthropogenic emissions from the neighbouring urban environments.

  11. Molecular Characterization of Biomass Burning Aerosols Using High Resolution Mass Spectrometry

    SciTech Connect

    Smith, Jeffrey S.; Laskin, Alexander; Laskin, Julia

    2009-02-13

    Chemical characterizations of atmospheric aerosols is a serious analytical challenge because of the complexity of particulate matter analyte composed of a large number of compounds with a wide range of molecular structures, physico-chemical properties, and reactivity. In this study chemical composition of biomass burning organic aerosol (BBOA) samples is characterized by high resolution electrospray ionization mass spectrometry (ESI/MS). Accurate mass measurement combined with Kendrick analysis allowed us to assign elemental composition for hundreds of compounds in the range of m/z values of 50-1000. ESI/MS spectra of different BBOA samples contain a variety of distinct, sample specific, characteristic peaks that can be used as unique markers for different types of biofuels. Our results indicate that a significant number of high-MW organic compounds in BBOA samples are highly oxidized polar species that can be efficiently detected using ESI/MS but are difficult to observe using the conventional GCMS analysis of aerosol samples. The average O:C ratios obtained for each of the BBOA samples studied in this work are in a strikingly good agreement with the previously reported values obtained using STXM/NEXAFS. The degree of unsaturation of detected organic compounds shows a clear decrease with increase in the molecular weight of the anyalyte molecules. The decrease is particularly pronounced for the samples containing a large number of CH2-based homologous series.

  12. Development of Soft Ionization for Particulate Organic Detection with the Aerodyne Aerosol Mass Spectrometer

    SciTech Connect

    Trimborn, A; Williams, L R; Jayne, J T; Worsnop, D R

    2008-06-19

    During this DOE SBIR Phase II project, we have successfully developed several soft ionization techniques, i.e., ionization schemes which involve less fragmentation of the ions, for use with the Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS). Vacuum ultraviolet single photon ionization was demonstrated in the laboratory and deployed in field campaigns. Vacuum ultraviolet single photon ionization allows better identification of organic species in aerosol particles as shown in laboratory experiments on single component particles, and in field measurements on complex multi-component particles. Dissociative electron attachment with lower energy electrons (less than 30 eV) was demonstrated in the measurement of particulate organics in chamber experiments in Switzerland, and is now a routine approach with AMS systems configured for bipolar, negative ion detection. This technique is particularly powerful for detection of acidic and other highly oxygenated secondary organic aerosol (SOA) chemical functionality. Low energy electron ionization (10 to 12 eV) is also a softer ionization approach routinely available to AMS users. Finally, Lithium ion attachment has been shown to be sensitive to more alkyl-like chemical functionality in SOA. Results from Mexico City are particularly exciting in observing changes in SOA molecular composition under different photochemical/meteorological conditions. More recent results detecting biomass burns at the Montana fire lab have demonstrated quantitative and selective detection of levoglucosan. These soft ionization techniques provide the ToF-AMS with better capability for identifying organic species in ambient atmospheric aerosol particles. This, in turn, will allow more detailed study of the sources, transformations and fate of organic-containing aerosol.

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

    PubMed

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

    2007-08-15

    Single-particle aerosol mass spectrometry (SPAMS) was used for the real-time detection of liquid nerve agent simulants. A total of 1000 dual-polarity time-of-flight mass spectra were obtained for micrometer-sized single particles each of dimethyl methyl phosphonate, diethyl ethyl phosphonate, diethyl phosphoramidate, and diethyl phthalate using laser fluences between 0.58 and 7.83 nJ/microm2, and mass spectral variation with laser fluence was studied. The mass spectra obtained allowed identification of single particles of the chemical warfare agent (CWA) simulants at each laser fluence used although lower laser fluences allowed more facile identification. SPAMS is presented as a promising real-time detection system for the presence of CWAs. PMID:17630721

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

    PubMed

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

    2007-08-15

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

  15. Evolution of wavelength-dependent mass absorption cross sections of carbonaceous aerosols during the 2010 DOE CARES campaign

    NASA Astrophysics Data System (ADS)

    Flowers, B. A.; Dubey, M. K.; Subramanian, R.; Sedlacek, A. J.; Kelley, P.; Luke, W. T.; Jobson, B. T.; Zaveri, R. A.

    2011-12-01

    Predictions of aerosol radiative forcing require process level optical property models that are built on precise and accurate field observations. Evolution of aerosol optical properties for urban influenced carbonaceous aerosol undergoing transport and mixing with rural air masses was a focal point of the DOE Carbonaceous Aerosol and Radiative Effects (CARES) campaign near Sacramento, CA in summer 2010. Urban aerosol was transported from Sacramento, CA (T0) to the foothills of the Sierra Nevada Mountains to a rural site located near Cool, CA (T1). Aerosol absorption and scattering coefficients were measured at the T0 and T1 sites using integrated photoacoustic acoustic/nephelometer instruments (PASS-3 and PASS-UV) at 781, 532, 405, and 375 nm. Single particle soot photometry (SP2) instrumentation was used to monitor black carbon (BC) mass at both sites. Combining data from these sensors allows estimate of the wavelength-dependent mass absorption coefficient (MAC(λ)) and partitioning of MAC(λ) into contributions from the BC core and from enhancements from coating of BC cores. MAC(λ) measured in this way is free of artifacts associated with filter-based aerosol absorption measurements and takes advantage of the single particle sensitivity of the SP2 instrument, allowing observation of MAC(λ) on 10 minute and faster time scales. Coating was observed to enhance MAC(λ) by 20 - 30 % and different wavelength dependence for MAC(λ) was observed for urban and biomass burning aerosol. Further, T0 - T1 evolution of MAC(λ) was correlated with separately measured NO/NOy ratios and CO/CO2 ratios to understand the effects of aging & transport on MAC(λ) and the implications of aerosol processing that links air quality to radiative forcing on a regional scale. Aircraft observations made from the Gulfstream-1 during CARES are also analyzed to enhance process level understanding of the optical properties of fresh and aged carbonaceous aerosol in the urban-rural interface.

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

    NASA Astrophysics Data System (ADS)

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

    2009-04-01

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

  17. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically-resolved aerosol fluxes

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2010-12-01

    Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocity for total NR-PM1 aerosol at noon was 2.05 ± 0.04 mm/s. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm/s and are dominated by deposition of ammonium sulphate.

  18. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

    NASA Astrophysics Data System (ADS)

    Farmer, D. K.; Kimmel, J. R.; Phillips, G.; Docherty, K. S.; Worsnop, D. R.; Sueper, D.; Nemitz, E.; Jimenez, J. L.

    2011-06-01

    Although laboratory studies show that biogenic volatile organic compounds (VOCs) yield substantial secondary organic aerosol (SOA), production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS) in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR) PM1 fluxes. Average deposition velocities for total NR-PM1 aerosol at noon were 2.05 ± 0.04 mm s-1. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s-1 and are dominated by deposition of ammonium sulphate.

  19. Characterization of cumulus cloud fields using trajectories in the center of gravity versus water mass phase space: 2. Aerosol effects on warm convective clouds

    NASA Astrophysics Data System (ADS)

    Heiblum, Reuven H.; Altaratz, Orit; Koren, Ilan; Feingold, Graham; Kostinski, Alexander B.; Khain, Alexander P.; Ovchinnikov, Mikhail; Fredj, Erick; Dagan, Guy; Pinto, Lital; Yaish, Ricki; Chen, Qian

    2016-06-01

    In Part I of this work a 3-D cloud tracking algorithm and phase space of center of gravity altitude versus cloud liquid water mass (CvM space) were introduced and described in detail. We showed how new physical insight can be gained by following cloud trajectories in the CvM space. Here this approach is used to investigate aerosol effects on cloud fields of warm cumuli. We show a clear effect of the aerosol loading on the shape and size of CvM clusters. We also find fundamental differences in the CvM space between simulations using bin versus bulk microphysical schemes, with the bin scheme precipitation expressing much higher sensitivity to changes in aerosol concentrations. Using the bin microphysical scheme, we find that the increase in cloud center of gravity altitude with increase in aerosol concentrations occurs for a wide range of cloud sizes. This is attributed to reduced sedimentation, increased buoyancy and vertical velocities, and increased environmental instability, all of which are tightly coupled to inhibition of precipitation processes and subsequent feedbacks of clouds on their environment. Many of the physical processes shown here are consistent with processes typically associated with cloud invigoration.

  20. Towards a quasi-complete reconstruction of past atmospheric aerosol load and composition (organic and inorganic) over Europe since 1920 inferred from Alpine ice cores

    NASA Astrophysics Data System (ADS)

    Preunkert, S.; Legrand, M.

    2013-02-01

    Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps) are here revisited in view to reconstruct past aerosol load of the free European troposphere from prior World War II to present. The extended array of inorganic (Na+, Ca2+, NH4+, Cl-, NO3-, and SO42-) and organic (carboxylates, HCHO, HUmic LIke Substances, dissolved organic carbon, water insoluble organic carbon, and black carbon) compounds and fractions already investigated permit to examine the overall aerosol composition and its change over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921-1951 to 1971-1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). It is shown that not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarii dealing with climate forcing by atmospheric aerosol.

  1. Towards a quasi-complete reconstruction of past atmospheric aerosol load and composition (organic and inorganic) over Europe since 1920 inferred from Alpine ice cores

    NASA Astrophysics Data System (ADS)

    Preunkert, S.; Legrand, M.

    2013-07-01

    Seasonally resolved chemical ice core records available from the Col du Dôme glacier (4250 m elevation, French Alps), are here used to reconstruct past aerosol load and composition of the free European troposphere from before World War II to present. Available ice core records include inorganic (Na+, Ca2+, NH4+, Cl-, NO3-, and SO42-) and organic (carboxylates, HCHO, humic-like substances, dissolved organic carbon, water-insoluble organic carbon, and black carbon) compounds and fractions that permit reconstructing the key aerosol components and their changes over the past. It is shown that the atmospheric load of submicron aerosol has been increased by a factor of 3 from the 1921-1951 to 1971-1988 years, mainly as a result of a large increase of sulfate (a factor of 5), ammonium and water-soluble organic aerosol (a factor of 3). Thus, not only growing anthropogenic emissions of sulfur dioxide and ammonia have caused the enhancement of the atmospheric aerosol load but also biogenic emissions producing water-soluble organic aerosol. This unexpected change of biospheric source of organic aerosol after 1950 needs to be considered and further investigated in scenarios dealing with climate forcing by atmospheric aerosol.

  2. 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

  3. Demonstration of a VUV lamp photoionization source for improvedorganic speciation in an aerosol mass spectrometer

    SciTech Connect

    Northway, M.J.; Jayne, J.T.; Toohey, D.W.; Canagaratna, M.R.; Trimborn, A.; Akiyama, K-I.; Shimono, A.; Jimenez, J.L.; DeCarlo, P.F.; Wilson, K.R.; Worsnop, D.R.

    2007-10-03

    In recent years, the Aerodyne AerosolMass Spectrometer(AMS) has become a widely used tool for determining aerosol sizedistributions and chemical composition for non-refractory inorganic andorganic aerosol. The current version of the AMS uses a combination offlash thermal vaporization and 70 eV electron impact (EI) ionization.However, EI causes extensive fragmentation and mass spectra of organicaerosols are difficult to deconvolute because they are composites of theoverlapping fragmentation patterns of all species present. Previous AMSstudies have been limited to classifying organics in broad categoriessuch as oxidized and hydrocarbon-like." In this manuscript we present newefforts to gain more information about organic aerosol composition byemploying the softer technique of vacuum ultraviolet (VUV) ionization ina Time-of-Flight AMS (ToF-AMS). In our novel design a VUV lamp is placedin direct proximity of the ionization region of the AMS, with only awindow separating the lamp and the ionizer. This design allows foralternation of photoionization and electron impact ionization within thesame instrument on the timescale of minutes. Thus, the EI-basedquantification capability of the AMS is retained while improved spectralinterpretation is made possible by combined analysis of the complementaryVUV and EI ionization spectra. Photoionization and electron impactionization spectra are compared for a number of compounds including oleicacid, long chain hydrocarbons, and cigarette smoke. In general, the VUVspectra contain much less fragmentation than the EI spectra and for manycompounds the parent ion is the dominant ion in the VUV spectrum. As anexample of the usefulness of the integration of PI within the fullcapability of the ToF-AMS, size distributions and size-segregated massspectra are examined for the cigarette smoke analysis. As a finalevaluation of the new VUV module, spectra for oleic acid are compared tosimilar experiments conducted using the tunable VUV radiation

  4. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE PAGES

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2015-01-16

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1–2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction productsmore » of both aromatics and alkanes, especially those with relatively low carbon numbers (C4–15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  5. Multiday production of condensing organic aerosol mass in urban and forest outflow

    NASA Astrophysics Data System (ADS)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2014-07-01

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1-2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products of both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.

  6. Multiday production of condensing organic aerosol mass in urban and forest outflow

    NASA Astrophysics Data System (ADS)

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2015-01-01

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for multiple days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (~50%) and of shorter duration (1-2 days). The multiday production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products of both aromatics and alkanes, especially those with relatively low carbon numbers (C4-15). In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions and different vapor pressure schemes, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.

  7. Multiday production of condensing organic aerosol mass in urban and forest outflow

    DOE PAGES

    Lee-Taylor, J.; Hodzic, A.; Madronich, S.; Aumont, B.; Camredon, M.; Valorso, R.

    2014-07-03

    Secondary organic aerosol (SOA) production in air masses containing either anthropogenic or biogenic (terpene-dominated) emissions is investigated using the explicit gas-phase chemical mechanism generator GECKO-A. Simulations show several-fold increases in SOA mass continuing for several days in the urban outflow, even as the initial air parcel is diluted into the regional atmosphere. The SOA mass increase in the forest outflow is more modest (∼50%) and of shorter duration (1–2 days). The production in the urban outflow stems from continuing oxidation of gas-phase precursors which persist in equilibrium with the particle phase, and can be attributed to multigenerational reaction products ofmore » both aromatics and alkanes. In particular we find large contributions from substituted maleic anhydrides and multi-substituted peroxide-bicyclic alkenes. The results show that the predicted production is a robust feature of our model even under changing atmospheric conditions, and contradict the notion that SOA undergoes little mass production beyond a short initial formation period. The results imply that anthropogenic aerosol precursors could influence the chemical and radiative characteristics of the atmosphere over an extremely wide region, and that SOA measurements near precursor sources may routinely underestimate this influence.« less

  8. Mass loading in the CRIT II CIV experiment

    SciTech Connect

    Brenning, N.; Bolin, O.

    1995-12-31

    The CRIT II rocket was launched in 1989 from Wallops Island with the objective of studying the critical ionization velocity (CIV) phenomenon. The experiment consisted of two payloads located on close to the same magnetic field line. At an altitude of approximately 400 km two shaped charge explosions of neutral barium, aimed directly at the main payload, took place. Full three dimensional vector measurements were made, at both the main and the sub payload, of the electric and magnetic fields resulting from the interaction of these neutral barium beams with the ambient ionosphere. The analysis of the electric and magnetic data shows rather clearly that one may consider the low frequency features, below the ambient oxygen gyro frequency, in the CRIT II experiment as being well understood. The analysis also resolves the competition between the homogeneous and the inhomogeneous model for CIV, and a combined model is emerging with components of both. A gradual transition from one to the other, depending on the ionization rate as originally proposed by Haerendel, agrees with CRIT II observations, and gives a natural coupling between the energy and momentum transfer mechanisms. The only assumptions are (1) that instability-associated Hall currents flow along the wave fronts, and (2) these high frequency Hall currents merge into field-aligned mass loading currents in a macroscopic low frequency current system. The authors propose a matching region, where this merging takes place, to exist between the beam and the distant ionosphere.

  9. Influence of dust loading on the alpha-particle energy resolution of continuous air monitors for thin deposits of radioactive aerosols.

    PubMed

    Huang, Suilou; Schery, Stephen D; Alcantara, Raul E; Rodgers, John C; Wasiolek, Piotr T

    2002-12-01

    Alpha-particle continuous air monitors must sometimes be operated in dusty environments where significant dust loading of the filter can be anticipated. It is important to understand how this dust loading affects the response of the continuous air monitors. Not only must a filter be changed if there is a reduction in airflow, but a change may be necessary if the energy resolution deteriorates and the continuous air monitor loses sensitivity and specificity for the radioactive aerosols of interest. A series of experiments were conducted to investigate alpha-particle energy resolution of continuous air monitor filters, particularly under dust loading conditions. Aerosol particles of various sizes were tagged with radon decay products to serve as surrogates for radioactive aerosols of interest such as plutonium or uranium. While the size of radioactive aerosols, filter type, and dust type affected the energy resolution, the thickness of an underlying (nonradioactive) dust layer did not show significant effect for the materials studied and a loading range of 0.01-10 mg x cm(-2). Our results indicate that it is possible for continuous air monitors to detect the release of radioactive aerosols with little deterioration in energy resolution under conditions of significant dust loading provided that the deposited layer of radioactive aerosols remains thin (< or = 0.1 mg x cm(-2)).

  10. Spatially detailed quantification of metal loading for decision making: Metal mass loading to American fork and Mary Ellen Gulch, Utah

    USGS Publications Warehouse

    Kimball, B.A.; Runkel, R.L.

    2009-01-01

    Effective remediation requires an understanding of the relative contributions of metals from all sources in a catchment, and that understanding must be based on a spatially detailed quantification of metal loading. A traditional approach to quantifying metal loading has been to measure discharge and chemistry at a catchment outlet. This approach can quantify annual loading and the temporal changes in load, but does not provide the needed spatial detail to evaluate specific sources, which is needed to support remediation decisions. A catchment or massloading approach provides spatial detail by combining tracer-injection and synoptic-sampling methods to quantify loading. Examples of studies in American Fork, Utah, and its tributary Mary Ellen Gulch illustrate this different approach. The mass-loading study in American Fork treated Mary Ellen Gulch as a single inflow. From that point of view, Mary Ellen Gulch was one of the greatest sources of Fe, Mn, Zn, and colloidal Pb loads to American Fork. But when Mary Ellen Gulch was evaluated in a separate catchment study, the detailed locations of metal loading were identified, and the extent of metal attenuation upstream from the mouth of Mary Ellen Gulch was quantified. The net, instantaneous load measured at the mouth of Mary Ellen Gulch for remediation planning would greatly underestimate the contributions of principal sources within the catchment. Extending the detailed sampling downstream from Mary Ellen Gulch indicated the possibility of diffuse groundwater inflow from Mary Ellen Gulch to American Fork. Comparing loads for Mary Ellen Gulch in the two studies indicates that metal loads could be substantially underestimated for planning purposes without the detailed catchment approach for the low-flow conditions in these studies. A mass-loading approach provides both the needed quantification of metal loading and the spatial detail to guide remediation decisions that would be the most effective in the catchments

  11. On the correlation of atmospheric aerosol components of mass size distributions in the larger region of a central European city

    NASA Astrophysics Data System (ADS)

    Berner, A.; Galambos, Z.; Ctyroky, P.; Frühauf, P.; Hitzenberger, R.; Gomišček, B.; Hauck, H.; Preining, O.; Puxbaum, H.

    Mass size distributions of atmospheric aerosols have been sampled in the region of Vienna, a typical city in central Europe, at an urban and a rural site. The aerosol was collected simultaneously by cascade impactors. Two experiments which had a duration of 4 weeks each, were performed in August 1999 and in January/February 2000. Daily sampling periods were from 8:00 to 20:00, and from 20:00 to 8:00. An evaluation of the mass size distributions is represented in this paper. Emphasis is on the relationships of different aerosol components in a local and a regional context. The main results are as follows. The main components of the atmospheric aerosol are a fine aerosol, the accumulation aerosol, and a coarse aerosol. Specific coarse modes with modal diameters of 4.7 μm average and geometric standard deviations of about 3 occur at the urban and at the rural site, some times surprisingly strong. The fine and the coarse modes are very likely related to motor-car traffic. Usually the PM 2.5 and PM 10 aerosols are regionally strongly correlated. Occasionally, this correlation is effectively disturbed by local and/or regional emissions. Time series of correlation coefficients reveal an episodic character of the atmospheric aerosol. Periods of strong inter-site correlations of PM 2.5 and PM 10 indicate the dominance and the co-variation of the accumulation aerosols or the dominance and the co-variation of the coarse modes.

  12. Characterization of primary organic aerosol emissions from meat cooking, trash burning, and motor vehicles with high-resolution aerosol mass spectrometry and comparison with ambient and chamber observations.

    PubMed

    Mohr, Claudia; Huffman, Alex; Cubison, Michael J; Aiken, Allison C; Docherty, Kenneth S; Kimmel, Joel R; Ulbrich, Ingrid M; Hannigan, Michael; Jimenez, Jose L

    2009-04-01

    Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS). High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning emissions contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to those from ambient hydrocarbon-like OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from these sources is unlikelyto be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/zs that may be useful for differentiating some of these sources. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, whereas motor vehicle emissions have very low signal at this m/z.

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

    NASA Astrophysics Data System (ADS)

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

    2016-05-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

  15. High-Resolution Desorption Electrospray Ionization Mass Spectrometry for Chemical Characterization of Organic Aerosols

    SciTech Connect

    Laskin, Julia; Laskin, Alexander; Roach, Patrick J.; Slysz, Gordon W.; Anderson, Gordon A.; Nizkorodov, Serguei; Bones, David L.; Nguyen, Lucas

    2010-03-01

    Characterization of the chemical composition and chemical transformations of secondary organic aerosol (SOA) is both a major challenge and the area of greatest uncertainty in current aerosol research. This study presents the first application of desorption electrospray ionization combined with high-resolution mass spectrometry (DESI-MS) for detailed chemical characterization and studies of chemical aging of OA collected on Teflon substrates. DESI-MS offers unique advantages both for detailed characterization of chemically labile components in OA that cannot be detected using more traditional electrospray ionization mass spectrometry (ESI-MS) and for studying chemical aging of OA. DESI-MS enables rapid characterization of OA samples collected on substrates by eliminating the sample preparation stage. In addition, it enables detection and structural characterization of chemically labile molecules in OA samples by minimizing the residence time of analyte in the solvent. SOA produced by the ozonolysis of limonene (LSOA) was allowed to react with gaseous ammonia. Chemical aging resulted in measurable changes in the optical properties of LSOA observed using UV- visible spectroscopy. DESI-MS combined with tandem mass spectrometry experiments (MS/MS) enabled identification of species in aged LSOA responsible for absorption of the visible light. Detailed analysis of the experimental data allowed us to identify chemical changes induced by reactions of LSOA constituents with ammonia and distinguish between different mechanisms of chemical aging.

  16. Molecular Chemistry of Organic Aerosols Through the Application of High Resolution Mass Spectrometry

    SciTech Connect

    Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2011-01-05

    Understanding of molecular composition and fundamental chemical transformations of organic aerosols (OA) during their formation and aging is both a major challenge and the area of greatest uncertainty in atmospheric research. Particularly little is known about fundamental relationship between the chemical composition and physicochemical properties of OA, their atmospheric history, evolution, and impact on the environment. Ambient soft-ionization methods combined with high-resolution mass spectrometry (HR-MS) analysis provide detailed information on the molecular content of OA that is pivotal for improved understanding of their complex composition, multi-phase aging chemistry, direct (light absorption and scattering) and indirect (aerosol-cloud interactions) effects on atmospheric radiation and climate, and health effects. The HR-MS methods can detect thousands of individual OA constituents at once, provide their elemental formulae from accurate mass measurements, and provide structural information based on tandem mass spectrometry. Integration with additional analytical tools, such as chromatography and UV/Vis absorption spectroscopy, makes it possible to further separate OA compounds by their polarity and ability to absorb solar radiation. The goal of this perspective is to describe modern HR-MS methods, review recent applications to field and laboratory studies of OA, and explain how the information obtained from HR-MS methods can be translated into improved understanding of OA chemistry.

  17. Comment on "Large volcanic aerosol load in the stratosphere linked to Asian monsoon transport".

    PubMed

    Fromm, Michael; Nedoluha, Gerald; Charvát, Zdenek

    2013-02-01

    Bourassa et al. (Reports, 6 July 2012, p. 78) report on the 13 June 2011 eruption of the Nabro volcano and satellite observations of stratospheric aerosol that they attribute to troposphere to stratosphere ascent via the Asian monsoon. They claim (citing another source) that the 13 June top injection height was well below the tropopause. We will show that the 13 June Nabro eruption plume was clearly stratospheric and contained both volcanic gases and aerosols. Moreover, we will show height-resolved stratospheric sulfur dioxide and volcanic aerosol enhancements 1 to 3 days old, unaffected by the Asian monsoon, precisely connected to the volcano. The observed stratospheric aerosols and gases are fully explained by the 13 June eruption and do not require a monsoon vehicle. PMID:23393246

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

    NASA Astrophysics Data System (ADS)

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

    2011-12-01

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

  19. Real-time analysis of organic compounds in ship engine aerosol emissions using resonance-enhanced multiphoton ionisation and proton transfer mass spectrometry.

    PubMed

    Radischat, Christian; Sippula, Olli; Stengel, Benjamin; Klingbeil, Sophie; Sklorz, Martin; Rabe, Rom; Streibel, Thorsten; Harndorf, Horst; Zimmermann, Ralf

    2015-08-01

    Organic combustion aerosols from a marine medium-speed diesel engine, capable to run on distillate (diesel fuel) and residual fuels (heavy fuel oil), were investigated under various operating conditions and engine parameters. The online chemical characterisation of the organic components was conducted using a resonance-enhanced multiphoton ionisation time-of-flight mass spectrometer (REMPI TOF MS) and a proton transfer reaction-quadrupole mass spectrometer (PTR-QMS). Oxygenated species, alkenes and aromatic hydrocarbons were characterised. Especially the aromatic hydrocarbons and their alkylated derivatives were very prominent in the exhaust of both fuels. Emission factors of known health-hazardous compounds (e.g. mono- and poly-aromatic hydrocarbons) were calculated and found in higher amounts for heavy fuel oil (HFO) at typical engine loadings. Lower engine loads lead in general to increasing emissions for both fuels for almost every compound, e.g. naphthalene emissions varied for diesel fuel exhaust between 0.7 mg/kWh (75 % engine load, late start of injection (SOI)) and 11.8 mg/kWh (10 % engine load, late SOI) and for HFO exhaust between 3.3 and 60.5 mg/kWh, respectively. Both used mass spectrometric techniques showed that they are particularly suitable methods for online monitoring of combustion compounds and very helpful for the characterisation of health-relevant substances. Graphical abstract Three-dimensional REMPI data of organic species in diesel fuel and heavy fuel oil exhaust.

  20. Implications of MODIS impression of aerosol loading over urban and rural settlements in Nigeria: Possible links to energy consumption patterns in the country

    NASA Astrophysics Data System (ADS)

    Dom Onyeuwaoma, Nnaemeka

    2016-07-01

    A study of aerosol loading patterns in some selected cities in Nigeria was carried out using MODIS, TOMS/OMI AND AIRS satellite imageries for a period of 10 years. The results showed that an aerosol optical depth (AOD) loading obtained ranged from 0.02-0.9, UV aerosol index (AI) and carbon monoxide (CO) results ranged from 1.32- 2.43 and 2.22-2.6 molecule/cm2, respectively. The CO data was used to infer the presence of carbonecous aerosols from biomass, fossil combustion and industrial activities. This result indicates that areas with higher AOD and AI do not correspond in high CO loading. From the HYSPLIT and HAT analysis conducted it showed that advection plays important role in the dispersion of aerosols. This implies that aerosols can reside in a place remote from where they are generated. Also, the high concentration of CO aerosol in the southern cities suggests a high rate of industrial pollution as a result of fossil fuel burning, vehicular emissions, high population density and gas flaring. Therefore, emphasis should be on the need to switch to renewable energy options as an alternative to fossil fuel. Furthermore, plans for mitigations should not be limited to industrialized cities only but extended to other cities which might be bearing the real brunt of industrial emissions as shown in this work.

  1. Extensive aerosol optical properties and aerosol mass related measurements during TRAMP/TexAQS 2006 - Implications for PM compliance and planning

    NASA Astrophysics Data System (ADS)

    Wright, Monica E.; Atkinson, Dean B.; Ziemba, Luke; Griffin, Robert; Hiranuma, Naruki; Brooks, Sarah; Lefer, Barry; Flynn, James; Perna, Ryan; Rappenglück, Bernhard; Luke, Winston; Kelley, Paul

    2010-10-01

    Extensive aerosol optical properties, particle size distributions, and Aerodyne quadrupole aerosol mass spectrometer measurements collected during TRAMP/TexAQS 2006 were examined in light of collocated meteorological and chemical measurements. Much of the evident variability in the observed aerosol-related air quality is due to changing synoptic meteorological situations that direct emissions from various sources to the TRAMP site near the center of the Houston-Galveston-Brazoria (HGB) metropolitan area. In this study, five distinct long-term periods have been identified. During each of these periods, observed aerosol properties have implications that are of interest to environmental quality management agencies. During three of the periods, long range transport (LRT), both intra-continental and intercontinental, appears to have played an important role in producing the observed aerosol. During late August 2006, southerly winds brought super-micron Saharan dust and sea salt to the HGB area, adding mass to fine particulate matter (PM 2.5) measurements, but apparently not affecting secondary particle growth or gas-phase air pollution. A second type of LRT was associated with northerly winds in early September 2006 and with increased ozone and sub-micron particulate matter in the HGB area. Later in the study, LRT of emissions from wildfires appeared to increase the abundance of absorbing aerosols (and carbon monoxide and other chemical tracers) in the HGB area. However, the greatest impacts on Houston PM 2.5 air quality are caused by periods with low-wind-speed sea breeze circulation or winds that directly transport pollutants from major industrial areas, i.e., the Houston Ship Channel, into the city center.

  2. Comparative Analysis of Urban Atmospheric Aerosol by Particle-Induced X-ray Emission (PIXE), Proton Elastic Scattering Analysis (PESA), and Aerosol Mass Spectrometry (AMS)

    SciTech Connect

    Johnson, Kirsten S; Laskin, Alexander; Jimenez, Jose L; Shutthanandan, V; Molina, Luisa T; Salcedo, D; Dzepina, K; Molina, Mario J

    2008-09-01

    A multifaceted approach to atmospheric aerosol analysis is often desirable in field studies where an understanding of technical comparability among different measurement techniques is essential. Herein we report quantitative intercomparisons of Particle-Induced X-ray Emission (PIXE) and Proton Elastic Scattering Analysis (PESA), performed off-line under vacuum, with analysis by Aerosol Mass Spectrometry (AMS) carried out in real-time during the MCMA-2003 Field Campaign in the Mexico City Metropolitan Area. Good agreement was observed for mass concentrations of PIXE-measured sulfur (assuming it was dominated by SO42-) and AMS-measured sulfate during the most of the campaign. PESA-measured hydrogen mass was separated into sulfate H and organic H mass fractions assuming the only major contributions were (NH4)2SO4 and organic compounds. Comparison of the organic H mass with AMS organic aerosol measurements indicates that about 75% of the mass of these species evaporated under vacuum. However ~25% of the organics does remain under vacuum, which is only possible with low vapor pressure compounds, and which supports the presence of high molecular weight and/or highly oxidized organics consistent with atmospheric aging. Approximately 10% of the chloride detected by AMS was measured by PIXE, possibly in the form of metal-chloride complexes, while the majority of Cl was likely present as more volatile species including NH4Cl. This is the first comparison of PIXE/PESA and AMS, and to our knowledge also the first report of PESA hydrogen measurements for urban organic aerosols.

  3. 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

  4. Overview of aerosol properties associated with air masses sampled by the ATR-42 during the EUCAARI campaign (2008)

    NASA Astrophysics Data System (ADS)

    Crumeyrolle, S.; Schwarzenboeck, A.; Roger, J. C.; Sellegri, K.; Burkhart, J. F.; Stohl, A.; Gomes, L.; Quennehen, B.; Roberts, G.; Weigel, R.; Villani, P.; Pichon, J. M.; Bourrianne, T.; Laj, P.

    2013-05-01

    Within the frame of the European Aerosol Cloud Climate and Air Quality Interactions (EUCAARI) project, the Météo-France aircraft ATR-42 performed 22 research flights over central Europe and the North Sea during the intensive observation period in May 2008. For the campaign, the ATR-42 was equipped to study the aerosol physical, chemical, hygroscopic and optical properties, as well as cloud microphysics. For the 22 research flights, retroplume analyses along the flight tracks were performed with FLEXPART in order to classify air masses into five sectors of origin, allowing for a qualitative evaluation of emission influence on the respective air parcel. This study shows that the extensive aerosol parameters (aerosol mass and number concentrations) show vertical decreasing gradients and in some air masses maximum mass concentrations (mainly organics) in an intermediate layer (1-3 km). The observed mass concentrations (in the boundary layer (BL): between 10 and 30 μg m-3; lower free troposphere (LFT): 0.8 and 14 μg m-3) are high especially in comparison with the 2015 European norms for PM2.5 (25 μg m-3) and with previous airborne studies performed over England (Morgan et al., 2009; McMeeking et al., 2012). Particle number size distributions show a larger fraction of particles in the accumulation size range in the LFT compared to BL. The chemical composition of submicron aerosol particles is dominated by organics in the BL, while ammonium sulphate dominates the submicron aerosols in the LFT, especially in the aerosol particles originated from north-eastern Europe (~ 80%), also experiencing nucleation events along the transport. As a consequence, first the particle CCN acting ability, shown by the CCN/CN ratio, and second the average values of the scattering cross sections of optically active particles (i.e. scattering coefficient divided by the optical active particle concentration) are increased in the LFT compared to BL.

  5. Tropospheric Aerosols

    NASA Astrophysics Data System (ADS)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    m, PM10=1.1 μg m-3; estimated coefficient of light scattering by particulate matter, σep, at 570 nm=12 Mm-1). (b) High aerosol concentration (PM2.5=43.9 μg m-3; PM10=83.4 μg m-3; estimated σep at 570 nm=245 Mm-1) (reproduced by permission of National Park Service, 2002). Although comprising only a small fraction of the mass of Earth's atmosphere, aerosol particles are highly important constituents of the atmosphere. Special interest has focused on aerosols in the troposphere, the lowest part of the atmosphere, extending from the land or ocean surface typically to ˜8 km at high latitudes, ˜12 km in mid-latitudes, and ˜16 km at low latitudes. That interest arises in large part because of the importance of aerosol particles in geophysical processes, human health impairment through inhalation, environmental effects through deposition, visibility degradation, and influences on atmospheric radiation and climate.Anthropogenic aerosols are thought to exert a substantial influence on Earth's climate, and the need to quantify this influence has sparked much of the current interest in and research on tropospheric aerosols. The principal mechanisms by which aerosols influence the Earth radiation budget are scattering and absorbing solar radiation (the so-called "direct effects") and modifying clouds and precipitation, thereby affecting both radiation and hydrology (the so-called "indirect effects"). Light scattering by aerosols increases the brightness of the planet, producing a cooling influence. Light-absorbing aerosols such as black carbon exert a warming influence. Aerosols increase the reflectivity of clouds, another cooling influence. These radiative influences are quantified as forcings, where a forcing is a perturbation to the energy balance of the atmosphere-Earth system, expressed in units of watts per square meter, W m-2. A warming influence is denoted a positive forcing, and a cooling influence, negative. The radiative direct and indirect forcings by

  6. Determination of the organic aerosol mass to organic carbon ratio in IMPROVE samples.

    PubMed

    El-Zanan, Hazem S; Lowenthal, Douglas H; Zielinska, Barbara; Chow, Judith C; Kumar, Naresh

    2005-07-01

    The ratio of organic mass (OM) to organic carbon (OC) in PM(2.5) aerosols at US national parks in the IMPROVE network was estimated experimentally from solvent extraction of sample filters and from the difference between PM(2.5) mass and chemical constituents other than OC (mass balance) in IMPROVE samples from 1988 to 2003. Archived IMPROVE filters from five IMPROVE sites were extracted with dichloromethane (DCM), acetone and water. The extract residues were weighed to determine OM and analyzed for OC by thermal optical reflectance (TOR). On average, successive extracts of DCM, acetone, and water contained 64%, 21%, and 15%, respectively, of the extractable OC, respectively. On average, the non-blank-corrected recovery of the OC initially measured in these samples by TOR was 115+/-42%. OM/OC ratios from the combined DCM and acetone extracts averaged 1.92 and ranged from 1.58 at Indian Gardens, AZ in the Grand Canyon to 2.58 at Mount Rainier, WA. The average OM/OC ratio determined by mass balance was 2.07 across the IMPROVE network. The sensitivity of this ratio to assumptions concerning sulfate neutralization, water uptake by hygroscopic species, soil mass, and nitrate volatilization were evaluated. These results suggest that the value of 1.4 for the OM/OC ratio commonly used for mass and light extinction reconstruction in IMPROVE is too low.

  7. Determination of the organic aerosol mass to organic carbon ratio in IMPROVE samples.

    PubMed

    El-Zanan, Hazem S; Lowenthal, Douglas H; Zielinska, Barbara; Chow, Judith C; Kumar, Naresh

    2005-07-01

    The ratio of organic mass (OM) to organic carbon (OC) in PM(2.5) aerosols at US national parks in the IMPROVE network was estimated experimentally from solvent extraction of sample filters and from the difference between PM(2.5) mass and chemical constituents other than OC (mass balance) in IMPROVE samples from 1988 to 2003. Archived IMPROVE filters from five IMPROVE sites were extracted with dichloromethane (DCM), acetone and water. The extract residues were weighed to determine OM and analyzed for OC by thermal optical reflectance (TOR). On average, successive extracts of DCM, acetone, and water contained 64%, 21%, and 15%, respectively, of the extractable OC, respectively. On average, the non-blank-corrected recovery of the OC initially measured in these samples by TOR was 115+/-42%. OM/OC ratios from the combined DCM and acetone extracts averaged 1.92 and ranged from 1.58 at Indian Gardens, AZ in the Grand Canyon to 2.58 at Mount Rainier, WA. The average OM/OC ratio determined by mass balance was 2.07 across the IMPROVE network. The sensitivity of this ratio to assumptions concerning sulfate neutralization, water uptake by hygroscopic species, soil mass, and nitrate volatilization were evaluated. These results suggest that the value of 1.4 for the OM/OC ratio commonly used for mass and light extinction reconstruction in IMPROVE is too low. PMID:15950041

  8. 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

  9. Investigation of biomass burning and aerosol loading and transport in South America utilizing geostationary satellites

    NASA Technical Reports Server (NTRS)

    Menzel, Paul; Prins, Elaine

    1995-01-01

    This study attempts to assess the extent of burning and associated aerosol transport regimes in South America and the South Atlantic using geostationary satellite observations, in order to explore the possible roles of biomass burning in climate change and more directly in atmospheric chemistry and radiative transfer processes. Modeling and analysis efforts have suggested that the direct and indirect radiative effects of aerosols from biomass burning may play a major role in the radiative balance of the earth and are an important factor in climate change calculations. One of the most active regions of biomass burning is located in South America, associated with deforestation in the selva (forest), grassland management, and other agricultural practices. As part of the NASA Aerosol Interdisciplinary Program, we are utilizing GOES-7 (1988) and GOES-8 (1995) visible and multispectral infrared data (4, 11, and 12 microns) to document daily biomass burning activity in South America and to distinguish smoke/aerosols from other multi-level clouds and low-level moisture. This study catalogues the areal extent and transport of smoke/aerosols throughout the region and over the Atlantic Ocean for the 1988 (July-September) and 1995 (June-October) biomass burning seasons. The smoke/haze cover estimates are compared to the locations of fires to determine the source and verify the haze is actually associated with biomass burning activities. The temporal resolution of the GOES data (half-hourly in South America) makes it possible to determine the prevailing circulation and transport of aerosols by considering a series of visible and infrared images and tracking the motion of smoke, haze and adjacent clouds. The study area extends from 40 to 70 deg W and 0 to 40 deg S with aerosol coverage extending over the Atlantic Ocean when necessary. Fire activity is estimated with the GOES Automated Biomass Burning Algorithm (ABBA). To date, our efforts have focused on GOES-7 and GOES-8 ABBA

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

    PubMed

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

    2016-04-01

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

  11. The Effect of Solvent on the Analysis of Secondary Organic Aerosol Using Electrospray Ionization Mass Spectrometry

    SciTech Connect

    Bateman, Adam P.; Walser, Maggie L.; Dessiaterik, Yury; Laskin, Julia; Laskin, Alexander; Nizkorodov, Serguei

    2008-08-29

    Solvent-analyte reactions in organic aerosol (OA) extracts prepared for analysis by electrospray ionization mass spectrometry (ESI-MS) were examined. Secondary organic aerosol (SOA) produced by ozonation of d-limonene as well as several test organic chemicals with functional groups typical for OA constituents were dissolved and stored in methanol, d3-methanol, acetonitrile, and d3-acetonitrile to investigate the extent and relative rates of reactions between analyte and solvent. High resolution ESI-MS showed that reactions of carbonyls with methanol produce significant amounts of hemiacetals and acetals on time scales ranging from several minutes to several days, with the reaction rates increasing in acidified solutions. Carboxylic acid groups were observed to react with methanol resulting in the formation of esters. In contrast, acetonitrile extracts showed no evidence of reactions with analyte molecules, suggesting that acetonitrile is the preferred solvent for SOA extraction. The use of solvent-analyte reactivity as an analytical chemistry tool for the improved characterization of functional groups in complex organic mixtures was also demonstrated. Direct comparison between ESI mass spectra of the same SOA samples extracted in reactive (methanol) versus non-reactive (acetonitrile) solvents was used to estimate the relative fractions of ketones (≥38%), aldehydes (≥6%), and carboxylic acids (≥55%) in d-limonene SOA.

  12. Performance of an improved monodisperse aerosol generation interface for liquid chromatography/mass spectrometry

    SciTech Connect

    Winkler, P.C.; Perkins, D.D.; Williams, W.K.; Browner, R.F.

    1988-03-01

    An improved monodisperse aerosol generation interface for liquid chromatography/mass spectrometry interfacing (MAG-IC-LC/MS) is described. The interface has an aerodynamically superior momentum separator, which results in decreased analyte loss in passing through the interface. The interface is shown to perform well with a quadrupole mass spectrometer, in addition to earlier studies with a magnetic sector instrument. A new method of forming aerosol has been developed, which reduces the dead volume significantly over earlier designs. The performance of the interface has been evaluated by studying its capabilities for (1) generating electron impact spectra of searchable quality for selected compounds of interest, (2) operating with typical liquid chromatographic separation conditions, including reverse phase and gradient elution, and (3) providing low detection limits for both full scan and selective ion monitoring detection of a range of compounds. Studies include identification of the components of a mixture of cis and trans isomers of the thermally labile compound retinol (vitamin A) acetate. Full scan (m/z 80-350) electron impact spectra were readily obtained with 50-ng injection on-column. Detection limits for this compound were 10 ng full scan and 1 ng with selected ion monitoring. Identification of a free (nonderivatized) fatty acid mixture was also readily obtained, using a reversed-phase separation in gradient mode.

  13. Impact of maritime air mass trajectories on the Western European coast urban aerosol.

    PubMed

    Almeida, S M; Silva, A I; Freitas, M C; Dzung, H M; Caseiro, A; Pio, C A

    2013-01-01

    Lisbon is the largest urban area in the Western European coast. Due to this geographical position the Atlantic Ocean serves as an important source of particles and plays an important role in many atmospheric processes. The main objectives of this study were to (1) perform a chemical characterization of particulate matter (PM2.5) sampled in Lisbon, (2) identify the main sources of particles, (3) determine PM contribution to this urban area, and (4) assess the impact of maritime air mass trajectories on concentration and composition of respirable PM sampled in Lisbon. During 2007, PM2.5 was collected on a daily basis in the center of Lisbon with a Partisol sampler. The exposed Teflon filters were measured by gravimetry and cut into two parts: one for analysis by instrumental neutron activation analysis (INAA) and the other by ion chromatography (IC). Principal component analysis (PCA) and multilinear regression analysis (MLRA) were used to identify possible sources of PM2.5 and determine mass contribution. Five main groups of sources were identified: secondary aerosols, traffic, calcium, soil, and sea. Four-day backtracking trajectories ending in Lisbon at the starting sampling time were calculated using the HYSPLIT model. Results showed that maritime transport scenarios were frequent. These episodes were characterized by a significant decrease of anthropogenic aerosol concentrations and exerted a significant role on air quality in this urban area.

  14. Properties of mass-loading shocks. II - Magnetohydrodynamics. [of Giacobini-Zinner and Halley comets

    NASA Technical Reports Server (NTRS)

    Zank, G. P.; Oughton, S.; Neubauer, F. M.; Webb, G. M.

    1992-01-01

    The one-dimensional magnetohydrodynamics of mass-loading shocks is examined. These shocks, which are distinct from MHD shocks of classical nonreacting fluid dynamics and of combustion theory and which are characterized by the addition of mass within the shock transition, are to be found at comets and, depending upon circumstances, at nonmagnetized and weakly magnetized planets such as Venus and Mars. A completely general mass-loading form of the Hugoniot equation is derived, and some of the most important differences between mass-loading and nonreacting classical MHD shocks are identified. Two new types of MHD shocks are described which have no classical MHD analogues.

  15. Characterization of Primary Organic Aerosol Emissions from Meat Cooking, Trash Burning, and Combustion Engines with High-Resolution Aerosol Mass Spectrometry and Comparison with Ambient and Chamber Observations

    NASA Astrophysics Data System (ADS)

    Mohr, C.; Huffman, J. A.; Cubison, M. J.; Aiken, A. C.; Docherty, K. S.; Kimmel, J. R.; Ulbrich, I. M.; Hannigan, M.; Garcia, J.; Jimenez, J. L.

    2009-04-01

    Organic aerosol (OA) emissions from motor vehicles, meat-cooking and trash burning are analyzed here using a high-resolution aerosol mass spectrometer (AMS) and supporting instrumentation. A semi-quantitative comparison of emission factors highlights the potential importance of meat cooking as an OA source. GC-MS and AMS mass spectra are compared for the first time and show high similarity, but with more fragmentation in the AMS due to higher vaporization temperatures. High resolution data show that aerosols emitted by combustion engines and plastic burning are dominated by hydrocarbon-like organic compounds. Meat cooking and especially paper burning contain significant fractions of oxygenated organic compounds; however, their unit-resolution mass spectral signatures are very similar to mass spectral signatures from hydrocarbon-like OA or primary OA, and very different from the mass spectra of ambient secondary or oxygenated OA (OOA). Thus, primary OA from any of these sources is very unlikely to be a significant direct source of ambient OOA. There are significant differences in high-resolution tracer m/z's that may be useful for differentiating these sources from each other. Unlike in most ambient spectra, all of these sources have low total m/z 44 and this signal is not dominated by the CO2+ ion. All sources have high m/z 57, which is low during high OOA ambient periods. Spectra from paper burning are similar to some types of biomass burning OA, with elevated m/z 60. Meat cooking aerosols also have slightly elevated m/z 60, while motor vehicle emissions have very low signal at this m/z.

  16. Hanford Apatite Treatability Test Report Errata: Apatite Mass Loading Calculation

    SciTech Connect

    Szecsody, James E.; Vermeul, Vincent R.; Williams, Mark D.; Truex, Michael J.

    2014-05-19

    The objective of this errata report is to document an error in the apatite loading (i.e., treatment capacity) estimate reported in previous apatite treatability test reports and provide additional calculation details for estimating apatite loading and barrier longevity. The apatite treatability test final report (PNNL-19572; Vermeul et al. 2010) documents the results of the first field-scale evaluation of the injectable apatite PRB technology. The apatite loading value in units of milligram-apatite per gram-sediment is incorrect in this and some other previous reports. The apatite loading in units of milligram phosphate per gram-sediment, however, is correct, and this is the unit used for comparison to field core sample measurements.

  17. 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.

  18. Real-Time Chemical Analysis of E-Cigarette Aerosols By Means Of Secondary Electrospray Ionization Mass Spectrometry.

    PubMed

    García-Gómez, Diego; Gaisl, Thomas; Barrios-Collado, César; Vidal-de-Miguel, Guillermo; Kohler, Malcolm; Zenobi, Renato

    2016-02-12

    Chemical analysis of aerosols collected from electronic cigarettes (ECs) has shown that these devices produce vapors that contain harmful and potentially harmful compounds. Conventional analytical methods used for the analysis of electronic cigarettes do not reflect the actual composition of the aerosols generated because they usually neglect the changes in the chemical composition that occur during the aerosol generation process and after collection. The aim of this work was to develop and apply a method for the real-time analysis of electronic cigarette aerosols, based on the secondary electrospray ionization technique coupled to high-resolution mass spectrometry, by mimicking the "vaping" process. Electronic cigarette aerosols were successfully analyzed and quantitative differences were found between the liquids and aerosols. Thanks to the high sensitivity shown by this method, more than 250 chemical substances were detected in the aerosols, some of them showing a high correlation with the operating power of the electronic cigarettes. The method also allows proper quantification of several chemical components such as alkaloids and flavor compounds.

  19. 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

  20. Fundamental studies with a monodisperse aerosol-based liquid chromatography/mass spectrometry interface (MAGIC-LC/MS)

    SciTech Connect

    Browner, R.F.

    1990-10-01

    Accomplishments on the fundamental studies with a monodisperse aerosol-based liquid chromatography/mass spectrometry (LC/MS) interface during the period 1 December 1989 to 30 November 1990 are summarized. In order to determine the influence of temperature on the vaporization and decomposition properties of molecules, test have been carried out on both thermally stable and thermally labile molecules. The test compounds used were a series of polynuclear aromatic (PAH) compounds covering a wide range of molecular weights from two-ring naphthalene to twelve-ring perylene. The less thermally stable species examined were aldicarb, a highly thermally labile pesticide, and cholesterol, which readily loses water when subjected to high temperatures. A new, externally heated probe, which can be raised to temperatures as high as 500{degree}C was also used. Matrix loading effects for a range of surface active and non-surface active compounds in three different matrices: glycerol, 3-nitrobenzyl alcohol, and thioglycerol for fast atom bombardment (FAB) particle beam LC/MS have been studied. The time dependence of FAB spectra generation in the particle beam system has been examined and contrasted with ion generation in normal probe FAB work. Future FAB LC/MS research is outlined. 3 refs. (BM)

  1. Effects of Relative Humidity and Spraying Medium on UV Decontamination of Filters Loaded with Viral Aerosols

    PubMed Central

    Woo, Myung-Heui; Grippin, Adam; Anwar, Diandra; Smith, Tamara; Wander, Joseph D.

    2012-01-01

    Although respirators and filters are designed to prevent the spread of pathogenic aerosols, a stockpile shortage is anticipated during the next flu pandemic. Contact transfer and reaerosolization of collected microbes from used respirators are also a concern. An option to address these potential problems is UV irradiation, which inactivates microbes by dimerizing thymine/uracil in nucleic acids. The objective of this study was to determine the effects of transmission mode and environmental conditions on decontamination efficiency by UV. In this study, filters were contaminated by different transmission pathways (droplet and aerosol) using three spraying media (deionized water [DI], beef extract [BE], and artificial saliva [AS]) under different humidity levels (30% [low relative humidity {LRH}], 60% [MRH], and 90% [HRH]). UV irradiation at constant intensity was applied for two time intervals at each relative humidity condition. The highest inactivation efficiency (IE), around 5.8 logs, was seen for DI aerosols containing MS2 on filters at LRH after applying a UV intensity of 1.0 mW/cm2 for 30 min. The IE of droplets containing MS2 was lower than that of aerosols containing MS2. Absorption of UV by high water content and shielding of viruses near the center of the aggregate are considered responsible for this trend. Across the different media, IEs in AS and in BE were much lower than in DI for both aerosol and droplet transmission, indicating that solids present in AS and BE exhibited a protective effect. For particles sprayed in a protective medium, RH is not a significant parameter. PMID:22685135

  2. Vegetation fires in the himalayan region - Aerosol load, black carbon emissions and smoke plume heights

    NASA Astrophysics Data System (ADS)

    Vadrevu, Krishna Prasad; Ellicott, Evan; Giglio, Louis; Badarinath, K. V. S.; Vermote, Eric; Justice, Chris; Lau, William K. M.

    2012-02-01

    In this study, we investigate the potential of multi-satellite datasets for quantifying the biomass burning emissions from the Himalayan region. A variety of satellite products were used for characterizing fire events including active fire counts, burnt areas, aerosol optical depth (AOD) variations, aerosol index and smoke plume heights. Results from the MODerate-resolution Imaging Spectroradiometer (MODIS) fire product suggest March-June as the major fire season with the peak during the April. An average of 3908 fire counts per year were recorded with sixty four percent of the fires occurring in the low elevation areas in the Himalayan Region. We estimate average burnt areas of 1129 sq. km, with the black carbon emissions of 431 Mg, per year. The mean AOD (2005-2010) was 0.287 ± 0.105 (one sigma) with peak values in May. Correlation analysis between the fire counts and AOD resulted in a Pearson correlation coefficient of 0.553; the correlation between the FRP and AOD is relatively weaker ( r = 0.499). Planetary boundary layer height retrieved from the Modern Era Retrospective-Analysis For Research And Applications (MERRA) product suggests typical PBL height of 1000-1200 m during the April-May peak biomass burning season. Cloud-Aerosol Lidar Orthogonal Polarisation (CALIOP) retrievals show the extent of smoke plume heights beyond the planetary boundary layer during the peak biomass burning month of April. However, comparison of fires in the Himalayan region with other regions and comparisons to aerosol index data from the Ozone Monitoring Instrument (OMI) suggest smoke plumes reaching less than 3 km. Our results on fires and smoke plume height relationships provide valuable information for addressing aerosol transport in the region.

  3. Mass Spectra of Individual Aerosol Particles Acquired During Intercepts of a Space Shuttle Exhaust Plume

    NASA Astrophysics Data System (ADS)

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

    2001-12-01

    The WB-57 aircraft accomplished fourteen distinct stratospheric intercepts of the exhaust plume from a space shuttle during ACCENT 2000. Liftoff of the shuttle Atlantis for STS-106 occurred at 8:46 am local (12:46 UTC) with intercepts occurring from 5 to 90 minutes afterward. The Particle Analysis by Laser Mass Spectrometry (PALMS) instrument, mounted in the nose of the aircraft, was used to acquire individual mass spectra of over 2500 particles during these intercepts. The majority of positive mass spectra indicate the presence of the metals Al, Fe, Zn, Ga, and V, all components found in the solid rocket fuel. Organic material, presumably from binding and curing agents, was also present. Negative mass spectra showed Cl from the oxidizer, ammonium perchlorate, as well as water. Rare exotic particles, for example those containing Ti and Ag and possibly formed during engine or seal ablation, were also detected. Particles originating from shuttle exhaust but also containing significant sulfuric acid were common toward the outer edge of the plume, especially during late encounters, suggesting that deposition or aerosol collision had occurred.

  4. High-Resolution Mass Spectrometric Analysis of Secondary Organic Aerosol Produced by Ozonation of Limonene

    SciTech Connect

    Walser, Maggie L.; Dessiaterik, Yury; Laskin, Julia; Laskin, Alexander; Nizkorodov, Serguei

    2008-02-08

    Secondary organic aerosol (SOA) particles formed from the ozone-initiated oxidation of limonene are characterized by high-resolution electrospray ionization mass spectrometry in both the positive and negative ion modes. The mass spectra reveal a large number of both monomeric (m/z < 300) and oligomeric (m/z > 300) products of oxidation. A combination of high resolving power (m/Δm ~60,000) and Kendrick mass defect analysis makes it possible to unambiguously determine the composition for hundreds of individual compounds in SOA samples. Van Krevelen analysis shows that the SOA compounds are heavily oxidized, with average O:C ratios of 0.43 and 0.50 determined from the positive and negative ion mode spectra, respectively. An extended reaction mechanism for the formation of the first generation SOA molecular components is proposed. The mechanism includes known isomerization and addition reactions of the carbonyl oxide intermediates generated during the ozonation of limonene, and numerous isomerization pathways for alkoxy radicals resulting from the decomposition of unstable carbonyl oxides. The isomerization reactions yield numerous products with a progressively increasing number of alcohol and carbonyl groups, whereas C-C bond scission reactions in alkoxy radicals shorten the carbon chain. Together these reactions yield a large number of isomeric products with broadly distributed masses. A qualitative agreement is found between the number and degree of oxidation of the predicted and measured reaction products in the monomer range.

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

    NASA Astrophysics Data System (ADS)

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

    2015-12-01

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

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

    PubMed

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

    2012-06-28

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

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

    PubMed

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

    2012-06-28

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

  8. Numerical Simulations of Mass Loading in the Solar Wind Interaction with Venus

    NASA Technical Reports Server (NTRS)

    Murawski, K.; Steinolfson, R. S.

    1996-01-01

    Numerical simulations are performed in the framework of nonlinear two-dimensional magnetohydrodynamics to investigate the influence of mass loading on the solar wind interaction with Venus. The principal physical features of the interaction of the solar wind with the atmosphere of Venus are presented. The formation of the bow shock, the magnetic barrier, and the magnetotail are some typical features of the interaction. The deceleration of the solar wind due to the mass loading near Venus is an additional feature. The effect of the mass loading is to push the shock farther outward from the planet. The influence of different values of the magnetic field strength on plasma evolution is considered.

  9. Evaluation of Ag nanoparticle coated air filter against aerosolized virus: Anti-viral efficiency with dust loading.

    PubMed

    Joe, Yun Haeng; Park, Dae Hoon; Hwang, Jungho

    2016-01-15

    In this study, the effect of dust loading on the anti-viral ability of an anti-viral air filter was investigated. Silver nanoparticles approximately 11 nm in diameter were synthesized via a spark discharge generation system and were used as anti-viral agents coated onto a medium air filter. The pressure drop, filtration efficiency, and anti-viral ability of the filter against aerosolized bacteriophage MS2 virus particles were tested with dust loading. The filtration efficiency and pressure drop increased with dust loading, while the anti-viral ability decreased. Theoretical analysis of anti-viral ability with dust loading was carried out using a mathematical model based on that presented by Joe et al. (J. Hazard. Mater.; 280: 356-363, 2014). Our model can be used to compare anti-viral abilities of various anti-viral agents, determine appropriate coating areal density of anti-viral agent on a filter, and predict the life cycle of an anti-viral filter. PMID:26434534

  10. 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

  11. Evaluation of watershed-derived mass loads to prioritize TMDL decision-making.

    PubMed

    Gulati, S; Stubblefield, A A; Hanlon, J S; Spier, C L; Camarillo, M K; Stringfellow, W T

    2016-01-01

    A total maximum daily load (TMDL) for oxygen demanding substances is being implemented in the San Joaquin River (SJR) in California (USA) due to frequently occurring low dissolved oxygen conditions. The SJR is a eutrophic river, heavily impacted by agriculture. A mass balance was developed to identify the sources of oxygen-demanding substances and nutrients to the river with the objective of providing a scientific basis for management actions needed to meet TMDL requirements. Data were collected for flow and water quality and mass loads calculated for sites within the main stem of the SJR, river inputs (tributaries), and diversions in the study area. Using a quadrant analysis, tributary flows and loads are ranked to identify targets for water quality improvement efforts. Additionally, all mass loads were summed (inputs minus diversions) and compared with observed loads at the downstream limit of the study area. The mass balance analysis identifies major contributors of mass loads and mass balance closure is assessed for each constituent. These analysis methods inform the TMDL process which includes a load allocation, and is useful for determining locations for implementation of improvement projects needed to improve the health of the river. PMID:26877050

  12. Tungsten quasispherical wire loads with a profiled mass

    SciTech Connect

    Grabovskii, E. V.; Dzhangobegov, V. V. Oleinik, G. M.; Rodionov, R. N.

    2015-12-15

    Wire arrays made from micrometer tungsten wires with linear mass profiled along their height are developed for experiments on the generation of X-ray radiation upon pinch compression with a current of ∼3 MA at a pulse duration of ∼100 ns. Wires are imaged with a scanning electron microscope, and their diameter is determined. It is shown that the arrays have such a profile of height distribution of linear mass that allows for compact spherical compression upon current implosion.

  13. Molecular Characterization of Organic Aerosols Using Nanospray Desorption/Electrospray Ionization-Mass Spectrometry

    SciTech Connect

    Roach, Patrick J.; Laskin, Julia; Laskin, Alexander

    2010-10-01

    Nanospray desorption electrospray ionization (Nano-DESI) combined with high-resolution mass spectrometry (HR/MS) is a promising approach for detailed chemical characterization of atmospheric organic aerosol (OA) collected in laboratory and field experiments. In Nano-DESI analyte is desorbed into a solvent bridge formed between two capillaries and the analysis surface, which enables fast and efficient characterization of OA collected on substrates without special sample preparation. Stable signals achieved using Nano-DESI make it possible to obtain high-quality HR/MS data using only a small amount of material (<10 ng). Furthermore, Nano-DESI enables efficient detection of chemically labile compounds in OA, which is important for understanding chemical aging phenomena.

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

    SciTech Connect

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

    2009-09-01

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

  15. The post-pinatubo evolution of stratospheric aerosol surface area density as inferred from SAGE 2

    NASA Technical Reports Server (NTRS)

    Poole, L. R.; Thomason, L. W.

    1994-01-01

    Following the eruption of Mount Pinatubo in June of 1991, the aerosol mass loading of the stratosphere increased from -1 Mt to approximately 30 Mt. This change in aerosol loading was responsible for numerous radiative and chemical changes observed within the stratosphere. As a result, the ability to quantify aerosol properties on a global basis during this period is important. Aerosol surface area density is a critical parameter in governing the rates of heterogeneous reactions, such as ClONO2 plus H2O yields HNO3 plus HOCl, which influence the stratospheric abundance of ozone. Following the eruption of Mt. Pinatubo, measurements by the Stratospheric Aerosol and Gas Experiment (SAGE 2) indicated that the stratospheric aerosol surface area density increased by as much as a factor of 100. Using SAGE 2 multi-wavelength aerosol extinction data, aerosol surface area density as well as mass are derived for the period following the eruption of Mt. Pinatubo through the present.

  16. Maximum von Mises Stress in the Loading Environment of Mass Acceleration Curve

    NASA Technical Reports Server (NTRS)

    Glaser, Robert J.; Chen, Long Y.

    2006-01-01

    Method for calculating stress due to acceleration loading: 1) Part has been designed by FEA and hand calculation in one critical loading direction judged by the analyst; 2) Maximum stress can be due to loading in another direction; 3) Analysis procedure to be presented determines: a) The maximum Mises stress at any point; and b) The direction of maximum loading associated with the "stress". Concept of Mass Acceleration Curves (MAC): 1) Developed by JPL to perform preliminary structural sizing (i.e. Mariners, Voyager, Galileo, Pathfinder, MER,...MSL); 2) Acceleration of physical masses are bounded by a curve; 3) G-levels of vibro-acoustic and transient environments; 4) Convergent process before the couple loads cycle; and 5) Semi-empirical method to effectively bound the loads, not a simulation of the actual response.

  17. 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

  18. Diffusion loading and drug delivery characteristics of alginate gel microparticles produced by a novel impinging aerosols method.

    PubMed

    Hariyadi, Dewi M; Lin, Sharon Chien-Yu; Wang, Yiwei; Bostrom, Thor; Turner, Mark S; Bhandari, Bhesh; Coombes, Allan G A

    2010-12-01

    Microencapsulation of a hydrophilic active (gentamicin sulphate (GS)) and a hydrophobic non-steroidal anti-inflammatory drug (ibuprofen) in alginate gel microparticles was accomplished by molecular diffusion of the drug species into microparticles produced by impinging aerosols of alginate solution and CaCl(2) cross-linking solution. A mean particle size in the range of 30-50 µm was measured using laser light scattering and high drug loadings of around 35 and 29% weight/dry microparticle weight were obtained for GS and ibuprofen respectively. GS release was similar in simulated intestinal fluid (phosphate buffer saline (PBS), pH 7.4, 37°C) and simulated gastric fluid (SGF) (HCl, pH 1.2, 37°C) but was accelerated in PBS following incubation of microparticles in HCl. Ibuprofen release was restricted in SGF but occurred freely on transfer of microparticles into PBS with almost 100% efficiency. GS released in PBS over 7 h, following incubation of microparticles in HCl for 2 h was found to retain at least 80% activity against Staphylococcus epidermidis while Ibuprofen retained around 50% activity against Candida albicans. The impinging aerosols technique shows potential for producing alginate gel microparticles of utility for protection and controlled delivery of a range of therapeutic molecules.

  19. Extremely high aerosol loading over Arabian Sea during June 2008: The specific role of the atmospheric dynamics and Sistan dust storms

    NASA Astrophysics Data System (ADS)

    Kaskaoutis, D. G.; Rashki, A.; Houssos, E. E.; Goto, D.; Nastos, P. T.

    2014-09-01

    This study focuses on analyzing the extreme aerosol loading and the mechanisms, source areas and meteorological conditions that favored the abnormal dust exposure towards Arabian Sea during June 2008. The analysis reveals that the spatial-averaged aerosol optical depth (AOD) over Arabian Sea in June 2008 is 0.5 (78.2%) higher than the 2000-2013 mean June value and is mostly attributed to the enhanced dust activity and several (18) dust storms originated from the Sistan region (Iran-Afghanistan borders). Landsat images show that the marshy lakes in Sistan basin got dried during the second half of June 2008 and the alluvial silt and saline material got easily eroded by the intense Levar winds, which were stronger (>15-20 m s-1) than the climatological mean for the month of June. These conditions led to enhanced dust exposure from Sistan that strongly affected the northern and central parts of the Arabian Sea, as forward air-mass trajectories show. The NCEP/NCAR reanalysis reveals an abnormal intensification and spatial expansion of the Indian low pressure system towards northern Arabian Sea in June 2008. This suggests strengthening of the convection over the arid southwest Asia and exposure of significant amount of dust, which can reach further south over Arabian Sea favored by the enhanced cyclonic circulation. MODIS imagery highlighted several dust storms originated from Sistan and affecting Arabian Sea during June 2008, while the SPRINTARS model simulations of increased AOD and dust concentration over Sistan and downwind areas are in agreement with ground-based and satellite observations.

  20. Realization of polyaspartamide-based nanoparticles and in vivo lung biodistribution evaluation of a loaded glucocorticoid after aerosolization in mice.

    PubMed

    Craparo, E F; Di Gioia, S; Trapani, A; Cellamare, S; Belgiovine, G; Mandracchia, D; Giammona, G; Cavallaro, G; Conese, M

    2016-08-20

    In this study, novel polymeric nanoparticles (NPs) were developed and their potential as carriers for beclomethasone dipropionate (BDP) into the lung after aerosolization was demonstrated by in vivo studies in mice. In particular, these NPs were obtained starting from two polyaspartamide-based copolymers which were synthesized by chemical reaction of α,β-poly(N-2-hydroxyethyl)-dl-aspartamide (PHEA) and its pegylated derivative (PHEA-PEG2000) with poly(lactic acid) (PLA). To obtain nanosized particles, the high pressure homogenization (HPH)-solvent evaporation method was followed by using an organic phase containing both PHEA-PLA and PHEA-PEG2000-PLA (at a weight ratio equal to 1:1), lactose as cryoprotectant and no surfactant was adopted. PHEA-PLA/PHEA-PEG2000-PLA NPs were characterized by a quite spherical shape, ζ potential slightly negative, and size lower than 50 and 200nm, respectively, for empty and BDP-loaded NPs. In vivo biodistribution of BDP and its metabolites in various lung compartments, i.e. bronchoalveolar lavage fluid (BALF), alveolar macrophages (MPG) obtained from BALF, and lung tissue, was carried out at 3h post-administration in mice by aerosolization of BDP-loaded NPs or free BDP (commercial formulation, Clenil(®)) at the dose of 0.5mg/kg BDP. Results demonstrated that BDP entrapped into NPs reached all analyzed lung compartments and were internalized by both alveolar MPG and respiratory epithelial cells, and detected amounts were comparable to those of Clenil-treated mice. Moreover, the entrapment into NPs protects the drug from the enzymatic hydrolysis, allowing a significant lower amount of beclomethasone (BOH) into the lung tissue and BALF than that obtained after Clenil administration. PMID:27326484

  1. Mass spectrometric analysis and aerodynamic properties of various types of combustion-related aerosol particles

    NASA Astrophysics Data System (ADS)

    Schneider, J.; Weimer, S.; Drewnick, F.; Borrmann, S.; Helas, G.; Gwaze, P.; Schmid, O.; Andreae, M. O.; Kirchner, U.

    2006-12-01

    Various types of combustion-related particles in the size range between 100 and 850 nm were analyzed with an aerosol mass spectrometer and a differential mobility analyzer. The measurements were performed with particles originating from biomass burning, diesel engine exhaust, laboratory combustion of diesel fuel and gasoline, as well as from spark soot generation. Physical and morphological parameters like fractal dimension, effective density, bulk density and dynamic shape factor were derived or at least approximated from the measurements of electrical mobility diameter and vacuum aerodynamic diameter. The relative intensities of the mass peaks in the mass spectra obtained from particles generated by a commercial diesel passenger car, by diesel combustion in a laboratory burner, and by evaporating and re-condensing lubrication oil were found to be very similar. The mass spectra from biomass burning particles show signatures identified as organic compounds like levoglucosan but also others which are yet unidentified. The aerodynamic behavior yielded a fractal dimension (Df) of 2.09 +/- 0.06 for biomass burning particles from the combustion of dry beech sticks, but showed values around three, and hence more compact particle morphologies, for particles from combustion of more natural oak. Scanning electron microscope images confirmed the finding that the beech combustion particles were fractal-like aggregates, while the oak combustion particles displayed a much more compact shape. For particles from laboratory combusted diesel fuel, a Df value of 2.35 was found, for spark soot particles, Df [approximate] 2.10. The aerodynamic properties of fractal-like particles from dry beech wood combustion indicate an aerodynamic shape factor [chi] that increases with electrical mobility diameter, and a bulk density of 1.92 g cm-3. An upper limit of [chi] [approximate] 1.2 was inferred for the shape factor of the more compact particles from oak combustion.

  2. High-Resolution Mass Spectroscopic Analysis of Secondary Organic Aerosol Generated by Ozonolysis of Isoprene

    SciTech Connect

    Nguyen, Tran B; Bateman, Adam P; Bones, David L; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2010-02-01

    The chemical composition of secondary organic aerosol (SOA) generated from the ozonolysis of isoprene (C5H8) in the presence of an OH scavenger was examined using high-resolution electrospray ionization mass spectrometry (ESI-MS). The chemical composition of SOA is complex, with more than 1000 assigned peaks observed in the positive and negative ion mode spectra. Only a small fraction of peaks corresponds to known products of isoprene oxidation, such as pyruvic acid, glycolic acid, methylglyoxal, etc. The absolute majority of the detected peaks correspond to highly oxidized oligomeric constituents of SOA, with an average O:C molar ratio of ~0.6. The corresponding organic mass (OM) to organic oxygen (OO) ratio is OM/OO ~2.4. Approximately 8% of oxygen atoms in SOA are in the form of peroxides as quantified with an iodide test. Double bond equivalency (DBE) factors, representing the sum of all double bonds and rings, increase by 1 for every 2-3 additional carbon atoms in the molecule. The prevalent oligomer building blocks are therefore carbonyls or carboxylic acids with a C2-C3 skeleton. Kendrick analysis suggests that simple aldehydes, specifically formaldehyde, acetaldehyde, and methylglyoxal can serve as monomeric building blocks in the observed oligomers. The large number of reactive functional groups, especially organic peroxides and carbonyls, suggests that isoprene/O3 SOA should be prone to chemical and photochemical aging.

  3. Ion mobility-mass spectrometry with a radial opposed migration ion and aerosol classifier (ROMIAC).

    PubMed

    Mui, Wilton; Thomas, Daniel A; Downard, Andrew J; Beauchamp, Jesse L; Seinfeld, John H; Flagan, Richard C

    2013-07-01

    The first application of a novel differential mobility analyzer, the radial opposed migration ion and aerosol classifier (ROMIAC), is demonstrated. The ROMIAC uses antiparallel forces from an electric field and a cross-flow gas to both scan ion mobilities and continuously transmit target mobility ions with 100% duty cycle. In the ROMIAC, diffusive losses are minimized, and resolution of ions, with collisional cross-sections of 200-2000 Å(2), is achieved near the nondispersive resolution of ~20. Higher resolution is theoretically possible with greater cross-flow rates. The ROMIAC was coupled to a linear trap quadrupole mass spectrometer and used to classify electrosprayed C2-C12 tetra-alkyl ammonium ions, bradykinin, angiotensin I, angiotensin II, bovine ubiquitin, and two pairs of model peptide isomers. Instrument and mobility calibrations of the ROMIAC show that it exhibits linear responses to changes in electrode potential, making the ROMIAC suitable for mobility and cross-section measurements. The high resolution of the ROMIAC facilitates separation of isobaric isomeric peptides. Monitoring distinct dissociation pathways associated with peptide isomers fully resolves overlapping peaks in the ion mobility data. The ability of the ROMIAC to operate at atmospheric pressure and serve as a front-end analyzer to continuously transmit ions with a particular mobility facilitates extensive studies of target molecules using a variety of mass spectrometric methods. PMID:23730869

  4. Method for characterization of low molecular weight organic acids in atmospheric aerosols using ion chromatography mass spectrometry.

    PubMed

    Brent, Lacey C; Reiner, Jessica L; Dickerson, Russell R; Sander, Lane C

    2014-08-01

    The structural composition of PM2.5 monitored in the atmosphere is usually divided by the analysis of organic carbon, black (also called elemental) carbon, and inorganic salts. The characterization of the chemical composition of aerosols represents a significant challenge to analysts, and studies are frequently limited to determination of aerosol bulk properties. To better understand the potential health effects and combined interactions of components in aerosols, a variety of measurement techniques for individual analytes in PM2.5 need to be implemented. The method developed here for the measurement of organic acids achieves class separation of aliphatic monoacids, aliphatic diacids, aromatic acids, and polyacids. The selective ion monitoring capability of a triple quadropole mass analyzer was frequently capable of overcoming instances of incomplete separations. Standard Reference Material (SRM) 1649b Urban Dust was characterized; 34 organic acids were qualitatively identified, and 6 organic acids were quantified.

  5. [Application of on-line single particle aerosol mass spectrometry (SPAMS) for studying major components in fine particulate matter].

    PubMed

    Fu, Huai-yu; Yan, Cai-qing; Zheng, Mei; Cai, Jing; Li, Xiao-ying; Zhang, Yan-jun; Zhou Zhen; Fu, Zhong; Li, Mei; Li, Lei; Zhang, Yuan-Hang

    2014-11-01

    Based on preliminary studies by aerosol time-of-flight mass spectrometer (ATOFMS) and single particle aerosol mass spectrometer (SPAMS), typical methods for identifying the number of particles (or particle count) for five major components including sulfate, nitrate, ammonium, organic carbon (OC), and elemental carbon (EC) in China and abroad were summarized. In this study, combined with the characteristics of single particle mass spectrum by SPAMS, an optimized method is proposed. With field measurement using SPAMS during January 2013 in Beijing, particle counts of sulfate, nitrate, ammonium, OC, and EC determined by different methods were compared. The comparison with results of off-line filter analyses for these five components proved that the method proposed in this study is comparable and optimized. We also suggest factors needed to be considered in future application of SPAMS and other areas that require in-depth research. PMID:25639078

  6. A correlation equation for the mass median aerodynamic diameter of the aerosol emitted by solution metered dose inhalers.

    PubMed

    Ivey, James W; Lewis, David; Church, Tanya; Finlay, Warren H; Vehring, Reinhard

    2014-04-25

    A correlation equation for the mass median aerodynamic diameter (MMAD) of the aerosol emitted by solution metered dose inhalers (MDIs) is presented. A content equivalent diameter is defined and used to describe aerosols generated by evaporating metered dose inhaler sprays. A large set of cascade impaction data is analyzed, and the MMAD and geometric standard deviation is calculated for each datum. Using dimensional analysis, the mass median content equivalent diameter is correlated with formulation variables. Based on this correlation in combination with mass balance considerations and the definition of the aerodynamic diameter, an equation for prediction of the MMAD of an inhaler given the pressure of the propellant in the metering chamber of the MDI valve and the surface tension of the propellant is derived. The accuracy of the correlation equation is verified by comparison with literature results. The equation is applicable to both HFA (hydrofluoroalkane) propellants 134a and 227ea, with varying levels of co-solvent ethanol.

  7. [Application of on-line single particle aerosol mass spectrometry (SPAMS) for studying major components in fine particulate matter].

    PubMed

    Fu, Huai-yu; Yan, Cai-qing; Zheng, Mei; Cai, Jing; Li, Xiao-ying; Zhang, Yan-jun; Zhou Zhen; Fu, Zhong; Li, Mei; Li, Lei; Zhang, Yuan-Hang

    2014-11-01

    Based on preliminary studies by aerosol time-of-flight mass spectrometer (ATOFMS) and single particle aerosol mass spectrometer (SPAMS), typical methods for identifying the number of particles (or particle count) for five major components including sulfate, nitrate, ammonium, organic carbon (OC), and elemental carbon (EC) in China and abroad were summarized. In this study, combined with the characteristics of single particle mass spectrum by SPAMS, an optimized method is proposed. With field measurement using SPAMS during January 2013 in Beijing, particle counts of sulfate, nitrate, ammonium, OC, and EC determined by different methods were compared. The comparison with results of off-line filter analyses for these five components proved that the method proposed in this study is comparable and optimized. We also suggest factors needed to be considered in future application of SPAMS and other areas that require in-depth research.

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

    PubMed

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

    2013-06-01

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

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

    PubMed

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

    2013-06-01

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

  10. The impact of natural aerosols on Indian summer monsoon

    NASA Astrophysics Data System (ADS)

    Vinoj, V.; Wang, H.; Yoon, J.; Rasch, P.

    2011-12-01

    Atmospheric aerosols emitted from a variety of natural and anthropogenic sources impact the earth's radiation and water budget. Most of the studies in the recent past have been focusing on anthropogenic aerosols and their impact. However, natural aerosols like sea-salt and dust form the bulk of the aerosol mass loading in the atmosphere. For example, oceans cover about 70% of the earth's surface area and are a major source of sea-salt aerosols in the atmosphere. Sea-salt emission is the single largest contributor to natural aerosols and accounts for nearly half of the global aerosol optical depth. Dust emission, the counterpart over land, also contributes substantially to natural atmospheric aerosols. In addition to their direct effect on solar radiation, these aerosols also actively participate in cloud formation by acting as cloud condensation and ice nuclei and have indirect effects on clouds. Both sea-salt and dust particles are primarily formed by the action of winds that largely determine seasonal/annual variations in their source strength and atmospheric loading. Over the Indian Ocean region, especially the Arabian Sea is characterized by high winds during the monsoon that generate a large amount of sea-salt aerosols. Also these high winds mobilize large amount of dust aerosols in the northern Arabian Sea depending on wind direction. These natural aerosols together with anthropogenic emissions impact Indian monsoon precipitation. We use satellite observation of precipitation and column aerosol loading along with a global climate model (Community Atmosphere Model version 5, CAM5) to show that the variability of natural aerosols (i.e., sea-salt and dust) play an important role in modulating the Indian monsoon precipitation and the response of the monsoon system to anthropogenic aerosols. The effect of dust and sea-salt on precipitation is found to be opposite to each other. Our study suggests that the observed spatial and temporal trends in precipitation

  11. Two-dimensional titanium carbide electrode with large mass loading for supercapacitor

    NASA Astrophysics Data System (ADS)

    Lin, Shuang-Yan; Zhang, Xitian

    2015-10-01

    Layered titanium carbide (Ti3C2) has been synthesized by exfoliation of ternary carbides Ti3AlC2 and evaluated as working electrodes with different mass loading from 1.8 mg to 7.6 mg. The effect of mass loading on the electrochemical properties of Ti3C2 electrodes was studied by cyclic voltammetry (CV), galvanostatic charge-discharge (GCD) and impedance spectrum test. With increasing of Ti3C2 mass from 1.8 to 7.6 mg/cm2 in electrode, the specific capacitance calculated from the CV curves at 2 mV/s decreases at first from 117 to 78 F/g then maintains at 76 F/g, while areal capacitance increases from 211 to 579 mF/cm2. Moreover, both electrodes with low mass loading (1.8 mg) and large mass loading (7.6 mg) have delivered good cycling performances with capacitance retention of 97% and 98% after 10000 cycles. These results indicate that large mass loading electrode retains high specific capacitance and good cycling stability, due to the excellent electronic conductivity and layered structure of Ti3C2.

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

    NASA Astrophysics Data System (ADS)

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

    2012-02-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2016-03-01

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

  14. Effect of tubing deposition, breathing pattern, and temperature on aerosol mass distribution measured by cascade impactor.

    PubMed

    Gurses, Burak K; Smaldone, Gerald C

    2003-01-01

    Aerosols produced by nebulizers are often characterized on the bench using cascade impactors. We studied the effects of connecting tubing, breathing pattern, and temperature on mass-weighted aerodynamic particle size aerosol distributions (APSD) measured by cascade impaction. Our experimental setup consisted of a piston ventilator, low-flow (1.0 L/min) cascade impactor, two commercially available nebulizers that produced large and small particles, and two "T"-shaped tubes called "Tconnector(cascade)" and "Tconnector(nebulizer)" placed above the impactor and the nebulizer, respectively. Radiolabeled normal saline was nebulized using an airtank at 50 PSIG; APSD, mass balance, and Tconnector(cascade) deposition were measured with a gamma camera and radioisotope calibrator. Flow through the circuit was defined by the air tank (standing cloud, 10 L/min) with or without a piston pump, which superimposed a sinusoidal flow on the flow from the air tank (tidal volume and frequency of breathing). Experiments were performed at room temperature and in a cooled environment. With increasing tidal volume and frequency, smaller particles entered the cascade impactor (decreasing MMAD; e.g., Misty-Neb, 4.2 +/- 0.9 microm at lowest ventilation and 2.7 +/- 0.1 microm at highest, p = 0.042). These effects were reduced in magnitude for the nebulizer that produced smaller particles (AeroTech II, MMAD 1.8 +/- 0.1 to 1.3 +/- 0.1 microm; p = 0.0044). Deposition on Tconnector(cascade) increased with ventilation but was independent of cascade impactor flow. Imaging of the Tconnector(cascade) revealed a pattern of deposition unaffected by cascade impactor flow. These measurements suggest that changes in MMAD with ventilation were not artifacts of tubing deposition in the Tconnector(cascade). At lower temperatures, APSD distributions were more polydisperse. Our data suggest that, during patient inhalation, changes in particle distribution occur that are related to conditions in the tubing and

  15. 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

  16. 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.

  17. Characterization of the sources and processes of organic and inorganic aerosols in New York city with a high-resolution time-of-flight aerosol mass apectrometer

    NASA Astrophysics Data System (ADS)

    Sun, Y.-L.; Zhang, Q.; Schwab, J. J.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2011-02-01

    Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer during the summer 2009 Field Intensive Study at Queens College in New York, NY. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of the total PM1 mass. The average mass-based size distribution of OA presents a small mode peaking at ~150 nm (Dva) and an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of both sulfate and OA peak between 01:00-02:00 p.m. EST due to photochemical production. The average (±σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012 (±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62 (±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified two primary OA (POA) sources, traffic and cooking, and three secondary OA (SOA) components including a highly oxidized, regional low-volatility oxygenated OA (LV-OOA; O/C = 0.63), a less oxidized, semi-volatile SV-OOA (O/C = 0.38) and a unique nitrogen-enriched OA (NOA; N/C = 0.053) characterized with prominent CxH2x + 2N+ peaks likely from amino compounds. Our results indicate that cooking and traffic are two distinct and mass-equivalent POA sources in NYC, together contributing ~30% of the total OA mass during this study. The OA composition is dominated by secondary species, especially during high PM events. SV-OOA and LV-OOA on average account for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC appears to progress with a continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA) presents evidence that organic nitrogen

  18. Characterization of the sources and processes of organic and inorganic 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.; Demerjian, K. L.; Chen, W.-N.; Bae, M.-S.; Hung, H.-M.; Hogrefe, O.; Frank, B.; Rattigan, O. V.; Lin, Y.-C.

    2010-10-01

    Submicron aerosol particles (PM1) were measured in-situ using a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) during the summer 2009 Field Intensive Study at Queens College in New York City. Organic aerosol (OA) and sulfate are the two dominant species, accounting for 54% and 24%, respectively, of total PM1 mass on average. The average mass size distribution of OA presents a small mode peaking at ~150 nm (Dva) in addition to an accumulation mode (~550 nm) that is internally mixed with sulfate, nitrate, and ammonium. The diurnal cycles of sulfate and OA both show pronounced peaks between 01:00-02:00 p.m. EST due to photochemical production. The average (±1σ) oxygen-to-carbon (O/C), hydrogen-to-carbon (H/C), and nitrogen-to-carbon (N/C) ratios of OA in NYC are 0.36 (±0.09), 1.49 (±0.08), and 0.012(±0.005), respectively, corresponding to an average organic mass-to-carbon (OM/OC) ratio of 1.62(±0.11). Positive matrix factorization (PMF) of the high resolution mass spectra identified five OA components: a hydrocarbon-like OA (HOA), two types of oxygenated OA (OOA) including a low-volatility OOA (LV-OOA) and a semi-volatile OOA (SV-OOA), a cooking-emission related OA (COA), and a unique nitrogen-enriched OA (NOA). HOA appears to represent primary OA (POA) from urban traffic emissions. It comprises primarily of reduced species (H/C=1.83; O/C=0.06) and shows a mass spectral pattern very similar to those of POA from fossil fuel combustion, and correlates tightly with traffic emission tracers including elemental carbon and NOx. LV-OOA, which is highly oxidized (O/C=0.63) and correlates well with sulfate, appears to be representative for regional, aged secondary OA (SOA). SV-OOA, which is less oxidized (O/C=0.38) and correlates well with non-refractory chloride, likely represents less photo-chemically aged, semi-volatile SOA. COA shows a similar spectral pattern to the reference spectra of POA from cooking emissions and a distinct diurnal pattern

  19. Assessment of the Interactions Among Tropospheric Aerosol Loading, Radiative Balance and Clouds Through Examination of Their Multi-decadal Trends

    EPA Science Inventory

    While aerosol radiative effects have been recognized as some of the largest sources of uncertainty among the forcers of climate change, the verification of the spatial and temporal variability of aerosol radiative forcing has remained challenging. Anthropogenic emissions of prima...

  20. Chemical Analysis of Organic Aerosols Using Reactive Nanospray Desorption Electrospray Ionization Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Laskin, A.; Laskin, J.; Nizkorodov, S.

    2013-12-01

    Nanospray Desorption Electrospray Ionization (nano-DESI) technique integrated with high resolution mass spectrometry (HR-MS) enables molecular level analysis of organic aerosol (OA) samples. In nano-DESI, analyte is desorbed into a small volume solvent bridge formed between two capillaries positioned in contact with analyte and enables fast and efficient characterization of OA collected on substrates without sample preparation. We report applications of the nano-DESI/HR-MS approach in a number of our recent studies focused on molecular identification of organic compounds in laboratory and in field collected OA samples. Reactive nano-DESI approach where selected reagent is added to the solvent is used for examining the presence of individual species containing specific functional groups and for their quantification within complex mixtures of OA. Specifically, we use the Girard's reagent T (GT) to probe and quantify carbonyl compounds in the SOA mixtures. We estimate for the first time the amounts of dimers and trimers in the SOA mixtures. We found that the most abundant dimer in limonene/O3 SOA was detected at the ˜0.5 pg level and the total amount of dimers and trimers in the analyzed sample was ˜11 pg. Understanding of the OA composition at the molecular level allowed us to identify key aging reactions, including the transformation of carbonyls to imines and carbonyl-imine oligomerization, that may contribute to the formation of brown carbon in the atmosphere.

  1. 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

  2. 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

  3. Characterization of a real-time tracer for isoprene epoxydiols-derived secondary organic aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    DOE PAGES

    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

  4. Impact of plasma induced liquid chemistry and charge on bacteria loaded aerosol droplets

    NASA Astrophysics Data System (ADS)

    Rutherford, David; McDowell, David; Mariotti, Davide; Mahony, Charles; Diver, Declan; Potts, Hugh; Bennet, Euan; Maguire, Paul

    2014-10-01

    The introduction of living organisms, such as bacteria, into atmospheric pressure microplasmas offers a unique opportunity to study the local chemical and electrical effects on cell structure and viability. Individual bacteria, each encapsulated in an aerosol droplet, were successfully transmitted through a non-thermal equilibrium RF coaxial plasma, using a custom-design concentric double gas shroud interface and via adjustment of transit times and plasma parameters, we can control cell viability. Plasma electrical characteristics (ne ~ 1013 cm-3), droplet velocity profiles and aspects of plasma-induced droplet chemistry were determined in order to establish the nature of the bacteria in droplet environment. Plasma-exposed viable E coli cells were subsequently cultured and the growth rate curves (lag and exponential phase gradient) used to explore the effect of radical chemistry and electron bombardment on cell stress. The extent and nature of membrane disruption in viable and non-viable cells were investigated through genomic and protein/membrane lipid content estimation. We will also compare our results with simulations of the effect of bacterial presence on plasma induced droplet charging and evaporation. Funding from EPSRC acknowledged (Grants EP/K006088/1 and EP/K006142/1).

  5. High loading of nanostructured ceramics in polymer composite thick films by aerosol deposition

    PubMed Central

    2012-01-01

    Low temperature fabrication of Al2O3-polyimide composite substrates was carried out by an aerosol deposition process using a mixture of Al2O3 and polyimide starting powders. The microstructures and dielectric properties of the composite thick films in relation to their Al2O3 contents were characterized by X-ray diffraction analysis. As a result, the crystallite size of α-Al2O3 calculated from Scherrer's formula was increased from 26 to 52 nm as the polyimide ratio in the starting powders increased from 4 to 12 vol.% due to the crushing of the Al2O3 powder being reduced by the shock-absorbing effect of the polyimide powder. The Al2O3-polyimide composite thick films showed a high loss tangent with a large frequency dependence when a mixed powder of 12 vol.% polyimide was used due to the nonuniform microstructure with a rough surface. The Al2O3-polyimide composite thick films showed uniform composite structures with a low loss tangent of less than 0.01 at 1 MHz and a high Al2O3 content of more than 75 vol.% when a mixed powder of 8 vol.% polyimide was used. Moreover, the Al2O3-polyimide composite thick films had extremely high Al2O3 contents of 95 vol.% and showed a dense microstructure close to that of the Al2O3 thick films when a mixed powder of 4 vol.% polyimide was used. PMID:22283973

  6. 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.

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

    SciTech Connect

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

    2010-10-01

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

  8. The Structure of Magnetocentrifugal Jets and Winds I. Steady Mass Loading

    SciTech Connect

    Anderson, J.

    2004-12-15

    We present the results of a series of time-dependent numerical simulations of cold, magnetocentrifugally launched winds from accretion disks. The goal of this study is to determine how the mass loading from the disk affects the structure and dynamics of the wind for a given distribution of magnetic field. Our simulations span four and half decades of mass loading; in the context of a disk with a launching region from 0.1 AU to 1.0 AU around a 1M{circle_dot} star and a field strength of about 20 G at the inner disk edge, this amounts to mass loss rates of 1 x 10{sup -9} - 3 x 10{sup -5} M{circle_dot} yr{sup -1} from each side of the disk. We find that, as expected intuitively, the degree of collimation of the wind increases with mass loading; however even the ''lightest'' wind simulated is significantly collimated compared with the force-free magnetic configuration of the same magnetic flux distribution at the launching surface, which becomes radial at large distances. The implication is that for flows from young stellar objects a radial field approximation is inappropriate. Surprisingly, the terminal velocity of the wind and the magnetic lever arm are still well-described by the analytical solutions for a radial field geometry. We also find that the isodensity contours and Alfven surface are very nearly self-similar in mass loading. The wind becomes unsteady above some critical mass loading rate. The exact value of the critical rate depends on the (small) velocity with which we inject the material into the wind. For a small enough injection speed, we are able to obtain the first examples of a class of heavily-loaded magnetocentrifugal winds with magnetic fields completely dominated by the toroidal component all the way to the launching surface. The stability of such toroidally dominated winds in 3D will be the subject of a future investigation.

  9. Floating Offshore WTG Integrated Load Analysis & Optimization Employing a Tuned Mass Damper

    SciTech Connect

    Rodriguez Tsouroukdissian, Arturo; Lackner, Matt; Cross-Whiter, John; Ackers, Ben; Arora, Dhiraj; Park, Semiung

    2015-09-25

    Floating offshore wind turbines (FOWTs) present complex design challenges due to the coupled dynamics of the platform motion, mooring system, and turbine control systems, in response to wind and wave loading. This can lead to higher extreme and fatigue loads than a comparable fixed bottom or onshore system. Previous research[1] has shown the potential to reduced extreme and fatigue loads on FOWT using tuned mass dampers (TMD) for structural control. This project aims to reduce maximum loads using passive TMDs located at the tower top during extreme storm events, when grid supplied power for other controls systems may not be available. The Alstom Haliade 6MW wind turbine is modelled on the Glosten Pelastar tension-leg platform (TLP). The primary objectives of this project are to provide a preliminary assessment of the load reduction potential of passive TMDs on real wind turbine and TLP designs.

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

    SciTech Connect

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

    2012-09-11

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

  11. On the deceleration of Fanaroff-Riley Class I jets: mass loading by stellar winds

    NASA Astrophysics Data System (ADS)

    Perucho, M.; Martí, J. M.; Laing, R. A.; Hardee, P. E.

    2014-06-01

    Jets in low-luminosity radio galaxies are known to decelerate from relativistic speeds on parsec scales to mildly or subrelativistic speeds on kiloparsec scales. Several mechanisms have been proposed to explain this effect, including strong reconfinement shocks and the growth of instabilities (both leading to boundary-layer entrainment) and mass loading from stellar winds or molecular clouds. We have performed a series of axisymmetric simulations of the early evolution of jets in a realistic ambient medium to probe the effects of mass loading from stellar winds using the code RATPENAT. We study the evolution of Fanaroff-Riley Class I (FR I) jets, with kinetic powers Lj ˜ 1041-1044 erg s-1, within the first 2 kpc of their evolution, where deceleration by stellar mass loading should be most effective. Mass entrainment rates consistent with present models of stellar mass loss in elliptical galaxies produce deceleration and effective decollimation of weak FR I jets within the first kiloparsec. However, powerful FR I jets are not decelerated significantly. In those cases where the mass loading is important, the jets show larger opening angles and decollimate at smaller distances, but the overall structure and dynamics of the bow shock are similar to those of unloaded jets with the same power and thrust. According to our results, the flaring observed on kiloparsec scales is initiated by mass loading in the weaker FR I jets and by reconfinement shocks or the growth of instabilities in the more powerful jets. The final mechanism of decollimation and deceleration is always the development of disruptive pinching modes.

  12. Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications

    DOE PAGES

    Canagaratna, M. R.; Jimenez, J. L.; Kroll, J. H.; Chen, Q.; Kessler, S. H.; Massoli, P.; Hildebrandt Ruiz, L.; Fortner, E.; Williams, L. R.; Wilson, K. R.; et al

    2015-01-12

    Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), and organic mass-to-organic carbon (OM : OC) ratios, and of carbon oxidation state (OS C) for a vastly expanded laboratory data set of multifunctional oxidized OA standards. For the expanded standard data set, the method introduced by Aiken et al. (2008), which uses experimentally measured ion intensities at all ions to determinemore » elemental ratios (referred to here as "Aiken-Explicit"), reproduces known O : C and H : C ratio values within 20% (average absolute value of relative errors) and 12%, respectively. The more commonly used method, which uses empirically estimated H2O+ and CO+ ion intensities to avoid gas phase air interferences at these ions (referred to here as "Aiken-Ambient"), reproduces O : C and H : C of multifunctional oxidized species within 28 and 14% of known values. The values from the latter method are systematically biased low, however, with larger biases observed for alcohols and simple diacids. A detailed examination of the H2O+, CO+, and CO2+ fragments in the high-resolution mass spectra of the standard compounds indicates that the Aiken-Ambient method underestimates the CO+ and especially H2O+ produced from many oxidized species. Combined AMS–vacuum ultraviolet (VUV) ionization measurements indicate that these ions are produced by dehydration and decarboxylation on the AMS vaporizer (usually operated at 600 °C). Thermal decomposition is observed to be efficient at vaporizer temperatures down to 200 °C. These results are used together to develop an "Improved-Ambient" elemental analysis method for AMS spectra measured in air. The Improved-Ambient method uses specific ion

  13. Elemental ratio measurements of organic compounds using aerosol mass spectrometry: characterization, improved calibration, and implications

    DOE PAGES

    Canagaratna, M. R.; Jimenez, J. L.; Kroll, J. H.; Chen, Q.; Kessler, S. H.; Massoli, P.; Hildebrandt Ruiz, L.; Fortner, E.; Williams, L. R.; Wilson, K. R.; et al

    2014-07-31

    Elemental compositions of organic aerosol (OA) particles provide useful constraints on OA sources, chemical evolution, and effects. The Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) is widely used to measure OA elemental composition. This study evaluates AMS measurements of atomic oxygen-to-carbon (O : C), hydrogen-to-carbon (H : C), organic mass-to-organic carbon (OM : OC), and carbon oxidation state (OSC) for a vastly expanded laboratory dataset of multifunctional oxidized OA standards. For the expanded standard dataset, the "Aiken-Explicit" method (Aiken et al., 2008), which uses experimentally measured ion intensities at all ions to determine elemental ratios, reproduces known molecular O :more » C and H : C ratio values within 20% (average absolute value of relative errors) and 12% respectively. The more commonly used "Aiken-Ambient" method, which uses empirically estimated H2O+ and CO+ ion intensities to avoid gas phase air interferences at these ions, reproduces O : C and H : C of multifunctional oxidized species within 28% and 14% of known values. These values are systematically biased low, however, with larger biases observed for alcohols and simple diacids. A detailed examination of the H2O+, CO+, and CO2+ fragments in the high-resolution mass spectra of the standard compounds indicates that the Aiken-Ambient method underestimates the CO+ and H2O+ produced from many oxidized species. Combined AMS-vacuum ultraviolet (VUV) ionization measurements indicate that these ions are produced by dehydration and decarboxylation on the AMS vaporizer (usually operated at 600 °C). Thermal decomposition is observed to be efficient at vaporizer temperatures down to 200 °C. These results are used together to develop an "Improved-Ambient" elemental analysis method for AMS spectra measured in air. The Improved-Ambient method reduces the systematic biases and reproduces O : C (H : C) ratios of individual oxidized standards within 28% (13

  14. Isotopic mass independent signature of black crusts: a proxy for atmospheric aerosols formation in the Paris area (France).

    NASA Astrophysics Data System (ADS)

    Genot, Isabelle; Martin, Erwan; Yang, David Au; De Rafelis, Marc; Cartigny, Pierre; Wing, Boswell; Le Gendre, Erwann; Bekki, Slimane

    2016-04-01

    In view of the negative forcing of the sulfate aerosols on climate, a more accurate understanding of the formation of these particles is crucial. Indeed, despite the knowledge of their effects, uncertainties remain regarding the formation of sulfate aerosols, particularly the oxidation processes of S-bearing gases. Since the discovery of oxygen and sulfur mass independent fractionation (O- and S-MIF) processes on Earth, the sulfate isotopic composition became essential to investigate the atmospheric composition evolution and its consequences on the climate and the biosphere. Large amount of S-bearing compounds (SO2 mainly) is released into the atmosphere by anthropogenic and natural sources. Their oxidation in the atmosphere generates sulfate aerosols, H2SO4, which precipitate on the earth surface mainly as acid rain. One consequence of this precipitation is the formation of black crust on buildings made of carbonate stones. Indeed the chemical alteration of CaCO3 by H2SO4 leads to gypsum (CaSO4·2H2O) concretions on building walls. Associated to other particles, gypsum forms black-crusts. Therefore, black crusts acts as 'sulfate aerosol traps', meaning that their isotopic composition reveals the composition and thus the source and formation processes of sulfate aerosols in the atmosphere in a specific region. In this study we collected 37 black crusts on a 300km NW-SE profile centered on Paris (France). In our samples, sulfate represent 40wt.% and other particles 60wt.% of the black crusts. After sulfate extraction from each samples we measured their O- and S-isotopes composition. Variations of about 10‰ in δ18O and δ34S are observed and both O-MIF (Δ17O from 0 to 1.4‰) and S-MIF (Δ33S from 0 to -0.3‰) compositions have been measured. In regards to these compositions we can discuss the source and formation (oxidation pathways) of the sulfate aerosols in troposphere above the Paris region that covers urban, rural and coastal environments. Furthermore

  15. Weekly periodicities of aerosol properties observed at an urban location in India

    SciTech Connect

    Satheesh, S K; Vinoj, V; Moorthy, K Krishna

    2011-07-01

    Multi-year (~7 years) observations of aerosol optical and microphysical properties were conducted at a tropical urban location in Bangalore, India. As a consequence of rapid urbanization, Bangalore presents high local atmospheric emissions, which makes it an interesting site to study the effect of anthropogenic activities on aerosol properties. It has been found that both column (aerosol optical depth, AOD) and ground-level measurements (black carbon (BC) and composite aerosol mass) exhibit a weekly cycle with low aerosol concentrations on weekends. In comparison to the weekdays, the weekend reductions of aerosol optical depth, black carbon and composite aerosol mass concentrations were ~15%, 25% and 24%, respectively. The magnitude of weekend reduction of black carbon is as much as ~1 μg m-3. The similarity in the weekly cycle between the column and surface measurements suggests that the aerosol column loading at this location is governed by local anthropogenic emissions. The strongest weekly cycle in composite aerosol mass concentration was observed in the super micron mass range (>1 μm). The weekly cycle of composite aerosol mass in the sub micron mass range (<1 μm) was weak in comparison to the super micron aerosol mass.

  16. Chemical characterization of emissions from vegetable oil processing and their contribution to aerosol mass using the organic molecular markers approach.

    PubMed

    Kavouras, I G; Stratigakis, N; Stephanou, E G

    2001-04-01

    The organic fraction of aerosol emitted from a vegetable oil processing plant was studied to investigate the contribution of emissions to ambient particles in the surrounding area. Solvent-soluble particulate organic compounds emitted from the plant accounted for 10% of total suspended particles. This percentage was lower in the receptor sites (less than 6% of total aerosol mass). Nonpolar, moderate polar, polar, and acidic compounds were detected in both emitted and ambient aerosol samples. The processing and combustion of olive pits yielded a source with strong biogenic characteristics, such as the high values of the carbon preference index (CPI) for all compound classes. Polycyclic aromatic hydrocarbons (PAHs) detected in emissions were associated with both olive pits and diesel combustion. The chromatographic profile of dimethylphenanthrenes (DMPs) was characteristic of olive pit combustion. Organic aerosols collected in two receptor sites provided a different pattern. The significant contribution of vehicular emissions was identified by CPI values (approximately 1) of n-alkanes and the presence of the unresolved complex mixture (UCM). In addition, PAH concentration diagnostic ratios indicated that emissions from catalyst and noncatalyst automobiles and heavy trucks were significant. The strong even-to-odd predominance of n-alkanols, n-alkanoic acids, and their salts indicated the contribution of a source with biogenic characteristics. However, the profile of DMPs at receptor sites was similar to that observed for diesel particulates. These differences indicated that the contribution of vegetable oil processing emissions to the atmosphere was negligible.

  17. 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.

  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. 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

  20. Probing the spatial and temporal variability of Enceladus mass-loading from ion cyclotron waves

    NASA Astrophysics Data System (ADS)

    Wei, H.; Russell, C. T.; Powell, R. L.; Cowee, M.; Leisner, J. S.; Jia, Y.; Dougherty, M. K.

    2013-12-01

    Enceladus plays a critical role in the Saturnian system by loading a significant amount of neutrals, ions and dust into the inner magnetosphere. Enceladus is also considered as the ultimate source for the dusty E-ring and the extended neutral cloud from 3.5 to 6.5 Saturn radii. When the freshly-added neutrals are ionized and accelerated by the electric and magnetic fields, left-handed electromagnetic waves, called ion cyclotron waves (ICW), grow from the free energy of the highly anisotropic distribution of these ions. The ICWs have been widely used to probe the rate of mass loading in different plasma environments in the solar system, because the wave power is proportional to the density and energy of the pickup ions. At Enceladus, ICWs are detected by Cassini not only near the moon but throughout the extended neutral cloud in all local times. However, the wave power is largely enhanced near the moon's longitude rather than far away from it. This indicates that on top of the relatively azimuthally-symmetric mass-loading source of the neutral cloud, there is a much denser cloud of neutrals centered on the moon and rotating with it. The latter source is the instantaneous mass-loading from plume of Enceladus, and it leads to asymmetry and dynamics in the magnetosphere. We investigate all available Cassini Enceladus flyby data to obtain a 3D spatial profile of the ICW power near the moon. By comparing with waves at longitudes far away from the moon, we investigate how significant is the plume mass-loading with respect to the neutral cloud mass-loading. We also compare the waves along several groups of identical trajectories to examine the temporal variability of the plume.

  1. Ion mobility spectrometry-mass spectrometry (IMS-MS) for on- and offline analysis of atmospheric gas and aerosol species

    NASA Astrophysics Data System (ADS)

    Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; Budisulistiorini, Sri H.; Zhang, Haofei; Surratt, Jason D.; Knochenmuss, Richard; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis; Canagaratna, Manjula R.

    2016-07-01

    Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS-MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS-MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI-IMS-MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS-MS signals are consistent with laboratory IMS-MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS-MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS-MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the

  2. Mass-analysis of Charged Aerosol Particles in a PMSE/NLC Layer by a Rocket-borne Spectrometer

    NASA Astrophysics Data System (ADS)

    Robertson, Scott; Knappmiller, Scott; Horanyi, Mihaly; Sternovsky, Zoltan; Baumgarten, Gerd; Latteck, Ralph; Rapp, Markus; Holzworth, Robert; Shimogawa, Michael; Gumbel, Jorg; Megner, Ms Linda; Friedrich, Martin

    Two "MASS" rockets (Mesospheric Aerosol Sampling Spectrometer) were launched from the Andoya Rocket Range (Norway) the first week of August 2007. The payloads carried an electrostatic mass analyzer for the charged fraction of the aerosol particles, electric field booms, a photometer for cloud brightness, and Faraday rotation antennas for electron density. Aerosol particles with different ranges of charge-to-mass ratio were collected within the instrument housing on two sets of four biased collector plates, with one set for positive particles and one set for negative particles. The first rocket was launched into PMSE and NLC on 3 August. The sun was 4 degrees below the horizon and NLC were seen in the previous hour at 83 km by the ALOMAR RMR lidar. NLC were detected at the same altitude by rocket-borne photometer measurements. The charged aerosol data shows the density of negative particles with radius greater than 3 nm rising sharply at 83 km and continuing to 89 km, collocated with PMSE detected by the ALWIN radar. Particles with 1-2 nm radii with both signs of charge and particles with less than 1 nm radius charged positively were detected at 86-88 km. The occurrence of the positive particles in the smallest size range in the region of lowest temperature suggests that their origin is nucleation and growth on ions. Initial charge-density estimates are several thousands per cubic centimeter for each of these size ranges. The second launch was 6 August into PMSE without NLC. The 1-2 nm particles were seen from 85.4 to 87.4 km, again with both signs of charge. Larger sizes were nearly absent.

  3. Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

    DOE PAGES

    Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; et al

    2016-07-25

    Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambientmore » field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of

  4. Impact of Manaus City on the Amazon Green Ocean atmosphere: ozone production, precursor sensitivity and aerosol load

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Ganzeveld, L.; Thielmann, A.; Dindorf, T.; Schebeske, G.; Welling, M.; Sciare, J.; Roberts, G.; Meixner, F. X.; Kesselmeier, J.; Lelieveld, J.; Kolle, O.; Ciccioli, P.; Lloyd, J.; Trentmann, J.; Artaxo, P.; Andreae, M. O.

    2010-05-01

    As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O3, NO, NO2, CO, VOC, CO2, and H2O. Aerosol loads were characterized by total aerosol number concentration (CN) and cloud condensation nuclei (CCN) concentrations, and light scattering properties. Measurements over pristine rainforest areas during the campaign showed low levels of pollution from biomass burning or industrial emissions, representative of wet season background conditions. The urban plume of Manaus City was found to be joined by plumes from power plants south of the city, all showing evidence of very strong photochemical ozone formation. One episode is discussed in detail, where a threefold increase in ozone mixing ratios in the atmospheric boundary layer occurred within a 100 km travel distance downwind of Manaus. Observation-based estimates of the ozone production rates in the plume reached 15 ppb h-1. Within the plume core, aerosol concentrations were strongly enhanced, with ΔCN/ΔCO ratios about one order of magnitude higher than observed in Amazon biomass burning plumes. ΔCN/ΔCO ratios tended to decrease with increasing transport time, indicative of a significant reduction in particle number by coagulation, and without substantial new particle nucleation occurring within the time/space observed. While in the background atmosphere a large fraction of the total particle number served as CCN (about 60-80% at 0.6% supersaturation), the CCN/CN ratios within the plume indicated that only a small fraction (16 ± 12%) of the plume particles were

  5. Impact of Manaus City on the Amazon Green Ocean atmosphere: ozone production, precursor sensitivity and aerosol load

    NASA Astrophysics Data System (ADS)

    Kuhn, U.; Ganzeveld, L.; Thielmann, A.; Dindorf, T.; Schebeske, G.; Welling, M.; Sciare, J.; Roberts, G.; Meixner, F. X.; Kesselmeier, J.; Lelieveld, J.; Kolle, O.; Ciccioli, P.; Lloyd, J.; Trentmann, J.; Artaxo, P.; Andreae, M. O.

    2010-10-01

    As a contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia - Cooperative LBA Airborne Regional Experiment (LBA-CLAIRE-2001) field campaign in the heart of the Amazon Basin, we analyzed the temporal and spatial dynamics of the urban plume of Manaus City during the wet-to-dry season transition period in July 2001. During the flights, we performed vertical stacks of crosswind transects in the urban outflow downwind of Manaus City, measuring a comprehensive set of trace constituents including O3, NO, NO2, CO, VOC, CO2, and H2O. Aerosol loads were characterized by concentrations of total aerosol number (CN) and cloud condensation nuclei (CCN), and by light scattering properties. Measurements over pristine rainforest areas during the campaign showed low levels of pollution from biomass burning or industrial emissions, representative of wet season background conditions. The urban plume of Manaus City was found to be joined by plumes from power plants south of the city, all showing evidence of very strong photochemical ozone formation. One episode is discussed in detail, where a threefold increase in ozone mixing ratios within the atmospheric boundary layer occurred within a 100 km travel distance downwind of Manaus. Observation-based estimates of the ozone production rates in the plume reached 15 ppb h-1. Within the plume core, aerosol concentrations were strongly enhanced, with ΔCN/ΔCO ratios about one order of magnitude higher than observed in Amazon biomass burning plumes. ΔCN/ΔCO ratios tended to decrease with increasing transport time, indicative of a significant reduction in particle number by coagulation, and without substantial new particle nucleation occurring within the time/space observed. While in the background atmosphere a large fraction of the total particle number served as CCN (about 60-80% at 0.6% supersaturation), the CCN/CN ratios within the plume indicated that only a small fraction (16±12%) of the plume particles were CCN

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

    DOE PAGES

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

    2015-09-25

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

  7. 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... Concentration (µg/m3) Estimated Mass Concentration Measurement (µg/m3) Ideal Sampler Fractional...

  8. 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... Concentration (µg/m3) Estimated Mass Concentration Measurement (µg/m3) Ideal Sampler Fractional...

  9. 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... Concentration (µg/m 3) Estimated Mass Concentration Measurement (µg/m 3) Ideal Sampler Fractional...

  10. Interactive effects of mass proportions and coupling properties on external loading in simulated forefoot impact landings.

    PubMed

    Gittoes, Marianne J R; Kerwin, David G

    2009-08-01

    This study aimed to gain insight into the individual and interactive effects of segmental mass proportions and coupling properties on external loading in simulated forefoot landings. An evaluated four-segment wobbling mass model replicated forefoot drop landings (height: 0.46 m) performed by two subjects. A comparison of the peak impact forces (GFzmax) produced during the evaluated landing and further simulated landings performed using modified (+/-5% perturbation) mass proportions and coupling properties was made. Independent segmental mass proportion changes, particularly in the upper body, produced a prominent change in GFzmax of up to 0.32 bodyweight (BW) whereas independent mass coupling stiffness and damping alterations had less effect on GFzmax (change in GFzmax of up to 0.18 BW). When combining rigid mass proportion reductions with damping modifications, an additional GFzmax attenuation of up to 0.13 BW was produced. An individual may be predisposed to high loading and traumatic and overuse injury during forefoot landings owing to their inherent inertia profile. Subject-specific neuromuscular modifications to mass coupling properties may not be beneficial in overriding the increased forces associated with larger rigid mass proportions. PMID:19827473

  11. Steps Toward an EOS-Era Aerosol Air Mass Type Climatology

    NASA Technical Reports Server (NTRS)

    Kahn, Ralph A.

    2012-01-01

    We still have a way to go to develop a global climatology of aerosol type from the EOS-era satellite data record that currently spans more than 12 years of observations. We have demonstrated the ability to retrieve aerosol type regionally, providing a classification based on the combined constraints on particle size, shape, and single-scattering albedo (SSA) from the MISR instrument. Under good but not necessarily ideal conditions, the MISR data can distinguish three-to-five size bins, two-to-four bins in SSA, and spherical vs. non-spherical particles. However, retrieval sensitivity varies enormously with scene conditions. So, for example, there is less information about aerosol type when the mid-visible aerosol optical depth (AOD) is less that about 0.15 or 0.2.

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

    EPA Science Inventory

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

  13. Effects of anthropogenic emissions on the molecular composition of urban organic aerosols: An ultrahigh resolution mass spectrometry study

    NASA Astrophysics Data System (ADS)

    Kourtchev, I.; O'Connor, I. P.; Giorio, C.; Fuller, S. J.; Kristensen, K.; Maenhaut, W.; Wenger, J. C.; Sodeau, J. R.; Glasius, M.; Kalberer, M.

    2014-06-01

    Identification of the organic composition of atmospheric aerosols is necessary to develop effective air pollution mitigation strategies. However, the majority of the organic aerosol mass is poorly characterized and its detailed analysis is a major analytical challenge. In this study, we applied state-of-the-art direct infusion nano-electrospray (nanoESI) ultrahigh resolution mass spectrometry (UHRMS) and liquid chromatography ESI Quadrupole Time-of-Flight (Q-TOF) MS for the analysis of the organic fraction of fine particulate matter (PM2.5) collected at an urban location in Cork, Ireland. Comprehensive mass spectral data evaluation methods (e.g., Kendrick Mass Defect and Van Krevelen) were used to identify compound classes and mass distributions of the detected species. Up to 850 elemental formulae were identified in negative mode nanoESI-UHR-MS. Nitrogen and/or sulphur containing organic species contributed up to 40% of the total identified formulae and exhibited strong diurnal variations suggesting the importance of night-time NO3 chemistry at the site. The presence of a large number of oxidised aromatic and nitroaromatic compounds in the samples indicated a strong anthropogenic influence, i.e., from traffic emissions and domestic solid fuel (DSF) burning. Most of the identified biogenic secondary organic aerosol (SOA) compounds are later-generation nitrogen- and sulphur-containing products, indicating that SOA composition is strongly affected by anthropogenic species such as NOx and SO2. Unsaturated and saturated C12-C20 fatty acids were found to be the most abundant homologs with a composition reflecting a primary marine origin. The results of this work demonstrate that the studied site is a very complex environment affected by a variety of anthropogenic activities and natural sources.

  14. To what extent is mass loading responsible for the Venus bowshock precursor?

    NASA Technical Reports Server (NTRS)

    Fontheim, Ernest G.; Brace, Larry H.

    1988-01-01

    Significant ion and electron flux enhancements immediately upstream of the Venus bow shock were observed by the Electron Temperature Probe on the Pioneer Venus Orbiter. It is shown that mass loading of the solar wind by oxygen ions accounts for only about 10 percent of the observed effect.

  15. To what extent is mass loading responsible for the Venus bowshock precursor

    SciTech Connect

    Fontheim, E.G.; Brace, L.H.

    1988-03-01

    Significant ion and electron flux enhancements immediately upstream of the Venus bow shock were observed by the Electron Temperature Probe on the Pioneer Venus Orbiter. It is shown that mass loading of the solar wind by oxygen ions accounts for only about 10 percent of the observed effect.

  16. Mass load estimation errors utilizing grab sampling strategies in a karst watershed

    USGS Publications Warehouse

    Fogle, A.W.; Taraba, J.L.; Dinger, J.S.

    2003-01-01

    Developing a mass load estimation method appropriate for a given stream and constituent is difficult due to inconsistencies in hydrologic and constituent characteristics. The difficulty may be increased in flashy flow conditions such as karst. Many projects undertaken are constrained by budget and manpower and do not have the luxury of sophisticated sampling strategies. The objectives of this study were to: (1) examine two grab sampling strategies with varying sampling intervals and determine the error in mass load estimates, and (2) determine the error that can be expected when a grab sample is collected at a time of day when the diurnal variation is most divergent from the daily mean. Results show grab sampling with continuous flow to be a viable data collection method for estimating mass load in the study watershed. Comparing weekly, biweekly, and monthly grab sampling, monthly sampling produces the best results with this method. However, the time of day the sample is collected is important. Failure to account for diurnal variability when collecting a grab sample may produce unacceptable error in mass load estimates. The best time to collect a sample is when the diurnal cycle is nearest the daily mean.

  17. 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.

  18. Origin of atmospheric aerosols at the Pierre Auger Observatory using studies of air mass trajectories in South America

    NASA Astrophysics Data System (ADS)

    Aab, A.; Abreu, P.; Aglietta, M.; Ahlers, M.; Ahn, E. J.; Albuquerque, I. F. M.; Allekotte, I.; Allen, J.; Allison, P.; Almela, A.; Alvarez Castillo, J.; Alvarez-Muñiz, J.; Alves Batista, R.; Ambrosio, M.; Aminaei, A.; Anchordoqui, L.; Andringa, S.; Antičić, T.; Aramo, C.; Arqueros, F.; Asorey, H.; Assis, P.; Aublin, J.; Ave, M.; Avenier, M.; Avila, G.; Badescu, A. M.; Barber, K. B.; Bardenet, R.; Bäuml, J.; Baus, C.; Beatty, J. J.; Becker, K. H.; Bellido, J. A.; BenZvi, S.; Berat, C.; Bertou, X.; Biermann, P. L.; Billoir, P.; Blanco, F.; Blanco, M.; Bleve, C.; Blümer, H.; Boháčová, M.; Boncioli, D.; Bonifazi, C.; Bonino, R.; Borodai, N.; Brack, J.; Brancus, I.; Brogueira, P.; Brown, W. C.; Buchholz, P.; Bueno, A.; Buscemi, M.; Caballero-Mora, K. S.; Caccianiga, B.; Caccianiga, L.; Candusso, M.; Caramete, L.; Caruso, R.; Castellina, A.; Cataldi, G.; Cazon, L.; Cester, R.; Cheng, S. H.; Chiavassa, A.; Chinellato, J. A.; Chudoba, J.; Cilmo, M.; Clay, R. W.; Cocciolo, G.; Colalillo, R.; Collica, L.; Coluccia, M. R.; Conceição, R.; Contreras, F.; Cooper, M. J.; Coutu, S.; Covault, C. E.; Criss, A.; Cronin, J.; Curutiu, A.; Dallier, R.; Daniel, B.; Dasso, S.; Daumiller, K.; Dawson, B. R.; de Almeida, R. M.; De Domenico, M.; de Jong, S. J.; De La Vega, G.; de Mello Junior, W. J. M.; de Mello Neto, J. R. T.; De Mitri, I.; de Souza, V.; de Vries, K. D.; del Peral, L.; Deligny, O.; Dembinski, H.; Dhital, N.; Di Giulio, C.; Di Matteo, A.; Diaz, J. C.; Díaz Castro, M. L.; Diep, P. N.; Diogo, F.; Dobrigkeit, C.; Docters, W.; D'Olivo, J. C.; Dong, P. N.; Dorofeev, A.; dos Anjos, J. C.; Dova, M. T.; Ebr, J.; Engel, R.; Erdmann, M.; Escobar, C. O.; Espadanal, J.; Etchegoyen, A.; Facal San Luis, P.; Falcke, H.; Fang, K.; Farrar, G.; Fauth, A. C.; Fazzini, N.; Ferguson, A. P.; Fick, B.; Figueira, J. M.; Filevich, A.; Filipčič, A.; Foerster, N.; Fox, B. D.; Fracchiolla, C. E.; Fraenkel, E. D.; Fratu, O.; Fröhlich, U.; Fuchs, B.; Gaior, R.; Gamarra, R. F.; Gambetta, S.; García, B.; Garcia Roca, S. T.; Garcia-Gamez, D.; Garcia-Pinto, D.; Garilli, G.; Gascon Bravo, A.; Gemmeke, H.; Ghia, P. L.; Giammarchi, M.; Giller, M.; Gitto, J.; Glaser, C.; Glass, H.; Gomez Albarracin, F.; Gómez Berisso, M.; Gómez Vitale, P. F.; Gonçalves, P.; Gonzalez, J. G.; Gookin, B.; Gorgi, A.; Gorham, P.; Gouffon, P.; Grebe, S.; Griffith, N.; Grillo, A. F.; Grubb, T. D.; Guardincerri, Y.; Guarino, F.; Guedes, G. P.; Hansen, P.; Harari, D.; Harrison, T. A.; Harton, J. L.; Haungs, A.; Hebbeker, T.; Heck, D.; Herve, A. E.; Hill, G. C.; Hojvat, C.; Hollon, N.; Holt, E.; Homola, P.; Hörandel, J. R.; Horvath, P.; Hrabovský, M.; Huber, D.; Huege, T.; Insolia, A.; Isar, P. G.; Jansen, S.; Jarne, C.; Josebachuili, M.; Kadija, K.; Kambeitz, O.; Kampert, K. H.; Karhan, P.; Kasper, P.; Katkov, I.; Kégl, B.; Keilhauer, B.; Keivani, A.; Kemp, E.; Kieckhafer, R. M.; Klages, H. O.; Kleifges, M.; Kleinfeller, J.; Knapp, J.; Krause, R.; Krohm, N.; Krömer, O.; Kruppke-Hansen, D.; Kuempel, D.; Kunka, N.; La Rosa, G.; LaHurd, D.; Latronico, L.; Lauer, R.; Lauscher, M.; Lautridou, P.; Le Coz, S.; Leão, M. S. A. B.; Lebrun, D.; Lebrun, P.; Leigui de Oliveira, M. A.; Letessier-Selvon, A.; Lhenry-Yvon, I.; Link, K.; López, R.; Lopez Agüera, A.; Louedec, K.; Lozano Bahilo, J.; Lu, L.; Lucero, A.; Ludwig, M.; Lyberis, H.; Maccarone, M. C.; Malacari, M.; Maldera, S.; Maller, J.; Mandat, D.; Mantsch, P.; Mariazzi, A. G.; Marin, V.; Mariş, I. C.; Marquez Falcon, H. R.; Marsella, G.; Martello, D.; Martin, L.; Martinez, H.; Martínez Bravo, O.; Martraire, D.; Masías Meza, J. J.; Mathes, H. J.; Matthews, J.; Matthews, J. A. J.; Matthiae, G.; Maurel, D.; Maurizio, D.; Mayotte, E.; Mazur, P. O.; Medina, C.; Medina-Tanco, G.; Melissas, M.; Melo, D.; Menichetti, E.; Menshikov, A.; Messina, S.; Meyhandan, R.; Mićanović, S.; Micheletti, M. I.; Middendorf, L.; Minaya, I. A.; Miramonti, L.; Mitrica, B.; Molina-Bueno, L.; Mollerach, S.; Monasor, M.; Monnier Ragaigne, D.; Montanet, F.; Morales, B.; Morello, C.; Moreno, J. C.; Mostafá, M.; Moura, C. A.; Muller, M. A.; Müller, G.; Münchmeyer, M.; Mussa, R.; Navarra, G.; Navarro, J. L.; Navas, S.; Necesal, P.; Nellen, L.; Nelles, A.; Neuser, J.; Nhung, P. T.; Niechciol, M.; Niemietz, L.; Niggemann, T.; Nitz, D.; Nosek, D.; Nožka, L.; Oehlschläger, J.; Olinto, A.; Oliveira, M.; Ortiz, M.; Pacheco, N.; Pakk Selmi-Dei, D.; Palatka, M.; Pallotta, J.; Palmieri, N.; Parente, G.; Parra, A.; Pastor, S.; Paul, T.; Pech, M.; Pȩkala, J.; Pelayo, R.; Pepe, I. M.; Perrone, L.; Pesce, R.; Petermann, E.; Petrera, S.; Petrolini, A.; Petrov, Y.; Piegaia, R.; Pierog, T.; Pieroni, P.; Pimenta, M.; Pirronello, V.; Platino, M.; Plum, M.; Pontz, M.; Porcelli, A.; Preda, T.; Privitera, P.; Prouza, M.; Quel, E. J.; Querchfeld, S.; Quinn, S.; Rautenberg, J.; Ravel, O.; Ravignani, D.; Revenu, B.; Ridky, J.; Riggi, S.; Risse, M.; Ristori, P.; Rivera, H.; Rizi, V.; Roberts, J.; Rodrigues de Carvalho, W.; Rodriguez Cabo, I.; Rodriguez Fernandez, G.; Rodriguez Martino, J.; Rodriguez Rojo, J.; Rodríguez-Frías, M. D.; Ros, G.; Rosado, J.; Rossler, T.; Roth, M.; Rouillé-d'Orfeuil, B.; Roulet, E.; Rovero, A. C.; Rühle, C.; Saffi, S. J.; Saftoiu, A.; Salamida, F.; Salazar, H.; Salesa Greus, F.; Salina, G.; Sánchez, F.; Sanchez-Lucas, P.; Santo, C. E.; Santos, E.; Santos, E. M.; Sarazin, F.; Sarkar, B.; Sarmento, R.; Sato, R.; Scharf, N.; Scherini, V.; Schieler, H.; Schiffer, P.; Schmidt, A.; Scholten, O.; Schoorlemmer, H.; Schovánek, P.; Schröder, F. G.; Schulz, A.; Schulz, J.; Sciutto, S. J.; Scuderi, M.; Segreto, A.; Settimo, M.; Shadkam, A.; Shellard, R. C.; Sidelnik, I.; Sigl, G.; Sima, O.; Śmiałkowski, A.; Šmída, R.; Snow, G. R.; Sommers, P.; Sorokin, J.; Spinka, H.; Squartini, R.; Srivastava, Y. N.; Stanič, S.; Stapleton, J.; Stasielak, J.; Stephan, M.; Straub, M.; Stutz, A.; Suarez, F.; Suomijärvi, T.; Supanitsky, A. D.; Šuša, T.; Sutherland, M. S.; Swain, J.; Szadkowski, Z.; Szuba, M.; Tapia, A.; Tartare, M.; Taşcău, O.; Thao, N. T.; Tiffenberg, J.; Timmermans, C.; Tkaczyk, W.; Todero Peixoto, C. J.; Toma, G.; Tomankova, L.; Tomé, B.; Tonachini, A.; Torralba Elipe, G.; Torres Machado, D.; Travnicek, P.; Tridapalli, D. B.; Trovato, E.; Tueros, M.; Ulrich, R.; Unger, M.; Valdés Galicia, J. F.; Valiño, I.; Valore, L.; van Aar, G.; van den Berg, A. M.; van Velzen, S.; van Vliet, A.; Varela, E.; Vargas Cárdenas, B.; Varner, G.; Vázquez, J. R.; Vázquez, R. A.; Veberič, D.; Verzi, V.; Vicha, J.; Videla, M.; Villaseñor, L.; Wahlberg, H.; Wahrlich, P.; Wainberg, O.; Walz, D.; Watson, A. A.; Weber, M.; Weidenhaupt, K.; Weindl, A.; Werner, F.; Westerhoff, S.; Whelan, B. J.; Widom, A.; Wieczorek, G.; Wiencke, L.; Wilczyńska, B.; Wilczyński, H.; Will, M.; Williams, C.; Winchen, T.; Wundheiler, B.; Wykes, S.; Yamamoto, T.; Yapici, T.; Younk, P.; Yuan, G.; Yushkov, A.; Zamorano, B.; Zas, E.; Zavrtanik, D.; Zavrtanik, M.; Zaw, I.; Zepeda, A.; Zhou, J.; Zhu, Y.; Zimbres Silva, M.; Ziolkowski, M.; Curci, G.

    2014-11-01

    The Pierre Auger Observatory is making significant contributions towards understanding the nature and origin of ultra-high energy cosmic rays. One of its main challenges is the monitoring of the atmosphere, both in terms of its state variables and its optical properties. The aim of this work is to analyse aerosol optical depth τa(z) values measured from 2004 to 2012 at the observatory, which is located in a remote and relatively unstudied area of Pampa Amarilla, Argentina. The aerosol optical depth is in average quite low - annual mean τa(3.5 km) ∼ 0.04 - and shows a seasonal trend with a winter minimum - τa(3.5 km) ∼ 0.03 -, and a summer maximum - τa(3.5 km) ∼ 0.06 -, and an unexpected increase from August to September - τa(3.5 km) ∼ 0.055. We computed backward trajectories for the years 2005 to 2012 to interpret the air mass origin. Winter nights with low aerosol concentrations show air masses originating from the Pacific Ocean. Average concentrations are affected by continental sources (wind-blown dust and urban pollution), whilst the peak observed in September and October could be linked to biomass burning in the northern part of Argentina or air pollution coming from surrounding urban areas.

  19. Molecular composition of aged secondary organic aerosol generated from a mixture of biogenic volatile compounds using ultrahigh resolution mass spectrometry

    NASA Astrophysics Data System (ADS)

    Kourtchev, I.; Doussin, J.-F.; Giorio, C.; Mahon, B.; Wilson, E. M.; Maurin, N.; Pangui, E.; Venables, D. S.; Wenger, J. C.; Kalberer, M.

    2015-02-01

    Field observations over the past decade indicate that a significant fraction of organic aerosol in remote areas may contain highly oxidised molecules. Aerosol processing or further oxidation (ageing) of organic aerosol has been suggested to be responsible for their formation through heterogeneous uptake of oxidants and multigenerational oxidation of vapours by OH radicals. In this study we investigated the influence of several ageing processes on the molecular composition of secondary organic aerosols (SOA) using direct infusion and liquid chromatography ultrahigh resolution mass spectrometry. SOA was formed in simulation chamber experiments from ozonolysis of a mixture of four biogenic volatile organic compounds (BVOC): α-pinene, β-pinene, Δ3-carene and isoprene. The SOA was subsequently aged under three different sets of conditions: in the dark in the presence of residual ozone, with UV irradiation and OH radicals, and using UV light only. Among all studied conditions, only OH radical-initiated ageing was found to influence the molecular composition of the aerosol and showed an increase in carbon oxidation state (OSC) and elemental O/C ratios of the SOA components. None of the ageing processes produced an observable effect on the oligomers formed from ozonolysis of the BVOC mixture, which were found to be equally abundant in both "fresh" and "aged" SOA. Additional experiments using α-pinene as the sole precursor demonstrated that oligomers are an important group of compounds in SOA produced from both ozonolysis and OH radical-initiated oxidation processes; however, a completely different set of oligomers is formed under these two oxidation regimes. SOA from the OH radical-initiated α-pinene oxidation had a significantly higher overall OSC and O/C compared to that from pure ozonolysis experiments confirming that the OH radical reaction is more likely to be responsible for the occurrence of highly oxidised species in ambient biogenic SOA.

  20. 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

  1. Climatology of aerosol optical properties and black carbon mass absorption cross section at a remote high-altitude site in the western Mediterranean Basin

    NASA Astrophysics Data System (ADS)

    Pandolfi, M.; Ripoll, A.; Querol, X.; Alastuey, A.

    2014-06-01

    Aerosol light scattering (σsp), backscattering (σbsp) and absorption (σap) were measured at Montsec (MSC; 42°3' N, 0°44' E, 1570 m a.s.l.), a remote high-altitude site in the western Mediterranean Basin. Mean (±SD) σsp, σbsp and σap were 18.9 ± 20.8, 2.6 ± 2.8 and 1.5 ± 1.4 Mm-1, respectively at 635 nm during the period under study (June 2011-June 2013). Mean values of single-scattering albedo (SSA, 635 nm), the scattering Ångström exponent (SAE, 450-635 nm), backscatter-to-scatter ratio (B / S, 635 nm), asymmetry parameter (g, 635 nm), black carbon mass absorption cross section (MAC, 637 nm) and PM2.5 mass scattering cross section (MSCS, 635 nm) were 0.92 ± 0.03, 1.56 ± 0.88, 0.16 ± 0.09, 0.53 ± 0.16, 10.9 ± 3.5 m2 g-1 and 2.5 ± 1.3 m2 g-1, respectively. The scattering measurements performed at MSC were in the medium/upper range of values reported by Andrews et al. (2011) for other mountaintop sites in Europe due to the frequent regional recirculation scenarios (SREG) and Saharan dust episodes (NAF) occurring mostly in spring/summer and causing the presence of polluted layers at the MSC altitude. However, the development of upslope winds and the possible presence of planetary boundary layer air at MSC altitude in summer may also have contributed to the high scattering observed. Under these summer conditions no clear diurnal cycles were observed for the measured extensive aerosol optical properties (σsp, σbsp and σap). Conversely, low σsp and σap at MSC were measured during Atlantic advections (AA) and winter regional anticyclonic episodes (WREG) typically observed during the cold season in the western Mediterranean. Therefore, a season-dependent decrease in the magnitude of aerosol extensive properties was observed when MSC was in the free troposphere, with the highest free-troposphere vs. all-data difference observed in winter and the lowest in spring/summer. The location of MSC station allowed for a reliable characterization of aerosols

  2. MHD simulations of boundary layer formation along the dayside Venus ionopause due to mass loading

    NASA Technical Reports Server (NTRS)

    Mcgary, J. E.; Pontius, D. H., Jr.

    1994-01-01

    A two-dimensional magnetohydrodynamic (MHD) simulation of mass-loaded solar wind flow around the dayside of Venus is presented. For conditions appropriate to a low-altitude ionopause the simulations show that mass loading from the pickup of oxygen ions produces a boundary layer of finite thickness along the ionopause. Within this layer the temperatures exhibit strong gradients normal to and away from the ionopause. Furthermore, there is a shear in the bulk flow velocity across the boundary layer, such that the (predominantly tangential) flow decreases in speed as the ionopause is approached and remains small along the ionopause, consistent with Pioneer Venus observations. The total mass density increases significantly as the flow approaches the ionopause, where the contribution of O(+) to the total number density is a few percent. Numerical simulations are carried out for various mass addition rates and demonstrate that the boundary layer develops when oxygen ion production exceeds approximately 2 x 10(exp 5)/cu m/s. For the upstream solar wind parameters and mass loading rates chosen for these simulations, the results are consistent with observations made on the dayside of Venus for average ionopause conditions near 300 km.

  3. MHD simulations of boundary layer formation along the dayside Venus ionopause due to mass loading

    NASA Astrophysics Data System (ADS)

    McGary, J. E.; Pontius, D. H.

    1994-02-01

    A two-dimensional magnetohydrodynamic (MHD) simulation of mass-loaded solar wind flow around the dayside of Venus is presented. For conditions appropriate to a low-altitude ionopause the simulations show that mass loading from the pickup of oxygen ions produces a boundary layer of finite thickness along the ionopause. Within this layer the temperatures exhibit strong gradients normal to and away from the ionopause. Furthermore, there is a shear in the bulk flow velocity across the boundary layer, such that the (predominantly tangential) flow decreases in speed as the ionopause is approached and remains small along the ionopause, consistent with Pioneer Venus observations. The total mass density increases significantly as the flow approaches the ionopause, where the contribution of O(+) to the total number density is a few percent. Numerical simulations are carried out for various mass addition rates and demonstrate that the boundary layer develops when oxygen ion production exceeds approximately 2 x 105/cu m/s. For the upstream solar wind parameters and mass loading rates chosen for these simulations, the results are consistent with observations made on the dayside of Venus for average ionopause conditions near 300 km.

  4. Reconciling different observations of the CO2 ice mass loading of the Martian north polar cap

    USGS Publications Warehouse

    Haberle, R.M.; Mattingly, B.; Titus, T.N.

    2004-01-01

    The GRS measurements of the peak mass loading of the north polar CO2 ice cap on Mars are about 60% lower than those calculated from MGS TES radiation data and those inferred from the MOLA cap thicknesses. However, the GRS data provide the most accurate measurement of the mass loading. We show that the TES and MOLA data can be reconciled with the GRS data if (1) subsurface heat conduction and atmospheric heat transport are included in the TES mass budget calculations, and (2) the density of the polar deposits is ???600 kg m-3. The latter is much less than that expected for slab ice (???1600 kg m-3) and suggests that processes unique to the north polar region are responsible for the low cap density. Copyright 2004 by the American Geophysical Union.

  5. 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

  6. Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

    2014-07-01

    Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as directly in the exhaust plumes of individual heavy-duty (HD) diesel trucks. BC emission factor distributions for HD trucks were more skewed than OA distributions (N = 293), with the highest 10% of trucks accounting for 56 and 42% of total measured BC and OA emissions, respectively. OA mass spectra measured for HD truck exhaust plumes show cycloalkanes are predominate in exhaust OA emissions relative to saturated alkanes (i.e., normal and iso-paraffins), suggesting that lubricating oil rather than fuel is the dominant source of primary organic aerosol (POA) emissions in diesel vehicle exhaust. This finding is supported by the detection of trace elements such as zinc and phosphorus in the exhaust plumes of individual trucks. Trace elements were emitted relative to total OA at levels that are consistent with typical weight fractions of commonly used additives present in lubricating oil. A comparison of measured OA and BC mass spectra across various sampling periods revealed a high degree of similarity in OA and BC emitted by gasoline and diesel engines. This finding indicates a large fraction of OA in gasoline exhaust is lubricant-derived as well. The similarity in OA and BC mass spectra for gasoline and diesel engine exhaust is likely to confound ambient source apportionment efforts to determine contributions to air pollution from these two important sources.

  7. Towards inferring elastic structural variations from Earth's response to surface mass loading

    NASA Astrophysics Data System (ADS)

    Martens, H. R.; Simons, M.; Rivera, L. A.; Owen, S. E.

    2015-12-01

    We explore the sensitivity of surface mass loading displacement response to perturbations in elastic structure, with the goal to refine profiles of elastic moduli and density through the crust and upper mantle. Examples of surface mass loads include tidal and non-tidal ocean loads, atmospheric loads and hydrological loads. Using software developed in-house (LoadDef), we derive sensitivity kernels for Love numbers and load Green's functions (LGFs) using calculus of variations and finite difference methods. Perturbations to the two elastic moduli and density exhibit unique LGF sensitivity patterns, retaining the possibility that the material parameters may be independently constrained given a spatially distributed set of sufficiently accurate loading response observations. To further elucidate the ability to invert for structure in a particular region, a thorough investigation into model resolution must also be performed. We garner a more palpable sense for the effects of structural variations on the response to surface mass loading by calculating and comparing sets of predicted ocean tidal loading (OTL) displacement responses across a global network of land-based locations, generated from convolutions of an ocean tide model with LGFs derived from a variety of reference Earth models. We find that discrepancies between predictions for the M2 harmonic differ by less than 0.2 mm at over 95% of the locations considered, a value generally exceeded, albeit not substantially, by current observational and forward modeling errors. Although predicted discrepancies can reach 2 mm or more at some coastal locations, errors in the ocean tide models and convolution algorithms are also largest near the coasts. As a case study, we examine the residuals between Global Positioning System (GPS) observations and modeled predictions of OTL response across the South American continent. A comparison of ocean models suggests that a common mode (mean displacement) accounts for a dominant

  8. 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

  9. Characterization of a real-time tracer for Isoprene Epoxydiols-derived Secondary Organic Aerosol (IEPOX-SOA) from aerosol mass spectrometer measurements

    DOE PAGES

    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

  10. Comparison of Two Parametric Methods to Estimate Pesticide Mass Loads in California's Central Valley

    USGS Publications Warehouse

    Saleh, D.K.; Lorenz, D.L.; Domagalski, J.L.

    2011-01-01

    Mass loadings were calculated for four pesticides in two watersheds with different land uses in the Central Valley, California, by using two parametric models: (1) the Seasonal Wave model (SeaWave), in which a pulse signal is used to describe the annual cycle of pesticide occurrence in a stream, and (2) the Sine Wave model, in which first-order Fourier series sine and cosine terms are used to simulate seasonal mass loading patterns. The models were applied to data collected during water years 1997 through 2005. The pesticides modeled were carbaryl, diazinon, metolachlor, and molinate. Results from the two models show that the ability to capture seasonal variations in pesticide concentrations was affected by pesticide use patterns and the methods by which pesticides are transported to streams. Estimated seasonal loads compared well with results from previous studies for both models. Loads estimated by the two models did not differ significantly from each other, with the exceptions of carbaryl and molinate during the precipitation season, where loads were affected by application patterns and rainfall. However, in watersheds with variable and intermittent pesticide applications, the SeaWave model is more suitable for use on the basis of its robust capability of describing seasonal variation of pesticide concentrations. ?? 2010 American Water Resources Association. This article is a US Government work and is in the public domain in the USA.

  11. Comparison of two parametric methods to estimate pesticide mass loads in California's Central Valley

    USGS Publications Warehouse

    Saleh, Dina K.; Lorenz, David L.; Domagalski, Joseph L.

    2011-01-01

    Mass loadings were calculated for four pesticides in two watersheds with different land uses in the Central Valley, California, by using two parametric models: (1) the Seasonal Wave model (SeaWave), in which a pulse signal is used to describe the annual cycle of pesticide occurrence in a stream, and (2) the Sine Wave model, in which first-order Fourier series sine and cosine terms are used to simulate seasonal mass loading patterns. The models were applied to data collected during water years 1997 through 2005. The pesticides modeled were carbaryl, diazinon, metolachlor, and molinate. Results from the two models show that the ability to capture seasonal variations in pesticide concentrations was affected by pesticide use patterns and the methods by which pesticides are transported to streams. Estimated seasonal loads compared well with results from previous studies for both models. Loads estimated by the two models did not differ significantly from each other, with the exceptions of carbaryl and molinate during the precipitation season, where loads were affected by application patterns and rainfall. However, in watersheds with variable and intermittent pesticide applications, the SeaWave model is more suitable for use on the basis of its robust capability of describing seasonal variation of pesticide concentrations.

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

    NASA Technical Reports Server (NTRS)

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

    2013-01-01

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

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

    NASA Astrophysics Data System (ADS)

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

    2013-09-01

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

  14. Characterization of Speciated Aerosol Direct Radiative Forcing Over California

    SciTech Connect

    Zhao, Chun; Leung, Lai-Yung R.; Easter, Richard C.; Hand, Jenny; Avise, J.

    2013-03-16

    A fully coupled meteorology-chemistry model (WRF-Chem) with added capability of diagnosing the spatial and seasonal distribution of radiative forcings for individual aerosol species over California is used to characterize the radiative forcing of speciated aerosols in California. Model simulations for the year of 2005 are evaluated with various observations including meteorological data from California Irrigation Management Information System (CIMIS), aerosol mass concentrations from US EPA Chemical Speciation Network (CSN) and Interagency Monitoring of Protected Visual Environments (IMPROVE), and aerosol optical depth from AErosol RObotic NETwork (AERONET) and satellites. The model well captures the observed seasonal meteorological conditions over California. Overall, the simulation is able to reproduce the observed spatial and seasonal distribution of mass concentration of total PM2.5 and the relative contribution from individual aerosol species, except the model significantly underestimates the surface concentrations of organic matter (OM) and elemental carbon (EC), potentially due to uncertainty in the anthropogenic emissions of OM and EC and the outdated secondary organic aerosol mechanism used in the model. A sensitivity simulation with anthropogenic EC emission doubled significantly reduces the model low bias of EC. The simulation reveals high anthropogenic aerosol loading over the Central Valley and the Los Angeles metropolitan regions and high natural aerosol (dust) loading over southeastern California. The seasonality of aerosol surface concentration is mainly determined by vertical turbulent mixing, ventilation, and photochemical activity, with distinct characteristics for individual aerosol species and between urban and rural areas. The simulations show that anthropogenic aerosols dominate the aerosol optical depth (AOD). The ratio of AOD to AAOD (aerosol absorption optical depth) shows distinct seasonality with a winter maximum and a summer minimum

  15. Characterization of the organic matter in submicron urban aerosols using a Thermo-Desorption Proton-Transfer-Reaction Time-of-Flight Mass Spectrometer (TD-PTR-TOF-MS)

    NASA Astrophysics Data System (ADS)

    Salvador, Christian Mark; Ho, T.-T.; Chou, Charles C.-K.; Chen, M.-J.; Huang, W.-R.; Huang, S.-H.

    2016-09-01

    Organic matter is the most complicated and unresolved major component of atmospheric aerosol particles. Its sources and global budget are still highly uncertain and thereby necessitate further research efforts with state-of-the-art instrument. This study employed a Thermo-Desorption Proton-Transfer-Reaction Time-of-Flight Mass Spectrometer (TD-PTR-TOF-MS) for characterization of ambient organic aerosols. First, five authentic standard substances, which include phthalic acid, levoglucosan, arabitol, cis-pinonic acid and glutaric acid, were utilized to examine the response of the instrument. The results demonstrated the linearity of the TD-PTR-TOF-MS signals against a range of mass loading of specific species on filters. However, it was found that significant fragmentation happened to those challenging compounds, although the proton-transfer-reaction (PTR) was recognized as a soft ionization technique. Consequently, quantitative characterization of aerosols with the TD-PTR-TOF-MS depended on the availability of the fragmentation pattern in mass spectra and the recovery rate with the quantification ion peak(s). The instrument was further deployed to analyze a subset of submicron aerosol samples collected at the TARO (Taipei Aerosol and Radiation Observatory) in Taipei, Taiwan during August 2013. The results were compared with the measurements from a conventional DRI thermo-optical carbon analyzer. The inter-comparison indicated that the TD-PTR-TOF-MS underestimated the mass of total organic matter (TOM) in aerosol samples by 27%. The underestimation was most likely due to the thermo-decomposition during desorption processes and fragmentation in PTR drift tube, where undetectable fragments were formed. Besides, condensation loss of low vapor pressure species in the transfer components was also responsible for the underestimation to a certain degree. Nevertheless, it was showed that the sum of the mass concentrations of the major detected ion peaks correlated strongly

  16. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a.

  17. Sources and characteristics of fine particles over the Yellow Sea and Bohai Sea using online single particle aerosol mass spectrometer.

    PubMed

    Fu, Huaiyu; Zheng, Mei; Yan, Caiqing; Li, Xiaoying; Gao, Huiwang; Yao, Xiaohong; Guo, Zhigang; Zhang, Yuanhang

    2015-03-01

    Marine aerosols over the East China Seas are heavily polluted by continental sources. During the Chinese Comprehensive Ocean Experiment in November 2012, size and mass spectra of individual atmospheric particles in the size range from 0.2 to 2.0 μm were measured on board by a single particle aerosol mass spectrometer (SPAMS). The average hourly particle number (PN) was around 4560±3240 in the South Yellow Sea (SYS), 2900±3970 in the North Yellow Sea (NYS), and 1700±2220 in the Bohai Sea (BS). PN in NYS and BS varied greatly over 3 orders of magnitude, while that in SYS varied slightly. The size distributions were fitted with two log-normal modes. Accumulation mode dominated in NYS and BS, especially during episodic periods. Coarse mode particles played an important role in SYS. Particles were classified using an adaptive resonance theory based neural network algorithm (ART-2a). Six particle types were identified with secondary-containing, aged sea-salt, soot-like, biomass burning, fresh sea-salt, and lead-containing particles accounting for 32%, 21%, 18%, 16%, 4%, and 3% of total PN, respectively. Aerosols in BS were relatively enriched in particles from anthropogenic sources compared to SYS, probably due to emissions from more developed upwind regions and indicating stronger influence of continental outflow on marine environment. Variation of source types depended mainly on origins of transported air masses. This study examined rapid changes in PN, size distribution and source types of fine particles in marine atmospheres. It also demonstrated the effectiveness of high-time-resolution source apportionment by ART-2a. PMID:25766014

  18. Receptor modeling of near-roadway aerosol mass spectrometer data in Las Vegas, Nevada, with EPA PMF

    NASA Astrophysics Data System (ADS)

    Brown, S. G.; Lee, T.; Norris, G. A.; Roberts, P. T.; Collett, J. L., Jr.; Paatero, P.; Worsnop, D. R.

    2011-08-01

    Ambient non-refractory PM1 aerosol particles were measured with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) at an elementary school 20 m from the US 95 freeway in Las Vegas, Nevada, during January 2008. Additional collocated continuous measurements of black carbon (BC), carbon monoxide (CO), nitrogen oxides (NOx), and meteorological data were collected. The US Environmental Protection Agency's (EPA) positive matrix factorization (PMF) data analysis tool was used to apportion organic matter (OM) as measured by HR-AMS, and rotational tools in EPA PMF were used to better characterize the solution space and pull resolved factors toward known source profiles. Three- to six-factor solutions were resolved. The four-factor solution was the most interpretable, with the typical AMS PMF factors of hydrocarbon-like organic aerosol (HOA), low-volatility oxygenated organic aerosol (LV-OOA), biomass burning organic aerosol (BBOA), and semi-volatile oxygenated organic aerosol (SV-OOA). When the measurement site was downwind of the freeway, HOA composed about half the OM, with SV-OOA and LV-OOA accounting for the rest. Attempts to pull the PMF factor profiles toward source profiles were successful but did not qualitatively change the results, indicating that these factors are very stable. Oblique edges were present in G-space plots, suggesting that the obtained rotation may not be the most plausible one. Since solutions found by pulling the profiles or using Fpeak retained these oblique edges, there appears to be little rotational freedom in the base solution. On average, HOA made up 26 % of the OM, and it made up nearly half of the OM when the monitoring site was downwind of US 95 during morning rush hour. LV-OOA was highest in the afternoon and accounted for 26 % of the OM. BBOA occurred in the evening hours, was predominantly from the residential area to the north, and on average constituted 12 % of the OM; SV-OOA accounted for the remaining

  19. Receptor modeling of near-roadway aerosol mass spectrometer data in Las Vegas, Nevada, with EPA PMF

    NASA Astrophysics Data System (ADS)

    Brown, S. G.; Lee, T.; Norris, G. A.; Roberts, P. T.; Collett, J. L., Jr.; Paatero, P.; Worsnop, D. R.

    2012-01-01

    Ambient non-refractory PM1 aerosol particles were measured with an Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-AMS) at an elementary school 18 m from the US 95 freeway soundwall in Las Vegas, Nevada, during January 2008. Additional collocated continuous measurements of black carbon (BC), carbon monoxide (CO), nitrogen oxides (NOx), and meteorological data were collected. The US~Environmental Protection Agency's~(EPA) positive matrix factorization (PMF) data analysis tool was used to apportion organic matter (OM) as measured by HR-AMS, and rotational tools in EPA PMF were used to better characterize the solution space and pull resolved factors toward known source profiles. Three- to six-factor solutions were resolved. The four-factor solution was the most interpretable, with the typical AMS PMF factors of hydrocarbon-like organic aerosol (HOA), low-volatility oxygenated organic aerosol (LV-OOA), biomass burning organic aerosol (BBOA), and semi-volatile oxygenated organic aerosol (SV-OOA). When the measurement site was downwind of the freeway, HOA composed about half the OM, with SV-OOA and LV-OOA accounting for the rest. Attempts to pull the PMF factor profiles toward source profiles were successful but did not qualitatively change the results, indicating that these factors are very stable. Oblique edges were present in G-space plots, suggesting that the obtained rotation may not be the most plausible one. Since solutions found by pulling the profiles or using Fpeak retained these oblique edges, there appears to be little rotational freedom in the base solution. On average, HOA made up 26% of the OM, while LV-OOA was highest in the afternoon and accounted for 26% of the OM. BBOA occurred in the evening hours, was predominantly from the residential area to the north, and on average constituted 12% of the OM; SV-OOA accounted for the remaining third of the OM. Use of the pulling techniques available in EPA PMF and ME-2 suggested that the four

  20. Evaluating mass loading products by comparison to GPS array daily solutions

    NASA Astrophysics Data System (ADS)

    Xu, Chang

    2016-10-01

    We evaluate the benefit of different global geophysical loading products on the internal scatter of GPS position time series from 240 globally distributed sites. We focus on the non-tidal atmospheric pressure loading predicted from NASA's Modern-Era Retrospective Analysis for Research and Applications (MERRA-NATML) and the European Center for Medium-Range Weather Forecasts operational model (ECMWF-NATML), non-tidal ocean loading predicted from the Ocean Model for Circulation and Tides model (OMCT-NTOL), and the continental water storage loading predicted from the MERRA model (MERRA-CWSL) and the GFZ's Land Surface Discharge Model (LSDM-CWSL), respectively. The result shows that the root mean square (RMS) discrepancy of different CWSL models is larger than that of NATML models in the vertical component due to the varying model parameters and input data choices. We discuss the performance of different loading models and their combination to reduce the weighted RMS of GPS up-coordinates. MERRA-NATML & OMCT-NTOL & MERRA-CWSL reduced the weighted RMS (WRMS) in 96% (JPL solutions) and 86% (SOPAC solutions) of the cases, and ECMWF-NATML & OMCT-NTOL & LSDM-CWSL reduced the WRMS in 95% (JPL solutions) and 88% (SOPAC solutions) of the cases. The result shows that local effects and technical uncertainties in GPS time series hamper the meaningful comparison between GPS observations and mass loading models. Hence, simply using the RMS of the time series as the assessment criteria may lead to biased comparison results. Nonetheless, we give a detailed comparison (differences in phase and amplitude at seasonal timescales) for 8 representative stations located adjacent to great rivers, lakes, and reservoirs. We find that LSDM can provide a complementary model to study the small-scale hydrological loading like loading extremes along river channels. However, such small-scale hydrological loading effects are still instable to be modeled in some regions with its current accuracy

  1. 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.

  2. 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.

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

    NASA Astrophysics Data System (ADS)

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

    2013-04-01

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

  4. Enhancement of effective electromechanical coupling factor by mass loading in layered surface acoustic wave device structures

    NASA Astrophysics Data System (ADS)

    Tang, Gongbin; Han, Tao; Teshigahara, Akihiko; Iwaki, Takao; Hashimoto, Ken-ya

    2016-07-01

    This paper describes a drastic enhancement of the effective coupling factor K\\text{e}2 by mass loading in layered surface acoustic wave (SAW) device structures such as the ScAlN film/Si substrate structure. This phenomenon occurs when the piezoelectric layer exhibits a high acoustic wave velocity. The mass loading decreases the SAW velocity and causes SAW energy confinement close to the top surface where an interdigital transducer is placed. It is shown that this phenomenon is obvious even when an amorphous SiO2 film is deposited on the top surface for temperature compensation. This K\\text{e}2 enhancement was also found in various combinations of electrode, piezoelectric layer, and/or substrate materials. The existence of this phenomenon was verified experimentally using the ScAlN film/Si substrate structure.

  5. Sparing of muscle mass and function by passive loading in an experimental intensive care unit model.

    PubMed

    Renaud, Guillaume; Llano-Diez, Monica; Ravara, Barbara; Gorza, Luisa; Feng, Han-Zhong; Jin, Jian-Ping; Cacciani, Nicola; Gustafson, Ann-Marie; Ochala, Julien; Corpeno, Rebeca; Li, Meishan; Hedström, Yvette; Ford, G Charles; Nair, K Sreekumaran; Larsson, Lars

    2013-03-01

    The response to mechanical stimuli, i.e., tensegrity, plays an important role in regulating cell physiological and pathophysiological function, and the mechanical silencing observed in intensive care unit (ICU) patients leads to a severe and specific muscle wasting condition. This study aims to unravel the underlying mechanisms and the effects of passive mechanical loading on skeletal muscle mass and function at the gene, protein and cellular levels. A unique experimental rat ICU model has been used allowing long-term (weeks) time-resolved analyses of the effects of standardized unilateral passive mechanical loading on skeletal muscle size and function and underlying mechanisms. Results show that passive mechanical loading alleviated the muscle wasting and the loss of force-generation associated with the ICU intervention, resulting in a doubling of the functional capacity of the loaded versus the unloaded muscles after a 2-week ICU intervention. We demonstrate that the improved maintenance of muscle mass and function is probably a consequence of a reduced oxidative stress revealed by lower levels of carbonylated proteins, and a reduced loss of the molecular motor protein myosin. A complex temporal gene expression pattern, delineated by microarray analysis, was observed with loading-induced changes in transcript levels of sarcomeric proteins, muscle developmental processes, stress response, extracellular matrix/cell adhesion proteins and metabolism. Thus, the results from this study show that passive mechanical loading alleviates the severe negative consequences on muscle size and function associated with the mechanical silencing in ICU patients, strongly supporting early and intense physical therapy in immobilized ICU patients. PMID:23266938

  6. 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... Concentration Measurement of PM2.5 for Idealized Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  7. 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... Concentration Measurement of PM 2.5 for Idealized Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  8. 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... Concentration Measurement of PM 2.5 for Idealized Fine Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m3) Estimated...

  9. 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... Concentration Measurement of PM 2.5 for Idealized Fine Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m 3)...

  10. 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... Concentration Measurement of PM2.5 for Idealized Fine Aerosol Size Distribution Particle Aerodynamic Diameter (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, 2013 CFR

    2013-07-01

    ... 40 Protection of Environment 6 2013-07-01 2013-07-01 false Estimated Mass Concentration... Concentration Measurement of PM 2.5 for Idealized Coarse Aerosol Size Distribution Particle Aerodynamic Diameter (µm) Test Sampler Fractional Sampling Effectiveness Interval Mass Concentration (µg/m 3)...

  12. 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...

  13. High illness loads (physical and social) do not always force high levels of mass religiosity.

    PubMed

    Paul, Gregory S

    2012-04-01

    The hypothesis that high levels of religiosity are partly caused by high disease loads is in accord with studies showing that societal dysfunction promotes mass supernaturalism. However, some cultures suffering from high rates of disease and other socioeconomic dysfunction exhibit low levels of popular religiosity. At this point, it appears that religion is hard pressed to thrive in healthy societies, but poor conditions do not always make religion popular, either.

  14. SWAP-SECCHI OBSERVATIONS OF A MASS-LOADING TYPE SOLAR ERUPTION

    SciTech Connect

    Seaton, Daniel B.; Mierla, Marilena; Berghmans, David; Zhukov, Andrei N.; Dolla, Laurent

    2011-01-20

    We present a three-dimensional reconstruction of an eruption that occurred on 2010 April 3 using observations from SWAP on board PROBA2 and SECCHI on board STEREO. The event unfolded in two parts: an initial flow of cooler material confined to a height low in the corona, followed by a flux rope eruption higher in the corona. We conclude that mass off-loading from the first part triggered a rise and, subsequently, catastrophic loss of equilibrium of the flux rope.

  15. Background Southeast United States Aerosol Optical Properties and Their Dependence Upon Meteorology

    NASA Astrophysics Data System (ADS)

    Pawlyszyn, C.; West, M.; Sherman, J. P.; Link, M.; Zhou, Y.

    2015-12-01

    Aerosol effects on SE U.S. radiation budget are highly-seasonal. Aerosol loading is much higher in summer, due largely to high levels of biogenic secondary organic aerosol and sulfates. Aerosol loading is lowest in winter. Aerosol optical properties relevant to radiative forcing have been measured continuously at the Appalachian Atmospheric Interdisciplinary Research facility (AppalAIR) since the summer of 2009. AppalAIR is the only site in the eastern US to house co-located NOAA ESRL and NASA AeroNET instrumentation and is located in the mountains of Boone, NC. Lower tropospheric sub-micron (PM1) light scattering and absorption coefficients measured over seven summers and six winters are presented here, in addition to PM1 organic and sulfate aerosol mass concentrations measured during summers 2012-2013 as well as winter 2013. The objective is to determine the influence of aerosol sources and meteorology along the air mass back-trajectories on aerosol loading and composition. PM1 aerosol mass was dominated by organic aerosol and sulfate during the periods measured. Aerosol light scattering and organic aerosol concentrations were positively correlated during summer with temperature and solar flux along the parcel back-trajectory and negatively-correlated with rainfall along the back-trajectory. Wet deposition was a major factor in the difference between the upper and lower scattering coefficient quartiles for both summer and winter. Summer PM1 light scattering coefficient declined by approximately 30-40% since 2009, with smaller decreases during winter months. Long-term studies of aerosol optical properties from the regionally-representative AppalAIR site are necessary to determine the relationships between changing SE U.S. air quality and aerosol effects on regional climate and weather.

  16. 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

  17. Concentrations and mass loadings of hormones, alkylphenols, and alkylphenol ethoxylates in healthcare facility wastewaters.

    PubMed

    Nagarnaik, P M; Mills, M A; Boulanger, B

    2010-02-01

    Healthcare facility wastewaters are an anticipated source of known endocrine disrupting chemicals to the environment. In this study, the composition and magnitude of eight steroid hormones, octylphenol (OP), nonylphenol (NP), 16 nonylphenol ethoxylates (NPEOs), and 10 octylphenol ethoxylates (OPEOs) in wastewater from a(n) hospital, nursing facility, assisted living facility, and independent living facility are presented. Steroid hormone concentrations were variable for each sampling location, ranging from a non-detectable concentration of 17beta-ethynylestradiol in all samples to 127ngL(-1) androstenedione in the hospital's wastewater composite. OP and NP were not detected in any site's samples. However, NPEOs were found at each sampling location with a maximum combined concentration of 260microgL(-1) for NPEOs with a chain length between 3 and 18 units in the assisted living facility composite sample. OPEOs were only found in the hospital and nursing facilities samples with a maximum combined OPEO concentration of 13microgL(-1) for OPEOs with a chain length between 2 and 12 units in hospital wastewater. The total mass loading of hormones to the municipal sewer system from each facility ranged from 2.5mgd(-1) at the assisted living facility to 138mgd(-1) at the hospital. The total mass loading of the alklyphenol ethoxylates (NPEO+OPEO) is considerably higher than the estimated hormone mass loadings, ranging from 1.8gd(-1) at the independent living facility to 54gd(-1) at the hospital facility. PMID:20079514

  18. Characterization of particulate matter emissions from on-road gasoline and diesel vehicles using a soot particle aerosol mass spectrometer

    NASA Astrophysics Data System (ADS)

    Dallmann, T. R.; Onasch, T. B.; Kirchstetter, T. W.; Worton, D. R.; Fortner, E. C.; Herndon, S. C.; Wood, E. C.; Franklin, J. P.; Worsnop, D. R.; Goldstein, A. H.; Harley, R. A.

    2014-02-01

    Particulate matter (PM) emissions were measured in July 2010 from on-road motor vehicles driving through a highway tunnel in the San Francisco Bay area. A soot particle aerosol mass spectrometer (SP-AMS) was used to measure the chemical composition of PM emitted by gasoline and diesel vehicles at high time resolution. Organic aerosol (OA) and black carbon (BC) concentrations were measured during various time periods that had different levels of diesel influence, as well as directly in the exhaust plumes of individual heavy-duty (HD) diesel trucks. BC emission factor distributions for HD trucks were more skewed than OA distributions, with the highest 10% of trucks accounting for 56 and 42% of total measured BC and OA emissions, respectively. A comparison of measured OA and BC mass spectra across various sampling periods revealed a high degree of similarity in BC and OA emitted by gasoline and diesel engines. Cycloalkanes predominate in exhaust OA emissions relative to saturated alkanes (i.e., normal and iso-paraffins), suggesting that lubricating oil rather than fuel is the dominant source of primary organic aerosol (POA) emissions in diesel vehicle exhaust. This finding is supported by the detection of trace elements such as zinc and phosphorus in the exhaust plumes of individual trucks. Trace elements were emitted relative to total OA at levels that are consistent with typical weight fractions of commonly used additives present in lubricating oil. The presence of trace elements in vehicle exhaust raises the concern that ash deposits may accumulate over time in diesel particle filter systems, and may eventually lead to performance problems that require servicing.

  19. Molecular composition of biogenic secondary organic aerosols using ultrahigh-resolution mass spectrometry: comparing laboratory and field studies

    NASA Astrophysics Data System (ADS)

    Kourtchev, I.; Fuller, S. J.; Giorio, C.; Healy, R. M.; Wilson, E.; O'Connor, I.; Wenger, J. C.; McLeod, M.; Aalto, J.; Ruuskanen, T. M.; Maenhaut, W.; Jones, R.; Venables, D. S.; Sodeau, J. R.; Kulmala, M.; Kalberer, M.

    2014-02-01

    Numerous laboratory experiments have been performed in an attempt to mimic atmospheric secondary organic aerosol (SOA) formation. However, it is still unclear how close the aerosol particles generated in laboratory experiments resemble atmospheric SOA with respect to their detailed chemical composition. In this study, we generated SOA in a simulation chamber from the ozonolysis of α-pinene and a biogenic volatile organic compound (BVOC) mixture containing α- and β-pinene, Δ3-carene, and isoprene. The detailed molecular composition of laboratory-generated SOA was compared with that of background ambient aerosol collected at a boreal forest site (Hyytiälä, Finland) and an urban location (Cork, Ireland) using direct infusion nanoelectrospray ultrahigh-resolution mass spectrometry. Kendrick mass defect and van Krevelen approaches were used to identify and compare compound classes and distributions of the detected species. The laboratory-generated SOA contained a distinguishable group of dimers that was not observed in the ambient samples. The presence of dimers was found to be less pronounced in the SOA from the BVOC mixtures when compared to the one component precursor system. The molecular composition of SOA from both the BVOC mixture and α-pinene represented the overall composition of the ambient sample from the boreal forest site reasonably well, with 72.3 ± 2.5% (n = 3) and 69.1 ± 3.0% (n = 3) common ions, respectively. In contrast, large differences were found between the laboratory-generated BVOC samples and the ambient urban sample. To our knowledge this is the first direct comparison of molecular composition of laboratory-generated SOA from BVOC mixtures and ambient samples.

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

    NASA Astrophysics Data System (ADS)

    Kourtchev, I.; Fuller, S. J.; Giorio, C.; Healy, R. M.; Wilson, E.; O'Connor, I. P.; Wenger, J. C.; McLeod, M.; Aalto, J.; Ruuskanen, T. M.; Maenhaut, W.; Jones, R.; Venables, D. S.; Sodeau, J. R.; Kulmala, M.; Kalberer, M.

    2013-11-01

    Numerous laboratory experiments have been performed in an attempt to mimic atmospheric secondary organic aerosol (SOA) formation. However, it is still unclear how close the aerosol particles generated in laboratory experiments resemble atmospheric SOA with respect to their detailed chemical composition. In this study, we generated SOA in a simulation chamber from the ozonolysis of α-pinene and a biogenic volatile organic compound (BVOC) mixture containing α- and β-pinene, Δ3-carene, and isoprene. The detailed molecular composition of laboratory-generated SOA was compared with that of background ambient aerosol collected at a boreal forest site (Hyytiälä, Finland) and an urban location (Cork, Ireland) using direct infusion nanoelectrospray ultrahigh resolution mass spectrometry. Kendrick Mass Defect and Van Krevelen approaches were used to identify and compare compound classes and distributions of the detected species. The laboratory-generated SOA contained a distinguishable group of dimers that was not observed in the ambient samples. The presence of dimers was found to be less pronounced in the SOA from the VOC mixtures when compared to the one component precursor system. The elemental composition of the compounds identified in the monomeric region from the ozonolysis of both α-pinene and VOC mixtures represented the ambient organic composition of particles collected at the boreal forest site reasonably well, with about 70% of common molecular formulae. In contrast, large differences were found between the laboratory-generated BVOC samples and the ambient urban sample. To our knowledge this is the first direct comparison of molecular composition of laboratory-generated SOA from BVOC mixtures and ambient samples.

  1. Influence of marine aerosols and aerotechnogenic load on chemical composition of rainwaters on small islands (ludas) of the White Sea

    NASA Astrophysics Data System (ADS)

    Gorbacheva, Tamara; Mazukhina, Svetlana; Isaeva, Ludmila; Shumilov, Oleg

    2013-04-01

    In June 2001 intensive monitoring plots were established on the island part of Kandalaksha Bay of the White Sea (the island Tonnaya Luda; 67o06'60"N; 32o24'12"E) with the installation of stationary rainwater collectors. The purpose was studying the chemical composition of rain waters in the zone of cumulative influence of marine aerosols and aerotechnogenic load. Water sampling was carried out monthly during the vegetative season of 2001 and 2002. pH of rain water was determined by potentiometric method without preliminary filtration. The samples were passed through the paper filter with the pore diameter of 1-2.5 microns, the analysis of filtrate carried out by methods of atomic emission spectrometry (K, Na) and atomic absorption spectrometry (Ca, Mg, Zn, Mn, Cu, Ni, Al, Fe), total P and P of phosphates, Si and NH4+ - by photocolorimetry, total carbon - by bichromate method, NO3-, SO42-, Cl--by ion exchange chromatography method. Balance method was chosen as a research basis to determine the interrelation of rain water organic matter and dynamics of its redistribution under the influence of natural and technogenic factors. The difference between the cations sum (including NH4+and H+) and mineral acids anions sum (SO42-, Cl-, NO3-) was identified as organic acids anions concentration (μeq l-1). The level of Na, Cl-, K, Ca, Mg, SO42-, Sr in rainwaters on the island and the remote areas is indicative of the possible influence of marine aerosols on the island part of the White Sea. The increase of Al, Cu, Ni, Cd, Co concentrations in rainwaters up to one order against the background values points to the cumulative influence of the emissions of industrial enterprises located in the region. The relative stability of pH values of rain waters during all seasons indicates to the buffer action of weak organic acids anions. The correlation analysis of ionic structure in normal concentrations has allowed us to estimate the distribution of the cationic part from the

  2. Black carbon mass size distributions of diesel exhaust and urban aerosols measured using differential mobility analyzer in tandem with Aethalometer

    NASA Astrophysics Data System (ADS)

    Ning, Zhi; Chan, K. L.; Wong, K. C.; Westerdahl, Dane; Močnik, Griša; Zhou, J. H.; Cheung, C. S.

    2013-12-01

    Black carbon (BC) is the dominant component of the light absorbing aerosols in the atmosphere, changing earth's radiative balance and affecting the climate. The mixing state and size distribution of atmospheric BC are largely unknown and cause uncertainties in climate models. BC is also a major component of diesel PM emissions, recently classified by World Health Organization as Category I Carcinogen, and has been associated with various adverse health effects. This study presents a novel approach of direct and continuous measurement of BC mass size distribution by tandem operation of a differential mobility spectrometry and a refined Aethalometer. A condensation particle counter was deployed in parallel with the Aethalometer to determine particle number size distribution. A wide range of particle sizes (20-600 nm) was investigated to determine the BC modal characteristics in fresh diesel engine tailpipe emissions and in different urban environments including a typical urban ambient site and a busy roadside. The study provided a demonstration of a new analytic approach and showed the evolution of BC mass size distribution from fresh engine emissions to the aged aerosols in the roadside and ambient environments. The results potentially can be used to refine the input for climate modeling to determine the effect of particle-bound atmospheric BC on the global climate.

  3. Aging of secondary organic aerosol from small aromatic VOCs. Changes in chemical composition, mass yield, volatility and hygroscopicity

    DOE PAGES

    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

  4. 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

  5. Time-Resolved Molecular Characterization of Limonene/Ozone Aerosol using High-Resolution Electrospray Ionization Mass Spectrometry

    SciTech Connect

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

    2009-09-09

    Molecular composition of limonene/O3 secondary organic aerosol (SOA) was investigated using high-resolution electrospray ionization mass spectrometry (HR-ESI-MS) as a function of reaction time. SOA was generated by ozonation of D-limonene in a reaction chamber and sampled at different time intervals using a cascade impactor. The SOA samples were extracted into acetonitrile and analyzed using a HR-ESI-MS instrument with a resolving power of 100,000 (m/Δm). The resulting mass spectra provided detailed information about the extent of oxidation inferred from the O:C ratios, double bond equivalency (DBE) factors, and aromaticity indexes (AI) in hundreds of identified individual SOA species.

  6. BioAerosol Mass Spectrometry: Reagentless Detection of Individual Airborne Spores and Other Bioagent Particles Based on Laser Desorption/Ionization Mass Spectrometry

    SciTech Connect

    Steele, Paul Thomas

    2004-09-01

    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.

  7. Calibration of microbolometer infrared cameras for measuring volcanic ash mass loading

    NASA Astrophysics Data System (ADS)

    Carroll, Russell C.

    Small spacecraft with thermal infrared (TIR) imaging capabilities are needed to detect dangerous levels of volcanic ash that can severely damage jet aircraft engines and must be avoided. Grounding aircraft after a volcanic eruption may cost the airlines millions of dollars per day, while accurate knowledge of volcanic ash density might allow for safely routing aircraft around dangerous levels of volcanic ash. There are currently limited numbers of satellites with TIR imaging capabilities so the elapsed time between revisits can be large, and these instruments can only resolve total mass loading along the line-of-sight. Multiple small satellites could allow for decreased revisit times as well as multiple viewing angles to reveal the three-dimensional structure of the ash cloud through stereoscopic techniques. This paper presents the design and laboratory evaluation of a TIR imaging system that is designed to fit within the resource constraints of a multi-unit CubeSat to detect volcanic ash mass loading. The laboratory prototype of this TIR imaging system uses a commercial off-the shelf (COTS) camera with an uncooled microbolometer sensor, two narrowband filters, a black body source and a custom filter wheel. The infrared imaging system detects the difference in attenuation of volcanic ash at 11 mum and 12 mum by measuring the brightness temperature at each band. The brightness temperature difference method is used to measure the column mass loading. Multi-aspect images and stereoscopic techniques are needed to estimate the mass density from the mass loading, which is the measured mass per unit area. Laboratory measurements are used to characterize the noise level and thermal stability of the sensor. A calibration technique is developed to compensate for sensor temperature drift. The detection threshold of volcanic ash density of this TIR imaging system is found to be from 0.35 mg/m3 to 26 mg/m3 for ash clouds that have thickness of 1 km, while ash cloud densities

  8. 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.

  9. Aerosol characterization over the southeastern United States using high-resolution aerosol mass spectrometry: spatial and seasonal variation of aerosol composition and sources with a focus on organic nitrates

    NASA Astrophysics Data System (ADS)

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

    2015-07-01

    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 particulate matter (NR-PM1) in the southeastern USA. Measurements were performed in both rural and urban sites in the greater Atlanta area, Georgia (GA), and Centreville, Alabama (AL), for approximately 1 year as part of Southeastern Center for Air Pollution and Epidemiology study (SCAPE) and Southern Oxidant and Aerosol Study (SOAS). Organic aerosol (OA) accounts for more than half of NR-PM1 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 (i.e., 21-38 % of total OA depending on site and season). 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 factor (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

  10. Fine Mode Aerosol over the United Arab Emirates

    NASA Astrophysics Data System (ADS)

    Ross, K. E.; Piketh, S. J.; Reid, J. S.; Reid, E. A.

    2005-12-01

    The aerosol loading of the atmosphere over the Arabian Gulf region is extremely diverse and is composed not only of dust, but also of pollution that is derived largely from oil-related activities. Fine mode pollution particles are most efficient at scattering incoming solar radiation and have the potential to act as cloud condensation nuclei (CCN), and may therefore have implications for climate change. The smaller aerosols may also pose a health hazard if present in high concentrations. The United Arab Emirates Unified Aerosol Experiment (UAE2) was designed to investigate aerosol and meteorological characteristics over the region using ground-based, aircraft and satellite measurements, and was conducted in August and September 2004. Aerosol chemical composition has been obtained from filters that were collected at the site of the Mobile Atmospheric Aerosol and Radiation Characterization Observatory (MAARCO) on the coast of the UAE between Abu Dhabi and Dubai. Filter samples were also collected on an airborne platform in order to assess how aerosol chemical composition varies across the region and throughout the depth of the boundary layer. Results of the analysis of the PM2.5 coastal samples show that ammonium sulphate is the most prevalent constituent of the fine mode aerosol in the region (>50% of the mass), followed by organic matter, alumino-silicates, calcium carbonate and black carbon. Source apportionment indicates that most of the fine aerosol mass is derived from fossil fuel combustion, while mineral dust and local vehicle emissions also contribute to the fine aerosol loading. The organic carbon-to-total carbon ratio of the aerosol is 0.65, which is typical of fossil fuel combustion. The dominance of sulphates means that the fine mode aerosol in the region is probably responsible for a negative radiative forcing, and that the polluting emissions significantly elevate the concentration of CCN.

  11. Cascade model for particle concentration and enstrophy in fully developed turbulence with mass-loading feedback.

    PubMed

    Hogan, R C; Cuzzi, J N

    2007-05-01

    A cascade model is described based on multiplier distributions determined from three-dimensional (3D) direct numerical simulations (DNS) of turbulent particle laden flows, which include two-way coupling between the phases at global mass loadings equal to unity. The governing Eulerian equations are solved using psuedospectral methods on up to 512(3) computional grid points. DNS results for particle concentration and enstrophy at Taylor microscale Reynolds numbers in the range 34-170 were used to directly determine multiplier distributions on spatial scales three times the Kolmogorov length scale. The multiplier probability distribution functions (PDFs) are well characterized by the beta distribution function. The width of the PDFs, which is a measure of intermittency, decreases with increasing mass loading within the local region where the multipliers are measured. The functional form of this dependence is not sensitive to Reynolds numbers in the range considered. A partition correlation probability is included in the cascade model to account for the observed spatial anticorrelation between particle concentration and enstrophy. Joint probability distribution functions of concentration and enstrophy generated using the cascade model are shown to be in excellent agreement with those derived directly from our 3D simulations. Probabilities predicted by the cascade model are presented at Reynolds numbers well beyond what is achievable by direct simulation. These results clearly indicate that particle mass loading significantly reduces the probabilities of high particle concentration and enstrophy relative to those resulting from unloaded runs. Particle mass density appears to reach a limit at around 100 times the gas density. This approach has promise for significant computational savings in certain applications.

  12. Introducing the aerosol-climate model MAECHAM5-SAM2

    NASA Astrophysics Data System (ADS)

    Hommel, R.; Timmreck, C.; Graf, H. F.

    2009-04-01

    We are presenting a new global aerosol model MAECHAM5-SAM2 to study the aerosol dynamics in the UTLS under background and volcanic conditions. The microphysical core modul SAM2 treats the formation, the evolution and the transport of stratospheric sulphuric acid aerosol. The aerosol size distribution and the weight percentage of the sulphuric acid solution is calculated dependent on the concentrations of H2SO4 and H2O, their vapor pressures, the atmospheric temperature and pressure. The fixed sectional method is used to resolve an aerosol distribution between 1 nm and 2.6 micron in particle radius. Homogeneous nucleation, condensation and evaporation, coagulation, water-vapor growth, sedimentation and sulphur chemistry are included. The module is applied in the middle-atmosphere MAECHAM5 model, resolving the atmosphere up to 0.01 hPa (~80 km) in 39 layers. It is shown here that MAECHAM5-SAM2 well represents in-situ measured size distributions of stratospheric background aerosol in the northern hemisphere mid-latitudes. Distinct differences can be seen when derived integrated aerosol parameters (surface area, effective radius) are compared with aerosol climatologies based on the SAGE II satellite instrument (derived by the University of Oxford and the NASA AMES laboratory). The bias between the model and the SAGE II data increases as the moment of the aerosol size distribution decreases. Thus the modeled effective radius show the strongest bias, followed by the aerosol surface area density. Correspondingly less biased are the higher moments volume area density and the mass density of the global stratospheric aerosol coverage. This finding supports the key finding No. 2 of the SPARC Assessment of Stratospheric Aerosol Properties (2006), where it was shown that during periods of very low aerosol load in the stratosphere, the consistency between in-situ and satellite measurements, which exist in a volcanically perturbed stratosphere, breaks down and significant

  13. Influence of seed aerosol surface area and oxidation rate on vapor wall deposition and SOA mass yields: a case study with α-pinene ozonolysis

    NASA Astrophysics Data System (ADS)

    Nah, Theodora; McVay, Renee C.; Zhang, Xuan; Boyd, Christopher M.; Seinfeld, John H.; Ng, Nga L.

    2016-07-01

    Laboratory chambers, invaluable in atmospheric chemistry and aerosol formation studies, are subject to particle and vapor wall deposition, processes that need to be accounted for in order to accurately determine secondary organic aerosol (SOA) mass yields. Although particle wall deposition is reasonably well understood and usually accounted for, vapor wall deposition is less so. The effects of vapor wall deposition on SOA mass yields in chamber experiments can be constrained experimentally by increasing the seed aerosol surface area to promote the preferential condensation of SOA-forming vapors onto seed aerosol. Here, we study the influence of seed aerosol surface area and oxidation rate on SOA formation in α-pinene ozonolysis. The observations are analyzed using a coupled vapor-particle dynamics model to interpret the roles of gas-particle partitioning (quasi-equilibrium vs. kinetically limited SOA growth) and α-pinene oxidation rate in influencing vapor wall deposition. We find that the SOA growth rate and mass yields are independent of seed surface area within the range of seed surface area concentrations used in this study. This behavior arises when the condensation of SOA-forming vapors is dominated by quasi-equilibrium growth. Faster α-pinene oxidation rates and higher SOA mass yields are observed at increasing O3 concentrations for the same initial α-pinene concentration. When the α-pinene oxidation rate increases relative to vapor wall deposition, rapidly produced SOA-forming oxidation products condense more readily onto seed aerosol particles, resulting in higher SOA mass yields. Our results indicate that the extent to which vapor wall deposition affects SOA mass yields depends on the particular volatility organic compound system and can be mitigated through the use of excess oxidant concentrations.

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

    NASA Astrophysics Data System (ADS)

    Cross, E. S.; Onasch, T. B.; Canagaratna, M.; Jayne, J. T.; Kimmel, J.; Yu, X.-Y.; Alexander, M. L.; Worsnop, D. R.; Davidovits, P.

    2008-12-01

    We present the first single particle results obtained using an Aerodyne time-of-flight aerosol mass spectrometer coupled with a light scattering module (LS-ToF-AMS). The instrument was deployed at the T1 ground site approximately 40 km northeast of the Mexico City Metropolitan Area (MCMA) as part of the MILAGRO field study in March of 2006. The instrument was operated as a standard AMS from 12-30 March, acquiring average chemical composition and size distributions for the ambient aerosol, and in single particle mode from 27-30 March. Over a 75-h sampling period, 12 853 single particle mass spectra were optically triggered, saved, and analyzed. The correlated optical and chemical detection allowed detailed examination of single particle collection and quantification within the LS-ToF-AMS. The single particle data enabled the mixing states of the ambient aerosol to be characterized within the context of the size-resolved ensemble chemical information. The particulate mixing states were examined as a function of sampling time and most of the particles were found to be internal mixtures containing many of the organic and inorganic species identified in the ensemble analysis. The single particle mass spectra were deconvolved, using techniques developed for ensemble AMS data analysis, into HOA, OOA, NH4NO3, (NH4)2SO4, and NH4Cl fractions. Average single particle mass and chemistry measurements are shown to be in agreement with ensemble MS and PTOF measurements. While a significant fraction of ambient particles were internal mixtures of varying degrees, single particle measurements of chemical composition allowed the identification of time periods during which the ambient ensemble was externally mixed. In some cases the chemical composition of the particles suggested a likely source. Throughout the full sampling period, the ambient ensemble was an external mixture of combustion-generated HOA particles from local sources (e.g. traffic), with number concentrations peaking

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

    PubMed

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

    2015-05-14

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

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

    PubMed

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

    2015-05-14

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

  17. 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

  18. Axisymmetric modeling of cometary mass loading on an adaptively refined grid: MHD results

    NASA Technical Reports Server (NTRS)

    Gombosi, Tamas I.; Powell, Kenneth G.; De Zeeuw, Darren L.

    1994-01-01

    The first results of an axisymmetric magnetohydrodynamic (MHD) model of the interaction of an expanding cometary atmosphere with the solar wind are presented. The model assumes that far upstream the plasma flow lines are parallel to the magnetic field vector. The effects of mass loading and ion-neutral friction are taken into account by the governing equations, whcih are solved on an adaptively refined unstructured grid using a Monotone Upstream Centered Schemes for Conservative Laws (MUSCL)-type numerical technique. The combination of the adaptive refinement with the MUSCL-scheme allows the entire cometary atmosphere to be modeled, while still resolving both the shock and the near nucleus of the comet. The main findingsare the following: (1) A shock is formed approximately = 0.45 Mkm upstream of the comet (its location is controlled by the sonic and Alfvenic Mach numbers of the ambient solar wind flow and by the cometary mass addition rate). (2) A contact surface is formed approximately = 5,600 km upstream of the nucleus separating an outward expanding cometary ionosphere from the nearly stagnating solar wind flow. The location of the contact surface is controlled by the upstream flow conditions, the mass loading rate and the ion-neutral drag. The contact surface is also the boundary of the diamagnetic cavity. (3) A closed inner shock terminates the supersonic expansion of the cometary ionosphere. This inner shock is closer to the nucleus on dayside than on the nightside.

  19. Effect of hydrophilic organic seed aerosols on secondary organic aerosol formation from ozonolysis of α-pinene.

    PubMed

    Song, Chen; Zaveri, Rahul A; Shilling, John E; Alexander, M Lizabeth; Newburn, Matt

    2011-09-01

    Gas-particle partitioning theory is widely used in atmospheric models to predict organic aerosol loadings. This theory predicts that secondary organic aerosol (SOA) yield of an oxidized volatile organic compound product will increase as the mass loading of preexisting organic aerosol increases. In a previous work, we showed that the presence of model hydrophobic primary organic aerosol (POA) had no detectable effect on the SOA yields from ozonolysis of α-pinene, suggesting that the condensing SOA compounds form a separate phase from the preexisting POA. However, a substantial faction of atmospheric aerosol is composed of polar, hydrophilic organic compounds. In this work, we investigate the effects of model hydrophilic organic aerosol (OA) species such as fulvic acid, adipic acid, and citric acid on the gas-particle partitioning of SOA from α-pinene ozonolysis. The results show that only citric acid seed significantly enhances the absorption of α-pinene SOA into the particle-phase. The other two seed particles have a negligible effect on the α-pinene SOA yields, suggesting that α-pinene SOA forms a well-mixed organic aerosol phase with citric acid and a separate phase with adipic acid and fulvic acid. This finding highlights the need to improve the thermodynamics treatment of organics in current aerosol models that simply lump all hydrophilic organic species into a single phase, thereby potentially introducing an erroneous sensitivity of SOA mass to emitted OA species. PMID:21790137

  20. Characterization of aromaticity in analogues of titan's atmospheric aerosols with two-step laser desorption ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

    Mahjoub, Ahmed; Schwell, Martin; Carrasco, Nathalie; Benilan, Yves; Cernogora, Guy; Szopa, Cyril; Gazeau, Marie-Claire

    2016-10-01

    The role of polycyclic aromatic hydrocarbons (PAH) and Nitrogen containing PAH (PANH) as intermediates of aerosol production in the atmosphere of Titan has been a subject of controversy for a long time. An analysis of the atmospheric emission band observed by the Visible and Infrared Mapping Spectrometer (VIMS) at 3.28 μm suggests the presence of neutral polycyclic aromatic species in the upper atmosphere of Titan. These molecules are seen as the counter part of negative and positive aromatics ions suspected by the Plasma Spectrometer onboard the Cassini spacecraft, but the low resolution of the instrument hinders any molecular speciation. In this work we investigate the specific aromatic content of Titan's atmospheric aerosols through laboratory simulations. We report here the selective detection of aromatic compounds in tholins, Titan's aerosol analogs, produced with a capacitively coupled plasma in a N2:CH4 95:5 gas mixture. For this purpose, Two-Step Laser Desorption Ionization Time-of-Flight Mass Spectrometry (L2DI-TOF-MS) technique is used to analyze the so produced analogs. This analytical technique is based on the ionization of molecules by Resonance Enhanced Multi-Photon Ionization (REMPI) using a λ=248 nm wavelength laser which is selective for aromatic species. This allows for the selective identification of compounds having at least one aromatic ring. Our experiments show that tholins contain a trace amount of small PAHs with one to three aromatic rings. Nitrogen containing PAHs (PANHs) are also detected as constituents of tholins. Molecules relevant to astrobiology are detected as is the case of the substituted DNA base adenine.

  1. Development of a Metastable Atom Bombardment (MAB) Source for Penning Ionization Time-of-flight Aerosol Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Robinson, C. B.; Kimmel, J. R.; David, D.; Jayne, J. T.; Trimborn, A.; Worsnop, D. R.; Jimenez, J. L.

    2009-12-01

    The Aerodyne time-of-flight aerosol mass spectrometer (ToF-AMS) utilizes thermal vaporization followed by electron ionization (EI) to convert aerosol components to gas-phase ions. The method enables quantification of chemical classes, but the extensive fragmentation caused by EI limits the specificity of both chemical analysis and source identification by factor analysis. To better identify the molecular components of aerosols, we have constructed a metastable atom bombardment (MAB) ionization source that can be interfaced to standard ToF-AMS hardware. A beam of metastable rare gas atoms is produced by a low-voltage DC discharge and focused toward the vaporization plume, yielding Penning Ionization of the analyte molecules. By changing gases, the excited energies of the metastables can be adjusted between 20.61 eV (He) and 9.92 eV (Kr). Source parameters, including pressures, current, geometry, and materials, were optimized for He, Ar, and Kr. Instrument sensitivity and induced fragmentation was characterized for each using lab-generated oleic acid particles. The demonstrated sensitivities are 0.1% of EI (3% of the SNR of EI in the V-mode, comparable to the Q-AMS SNR), which is sufficient for ambient monitoring. A metastable flux of 2.6e14 sr-1sec-1 has been achieved. The MAB-AMS has been deployed to the FLAME-3 campaign at the USDA Fire Sciences Laboratory in Missoula, MT, and used to sample smoke from open burning of different biomass samples. Preliminary results from FLAME-3 will be presented.

  2. A decade of dust: Asian dust and springtime aerosol load in the U.S. Pacific Northwest

    NASA Astrophysics Data System (ADS)

    Fischer, E. V.; Hsu, N. C.; Jaffe, D. A.; Jeong, M.-J.; Gong, S. L.

    2009-02-01

    We integrate SeaWiFS aerosol optical thickness (AOT) over the Taklamakan and Gobi Deserts with U.S. aerosol observations to study surface aerosol variability in the Northwest U.S. in relation to Asian dust emissions. The results indicate that ~50% of the interannual variability in springtime average PM2.5 and PM10 can be explained by changes in Asian dust emissions. On a seasonal timescale, variations in dust emissions appear to be more important in determining the total material crossing the Pacific than the variations in meteorology represented by the PNA or the LRT3 indices. We are able to explain ~80% of the interannual variability using three variables: AOT, a transport index, and regional precipitation. This suggests that a strong source, favorable transport and sufficient residence time are needed for Asian dust to have a maximum seasonal impact in the Northwest. The results contextualize case studies and demonstrate the utility of the Deep Blue algorithm.

  3. 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.

  4. Comparing momentum and mass (aerosol source function) fluxes for the North Atlantic and the European Arctic using different parameterizations

    NASA Astrophysics Data System (ADS)

    Wróbel, Iwona; Piskozub, Jacek

    2016-04-01

    Wind speed has a disproportionate role in the forming of the climate as well it is important part in calculate of the air-sea interaction thanks which we can study climate change. It influences on mass, momentum and energy fluxes and the standard way of parametrizing those fluxes is use this variable. However, the very functions used to calculate fluxes from winds have evolved over time and still have large differences (especially in the case of aerosol sources function). As we have shown last year at the EGU conference (PICO presentation EGU2015-11206-1) and in recent public article (OSD 12,C1262-C1264,2015) there is a lot of uncertainties in the case of air-sea CO2 fluxes. In this study we calculated regional and global mass and momentum fluxes based on several wind speed climatologies. To do this we use wind speed from satellite data in FluxEngine software created within OceanFlux GHG Evolution project. Our main area of interest is European Arctic because of the interesting air-sea interaction physics (six-monthly cycle, strong wind and ice cover) but because of better data coverage we have chosen the North Atlantic as a study region to make it possible to compare the calculated fluxes to measured ones. An additional reason was the importance of the area for the North Hemisphere climate, and especially for Europe. The study is related to an ESA funded OceanFlux GHG Evolution project and is meant to be part of a PhD thesis (of I.W) funded by Centre of Polar Studies "POLAR-KNOW" (a project of the Polish Ministry of Science). We have used a modified version FluxEngine, a tool created within an earlier ESA funded project (OceanFlux Greenhouse Gases) for calculating trace gas fluxes to derive two purely wind driven (at least in the simplified form used in their parameterizations) fluxes. The modifications included removing gas transfer velocity formula from the toolset and replacing it with the respective formulas for momentum transfer and mass (aerosol production

  5. Retrieval of Spectral Aerosol Optical Properties and Their Relationship to Aerosol Chemistry During ARCTAS

    NASA Astrophysics Data System (ADS)

    Corr, C. A.; Hall, S. R.; Ullmann, K.; Shetter, R.; Anderson, B. E.; Beyersdorf, A. J.; Thornhill, K. L.; Cubison, M.; Jimenez, J. L.; Dibb, J. E.

    2010-12-01

    Aerosols are known to both absorb and scatter radiation at UV wavelengths with the degree of absorption/scattering largely dependent on aerosol chemistry. The interactions of aerosols with the UV radiation field were examined during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS). Analysis focused on two case studies; one flight from the first phase of ARCTAS over Alaska and the Arctic ocean (Flight 10, April 2008) and the other from the second phase over northern Canada (Flight 17, June 2008). These flights were chosen based on availability of aircraft profiles through pollution layers and biomass burning smoke plumes with high loadings of organic aerosol during flight. Aerosol single scattering albedo (ω) was retrieved at near-UV (350-400nm) wavelengths at 1nm resolution from spectral actinic flux data collected aboard the NASA DC-8 aircraft during ARCTAS using two CCD Actinic Flux Spectroradiometers. Retrievals were performed using the Tropospheric Ultraviolet Model version 4.6 (TUV 4.6). Inputs of trace gas (e.g., NO2, SO2) concentrations, aerosol optical depth, location, time, pressure, etc. required by TUV were determined from ancillary aircraft measurements made from the DC-8. Values of ω were subsequently used to determine absorption optical depth (τabs) for each of the examined flights. Retrieval and calculation results were compared to aerosol optical properties in the visible (calculated from measurements of absorption and scattering aboard the DC-8) and the spectral dependencies characterized. Spectral ω and τabs were compared with aerosol chemistry data collected by an Aerosol Mass Spectrometer (AMS) to provide insight into the role of aerosol composition on absorption in the UV wavelength range. In particular, spectral dependencies were compared to the oxidation state of the organic aerosol (determined from AMS data) to examine the impact of aerosol processing/aging on spectral ω and τabs.

  6. 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

  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.

  8. Aerosol-Cloud Interactions in the South-East Atlantic

    NASA Astrophysics Data System (ADS)

    Andersen, Hendrik; Cermak, Jan

    2014-05-01

    thus not very credible (aerosols and cloud fraction correlate with the same meteorological parameters). The markedness of ACI is strongly dependent on the weather type. Of the examined meteorological parameters, lower tropospheric stability (LTS) seems to have the biggest impact on the statistical relationships between aerosol and cloud properties. A low LTS and the accompanied enhanced vertical transport of air masses seems to cause stronger ACI. Aerosol loading also impacts the strength of ACI, with low aerosol loadings generally associated with stronger cloud adjustments. This implies a saturation of ACI with high aerosol concentration.

  9. In situ submicron organic aerosol characterization at a boreal forest research station during HUMPPA-COPEC 2010 using soft and hard ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

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

    2013-11-01

    The chemical composition of submicron aerosol during the comprehensive field campaign HUMPPA-COPEC 2010 at Hyytiälä, Finland, is presented. The focus lies on online measurements of organic acids, which were achieved by using atmospheric pressure chemical ionization (APCI) ion trap mass spectrometry (IT-MS). These measurements were accompanied by aerosol mass spectrometry (AMS) measurements and Fourier transform infrared spectroscopy (FTIR) of filter samples, all showing a high degree of correlation. The soft ionization mass spectrometer alternated between gas-phase measurements solely and measuring the sum of gas and particle phase. The AMS measurements of C, H and O elemental composition show that the aerosol during the campaign was highly oxidized, which appears reasonable due to high and prolonged radiation during the boreal summer measurement period as well as the long transport times of some of the aerosol. In order to contrast ambient and laboratory aerosol, an average organic acid pattern, measured by APCI-IT-MS during the campaign, was compared to terpene ozonolysis products in a laboratory reaction chamber. Identification of single organic acid species remains a major challenge due to the complexity of the boreal forest aerosol. Unambiguous online species identification was attempted by the combinatorial approach of identifying unique fragments in the MS2 mode of standards, and then comparing these results with MS2 field spectra. During the campaign, unique fragments of limonene-derived organic acids (limonic acid and ketolimononic acid) and of the biomass burning tracer vanillic acid were detected. Other specific fragments (neutral loss of 28 Da) in the MS2 suggest the occurrence of semialdehydes. Furthermore, an approach to determine the average molecular weight of the aerosol is presented. The campaign average organic molecular weight was determined to be 300 g mol-1. However, a plume of aged biomass burning aerosol, arriving at Hyytiälä from Russia

  10. In-situ submicron organic aerosol characterization at a boreal forest research station during HUMPPA-COPEC 2010 using soft and hard ionization mass spectrometry

    NASA Astrophysics Data System (ADS)

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

    2013-07-01

    The chemical composition of submicron aerosol during the comprehensive field campaign HUMPPA-COPEC 2010 at Hyytiälä, Finland is presented. The focus lies on online measurements of organic acids, which was achieved by using atmospheric pressure chemical ionization (APCI) ion trap mass spectrometry (IT-MS). These measurements were accompanied by Aerosol Mass Spectrometry (AMS) measurements and Fourier-Transform Infrared Spectroscopy (FTIR) of filter samples, all showing a high degree of correlation. The soft ionization mass spectrometer alternated between gas phase measurements solely and measuring the sum of gas- and particle-phase. The AMS measurements of C, H and O elemental composition show that the aerosol during the campaign was highly oxidized, which appears reasonable due to high and prolonged radiation during the boreal summer measurement period as well as the long transport times of some of the aerosol. In order to contrast ambient and laboratory aerosol, an average organic acid pattern, measured by APCI-IT-MS during the campaign, was compared to terpene ozonolysis products in a laboratory reaction chamber. Identification of single organic acid species remains a major challenge due to the complexity of the boreal forest aerosol. Unambiguous online species identification was attempted by the combinatorial approach of identifying unique fragments in the MS2-mode of standards, and then comparing these results with MS2 field spectra. During the campaign, unique fragments of limonene derived organic acids (limonic acid and ketolimononic acid) and of the biomass burning tracer vanillic acid were detected. Other specific fragments (neutral loss of 28 Da) in the MS2 suggest the occurrence of semialdehydes. Furthermore, an approach to determine the average molecular weight of the aerosol is presented. The campaign average organic molecular weight was determined to be 300 g mol-1. However, a plume of aged biomass burning aerosol, arriving at Hyytiälä from Russia

  11. Integrated Analyses of Multiple Worldwide Aerosol Mass Spectrometer Datasets for Improved Understanding of Aerosol Sources and Processes and for Comparison with Global Models

    SciTech Connect

    Zhang, Qi; Jose, Jimenez Luis

    2014-04-28

    The AMS is the only current instrument that provides real-time, quantitative, and size-resolved data on submicron non-refractory aerosol species with a time resolution of a few minutes or better. The AMS field data are multidimensional and massive, containing extremely rich information on aerosol chemistry, microphysics and dynamics—basic information that is required to evaluate and quantify the radiative climate forcing of atmospheric aerosols. The high time resolution of the AMS data also reveals details of aerosol dynamic variations that are vital to understanding the physico-chemical processes of atmospheric aerosols that govern aerosol properties relevant to the climate. There are two primary objectives of this 3-year project. Our first objective is to perform highly integrated analysis of dozens of AMS datasets acquired from various urban, forested, coastal, marine, mountain peak, and rural/remote locations around the world and synthesize and inter-compare results with a focus on the sources and the physico-chemical processes that govern aerosol properties relevant to aerosol climate forcing. Our second objective is to support our collaboration with global aerosol modelers, in which we will supply the size-resolved aerosol composition and temporal variation data (via a public web interface) and our analysis results for use in model testing and validation and for translation of the rich AMS database into model constraints that can improve climate forcing simulations. Several prominent global aerosol modelers have expressed enthusiastic support for this collaboration. The specific tasks that we propose to accomplish include 1) to develop, validate, and apply multivariate analysis techniques for improved characterization and source apportionment of organic aerosols; 2) to evaluate aerosol source regions and relative contributions based on back-trajectory integration (PSCF method); 3) to summarize and synthesize submicron aerosol information, including

  12. 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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

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

    NASA Astrophysics Data System (ADS)

    Xu, Lingling; Chen, Jinsheng

    2016-04-01

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

  15. Mass loading in the solar wind interaction with Venus and Mars

    SciTech Connect

    Breus, T.K.; Bauer, S.J.; Krymskii, A.M.; Mitnitskii, V.Y.

    1989-03-01

    An analysis of available experimental data and theoretical concepts indicates that the interaction of the solar wind (SW) on the subsolar side with Venus, which has no intrinsic magnetic field, and with Mars, which has a small intrinsic magnetic field, is determined by the solar wind dynamic pressure with a contribution from the neutral planetary atmosphere to this interaction. The pattern of the SW interaction with these planets is different in principle for high and low dynamic pressures of the SW and is related to the varying intensity of ion formation processes (the SW Mass loading effect) in the vicinity of the SW obstacle boundary, which moves for different SW dynamic pressures into regions of different neutral atmosphere density. For moderate or high SW dynamic pressures, the subsolar Martian magnetosphere is also affected by this process. Results of numerical simulations of the SE-Mars interaction for a magnetospheric obstacle boundary at an altitude of 300 km are presented. To estimate the relative role of photoionization and charge exchange processes and their effect on the shock front position, different versions of the mass loading effect were separately calculated. copyright American Geophysical Union 1989

  16. Determination of Comet Halley gas emission characteristics from mass loading of the solar wind

    NASA Astrophysics Data System (ADS)

    Huddleston, D. E.; Johnstone, A. D.; Coates, A. J.

    1990-01-01

    The velocity profile of the solar wind during Giotto's approach to Comet Halley is fitted with the mass loading produced by a simple model of the neutral particle distribution. The model is used to calculate the implanted ion flux at Giotto for any given time and position along the spacecraft trajectory. Comparing the added flux with Giotto's solar wind proton data from the inbound leg outside the bow shock, the ratio of the total mass-loaded ion flux to the solar wind flux at the spacecraft is computed. Hence, using equations given by Galeev et al. (1985) values of the solar wind velocity, u-infinity, far upstream from the comet are inferred. Imposing the condition that u-infinity should be as nearly as possible constant in time, values of gas production rate and the ratio between radial expansion velocity and ionization rate required to fit the model to data are derived. The values obtained are consistent with those derived by more direct methods.

  17. Predicting runoff induced mass loads in urban watersheds: Linking land use and pyrethroid contamination.

    PubMed

    Chinen, Kazue; Lau, Sim-Lin; Nonezyan, Michael; McElroy, Elizabeth; Wolfe, Becky; Suffet, Irwin H; Stenstrom, Michael K

    2016-10-01

    Pyrethroid pesticide mass loadings in the Ballona Creek Watershed were calculated using the volume-concentration method with a Geographic Information Systems (GIS) to explore potential relationships between urban land use, impervious surfaces, and pyrethroid runoff flowing into an urban stream. A calibration of the GIS volume-concentration model was performed using 2013 and 2014 wet-weather sampling data. Permethrin and lambda-cyhalothrin were detected as the highest concentrations; deltamethrin, lambda-cyhalothrin, permethrin and cyfluthrin were the most frequently detected synthetic pyrethroids. Eight neighborhoods within the watershed were highlighted as target areas based on a Weighted Overlay Analysis (WOA) in GIS. Water phase concentration of synthetic pyrethroids (SPs) were calculated from the reported usage. The need for stricter BMP and consumer product controls was identified as a possible way of reducing the detections of pyrethroids in Ballona Creek. This model has significant implications for determining mass loadings due to land use influence, and offers a flexible method to extrapolate data for a limited amount of samplings for a larger watershed, particularly for chemicals that are not subject to environmental monitoring. Offered as a simple approach to watershed management, the GIS-volume concentration model has the potential to be applied to other target pesticides and is useful for simulating different watershed scenarios. Further research is needed to compare results against other similar urban watersheds situated in mediterranean climates. PMID:27475081

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

    SciTech Connect

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

    2014-11-27

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

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

    DOE PAGES

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

    2014-11-27

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

  20. Characterization of Organic Nitrate Formation in Limonene Secondary Organic Aerosol using High-Resolution Chemical Ionization Mass Spectrometry

    NASA Astrophysics Data System (ADS)

    Faxon, Cameron; Hammes, Julia; Peng, Jianfei; Hallquist, Mattias; Pathak, Ravi

    2016-04-01

    Previous work has shown that organic nitrates (RONO2) are prevalent in the boundary layer, and can contribute significantly to secondary organic aerosol formation. Monoterpenes, including limonene, have been shown to be precursors for the formation of these organic nitrates. Limonene has two double bonds, either of which may be oxidized by NO3 or O3. This leads to the generation of products that can subsequently condense or partition into the particle phase, producing secondary organic aerosol. In order to further elucidate the particle and gas phase product distribution of organic nitrates forming from the reactions of limonene and the nitrate radical (NO3), a series of experiments were performed in the Gothenburg Flow Reactor for Oxidation Studies at Low Temperatures (G-FROST), described by previous work. N2O5 was used as the source for NO3 and NO2, and a characterized diffusion source was used to introduce limonene into the flow reactor. All experiments were conducted in the absence of light, and the concentration of limonene was increased step-wise throughout each experiment to modify the ratio of N2O5to limonene. The experiments were conducted such that both limonene- and N2O5-limited regimes were present. Gas and particle phase products were measured using an iodide High-Resolution Time-of-Flight Mass Spectrometer (HR-ToF-CIMS) coupled to a Filter Inlet for Gases and AEROsols (FIGAERO, and particle size and SOA mass concentrations were derived using a Scanning Mobility Particle Sizer (SMPS). CIMS measurement techniques have previously been employed for the measurement of organic nitrate products of such compounds using multiple reagent ions. The use of this instrumentation allowed for the identification of chemical formulas for gas and particle phase species. The findings from the experiments will be presented in terms of the relative gas-particle partitioning of major products and the effects of N2O5/limonene ratios on product distributions. Additionally, a

  1. Thermal Extraction–Two-Dimensional Gas Chromatography–Mass Spectrometry with Heart-Cutting for Nitrogen Heterocyclics in Biomass Burning Aerosols

    EPA Science Inventory

    A thermal extraction-two-dimensional gas chromatography-mass spectrometry (TE-GC-MS) method (with heart-cutting) is developed for quantitatively assessing nitrogen (N-bearing organic species (e.g., pyrrole, pyridine, nitriles, and amines) in aerosols emitted from agricultural fir...

  2. THERMAL DESORPTION MASS SPECTROMETRIC ANALYSIS OF ORGANIC AEROSOL FORMED FROM REACTIONS OF 1-TETRADECENE AND O3 IN THE PRESENCE OF ALCOHOLS AND CARBOXYLIC ACIDS. (R826235)

    EPA Science Inventory

    The chemistry of secondary organic aerosol formation from reactions of
    1-tetradecene and O3 in dry air in the presence of excess alcohols
    and carboxylic acids was investigated in an environmental chamber using a
    thermal desorption particle beam mass spec...

  3. ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS

    EPA Science Inventory

    ANALYSIS OF RESPIRATORY DEPOSITION OF INHALED PARTICLES FOR DIFFERENT DOSE METRICS: COMPARISON OF NUMBER, SURFACE AREA AND MASS DOSE OF TYPICAL AMBIENT BI-MODAL AEROSOLS.
    Chong S. Kim, SC. Hu*, PA Jaques*, US EPA, National Health and Environmental Effects Research Laboratory, ...

  4. A Comparative Study of Mass Removal Loads for a Range of Stormwater Treatment Strategies

    NASA Astrophysics Data System (ADS)

    Avellaneda, P. M.; Houle, J. J.; Roseen, R. M.; Ballestero, T. P.

    2005-05-01

    When evaluating performance efficiencies for stormwater BMPs, there are significant challenges with regards to normalizing the variations in design, and hydraulic and hydrological conditions. There can be significant variations that must be considered such as rainfall intensity and duration, influent quality, watershed characteristics, loading functions, antecedent dry period, and maintenance. This study assessed mass removal loads for different stormwater management measures, all located in the same facility. The research facility is unique because it enables monitoring of 12 different treatment devices in parallel. For this purpose, a 9-acre commuter parking lot at the University of New Hampshire was chosen to provide runoff. There are three classes of devices examined at the site, conventional structural Best Management Practices (BMP), Low Impact Development (LID) designs, and manufactured devices. These include a subsurface gravel wetland, a detention pond, a sand filter, a bioretention system, a vegetated swale, and 7 different manufactured devices. Flow was evenly distributed and piped to each stormwater treatment. An on-site rain gauge provided rainfall data and samples of stormwater influent and effluent (for each stormwater treatment) were collected during monitoring rainfall events between August (2004) and April (2005). Temperature, dissolved oxygen and conductivity were measured continuously. Runoff constituents such as TSS, TP, TN, Cu, metals, nutrients and bacteria were measured in temporal water samples for each monitoring rainfall event. Results are presented as both concentration and Event Mean Concentrations (EMCs) to evaluate mass load removal. The watershed rainfall-runoff pattern was investigated as well as a statistical analysis to determine whether or not the differences between inflow and effluent water quality parameters were statistically significant. Earlier results have shown significant differences in the effluent water quality

  5. Applications of High-Resolution Electrospray Ionization Mass Spectrometry to Measurements of Average Oxygen to Carbon Ratios in Secondary Organic Aerosols

    SciTech Connect

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

    2012-07-02

    The applicability of high resolution electrospray ionization mass spectrometry (HR ESI-MS) to measurements of the average oxygen to carbon ratio (O/C) in organic aerosols was investigated. Solutions with known average O/C containing up to 10 standard compounds representative of secondary organic aerosol (SOA) were analyzed and corresponding electrospray ionization efficiencies were quantified. The assumption of equal ionization efficiency commonly used in estimating O/C ratios of organic aerosols was found to be reasonably accurate. We found that the accuracy of the measured O/C ratios increases by averaging the values obtained from both (+) and (-) modes. A correlation was found between the ratio of the ionization efficiencies in the positive and negative ESI modes with the octanol-water partition constant, and more importantly, with the compound's O/C. To demonstrate the utility of this correlation for estimating average O/C values of unknown mixtures, we analyzed the ESI (+) and ESI (-) data for SOA produced by oxidation of limonene and isoprene and compared to online O/C measurements using an aerosol mass spectrometer (AMS). This work demonstrates that the accuracy of the HR ESI-MS methods is comparable to that of the AMS, with the added benefit of molecular identification of the aerosol constituents.

  6. Mass-mobility characterization of flame-made ZrO2 aerosols: primary particle diameter and extent of aggregation.

    PubMed

    Eggersdorfer, M L; Gröhn, A J; Sorensen, C M; McMurry, P H; Pratsinis, S E

    2012-12-01

    Gas-borne nanoparticles undergoing coagulation and sintering form irregular or fractal-like structures affecting their transport, light scattering, effective surface area, and density. Here, zirconia (ZrO(2)) nanoparticles are generated by scalable spray combustion, and their mobility diameter and mass are obtained nearly in situ by differential mobility analyzer (DMA) and aerosol particle mass (APM) measurements. Using these data, the density of ZrO(2) and a power law between mobility and primary particle diameters, the structure of fractal-like particles is determined (mass-mobility exponent, prefactor and average number, and surface area mean diameter of primary particles, d(va)). The d(va) determined by DMA-APM measurements and this power law is in good agreement with the d(va) obtained by ex situ nitrogen adsorption and microscopic analysis. Using this combination of measurements and above power law, the effect of flame spray process parameters (e.g., precursor solution and oxygen flow rate as well as zirconium concentration) on fractal-like particle structure characteristics is investigated in detail. This reveals that predominantly agglomerates (physically-bonded particles) and aggregates (chemically- or sinter-bonded particles) of nanoparticles are formed at low and high particle concentrations, respectively. PMID:22959835

  7. Mass-Mobility Characterization of Flame-made ZrO2 Aerosols: Primary Particle Diameter & Extent of Aggregation

    PubMed Central

    Eggersdorfer, M.L.; Gröhn, A.J.; Sorensen, C.M.; McMurry, P.H.; Pratsinis, S.E.

    2013-01-01

    Gas-borne nanoparticles undergoing coagulation and sintering form irregular or fractal-like structures affecting their transport, light scattering, effective surface area and density. Here, zirconia (ZrO2) nanoparticles are generated by scalable spray combustion, and their mobility diameter and mass are obtained nearly in-situ by differential mobility analyzer (DMA) and aerosol particle mass (APM) measurements. Using these data, the density of ZrO2 and a power law between mobility and primary particle diameters, the structure of fractal-like particles is determined (mass-mobility exponent, prefactor and average number and surface area mean diameter of primary particles, dva). The dva determined by DMA-APM measurements and this power law is in good agreement with the dva obtained by ex-situ nitrogen adsorption and microscopic analysis. Using this combination of measurements and above power law, the effect of flame spray process parameters (e.g. precursor solution and oxygen flow rate as well as zirconium concentration) on fractal-like particle structure characteristics is investigated in detail. This reveals that predominantly agglomerates (physically-bonded particles) and aggregates (chemically- or sinter-bonded particles) of nanoparticles are formed at low and high particle concentrations, respectively. PMID:22959835

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

    PubMed

    Klems, Joseph P; Johnston, Murray V

    2013-09-01

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

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

    SciTech Connect

    Martin, Audrey Noreen

    2006-01-01

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

  10. Simultaneous analysis of heparosan oligosaccharides by isocratic liquid chromatography with charged aerosol detection/mass spectrometry.

    PubMed

    Ji, Xiaohu; Hu, Guixin; Zhang, Qiongyan; Wang, Fengshan; Liu, Chunhui

    2016-11-01

    Uncovering the biological roles of heparosan oligosaccharides requires a simple and robust method for their separation and identification. We reported on systematic investigations of the retention behaviors of synthetic heparosan oligosaccharides on porous graphitic carbon (PGC) column by HPLC with charged aerosol detection. Oligosaccharides were strongly retained by PGC material in water-acetonitrile mobile phase, and eluted by trifluoroacetic acid occurring as narrow peaks. Addition of small fraction of methanol led to better selectivity of PGC to oligosaccharides than acetonitrile modifier alone, presumably, resulting from displacement of methanol to give different chemical environment at the PGC surface. Van't-Hoff plots demonstrated that retention behaviors highly depended on the column temperature and oligosaccharide moieties. By implementing the optimal MeOH content and temperature, a novel isocratic elution method was successfully developed for baseline resolution and identification of seven heparosan oligosaccharides using PGC-HPLC-CAD/MS. This approach allows for rapid analysis of heparosan oligosaccharides from various sources. PMID:27516280

  11. The Regional Environmental Impacts of Atmospheric Aerosols over Egypt

    NASA Astrophysics Data System (ADS)

    Zakey, Ashraf; Ibrahim, Alaa

    2015-04-01

    Identifying the origin (natural versus anthropogenic) and the dynamics of aerosols over Egypt at varying temporal and spatial scales provide valuable knowledge on the regional climate impacts of aerosols and their ultimate connections to the Earth's regional climate system at the MENA region. At regional scale, Egypt is exposed to air pollution with levels exceeding typical air-quality standards. This is particularly true for the Nile Delta region, being at the crossroads of different aerosol species originating from local urban-industrial and biomass-burning activities, regional dust sources, and European pollution from the north. The Environmental Climate Model (EnvClimA) is used to investigate both of the biogenic and anthropogenic aerosols over Egypt. The dominant natural aerosols over Egypt are due to the sand and dust storms, which frequently occur during the transitional seasons (spring and autumn). In winter, the maximum frequency reaches 2 to 3 per day in the north, which decreases gradually southward with a frequency of 0.5-1 per day. Monitoring one of the most basic aerosol parameters, the aerosol optical depth (AOD), is a main experimental and modeling task in aerosol studies. We used the aerosol optical depth to quantify the amount and variability of aerosol loading in the atmospheric column over a certain areas. The aerosols optical depth from the model is higher in spring season due to the impacts of dust activity over Egypt as results of the westerly wind, which carries more dust particles from the Libyan Desert. The model result shows that the mass load of fine aerosols has a longer life-time than the coarse aerosols. In autumn season, the modelled aerosol optical depth tends to increase due to the biomass burning in the delta of Egypt. Natural aerosol from the model tends to scatter the solar radiation while most of the anthropogenic aerosols tend to absorb the longwave solar radiation. The overall results indicate that the AOD is lowest in winter

  12. 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

  13. High-Resolution Mass Spectrometry and Molecular Characterization of Aqueous Photochemistry Products of Common Types of Secondary Organic Aerosols

    SciTech Connect

    Romonosky, Dian E.; Laskin, Alexander; Laskin, Julia; Nizkorodov, Sergey

    2015-03-19

    A significant fraction of atmospheric organic compounds is predominantly found in condensed phases, such as aerosol particles and cloud droplets. Many of these compounds are photolabile and can degrade through direct photolysis or indirect photooxidation processes on time scales that are comparable to the typical lifetimes of aqueous droplets (hours) and particles (days). This paper presents a systematic investigation of the molecular level composition and the extent of aqueous photochemical processing in different types of secondary organic aerosol (SOA) from biogenic and anthropogenic precursors including α-pinene, β-pinene, β-myrcene, d- limonene, α-humulene, 1,3,5-trimethylbenzene, and guaiacol, oxidized by ozone (to simulate a remote atmosphere) or by OH in the presence of NOx (to simulate an urban atmosphere). Chamber- and flow tube-generated SOA samples were collected, extracted in a methanol/water solution, and photolyzed for 1 h under identical irradiation conditions. In these experiments, the irradiation was equivalent to about 3-8 h of exposure to the sun in its zenith. The molecular level composition of the dissolved SOA was probed before and after photolysis with direct-infusion electrospray ionization high-resolution mass spectrometry (ESI-HR-MS). The mass spectra of unphotolyzed SOA generated by ozone oxidation of monoterpenes showed qualitatively similar features, and contained largely overlapping subsets of identified compounds. The mass spectra of OH/NOx generated SOA had more unique visual appearance, and indicated a lower extent of products overlap. Furthermore, the fraction of nitrogen containing species (organonitrates and nitroaromatics) was highly sensitive to the SOA precursor. These observations suggest that attribution of high-resolution mass spectra in field SOA samples to specific SOA precursors should be more straightforward under OH/NOx oxidation conditions compared to the ozone driven oxidation. Comparison of the SOA constituents

  14. Saharan dust aerosol over the central Mediterranean Sea: optical columnar measurements vs. aerosol load, chemical composition and marker solubility at ground level

    NASA Astrophysics Data System (ADS)

    Marconi, M.; Sferlazzo, D. M.; Becagli, S.; Bommarito, C.; Calzolai, G.; Chiari, M.; di Sarra, A.; Ghedini, C.; Gómez-Amo, J. L.; Lucarelli, F.; Meloni, D.; Monteleone, F.; Nava, S.; Pace, G.; Piacentino, S.; Rugi, F.; Severi, M.; Traversi, R.; Udisti, R.

    2013-08-01

    This study aims at the determination of the mineral contribution to PM10 in the central Mediterranean Sea on the basis of 7 yr of PM10 chemical composition daily measurements made on the island of Lampedusa (35.5° N, 12.6° E). Aerosol optical depth measurements are carried out in parallel while sampling with a multi-stage impactor, and observations with an optical particle counter were performed in selected periods. Based on daily samples, the total content and soluble fraction of selected metals are used to identify and characterize the dust events. The total contribution is determined by PIXE (particle-induced X-ray emission) while the composition of the soluble fraction by ICP-AES (inductively coupled plasma atomic emission spectroscopy) after extraction with HNO3 at pH 1.5. The average PM10 concentration at Lampedusa calculated over the period June 2004-December 2010 is 31.5 μg m-3, with low interannual variability. The annual means are below the EU annual standard for PM10, but 9.9% of the total number of daily data exceed the daily threshold value established by the European Commission for PM (50 μg m-3, European Community, EC/30/1999). The Saharan dust contribution to PM10 was derived by calculating the contribution of Al, Si, Fe, Ti, non-sea-salt (nss) Ca, nssNa, and nssK oxides in samples in which PIXE data were available. Cases with crustal content exceeding the 75th percentile of the crustal oxide content distribution were identified as dust events. Using this threshold we identify 175 events; 31.6% of them (55 events) present PM10 higher than 50 μg m-3, with dust contributing by 33% on average. The annual average crustal contribution to PM10 is 5.42 μg m-3, reaching a value as high as 67.9 μg m-3, 49% of PM10, during an intense Saharan dust event. The crustal aerosol amount and contribution to PM10 shows a very small seasonal dependence; conversely, the dust columnar burden displays an evident annual cycle, with a strong summer maximum (monthly

  15. 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