Articles | Volume 14, issue 10
https://doi.org/10.5194/amt-14-6395-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-14-6395-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
05 Oct 2021
Research article |
| 05 Oct 2021
| 05 Oct 2021
Bromine speciation in volcanic plumes: new in situ derivatization LC-MS method for the determination of gaseous hydrogen bromide by gas diffusion denuder sampling
Alexandra Gutmann
CORRESPONDING AUTHOR
Department of Chemistry, Johannes Gutenberg University, Mainz, Germany
now at: Institute of Geosciences, Johannes Gutenberg University, Mainz, Germany
now at: Max Planck Institute for Chemistry, Mainz, Germany
Nicole Bobrowski
Max Planck Institute for Chemistry, Mainz, Germany
Institute for Environmental Physics, University of Heidelberg,
Heidelberg, Germany
Marcello Liotta
Instituto Nazionale di Geofisica e Vulcanologia, Sezione di Palermo, Italy
Thorsten Hoffmann
CORRESPONDING AUTHOR
Department of Chemistry, Johannes Gutenberg University, Mainz, Germany
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Patrick Dewald, Tobias Seubert, Laura Wüst, Jan Schuladen, Frank Drewnick, Friederike Fachinger, Thorsten Hoffmann, and John N. Crowley
Atmos. Meas. Tech., 19, 3445–3457, https://doi.org/10.5194/amt-19-3445-2026, https://doi.org/10.5194/amt-19-3445-2026, 2026
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We have developed and tested an instrument that quantitatively detects particulate nitrate. Gas-phase reactive nitrogen species are denuded using an active-carbon surface and particle nitrate is converted to NO2, which is detected using cavity-ringdown-spectroscopy. Key to accurate measurement of particulate nitrate is drying of the sampled air. Excellent agreement with an aerosol-mass-spectrometer indicates that the instrument detects both organic and inorganic nitrate particle mass accurately.
Johannes Degen, Nicole Bobrowski, Mélisende M. Bossard, Lucie Boucher, Huilin Chen, Andreas Engel, Bastien H. Geil, Giovanni B. Giuffrida, Steven van Heuven, Thorsten Hoffmann, Niklas Karbach, Gianluigi Ortenzi, and Tanja J. Schuck
EGUsphere, https://doi.org/10.5194/egusphere-2026-1865, https://doi.org/10.5194/egusphere-2026-1865, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Observations in volcanic plumes often rely on Uncrewed Aerial Systems (UAS). In July 2024, we used the active AirCore technique with UAS to probe the plumes of Mount Etna (Italy). This was the first time to use this technique inside volcanic plumes. AirCore samples are stored in long coils for laboratory analyses delivering high-quality trace gas measurements. We observed enhanced mole fractions of CO2 and often also of CO. allowing conclusions on oxidation processes inside the crater.
Niklas Karbach, Pauline Pouyes, Emilie Perraudin, Eric Villenave, and Thorsten Hoffmann
EGUsphere, https://doi.org/10.5194/egusphere-2026-2473, https://doi.org/10.5194/egusphere-2026-2473, 2026
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
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We investigated the chemical composition of organic aerosol near Paris to distinguish contributions from urban emissions and surrounding biogenic sources. By combining high resolution mass spectrometry with statistical clustering and wind information, we identified clear source specific patterns. Urban influence was associated with sulfur and nitrogen containing compounds, whereas biogenic influence was dominated by oxidized organic compounds.
Maja Rüth, Nicole Bobrowski, Ellen Bräutigam, Alexander Nies, Jonas Kuhn, Thorsten Hoffmann, Niklas Karbach, Bastien Geil, Ralph Kleinschek, Stefan Schmitt, and Ulrich Platt
Atmos. Meas. Tech., 19, 2047–2059, https://doi.org/10.5194/amt-19-2047-2026, https://doi.org/10.5194/amt-19-2047-2026, 2026
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UV absorption and electrochemical O3 sensor measurement techniques suffer from interferences, especially from SO2, which is a main constituent of volcanic plumes. Only chemiluminescence (CL) O3 monitors have no known interference with SO2. However, modern CL O3 monitors are impractical because they are heavy and bulky. We developed and applied a lightweight version of a CL O3 instrument (l.5 kg, shoebox size) and present the result of those drone based CL O3 measurements.
Tobias Dieter Schmitt, Moritz Sindram, Benedikt Alexander Löw, Lukas Weis, Ralph Kleinschek, Nicole Bobrowski, and André Butz
EGUsphere, https://doi.org/10.5194/egusphere-2026-1387, https://doi.org/10.5194/egusphere-2026-1387, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
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Current monitoring systems for volcanic gases use ultra-violet and visible light, since the sky is bright in these regions. We analyzed if it is possible to extend their measurement concept to the near-infrared, where other important gases like CO2, HF and HCl are accessible. Our results indicate that this is unrealistic for CO2, but possible for HF and HCl, at least for some volcanos. In the future, this could contribute to a better understanding of volcanic processes and eruption risks.
Denis Leppla, Stefanie Hildmann, Nora Zannoni, Leslie A. Kremper, Bruna A. Holanda, Jonathan Williams, Christopher Pöhlker, Stefan Wolff, Marta Sà, Maria Christina Solci, Ulrich Pöschl, and Thorsten Hoffmann
Atmos. Chem. Phys., 26, 365–390, https://doi.org/10.5194/acp-26-365-2026, https://doi.org/10.5194/acp-26-365-2026, 2026
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The chemical composition of organic particles in the Amazon rainforest was investigated to understand how biogenic and human emissions influence the atmosphere in this unique ecosystem. Seasonal patterns were found where wet seasons were dominated by biogenic compounds from natural sources while dry seasons showed increased fire-related pollutants. These findings reveal how emissions, fires and long-range transport affect atmospheric chemistry, with implications for climate models.
Jackson Seymore, Miklós Szakáll, Alexander Theis, Subir K. Mitra, Christine Borchers, and Thorsten Hoffmann
Atmos. Chem. Phys., 25, 18249–18265, https://doi.org/10.5194/acp-25-18249-2025, https://doi.org/10.5194/acp-25-18249-2025, 2025
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Laboratory studies examined carbonyl deposition into ice crystals using a flowtube setup. Ice crystals were grown under conditions that mimic cirrus clouds in the presence of carbonyl vapors. Ice and gas samples were collected and analyzed to calculate ice uptake coefficients for 14 carbonyls at different temperatures. This revealed an inverse relationship between uptake and temperature. Vapor pressure and molar mass were found to be the most significant factors in uptake.
Christine Borchers, Lasse Moormann, Bastien Geil, Niklas Karbach, David Wasserzier, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 7231–7242, https://doi.org/10.5194/amt-18-7231-2025, https://doi.org/10.5194/amt-18-7231-2025, 2025
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A three-dimensionally printed filter holder is connected to a lightweight, high-performance pump. This sampling system allows for easy and cost-effective measurements of organic aerosols at different heights and locations. By elucidating the chemical composition of organic aerosol, sources and processing of the compounds can be identified. Measurements at different altitudes and times of the day provide insight into the chemical aging and daytime trends of the aerosol particles.
Anna Breuninger, Philipp Joppe, Jonas Wilsch, Cornelis Schwenk, Heiko Bozem, Nicolas Emig, Laurin Merkel, Rainer Rossberg, Timo Keber, Arthur Kutschka, Philipp Waleska, Stefan Hofmann, Sarah Richter, Florian Ungeheuer, Konstantin Dörholt, Thorsten Hoffmann, Annette Miltenberger, Johannes Schneider, Peter Hoor, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 16533–16551, https://doi.org/10.5194/acp-25-16533-2025, https://doi.org/10.5194/acp-25-16533-2025, 2025
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This study investigates molecular organic aerosol composition in the upper troposphere and lower stratosphere from an airborne campaign over Central Europe in summer 2024. Via ultra-high-performance liquid chromatography and high-resolution mass spectrometry of tropospheric and stratospheric filter samples, we identified various organic compounds. Our findings underscore the significant cross-tropopause transport of biogenic secondary organic aerosol and anthropogenic pollutants.
Jackson Seymore, Martanda Gautam, Miklós Szakáll, Alexander Theis, Thorsten Hoffmann, Jialiang Ma, Lingli Zhou, and Alexander L. Vogel
Atmos. Chem. Phys., 25, 11829–11845, https://doi.org/10.5194/acp-25-11829-2025, https://doi.org/10.5194/acp-25-11829-2025, 2025
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We investigated the chemical retention of water-soluble organic compounds in Beijing aerosols using an acoustic levitator and drop-freezing experiments. Samples from PM2.5 filter extracts were frozen at -15 °C in an acoustic levitator without artificial nucleators and analyzed using ultra-high resolution mass spectrometry. Our findings reveal a non-normal distribution of retention coefficients that differs from current literature on cloud droplets.
Jade Margerum, Julia Homann, Stuart Umbo, Gernot Nehrke, Thorsten Hoffmann, Anton Vaks, Aleksandr Kononov, Alexander Osintsev, Alena Giesche, Andrew Mason, Franziska A. Lechleitner, Gideon M. Henderson, Ola Kwiecien, and Sebastian F. M. Breitenbach
Clim. Past, 21, 661–677, https://doi.org/10.5194/cp-21-661-2025, https://doi.org/10.5194/cp-21-661-2025, 2025
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We analyse a southern Siberian stalagmite to reconstruct soil respiration, wildfire, and vegetation trends during the Last Interglacial (LIG) (124.1–118.8 ka) and the Holocene (10–0 ka). Wildfires were more prevalent during the LIG than the Holocene and were supported by fire-prone species, low soil respiration, and a greater difference between summer and winter temperature. We show that vegetation type and summer/winter temperature contrast are strong drivers of Siberian wildfires.
Johanna Schäfer, Anja Beschnitt, François Burgay, Thomas Singer, Margit Schwikowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 18, 421–430, https://doi.org/10.5194/amt-18-421-2025, https://doi.org/10.5194/amt-18-421-2025, 2025
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Glaciers preserve organic compounds from atmospheric aerosols, which can serve as markers for emission sources. Most studies overlook the enantiomers of chiral compounds. We developed a two-dimensional liquid chromatography method to determine the chiral ratios of the monoterpene oxidation products cis-pinic acid and cis-pinonic acid in ice-core samples. Applied to samples from the Belukha Glacier (1870–1970 CE), the method revealed fluctuating chiral ratios for the analytes.
Christine Borchers, Jackson Seymore, Martanda Gautam, Konstantin Dörholt, Yannik Müller, Andreas Arndt, Laura Gömmer, Florian Ungeheuer, Miklós Szakáll, Stephan Borrmann, Alexander Theis, Alexander L. Vogel, and Thorsten Hoffmann
Atmos. Chem. Phys., 24, 13961–13974, https://doi.org/10.5194/acp-24-13961-2024, https://doi.org/10.5194/acp-24-13961-2024, 2024
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Riming, a crucial process in cloud dynamics, influences the vertical distribution of compounds in the atmosphere. Experiments in Mainz's wind tunnel investigated retention coefficients of organic compounds under varying conditions. Findings suggest a correlation between the Henry's law constant and retention, applicable even to complex organic molecules.
Niklas Karbach, Lisa Höhler, Peter Hoor, Heiko Bozem, Nicole Bobrowski, and Thorsten Hoffmann
Atmos. Meas. Tech., 17, 4081–4086, https://doi.org/10.5194/amt-17-4081-2024, https://doi.org/10.5194/amt-17-4081-2024, 2024
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The system presented here can accurately generate and reproduce a stable flow of gas mixtures of known concentrations over several days using ambient air as a dilution medium. In combination with the small size and low weight of the system, this enables the calibration of hydrogen sensors in the field, reducing the influence of matrix effects on the accuracy of the sensor. The system is inexpensive to assemble and easy to maintain, which is the key to reliable measurement results.
Simon Warnach, Holger Sihler, Christian Borger, Nicole Bobrowski, Steffen Beirle, Ulrich Platt, and Thomas Wagner
Atmos. Meas. Tech., 16, 5537–5573, https://doi.org/10.5194/amt-16-5537-2023, https://doi.org/10.5194/amt-16-5537-2023, 2023
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BrO inside volcanic gas plumes but can be used in combination with SO2 to characterize the volcanic property and its activity state. High-quality satellite observations can provide a global inventory of this important quantity. This paper investigates how to accurately detect BrO inside volcanic plumes from the satellite UV spectrum. A sophisticated novel non-volcanic background correction scheme is presented, and systematic errors including cross-interference with formaldehyde are minimized.
Julia Homann, Niklas Karbach, Stacy A. Carolin, Daniel H. James, David Hodell, Sebastian F. M. Breitenbach, Ola Kwiecien, Mark Brenner, Carlos Peraza Lope, and Thorsten Hoffmann
Biogeosciences, 20, 3249–3260, https://doi.org/10.5194/bg-20-3249-2023, https://doi.org/10.5194/bg-20-3249-2023, 2023
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Cave stalagmites contain substances that can be used to reconstruct past changes in local and regional environmental conditions. We used two classes of biomarkers (polycyclic aromatic hydrocarbons and monosaccharide anhydrides) to detect the presence of fire and to also explore changes in fire regime (e.g. fire frequency, intensity, and fuel source). We tested our new method on a stalagmite from Mayapan, a large Maya city on the Yucatán Peninsula.
Thomas Wagner, Simon Warnach, Steffen Beirle, Nicole Bobrowski, Adrian Jost, Janis Puķīte, and Nicolas Theys
Atmos. Meas. Tech., 16, 1609–1662, https://doi.org/10.5194/amt-16-1609-2023, https://doi.org/10.5194/amt-16-1609-2023, 2023
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We investigate 3D effects of volcanic plumes on the retrieval results of satellite and ground-based UV–Vis observations. With its small ground pixels of 3.5 x 5.5 km², the TROPOMI instrument can detect much smaller volcanic plumes than previous instruments. At the same time, 3D effects become important. The effect of horizontal photon paths especially can lead to a strong underestimation of the derived plume contents of up to > 50 %, which can be further increased for strong absorbers like SO2.
Denis Leppla, Nora Zannoni, Leslie Kremper, Jonathan Williams, Christopher Pöhlker, Marta Sá, Maria Christina Solci, and Thorsten Hoffmann
Atmos. Chem. Phys., 23, 809–820, https://doi.org/10.5194/acp-23-809-2023, https://doi.org/10.5194/acp-23-809-2023, 2023
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Chiral chemodiversity plays a critical role in biochemical processes such as insect and plant communication. Here we report on the measurement of chiral-specified secondary organic aerosol in the Amazon rainforest. The results show that the chiral ratio is mainly determined by large-scale emission processes. Characteristic emissions of chiral aerosol precursors from different forest ecosystems can thus provide large-scale information on different biogenic sources via chiral particle analysis.
Yunfan Liu, Hang Su, Siwen Wang, Chao Wei, Wei Tao, Mira L. Pöhlker, Christopher Pöhlker, Bruna A. Holanda, Ovid O. Krüger, Thorsten Hoffmann, Manfred Wendisch, Paulo Artaxo, Ulrich Pöschl, Meinrat O. Andreae, and Yafang Cheng
Atmos. Chem. Phys., 23, 251–272, https://doi.org/10.5194/acp-23-251-2023, https://doi.org/10.5194/acp-23-251-2023, 2023
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The origins of the abundant cloud condensation nuclei (CCN) in the upper troposphere (UT) of the Amazon remain unclear. With model developments of new secondary organic aerosol schemes and constrained by observation, we show that strong aerosol nucleation and condensation in the UT is triggered by biogenic organics, and organic condensation is key for UT CCN production. This UT CCN-producing mechanism may prevail over broader vegetation canopies and deserves emphasis in aerosol–climate feedback.
Jing Duan, Ru-Jin Huang, Yifang Gu, Chunshui Lin, Haobin Zhong, Wei Xu, Quan Liu, Yan You, Jurgita Ovadnevaite, Darius Ceburnis, Thorsten Hoffmann, and Colin O'Dowd
Atmos. Chem. Phys., 22, 10139–10153, https://doi.org/10.5194/acp-22-10139-2022, https://doi.org/10.5194/acp-22-10139-2022, 2022
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Biomass-burning-influenced oxygenated organic aerosol (OOA-BB), formed from the photochemical oxidation and aging of biomass burning OA (BBOA), was resolved in urban Xi’an. The aqueous-phase processed oxygenated OA (aq-OOA) concentration was more dependent on secondary inorganic aerosol (SIA) content and aerosol liquid water content (ALWC). The increased aq-OOA contribution during SIA-enhanced periods likely reflects OA evolution due to the addition of alcohol or peroxide groups
Jonas Kuhn, Nicole Bobrowski, Thomas Wagner, and Ulrich Platt
Atmos. Meas. Tech., 14, 7873–7892, https://doi.org/10.5194/amt-14-7873-2021, https://doi.org/10.5194/amt-14-7873-2021, 2021
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We propose spectrograph implementations using Fabry–Pérot interferometers for atmospheric trace gas remote sensing. Compared with widely used grating spectrographs, we find substantial light throughput and mobility advantages for high resolving powers. Besides lowering detection limits and increasing the spatial and temporal resolution of many atmospheric trace gas measurements, this approach might enable remote sensing of further important gases such as tropospheric OH radicals.
Haijie Tong, Fobang Liu, Alexander Filippi, Jake Wilson, Andrea M. Arangio, Yun Zhang, Siyao Yue, Steven Lelieveld, Fangxia Shen, Helmi-Marja K. Keskinen, Jing Li, Haoxuan Chen, Ting Zhang, Thorsten Hoffmann, Pingqing Fu, William H. Brune, Tuukka Petäjä, Markku Kulmala, Maosheng Yao, Thomas Berkemeier, Manabu Shiraiwa, and Ulrich Pöschl
Atmos. Chem. Phys., 21, 10439–10455, https://doi.org/10.5194/acp-21-10439-2021, https://doi.org/10.5194/acp-21-10439-2021, 2021
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We measured radical yields of aqueous PM2.5 extracts and found lower yields at higher concentrations of PM2.5. Abundances of water-soluble transition metals and aromatics in PM2.5 were positively correlated with the relative fraction of •OH but negatively correlated with the relative fraction of C-centered radicals among detected radicals. Composition-dependent reactive species yields may explain differences in the reactivity and health effects of PM2.5 in clean versus polluted air.
Florian Dinger, Timo Kleinbek, Steffen Dörner, Nicole Bobrowski, Ulrich Platt, Thomas Wagner, Martha Ibarra, and Eveling Espinoza
Atmos. Chem. Phys., 21, 9367–9404, https://doi.org/10.5194/acp-21-9367-2021, https://doi.org/10.5194/acp-21-9367-2021, 2021
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Monitoring magnitude or chemical composition of volcanic gas emissions can help to forecast volcanic eruptions and provides empirical data on the impact of volcanoes on the chemistry in the local and global atmosphere. This study reports and discusses continuous time series of the sulfur and bromine emission fluxes of Masaya from 2014 to 2020. We observed an annual cyclicity in the BrO / SO2 molar ratio, possibly caused by the annual variability in the atmospheric humidity.
Kai Wang, Ru-Jin Huang, Martin Brüggemann, Yun Zhang, Lu Yang, Haiyan Ni, Jie Guo, Meng Wang, Jiajun Han, Merete Bilde, Marianne Glasius, and Thorsten Hoffmann
Atmos. Chem. Phys., 21, 9089–9104, https://doi.org/10.5194/acp-21-9089-2021, https://doi.org/10.5194/acp-21-9089-2021, 2021
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Here we present the detailed molecular composition of the organic aerosol collected in three eastern Chinese cities from north to south, Changchun, Shanghai and Guangzhou, by applying LC–Orbitrap analysis. Accordingly, the aromaticity degree of chemical compounds decreases from north to south, while the oxidation degree increases from north to south, which can be explained by the different anthropogenic emissions and photochemical oxidation processes.
Bo Galle, Santiago Arellano, Nicole Bobrowski, Vladimir Conde, Tobias P. Fischer, Gustav Gerdes, Alexandra Gutmann, Thorsten Hoffmann, Ima Itikarai, Tomas Krejci, Emma J. Liu, Kila Mulina, Scott Nowicki, Tom Richardson, Julian Rüdiger, Kieran Wood, and Jiazhi Xu
Atmos. Meas. Tech., 14, 4255–4277, https://doi.org/10.5194/amt-14-4255-2021, https://doi.org/10.5194/amt-14-4255-2021, 2021
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Measurements of volcanic gases are important for geophysical research, risk assessment and environmental impact studies. Some gases, like SO2 and BrO, may be studied from the ground at a safe distance using remote sensing techniques. Many other gases require in situ access to the gas plume. Here, a drone may be an attractive alternative. This paper describes a drone specially adapted for volcanic gas studies and demonstrates its use in a field campaign at Manam volcano in Papua New Guinea.
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Short summary
Motivated by a special interest in bromine chemistry in volcanic plumes, the study presented here describes a new method for the quantitative collection of gaseous hydrogen bromide in gas diffusion denuders. The hydrogen bromide reacted during sampling with appropriate epoxides applied to the denuder walls. The denuder sampling assembly was successfully deployed in the volcanic plume of Masaya volcano, Nicaragua.
Motivated by a special interest in bromine chemistry in volcanic plumes, the study presented...
