Articles | Volume 20, issue 19
https://doi.org/10.5194/acp-20-11387-2020
© Author(s) 2020. 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-20-11387-2020
© Author(s) 2020. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
06 Oct 2020
Research article |
| 06 Oct 2020
| 06 Oct 2020
Complex plant-derived organic aerosol as ice-nucleating particles – more than the sums of their parts?
Isabelle Steinke
CORRESPONDING AUTHOR
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
now at: Atmospheric Sciences and Global Change Division, Pacific Northwest
National Laboratory, Richland, USA
Naruki Hiranuma
Department of Life, Earth, and Environmental Sciences, West Texas A&M
University, Canyon, Texas, USA
Roger Funk
Working Group Landscape Pedology, Leibniz Centre for Agricultural Landscape
Research (ZALF), Müncheberg, Germany
Kristina Höhler
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
Nadine Tüllmann
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
Nsikanabasi Silas Umo
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
Peter G. Weidler
Institute of Functional Interfaces, Karlsruhe Institute of Technology,
Karlsruhe, Germany
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
Thomas Leisner
Institute of Meteorology and Climate Research – Atmospheric Aerosol
Research (IMK–AAF), Karlsruhe Institute of Technology, Karlsruhe, Germany
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Atmos. Chem. Phys., 22, 847–859, https://doi.org/10.5194/acp-22-847-2022, https://doi.org/10.5194/acp-22-847-2022, 2022
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Manuel Baumgartner, Christian Rolf, Jens-Uwe Grooß, Julia Schneider, Tobias Schorr, Ottmar Möhler, Peter Spichtinger, and Martina Krämer
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An important mechanism for the appearance of ice particles in the upper troposphere at low temperatures is homogeneous nucleation. This process is commonly described by the
Koop line, predicting the humidity at freezing. However, laboratory measurements suggest that the freezing humidities are above the Koop line, motivating the present study to investigate the influence of different physical parameterizations on the homogeneous freezing with the help of a detailed numerical model.
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
Atmos. Chem. Phys., 21, 17099–17114, https://doi.org/10.5194/acp-21-17099-2021, https://doi.org/10.5194/acp-21-17099-2021, 2021
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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.
Matteo Rinaldi, Naruki Hiranuma, Gianni Santachiara, Mauro Mazzola, Karam Mansour, Marco Paglione, Cheyanne A. Rodriguez, Rita Traversi, Silvia Becagli, David Cappelletti, and Franco Belosi
Atmos. Chem. Phys., 21, 14725–14748, https://doi.org/10.5194/acp-21-14725-2021, https://doi.org/10.5194/acp-21-14725-2021, 2021
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This study aims to add to the still scant ice-nucleating particle (INP) observations in the Arctic environment, investigating INP concentrations and potential sources, during spring and summertime, at the ground-level site of GVB. The lack of a clear concentration seasonal trend, in contrast with previous works, shows an important interannual variability of Arctic INP sources, which may be both terrestrial and marine, outside the Arctic haze period.
Haoran Li, Ottmar Möhler, Tuukka Petäjä, and Dmitri Moisseev
Atmos. Chem. Phys., 21, 14671–14686, https://doi.org/10.5194/acp-21-14671-2021, https://doi.org/10.5194/acp-21-14671-2021, 2021
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In natural clouds, ice-nucleating particles are expected to be rare above –10 °C. In the current paper, we found that the formation of ice columns is frequent in stratiform clouds and is associated with increased precipitation intensity and liquid water path. In single-layer shallow clouds, the production of ice columns was attributed to secondary ice production, despite the rime-splintering process not being expected to take place in such clouds.
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.
Robert Wagner, Luisa Ickes, Allan K. Bertram, Nora Els, Elena Gorokhova, Ottmar Möhler, Benjamin J. Murray, Nsikanabasi Silas Umo, and Matthew E. Salter
Atmos. Chem. Phys., 21, 13903–13930, https://doi.org/10.5194/acp-21-13903-2021, https://doi.org/10.5194/acp-21-13903-2021, 2021
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Sea spray aerosol particles are a mixture of inorganic salts and organic matter from phytoplankton organisms. At low temperatures in the upper troposphere, both inorganic and organic constituents can induce the formation of ice crystals and thereby impact cloud properties and climate. In this study, we performed experiments in a cloud simulation chamber with particles produced from Arctic seawater samples to quantify the relative contribution of inorganic and organic species in ice formation.
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).
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.
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.
Matthias Faust, Ralf Wolke, Steffen Münch, Roger Funk, and Kerstin Schepanski
Geosci. Model Dev., 14, 2205–2220, https://doi.org/10.5194/gmd-14-2205-2021, https://doi.org/10.5194/gmd-14-2205-2021, 2021
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Trajectory dispersion models are powerful and intuitive tools for tracing air pollution through the atmosphere. But the turbulent nature of the atmospheric boundary layer makes it challenging to provide accurate predictions near the surface. To overcome this, we propose an approach using wind and turbulence information at high temporal resolution. Finally, we demonstrate the strength of our approach in a case study on dust emissions from agriculture.
Hemanth S. K. Vepuri, Cheyanne A. Rodriguez, Dimitrios G. Georgakopoulos, Dustin Hume, James Webb, Gregory D. Mayer, and Naruki Hiranuma
Atmos. Chem. Phys., 21, 4503–4520, https://doi.org/10.5194/acp-21-4503-2021, https://doi.org/10.5194/acp-21-4503-2021, 2021
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Due to a high frequency of storm events, West Texas is an ideal location to study ice-nucleating particles (INPs) in severe precipitation. Our results present that cumulative INP concentration in our precipitation samples below −20 °C could be high in the samples collected while observing > 10 mm h−1 precipitation with notably large hydrometeor sizes and an implication of cattle feedyard bacteria inclusion. Marine bacteria were found in a subset of our precipitation and cattle feedyard samples.
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.
Ottmar Möhler, Michael Adams, Larissa Lacher, Franziska Vogel, Jens Nadolny, Romy Ullrich, Cristian Boffo, Tatjana Pfeuffer, Achim Hobl, Maximilian Weiß, Hemanth S. K. Vepuri, Naruki Hiranuma, and Benjamin J. Murray
Atmos. Meas. Tech., 14, 1143–1166, https://doi.org/10.5194/amt-14-1143-2021, https://doi.org/10.5194/amt-14-1143-2021, 2021
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The Earth's climate is influenced by clouds, which are impacted by ice-nucleating particles (INPs), a minor fraction of atmospheric aerosols. INPs induce ice formation in clouds and thus often initiate precipitation formation. The Portable Ice Nucleation Experiment (PINE) is the first fully automated instrument to study cloud ice formation and to obtain long-term records of INPs. This is a timely development, and the capabilities it offers for research and atmospheric monitoring are significant.
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.
Gourihar Kulkarni, Naruki Hiranuma, Ottmar Möhler, Kristina Höhler, Swarup China, Daniel J. Cziczo, and Paul J. DeMott
Atmos. Meas. Tech., 13, 6631–6643, https://doi.org/10.5194/amt-13-6631-2020, https://doi.org/10.5194/amt-13-6631-2020, 2020
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This study presents a new continuous-flow-diffusion-chamber-style operated ice chamber (Modified Compact Ice Chamber, MCIC) to measure the immersion-freezing efficiency of atmospheric particles. MCIC allowed us to obtain maximum droplet-freezing efficiency at higher time resolution without droplet breakthrough ambiguity. Its evaluation was performed by reproducing published data from the recent ice nucleation workshop and past laboratory data for standard and airborne ice-nucleating particles.
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.
Luisa Ickes, Grace C. E. Porter, Robert Wagner, Michael P. Adams, Sascha Bierbauer, Allan K. Bertram, Merete Bilde, Sigurd Christiansen, Annica M. L. Ekman, Elena Gorokhova, Kristina Höhler, Alexei A. Kiselev, Caroline Leck, Ottmar Möhler, Benjamin J. Murray, Thea Schiebel, Romy Ullrich, and Matthew E. Salter
Atmos. Chem. Phys., 20, 11089–11117, https://doi.org/10.5194/acp-20-11089-2020, https://doi.org/10.5194/acp-20-11089-2020, 2020
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The Arctic is a region where aerosols are scarce. Sea spray might be a potential source of aerosols acting as ice-nucleating particles. We investigate two common phytoplankton species (Melosira arctica and Skeletonema marinoi) and present their ice nucleation activity in comparison with Arctic seawater microlayer samples from different field campaigns. We also aim to understand the aerosolization process of marine biological samples and the potential effect on the ice nucleation activity.
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.
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.
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.
Xianda Gong, Heike Wex, Thomas Müller, Alfred Wiedensohler, Kristina Höhler, Konrad Kandler, Nan Ma, Barbara Dietel, Thea Schiebel, Ottmar Möhler, and Frank Stratmann
Atmos. Chem. Phys., 19, 10883–10900, https://doi.org/10.5194/acp-19-10883-2019, https://doi.org/10.5194/acp-19-10883-2019, 2019
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For the diverse aerosol on Cyprus, we found the following: new particle formation can be a source of cloud condensation nuclei. Particle hygroscopicity showed that particles ~<100 nm contained mostly organic material, while larger ones were more hygroscopic. Two separate methods obtained similar concentrations of ice-nucleating particles (INP), with mostly no evidence of a local origin. Different parameterizations overestimated INP concentration in this rather polluted region.
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.
Naruki Hiranuma, Kouji Adachi, David M. Bell, Franco Belosi, Hassan Beydoun, Bhaskar Bhaduri, Heinz Bingemer, Carsten Budke, Hans-Christian Clemen, Franz Conen, Kimberly M. Cory, Joachim Curtius, Paul J. DeMott, Oliver Eppers, Sarah Grawe, Susan Hartmann, Nadine Hoffmann, Kristina Höhler, Evelyn Jantsch, Alexei Kiselev, Thomas Koop, Gourihar Kulkarni, Amelie Mayer, Masataka Murakami, Benjamin J. Murray, Alessia Nicosia, Markus D. Petters, Matteo Piazza, Michael Polen, Naama Reicher, Yinon Rudich, Atsushi Saito, Gianni Santachiara, Thea Schiebel, Gregg P. Schill, Johannes Schneider, Lior Segev, Emiliano Stopelli, Ryan C. Sullivan, Kaitlyn Suski, Miklós Szakáll, Takuya Tajiri, Hans Taylor, Yutaka Tobo, Romy Ullrich, Daniel Weber, Heike Wex, Thomas F. Whale, Craig L. Whiteside, Katsuya Yamashita, Alla Zelenyuk, and Ottmar Möhler
Atmos. Chem. Phys., 19, 4823–4849, https://doi.org/10.5194/acp-19-4823-2019, https://doi.org/10.5194/acp-19-4823-2019, 2019
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A total of 20 ice nucleation measurement techniques contributed to investigate the immersion freezing behavior of cellulose particles – natural polymers. Our data showed several types of cellulose are able to nucleate ice as efficiently as some mineral dust samples and cellulose has the potential to be an important atmospheric ice-nucleating particle. Continued investigation/collaboration is necessary to obtain further insight into consistency or diversity of ice nucleation measurements.
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.
Nicholas A. Marsden, Romy Ullrich, Ottmar Möhler, Stine Eriksen Hammer, Konrad Kandler, Zhiqiang Cui, Paul I. Williams, Michael J. Flynn, Dantong Liu, James D. Allan, and Hugh Coe
Atmos. Chem. Phys., 19, 2259–2281, https://doi.org/10.5194/acp-19-2259-2019, https://doi.org/10.5194/acp-19-2259-2019, 2019
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The composition of airborne dust influences climate and ecosystems but its measurements presents a huge analytical challenge. Using online single-particle mass spectrometry, we demonstrate differences in mineralogy and mixing state can be detected in real time in both laboratory studies and ambient measurements. The results provide insights into the temporal and spatial evolution of dust properties that will be useful for aerosol–cloud interaction studies and dust cycle modelling.
Kaitlyn J. Suski, David M. Bell, Naruki Hiranuma, Ottmar Möhler, Dan Imre, and Alla Zelenyuk
Atmos. Chem. Phys., 18, 17497–17513, https://doi.org/10.5194/acp-18-17497-2018, https://doi.org/10.5194/acp-18-17497-2018, 2018
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This work investigates the cloud condensation nuclei and ice nucleation activity of bacteria using cloud chamber data and a single particle mass spectrometer. The size and chemical composition of the cloud residuals show that bacterial fragments mixed with agar growth media activate preferentially over intact bacteria cells as cloud condensation nuclei. Intact bacteria cells do not make it into cloud droplets; they thus cannot serve as immersion-mode ice nucleating particles.
Paul J. DeMott, Ottmar Möhler, Daniel J. Cziczo, Naruki Hiranuma, Markus D. Petters, Sarah S. Petters, Franco Belosi, Heinz G. Bingemer, Sarah D. Brooks, Carsten Budke, Monika Burkert-Kohn, Kristen N. Collier, Anja Danielczok, Oliver Eppers, Laura Felgitsch, Sarvesh Garimella, Hinrich Grothe, Paul Herenz, Thomas C. J. Hill, Kristina Höhler, Zamin A. Kanji, Alexei Kiselev, Thomas Koop, Thomas B. Kristensen, Konstantin Krüger, Gourihar Kulkarni, Ezra J. T. Levin, Benjamin J. Murray, Alessia Nicosia, Daniel O'Sullivan, Andreas Peckhaus, Michael J. Polen, Hannah C. Price, Naama Reicher, Daniel A. Rothenberg, Yinon Rudich, Gianni Santachiara, Thea Schiebel, Jann Schrod, Teresa M. Seifried, Frank Stratmann, Ryan C. Sullivan, Kaitlyn J. Suski, Miklós Szakáll, Hans P. Taylor, Romy Ullrich, Jesus Vergara-Temprado, Robert Wagner, Thomas F. Whale, Daniel Weber, André Welti, Theodore W. Wilson, Martin J. Wolf, and Jake Zenker
Atmos. Meas. Tech., 11, 6231–6257, https://doi.org/10.5194/amt-11-6231-2018, https://doi.org/10.5194/amt-11-6231-2018, 2018
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The ability to measure ice nucleating particles is vital to quantifying their role in affecting clouds and precipitation. Methods for measuring droplet freezing were compared while co-sampling relevant particle types. Measurement correspondence was very good for ice nucleating particles of bacterial and natural soil origin, and somewhat more disparate for those of mineral origin. Results reflect recently improved capabilities and provide direction toward addressing remaining measurement issues.
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.
Matthias Hummel, Corinna Hoose, Bernhard Pummer, Caroline Schaupp, Janine Fröhlich-Nowoisky, and Ottmar Möhler
Atmos. Chem. Phys., 18, 15437–15450, https://doi.org/10.5194/acp-18-15437-2018, https://doi.org/10.5194/acp-18-15437-2018, 2018
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How important for clouds is the ability of biological particles to glaciate droplets at little supercooling? In a case study, the regional atmospheric model COSMO–ART is used. Perturbed and control runs are compared.
The number of ice particles that are nucleated by biological particles is highest at around −10 °C. No significant influence on the average state of the cloud ice phase was found. However, the number of ice crystals is slightly enhanced in the absence of other ice nucleators.
Costa D. Christopoulos, Sarvesh Garimella, Maria A. Zawadowicz, Ottmar Möhler, and Daniel J. Cziczo
Atmos. Meas. Tech., 11, 5687–5699, https://doi.org/10.5194/amt-11-5687-2018, https://doi.org/10.5194/amt-11-5687-2018, 2018
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Compositional analysis of atmospheric and laboratory aerosols is often conducted with mass spectrometry. In this study, machine learning is used to automatically differentiate particles on the basis of chemistry and size. The ability of the machine learning algorithm was then tested on a data set for which the particles were not initially known to judge its ability.
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.
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.
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
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.
Leonid Nichman, Emma Järvinen, James Dorsey, Paul Connolly, Jonathan Duplissy, Claudia Fuchs, Karoliina Ignatius, Kamalika Sengupta, Frank Stratmann, Ottmar Möhler, Martin Schnaiter, and Martin Gallagher
Atmos. Meas. Tech., 10, 3231–3248, https://doi.org/10.5194/amt-10-3231-2017, https://doi.org/10.5194/amt-10-3231-2017, 2017
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Optical probes are frequently used for the detection of cloud particles. The detected microphysical properties may affect particle growth and accretion mechanisms and the light scattering properties of cirrus clouds. In the CLOUD chamber study at CERN, we compared four optical measurement techniques. We show that shape derivation alone is not sufficient to determine the phase of the small cloud particles. None of the instruments were able to unambiguously determine the phase of small particles.
Giancarlo Ciarelli, Imad El Haddad, Emily Bruns, Sebnem Aksoyoglu, Ottmar Möhler, Urs Baltensperger, and André S. H. Prévôt
Geosci. Model Dev., 10, 2303–2320, https://doi.org/10.5194/gmd-10-2303-2017, https://doi.org/10.5194/gmd-10-2303-2017, 2017
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In Europe, residential wood-burning emissions constitute one of the main anthropogenic sources of air pollution. Novel wood-burning experiments performed in a state-of-the-art smog chamber provide valuable information on the chemical properties of wood-burning emissions and the transformation in the atmosphere. In this study, these new data were used in a box model to constrain a parameterization suitable for predicting the contribution of wood burning to air pollution with large-scale models.
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.
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.
Naruki Hiranuma, Ottmar Möhler, Gourihar Kulkarni, Martin Schnaiter, Steffen Vogt, Paul Vochezer, Emma Järvinen, Robert Wagner, David M. Bell, Jacqueline Wilson, Alla Zelenyuk, and Daniel J. Cziczo
Atmos. Meas. Tech., 9, 3817–3836, https://doi.org/10.5194/amt-9-3817-2016, https://doi.org/10.5194/amt-9-3817-2016, 2016
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A new pumped counterflow virtual impactor (PCVI) called the ice-selecting PCVI (IS-PCVI) has been developed to collect ice crystal residuals for investigating physico-chemical properties of ice-nucleating particles. The results show that the ice crystals of volume-equivalent diameter ~ 10 to 30 µm can be efficiently separated from the supercooled droplets and interstitial particles. The IS-PCVI is efficient when the counterflow-to-input flow ratio is within 0.09 to 0.18.
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.
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.
G. Vali, P. J. DeMott, O. Möhler, and T. F. Whale
Atmos. Chem. Phys., 15, 10263–10270, https://doi.org/10.5194/acp-15-10263-2015, https://doi.org/10.5194/acp-15-10263-2015, 2015
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Clarification is needed in the terminology used to discuss ice nucleation in the literature. Conflicting interpretations coupled with uncertainties about the details of the processes have led to difficulties in the clear communication of results and ideas. This paper contains a proposal for future usage. This proposed terminology was arrived at as a result of a year-long exchange of suggestions by a number of scientists.
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. 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
T. F. Whale, B. J. Murray, D. O'Sullivan, T. W. Wilson, N. S. Umo, K. J. Baustian, J. D. Atkinson, D. A. Workneh, and G. J. Morris
Atmos. Meas. Tech., 8, 2437–2447, https://doi.org/10.5194/amt-8-2437-2015, https://doi.org/10.5194/amt-8-2437-2015, 2015
P. Amato, M. Joly, C. Schaupp, E. Attard, O. Möhler, C. E. Morris, Y. Brunet, and A.-M. Delort
Atmos. Chem. Phys., 15, 6455–6465, https://doi.org/10.5194/acp-15-6455-2015, https://doi.org/10.5194/acp-15-6455-2015, 2015
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Mortality rate of typical bacterial aerosols (Pseudomonas species) was determined in a cloud simulation chamber. Ice nucleation activity remained unchanged for several hours in aerosolized cells, whether they were viable or not. Cloud increased the specific removal of ice nucleation active cells by precipitation. Survival was negatively impacted by the presence of cloud and by sulfates.
N. S. Umo, B. J. Murray, M. T. Baeza-Romero, J. M. Jones, A. R. Lea-Langton, T. L. Malkin, D. O'Sullivan, L. Neve, J. M. C. Plane, and A. Williams
Atmos. Chem. Phys., 15, 5195–5210, https://doi.org/10.5194/acp-15-5195-2015, https://doi.org/10.5194/acp-15-5195-2015, 2015
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Combustion ash particles nucleate ice in the immersion mode at conditions relevant to mixed-phase clouds. Hence, combustion ashes could play an important role in primary ice formation in mixed-phase clouds, especially in clouds that are formed near the emission source of these aerosol particles. From this study, there is a need to quantify the atmospheric abundance of combustion ashes in order to quantitatively assess the impact of combustion ashes on mixed-phase clouds.
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.
H. Wex, S. Augustin-Bauditz, Y. Boose, C. Budke, J. Curtius, K. Diehl, A. Dreyer, F. Frank, S. Hartmann, N. Hiranuma, E. Jantsch, Z. A. Kanji, A. Kiselev, T. Koop, O. Möhler, D. Niedermeier, B. Nillius, M. Rösch, D. Rose, C. Schmidt, I. Steinke, and F. Stratmann
Atmos. Chem. Phys., 15, 1463–1485, https://doi.org/10.5194/acp-15-1463-2015, https://doi.org/10.5194/acp-15-1463-2015, 2015
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Immersion freezing measurements from seven different measurement techniques were intercompared using a biological ice nucleating material from bacteria. Although different techniques examined differently concentrated droplets, it was possible to find a uniform description, which showed that results from all experiments were generally in good agreement and were also in agreement with parameterizations published earlier in literature.
P. J. DeMott, A. J. Prenni, G. R. McMeeking, R. C. Sullivan, M. D. Petters, Y. Tobo, M. Niemand, O. Möhler, J. R. Snider, Z. Wang, and S. M. Kreidenweis
Atmos. Chem. Phys., 15, 393–409, https://doi.org/10.5194/acp-15-393-2015, https://doi.org/10.5194/acp-15-393-2015, 2015
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Laboratory and field data are used together to develop an empirical relation between the concentrations of mineral dust particles at sizes above 0.5 microns, approximated as a single compositional type, and ice nucleating particle concentrations measured versus temperature. This should be useful in global modeling of ice cloud formation. The utility of laboratory data for parameterization development is reinforced, and the need for careful interpretation of ice nucleation data is emphasized.
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. Hiranuma, N. Hoffmann, A. Kiselev, A. Dreyer, K. Zhang, G. Kulkarni, T. Koop, and O. Möhler
Atmos. Chem. Phys., 14, 2315–2324, https://doi.org/10.5194/acp-14-2315-2014, https://doi.org/10.5194/acp-14-2315-2014, 2014
D. O'Sullivan, B. J. Murray, T. L. Malkin, T. F. Whale, N. S. Umo, J. D. Atkinson, H. C. Price, K. J. Baustian, J. Browse, and M. E. Webb
Atmos. Chem. Phys., 14, 1853–1867, https://doi.org/10.5194/acp-14-1853-2014, https://doi.org/10.5194/acp-14-1853-2014, 2014
S. M. Platt, I. El Haddad, A. A. Zardini, M. Clairotte, C. Astorga, R. Wolf, J. G. Slowik, B. Temime-Roussel, N. Marchand, I. Ježek, L. Drinovec, G. Močnik, O. Möhler, R. Richter, P. Barmet, F. Bianchi, U. Baltensperger, and A. S. H. Prévôt
Atmos. Chem. Phys., 13, 9141–9158, https://doi.org/10.5194/acp-13-9141-2013, https://doi.org/10.5194/acp-13-9141-2013, 2013
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)
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
Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole
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
Technical Note: A Technique to Convert NO2 to NO2– with S(IV) and its Application to Measuring Nitrate Photolysis
Suppressed atmospheric chemical aging of cooking organic aerosol particles in wintertime conditions
Bulk and molecular-level composition of primary organic aerosol from wood, straw, cow dung, and plastic burning
Formation and Loss of Light Absorbance by Phenolic Aqueous SOA by OH and an Organic Triplet Excited State
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
Photoenhanced sulfates formation by the heterogeneous uptake of SO2 on non-photoactive mineral dust
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
Effects of storage conditions on the molecular-level composition of organic aerosol particles
Characterization of gas and particle emissions from open burning of household solid waste from South Africa
Chemically distinct particle-phase emissions from highly controlled pyrolysis of three wood types
Predicting photooxidant concentrations in aerosol liquid water based on laboratory extracts of ambient particles
Physicochemical characterization of free troposphere and marine boundary layer ice-nucleating particles collected by aircraft in the eastern North Atlantic
Large differences of highly oxygenated organic molecules (HOMs) and low-volatile species in secondary organic aerosols (SOAs) formed from ozonolysis of β-pinene and limonene
Impact of fossil and non-fossil fuel sources on the molecular compositions of water-soluble humic-like substances in PM2.5 at a suburban site of Yangtze River Delta, China
Technical note: Improved synthetic routes to cis- and trans-(2-methyloxirane-2,3-diyl)dimethanol (cis- and trans-β-isoprene epoxydiol)
Technical note: Intercomparison study of the elemental carbon radiocarbon analysis methods using synthetic known samples
Chemical evolution of primary and secondary biomass burning aerosols during daytime and nighttime
Formation of highly oxygenated organic molecules from the oxidation of limonene by OH radical: significant contribution of H-abstraction pathway
Measurement report: Atmospheric aging of combustion-derived particles – impact on stable free radical concentration and its ability to produce reactive oxygen species in aqueous media
Photoaging of phenolic secondary organic aerosol in the aqueous phase: evolution of chemical and optical properties and effects of oxidants
An intercomparison study of four different techniques for measuring the chemical composition of nanoparticles
Simultaneous formation of sulfate and nitrate via co-uptake of SO2 and NO2 by aqueous NaCl droplets: combined effect of nitrate photolysis and chlorine chemistry
Photo-induced shrinking of aqueous glycine aerosol droplets
Sulfate formation via aerosol-phase SO2 oxidation by model biomass burning photosensitizers: 3,4-dimethoxybenzaldehyde, vanillin and syringaldehyde using single-particle mixing-state analysis
Yields and molecular composition of gas-phase and secondary organic aerosol from the photooxidation of the volatile consumer product benzyl alcohol: formation of highly oxygenated and hydroxy nitro-aromatic compounds
A combined gas- and particle-phase analysis of highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis
Comparison of aqueous secondary organic aerosol (aqSOA) product distributions from guaiacol oxidation by non-phenolic and phenolic methoxybenzaldehydes as photosensitizers in the absence and presence of ammonium nitrate
Technical note: Chemical composition and source identification of fluorescent components in atmospheric water-soluble brown carbon by excitation–emission matrix spectroscopy with parallel factor analysis – potential limitations and applications
Insoluble lipid film mediates transfer of soluble saccharides from the sea to the atmosphere: the role of hydrogen bonding
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.
Feng Jiang, Kyla Siemens, Claudia Linke, Yanxia Li, Yiwei Gong, Thomas Leisner, Alexander Laskin, and Harald Saathoff
Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, https://doi.org/10.5194/acp-24-2639-2024, 2024
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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.
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.
Aaron Lieberman, Julietta Picco, Murat Onder, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2023-2876, https://doi.org/10.5194/egusphere-2023-2876, 2023
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We developed a method that uses S(IV) in aqueous solution to quantitatively convert NO2 to NO2–. This allows both species to be quantified using the Griess method. As an example of the utility of the method, we used it to quantify 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.
Wenli Liu, Longkun He, Yingjun Liu, Keren Liao, Qi Chen, and Mikinori Kuwata
EGUsphere, https://doi.org/10.5194/egusphere-2023-2657, https://doi.org/10.5194/egusphere-2023-2657, 2023
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Cooking is one of the major particle sources in urban areas. Previous laboratory studies demonstrated the chemical lifetimes of cooking organic aerosols 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.
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.
Stephanie Arciva, Lan Ma, Camille Mavis, Chrystal Guzman, and Cort Anastasio
EGUsphere, https://doi.org/10.5194/egusphere-2023-2719, https://doi.org/10.5194/egusphere-2023-2719, 2023
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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.
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.
Chong Han, Jiawei Ma, Wangjin Yang, and Hongxing Yang
EGUsphere, https://doi.org/10.5194/egusphere-2023-1273, https://doi.org/10.5194/egusphere-2023-1273, 2023
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We provide direct evidences that light prominently enhances the conversion of SO2 to sulfates on non-photoactive mineral dust, where 3SO2 can act as a pivotal trigger to generate sulfates. Photochemical sulfate formation depends on H2O, O2, and basicity of mineral dust. It is suggested that the SO2 photochemistry on non-photoactive mineral dust significantly contributes to sulfates, highlighting previously unknown pathway to better explain the missing sources of atmospheric sulfates.
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.
Julian Resch, Kate Wolfer, Alexandre Barth, and Markus Kalberer
Atmos. Chem. Phys., 23, 9161–9171, https://doi.org/10.5194/acp-23-9161-2023, https://doi.org/10.5194/acp-23-9161-2023, 2023
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Detailed chemical analysis of organic aerosols is necessary to better understand their effects on climate and health. Aerosol samples are often stored for days to months before analysis. We examined the effects of storage conditions (i.e., time, temperature, and aerosol storage on filters or as solvent extracts) on composition and found significant changes in the concentration of individual compounds, indicating that sample storage can strongly affect the detailed chemical particle composition.
Xiaoliang Wang, Hatef Firouzkouhi, Judith C. Chow, John G. Watson, Warren Carter, and Alexandra S. M. De Vos
Atmos. Chem. Phys., 23, 8921–8937, https://doi.org/10.5194/acp-23-8921-2023, https://doi.org/10.5194/acp-23-8921-2023, 2023
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Open burning of household and municipal solid waste is a common practice in developing countries and is a significant source of air pollution. However, few studies have measured emissions from open burning of waste. This study determined gas and particulate emissions from open burning of 10 types of household solid-waste materials. These results can improve emission inventories, air quality management, and assessment of the health and climate effects of open burning of household waste.
Anita M. Avery, Mariam Fawaz, Leah R. Williams, Tami Bond, and Timothy B. Onasch
Atmos. Chem. Phys., 23, 8837–8854, https://doi.org/10.5194/acp-23-8837-2023, https://doi.org/10.5194/acp-23-8837-2023, 2023
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Pyrolysis is the thermal decomposition of fuels like wood which occurs during combustion or as an isolated process. During combustion, some pyrolysis products are emitted directly, while others are oxidized in the combustion process. This work describes the chemical composition of particle-phase pyrolysis products in order to investigate both the uncombusted emissions from wildfires and the fuel that participates in combustion.
Lan Ma, Reed Worland, Wenqing Jiang, Christopher Niedek, Chrystal Guzman, Keith J. Bein, Qi Zhang, and Cort Anastasio
Atmos. Chem. Phys., 23, 8805–8821, https://doi.org/10.5194/acp-23-8805-2023, https://doi.org/10.5194/acp-23-8805-2023, 2023
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Although photooxidants are important in airborne particles, little is known of their concentrations. By measuring oxidants in a series of particle dilutions, we predict their concentrations in aerosol liquid water (ALW). We find •OH concentrations in ALW are on the order of 10−15 M, similar to their cloud/fog values, while oxidizing triplet excited states and singlet molecular oxygen have ALW values of ca. 10−13 M and 10−12 M, respectively, roughly 10–100 times higher than in cloud/fog drops.
Daniel A. Knopf, Peiwen Wang, Benny Wong, Jay M. Tomlin, Daniel P. Veghte, Nurun N. Lata, Swarup China, Alexander Laskin, Ryan C. Moffet, Josephine Y. Aller, Matthew A. Marcus, and Jian Wang
Atmos. Chem. Phys., 23, 8659–8681, https://doi.org/10.5194/acp-23-8659-2023, https://doi.org/10.5194/acp-23-8659-2023, 2023
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Ambient particle populations and associated ice-nucleating particles (INPs)
were examined from particle samples collected on board aircraft in the marine
boundary layer and free troposphere in the eastern North Atlantic during
summer and winter. Chemical imaging shows distinct differences in the
particle populations seasonally and with sampling altitudes, which are
reflected in the INP types. Freezing parameterizations are derived for
implementation in cloud-resolving and climate models.
Dandan Liu, Yun Zhang, Shujun Zhong, Shuang Chen, Qiaorong Xie, Donghuan Zhang, Qiang Zhang, Wei Hu, Junjun Deng, Libin Wu, Chao Ma, Haijie Tong, and Pingqing Fu
Atmos. Chem. Phys., 23, 8383–8402, https://doi.org/10.5194/acp-23-8383-2023, https://doi.org/10.5194/acp-23-8383-2023, 2023
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Based on ultra-high-resolution mass spectrometry analysis, we found that β-pinene oxidation-derived highly oxygenated organic molecules (HOMs) exhibit higher yield at high ozone concentration, while limonene oxidation-derived HOMs exhibit higher yield at moderate ozone concentration. The distinct molecular response of HOMs and low-volatile species in different biogenic secondary organic aerosols to ozone concentrations provides a new clue for more accurate air quality prediction and management.
Mengying Bao, Yan-Lin Zhang, Fang Cao, Yihang Hong, Yu-Chi Lin, Mingyuan Yu, Hongxing Jiang, Zhineng Cheng, Rongshuang Xu, and Xiaoying Yang
Atmos. Chem. Phys., 23, 8305–8324, https://doi.org/10.5194/acp-23-8305-2023, https://doi.org/10.5194/acp-23-8305-2023, 2023
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The interaction between the sources and molecular compositions of humic-like substances (HULIS) at Nanjing, China, was explored. Significant fossil fuel source contributions to HULIS were found in the 14C results from biomass burnng and traffic emissions. Increasing biogenic secondary organic aerosol (SOA) products and anthropogenic aromatic compounds were detected in summer and winter, respectively.
Molly Frauenheim, Jason D. Surratt, Zhenfa Zhang, and Avram Gold
Atmos. Chem. Phys., 23, 7859–7866, https://doi.org/10.5194/acp-23-7859-2023, https://doi.org/10.5194/acp-23-7859-2023, 2023
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We report synthesis of the isoprene-derived photochemical oxidation products trans- and cis-β-epoxydiols in high overall yields from inexpensive, readily available starting compounds. Protection/deprotection steps or time-consuming purification is not required, and the reactions can be scaled up to gram quantities. The procedures provide accessibility of these important compounds to atmospheric chemistry laboratories with only basic capabilities in organic synthesis.
Xiangyun Zhang, Jun Li, Sanyuan Zhu, Junwen Liu, Ping Ding, Shutao Gao, Chongguo Tian, Yingjun Chen, Ping'an Peng, and Gan Zhang
Atmos. Chem. Phys., 23, 7495–7502, https://doi.org/10.5194/acp-23-7495-2023, https://doi.org/10.5194/acp-23-7495-2023, 2023
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The results show that 14C elemental carbon (EC) was not only related to the isolation method but also to the types and proportions of the biomass sources in the sample. The hydropyrolysis (Hypy) method, which can be used to isolate a highly stable portion of ECHypy and avoid charring, is a more effective and stable approach for the matrix-independent 14C quantification of EC in aerosols, and the 13C–ECHypy and non-fossil ECHypy values of SRM1649b were –24.9 ‰ and 11 %, respectively.
Amir Yazdani, Satoshi Takahama, John K. Kodros, Marco Paglione, Mauro Masiol, Stefania Squizzato, Kalliopi Florou, Christos Kaltsonoudis, Spiro D. Jorga, Spyros N. Pandis, and Athanasios Nenes
Atmos. Chem. Phys., 23, 7461–7477, https://doi.org/10.5194/acp-23-7461-2023, https://doi.org/10.5194/acp-23-7461-2023, 2023
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Organic aerosols directly emitted from wood and pellet stove combustion are found to chemically transform (approximately 15 %–35 % by mass) under daytime aging conditions simulated in an environmental chamber. A new marker for lignin-like compounds is found to degrade at a different rate than previously identified biomass burning markers and can potentially provide indication of aging time in ambient samples.
Hao Luo, Luc Vereecken, Hongru Shen, Sungah Kang, Iida Pullinen, Mattias Hallquist, Hendrik Fuchs, Andreas Wahner, Astrid Kiendler-Scharr, Thomas F. Mentel, and Defeng Zhao
Atmos. Chem. Phys., 23, 7297–7319, https://doi.org/10.5194/acp-23-7297-2023, https://doi.org/10.5194/acp-23-7297-2023, 2023
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Oxidation of limonene, an element emitted by trees and chemical products, by OH, a daytime oxidant, forms many highly oxygenated organic molecules (HOMs), including C10-20 compounds. HOMs play an important role in new particle formation and growth. HOM formation can be explained by the chemistry of peroxy radicals. We found that a minor branching ratio initial pathway plays an unexpected, significant role. Considering this pathway enables accurate simulations of HOMs and other concentrations.
Heather L. Runberg and Brian J. Majestic
Atmos. Chem. Phys., 23, 7213–7223, https://doi.org/10.5194/acp-23-7213-2023, https://doi.org/10.5194/acp-23-7213-2023, 2023
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Environmentally persistent free radicals (EPFRs) are an emerging pollutant found in soot particles. Understanding how these change as they move through the atmosphere is important to human health. Here, soot was generated in the laboratory and exposed to simulated sunlight. The concentrations and characteristics of EPFRs in the soot were measured and found to be unchanged. However, it was also found that the ability of soot to form hydroxyl radicals was stronger for fresh soot.
Wenqing Jiang, Christopher Niedek, Cort Anastasio, and Qi Zhang
Atmos. Chem. Phys., 23, 7103–7120, https://doi.org/10.5194/acp-23-7103-2023, https://doi.org/10.5194/acp-23-7103-2023, 2023
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We studied how aqueous-phase secondary organic aerosol (aqSOA) form and evolve from a phenolic carbonyl commonly present in biomass burning smoke. The composition and optical properties of the aqSOA are significantly affected by photochemical reactions and are dependent on the oxidants' concentration and identity in water. During photoaging, the aqSOA initially becomes darker, but prolonged aging leads to the formation of volatile products, resulting in significant mass loss and photobleaching.
Lucía Caudillo, Mihnea Surdu, Brandon Lopez, Mingyi Wang, Markus Thoma, Steffen Bräkling, Angela Buchholz, Mario Simon, Andrea C. Wagner, Tatjana Müller, Manuel Granzin, Martin Heinritzi, Antonio Amorim, David M. Bell, Zoé Brasseur, Lubna Dada, Jonathan Duplissy, Henning Finkenzeller, Xu-Cheng He, Houssni Lamkaddam, Naser G. A. Mahfouz, Vladimir Makhmutov, Hanna E. Manninen, Guillaume Marie, Ruby Marten, Roy L. Mauldin, Bernhard Mentler, Antti Onnela, Tuukka Petäjä, Joschka Pfeifer, Maxim Philippov, Ana A. Piedehierro, Birte Rörup, Wiebke Scholz, Jiali Shen, Dominik Stolzenburg, Christian Tauber, Ping Tian, António Tomé, Nsikanabasi Silas Umo, Dongyu S. Wang, Yonghong Wang, Stefan K. Weber, André Welti, Marcel Zauner-Wieczorek, Urs Baltensperger, Richard C. Flagan, Armin Hansel, Jasper Kirkby, Markku Kulmala, Katrianne Lehtipalo, Douglas R. Worsnop, Imad El Haddad, Neil M. Donahue, Alexander L. Vogel, Andreas Kürten, and Joachim Curtius
Atmos. Chem. Phys., 23, 6613–6631, https://doi.org/10.5194/acp-23-6613-2023, https://doi.org/10.5194/acp-23-6613-2023, 2023
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In this study, we present an intercomparison of four different techniques for measuring the chemical composition of nanoparticles. The intercomparison was performed based on the observed chemical composition, calculated volatility, and analysis of the thermograms. We found that the methods generally agree on the most important compounds that are found in the nanoparticles. However, they do see different parts of the organic spectrum. We suggest potential explanations for these differences.
Ruifeng Zhang and Chak Keung Chan
Atmos. Chem. Phys., 23, 6113–6126, https://doi.org/10.5194/acp-23-6113-2023, https://doi.org/10.5194/acp-23-6113-2023, 2023
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Research into sulfate and nitrate formation from co-uptake of NO2 and SO2, especially under irradiation, is rare. We studied the co-uptake of NO2 and SO2 by NaCl droplets under various conditions, including irradiation and dark, and RHs, using Raman spectroscopy flow cell and kinetic model simulation. Significant nitrate formation from NO2 hydrolysis can be photolyzed to generate OH radicals that can further react with chloride to produce reactive chlorine species and promote sulfate formation.
Shinnosuke Ishizuka, Oliver Reich, Grégory David, and Ruth Signorell
Atmos. Chem. Phys., 23, 5393–5402, https://doi.org/10.5194/acp-23-5393-2023, https://doi.org/10.5194/acp-23-5393-2023, 2023
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Photosensitizers play an important role in the photochemistry of atmospheric aerosols. Our study provides evidence that mesoscopic glycine clusters forming in aqueous droplets act as unconventional photosensitizers in the visible light spectrum. We observed the influence of these photoactive molecular aggregates in single optically trapped aqueous droplets. Such mesoscopic photosensitizers might be more important for aerosol photochemistry than previously anticipated.
Liyuan Zhou, Zhancong Liang, Beatrix Rosette Go Mabato, Rosemarie Ann Infante Cuevas, Rongzhi Tang, Mei Li, Chunlei Cheng, and Chak K. Chan
Atmos. Chem. Phys., 23, 5251–5261, https://doi.org/10.5194/acp-23-5251-2023, https://doi.org/10.5194/acp-23-5251-2023, 2023
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This study reveals the sulfate formation in photosensitized particles from biomass burning under UV and SO2, of which the relative atmospheric importance in sulfate production was qualitatively compared to nitrate photolysis. On the basis of single-particle aerosol mass spectrometry measurements, the number percentage of sulfate-containing particles and relative peak area of sulfate in single-particle spectra exhibited a descending order of 3,4-dimethoxybenzaldehyde > vanillin > syringaldehyde.
Mohammed Jaoui, Kenneth S. Docherty, Michael Lewandowski, and Tadeusz E. Kleindienst
Atmos. Chem. Phys., 23, 4637–4661, https://doi.org/10.5194/acp-23-4637-2023, https://doi.org/10.5194/acp-23-4637-2023, 2023
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VCPs are a class of chemicals widely used in industrial and consumer products (e.g., coatings, adhesives, inks, personal care products) and are an important component of total VOCs in urban atmospheres. This study provides SOA yields and detailed chemical analysis of the gas- and aerosol-phase products of the photooxidation of one of these VCPs, benzyl alcohol. These results will allow better links between characterized sources and their resulting criteria for pollutant formation.
Jian Zhao, Ella Häkkinen, Frans Graeffe, Jordan E. Krechmer, Manjula R. Canagaratna, Douglas R. Worsnop, Juha Kangasluoma, and Mikael Ehn
Atmos. Chem. Phys., 23, 3707–3730, https://doi.org/10.5194/acp-23-3707-2023, https://doi.org/10.5194/acp-23-3707-2023, 2023
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Based on the combined measurements of gas- and particle-phase highly oxygenated organic molecules (HOMs) from α-pinene ozonolysis, enhancement of dimers in particles was observed. We conducted experiments wherein the dimer to monomer (D / M) ratios of HOMs in the gas phase were modified (adding CO / NO) to investigate the effects of the corresponding D / M ratios in the particles. These results are important for a better understanding of secondary organic aerosol formation in the atmosphere.
Beatrix Rosette Go Mabato, Yong Jie Li, Dan Dan Huang, Yalin Wang, and Chak K. Chan
Atmos. Chem. Phys., 23, 2859–2875, https://doi.org/10.5194/acp-23-2859-2023, https://doi.org/10.5194/acp-23-2859-2023, 2023
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We compared non-phenolic and phenolic methoxybenzaldehydes as photosensitizers for aqueous secondary organic aerosol (aqSOA) formation under cloud and fog conditions. We showed that the structural features of photosensitizers affect aqSOA formation. We also elucidated potential interactions between photosensitization and ammonium nitrate photolysis. Our findings are useful for evaluating the importance of photosensitized reactions on aqSOA formation, which could improve aqSOA predictive models.
Tao Cao, Meiju Li, Cuncun Xu, Jianzhong Song, Xingjun Fan, Jun Li, Wanglu Jia, and Ping'an Peng
Atmos. Chem. Phys., 23, 2613–2625, https://doi.org/10.5194/acp-23-2613-2023, https://doi.org/10.5194/acp-23-2613-2023, 2023
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This work comprehensively investigated the fluorescence data of light-absorbing organic compounds, water-soluble organic matter in different types of aerosol samples, soil dust, and fulvic and humic acids using an excitation–emission matrix (EEM) method and parallel factor modeling. The results revealed which light-absorbing species can be detected by EEM and also provided important information for identifying the chemical composition and possible sources of these species in atmospheric samples.
Minglan Xu, Narcisse Tsona Tchinda, Jianlong Li, and Lin Du
Atmos. Chem. Phys., 23, 2235–2249, https://doi.org/10.5194/acp-23-2235-2023, https://doi.org/10.5194/acp-23-2235-2023, 2023
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The promotion of soluble saccharides on sea spray aerosol (SSA) generation and the changes in particle morphology were observed. On the contrary, the coexistence of surface insoluble fatty acid film and soluble saccharides significantly inhibited the production of SSA. This is the first demonstration that hydrogen bonding mediated by surface-insoluble fatty acids contributes to saccharide transfer in seawater, providing a new mechanism for saccharide enrichment in SSA.
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Short summary
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.
In this study, we highlight the potential impact of particles from certain terrestrial sources...
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