Articles | Volume 25, issue 3
https://doi.org/10.5194/acp-25-1917-2025
© Author(s) 2025. 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-25-1917-2025
© Author(s) 2025. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Measurement report
| 
12 Feb 2025
Measurement report |
| 12 Feb 2025
| 12 Feb 2025
Measurement report: Brown carbon aerosol in rural Germany – sources, chemistry, and diurnal variations
Feng Jiang
CORRESPONDING AUTHOR
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Institute of Applied Geosciences, Working Group for Environmental Mineralogy and Environmental System Analysis, Karlsruhe Institute of Technology, 76131 Karlsruhe, Germany
now at: Paul H. O'Neill School of Public & Environmental Affairs, Indiana University, Bloomington, IN 47405, United States
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Uzoamaka Ezenobi
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Junwei Song
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Hengheng Zhang
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Linyu Gao
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Thomas Leisner
Institute of Meteorology and Climate Research, Karlsruhe Institute of Technology, 76344 Eggenstein–Leopoldshafen, Germany
Institute of Environmental Physics, Heidelberg University, 69120 Heidelberg, Germany
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Back carbon is an atmospheric pollutant from combustion, contributes to the Arctic warming. However, its properties change as it travels through the atmosphere, affecting its impact. We recreated Arctic transport conditions in a laboratory to study how black carbon evolves over time. Our findings show that temperature and altitude strongly influence its transformation, providing key insights for improving climate models and understanding Arctic pollution.
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This study presents concurrent online measurements of organic gas and particles (VOCs and OA) at a forested site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contributed significantly to nighttime particle growth. The results help us to understand the causes of nighttime particle growth regularly observed in summer in central European rural forested environments.
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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.
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Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
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We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
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This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
Feng Jiang, Junwei Song, Jonas Bauer, Linyu Gao, Magdalena Vallon, Reiner Gebhardt, Thomas Leisner, Stefan Norra, and Harald Saathoff
Atmos. Chem. Phys., 22, 14971–14986, https://doi.org/10.5194/acp-22-14971-2022, https://doi.org/10.5194/acp-22-14971-2022, 2022
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We studied brown carbon aerosol during typical summer and winter periods in downtown Karlsruhe in southwestern Germany. The chromophore and chemical composition of brown carbon was determined by excitation–emission spectroscopy and mass spectrometry. The chromophore types and sources were substantially different in winter and summer. Humic-like chromophores of different degrees of oxidation dominated and were associated with molecules of different molecular weight and nitrogen content.
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Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
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We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Magdalena Vallon, Linyu Gao, Feng Jiang, Bianca Krumm, Jens Nadolny, Junwei Song, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 15, 1795–1810, https://doi.org/10.5194/amt-15-1795-2022, https://doi.org/10.5194/amt-15-1795-2022, 2022
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A LED-based light source has been constructed for the AIDA simulation chamber at the Karlsruhe Institute of Technology. It allows aerosol formation and ageing studies under atmospherically relevant illumination intensities and spectral characteristics at temperatures from –90 °C to 30 °C with the possibility of changing the photon flux and irradiation spectrum at any point. The first results of photolysis experiments with 2,3-pentanedione, iron oxalate and a brown carbon component are shown.
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Clouds and aerosol are important for weather and climate. Typically, pure water cloud droplets stay liquid until around −35 °C, unless they come into contact with ice-nucleating particles (INPs). INPs are a rare subset of aerosol particles. Using uncrewed aerial vehicles (UAVs), it is possible to collect aerosol particles and analyse their ice-nucleating ability. This study describes the test and validation of a sampling set-up that can be used to collect aerosol particles onto a filter.
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Atmos. Meas. Tech., 18, 3051–3072, https://doi.org/10.5194/amt-18-3051-2025, https://doi.org/10.5194/amt-18-3051-2025, 2025
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It is of increasing importance to monitor nitrate pollution that can harm ecosystems. However, commonly used aerosol monitoring equipment cannot distinguish inorganic from organic forms of nitrate, which may have different consequences for the environment. We describe a method to differentiate types of nitrates that can be applied to ambient monitoring to improve understanding of its formation and impact.
Simone Brunamonti, Harald Saathoff, Albert Hertzog, Glenn Diskin, Masatomo Fujiwara, Karen Rosenlof, Ottmar Möhler, Béla Tuzson, Lukas Emmenegger, Nadir Amarouche, Georges Durry, Fabien Frérot, Jean-Christophe Samake, Claire Cenac, Julio Lopez, Paul Monnier, and Mélanie Ghysels
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Back carbon is an atmospheric pollutant from combustion, contributes to the Arctic warming. However, its properties change as it travels through the atmosphere, affecting its impact. We recreated Arctic transport conditions in a laboratory to study how black carbon evolves over time. Our findings show that temperature and altitude strongly influence its transformation, providing key insights for improving climate models and understanding Arctic pollution.
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Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2025-87, https://doi.org/10.5194/essd-2025-87, 2025
Revised manuscript under review for ESSD
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Clouds play a key role in weather and climate. Pure liquid water droplets are liquid until about -35 °C without the presence of a small subset of aerosols, ice-nucleating particles (INPs). These INPs lead to primary ice formation and therefore impact the phase of clouds. The dataset described herein provides INP concentration measurements at two altitudes. Connecting this data to synoptic conditions and ambient data might provide a better understanding of INPs in Finnish Lapland.
Junwei Song, Georgios I. Gkatzelis, Ralf Tillmann, Nicolas Brüggemann, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 13199–13217, https://doi.org/10.5194/acp-24-13199-2024, https://doi.org/10.5194/acp-24-13199-2024, 2024
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Biogenic volatile organic compounds (BVOCs) and organic aerosol (OA) particles were measured online in a stressed spruce-dominated forest. OA was mainly attributed to the monoterpene oxidation products. The mixing ratios of BVOCs were higher than the values previously measured in other temperate forests. The results demonstrate that BVOCs are influenced not only by meteorology and biogenic emissions but also by local anthropogenic emissions and subsequent chemical transformation processes.
Xiaoli Shen, David M. Bell, Hugh Coe, Naruki Hiranuma, Fabian Mahrt, Nicholas A. Marsden, Claudia Mohr, Daniel M. Murphy, Harald Saathoff, Johannes Schneider, Jacqueline Wilson, Maria A. Zawadowicz, Alla Zelenyuk, Paul J. DeMott, Ottmar Möhler, and Daniel J. Cziczo
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Single-particle mass spectrometry (SPMS) is commonly used to measure the chemical composition and mixing state of aerosol particles. Intercomparison of SPMS instruments was conducted. All instruments reported similar size ranges and common spectral features. The instrument-specific detection efficiency was found to be more dependent on particle size than type. All differentiated secondary organic aerosol, soot, and soil dust but had difficulties differentiating among minerals and dusts.
Hengheng Zhang, Wei Huang, Xiaoli Shen, Ramakrishna Ramisetty, Junwei Song, Olga Kiseleva, Christopher Claus Holst, Basit Khan, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 10617–10637, https://doi.org/10.5194/acp-24-10617-2024, https://doi.org/10.5194/acp-24-10617-2024, 2024
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Our study unravels how stagnant winter conditions elevate aerosol levels in Stuttgart. Cloud cover at night plays a pivotal role, impacting morning air quality. Validating a key model, our findings aid accurate air quality predictions, crucial for effective pollution mitigation in urban areas.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
Atmos. Chem. Phys., 24, 6699–6717, https://doi.org/10.5194/acp-24-6699-2024, https://doi.org/10.5194/acp-24-6699-2024, 2024
Short summary
Short summary
This study presents concurrent online measurements of organic gas and particles (VOCs and OA) at a forested site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contributed significantly to nighttime particle growth. The results help us to understand the causes of nighttime particle growth regularly observed in summer in central European rural forested environments.
Hengheng Zhang, Christian Rolf, Ralf Tillmann, Christian Wesolek, Frank Gunther Wienhold, Thomas Leisner, and Harald Saathoff
Aerosol Research, 2, 135–151, https://doi.org/10.5194/ar-2-135-2024, https://doi.org/10.5194/ar-2-135-2024, 2024
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Our study employs advanced tools, including scanning lidar, balloons, and UAVs, to explore aerosol particles in the atmosphere. The scanning lidar offers distinctive near-ground-level insights, enriching our comprehension of aerosol distribution from ground level to the free troposphere. This research provides valuable data for comparing remote sensing and in situ aerosol measurements, advancing our understanding of aerosol impacts on radiative transfer, clouds, and air quality.
Johanna S. Seidel, Alexei A. Kiselev, Alice Keinert, Frank Stratmann, Thomas Leisner, and Susan Hartmann
Atmos. Chem. Phys., 24, 5247–5263, https://doi.org/10.5194/acp-24-5247-2024, https://doi.org/10.5194/acp-24-5247-2024, 2024
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Clouds often contain several thousand times more ice crystals than aerosol particles catalyzing ice formation. This phenomenon, commonly known as ice multiplication, is often explained by secondary ice formation due to the collisions between falling ice particles and droplets. In this study, we mimic this riming process. Contrary to earlier experiments, we found no efficient ice multiplication, which fundamentally questions the importance of the rime-splintering mechanism.
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
Short summary
Short summary
We investigated the optical properties, chemical composition, and formation mechanisms of secondary organic aerosol (SOA) and brown carbon (BrC) from the oxidation of indole with and without NO2 in the Aerosol Interaction and Dynamics in the Atmosphere (AIDA) simulation chamber. This work is one of the very few to link the optical properties and chemical composition of indole SOA with and without NO2 by simulation chamber experiments.
Wei Huang, Cheng Wu, Linyu Gao, Yvette Gramlich, Sophie L. Haslett, Joel Thornton, Felipe D. Lopez-Hilfiker, Ben H. Lee, Junwei Song, Harald Saathoff, Xiaoli Shen, Ramakrishna Ramisetty, Sachchida N. Tripathi, Dilip Ganguly, Feng Jiang, Magdalena Vallon, Siegfried Schobesberger, Taina Yli-Juuti, and Claudia Mohr
Atmos. Chem. Phys., 24, 2607–2624, https://doi.org/10.5194/acp-24-2607-2024, https://doi.org/10.5194/acp-24-2607-2024, 2024
Short summary
Short summary
We present distinct molecular composition and volatility of oxygenated organic aerosol particles in different rural, urban, and mountain environments. We do a comprehensive investigation of the relationship between the chemical composition and volatility of oxygenated organic aerosol particles across different systems and environments. This study provides implications for volatility descriptions of oxygenated organic aerosol particles in different model frameworks.
Yiwei Gong, Feng Jiang, Yanxia Li, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 24, 167–184, https://doi.org/10.5194/acp-24-167-2024, https://doi.org/10.5194/acp-24-167-2024, 2024
Short summary
Short summary
This study investigates the role of the important atmospheric reactive intermediates in the formation of dimers and aerosol in monoterpene ozonolysis at different temperatures. Through conducting a series of chamber experiments and utilizing chemical kinetic and aerosol dynamic models, the SOA formation processes are better described, especially for colder regions. The results can be used to improve the chemical mechanism modeling of monoterpenes and SOA parameterization in transport models.
Mohit Singh, Stephanie Helen Jones, Alexei Kiselev, Denis Duft, and Thomas Leisner
Atmos. Meas. Tech., 16, 5205–5215, https://doi.org/10.5194/amt-16-5205-2023, https://doi.org/10.5194/amt-16-5205-2023, 2023
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We introduce a novel method for simultaneous measurement of the viscosity and surface tension of metastable liquids. Our approach is based on the phase analysis of excited shape oscillations in levitated droplets. It is applicable to a wide range of atmospheric conditions and can monitor changes in real time. The technique holds great promise for investigating the effect of atmospheric processing on the viscosity and surface tension of solution droplets in equilibrium with water vapour.
Robert Wagner, Alexander D. James, Victoria L. Frankland, Ottmar Möhler, Benjamin J. Murray, John M. C. Plane, Harald Saathoff, Ralf Weigel, and Martin Schnaiter
Atmos. Chem. Phys., 23, 6789–6811, https://doi.org/10.5194/acp-23-6789-2023, https://doi.org/10.5194/acp-23-6789-2023, 2023
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Polar stratospheric clouds (PSCs) play an important role in the depletion of stratospheric ozone. They can consist of different chemical species, including crystalline nitric acid hydrates. We found that mineral dust or meteoric ablation material can efficiently catalyse the formation of a specific phase of nitric acid dihydrate crystals. We determined predominant particle shapes and infrared optical properties of these crystals, which are important inputs for remote sensing detection of PSCs.
Kara D. Lamb, Jerry Y. Harrington, Benjamin W. Clouser, Elisabeth J. Moyer, Laszlo Sarkozy, Volker Ebert, Ottmar Möhler, and Harald Saathoff
Atmos. Chem. Phys., 23, 6043–6064, https://doi.org/10.5194/acp-23-6043-2023, https://doi.org/10.5194/acp-23-6043-2023, 2023
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This study investigates how ice grows directly from vapor in cirrus clouds by comparing observations of populations of ice crystals growing in a cloud chamber against models developed in the context of single-crystal laboratory studies. We demonstrate that previous discrepancies between different experimental measurements do not necessarily point to different physical interpretations but are rather due to assumptions that were made in terms of how experiments were modeled in previous studies.
Feng Jiang, Junwei Song, Jonas Bauer, Linyu Gao, Magdalena Vallon, Reiner Gebhardt, Thomas Leisner, Stefan Norra, and Harald Saathoff
Atmos. Chem. Phys., 22, 14971–14986, https://doi.org/10.5194/acp-22-14971-2022, https://doi.org/10.5194/acp-22-14971-2022, 2022
Short summary
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We studied brown carbon aerosol during typical summer and winter periods in downtown Karlsruhe in southwestern Germany. The chromophore and chemical composition of brown carbon was determined by excitation–emission spectroscopy and mass spectrometry. The chromophore types and sources were substantially different in winter and summer. Humic-like chromophores of different degrees of oxidation dominated and were associated with molecules of different molecular weight and nitrogen content.
Fritz Waitz, Martin Schnaiter, Thomas Leisner, and Emma Järvinen
Atmos. Chem. Phys., 22, 7087–7103, https://doi.org/10.5194/acp-22-7087-2022, https://doi.org/10.5194/acp-22-7087-2022, 2022
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Riming, i.e., the accretion of small droplets on the surface of ice particles via collision, is one of the major uncertainties in model prediction of mixed-phase clouds. We discuss the occurrence (up to 50% of particles) and aging of rimed ice particles and show correlations of the occurrence and the degree of riming with ambient meteorological parameters using data gathered by the Particle Habit Imaging and Polar Scattering (PHIPS) probe during three airborne in situ field campaigns.
Linyu Gao, Junwei Song, Claudia Mohr, Wei Huang, Magdalena Vallon, Feng Jiang, Thomas Leisner, and Harald Saathoff
Atmos. Chem. Phys., 22, 6001–6020, https://doi.org/10.5194/acp-22-6001-2022, https://doi.org/10.5194/acp-22-6001-2022, 2022
Short summary
Short summary
We study secondary organic aerosol (SOA) from β-caryophyllene (BCP) ozonolysis with and without nitrogen oxides over 213–313 K in the simulation chamber. The yields and the rate constants were determined at 243–313 K. Chemical compositions varied at different temperatures, indicating a strong impact on the BCP ozonolysis pathways. This work helps to better understand the SOA from BCP ozonolysis for conditions representative of the real atmosphere from the boundary layer to the upper troposphere.
Magdalena Vallon, Linyu Gao, Feng Jiang, Bianca Krumm, Jens Nadolny, Junwei Song, Thomas Leisner, and Harald Saathoff
Atmos. Meas. Tech., 15, 1795–1810, https://doi.org/10.5194/amt-15-1795-2022, https://doi.org/10.5194/amt-15-1795-2022, 2022
Short summary
Short summary
A LED-based light source has been constructed for the AIDA simulation chamber at the Karlsruhe Institute of Technology. It allows aerosol formation and ageing studies under atmospherically relevant illumination intensities and spectral characteristics at temperatures from –90 °C to 30 °C with the possibility of changing the photon flux and irradiation spectrum at any point. The first results of photolysis experiments with 2,3-pentanedione, iron oxalate and a brown carbon component are shown.
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.
Julia Schneider, Kristina Höhler, Robert Wagner, Harald Saathoff, Martin Schnaiter, Tobias Schorr, Isabelle Steinke, Stefan Benz, Manuel Baumgartner, Christian Rolf, Martina Krämer, Thomas Leisner, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14403–14425, https://doi.org/10.5194/acp-21-14403-2021, https://doi.org/10.5194/acp-21-14403-2021, 2021
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Homogeneous freezing is a relevant mechanism for the formation of cirrus clouds in the upper troposphere. Based on an extensive set of homogeneous freezing experiments at the AIDA chamber with aqueous sulfuric acid aerosol, we provide a new fit line for homogeneous freezing onset conditions of sulfuric acid aerosol focusing on cirrus temperatures. In the atmosphere, homogeneous freezing thresholds have important implications on the cirrus cloud occurrence and related cloud radiative effects.
Naruki Hiranuma, Brent W. Auvermann, Franco Belosi, Jack Bush, Kimberly M. Cory, Dimitrios G. Georgakopoulos, Kristina Höhler, Yidi Hou, Larissa Lacher, Harald Saathoff, Gianni Santachiara, Xiaoli Shen, Isabelle Steinke, Romy Ullrich, Nsikanabasi S. Umo, Hemanth S. K. Vepuri, Franziska Vogel, and Ottmar Möhler
Atmos. Chem. Phys., 21, 14215–14234, https://doi.org/10.5194/acp-21-14215-2021, https://doi.org/10.5194/acp-21-14215-2021, 2021
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We present laboratory and field studies showing that an open-lot livestock facility is a substantial source of atmospheric ice-nucleating particles (INPs). The ambient concentration of INPs from livestock facilities in Texas is very high. It is up to several thousand INPs per liter below –20 °C and may impact regional aerosol–cloud interactions. About 50% of feedlot INPs were supermicron in diameter. No notable amount of known ice-nucleating microorganisms was found in our feedlot samples.
Alexei A. Kiselev, Alice Keinert, Tilia Gaedeke, Thomas Leisner, Christoph Sutter, Elena Petrishcheva, and Rainer Abart
Atmos. Chem. Phys., 21, 11801–11814, https://doi.org/10.5194/acp-21-11801-2021, https://doi.org/10.5194/acp-21-11801-2021, 2021
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Alkali feldspar is the most abundant mineral in the Earth's crust and is often present in mineral dust aerosols that are responsible for the formation of rain and snow in clouds. However, the cloud droplets containing pure potassium-rich feldspar would not freeze unless cooled down to a very low temperature. Here we show that partly replacing potassium with sodium would induce fracturing of feldspar, exposing a crystalline surface that could initiate freezing at higher temperature.
Hengheng Zhang, Frank Wagner, Harald Saathoff, Heike Vogel, Gholam Ali Hoshyaripour, Vanessa Bachmann, Jochen Förstner, and Thomas Leisner
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2021-193, https://doi.org/10.5194/amt-2021-193, 2021
Revised manuscript not accepted
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The evolution and the properties of Saharan dust plume were characterized by LIDARs, a sun photometer, and a regional transport model. Comparison between LIDAR measurements, sun photometer and ICON-ART predictions shows a good agreement for dust arrival time, dust layer height, and dust structure but also that the model overestimates the backscatter coefficients by a factor of (2.2 ± 0.16) and underestimate aerosol optical depth by a factor of (1.5 ± 0.11).
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.
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.
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.
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.
Isabelle Steinke, Naruki Hiranuma, Roger Funk, Kristina Höhler, Nadine Tüllmann, Nsikanabasi Silas Umo, Peter G. Weidler, Ottmar Möhler, and Thomas Leisner
Atmos. Chem. Phys., 20, 11387–11397, https://doi.org/10.5194/acp-20-11387-2020, https://doi.org/10.5194/acp-20-11387-2020, 2020
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In this study, we highlight the potential impact of particles from certain terrestrial sources on the formation of ice crystals in clouds. In particular, we focus on biogenic particles consisting of various organic compounds, which makes it very difficult to predict the ice nucleation properties of complex ambient particles. We find that these ambient particles are often more ice active than individual components.
Cited articles
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Huang, W., Saathoff, H., Pajunoja, A., Shen, X., Naumann, K.-H., Wagner, R., Virtanen, A., Leisner, T., and Mohr, C.: α-Pinene secondary organic aerosol at low temperature: chemical composition and implications for particle viscosity, Atmos. Chem. Phys., 18, 2883–2898, https://doi.org/10.5194/acp-18-2883-2018, 2018.
Huang, W., Saathoff, H., Shen, X., Ramisetty, R., Leisner, T., and Mohr, C.: Chemical Characterization of Highly Functionalized Organonitrates Contributing to Night-Time Organic Aerosol Mass Loadings and Particle Growth, Environ. Sci. Technol., 53, 1165–1174, https://doi.org/10.1021/acs.est.8b05826, 2019.
Jiang, F., Song, J., Bauer, J., Gao, L., Vallon, M., Gebhardt, R., Leisner, T., Norra, S., and Saathoff, H.: Chromophores and chemical composition of brown carbon characterized at an urban kerbside by excitation–emission spectroscopy and mass spectrometry, Atmos. Chem. Phys., 22, 14971–14986, https://doi.org/10.5194/acp-22-14971-2022, 2022.
Jiang, F., Saathoff, H., Ezenobi, U., Song, J., Zhang, H., Gao, L., and Leisner, T.: Dataset for the publication: Brown carbon aerosol in rural Germany: sources, chemistry, and diurnal variations, Karlsruhe Institute of Technology [data set], https://doi.org/10.35097/d0prpzkxqkq2t09y, 2024a.
Jiang, F., Siemens, K., Linke, C., Li, Y., Gong, Y., Leisner, T., Laskin, A., and Saathoff, H.: Molecular analysis of secondary organic aerosol and brown carbon from the oxidation of indole, Atmos. Chem. Phys., 24, 2639–2649, https://doi.org/10.5194/acp-24-2639-2024, 2024b.
Lack, D. A. and Langridge, J. M.: On the attribution of black and brown carbon light absorption using the Ångström exponent, Atmos. Chem. Phys., 13, 10535–10543, https://doi.org/10.5194/acp-13-10535-2013, 2013.
Laskin, A., Laskin, J., and Nizkorodov, S. A.: Chemistry of Atmospheric Brown Carbon, Chem. Rev., 115, 4335–4382, https://doi.org/10.1021/cr5006167, 2015.
Lee, B. H., Lopez-Hilfiker, F. D., D'Ambro, E. L., Zhou, P., Boy, M., Petäjä, T., Hao, L., Virtanen, A., and Thornton, J. A.: Semi-volatile and highly oxygenated gaseous and particulate organic compounds observed above a boreal forest canopy, Atmos. Chem. Phys., 18, 11547–11562, https://doi.org/10.5194/acp-18-11547-2018, 2018.
Lin, P., Liu, J., Shilling, J. E., Kathmann, S. M., Laskin, J., and Laskin, A.: Molecular characterization of brown carbon (BrC) chromophores in secondary organic aerosol generated from photo-oxidation of toluene, Phys. Chem. Chem. Phys., 17, 23312–23325, https://doi.org/10.1039/c5cp02563j, 2015.
Lin, P., Aiona, P. K., Li, Y., Shiraiwa, M., Laskin, J., Nizkorodov, S. A., and Laskin, A.: Molecular Characterization of Brown Carbon in Biomass Burning Aerosol Particles, Environ. Sci. Technol., 50, 11815–11824, https://doi.org/10.1021/acs.est.6b03024, 2016.
Lin, P., Fleming, L. T., Nizkorodov, S. A., Laskin, J., and Laskin, A.: Comprehensive Molecular Characterization of Atmospheric Brown Carbon by High Resolution Mass Spectrometry with Electrospray and Atmospheric Pressure Photoionization, Anal. Chem., 90, 12493–12502, https://doi.org/10.1021/acs.analchem.8b02177, 2018.
Linke, C., Ibrahim, I., Schleicher, N., Hitzenberger, R., Andreae, M. O., Leisner, T., and Schnaiter, M.: A novel single-cavity three-wavelength photoacoustic spectrometer for atmospheric aerosol research, Atmos. Meas. Tech., 9, 5331–5346, https://doi.org/10.5194/amt-9-5331-2016, 2016.
Liu, X., Wang, H., Wang, F., Lv, S., Wu, C., Zhao, Y., Zhang, S., Liu, S., Xu, X., Lei, Y., and Wang, G.: Secondary Formation of Atmospheric Brown Carbon in China Haze: Implication for an Enhancing Role of Ammonia, Environ. Sci. Technol., 57, 11163–11172, https://doi.org/10.1021/acs.est.3c03948, 2023.
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Lopez-Hilfiker, F. D., Mohr, C., Ehn, M., Rubach, F., Kleist, E., Wildt, J., Mentel, Th. F., Lutz, A., Hallquist, M., Worsnop, D., and Thornton, J. A.: A novel method for online analysis of gas and particle composition: description and evaluation of a Filter Inlet for Gases and AEROsols (FIGAERO), Atmos. Meas. Tech., 7, 983–1001, https://doi.org/10.5194/amt-7-983-2014, 2014.
Lopez-Hilfiker, F. D., Iyer, S., Mohr, C., Lee, B. H., D'Ambro, E. L., Kurtén, T., and Thornton, J. A.: Constraining the sensitivity of iodide adduct chemical ionization mass spectrometry to multifunctional organic molecules using the collision limit and thermodynamic stability of iodide ion adducts, Atmos. Meas. Tech., 9, 1505–1512, https://doi.org/10.5194/amt-9-1505-2016, 2016.
Mohr, C., Lopez-Hilfiker, F. D., Zotter, P., Prevot, A. S. H., Xu, L., Ng, N. L., Herndon, S. C., Williams, L. R., Franklin, J. P., Zahniser, M. S., Worsnop, D. R., Knighton, W. B., Aiken, A. C., Gorkowski, K. J., Dubey, M. K., Allan, J. D., and Thornton, J. A.: Contribution of Nitrated Phenols to Wood Burning Brown Carbon Light Absorption in Detling, United Kingdom during Winter Time, Environ. Sci. Technol., 47, 6316–6324, https://doi.org/10.1021/es400683v, 2013.
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Montoya-Aguilera, J., Horne, J. R., Hinks, M. L., Fleming, L. T., Perraud, V., Lin, P., Laskin, A., Laskin, J., Dabdub, D., and Nizkorodov, S. A.: Secondary organic aerosol from atmospheric photooxidation of indole, Atmos. Chem. Phys., 17, 11605–11621, https://doi.org/10.5194/acp-17-11605-2017, 2017.
Moschos, V., Kumar, N. K., Daellenbach, K. R., Baltensperger, U., Prevot, A. S. H., and El Haddad, I.: Source Apportionment of Brown Carbon Absorption by Coupling Ultraviolet-Visible Spectroscopy with Aerosol Mass Spectrometry, Environ. Sci. Tech. Let., 5, 302–308, https://doi.org/10.1021/acs.estlett.8b00118, 2018.
Moschos, V., Gysel-Beer, M., Modini, R. L., Corbin, J. C., Massabò, D., Costa, C., Danelli, S. G., Vlachou, A., Daellenbach, K. R., Szidat, S., Prati, P., Prévôt, A. S. H., Baltensperger, U., and El Haddad, I.: Source-specific light absorption by carbonaceous components in the complex aerosol matrix from yearly filter-based measurements, Atmos. Chem. Phys., 21, 12809–12833, https://doi.org/10.5194/acp-21-12809-2021, 2021.
Palm, B. B., Peng, Q. Y., Fredrickson, C. D., Lee, B., Garofalo, L. A., Pothier, M. A., Kreidenweis, S. M., Farmer, D. K., Pokhrel, R. P., Shen, Y. J., Murphy, S. M., Permar, W., Hu, L., Campos, T. L., Hall, S. R., Ullmann, K., Zhang, X., Flocke, F., Fischer, E. V., and Thornton, J. A.: Quantification of organic aerosol and brown carbon evolution in fresh wildfire plumes, P. Natl. Acad. Sci. USA., 117, 29469–29477, https://doi.org/10.1073/pnas.2012218117, 2020.
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Saarikoski, S., Niemi, J. V., Aurela, M., Pirjola, L., Kousa, A., Rönkkö, T., and Timonen, H.: Sources of black carbon at residential and traffic environments obtained by two source apportionment methods, Atmos. Chem. Phys., 21, 14851–14869, https://doi.org/10.5194/acp-21-14851-2021, 2021.
Saathoff, H., Naumann, K. H., Schnaiter, M., Schöck, W., Möhler, O., Schurath, U., Weingartner, E., Gysel, M., and Baltensperger, U.: Coating of soot and (NH4)2SO4 particles by ozonolysis products of α-pinene, J. Aerosol Sci., 34, 1297–321, https://doi.org/10.1016/S0021-8502(03)00364-1, 2003.
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Sandradewi, J., Prévôt, A. S. H., Szidat, S., Perron, N., Alfarra, M. R., Lanz, V. A., Weingartner, E., and Baltensperger, U.: Using aerosol light absorption measurements for the quantitative determination of wood burning and traffic emission contributions to particulate matter, Environ. Sci. Technol., 42, 3316–3323, https://doi.org/10.1021/es702253m, 2008a.
Sandradewi, J., Prévôt, A. S. H., Weingartner, E., Schmidhauser, R., Gysel, M., and Baltensperger, U.: A study of wood burning and traffic aerosols in an Alpine valley using a multi-wavelength Aethalometer, Atmos. Environ., 42, 101–112, https://doi.org/10.1016/j.atmosenv.2007.09.034, 2008b.
Satish, R., Shamjad, P., Thamban, N., Tripathi, S., and Rastogi, N.: Temporal Characteristics of Brown Carbon over the Central Indo-Gangetic Plain, Environ. Sci. Technol., 51, 6765–6772, https://doi.org/10.1021/acs.est.7b00734, 2017.
Shen, X., Vogel, H., Vogel, B., Huang, W., Mohr, C., Ramisetty, R., Leisner, T., Prévôt, A. S. H., and Saathoff, H.: Composition and origin of PM2.5 aerosol particles in the upper Rhine valley in summer, Atmos. Chem. Phys., 19, 13189–13208, https://doi.org/10.5194/acp-19-13189-2019, 2019.
Siemens, K., Morales, A., He, Q., Li, C., Hettiyadura, A. P. S., Rudich, Y., and Laskin, A.: Molecular Analysis of Secondary Brown Carbon Produced from the Photooxidation of Naphthalene, Environ. Sci. Technol., 56, 3340–3353, https://doi.org/10.1021/acs.est.1c03135, 2022.
Sumlin, B. J., Pandey, A., Walker, M. J., Pattison, R. S., Williams, B. J., and Chakrabarty, R. K.: Atmospheric Photooxidation Diminishes Light Absorption by Primary Brown Carbon Aerosol from Biomass Burning, Environ. Sci. Technol. Let., 4, 540–545, https://doi.org/10.1021/acs.estlett.7b00393, 2017.
Tang, J., Li, J., Su, T., Han, Y., Mo, Y., Jiang, H., Cui, M., Jiang, B., Chen, Y., Tang, J., Song, J., Peng, P., and Zhang, G.: Molecular compositions and optical properties of dissolved brown carbon in biomass burning, coal combustion, and vehicle emission aerosols illuminated by excitation–emission matrix spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry analysis, Atmos. Chem. Phys., 20, 2513–2532, https://doi.org/10.5194/acp-20-2513-2020, 2020.
Teich, M., van Pinxteren, D., Kecorius, S., Wang, Z. B., and Herrmann, H.: First Quantification of Imidazoles in Ambient Aerosol Particles: Potential Photosensitizers, Brown Carbon Constituents, and Hazardous Components, Environ. Sci. Technol., 50, 1166–1173, https://doi.org/10.1021/acs.est.5b05474, 2016.
Teich, M., van Pinxteren, D., Wang, M., Kecorius, S., Wang, Z., Müller, T., Močnik, G., and Herrmann, H.: Contributions of nitrated aromatic compounds to the light absorption of water-soluble and particulate brown carbon in different atmospheric environments in Germany and China, Atmos. Chem. Phys., 17, 1653–1672, https://doi.org/10.5194/acp-17-1653-2017, 2017.
Thieringer, J. R. D., Szabadi, J., Meyer, J., and Dittler, A.: Impact of Residential Real-World Wood Stove Operation on Air Quality concerning PM2.5 Immission, Processes, 10, 545, https://doi.org/10.3390/pr10030545, 2022.
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Short summary
The chemical composition of brown carbon in the particle and gas phase was determined by mass spectrometry. BrC in the gas phase was mainly controlled by secondary formation and particle-to-gas partitioning. BrC in the particle phase was mainly from secondary formation. This work helps to get a better understanding of diurnal variations and the sources of brown carbon aerosol at a rural location in central Europe.
The chemical composition of brown carbon in the particle and gas phase was determined by mass...
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