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28 results on '"Cubison, Michael J."'

1. Chemical transport models often underestimate inorganic aerosol acidity in remote regions of the atmosphere

Author

Nault, Benjamin A., Campuzano-Jost, Pedro, Day, Douglas A., Jo, Duseong S., Schroder, Jason C., Allen, Hannah M., Bahreini, Roya, Bian, Huisheng, Blake, Donald R., Chin, Mian, Clegg, Simon L., Colarco, Peter R., Crounse, John D., Cubison, Michael J., DeCarlo, Peter F., Dibb, Jack E., Diskin, Glenn S., Hodzic, Alma, Hu, Weiwei, Katich, Joseph M., Kim, Michelle J., Kodros, John K., Kupc, Agnieszka, Lopez-Hilfiker, Felipe D., Marais, Eloise A., Middlebrook, Ann M., Andrew Neuman, J., Nowak, John B., Palm, Brett B., Paulot, Fabien, Pierce, Jeffrey R., Schill, Gregory P., Scheuer, Eric, Thornton, Joel A., Tsigaridis, Kostas, Wennberg, Paul O., Williamson, Christina J., and Jimenez, Jose L.

Published
2021
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5. Evaluating Model Parameterizations of Submicron Aerosol Scattering and Absorption with in situ Data from ARCTAS 2008

Author

Alvarado, Matthew J, Lonsdale, Chantelle R, Macintyre, Helen L, Bian, Huisheng, Chin, Mian, Ridley, David A, Heald, Colette L, Thornhill, Kenneth L, Anderson, Bruce E, Cubison, Michael J, Jimenez, Jose. L, Kondo, Yutaka, Sahu, Lokesh K, Dibb, Jack E, and Wang, Chien

Subjects
Geophysics, Environment Pollution
Abstract

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9- 02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10-23 percent, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GCRT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout the aerosol size distribution. Using a core-shell mixing rule in ASP overestimates aerosol absorption, especially for the fresh biomass burning aerosol measured in ARCTAS-B, suggesting the need for modeling the time-varying mixing states of aerosols in future versions of ASP.

Published
2016
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6. New SOA Treatments Within the Energy Exascale Earth System Model (E3SM): Strong Production and Sinks Govern Atmospheric SOA Distributions and Radiative Forcing

Author

Lou, Sijia, primary, Shrivastava, Manish, additional, Easter, Richard C., additional, Yang, Yang, additional, Ma, Po‐Lun, additional, Wang, Hailong, additional, Cubison, Michael J., additional, Campuzano‐Jost, Pedro, additional, Jimenez, Jose L., additional, Zhang, Qi, additional, Rasch, Philip J., additional, Shilling, John E., additional, Zelenyuk, Alla, additional, Dubey, Manvendra, additional, Cameron‐Smith, Philip, additional, Martin, Scot T., additional, Schneider, Johannes, additional, and Schulz, Christiane, additional

Published
2020
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7. Interferences with aerosol acidity quantification due to gas-phase ammonia uptake onto acidic sulfate filter samples

Author

Nault, Benjamin A., primary, Campuzano-Jost, Pedro, additional, Day, Douglas A., additional, Guo, Hongyu, additional, Jo, Duseong S., additional, Handschy, Anne V., additional, Pagonis, Demetrios, additional, Schroder, Jason C., additional, Schueneman, Melinda K., additional, Cubison, Michael J., additional, Dibb, Jack E., additional, Hodzic, Alma, additional, Hu, Weiwei, additional, Palm, Brett B., additional, and Jimenez, Jose L., additional

Published
2020
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8. Supplementary material to "Interferences on Aerosol Acidity Quantification due to Gas-phase Ammonia Uptake onto Acidic Sulfate Filter Samples"

Author

Nault, Benjamin A., primary, Campuzano-Jost, Pedro, additional, Day, Douglas A., additional, Guo, Hongyu, additional, Jo, Duesong S., additional, Handscy, Anne V., additional, Pagonis, Demetrios, additional, Schroder, Jason C., additional, Schueneman, Melinda K., additional, Cubison, Michael J., additional, Dibb, Jack E., additional, Hodzic, Alma, additional, Hu, Weiwei, additional, Palm, Brett B., additional, and Jimenez, Jose L., additional

Published
2020
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9. Interferences on Aerosol Acidity Quantification due to Gas-phase Ammonia Uptake onto Acidic Sulfate Filter Samples

Author

Nault, Benjamin A., primary, Campuzano-Jost, Pedro, additional, Day, Douglas A., additional, Guo, Hongyu, additional, Jo, Duesong S., additional, Handscy, Anne V., additional, Pagonis, Demetrios, additional, Schroder, Jason C., additional, Schueneman, Melinda K., additional, Cubison, Michael J., additional, Dibb, Jack E., additional, Hodzic, Alma, additional, Hu, Weiwei, additional, Palm, Brett B., additional, and Jimenez, Jose L., additional

Published
2020
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10. Interferences on Aerosol Acidity Quantification due to Gas-phase Ammonia Uptake onto Acidic Sulfate Filter Samples.

Author

Nault, Benjamin A., Campuzano-Jost, Pedro, Day, Douglas A., Hongyu Guo, Jo, Duesong S., Handscy, Anne V., Pagonis, Demetrios, Schroder, Jason C., Schueneman, Melinda K., Cubison, Michael J., Dibb, Jack E., Hodzic, Alma, Weiwei Hu, Palm, Brett B., and Jimenez, Jose L.

Subjects
AEROSOLS, CHEMICAL processes, CHEMICAL speciation, AMMONIUM, AMMONIA, FILTERS & filtration, ACIDITY, MASS spectrometers
Abstract

Measurements of the mass concentration and chemical speciation of aerosols are important to investigate their chemical and physical processing from near emission sources to the most remote regions of the atmosphere. A common method to analyze aerosols is to collect them onto filters and to analyze filters off-line; however, biases in some chemical components are possible due to changes in the accumulated particles during the handling of the samples. Any biases would impact the measured chemical composition, which in turn affects our understanding of numerous physico-chemical processes and aerosol radiative properties. We show, using filters collected onboard the NASA DC-8 and NSF C-130 during six different aircraft campaigns, a consistent, substantial difference in ammonium mass concentration and ammonium-to- anion ratios, when comparing the aerosols collected on filters versus the Aerodyne Aerosol Mass Spectrometer (AMS). Another on-line measurement is consistent with the AMS in showing that the aerosol has lower ammonium-to-anion ratios than obtained by the filters. Using a gas uptake model with literature values for accommodation coefficients, we show that for ambient ammonia mixing ratios greater than 10 ppbv, the time scale for ammonia reacting with acidic aerosol on filter substrates is less than 30 s (typical filter handling time in the aircraft) for typical aerosol volume distributions. Measurements of gas-phase ammonia inside the cabin of the DC-8 show ammonia mixing ratios of 45 ± 20 ppbv, consistent with mixing ratios observed in other indoor environments. This analysis enables guidelines for filter handling to reduce ammonia uptake. Finally, a more meaningful limit-of-detection for filters that either do not have an ammonia scrubber and/or are handled in the presence of human emissions is ~0.2 µg m-3 ammonium, which is substantially higher than the limit-of -detection of the ion chromatography. [ABSTRACT FROM AUTHOR]

Published
2020
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11. Evaluating model parameterizations of submicron aerosol scattering and absorption with in situ data from ARCTAS 2008

Author

Massachusetts Institute of Technology. Center for Global Change Science, Massachusetts Institute of Technology. Department of Civil and Environmental Engineering, Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences, Macintyre, Helen, Ridley, David Andrew, Heald, Colette L., Wang, Chien, Alvarado, Matthew J., Lonsdale, Chantelle R., Bian, Huisheng, Chin, Mian, Thornhill, Kenneth L., Anderson, Bruce E., Cubison, Michael J., Jimenez, Jose L., Kondo, Yutaka, Sahu, Lokesh K., Dibb, Jack E., Massachusetts Institute of Technology. Center for Global Change Science, Massachusetts Institute of Technology. Department of Civil and Environmental Engineering, Massachusetts Institute of Technology. Department of Earth, Atmospheric, and Planetary Sciences, Macintyre, Helen, Ridley, David Andrew, Heald, Colette L., Wang, Chien, Alvarado, Matthew J., Lonsdale, Chantelle R., Bian, Huisheng, Chin, Mian, Thornhill, Kenneth L., Anderson, Bruce E., Cubison, Michael J., Jimenez, Jose L., Kondo, Yutaka, Sahu, Lokesh K., and Dibb, Jack E.

Abstract

Accurate modeling of the scattering and absorption of ultraviolet and visible radiation by aerosols is essential for accurate simulations of atmospheric chemistry and climate. Closure studies using in situ measurements of aerosol scattering and absorption can be used to evaluate and improve models of aerosol optical properties without interference from model errors in aerosol emissions, transport, chemistry, or deposition rates. Here we evaluate the ability of four externally mixed, fixed size distribution parameterizations used in global models to simulate submicron aerosol scattering and absorption at three wavelengths using in situ data gathered during the 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) campaign. The four models are the NASA Global Modeling Initiative (GMI) Combo model, GEOS-Chem v9-02, the baseline configuration of a version of GEOS-Chem with online radiative transfer calculations (called GC-RT), and the Optical Properties of Aerosol and Clouds (OPAC v3.1) package. We also use the ARCTAS data to perform the first evaluation of the ability of the Aerosol Simulation Program (ASP v2.1) to simulate submicron aerosol scattering and absorption when in situ data on the aerosol size distribution are used, and examine the impact of different mixing rules for black carbon (BC) on the results. We find that the GMI model tends to overestimate submicron scattering and absorption at shorter wavelengths by 10–23 %, and that GMI has smaller absolute mean biases for submicron absorption than OPAC v3.1, GEOS-Chem v9-02, or GC-RT. However, the changes to the density and refractive index of BC in GC-RT improve the simulation of submicron aerosol absorption at all wavelengths relative to GEOS-Chem v9-02. Adding a variable size distribution, as in ASP v2.1, improves model performance for scattering but not for absorption, likely due to the assumption in ASP v2.1 that BC is present at a constant mass fraction throughout, United States. National Aeronautics and Space Administration (NN14AP38G), United States. National Aeronautics and Space Administration (NNX11AN72G)

Published
2017

12. Highly Oxygenated Multifunctional Compounds in α-Pinene Secondary Organic Aerosol

Author

Zhang, Xuan, primary, Lambe, Andrew T., additional, Upshur, Mary Alice, additional, Brooks, William A., additional, Gray Bé, Ariana, additional, Thomson, Regan J., additional, Geiger, Franz M., additional, Surratt, Jason D., additional, Zhang, Zhenfa, additional, Gold, Avram, additional, Graf, Stephan, additional, Cubison, Michael J., additional, Groessl, Michael, additional, Jayne, John T., additional, Worsnop, Douglas R., additional, and Canagaratna, Manjula R., additional

Published
2017
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13. Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

Author

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

Published
2016
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14. Real-time measurements of secondary organic aerosol formation and aging from ambient air in an oxidation flow reactor in the Los Angeles area

Author

Ortega, Amber M., primary, Hayes, Patrick L., additional, Peng, Zhe, additional, Palm, Brett B., additional, Hu, Weiwei, additional, Day, Douglas A., additional, Li, Rui, additional, Cubison, Michael J., additional, Brune, William H., additional, Graus, Martin, additional, Warneke, Carsten, additional, Gilman, Jessica B., additional, Kuster, William C., additional, de Gouw, Joost, additional, Gutiérrez-Montes, Cándido, additional, and Jimenez, Jose L., additional

Published
2016
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15. Ion Mobility Spectrometry-Mass Spectrometry (IMS-MS) for on- and off-line analysis of atmospheric gas and aerosol species

Author

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

Published
2016
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16. Supplementary material to "Ion Mobility Spectrometry-Mass Spectrometry (IMS-MS) for on- and off-line analysis of atmospheric gas and aerosol species"

Author

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

Published
2016
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17. Estimating the contribution of organic acids to northern hemispheric continental organic aerosol

Author

Yatavelli, Reddy L. N., primary, Mohr, Claudia, additional, Stark, Harald, additional, Day, Douglas A., additional, Thompson, Samantha L., additional, Lopez‐Hilfiker, Felipe D., additional, Campuzano‐Jost, Pedro, additional, Palm, Brett B., additional, Vogel, Alexander L., additional, Hoffmann, Thorsten, additional, Heikkinen, Liine, additional, Äijälä, Mikko, additional, Ng, Nga L., additional, Kimmel, Joel R., additional, Canagaratna, Manjula R., additional, Ehn, Mikael, additional, Junninen, Heikki, additional, Cubison, Michael J., additional, Petäjä, Tuukka, additional, Kulmala, Markku, additional, Jayne, John T., additional, Worsnop, Douglas R., additional, and Jimenez, Jose L., additional

Published
2015
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18. Observational Insights into Aerosol Formation from Isoprene

Author

Worton, David R., primary, Surratt, Jason D., additional, LaFranchi, Brian W., additional, Chan, Arthur W. H., additional, Zhao, Yunliang, additional, Weber, Robin J., additional, Park, Jeong-Hoo, additional, Gilman, Jessica B., additional, de Gouw, Joost, additional, Park, Changhyoun, additional, Schade, Gunnar, additional, Beaver, Melinda, additional, Clair, Jason M. St., additional, Crounse, John, additional, Wennberg, Paul, additional, Wolfe, Glenn M., additional, Harrold, Sara, additional, Thornton, Joel A., additional, Farmer, Delphine K., additional, Docherty, Kenneth S., additional, Cubison, Michael J., additional, Jimenez, Jose-Luis, additional, Frossard, Amanda A., additional, Russell, Lynn M., additional, Kristensen, Kasper, additional, Glasius, Marianne, additional, Mao, Jingqiu, additional, Ren, Xinrong, additional, Brune, William, additional, Browne, Eleanor C., additional, Pusede, Sally E., additional, Cohen, Ronald C., additional, Seinfeld, John H., additional, and Goldstein, Allen H., additional

Published
2013
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19. Comparison of chemical characteristics of 495 biomass burning plumes intercepted by the NASA DC-8 aircraft during the ARCTAS/CARB-2008 field campaign

Author

Hecobian, Arsineh, Liu, Zhen, Hennigan, Christopher J., Huey, L. Gregory, Jimenez, Jose Luis, Cubison, Michael J., Vay, Stephanie, Diskin, Glenn S., Sachse, Glen W., Wisthaler, Armin, Mikoviny, Tomas, Weinheimer, Andrew J., Liao, Jin, Knapp, David J., Wennberg, Paul O., Kürten, Christoph Andreas, Crounse, John D., St. Clair, Jason M., Wang, Yuxuan, Weber, Rodney J., Hecobian, Arsineh, Liu, Zhen, Hennigan, Christopher J., Huey, L. Gregory, Jimenez, Jose Luis, Cubison, Michael J., Vay, Stephanie, Diskin, Glenn S., Sachse, Glen W., Wisthaler, Armin, Mikoviny, Tomas, Weinheimer, Andrew J., Liao, Jin, Knapp, David J., Wennberg, Paul O., Kürten, Christoph Andreas, Crounse, John D., St. Clair, Jason M., Wang, Yuxuan, and Weber, Rodney J.

Abstract

This paper compares measurements of gaseous and particulate emissions from a wide range of biomass-burning plumes intercepted by the NASA DC-8 research aircraft during the three phases of the ARCTAS-2008 experiment: ARCTAS-A, based out of Fairbanks, Alaska, USA (3 April to 19 April 2008); ARCTAS-B based out of Cold Lake, Alberta, Canada (29 June to 13 July 2008); and ARCTAS-CARB, based out of Palmdale, California, USA (18 June to 24 June 2008). Approximately 500 smoke plumes from biomass burning emissions that varied in age from minutes to days were segregated by fire source region and urban emission influences. The normalized excess mixing ratios (NEMR) of gaseous (carbon dioxide, acetonitrile, hydrogen cyanide, toluene, benzene, methane, oxides of nitrogen and ozone) and fine aerosol particulate components (nitrate, sulfate, ammonium, chloride, organic aerosols and water soluble organic carbon) of these plumes were compared. A detailed statistical analysis of the different plume categories for different gaseous and aerosol species is presented in this paper. The comparison of NEMR values showed that CH4 concentrations were higher in air-masses that were influenced by urban emissions. Fresh biomass burning plumes mixed with urban emissions showed a higher degree of oxidative processing in comparison with fresh biomass burning only plumes. This was evident in higher concentrations of inorganic aerosol components such as sulfate, nitrate and ammonium, but not reflected in the organic components. Lower NOx NEMRs combined with high sulfate, nitrate and ammonium NEMRs in aerosols of plumes subject to long-range transport, when comparing all plume categories, provided evidence of advanced processing of these plumes.

Published
2011

20. A Chemical Ionization High-Resolution Time-of-Flight Mass Spectrometer Coupled to a Micro Orifice Volatilization Impactor (MOVI-HRToF-CIMS) for Analysis of Gas and Particle-Phase Organic Species

Author

Yatavelli, Reddy L. N., primary, Lopez-Hilfiker, Felipe, additional, Wargo, Julia D., additional, Kimmel, Joel R., additional, Cubison, Michael J., additional, Bertram, Timothy H., additional, Jimenez, Jose L., additional, Gonin, Marc, additional, Worsnop, Douglas R., additional, and Thornton, Joel A., additional

Published
2012
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21. Sectoral and geographical contributions to summertime continental United States (CONUS) black carbon spatial distributions

Author

Huang, Min, primary, Carmichael, Gregory R., additional, Kulkarni, Sarika, additional, Streets, David G., additional, Lu, Zifeng, additional, Zhang, Qiang, additional, Pierce, R. Bradley, additional, Kondo, Yutaka, additional, Jimenez, Jose L., additional, Cubison, Michael J., additional, Anderson, Bruce, additional, and Wisthaler, Armin, additional

Published
2012
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22. Sources, distribution, and acidity of sulfate–ammonium aerosol in the Arctic in winter–spring

Author

Fisher, Jenny A., primary, Jacob, Daniel J., additional, Wang, Qiaoqiao, additional, Bahreini, Roya, additional, Carouge, Claire C., additional, Cubison, Michael J., additional, Dibb, Jack E., additional, Diehl, Thomas, additional, Jimenez, Jose L., additional, Leibensperger, Eric M., additional, Lu, Zifeng, additional, Meinders, Marcel B.J., additional, Pye, Havala O.T., additional, Quinn, Patricia K., additional, Sharma, Sangeeta, additional, Streets, David G., additional, van Donkelaar, Aaron, additional, and Yantosca, Robert M., additional

Published
2011
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23. 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

Author

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

Published
2009
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24. Applications of broadband cavity enhanced spectroscopy

Author

Washenfelder, Rebecca A., Flores, Jorge M., Young, Cora J., Brown, Steven S., Brock, Charles A., Rudich, Yinon, Angevine, Wayne M., Atlas, Elliot L., Blake, Donald R., Bon, Daniel M., Cubison, Michael J., Gouw, Joost A., Dusanter, Sebastien, Flynn, James, Gilman, Jessica B., Grauss, Martin, Griffith, Stephen, Grossberg, Nicole, Hayes, Patrick L., Jose L Jimenez, Kuster, William C., Lefer, Barry L., Pollack, Ilana B., Ryerson, Thomas B., Stark, Harald, Stevens, Philip S., and Trainer, Michael K.

25. Effects of aging on organic aerosol from open biomass burning smoke in aircraft & lab studies

Author

Jose L Jimenez, Cubison, Michael J., Ortega, Amber M., Hayes, Patrick L., Farmer, Delphine K., Day, Douglas A., Lechner, Michael J., Brune, William H., Apel, Eric, Diskin, Glenn S., Fisher, Jenny A., Fuelberg, Henry A., Hecobian, Arsineh, Knapp, David J., Mikoviny, Tomas, Riemer, Daniel, Sachse, Glen W., Sessions, Walter, Weber, Rodney J., Weinheimer, Andrew J., and Wisthaler, Armin

27. Significance of supermicron particles for atmospheric nitrogen oxides

Author

Murphy, Jennifer G., Ellis, Raluca A., Markovic, Milos Z., Vandenboer, Trevor C., Petroff, Alexandre, Gregoire, Phillip, Wentworth, Gregory, Hayes, Patrick L., Cubison, Michael J., Ortega, Amber M., Jose L Jimenez, Liu, Jiumeng, Weber, Rodney J., Veres, Patrick, Cochran, Anthony K., Roberts, Jim M., and Brown, Steven S.

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

Author

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

Subjects
13. Climate action
Abstract

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 presence of the organosulfate functional group.

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