Articles | Volume 24, issue 4
https://doi.org/10.5194/acp-24-2639-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-24-2639-2024
© Author(s) 2024. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
29 Feb 2024
Research article |
| 29 Feb 2024
| 29 Feb 2024
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
Feng Jiang
CORRESPONDING AUTHOR
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Institute of Applied Geosciences, Working Group for Environmental Mineralogy and Environmental System Analysis, Karlsruhe Institute of Technology, 76131 Karlsruhe, Germany
Kyla Siemens
Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States
Claudia Linke
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Yanxia Li
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Yiwei Gong
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Thomas Leisner
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Institute of Environmental Physics, Heidelberg University, 69120 Heidelberg, Germany
Alexander Laskin
Department of Chemistry, Purdue University, West Lafayette, Indiana 47907, United States
Department of Earth, Atmospheric and Planetary Sciences, Purdue University, West Lafayette, Indiana 47907, United States
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
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Short summary
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Jay M. Tomlin, Kevin A. Jankowski, Daniel P. Veghte, Swarup China, Peiwen Wang, Matthew Fraund, Johannes Weis, Guangjie Zheng, Yang Wang, Felipe Rivera-Adorno, Shira Raveh-Rubin, Daniel A. Knopf, Jian Wang, Mary K. Gilles, Ryan C. Moffet, and Alexander Laskin
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Lucía Caudillo, Birte Rörup, Martin Heinritzi, Guillaume Marie, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Antonio Amorim, Farnoush Ataei, Rima Baalbaki, Barbara Bertozzi, Zoé Brasseur, Randall Chiu, Biwu Chu, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Loïc Gonzalez Carracedo, Xu-Cheng He, Victoria Hofbauer, Weimeng Kong, Houssni Lamkaddam, Chuan P. Lee, Brandon Lopez, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Ruby Marten, Dario Massabò, Roy L. Mauldin, Bernhard Mentler, Ugo Molteni, Antti Onnela, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Meredith Schervish, Wiebke Scholz, Benjamin Schulze, Jiali Shen, Dominik Stolzenburg, Yuri Stozhkov, Mihnea Surdu, Christian Tauber, Yee Jun Tham, Ping Tian, António Tomé, Steffen Vogt, Mingyi Wang, Dongyu S. Wang, Stefan K. Weber, André Welti, Wang Yonghong, Wu Yusheng, Marcel Zauner-Wieczorek, Urs Baltensperger, Imad El Haddad, Richard C. Flagan, Armin Hansel, Kristina Höhler, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Ottmar Möhler, Harald Saathoff, Rainer Volkamer, Paul M. Winkler, Neil M. Donahue, Andreas Kürten, and Joachim Curtius
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We performed experiments in the CLOUD chamber at CERN at low temperatures to simulate new particle formation in the upper free troposphere (at −30 ºC and −50 ºC). We measured the particle and gas phase and found that most of the compounds present in the gas phase are detected as well in the particle phase. The major compounds in the particles are C8–10 and C18–20. Specifically, we showed that C5 and C15 compounds are detected in a mixed system with isoprene and α-pinene at −30 ºC, 20 % RH.
Larissa Lacher, Hans-Christian Clemen, Xiaoli Shen, Stephan Mertes, Martin Gysel-Beer, Alireza Moallemi, Martin Steinbacher, Stephan Henne, Harald Saathoff, Ottmar Möhler, Kristina Höhler, Thea Schiebel, Daniel Weber, Jann Schrod, Johannes Schneider, and Zamin A. Kanji
Atmos. Chem. Phys., 21, 16925–16953, https://doi.org/10.5194/acp-21-16925-2021, https://doi.org/10.5194/acp-21-16925-2021, 2021
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We investigate ice-nucleating particle properties at Jungfraujoch during the 2017 joint INUIT/CLACE field campaign, to improve the knowledge about those rare particles in a cloud-relevant environment. By quantifying ice-nucleating particles in parallel to single-particle mass spectrometry measurements, we find that mineral dust and aged sea spray particles are potential candidates for ice-nucleating particles. Our findings are supported by ice residual analysis and source region modeling.
Ulrich Platt, Thomas Wagner, Jonas Kuhn, and Thomas Leisner
Atmos. Meas. Tech., 14, 6867–6883, https://doi.org/10.5194/amt-14-6867-2021, https://doi.org/10.5194/amt-14-6867-2021, 2021
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Absorption spectroscopy of scattered sunlight is extremely useful for the analysis of atmospheric trace gas distributions. A central parameter for the achievable sensitivity of spectroscopic instruments is the light throughput, which can be enhanced in a number of ways. We present new ideas and considerations of how instruments could be optimized. Particular emphasis is on arrays of massively parallel instruments. Such arrays can reduce the size and weight of instruments by orders of magnitude.
Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Homogeneous freezing is a relevant mechanism for the formation of cirrus clouds in the upper troposphere. Based on an extensive set of homogeneous freezing experiments at the AIDA chamber with aqueous sulfuric acid aerosol, we provide a new fit line for homogeneous freezing onset conditions of sulfuric acid aerosol focusing on cirrus temperatures. In the atmosphere, homogeneous freezing thresholds have important implications on the cirrus cloud occurrence and related cloud radiative effects.
Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14215–14234, https://doi.org/10.5194/acp-21-14215-2021, https://doi.org/10.5194/acp-21-14215-2021, 2021
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We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.
Alexei A. Kiselev, Alice Keinert, Tilia Gaedeke, Thomas Leisner, Christoph Sutter, Elena Petrishcheva, and Rainer Abart
Atmos. Chem. Phys., 21, 11801–11814, https://doi.org/10.5194/acp-21-11801-2021, https://doi.org/10.5194/acp-21-11801-2021, 2021
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Alkali feldspar is the most abundant mineral in the Earth's crust and is often present in mineral dust aerosols that are responsible for the formation of rain and snow in clouds. However, the cloud droplets containing pure potassium-rich feldspar would not freeze unless cooled down to a very low temperature. Here we show that partly replacing potassium with sodium would induce fracturing of feldspar, exposing a crystalline surface that could initiate freezing at higher temperature.
Hengheng Zhang, Frank Wagner, Harald Saathoff, Heike Vogel, Gholam Ali Hoshyaripour, Vanessa Bachmann, Jochen Förstner, and Thomas Leisner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-193, https://doi.org/10.5194/amt-2021-193, 2021
Revised manuscript not accepted
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The evolution and the properties of Saharan dust plume were characterized by LIDARs, a sun photometer, and a regional transport model. Comparison between LIDAR measurements, sun photometer and ICON-ART predictions shows a good agreement for dust arrival time, dust layer height, and dust structure but also that the model overestimates the backscatter coefficients by a factor of (2.2 ± 0.16) and underestimate aerosol optical depth by a factor of (1.5 ± 0.11).
Yang Wang, Guangjie Zheng, Michael P. Jensen, Daniel A. Knopf, Alexander Laskin, Alyssa A. Matthews, David Mechem, Fan Mei, Ryan Moffet, Arthur J. Sedlacek, John E. Shilling, Stephen Springston, Amy Sullivan, Jason Tomlinson, Daniel Veghte, Rodney Weber, Robert Wood, Maria A. Zawadowicz, and Jian Wang
Atmos. Chem. Phys., 21, 11079–11098, https://doi.org/10.5194/acp-21-11079-2021, https://doi.org/10.5194/acp-21-11079-2021, 2021
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This paper reports the vertical profiles of trace gas and aerosol properties over the eastern North Atlantic, a region of persistent but diverse subtropical marine boundary layer (MBL) clouds. We examined the key processes that drive the cloud condensation nuclei (CCN) population and how it varies with season and synoptic conditions. This study helps improve the model representation of the aerosol processes in the remote MBL, reducing the simulated aerosol indirect effects.
Barbara Bertozzi, Robert Wagner, Junwei Song, Kristina Höhler, Joschka Pfeifer, Harald Saathoff, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 10779–10798, https://doi.org/10.5194/acp-21-10779-2021, https://doi.org/10.5194/acp-21-10779-2021, 2021
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Internally mixed particles composed of sulfate and organics are among the most abundant aerosol types. Their ice nucleation (IN) ability influences the formation of cirrus and, thus, the climate. We show that the presence of a thin organic coating suppresses the heterogeneous IN ability of crystalline ammonium sulfate particles. However, the IN ability of the same particle can substantially change if subjected to atmospheric processing, mainly due to differences in the resulting morphology.
Yue Zhou, Christopher P. West, Anusha P. S. Hettiyadura, Xiaoying Niu, Hui Wen, Jiecan Cui, Tenglong Shi, Wei Pu, Xin Wang, and Alexander Laskin
Atmos. Chem. Phys., 21, 8531–8555, https://doi.org/10.5194/acp-21-8531-2021, https://doi.org/10.5194/acp-21-8531-2021, 2021
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We present a comprehensive characterization of water-soluble organic carbon (WSOC) in seasonal snow of northwestern China. We applied complementary multimodal analytical techniques to investigate bulk and molecular-level composition, optical properties, and sources of WSOC. For the first time, we estimated the extent of radiative forcing due to WSOC in snow using a model simulation and showed the profound influences of WSOC on the energy budget of midlatitude seasonal snowpack.
Fritz Waitz, Martin Schnaiter, Thomas Leisner, and Emma Järvinen
Atmos. Meas. Tech., 14, 3049–3070, https://doi.org/10.5194/amt-14-3049-2021, https://doi.org/10.5194/amt-14-3049-2021, 2021
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A major challenge in the observations of mixed-phase clouds remains the phase discrimination and sizing of cloud droplets and ice crystals, especially for particles with diameters smaller than 0.1 mm. Here, we present a new method to derive the phase and size of single cloud particles using their angular-light-scattering information. Comparisons with other in situ instruments in three case studies show good agreement.
Julia Schneider, Kristina Höhler, Paavo Heikkilä, Jorma Keskinen, Barbara Bertozzi, Pia Bogert, Tobias Schorr, Nsikanabasi Silas Umo, Franziska Vogel, Zoé Brasseur, Yusheng Wu, Simo Hakala, Jonathan Duplissy, Dmitri Moisseev, Markku Kulmala, Michael P. Adams, Benjamin J. Murray, Kimmo Korhonen, Liqing Hao, Erik S. Thomson, Dimitri Castarède, Thomas Leisner, Tuukka Petäjä, and Ottmar Möhler
Atmos. Chem. Phys., 21, 3899–3918, https://doi.org/10.5194/acp-21-3899-2021, https://doi.org/10.5194/acp-21-3899-2021, 2021
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By triggering the formation of ice crystals, ice-nucleating particles (INP) strongly influence cloud formation. Continuous, long-term measurements are needed to characterize the atmospheric INP variability. Here, a first long-term time series of INP spectra measured in the boreal forest for more than 1 year is presented, showing a clear seasonal cycle. It is shown that the seasonal dependency of INP concentrations and prevalent INP types is driven by the abundance of biogenic aerosol.
Robert Wagner, Baptiste Testa, Michael Höpfner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, Jörn Ungermann, and Thomas Leisner
Atmos. Meas. Tech., 14, 1977–1991, https://doi.org/10.5194/amt-14-1977-2021, https://doi.org/10.5194/amt-14-1977-2021, 2021
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During the Asian summer monsoon period, air pollutants are transported from layers near the ground to high altitudes of 13 to 18 km in the atmosphere. Infrared measurements have shown that particles composed of solid ammonium nitrate are a major part of these pollutants. To enable the quantitative analysis of the infrared spectra, we have determined for the first time accurate optical constants of ammonium nitrate for the low-temperature conditions of the upper atmosphere.
Demetrios Pagonis, Pedro Campuzano-Jost, Hongyu Guo, Douglas A. Day, Melinda K. Schueneman, Wyatt L. Brown, Benjamin A. Nault, Harald Stark, Kyla Siemens, Alex Laskin, Felix Piel, Laura Tomsche, Armin Wisthaler, Matthew M. Coggon, Georgios I. Gkatzelis, Hannah S. Halliday, Jordan E. Krechmer, Richard H. Moore, David S. Thomson, Carsten Warneke, Elizabeth B. Wiggins, and Jose L. Jimenez
Atmos. Meas. Tech., 14, 1545–1559, https://doi.org/10.5194/amt-14-1545-2021, https://doi.org/10.5194/amt-14-1545-2021, 2021
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We describe the airborne deployment of an extractive electrospray time-of-flight mass spectrometer (EESI-MS). The instrument provides a quantitative 1 Hz measurement of the chemical composition of organic aerosol up to altitudes of
7 km, with single-compound detection limits as low as 50 ng per standard cubic meter.
Michael Krayer, Agathe Chouippe, Markus Uhlmann, Jan Dušek, and Thomas Leisner
Atmos. Chem. Phys., 21, 561–575, https://doi.org/10.5194/acp-21-561-2021, https://doi.org/10.5194/acp-21-561-2021, 2021
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We address the phenomenon of ice enhancement in the vicinity of warm hydrometeors using highly accurate flow simulation techniques. It is found that the transiently supersaturated zones induced by the hydrometeor's wake are by far larger than what has been previously estimated. The ice enhancement is quantified on the micro- and macroscale, and its relevance is discussed. The results provided may contribute to a (currently unavailable) parametrization of the phenomenon.
Ana C. Morales, Thilina Jayarathne, Jonathan H. Slade, Alexander Laskin, and Paul B. Shepson
Atmos. Chem. Phys., 21, 129–145, https://doi.org/10.5194/acp-21-129-2021, https://doi.org/10.5194/acp-21-129-2021, 2021
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Organic nitrates formed from the oxidation of biogenic volatile organic compounds impact both ozone and particulate matter as they remove nitrogen oxides, but they represent important aerosol precursors. We conducted a series of reaction chamber experiments that quantified the total organic nitrate and secondary organic aerosol yield from the OH-radical-initiated oxidation of ocimene, and also measured their hydrolysis lifetimes in the aqueous phase, as a function of pH.
Alexei Korolev and Thomas Leisner
Atmos. Chem. Phys., 20, 11767–11797, https://doi.org/10.5194/acp-20-11767-2020, https://doi.org/10.5194/acp-20-11767-2020, 2020
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Secondary ice production (SIP) plays a key role in the formation of ice particles in tropospheric clouds. This work presents a critical review of the laboratory studies related to secondary ice production. It aims to identify gaps in our knowledge of SIP as well as to stimulate further laboratory studies focused on obtaining a quantitative description of efficiencies for each SIP mechanism.
Matthew Fraund, Daniel J. Bonanno, Swarup China, Don Q. Pham, Daniel Veghte, Johannes Weis, Gourihar Kulkarni, Ken Teske, Mary K. Gilles, Alexander Laskin, and Ryan C. Moffet
Atmos. Chem. Phys., 20, 11593–11606, https://doi.org/10.5194/acp-20-11593-2020, https://doi.org/10.5194/acp-20-11593-2020, 2020
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High viscosity organic particles (HVOPs) in the Southern Great Plains have been analyzed, and two particle types were found. Previously studied tar balls and the recently discovered airborne soil organic particles (ASOPs) are both shown to be brown carbon (BrC). These particle types can be identified in bulk by an absorption Ångström exponent approaching 2.6. HVOP types can be differentiated by comparing carbon absorption spectrum peak ratios between the carboxylic acid, alcohol, and sp2 peaks.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
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In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Benjamin W. Clouser, Kara D. Lamb, Laszlo C. Sarkozy, Jan Habig, Volker Ebert, Harald Saathoff, Ottmar Möhler, and Elisabeth J. Moyer
Atmos. Chem. Phys., 20, 1089–1103, https://doi.org/10.5194/acp-20-1089-2020, https://doi.org/10.5194/acp-20-1089-2020, 2020
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Previous measurements of water vapor in the upper troposphere and lower stratosphere (UT/LS) have shown unexpectedly high concentrations of water vapor in ice clouds, which may be due to an incomplete understanding of the structure of ice and the behavior of ice growth in this part of the atmosphere. Water vapor measurements during the 2013 IsoCloud campaign at the AIDA cloud chamber show no evidence of this
anomalous supersaturationin conditions similar to the real atmosphere.
Lauren T. Fleming, Peng Lin, James M. Roberts, Vanessa Selimovic, Robert Yokelson, Julia Laskin, Alexander Laskin, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 20, 1105–1129, https://doi.org/10.5194/acp-20-1105-2020, https://doi.org/10.5194/acp-20-1105-2020, 2020
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We have explored the nature and stability of molecules that give biomass burning smoke its faint brown color. Different types of biomass fuels were burned and the resulting smoke was collected for a detailed chemical analysis. We found that brown molecules in smoke become less colored when they are irradiated by sunlight, but this photobleaching process is very slow. This means that biomass burning smoke will remain brown-colored for a long time and efficiently warm up the atmosphere.
Xiaoli Shen, Heike Vogel, Bernhard Vogel, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, Thomas Leisner, André S. H. Prévôt, and Harald Saathoff
Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, https://doi.org/10.5194/acp-19-13189-2019, 2019
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This study provides good insight into the chemical nature and complex origin of aerosols by combining comprehensive field observations and transport modelling. We suggest that factors related to topography, metrological conditions, local emissions, in situ formation and growth, regional transport, and the interaction of biogenic and anthropogenic compounds need to be considered for a comprehensive understanding of aerosol processes.
Tasha Aylett, James S. A. Brooke, Alexander D. James, Mario Nachbar, Denis Duft, Thomas Leisner, and John M. C. Plane
Atmos. Chem. Phys., 19, 12767–12777, https://doi.org/10.5194/acp-19-12767-2019, https://doi.org/10.5194/acp-19-12767-2019, 2019
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Interplanetary dust particles entering the Earth's atmosphere often melt and evaporate, injecting metals such as iron and magnesium into the atmosphere between 80 and 105 km. These metals become oxidized and then coagulate into small particles a few nanometres is size, known as meteoric smoke. In this study, iron oxide smoke particles were created in the laboratory, and their composition and optical properties were determined in order to understand satellite measurements.
Mijung Song, Adrian M. Maclean, Yuanzhou Huang, Natalie R. Smith, Sandra L. Blair, Julia Laskin, Alexander Laskin, Wing-Sy Wong DeRieux, Ying Li, Manabu Shiraiwa, Sergey A. Nizkorodov, and Allan K. Bertram
Atmos. Chem. Phys., 19, 12515–12529, https://doi.org/10.5194/acp-19-12515-2019, https://doi.org/10.5194/acp-19-12515-2019, 2019
Wei Huang, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 19, 11687–11700, https://doi.org/10.5194/acp-19-11687-2019, https://doi.org/10.5194/acp-19-11687-2019, 2019
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We investigate the molecular composition and volatility of oxygenated organic aerosol (OOA) particles in summer and winter in Stuttgart, Germany. OOA in summer is more influenced by biogenic emissions, while in winter biomass burning emissions are an important source. OOA in winter is also less volatile. Potential reasons are discussed in our paper. Our study shows the important contributions of nonfossil OA from biogenic and biomass burning even in an urban area with high traffic emissions.
Martin Schnaiter, Claudia Linke, Inas Ibrahim, Alexei Kiselev, Fritz Waitz, Thomas Leisner, Stefan Norra, and Till Rehm
Atmos. Chem. Phys., 19, 10829–10844, https://doi.org/10.5194/acp-19-10829-2019, https://doi.org/10.5194/acp-19-10829-2019, 2019
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When combustion particles are deposited to the ground, they darken Earth's snow and ice surfaces by even tiny quantities. This darkening reduces the back reflection of sunlight and induces an additional climate warming. Particles from fresh snow samples were investigated according to their light absorption strength. Enhanced absorption was found in the snow that cannot fully be attributed to combustion particles. Dust and biogenic matter are likely the cause of this additional snow darkening.
Nsikanabasi Silas Umo, Robert Wagner, Romy Ullrich, Alexei Kiselev, Harald Saathoff, Peter G. Weidler, Daniel J. Cziczo, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 19, 8783–8800, https://doi.org/10.5194/acp-19-8783-2019, https://doi.org/10.5194/acp-19-8783-2019, 2019
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Annually, over 600 Tg of coal fly ash (CFA) is produced; a significant proportion of this amount is injected into the atmosphere, which could significantly contribute to heterogeneous ice formation in clouds. This study presents an improved understanding of CFA particles' behaviour in forming ice in clouds, especially when exposed to lower temperatures before being re-circulated in the upper troposphere or entrained into the lower troposphere.
Zamin A. Kanji, Ryan C. Sullivan, Monika Niemand, Paul J. DeMott, Anthony J. Prenni, Cédric Chou, Harald Saathoff, and Ottmar Möhler
Atmos. Chem. Phys., 19, 5091–5110, https://doi.org/10.5194/acp-19-5091-2019, https://doi.org/10.5194/acp-19-5091-2019, 2019
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The ice nucleation ability of two natural desert dusts coated with a proxy of secondary organic aerosol is presented for temperatures and relative humidity conditions relevant for mixed-phase clouds. We find that at the tested conditions, there is no effect on the ice nucleation ability of the particles due to the organic coating. Furthermore, the two dust samples do not show variability within measurement uncertainty. Particle size and surface area may play a role in any difference observed.
Xiaoli Shen, Harald Saathoff, Wei Huang, Claudia Mohr, Ramakrishna Ramisetty, and Thomas Leisner
Atmos. Meas. Tech., 12, 2219–2240, https://doi.org/10.5194/amt-12-2219-2019, https://doi.org/10.5194/amt-12-2219-2019, 2019
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Based on single-particle mass spectra from field measurements in the upper Rhine valley, we identified characteristic particle classes and estimated their mass contributions without the need of a reference instrument in the field. Our study provides a good example for quantitative interpretation of single-particle data. Together with the complimentary results from bulk measurements, we have shown how a better understanding of the mixing state of ambient aerosol particles can be achieved.
Mario Nachbar, Henrike Wilms, Denis Duft, Tasha Aylett, Kensei Kitajima, Takuya Majima, John M. C. Plane, Markus Rapp, and Thomas Leisner
Atmos. Chem. Phys., 19, 4311–4322, https://doi.org/10.5194/acp-19-4311-2019, https://doi.org/10.5194/acp-19-4311-2019, 2019
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Polar mesospheric clouds (PMC) are water ice clouds forming on nanoparticles in the polar summer mesopause. We investigate the impact of solar radiation on PMC formation in the laboratory. We show that Mie theory calculations combined with an equilibrium temperature model presented in this work predict the warming of the particles very well. Using this model we demonstrate that the impact of solar radiation on ice particle formation is significantly lower than previously assumed.
Denis Duft, Mario Nachbar, and Thomas Leisner
Atmos. Chem. Phys., 19, 2871–2879, https://doi.org/10.5194/acp-19-2871-2019, https://doi.org/10.5194/acp-19-2871-2019, 2019
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How ice particles form in polar mesospheric clouds is still a challenging question. We measured the water adsorption and onset conditions for ice growth on meteoric smoke analogue particles in the laboratory. We find that the particles activate by growth of amorphous ice and at much warmer conditions than previously assumed, affirming meteoric smoke as likely seeds in mesospheric ice clouds. We propose an ice-activation model and show that the particle charge does not play a significant role.
Victoria E. Irish, Sarah J. Hanna, Megan D. Willis, Swarup China, Jennie L. Thomas, Jeremy J. B. Wentzell, Ana Cirisan, Meng Si, W. Richard Leaitch, Jennifer G. Murphy, Jonathan P. D. Abbatt, Alexander Laskin, Eric Girard, and Allan K. Bertram
Atmos. Chem. Phys., 19, 1027–1039, https://doi.org/10.5194/acp-19-1027-2019, https://doi.org/10.5194/acp-19-1027-2019, 2019
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Ice nucleating particles (INPs) are atmospheric particles that catalyse the formation of ice crystals in clouds. INPs influence the Earth's radiative balance and hydrological cycle. In this study we measured the concentrations of INPs in the Canadian Arctic marine boundary layer. Average INP concentrations fell within the range measured in other marine boundary layer locations. We also found that mineral dust is a more important contributor to the INP population than sea spray aerosol.
Chunlin Li, Quanfu He, Julian Schade, Johannes Passig, Ralf Zimmermann, Daphne Meidan, Alexander Laskin, and Yinon Rudich
Atmos. Chem. Phys., 19, 139–163, https://doi.org/10.5194/acp-19-139-2019, https://doi.org/10.5194/acp-19-139-2019, 2019
Emma Järvinen, Olivier Jourdan, David Neubauer, Bin Yao, Chao Liu, Meinrat O. Andreae, Ulrike Lohmann, Manfred Wendisch, Greg M. McFarquhar, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 18, 15767–15781, https://doi.org/10.5194/acp-18-15767-2018, https://doi.org/10.5194/acp-18-15767-2018, 2018
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Using light diffraction it is possible to detect microscopic features within ice particles that have not yet been fully characterized. Here, this technique was applied in airborne measurements, where it was found that majority of atmospheric ice particles have features that significantly change the way ice particles interact with solar light. The microscopic features make ice-containing clouds more reflective than previously thought, which could have consequences for predicting our climate.
Amy L. Bondy, Daniel Bonanno, Ryan C. Moffet, Bingbing Wang, Alexander Laskin, and Andrew P. Ault
Atmos. Chem. Phys., 18, 12595–12612, https://doi.org/10.5194/acp-18-12595-2018, https://doi.org/10.5194/acp-18-12595-2018, 2018
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To determine important sources of aerosols during the Southern Oxidant and Aerosol Study (SOAS), as well as their mixing with secondary species, individual particles were analyzed with electron and X-ray microscopy to determine size and chemical composition. Secondary organic aerosol, sea spray aerosol, and mineral dust each dominated during different periods. Particles were less similar chemically to each other than is commonly assumed, which is important for air quality and climate models.
Ramakrishna Ramisetty, Ahmed Abdelmonem, Xiaoli Shen, Harald Saathoff, Thomas Leisner, and Claudia Mohr
Atmos. Meas. Tech., 11, 4345–4360, https://doi.org/10.5194/amt-11-4345-2018, https://doi.org/10.5194/amt-11-4345-2018, 2018
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In this study we coupled a laser ablation aerosol time-of-flight (LAAPTOF) single-particle mass spectrometer, originally equipped with an excimer laser, to a femtosecond laser. The objective was to assess the influence of the higher laser power density of the femtosecond laser on ablation–ionization of atmospheric particles, ion signal, and ultimately quantitative abilities of the single-particle mass spectrometer.
Wing-Sy Wong DeRieux, Ying Li, Peng Lin, Julia Laskin, Alexander Laskin, Allan K. Bertram, Sergey A. Nizkorodov, and Manabu Shiraiwa
Atmos. Chem. Phys., 18, 6331–6351, https://doi.org/10.5194/acp-18-6331-2018, https://doi.org/10.5194/acp-18-6331-2018, 2018
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The phase transition of organic particles between glassy and semi-solid states occurs at the glass transition temperature. We developed a method to predict glass transition temperatures and the viscosity of secondary organic aerosols using molecular composition, with consistent results with viscosity measurements. The viscosity of biomass burning particles was also estimated using the chemical composition measured by high-resolution mass spectrometry with two different ionization techniques.
Xiaoli Shen, Ramakrishna Ramisetty, Claudia Mohr, Wei Huang, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 11, 2325–2343, https://doi.org/10.5194/amt-11-2325-2018, https://doi.org/10.5194/amt-11-2325-2018, 2018
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This paper presents performance data and reference spectra from the commercially available single-particle mass spectrometer LAAPTOF. The main characteristics of the instrument, like its detection efficiency, are given for a wide particle size range. Furthermore, reference mass spectra for 32 well-defined different particle types relevant for atmospheric aerosol compounds are presented. It is shown that these reference mass spectra are very useful in analysis of atmospheric aerosol particles.
Rachel M. Kirpes, Amy L. Bondy, Daniel Bonanno, Ryan C. Moffet, Bingbing Wang, Alexander Laskin, Andrew P. Ault, and Kerri A. Pratt
Atmos. Chem. Phys., 18, 3937–3949, https://doi.org/10.5194/acp-18-3937-2018, https://doi.org/10.5194/acp-18-3937-2018, 2018
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Arctic atmospheric particles have important climate impacts via cloud formation and precipitation, particularly in the wintertime. We show that sulfate, formed during atmospheric transport, is within individual sea spray particles and organic particles measured in the Alaskan Arctic. Greater contributions of combustion emissions were observed when the wind direction came from the Prudhoe Bay oil fields, showing its regional influence.
Mario Nachbar, Denis Duft, and Thomas Leisner
Atmos. Chem. Phys., 18, 3419–3431, https://doi.org/10.5194/acp-18-3419-2018, https://doi.org/10.5194/acp-18-3419-2018, 2018
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The crystallization process of amorphous ice below 160 K forms nano-crystalline ice. We report high-quality vapor pressure measurements over ice crystallized from amorphous ice below 160 K. We show that the vapor pressure is increased by more than 100 % compared to bulk crystalline ice and that amorphous ice always forms first, followed by the crystallization of nano-crystalline ice. Our findings are relevant for cold ice clouds in the atmospheres of planets, e.g., Earth and Mars.
Wei Huang, Harald Saathoff, Aki Pajunoja, Xiaoli Shen, Karl-Heinz Naumann, Robert Wagner, Annele Virtanen, Thomas Leisner, and Claudia Mohr
Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, https://doi.org/10.5194/acp-18-2883-2018, 2018
Lauren T. Fleming, Peng Lin, Alexander Laskin, Julia Laskin, Robert Weltman, Rufus D. Edwards, Narendra K. Arora, Ankit Yadav, Simone Meinardi, Donald R. Blake, Ajay Pillarisetti, Kirk R. Smith, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 2461–2480, https://doi.org/10.5194/acp-18-2461-2018, https://doi.org/10.5194/acp-18-2461-2018, 2018
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Household cooking emissions in India, which rely on traditional meal preparation with dung- and brushwood-fueled cookstoves, produce copious amounts of particulate matter. Detailed chemical analysis of the compounds found in this particulate matter detected a large number of previously unidentified nitrogen-containing organic compounds, originating from dung-fueled cookstoves.
Mallory L. Hinks, Julia Montoya-Aguilera, Lucas Ellison, Peng Lin, Alexander Laskin, Julia Laskin, Manabu Shiraiwa, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 18, 1643–1652, https://doi.org/10.5194/acp-18-1643-2018, https://doi.org/10.5194/acp-18-1643-2018, 2018
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We have observed a strong effect of relative humidity on the composition of particulate matter produced from the oxidation of toluene in clean air. At higher relative humidity, there was a significant reduction in the fraction of high-molecular-weight compounds present in the particles. The amount of particulate matter also decreased at higher relative humidity. The main implication of this study is that water vapor participates in the photooxidation of toluene in a complicated way.
Sylvia C. Sullivan, Corinna Hoose, Alexei Kiselev, Thomas Leisner, and Athanasios Nenes
Atmos. Chem. Phys., 18, 1593–1610, https://doi.org/10.5194/acp-18-1593-2018, https://doi.org/10.5194/acp-18-1593-2018, 2018
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Ice multiplication (IM) processes can have a profound impact on cloud and precipitation development but are poorly understood. Here we study whether a lower limit of ice nuclei exists to initiate IM. The lower limit is found to be extremely low (0.01 per liter or less). A counterintuitive but profound conclusion thus emerges: IM requires cloud formation around a thermodynamic
sweet spotand is sensitive to fluctuations in cloud condensation nuclei concentration alone.
Martin Schnaiter, Emma Järvinen, Ahmed Abdelmonem, and Thomas Leisner
Atmos. Meas. Tech., 11, 341–357, https://doi.org/10.5194/amt-11-341-2018, https://doi.org/10.5194/amt-11-341-2018, 2018
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PHIPS-HALO is a novel aircraft instrument for cloud research. It combines microscopic imaging of single cloud particles with the measurement of their spacial light scattering properties. The knowledge of how atmospheric ice particles in clouds scatter visible light is important for improving future climate models.
Ryan D. Cook, Ying-Hsuan Lin, Zhuoyu Peng, Eric Boone, Rosalie K. Chu, James E. Dukett, Matthew J. Gunsch, Wuliang Zhang, Nikola Tolic, Alexander Laskin, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 15167–15180, https://doi.org/10.5194/acp-17-15167-2017, https://doi.org/10.5194/acp-17-15167-2017, 2017
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Reactions occur within water in both atmospheric particles and cloud droplets, yet little is known about the organic compounds in cloud water. In this work, cloud water samples were collected at Whiteface Mountain, New York, and analyzed using ultra-high-resolution mass spectrometry to investigate the molecular composition of the dissolved organic compounds. The results focus on changes in cloud water composition with air mass origin – influences of forest, urban, and wildfire emissions.
Julia Montoya-Aguilera, Jeremy R. Horne, Mallory L. Hinks, Lauren T. Fleming, Véronique Perraud, Peng Lin, Alexander Laskin, Julia Laskin, Donald Dabdub, and Sergey A. Nizkorodov
Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, https://doi.org/10.5194/acp-17-11605-2017, 2017
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Various plant species emit a chemical compound called indole under stressed conditions or during flowering events. Our experiments show that indole can be oxidized in the atmosphere to produce a brownish haze containing well-known indole-derived dyes, such as indigo dye. An airshed model that includes indole chemistry shows that indole aerosol makes a significant contribution to the total aerosol burden and to visibility.
Yevgeny Derimian, Marie Choël, Yinon Rudich, Karine Deboudt, Oleg Dubovik, Alexander Laskin, Michel Legrand, Bahaiddin Damiri, Ilan Koren, Florin Unga, Myriam Moreau, Meinrat O. Andreae, and Arnon Karnieli
Atmos. Chem. Phys., 17, 11331–11353, https://doi.org/10.5194/acp-17-11331-2017, https://doi.org/10.5194/acp-17-11331-2017, 2017
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We present influence of daily occurrence of the sea breeze flow from the Mediterranean Sea on physicochemical and optical properties of atmospheric aerosol deep inland in the Negev Desert of Israel. Sampled airborne dust was found be internally mixed with sea-salt particles and reacted with anthropogenic pollution, which makes the dust highly hygroscopic and a liquid coating of particles appears. These physicochemical transformations are associated with a change in aerosol radiative properties.
Matthew J. Gunsch, Rachel M. Kirpes, Katheryn R. Kolesar, Tate E. Barrett, Swarup China, Rebecca J. Sheesley, Alexander Laskin, Alfred Wiedensohler, Thomas Tuch, and Kerri A. Pratt
Atmos. Chem. Phys., 17, 10879–10892, https://doi.org/10.5194/acp-17-10879-2017, https://doi.org/10.5194/acp-17-10879-2017, 2017
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Arctic sea ice loss is leading to increasing petroleum extraction and shipping. It is necessary to identify emissions from these activities for improved Arctic air quality and climate assessment. Atmospheric particles were measured from August to September 2015 in Utqiaġvik, AK. For periods influenced by Prudhoe Bay, significant influence associated with combustion emissions was observed, compared to fresh sea spray influence during Arctic Ocean periods.
Adam P. Bateman, Zhaoheng Gong, Tristan H. Harder, Suzane S. de Sá, Bingbing Wang, Paulo Castillo, Swarup China, Yingjun Liu, Rachel E. O'Brien, Brett B. Palm, Hung-Wei Shiu, Glauber G. Cirino, Ryan Thalman, Kouji Adachi, M. Lizabeth Alexander, Paulo Artaxo, Allan K. Bertram, Peter R. Buseck, Mary K. Gilles, Jose L. Jimenez, Alexander Laskin, Antonio O. Manzi, Arthur Sedlacek, Rodrigo A. F. Souza, Jian Wang, Rahul Zaveri, and Scot T. Martin
Atmos. Chem. Phys., 17, 1759–1773, https://doi.org/10.5194/acp-17-1759-2017, https://doi.org/10.5194/acp-17-1759-2017, 2017
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The occurrence of nonliquid and liquid physical states of submicron atmospheric particulate matter (PM) downwind of an urban region in central Amazonia was investigated. Air masses representing background conditions, urban pollution, and regional- and continental-scale biomass were measured. Anthropogenic influences contributed to the presence of nonliquid PM in the atmospheric particle population, while liquid PM dominated during periods of biogenic influence.
Ryan C. Moffet, Rachel E. O'Brien, Peter A. Alpert, Stephen T. Kelly, Don Q. Pham, Mary K. Gilles, Daniel A. Knopf, and Alexander Laskin
Atmos. Chem. Phys., 16, 14515–14525, https://doi.org/10.5194/acp-16-14515-2016, https://doi.org/10.5194/acp-16-14515-2016, 2016
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Atmospheric black carbon (BC), commonly known as soot, is an important constituent of the earth that imparts a warming similar to that of carbon dioxide. However, BC is much shorter lived and has uncertain warming due to its mixture with other solid and liquid components. Here, advanced microscopic methods have provided a detailed look at thousands of BC particles sampled from central California; these measurements will lead towards a better understanding of the effects that BC has on climate.
Claudia Linke, Inas Ibrahim, Nina Schleicher, Regina Hitzenberger, Meinrat O. Andreae, Thomas Leisner, and Martin Schnaiter
Atmos. Meas. Tech., 9, 5331–5346, https://doi.org/10.5194/amt-9-5331-2016, https://doi.org/10.5194/amt-9-5331-2016, 2016
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Various carbonaceous materials are present in the atmosphere. Besides gaseous organic compounds, carbonaceous particles like soot are emitted into the air from traffic sources, residential wood combustion, or wildfires. Variable chemical compositions of such materials, which often result from incomplete combustion processes, show differences in the absorption behavior at visible wavelengths. Our instrument is able to measure the absorption at three visible wavelengths.
Jiumeng Liu, Peng Lin, Alexander Laskin, Julia Laskin, Shawn M. Kathmann, Matthew Wise, Ryan Caylor, Felisha Imholt, Vanessa Selimovic, and John E. Shilling
Atmos. Chem. Phys., 16, 12815–12827, https://doi.org/10.5194/acp-16-12815-2016, https://doi.org/10.5194/acp-16-12815-2016, 2016
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Light absorbing organic aerosols (BrC) absorb sunlight thereby influencing climate; however, understanding of the link between their optical properties and environmental variables remains limited. Our chamber experiment results suggest that variables including NOx concentration, RH level, and photolysis time have considerable influence on secondary BrC optical properties. The results contribute to a more accurate characterization of the impacts of aerosols on climate, especially in urban areas.
Andreas Peckhaus, Alexei Kiselev, Thibault Hiron, Martin Ebert, and Thomas Leisner
Atmos. Chem. Phys., 16, 11477–11496, https://doi.org/10.5194/acp-16-11477-2016, https://doi.org/10.5194/acp-16-11477-2016, 2016
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The precipitation in midlatitude clouds proceeds predominantly via nucleation of ice in the supercooled droplets containing foreign inclusions, like feldspar mineral dust, that have been recently identified as one of the most active ice nucleating agents in the atmosphere. We have built an apparatus to observe the freezing of feldspar immersed in up to 1500 identical droplets simultaneously. With this setup we investigated four feldspar samples and show that it can induce freezing at −5 °C.
Yvonne Boose, Berko Sierau, M. Isabel García, Sergio Rodríguez, Andrés Alastuey, Claudia Linke, Martin Schnaiter, Piotr Kupiszewski, Zamin A. Kanji, and Ulrike Lohmann
Atmos. Chem. Phys., 16, 9067–9087, https://doi.org/10.5194/acp-16-9067-2016, https://doi.org/10.5194/acp-16-9067-2016, 2016
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Mineral dust is known to be among the most prevalent ice-nucleating particles (INPs) in the atmosphere, playing a crucial role for ice cloud formation. We present 2 months of ground-based in situ measurements of INP concentrations in the free troposphere close to the largest global dust source, the Sahara. We find that some atmospheric processes such as mixing with biological particles and ammonium increase the dust INP ability. This is important when predicting INPs based on emissions.
Ahmed Abdelmonem, Emma Järvinen, Denis Duft, Edwin Hirst, Steffen Vogt, Thomas Leisner, and Martin Schnaiter
Atmos. Meas. Tech., 9, 3131–3144, https://doi.org/10.5194/amt-9-3131-2016, https://doi.org/10.5194/amt-9-3131-2016, 2016
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The properties of ice crystals present in mixed-phase and ice clouds influence the radiation properties, precipitation occurrence and lifetime of these clouds. It is necessary to investigate the optical and microphysical properties of cloud particles particularly in situ, and to get correlation between these properties. To this end we have developed PHIPS-HALO to measure the optical properties and the corresponding microphysical parameters of individual cloud particles simultaneously.
Karoliina Ignatius, Thomas B. Kristensen, Emma Järvinen, Leonid Nichman, Claudia Fuchs, Hamish Gordon, Paul Herenz, Christopher R. Hoyle, Jonathan Duplissy, Sarvesh Garimella, Antonio Dias, Carla Frege, Niko Höppel, Jasmin Tröstl, Robert Wagner, Chao Yan, Antonio Amorim, Urs Baltensperger, Joachim Curtius, Neil M. Donahue, Martin W. Gallagher, Jasper Kirkby, Markku Kulmala, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Antonio Tomé, Annele Virtanen, Douglas Worsnop, and Frank Stratmann
Atmos. Chem. Phys., 16, 6495–6509, https://doi.org/10.5194/acp-16-6495-2016, https://doi.org/10.5194/acp-16-6495-2016, 2016
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Viscous solid or semi-solid secondary organic aerosol (SOA) may influence cloud properties through ice nucleation in the atmosphere. Here, we observed heterogeneous ice nucleation of viscous α-pinene SOA at temperatures between −39 °C and −37.2 °C with ice saturation ratios significantly below the homogeneous freezing limit. Global modelling suggests that viscous biogenic SOA are present in regions where cirrus formation takes place and could contribute to the global ice nuclei budget.
Lu Yu, Jeremy Smith, Alexander Laskin, Katheryn M. George, Cort Anastasio, Julia Laskin, Ann M. Dillner, and Qi Zhang
Atmos. Chem. Phys., 16, 4511–4527, https://doi.org/10.5194/acp-16-4511-2016, https://doi.org/10.5194/acp-16-4511-2016, 2016
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The chemical evolution of SOA formed during aqueous reactions of phenolic compounds is studied via combined bulk and molecular analysis. Phenolic SOA evolve dynamically during photochemical aging, with different reaction mechanisms (oligomerization, fragmentation, and functionalization) leading to different generations of products that span an enormous range in volatilities and a large range in oxidation state and composition. Aqueous reactions of phenols are likely an important source of ELVOC.
Emma Järvinen, Karoliina Ignatius, Leonid Nichman, Thomas B. Kristensen, Claudia Fuchs, Christopher R. Hoyle, Niko Höppel, Joel C. Corbin, Jill Craven, Jonathan Duplissy, Sebastian Ehrhart, Imad El Haddad, Carla Frege, Hamish Gordon, Tuija Jokinen, Peter Kallinger, Jasper Kirkby, Alexei Kiselev, Karl-Heinz Naumann, Tuukka Petäjä, Tamara Pinterich, Andre S. H. Prevot, Harald Saathoff, Thea Schiebel, Kamalika Sengupta, Mario Simon, Jay G. Slowik, Jasmin Tröstl, Annele Virtanen, Paul Vochezer, Steffen Vogt, Andrea C. Wagner, Robert Wagner, Christina Williamson, Paul M. Winkler, Chao Yan, Urs Baltensperger, Neil M. Donahue, Rick C. Flagan, Martin Gallagher, Armin Hansel, Markku Kulmala, Frank Stratmann, Douglas R. Worsnop, Ottmar Möhler, Thomas Leisner, and Martin Schnaiter
Atmos. Chem. Phys., 16, 4423–4438, https://doi.org/10.5194/acp-16-4423-2016, https://doi.org/10.5194/acp-16-4423-2016, 2016
Leonid Nichman, Claudia Fuchs, Emma Järvinen, Karoliina Ignatius, Niko Florian Höppel, Antonio Dias, Martin Heinritzi, Mario Simon, Jasmin Tröstl, Andrea Christine Wagner, Robert Wagner, Christina Williamson, Chao Yan, Paul James Connolly, James Robert Dorsey, Jonathan Duplissy, Sebastian Ehrhart, Carla Frege, Hamish Gordon, Christopher Robert Hoyle, Thomas Bjerring Kristensen, Gerhard Steiner, Neil McPherson Donahue, Richard Flagan, Martin William Gallagher, Jasper Kirkby, Ottmar Möhler, Harald Saathoff, Martin Schnaiter, Frank Stratmann, and António Tomé
Atmos. Chem. Phys., 16, 3651–3664, https://doi.org/10.5194/acp-16-3651-2016, https://doi.org/10.5194/acp-16-3651-2016, 2016
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Processes in the atmosphere are often governed by the physical and chemical properties of small cloud particles. Ice, water, and mixed clouds, as well as viscous aerosols, were formed under controlled conditions at the CLOUD-CERN facility. The experimental results show a link between cloud particle properties and their unique optical fingerprints. The classification map presented here allows easier discrimination between various particles such as viscous organic aerosol, salt, ice, and liquid.
Robert Wagner, Alexei Kiselev, Ottmar Möhler, Harald Saathoff, and Isabelle Steinke
Atmos. Chem. Phys., 16, 2025–2042, https://doi.org/10.5194/acp-16-2025-2016, https://doi.org/10.5194/acp-16-2025-2016, 2016
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We have investigated the enhancement of the ice nucleation ability of well-known and abundant ice nucleating particles like dust grains due to pre-activation. Temporary exposure to a low temperature (228 K) provokes that pores and surface cracks of the particles are filled with ice, which makes them better nuclei for the growth of macroscopic ice crystals at high temperatures (245–260 K).
C. R. Hoyle, C. Fuchs, E. Järvinen, H. Saathoff, A. Dias, I. El Haddad, M. Gysel, S. C. Coburn, J. Tröstl, A.-K. Bernhammer, F. Bianchi, M. Breitenlechner, J. C. Corbin, J. Craven, N. M. Donahue, J. Duplissy, S. Ehrhart, C. Frege, H. Gordon, N. Höppel, M. Heinritzi, T. B. Kristensen, U. Molteni, L. Nichman, T. Pinterich, A. S. H. Prévôt, M. Simon, J. G. Slowik, G. Steiner, A. Tomé, A. L. Vogel, R. Volkamer, A. C. Wagner, R. Wagner, A. S. Wexler, C. Williamson, P. M. Winkler, C. Yan, A. Amorim, J. Dommen, J. Curtius, M. W. Gallagher, R. C. Flagan, A. Hansel, J. Kirkby, M. Kulmala, O. Möhler, F. Stratmann, D. R. Worsnop, and U. Baltensperger
Atmos. Chem. Phys., 16, 1693–1712, https://doi.org/10.5194/acp-16-1693-2016, https://doi.org/10.5194/acp-16-1693-2016, 2016
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A significant portion of sulphate, an important constituent of atmospheric aerosols, is formed via the aqueous phase oxidation of sulphur dioxide by ozone. The rate of this reaction has previously only been measured over a relatively small temperature range. Here, we use the state of the art CLOUD chamber at CERN to perform the first measurements of this reaction rate in super-cooled droplets, confirming that the existing extrapolation of the reaction rate to sub-zero temperatures is accurate.
P. Vochezer, E. Järvinen, R. Wagner, P. Kupiszewski, T. Leisner, and M. Schnaiter
Atmos. Meas. Tech., 9, 159–177, https://doi.org/10.5194/amt-9-159-2016, https://doi.org/10.5194/amt-9-159-2016, 2016
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To study clouds constituting of liquid droplets as well as ice particles we used the latest versions of the Small Ice Detector which record high resolution scattering patterns of individual small cloud particles. In the case of a droplet its precise size is obtained and for ice particles its shape is deduced from the scattering pattern.We present results from artificial clouds at the AIDA cloud chamber and natural clouds probed at a mountain top station as well as from an aircraft in the arctic.
H. M. Allen, D. C. Draper, B. R. Ayres, A. Ault, A. Bondy, S. Takahama, R. L. Modini, K. Baumann, E. Edgerton, C. Knote, A. Laskin, B. Wang, and J. L. Fry
Atmos. Chem. Phys., 15, 10669–10685, https://doi.org/10.5194/acp-15-10669-2015, https://doi.org/10.5194/acp-15-10669-2015, 2015
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We report ion chromatographic measurements of gas- and aerosol-phase inorganic species at the SOAS 2013 field study. Our particular focus is on inorganic nitrate aerosol formation via HNO3 uptake onto coarse-mode dust and sea salt particles, which we find to be the dominant source of episodic inorganic nitrate at this site, due to the high acidity of the particles preventing formation of NH4NO3. We calculate a production rate of inorganic nitrate aerosol.
A. Abdelmonem, J. Lützenkirchen, and T. Leisner
Atmos. Meas. Tech., 8, 3519–3526, https://doi.org/10.5194/amt-8-3519-2015, https://doi.org/10.5194/amt-8-3519-2015, 2015
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This manuscript belongs and is important to the environmental and atmospheric science, particularly cloud formation and cloud seeding, and presents a setup to apply Second Harmonic Generation spectroscopy to heterogeneous freezing research. We describe the setup and provide first results on temperature-dependent structural changes of water on the surfaces of two relevant atmospheric aerosol substances (sapphire and mica as poor and good ice nucleators, respectively).
J. Diab, T. Streibel, F. Cavalli, S. C. Lee, H. Saathoff, A. Mamakos, J. C. Chow, L.-W. A. Chen, J. G. Watson, O. Sippula, and R. Zimmermann
Atmos. Meas. Tech., 8, 3337–3353, https://doi.org/10.5194/amt-8-3337-2015, https://doi.org/10.5194/amt-8-3337-2015, 2015
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This paper depicts several fields of application of a new analytical method, which expands the well-established EC/OC method, which enables one to measure the carbon content (organic and elemental) of particulate aerosols. It was coupled to photo-ionization mass spectrometry to get structural information of the evolving carbonaceous species. Application fields such as smoke chamber-, ambient - and wood combustion particles were addressed, covering exemplary primary and secondary aerosol sources.
J. Meyer, C. Rolf, C. Schiller, S. Rohs, N. Spelten, A. Afchine, M. Zöger, N. Sitnikov, T. D. Thornberry, A. W. Rollins, Z. Bozóki, D. Tátrai, V. Ebert, B. Kühnreich, P. Mackrodt, O. Möhler, H. Saathoff, K. H. Rosenlof, and M. Krämer
Atmos. Chem. Phys., 15, 8521–8538, https://doi.org/10.5194/acp-15-8521-2015, https://doi.org/10.5194/acp-15-8521-2015, 2015
I. Steinke, C. Hoose, O. Möhler, P. Connolly, and T. Leisner
Atmos. Chem. Phys., 15, 3703–3717, https://doi.org/10.5194/acp-15-3703-2015, https://doi.org/10.5194/acp-15-3703-2015, 2015
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Ice nucleation in clouds has a significant influence on the global radiative budget and the hydrological cycle. Several studies have investigated the ice formation in droplets and parameterizations have been developed in order to include immersion freezing in climate models. In contrast, there are fewer studies regarding the conversion of water vapor into ice (so-called deposition nucleation) which is the topic of this paper which investigates deposition nucleation by Arizona Test dust in detail
N. Hiranuma, S. Augustin-Bauditz, H. Bingemer, C. Budke, J. Curtius, A. Danielczok, K. Diehl, K. Dreischmeier, M. Ebert, F. Frank, N. Hoffmann, K. Kandler, A. Kiselev, T. Koop, T. Leisner, O. Möhler, B. Nillius, A. Peckhaus, D. Rose, S. Weinbruch, H. Wex, Y. Boose, P. J. DeMott, J. D. Hader, T. C. J. Hill, Z. A. Kanji, G. Kulkarni, E. J. T. Levin, C. S. McCluskey, M. Murakami, B. J. Murray, D. Niedermeier, M. D. Petters, D. O'Sullivan, A. Saito, G. P. Schill, T. Tajiri, M. A. Tolbert, A. Welti, T. F. Whale, T. P. Wright, and K. Yamashita
Atmos. Chem. Phys., 15, 2489–2518, https://doi.org/10.5194/acp-15-2489-2015, https://doi.org/10.5194/acp-15-2489-2015, 2015
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Seventeen ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of illite NX. All data showed a similar temperature trend, but the measured ice nucleation activity was on average smaller for the wet suspended samples and higher for the dry-dispersed aerosol samples at high temperatures. A continued investigation and collaboration is necessary to obtain further insights into consistency or diversity of ice nucleation measurements.
N. Hiranuma, M. Paukert, I. Steinke, K. Zhang, G. Kulkarni, C. Hoose, M. Schnaiter, H. Saathoff, and O. Möhler
Atmos. Chem. Phys., 14, 13145–13158, https://doi.org/10.5194/acp-14-13145-2014, https://doi.org/10.5194/acp-14-13145-2014, 2014
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A new heterogeneous ice nucleation parameterization is developed and implemented in cloud models. The results of our simulations suggest stronger influence of dust particles lifted to the upper troposphere on heterogeneous nucleation and more ice nucleation at temperature and humidity conditions relevant to both mixed-phase and cirrus clouds when compared to the existing parametrical frameworks.
D. W. Fahey, R.-S. Gao, O. Möhler, H. Saathoff, C. Schiller, V. Ebert, M. Krämer, T. Peter, N. Amarouche, L. M. Avallone, R. Bauer, Z. Bozóki, L. E. Christensen, S. M. Davis, G. Durry, C. Dyroff, R. L. Herman, S. Hunsmann, S. M. Khaykin, P. Mackrodt, J. Meyer, J. B. Smith, N. Spelten, R. F. Troy, H. Vömel, S. Wagner, and F. G. Wienhold
Atmos. Meas. Tech., 7, 3177–3213, https://doi.org/10.5194/amt-7-3177-2014, https://doi.org/10.5194/amt-7-3177-2014, 2014
N. Hoffmann, A. Kiselev, D. Rzesanke, D. Duft, and T. Leisner
Atmos. Meas. Tech., 6, 2373–2382, https://doi.org/10.5194/amt-6-2373-2013, https://doi.org/10.5194/amt-6-2373-2013, 2013
H. Saathoff, S. Henin, K. Stelmaszczyk, M. Petrarca, R. Delagrange, Z. Hao, J. Lüder, O. Möhler, Y. Petit, P. Rohwetter, M. Schnaiter, J. Kasparian, T. Leisner, J.-P. Wolf, and L. Wöste
Atmos. Chem. Phys., 13, 4593–4604, https://doi.org/10.5194/acp-13-4593-2013, https://doi.org/10.5194/acp-13-4593-2013, 2013
J. Skrotzki, P. Connolly, M. Schnaiter, H. Saathoff, O. Möhler, R. Wagner, M. Niemand, V. Ebert, and T. Leisner
Atmos. Chem. Phys., 13, 4451–4466, https://doi.org/10.5194/acp-13-4451-2013, https://doi.org/10.5194/acp-13-4451-2013, 2013
M. Laborde, M. Schnaiter, C. Linke, H. Saathoff, K.-H. Naumann, O. Möhler, S. Berlenz, U. Wagner, J. W. Taylor, D. Liu, M. Flynn, J. D. Allan, H. Coe, K. Heimerl, F. Dahlkötter, B. Weinzierl, A. G. Wollny, M. Zanatta, J. Cozic, P. Laj, R. Hitzenberger, J. P. Schwarz, and M. Gysel
Atmos. Meas. Tech., 5, 3077–3097, https://doi.org/10.5194/amt-5-3077-2012, https://doi.org/10.5194/amt-5-3077-2012, 2012
Related subject area
Subject: Aerosols | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Heterogeneous phototransformation of halogenated polycyclic aromatic hydrocarbons: influencing factors, mechanisms and products
Boosting aerosol surface effects: strongly enhanced cooperative surface propensity of atmospherically relevant organic molecular ions in aqueous solution
The lifetimes and potential change in planetary albedo owing to the oxidation of thin surfactant organic films extracted from atmospheric aerosol by hydroxyl (OH) radicals at the air–water interface of particles
Exometabolomic exploration of culturable airborne microorganisms from an urban atmosphere
Measurement Report: Changes in ammonia emissions since the 18th century in south-eastern Europe inferred from an Elbrus (Caucasus, Russia) ice-core record
Atmospheric oxidation of 1,3-butadiene: influence of seed aerosol acidity and relative humidity on SOA composition and the production of air toxic compounds
Enhanced sulfate formation in mixed biomass burning and sea-salt interactions mediated by photosensitization: effects of chloride, nitrogen-containing compounds, and atmospheric aging
Heterogeneous formation and light absorption of secondary organic aerosols from acetone photochemical reactions: remarkably enhancing effects of seeds and ammonia
Secondary Organic Aerosol Formation from Nitrate Radical Oxidation of Styrene: Aerosol Yields, Chemical Composition, and Hydrolysis of Organic Nitrates
Experimental observation of the impact of nanostructure on hygroscopicity and reactivity of fatty acid atmospheric aerosol proxies
Technical note: High-resolution analyses of concentrations and sizes of refractory black carbon particles deposited in northwestern Greenland over the past 350 years – Part 1: Continuous flow analysis of the SIGMA-D ice core using the wide-range Single-Particle Soot Photometer and a high-efficiency nebulizer
The role of surface-active macromolecules in the ice nucleating ability of lignin, Snomax, and agricultural soil extracts
HOMs and SOA formation from the oxidation of α- and β-phellandrenes by NO3 radicals
Particulate emissions from cooking: emission factors, emission dynamics, and mass spectrometric analysis for different cooking methods
Hydrogen Peroxide Photoformation in Particulate Matter and its Contribution to S(IV) Oxidation During Winter in Fairbanks, Alaska
Nocturnal atmospheric synergistic oxidation reduces the formation of low-volatility organic compounds from biogenic emissions
The interplay between aqueous replacement reaction and the phase state of internally mixed organic/ammonium aerosols
Measurement report: The Fifth International Workshop on Ice Nucleation phase 1 (FIN-01): intercomparison of single-particle mass spectrometers
The importance of burning conditions on the composition of domestic biomass burning organic aerosol and the impact of atmospheric aging
Characterization of the particle size distribution, mineralogy, and Fe mode of occurrence of dust-emitting sediments from the Mojave Desert, California, USA
Measurement report: Effects of transition metal ions on the optical properties of humic-like substances (HULIS) reveal a structural preference – a case study of PM2.5 in Beijing, China
Probing Iceland's dust-emitting sediments: particle size distribution, mineralogy, cohesion, Fe mode of occurrence, and reflectance spectra signatures
Photoenhanced sulfate formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
Comparison of water-soluble and water-insoluble organic compositions attributing to different light absorption efficiency between residential coal and biomass burning emissions
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Formation and loss of light absorbance by phenolic aqueous SOA by ●OH and an organic triplet excited state
Technical Note: A technique to convert NO2 to NO2− with S(IV) and its application to measuring nitrate photolysis
Distribution, chemical, and molecular composition of high and low molecular weight humic-like substances in ambient aerosols
Desorption lifetimes and activation energies influencing gas–surface interactions and multiphase chemical kinetics
Secondary organic aerosol formed by Euro 5 gasoline vehicle emissions: chemical composition and gas-to-particle phase partitioning
Assessment of the contribution of residential waste burning to ambient PM10 concentrations in Hungary and Romania
Source differences in the components and cytotoxicity of PM2.5 from automobile exhaust, coal combustion, and biomass burning contributing to urban aerosol toxicity
Chamber studies of OH + dimethyl sulfoxide and dimethyl disulfide: insights into the dimethyl sulfide oxidation mechanism
Low-temperature ice nucleation of sea spray and secondary marine aerosols under cirrus cloud conditions
Temperature-dependent aqueous OH kinetics of C2–C10 linear and terpenoid alcohols and diols: new rate coefficients, structure–activity relationship, and atmospheric lifetimes
A possible unaccounted source of nitrogen-containing compound formation in aerosols: amines reacting with secondary ozonides
Seasonal variations in photooxidant formation and light absorption in aqueous extracts of ambient particles
Variability in sediment particle size, mineralogy, and Fe mode of occurrence across dust-source inland drainage basins: the case of the lower Drâa Valley, Morocco
Gas–particle partitioning of toluene oxidation products: an experimental and modeling study
Chemically speciated air pollutant emissions from open burning of household solid waste from South Africa
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Volatile oxidation products and secondary organosiloxane aerosol from D5 + OH at varying OH exposures
Molecular fingerprints and health risks of smoke from home-use incense burning
High enrichment of heavy metals in fine particulate matter through dust aerosol generation
Production of ice-nucleating particles (INPs) by fast-growing phytoplankton
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)
Contrasting impacts of humidity on the ozonolysis of monoterpenes: insights into the multi-generation chemical mechanism
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
Yueyao Yang, Yahui Liu, Guohua Zhu, Bingcheng Lin, Shanshan Zhang, Xin Li, Fangxi Xu, He Niu, Rong Jin, and Minghui Zheng
Atmos. Chem. Phys., 25, 3981–3994, https://doi.org/10.5194/acp-25-3981-2025, https://doi.org/10.5194/acp-25-3981-2025, 2025
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Halogenated polycyclic aromatic hydrocarbons (XPAHs) are emerging pollutants. Stability during atmospheric transformation processes is crucial for predicting their environmental fate and assessing the associated risks. Here, we conducted field studies and laboratory simulation experiments to reveal the mechanisms, influencing factors and products for XPAHs' heterogeneous phototransformation. Results revealed that the conversion of XPAHs led to a reduction in environmental risk.
Harmanjot Kaur, Stephan Thürmer, Shirin Gholami, Bruno Credidio, Florian Trinter, Debora Vasconcelos, Ricardo Marinho, Joel Pinheiro, Hendrik Bluhm, Arnaldo Naves de Brito, Gunnar Öhrwall, Bernd Winter, and Olle Björneholm
Atmos. Chem. Phys., 25, 3503–3518, https://doi.org/10.5194/acp-25-3503-2025, https://doi.org/10.5194/acp-25-3503-2025, 2025
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Understanding the surface composition of aerosols is crucial for advancing climate models. We investigated the interface of single-component and mixed aqueous solutions of atmospherically relevant carboxylic acid and alkyl-ammonium ions using liquid-jet photoelectron spectroscopy. An exponential increase in surface propensity as a function of chain length was found for the single species, and cooperative effects in the mixtures cause a further drastic increase in surface solute concentration.
Rosalie H. Shepherd, Martin D. King, Andrew D. Ward, Edward J. Stuckey, Rebecca J. L. Welbourn, Neil Brough, Adam Milsom, Christian Pfrang, and Thomas Arnold
Atmos. Chem. Phys., 25, 2569–2588, https://doi.org/10.5194/acp-25-2569-2025, https://doi.org/10.5194/acp-25-2569-2025, 2025
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Thin film formation at the air–water interface from material extracted from atmospheric aerosol was demonstrated, supporting the core–shell morphology. Film thicknesses were approximately 10 Å and 17 Å for urban and remote extracts, respectively. Exposure to gas-phase OH radicals showed fast reactions and short lifetimes of around 1 h. The effect on the Earth's radiative balance indicated that removing half of the film could significantly increase the top-of-atmosphere albedo for urban films.
Rui Jin, Wei Hu, Peimin Duan, Ming Sheng, Dandan Liu, Ziye Huang, Mutong Niu, Libin Wu, Junjun Deng, and Pingqing Fu
Atmos. Chem. Phys., 25, 1805–1829, https://doi.org/10.5194/acp-25-1805-2025, https://doi.org/10.5194/acp-25-1805-2025, 2025
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The metabolic capacity of atmospheric microorganisms after settling into habitats is poorly understood. We studied the molecular composition of exometabolites for cultured typical airborne microbes and traced their metabolic processes. Bacteria and fungi produce highly oxidized exometabolites and have significant variations in metabolism among different strains. These insights are pivotal for assessing the biogeochemical impacts of atmospheric microorganisms following their deposition.
Michel Legrand, Mstislav Vorobyev, Daria Bokuchava, Stanislav Kutuzov, Andreas Plach, Andreas Stohl, Alexandra Khairedinova, Vladimir Mikhalenko, Maria Vinogradova, Sabine Eckhardt, and Susanne Preunkert
Atmos. Chem. Phys., 25, 1385–1399, https://doi.org/10.5194/acp-25-1385-2025, https://doi.org/10.5194/acp-25-1385-2025, 2025
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Past atmospheric NH3 pollution in south-eastern Europe was reconstructed by analysing ammonium in an ice core drilled at the Mount Elbrus (Caucasus, Russia). The observed 3.5-fold increase in ice concentrations between 1750 and 1990 CE is in good agreement with estimated past dominant ammonia emissions from agriculture, mainly from south European Russia and Türkiye. In contrast to present-day conditions, the ammonium level observed in 1750 CE indicates significant natural emissions at that time.
Mohammed Jaoui, Klara Nestorowicz, Krzysztof J. Rudzinski, Michael Lewandowski, Tadeusz E. Kleindienst, Julio Torres, Ewa Bulska, Witold Danikiewicz, and Rafal Szmigielski
Atmos. Chem. Phys., 25, 1401–1432, https://doi.org/10.5194/acp-25-1401-2025, https://doi.org/10.5194/acp-25-1401-2025, 2025
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Recent research has established the contribution of 1,3-butadiene (13BD) to organic aerosol formation with negative implications for urban air quality. Health effect studies have focused on whole particulate matter, but compounds responsible for adverse health effects remain uncertain. This study provides the effect of relative humidity and seed aerosol acidity on the chemical composition of aerosol formed from 13BD photooxidation.
Rongzhi Tang, Jialiang Ma, Ruifeng Zhang, Weizhen Cui, Yuanyuan Qin, Yangxi Chu, Yiming Qin, Alexander L. Vogel, and Chak K. Chan
Atmos. Chem. Phys., 25, 425–439, https://doi.org/10.5194/acp-25-425-2025, https://doi.org/10.5194/acp-25-425-2025, 2025
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This study provides laboratory evidence that the photosensitizers in biomass burning extracts can enhance sulfate formation in NaCl particles, primarily by triggering the formation of secondary oxidants under light and air conditions, with a lower contribution of direct photosensitization via triplets.
Si Zhang, Yining Gao, Xinbei Xu, Luyao Chen, Can Wu, Zheng Li, Rongjie Li, Binyu Xiao, Xiaodi Liu, Rui Li, Fan Zhang, and Gehui Wang
Atmos. Chem. Phys., 24, 14177–14190, https://doi.org/10.5194/acp-24-14177-2024, https://doi.org/10.5194/acp-24-14177-2024, 2024
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Secondary organic aerosols (SOAs) from acetone photooxidation in the presence of various seeds were studied to illustrate SOA formation kinetics under ammonia-rich conditions. The oxidation mechanism of acetone was investigated using an observation-based model incorporating a Master Chemical Mechanism model. A higher SOA yield of acetone was observed compared to methylglyoxal due to an enhanced uptake of the small photooxidation products of acetone.
Yuchen Wang, Xiang Zhang, Yuanlong Huang, Yutong Liang, and Nga L. Ng
EGUsphere, https://doi.org/10.5194/egusphere-2024-3849, https://doi.org/10.5194/egusphere-2024-3849, 2024
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This work provides the first fundamental laboratory data to evaluate SOA production from styrene+NO3 chemistry. Additionally, the formation mechanisms of aromatic ONs are reported for the first time, highlighting that previously identified nitroaromatics in ambient field campaigns can be aromatic ONs. Finally, the hydrolysis lifetime observed for ONs generated from styrene+NO3 oxidation can serve as experimentally constrained parameter for modeling hydrolysis of aromatic ONs in general.
Adam Milsom, Adam M. Squires, Ben Laurence, Ben Wōden, Andrew J. Smith, Andrew D. Ward, and Christian Pfrang
Atmos. Chem. Phys., 24, 13571–13586, https://doi.org/10.5194/acp-24-13571-2024, https://doi.org/10.5194/acp-24-13571-2024, 2024
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We followed nano-structural changes in mixtures found in urban organic aerosol emissions (oleic acid, sodium oleate and fructose) during humidity change and ozone exposure. We demonstrate that self-assembly of fatty acid nanostructures can impact water uptake and chemical reactivity, affecting atmospheric lifetimes, urban air quality (preventing harmful emissions from degradation and enabling their long-range transport) and climate (affecting cloud formation), with implications for human health.
Kumiko Goto-Azuma, Remi Dallmayr, Yoshimi Ogawa-Tsukagawa, Nobuhiro Moteki, Tatsuhiro Mori, Sho Ohata, Yutaka Kondo, Makoto Koike, Motohiro Hirabayashi, Jun Ogata, Kyotaro Kitamura, Kenji Kawamura, Koji Fujita, Sumito Matoba, Naoko Nagatsuka, Akane Tsushima, Kaori Fukuda, and Teruo Aoki
Atmos. Chem. Phys., 24, 12985–13000, https://doi.org/10.5194/acp-24-12985-2024, https://doi.org/10.5194/acp-24-12985-2024, 2024
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We developed a continuous flow analysis system to analyze an ice core from northwestern Greenland and coupled it with an improved refractory black carbon (rBC) measurement technique. This allowed accurate high-resolution analyses of size distributions and concentrations of rBC particles with diameters of 70 nm–4 μm for the past 350 years. Our results provide crucial insights into rBC's climatic effects. We also found previous ice core studies substantially underestimated rBC mass concentrations.
Kathleen A. Thompson, Paul Bieber, Anna J. Miller, Nicole Link, Benjamin J. Murray, and Nadine Borduas-Dedekind
EGUsphere, https://doi.org/10.5194/egusphere-2024-2827, https://doi.org/10.5194/egusphere-2024-2827, 2024
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Lignin and Snomax are surface-active macromolecules that show a relationship between increasing concentrations, decreasing surface tension, and increasing ice-nucleating ability. However, this relationship did not hold for agricultural soil extracts collected in the UK and Canada. Hydrophobic interfaces play an important role in the ice-nucleating activity of organic matter; as the complexity of the sample increases, the hydrophobic interfaces in the bulk compete with the air-water interface.
Sergio Harb, Manuela Cirtog, Stéphanie Alage, Christopher Cantrell, Mathieu Cazaunau, Vincent Michoud, Edouard Pangui, Antonin Bergé, Chiara Giorio, Francesco Battaglia, and Bénédicte Picquet-Varrault
EGUsphere, https://doi.org/10.5194/egusphere-2024-3419, https://doi.org/10.5194/egusphere-2024-3419, 2024
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We investigated the reactions of α- and β-phellandrenes (from vegetation emissions) with NO3 radicals, a major nighttime oxidant from human activities. Using lab-based simulations, we examined these reactions and measured particle formation and by-products. Our findings reveal that α- and β-phellandrenes are efficient particle sources and enhance our understanding of biogenic-anthropogenic interactions and their contributions to atmospheric changes affecting climate and health.
Julia Pikmann, Frank Drewnick, Friederike Fachinger, and Stephan Borrmann
Atmos. Chem. Phys., 24, 12295–12321, https://doi.org/10.5194/acp-24-12295-2024, https://doi.org/10.5194/acp-24-12295-2024, 2024
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Cooking activities can contribute substantially to indoor and ambient aerosol. We performed a comprehensive study with laboratory measurements cooking 19 different dishes and ambient measurements at two Christmas markets measuring various particle properties and trace gases of emissions in real time. Similar emission characteristics were observed for dishes with the same preparation method, mainly due to similar cooking temperature and use of oil, with barbecuing as an especially strong source.
Michael Oluwatoyin Sunday, Laura Marie Dahler Heinlein, Junwei He, Allison Moon, Sukriti Kapur, Ting Fang, Kasey C. Edwards, Fangzhou Guo, Jack Dibb, James H. Flynn III, Becky Alexander, Manabu Shiraiwa, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2024-3272, https://doi.org/10.5194/egusphere-2024-3272, 2024
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Hydrogen peroxide (HOOH) is an important oxidant that forms atmospheric sulfate. We demonstrate that illumination of brown carbon can rapidly form HOOH within particles, even under the low sunlight conditions of Fairbanks, Alaska during winter. This in-particle formation of HOOH is fast enough that it forms sulfate at significant rates. In contrast, the formation of HOOH in the gas phase during the campaign is expected to be negligible because of high NOx levels.
Han Zang, Zekun Luo, Chenxi Li, Ziyue Li, Dandan Huang, and Yue Zhao
Atmos. Chem. Phys., 24, 11701–11716, https://doi.org/10.5194/acp-24-11701-2024, https://doi.org/10.5194/acp-24-11701-2024, 2024
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Atmospheric organics are subject to synergistic oxidation by different oxidants, yet the mechanisms of such processes are poorly understood. Here, using direct measurements and kinetic modeling, we probe the nocturnal synergistic-oxidation mechanism of α-pinene by O3 and NO3 radicals and in particular the fate of peroxy radical intermediates of different origins, which will deepen our understanding of the monoterpene oxidation chemistry and its contribution to atmospheric particle formation.
Hui Yang, Fengfeng Dong, Li Xia, Qishen Huang, Shufeng Pang, and Yunhong Zhang
Atmos. Chem. Phys., 24, 11619–11635, https://doi.org/10.5194/acp-24-11619-2024, https://doi.org/10.5194/acp-24-11619-2024, 2024
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Atmospheric secondary aerosols, composed of organic and inorganic components, undergo complex reactions that impact their phase state. Using molecular spectroscopy, we showed that ammonium-promoted aqueous replacement reaction, unique to these aerosols, is closely linked to phase behavior. The interplay between reactions and aerosol phase state can cause atypical phase transition and irreversible changes in aerosol composition during hygroscopic cycles, further impacting atmospheric processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Chem. Phys., 24, 10869–10891, https://doi.org/10.5194/acp-24-10869-2024, https://doi.org/10.5194/acp-24-10869-2024, 2024
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Rhianna Louise Evans, Daniel Jack Bryant, Aristeidis Voliotis, Dawei Hu, Huihui Wu, Sara Aisyah Syafira, Osayomwanbor Ebenezer Oghama, Gordon McFiggans, Jacqueline Fiona Hamilton, and Andrew Robert Rickard
EGUsphere, https://doi.org/10.5194/egusphere-2024-2642, https://doi.org/10.5194/egusphere-2024-2642, 2024
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The chemical composition of organic aerosol derived from wood burning emissions under different burning conditions was characterised. Fresh emissions from flaming and smouldering were largely aromatic in nature whereas upon aging the aromatic content decreased. This decrease was greater for smouldering due to the loss of toxic polyaromatic species. Whereas under flaming conditions highly toxic polyaromatic species were produced. These differences present an important challenge for policy.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Melani Hernández-Chiriboga, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert Green, Paul Ginoux, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 9155–9176, https://doi.org/10.5194/acp-24-9155-2024, https://doi.org/10.5194/acp-24-9155-2024, 2024
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In this research, we studied the dust-emitting properties of crusts and aeolian ripples from the Mojave Desert. These properties are key to understanding the effect of dust upon climate. We found two different playa lakes according to the groundwater regime, which implies differences in crusts' cohesion state and mineralogy, which can affect the dust emission potential and properties. We also compare them with Moroccan Sahara crusts and Icelandic top sediments.
Juanjuan Qin, Leiming Zhang, Yuanyuan Qin, Shaoxuan Shi, Jingnan Li, Zhao Shu, Yuwei Gao, Ting Qi, Jihua Tan, and Xinming Wang
Atmos. Chem. Phys., 24, 7575–7589, https://doi.org/10.5194/acp-24-7575-2024, https://doi.org/10.5194/acp-24-7575-2024, 2024
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The present research unveiled that acidity dominates while transition metal ions harmonize with the light absorption properties of humic-like substances (HULIS). Cu2+ has quenching effects on HULIS by complexation, hydrogen substitution, or electrostatic adsorption, with aromatic structures of HULIS. Such effects are less pronounced if from Mn2+, Ni2+, Zn2+, and Cu2+. Oxidized HULIS might contain electron-donating groups, whereas N-containing compounds might contain electron-withdrawing groups.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Patricia Córdoba, Andres Alastuey, Natalia Moreno, Konrad Kandler, Martina Klose, Roger N. Clark, Bethany L. Ehlmann, Rebecca N. Greenberger, Abigail M. Keebler, Phil Brodrick, Robert O. Green, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 24, 6883–6910, https://doi.org/10.5194/acp-24-6883-2024, https://doi.org/10.5194/acp-24-6883-2024, 2024
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The knowledge of properties from dust emitted in high latitudes such as in Iceland is scarce. This study focuses on the particle size, mineralogy, cohesion, and iron mode of occurrence and reflectance spectra of dust-emitting sediments. Icelandic top sediments have lower cohesion state, coarser particle size, distinctive mineralogy, and 3-fold bulk Fe content, with a large presence of magnetite compared to Saharan crusts.
Wangjin Yang, Jiawei Ma, Hongxing Yang, Fu Li, and Chong Han
Atmos. Chem. Phys., 24, 6757–6768, https://doi.org/10.5194/acp-24-6757-2024, https://doi.org/10.5194/acp-24-6757-2024, 2024
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We provide evidence that light enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where triplet states of SO2 (3SO2) can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. The SO2 photochemistry on non-photoactive mineral dust contributes to sulfates, highlighting previously unknown pathways to better explain the missing sources of atmospheric sulfates.
Lu Zhang, Jin Li, Yaojie Li, Xinlei Liu, Zhihan Luo, Guofeng Shen, and Shu Tao
Atmos. Chem. Phys., 24, 6323–6337, https://doi.org/10.5194/acp-24-6323-2024, https://doi.org/10.5194/acp-24-6323-2024, 2024
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Brown carbon (BrC) is related to radiative forcing and climate change. The BrC fraction from residential coal and biomass burning emissions, which were the major source of BrC, was characterized at the molecular level. The CHOS aromatic compounds explained higher light absorption efficiencies of biomass burning emissions compared to coal. The unique formulas of coal combustion aerosols were characterized by higher unsaturated compounds, and such information could be used for source appointment.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
Atmos. Chem. Phys., 24, 5625–5636, https://doi.org/10.5194/acp-24-5625-2024, https://doi.org/10.5194/acp-24-5625-2024, 2024
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Cooking is a major source of particles in urban areas. Previous studies demonstrated that the chemical lifetimes of cooking organic aerosols (COAs) were much shorter (~minutes) than the values reported by field observations (~hours). We conducted laboratory experiments to resolve the discrepancy by considering suppressed reactivity under low temperature. The parameterized k2–T relationships and observed surface temperature data were used to estimate the chemical lifetimes of COA particles.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
Atmos. Chem. Phys., 24, 4473–4485, https://doi.org/10.5194/acp-24-4473-2024, https://doi.org/10.5194/acp-24-4473-2024, 2024
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We measured changes in light absorption during the aqueous oxidation of six phenols with hydroxyl radical (●OH) or an organic triplet excited state (3C*). All the phenols formed light-absorbing secondary brown carbon (BrC), which then decayed with continued oxidation. Extrapolation to ambient conditions suggest ●OH is the dominant sink of secondary phenolic BrC in fog/cloud drops, while 3C* controls the lifetime of this light absorption in particle water.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
Atmos. Chem. Phys., 24, 4411–4419, https://doi.org/10.5194/acp-24-4411-2024, https://doi.org/10.5194/acp-24-4411-2024, 2024
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We developed a method that uses aqueous S(IV) to quantitatively convert NO2 to NO2−, which allows both species to be quantified using the Griess method. As an example of the utility of the method, we quantified both photolysis channels of nitrate, with and without a scavenger for hydroxyl radical (·OH). The results show that without a scavenger, ·OH reacts with nitrite to form nitrogen dioxide, suppressing the apparent quantum yield of NO2− and enhancing that of NO2.
Xingjun Fan, Ao Cheng, Xufang Yu, Tao Cao, Dan Chen, Wenchao Ji, Yongbing Cai, Fande Meng, Jianzhong Song, and Ping'an Peng
Atmos. Chem. Phys., 24, 3769–3783, https://doi.org/10.5194/acp-24-3769-2024, https://doi.org/10.5194/acp-24-3769-2024, 2024
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Molecular-level characteristics of high molecular weight (HMW) and low MW (LMW) humic-like substances (HULIS) were comprehensively investigated, where HMW HULIS had larger chromophores and larger molecular size than LMW HULIS and exhibited higher aromaticity and humification. Electrospray ionization high-resolution mass spectrometry revealed more aromatic molecules in HMW HULIS. HMW HULIS had more CHON compounds, while LMW HULIS had more CHO compounds.
Daniel A. Knopf, Markus Ammann, Thomas Berkemeier, Ulrich Pöschl, and Manabu Shiraiwa
Atmos. Chem. Phys., 24, 3445–3528, https://doi.org/10.5194/acp-24-3445-2024, https://doi.org/10.5194/acp-24-3445-2024, 2024
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The initial step of interfacial and multiphase chemical processes involves adsorption and desorption of gas species. This study demonstrates the role of desorption energy governing the residence time of the gas species at the environmental interface. A parameterization is formulated that enables the prediction of desorption energy based on the molecular weight, polarizability, and oxygen-to-carbon ratio of the desorbing chemical species. Its application to gas–particle interactions is discussed.
Evangelia Kostenidou, Baptiste Marques, Brice Temime-Roussel, Yao Liu, Boris Vansevenant, Karine Sartelet, and Barbara D'Anna
Atmos. Chem. Phys., 24, 2705–2729, https://doi.org/10.5194/acp-24-2705-2024, https://doi.org/10.5194/acp-24-2705-2024, 2024
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Secondary organic aerosol (SOA) from gasoline vehicles can be a significant source of particulate matter in urban areas. Here the chemical composition of secondary volatile organic compounds and SOA produced by photo-oxidation of Euro 5 gasoline vehicle emissions was studied. The volatility of the SOA formed was calculated. Except for the temperature and the concentration of the aerosol, additional parameters may play a role in the gas-to-particle partitioning.
András Hoffer, Aida Meiramova, Ádám Tóth, Beatrix Jancsek-Turóczi, Gyula Kiss, Ágnes Rostási, Erika Andrea Levei, Luminita Marmureanu, Attila Machon, and András Gelencsér
Atmos. Chem. Phys., 24, 1659–1671, https://doi.org/10.5194/acp-24-1659-2024, https://doi.org/10.5194/acp-24-1659-2024, 2024
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Specific tracer compounds identified previously in controlled test burnings of different waste types in the laboratory were detected and quantified in ambient PM10 samples collected in five Hungarian and four Romanian settlements. Back-of-the-envelope calculations based on the relative emission factors of individual tracers suggested that the contribution of solid waste burning particulate emissions to ambient PM10 mass concentrations may be as high as a few percent.
Xiao-San Luo, Weijie Huang, Guofeng Shen, Yuting Pang, Mingwei Tang, Weijun Li, Zhen Zhao, Hanhan Li, Yaqian Wei, Longjiao Xie, and Tariq Mehmood
Atmos. Chem. Phys., 24, 1345–1360, https://doi.org/10.5194/acp-24-1345-2024, https://doi.org/10.5194/acp-24-1345-2024, 2024
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PM2.5 are air pollutants threatening health globally, but they are a mixture of chemical compositions from many sources and result in unequal toxicity. Which composition from which source of PM2.5 as the most hazardous object is a question hindering effective pollution control policy-making. With chemical and toxicity experiments, we found automobile exhaust and coal combustion to be priority emissions with higher toxic compositions for precise air pollution control, ensuring public health.
Matthew B. Goss and Jesse H. Kroll
Atmos. Chem. Phys., 24, 1299–1314, https://doi.org/10.5194/acp-24-1299-2024, https://doi.org/10.5194/acp-24-1299-2024, 2024
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The chemistry driving dimethyl sulfide (DMS) oxidation and subsequent sulfate particle formation in the atmosphere is poorly constrained. We oxidized two related compounds (dimethyl sulfoxide and dimethyl disulfide) in the laboratory under varied NOx conditions and measured the gas- and particle-phase products. These results demonstrate that both the OH addition and OH abstraction pathways for DMS oxidation contribute to particle formation via mechanisms that do not involve the SO2 intermediate.
Ryan J. Patnaude, Kathryn A. Moore, Russell J. Perkins, Thomas C. J. Hill, Paul J. DeMott, and Sonia M. Kreidenweis
Atmos. Chem. Phys., 24, 911–928, https://doi.org/10.5194/acp-24-911-2024, https://doi.org/10.5194/acp-24-911-2024, 2024
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In this study we examined the effect of atmospheric aging on sea spray aerosols (SSAs) to form ice and how newly formed secondary marine aerosols (SMAs) may freeze at cirrus temperatures (< −38 °C). Results show that SSAs freeze at different relative humidities (RHs) depending on the temperature and that the ice-nucleating ability of SSA was not hindered by atmospheric aging. SMAs are shown to freeze at high RHs and are likely inefficient at forming ice at cirrus temperatures.
Bartłomiej Witkowski, Priyanka Jain, Beata Wileńska, and Tomasz Gierczak
Atmos. Chem. Phys., 24, 663–688, https://doi.org/10.5194/acp-24-663-2024, https://doi.org/10.5194/acp-24-663-2024, 2024
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This article reports the results of the kinetic measurements for the aqueous oxidation of the 29 aliphatic alcohols by hydroxyl radical (OH) at different temperatures. The data acquired and the literature data were used to optimize a model for predicting the aqueous OH reactivity of alcohols and carboxylic acids and to estimate the atmospheric lifetimes of five terpenoic alcohols. The kinetic data provided new insights into the mechanism of aqueous oxidation of aliphatic molecules by the OH.
Junting Qiu, Xinlin Shen, Jiangyao Chen, Guiying Li, and Taicheng An
Atmos. Chem. Phys., 24, 155–166, https://doi.org/10.5194/acp-24-155-2024, https://doi.org/10.5194/acp-24-155-2024, 2024
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We studied reactions of secondary ozonides (SOZs) with amines. SOZs formed from ozonolysis of β-caryophyllene and α-humulene are found to be reactive to ethylamine and methylamine. Products from SOZs with various conformations reacting with the same amine had different functional groups. Our findings indicate that interaction of SOZs with amines in the atmosphere is very complicated, which is potentially a hitherto unrecognized source of N-containing compound formation.
Lan Ma, Reed Worland, Laura Heinlein, Chrystal Guzman, Wenqing Jiang, Christopher Niedek, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 24, 1–21, https://doi.org/10.5194/acp-24-1-2024, https://doi.org/10.5194/acp-24-1-2024, 2024
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We measured concentrations of three photooxidants – the hydroxyl radical, triplet excited states of organic carbon, and singlet molecular oxygen – in fine particles collected over a year. Concentrations are highest in extracts of fresh biomass burning particles, largely because they have the highest particle concentrations and highest light absorption. When normalized by light absorption, rates of formation for each oxidant are generally similar for the four particle types we observed.
Adolfo González-Romero, Cristina González-Flórez, Agnesh Panta, Jesús Yus-Díez, Cristina Reche, Patricia Córdoba, Natalia Moreno, Andres Alastuey, Konrad Kandler, Martina Klose, Clarissa Baldo, Roger N. Clark, Zongbo Shi, Xavier Querol, and Carlos Pérez García-Pando
Atmos. Chem. Phys., 23, 15815–15834, https://doi.org/10.5194/acp-23-15815-2023, https://doi.org/10.5194/acp-23-15815-2023, 2023
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The effect of dust emitted from desertic surfaces upon climate and ecosystems depends on size and mineralogy, but data from soil mineral atlases of desert soils are scarce. We performed particle-size distribution, mineralogy, and Fe speciation in southern Morocco. Results show coarser particles with high quartz proportion are near the elevated areas, while in depressed areas, sizes are finer, and proportions of clays and nano-Fe oxides are higher. This difference is important for dust modelling.
Victor Lannuque, Barbara D'Anna, Evangelia Kostenidou, Florian Couvidat, Alvaro Martinez-Valiente, Philipp Eichler, Armin Wisthaler, Markus Müller, Brice Temime-Roussel, Richard Valorso, and Karine Sartelet
Atmos. Chem. Phys., 23, 15537–15560, https://doi.org/10.5194/acp-23-15537-2023, https://doi.org/10.5194/acp-23-15537-2023, 2023
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Large uncertainties remain in understanding secondary organic aerosol (SOA) formation from toluene oxidation. In this study, speciation measurements in gaseous and particulate phases were carried out, providing partitioning and volatility data on individual toluene SOA components at different temperatures. A new detailed oxidation mechanism was developed to improve modeled speciation, and effects of different processes involved in gas–particle partitioning at the molecular scale are explored.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Steven Sai Hang Ho, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 15375–15393, https://doi.org/10.5194/acp-23-15375-2023, https://doi.org/10.5194/acp-23-15375-2023, 2023
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Open burning of municipal solid waste emits chemicals that are harmful to the environment. This paper reports source profiles and emission factors for PM2.5 species and acidic/alkali gases from laboratory combustion of 10 waste categories (including plastics and biomass) that represent open burning in South Africa. Results will be useful for health and climate impact assessments, speciated emission inventories, source-oriented dispersion models, and receptor-based source apportionment.
Jun Zhang, Kun Li, Tiantian Wang, Erlend Gammelsæter, Rico K. Y. Cheung, Mihnea Surdu, Sophie Bogler, Deepika Bhattu, Dongyu S. Wang, Tianqu Cui, Lu Qi, Houssni Lamkaddam, Imad El Haddad, Jay G. Slowik, Andre S. H. Prevot, and David M. Bell
Atmos. Chem. Phys., 23, 14561–14576, https://doi.org/10.5194/acp-23-14561-2023, https://doi.org/10.5194/acp-23-14561-2023, 2023
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We conducted burning experiments to simulate various types of solid fuel combustion, including residential burning, wildfires, agricultural burning, cow dung, and plastic bag burning. The chemical composition of the particles was characterized using mass spectrometers, and new potential markers for different fuels were identified using statistical analysis. This work improves our understanding of emissions from solid fuel burning and offers support for refined source apportionment.
Hyun Gu Kang, Yanfang Chen, Yoojin Park, Thomas Berkemeier, and Hwajin Kim
Atmos. Chem. Phys., 23, 14307–14323, https://doi.org/10.5194/acp-23-14307-2023, https://doi.org/10.5194/acp-23-14307-2023, 2023
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D5 is an emerging anthropogenic pollutant that is ubiquitous in indoor and urban environments, and the OH oxidation of D5 forms secondary organosiloxane aerosol (SOSiA). Application of a kinetic box model that uses a volatility basis set (VBS) showed that consideration of oxidative aging (aging-VBS) predicts SOSiA formation much better than using a standard-VBS model. Ageing-dependent parameterization is needed to accurately model SOSiA to assess the implications of siloxanes for air quality.
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, Maosheng Yao, and Song Guo
Atmos. Chem. Phys., 23, 13585–13595, https://doi.org/10.5194/acp-23-13585-2023, https://doi.org/10.5194/acp-23-13585-2023, 2023
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Incense burning is common in Asia, posing 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. Intermediate-volatility volatile organic compounds (IVOCs) are crucial organics accounting for 19.2 % of the total emission factors (EFs) and 40.0 % of the secondary organic aerosol (SOA) estimation, highlighting the importance of incorporating IVOCs into SOA models.
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., 23, 13049–13060, https://doi.org/10.5194/acp-23-13049-2023, https://doi.org/10.5194/acp-23-13049-2023, 2023
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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-dust (PM2.5) aerosols. In addition, estimation of heavy metal emissions from dust generation by air quality models may have errors without using proper dust profiles.
Daniel C. O. Thornton, Sarah D. Brooks, Elise K. Wilbourn, Jessica Mirrielees, Alyssa N. Alsante, Gerardo Gold-Bouchot, Andrew Whitesell, and Kiana McFadden
Atmos. Chem. Phys., 23, 12707–12729, https://doi.org/10.5194/acp-23-12707-2023, https://doi.org/10.5194/acp-23-12707-2023, 2023
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A major uncertainty in our understanding of clouds and climate is the sources and properties of the aerosol on which clouds grow. We found that aerosol containing organic matter from fast-growing marine phytoplankton was 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 that ecosystem processes and the properties of sea spray aerosol are linked.
Adam Milsom, Shaojun Qi, Ashmi Mishra, Thomas Berkemeier, Zhenyu Zhang, and Christian Pfrang
Atmos. Chem. Phys., 23, 10835–10843, https://doi.org/10.5194/acp-23-10835-2023, https://doi.org/10.5194/acp-23-10835-2023, 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.
Shan Zhang, Lin Du, Zhaomin Yang, Narcisse Tsona Tchinda, Jianlong Li, and Kun Li
Atmos. Chem. Phys., 23, 10809–10822, https://doi.org/10.5194/acp-23-10809-2023, https://doi.org/10.5194/acp-23-10809-2023, 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 in aerosol formation and inform ongoing research on particle environmental effects and applications in models.
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.
Cited articles
Andreae, M. O. and Gelencsér, A.: Black carbon or brown carbon? The nature of light-absorbing carbonaceous aerosols, Atmos. Chem. Phys., 6, 3131–3148, https://doi.org/10.5194/acp-6-3131-2006, 2006.
Atkinson, R., Tuazon, E. C., Arey, J., and Aschmann, S. M.: Atmospheric and Indoor Chemistry of Gas-phase Indole, Quinoline, and Isoquinoline, Atmos. Environ., 29, 3423–3432, https://doi.org/10.1016/1352-2310(95)00103-6, 1995.
Baboomian, V. J., He, Q., Montoya-Aguilera, J., Ali, N., Fleming, L. T., Lin, P., Laskin, A., Laskin, J., Rudich, Y., and Nizkorodov, S. A.: Light absorption and scattering properties of indole secondary organic aerosol prepared under various oxidant and relative humidity conditions, Aerosol Sci. Tech., 57, 532–545, https://doi.org/10.1080/02786826.2023.2193235, 2023.
Bloss, C., Wagner, V., Jenkin, M. E., Volkamer, R., Bloss, W. J., Lee, J. D., Heard, D. E., Wirtz, K., Martin-Reviejo, M., Rea, G., Wenger, J. C., and Pilling, M. J.: Development of a detailed chemical mechanism (MCMv3.1) for the atmospheric oxidation of aromatic hydrocarbons, Atmos. Chem. Phys., 5, 641–664, https://doi.org/10.5194/acp-5-641-2005, 2005.
Erb, M., Veyrat, N., Robert, C. A. M., Xu, H., Frey, M., Ton, J., and Turlings, T. C. J.: Indole is an essential herbivore-induced volatile priming signal in maize, Nat. Commun., 6, 6273, https://doi.org/10.1038/ncomms7273, 2015.
Feng, Y., Ramanathan, V., and Kotamarthi, V. R.: Brown carbon: a significant atmospheric absorber of solar radiation?, Atmos. Chem. Phys., 13, 8607–8621, https://doi.org/10.5194/acp-13-8607-2013, 2013.
Gao, L., Song, J., Mohr, C., Huang, W., Vallon, M., Jiang, F., Leisner, T., and Saathoff, H.: Kinetics, SOA yields, and chemical composition of secondary organic aerosol from β-caryophyllene ozonolysis with and without nitrogen oxides between 213 and 313 K, Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, 2022.
Gentner, D. R., Ormeño, E., Fares, S., Ford, T. B., Weber, R., Park, J.-H., Brioude, J., Angevine, W. M., Karlik, J. F., and Goldstein, A. H.: Emissions of terpenoids, benzenoids, and other biogenic gas-phase organic compounds from agricultural crops and their potential implications for air quality, Atmos. Chem. Phys., 14, 5393–5413, https://doi.org/10.5194/acp-14-5393-2014, 2014.
Hallquist, M., Wenger, J. C., Baltensperger, U., Rudich, Y., Simpson, D., Claeys, M., Dommen, J., Donahue, N. M., George, C., Goldstein, A. H., Hamilton, J. F., Herrmann, H., Hoffmann, T., Iinuma, Y., Jang, M., Jenkin, M. E., Jimenez, J. L., Kiendler-Scharr, A., Maenhaut, W., McFiggans, G., Mentel, Th. F., Monod, A., Prévôt, A. S. H., Seinfeld, J. H., Surratt, J. D., Szmigielski, R., and Wildt, J.: The formation, properties and impact of secondary organic aerosol: current and emerging issues, Atmos. Chem. Phys., 9, 5155–5236, https://doi.org/10.5194/acp-9-5155-2009, 2009.
He, Q. F., Li, C. L., Siemens, K., Morales, A. C., Hettiyadura, A. P. S., Laskin, A., and Rudich, Y.: Optical Properties of Secondary Organic Aerosol Produced by Photooxidation of Naphthalene under NOx Condition, Environ. Sci. Technol., 56, 4816–4827, https://doi.org/10.1021/acs.est.1c07328, 2022.
Hecobian, A., Zhang, X., Zheng, M., Frank, N., Edgerton, E. S., and Weber, R. J.: Water-Soluble Organic Aerosol material and the light-absorption characteristics of aqueous extracts measured over the Southeastern United States, Atmos. Chem. Phys., 10, 5965–5977, https://doi.org/10.5194/acp-10-5965-2010, 2010.
Hettiyadura, A. P. S. and Laskin, A.: Quantitative analysis of polycyclic aromatic hydrocarbons using high-performance liquid chromatography-photodiode array-high-resolution mass spectrometric detection platform coupled to electrospray and atmospheric pressure photoionization sources, J. Mass Spectrom., 57, e4804, https://doi.org/10.1002/jms.4804, 2022.
Hettiyadura, A. P. S., Garcia, V., Li, C., West, C. P., Tomlin, J., He, Q., Rudich, Y., and Laskin, A.: Chemical Composition and Molecular-Specific Optical Properties of Atmospheric Brown Carbon Associated with Biomass Burning, Environ. Sci. Technol., 55, 2511–2521, https://doi.org/10.1021/acs.est.0c05883, 2021.
Jiang, F., Song, J., Bauer, J., Gao, L., Vallon, M., Gebhardt, R., Leisner, T., Norra, S., and Saathoff, H.: Chromophores and chemical composition of brown carbon characterized at an urban kerbside by excitation–emission spectroscopy and mass spectrometry, Atmos. Chem. Phys., 22, 14971–14986, https://doi.org/10.5194/acp-22-14971-2022, 2022.
Jiang, F., Siemens, K., Linke, C., Li, Y., Gong, Y., Leisner, T., Laskin, A., and Saathoff, H.: Molecular Analysis of Secondary Organic Aerosol and Brown Carbon from the Oxidation of Indole, Karlsruhe Institute of Technology [data set], https://doi.org/10.35097/1904, 2024.
Jiang, H. H., Frie, A. L., Lavi, A., Chen, J. Y., Zhang, H. F., Bahreini, R., and Lin, Y. H.: Brown Carbon Formation from Nighttime Chemistry of Unsaturated Heterocyclic Volatile Organic Compounds, Environ. Sci. Tech. Let., 6, 184–190, https://doi.org/10.1021/acs.estlett.9b00017, 2019.
Kostenidou, E., Pathak, R. K., and Pandis, S. N.: An algorithm for the calculation of secondary organic aerosol density combining AMS and SMPS data, Aerosol Sci. Tech., 41, 1002–1010, https://doi.org/10.1080/02786820701666270, 2007.
Lambe, A. T., Zhang, J. Y., Sage, A. M., and Donahue, N. M.: Controlled OH radical production via ozone-alkene reactions for use in aerosol aging studies, Environ. Sci. Technol., 41, 2357–2363, https://doi.org/10.1021/es061878e, 2007.
Laskin, A., Smith, J. S., and Laskin, J.: Molecular Characterization of Nitrogen-Containing Organic Compounds in Biomass Burning Aerosols Using High-Resolution Mass Spectrometry, Environ. Sci. Technol., 43, 3764–3771, https://doi.org/10.1021/es803456n, 2009.
Laskin, J., Laskin, A., Nizkorodov, S. A., Roach, P., Eckert, P., Gilles, M. K., Wang, B. B., Lee, H. J., and Hu, Q. C.: Molecular Selectivity of Brown Carbon Chromophores, Environ. Sci. Technol., 48, 12047–12055, https://doi.org/10.1021/es503432r, 2014.
Laskin, A., Laskin, J., and Nizkorodov, S. A.: Chemistry of Atmospheric Brown Carbon, Chem. Rev., 115, 4335–4382, https://doi.org/10.1021/cr5006167, 2015.
Li, C. L., Windwer, E., Fang, Z., Nissenbaum, D., and Rudich, Y.: Correcting micro-aethalometer absorption measurements for brown carbon aerosol, Sci. Total Environ., 777, 146143, https://doi.org/10.1016/j.scitotenv.2021.146143, 2021.
Li, Y. X., Zhao, J. Y., Wang, Y., Seinfeld, J. H., and Zhang, R. Y.: Multigeneration Production of Secondary Organic Aerosol from Toluene Photooxidation, Environ. Sci. Technol., 55, 8592–8603, https://doi.org/10.1021/acs.est.1c02026, 2021.
Lin, P., Liu, J., Shilling, J. E., Kathmann, S. M., Laskin, J., and Laskin, A.: Molecular characterization of brown carbon (BrC) chromophores in secondary organic aerosol generated from photo-oxidation of toluene, Phys. Chem. Chem. Phys., 17, 23312–23325, https://doi.org/10.1039/c5cp02563j, 2015.
Linke, C., Ibrahim, I., Schleicher, N., Hitzenberger, R., Andreae, M. O., Leisner, T., and Schnaiter, M.: A novel single-cavity three-wavelength photoacoustic spectrometer for atmospheric aerosol research, Atmos. Meas. Tech., 9, 5331–5346, https://doi.org/10.5194/amt-9-5331-2016, 2016.
Liu, S., Huang, D., Wang, Y., Zhang, S., Liu, X., Wu, C., Du, W., and Wang, G.: Synergetic effects of NH3 and NOx on the production and optical absorption of secondary organic aerosol formation from toluene photooxidation, Atmos. Chem. Phys., 21, 17759–17773, https://doi.org/10.5194/acp-21-17759-2021, 2021.
Lopez-Hilfiker, F. D., Mohr, C., Ehn, M., Rubach, F., Kleist, E., Wildt, J., Mentel, Th. F., Lutz, A., Hallquist, M., Worsnop, D., and Thornton, J. A.: A novel method for online analysis of gas and particle composition: description and evaluation of a Filter Inlet for Gases and AEROsols (FIGAERO), Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, 2014.
Lopez-Hilfiker, F. D., Iyer, S., Mohr, C., Lee, B. H., D'Ambro, E. L., Kurtén, T., and Thornton, J. A.: Constraining the sensitivity of iodide adduct chemical ionization mass spectrometry to multifunctional organic molecules using the collision limit and thermodynamic stability of iodide ion adducts, Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, 2016.
Mayorga, R., Chen, K., Raeofy, N., Woods, M., Lum, M., Zhao, Z., Zhang, W., Bahreini, R., Lin, Y.-H., and Zhang, H.: Chemical Structure Regulates the Formation of Secondary Organic Aerosol and Brown Carbon in Nitrate Radical Oxidation of Pyrroles and Methylpyrroles, Environ. Sci. Technol., 56, 7761–7770, https://doi.org/10.1021/acs.est.2c02345, 2022.
Misztal, P. K., Hewitt, C. N., Wildt, J., Blande, J. D., Eller, A. S. D., Fares, S., Gentner, D. R., Gilman, J. B., Graus, M., Greenberg, J., Guenther, A. B., Hansel, A., Harley, P., Huang, M., Jardine, K., Karl, T., Kaser, L., Keutsch, F. N., Kiendler-Scharr, A., Kleist, E., Lerner, B. M., Li, T., Mak, J., Nolscher, A. C., Schnitzhofer, R., Sinha, V., Thornton, B., Warneke, C., Wegener, F., Werner, C., Williams, J., Worton, D. R., Yassaa, N., and Goldstein, A. H.: Atmospheric benzenoid emissions from plants rival those from fossil fuels, Sci. Rep., 5, 12064, https://doi.org/10.1038/srep12064, 2015.
Moise, T., Flores, J. M., and Rudich, Y.: Optical Properties of Secondary Organic Aerosols and Their Changes by Chemical Processes, Chem. Rev., 115, 4400–4439, https://doi.org/10.1021/cr5005259, 2015.
Montoya-Aguilera, J., Horne, J. R., Hinks, M. L., Fleming, L. T., Perraud, V., Lin, P., Laskin, A., Laskin, J., Dabdub, D., and Nizkorodov, S. A.: Secondary organic aerosol from atmospheric photooxidation of indole, Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, 2017.
Moschos, V., Kumar, N. K., Daellenbach, K. R., Baltensperger, U., Prevot, A. S. H., and El Haddad, I.: Source Apportionment of Brown Carbon Absorption by Coupling Ultraviolet-Visible Spectroscopy with Aerosol Mass Spectrometry, Environ. Sci. Tech. Let., 5, 302–308, https://doi.org/10.1021/acs.estlett.8b00118, 2018.
Ng, N. L., Kroll, J. H., Chan, A. W. H., Chhabra, P. S., Flagan, R. C., and Seinfeld, J. H.: Secondary organic aerosol formation from m-xylene, toluene, and benzene, Atmos. Chem. Phys., 7, 3909–3922, https://doi.org/10.5194/acp-7-3909-2007, 2007.
Orlando, J. J. and Tyndall, G. S.: Laboratory studies of organic peroxy radical chemistry: an overview with emphasis on recent issues of atmospheric significance, Chem. Soc. Rev., 41, 6294–6317, https://doi.org/10.1039/C2CS35166H, 2012.
Saathoff, H., Naumann, K.-H., Möhler, O., Jonsson, Å. M., Hallquist, M., Kiendler-Scharr, A., Mentel, Th. F., Tillmann, R., and Schurath, U.: Temperature dependence of yields of secondary organic aerosols from the ozonolysis of α-pinene and limonene, Atmos. Chem. Phys., 9, 1551–1577, https://doi.org/10.5194/acp-9-1551-2009, 2009.
Salo, K., Hallquist, M., Jonsson, Å. M., Saathoff, H., Naumann, K.-H., Spindler, C., Tillmann, R., Fuchs, H., Bohn, B., Rubach, F., Mentel, Th. F., Müller, L., Reinnig, M., Hoffmann, T., and Donahue, N. M.: Volatility of secondary organic aerosol during OH radical induced ageing, Atmos. Chem. Phys., 11, 11055–11067, https://doi.org/10.5194/acp-11-11055-2011, 2011.
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Short summary
We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
We investigated the optical properties, chemical composition, and formation mechanisms of...
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