Articles | Volume 16, issue 3
https://doi.org/10.5194/acp-16-1747-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/acp-16-1747-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Secondary organic aerosol formation from isoprene photooxidation during cloud condensation–evaporation cycles
L. Brégonzio-Rozier
CORRESPONDING AUTHOR
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
C. Giorio
Department of Chemistry, University of Cambridge,
Cambridge CB2 1EW, UK
Dipartimento di Scienze Chimiche, Università degli
Studi di Padova, Padova, 35131, Italy
F. Siekmann
Aix-Marseille Université, CNRS, LCE FRE 3416, 13331,
Marseille, France
E. Pangui
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
S. B. Morales
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
B. Temime-Roussel
Aix-Marseille Université, CNRS, LCE FRE 3416, 13331,
Marseille, France
A. Gratien
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
V. Michoud
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
M. Cazaunau
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
H. L. DeWitt
Aix-Marseille Université, CNRS, LCE FRE 3416, 13331,
Marseille, France
A. Tapparo
Dipartimento di Scienze Chimiche, Università degli
Studi di Padova, Padova, 35131, Italy
A. Monod
CORRESPONDING AUTHOR
Aix-Marseille Université, CNRS, LCE FRE 3416, 13331,
Marseille, France
J.-F. Doussin
Laboratoire Interuniversitaire des Systèmes
Atmosphériques (LISA), UMR7583, CNRS,
Université Paris-Est-Créteil (UPEC) et Université Paris Diderot
(UPD), Institut Pierre Simon
Laplace (IPSL), Créteil, France
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First- and higher order -generation products formed from the oxidation of isoprene and methacrolein with OH radicals in the presence of NOx have been studied in a simulation chamber. Differences in light source are proposed to partially explain the discrepancies observed between different studies in the literature for both isoprene- and methacrolein-SOA mass yields. According to our results, these SOA yields in the atmosphere could be lower than suggested by most of the current chamber studies.
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Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Sylvain Ravier, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 23, 5851–5866, https://doi.org/10.5194/acp-23-5851-2023, https://doi.org/10.5194/acp-23-5851-2023, 2023
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Atmos. Meas. Tech., 15, 3859–3874, https://doi.org/10.5194/amt-15-3859-2022, https://doi.org/10.5194/amt-15-3859-2022, 2022
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This work quantified and tentatively identified the organic impurities on ammonium sulfate aerosols generated in the laboratory. They are likely low volatile and high mass molecules containing oxygen, nitrogen, and/or sulfur. Our results show that these organic impurities likely originate from the commercial AS crystals. It is recommended to use AS seeds with caution, especially when small particles are used, in terms of AS purity and water purity when aqueous solutions are used for atomization.
Karine Desboeufs, Franck Fu, Matthieu Bressac, Antonio Tovar-Sánchez, Sylvain Triquet, Jean-François Doussin, Chiara Giorio, Patrick Chazette, Julie Disnaquet, Anaïs Feron, Paola Formenti, Franck Maisonneuve, Araceli Rodríguez-Romero, Pascal Zapf, François Dulac, and Cécile Guieu
Atmos. Chem. Phys., 22, 2309–2332, https://doi.org/10.5194/acp-22-2309-2022, https://doi.org/10.5194/acp-22-2309-2022, 2022
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This article reports the first concurrent sampling of wet deposition samples and surface seawater and was performed during the PEACETIME cruise in the remote Mediterranean (May–June 2017). Through the chemical composition of trace metals (TMs) in these samples, it emphasizes the decrease of atmospheric metal pollution in this area during the last few decades and the critical role of wet deposition as source of TMs for Mediterranean surface seawater, especially for intense dust deposition events.
Boris Vansevenant, Cédric Louis, Corinne Ferronato, Ludovic Fine, Patrick Tassel, Pascal Perret, Evangelia Kostenidou, Brice Temime-Roussel, Barbara D'Anna, Karine Sartelet, Véronique Cerezo, and Yao Liu
Atmos. Meas. Tech., 14, 7627–7655, https://doi.org/10.5194/amt-14-7627-2021, https://doi.org/10.5194/amt-14-7627-2021, 2021
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Alexandre Kukui, Michel Chartier, Jinhe Wang, Hui Chen, Sébastien Dusanter, Stéphane Sauvage, Vincent Michoud, Nadine Locoge, Valérie Gros, Thierry Bourrianne, Karine Sellegri, and Jean-Marc Pichon
Atmos. Chem. Phys., 21, 13333–13351, https://doi.org/10.5194/acp-21-13333-2021, https://doi.org/10.5194/acp-21-13333-2021, 2021
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Sulfuric acid, H2SO4, plays a key role in formation of secondary atmospheric aerosol particles. It is generally accepted that the major atmospheric source of H2SO4 is the reaction of OH radicals with SO2. In this study, importance of an additional H2SO4 source via oxidation of SO2 by stabilized Criegee intermediates was estimated based on measurements at a remote site on Cape Corsica. It was found that the oxidation of SO2 by SCI may be an important source of H2SO4, especially during nighttime.
Hongming Yi, Mathieu Cazaunau, Aline Gratien, Vincent Michoud, Edouard Pangui, Jean-Francois Doussin, and Weidong Chen
Atmos. Meas. Tech., 14, 5701–5715, https://doi.org/10.5194/amt-14-5701-2021, https://doi.org/10.5194/amt-14-5701-2021, 2021
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HONO and NO2 play a crucial role in the atmospheric oxidation capacity that affects the regional air quality and global climate. Accurate measurements of HONO are challenging due to the drawback of existing detection methods. Calibration-free high-sensitivity direct, simultaneous measurements of NO2, HONO and CH2O with UV-IBBCEAS provide accurate and fast quantitative analysis of their concentration variation within their lifetime by intercomparison with NOx, FTIR and NitroMAC sensors.
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Atmos. Chem. Phys., 21, 10911–10937, https://doi.org/10.5194/acp-21-10911-2021, https://doi.org/10.5194/acp-21-10911-2021, 2021
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Benjamin Chazeau, Brice Temime-Roussel, Grégory Gille, Boualem Mesbah, Barbara D'Anna, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 21, 7293–7319, https://doi.org/10.5194/acp-21-7293-2021, https://doi.org/10.5194/acp-21-7293-2021, 2021
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The temporal trends in the chemical composition and particle number of the submicron aerosols in a Mediterranean city, Marseille, are investigated over 14 months. Fifteen days were found to exceed the WHO PM2.5 daily limit (25 µg m−3) only during the cold period, with two distinct origins: local pollution events with an increased fraction of the carbonaceous fraction due to domestic wood burning and long-range pollution events with a high level of oxygenated organic aerosol and ammonium nitrate.
Juan Miguel González-Sánchez, Nicolas Brun, Junteng Wu, Julien Morin, Brice Temime-Roussel, Sylvain Ravier, Camille Mouchel-Vallon, Jean-Louis Clément, and Anne Monod
Atmos. Chem. Phys., 21, 4915–4937, https://doi.org/10.5194/acp-21-4915-2021, https://doi.org/10.5194/acp-21-4915-2021, 2021
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Organic nitrates play a crucial role in air pollution as they are considered NOx reservoirs. This work lights up the importance of their reactions with OH radicals in the aqueous phase (cloud/fog, wet aerosol), which is slower than in the gas phase. For compounds that significantly partition in water such as polyfunctional biogenic nitrates, these aqueous-phase reactions should drive their atmospheric removal, leading to a broader spatial distribution of NOx than previously accounted for.
Evangelia Kostenidou, Alvaro Martinez-Valiente, Badr R'Mili, Baptiste Marques, Brice Temime-Roussel, Amandine Durand, Michel André, Yao Liu, Cédric Louis, Boris Vansevenant, Daniel Ferry, Carine Laffon, Philippe Parent, and Barbara D'Anna
Atmos. Chem. Phys., 21, 4779–4796, https://doi.org/10.5194/acp-21-4779-2021, https://doi.org/10.5194/acp-21-4779-2021, 2021
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Passenger vehicle emissions can be a significant source of particulate matter in urban areas. In this study the particle-phase emissions of seven Euro 5 passenger vehicles were characterized. Changes in engine technologies and after-treatment devices can alter the chemical composition and the size of the emitted particulate matter. The condition of the diesel particle filter (DPF) plays an important role in the emitted pollutants.
Danitza Klopper, Paola Formenti, Andreas Namwoonde, Mathieu Cazaunau, Servanne Chevaillier, Anaïs Feron, Cécile Gaimoz, Patrick Hease, Fadi Lahmidi, Cécile Mirande-Bret, Sylvain Triquet, Zirui Zeng, and Stuart J. Piketh
Atmos. Chem. Phys., 20, 15811–15833, https://doi.org/10.5194/acp-20-15811-2020, https://doi.org/10.5194/acp-20-15811-2020, 2020
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The chemical composition of aerosol particles is very important as it determines to which extent they can affect the Earth's climate by acting with solar light and modifying the properties of clouds. The South Atlantic region is a remote and under-explored region to date where these effects could be important. The measurements presented in this paper consist in the analysis of samples collected at a coastal site in Namibia. The first long-term source apportionment is presented and discussed.
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Jean-François Doussin, and Bénédicte Picquet-Varrault
Atmos. Chem. Phys., 20, 15167–15189, https://doi.org/10.5194/acp-20-15167-2020, https://doi.org/10.5194/acp-20-15167-2020, 2020
Axel Fouqueau, Manuela Cirtog, Mathieu Cazaunau, Edouard Pangui, Pascal Zapf, Guillaume Siour, Xavier Landsheere, Guillaume Méjean, Daniele Romanini, and Bénédicte Picquet-Varrault
Atmos. Meas. Tech., 13, 6311–6323, https://doi.org/10.5194/amt-13-6311-2020, https://doi.org/10.5194/amt-13-6311-2020, 2020
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An incoherent broadband cavity-enhanced absorption spectroscopy (IBBCEAS) technique has been developed for the in situ monitoring of NO3 radicals in the CSA simulation chamber at LISA. The optical cavity allows a high sensitivity for NO3 detection up to 6 ppt for an integration time of 10 s. The technique is now fully operational and can be used to determine rate constants for fast reactions involving complex volatile organic compounds (with rate constants up to 10−10 cm3 molecule−1 s−1).
Clarissa Baldo, Paola Formenti, Sophie Nowak, Servanne Chevaillier, Mathieu Cazaunau, Edouard Pangui, Claudia Di Biagio, Jean-Francois Doussin, Konstantin Ignatyev, Pavla Dagsson-Waldhauserova, Olafur Arnalds, A. Robert MacKenzie, and Zongbo Shi
Atmos. Chem. Phys., 20, 13521–13539, https://doi.org/10.5194/acp-20-13521-2020, https://doi.org/10.5194/acp-20-13521-2020, 2020
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We showed that Icelandic dust has a fundamentally different chemical and mineralogical composition from low-latitude dust. In particular, magnetite is as high as 1 %–2 % of the total dust mass. Our results suggest that Icelandic dust may have an important impact on the radiation balance in the subpolar and polar regions.
James Brean, David C. S. Beddows, Zongbo Shi, Brice Temime-Roussel, Nicolas Marchand, Xavier Querol, Andrés Alastuey, María Cruz Minguillón, and Roy M. Harrison
Atmos. Chem. Phys., 20, 10029–10045, https://doi.org/10.5194/acp-20-10029-2020, https://doi.org/10.5194/acp-20-10029-2020, 2020
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New particle formation is a key process influencing both local air quality and climatically active cloud condensation nuclei concentrations. This study has carried out fundamental measurements of nucleation processes in Barcelona, Spain, and concludes that a mechanism involving stabilisation of sulfuric acid clusters by low molecular weight amines is primarily responsible for new particle formation events.
David O. De Haan, Lelia N. Hawkins, Kevin Jansen, Hannah G. Welsh, Raunak Pednekar, Alexia de Loera, Natalie G. Jimenez, Margaret A. Tolbert, Mathieu Cazaunau, Aline Gratien, Antonin Bergé, Edouard Pangui, Paola Formenti, and Jean-François Doussin
Atmos. Chem. Phys., 20, 9581–9590, https://doi.org/10.5194/acp-20-9581-2020, https://doi.org/10.5194/acp-20-9581-2020, 2020
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When exposed to glyoxal in chamber experiments, dry ammonium or methylammonium sulfate particles turn brown immediately and reversibly without increasing in size. Much less browning was observed on wet aerosol particles, and no browning was observed with sodium sulfate aerosol. While estimated dry aerosol light absorption caused by background glyoxal (70 ppt) is insignificant compared to that of secondary brown carbon overall, in polluted regions this process could be a source of brown carbon.
August Andersson, Elena N. Kirillova, Stefano Decesari, Langley DeWitt, Jimmy Gasore, Katherine E. Potter, Ronald G. Prinn, Maheswar Rupakheti, Jean de Dieu Ndikubwimana, Julius Nkusi, and Bonfils Safari
Atmos. Chem. Phys., 20, 4561–4573, https://doi.org/10.5194/acp-20-4561-2020, https://doi.org/10.5194/acp-20-4561-2020, 2020
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Large-scale biomass burning events seasonally cover sub-Saharan Africa with air particles. In this study, we find that the concentrations of these particles at a remote mountain site in Rwanda may increase by a factor of 10 during such dry biomass burning periods, with strong implications for the regional climate and human health. These results provide quantitative constraints that could contribute to reducing the large uncertainties regarding the environmental impact of these fires.
Bénédicte Picquet-Varrault, Ricardo Suarez-Bertoa, Marius Duncianu, Mathieu Cazaunau, Edouard Pangui, Marc David, and Jean-François Doussin
Atmos. Chem. Phys., 20, 487–498, https://doi.org/10.5194/acp-20-487-2020, https://doi.org/10.5194/acp-20-487-2020, 2020
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Multifunctional organic nitrates are important atmospheric species that are known to play a key role in the transport of reactive nitrogen and in aerosol composition. However, very little is known about their atmospheric reactivity. Here we provide an experimental study on the photolysis and reaction of two carbonyl nitrates with OH radicals. Atmospheric implications and the influence of the chemical structure on the reactivity are discussed.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Atmos. Chem. Phys., 19, 15503–15531, https://doi.org/10.5194/acp-19-15503-2019, https://doi.org/10.5194/acp-19-15503-2019, 2019
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This paper presents a new dataset of laboratory measurements of the shortwave (SW) spectral complex refractive index and single-scattering albedo (SSA) for global mineral dust aerosols of varying origin and composition. Our results show that the dust refractive index and SSA vary strongly from source to source, mostly due to particle iron content changes. We recommend that source-dependent values of the SW spectral refractive index and SSA be used in models and remote sensing applications.
Patrick Chazette, Cyrille Flamant, Julien Totems, Marco Gaetani, Gwendoline Smith, Alexandre Baron, Xavier Landsheere, Karine Desboeufs, Jean-François Doussin, and Paola Formenti
Atmos. Chem. Phys., 19, 14979–15005, https://doi.org/10.5194/acp-19-14979-2019, https://doi.org/10.5194/acp-19-14979-2019, 2019
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Evolution of the vertical distribution and optical properties of aerosols in the free troposphere is analysed for the first time over the Namibian coast, a region where uncertainties on aerosol–cloud coupling in climate simulations are significant. The high variability of atmospheric aerosol composition is highlighted using a combination of ground-based, airborne and space-borne lidar. Aerosols are mainly transported from Angola, but part of the highest aerosol layer may come from South America.
Marc D. Mallet, Barbara D'Anna, Aurélie Même, Maria Chiara Bove, Federico Cassola, Giandomenico Pace, Karine Desboeufs, Claudia Di Biagio, Jean-Francois Doussin, Michel Maille, Dario Massabò, Jean Sciare, Pascal Zapf, Alcide Giorgio di Sarra, and Paola Formenti
Atmos. Chem. Phys., 19, 11123–11142, https://doi.org/10.5194/acp-19-11123-2019, https://doi.org/10.5194/acp-19-11123-2019, 2019
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We present findings from a summertime field campaign at the remote island of Lampedusa in the central Mediterranean Sea. We show that the aerosol loading is similar to coastal sites around the Mediterranean. We observe higher loadings of sulfate and aged organic aerosol from air masses transported over the central and eastern Mediterranean in comparison to those from the western Mediterranean. These results highlight the rarity of pristine air masses, even in remote marine environments.
H. Langley DeWitt, Jimmy Gasore, Maheswar Rupakheti, Katherine E. Potter, Ronald G. Prinn, Jean de Dieu Ndikubwimana, Julius Nkusi, and Bonfils Safari
Atmos. Chem. Phys., 19, 2063–2078, https://doi.org/10.5194/acp-19-2063-2019, https://doi.org/10.5194/acp-19-2063-2019, 2019
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Air quality in rapidly developing East Africa is a growing but understudied concern. We analyzed long-term black carbon, carbon monoxide, and ozone measurements from the remote Rwanda Climate Observatory and found that seasonal regional biomass burning raised black carbon levels to above-urban concentrations 6 months out of the year. Additional local pollution could exacerbate this issue. More regional monitoring needs to be done to understand and reduce air pollution in this region.
Paola Formenti, Stuart John Piketh, Andreas Namwoonde, Danitza Klopper, Roelof Burger, Mathieu Cazaunau, Anaïs Feron, Cécile Gaimoz, Stephen Broccardo, Nicola Walton, Karine Desboeufs, Guillaume Siour, Mattheus Hanghome, Samuel Mafwila, Edosa Omoregie, Wolfgang Junkermann, and Willy Maenhaut
Atmos. Chem. Phys., 18, 17003–17016, https://doi.org/10.5194/acp-18-17003-2018, https://doi.org/10.5194/acp-18-17003-2018, 2018
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Three-years of continuous measurements at the Henties Bay Aerosol Observatory (HBAO; 22°S, 14°05’E), Namibia, show that during the austral wintertime, long- and medium-range transport of pollution from biomass and fossil fuel burning give rise to peaks of light-absorbing black carbon aerosols into the marine boundary layer ahead of the main biomass burning season. This could affect the cloud properties.
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.
Dario Massabò, Silvia Giulia Danelli, Paolo Brotto, Antonio Comite, Camilla Costa, Andrea Di Cesare, Jean François Doussin, Federico Ferraro, Paola Formenti, Elena Gatta, Laura Negretti, Maddalena Oliva, Franco Parodi, Luigi Vezzulli, and Paolo Prati
Atmos. Meas. Tech., 11, 5885–5900, https://doi.org/10.5194/amt-11-5885-2018, https://doi.org/10.5194/amt-11-5885-2018, 2018
Vincent Michoud, Stéphane Sauvage, Thierry Léonardis, Isabelle Fronval, Alexandre Kukui, Nadine Locoge, and Sébastien Dusanter
Atmos. Meas. Tech., 11, 5729–5740, https://doi.org/10.5194/amt-11-5729-2018, https://doi.org/10.5194/amt-11-5729-2018, 2018
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This study presents the first measurements of ambient methylglyoxal, an important atmospheric α-dicarbonyl, using proton transfer reaction time-of-flight mass spectrometry. These measurements mostly agree with concomitant measurements from a reference technique: the DNPH derivatization technique and high-performance liquid chromatography with UV detection. In addition, a careful investigation of the differences between the two techniques is carried out to explain the disagreements observed.
Anne-Cyrielle Genard-Zielinski, Christophe Boissard, Elena Ormeño, Juliette Lathière, Ilja M. Reiter, Henri Wortham, Jean-Philippe Orts, Brice Temime-Roussel, Bertrand Guenet, Svenja Bartsch, Thierry Gauquelin, and Catherine Fernandez
Biogeosciences, 15, 4711–4730, https://doi.org/10.5194/bg-15-4711-2018, https://doi.org/10.5194/bg-15-4711-2018, 2018
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From seasonal in situ observations on how a Mediterranean ecosystem responds to drought, a specific isoprene emission (ER, emission rates) algorithm was developed, upon which 2100 projections (IPCC RCP2.6 and RCP8.5 scenarios) were made. Emission rates were found to be mainly sensitive to future temperature changes and poorly represented by current empirical emission models. Drought was found to aggravate thermal stress on emission rates.
Amelie Bertrand, Giulia Stefenelli, Simone M. Pieber, Emily A. Bruns, Brice Temime-Roussel, Jay G. Slowik, Henri Wortham, André S. H. Prévôt, Imad El Haddad, and Nicolas Marchand
Atmos. Chem. Phys., 18, 10915–10930, https://doi.org/10.5194/acp-18-10915-2018, https://doi.org/10.5194/acp-18-10915-2018, 2018
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We model the evolution of several BBOA markers including levoglucosan during aging experiments conducted in an atmospheric Teflon chamber, in order to evaluate the influence of vapor wall loss on the determination of the rate constants of the compounds with hydroxyl radicals (OH).
Amelie Bertrand, Giulia Stefenelli, Coty N. Jen, Simone M. Pieber, Emily A. Bruns, Haiyan Ni, Brice Temime-Roussel, Jay G. Slowik, Allen H. Goldstein, Imad El Haddad, Urs Baltensperger, André S. H. Prévôt, Henri Wortham, and Nicolas Marchand
Atmos. Chem. Phys., 18, 7607–7624, https://doi.org/10.5194/acp-18-7607-2018, https://doi.org/10.5194/acp-18-7607-2018, 2018
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A thermal desorption aerosol gas chromatograph coupled to an aerosol mass spectrometer (TAG–AMS) is connected to an atmospheric chamber. The setup serves the quantitative study of the impact of combustion conditions and atmospheric aging on the chemical fingerprint at the molecular level of biomass burning organic aerosol.
Arineh Cholakian, Matthias Beekmann, Augustin Colette, Isabelle Coll, Guillaume Siour, Jean Sciare, Nicolas Marchand, Florian Couvidat, Jorge Pey, Valerie Gros, Stéphane Sauvage, Vincent Michoud, Karine Sellegri, Aurélie Colomb, Karine Sartelet, Helen Langley DeWitt, Miriam Elser, André S. H. Prévot, Sonke Szidat, and François Dulac
Atmos. Chem. Phys., 18, 7287–7312, https://doi.org/10.5194/acp-18-7287-2018, https://doi.org/10.5194/acp-18-7287-2018, 2018
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In this work, four schemes for the simulation of organic aerosols in the western Mediterranean basin are added to the CHIMERE chemistry–transport model; the resulting simulations are then compared to measurements obtained from ChArMEx. It is concluded that the scheme taking into account the fragmentation and the formation of nonvolatile organic aerosols corresponds better to measurements; the major source of this aerosol in the western Mediterranean is found to be of biogenic origin.
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.
Allison N. Schwier, Karine Sellegri, Sébastien Mas, Bruno Charrière, Jorge Pey, Clémence Rose, Brice Temime-Roussel, Jean-Luc Jaffrezo, David Parin, David Picard, Mickael Ribeiro, Greg Roberts, Richard Sempéré, Nicolas Marchand, and Barbara D'Anna
Atmos. Chem. Phys., 17, 14645–14660, https://doi.org/10.5194/acp-17-14645-2017, https://doi.org/10.5194/acp-17-14645-2017, 2017
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In the present paper, we quantify sea-to-air emission fluxes of aerosol to the atmosphere and characterize their physical and chemical properties as a function of the seawater biochemical and physical properties. Fluxes are evaluated with an original approach, a "lab in the field" experiment that preserves the seawater and atmospheric complexity while isolating air-to-sea exchanges from their surroundings. We show different features of the aerosol emission fluxes compared to previous findings.
Peter J. Gallimore, Chiara Giorio, Brendan M. Mahon, and Markus Kalberer
Atmos. Chem. Phys., 17, 14485–14500, https://doi.org/10.5194/acp-17-14485-2017, https://doi.org/10.5194/acp-17-14485-2017, 2017
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This work helps to better understand the potential climate and health impacts of airborne aerosol particles. We applied a new technique to provide a diagnostic fingerprint of the organic compounds present in aerosols. We followed changes in this fingerprint over time in lab experiments which mimic the conversion of plant emissions into aerosols. Our results compare well with computer simulations of the reactions and we conclude that the technique merits continuing use and development in future.
Hendrik Fuchs, Anna Novelli, Michael Rolletter, Andreas Hofzumahaus, Eva Y. Pfannerstill, Stephan Kessel, Achim Edtbauer, Jonathan Williams, Vincent Michoud, Sebastien Dusanter, Nadine Locoge, Nora Zannoni, Valerie Gros, Francois Truong, Roland Sarda-Esteve, Danny R. Cryer, Charlotte A. Brumby, Lisa K. Whalley, Daniel Stone, Paul W. Seakins, Dwayne E. Heard, Coralie Schoemaecker, Marion Blocquet, Sebastien Coudert, Sebastien Batut, Christa Fittschen, Alexander B. Thames, William H. Brune, Cheryl Ernest, Hartwig Harder, Jennifer B. A. Muller, Thomas Elste, Dagmar Kubistin, Stefanie Andres, Birger Bohn, Thorsten Hohaus, Frank Holland, Xin Li, Franz Rohrer, Astrid Kiendler-Scharr, Ralf Tillmann, Robert Wegener, Zhujun Yu, Qi Zou, and Andreas Wahner
Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, https://doi.org/10.5194/amt-10-4023-2017, 2017
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Hydroxyl radical reactivity (k(OH)) is closely related to processes that lead to the formation of oxidised, secondary pollutants such as ozone and aerosol. In order to compare the performances of instruments measuring k(OH), experiments were conducted in the simulation chamber SAPHIR. Chemical conditions were chosen either to be representative of the atmosphere or to test potential limitations of instruments. Overall, the results show that instruments are capable of measuring k(OH).
Nora Zannoni, Valerie Gros, Roland Sarda Esteve, Cerise Kalogridis, Vincent Michoud, Sebastien Dusanter, Stephane Sauvage, Nadine Locoge, Aurelie Colomb, and Bernard Bonsang
Atmos. Chem. Phys., 17, 12645–12658, https://doi.org/10.5194/acp-17-12645-2017, https://doi.org/10.5194/acp-17-12645-2017, 2017
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Our paper presents results of hydroxyl radical (OH) reactivity from a field study conducted during summer 2013 in a western Mediterranean coastal site (Corsica, France). Here, the total OH reactivity, measured with the comparative reactivity method, is compared with the summed OH reactivity from the reactive gases measured with a multitude of different technologies. Our results demonstrate the relatively high observed reactivity and the large impact of biogenic compounds.
Peter J. Gallimore, Brendan M. Mahon, Francis P. H. Wragg, Stephen J. Fuller, Chiara Giorio, Ivan Kourtchev, and Markus Kalberer
Atmos. Chem. Phys., 17, 9853–9868, https://doi.org/10.5194/acp-17-9853-2017, https://doi.org/10.5194/acp-17-9853-2017, 2017
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Limonene is emitted in substantial quantities by plants, and also has indoor sources from
air freshenersand cleaning products. We studied particle formation from the oxidation of limonene and found substantial quantities of oxidising components which are thought to be associated with the negative health effects of particulates. State-of-the-art measurements of the products of limonene–ozone chemistry were also presented.
Claudia Di Biagio, Paola Formenti, Mathieu Cazaunau, Edouard Pangui, Nicolas Marchand, and Jean-François Doussin
Atmos. Meas. Tech., 10, 2923–2939, https://doi.org/10.5194/amt-10-2923-2017, https://doi.org/10.5194/amt-10-2923-2017, 2017
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Mineral dust is one of the most abundant aerosol species at the global scale and an accurate estimation of its absorption at solar wavelengths is crucial to assess its impact on climate. In this work we provide an estimate of the Aethalometer multiple scattering correction for mineral dust aerosols at 450 and 660 nm. Our results suggest that the use of an optimized correction factor can lead to up to 11 % higher absorption coefficient and to 3 % higher single scattering albedo for mineral dust.
Vincent Michoud, Jean Sciare, Stéphane Sauvage, Sébastien Dusanter, Thierry Léonardis, Valérie Gros, Cerise Kalogridis, Nora Zannoni, Anaïs Féron, Jean-Eudes Petit, Vincent Crenn, Dominique Baisnée, Roland Sarda-Estève, Nicolas Bonnaire, Nicolas Marchand, H. Langley DeWitt, Jorge Pey, Aurélie Colomb, François Gheusi, Sonke Szidat, Iasonas Stavroulas, Agnès Borbon, and Nadine Locoge
Atmos. Chem. Phys., 17, 8837–8865, https://doi.org/10.5194/acp-17-8837-2017, https://doi.org/10.5194/acp-17-8837-2017, 2017
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The ChArMEx SOP2 field campaign took place from 15 July to 5 August 2013 in the western Mediterranean Basin at Ersa, a remote site in Cape Corse. Exhaustive descriptions of the chemical composition of air masses in gas and aerosol phase were performed. An analysis of these measurements was performed using various source-receptor approaches. This led to the identification of several factors linked to primary sources but also to secondary processes of both biogenic and anthropogenic origin.
Amélie Saunier, Elena Ormeño, Christophe Boissard, Henri Wortham, Brice Temime-Roussel, Caroline Lecareux, Alexandre Armengaud, and Catherine Fernandez
Atmos. Chem. Phys., 17, 7555–7566, https://doi.org/10.5194/acp-17-7555-2017, https://doi.org/10.5194/acp-17-7555-2017, 2017
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We investigated the BVOC emissions variations of Quercus Pubescens, under natural and amplified drought, in situ, in order to determine the dependency to light and/or temperature of these emissions. Our results showed that all BVOC emissions were reduced with amplified drought.
Moreover, we highlighted two dependences: (i) light and temperature and (ii) light and temperature during the day and to temperature during the night. These results can be useful to enhance emission models.
Lorenzo Caponi, Paola Formenti, Dario Massabó, Claudia Di Biagio, Mathieu Cazaunau, Edouard Pangui, Servanne Chevaillier, Gautier Landrot, Meinrat O. Andreae, Konrad Kandler, Stuart Piketh, Thuraya Saeed, Dave Seibert, Earle Williams, Yves Balkanski, Paolo Prati, and Jean-François Doussin
Atmos. Chem. Phys., 17, 7175–7191, https://doi.org/10.5194/acp-17-7175-2017, https://doi.org/10.5194/acp-17-7175-2017, 2017
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This paper presents new laboratory measurements of the shortwave mass absorption efficiency (MAE) used by climate models for mineral dust of different origin and at different sizes. We found that small particles are more efficient, by given mass, in absorbing radiation, particularly at shorter wavelength. Because dust has high concentrations in the atmosphere, light absorption by mineral dust can be competitive to other absorbing atmospheric aerosols such as black and brown carbon.
Sebastian Laufs, Mathieu Cazaunau, Patrick Stella, Ralf Kurtenbach, Pierre Cellier, Abdelwahid Mellouki, Benjamin Loubet, and Jörg Kleffmann
Atmos. Chem. Phys., 17, 6907–6923, https://doi.org/10.5194/acp-17-6907-2017, https://doi.org/10.5194/acp-17-6907-2017, 2017
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Sources of nitrous acid (HONO), a major precursor of the OH radical, are still under controversial discussion. Since mainly ground surface sources have been proposed, HONO fluxes were measured above an agricultural field. Positive daytime fluxes were observed which showed strong correlation with the product of the NO2 concentration and J(NO2). These results indicate HONO formation by photosensitized heterogeneous conversion of NO2 on soil surfaces as observed in recent laboratory studies.
Marius Duncianu, Marc David, Sakthivel Kartigueyane, Manuela Cirtog, Jean-François Doussin, and Benedicte Picquet-Varrault
Atmos. Meas. Tech., 10, 1445–1463, https://doi.org/10.5194/amt-10-1445-2017, https://doi.org/10.5194/amt-10-1445-2017, 2017
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A commercial PTR-ToF-MS has been optimized in order to allow the measurement of individual organic nitrates in the atmosphere. This has been accomplished by shifting the distribution between different ionizing analytes. The proposed approach has been proved to be appropriate for the online detection of individual alkyl nitrates and functionalized nitrates.
Camille Mouchel-Vallon, Laurent Deguillaume, Anne Monod, Hélène Perroux, Clémence Rose, Giovanni Ghigo, Yoann Long, Maud Leriche, Bernard Aumont, Luc Patryl, Patrick Armand, and Nadine Chaumerliac
Geosci. Model Dev., 10, 1339–1362, https://doi.org/10.5194/gmd-10-1339-2017, https://doi.org/10.5194/gmd-10-1339-2017, 2017
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The Cloud Explicit Physico-chemical Scheme (CLEPS 1.0) describes oxidation of water-soluble organic compounds resulting from isoprene oxidation. It is based on structure activity relationships (SARs) (global rate constants and branching ratios for HO• abstraction and addition) and GROMHE SAR (Henry's law constants for undocumented species). It is coupled to the MCM gas phase mechanism and is included in a model using the DSMACC model and KPP to analyze experimental and field data.
Claudia Di Biagio, Paola Formenti, Yves Balkanski, Lorenzo Caponi, Mathieu Cazaunau, Edouard Pangui, Emilie Journet, Sophie Nowak, Sandrine Caquineau, Meinrat O. Andreae, Konrad Kandler, Thuraya Saeed, Stuart Piketh, David Seibert, Earle Williams, and Jean-François Doussin
Atmos. Chem. Phys., 17, 1901–1929, https://doi.org/10.5194/acp-17-1901-2017, https://doi.org/10.5194/acp-17-1901-2017, 2017
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Modeling the interaction of dust with long-wave (LW) radiation is still a challenge due to the scarcity of information on their refractive index. In this paper, we present a unique dataset of dust refractive indices obtained from in situ measurements in a large smog chamber. Our results show that the dust LW refractive index varies strongly from source to source due to particle composition changes. We recommend taking this variability into account in climate and remote sensing applications.
Emily A. Bruns, Jay G. Slowik, Imad El Haddad, Dogushan Kilic, Felix Klein, Josef Dommen, Brice Temime-Roussel, Nicolas Marchand, Urs Baltensperger, and André S. H. Prévôt
Atmos. Chem. Phys., 17, 705–720, https://doi.org/10.5194/acp-17-705-2017, https://doi.org/10.5194/acp-17-705-2017, 2017
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We characterize primary and aged gaseous emissions from residential wood combustion using proton transfer reaction time-of-flight mass spectrometry. This approach allows for improved characterization, particularly of oxygenated gases, which are a considerable fraction of the total gaseous mass emitted during residential wood combustion. This study is the first thorough characterization of organic gases from this source and provides a benchmark for future studies.
Rachel Gemayel, Stig Hellebust, Brice Temime-Roussel, Nathalie Hayeck, Johannes T. Van Elteren, Henri Wortham, and Sasho Gligorovski
Atmos. Meas. Tech., 9, 1947–1959, https://doi.org/10.5194/amt-9-1947-2016, https://doi.org/10.5194/amt-9-1947-2016, 2016
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LAAP-ToF-MS has been optimized for particle size and number concentration evolution and characterization of the chemical composition of ambient particles by following specific ions.
The advantage of this instrument is that it can analyze the ambient particles online and continuously. It is capable of analyzing inorganic material in ambient particles; in particular the presence of metals can be analyzed. Last but not least, it is a compact and easily transportable tool for field measurements.
S. Mailler, L. Menut, A. G. di Sarra, S. Becagli, T. Di Iorio, B. Bessagnet, R. Briant, P. Formenti, J.-F. Doussin, J. L. Gómez-Amo, M. Mallet, G. Rea, G. Siour, D. M. Sferlazzo, R. Traversi, R. Udisti, and S. Turquety
Atmos. Chem. Phys., 16, 1219–1244, https://doi.org/10.5194/acp-16-1219-2016, https://doi.org/10.5194/acp-16-1219-2016, 2016
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We studied the impact of aerosols on tropospheric photolysis rates at Lampedusa during the CharMEx/ADRIMED campaign in June 2013. It is shown by using the CHIMERE chemistry-transport model (CTM) as well as in situ and remote-sensing measurements that taking into account the radiative effect of the tropospheric aerosols improves the ability of the model to reproduce the observed photolysis rates. It is hence important for CTMs to include the radiative effect of aerosols on photochemistry.
M. Mallet, F. Dulac, P. Formenti, P. Nabat, J. Sciare, G. Roberts, J. Pelon, G. Ancellet, D. Tanré, F. Parol, C. Denjean, G. Brogniez, A. di Sarra, L. Alados-Arboledas, J. Arndt, F. Auriol, L. Blarel, T. Bourrianne, P. Chazette, S. Chevaillier, M. Claeys, B. D'Anna, Y. Derimian, K. Desboeufs, T. Di Iorio, J.-F. Doussin, P. Durand, A. Féron, E. Freney, C. Gaimoz, P. Goloub, J. L. Gómez-Amo, M. J. Granados-Muñoz, N. Grand, E. Hamonou, I. Jankowiak, M. Jeannot, J.-F. Léon, M. Maillé, S. Mailler, D. Meloni, L. Menut, G. Momboisse, J. Nicolas, T. Podvin, V. Pont, G. Rea, J.-B. Renard, L. Roblou, K. Schepanski, A. Schwarzenboeck, K. Sellegri, M. Sicard, F. Solmon, S. Somot, B Torres, J. Totems, S. Triquet, N. Verdier, C. Verwaerde, F. Waquet, J. Wenger, and P. Zapf
Atmos. Chem. Phys., 16, 455–504, https://doi.org/10.5194/acp-16-455-2016, https://doi.org/10.5194/acp-16-455-2016, 2016
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The aim of this article is to present an experimental campaign over the Mediterranean focused on aerosol-radiation measurements and modeling. Results indicate an important atmospheric loading associated with a moderate absorbing ability of mineral dust. Observations suggest a complex vertical structure and size distributions characterized by large aerosols within dust plumes. The radiative effect is highly variable, with negative forcing over the Mediterranean and positive over northern Africa.
Q. J. Zhang, M. Beekmann, E. Freney, K. Sellegri, J. M. Pichon, A. Schwarzenboeck, A. Colomb, T. Bourrianne, V. Michoud, and A. Borbon
Atmos. Chem. Phys., 15, 13973–13992, https://doi.org/10.5194/acp-15-13973-2015, https://doi.org/10.5194/acp-15-13973-2015, 2015
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Secondary organic aerosol (SOA) is an important pollutant formed from megacity emissions at a regional scale. An original method based on ratios of different pollutants is used to specifically validate the aerosol scheme (the volatility basis set approach) within a CTM. The method is applied to airborne measurements performed within the Paris plume during the MEGAPOLI summer campaign. Simulations indicate that SOA of anthropogenic origin has a significant impact on regional air quality.
N. Zannoni, S. Dusanter, V. Gros, R. Sarda Esteve, V. Michoud, V. Sinha, N. Locoge, and B. Bonsang
Atmos. Meas. Tech., 8, 3851–3865, https://doi.org/10.5194/amt-8-3851-2015, https://doi.org/10.5194/amt-8-3851-2015, 2015
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Our manuscript shows results of an intercomparison exercise conducted on two home-built comparative reactivity method (CRM) instruments operating under the same settings for measuring total OH reactivity. Despite the corrections of the raw data sets for instrumental artifacts having different weights on the two CRMs, we found very consistent results for the final processed data of ambient OH reactivity. Furthermore, we present in detail how to validate the instruments and process the raw data.
H. Petetin, M. Beekmann, A. Colomb, H. A. C. Denier van der Gon, J.-C. Dupont, C. Honoré, V. Michoud, Y. Morille, O. Perrussel, A. Schwarzenboeck, J. Sciare, A. Wiedensohler, and Q. J. Zhang
Atmos. Chem. Phys., 15, 9799–9818, https://doi.org/10.5194/acp-15-9799-2015, https://doi.org/10.5194/acp-15-9799-2015, 2015
V. Michoud, R. F. Hansen, N. Locoge, P. S. Stevens, and S. Dusanter
Atmos. Meas. Tech., 8, 3537–3553, https://doi.org/10.5194/amt-8-3537-2015, https://doi.org/10.5194/amt-8-3537-2015, 2015
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This study presents the results of an exhaustive characterization of a CRM instrument developed at Mines Douai to measure total OH reactivity in the troposphere. To do so, a suite of laboratory experiments was conducted to assess the different corrections that need to be applied during data processing. The results were then compared to simulations from a 0-D box model, including two different chemical mechanisms, leading to reasonable agreement.
M. Beekmann, A. S. H. Prévôt, F. Drewnick, J. Sciare, S. N. Pandis, H. A. C. Denier van der Gon, M. Crippa, F. Freutel, L. Poulain, V. Ghersi, E. Rodriguez, S. Beirle, P. Zotter, S.-L. von der Weiden-Reinmüller, M. Bressi, C. Fountoukis, H. Petetin, S. Szidat, J. Schneider, A. Rosso, I. El Haddad, A. Megaritis, Q. J. Zhang, V. Michoud, J. G. Slowik, S. Moukhtar, P. Kolmonen, A. Stohl, S. Eckhardt, A. Borbon, V. Gros, N. Marchand, J. L. Jaffrezo, A. Schwarzenboeck, A. Colomb, A. Wiedensohler, S. Borrmann, M. Lawrence, A. Baklanov, and U. Baltensperger
Atmos. Chem. Phys., 15, 9577–9591, https://doi.org/10.5194/acp-15-9577-2015, https://doi.org/10.5194/acp-15-9577-2015, 2015
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A detailed characterization of air quality in the Paris (France) agglomeration, a megacity, during two summer and winter intensive campaigns and from additional 1-year observations, revealed that about 70% of the fine particulate matter (PM) at urban background is transported into the megacity from upwind regions. Unexpectedly, a major part of organic PM is of modern origin (woodburning and cooking activities, secondary formation from biogenic VOC).
B. Ervens, P. Renard, S. Tlili, S. Ravier, J.-L. Clément, and A. Monod
Atmos. Chem. Phys., 15, 9109–9127, https://doi.org/10.5194/acp-15-9109-2015, https://doi.org/10.5194/acp-15-9109-2015, 2015
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A detailed chemical mechanism is developed based on laboratory studies that predicts the formation of high molecular weight compounds in the aqueous phase of atmospheric aerosol particles. Model simulations using this mechanism for atmospheric conditions show that these pathways are likely not a substantial source of particle mass, unless unidentified precursors for these compounds exist that were not taken into account so far and/or the solubility of oxygen in aerosol water is overestimated.
I. Kourtchev, J.-F. Doussin, C. Giorio, B. Mahon, E. M. Wilson, N. Maurin, E. Pangui, D. S. Venables, J. C. Wenger, and M. Kalberer
Atmos. Chem. Phys., 15, 5683–5695, https://doi.org/10.5194/acp-15-5683-2015, https://doi.org/10.5194/acp-15-5683-2015, 2015
H. L. DeWitt, S. Hellebust, B. Temime-Roussel, S. Ravier, L. Polo, V. Jacob, C. Buisson, A. Charron, M. André, A. Pasquier, J. L. Besombes, J. L. Jaffrezo, H. Wortham, and N. Marchand
Atmos. Chem. Phys., 15, 4373–4387, https://doi.org/10.5194/acp-15-4373-2015, https://doi.org/10.5194/acp-15-4373-2015, 2015
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By performing source-apportionment modeling, the amount of primary and secondary organic emissions was resolved from a bulk aerosol data set measured adjacent to a major highway in France. Over 70% of vehicles on this highway were diesel, and a high concentration of BC and NOx were measured. Even close to a major highway, the bulk of the aerosol mass was secondary in nature. Radiocarbon data revealed that most of the fossil organic carbon was from primary vehicular emissions and not from SOA.
C. Denjean, P. Formenti, B. Picquet-Varrault, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, A. Monod, B. Temime-Roussel, P. Decorse, C. Mangeney, and J. F. Doussin
Atmos. Chem. Phys., 15, 3339–3358, https://doi.org/10.5194/acp-15-3339-2015, https://doi.org/10.5194/acp-15-3339-2015, 2015
L. Brégonzio-Rozier, F. Siekmann, C. Giorio, E. Pangui, S. B. Morales, B. Temime-Roussel, A. Gratien, V. Michoud, S. Ravier, M. Cazaunau, A. Tapparo, A. Monod, and J.-F. Doussin
Atmos. Chem. Phys., 15, 2953–2968, https://doi.org/10.5194/acp-15-2953-2015, https://doi.org/10.5194/acp-15-2953-2015, 2015
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First- and higher order -generation products formed from the oxidation of isoprene and methacrolein with OH radicals in the presence of NOx have been studied in a simulation chamber. Differences in light source are proposed to partially explain the discrepancies observed between different studies in the literature for both isoprene- and methacrolein-SOA mass yields. According to our results, these SOA yields in the atmosphere could be lower than suggested by most of the current chamber studies.
C. Denjean, P. Formenti, B. Picquet-Varrault, M. Camredon, E. Pangui, P. Zapf, Y. Katrib, C. Giorio, A. Tapparo, B. Temime-Roussel, A. Monod, B. Aumont, and J. F. Doussin
Atmos. Chem. Phys., 15, 883–897, https://doi.org/10.5194/acp-15-883-2015, https://doi.org/10.5194/acp-15-883-2015, 2015
P. Renard, F. Siekmann, G. Salque, C. Demelas, B. Coulomb, L. Vassalo, S. Ravier, B. Temime-Roussel, D. Voisin, and A. Monod
Atmos. Chem. Phys., 15, 21–35, https://doi.org/10.5194/acp-15-21-2015, https://doi.org/10.5194/acp-15-21-2015, 2015
W. Ait-Helal, A. Borbon, S. Sauvage, J. A. de Gouw, A. Colomb, V. Gros, F. Freutel, M. Crippa, C. Afif, U. Baltensperger, M. Beekmann, J.-F. Doussin, R. Durand-Jolibois, I. Fronval, N. Grand, T. Leonardis, M. Lopez, V. Michoud, K. Miet, S. Perrier, A. S. H. Prévôt, J. Schneider, G. Siour, P. Zapf, and N. Locoge
Atmos. Chem. Phys., 14, 10439–10464, https://doi.org/10.5194/acp-14-10439-2014, https://doi.org/10.5194/acp-14-10439-2014, 2014
V. Michoud, A. Colomb, A. Borbon, K. Miet, M. Beekmann, M. Camredon, B. Aumont, S. Perrier, P. Zapf, G. Siour, W. Ait-Helal, C. Afif, A. Kukui, M. Furger, J. C. Dupont, M. Haeffelin, and J. F. Doussin
Atmos. Chem. Phys., 14, 2805–2822, https://doi.org/10.5194/acp-14-2805-2014, https://doi.org/10.5194/acp-14-2805-2014, 2014
E. J. Freney, K. Sellegri, F. Canonaco, A. Colomb, A. Borbon, V. Michoud, J.-F. Doussin, S. Crumeyrolle, N. Amarouche, J.-M. Pichon, T. Bourianne, L. Gomes, A. S. H. Prevot, M. Beekmann, and A. Schwarzenböeck
Atmos. Chem. Phys., 14, 1397–1412, https://doi.org/10.5194/acp-14-1397-2014, https://doi.org/10.5194/acp-14-1397-2014, 2014
C. Denjean, P. Formenti, B. Picquet-Varrault, Y. Katrib, E. Pangui, P. Zapf, and J. F. Doussin
Atmos. Meas. Tech., 7, 183–197, https://doi.org/10.5194/amt-7-183-2014, https://doi.org/10.5194/amt-7-183-2014, 2014
J.-F. Doussin and A. Monod
Atmos. Chem. Phys., 13, 11625–11641, https://doi.org/10.5194/acp-13-11625-2013, https://doi.org/10.5194/acp-13-11625-2013, 2013
P. Renard, F. Siekmann, A. Gandolfo, J. Socorro, G. Salque, S. Ravier, E. Quivet, J.-L. Clément, M. Traikia, A.-M. Delort, D. Voisin, V. Vuitton, R. Thissen, and A. Monod
Atmos. Chem. Phys., 13, 6473–6491, https://doi.org/10.5194/acp-13-6473-2013, https://doi.org/10.5194/acp-13-6473-2013, 2013
Q. J. Zhang, M. Beekmann, F. Drewnick, F. Freutel, J. Schneider, M. Crippa, A. S. H. Prevot, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, V. Gros, A. Borbon, A. Colomb, V. Michoud, J.-F. Doussin, H. A. C. Denier van der Gon, M. Haeffelin, J.-C. Dupont, G. Siour, H. Petetin, B. Bessagnet, S. N. Pandis, A. Hodzic, O. Sanchez, C. Honoré, and O. Perrussel
Atmos. Chem. Phys., 13, 5767–5790, https://doi.org/10.5194/acp-13-5767-2013, https://doi.org/10.5194/acp-13-5767-2013, 2013
F. Freutel, J. Schneider, F. Drewnick, S.-L. von der Weiden-Reinmüller, M. Crippa, A. S. H. Prévôt, U. Baltensperger, L. Poulain, A. Wiedensohler, J. Sciare, R. Sarda-Estève, J. F. Burkhart, S. Eckhardt, A. Stohl, V. Gros, A. Colomb, V. Michoud, J. F. Doussin, A. Borbon, M. Haeffelin, Y. Morille, M. Beekmann, and S. Borrmann
Atmos. Chem. Phys., 13, 933–959, https://doi.org/10.5194/acp-13-933-2013, https://doi.org/10.5194/acp-13-933-2013, 2013
V. Michoud, A. Kukui, M. Camredon, A. Colomb, A. Borbon, K. Miet, B. Aumont, M. Beekmann, R. Durand-Jolibois, S. Perrier, P. Zapf, G. Siour, W. Ait-Helal, N. Locoge, S. Sauvage, C. Afif, V. Gros, M. Furger, G. Ancellet, and J. F. Doussin
Atmos. Chem. Phys., 12, 11951–11974, https://doi.org/10.5194/acp-12-11951-2012, https://doi.org/10.5194/acp-12-11951-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Quantifying the seasonal variations in and regional transport of PM2.5 in the Yangtze River Delta region, China: characteristics, sources, and health risks
Opinion: Atmospheric multiphase chemistry – past, present, and future
Distinct photochemistry in glycine particles mixed with different atmospheric nitrate salts
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime
Formation of highly oxygenated organic molecules from the oxidation of limonene by OH radical: significant contribution of H-abstraction pathway
Measurement report: Atmospheric aging of combustion-derived particles – impact on stable free radical concentration and its ability to produce reactive oxygen species in aqueous media
Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants
An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
Molecular fingerprints and health risks of home-use incense burning smoke
Technical note: in-situ measurements and modelling of the oxidation kinetics in films of a cooking aerosol proxy using a Quartz Crystal Microbalance with Dissipation monitoring (QCM-D)
Simultaneous formation of sulfate and nitrate via co-uptake of SO2 and NO2 by aqueous NaCl droplets: combined effect of nitrate photolysis and chlorine chemistry
Photo-induced shrinking of aqueous glycine aerosol droplets
Sulfate formation via aerosol-phase SO2 oxidation by model biomass burning photosensitizers: 3,4-dimethoxybenzaldehyde, vanillin and syringaldehyde using single-particle mixing-state analysis
Yields and molecular composition of gas-phase and secondary organic aerosol from the photooxidation of the volatile consumer product benzyl alcohol: formation of highly oxygenated and hydroxy nitro-aromatic compounds
A combined gas- and particle-phase analysis of highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
Comparison of aqueous secondary organic aerosol (aqSOA) product distributions from guaiacol oxidation by non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
Technical note: Chemical composition and source identification of fluorescent components in atmospheric water-soluble brown carbon by excitation–emission matrix spectroscopy with parallel factor analysis – potential limitations and applications
High Enrichment of Heavy Metals in Fine Particulate Matter through Dust Aerosol Generation
Insoluble lipid film mediates transfer of soluble saccharides from the sea to the atmosphere: the role of hydrogen bonding
Production of aerosol containing ice nucleating particles (INPs) by fast growing phytoplankton
Magnetic fraction of the atmospheric dust in Kraków – physicochemical characteristics and possible environmental impact
Modeling daytime and nighttime secondary organic aerosol formation via multiphase reactions of biogenic hydrocarbons
SO2 enhances aerosol formation from anthropogenic volatile organic compound ozonolysis by producing sulfur-containing compounds
Isothermal evaporation of α-pinene secondary organic aerosol particles formed under low NOx and high NOx conditions
Chemical characterization of organic compounds involved in iodine-initiated new particle formation from coastal macroalgal emission
The Urmia playa as a source of airborne dust and ice-nucleating particles – Part 2: Unraveling the relationship between soil dust composition and ice nucleation activity
Winter brown carbon over six of China's megacities: light absorption, molecular characterization, and improved source apportionment revealed by multilayer perceptron neural network
Chamber investigation of the formation and transformation of secondary organic aerosol in mixtures of biogenic and anthropogenic volatile organic compounds
Not all types of secondary organic aerosol mix: two phases observed when mixing different secondary organic aerosol types
Comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) from heavy-duty diesel vehicles using two-dimensional gas chromatography time-of-flight mass spectrometry
Measurement report: Investigation of pH- and particle-size-dependent chemical and optical properties of water-soluble organic carbon: implications for its sources and aging processes
The influence of the addition of isoprene on the volatility of particles formed from the photo-oxidation of anthropogenic–biogenic mixtures
Significant formation of sulfate aerosols contributed by the heterogeneous drivers of dust surface
Particle-phase processing of α-pinene NO3 secondary organic aerosol in the dark
Chemical characteristics and sources of PM2.5 in Hohhot, a semi-arid city in northern China: insight from the COVID-19 lockdown
The positive effect of formaldehyde on the photocatalytic renoxification of nitrate on TiO2 particles
Identification of highly oxygenated organic molecules and their role in aerosol formation in the reaction of limonene with nitrate radical
A comprehensive study on hygroscopic behaviour and nitrate depletion of NaNO3 and dicarboxylic acid mixtures: implications for nitrate depletion in tropospheric aerosols
Secondary organic aerosols from OH oxidation of cyclic volatile methyl siloxanes as an important Si source in the atmosphere
Effects of OH radical and SO2 concentrations on photochemical reactions of mixed anthropogenic organic gases
Yangzhihao Zhan, Min Xie, Wei Zhao, Tijian Wang, Da Gao, Pulong Chen, Jun Tian, Kuanguang Zhu, Shu Li, Bingliang Zhuang, Mengmeng Li, Yi Luo, and Runqi Zhao
Atmos. Chem. Phys., 23, 9837–9852, https://doi.org/10.5194/acp-23-9837-2023, https://doi.org/10.5194/acp-23-9837-2023, 2023
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Although the main source contribution of pollution is secondary inorganic aerosols in Nanjing, health risks mainly come from industry sources and vehicle emissions. Therefore, the development of megacities should pay more attention to the health burden of vehicle emissions, coal combustion, and industrial processes. This study provides new insight into assessing the relationship between source apportionment and health risks and can provide valuable insight into air pollution strategies.
Jonathan P. D. Abbatt and A. R. Ravishankara
Atmos. Chem. Phys., 23, 9765–9785, https://doi.org/10.5194/acp-23-9765-2023, https://doi.org/10.5194/acp-23-9765-2023, 2023
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With important climate and air quality impacts, atmospheric multiphase chemistry involves gas interactions with aerosol particles and cloud droplets. We summarize the status of the field and discuss potential directions for future growth. We highlight the importance of a molecular-level understanding of the chemistry, along with atmospheric field studies and modeling, and emphasize the necessity for atmospheric multiphase chemists to interact widely with scientists from neighboring disciplines.
Zhancong Liang, Zhihao Cheng, Ruifeng Zhang, Yiming Qin, and Chak K. Chan
Atmos. Chem. Phys., 23, 9585–9595, https://doi.org/10.5194/acp-23-9585-2023, https://doi.org/10.5194/acp-23-9585-2023, 2023
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In this study, we found that the photolysis of sodium nitrate leads to a much quicker decay of free amino acids (FAAs, with glycine as an example) in the particle phase than ammonium nitrate photolysis, which is likely due to the molecular interactions between FAAs and different nitrate salts. Since sodium nitrate likely co-exists with FAAs in the coarse-mode particles, particulate nitrate photolysis can possibly contribute to a rapid decay of FAAs and affect atmospheric nitrogen cycling.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
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The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
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We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
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The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Hao Luo, Luc Vereecken, Hongru Shen, Sungah Kang, Iida Pullinen, Mattias Hallquist, Hendrik Fuchs, Andreas Wahner, Astrid Kiendler-Scharr, Thomas F. Mentel, and Defeng Zhao
Atmos. Chem. Phys., 23, 7297–7319, https://doi.org/10.5194/acp-23-7297-2023, https://doi.org/10.5194/acp-23-7297-2023, 2023
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Oxidation of limonene, an element emitted by trees and chemical products, by OH, a daytime oxidant, forms many highly oxygenated organic molecules (HOMs), including C10-20 compounds. HOMs play an important role in new particle formation and growth. HOM formation can be explained by the chemistry of peroxy radicals. We found that a minor branching ratio initial pathway plays an unexpected, significant role. Considering this pathway enables accurate simulations of HOMs and other concentrations.
Heather L. Runberg and Brian J. Majestic
Atmos. Chem. Phys., 23, 7213–7223, https://doi.org/10.5194/acp-23-7213-2023, https://doi.org/10.5194/acp-23-7213-2023, 2023
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Environmentally persistent free radicals (EPFRs) are an emerging pollutant found in soot particles. Understanding how these change as they move through the atmosphere is important to human health. Here, soot was generated in the laboratory and exposed to simulated sunlight. The concentrations and characteristics of EPFRs in the soot were measured and found to be unchanged. However, it was also found that the ability of soot to form hydroxyl radicals was stronger for fresh soot.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, https://doi.org/10.5194/acp-23-7103-2023, 2023
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Kai Song, Rongzhi Tang, Jingshun Zhang, Zichao Wan, Yuan Zhang, Kun Hu, Yuanzheng Gong, Daqi Lv, Sihua Lu, Yu Tan, Ruifeng Zhang, Ang Li, Shuyuan Yan, Shichao Yan, Baoming Fan, Wenfei Zhu, Chak K. Chan, and Song Guo
EGUsphere, https://doi.org/10.5194/egusphere-2023-1225, https://doi.org/10.5194/egusphere-2023-1225, 2023
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Incense burning is a common practice in Asia, posing great threats to human health and air quality. However, less is known about its emissions and health risks. Full volatility organic species from incense burning smoke are detected and quantified for the first time. IVOCs are crucial organics accounting for 19.2 % of the total EFs and 40.0 % of the SOA estimation, highlighting the importance of incorporating IVOCs into SOA models.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1207, https://doi.org/10.5194/egusphere-2023-1207, 2023
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Aerosols and films are found indoors and outdoors. Our study measures and models reactions of a cooking aerosol proxy with the atmospheric oxidant ozone relying on a low-cost, but sensitive technique based on mass changes and film rigidity. We found that film morphology changed and film rigidity increased with evidence of surface crust formation during ozone exposure. Our modelling results demonstrate clear potential to take this robust method to the field for reaction monitoring.
Ruifeng Zhang and Chak Keung Chan
Atmos. Chem. Phys., 23, 6113–6126, https://doi.org/10.5194/acp-23-6113-2023, https://doi.org/10.5194/acp-23-6113-2023, 2023
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Research into sulfate and nitrate formation from co-uptake of NO2 and SO2, especially under irradiation, is rare. We studied the co-uptake of NO2 and SO2 by NaCl droplets under various conditions, including irradiation and dark, and RHs, using Raman spectroscopy flow cell and kinetic model simulation. Significant nitrate formation from NO2 hydrolysis can be photolyzed to generate OH radicals that can further react with chloride to produce reactive chlorine species and promote sulfate formation.
Shinnosuke Ishizuka, Oliver Reich, Grégory David, and Ruth Signorell
Atmos. Chem. Phys., 23, 5393–5402, https://doi.org/10.5194/acp-23-5393-2023, https://doi.org/10.5194/acp-23-5393-2023, 2023
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Photosensitizers play an important role in the photochemistry of atmospheric aerosols. Our study provides evidence that mesoscopic glycine clusters forming in aqueous droplets act as unconventional photosensitizers in the visible light spectrum. We observed the influence of these photoactive molecular aggregates in single optically trapped aqueous droplets. Such mesoscopic photosensitizers might be more important for aerosol photochemistry than previously anticipated.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
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This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Mohammed Jaoui, Kenneth S. Docherty, Michael Lewandowski, and Tadeusz E. Kleindienst
Atmos. Chem. Phys., 23, 4637–4661, https://doi.org/10.5194/acp-23-4637-2023, https://doi.org/10.5194/acp-23-4637-2023, 2023
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VCPs are a class of chemicals widely used in industrial and consumer products (e.g., coatings, adhesives, inks, personal care products) and are an important component of total VOCs in urban atmospheres. This study provides SOA yields and detailed chemical analysis of the gas- and aerosol-phase products of the photooxidation of one of these VCPs, benzyl alcohol. These results will allow better links between characterized sources and their resulting criteria for pollutant formation.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
EGUsphere, https://doi.org/10.5194/egusphere-2023-195, https://doi.org/10.5194/egusphere-2023-195, 2023
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In this study, we have investigated the distinct impacts of humidity on the ozonolysis of two structurally different monoterpenes (limonene and Δ3-carene), We found that the molecular structure of precursors can largely influence the SOA formation under high RH by impacting the multi-generation reactions. Our results could advance knowledge on the roles of water content on aerosol formation, and inform ongoing research on particle environmental effects and applications in models.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive models.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping'an Peng
Atmos. Chem. Phys., 23, 2613–2625, https://doi.org/10.5194/acp-23-2613-2023, https://doi.org/10.5194/acp-23-2613-2023, 2023
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This work comprehensively investigated the fluorescence data of light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic and humic acids using an excitation–emission matrix (EEM) method and parallel factor modeling. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical composition and possible sources of these species in atmospheric samples.
Qianqian Gao, Shengqiang Zhu, Kaili Zhou, Jinghao Zhai, Shaodong Chen, Qihuang Wang, Shurong Wang, Jin Han, Xiaohui Lu, Hong Chen, Liwu Zhang, Lin Wang, Zimeng Wang, Xin Yang, Qi Ying, Hongliang Zhang, Jianmin Chen, and Xiaofei Wang
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-802, https://doi.org/10.5194/acp-2022-802, 2023
Revised manuscript accepted for ACP
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Dust is a major source of atmospheric aerosols. Its chemical composition is often assumed to be similar to the parent soil. However, this assumption has not been rigorously verified. Dust aerosols are mainly generated by wind erosion, which may have some chemical selectivity. Mn, Cd and Pb were found to be highly enriched in fine (PM2.5) dust aerosols. In addition, estimation of heavy metal emission from dust generation by air quality models may have errors without using proper dust profiles.
Minglan Xu, Narcisse Tsona Tchinda, Jianlong Li, and Lin Du
Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
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The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
Daniel Conrad Ogilvie Thornton, Sarah Dickerson Brooks, Elise Katherine Wilbourn, Jessica Mirrielees, Alyssa Nicole Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana Kiana McFadden
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-806, https://doi.org/10.5194/acp-2022-806, 2023
Revised manuscript accepted for ACP
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A major uncertainty in our understanding of clouds and climate are the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast growing marine phytoplankton were a source of ice nucleating particles (INPs). INPs facilitate freezing of ice crystals at warmer temperatures than otherwise possible, and therefore change cloud formation and properties. Our results show ecosystem processes and the properties of sea spray aerosol are linked.
Jan M. Michalik, Wanda Wilczyńska-Michalik, Łukasz Gondek, Waldemar Tokarz, Jan Żukrowski, Marta Gajewska, and Marek Michalik
Atmos. Chem. Phys., 23, 1449–1464, https://doi.org/10.5194/acp-23-1449-2023, https://doi.org/10.5194/acp-23-1449-2023, 2023
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The magnetic fraction of the aerosols in Kraków was collected and analysed using scanning and transmission electron microscopy with energy-dispersive spectrometry, X-ray diffraction, Mössbauer spectrometry, and magnetometry. It contains metallic Fe or Fe-rich alloy and Fe oxides. The occurrence of nanometre-scale Fe3O4 particles (predominantly of anthropogenic origin) is shown. Our results can help to determine the sources and transport of pollutants, potential harmful effects, etc.
Sanghee Han and Myoseon Jang
Atmos. Chem. Phys., 23, 1209–1226, https://doi.org/10.5194/acp-23-1209-2023, https://doi.org/10.5194/acp-23-1209-2023, 2023
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The diurnal pattern in biogenic secondary organic aerosol (SOA) formation is simulated by using the UNIPAR model, which predicts SOA growth via multiphase reactions of hydrocarbons under varying NOx levels, aerosol acidity, humidity, and temperature. The simulation suggests that nighttime SOA formation, even in urban environments, where anthropogenic emission is high, is dominated by products from ozonolysis and NO3-initiated oxidation of biogenic hydrocarbons.
Zhaomin Yang, Kun Li, Narcisse T. Tsona, Xin Luo, and Lin Du
Atmos. Chem. Phys., 23, 417–430, https://doi.org/10.5194/acp-23-417-2023, https://doi.org/10.5194/acp-23-417-2023, 2023
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SO2 significantly promotes particle formation during cyclooctene ozonolysis. Carboxylic acids and their dimers were major products in particles formed in the absence of SO2. SO2 can induce production of organosulfates with stronger particle formation ability than their precursors, leading to the enhancement in particle formation. Formation mechanisms and structures of organosulfates were proposed, which is helpful for better understanding how SO2 perturbs the formation and fate of particles.
Zijun Li, Angela Buchholz, Luis M. F. Barreira, Arttu Ylisirniö, Liqing Hao, Iida Pullinen, Siegfried Schobesberger, and Annele Virtanen
Atmos. Chem. Phys., 23, 203–220, https://doi.org/10.5194/acp-23-203-2023, https://doi.org/10.5194/acp-23-203-2023, 2023
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Interaction between NOx and biogenic emissions can be important in suburban areas. Our study showed that the addition of NOx during α-pinene SOA formation produced considerable amounts of organic nitrates and affected the composition of non-nitrated organic compounds. The compositional difference consequently altered the primary type of aqueous-phase processes during the isothermal particle evaporation.
Yibei Wan, Xiangpeng Huang, Chong Xing, Qiongqiong Wang, Xinlei Ge, and Huan Yu
Atmos. Chem. Phys., 22, 15413–15423, https://doi.org/10.5194/acp-22-15413-2022, https://doi.org/10.5194/acp-22-15413-2022, 2022
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The organic compounds involved in continental new particle formation have been investigated in depth in the last 2 decades. In contrast, no prior work has studied the exact chemical composition of organic compounds and their role in coastal new particle formation. We present a complementary study to the ongoing laboratory and field research on iodine nucleation in the coastal atmosphere. This study provided a more complete story of coastal I-NPF from low-tide macroalgal emission.
Nikou Hamzehpour, Claudia Marcolli, Kristian Klumpp, Debora Thöny, and Thomas Peter
Atmos. Chem. Phys., 22, 14931–14956, https://doi.org/10.5194/acp-22-14931-2022, https://doi.org/10.5194/acp-22-14931-2022, 2022
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Dust aerosols from dried lakebeds contain mineral particles, as well as soluble salts and (bio-)organic compounds. Here, we investigate ice nucleation (IN) activity of dust samples from Lake Urmia playa, Iran. We find high IN activity of the untreated samples that decreases after organic matter removal but increases after removing soluble salts and carbonates, evidencing inhibiting effects of soluble salts and carbonates on the IN activity of organic matter and minerals, especially microcline.
Diwei Wang, Zhenxing Shen, Qian Zhang, Yali Lei, Tian Zhang, Shasha Huang, Jian Sun, Hongmei Xu, and Junji Cao
Atmos. Chem. Phys., 22, 14893–14904, https://doi.org/10.5194/acp-22-14893-2022, https://doi.org/10.5194/acp-22-14893-2022, 2022
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The optical properties and molecular structure of atmospheric brown carbon (BrC) in winter of several megacities in China were analyzed, and the source contribution of brown carbon was improved by using positive matrix factorization coupled with a multilayer perceptron neural network. These results can provide a basis for the more effective control of BrC to reduce its impacts on regional climates and human health.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, M. Rami Alfarra, Thomas J. Bannan, Dawei Hu, Kelly L. Pereira, Jaqueline F. Hamilton, Mattias Hallquist, Thomas F. Mentel, and Gordon McFiggans
Atmos. Chem. Phys., 22, 14147–14175, https://doi.org/10.5194/acp-22-14147-2022, https://doi.org/10.5194/acp-22-14147-2022, 2022
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Mixing experiments are crucial and highly beneficial for our understanding of atmospheric chemical interactions. However, interpretation quickly becomes complex, and both the experimental design and evaluation need to be scrutinised carefully. Advanced online and offline compositional measurements can reveal substantial additional information to aid in the interpretation of yield data, including components uniquely found in mixtures and property changes in SOA formed from mixtures of VOCs.
Fabian Mahrt, Long Peng, Julia Zaks, Yuanzhou Huang, Paul E. Ohno, Natalie R. Smith, Florence K. A. Gregson, Yiming Qin, Celia L. Faiola, Scot T. Martin, Sergey A. Nizkorodov, Markus Ammann, and Allan K. Bertram
Atmos. Chem. Phys., 22, 13783–13796, https://doi.org/10.5194/acp-22-13783-2022, https://doi.org/10.5194/acp-22-13783-2022, 2022
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The number of condensed phases in mixtures of different secondary organic aerosol (SOA) types determines their impact on air quality and climate. Here we observe the number of phases in individual particles that contain mixtures of two different types of SOA. We find that SOA mixtures can form one- or two-phase particles, depending on the difference in the average oxygen-to-carbon (O / C) ratios of the two SOA types that are internally mixed within individual particles.
Xiao He, Xuan Zheng, Shaojun Zhang, Xuan Wang, Ting Chen, Xiao Zhang, Guanghan Huang, Yihuan Cao, Liqiang He, Xubing Cao, Yuan Cheng, Shuxiao Wang, and Ye Wu
Atmos. Chem. Phys., 22, 13935–13947, https://doi.org/10.5194/acp-22-13935-2022, https://doi.org/10.5194/acp-22-13935-2022, 2022
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With the use of two-dimensional gas chromatography time-of-flight mass spectrometry (GC × GC ToF-MS), we successfully give a comprehensive characterization of particulate intermediate-volatility and semi-volatile organic compounds (I/SVOCs) emitted from heavy-duty diesel vehicles. I/SVOCs are speciated, identified, and quantified based on the patterns of the mass spectrum, and the gas–particle partitioning is fully addressed.
Yuanyuan Qin, Juanjuan Qin, Xiaobo Wang, Kang Xiao, Ting Qi, Yuwei Gao, Xueming Zhou, Shaoxuan Shi, Jingnan Li, Jingsi Gao, Ziyin Zhang, Jihua Tan, Yang Zhang, and Rongzhi Chen
Atmos. Chem. Phys., 22, 13845–13859, https://doi.org/10.5194/acp-22-13845-2022, https://doi.org/10.5194/acp-22-13845-2022, 2022
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Deep interrogation of water-soluble organic carbon (WSOC) in aerosols is critical and challenging considering its involvement in many key aerosol-associated chemical reactions. This work examined how the chemical structures (functional groups) and optical properties (UV/fluorescence properties) of WSOC were affected by pH and particle size. We found that the pH- and particle-size-dependent behaviors could be used to reveal the structures, sources, and aging of aerosol WSOC.
Aristeidis Voliotis, Mao Du, Yu Wang, Yunqi Shao, Thomas J. Bannan, Michael Flynn, Spyros N. Pandis, Carl J. Percival, M. Rami Alfarra, and Gordon McFiggans
Atmos. Chem. Phys., 22, 13677–13693, https://doi.org/10.5194/acp-22-13677-2022, https://doi.org/10.5194/acp-22-13677-2022, 2022
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The addition of a low-yield precursor to the reactive mixture of aVOC and bVOC can increase or decrease the SOA volatility that is system-dependent. Therefore, the SOA volatility of the mixtures cannot always be predicted based on the additivity. In complex mixtures the formation of lower-volatility products likely outweighs the formation of products with higher volatility. The unique products of each mixture contribute significantly to the signal, suggesting interactions can be important.
Tao Wang, Yangyang Liu, Hanyun Cheng, Zhenzhen Wang, Hongbo Fu, Jianmin Chen, and Liwu Zhang
Atmos. Chem. Phys., 22, 13467–13493, https://doi.org/10.5194/acp-22-13467-2022, https://doi.org/10.5194/acp-22-13467-2022, 2022
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This study compared the gas-phase, aqueous-phase, and heterogeneous SO2 oxidation pathways by combining laboratory work with a modelling study. The heterogeneous oxidation, particularly that induced by the dust surface drivers, presents positive implications for the removal of airborne SO2 and formation of sulfate aerosols. This work highlighted the atmospheric significance of heterogeneous oxidation and suggested a comparison model to evaluate the following heterogeneous laboratory research.
David M. Bell, Cheng Wu, Amelie Bertrand, Emelie Graham, Janne Schoonbaert, Stamatios Giannoukos, Urs Baltensperger, Andre S. H. Prevot, Ilona Riipinen, Imad El Haddad, and Claudia Mohr
Atmos. Chem. Phys., 22, 13167–13182, https://doi.org/10.5194/acp-22-13167-2022, https://doi.org/10.5194/acp-22-13167-2022, 2022
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A series of studies designed to investigate the evolution of organic aerosol were performed in an atmospheric simulation chamber, using a common oxidant found at night (NO3). The chemical composition steadily changed from its initial composition via different chemical reactions that were taking place inside of the aerosol particle. These results show that the composition of organic aerosol steadily changes during its lifetime in the atmosphere.
Haijun Zhou, Tao Liu, Bing Sun, Yongli Tian, Xingjun Zhou, Feng Hao, Xi Chun, Zhiqiang Wan, Peng Liu, Jingwen Wang, and Dagula Du
Atmos. Chem. Phys., 22, 12153–12166, https://doi.org/10.5194/acp-22-12153-2022, https://doi.org/10.5194/acp-22-12153-2022, 2022
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A single year’s offline measurement was conducted in Hohhot to reveal the chemical characteristics and sources of PM2.5 in a semi-arid region. We believe that our study makes a significant contribution to the literature because relatively few studies have focused on the chemical composition and sources of PM2.5 with offline measurements. A knowledge gap exists concerning how chemical composition and sources respond to implemented control measures for aerosols, particularly in a semi-arid region.
Yuhan Liu, Xuejiao Wang, Jing Shang, Weiwei Xu, Mengshuang Sheng, and Chunxiang Ye
Atmos. Chem. Phys., 22, 11347–11358, https://doi.org/10.5194/acp-22-11347-2022, https://doi.org/10.5194/acp-22-11347-2022, 2022
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In this study, the influence of HCHO on renoxification on nitrate-doped TiO2 particles is investigated by using an experimental chamber. Mass NOx release is suggested to follow the NO−3-NO3·-HNO3-NOx pathway, with HCHO involved in the transformation of NO3· to HNO3 through hydrogen abstraction. Our proposed reaction mechanism by which HCHO promotes photocatalytic renoxification is helpful for deeply understanding the atmospheric photochemical processes and nitrogen cycling.
Yindong Guo, Hongru Shen, Iida Pullinen, Hao Luo, Sungah Kang, Luc Vereecken, Hendrik Fuchs, Mattias Hallquist, Ismail-Hakki Acir, Ralf Tillmann, Franz Rohrer, Jürgen Wildt, Astrid Kiendler-Scharr, Andreas Wahner, Defeng Zhao, and Thomas F. Mentel
Atmos. Chem. Phys., 22, 11323–11346, https://doi.org/10.5194/acp-22-11323-2022, https://doi.org/10.5194/acp-22-11323-2022, 2022
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The oxidation of limonene, a common volatile emitted by trees and chemical products, by NO3, a nighttime oxidant, forms many highly oxygenated organic molecules (HOM), including C10-30 compounds. Most of the HOM are second-generation organic nitrates, in which carbonyl-substituted C10 nitrates accounted for a major fraction. Their formation can be explained by chemistry of peroxy radicals. HOM, especially low-volatile ones, play an important role in nighttime new particle formation and growth.
Shuaishuai Ma, Qiong Li, and Yunhong Zhang
Atmos. Chem. Phys., 22, 10955–10970, https://doi.org/10.5194/acp-22-10955-2022, https://doi.org/10.5194/acp-22-10955-2022, 2022
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The nitrate phase state can play a critical role in determining the occurrence and extent of nitrate depletion in internally mixed NaNO3–DCA particles, which may be instructive for relevant aerosol reaction systems. Besides, organic acids have a potential to deplete nitrate based on the comprehensive consideration of acidity, particle-phase state, droplet water activity, and HNO3 gas-phase diffusion.
Chong Han, Hongxing Yang, Kun Li, Patrick Lee, John Liggio, Amy Leithead, and Shao-Meng Li
Atmos. Chem. Phys., 22, 10827–10839, https://doi.org/10.5194/acp-22-10827-2022, https://doi.org/10.5194/acp-22-10827-2022, 2022
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We presented yields and compositions of Si-containing SOAs generated from the reaction of cVMSs (D3–D6) with OH radicals. NOx played a negative role in cVMS SOA formation, while ammonium sulfate seeds enhanced D3–D5 SOA yields at short photochemical ages under high-NOx conditions. The aerosol mass spectra confirmed that the components of cVMS SOAs significantly relied on OH exposure. A global cVMS-derived SOA source strength was estimated in order to understand SOA formation potentials of cVMSs.
Junling Li, Kun Li, Hao Zhang, Xin Zhang, Yuanyuan Ji, Wanghui Chu, Yuxue Kong, Yangxi Chu, Yanqin Ren, Yujie Zhang, Haijie Zhang, Rui Gao, Zhenhai Wu, Fang Bi, Xuan Chen, Xuezhong Wang, Weigang Wang, Hong Li, and Maofa Ge
Atmos. Chem. Phys., 22, 10489–10504, https://doi.org/10.5194/acp-22-10489-2022, https://doi.org/10.5194/acp-22-10489-2022, 2022
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Ozone formation is enhanced by higher OH concentration and higher temperature but is influenced little by SO2. SO2 can largely enhance the particle formation. Organo-sulfates and organo-nitrates are detected in the formed particles, and the presence of SO2 can promote the formation of organo-sulfates. The results provide a scientific basis for systematically evaluating the effects of SO2, OH concentration, and temperature on the oxidation of mixed organic gases in the atmosphere.
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Short summary
The impact of cloud events on isoprene secondary organic aerosol (SOA) formation has been studied from an isoprene/ NOx/light system in an atmospheric simulation chamber. aqSOA formation can be linked to water soluble volatile organic compounds' dissolution in the aqueous phase and to further aqueous phase reactions. Cloud-induced SOA formation is experimentally demonstrated in this study, thus highlighting the importance of aqueous multiphase systems in atmospheric SOA formation estimations.
The impact of cloud events on isoprene secondary organic aerosol (SOA) formation has been...
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