Articles | Volume 16, issue 2
https://doi.org/10.5194/acp-16-703-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-703-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
21 Jan 2016
Research article |
| 21 Jan 2016
Solubility and reactivity of HNCO in water: insights into HNCO's fate in the atmosphere
N. Borduas
Department of Chemistry, University of Toronto, Toronto,
Ontario, Canada
B. Place
Department of Chemistry, University of Toronto, Toronto,
Ontario, Canada
G. R. Wentworth
Department of Chemistry, University of Toronto, Toronto,
Ontario, Canada
J. P. D. Abbatt
Department of Chemistry, University of Toronto, Toronto,
Ontario, Canada
Department of Chemistry, University of Toronto, Toronto,
Ontario, Canada
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Sophie Bogler and Nadine Borduas-Dedekind
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We present airborne trace gas measurements in the European and Canadian Arctic for July 2014 and April 2015. Based on CO and CO2 in situ data as well as 10 d kinematic back trajectories, we characterize the prevailing transport regimes and derive a tracer-based diagnostic for the determination of the polar dome boundary. Using the tracer-derived boundary, an analysis of the recent transport history of air masses within the polar dome reveals significant differences between spring and summer.
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Nadine Borduas-Dedekind, Rachele Ossola, Robert O. David, Lin S. Boynton, Vera Weichlinger, Zamin A. Kanji, and Kristopher McNeill
Atmos. Chem. Phys., 19, 12397–12412, https://doi.org/10.5194/acp-19-12397-2019, https://doi.org/10.5194/acp-19-12397-2019, 2019
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Alex K. Y. Lee, Max G. Adam, John Liggio, Shao-Meng Li, Kun Li, Megan D. Willis, Jonathan P. D. Abbatt, Travis W. Tokarek, Charles A. Odame-Ankrah, Hans D. Osthoff, Kevin Strawbridge, and Jeffery R. Brook
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Erin E. McDuffie, Caroline C. Womack, Dorothy L. Fibiger, William P. Dube, Alessandro Franchin, Ann M. Middlebrook, Lexie Goldberger, Ben H. Lee, Joel A. Thornton, Alexander Moravek, Jennifer G. Murphy, Munkhbayar Baasandorj, and Steven S. Brown
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The ocean is a source of atmospheric ice-nucleating particles (INPs). In this study we compared INPs measured in microlayer and bulk seawater in the Canadian Arctic in 2016 to those measured in 2014. A strong negative correlation between salinity and freezing temperatures was observed, possibly due to INPs associated with melting sea ice. In addition, although spatial patterns of INPs and salinities were similar in 2014 and 2016, the concentrations of INPs were on average higher in 2016.
Betty Croft, Randall V. Martin, W. Richard Leaitch, Julia Burkart, Rachel Y.-W. Chang, Douglas B. Collins, Patrick L. Hayes, Anna L. Hodshire, Lin Huang, John K. Kodros, Alexander Moravek, Emma L. Mungall, Jennifer G. Murphy, Sangeeta Sharma, Samantha Tremblay, Gregory R. Wentworth, Megan D. Willis, Jonathan P. D. Abbatt, and Jeffrey R. Pierce
Atmos. Chem. Phys., 19, 2787–2812, https://doi.org/10.5194/acp-19-2787-2019, https://doi.org/10.5194/acp-19-2787-2019, 2019
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Summertime Arctic atmospheric aerosols are strongly controlled by processes related to natural regional sources. We use a chemical transport model with size-resolved aerosol microphysics to interpret measurements made during summertime 2016 in the Canadian Arctic Archipelago. Our results explore the processes that control summertime aerosol size distributions and support a climate-relevant role for Arctic marine secondary organic aerosol formed from precursor vapors with Arctic marine sources.
Jonathan P. D. Abbatt, W. Richard Leaitch, Amir A. Aliabadi, Allan K. Bertram, Jean-Pierre Blanchet, Aude Boivin-Rioux, Heiko Bozem, Julia Burkart, Rachel Y. W. Chang, Joannie Charette, Jai P. Chaubey, Robert J. Christensen, Ana Cirisan, Douglas B. Collins, Betty Croft, Joelle Dionne, Greg J. Evans, Christopher G. Fletcher, Martí Galí, Roya Ghahreman, Eric Girard, Wanmin Gong, Michel Gosselin, Margaux Gourdal, Sarah J. Hanna, Hakase Hayashida, Andreas B. Herber, Sareh Hesaraki, Peter Hoor, Lin Huang, Rachel Hussherr, Victoria E. Irish, Setigui A. Keita, John K. Kodros, Franziska Köllner, Felicia Kolonjari, Daniel Kunkel, Luis A. Ladino, Kathy Law, Maurice Levasseur, Quentin Libois, John Liggio, Martine Lizotte, Katrina M. Macdonald, Rashed Mahmood, Randall V. Martin, Ryan H. Mason, Lisa A. Miller, Alexander Moravek, Eric Mortenson, Emma L. Mungall, Jennifer G. Murphy, Maryam Namazi, Ann-Lise Norman, Norman T. O'Neill, Jeffrey R. Pierce, Lynn M. Russell, Johannes Schneider, Hannes Schulz, Sangeeta Sharma, Meng Si, Ralf M. Staebler, Nadja S. Steiner, Jennie L. Thomas, Knut von Salzen, Jeremy J. B. Wentzell, Megan D. Willis, Gregory R. Wentworth, Jun-Wei Xu, and Jacqueline D. Yakobi-Hancock
Atmos. Chem. Phys., 19, 2527–2560, https://doi.org/10.5194/acp-19-2527-2019, https://doi.org/10.5194/acp-19-2527-2019, 2019
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The Arctic is experiencing considerable environmental change with climate warming, illustrated by the dramatic decrease in sea-ice extent. It is important to understand both the natural and perturbed Arctic systems to gain a better understanding of how they will change in the future. This paper summarizes new insights into the relationships between Arctic aerosol particles and climate, as learned over the past five or so years by a large Canadian research consortium, NETCARE.
Hannes Schulz, Marco Zanatta, Heiko Bozem, W. Richard Leaitch, Andreas B. Herber, Julia Burkart, Megan D. Willis, Daniel Kunkel, Peter M. Hoor, Jonathan P. D. Abbatt, and Rüdiger Gerdes
Atmos. Chem. Phys., 19, 2361–2384, https://doi.org/10.5194/acp-19-2361-2019, https://doi.org/10.5194/acp-19-2361-2019, 2019
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Aircraft vertical profiles of black carbon (BC) aerosol from the High Canadian Arctic have shown systematic variability in different levels of the cold, stably stratified polar dome. During spring and summer, efficiencies of BC supply by transport (often from gas flaring and wildfire-affected regions) were different in the lower dome than at higher levels, as apparent from changes in mean particle size and mixing ratios with CO. Summer BC concentrations were a factor of 10 lower than in spring.
Xiaoxiao Li, Sabrina Chee, Jiming Hao, Jonathan P. D. Abbatt, Jingkun Jiang, and James N. Smith
Atmos. Chem. Phys., 19, 1555–1570, https://doi.org/10.5194/acp-19-1555-2019, https://doi.org/10.5194/acp-19-1555-2019, 2019
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We performed lab experiments to explore the role of relative humidity, RH, in atmospheric monoterpene oxidation and new particle formation. These studies will provide insights into the most important steps in the process, while also more accurately representing the real atmosphere. We found that the detected compounds did not change with RH, and in fact could mostly be fully explained by the autoxidation of organic peroxy radicals followed by bimolecular reactions with other peroxy radicals.
Victoria E. Irish, Sarah J. Hanna, Megan D. Willis, Swarup China, Jennie L. Thomas, Jeremy J. B. Wentzell, Ana Cirisan, Meng Si, W. Richard Leaitch, Jennifer G. Murphy, Jonathan P. D. Abbatt, Alexander Laskin, Eric Girard, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1027–1039, https://doi.org/10.5194/acp-19-1027-2019, https://doi.org/10.5194/acp-19-1027-2019, 2019
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Ice nucleating particles (INPs) are atmospheric particles that catalyse the formation of ice crystals in clouds. INPs influence the Earth's radiative balance and hydrological cycle. In this study we measured the concentrations of INPs in the Canadian Arctic marine boundary layer. Average INP concentrations fell within the range measured in other marine boundary layer locations. We also found that mineral dust is a more important contributor to the INP population than sea spray aerosol.
Megan D. Willis, Heiko Bozem, Daniel Kunkel, Alex K. Y. Lee, Hannes Schulz, Julia Burkart, Amir A. Aliabadi, Andreas B. Herber, W. Richard Leaitch, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 19, 57–76, https://doi.org/10.5194/acp-19-57-2019, https://doi.org/10.5194/acp-19-57-2019, 2019
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The vertical distribution of Arctic aerosol is an important driver of its climate impacts. We present vertically resolved measurements of aerosol composition and properties made in the High Arctic during spring on an aircraft platform. We explore how aerosol properties are related to transport history and show evidence of vertical trends in aerosol sources, transport mechanisms and composition. These results will help us to better understand aerosol–climate interactions in the Arctic.
Travis W. Tokarek, Charles A. Odame-Ankrah, Jennifer A. Huo, Robert McLaren, Alex K. Y. Lee, Max G. Adam, Megan D. Willis, Jonathan P. D. Abbatt, Cristian Mihele, Andrea Darlington, Richard L. Mittermeier, Kevin Strawbridge, Katherine L. Hayden, Jason S. Olfert, Elijah G. Schnitzler, Duncan K. Brownsey, Faisal V. Assad, Gregory R. Wentworth, Alex G. Tevlin, Douglas E. J. Worthy, Shao-Meng Li, John Liggio, Jeffrey R. Brook, and Hans D. Osthoff
Atmos. Chem. Phys., 18, 17819–17841, https://doi.org/10.5194/acp-18-17819-2018, https://doi.org/10.5194/acp-18-17819-2018, 2018
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Measurements of air pollutants at a ground site near Fort McKay in the Athabasca oil sands region in the summer of 2013 are presented. A large number of intermediate-volatility organic compounds (IVOCs) were observed; these molecules were shown previously to generate atmospheric particles downwind of the region. A principal component analysis was performed to identify major pollution source types, including which source(s) is(are) associated with IVOC emissions (e.g., freshly mined bitumen).
Alessandro Franchin, Dorothy L. Fibiger, Lexie Goldberger, Erin E. McDuffie, Alexander Moravek, Caroline C. Womack, Erik T. Crosman, Kenneth S. Docherty, William P. Dube, Sebastian W. Hoch, Ben H. Lee, Russell Long, Jennifer G. Murphy, Joel A. Thornton, Steven S. Brown, Munkhbayar Baasandorj, and Ann M. Middlebrook
Atmos. Chem. Phys., 18, 17259–17276, https://doi.org/10.5194/acp-18-17259-2018, https://doi.org/10.5194/acp-18-17259-2018, 2018
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We present the results of aerosol and trace gas measurements from airborne and ground-based platforms. The measurements took place in January–February 2017 in northern Utah as part of the Utah Winter Fine Particulate Study (UWFPS). We characterized the chemical composition of PM1 on a regional scale, also probing the vertical dimension. We used a thermodynamic model to study the effectiveness of limiting total ammonium or total nitrate as a strategy to control aerosol concentrations.
Meng Si, Victoria E. Irish, Ryan H. Mason, Jesús Vergara-Temprado, Sarah J. Hanna, Luis A. Ladino, Jacqueline D. Yakobi-Hancock, Corinne L. Schiller, Jeremy J. B. Wentzell, Jonathan P. D. Abbatt, Ken S. Carslaw, Benjamin J. Murray, and Allan K. Bertram
Atmos. Chem. Phys., 18, 15669–15685, https://doi.org/10.5194/acp-18-15669-2018, https://doi.org/10.5194/acp-18-15669-2018, 2018
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Using the concentrations of ice-nucleating particles (INPs) and total aerosol particles measured at three coastal marine sites, the ice-nucleating ability of aerosol particles on a per number basis and a per surface-area basis were determined as a function of size. The ice-nucleating ability was strongly dependent on size, with larger particles being more efficient. This type of information can help determine the sources of INPs and constrain the future modelling of INPs and mixed-phase clouds.
Tracey Leah Laban, Pieter Gideon van Zyl, Johan Paul Beukes, Ville Vakkari, Kerneels Jaars, Nadine Borduas-Dedekind, Miroslav Josipovic, Anne Mee Thompson, Markku Kulmala, and Lauri Laakso
Atmos. Chem. Phys., 18, 15491–15514, https://doi.org/10.5194/acp-18-15491-2018, https://doi.org/10.5194/acp-18-15491-2018, 2018
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Surface O3 was measured at four sites in the north-eastern interior of South Africa, which revealed that O3 is a regional problem in continental South Africa, with elevated O3 levels found at rural background and industrial sites. Increased O3 concentrations were associated with high CO levels predominantly related to regional biomass burning, while the O3 production regime was established to be predominantly VOC limited. Increased O3 is associated with strong seasonality of precursor sources.
Elijah G. Schnitzler and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 18, 14539–14553, https://doi.org/10.5194/acp-18-14539-2018, https://doi.org/10.5194/acp-18-14539-2018, 2018
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Brown carbon (BrC) has significant but poorly constrained effects on climate. In this work, we investigate the effects of the OH radical on optical properties of secondary BrC in a series of smog chamber experiments. At high relative humidity (RH), we find that the evolution of the particles is complex, exhibiting rapid absorption enhancement followed by slow bleaching. At low RH, bleaching does not occur. These results further our understanding of the highly variable evolution of ambient BrC.
John K. Kodros, Sarah J. Hanna, Allan K. Bertram, W. Richard Leaitch, Hannes Schulz, Andreas B. Herber, Marco Zanatta, Julia Burkart, Megan D. Willis, Jonathan P. D. Abbatt, and Jeffrey R. Pierce
Atmos. Chem. Phys., 18, 11345–11361, https://doi.org/10.5194/acp-18-11345-2018, https://doi.org/10.5194/acp-18-11345-2018, 2018
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The mixing state of black carbon is one of the key uncertainties limiting the ability of models to estimate the direct radiative effect. In this work, we present aircraft measurements from the Canadian Arctic of coating thickness as a function of black carbon core diameter and black-carbon-containing particle number fractions. We use these measurements to inform estimates of the direct radiative effect in Arctic aerosol simulations.
Emma L. Mungall, Jonathan P. D. Abbatt, Jeremy J. B. Wentzell, Gregory R. Wentworth, Jennifer G. Murphy, Daniel Kunkel, Ellen Gute, David W. Tarasick, Sangeeta Sharma, Christopher J. Cox, Taneil Uttal, and John Liggio
Atmos. Chem. Phys., 18, 10237–10254, https://doi.org/10.5194/acp-18-10237-2018, https://doi.org/10.5194/acp-18-10237-2018, 2018
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We measured gas-phase formic and acetic acid at Alert, Nunavut. These acids play an important role in cloud water acidity in remote environments, yet they are not well represented in chemical transport models, particularly in the Arctic. We observed high levels of formic and acetic acid under both cold, wet, and cloudy and warm, sunny, and dry conditions, suggesting that multiple sources significantly contribute to gas-phase concentrations of these species in the summer Arctic.
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
Jianhuai Ye, Jonathan P. D. Abbatt, and Arthur W. H. Chan
Atmos. Chem. Phys., 18, 5549–5565, https://doi.org/10.5194/acp-18-5549-2018, https://doi.org/10.5194/acp-18-5549-2018, 2018
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Synergistic effects between SOA formation and SO2 oxidation through Criegee chemistry and reactive uptake by organic peroxides were observed. The relative importance of these two pathways (Criegee vs. peroxide) varies with relative humidity. The latter SO2 loss mechanism to organic peroxides in SOA has not previously been identified. Our results suggest a new pathway of atmospheric SO2 oxidation, which may contribute to the missing mechanisms of high-sulfate production in the polluted areas.
Katrina M. Macdonald, Sangeeta Sharma, Desiree Toom, Alina Chivulescu, Andrew Platt, Mike Elsasser, Lin Huang, Richard Leaitch, Nathan Chellman, Joseph R. McConnell, Heiko Bozem, Daniel Kunkel, Ying Duan Lei, Cheol-Heon Jeong, Jonathan P. D. Abbatt, and Greg J. Evans
Atmos. Chem. Phys., 18, 3485–3503, https://doi.org/10.5194/acp-18-3485-2018, https://doi.org/10.5194/acp-18-3485-2018, 2018
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The sources of key contaminants in Arctic snow may be an important factor in understanding the rapid climate changes observed in the Arctic. Fresh snow samples collected frequently through the winter season were analyzed for major constituents. Temporally refined source apportionment via positive matrix factorization in conjunction with FLEXPART suggested potential source characteristics and locations. The identity of these sources and their relative contribution to key analytes is discussed.
Stephanie C. Pugliese, Jennifer G. Murphy, Felix R. Vogel, Michael D. Moran, Junhua Zhang, Qiong Zheng, Craig A. Stroud, Shuzhan Ren, Douglas Worthy, and Gregoire Broquet
Atmos. Chem. Phys., 18, 3387–3401, https://doi.org/10.5194/acp-18-3387-2018, https://doi.org/10.5194/acp-18-3387-2018, 2018
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We developed the Southern Ontario CO2 Emissions (SOCE) inventory, which identifies the spatial and temporal distribution (2.5 km and hourly, respectively) of CO2 emissions from seven source sectors. When the SOCE inventory was used with a chemistry transport model, we found strong agreement between modelled and measured mixing ratios. We were able to quantify that natural gas combustion contributes > 80 % of CO2 emissions at nighttime while on-road emissions contribute > 70 % during the day.
Cynthia H. Whaley, Paul A. Makar, Mark W. Shephard, Leiming Zhang, Junhua Zhang, Qiong Zheng, Ayodeji Akingunola, Gregory R. Wentworth, Jennifer G. Murphy, Shailesh K. Kharol, and Karen E. Cady-Pereira
Atmos. Chem. Phys., 18, 2011–2034, https://doi.org/10.5194/acp-18-2011-2018, https://doi.org/10.5194/acp-18-2011-2018, 2018
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Using a modified air quality forecasting model, we have found that a significant fraction (> 50 %) of ambient ammonia comes from re-emission from plants and soils in the broader Athabasca Oil Sands region and much of Alberta and Saskatchewan. We also found that about 20 % of ambient ammonia in Alberta and Saskatchewan came from forest fires in the summer of 2013. The addition of these two processes improved modelled ammonia, which was a motivating factor in undertaking this research.
Franziska Köllner, Johannes Schneider, Megan D. Willis, Thomas Klimach, Frank Helleis, Heiko Bozem, Daniel Kunkel, Peter Hoor, Julia Burkart, W. Richard Leaitch, Amir A. Aliabadi, Jonathan P. D. Abbatt, Andreas B. Herber, and Stephan Borrmann
Atmos. Chem. Phys., 17, 13747–13766, https://doi.org/10.5194/acp-17-13747-2017, https://doi.org/10.5194/acp-17-13747-2017, 2017
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We conducted aircraft-based single particle chemical composition measurements in the Canadian high Arctic during summer. Our results provide evidence for a marine-biogenic influence on secondary formation of particulate trimethylamine in the Arctic boundary layer. Understanding emission sources and further processes controlling aerosol number concentration and chemical composition in the pristine Arctic summer is crucial for modeling future climate in the area.
Douglas B. Collins, Julia Burkart, Rachel Y.-W. Chang, Martine Lizotte, Aude Boivin-Rioux, Marjolaine Blais, Emma L. Mungall, Matthew Boyer, Victoria E. Irish, Guillaume Massé, Daniel Kunkel, Jean-Éric Tremblay, Tim Papakyriakou, Allan K. Bertram, Heiko Bozem, Michel Gosselin, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 13119–13138, https://doi.org/10.5194/acp-17-13119-2017, https://doi.org/10.5194/acp-17-13119-2017, 2017
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The sources of aerosol particles and their growth to sizes large enough to act as cloud droplet seeds is of major importance to climate since clouds exert substantial control over the atmospheric energy balance. Using ship-board measurements from two summers in the Canadian Arctic, aerosol formation events were related to co-sampled atmospheric and oceanic parameters, providing insight into factors that drive particle formation and motivating further study of ocean–atmosphere interactions.
Jun-Wei Xu, Randall V. Martin, Andrew Morrow, Sangeeta Sharma, Lin Huang, W. Richard Leaitch, Julia Burkart, Hannes Schulz, Marco Zanatta, Megan D. Willis, Daven K. Henze, Colin J. Lee, Andreas B. Herber, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 11971–11989, https://doi.org/10.5194/acp-17-11971-2017, https://doi.org/10.5194/acp-17-11971-2017, 2017
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We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem model and its adjoint to attribute the sources of Arctic BC. Anthropogenic emissions in eastern and southern Asia make the largest contribution to Arctic BC. Gas flaring emissions from oilfields in western Siberia and from the Tarim oilfield in western China could have striking impacts on Arctic BC loadings.
Victoria E. Irish, Pablo Elizondo, Jessie Chen, Cédric Chou, Joannie Charette, Martine Lizotte, Luis A. Ladino, Theodore W. Wilson, Michel Gosselin, Benjamin J. Murray, Elena Polishchuk, Jonathan P. D. Abbatt, Lisa A. Miller, and Allan K. Bertram
Atmos. Chem. Phys., 17, 10583–10595, https://doi.org/10.5194/acp-17-10583-2017, https://doi.org/10.5194/acp-17-10583-2017, 2017
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The ocean is a possible source of atmospheric ice-nucleating particles (INPs). In this study we found that INPs were ubiquitous in the sea-surface microlayer and bulk seawater in the Canadian Arctic. A strong negative correlation was observed between salinity and freezing temperatures (after correcting for freezing point depression). Heat and filtration treatments of the samples showed that the INPs were likely biological material with sizes between 0.02 μm and 0.2 μm in diameter.
Katrina M. Macdonald, Sangeeta Sharma, Desiree Toom, Alina Chivulescu, Sarah Hanna, Allan K. Bertram, Andrew Platt, Mike Elsasser, Lin Huang, David Tarasick, Nathan Chellman, Joseph R. McConnell, Heiko Bozem, Daniel Kunkel, Ying Duan Lei, Greg J. Evans, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 17, 5775–5788, https://doi.org/10.5194/acp-17-5775-2017, https://doi.org/10.5194/acp-17-5775-2017, 2017
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Rapid climate changes within the Arctic have highlighted existing uncertainties in the transport of contaminants to Arctic snow. Fresh snow samples collected frequently through the winter season were analyzed for major constituents creating a unique record of Arctic snow. Comparison with simultaneous atmospheric measurements provides insight into the driving processes in the transfer of contaminants from air to snow. The relative importance of deposition mechanisms over the season is proposed.
Julia Burkart, Megan D. Willis, Heiko Bozem, Jennie L. Thomas, Kathy Law, Peter Hoor, Amir A. Aliabadi, Franziska Köllner, Johannes Schneider, Andreas Herber, Jonathan P. D. Abbatt, and W. Richard Leaitch
Atmos. Chem. Phys., 17, 5515–5535, https://doi.org/10.5194/acp-17-5515-2017, https://doi.org/10.5194/acp-17-5515-2017, 2017
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Our aircraft study for the first time systematically investigates aerosol size distributions, including ultrafine particles (5–20 nm in diameter), in the Arctic summertime atmosphere. We find that ultrafine particles occur very frequently in the boundary layer and not aloft, suggesting a surface source of these particles. Understanding aerosol properties and sources is crucial to predict climate and especially important in the Arctic as this region responds extremely fast to climate change.
Chantelle R. Lonsdale, Jennifer D. Hegarty, Karen E. Cady-Pereira, Matthew J. Alvarado, Daven K. Henze, Matthew D. Turner, Shannon L. Capps, John B. Nowak, J. Andy Neuman, Ann M. Middlebrook, Roya Bahreini, Jennifer G. Murphy, Milos Z. Markovic, Trevor C. VandenBoer, Lynn M. Russell, and Amy Jo Scarino
Atmos. Chem. Phys., 17, 2721–2739, https://doi.org/10.5194/acp-17-2721-2017, https://doi.org/10.5194/acp-17-2721-2017, 2017
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This study takes advantage of the high-resolution observations of NH3(g) made by the TES satellite instrument over Bakersfield during the CalNex campaign, along with campaign measurements, to compare CMAQ model results in the San Joaquin Valley, California. Additionally we evaluate the CMAQ bi-directional ammonia flux results using the CARB emissions inventory against these satellite and campaign measurements, not previously explored in combination.
Quentin Libois, Liviu Ivanescu, Jean-Pierre Blanchet, Hannes Schulz, Heiko Bozem, W. Richard Leaitch, Julia Burkart, Jonathan P. D. Abbatt, Andreas B. Herber, Amir A. Aliabadi, and Éric Girard
Atmos. Chem. Phys., 16, 15689–15707, https://doi.org/10.5194/acp-16-15689-2016, https://doi.org/10.5194/acp-16-15689-2016, 2016
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The first airborne measurements performed with the FIRR are presented. Vertical profiles of upwelling spectral radiance in the far-infrared are measured in the Arctic atmosphere for the first time. They show the impact of the temperature inversion on the radiative budget of the atmosphere, especially in the far-infrared. The presence of ice clouds also significantly alters the far-infrared budget, highlighting the critical interplay between water vapour and clouds in this very dry region.
W. Richard Leaitch, Alexei Korolev, Amir A. Aliabadi, Julia Burkart, Megan D. Willis, Jonathan P. D. Abbatt, Heiko Bozem, Peter Hoor, Franziska Köllner, Johannes Schneider, Andreas Herber, Christian Konrad, and Ralf Brauner
Atmos. Chem. Phys., 16, 11107–11124, https://doi.org/10.5194/acp-16-11107-2016, https://doi.org/10.5194/acp-16-11107-2016, 2016
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Thought to be mostly unimportant for summertime Arctic liquid-water clouds, airborne observations show that atmospheric aerosol particles 50 nm in diameter or smaller and most likely from natural sources are often involved in cloud formation in the pristine Arctic summer. The result expands the reference for aerosol forcing of climate. Further, for extremely low droplet concentrations, no evidence is found for a connection between cloud liquid water and aerosol particle concentrations.
Sarvesh Garimella, Thomas Bjerring Kristensen, Karolina Ignatius, Andre Welti, Jens Voigtländer, Gourihar R. Kulkarni, Frank Sagan, Gregory Lee Kok, James Dorsey, Leonid Nichman, Daniel Alexander Rothenberg, Michael Rösch, Amélie Catharina Ruth Kirchgäßner, Russell Ladkin, Heike Wex, Theodore W. Wilson, Luis Antonio Ladino, Jon P. D. Abbatt, Olaf Stetzer, Ulrike Lohmann, Frank Stratmann, and Daniel James Cziczo
Atmos. Meas. Tech., 9, 2781–2795, https://doi.org/10.5194/amt-9-2781-2016, https://doi.org/10.5194/amt-9-2781-2016, 2016
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The SPectrometer for Ice Nuclei (SPIN) is a commercially available ice nuclei counter manufactured by Droplet Measurement Technologies in Boulder, CO. This study characterizes the SPIN chamber, reporting data from laboratory measurements and quantifying uncertainties. Overall, we report that the SPIN is able to reproduce previous CFDC ice nucleation measurements.
Amir A. Aliabadi, Jennie L. Thomas, Andreas B. Herber, Ralf M. Staebler, W. Richard Leaitch, Hannes Schulz, Kathy S. Law, Louis Marelle, Julia Burkart, Megan D. Willis, Heiko Bozem, Peter M. Hoor, Franziska Köllner, Johannes Schneider, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 7899–7916, https://doi.org/10.5194/acp-16-7899-2016, https://doi.org/10.5194/acp-16-7899-2016, 2016
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For the first time, ship emissions of an ice-breaker, the Amundsen, is characterized while breaking ice in the Canadian Arctic using the plume intercepts by the Polar 6 aircraft. The study is novel, estimating lower plume expansion rates over the stable Arctic marine boundary layer and different emissions factors for oxides of nitrogen, black carbon, and carbon monoxide, compared to plume intercept studies in mid latitudes. These results can inform policy making and emission inventory datasets.
Megan D. Willis, Julia Burkart, Jennie L. Thomas, Franziska Köllner, Johannes Schneider, Heiko Bozem, Peter M. Hoor, Amir A. Aliabadi, Hannes Schulz, Andreas B. Herber, W. Richard Leaitch, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 7663–7679, https://doi.org/10.5194/acp-16-7663-2016, https://doi.org/10.5194/acp-16-7663-2016, 2016
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We present a case study focused on an aerosol growth event observed in the Canadian High Arctic during summer. Using measurements of aerosol chemical and physical properties we find evidence for aerosol growth into cloud condensation nuclei-active sizes, through marine-influenced secondary organic aerosol formation. Understanding the mechanisms that control the formation and growth of aerosol is crucial for our ability to predict cloud properties, and therefore radiative balance and climate.
Gregory R. Wentworth, Jennifer G. Murphy, Katherine B. Benedict, Evelyn J. Bangs, and Jeffrey L. Collett Jr.
Atmos. Chem. Phys., 16, 7435–7449, https://doi.org/10.5194/acp-16-7435-2016, https://doi.org/10.5194/acp-16-7435-2016, 2016
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The influence of dew on atmospheric composition is poorly understood. Results from this work show that dew can uptake a significant fraction (roughly two-thirds) of boundary layer gas-phase ammonia. Furthermore, an average of 95 % of the ammonia sequestered in dew is released back to the atmosphere the following morning during dew evaporation. Dew has the ability to affect air quality and N-deposition and should be considered when modelling ammonia concentrations, as well as other soluble gases.
Alex K. Y. Lee, Jonathan P. D. Abbatt, W. Richard Leaitch, Shao-Meng Li, Steve J. Sjostedt, Jeremy J. B. Wentzell, John Liggio, and Anne Marie Macdonald
Atmos. Chem. Phys., 16, 6721–6733, https://doi.org/10.5194/acp-16-6721-2016, https://doi.org/10.5194/acp-16-6721-2016, 2016
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Substantial biogenic secondary organic aerosol (BSOA) formation was investigated in a coniferous forest mountain region in Whistler, British Columbia. A largely biogenic aerosol growth episode was observed, providing a unique opportunity to investigate BSOA formation chemistry in a forested environment. In particular, our observations provide insights into the relative importance of different oxidation mechanisms between day and night.
Emma L. Mungall, Betty Croft, Martine Lizotte, Jennie L. Thomas, Jennifer G. Murphy, Maurice Levasseur, Randall V. Martin, Jeremy J. B. Wentzell, John Liggio, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 6665–6680, https://doi.org/10.5194/acp-16-6665-2016, https://doi.org/10.5194/acp-16-6665-2016, 2016
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Previous work has suggested that marine emissions of dimethyl sulfide (DMS) could impact the Arctic climate through interactions with clouds. We made the first high-time-resolution measurements of summertime atmospheric DMS in the Canadian Arctic, and performed source sensitivity simulations. We found that regional marine sources dominated, but do not appear to be sufficient to explain our observations. Understanding DMS sources in the Arctic is necessary to model future climate in the region.
Alex K. Y. Lee, Megan D. Willis, Robert M. Healy, Jon M. Wang, Cheol-Heon Jeong, John C. Wenger, Greg J. Evans, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 5561–5572, https://doi.org/10.5194/acp-16-5561-2016, https://doi.org/10.5194/acp-16-5561-2016, 2016
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Single-particle measurements from a soot-particle aerosol mass spectrometer were performed to examine the mixing state of aerosol particles in an air mass influenced by aged biomass burning. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and potassium content, and illustrate that high molecular weight organic compounds can be a key contributor to low-volatility BrC observed in biomass burning organic aerosols.
Roya Ghahreman, Ann-Lise Norman, Jonathan P. D. Abbatt, Maurice Levasseur, and Jennie L. Thomas
Atmos. Chem. Phys., 16, 5191–5202, https://doi.org/10.5194/acp-16-5191-2016, https://doi.org/10.5194/acp-16-5191-2016, 2016
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Aerosols in six size fractions (> 0.49–7.0 microns) were collected in the Arctic (July 2014). The isotopic composition of sulfate aerosols was measured to determine the role of biogenic and anthropogenic sources in the growth of aerosols. More than 63 % of the average sulfate concentration in the fine aerosols (> 0.49 microns) was from biogenic sources. For some samples, the S isotope ratio values for SO2 and fine aerosols were close together, suggesting the same source for SO2 and aerosol sulfur.
Megan D. Willis, Robert M. Healy, Nicole Riemer, Matthew West, Jon M. Wang, Cheol-Heon Jeong, John C. Wenger, Greg J. Evans, Jonathan P. D. Abbatt, and Alex K. Y. Lee
Atmos. Chem. Phys., 16, 4693–4706, https://doi.org/10.5194/acp-16-4693-2016, https://doi.org/10.5194/acp-16-4693-2016, 2016
Gregory R. Wentworth, Jennifer G. Murphy, Betty Croft, Randall V. Martin, Jeffrey R. Pierce, Jean-Sébastien Côté, Isabelle Courchesne, Jean-Éric Tremblay, Jonathan Gagnon, Jennie L. Thomas, Sangeeta Sharma, Desiree Toom-Sauntry, Alina Chivulescu, Maurice Levasseur, and Jonathan P. D. Abbatt
Atmos. Chem. Phys., 16, 1937–1953, https://doi.org/10.5194/acp-16-1937-2016, https://doi.org/10.5194/acp-16-1937-2016, 2016
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Air near the surface in the summertime Arctic is extremely clean and typically has very low concentrations of both gases and particles. However, atmospheric measurements taken throughout the Canadian Arctic in the summer of 2014 revealed higher-than-expected amounts of gaseous ammonia. It is likely the majority of this ammonia is coming from migratory seabird colonies throughout the Arctic. Seabird guano (dung) releases ammonia which could impact climate and sensitive Arctic ecosystems.
R. H. Mason, M. Si, C. Chou, V. E. Irish, R. Dickie, P. Elizondo, R. Wong, M. Brintnell, M. Elsasser, W. M. Lassar, K. M. Pierce, W. R. Leaitch, A. M. MacDonald, A. Platt, D. Toom-Sauntry, R. Sarda-Estève, C. L. Schiller, K. J. Suski, T. C. J. Hill, J. P. D. Abbatt, J. A. Huffman, P. J. DeMott, and A. K. Bertram
Atmos. Chem. Phys., 16, 1637–1651, https://doi.org/10.5194/acp-16-1637-2016, https://doi.org/10.5194/acp-16-1637-2016, 2016
R. H. Mason, M. Si, J. Li, C. Chou, R. Dickie, D. Toom-Sauntry, C. Pöhlker, J. D. Yakobi-Hancock, L. A. Ladino, K. Jones, W. R. Leaitch, C. L. Schiller, J. P. D. Abbatt, J. A. Huffman, and A. K. Bertram
Atmos. Chem. Phys., 15, 12547–12566, https://doi.org/10.5194/acp-15-12547-2015, https://doi.org/10.5194/acp-15-12547-2015, 2015
K. M. Badali, S. Zhou, D. Aljawhary, M. Antiñolo, W. J. Chen, A. Lok, E. Mungall, J. P. S. Wong, R. Zhao, and J. P. D. Abbatt
Atmos. Chem. Phys., 15, 7831–7840, https://doi.org/10.5194/acp-15-7831-2015, https://doi.org/10.5194/acp-15-7831-2015, 2015
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This is the first paper to demonstrate that SOA material forms OH radicals upon UV illumination. We quantify the OH formation rates in solution and show species other than H2O2, mostly probably ROOH molecules, are the likely source of the OH. The importance of an OH source from SOA is that photochemical processing within both cloudwater and aerosol particles may arise subsequent to the formation of these radicals.
R. Zhao, A. K. Y. Lee, L. Huang, X. Li, F. Yang, and J. P. D. Abbatt
Atmos. Chem. Phys., 15, 6087–6100, https://doi.org/10.5194/acp-15-6087-2015, https://doi.org/10.5194/acp-15-6087-2015, 2015
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Aqueous-phase photochemical decay of light absorbing organic compounds, or atmospheric brown carbon (BrC), is investigated in this study. The absorptive change of laboratory surrogates of BrC, as well as biofuel combustion samples, were monitored during photolysis and OH oxidation experiments. The major finding is the rapid change in the absorptivity of BrC during such photochemical processing. This change should be taken into account to evaluate the importance of BrC in the atmosphere.
F. Wania, Y. D. Lei, C. Wang, J. P. D. Abbatt, and K.-U. Goss
Atmos. Chem. Phys., 15, 3395–3412, https://doi.org/10.5194/acp-15-3395-2015, https://doi.org/10.5194/acp-15-3395-2015, 2015
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The manuscript presents a new way to graphically illustrate some of the processes that occur when organic particles form in the atmosphere. In particular, this method makes it possible to see how factors such as the composition of the atmosphere and temperature affect these processes.
A. K. Y. Lee, M. D. Willis, R. M. Healy, T. B. Onasch, and J. P. D. Abbatt
Atmos. Chem. Phys., 15, 1823–1841, https://doi.org/10.5194/acp-15-1823-2015, https://doi.org/10.5194/acp-15-1823-2015, 2015
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Understanding the impact of black carbon (BC) particles on human health and radiative forcing requires knowledge of the BC mixing state. This work investigates the mixing state of BC and other aerosol species in a typical urban area using a single particle mass spectrometry technique. Our results provide quantitative insight into the physical and chemical nature of BC-containing particles near emission and can be used as a basis for our developing understanding of BC evolution in the atmosphere.
M. D. Willis, A. K. Y. Lee, T. B. Onasch, E. C. Fortner, L. R. Williams, A. T. Lambe, D. R. Worsnop, and J. P. D. Abbatt
Atmos. Meas. Tech., 7, 4507–4516, https://doi.org/10.5194/amt-7-4507-2014, https://doi.org/10.5194/amt-7-4507-2014, 2014
F. Wania, Y. D. Lei, C. Wang, J. P. D. Abbatt, and K.-U. Goss
Atmos. Chem. Phys., 14, 13189–13204, https://doi.org/10.5194/acp-14-13189-2014, https://doi.org/10.5194/acp-14-13189-2014, 2014
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A description of the formation of secondary organic aerosol requires the prediction of the partitioning equilibrium of organic compounds with multiple functional groups between gas and organic particle phase. While this is typically done by predicting both the saturation vapour pressure and the activity coefficient in the organic particle phase, we demonstrate here that it is feasible to predict the partitioning equilibrium directly. This direct approach has greater precision.
J. D. Yakobi-Hancock, L. A. Ladino, A. K. Bertram, J. A. Huffman, K. Jones, W. R. Leaitch, R. H. Mason, C. L. Schiller, D. Toom-Sauntry, J. P. S. Wong, and J. P. D. Abbatt
Atmos. Chem. Phys., 14, 12307–12317, https://doi.org/10.5194/acp-14-12307-2014, https://doi.org/10.5194/acp-14-12307-2014, 2014
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As one aspect of the NETwork on Climate and Aerosols: addressing key uncertainties in Remote Canadian Environments, measurements of the cloud condensation nucleation properties of 50 nm and 100 nm aerosol particles were conducted at Ucluelet on the west coast of Vancouver Island in August 2013. The most efficient cloud condensation nuclei arose when the organic to sulfate ratio of the aerosol was lowest and when winds arrived from the west after transport through the marine boundary layer.
G. R. Wentworth, J. G. Murphy, P. K. Gregoire, C. A. L. Cheyne, A. G. Tevlin, and R. Hems
Biogeosciences, 11, 5675–5686, https://doi.org/10.5194/bg-11-5675-2014, https://doi.org/10.5194/bg-11-5675-2014, 2014
R. Zhao, E. L. Mungall, A. K. Y. Lee, D. Aljawhary, and J. P. D. Abbatt
Atmos. Chem. Phys., 14, 9695–9706, https://doi.org/10.5194/acp-14-9695-2014, https://doi.org/10.5194/acp-14-9695-2014, 2014
S. C. Pugliese, J. G. Murphy, J. A. Geddes, and J. M. Wang
Atmos. Chem. Phys., 14, 8197–8207, https://doi.org/10.5194/acp-14-8197-2014, https://doi.org/10.5194/acp-14-8197-2014, 2014
M. L. McGuire, R. Y.-W. Chang, J. G. Slowik, C.-H. Jeong, R. M. Healy, G. Lu, C. Mihele, J. P. D. Abbatt, J. R. Brook, and G. J. Evans
Atmos. Chem. Phys., 14, 8017–8042, https://doi.org/10.5194/acp-14-8017-2014, https://doi.org/10.5194/acp-14-8017-2014, 2014
E. A. Marais, D. J. Jacob, A. Guenther, K. Chance, T. P. Kurosu, J. G. Murphy, C. E. Reeves, and H. O. T. Pye
Atmos. Chem. Phys., 14, 7693–7703, https://doi.org/10.5194/acp-14-7693-2014, https://doi.org/10.5194/acp-14-7693-2014, 2014
D. R. Gentner, T. B. Ford, A. Guha, K. Boulanger, J. Brioude, W. M. Angevine, J. A. de Gouw, C. Warneke, J. B. Gilman, T. B. Ryerson, J. Peischl, S. Meinardi, D. R. Blake, E. Atlas, W. A. Lonneman, T. E. Kleindienst, M. R. Beaver, J. M. St. Clair, P. O. Wennberg, T. C. VandenBoer, M. Z. Markovic, J. G. Murphy, R. A. Harley, and A. H. Goldstein
Atmos. Chem. Phys., 14, 4955–4978, https://doi.org/10.5194/acp-14-4955-2014, https://doi.org/10.5194/acp-14-4955-2014, 2014
J. A. Geddes and J. G. Murphy
Atmos. Chem. Phys., 14, 2939–2957, https://doi.org/10.5194/acp-14-2939-2014, https://doi.org/10.5194/acp-14-2939-2014, 2014
S. Zhou, L. Gonzalez, A. Leithead, Z. Finewax, R. Thalman, A. Vlasenko, S. Vagle, L.A. Miller, S.-M. Li, S. Bureekul, H. Furutani, M. Uematsu, R. Volkamer, and J. Abbatt
Atmos. Chem. Phys., 14, 1371–1384, https://doi.org/10.5194/acp-14-1371-2014, https://doi.org/10.5194/acp-14-1371-2014, 2014
D. Aljawhary, A. K. Y. Lee, and J. P. D. Abbatt
Atmos. Meas. Tech., 6, 3211–3224, https://doi.org/10.5194/amt-6-3211-2013, https://doi.org/10.5194/amt-6-3211-2013, 2013
J. D. Yakobi-Hancock, L. A. Ladino, and J. P. D. Abbatt
Atmos. Chem. Phys., 13, 11175–11185, https://doi.org/10.5194/acp-13-11175-2013, https://doi.org/10.5194/acp-13-11175-2013, 2013
S. N. Wren, D. J. Donaldson, and J. P. D. Abbatt
Atmos. Chem. Phys., 13, 9789–9800, https://doi.org/10.5194/acp-13-9789-2013, https://doi.org/10.5194/acp-13-9789-2013, 2013
R. D. McWhinney, S. Zhou, and J. P. D. Abbatt
Atmos. Chem. Phys., 13, 9731–9744, https://doi.org/10.5194/acp-13-9731-2013, https://doi.org/10.5194/acp-13-9731-2013, 2013
J. M. Wang, J. G. Murphy, J. A. Geddes, C. L. Winsborough, N. Basiliko, and S. C. Thomas
Biogeosciences, 10, 4371–4382, https://doi.org/10.5194/bg-10-4371-2013, https://doi.org/10.5194/bg-10-4371-2013, 2013
R. Zhao, A. K. Y. Lee, R. Soong, A. J. Simpson, and J. P. D. Abbatt
Atmos. Chem. Phys., 13, 5857–5872, https://doi.org/10.5194/acp-13-5857-2013, https://doi.org/10.5194/acp-13-5857-2013, 2013
Related subject area
Subject: Gases | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Secondary reactions of aromatics-derived oxygenated organic molecules lead to plentiful highly oxygenated organic molecules within an intraday OH exposure
Formation and temperature dependence of Highly Oxygenated Organic Molecules (HOM) from Δ3-carene ozonolysis
Impact of HO2∕RO2 ratio on highly oxygenated α-pinene photooxidation products and secondary organic aerosol formation potential
Negligible temperature dependence of the ozone–iodide reaction and implications for oceanic emissions of iodine
Extension, development, and evaluation of the representation of the OH-initiated dimethyl sulfide (DMS) oxidation mechanism in the Master Chemical Mechanism (MCM) v3.3.1 framework
Mechanistic insight into the kinetic fragmentation of Norpinonic Acid in the gas phase: An experimental and DFT study
On the potential use of highly oxygenated organic molecules (HOMs) as indicators for ozone formation sensitivity
Oxygenated organic molecules produced by low-NOx photooxidation of aromatic compounds: contributions to secondary organic aerosol and steric hindrance
Impact of temperature on the role of Criegee intermediates and peroxy radicals in dimer formation from β-pinene ozonolysis
Atmospheric impact of 2-methylpentanal emissions: kinetics, photochemistry, and formation of secondary pollutants
Technical note: Gas-phase nitrate radical generation via irradiation of aerated ceric ammonium nitrate mixtures
Direct probing of acylperoxy radicals during ozonolysis of α-pinene: constraints on radical chemistry and production of highly oxygenated organic molecules
Atmospheric photooxidation and ozonolysis of sabinene: reaction rate coefficients, product yields, and chemical budget of radicals
Compilation of Henry's law constants (version 5.0.0) for water as solvent
Measurement report: Carbonyl sulfide production during dimethyl sulfide oxidation in the atmospheric simulation chamber SAPHIR
An aldehyde as a rapid source of secondary aerosol precursors: theoretical and experimental study of hexanal autoxidation
Measuring and modeling investigation of the net photochemical ozone production rate via an improved dual-channel reaction chamber technique
Evolution of organic carbon in the laboratory oxidation of biomass-burning emissions
Atmospheric oxidation of new “green” solvents – Part 2: methyl pivalate and pinacolone
On the formation of highly oxidized pollutants by autoxidation of terpenes under low-temperature-combustion conditions: the case of limonene and α-pinene
Selective deuteration as a tool for resolving autoxidation mechanisms in α-pinene ozonolysis
Comparison of isoprene chemical mechanisms under atmospheric night-time conditions in chamber experiments: evidence of hydroperoxy aldehydes and epoxy products from NO3 oxidation
Measurement of Henry's law and liquid-phase loss rate constants of peroxypropionic nitric anhydride (PPN) in deionized water and in n-octanol
Product distribution, kinetics, and aerosol formation from the OH oxidation of dimethyl sulfide under different RO2 regimes
Atmospheric breakdown chemistry of the new “green” solvent 2,2,5,5-tetramethyloxolane via gas-phase reactions with OH and Cl radicals
Impact of cooking style and oil on semi-volatile and intermediate volatility organic compound emissions from Chinese domestic cooking
Observations of gas-phase products from the nitrate-radical-initiated oxidation of four monoterpenes
Investigation of the limonene photooxidation by OH at different NO concentrations in the atmospheric simulation chamber SAPHIR (Simulation of Atmospheric PHotochemistry In a large Reaction Chamber)
Kinetic study of the atmospheric oxidation of a series of epoxy compounds by OH radicals
An experimental study of the reactivity of terpinolene and β-caryophyllene with the nitrate radical
Oxidation product characterization from ozonolysis of the diterpene ent-kaurene
Kinetics of OH + SO2 + M: temperature-dependent rate coefficients in the fall-off regime and the influence of water vapour
Formation of organic sulfur compounds through SO2-initiated photochemistry of PAHs and dimethylsulfoxide at the air-water interface
Stable carbon isotopic composition of biomass burning emissions – implications for estimating the contribution of C3 and C4 plants
Evaluation of the daytime tropospheric loss of 2-methylbutanal
Investigations into the gas-phase photolysis and OH radical kinetics of nitrocatechols: implications of intramolecular interactions on their atmospheric behaviour
Reproducing Arctic springtime tropospheric ozone and mercury depletion events in an outdoor mesocosm sea ice facility
N2O5 uptake onto saline mineral dust: a potential missing source of tropospheric ClNO2 in inland China
NO3 chemistry of wildfire emissions: a kinetic study of the gas-phase reactions of furans with the NO3 radical
Marine gas-phase sulfur emissions during an induced phytoplankton bloom
Biomass burning plume chemistry: OH-radical-initiated oxidation of 3-penten-2-one and its main oxidation product 2-hydroxypropanal
Atmospheric photo-oxidation of myrcene: OH reaction rate constant, gas-phase oxidation products and radical budgets
Characterization of ambient volatile organic compounds, source apportionment, and the ozone–NOx–VOC sensitivities in a heavily polluted megacity of central China: effect of sporting events and emission reductions
Atmospheric oxidation of α,β-unsaturated ketones: kinetics and mechanism of the OH radical reaction
Reactions of NO3 with aromatic aldehydes: gas-phase kinetics and insights into the mechanism of the reaction
Atmospheric photooxidation and ozonolysis of Δ3-carene and 3-caronaldehyde: rate constants and product yields
Measurement report: Biogenic volatile organic compound emission profiles of rapeseed leaf litter and its secondary organic aerosol formation potential
Highly oxygenated organic molecules produced by the oxidation of benzene and toluene in a wide range of OH exposure and NOx conditions
Molecular composition and volatility of multi-generation products formed from isoprene oxidation by nitrate radical
Highly oxygenated organic molecule (HOM) formation in the isoprene oxidation by NO3 radical
Yuwei Wang, Chuang Li, Ying Zhang, Yueyang Li, Gan Yang, Xueyan Yang, Yizhen Wu, Lei Yao, Hefeng Zhang, and Lin Wang
Atmos. Chem. Phys., 24, 7961–7981, https://doi.org/10.5194/acp-24-7961-2024, https://doi.org/10.5194/acp-24-7961-2024, 2024
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The formation and evolution mechanisms of aromatics-derived highly oxygenated organic molecules (HOMs) are essential to understand the formation of secondary organic aerosol pollution. Our conclusion highlights an underappreciated formation pathway of aromatics-derived HOMs and elucidates detailed formation mechanisms of certain HOMs, which advances our understanding of HOMs and potentially explains the existing gap between model prediction and ambient measurement of the HOMs' concentrations.
Yuanyuan Luo, Ditte Thomsen, Emil Mark Iversen, Pontus Roldin, Jane Tygesen Skønager, Linjie Li, Michael Priestley, Henrik B. Pedersen, Mattias Hallquist, Merete Bilde, Marianne Glasius, and Mikael Ehn
EGUsphere, https://doi.org/10.5194/egusphere-2024-1386, https://doi.org/10.5194/egusphere-2024-1386, 2024
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∆3-carene is abundantly emitted from vegetation, but its atmospheric oxidation chemistry has received limited attention. We explored highly oxygenated organic molecules (HOM) formation from ∆3-carene ozonolysis in chambers and investigated the impact of temperature and relative humidity on HOM formation. Our findings provide new insights into ∆3-carene oxidation pathways and its potential to impact atmospheric aerosol.
Yarê Baker, Sungah Kang, Hui Wang, Rongrong Wu, Jian Xu, Annika Zanders, Quanfu He, Thorsten Hohaus, Till Ziehm, Veronica Geretti, Thomas J. Bannan, Simon P. O'Meara, Aristeidis Voliotis, Mattias Hallquist, Gordon McFiggans, Sören R. Zorn, Andreas Wahner, and Thomas F. Mentel
Atmos. Chem. Phys., 24, 4789–4807, https://doi.org/10.5194/acp-24-4789-2024, https://doi.org/10.5194/acp-24-4789-2024, 2024
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Highly oxygenated organic molecules are important contributors to secondary organic aerosol. Their yield depends on detailed atmospheric chemical composition. One important parameter is the ratio of hydroperoxy radicals to organic peroxy radicals (HO2/RO2), and we show that higher HO2/RO2 ratios lower the secondary organic aerosol yield. This is of importance as laboratory studies are often biased towards organic peroxy radicals.
Lucy V. Brown, Ryan J. Pound, Lyndsay S. Ives, Matthew R. Jones, Stephen J. Andrews, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 3905–3923, https://doi.org/10.5194/acp-24-3905-2024, https://doi.org/10.5194/acp-24-3905-2024, 2024
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Ozone is deposited from the lower atmosphere to the surface of the ocean; however, the chemical reactions which drive this deposition are currently not well understood. Of particular importance is the reaction between ozone and iodide, and this work measures the kinetics of this reaction and its temperature dependence, which we find to be negligible. We then investigate the subsequent emissions of iodine-containing species from the surface ocean, which can further impact ozone.
Lorrie Simone Denise Jacob, Chiara Giorio, and Alexander Thomas Archibald
Atmos. Chem. Phys., 24, 3329–3347, https://doi.org/10.5194/acp-24-3329-2024, https://doi.org/10.5194/acp-24-3329-2024, 2024
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Recent studies on DMS have provided new challenges to our mechanistic understanding. Here we synthesise a number of recent studies to further develop and extend a state-of-the-art mechanism. Our new mechanism is shown to outperform all existing mechanisms when compared over a wide set of conditions. The development of an improved DMS mechanism will help lead the way to better the understanding the climate impacts of DMS emissions in past, present, and future atmospheric conditions.
Izabela Kurzydym, Agata Błaziak, Kinga Podgórniak, Karol Kułacz, and Kacper Błaziak
EGUsphere, https://doi.org/10.5194/egusphere-2024-679, https://doi.org/10.5194/egusphere-2024-679, 2024
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The submitted paper outlines a unique scientific strategy for studying the reactivity of atmospherically relevant – Norpinonic Acid (NA). Publication offer a new toolbox, illustrating NA's fragmentation and kinetic degradation pattern leading to the formation of new small molecules. Furthermore, the research strategy presented here demonstrates how the Mass Spectrometer can function as a gas-phase reactor and the quantum chemistry method can serve as a reaction model builder.
Jiangyi Zhang, Jian Zhao, Yuanyuan Luo, Valter Mickwitz, Douglas Worsnop, and Mikael Ehn
Atmos. Chem. Phys., 24, 2885–2911, https://doi.org/10.5194/acp-24-2885-2024, https://doi.org/10.5194/acp-24-2885-2024, 2024
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Due to the intrinsic connection between the formation pathways of O3 and HOMs, the ratio of HOM dimers or non-nitrate monomers to HOM organic nitrates could be used to determine O3 formation regimes. Owing to the fast formation and short lifetimes of HOMs, HOM-based indicating ratios can describe O3 formation in real time. Despite the success of our approach in this simple laboratory system, applicability to the much more complex atmosphere remains to be determined.
Xi Cheng, Yong Jie Li, Yan Zheng, Keren Liao, Theodore K. Koenig, Yanli Ge, Tong Zhu, Chunxiang Ye, Xinghua Qiu, and Qi Chen
Atmos. Chem. Phys., 24, 2099–2112, https://doi.org/10.5194/acp-24-2099-2024, https://doi.org/10.5194/acp-24-2099-2024, 2024
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In this study we conducted laboratory measurements to investigate the formation of gas-phase oxygenated organic molecules (OOMs) from six aromatic volatile organic compounds (VOCs). We provide a thorough analysis on the effects of precursor structure (substituents and ring numbers) on product distribution and highlight from a laboratory perspective that heavy (e.g., double-ring) aromatic VOCs are important in initial particle growth during secondary organic aerosol formation.
Yiwei Gong, Feng Jiang, Yanxia Li, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 167–184, https://doi.org/10.5194/acp-24-167-2024, https://doi.org/10.5194/acp-24-167-2024, 2024
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This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
María Asensio, Sergio Blázquez, María Antiñolo, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 23, 14115–14126, https://doi.org/10.5194/acp-23-14115-2023, https://doi.org/10.5194/acp-23-14115-2023, 2023
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In this work, we focus on the atmospheric chemistry and consequences for air quality of 2-methylpentanal (2MP), which is widely used as a flavoring ingredient and as an intermediate in the synthesis of dyes, resins, and pharmaceuticals. Measurements are presented on how fast 2MP is degraded by sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms and what products are generated. We conclude that 2MP will be degraded in a few hours, affecting local air quality.
Andrew T. Lambe, Bin Bai, Masayuki Takeuchi, Nicole Orwat, Paul M. Zimmerman, Mitchell W. Alton, Nga L. Ng, Andrew Freedman, Megan S. Claflin, Drew R. Gentner, Douglas R. Worsnop, and Pengfei Liu
Atmos. Chem. Phys., 23, 13869–13882, https://doi.org/10.5194/acp-23-13869-2023, https://doi.org/10.5194/acp-23-13869-2023, 2023
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We developed a new method to generate nitrate radicals (NO3) for atmospheric chemistry applications that works by irradiating mixtures containing ceric ammonium nitrate with a UV light at room temperature. It has several advantages over traditional NO3 sources. We characterized its performance over a range of mixture and reactor conditions as well as other irradiation products. Proof of concept was demonstrated by generating and characterizing oxidation products of the β-pinene + NO3 reaction.
Han Zang, Dandan Huang, Jiali Zhong, Ziyue Li, Chenxi Li, Huayun Xiao, and Yue Zhao
Atmos. Chem. Phys., 23, 12691–12705, https://doi.org/10.5194/acp-23-12691-2023, https://doi.org/10.5194/acp-23-12691-2023, 2023
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Acylperoxy radicals (RO2) are key intermediates in the atmospheric oxidation of organic compounds, yet our knowledge of their identities and chemistry remains poor. Using direct measurements and kinetic modeling, we identify the composition and formation pathways of acyl RO2 and quantify their contribution to highly oxygenated organic molecules during α-pinene ozonolysis, which will help to understand oxidation chemistry of monoterpenes and sources of low-volatility organics in the atmosphere.
Jacky Y. S. Pang, Florian Berg, Anna Novelli, Birger Bohn, Michelle Färber, Philip T. M. Carlsson, René Dubus, Georgios I. Gkatzelis, Franz Rohrer, Sergej Wedel, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 12631–12649, https://doi.org/10.5194/acp-23-12631-2023, https://doi.org/10.5194/acp-23-12631-2023, 2023
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In this study, the oxidations of sabinene by OH radicals and ozone were investigated with an atmospheric simulation chamber. Reaction rate coefficients of the OH-oxidation reaction at temperatures between 284 to 340 K were determined for the first time in the laboratory by measuring the OH reactivity. Product yields determined in chamber experiments had good agreement with literature values, but discrepancies were found between experimental yields and expected yields from oxidation mechanisms.
Rolf Sander
Atmos. Chem. Phys., 23, 10901–12440, https://doi.org/10.5194/acp-23-10901-2023, https://doi.org/10.5194/acp-23-10901-2023, 2023
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According to Henry's law, the equilibrium ratio between the abundances in the gas phase and in the aqueous phase is constant for a dilute solution. Henry’s law constants of trace gases of potential importance in environmental chemistry have been collected and converted into a uniform format. The compilation contains 46 434 values of Henry's law constants for 10 173 species, collected from 995 references. It is also available on the internet at https://www.henrys-law.org.
Marc von Hobe, Domenico Taraborrelli, Sascha Alber, Birger Bohn, Hans-Peter Dorn, Hendrik Fuchs, Yun Li, Chenxi Qiu, Franz Rohrer, Roberto Sommariva, Fred Stroh, Zhaofeng Tan, Sergej Wedel, and Anna Novelli
Atmos. Chem. Phys., 23, 10609–10623, https://doi.org/10.5194/acp-23-10609-2023, https://doi.org/10.5194/acp-23-10609-2023, 2023
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The trace gas carbonyl sulfide (OCS) transports sulfur from the troposphere to the stratosphere, where sulfate aerosols are formed that influence climate and stratospheric chemistry. An uncertain OCS source in the troposphere is chemical production form dimethyl sulfide (DMS), a gas released in large quantities from the oceans. We carried out experiments in a large atmospheric simulation chamber to further elucidate the chemical mechanism of OCS production from DMS.
Shawon Barua, Siddharth Iyer, Avinash Kumar, Prasenjit Seal, and Matti Rissanen
Atmos. Chem. Phys., 23, 10517–10532, https://doi.org/10.5194/acp-23-10517-2023, https://doi.org/10.5194/acp-23-10517-2023, 2023
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This work illustrates how a common volatile hydrocarbon, hexanal, has the potential to undergo atmospheric autoxidation that leads to prompt formation of condensable material that subsequently contributes to aerosol formation, deteriorating the air quality of urban atmospheres. We used the combined state-of-the-art quantum chemical modeling and experimental flow reactor experiments under atmospheric conditions to resolve the autoxidation mechanism of hexanal initiated by a common oxidant.
Yixin Hao, Jun Zhou, Jie-Ping Zhou, Yan Wang, Suxia Yang, Yibo Huangfu, Xiao-Bing Li, Chunsheng Zhang, Aiming Liu, Yanfeng Wu, Yaqing Zhou, Shuchun Yang, Yuwen Peng, Jipeng Qi, Xianjun He, Xin Song, Yubin Chen, Bin Yuan, and Min Shao
Atmos. Chem. Phys., 23, 9891–9910, https://doi.org/10.5194/acp-23-9891-2023, https://doi.org/10.5194/acp-23-9891-2023, 2023
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By employing an improved net photochemical ozone production rate (NPOPR) detection system based on the dual-channel reaction chamber technique, we measured the net photochemical ozone production rate in the Pearl River Delta in China. The photochemical ozone formation mechanisms in the reaction and reference chambers were investigated using the observation-data-constrained box model, which helped us to validate the NPOPR detection system and understand photochemical ozone formation mechanism.
Kevin J. Nihill, Matthew M. Coggon, Christopher Y. Lim, Abigail R. Koss, Bin Yuan, Jordan E. Krechmer, Kanako Sekimoto, Jose L. Jimenez, Joost de Gouw, Christopher D. Cappa, Colette L. Heald, Carsten Warneke, and Jesse H. Kroll
Atmos. Chem. Phys., 23, 7887–7899, https://doi.org/10.5194/acp-23-7887-2023, https://doi.org/10.5194/acp-23-7887-2023, 2023
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In this work, we collect emissions from controlled burns of biomass fuels that can be found in the western United States into an environmental chamber in order to simulate their oxidation as they pass through the atmosphere. These findings provide a detailed characterization of the composition of the atmosphere downwind of wildfires. In turn, this will help to explore the effects of these changing emissions on downwind populations and will also directly inform atmospheric and climate models.
Caterina Mapelli, James K. Donnelly, Úna E. Hogan, Andrew R. Rickard, Abbie T. Robinson, Fergal Byrne, Con Rob McElroy, Basile F. E. Curchod, Daniel Hollas, and Terry J. Dillon
Atmos. Chem. Phys., 23, 7767–7779, https://doi.org/10.5194/acp-23-7767-2023, https://doi.org/10.5194/acp-23-7767-2023, 2023
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Solvents are chemical compounds with countless uses in the chemical industry, and they also represent one of the main sources of pollution in the chemical sector. Scientists are trying to develop new
greensafer solvents which present favourable advantages when compared to traditional solvents. Since the assessment of these green solvents often lacks air quality considerations, this study aims to understand the behaviour of these compounds, investigating their reactivity in the troposphere.
Roland Benoit, Nesrine Belhadj, Zahraa Dbouk, Maxence Lailliau, and Philippe Dagaut
Atmos. Chem. Phys., 23, 5715–5733, https://doi.org/10.5194/acp-23-5715-2023, https://doi.org/10.5194/acp-23-5715-2023, 2023
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We observed a surprisingly similar set of oxidation product chemical formulas from limonene and α-pinene, including oligomers, formed under cool-flame (present experiments) and simulated atmospheric oxidation (literature). Data analysis indicated that a subset of chemical formulas is common to all experiments independently of experimental conditions. Also, this study indicates that many detected chemical formulas can be ascribed to an autooxidation reaction.
Melissa Meder, Otso Peräkylä, Jonathan G. Varelas, Jingyi Luo, Runlong Cai, Yanjun Zhang, Theo Kurtén, Matthieu Riva, Matti Rissanen, Franz M. Geiger, Regan J. Thomson, and Mikael Ehn
Atmos. Chem. Phys., 23, 4373–4390, https://doi.org/10.5194/acp-23-4373-2023, https://doi.org/10.5194/acp-23-4373-2023, 2023
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We discuss and show the viability of a method where multiple isotopically labelled precursors are used for probing the formation pathways of highly oxygenated organic molecules (HOMs) from the oxidation of the monoterpene a-pinene. HOMs are very important for secondary organic aerosol (SOA) formation in forested regions, and monoterpenes are the single largest source of SOA globally. The fast reactions forming HOMs have thus far remained elusive despite considerable efforts over the last decade.
Philip T. M. Carlsson, Luc Vereecken, Anna Novelli, François Bernard, Steven S. Brown, Bellamy Brownwood, Changmin Cho, John N. Crowley, Patrick Dewald, Peter M. Edwards, Nils Friedrich, Juliane L. Fry, Mattias Hallquist, Luisa Hantschke, Thorsten Hohaus, Sungah Kang, Jonathan Liebmann, Alfred W. Mayhew, Thomas Mentel, David Reimer, Franz Rohrer, Justin Shenolikar, Ralf Tillmann, Epameinondas Tsiligiannis, Rongrong Wu, Andreas Wahner, Astrid Kiendler-Scharr, and Hendrik Fuchs
Atmos. Chem. Phys., 23, 3147–3180, https://doi.org/10.5194/acp-23-3147-2023, https://doi.org/10.5194/acp-23-3147-2023, 2023
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The investigation of the night-time oxidation of the most abundant hydrocarbon, isoprene, in chamber experiments shows the importance of reaction pathways leading to epoxy products, which could enhance particle formation, that have so far not been accounted for. The chemical lifetime of organic nitrates from isoprene is long enough for the majority to be further oxidized the next day by daytime oxidants.
Kevin D. Easterbrook, Mitchell A. Vona, Kiana Nayebi-Astaneh, Amanda M. Miller, and Hans D. Osthoff
Atmos. Chem. Phys., 23, 311–322, https://doi.org/10.5194/acp-23-311-2023, https://doi.org/10.5194/acp-23-311-2023, 2023
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The trace gas peroxypropionyl nitrate (PPN) is generated in photochemical smog, phytotoxic, a strong eye irritant, and possibly mutagenic. Here, its solubility and reactivity in water and in octanol were investigated using a bubble flow apparatus, yielding its Henry's law constant and octanol–water partition coefficient (Kow). The results allow the fate of PPN to be more accurately constrained in atmospheric chemical transport models, including its uptake on clouds, organic aerosol, and leaves.
Qing Ye, Matthew B. Goss, Jordan E. Krechmer, Francesca Majluf, Alexander Zaytsev, Yaowei Li, Joseph R. Roscioli, Manjula Canagaratna, Frank N. Keutsch, Colette L. Heald, and Jesse H. Kroll
Atmos. Chem. Phys., 22, 16003–16015, https://doi.org/10.5194/acp-22-16003-2022, https://doi.org/10.5194/acp-22-16003-2022, 2022
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The atmospheric oxidation of dimethyl sulfide (DMS) is a major natural source of sulfate particles in the atmosphere. However, its mechanism is poorly constrained. In our work, laboratory measurements and mechanistic modeling were conducted to comprehensively investigate DMS oxidation products and key reaction rates. We find that the peroxy radical (RO2) has a controlling effect on product distribution and aerosol yield, with the isomerization of RO2 leading to the suppression of aerosol yield.
Caterina Mapelli, Juliette V. Schleicher, Alex Hawtin, Conor D. Rankine, Fiona C. Whiting, Fergal Byrne, C. Rob McElroy, Claudiu Roman, Cecilia Arsene, Romeo I. Olariu, Iustinian G. Bejan, and Terry J. Dillon
Atmos. Chem. Phys., 22, 14589–14602, https://doi.org/10.5194/acp-22-14589-2022, https://doi.org/10.5194/acp-22-14589-2022, 2022
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Solvents represent an important source of pollution from the chemical industry. New "green" solvents aim to replace toxic solvents with new molecules made from renewable sources and designed to be less harmful. Whilst these new molecules are selected according to toxicity and other characteristics, no consideration has yet been included on air quality. Studying the solvent breakdown in air, we found that TMO has a lower impact on air quality than traditional solvents with similar properties.
Kai Song, Song Guo, Yuanzheng Gong, Daqi Lv, Yuan Zhang, Zichao Wan, Tianyu Li, Wenfei Zhu, Hui Wang, Ying Yu, Rui Tan, Ruizhe Shen, Sihua Lu, Shuangde Li, Yunfa Chen, and Min Hu
Atmos. Chem. Phys., 22, 9827–9841, https://doi.org/10.5194/acp-22-9827-2022, https://doi.org/10.5194/acp-22-9827-2022, 2022
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Emissions from four typical Chinese domestic cooking and fried chicken using four kinds of oils were investigated to illustrate the impact of cooking style and oil. Of the estimated SOA, 10.2 %–32.0 % could be explained by S/IVOC oxidation. Multiway principal component analysis (MPCA) emphasizes the importance of the unsaturated fatty acid-alkadienal volatile product mechanism (oil autoxidation) accelerated by the cooking and heating procedure.
Michelia Dam, Danielle C. Draper, Andrey Marsavin, Juliane L. Fry, and James N. Smith
Atmos. Chem. Phys., 22, 9017–9031, https://doi.org/10.5194/acp-22-9017-2022, https://doi.org/10.5194/acp-22-9017-2022, 2022
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We performed chamber experiments to measure the composition of the gas-phase reaction products of nitrate-radical-initiated oxidation of four monoterpenes. The total organic yield, effective oxygen-to-carbon ratio, and dimer-to-monomer ratio were correlated with the observed particle formation for the monoterpene systems with some exceptions. The Δ-carene system produced the most particles, followed by β-pinene, with the α-pinene and α-thujene systems producing no particles.
Jacky Yat Sing Pang, Anna Novelli, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Philip T. M. Carlsson, Changmin Cho, Hans-Peter Dorn, Andreas Hofzumahaus, Xin Li, Anna Lutz, Sascha Nehr, David Reimer, Franz Rohrer, Ralf Tillmann, Robert Wegener, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 22, 8497–8527, https://doi.org/10.5194/acp-22-8497-2022, https://doi.org/10.5194/acp-22-8497-2022, 2022
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This study investigates the radical chemical budget during the limonene oxidation at different atmospheric-relevant NO concentrations in chamber experiments under atmospheric conditions. It is found that the model–measurement discrepancies of HO2 and RO2 are very large at low NO concentrations that are typical for forested environments. Possible additional processes impacting HO2 and RO2 concentrations are discussed.
Carmen Maria Tovar, Ian Barnes, Iustinian Gabriel Bejan, and Peter Wiesen
Atmos. Chem. Phys., 22, 6989–7004, https://doi.org/10.5194/acp-22-6989-2022, https://doi.org/10.5194/acp-22-6989-2022, 2022
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This work explores the kinetics and reactivity of epoxides towards the OH radical using two different simulation chambers. Estimation of the rate coefficients has also been made using different structure–activity relationship (SAR) approaches. The results indicate a direct influence of the structural and geometric properties of the epoxides not considered in SAR estimations, influencing the reactivity of these compounds. The outcomes of this work are in very good agreement with previous studies.
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and Bénédicte Picquet-Varrault
Atmos. Chem. Phys., 22, 6411–6434, https://doi.org/10.5194/acp-22-6411-2022, https://doi.org/10.5194/acp-22-6411-2022, 2022
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Biogenic volatile organic compounds are intensely emitted by forests and crops and react with the nitrate radical during the nighttime to form functionalized products. The purpose of this study is to furnish kinetic and mechanistic data for terpinolene and β-caryophyllene, using simulation chamber experiments. Rate constants have been measured using both relative and absolute methods, and mechanistic studies have been conducted in order to identify and quantify the main reaction products.
Yuanyuan Luo, Olga Garmash, Haiyan Li, Frans Graeffe, Arnaud P. Praplan, Anssi Liikanen, Yanjun Zhang, Melissa Meder, Otso Peräkylä, Josep Peñuelas, Ana María Yáñez-Serrano, and Mikael Ehn
Atmos. Chem. Phys., 22, 5619–5637, https://doi.org/10.5194/acp-22-5619-2022, https://doi.org/10.5194/acp-22-5619-2022, 2022
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Diterpenes were only recently observed in the atmosphere, and little is known of their atmospheric fates. We explored the ozonolysis of the diterpene kaurene in a chamber, and we characterized the oxidation products for the first time using chemical ionization mass spectrometry. Our findings highlight similarities and differences between diterpenes and smaller terpenes during their atmospheric oxidation.
Wenyu Sun, Matias Berasategui, Andrea Pozzer, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 22, 4969–4984, https://doi.org/10.5194/acp-22-4969-2022, https://doi.org/10.5194/acp-22-4969-2022, 2022
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The reaction between OH and SO2 is a termolecular process that in the atmosphere results in the formation of H2SO4 and thus aerosols. We present the first temperature- and pressure-dependent measurements of the rate coefficients in N2. This is also the first study to examine the effects of water vapour on the kinetics of this reaction. Our results indicate the rate coefficient is larger than that recommended by evaluation panels, with deviations of up to 30 % in some parts of the atmosphere.
Haoyu Jiang, Yingyao He, Yiqun Wang, Sheng Li, Bin Jiang, Luca Carena, Xue Li, Lihua Yang, Tiangang Luan, Davide Vione, and Sasho Gligorovski
Atmos. Chem. Phys., 22, 4237–4252, https://doi.org/10.5194/acp-22-4237-2022, https://doi.org/10.5194/acp-22-4237-2022, 2022
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Heterogeneous oxidation of SO2 is suggested to be one of the most important pathways for sulfate formation during extreme haze events in China, yet the exact mechanism remains highly uncertain. Our study reveals that ubiquitous compounds at the sea surface PAHS and DMSO, when exposed to SO2 under simulated sunlight irradiation, generate abundant organic sulfur compounds, providing implications for air-sea interaction and secondary organic aerosols formation processes.
Roland Vernooij, Ulrike Dusek, Maria Elena Popa, Peng Yao, Anupam Shaikat, Chenxi Qiu, Patrik Winiger, Carina van der Veen, Thomas Callum Eames, Natasha Ribeiro, and Guido R. van der Werf
Atmos. Chem. Phys., 22, 2871–2890, https://doi.org/10.5194/acp-22-2871-2022, https://doi.org/10.5194/acp-22-2871-2022, 2022
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Landscape fires are a major source of greenhouse gases and aerosols, particularly in sub-tropical savannas. Stable carbon isotopes in emissions can be used to trace the contribution of C3 plants (e.g. trees or shrubs) and C4 plants (e.g. savanna grasses) to greenhouse gases and aerosols if the process is well understood. This helps us to link individual vegetation types to emissions, identify biomass burning emissions in the atmosphere, and improve the reconstruction of historic fire regimes.
María Asensio, María Antiñolo, Sergio Blázquez, José Albaladejo, and Elena Jiménez
Atmos. Chem. Phys., 22, 2689–2701, https://doi.org/10.5194/acp-22-2689-2022, https://doi.org/10.5194/acp-22-2689-2022, 2022
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The diurnal atmospheric degradation of 2-methylbutanal, 2 MB, emitted by sources like vegetation or the poultry industry is evaluated in this work. Sunlight and oxidants like hydroxyl (OH) radicals and chlorine (Cl) atoms initiate this degradation. Measurements of how fast 2 MB is degraded and what products are generated are presented. The lifetime of 2 MB is around 1 h at noon, when the OH reaction dominates. Thus, 2 MB will not be transported far, affecting only local air quality.
Claudiu Roman, Cecilia Arsene, Iustinian Gabriel Bejan, and Romeo Iulian Olariu
Atmos. Chem. Phys., 22, 2203–2219, https://doi.org/10.5194/acp-22-2203-2022, https://doi.org/10.5194/acp-22-2203-2022, 2022
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Gas-phase reaction rate coefficients of OH radicals with four nitrocatechols have been investigated for the first time by using ESC-Q-UAIC chamber facilities. The reactivity of all investigated nitrocatechols is influenced by the formation of the intramolecular H-bonds that are connected to the deactivating electromeric effect of the NO2 group. For the 3-nitrocatechol compounds, the electromeric effect of the
freeOH group is diminished by the deactivating E-effect of the NO2 group.
Zhiyuan Gao, Nicolas-Xavier Geilfus, Alfonso Saiz-Lopez, and Feiyue Wang
Atmos. Chem. Phys., 22, 1811–1824, https://doi.org/10.5194/acp-22-1811-2022, https://doi.org/10.5194/acp-22-1811-2022, 2022
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Every spring in the Arctic, a series of photochemical events occur over the ice-covered ocean, known as bromine explosion events, ozone depletion events, and mercury depletion events. Here we report the re-creation of these events at an outdoor sea ice facility in Winnipeg, Canada, far away from the Arctic. The success provides a new platform with new opportunities to uncover fundamental mechanisms of these Arctic springtime phenomena and how they may change in a changing climate.
Haichao Wang, Chao Peng, Xuan Wang, Shengrong Lou, Keding Lu, Guicheng Gan, Xiaohong Jia, Xiaorui Chen, Jun Chen, Hongli Wang, Shaojia Fan, Xinming Wang, and Mingjin Tang
Atmos. Chem. Phys., 22, 1845–1859, https://doi.org/10.5194/acp-22-1845-2022, https://doi.org/10.5194/acp-22-1845-2022, 2022
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Via combining laboratory and modeling work, we found that heterogeneous reaction of N2O5 with saline mineral dust aerosol could be an important source of tropospheric ClNO2 in inland regions.
Mike J. Newland, Yangang Ren, Max R. McGillen, Lisa Michelat, Véronique Daële, and Abdelwahid Mellouki
Atmos. Chem. Phys., 22, 1761–1772, https://doi.org/10.5194/acp-22-1761-2022, https://doi.org/10.5194/acp-22-1761-2022, 2022
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Wildfires are increasing in extent and severity, driven by climate change. Such fires emit large amounts of volatile organic compounds (VOCs) to the atmosphere. Many of these, such as the furans studied here, are very reactive and are rapidly converted to other VOCs, which are expected to have negative health effects and to further impact the climate. Here, we establish the importance of the nitrate radical for removing these compounds both during the night and during the day.
Delaney B. Kilgour, Gordon A. Novak, Jon S. Sauer, Alexia N. Moore, Julie Dinasquet, Sarah Amiri, Emily B. Franklin, Kathryn Mayer, Margaux Winter, Clare K. Morris, Tyler Price, Francesca Malfatti, Daniel R. Crocker, Christopher Lee, Christopher D. Cappa, Allen H. Goldstein, Kimberly A. Prather, and Timothy H. Bertram
Atmos. Chem. Phys., 22, 1601–1613, https://doi.org/10.5194/acp-22-1601-2022, https://doi.org/10.5194/acp-22-1601-2022, 2022
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We report measurements of gas-phase volatile organosulfur molecules made during a mesocosm phytoplankton bloom experiment. Dimethyl sulfide (DMS), methanethiol (MeSH), and benzothiazole accounted for on average over 90 % of total gas-phase sulfur emissions. This work focuses on factors controlling the production and emission of DMS and MeSH and the role of non-DMS molecules (such as MeSH and benzothiazole) in secondary sulfate formation in coastal marine environments.
Niklas Illmann, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 18557–18572, https://doi.org/10.5194/acp-21-18557-2021, https://doi.org/10.5194/acp-21-18557-2021, 2021
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Understanding the chemistry of biomass burning plumes is of global interest. Within this work we investigated the OH radical reaction of 3-penten-2-one, which has been identified in biomass burning emissions. We observed the primary formation of peroxyacetyl nitrate (PAN), a key NOx reservoir species. Besides, PAN precursors were also identified as main oxidation products. 3-Penten-2-one is shown to be an example explaining rapid PAN formation within young biomass burning plumes.
Zhaofeng Tan, Luisa Hantschke, Martin Kaminski, Ismail-Hakki Acir, Birger Bohn, Changmin Cho, Hans-Peter Dorn, Xin Li, Anna Novelli, Sascha Nehr, Franz Rohrer, Ralf Tillmann, Robert Wegener, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 16067–16091, https://doi.org/10.5194/acp-21-16067-2021, https://doi.org/10.5194/acp-21-16067-2021, 2021
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The photo-oxidation of myrcene, a monoterpene species emitted by plants, was investigated at atmospheric conditions in the outdoor simulation chamber SAPHIR. The chemical structure of myrcene is partly similar to isoprene. Therefore, it can be expected that hydrogen shift reactions could play a role as observed for isoprene. In this work, their potential impact on the regeneration efficiency of hydroxyl radicals is investigated.
Shijie Yu, Fangcheng Su, Shasha Yin, Shenbo Wang, Ruixin Xu, Bing He, Xiangge Fan, Minghao Yuan, and Ruiqin Zhang
Atmos. Chem. Phys., 21, 15239–15257, https://doi.org/10.5194/acp-21-15239-2021, https://doi.org/10.5194/acp-21-15239-2021, 2021
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This study measured 106 VOC species using a GC-MS/FID. Meanwhile, the WRF-CMAQ model was used to investigate the nonlinearity of the O3 response to precursor reductions. This study highlights the effectiveness of stringent emission controls in relation to solvent utilization and coal combustion. However, unreasonable emission reduction may aggravate ozone pollution during control periods. It is suggested that emission-reduction ratios of the precursors (VOC : NOx) should be more than 2.
Niklas Illmann, Rodrigo Gastón Gibilisco, Iustinian Gabriel Bejan, Iulia Patroescu-Klotz, and Peter Wiesen
Atmos. Chem. Phys., 21, 13667–13686, https://doi.org/10.5194/acp-21-13667-2021, https://doi.org/10.5194/acp-21-13667-2021, 2021
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Within this work we determined the rate coefficients and products of the reaction of unsaturated ketones with OH radicals in an effort to complete the gaps in the knowledge needed for modelling chemistry in the atmosphere. Both substances are potentially emitted by biomass burning, industrial activities or formed in the troposphere by oxidation of terpenes. As products we identified aldehydes and ketones which in turn are known to be responsible for the transportation of NOx species.
Yangang Ren, Li Zhou, Abdelwahid Mellouki, Véronique Daële, Mahmoud Idir, Steven S. Brown, Branko Ruscic, Robert S. Paton, Max R. McGillen, and A. R. Ravishankara
Atmos. Chem. Phys., 21, 13537–13551, https://doi.org/10.5194/acp-21-13537-2021, https://doi.org/10.5194/acp-21-13537-2021, 2021
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Aromatic aldehydes are a family of compounds emitted into the atmosphere from both anthropogenic and biogenic sources that are formed from the degradation of aromatic hydrocarbons. Their atmospheric degradation may impact air quality. We report on their atmospheric degradation through reaction with NO3, which is useful to estimate their atmospheric lifetimes. We have also attempted to elucidate the mechanism of these reactions via studies of isotopic substitution and quantum chemistry.
Luisa Hantschke, Anna Novelli, Birger Bohn, Changmin Cho, David Reimer, Franz Rohrer, Ralf Tillmann, Marvin Glowania, Andreas Hofzumahaus, Astrid Kiendler-Scharr, Andreas Wahner, and Hendrik Fuchs
Atmos. Chem. Phys., 21, 12665–12685, https://doi.org/10.5194/acp-21-12665-2021, https://doi.org/10.5194/acp-21-12665-2021, 2021
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The reactions of Δ3-carene with ozone and the hydroxyl radical (OH) and the photolysis and OH reaction of caronaldehyde were investigated in the simulation chamber SAPHIR. Reaction rate constants of these reactions were determined. Caronaldehyde yields of the ozonolysis and OH reaction were determined. The organic nitrate yield of the reaction of Δ3-carene and caronaldehyde-derived peroxy radicals with NO was determined. The ROx budget (ROx = OH+HO2+RO2) was also investigated.
Letizia Abis, Carmen Kalalian, Bastien Lunardelli, Tao Wang, Liwu Zhang, Jianmin Chen, Sébastien Perrier, Benjamin Loubet, Raluca Ciuraru, and Christian George
Atmos. Chem. Phys., 21, 12613–12629, https://doi.org/10.5194/acp-21-12613-2021, https://doi.org/10.5194/acp-21-12613-2021, 2021
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Biogenic volatile organic compound (BVOC) emissions from rapeseed leaf litter have been investigated by means of a controlled atmospheric simulation chamber. The diversity of emitted VOCs increased also in the presence of UV light irradiation. SOA formation was observed when leaf litter was exposed to both UV light and ozone, indicating a potential contribution to particle formation or growth at local scales.
Xi Cheng, Qi Chen, Yong Jie Li, Yan Zheng, Keren Liao, and Guancong Huang
Atmos. Chem. Phys., 21, 12005–12019, https://doi.org/10.5194/acp-21-12005-2021, https://doi.org/10.5194/acp-21-12005-2021, 2021
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In this study, we conducted laboratory studies to investigate the formation of gas-phase highly oxygenated organic molecules (HOMs). We provide a thorough analysis on the importance of multistep auto-oxidation and multigeneration OH reactions. We also give an intensive investigation on the roles of high-NO2 conditions that represent a wide range of anthropogenically influenced environments.
Rongrong Wu, Luc Vereecken, Epameinondas Tsiligiannis, Sungah Kang, Sascha R. Albrecht, Luisa Hantschke, Defeng Zhao, Anna Novelli, Hendrik Fuchs, Ralf Tillmann, Thorsten Hohaus, Philip T. M. Carlsson, Justin Shenolikar, François Bernard, John N. Crowley, Juliane L. Fry, Bellamy Brownwood, Joel A. Thornton, Steven S. Brown, Astrid Kiendler-Scharr, Andreas Wahner, Mattias Hallquist, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 10799–10824, https://doi.org/10.5194/acp-21-10799-2021, https://doi.org/10.5194/acp-21-10799-2021, 2021
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Isoprene is the biogenic volatile organic compound with the largest emissions rates. The nighttime reaction of isoprene with the NO3 radical has a large potential to contribute to SOA. We classified isoprene nitrates into generations and proposed formation pathways. Considering the potential functionalization of the isoprene nitrates we propose that mainly isoprene dimers contribute to SOA formation from the isoprene NO3 reactions with at least a 5 % mass yield.
Defeng Zhao, Iida Pullinen, Hendrik Fuchs, Stephanie Schrade, Rongrong Wu, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Yindong Guo, Astrid Kiendler-Scharr, Andreas Wahner, Sungah Kang, Luc Vereecken, and Thomas F. Mentel
Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, https://doi.org/10.5194/acp-21-9681-2021, 2021
Short summary
Short summary
The reaction of isoprene, a biogenic volatile organic compound with the globally largest emission rates, with NO3, an nighttime oxidant influenced heavily by anthropogenic emissions, forms a large number of highly oxygenated organic molecules (HOM). These HOM are formed via one or multiple oxidation steps, followed by autoxidation. Their total yield is much higher than that in the daytime oxidation of isoprene. They may play an important role in nighttime organic aerosol formation and growth.
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Short summary
HNCO is a toxic molecule and can cause cardiovascular and cataract problems through protein carbamylation once inhaled. Recently reported ambient measurements of HNCO in North America raise concerns for human exposure. To better understand HNCO's loss processes and behaviour in the atmosphere, we provide thermochemical data on HNCO. The parameters allow for more accurate predictions of its lifetime in the atmosphere and consequently help define exposure of this toxic molecule.
HNCO is a toxic molecule and can cause cardiovascular and cataract problems through protein...
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