Articles | Volume 21, issue 11
https://doi.org/10.5194/acp-21-8999-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-21-8999-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
14 Jun 2021
Research article |
| 14 Jun 2021
| 14 Jun 2021
Towards a chemical mechanism of the oxidation of aqueous sulfur dioxide via isoprene hydroxyl hydroperoxides (ISOPOOH)
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
now at: Multiphase Chemistry Department, Max Planck Institute for Chemistry, 55128 Mainz, Germany
Kelvin H. Bates
Harvard University Center for the Environment, Cambridge, MA 02138, USA
Jean C. Rivera-Rios
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
now at: School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, GA 30332, USA
Joshua L. Cox
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
Joshua D. Shutter
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
Frank N. Keutsch
John A. Paulson School of Engineering and Applied Sciences, Harvard University, Cambridge, MA 02138, USA
Department of Chemistry and Chemical Biology, Harvard University, Cambridge, MA 02138, USA
Department of Earth and Planetary Sciences, Harvard University, Cambridge, MA 02138, USA
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Kelvin H. Bates, Guy J. P. Burke, James D. Cope, and Tran B. Nguyen
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Kelvin H. Bates, Daniel J. Jacob, Ke Li, Peter D. Ivatt, Mat J. Evans, Yingying Yan, and Jintai Lin
Atmos. Chem. Phys., 21, 18351–18374, https://doi.org/10.5194/acp-21-18351-2021, https://doi.org/10.5194/acp-21-18351-2021, 2021
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Dandan Wei, Hariprasad D. Alwe, Dylan B. Millet, Brandon Bottorff, Michelle Lew, Philip S. Stevens, Joshua D. Shutter, Joshua L. Cox, Frank N. Keutsch, Qianwen Shi, Sarah C. Kavassalis, Jennifer G. Murphy, Krystal T. Vasquez, Hannah M. Allen, Eric Praske, John D. Crounse, Paul O. Wennberg, Paul B. Shepson, Alexander A. T. Bui, Henry W. Wallace, Robert J. Griffin, Nathaniel W. May, Megan Connor, Jonathan H. Slade, Kerri A. Pratt, Ezra C. Wood, Mathew Rollings, Benjamin L. Deming, Daniel C. Anderson, and Allison L. Steiner
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Jack C. Hensley, Adam W. Birdsall, Gregory Valtierra, Joshua L. Cox, and Frank N. Keutsch
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Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
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Lei Zhu, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Kelly Chance, Eric C. Apel, Joshua P. DiGangi, Alan Fried, Thomas F. Hanisco, Rebecca S. Hornbrook, Lu Hu, Jennifer Kaiser, Frank N. Keutsch, Wade Permar, Jason M. St. Clair, and Glenn M. Wolfe
Atmos. Chem. Phys., 20, 12329–12345, https://doi.org/10.5194/acp-20-12329-2020, https://doi.org/10.5194/acp-20-12329-2020, 2020
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Abigail R. Koss, Manjula R. Canagaratna, Alexander Zaytsev, Jordan E. Krechmer, Martin Breitenlechner, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joseph R. Roscioli, Frank N. Keutsch, and Jesse H. Kroll
Atmos. Chem. Phys., 20, 1021–1041, https://doi.org/10.5194/acp-20-1021-2020, https://doi.org/10.5194/acp-20-1021-2020, 2020
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Alexander Zaytsev, Abigail R. Koss, Martin Breitenlechner, Jordan E. Krechmer, Kevin J. Nihill, Christopher Y. Lim, James C. Rowe, Joshua L. Cox, Joshua Moss, Joseph R. Roscioli, Manjula R. Canagaratna, Douglas R. Worsnop, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 15117–15129, https://doi.org/10.5194/acp-19-15117-2019, https://doi.org/10.5194/acp-19-15117-2019, 2019
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Aromatic hydrocarbons contribute significantly to the production of tropospheric ozone and secondary organic aerosol (SOA). Here later-generation low-volatility oxygenated products from toluene and 1,2,4-TMB oxidation by OH are detected in the gas and particle phases. We show that these products, previously identified as highly oxygenated molecules (HOMs), are formed in more than one pathway with differing numbers of reaction steps with OH. They also make up a significant fraction of SOA.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Adam W. Birdsall, Jack C. Hensley, Paige S. Kotowitz, Andrew J. Huisman, and Frank N. Keutsch
Atmos. Chem. Phys., 19, 14195–14209, https://doi.org/10.5194/acp-19-14195-2019, https://doi.org/10.5194/acp-19-14195-2019, 2019
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We have measured the evaporation rates of butenedial, a four-carbon dialdehyde produced in the atmosphere, from individual levitated particles. Effective vapor pressures and Henry's law constants, which characterize the compound's gas-particle partitioning behavior, were determined. The important role of hydration reactions was observed under both dry and humid conditions, as well as a salting-out effect in the presence of sodium chloride or sodium sulfate.
Joshua D. Shutter, Norton T. Allen, Thomas F. Hanisco, Glenn M. Wolfe, Jason M. St. Clair, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 6079–6089, https://doi.org/10.5194/amt-12-6079-2019, https://doi.org/10.5194/amt-12-6079-2019, 2019
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A new mid-infrared and ultra-portable formaldehyde (HCHO) sensor from Aeris Technologies is characterized and evaluated against well-established laser-induced fluorescence (LIF) instrumentation. The Aeris sensor displays linear behavior (R squared > 0.94) and shows good agreement with LIF instruments. While the compact sensor is not currently a replacement for the most sensitive research-grade instrumentation available, its sub-ppbv precision is sufficient for indoor and outdoor HCHO monitoring.
Eleni Dovrou, Christopher Y. Lim, Manjula R. Canagaratna, Jesse H. Kroll, Douglas R. Worsnop, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 5303–5315, https://doi.org/10.5194/amt-12-5303-2019, https://doi.org/10.5194/amt-12-5303-2019, 2019
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Measurement techniques commonly used to analyze particulate matter composition can result in the possible misidentification of sulfur-containing species, especially for the case of sulfate and hydroxymethanesulfonate (HMS). The efficiency and limitations of these techniques, along with a method that enables further studies of the contribution of sulfur-containing species, S(IV) versus S(VI), to particulate matter under low-light atmospheric conditions, are described in this work.
Alexander Zaytsev, Martin Breitenlechner, Abigail R. Koss, Christopher Y. Lim, James C. Rowe, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 12, 1861–1870, https://doi.org/10.5194/amt-12-1861-2019, https://doi.org/10.5194/amt-12-1861-2019, 2019
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Azimeh Zare, Paul S. Romer, Tran Nguyen, Frank N. Keutsch, Kate Skog, and Ronald C. Cohen
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Organic nitrates play an important role in concentrations and distribution of NOx, ozone and aerosol as the most important air pollutants. We develop a state-of-the-science detailed chemical mechanism representing individual organic nitrates, which is appropriate to use in air quality models and results in a more accurate simulation of atmospheric chemistry. Using this mechanism we explore production and removal processes of organic nitrates in a rural environment that are poorly constrained.
Hendrik Fuchs, Sascha Albrecht, Ismail–Hakki Acir, Birger Bohn, Martin Breitenlechner, Hans-Peter Dorn, Georgios I. Gkatzelis, Andreas Hofzumahaus, Frank Holland, Martin Kaminski, Frank N. Keutsch, Anna Novelli, David Reimer, Franz Rohrer, Ralf Tillmann, Luc Vereecken, Robert Wegener, Alexander Zaytsev, Astrid Kiendler-Scharr, and Andreas Wahner
Atmos. Chem. Phys., 18, 8001–8016, https://doi.org/10.5194/acp-18-8001-2018, https://doi.org/10.5194/acp-18-8001-2018, 2018
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The photooxidation of methyl vinyl ketone MVK, one of the most important products of isoprene that is emitted by plants, was investigated in the atmospheric simulation chamber SAPHIR for conditions found in forested areas. The comparison of measured trace gas time series with model calculations shows a gap in the understanding of radical chemistry in the MVK oxidation scheme. The possibility of unimolecular isomerization reactions were investigated by means of quantum-chemical calculations.
Shouming Zhou, Jean C. Rivera-Rios, Frank N. Keutsch, and Jonathan P. D. Abbatt
Atmos. Meas. Tech., 11, 3081–3089, https://doi.org/10.5194/amt-11-3081-2018, https://doi.org/10.5194/amt-11-3081-2018, 2018
Adam W. Birdsall, Ulrich K. Krieger, and Frank N. Keutsch
Atmos. Meas. Tech., 11, 33–47, https://doi.org/10.5194/amt-11-33-2018, https://doi.org/10.5194/amt-11-33-2018, 2018
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We have developed a laboratory system that provides mass spectra of individual particles, roughly 20 microns in diameter, after they have been levitated in an electric field. Measured evaporation of polyethylene glycol particles was found to agree with a kinetic model. The system can be used to study fundamental chemical and physical processes involving particles that are difficult to isolate and study with other techniques, and hence improve our understanding of atmospheric particles.
Abigail Koss, Bin Yuan, Carsten Warneke, Jessica B. Gilman, Brian M. Lerner, Patrick R. Veres, Jeff Peischl, Scott Eilerman, Rob Wild, Steven S. Brown, Chelsea R. Thompson, Thomas Ryerson, Thomas Hanisco, Glenn M. Wolfe, Jason M. St. Clair, Mitchell Thayer, Frank N. Keutsch, Shane Murphy, and Joost de Gouw
Atmos. Meas. Tech., 10, 2941–2968, https://doi.org/10.5194/amt-10-2941-2017, https://doi.org/10.5194/amt-10-2941-2017, 2017
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Oil and gas extraction activity can cause air quality issues through emission of reactive chemicals. VOCs related to extraction operations in the United States were measured by PTR-ToF-MS from aircraft during the SONGNEX campaign in March–April 2015. The detailed analysis in this work provides a guide to interpreting PTR-ToF measurements in oil- and gas-producing regions, and it includes fundamental observations of VOC speciation and mixing ratios.
Christopher Chan Miller, Daniel J. Jacob, Eloise A. Marais, Karen Yu, Katherine R. Travis, Patrick S. Kim, Jenny A. Fisher, Lei Zhu, Glenn M. Wolfe, Thomas F. Hanisco, Frank N. Keutsch, Jennifer Kaiser, Kyung-Eun Min, Steven S. Brown, Rebecca A. Washenfelder, Gonzalo González Abad, and Kelly Chance
Atmos. Chem. Phys., 17, 8725–8738, https://doi.org/10.5194/acp-17-8725-2017, https://doi.org/10.5194/acp-17-8725-2017, 2017
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The use of satellite glyoxal observations for estimating isoprene emissions has been limited by knowledge of the glyoxal yield from isoprene. We use SENEX aircraft observations over the southeast US to evaluate glyoxal yields from isoprene in a 3-D atmospheric model. The SENEX observations support a pathway for glyoxal formation in pristine regions that we propose here, which may have implications for improving isoprene emissions estimates from upcoming high-resolution geostationary satellites.
Anne-Kathrin Bernhammer, Martin Breitenlechner, Frank N. Keutsch, and Armin Hansel
Atmos. Chem. Phys., 17, 4053–4062, https://doi.org/10.5194/acp-17-4053-2017, https://doi.org/10.5194/acp-17-4053-2017, 2017
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Isoprene is the predominant non-methane compound emitted by the biosphere. In the atmosphere oxidation by OH under low NOx produces isoprene hydroxy hydroperoxides (ISOPOOHs). This work has found an effective conversion of ISOPOOHs to volatile carbonyls on metal environmental simulation chamber walls. Likely catalyzed decomposition reactions also occur for other hydroxyl hydroperoxides on metal surfaces.
Anusha P. S. Hettiyadura, Thilina Jayarathne, Karsten Baumann, Allen H. Goldstein, Joost A. de Gouw, Abigail Koss, Frank N. Keutsch, Kate Skog, and Elizabeth A. Stone
Atmos. Chem. Phys., 17, 1343–1359, https://doi.org/10.5194/acp-17-1343-2017, https://doi.org/10.5194/acp-17-1343-2017, 2017
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Organosulfates are components of secondary organic aerosol (SOA) formed in the presence of sulfate. Herein, their abundance, identity, and potential to form as sampling artifacts were studied in Centreville, AL, USA. The 10 most abundant signals accounted for 58–78 % of the total, with at least 20–200 other species accounting for the remainder. These major species were largely associated with biogenic gases, like isoprene and monoterpenes, and are proposed targets for future standard development.
Emma L. D'Ambro, Ben H. Lee, Jiumeng Liu, John E. Shilling, Cassandra J. Gaston, Felipe D. Lopez-Hilfiker, Siegfried Schobesberger, Rahul A. Zaveri, Claudia Mohr, Anna Lutz, Zhenfa Zhang, Avram Gold, Jason D. Surratt, Jean C. Rivera-Rios, Frank N. Keutsch, and Joel A. Thornton
Atmos. Chem. Phys., 17, 159–174, https://doi.org/10.5194/acp-17-159-2017, https://doi.org/10.5194/acp-17-159-2017, 2017
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We studied the formation and properties of secondary organic aerosol produced from isoprene. We find that a significant fraction (~50 %) of the mass is composed of low-volatility, highly oxidized compounds such as C5H12O6. A significant fraction of the remainder appears to be in the form of oligomeric material. Adding NOx maintained or decreased SOA yields while increasing the fraction of low-volatility material, possibly due to oligomers.
Jason M. St. Clair, Jean C. Rivera-Rios, John D. Crounse, Eric Praske, Michelle J. Kim, Glenn M. Wolfe, Frank N. Keutsch, Paul O. Wennberg, and Thomas F. Hanisco
Atmos. Meas. Tech., 9, 4561–4568, https://doi.org/10.5194/amt-9-4561-2016, https://doi.org/10.5194/amt-9-4561-2016, 2016
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Global isoprene emissions are the largest source of atmospheric non-methane hydrocarbons. Lab results show that ISOPOOH, a low-NOx isoprene oxidation product, can decompose on instrument surfaces to form high-NOx isoprene oxidation products, causing misinterpretation of oxidation conditions. This study investigated the potential formaldehyde artifact from ISOPOOH for the NASA ISAF instrument, and found that it does not significantly affect the accuracy of the ISAF field measurements.
J. Kaiser, K. M. Skog, K. Baumann, S. B. Bertman, S. B. Brown, W. H. Brune, J. D. Crounse, J. A. de Gouw, E. S. Edgerton, P. A. Feiner, A. H. Goldstein, A. Koss, P. K. Misztal, T. B. Nguyen, K. F. Olson, J. M. St. Clair, A. P. Teng, S. Toma, P. O. Wennberg, R. J. Wild, L. Zhang, and F. N. Keutsch
Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, https://doi.org/10.5194/acp-16-9349-2016, 2016
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OH reactivity can be used to assess the amount of reactive carbon in an air mass. “Missing” reactivity is commonly found in forested environments and is attributed to either direct emissions of unmeasured volatile organic compounds or to unmeasured/underpredicted oxidation products. Using a box model and measurements from the 2013 SOAS campaign, we find only small discrepancies in measured and calculated reactivity. Our results suggest the discrepancies stem from unmeasured direct emissions.
Carsten Warneke, Michael Trainer, Joost A. de Gouw, David D. Parrish, David W. Fahey, A. R. Ravishankara, Ann M. Middlebrook, Charles A. Brock, James M. Roberts, Steven S. Brown, Jonathan A. Neuman, Brian M. Lerner, Daniel Lack, Daniel Law, Gerhard Hübler, Iliana Pollack, Steven Sjostedt, Thomas B. Ryerson, Jessica B. Gilman, Jin Liao, John Holloway, Jeff Peischl, John B. Nowak, Kenneth C. Aikin, Kyung-Eun Min, Rebecca A. Washenfelder, Martin G. Graus, Mathew Richardson, Milos Z. Markovic, Nick L. Wagner, André Welti, Patrick R. Veres, Peter Edwards, Joshua P. Schwarz, Timothy Gordon, William P. Dube, Stuart A. McKeen, Jerome Brioude, Ravan Ahmadov, Aikaterini Bougiatioti, Jack J. Lin, Athanasios Nenes, Glenn M. Wolfe, Thomas F. Hanisco, Ben H. Lee, Felipe D. Lopez-Hilfiker, Joel A. Thornton, Frank N. Keutsch, Jennifer Kaiser, Jingqiu Mao, and Courtney D. Hatch
Atmos. Meas. Tech., 9, 3063–3093, https://doi.org/10.5194/amt-9-3063-2016, https://doi.org/10.5194/amt-9-3063-2016, 2016
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In this paper we describe the experimental approach, the science goals and early results of the NOAA SENEX campaign, which was focused on studying the interactions between biogenic and anthropogenic emissions to form secondary pollutants.
During SENEX, the NOAA WP-3D aircraft conducted 20 research flights between 27 May and 10 July 2013 based out of Smyrna, TN. The SENEX flights included day- and nighttime flights in the Southeast as well as flights over areas with intense shale gas extraction.
Amy P. Sullivan, Natasha Hodas, Barbara J. Turpin, Kate Skog, Frank N. Keutsch, Stefania Gilardoni, Marco Paglione, Matteo Rinaldi, Stefano Decesari, Maria Cristina Facchini, Laurent Poulain, Hartmut Herrmann, Alfred Wiedensohler, Eiko Nemitz, Marsailidh M. Twigg, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 8095–8108, https://doi.org/10.5194/acp-16-8095-2016, https://doi.org/10.5194/acp-16-8095-2016, 2016
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This paper presents the results from our measurements and approach for the investigation of aqueous secondary organic aerosol (aqSOA) formation in the ambient atmosphere. When local aqSOA formation was observed, a correlation of water-soluble organic carbon with organic aerosol, aerosol liquid water, relative humidity, and aerosol nitrate was found. Key factors of local aqSOA production include air mass stagnation, formation of local nitrate overnight, and significant amounts of ammonia.
Luping Su, Edward G. Patton, Jordi Vilà-Guerau de Arellano, Alex B. Guenther, Lisa Kaser, Bin Yuan, Fulizi Xiong, Paul B. Shepson, Li Zhang, David O. Miller, William H. Brune, Karsten Baumann, Eric Edgerton, Andrew Weinheimer, Pawel K. Misztal, Jeong-Hoo Park, Allen H. Goldstein, Kate M. Skog, Frank N. Keutsch, and John E. Mak
Atmos. Chem. Phys., 16, 7725–7741, https://doi.org/10.5194/acp-16-7725-2016, https://doi.org/10.5194/acp-16-7725-2016, 2016
Markus Müller, Bruce E. Anderson, Andreas J. Beyersdorf, James H. Crawford, Glenn S. Diskin, Philipp Eichler, Alan Fried, Frank N. Keutsch, Tomas Mikoviny, Kenneth L. Thornhill, James G. Walega, Andrew J. Weinheimer, Melissa Yang, Robert J. Yokelson, and Armin Wisthaler
Atmos. Chem. Phys., 16, 3813–3824, https://doi.org/10.5194/acp-16-3813-2016, https://doi.org/10.5194/acp-16-3813-2016, 2016
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Atmospheric emissions from small forest fires and their impact on regional air quality are still poorly characterized. We used an instrumented NASA P-3B aircraft to study emissions from a small forest understory fire in Georgia (USA) and to investigate chemical transformations in the fire plume in the 1 h downwind region. A state-of-the-art chemical model was able to accurately simulate key chemical processes in the aging plume.
G. M. Wolfe, J. Kaiser, T. F. Hanisco, F. N. Keutsch, J. A. de Gouw, J. B. Gilman, M. Graus, C. D. Hatch, J. Holloway, L. W. Horowitz, B. H. Lee, B. M. Lerner, F. Lopez-Hilifiker, J. Mao, M. R. Marvin, J. Peischl, I. B. Pollack, J. M. Roberts, T. B. Ryerson, J. A. Thornton, P. R. Veres, and C. Warneke
Atmos. Chem. Phys., 16, 2597–2610, https://doi.org/10.5194/acp-16-2597-2016, https://doi.org/10.5194/acp-16-2597-2016, 2016
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This study uses airborne trace gas observations acquired over the southeast US to examine how both natural (isoprene) and anthropogenic (NOx) emissions influence the production of formaldehyde (HCHO). We find a 3-fold increase in HCHO yield between rural and polluted environments. State-of-the-science chemical mechanisms are generally able to reproduce this behavior. These results add confidence to global hydrocarbon emission inventories constrained by spaceborne HCHO observations.
J. Kaiser, G. M. Wolfe, K. E. Min, S. S. Brown, C. C. Miller, D. J. Jacob, J. A. deGouw, M. Graus, T. F. Hanisco, J. Holloway, J. Peischl, I. B. Pollack, T. B. Ryerson, C. Warneke, R. A. Washenfelder, and F. N. Keutsch
Atmos. Chem. Phys., 15, 7571–7583, https://doi.org/10.5194/acp-15-7571-2015, https://doi.org/10.5194/acp-15-7571-2015, 2015
R. Thalman, M. T. Baeza-Romero, S. M. Ball, E. Borrás, M. J. S. Daniels, I. C. A. Goodall, S. B. Henry, T. Karl, F. N. Keutsch, S. Kim, J. Mak, P. S. Monks, A. Muñoz, J. Orlando, S. Peppe, A. R. Rickard, M. Ródenas, P. Sánchez, R. Seco, L. Su, G. Tyndall, M. Vázquez, T. Vera, E. Waxman, and R. Volkamer
Atmos. Meas. Tech., 8, 1835–1862, https://doi.org/10.5194/amt-8-1835-2015, https://doi.org/10.5194/amt-8-1835-2015, 2015
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Measurements of α-dicarbonyl compounds, like glyoxal (CHOCHO) and methyl glyoxal (CH3C(O)CHO), are informative about the rate of hydrocarbon oxidation, oxidative capacity, and secondary organic aerosol (SOA) formation in the atmosphere. We have compared nine instruments and seven techniques to measure α-dicarbonyl, using simulation chamber facilities in the US and Europe. We assess our understanding of calibration, precision, accuracy and detection limits, as well as possible sampling biases.
J. Kaiser, G. M. Wolfe, B. Bohn, S. Broch, H. Fuchs, L. N. Ganzeveld, S. Gomm, R. Häseler, A. Hofzumahaus, F. Holland, J. Jäger, X. Li, I. Lohse, K. Lu, A. S. H. Prévôt, F. Rohrer, R. Wegener, R. Wolf, T. F. Mentel, A. Kiendler-Scharr, A. Wahner, and F. N. Keutsch
Atmos. Chem. Phys., 15, 1289–1298, https://doi.org/10.5194/acp-15-1289-2015, https://doi.org/10.5194/acp-15-1289-2015, 2015
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Using measurements acquired from a Zeppelin airship during the PEGASOS 2012 campaign, we show that VOC oxidation alone cannot account for the formaldehyde concentrations observed in the morning over rural Italy. Vertical profiles suggest a ground-level source of HCHO. Incorporating this additional HCHO source into a photochemical model increases calculated O3 production by as much as 12%.
T. B. Nguyen, J. D. Crounse, R. H. Schwantes, A. P. Teng, K. H. Bates, X. Zhang, J. M. St. Clair, W. H. Brune, G. S. Tyndall, F. N. Keutsch, J. H. Seinfeld, and P. O. Wennberg
Atmos. Chem. Phys., 14, 13531–13549, https://doi.org/10.5194/acp-14-13531-2014, https://doi.org/10.5194/acp-14-13531-2014, 2014
J. Ortega, A. Turnipseed, A. B. Guenther, T. G. Karl, D. A. Day, D. Gochis, J. A. Huffman, A. J. Prenni, E. J. T. Levin, S. M. Kreidenweis, P. J. DeMott, Y. Tobo, E. G. Patton, A. Hodzic, Y. Y. Cui, P. C. Harley, R. S. Hornbrook, E. C. Apel, R. K. Monson, A. S. D. Eller, J. P. Greenberg, M. C. Barth, P. Campuzano-Jost, B. B. Palm, J. L. Jimenez, A. C. Aiken, M. K. Dubey, C. Geron, J. Offenberg, M. G. Ryan, P. J. Fornwalt, S. C. Pryor, F. N. Keutsch, J. P. DiGangi, A. W. H. Chan, A. H. Goldstein, G. M. Wolfe, S. Kim, L. Kaser, R. Schnitzhofer, A. Hansel, C. A. Cantrell, R. L. Mauldin, and J. N. Smith
Atmos. Chem. Phys., 14, 6345–6367, https://doi.org/10.5194/acp-14-6345-2014, https://doi.org/10.5194/acp-14-6345-2014, 2014
J. Kaiser, X. Li, R. Tillmann, I. Acir, F. Holland, F. Rohrer, R. Wegener, and F. N. Keutsch
Atmos. Meas. Tech., 7, 1571–1580, https://doi.org/10.5194/amt-7-1571-2014, https://doi.org/10.5194/amt-7-1571-2014, 2014
G. M. Wolfe, C. Cantrell, S. Kim, R. L. Mauldin III, T. Karl, P. Harley, A. Turnipseed, W. Zheng, F. Flocke, E. C. Apel, R. S. Hornbrook, S. R. Hall, K. Ullmann, S. B. Henry, J. P. DiGangi, E. S. Boyle, L. Kaser, R. Schnitzhofer, A. Hansel, M. Graus, Y. Nakashima, Y. Kajii, A. Guenther, and F. N. Keutsch
Atmos. Chem. Phys., 14, 4715–4732, https://doi.org/10.5194/acp-14-4715-2014, https://doi.org/10.5194/acp-14-4715-2014, 2014
T. B. Nguyen, M. M. Coggon, K. H. Bates, X. Zhang, R. H. Schwantes, K. A. Schilling, C. L. Loza, R. C. Flagan, P. O. Wennberg, and J. H. Seinfeld
Atmos. Chem. Phys., 14, 3497–3510, https://doi.org/10.5194/acp-14-3497-2014, https://doi.org/10.5194/acp-14-3497-2014, 2014
L. Kaser, T. Karl, A. Guenther, M. Graus, R. Schnitzhofer, A. Turnipseed, L. Fischer, P. Harley, M. Madronich, D. Gochis, F. N. Keutsch, and A. Hansel
Atmos. Chem. Phys., 13, 11935–11947, https://doi.org/10.5194/acp-13-11935-2013, https://doi.org/10.5194/acp-13-11935-2013, 2013
S. Kundu, T. A. Quraishi, G. Yu, C. Suarez, F. N. Keutsch, and E. A. Stone
Atmos. Chem. Phys., 13, 4865–4875, https://doi.org/10.5194/acp-13-4865-2013, https://doi.org/10.5194/acp-13-4865-2013, 2013
Related subject area
Subject: Clouds and Precipitation | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Retention of α-pinene oxidation products and nitro-aromatic compounds during riming
Direct formation of HONO through aqueous-phase photolysis of organic nitrates
On the importance of multiphase photolysis of organic nitrates on their global atmospheric removal
Effects of pH and light exposure on the survival of bacteria and their ability to biodegrade organic compounds in clouds: implications for microbial activity in acidic cloud water
On the importance of atmospheric loss of organic nitrates by aqueous-phase ●OH oxidation
Lignin's ability to nucleate ice via immersion freezing and its stability towards physicochemical treatments and atmospheric processing
Biodegradation of phenol and catechol in cloud water: comparison to chemical oxidation in the atmospheric multiphase system
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 2: Quartz and amorphous silica
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 3: Aluminosilicates
Aqueous reactions of organic triplet excited states with atmospheric alkenes
The quasi-liquid layer of ice revisited: the role of temperature gradients and tip chemistry in AFM studies
Ice nucleation activity of silicates and aluminosilicates in pure water and aqueous solutions – Part 1: The K-feldspar microcline
Direct molecular-level characterization of different heterogeneous freezing modes on mica – Part 1
Chemistry of riming: the retention of organic and inorganic atmospheric trace constituents
Surface-charge-induced orientation of interfacial water suppresses heterogeneous ice nucleation on α-alumina (0001)
Screening of cloud microorganisms isolated at the Puy de Dôme (France) station for the production of biosurfactants
Comparing contact and immersion freezing from continuous flow diffusion chambers
A better understanding of hydroxyl radical photochemical sources in cloud waters collected at the puy de Dôme station – experimental versus modelled formation rates
Deposition and immersion-mode nucleation of ice by three distinct samples of volcanic ash
Organic matter matters for ice nuclei of agricultural soil origin
Effect of atmospheric organic complexation on iron-bearing dust solubility
Are sesquiterpenes a good source of secondary organic cloud condensation nuclei (CCN)? Revisiting β-caryophyllene CCN
Ice nucleation efficiency of clay minerals in the immersion mode
Atmospheric chemistry of carboxylic acids: microbial implication versus photochemistry
Yields of hydrogen peroxide from the reaction of hydroxyl radical with organic compounds in solution and ice
In-cloud processes of methacrolein under simulated conditions – Part 1: Aqueous phase photooxidation
In-cloud processes of methacrolein under simulated conditions – Part 2: Formation of secondary organic aerosol
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Juan Miguel González-Sánchez, Miquel Huix-Rotllant, Nicolas Brun, Julien Morin, Carine Demelas, Amandine Durand, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 15135–15147, https://doi.org/10.5194/acp-23-15135-2023, https://doi.org/10.5194/acp-23-15135-2023, 2023
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Organic nitrates play a crucial role in air pollution, as they are nitrogen oxide (NOx) reservoirs. This work investigated the reaction products and mechanisms of their reactivity with light in the aqueous phase (cloud and fog conditions and wet aerosol). Our findings reveal that this chemistry leads to the formation of atmospheric nitrous acid (HONO).
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 5851–5866, https://doi.org/10.5194/acp-23-5851-2023, https://doi.org/10.5194/acp-23-5851-2023, 2023
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Organic nitrates play a crucial role in air pollution, as they are NOx reservoirs. This work investigated for the first time their reactivity with light in the aqueous phase (cloud and fog and wet aerosol), proving it slower than in the gas phase. Therefore, our findings reveal that partitioning of organic nitrates in the aqueous phase leads to longer atmospheric lifetimes of these compounds and thus a broader spatial distribution of their related pollution.
Yushuo Liu, Chee Kent Lim, Zhiyong Shen, Patrick K. H. Lee, and Theodora Nah
Atmos. Chem. Phys., 23, 1731–1747, https://doi.org/10.5194/acp-23-1731-2023, https://doi.org/10.5194/acp-23-1731-2023, 2023
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We investigated how cloud water pH and solar radiation impact the survival and energetic metabolism of two neutrophilic bacteria species and their biodegradation of organic acids. Experiments were performed using artificial cloud water that mimicked the pH and composition of cloud water in South China. We found that there is a minimum cloud water pH threshold at which neutrophilic bacteria will survive and biodegrade organic compounds in cloud water during the daytime and/or nighttime.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
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Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Sophie Bogler and Nadine Borduas-Dedekind
Atmos. Chem. Phys., 20, 14509–14522, https://doi.org/10.5194/acp-20-14509-2020, https://doi.org/10.5194/acp-20-14509-2020, 2020
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To study the role of organic matter in ice crystal formation, we investigated the ice nucleation ability of a subcomponent of organic aerosols, the biopolymer lignin, using a droplet-freezing technique. We found that lignin is an ice-active macromolecule with changing abilities based on dilutions. The effects of atmospheric processing and of physicochemical treatments on the ability of lignin solutions to freeze were negligible. Thus, lignin is a recalcitrant ice-nucleating macromolecule.
Saly Jaber, Audrey Lallement, Martine Sancelme, Martin Leremboure, Gilles Mailhot, Barbara Ervens, and Anne-Marie Delort
Atmos. Chem. Phys., 20, 4987–4997, https://doi.org/10.5194/acp-20-4987-2020, https://doi.org/10.5194/acp-20-4987-2020, 2020
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Current atmospheric multiphase models do not include biotransformations of organic compounds by bacteria, although many previous studies of our and other research groups have shown microbial activity in cloud water. The current lab/model study shows that for water-soluble aromatic compounds, biodegradation by bacteria may be as efficient as chemical reactions in cloud water.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6035–6058, https://doi.org/10.5194/acp-19-6035-2019, https://doi.org/10.5194/acp-19-6035-2019, 2019
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This paper not only interests the atmospheric science community but has a potential to cater to a broader audience. We discuss both long- and
short-term effects of various
atmospherically relevantchemical species on a fairly abundant mineral surface
Quartz. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Anand Kumar, Claudia Marcolli, and Thomas Peter
Atmos. Chem. Phys., 19, 6059–6084, https://doi.org/10.5194/acp-19-6059-2019, https://doi.org/10.5194/acp-19-6059-2019, 2019
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This paper not only interests the Atmospheric Science community but has a potential to cater to a broader audience. We discuss both long- and short-term effects of various
atmospherically relevantchemical species on fairly abundant mineral surfaces like feldspars and clays. We of course discuss these chemical interactions from the perspective of fate of airborne mineral dust but the same interactions could be interesting for studies on minerals at the ground level.
Richie Kaur, Brandi M. Hudson, Joseph Draper, Dean J. Tantillo, and Cort Anastasio
Atmos. Chem. Phys., 19, 5021–5032, https://doi.org/10.5194/acp-19-5021-2019, https://doi.org/10.5194/acp-19-5021-2019, 2019
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Organic triplets are an important class of aqueous photooxidants, but little is known about their reactions with most atmospheric organic compounds. We measured the reaction rate constants of a model triplet with 17 aliphatic alkenes; using their correlation with oxidation potential, we predicted rate constants for some atmospherically relevant alkenes. Depending on their reactivities, triplets can be minor to important sinks for isoprene- and limonene-derived alkenes in cloud or fog drops.
Julián Gelman Constantin, Melisa M. Gianetti, María P. Longinotti, and Horacio R. Corti
Atmos. Chem. Phys., 18, 14965–14978, https://doi.org/10.5194/acp-18-14965-2018, https://doi.org/10.5194/acp-18-14965-2018, 2018
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Numerous studies have shown that ice surface is actually coated by a thin layer of water even for temperatures below melting temperature. This quasi-liquid layer is relevant in the atmospheric chemistry of clouds, polar regions, glaciers, and other cold regions. We present new results of atomic force microscopy on pure ice, which suggests a thickness for this layer below 1 nm between -7 ºC and -2 ºC. We propose that in many cases previous authors have overestimated this thickness.
Anand Kumar, Claudia Marcolli, Beiping Luo, and Thomas Peter
Atmos. Chem. Phys., 18, 7057–7079, https://doi.org/10.5194/acp-18-7057-2018, https://doi.org/10.5194/acp-18-7057-2018, 2018
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We have performed immersion freezing experiments with microcline (most active ice nucleation, IN, K-feldspar polymorph) and investigated the effect of ammonium and non-ammonium solutes on its IN efficiency. We report increased IN efficiency of microcline in dilute ammonia- or ammonium-containing solutions, which opens up a pathway for condensation freezing occurring at a warmer temperature than immersion freezing.
Ahmed Abdelmonem
Atmos. Chem. Phys., 17, 10733–10741, https://doi.org/10.5194/acp-17-10733-2017, https://doi.org/10.5194/acp-17-10733-2017, 2017
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On the basis of supercooled SHG spectroscopy, I report molecular-level evidence for the existence of one- and two-step deposition freezing depending on the surface type and the supersaturation conditions. In addition, immersion freezing shows a transient ice phase with a lifetime of c. 1 min. This study provides new insights into atmospheric processes and can impact various industrial and research branches, particularly climate change, weather modification, and tracing water in the hydrosphere.
Alexander Jost, Miklós Szakáll, Karoline Diehl, Subir K. Mitra, and Stephan Borrmann
Atmos. Chem. Phys., 17, 9717–9732, https://doi.org/10.5194/acp-17-9717-2017, https://doi.org/10.5194/acp-17-9717-2017, 2017
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During riming of graupel and hail, soluble chemical trace constituents contained in the liquid droplets could be retained while freezing onto the glaciated particle, or released back to the air potentially at other altitudes as retained. Quantification of retention constitutes a major uncertainty in numerical models for atmospheric chemistry and improvements hinge upon experimental determination of retention for carboxylic acids, aldehydes, SO2, H2O2, NH2, and others, as presented in this paper.
Ahmed Abdelmonem, Ellen H. G. Backus, Nadine Hoffmann, M. Alejandra Sánchez, Jenée D. Cyran, Alexei Kiselev, and Mischa Bonn
Atmos. Chem. Phys., 17, 7827–7837, https://doi.org/10.5194/acp-17-7827-2017, https://doi.org/10.5194/acp-17-7827-2017, 2017
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We report the effect of surface charge on heterogeneous immersion freezing for the atmospherically relevant sapphire surface. Combining linear and nonlinear optical techniques and investigating isolated drops, we find that charge-induced surface templating is detrimental for ice nucleation on α-alumina surface. This study provides new insights into atmospheric processes and can impact various industrial and research branches, particularly climate change and tracing of water in the hydrosphere.
Pascal Renard, Isabelle Canet, Martine Sancelme, Nolwenn Wirgot, Laurent Deguillaume, and Anne-Marie Delort
Atmos. Chem. Phys., 16, 12347–12358, https://doi.org/10.5194/acp-16-12347-2016, https://doi.org/10.5194/acp-16-12347-2016, 2016
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A total of 480 microorganisms collected from 39 clouds sampled in France were isolated and identified. This unique collection was screened for biosurfactant production by measuring the surface tension. 41 % of the tested strains were active producers. Pseudomonas, the most frequently detected genus in clouds, was the dominant group for the production of biosurfactants. Further, the potential impact of the production of biosurfactants by cloud microorganisms on atmospheric processes is discussed.
Baban Nagare, Claudia Marcolli, André Welti, Olaf Stetzer, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 8899–8914, https://doi.org/10.5194/acp-16-8899-2016, https://doi.org/10.5194/acp-16-8899-2016, 2016
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The relative importance of contact freezing and immersion freezing at mixed-phase cloud temperatures is the subject of debate. We performed experiments using continuous-flow diffusion chambers to compare the freezing efficiency of ice-nucleating particles for both these nucleation modes. Silver iodide, kaolinite and Arizona Test Dust were used as ice-nucleating particles. We could not confirm the dominance of contact freezing over immersion freezing for our experimental conditions.
A. Bianco, M. Passananti, H. Perroux, G. Voyard, C. Mouchel-Vallon, N. Chaumerliac, G. Mailhot, L. Deguillaume, and M. Brigante
Atmos. Chem. Phys., 15, 9191–9202, https://doi.org/10.5194/acp-15-9191-2015, https://doi.org/10.5194/acp-15-9191-2015, 2015
G. P. Schill, K. Genareau, and M. A. Tolbert
Atmos. Chem. Phys., 15, 7523–7536, https://doi.org/10.5194/acp-15-7523-2015, https://doi.org/10.5194/acp-15-7523-2015, 2015
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Fine volcanic ash can influence cloud glaciation and, therefore, global climate. In this work we examined the heterogeneous ice nucleation properties of three distinct types of volcanic ash. We find that, in contrast to previous studies, these volcanic ash samples have different ice nucleation properties in the immersion mode. In the deposition mode, however, they nucleate ice with similar efficiency. We show that this behavior may be due to their mineralogy.
Y. Tobo, P. J. DeMott, T. C. J. Hill, A. J. Prenni, N. G. Swoboda-Colberg, G. D. Franc, and S. M. Kreidenweis
Atmos. Chem. Phys., 14, 8521–8531, https://doi.org/10.5194/acp-14-8521-2014, https://doi.org/10.5194/acp-14-8521-2014, 2014
R. Paris and K. V. Desboeufs
Atmos. Chem. Phys., 13, 4895–4905, https://doi.org/10.5194/acp-13-4895-2013, https://doi.org/10.5194/acp-13-4895-2013, 2013
X. Tang, D. R. Cocker III, and A. Asa-Awuku
Atmos. Chem. Phys., 12, 8377–8388, https://doi.org/10.5194/acp-12-8377-2012, https://doi.org/10.5194/acp-12-8377-2012, 2012
V. Pinti, C. Marcolli, B. Zobrist, C. R. Hoyle, and T. Peter
Atmos. Chem. Phys., 12, 5859–5878, https://doi.org/10.5194/acp-12-5859-2012, https://doi.org/10.5194/acp-12-5859-2012, 2012
M. Vaïtilingom, T. Charbouillot, L. Deguillaume, R. Maisonobe, M. Parazols, P. Amato, M. Sancelme, and A.-M. Delort
Atmos. Chem. Phys., 11, 8721–8733, https://doi.org/10.5194/acp-11-8721-2011, https://doi.org/10.5194/acp-11-8721-2011, 2011
T. Hullar and C. Anastasio
Atmos. Chem. Phys., 11, 7209–7222, https://doi.org/10.5194/acp-11-7209-2011, https://doi.org/10.5194/acp-11-7209-2011, 2011
Yao Liu, I. El Haddad, M. Scarfogliero, L. Nieto-Gligorovski, B. Temime-Roussel, E. Quivet, N. Marchand, B. Picquet-Varrault, and A. Monod
Atmos. Chem. Phys., 9, 5093–5105, https://doi.org/10.5194/acp-9-5093-2009, https://doi.org/10.5194/acp-9-5093-2009, 2009
I. El Haddad, Yao Liu, L. Nieto-Gligorovski, V. Michaud, B. Temime-Roussel, E. Quivet, N. Marchand, K. Sellegri, and A. Monod
Atmos. Chem. Phys., 9, 5107–5117, https://doi.org/10.5194/acp-9-5107-2009, https://doi.org/10.5194/acp-9-5107-2009, 2009
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Short summary
We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main isomers of isoprene hydroxyl hydroperoxides, via laboratory and model analysis. Two chemical mechanism pathways are proposed and the results provide an improved understanding of the broader atmospheric chemistry and role of multifunctional organic hydroperoxides, which should be the dominant VOC oxidation products under low-NO conditions, highlighting their significant contribution to sulfate formation.
We examined the mechanism and products of oxidation of dissolved sulfur dioxide with the main...
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