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5. Case study evaluation of size-resolved molecular composition and phase state of carbonaceous particles in wildfire influenced smoke from the Pacific Northwest

Author

Vandergrift, Gregory W., primary, Lata, Nurun Nahar, additional, Mathai, Susan, additional, Ijaz, Amna, additional, Cheng, Zezhen, additional, Shrivastava, Manish, additional, Zhang, Jie, additional, Md Shawon, Abu Sayeed, additional, Kulkarni, Gourihar, additional, Mazzoleni, Lynn R., additional, Kew, William, additional, and China, Swarup, additional

Published
2023
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10. Analytical determination of the Aerosol organic mass-to-organic carbon ratio

Author

Ei-Zanan, Hazem S., Zielinska, Barbara, Mazzoleni, Lynn R., and Hansen, D. Alan

Subjects
Extraction (Chemistry) -- Methods -- Environmental aspects, Organic compounds -- Composition -- Environmental aspects -- Methods, Air quality management -- Methods -- Environmental aspects, Particles -- Composition -- Environmental aspects -- Methods, Environmental services industry, Environmental issues, Science and technology
Abstract

ABSTRACT Particulate matter (PM) with an aerodynamic diameter ≤ 2.5 µm ([PM.sub.2.5]) was collected daily (mid-July 1998 to the end of December 1999) over a 24-hr sampling period in a [...]

Published
2009

11. An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry : Are we getting the same answer?

Author

Hawkes, Jeffrey A., D'Andrilli, Juliana, Agar, Jeffrey N., Barrow, Mark P., Berg, Stephanie M., Catalan, Nuria, Chen, Hongmei, Chu, Rosalie K., Cole, Richard B., Dittmar, Thorsten, Gavard, Remy, Gleixner, Gerd, Hatcher, Patrick G., He, Chen, Hess, Nancy J., Hutchins, Ryan H. S., Ijaz, Amna, Jones, Hugh E., Kew, William, Khaksari, Maryam, Lozano, Diana Catalina Palacio, Lv, Jitao, Mazzoleni, Lynn R., Noriega-Ortega, Beatriz E., Osterholz, Helena, Radoman, Nikola, Remucal, Christina K., Schmitt, Nicholas D., Schum, Simeon K., Shi, Quan, Simon, Carsten, Singer, Gabriel, Sleighter, Rachel L., Stubbins, Aron, Thomas, Mary J., Tolic, Nikola, Zhang, Shuzhen, Zito, Phoebe, Podgorski, David C., Hawkes, Jeffrey A., D'Andrilli, Juliana, Agar, Jeffrey N., Barrow, Mark P., Berg, Stephanie M., Catalan, Nuria, Chen, Hongmei, Chu, Rosalie K., Cole, Richard B., Dittmar, Thorsten, Gavard, Remy, Gleixner, Gerd, Hatcher, Patrick G., He, Chen, Hess, Nancy J., Hutchins, Ryan H. S., Ijaz, Amna, Jones, Hugh E., Kew, William, Khaksari, Maryam, Lozano, Diana Catalina Palacio, Lv, Jitao, Mazzoleni, Lynn R., Noriega-Ortega, Beatriz E., Osterholz, Helena, Radoman, Nikola, Remucal, Christina K., Schmitt, Nicholas D., Schum, Simeon K., Shi, Quan, Simon, Carsten, Singer, Gabriel, Sleighter, Rachel L., Stubbins, Aron, Thomas, Mary J., Tolic, Nikola, Zhang, Shuzhen, Zito, Phoebe, and Podgorski, David C.

Abstract

High-resolution mass spectrometry (HRMS) has become a vital tool for dissolved organic matter (DOM) characterization. The upward trend in HRMS analysis of DOM presents challenges in data comparison and interpretation among laboratories operating instruments with differing performance and user operating conditions. It is therefore essential that the community establishes metric ranges and compositional trends for data comparison with reference samples so that data can be robustly compared among research groups. To this end, four identically prepared DOM samples were each measured by 16 laboratories, using 17 commercially purchased instruments, using positive-ion and negative-ion mode electrospray ionization (ESI) HRMS analyses. The instruments identified similar to 1000 common ions in both negative- and positive-ion modes over a wide range of m/z values and chemical space, as determined by van Krevelen diagrams. Calculated metrics of abundance-weighted average indices (H/C, O/C, aromaticity and m/z) of the commonly detected ions showed that hydrogen saturation and aromaticity were consistent for each reference sample across the instruments, while average mass and oxygenation were more affected by differences in instrument type and settings. In this paper we present 32 metric values for future benchmarking. The metric values were obtained for the four different parameters from four samples in two ionization modes and can be used in future work to evaluate the performance of HRMS instruments.

Published
2020
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14. An international laboratory comparison of dissolved organic matter composition by high resolution mass spectrometry: Are we getting the same answer?

Author

Hawkes, Jeffrey A., primary, D'Andrilli, Juliana, additional, Agar, Jeffrey N., additional, Barrow, Mark P., additional, Berg, Stephanie M., additional, Catalán, Núria, additional, Chen, Hongmei, additional, Chu, Rosalie K., additional, Cole, Richard B., additional, Dittmar, Thorsten, additional, Gavard, Rémy, additional, Gleixner, Gerd, additional, Hatcher, Patrick G., additional, He, Chen, additional, Hess, Nancy J., additional, Hutchins, Ryan H. S., additional, Ijaz, Amna, additional, Jones, Hugh E., additional, Kew, William, additional, Khaksari, Maryam, additional, Palacio Lozano, Diana Catalina, additional, Lv, Jitao, additional, Mazzoleni, Lynn R, additional, Noriega‐Ortega, Beatriz E., additional, Osterholz, Helena, additional, Radoman, Nikola, additional, Remucal, Christina K., additional, Schmitt, Nicholas D., additional, Schum, Simeon K, additional, Shi, Quan, additional, Simon, Carsten, additional, Singer, Gabriel, additional, Sleighter, Rachel L., additional, Stubbins, Aron, additional, Thomas, Mary J., additional, Tolic, Nikola, additional, Zhang, Shuzhen, additional, Zito, Phoebe, additional, and Podgorski, David C., additional

Published
2020
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15. Extensive Soot Compaction by Cloud Processing from Laboratory and Field Observations

Author

Bhandari, Janarjan, primary, China, Swarup, additional, Chandrakar, Kamal Kant, additional, Kinney, Greg, additional, Cantrell, Will, additional, Shaw, Raymond A., additional, Mazzoleni, Lynn R., additional, Girotto, Giulia, additional, Sharma, Noopur, additional, Gorkowski, Kyle, additional, Gilardoni, Stefania, additional, Decesari, Stefano, additional, Facchini, Maria Cristina, additional, Zanca, Nicola, additional, Pavese, Giulia, additional, Esposito, Francesco, additional, Dubey, Manvendra K., additional, Aiken, Allison C., additional, Chakrabarty, Rajan K., additional, Moosmüller, Hans, additional, Onasch, Timothy B., additional, Zaveri, Rahul A., additional, Scarnato, Barbara V., additional, Fialho, Paulo, additional, and Mazzoleni, Claudio, additional

Published
2019
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26. Tropospheric Ozone Assessment Report: Database and metrics data of global surface ozone observations

Author

Schultz, Martin G., primary, Schröder, Sabine, additional, Lyapina, Olga, additional, Cooper, Owen R., additional, Galbally, Ian, additional, Petropavlovskikh, Irina, additional, von Schneidemesser, Erika, additional, Tanimoto, Hiroshi, additional, Elshorbany, Yasin, additional, Naja, Manish, additional, Seguel, Rodrigo J., additional, Dauert, Ute, additional, Eckhardt, Paul, additional, Feigenspan, Stefan, additional, Fiebig, Markus, additional, Hjellbrekke, Anne-Gunn, additional, Hong, You-Deog, additional, Kjeld, Peter Christian, additional, Koide, Hiroshi, additional, Lear, Gary, additional, Tarasick, David, additional, Ueno, Mikio, additional, Wallasch, Markus, additional, Baumgardner, Darrel, additional, Chuang, Ming-Tung, additional, Gillett, Robert, additional, Lee, Meehye, additional, Molloy, Suzie, additional, Moolla, Raeesa, additional, Wang, Tao, additional, Sharps, Katrina, additional, Adame, Jose A., additional, Ancellet, Gerard, additional, Apadula, Francesco, additional, Artaxo, Paulo, additional, Barlasina, Maria E., additional, Bogucka, Magdalena, additional, Bonasoni, Paolo, additional, Chang, Limseok, additional, Colomb, Aurelie, additional, Cuevas-Agulló, Emilio, additional, Cupeiro, Manuel, additional, Degorska, Anna, additional, Ding, Aijun, additional, Fröhlich, Marina, additional, Frolova, Marina, additional, Gadhavi, Harish, additional, Gheusi, Francois, additional, Gilge, Stefan, additional, Gonzalez, Margarita Y., additional, Gros, Valerie, additional, Hamad, Samera H., additional, Helmig, Detlev, additional, Henriques, Diamantino, additional, Hermansen, Ove, additional, Holla, Robert, additional, Hueber, Jacques, additional, Im, Ulas, additional, Jaffe, Daniel A., additional, Komala, Ninong, additional, Kubistin, Dagmar, additional, Lam, Ka-Se, additional, Laurila, Tuomas, additional, Lee, Haeyoung, additional, Levy, Ilan, additional, Mazzoleni, Claudio, additional, Mazzoleni, Lynn R., additional, McClure-Begley, Audra, additional, Mohamad, Maznorizan, additional, Murovec, Marijana, additional, Navarro-Comas, Monica, additional, Nicodim, Florin, additional, Parrish, David, additional, Read, Katie A., additional, Reid, Nick, additional, Ries, Ludwig, additional, Saxena, Pallavi, additional, Schwab, James J., additional, Scorgie, Yvonne, additional, Senik, Irina, additional, Simmonds, Peter, additional, Sinha, Vinayak, additional, Skorokhod, Andrey I., additional, Spain, Gerard, additional, Spangl, Wolfgang, additional, Spoor, Ronald, additional, Springston, Stephen R., additional, Steer, Kelvyn, additional, Steinbacher, Martin, additional, Suharguniyawan, Eka, additional, Torre, Paul, additional, Trickl, Thomas, additional, Weili, Lin, additional, Weller, Rolf, additional, Xiaobin, Xu, additional, Xue, Likun, additional, and Zhiqiang, Ma, additional

Published
2017
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27. Supplementary material to "Hygroscopic growth of water soluble organic carbon isolated from atmospheric aerosol collected at U.S. national parks and Storm Peak Laboratory"

Author

Taylor, Nathan F., primary, Collins, Don R., additional, Lowenthal, Douglas H., additional, Zielinska, Barbara, additional, Samburova, Vera, additional, Kumar, Naresh, additional, Hallar, A. Gannet, additional, Mazzoleni, Lynn R., additional, and McCubbin, Ian B., additional

Published
2016
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29. Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties

Author

Naval Postgraduate School (U.S.), Meteorology, China, Swarup, Scarnato, Barbara, Owen, Robert C., Zhang, Bo, Ampadu, Marian T., Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Fialho, Paulo, Perlinger, Judith A., Hueber, Jacques, Helmig, Detlev, Mazzoleni, Lynn R., Mazzoleni, Claudio, Naval Postgraduate School (U.S.), Meteorology, China, Swarup, Scarnato, Barbara, Owen, Robert C., Zhang, Bo, Ampadu, Marian T., Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Fialho, Paulo, Perlinger, Judith A., Hueber, Jacques, Helmig, Detlev, Mazzoleni, Lynn R., and Mazzoleni, Claudio

Abstract

The radiative properties of soot particles depend on their morphology and mixing state, but their evolution during transport is still elusive. Here we report observations from an electron microscopy analysis of individual particles transported in the free troposphere over long distances to the remote Pico Mountain Observatory in the Azores in the North Atlantic. Approximately 70% of the soot particles were highly compact and of those 26% were thinly coated. Discrete dipole approximation simulations indicate that this compaction results in an increase in soot single scattering albedo by a factor of ≤2.17. The top of the atmosphere direct radiative forcing is typically smaller for highly compact than mass-equivalent lacy soot. The forcing estimated using Mie theory is within 12% of the forcing estimated using the discrete dipole approximation for a high surface albedo, implying that Mie calculations may provide a reasonable approximation for compact soot above remote marine clouds.

Published
2015

30. Measurement of Aerosols and Trace Gases in the Free Troposphere at the Pico Mountain Observatory in the Azores

Author

Kramer, Louisa, Mazzoleni, Claudio, Mazzoleni, Lynn R., Fialho, Paulo, Helmig, Detlev, Olsen, Seth C., Owen, R. Chris, Dziobak, Michael P., Hueber, Jacques, Dzepina, Katja, and Kumar, Sumit

Subjects
Aerossol Atmosférico, Atmospheric Aerosol, Tropospheric Aerosol, Black Carbon, Azores, Pico Island (Azores)
Abstract

European Geosciences Union (EGU), General Assembly. Viena, Austria, 07 - 12 April 2013. Here, we present an overview of gas and aerosol data measured at the Pico Mountain Station. The primary objective of these measurements are to enhance our knowledge of anthropogenic and biomass burning emissions from North America and their relative impact on atmospheric composition and radiative forcing in the free troposphere of the North Atlantic.

Published
2013

31. Climatology and Atmospheric Chemistry of Non-Methane Hydrocarbon Emissions over the North Atlantic

Author

Muñoz, Mauricio, Helmig, Detlev, Hueber, Jacques, Mazzoleni, Claudio, Mazzoleni, Lynn R., Owen, Robert, Val Martin, Maria, Fialho, Paulo, and Plass-Duelmer, Christian

Subjects
Climatology, Atmospheric Chemistry, Azores, Pico Island (Azores)
Abstract

European Geosciences Union (EGU), General Assembly. Viena, Austria, 07 - 12 April 2013. Non-methane hydrocarbons (NMHC) covering the C2 to C7 volatility range have been monitored at the Pico Mountain Observatory, Pico Island, Azores, Portugal, since 2004. The Observatory is located at 2225 m a.s.l. in the caldera of the Pico Mountain volcano, and during most times receives lower free tropospheric air that has been transported across the North Atlantic. The 7-year NMHC record has been analyzed for seasonal behavior of photochemical processing, atmospheric transport time, and source region using ratios of NMHC species as indicators of photochemical aging and HYSPLIT model outputs. Transport conditions resulting in elevated and low NMHC conditions were specifically studied to investigate seasonal pollution transport in the North Atlantic region.

Published
2013

32. Properties of Aerosol in the North Atlantic Free Troposphere at the Pico Mountain Observatory, Azores

Author

Mazzoleni, Claudio, Mazzoleni, Lynn R., Fialho, Paulo, Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Kramer, Louisa, Olsen, Seth C., Owen, Robert, Helmig, Detlev, Hueber, Jacques, Wrigth, Kendra, Zhang, Bo, and China, Swarup

Subjects
Aerossol Atmosférico, Atmospheric Aerosol, Black Carbon, Azores, Pico Island (Azores)
Abstract

4th Atmospheric System Research (ASR), Science Team Meeting. Potomac, Maryland, March 18-21, 2013. The Pico Mountain Observatory is located at an altitude of 2225 meters above sea level in the summit caldera of the Pico volcano in the Azores, Portugal (38.47°N, 28.40°W). The scientific value of the station stems from the fact that this is the only permanent free-tropospheric monitoring station in the central North Atlantic, with negligible influence from local sources and that frequently samples air from the North American continent. Thus, it is an ideal site for studying long-range transported pollution. The station started operating in 2001 with a focus on gaseous species (e.g., ozone, carbon monoxide, nitrogen oxides, and non-methane hydrocarbons) and aerosol particles that absorb light (black carbon [BC] and aerosol dust). The absorbing aerosol mass concentrations, in units of equivalent black carbon mass concentrations, have been monitored using a seven-wavelength aethalometer (Magee scientific model AE31). Ancillary measurements at the station include meteorological parameters such as temperature, relative humidity, pressure, wind direction, and speed. Due to the harsh environmental conditions at the site, most measurements have been performed during the summer seasons. In the summer of 2012, new aerosol instrumentation and samplers were installed at the station. The new equipment includes a three-wavelength nephelometer (Ecotech model Aurora 3000) that measure aerosol scattering and backscattering fraction, a set of four high-volume samplers for the collection and chemical analysis of aerosol, a sequential sampler to collect aerosols on membranes and grids, and an optical particle counter. Membranes and grids are analysed offline with scanning and transmission electron microscopy to study morphological properties and elemental composition of the aged aerosols. In this poster we will discuss some of the analysis of the decadal BC mass concentration data, as well as some analysis of the new aerosol data with a focus on aerosol optical properties and morphology. Analysis of these properties is important for a better understanding of aerosol’s life cycle and ageing during their transport over the Atlantic, with implications on aerosol radiative properties and climate science.

Published
2013

33. Molecular and physical characteristics of aerosol at a remote marine free troposphere site: Implications for atmospheric aging.

Author

Schum, Simeon K., Bo Zhang, Dzepina, Katja, Fialho, Paulo, Mazzoleni, Claudio, and Mazzoleni, Lynn R.

Abstract

Aerosol properties are transformed by atmospheric processes during long-range transport and play a key role in the Earth's radiative balance. To understand the molecular and physical characteristics of free tropospheric aerosol, we studied samples collected at the Pico Mountain Observatory in the North Atlantic. The observatory is located in the marine free troposphere at 2225 m above sea level, on Pico Island in the Azores archipelago. The site is ideal for the study of long-range transported free tropospheric aerosol with minimal local influence. Three aerosol samples with elevated organic carbon concentrations were selected for detailed analysis. FLEXPART retroplumes indicated that two of the samples were influenced by North American wildfire emissions transported in the free troposphere and one by North American outflow mainly transported within the marine boundary layer. To determine the molecular composition of the samples, we used ultrahigh resolution Fourier transform ion cyclotron resonance mass spectrometry. Thousands of molecular formulas were assigned to each of the individual samples. On average ~ 60 % of the molecular formulas contained only carbon, hydrogen, and oxygen atoms (CHO), ~ 30 % contained nitrogen (CHNO), and ~ 10 % contained sulfur (CHOS). The molecular formula composition of the two wildfire influenced aerosol samples transported mainly in the free troposphere had relatively low average O/C ratios (0.46 ± 0.12 and 0.47 ± 0.15) despite 7–10 days of transport time according to FLEXPART. However, the molecular composition of the North American outflow transported mainly in the boundary layer had a higher average O/C ratio (0.55 ± 0.19) with 3 days of transport time. Thus, aerosol oxidation appears to be related to environmental factors during transport and not simply aging time. Meteorological conditions extracted from GFS analysis for model grids along the FLEXPART simulated transport pathways and the observed molecular chemistry were used to predict the phase state of the aerosol samples, indicating that the aerosol transported in the free troposphere was more likely to be solid and therefore less oxidized than the aerosol transported in the boundary layer. This suggests that biomass burning emissions injected into the free troposphere are longer-lived than emissions in the boundary layer. [ABSTRACT FROM AUTHOR]

Published
2018
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34. Ten Years of Black Carbon Measurements in the North Atlantic at the Pico Mountain Observatory, Azores (2225m asl)

Author

Kumar, Sumit, Fialho, Paulo, Mazzoleni, Lynn R., Olsen, Seth C., Owen, R. Chris, Helmig, Detlev, Hueber, Jacques, Dziobak, Michael P., Kramer, Louisa, and Mazzoleni, Claudio

Subjects
Aerossol Atmosférico, Tropospheric Aerosol, Black Carbon, Azores, Pico Island (Azores)
Abstract

45th annual Fall Meeting, AGU. San Francisco, California, 3-7 December. The Pico Mountain Observatory is located in the summit caldera of the Pico mountain, an inactive volcano on the Pico Island in the Azores, Portugal (38.47°N, 28.40°W, Altitude 2225m asl). The Azores are often impacted by polluted outflows from the North American continent and local sources have been shown to have a negligible influence at the observatory. The value of the station stems from the fact that this is the only permanent mountaintop monitoring station in the North Atlantic that is typically located above the marine boundary layer (average MBL heights are below 1200 m and rarely exceed 1300 m) and often receives air characteristic of the lower free troposphere. Measurements of black carbon (BC) mass have been carried out at the station since 2001, mostly in the summer seasons. Here we discuss the BC decadal dataset (2001-2011) collected at the site by using a seven-wavelength AE31 Magee Aethalometer. Measured BC mass and computed Angstrom exponent (AE) values were analysed to study seasonal and diurnal variations. There was a large day-to-day variability in the BC values due to varied meteorological conditions that resulted in different diurnal patterns for different months. The daily mean BC at this location ranged between 0 and ~430 ngm-3, with the most frequently occurring value in the range 0-100 ngm-3. The overall mean for the 10 year period is ~24 ngm-3, with a coefficient of variation of 150%. The BC values exhibited a consistent annual trend being low in winter months and high in summer months, barring year to year variations. To differentiate between BC and other absorbing particles, we analyzed the wavelength dependence of aerosol absorption coefficient and determined a best-fit exponent i.e., the Ångström exponent, for the whole dataset. Visible Ångström exponent (AE: 470-520-590-660 nm) values ranged between 0 and 3.5, with most frequently occurring values in the range 0.85 to 1.25. By making use of the aethalometer light attenuation measurements at different wavelengths and Hysplit back trajectories, we divided the data into two categories. One for periods characterized by AE values close to 1; these periods are typically correlated with back trajectories originating from Canada, North America or northern Europe, indicating the dominance of BC on the light attenuation. Another characterized by AE values substantially different from 1; these periods correlated with back trajectories originating from dust-prone regions (e.g., the Sahara desert).The above measurements, with the aid of ancillary satellite and ground-based measurements will be employed in estimating the radiaitve effects of BC in the North Atlantic.

Published
2012

35. Free Tropospheric Aerosol Measurements at the Pico Mountain Observatory, Azores (2225m asl)

Author

Mazzoleni, Claudio, Mazzoleni, Lynn R., Fialho, Paulo, Kumar, Sumit, Dzepina, Katja, Dziobak, Michael P., Kramer, Louisa, Olsen, Seth C., Owen, Robert, Helmig, Detlev, Hueber, Jacques, and China, Swarup

Subjects
Aerossol Atmosférico, Atmospheric Aerosol, Tropospheric Aerosol, Black Carbon, Azores, Pico Island (Azores)
Abstract

AAAR 31st Annual Conference. Minneapolis, Minnesota, October 8-12, 2012. In this poster we discuss a limited subset of the aerosol measurements performed at the Pico Mountain Observatory. The Black Carbon (BC) mass shows a clear seasonal pattern over a ten-years period. The 2012 scattering measurements show highly variable signals with events with high scattering and periods of very low aerosol loading. Dust events are clearly captured by the aethalometer, as well the nephelometer Ångström exponents. Particles have various shapes, and mixing states, and soot particles typically are very compacted.

Published
2012

36. Measurement of Free Tropospheric Aerosols in the North Atlantic at the Pico Mountain Observatory

Author

Dzepina, Katja, Kumar, Sumit, Mazzoleni, Claudio, Fialho, Paulo, Dziobak, Michael P., Hueber, Jacques, Helmig, Detlev, Kramer, Louisa, Olsen, Seth C., and Mazzoleni, Lynn R.

Subjects
Atmospheric Pollution, Tropospheric Aerosol, Black Carbon, Azores, Poluição Atmosférica, Pico Island (Azores)
Abstract

AAAR 31st Annual Conference. Minneapolis, Minnesota, October 8-12, 2012. The Pico Mountain Observatory is located at 2225 m amsl on an inactive volcano at Pico Island in the Azores archipelago in the North Atlantic ~3900 km east and downwind of North America (38º28'15''N; 28º24’'14''W). The unique location of the Observatory enables sampling of free tropospheric air transported over long, intercontinental distances and is rarely affected by local emissions. The Observatory is affected mainly by North American outflow after its trans-Atlantic transport. Therefore, its location is ideal for observations of long-range transported pollutants emitted from anthropogenic and biogenic continental sources. The composition of continental pollution outflow is altered during transport by mixing, chemical reactions, phase changes, and removal processes. Thus, the properties of aerosol and trace gases in downwind regions are impacted by the outflow of pollutants, their chemical transformation, and sinks. In previous work, the sampled air-mass measurements (including CO, O3, NOx, NOy, NMHC, black carbon and aerosol optical size) and the simulations of their dispersion indicated outflow of North American tropospheric ozone and its precursors. Although the measurements have been crucial in explaining the evolution of North American gaseous pollution, little is known regarding the nature of the aged aerosol. New work is currently underway at the Observatory to provide chemical characterization of the intercepted free tropospheric aerosols. Here, we show the preliminary results of the free tropospheric aerosol composition and its physical properties. Samples were collected using high-volume filter samplers with quartz filters and analyzed for organic and elemental carbon (OC and EC, respectively). We compare the observed OC and EC values to the collocated measurements of gas- and particle-phase species, meteorological parameters and to the values found in current literature. We highlight the future work in which we will select filter samples based on the arrival of highly polluted air masses from anthropological or biomass burning emissions for further detailed analysis.

Published
2012

37. Morphology and mixing state of aged soot particles at a remote marine free troposphere site: Implications for optical properties

Author

China, Swarup, primary, Scarnato, Barbara, additional, Owen, Robert C., additional, Zhang, Bo, additional, Ampadu, Marian T., additional, Kumar, Sumit, additional, Dzepina, Katja, additional, Dziobak, Michael P., additional, Fialho, Paulo, additional, Perlinger, Judith A., additional, Hueber, Jacques, additional, Helmig, Detlev, additional, Mazzoleni, Lynn R., additional, and Mazzoleni, Claudio, additional

Published
2015
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38. Chemical and hygroscopic properties of aerosol organics at Storm Peak Laboratory

Author

Hallar, A. Gannet, Lowenthal, Douglas H., Clegg, Simon L., Samburova, Vera, Taylor, Nathan, Mazzoleni, Lynn R., Zielinska, Barbara K., Kristensen, Thomas Bjerring, Chirokova, Galina, McCubbin, Ian B., Dodson, Craig, Collins, Don, Hallar, A. Gannet, Lowenthal, Douglas H., Clegg, Simon L., Samburova, Vera, Taylor, Nathan, Mazzoleni, Lynn R., Zielinska, Barbara K., Kristensen, Thomas Bjerring, Chirokova, Galina, McCubbin, Ian B., Dodson, Craig, and Collins, Don

Published
2013

39. Hygroscopic growth and CCN activity of HULIS from different environments

Author

Kristensen, Thomas Bjerring, Wex, Heike, Nekat, Bettina, Nøjgaard, Jacob Klenø, Pinxteren, Dominik van, Lowenthal, Douglas H., Mazzoleni, Lynn R., Dieckmann, Katrin, Bender Koch, Christian, Mentel, Thomas F., Herrmann, Hartmut, Hallar, A. Gannet, Stratmann, Frank, Bilde, Merete, Kristensen, Thomas Bjerring, Wex, Heike, Nekat, Bettina, Nøjgaard, Jacob Klenø, Pinxteren, Dominik van, Lowenthal, Douglas H., Mazzoleni, Lynn R., Dieckmann, Katrin, Bender Koch, Christian, Mentel, Thomas F., Herrmann, Hartmut, Hallar, A. Gannet, Stratmann, Frank, and Bilde, Merete

Abstract

Humic-like substances (HULIS) constitute a significant fraction of aerosol particles in different environments. Studies of the role of HULIS in hygroscopic growth and cloud condensation nuclei (CCN) activity of aerosol particles are scarce, and results differ significantly. In this work the hygroscopic growth and CCN activity of water extracts (WE) and HULIS extracted from particulate matter (PM) collected at a polluted urban site (Copenhagen, Denmark), a rural site (Melpitz, Germany) and the remote site Storm Peak Laboratory (Colorado, USA) were investigated. Measurements of inorganic ions, elemental carbon, organic carbon and water soluble organic carbon (WSOC) within the PM confirmed that the sources of aerosol particles most likely differed for the three samples. The hygroscopic properties of the filtered WE were characterized by hygroscopicity parameters for subsaturated conditions (k(GF)) of 0.25, 0.41 and 0.22, and for supersaturated conditions k(CCN) were 0.23, 0.29 and 0.22 respectively for the urban, rural and remote WE samples. The measured hygroscopic growth and CCN activity were almost identical for the three HULIS samples and could be well represented by k(GF) = 0.07 and k(CCN) = 0.08-0.10 respectively. Small amounts of inorganic ions were present in the HULIS samples so the actual values for pure HULIS are expected to be slightly lower (k(GF)(*) = 0.04-0.06 and k(CCN)(*) = 0.07-0.08). The HULIS samples are thus less hygroscopic compared to most previous studies. To aid direct comparison of hygroscopic properties of HULIS from different studies, we recommend that the fraction of inorganic species in the HULIS samples always is measured and reported.

Published
2012

40. Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

Author

Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Department of Civil and Environmental Engineering, Kroll, Jesse, Kessler, Sean Herbert, Donahue, Neil M., Jimenez, Jose L., Canagaratna, M. R., Wilson, Kevin R., Altieri, Katye E., Mazzoleni, Lynn R., Wozniak, Andrew S., Bluhm, Hendrik, Mysak, Erin R., Smith, Jared D., Kolb, Charles E., Worsnop, Douglas R., Massachusetts Institute of Technology. Department of Chemistry, Massachusetts Institute of Technology. Department of Civil and Environmental Engineering, Kroll, Jesse, Kessler, Sean Herbert, Donahue, Neil M., Jimenez, Jose L., Canagaratna, M. R., Wilson, Kevin R., Altieri, Katye E., Mazzoleni, Lynn R., Wozniak, Andrew S., Bluhm, Hendrik, Mysak, Erin R., Smith, Jared D., Kolb, Charles E., and Worsnop, Douglas R.

Abstract

A detailed understanding of the sources, transformations and fates of organic species in the environment is crucial because of the central roles that they play in human health, biogeochemical cycles and the Earth's climate. However, such an understanding is hindered by the immense chemical complexity of environmental mixtures of organics; for example, atmospheric organic aerosol consists of at least thousands of individual compounds, all of which likely evolve chemically over their atmospheric lifetimes. Here, we demonstrate the utility of describing organic aerosol (and other complex organic mixtures) in terms of average carbon oxidation state, a quantity that always increases with oxidation, and is readily measured using state-of-the-art analytical techniques. Field and laboratory measurements of the average carbon oxidation state, using several such techniques, constrain the chemical properties of the organics and demonstrate that the formation and evolution of organic aerosol involves simultaneous changes to both carbon oxidation state and carbon number., United States. Environmental Protection Agency (Science To Achieve Results (STAR) program (grant R833746)), United States. Dept. of Energy (DOE: grant DE-FG02-05ER63995), United States. Dept. of Energy (DOE: grant ATM-0449815), United States. Dept. of Energy (DOE: grant ATM-0919189), United States. National Oceanic and Atmospheric Administration (NOAA: grant NA08OAR4310565), United States. Dept. of Energy (Director, Office of Energy Research, Office of Basic Energy Sciences, and Chemical Sciences Division of the US DOE (contract no. DE-AC02-05CH11231)), Lawrence Berkeley National Laboratory (Laboratory Directed Research and Development Program), Henry & Camille Dreyfus Foundation

Published
2012

41. Chemical and hygroscopic properties of aerosol organics at Storm Peak Laboratory

Author

Hallar, A. Gannet, primary, Lowenthal, Douglas H., additional, Clegg, Simon L., additional, Samburova, Vera, additional, Taylor, Nathan, additional, Mazzoleni, Lynn R., additional, Zielinska, Barbara K., additional, Kristensen, Thomas B., additional, Chirokova, Galina, additional, McCubbin, Ian B., additional, Dodson, Craig, additional, and Collins, Don, additional

Published
2013
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43. Hygroscopic growth of water soluble organic carbon isolated from atmospheric aerosol collected at U.S. national parks and Storm Peak Laboratory.

Author

Taylor, Nathan F., Collins, Don R., Lowenthal, Douglas H., Zielinska, Barbara, Samburova, Vera, Kumar, Naresh, Hallar, A. Gannet, Mazzoleni, Lynn R., and McCubbin, Ian B.

Abstract

Due to the atmospheric abundance and chemical complexity of Water Soluble Organic Carbon (WSOC), its contribution to the hydration behavior of atmospheric aerosol is both significant and difficult to assess. For the present study, the hygroscopicity and CCN activity of isolated atmospheric WSOC particulate matter was measured without the compounding effects of common, soluble inorganic aerosol constituents. WSOC was extracted with high purity water from daily high-volume PM2.5 filter samples and separated from water soluble inorganic constituents using solid phase extraction. The WSOC filter extracts were concentrated and combined to provide sufficient mass for continuous generation of the WSOC-only aerosol over the combined measurement time of the tandem differential mobility analyzer and coupled scanning mobility particle sizer/CCN counter used for the analysis. Aerosol samples were taken at Great Smoky Mountains National Park during the summer of 2006 and fall-winter of 2007-08; Mount Rainier National Park during the summer of 2009; Storm Peak Laboratory (SPL) near Steamboat Springs, Colorado, during the summer of 2010; and Acadia National Park during the summer of 2011. Across all sampling locations and seasons, the hygroscopic growth of WSOC samples at 90% RH, expressed in terms of the hygroscopicity parameter, "kappa," ranged from 0.05-0.15. Comparisons between the hygroscopicity of WSOC and that of samples containing all soluble materials extracted from the filters implied a significant modification of the hydration behavior of inorganic components, including decreased hysteresis separating efflorescence and deliquescence and enhanced dissolution between 40 and 80% RH. [ABSTRACT FROM AUTHOR]

Published
2016
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44. Hygroscopic growth and CCN activity of HULIS from different environments

Author

Kristensen, Thomas B., primary, Wex, Heike, additional, Nekat, Bettina, additional, Nøjgaard, Jacob K., additional, van Pinxteren, Dominik, additional, Lowenthal, Douglas H., additional, Mazzoleni, Lynn R., additional, Dieckmann, Katrin, additional, Bender Koch, Christian, additional, Mentel, Thomas F., additional, Herrmann, Hartmut, additional, Gannet Hallar, A., additional, Stratmann, Frank, additional, and Bilde, Merete, additional

Published
2012
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48. Carbon oxidation state as a metric for describing the chemistry of atmospheric organic aerosol

Author

Kroll, Jesse H., primary, Donahue, Neil M., additional, Jimenez, Jose L., additional, Kessler, Sean H., additional, Canagaratna, Manjula R., additional, Wilson, Kevin R., additional, Altieri, Katye E., additional, Mazzoleni, Lynn R., additional, Wozniak, Andrew S., additional, Bluhm, Hendrik, additional, Mysak, Erin R., additional, Smith, Jared D., additional, Kolb, Charles E., additional, and Worsnop, Douglas R., additional

Published
2011
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