Articles | Volume 22, issue 3
https://doi.org/10.5194/acp-22-1811-2022
© Author(s) 2022. 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-22-1811-2022
© Author(s) 2022. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
08 Feb 2022
Research article |
| 08 Feb 2022
| 08 Feb 2022
Reproducing Arctic springtime tropospheric ozone and mercury depletion events in an outdoor mesocosm sea ice facility
Zhiyuan Gao
Centre for Earth Observation Science, and Department of Environment
and Geography, University of Manitoba, Winnipeg, MB R3T 2N2, Canada
Nicolas-Xavier Geilfus
Centre for Earth Observation Science, and Department of Environment
and Geography, University of Manitoba, Winnipeg, MB R3T 2N2, Canada
Alfonso Saiz-Lopez
Department of Atmospheric Chemistry and Climate, Institute of Physical
Chemistry Rocasolano, CSIC, 28006 Madrid, Spain
Centre for Earth Observation Science, and Department of Environment
and Geography, University of Manitoba, Winnipeg, MB R3T 2N2, Canada
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Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
Heesung Chong, Gonzalo González Abad, Caroline R. Nowlan, Christopher Chan Miller, Alfonso Saiz-Lopez, Rafael P. Fernandez, Hyeong-Ahn Kwon, Zolal Ayazpour, Huiqun Wang, Amir H. Souri, Xiong Liu, Kelly Chance, Ewan O'Sullivan, Jhoon Kim, Ja-Ho Koo, William R. Simpson, François Hendrick, Richard Querel, Glen Jaross, Colin Seftor, and Raid M. Suleiman
Atmos. Meas. Tech., 17, 2873–2916, https://doi.org/10.5194/amt-17-2873-2024, https://doi.org/10.5194/amt-17-2873-2024, 2024
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We present a new bromine monoxide (BrO) product derived using radiances measured from OMPS-NM on board the Suomi-NPP satellite. This product provides nearly a decade of global stratospheric and tropospheric column retrievals, a feature that is currently rare in publicly accessible datasets. Both stratospheric and tropospheric columns from OMPS-NM demonstrate robust performance, exhibiting good agreement with ground-based observations collected at three stations (Lauder, Utqiagvik, and Harestua).
Cyril Caram, Sophie Szopa, Anne Cozic, Slimane Bekki, Carlos A. Cuevas, and Alfonso Saiz-Lopez
Geosci. Model Dev., 16, 4041–4062, https://doi.org/10.5194/gmd-16-4041-2023, https://doi.org/10.5194/gmd-16-4041-2023, 2023
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We studied the role of halogenated compounds (containing chlorine, bromine and iodine), emitted by natural processes (mainly above the oceans), in the chemistry of the lower layers of the atmosphere. We introduced this relatively new chemistry in a three-dimensional climate–chemistry model and looked at how this chemistry will disrupt the ozone. We showed that the concentration of ozone decreases by 22 % worldwide and that of the atmospheric detergent, OH, by 8 %.
Manon Rocco, Erin Dunne, Alexia Saint-Macary, Maija Peltola, Theresa Barthelmeß, Neill Barr, Karl Safi, Andrew Marriner, Stacy Deppeler, James Harnwell, Anja Engel, Aurélie Colomb, Alfonso Saiz-Lopez, Mike Harvey, Cliff S. Law, and Karine Sellegri
EGUsphere, https://doi.org/10.5194/egusphere-2023-516, https://doi.org/10.5194/egusphere-2023-516, 2023
Preprint archived
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During the Sea2cloud campaign in the Southern Pacific Ocean, we measured air-sea emissions from phytopankton of two key atmospheric compounds: DMS and MeSH. These compounds are well-known to play a great role in atmospheric chemistry and climate. We see in this paper that these compounds are most emited by the nanophytoplankton population. We provide here parameters for climate models to predict future trends of the emissions of these compounds and their roles and impacts on the global warming.
François Burgay, Rafael Pedro Fernández, Delia Segato, Clara Turetta, Christopher S. Blaszczak-Boxe, Rachael H. Rhodes, Claudio Scarchilli, Virginia Ciardini, Carlo Barbante, Alfonso Saiz-Lopez, and Andrea Spolaor
The Cryosphere, 17, 391–405, https://doi.org/10.5194/tc-17-391-2023, https://doi.org/10.5194/tc-17-391-2023, 2023
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The paper presents the first ice-core record of bromine (Br) in the Antarctic plateau. By the observation of the ice core and the application of atmospheric chemical models, we investigate the behaviour of bromine after its deposition into the snowpack, with interest in the effect of UV radiation change connected to the formation of the ozone hole, the role of volcanic deposition, and the possible use of Br to reconstruct past sea ice changes from ice core collect in the inner Antarctic plateau.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Hisahiro Takashima, Yugo Kanaya, Saki Kato, Martina M. Friedrich, Michel Van Roozendael, Fumikazu Taketani, Takuma Miyakawa, Yuichi Komazaki, Carlos A. Cuevas, Alfonso Saiz-Lopez, and Takashi Sekiya
Atmos. Chem. Phys., 22, 4005–4018, https://doi.org/10.5194/acp-22-4005-2022, https://doi.org/10.5194/acp-22-4005-2022, 2022
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We have undertaken atmospheric iodine monoxide (IO) observations in the global marine boundary layer with a wide latitudinal coverage and sea surface temperature (SST) range. We conclude that atmospheric iodine is abundant over the Western Pacific warm pool, appearing as an iodine fountain, where ozone (O3) minima occur. Our study also found negative correlations between IO and O3 concentrations over IO maxima, which requires reconsideration of the initiation process of halogen activation.
Arseniy Karagodin-Doyennel, Eugene Rozanov, Timofei Sukhodolov, Tatiana Egorova, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Tomás Sherwen, Rainer Volkamer, Theodore K. Koenig, Tanguy Giroud, and Thomas Peter
Geosci. Model Dev., 14, 6623–6645, https://doi.org/10.5194/gmd-14-6623-2021, https://doi.org/10.5194/gmd-14-6623-2021, 2021
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Here, we present the iodine chemistry module in the SOCOL-AERv2 model. The obtained iodine distribution demonstrated a good agreement when validated against other simulations and available observations. We also estimated the iodine influence on ozone in the case of present-day iodine emissions, the sensitivity of ozone to doubled iodine emissions, and when considering only organic or inorganic iodine sources. The new model can be used as a tool for further studies of iodine effects on ozone.
Anoop S. Mahajan, Mriganka S. Biswas, Steffen Beirle, Thomas Wagner, Anja Schönhardt, Nuria Benavent, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 11829–11842, https://doi.org/10.5194/acp-21-11829-2021, https://doi.org/10.5194/acp-21-11829-2021, 2021
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Iodine plays a vital role in oxidation chemistry over Antarctica, with past observations showing highly elevated levels of iodine oxide (IO) leading to severe depletion of boundary layer ozone. We present IO observations over three summers (2015–2017) at the Indian Antarctic bases of Bharati and Maitri. IO was observed during all campaigns with mixing ratios below 2 pptv, which is lower than the peak levels observed in West Antarctica, showing the differences in regional chemistry and emissions.
Anoop S. Mahajan, Qinyi Li, Swaleha Inamdar, Kirpa Ram, Alba Badia, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 21, 8437–8454, https://doi.org/10.5194/acp-21-8437-2021, https://doi.org/10.5194/acp-21-8437-2021, 2021
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Using a regional model, we show that iodine-catalysed reactions cause large regional changes in the chemical composition in the northern Indian Ocean, with peak changes of up to 25 % in O3, 50 % in nitrogen oxides (NO and NO2), 15 % in hydroxyl radicals (OH), 25 % in hydroperoxyl radicals (HO2), and up to a 50 % change in the nitrate radical (NO3). These results show the importance of including iodine chemistry in modelling the atmosphere in this region.
David Garcia-Nieto, Nuria Benavent, Rafael Borge, and Alfonso Saiz-Lopez
Atmos. Meas. Tech., 14, 2941–2955, https://doi.org/10.5194/amt-14-2941-2021, https://doi.org/10.5194/amt-14-2941-2021, 2021
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Trace gases play a key role in the chemistry of urban atmospheres. Therefore, knowledge about their spatial distribution is needed to fully characterize the air quality in urban areas. Using a new Multi-AXis Differential Optical Absorption Spectroscopy two-dimensional (MAXDOAS-2D) instrument, along with inversion algorithms, we report for the first time two-dimensional maps of NO2 concentrations in the city of Madrid, Spain.
Swaleha Inamdar, Liselotte Tinel, Rosie Chance, Lucy J. Carpenter, Prabhakaran Sabu, Racheal Chacko, Sarat C. Tripathy, Anvita U. Kerkar, Alok K. Sinha, Parli Venkateswaran Bhaskar, Amit Sarkar, Rajdeep Roy, Tomás Sherwen, Carlos Cuevas, Alfonso Saiz-Lopez, Kirpa Ram, and Anoop S. Mahajan
Atmos. Chem. Phys., 20, 12093–12114, https://doi.org/10.5194/acp-20-12093-2020, https://doi.org/10.5194/acp-20-12093-2020, 2020
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Iodine chemistry is generating a lot of interest because of its impacts on the oxidising capacity of the marine boundary and depletion of ozone. However, one of the challenges has been predicting the right levels of iodine in the models, which depend on parameterisations for emissions from the sea surface. This paper discusses the different parameterisations available and compares them with observations, showing that our current knowledge is still insufficient, especially on a regional scale.
Yang Wang, Arnoud Apituley, Alkiviadis Bais, Steffen Beirle, Nuria Benavent, Alexander Borovski, Ilya Bruchkouski, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Henning Finkenzeller, Martina M. Friedrich, Udo Frieß, David Garcia-Nieto, Laura Gómez-Martín, François Hendrick, Andreas Hilboll, Junli Jin, Paul Johnston, Theodore K. Koenig, Karin Kreher, Vinod Kumar, Aleksandra Kyuberis, Johannes Lampel, Cheng Liu, Haoran Liu, Jianzhong Ma, Oleg L. Polyansky, Oleg Postylyakov, Richard Querel, Alfonso Saiz-Lopez, Stefan Schmitt, Xin Tian, Jan-Lukas Tirpitz, Michel Van Roozendael, Rainer Volkamer, Zhuoru Wang, Pinhua Xie, Chengzhi Xing, Jin Xu, Margarita Yela, Chengxin Zhang, and Thomas Wagner
Atmos. Meas. Tech., 13, 5087–5116, https://doi.org/10.5194/amt-13-5087-2020, https://doi.org/10.5194/amt-13-5087-2020, 2020
Thomas R. Lewis, Juan Carlos Gómez Martín, Mark A. Blitz, Carlos A. Cuevas, John M. C. Plane, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 10865–10887, https://doi.org/10.5194/acp-20-10865-2020, https://doi.org/10.5194/acp-20-10865-2020, 2020
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Iodine-bearing gasses emitted from the sea surface are chemically processed in the atmosphere, leading to iodine accumulation in aerosol and transport to continental ecosystems. Such processing involves light-induced break-up of large, particle-forming iodine oxides into smaller, ozone-depleting molecules. We combine experiments and theory to report the photolysis efficiency of iodine oxides required to assess the impact of iodine on ozone depletion and particle formation.
Javier Alejandro Barrera, Rafael Pedro Fernandez, Fernando Iglesias-Suarez, Carlos Alberto Cuevas, Jean-Francois Lamarque, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 20, 8083–8102, https://doi.org/10.5194/acp-20-8083-2020, https://doi.org/10.5194/acp-20-8083-2020, 2020
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The inclusion of biogenic very short-lived bromocarbons (VSLBr) in the CAM-chem model improves the model–satellite agreement of the total ozone columns at mid-latitudes and drives a persistent hemispheric asymmetry in lowermost stratospheric ozone loss. The seasonal VSLBr impact on mid-latitude lowermost stratospheric ozone is influenced by the heterogeneous reactivation processes of inorganic chlorine on ice crystals, with a clear increase in ozone destruction during spring and winter.
Karin Kreher, Michel Van Roozendael, Francois Hendrick, Arnoud Apituley, Ermioni Dimitropoulou, Udo Frieß, Andreas Richter, Thomas Wagner, Johannes Lampel, Nader Abuhassan, Li Ang, Monica Anguas, Alkis Bais, Nuria Benavent, Tim Bösch, Kristof Bognar, Alexander Borovski, Ilya Bruchkouski, Alexander Cede, Ka Lok Chan, Sebastian Donner, Theano Drosoglou, Caroline Fayt, Henning Finkenzeller, David Garcia-Nieto, Clio Gielen, Laura Gómez-Martín, Nan Hao, Bas Henzing, Jay R. Herman, Christian Hermans, Syedul Hoque, Hitoshi Irie, Junli Jin, Paul Johnston, Junaid Khayyam Butt, Fahim Khokhar, Theodore K. Koenig, Jonas Kuhn, Vinod Kumar, Cheng Liu, Jianzhong Ma, Alexis Merlaud, Abhishek K. Mishra, Moritz Müller, Monica Navarro-Comas, Mareike Ostendorf, Andrea Pazmino, Enno Peters, Gaia Pinardi, Manuel Pinharanda, Ankie Piters, Ulrich Platt, Oleg Postylyakov, Cristina Prados-Roman, Olga Puentedura, Richard Querel, Alfonso Saiz-Lopez, Anja Schönhardt, Stefan F. Schreier, André Seyler, Vinayak Sinha, Elena Spinei, Kimberly Strong, Frederik Tack, Xin Tian, Martin Tiefengraber, Jan-Lukas Tirpitz, Jeroen van Gent, Rainer Volkamer, Mihalis Vrekoussis, Shanshan Wang, Zhuoru Wang, Mark Wenig, Folkard Wittrock, Pinhua H. Xie, Jin Xu, Margarita Yela, Chengxin Zhang, and Xiaoyi Zhao
Atmos. Meas. Tech., 13, 2169–2208, https://doi.org/10.5194/amt-13-2169-2020, https://doi.org/10.5194/amt-13-2169-2020, 2020
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In September 2016, 36 spectrometers from 24 institutes measured a number of key atmospheric pollutants during an instrument intercomparison campaign (CINDI-2) at Cabauw, the Netherlands. Here we report on the outcome of this intercomparison exercise. The three major goals were to characterise the differences between the participating instruments, to define a robust methodology for performance assessment, and to contribute to the harmonisation of the measurement settings and retrieval methods.
Jian Zhu, Shanshan Wang, Hongli Wang, Shengao Jing, Shengrong Lou, Alfonso Saiz-Lopez, and Bin Zhou
Atmos. Chem. Phys., 20, 1217–1232, https://doi.org/10.5194/acp-20-1217-2020, https://doi.org/10.5194/acp-20-1217-2020, 2020
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To investigate the summer ozone pollution, observationally constrained modelling was carried out to study atmospheric oxidation capacity (AOC), OH reactivity, OH chain length, and HOx budget for three different ozone concentration levels in Shanghai, China. It shows that AOC, dominated by reactions involving OH radical during the daytime, has a positive correlation with ozone levels. Some key VOCs species are very important for the OH reactivity and also the ozone formation potential.
Niccolò Maffezzoli, Paul Vallelonga, Ross Edwards, Alfonso Saiz-Lopez, Clara Turetta, Helle Astrid Kjær, Carlo Barbante, Bo Vinther, and Andrea Spolaor
Clim. Past, 15, 2031–2051, https://doi.org/10.5194/cp-15-2031-2019, https://doi.org/10.5194/cp-15-2031-2019, 2019
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This study provides the first ice-core-based history of sea ice in the North Atlantic Ocean, reaching 120 000 years back in time. This record was obtained from bromine and sodium measurements in the RECAP ice core, drilled in east Greenland. We found that, during the last deglaciation, sea ice started to melt ~ 17 500 years ago. Over the 120 000 years of the last glacial cycle, sea ice extent was maximal during MIS2, while minimum sea ice extent exists for the Holocene.
Juan Pablo Corella, Niccolo Maffezzoli, Carlos Alberto Cuevas, Paul Vallelonga, Andrea Spolaor, Giulio Cozzi, Juliane Müller, Bo Vinther, Carlo Barbante, Helle Astrid Kjær, Ross Edwards, and Alfonso Saiz-Lopez
Clim. Past, 15, 2019–2030, https://doi.org/10.5194/cp-15-2019-2019, https://doi.org/10.5194/cp-15-2019-2019, 2019
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This study provides the first reconstruction of atmospheric iodine levels in the Arctic during the last 11 700 years from an ice core record in coastal Greenland. Dramatic shifts in iodine level variability coincide with abrupt climatic transitions in the North Atlantic. Since atmospheric iodine levels have significant environmental and climatic implications, this study may serve as a past analog to predict future changes in Arctic climate in response to global warming.
Qinyi Li, Rafael Borge, Golam Sarwar, David de la Paz, Brett Gantt, Jessica Domingo, Carlos A. Cuevas, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 19, 15321–15337, https://doi.org/10.5194/acp-19-15321-2019, https://doi.org/10.5194/acp-19-15321-2019, 2019
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The abundance and distribution of reactive halogen species and their impact on air quality in Europe are poorly understood. We adopt a state-of-the-art regional model (CMAQ) to evaluate such effects, and the results demonstrate the significant influence of halogen chemistry on the capacity of atmospheric oxidation and the formation of air pollutants in Europe. Our study highlights the necessity of including halogen chemistry in the formulation of air pollution control policy.
Elizabeth Asher, Rebecca S. Hornbrook, Britton B. Stephens, Doug Kinnison, Eric J. Morgan, Ralph F. Keeling, Elliot L. Atlas, Sue M. Schauffler, Simone Tilmes, Eric A. Kort, Martin S. Hoecker-Martínez, Matt C. Long, Jean-François Lamarque, Alfonso Saiz-Lopez, Kathryn McKain, Colm Sweeney, Alan J. Hills, and Eric C. Apel
Atmos. Chem. Phys., 19, 14071–14090, https://doi.org/10.5194/acp-19-14071-2019, https://doi.org/10.5194/acp-19-14071-2019, 2019
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Halogenated organic trace gases, which are a source of reactive halogens to the atmosphere, exert a disproportionately large influence on atmospheric chemistry and climate. This paper reports novel aircraft observations of halogenated compounds over the Southern Ocean in summer and evaluates hypothesized regional sources and emissions of these trace gases through their relationships to additional aircraft observations.
Andrea Spolaor, Elena Barbaro, David Cappelletti, Clara Turetta, Mauro Mazzola, Fabio Giardi, Mats P. Björkman, Federico Lucchetta, Federico Dallo, Katrine Aspmo Pfaffhuber, Hélène Angot, Aurelien Dommergue, Marion Maturilli, Alfonso Saiz-Lopez, Carlo Barbante, and Warren R. L. Cairns
Atmos. Chem. Phys., 19, 13325–13339, https://doi.org/10.5194/acp-19-13325-2019, https://doi.org/10.5194/acp-19-13325-2019, 2019
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The main aims of the study are to (a) detect whether mercury in the surface snow undergoes a daily cycle as determined in the atmosphere, (b) compare the mercury concentration in surface snow with the concentration in the atmosphere, (c) evaluate the effect of snow depositions, (d) detect whether iodine and bromine in the surface snow undergo a daily cycle, and (e) evaluate the role of metereological and atmospheric conditions. Different behaviours were determined during different seasons.
Thomas Wagner, Steffen Beirle, Nuria Benavent, Tim Bösch, Ka Lok Chan, Sebastian Donner, Steffen Dörner, Caroline Fayt, Udo Frieß, David García-Nieto, Clio Gielen, David González-Bartolome, Laura Gomez, François Hendrick, Bas Henzing, Jun Li Jin, Johannes Lampel, Jianzhong Ma, Kornelia Mies, Mónica Navarro, Enno Peters, Gaia Pinardi, Olga Puentedura, Janis Puķīte, Julia Remmers, Andreas Richter, Alfonso Saiz-Lopez, Reza Shaiganfar, Holger Sihler, Michel Van Roozendael, Yang Wang, and Margarita Yela
Atmos. Meas. Tech., 12, 2745–2817, https://doi.org/10.5194/amt-12-2745-2019, https://doi.org/10.5194/amt-12-2745-2019, 2019
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In this study the consistency between MAX-DOAS measurements and radiative transfer simulations of the atmospheric O4 absorption is investigated. The study is based on measurements (2 selected days during the MADCAT campaign) as well as synthetic spectra. The uncertainties of all relevant aspects (spectral retrieval and radiative transfer simulations) are quantified. For one of the selected days, measurements and simulations do not agree within their uncertainties.
Alba Badia, Claire E. Reeves, Alex R. Baker, Alfonso Saiz-Lopez, Rainer Volkamer, Theodore K. Koenig, Eric C. Apel, Rebecca S. Hornbrook, Lucy J. Carpenter, Stephen J. Andrews, Tomás Sherwen, and Roland von Glasow
Atmos. Chem. Phys., 19, 3161–3189, https://doi.org/10.5194/acp-19-3161-2019, https://doi.org/10.5194/acp-19-3161-2019, 2019
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The oceans have an impact on the composition and reactivity of the troposphere through the emission of gases and particles. Thus, a quantitative understanding of the marine atmosphere is crucial to examine the oxidative capacity and climate forcing. This study investigates the impact of halogens in the tropical troposphere and explores the sensitivity of this to uncertainties in the fluxes and their chemical processing. Our modelled tropospheric Ox loss due to halogens ranges from 20 % to 60 %.
Cristina Carnerero, Noemí Pérez, Cristina Reche, Marina Ealo, Gloria Titos, Hong-Ku Lee, Hee-Ram Eun, Yong-Hee Park, Lubna Dada, Pauli Paasonen, Veli-Matti Kerminen, Enrique Mantilla, Miguel Escudero, Francisco J. Gómez-Moreno, Elisabeth Alonso-Blanco, Esther Coz, Alfonso Saiz-Lopez, Brice Temime-Roussel, Nicolas Marchand, David C. S. Beddows, Roy M. Harrison, Tuukka Petäjä, Markku Kulmala, Kang-Ho Ahn, Andrés Alastuey, and Xavier Querol
Atmos. Chem. Phys., 18, 16601–16618, https://doi.org/10.5194/acp-18-16601-2018, https://doi.org/10.5194/acp-18-16601-2018, 2018
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The vertical distribution of new particle formation events was studied using tethered balloons carrying miniaturized instrumentation. Results show that new particle formation and growth occurs only in the lower layer of the atmosphere, where aerosols are mixed due to convection, especially when the atmosphere is clean. A comparison of urban and suburban surface stations was also made, suggesting that such events may have a significant impact on ultrafine particle concentrations in a wide area.
Xavier Querol, Andrés Alastuey, Gotzon Gangoiti, Noemí Perez, Hong K. Lee, Heeram R. Eun, Yonghee Park, Enrique Mantilla, Miguel Escudero, Gloria Titos, Lucio Alonso, Brice Temime-Roussel, Nicolas Marchand, Juan R. Moreta, M. Arantxa Revuelta, Pedro Salvador, Begoña Artíñano, Saúl García dos Santos, Mónica Anguas, Alberto Notario, Alfonso Saiz-Lopez, Roy M. Harrison, Millán Millán, and Kang-Ho Ahn
Atmos. Chem. Phys., 18, 6511–6533, https://doi.org/10.5194/acp-18-6511-2018, https://doi.org/10.5194/acp-18-6511-2018, 2018
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We show the main drivers of high O3 episodes in and around Madrid. High levels of ultrafine particles (UFPs) are evidenced, but we demonstrate that most O3 arises from the fumigation of high atmospheric layers, whereas UFPs are generated inside the PBL. O3 contributions from the fumigation of the vertical recirculation of regional air masses, hemispheric transport, and horizontally from direct urban plume transport are shown. Complexity arises from the need to quantify them to abate surface O3.
Theodore K. Koenig, Rainer Volkamer, Sunil Baidar, Barbara Dix, Siyuan Wang, Daniel C. Anderson, Ross J. Salawitch, Pamela A. Wales, Carlos A. Cuevas, Rafael P. Fernandez, Alfonso Saiz-Lopez, Mathew J. Evans, Tomás Sherwen, Daniel J. Jacob, Johan Schmidt, Douglas Kinnison, Jean-François Lamarque, Eric C. Apel, James C. Bresch, Teresa Campos, Frank M. Flocke, Samuel R. Hall, Shawn B. Honomichl, Rebecca Hornbrook, Jørgen B. Jensen, Richard Lueb, Denise D. Montzka, Laura L. Pan, J. Michael Reeves, Sue M. Schauffler, Kirk Ullmann, Andrew J. Weinheimer, Elliot L. Atlas, Valeria Donets, Maria A. Navarro, Daniel Riemer, Nicola J. Blake, Dexian Chen, L. Gregory Huey, David J. Tanner, Thomas F. Hanisco, and Glenn M. Wolfe
Atmos. Chem. Phys., 17, 15245–15270, https://doi.org/10.5194/acp-17-15245-2017, https://doi.org/10.5194/acp-17-15245-2017, 2017
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Tropospheric inorganic bromine (BrO and Bry) shows a C-shaped profile over the tropical western Pacific Ocean, and supports previous speculation that marine convection is a source for inorganic bromine from sea salt to the upper troposphere. The Bry profile in the tropical tropopause layer (TTL) is complex, suggesting that the total Bry budget in the TTL is not closed without considering aerosol bromide. The implications for atmospheric composition and bromine sources are discussed.
Heather Kyle, Søren Rysgaard, Feiyue Wang, and Mostafa Fayek
The Cryosphere Discuss., https://doi.org/10.5194/tc-2017-226, https://doi.org/10.5194/tc-2017-226, 2017
Revised manuscript not accepted
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Ikaite may play a major role in air-sea carbon fluxes, but its importance is not well known due to difficulties with quantification. A new technique for measuring ikaite was developed and tested and our findings showed this method is effective. Sea ice properties were also measured. Results indicate that ikaite is most abundant in the upper layers of first-year sea ice so will likely play a more significant role in air-sea carbon fluxes in future as seasonal sea ice becomes more common.
Maria A. Navarro, Alfonso Saiz-Lopez, Carlos A. Cuevas, Rafael P. Fernandez, Elliot Atlas, Xavier Rodriguez-Lloveras, Douglas Kinnison, Jean-Francois Lamarque, Simone Tilmes, Troy Thornberry, Andrew Rollins, James W. Elkins, Eric J. Hintsa, and Fred L. Moore
Atmos. Chem. Phys., 17, 9917–9930, https://doi.org/10.5194/acp-17-9917-2017, https://doi.org/10.5194/acp-17-9917-2017, 2017
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Inorganic bromine (Bry) plays an important role in ozone layer depletion. Based on aircraft observations of organic bromine species and chemistry simulations, we model the Bry abundances over the Pacific tropical tropopause. Our results show BrO and Br as the dominant species during daytime hours, and BrCl and BrONO2 as the nighttime dominant species over the western and eastern Pacific, respectively. The difference in the partitioning is due to changes in the abundance of O3, NO2, and Cly.
Enno Peters, Gaia Pinardi, André Seyler, Andreas Richter, Folkard Wittrock, Tim Bösch, Michel Van Roozendael, François Hendrick, Theano Drosoglou, Alkiviadis F. Bais, Yugo Kanaya, Xiaoyi Zhao, Kimberly Strong, Johannes Lampel, Rainer Volkamer, Theodore Koenig, Ivan Ortega, Olga Puentedura, Mónica Navarro-Comas, Laura Gómez, Margarita Yela González, Ankie Piters, Julia Remmers, Yang Wang, Thomas Wagner, Shanshan Wang, Alfonso Saiz-Lopez, David García-Nieto, Carlos A. Cuevas, Nuria Benavent, Richard Querel, Paul Johnston, Oleg Postylyakov, Alexander Borovski, Alexander Elokhov, Ilya Bruchkouski, Haoran Liu, Cheng Liu, Qianqian Hong, Claudia Rivera, Michel Grutter, Wolfgang Stremme, M. Fahim Khokhar, Junaid Khayyam, and John P. Burrows
Atmos. Meas. Tech., 10, 955–978, https://doi.org/10.5194/amt-10-955-2017, https://doi.org/10.5194/amt-10-955-2017, 2017
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This work is about harmonization of differential optical absorption spectroscopy retrieval codes, which is a remote sensing technique widely used to derive atmospheric trace gas amounts. The study is based on ground-based measurements performed during the Multi-Axis DOAS Comparison campaign for Aerosols and Trace gases (MAD-CAT) in Mainz, Germany, in summer 2013. In total, 17 international groups working in the field of the DOAS technique participated in this study.
Paul Vallelonga, Niccolo Maffezzoli, Andrew D. Moy, Mark A. J. Curran, Tessa R. Vance, Ross Edwards, Gwyn Hughes, Emily Barker, Gunnar Spreen, Alfonso Saiz-Lopez, J. Pablo Corella, Carlos A. Cuevas, and Andrea Spolaor
Clim. Past, 13, 171–184, https://doi.org/10.5194/cp-13-171-2017, https://doi.org/10.5194/cp-13-171-2017, 2017
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We present a study of bromine, iodine and sodium in an ice core from Law Dome, in coastal East Antarctica. We find that bromine and iodine variability at Law Dome is correlated to changes in the area of sea ice along the Law Dome coast as observed by satellite since the early 1970s. These findings are in agreement with a previous study based on MSA and confirm a long-term trend of sea ice decrease for this sector of Antarctica over the 20th century.
Rafael P. Fernandez, Douglas E. Kinnison, Jean-Francois Lamarque, Simone Tilmes, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 17, 1673–1688, https://doi.org/10.5194/acp-17-1673-2017, https://doi.org/10.5194/acp-17-1673-2017, 2017
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The inclusion of biogenic very-short lived bromine (VSLBr) in a chemistry-climate model produces an expansion of the ozone hole area of ~ 5 million km2, which is equivalent in magnitude to the recently estimated Antarctic ozone healing due to the reduction of anthropogenic CFCs and halons. The maximum Antarctic ozone hole depletion increases by up to 14 % when natural VSLBr are considered, but does not introduce a significant delay of the modelled ozone return date to 1980 October levels.
Alfonso Saiz-Lopez, John M. C. Plane, Carlos A. Cuevas, Anoop S. Mahajan, Jean-François Lamarque, and Douglas E. Kinnison
Atmos. Chem. Phys., 16, 15593–15604, https://doi.org/10.5194/acp-16-15593-2016, https://doi.org/10.5194/acp-16-15593-2016, 2016
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Electronic structure calculations are used to survey possible reactions that HOI and I2 could undergo at night in the lower troposphere, and hence reconcile measurements and models. The reactions NO3 + HOI and I2 + NO3 are included in two models to explore a new nocturnal iodine radical activation mechanism, leading to a reduction of nighttime HOI and I2. This chemistry can have a large impact on NO3 levels in the MBL, and hence upon the nocturnal oxidizing capacity of the marine atmosphere.
Qianqian Hong, Zhouqing Xie, Cheng Liu, Feiyue Wang, Pinhua Xie, Hui Kang, Jin Xu, Jiancheng Wang, Fengcheng Wu, Pengzhen He, Fusheng Mou, Shidong Fan, Yunsheng Dong, Haicong Zhan, Xiawei Yu, Xiyuan Chi, and Jianguo Liu
Atmos. Chem. Phys., 16, 13807–13821, https://doi.org/10.5194/acp-16-13807-2016, https://doi.org/10.5194/acp-16-13807-2016, 2016
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It is known that rapid industrialization in developing countries has led to an increase in air pollution. Here we firstly report the speciated atmospheric mercury during haze days based upon 1-year synchronous observations in an inland city in China. The findings provide direct evidence to understand the biogeochemical cycles of atmospheric mercury related to air pollution and an opportunity to evaluate the potential health risks of atmospheric mercury.
Shanshan Wang, Carlos A. Cuevas, Udo Frieß, and Alfonso Saiz-Lopez
Atmos. Meas. Tech., 9, 5089–5101, https://doi.org/10.5194/amt-9-5089-2016, https://doi.org/10.5194/amt-9-5089-2016, 2016
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Multi-axis differential optical absorption spectroscopy (MAX-DOAS) measurements were performed in the urban environment of Madrid, Spain, where Sahara dust intrusion sometimes occurs. The study shows a high performances in the retrieval of aerosol optical depth, the surface extinction coefficient and an elevated layer during dust episodes, validated by AERONET in situ and modeling data. It is essential to capture the extinction properties of both local aerosol and Saharan dust.
Óscar Gálvez, M. Teresa Baeza-Romero, Mikel Sanz, and Alfonso Saiz-Lopez
Atmos. Chem. Phys., 16, 12703–12713, https://doi.org/10.5194/acp-16-12703-2016, https://doi.org/10.5194/acp-16-12703-2016, 2016
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Reactive iodine species play a key role in the oxidation capacity of the polar troposphere, although sources and mechanisms are poorly understood. In this paper, the photolysis of frozen iodate salt has been studied, confirming that under near-UV–Vis radiation iodate is photolysed. Incorporating this result into an Antarctic atmospheric model, we have shown that it could increase the atmospheric IO levels and could constitute a pathway for the release of active iodine to the polar atmosphere
Tomás Sherwen, Johan A. Schmidt, Mat J. Evans, Lucy J. Carpenter, Katja Großmann, Sebastian D. Eastham, Daniel J. Jacob, Barbara Dix, Theodore K. Koenig, Roman Sinreich, Ivan Ortega, Rainer Volkamer, Alfonso Saiz-Lopez, Cristina Prados-Roman, Anoop S. Mahajan, and Carlos Ordóñez
Atmos. Chem. Phys., 16, 12239–12271, https://doi.org/10.5194/acp-16-12239-2016, https://doi.org/10.5194/acp-16-12239-2016, 2016
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We present a simulation of tropospheric Cl, Br, I chemistry within the GEOS-Chem CTM. We find a decrease in tropospheric ozone burden of 18.6 % and a 8.2 % decrease in global mean OH concentrations. Cl oxidation of some VOCs range from 15 to 27 % of the total loss. Bromine plays a small role in oxidising oVOCs. Surface ozone, ozone sondes, and methane lifetime are in general improved by the inclusion of halogens. We argue that simulated bromine and chlorine represent a lower limit.
Nicolas-Xavier Geilfus, Ryan J. Galley, Brent G. T. Else, Karley Campbell, Tim Papakyriakou, Odile Crabeck, Marcos Lemes, Bruno Delille, and Søren Rysgaard
The Cryosphere, 10, 2173–2189, https://doi.org/10.5194/tc-10-2173-2016, https://doi.org/10.5194/tc-10-2173-2016, 2016
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The fate of ikaite precipitation within sea ice is poorly understood. In this study, we estimated ikaite precipitation of up to 167 µmol kg-1 within sea ice, while its export and dissolution into the underlying seawater was responsible for a TA increase of 64–66 μmol kg-1. We estimated that more than half of the total ikaite precipitated was still contained in the ice when sea ice began to melt. The dissolution of the ikaite crystals in the water column kept the seawater pCO2 undersaturated.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
T. Sherwen, M. J. Evans, L. J. Carpenter, S. J. Andrews, R. T. Lidster, B. Dix, T. K. Koenig, R. Sinreich, I. Ortega, R. Volkamer, A. Saiz-Lopez, C. Prados-Roman, A. S. Mahajan, and C. Ordóñez
Atmos. Chem. Phys., 16, 1161–1186, https://doi.org/10.5194/acp-16-1161-2016, https://doi.org/10.5194/acp-16-1161-2016, 2016
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Using a global chemical transport model (GEOS-Chem) with additional iodine emissions, chemistry, and deposition we show that iodine is responsible for ~ 9 % of global ozone loss but has negligible impacts on global OH. Uncertainties are large in the chemistry and emissions and future research is needed in both. Measurements of iodine species (especially HOI) would be useful. We believe iodine chemistry should be considered in future chemistry-climate and in air quality modelling.
A. Spolaor, T. Opel, J. R. McConnell, O. J. Maselli, G. Spreen, C. Varin, T. Kirchgeorg, D. Fritzsche, A. Saiz-Lopez, and P. Vallelonga
The Cryosphere, 10, 245–256, https://doi.org/10.5194/tc-10-245-2016, https://doi.org/10.5194/tc-10-245-2016, 2016
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The role of sea ice in the Earth climate system is still under debate, although it is known to influence albedo, ocean circulation, and atmosphere-ocean heat and gas exchange. Here we present a reconstruction of 1950 to 1998 AD sea ice in the Laptev Sea based on the Akademii Nauk ice core (Severnaya Zemlya, Russian Arctic) and halogen measurements. The results suggest a connection between bromine and sea ice, as well as a connection between iodine concentration in snow and summer sea ice.
M. Gil-Ojeda, M. Navarro-Comas, L. Gómez-Martín, J. A. Adame, A. Saiz-Lopez, C. A. Cuevas, Y. González, O. Puentedura, E. Cuevas, J.-F. Lamarque, D. Kinninson, and S. Tilmes
Atmos. Chem. Phys., 15, 10567–10579, https://doi.org/10.5194/acp-15-10567-2015, https://doi.org/10.5194/acp-15-10567-2015, 2015
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The NO2 seasonal evolution in the free troposphere (FT) has been established for the first time, based on a remote sensing technique (MAXDOAS) and thus avoiding the problems of the local pollution of in situ instruments. A clear seasonality has been found, with background levels of 20-40pptv. Evidence has been found on fast, direct injection of surface air into the free troposphere. This result might have implications on the FT distribution of halogens and other species with marine sources.
A. Saiz-Lopez, C. S. Blaszczak-Boxe, and L. J. Carpenter
Atmos. Chem. Phys., 15, 9731–9746, https://doi.org/10.5194/acp-15-9731-2015, https://doi.org/10.5194/acp-15-9731-2015, 2015
S. Kang, F. Wang, U. Morgenstern, Y. Zhang, B. Grigholm, S. Kaspari, M. Schwikowski, J. Ren, T. Yao, D. Qin, and P. A. Mayewski
The Cryosphere, 9, 1213–1222, https://doi.org/10.5194/tc-9-1213-2015, https://doi.org/10.5194/tc-9-1213-2015, 2015
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N.-X. Geilfus, R. J. Galley, O. Crabeck, T. Papakyriakou, J. Landy, J.-L. Tison, and S. Rysgaard
Biogeosciences, 12, 2047–2061, https://doi.org/10.5194/bg-12-2047-2015, https://doi.org/10.5194/bg-12-2047-2015, 2015
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We investigated the evolution of inorganic carbon within landfast sea ice in Resolute Passage during the spring and summer melt period.
Low TA and TCO2 concentrations observed in sea ice and brine were associated with the percolation of meltwater from melt ponds. Meltwater was continuously supplied to the ponds which prevented melt ponds from fully equilibrating with the atmospheric CO2 concentration, promoting a continuous uptake of CO2 from the atmosphere.
F. Slemr, H. Angot, A. Dommergue, O. Magand, M. Barret, A. Weigelt, R. Ebinghaus, E.-G. Brunke, K. A. Pfaffhuber, G. Edwards, D. Howard, J. Powell, M. Keywood, and F. Wang
Atmos. Chem. Phys., 15, 3125–3133, https://doi.org/10.5194/acp-15-3125-2015, https://doi.org/10.5194/acp-15-3125-2015, 2015
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• Longer-term mercury measurement in the Southern Hemisphere is compared.
• Mercury, in terms of monthly and annual medians and averages, is more evenly distributed than hitherto believed.
• Consequently, trends observed at one or a few sites are likely to be representative of the whole hemisphere, and smaller trends can be detected in shorter time periods.
• We report a change in the trend sign at Cape Point from decreasing mercury concentrations in 1996-2004 to increasing ones since 2007.
C. Prados-Roman, C. A. Cuevas, R. P. Fernandez, D. E. Kinnison, J-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 15, 2215–2224, https://doi.org/10.5194/acp-15-2215-2015, https://doi.org/10.5194/acp-15-2215-2015, 2015
N.-X. Geilfus, J.-L. Tison, S. F. Ackley, R. J. Galley, S. Rysgaard, L. A. Miller, and B. Delille
The Cryosphere, 8, 2395–2407, https://doi.org/10.5194/tc-8-2395-2014, https://doi.org/10.5194/tc-8-2395-2014, 2014
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Temporal evolution of pCO2 profiles in sea ice in the Bellingshausen Sea, Antarctica (Oct. 2007), shows that physical and thermodynamic processes control the CO2 system in the ice. We show that each cooling/warming event was associated with an increase/decrease in the brine salinity, TA, TCO2, and in situ brine and bulk ice pCO2. Thicker snow covers reduced the amplitude of these changes. Both brine and bulk ice pCO2 were undersaturated, causing the sea ice to act as a sink for atmospheric CO2.
R. P. Fernandez, R. J. Salawitch, D. E. Kinnison, J.-F. Lamarque, and A. Saiz-Lopez
Atmos. Chem. Phys., 14, 13391–13410, https://doi.org/10.5194/acp-14-13391-2014, https://doi.org/10.5194/acp-14-13391-2014, 2014
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We propose the existence of a daytime “tropical ring of atomic bromine” surrounding the tropics at a height between 15 and 19km. Our simulations show that VSL bromocarbons produce increases of 3pptv for inorganic bromine and 2pptv for organic bromine in the tropical TTL on an annual average, resulting in a total stratospheric bromine injection of 5pptv. This result suggests that the inorganic bromine injected into the stratosphere may be larger than that from VSL bromocarbons.
A. Saiz-Lopez, R. P. Fernandez, C. Ordóñez, D. E. Kinnison, J. C. Gómez Martín, J.-F. Lamarque, and S. Tilmes
Atmos. Chem. Phys., 14, 13119–13143, https://doi.org/10.5194/acp-14-13119-2014, https://doi.org/10.5194/acp-14-13119-2014, 2014
O. Crabeck, B. Delille, D. Thomas, N.-X. Geilfus, S. Rysgaard, and J.-L. Tison
Biogeosciences, 11, 6525–6538, https://doi.org/10.5194/bg-11-6525-2014, https://doi.org/10.5194/bg-11-6525-2014, 2014
S. Rysgaard, F. Wang, R. J. Galley, R. Grimm, D. Notz, M. Lemes, N.-X. Geilfus, A. Chaulk, A. A. Hare, O. Crabeck, B. G. T. Else, K. Campbell, L. L. Sørensen, J. Sievers, and T. Papakyriakou
The Cryosphere, 8, 1469–1478, https://doi.org/10.5194/tc-8-1469-2014, https://doi.org/10.5194/tc-8-1469-2014, 2014
S. M. MacDonald, J. C. Gómez Martín, R. Chance, S. Warriner, A. Saiz-Lopez, L. J. Carpenter, and J. M. C. Plane
Atmos. Chem. Phys., 14, 5841–5852, https://doi.org/10.5194/acp-14-5841-2014, https://doi.org/10.5194/acp-14-5841-2014, 2014
J. Zhou, J.-L. Tison, G. Carnat, N.-X. Geilfus, and B. Delille
The Cryosphere, 8, 1019–1029, https://doi.org/10.5194/tc-8-1019-2014, https://doi.org/10.5194/tc-8-1019-2014, 2014
M. J. Lawler, A. S. Mahajan, A. Saiz-Lopez, and E. S. Saltzman
Atmos. Chem. Phys., 14, 2669–2678, https://doi.org/10.5194/acp-14-2669-2014, https://doi.org/10.5194/acp-14-2669-2014, 2014
F. Wang, A. Saiz-Lopez, A. S. Mahajan, J. C. Gómez Martín, D. Armstrong, M. Lemes, T. Hay, and C. Prados-Roman
Atmos. Chem. Phys., 14, 1323–1335, https://doi.org/10.5194/acp-14-1323-2014, https://doi.org/10.5194/acp-14-1323-2014, 2014
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
A. S. Mahajan, J. C. Gómez Martín, T. D. Hay, S.-J. Royer, S. Yvon-Lewis, Y. Liu, L. Hu, C. Prados-Roman, C. Ordóñez, J. M. C. Plane, and A. Saiz-Lopez
Atmos. Chem. Phys., 12, 11609–11617, https://doi.org/10.5194/acp-12-11609-2012, https://doi.org/10.5194/acp-12-11609-2012, 2012
Related subject area
Subject: Gases | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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
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
Secondary reactions of aromatics-derived oxygenated organic molecules lead to plentiful highly oxygenated organic molecules within an intraday OH exposure
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
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
Volatile organic compound emissions from solvent- and water-borne coatings – compositional differences and tracer compound identifications
Evaluated kinetic and photochemical data for atmospheric chemistry: volume VIII – gas-phase reactions of organic species with four, or more, carbon atoms ( ≥ C4)
Chemical characterisation of benzene oxidation products under high- and low-NOx conditions using chemical ionisation mass spectrometry
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.
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.
Yuwei Wang, Yueyang Li, Gan Yang, Xueyan Yang, Yizhen Wu, Chuang Li, Lei Yao, Hefeng Zhang, and Lin Wang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1702, https://doi.org/10.5194/egusphere-2023-1702, 2023
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The formation and evolution mechanisms of aromatics-derived highly oxygenated organic molecules (HOMs) is essential to understanding 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 on HOMs and potentially explains the existing gap between model prediction and ambient measurement on the HOMs concentrations.
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.
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
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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.
Chelsea E. Stockwell, Matthew M. Coggon, Georgios I. Gkatzelis, John Ortega, Brian C. McDonald, Jeff Peischl, Kenneth Aikin, Jessica B. Gilman, Michael Trainer, and Carsten Warneke
Atmos. Chem. Phys., 21, 6005–6022, https://doi.org/10.5194/acp-21-6005-2021, https://doi.org/10.5194/acp-21-6005-2021, 2021
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Volatile chemical products are emerging as a large source of petrochemical organics in urban environments. We identify markers for the coatings category by linking ambient observations to laboratory measurements, investigating volatile organic compound (VOC) composition, and quantifying key VOC emissions via controlled evaporation experiments. Ingredients and sales surveys are used to confirm the prevalence and usage trends to support the assignment of water and solvent-borne coating tracers.
Abdelwahid Mellouki, Markus Ammann, R. Anthony Cox, John N. Crowley, Hartmut Herrmann, Michael E. Jenkin, V. Faye McNeill, Jürgen Troe, and Timothy J. Wallington
Atmos. Chem. Phys., 21, 4797–4808, https://doi.org/10.5194/acp-21-4797-2021, https://doi.org/10.5194/acp-21-4797-2021, 2021
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Volatile organic compounds play an important role in atmospheric chemistry. This article, the eighth in the series, presents kinetic and photochemical data sheets evaluated by the IUPAC Task Group on Atmospheric Chemical Kinetic Data Evaluation. It covers the gas-phase reactions of organic species with four, or more, carbon atoms (≥ C4) including thermal reactions of closed-shell organic species with HO and NO3 radicals and their photolysis. These data are important for atmospheric models.
Michael Priestley, Thomas J. Bannan, Michael Le Breton, Stephen D. Worrall, Sungah Kang, Iida Pullinen, Sebastian Schmitt, Ralf Tillmann, Einhard Kleist, Defeng Zhao, Jürgen Wildt, Olga Garmash, Archit Mehra, Asan Bacak, Dudley E. Shallcross, Astrid Kiendler-Scharr, Åsa M. Hallquist, Mikael Ehn, Hugh Coe, Carl J. Percival, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 21, 3473–3490, https://doi.org/10.5194/acp-21-3473-2021, https://doi.org/10.5194/acp-21-3473-2021, 2021
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A significant fraction of emissions from human activity consists of aromatic hydrocarbons, e.g. benzene, which oxidise to form new compounds important for particle growth. Characterisation of benzene oxidation products highlights the range of species produced as well as their chemical properties and contextualises them within relevant frameworks, e.g. MCM. Cluster analysis of the oxidation product time series distinguishes behaviours of CHON compounds that could aid in identifying functionality.
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Short summary
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.
Every spring in the Arctic, a series of photochemical events occur over the ice-covered ocean,...
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