Articles | Volume 23, issue 3
https://doi.org/10.5194/acp-23-1893-2023
© Author(s) 2023. 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-23-1893-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
03 Feb 2023
Research article |
| 03 Feb 2023
| 03 Feb 2023
Chemical and dynamical identification of emission outflows during the HALO campaign EMeRGe in Europe and Asia
Eric Förster
CORRESPONDING AUTHOR
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
now at: DLR IPA – Deutsches Zentrum für Luft- und Raumfahrt, Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
Marco Neumaier
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
Florian Obersteiner
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
Andreas Zahn
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
Andreas Hilboll
IUP Bremen – Institut für Umweltphysik, Universität Bremen,
Bremen, Germany
deceased
Anna B. Kalisz Hedegaard
DLR IPA – Deutsches Zentrum für Luft- und Raumfahrt, Institut
für Physik der Atmosphäre, Oberpfaffenhofen, Germany
IUP Bremen – Institut für Umweltphysik, Universität Bremen,
Bremen, Germany
Nikos Daskalakis
IUP Bremen – Institut für Umweltphysik, Universität Bremen,
Bremen, Germany
Alexandros Panagiotis Poulidis
IUP Bremen – Institut für Umweltphysik, Universität Bremen,
Bremen, Germany
Mihalis Vrekoussis
IUP Bremen – Institut für Umweltphysik, Universität Bremen,
Bremen, Germany
Center for Marine Environmental Sciences (MARUM), University of
Bremen, Bremen, Germany
Energy, Environment and Water Research Centre, The Cyprus Institute
(CyI), Nicosia, Cyprus
Michael Lichtenstern
DLR IPA – Deutsches Zentrum für Luft- und Raumfahrt, Institut
für Physik der Atmosphäre, Oberpfaffenhofen, Germany
Peter Braesicke
KIT – Karlsruhe Institute of Technology, Institute of Meteorology and
Climate Research, Karlsruhe, Germany
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Laura N. Saunders, Kaley A. Walker, Gabriele P. Stiller, Thomas von Clarmann, Florian Haenel, Hella Garny, Harald Bönisch, Chris D. Boone, Ariana E. Castillo, Andreas Engel, Johannes C. Laube, Marianna Linz, Felix Ploeger, David A. Plummer, Eric A. Ray, and Patrick E. Sheese
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Yijuan Zhang, Guy Brasseur, Maria Kanakidou, Claire Granier, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Kun Qu, and Mihalis Vrekoussis
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Lena Feld, Pablo Schmid, Marios Mermigkas, Dimitrios Balis, Jochen Gross, Darko Dubravica, Carlos Alberti, Benedikt Herkommer, Stefan Versick, Roland Ruhnke, Frank Hase, and Peter Braesicke
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We introduce a helicopter-borne mass balance approach, utilizing the HELiPOD platform, to accurately quantify methane (CH₄) emissions from coal mining activities. The comparison of our top-down mass flux estimates (up to 3000 kg h-1) against those from bottom-up in-mine CH4 safety sensors revealed very good agreement. This approach also has a great potential in quantifying emission source strengths (down to 20 kg h-1) from a wide range of other CH4 emitters (e.g. landfills, oil & gas industry).
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Johannes Schneider, Christiane Schulz, Florian Rubach, Anna Ludwig, Jonas Wilsch, Philipp Joppe, Christian Gurk, Sergej Molleker, Laurent Poulain, Florian Obersteiner, Torsten Gehrlein, Harald Bönisch, Andreas Zahn, Peter Hoor, Nicolas Emig, Heiko Bozem, Stephan Borrmann, and Markus Hermann
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IAGOS-CARIBIC operates an instrumented container laboratory on commercial regular passenger flights to obtain a long-term representative data set on the composition of the upper troposphere and lowermost stratosphere. Here we report on the development on a fully automated aerosol mass spectrometer for this project. We present technical specifications, necessary modifications for the automation, instrument calibration and comparisons, detection limits, and first in-flight data.
Herman G.J. Smit, Torben Galle, Romain Blot, Florian Obersteiner, Philippe Nédélec, Andreas Zahn, Jean-Marc Cousin, Ulrich Bundke, Andreas Petzold, Valerie Thouret, and Hannah Clark
EGUsphere, https://doi.org/10.5194/egusphere-2024-3760, https://doi.org/10.5194/egusphere-2024-3760, 2025
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The two ozone instruments of IAGOS (In-service Aircraft for a Global Observation System) have been compared with the Ozone PhotoMeter (OPM) of the World Calibration Center of Ozone Sondes (WCCOS) in an atmospheric simulation chamber under realistic flight conditions of pressure, temperature, and ozone concentrations. The two IAGOS-instruments showed good agreement with the OPM within 5–6 %. The observed differences are small but systematic and reproducible during the intercomparison.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
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Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Phuc Thi Minh Ha, Yugo Kanaya, Kazuyo Yamaji, Syuichi Itahashi, Satoru Chatani, Takashi Sekiya, Maria Dolores Andrés Hernández, John Philip Burrows, Hans Schlager, Michael Lichtenstern, Mira Poehlker, and Bruna Holanda
EGUsphere, https://doi.org/10.5194/egusphere-2024-2064, https://doi.org/10.5194/egusphere-2024-2064, 2024
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Black carbon and CO are important to climate change. EMeRGe airborne observation can identify the suitability of emission inventories used in CMAQv5.0.2 model for Asian polluted regions. GFEDv4.1s is suitable for fire emissions. Anthropogenic BC and CO emissions from Philippines (REASv2.1) are insufficient. The estimated Chinese emissions in 2018 are 0.65±0.25 TgBC, 166±65 TgCO and 12.4±4.8 PgCO2, suggesting a reduction and increment for China's BC and CO emissions in the HTAPv2.2z inventory.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 2024
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This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
Randall Chiu, Florian Obersteiner, Alessandro Franchin, Teresa Campos, Adriana Bailey, Christopher Webster, Andreas Zahn, and Rainer Volkamer
Atmos. Meas. Tech., 17, 5731–5746, https://doi.org/10.5194/amt-17-5731-2024, https://doi.org/10.5194/amt-17-5731-2024, 2024
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The ozone sink into oceans and marine clouds is seldom studied and highly uncertain. Calculations suggest O3 destruction at aqueous surfaces (ocean, droplets) may be strongly accelerated, but field evidence is missing. Here we compare three fast airborne O3 instruments to measure eddy covariance fluxes of O3 over the remote ocean, in clear and cloudy air. We find O3 fluxes below clouds are consistently directed into clouds, while O3 fluxes into oceans are much smaller and spatially variable.
Luis F. Millán, Peter Hoor, Michaela I. Hegglin, Gloria L. Manney, Harald Boenisch, Paul Jeffery, Daniel Kunkel, Irina Petropavlovskikh, Hao Ye, Thierry Leblanc, and Kaley Walker
Atmos. Chem. Phys., 24, 7927–7959, https://doi.org/10.5194/acp-24-7927-2024, https://doi.org/10.5194/acp-24-7927-2024, 2024
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In the Observed Composition Trends And Variability in the UTLS (OCTAV-UTLS) Stratosphere-troposphere Processes And their Role in Climate (SPARC) activity, we have mapped multiplatform ozone datasets into coordinate systems to systematically evaluate the influence of these coordinates on binned climatological variability. This effort unifies the work of studies that focused on individual coordinate system variability. Our goal was to create the most comprehensive assessment of this topic.
Philipp Joppe, Johannes Schneider, Katharina Kaiser, Horst Fischer, Peter Hoor, Daniel Kunkel, Hans-Christoph Lachnitt, Andreas Marsing, Lenard Röder, Hans Schlager, Laura Tomsche, Christiane Voigt, Andreas Zahn, and Stephan Borrmann
Atmos. Chem. Phys., 24, 7499–7522, https://doi.org/10.5194/acp-24-7499-2024, https://doi.org/10.5194/acp-24-7499-2024, 2024
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From aircraft measurements in the upper troposphere/lower stratosphere, we find a correlation between the ozone and particulate sulfate in the lower stratosphere. The correlation exhibits some variability over the measurement period exceeding the background sulfate-to-ozone correlation. From our analysis, we conclude that gas-to-particle conversion of volcanic sulfur dioxide leads to observed enhanced sulfate aerosol mixing ratios.
Hella Garny, Roland Eichinger, Johannes C. Laube, Eric A. Ray, Gabriele P. Stiller, Harald Bönisch, Laura Saunders, and Marianna Linz
Atmos. Chem. Phys., 24, 4193–4215, https://doi.org/10.5194/acp-24-4193-2024, https://doi.org/10.5194/acp-24-4193-2024, 2024
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Transport circulation in the stratosphere is important for the distribution of tracers, but its strength is hard to measure. Mean transport times can be inferred from observations of trace gases with certain properties, such as sulfur hexafluoride (SF6). However, this gas has a chemical sink in the high atmosphere, which can lead to substantial biases in inferred transport times. In this paper we present a method to correct mean transport times derived from SF6 for the effects of chemical sinks.
Yunsong Liu, Jean-Daniel Paris, Gregoire Broquet, Violeta Bescós Roy, Tania Meixus Fernandez, Rasmus Andersen, Andrés Russu Berlanga, Emil Christensen, Yann Courtois, Sebastian Dominok, Corentin Dussenne, Travis Eckert, Andrew Finlayson, Aurora Fernández de la Fuente, Catlin Gunn, Ram Hashmonay, Juliano Grigoleto Hayashi, Jonathan Helmore, Soeren Honsel, Fabrizio Innocenti, Matti Irjala, Torgrim Log, Cristina Lopez, Francisco Cortés Martínez, Jonathan Martinez, Adrien Massardier, Helle Gottschalk Nygaard, Paula Agregan Reboredo, Elodie Rousset, Axel Scherello, Matthias Ulbricht, Damien Weidmann, Oliver Williams, Nigel Yarrow, Murès Zarea, Robert Ziegler, Jean Sciare, Mihalis Vrekoussis, and Philippe Bousquet
Atmos. Meas. Tech., 17, 1633–1649, https://doi.org/10.5194/amt-17-1633-2024, https://doi.org/10.5194/amt-17-1633-2024, 2024
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We investigated the performance of 10 methane emission quantification techniques in a blind controlled-release experiment at an inerted natural gas compressor station. We reported their respective strengths, weaknesses, and potential complementarity depending on the emission rates and atmospheric conditions. Additionally, we assess the dependence of emission quantification performance on key parameters such as wind speed, deployment constraints, and measurement duration.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-516, https://doi.org/10.5194/egusphere-2024-516, 2024
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This study assesses atmospheric composition using air quality models during aircraft campaigns in Europe and Asia, focusing on carbonaceous aerosols and trace gases. While carbon monoxide is well modeled, other pollutants have moderate to weak agreement with observations. Wind speed modeling is reliable for identifying pollution plumes, where models tend to overestimate concentrations. This highlights challenges in accurately modeling aerosol and trace gas composition, particularly in cities.
Adrien Deroubaix, Marco Vountas, Benjamin Gaubert, Maria Dolores Andrés Hernández, Stephan Borrmann, Guy Brasseur, Bruna Holanda, Yugo Kanaya, Katharina Kaiser, Flora Kluge, Ovid Oktavian Krüger, Inga Labuhn, Michael Lichtenstern, Klaus Pfeilsticker, Mira Pöhlker, Hans Schlager, Johannes Schneider, Guillaume Siour, Basudev Swain, Paolo Tuccella, Kameswara S. Vinjamuri, Mihalis Vrekoussis, Benjamin Weyland, and John P. Burrows
EGUsphere, https://doi.org/10.5194/egusphere-2024-521, https://doi.org/10.5194/egusphere-2024-521, 2024
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This study explores the proportional relationships between carbonaceous aerosols (black and organic carbon) and trace gases using airborne measurements from two campaigns in Europe and East Asia. Differences between regions were found, but air quality models struggled to reproduce them accurately. We show that these proportional relationships can help to constrain models and can be used to infer aerosol concentrations from satellite observations of trace gases, especially in urban areas.
Tanja J. Schuck, Johannes Degen, Eric Hintsa, Peter Hoor, Markus Jesswein, Timo Keber, Daniel Kunkel, Fred Moore, Florian Obersteiner, Matt Rigby, Thomas Wagenhäuser, Luke M. Western, Andreas Zahn, and Andreas Engel
Atmos. Chem. Phys., 24, 689–705, https://doi.org/10.5194/acp-24-689-2024, https://doi.org/10.5194/acp-24-689-2024, 2024
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We study the interhemispheric gradient of sulfur hexafluoride (SF6), a strong long-lived greenhouse gas. Its emissions are stronger in the Northern Hemisphere; therefore, mixing ratios in the Southern Hemisphere lag behind. Comparing the observations to a box model, the model predicts air in the Southern Hemisphere to be older. For a better agreement, the emissions used as model input need to be increased (and their spatial pattern changed), and we need to modify north–south transport.
Yann Cohen, Didier Hauglustaine, Bastien Sauvage, Susanne Rohs, Patrick Konjari, Ulrich Bundke, Andreas Petzold, Valérie Thouret, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 23, 14973–15009, https://doi.org/10.5194/acp-23-14973-2023, https://doi.org/10.5194/acp-23-14973-2023, 2023
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The upper troposphere–lower stratosphere (UTLS) is a key region regarding the lower atmospheric composition. This study consists of a comprehensive evaluation of an up-to-date chemistry–climate model in this layer, using regular in situ measurements based on passenger aircraft. For this purpose, a specific software (Interpol-IAGOS) has been updated and made publicly available. The model reproduces the carbon monoxide peaks due to biomass burning over the continental tropics particularly well.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 23, 14127–14158, https://doi.org/10.5194/acp-23-14127-2023, https://doi.org/10.5194/acp-23-14127-2023, 2023
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In this study, we used a regional chemical transport model to characterize the different parameters of atmospheric oxidative capacity in recent chemical environments in China. These parameters include the production and destruction rates of ozone and other oxidants, the ozone production efficiency, the OH reactivity, and the length of the reaction chain responsible for the formation of ozone and ROx. They are also affected by the aerosol burden in the atmosphere.
Monali Borthakur, Miriam Sinnhuber, Alexandra Laeng, Thomas Reddmann, Peter Braesicke, Gabriele Stiller, Thomas von Clarmann, Bernd Funke, Ilya Usoskin, Jan Maik Wissing, and Olesya Yakovchuk
Atmos. Chem. Phys., 23, 12985–13013, https://doi.org/10.5194/acp-23-12985-2023, https://doi.org/10.5194/acp-23-12985-2023, 2023
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Reduced ozone levels resulting from ozone depletion mean more exposure to UV radiation, which has various effects on human health. We analysed solar events to see what influence it has on the chemistry of Earth's atmosphere and how this atmospheric chemistry change can affect the ozone. To do this, we used an atmospheric model considering only chemistry and compared it with satellite data. The focus was mainly on the contribution of chlorine, and we found about 10 %–20 % ozone loss due to that.
Frederik Harzer, Hella Garny, Felix Ploeger, Harald Bönisch, Peter Hoor, and Thomas Birner
Atmos. Chem. Phys., 23, 10661–10675, https://doi.org/10.5194/acp-23-10661-2023, https://doi.org/10.5194/acp-23-10661-2023, 2023
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We study the statistical relation between year-by-year fluctuations in winter-mean ozone and the strength of the stratospheric polar vortex. In the latitude–pressure plane, regression analysis shows that anomalously weak polar vortex years are associated with three pronounced local ozone maxima over the polar cap relative to the winter climatology. These response maxima primarily reflect the non-trivial combination of different ozone transport processes with varying relative contributions.
Midhun George, Maria Dolores Andrés Hernández, Vladyslav Nenakhov, Yangzhuoran Liu, John Philip Burrows, Birger Bohn, Eric Förster, Florian Obersteiner, Andreas Zahn, Theresa Harlaß, Helmut Ziereis, Hans Schlager, Benjamin Schreiner, Flora Kluge, Katja Bigge, and Klaus Pfeilsticker
Atmos. Chem. Phys., 23, 7799–7822, https://doi.org/10.5194/acp-23-7799-2023, https://doi.org/10.5194/acp-23-7799-2023, 2023
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The applicability of photostationary steady-state (PSS) assumptions to estimate the amount of the sum of peroxy radicals (RO2*) during the EMeRGe airborne observations from the known radical chemistry and onboard measurements of RO2* precursors, photolysis frequencies, and other trace gases such as NOx and O3 was investigated. The comparison of the calculated RO2* with the actual measurements provides an insight into the main processes controlling their concentration in the air masses measured.
Kun Qu, Xuesong Wang, Xuhui Cai, Yu Yan, Xipeng Jin, Mihalis Vrekoussis, Maria Kanakidou, Guy P. Brasseur, Jin Shen, Teng Xiao, Limin Zeng, and Yuanhang Zhang
Atmos. Chem. Phys., 23, 7653–7671, https://doi.org/10.5194/acp-23-7653-2023, https://doi.org/10.5194/acp-23-7653-2023, 2023
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Basic understandings of ozone processes, especially transport and chemistry, are essential to support ozone pollution control, but studies often have different views on their relative importance. We developed a method to quantify their contributions in the ozone mass and concentration budgets based on the WRF-CMAQ model. Results in a polluted region highlight the differences between two budgets. For future studies, two budgets are both needed to fully understand the effects of ozone processes.
Christian Scharun, Roland Ruhnke, and Peter Braesicke
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2023-91, https://doi.org/10.5194/gmd-2023-91, 2023
Publication in GMD not foreseen
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The identification and quantification of greenhouse gas (GHG) emissions is an important task for monitoring mitigation strategies under climate change. With RICHARD 1.0, we developed a novel approach using spatiotemporal proxy data and a selection algorithm to detect GHG emission hotspots. By using a one year dataset of global climate model output we showed that RICHARD is able to determine and quantify the source strengths of GHG emission hotspots much more precisely than conventional methods.
Luis F. Millán, Gloria L. Manney, Harald Boenisch, Michaela I. Hegglin, Peter Hoor, Daniel Kunkel, Thierry Leblanc, Irina Petropavlovskikh, Kaley Walker, Krzysztof Wargan, and Andreas Zahn
Atmos. Meas. Tech., 16, 2957–2988, https://doi.org/10.5194/amt-16-2957-2023, https://doi.org/10.5194/amt-16-2957-2023, 2023
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The determination of atmospheric composition trends in the upper troposphere and lower stratosphere (UTLS) is still highly uncertain. We present the creation of dynamical diagnostics to map several ozone datasets (ozonesondes, lidars, aircraft, and satellite measurements) in geophysically based coordinate systems. The diagnostics can also be used to analyze other greenhouse gases relevant to surface climate and UTLS chemistry.
Aliki Christodoulou, Iasonas Stavroulas, Mihalis Vrekoussis, Maximillien Desservettaz, Michael Pikridas, Elie Bimenyimana, Jonilda Kushta, Matic Ivančič, Martin Rigler, Philippe Goloub, Konstantina Oikonomou, Roland Sarda-Estève, Chrysanthos Savvides, Charbel Afif, Nikos Mihalopoulos, Stéphane Sauvage, and Jean Sciare
Atmos. Chem. Phys., 23, 6431–6456, https://doi.org/10.5194/acp-23-6431-2023, https://doi.org/10.5194/acp-23-6431-2023, 2023
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Our study presents, for the first time, a detailed source identification of aerosols at an urban background site in Cyprus (eastern Mediterranean), a region strongly impacted by climate change and air pollution. Here, we identify an unexpected high contribution of long-range transported pollution from fossil fuel sources in the Middle East, highlighting an urgent need to further characterize these fast-growing emissions and their impacts on regional atmospheric composition, climate, and health.
Brendan Byrne, David F. Baker, Sourish Basu, Michael Bertolacci, Kevin W. Bowman, Dustin Carroll, Abhishek Chatterjee, Frédéric Chevallier, Philippe Ciais, Noel Cressie, David Crisp, Sean Crowell, Feng Deng, Zhu Deng, Nicholas M. Deutscher, Manvendra K. Dubey, Sha Feng, Omaira E. García, David W. T. Griffith, Benedikt Herkommer, Lei Hu, Andrew R. Jacobson, Rajesh Janardanan, Sujong Jeong, Matthew S. Johnson, Dylan B. A. Jones, Rigel Kivi, Junjie Liu, Zhiqiang Liu, Shamil Maksyutov, John B. Miller, Scot M. Miller, Isamu Morino, Justus Notholt, Tomohiro Oda, Christopher W. O'Dell, Young-Suk Oh, Hirofumi Ohyama, Prabir K. Patra, Hélène Peiro, Christof Petri, Sajeev Philip, David F. Pollard, Benjamin Poulter, Marine Remaud, Andrew Schuh, Mahesh K. Sha, Kei Shiomi, Kimberly Strong, Colm Sweeney, Yao Té, Hanqin Tian, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, John R. Worden, Debra Wunch, Yuanzhi Yao, Jeongmin Yun, Andrew Zammit-Mangion, and Ning Zeng
Earth Syst. Sci. Data, 15, 963–1004, https://doi.org/10.5194/essd-15-963-2023, https://doi.org/10.5194/essd-15-963-2023, 2023
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Changes in the carbon stocks of terrestrial ecosystems result in emissions and removals of CO2. These can be driven by anthropogenic activities (e.g., deforestation), natural processes (e.g., fires) or in response to rising CO2 (e.g., CO2 fertilization). This paper describes a dataset of CO2 emissions and removals derived from atmospheric CO2 observations. This pilot dataset informs current capabilities and future developments towards top-down monitoring and verification systems.
Chuan-Yao Lin, Wan-Chin Chen, Yi-Yun Chien, Charles C. K. Chou, Chian-Yi Liu, Helmut Ziereis, Hans Schlager, Eric Förster, Florian Obersteiner, Ovid O. Krüger, Bruna A. Holanda, Mira L. Pöhlker, Katharina Kaiser, Johannes Schneider, Birger Bohn, Klaus Pfeilsticker, Benjamin Weyland, Maria Dolores Andrés Hernández, and John P. Burrows
Atmos. Chem. Phys., 23, 2627–2647, https://doi.org/10.5194/acp-23-2627-2023, https://doi.org/10.5194/acp-23-2627-2023, 2023
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During the EMeRGe campaign in Asia, atmospheric pollutants were measured on board the HALO aircraft. The WRF-Chem model was employed to evaluate the biomass burning (BB) plume transported from Indochina and its impact on the downstream areas. The combination of BB aerosol enhancement with cloud water resulted in a reduction in incoming shortwave radiation at the surface in southern China and the East China Sea, which potentially has significant regional climate implications.
Marios Chatziparaschos, Nikos Daskalakis, Stelios Myriokefalitakis, Nikos Kalivitis, Athanasios Nenes, María Gonçalves Ageitos, Montserrat Costa-Surós, Carlos Pérez García-Pando, Medea Zanoli, Mihalis Vrekoussis, and Maria Kanakidou
Atmos. Chem. Phys., 23, 1785–1801, https://doi.org/10.5194/acp-23-1785-2023, https://doi.org/10.5194/acp-23-1785-2023, 2023
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Ice formation is enabled by ice-nucleating particles (INP) at higher temperatures than homogeneous formation and can profoundly affect the properties of clouds. Our global model results show that K-feldspar is the most important contributor to INP concentrations globally, affecting mid-level mixed-phase clouds. However, quartz can significantly contribute and dominates the lowest and the highest altitudes of dust-derived INP, affecting mainly low-level and high-level mixed-phase clouds.
Ewa M. Bednarz, Daniele Visioni, Ben Kravitz, Andy Jones, James M. Haywood, Jadwiga Richter, Douglas G. MacMartin, and Peter Braesicke
Atmos. Chem. Phys., 23, 687–709, https://doi.org/10.5194/acp-23-687-2023, https://doi.org/10.5194/acp-23-687-2023, 2023
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Building on Part 1 of this two-part study, we demonstrate the role of biases in climatological circulation and specific aspects of model microphysics in driving the differences in simulated sulfate distributions amongst three Earth system models. We then characterize the simulated changes in stratospheric and free-tropospheric temperatures, ozone, water vapor, and large-scale circulation, elucidating the role of the above aspects in the surface responses discussed in Part 1.
Laura Tomsche, Andreas Marsing, Tina Jurkat-Witschas, Johannes Lucke, Stefan Kaufmann, Katharina Kaiser, Johannes Schneider, Monika Scheibe, Hans Schlager, Lenard Röder, Horst Fischer, Florian Obersteiner, Andreas Zahn, Martin Zöger, Jos Lelieveld, and Christiane Voigt
Atmos. Chem. Phys., 22, 15135–15151, https://doi.org/10.5194/acp-22-15135-2022, https://doi.org/10.5194/acp-22-15135-2022, 2022
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The detection of sulfur compounds in the upper troposphere (UT) and lower stratosphere (LS) is a challenge. In-flight measurements of SO2 and sulfate aerosol were performed during the BLUESKY mission in spring 2020 under exceptional atmospheric conditions. Reduced sinks in the dry UTLS and lower but still significant air traffic influenced the enhanced SO2 in the UT, and aged volcanic plumes enhanced the LS sulfate aerosol impacting the atmospheric radiation budget and global climate.
Paul Konopka, Mengchu Tao, Marc von Hobe, Lars Hoffmann, Corinna Kloss, Fabrizio Ravegnani, C. Michael Volk, Valentin Lauther, Andreas Zahn, Peter Hoor, and Felix Ploeger
Geosci. Model Dev., 15, 7471–7487, https://doi.org/10.5194/gmd-15-7471-2022, https://doi.org/10.5194/gmd-15-7471-2022, 2022
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Pure trajectory-based transport models driven by meteorology derived from reanalysis products (ERA5) take into account only the resolved, advective part of transport. That means neither mixing processes nor unresolved subgrid-scale advective processes like convection are included. The Chemical Lagrangian Model of the Stratosphere (CLaMS) includes these processes. We show that isentropic mixing dominates unresolved transport. The second most important transport process is unresolved convection.
Simon F. Reifenberg, Anna Martin, Matthias Kohl, Sara Bacer, Zaneta Hamryszczak, Ivan Tadic, Lenard Röder, Daniel J. Crowley, Horst Fischer, Katharina Kaiser, Johannes Schneider, Raphael Dörich, John N. Crowley, Laura Tomsche, Andreas Marsing, Christiane Voigt, Andreas Zahn, Christopher Pöhlker, Bruna A. Holanda, Ovid Krüger, Ulrich Pöschl, Mira Pöhlker, Patrick Jöckel, Marcel Dorf, Ulrich Schumann, Jonathan Williams, Birger Bohn, Joachim Curtius, Hardwig Harder, Hans Schlager, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 22, 10901–10917, https://doi.org/10.5194/acp-22-10901-2022, https://doi.org/10.5194/acp-22-10901-2022, 2022
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In this work we use a combination of observational data from an aircraft campaign and model results to investigate the effect of the European lockdown due to COVID-19 in spring 2020. Using model results, we show that the largest relative changes to the atmospheric composition caused by the reduced emissions are located in the upper troposphere around aircraft cruise altitude, while the largest absolute changes are present at the surface.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
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Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Yunsong Liu, Jean-Daniel Paris, Mihalis Vrekoussis, Panayiota Antoniou, Christos Constantinides, Maximilien Desservettaz, Christos Keleshis, Olivier Laurent, Andreas Leonidou, Carole Philippon, Panagiotis Vouterakos, Pierre-Yves Quéhé, Philippe Bousquet, and Jean Sciare
Atmos. Meas. Tech., 15, 4431–4442, https://doi.org/10.5194/amt-15-4431-2022, https://doi.org/10.5194/amt-15-4431-2022, 2022
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This paper details laboratory-based and field developments of a cost-effective and compacted UAV CO2 sensor system to address the challenge of measuring CO2 with sufficient precision and acquisition frequency. We assess its performance extensively through laboratory and field tests and provide a case study in an urban area (Nicosia, Cyprus). We therefore expect that this portable system will be widely used for measuring CO2 emission and distribution in natural or urban environments.
Zaneta T. Hamryszczak, Andrea Pozzer, Florian Obersteiner, Birger Bohn, Benedikt Steil, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 9483–9497, https://doi.org/10.5194/acp-22-9483-2022, https://doi.org/10.5194/acp-22-9483-2022, 2022
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Hydrogen peroxide plays a pivotal role in the chemistry of the atmosphere. Together with organic hydroperoxides, it forms a reservoir for peroxy radicals, which are known to be the key contributors to the self-cleaning processes of the atmosphere. Hydroperoxides were measured over Europe during the BLUESKY campaign in May–June 2020. The paper gives an overview of the distribution of the species in the troposphere and investigates the impact of wet scavenging and deposition on the budget of H2O2.
Stefan Noël, Maximilian Reuter, Michael Buchwitz, Jakob Borchardt, Michael Hilker, Oliver Schneising, Heinrich Bovensmann, John P. Burrows, Antonio Di Noia, Robert J. Parker, Hiroshi Suto, Yukio Yoshida, Matthias Buschmann, Nicholas M. Deutscher, Dietrich G. Feist, David W. T. Griffith, Frank Hase, Rigel Kivi, Cheng Liu, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, Christof Petri, David F. Pollard, Markus Rettinger, Coleen Roehl, Constantina Rousogenous, Mahesh Kumar Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Mihalis Vrekoussis, and Thorsten Warneke
Atmos. Meas. Tech., 15, 3401–3437, https://doi.org/10.5194/amt-15-3401-2022, https://doi.org/10.5194/amt-15-3401-2022, 2022
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We present a new version (v3) of the GOSAT and GOSAT-2 FOCAL products.
In addition to an increased number of XCO2 data, v3 also includes products for XCH4 (full-physics and proxy), XH2O and the relative ratio of HDO to H2O (δD). For GOSAT-2, we also present first XCO and XN2O results. All FOCAL data products show reasonable spatial distribution and temporal variations and agree well with TCCON. Global XN2O maps show a gradient from the tropics to higher latitudes on the order of 15 ppb.
Eric A. Ray, Elliot L. Atlas, Sue Schauffler, Sofia Chelpon, Laura Pan, Harald Bönisch, and Karen H. Rosenlof
Atmos. Chem. Phys., 22, 6539–6558, https://doi.org/10.5194/acp-22-6539-2022, https://doi.org/10.5194/acp-22-6539-2022, 2022
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The movement of air masses and the trace gases they contain from the Earth’s surface into the upper troposphere and lower stratosphere (UTLS) can have important implications for the radiative and chemical balance of the atmosphere. In this study we build on recent techniques and use new ones to estimate a range of transport diagnostics based on simultaneously measured trace gases in the UTLS during the monsoon season in North America.
Clara M. Nussbaumer, Andrea Pozzer, Ivan Tadic, Lenard Röder, Florian Obersteiner, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 22, 6151–6165, https://doi.org/10.5194/acp-22-6151-2022, https://doi.org/10.5194/acp-22-6151-2022, 2022
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The European COVID-19 lockdowns have significantly reduced the emission of primary pollutants such as NOx, which impacts the tropospheric photochemical processes and the abundance of O3. In this study, we present how the lockdowns have affected tropospheric trace gases and ozone production based on in situ observations and modeling simulations. We additionally show that the chemical regime shifted from a transition point to a NOx limitation in the upper troposphere.
M. Dolores Andrés Hernández, Andreas Hilboll, Helmut Ziereis, Eric Förster, Ovid O. Krüger, Katharina Kaiser, Johannes Schneider, Francesca Barnaba, Mihalis Vrekoussis, Jörg Schmidt, Heidi Huntrieser, Anne-Marlene Blechschmidt, Midhun George, Vladyslav Nenakhov, Theresa Harlass, Bruna A. Holanda, Jennifer Wolf, Lisa Eirenschmalz, Marc Krebsbach, Mira L. Pöhlker, Anna B. Kalisz Hedegaard, Linlu Mei, Klaus Pfeilsticker, Yangzhuoran Liu, Ralf Koppmann, Hans Schlager, Birger Bohn, Ulrich Schumann, Andreas Richter, Benjamin Schreiner, Daniel Sauer, Robert Baumann, Mariano Mertens, Patrick Jöckel, Markus Kilian, Greta Stratmann, Christopher Pöhlker, Monica Campanelli, Marco Pandolfi, Michael Sicard, José L. Gómez-Amo, Manuel Pujadas, Katja Bigge, Flora Kluge, Anja Schwarz, Nikos Daskalakis, David Walter, Andreas Zahn, Ulrich Pöschl, Harald Bönisch, Stephan Borrmann, Ulrich Platt, and John P. Burrows
Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, https://doi.org/10.5194/acp-22-5877-2022, 2022
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EMeRGe provides a unique set of in situ and remote sensing airborne measurements of trace gases and aerosol particles along selected flight routes in the lower troposphere over Europe. The interpretation uses also complementary collocated ground-based and satellite measurements. The collected data help to improve the current understanding of the complex spatial distribution of trace gases and aerosol particles resulting from mixing, transport, and transformation of pollution plumes over Europe.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Helmut Ziereis, Peter Hoor, Jens-Uwe Grooß, Andreas Zahn, Greta Stratmann, Paul Stock, Michael Lichtenstern, Jens Krause, Vera Bense, Armin Afchine, Christian Rolf, Wolfgang Woiwode, Marleen Braun, Jörn Ungermann, Andreas Marsing, Christiane Voigt, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Chem. Phys., 22, 3631–3654, https://doi.org/10.5194/acp-22-3631-2022, https://doi.org/10.5194/acp-22-3631-2022, 2022
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Airborne observations were conducted in the lowermost Arctic stratosphere during the winter of 2015/2016. The observed distribution of reactive nitrogen shows clear indications of nitrification in mid-winter and denitrification in late winter. This was caused by the formation of polar stratospheric cloud particles, which were observed during several flights. The sedimentation and evaporation of these particles and the descent of air masses cause a redistribution of reactive nitrogen.
Florian Haenel, Wolfgang Woiwode, Jennifer Buchmüller, Felix Friedl-Vallon, Michael Höpfner, Sören Johansson, Farahnaz Khosrawi, Oliver Kirner, Anne Kleinert, Hermann Oelhaf, Johannes Orphal, Roland Ruhnke, Björn-Martin Sinnhuber, Jörn Ungermann, Michael Weimer, and Peter Braesicke
Atmos. Chem. Phys., 22, 2843–2870, https://doi.org/10.5194/acp-22-2843-2022, https://doi.org/10.5194/acp-22-2843-2022, 2022
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We compare remote sensing observations of H2O, O3, HNO3 and clouds in the upper troposphere–lowermost stratosphere during an Arctic winter long-range research flight with simulations by two different state-of-the-art model systems. We find good agreement for dynamical structures, trace gas distributions and clouds. We investigate model biases and sensitivities, with the goal of aiding model development and improving our understanding of processes in the upper troposphere–lowermost stratosphere.
Thomas E. Taylor, Christopher W. O'Dell, David Crisp, Akhiko Kuze, Hannakaisa Lindqvist, Paul O. Wennberg, Abhishek Chatterjee, Michael Gunson, Annmarie Eldering, Brendan Fisher, Matthäus Kiel, Robert R. Nelson, Aronne Merrelli, Greg Osterman, Frédéric Chevallier, Paul I. Palmer, Liang Feng, Nicholas M. Deutscher, Manvendra K. Dubey, Dietrich G. Feist, Omaira E. García, David W. T. Griffith, Frank Hase, Laura T. Iraci, Rigel Kivi, Cheng Liu, Martine De Mazière, Isamu Morino, Justus Notholt, Young-Suk Oh, Hirofumi Ohyama, David F. Pollard, Markus Rettinger, Matthias Schneider, Coleen M. Roehl, Mahesh Kumar Sha, Kei Shiomi, Kimberly Strong, Ralf Sussmann, Yao Té, Voltaire A. Velazco, Mihalis Vrekoussis, Thorsten Warneke, and Debra Wunch
Earth Syst. Sci. Data, 14, 325–360, https://doi.org/10.5194/essd-14-325-2022, https://doi.org/10.5194/essd-14-325-2022, 2022
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We provide an analysis of an 11-year record of atmospheric carbon dioxide (CO2) concentrations derived using an optimal estimation retrieval algorithm on measurements made by the GOSAT satellite. The new product (version 9) shows improvement over the previous version (v7.3) as evaluated against independent estimates of CO2 from ground-based sensors and atmospheric inversion systems. We also compare the new GOSAT CO2 values to collocated estimates from NASA's Orbiting Carbon Observatory-2.
Paul D. Hamer, Virginie Marécal, Ryan Hossaini, Michel Pirre, Gisèle Krysztofiak, Franziska Ziska, Andreas Engel, Stephan Sala, Timo Keber, Harald Bönisch, Elliot Atlas, Kirstin Krüger, Martyn Chipperfield, Valery Catoire, Azizan A. Samah, Marcel Dorf, Phang Siew Moi, Hans Schlager, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 16955–16984, https://doi.org/10.5194/acp-21-16955-2021, https://doi.org/10.5194/acp-21-16955-2021, 2021
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Bromoform is a stratospheric ozone-depleting gas released by seaweed and plankton transported to the stratosphere via convection in the tropics. We study the chemical interactions of bromoform and its derivatives within convective clouds using a cloud-scale model and observations. Our findings are that soluble bromine gases are efficiently washed out and removed within the convective clouds and that most bromine is transported vertically to the upper troposphere in the form of bromoform.
Christopher J. Diekmann, Matthias Schneider, Benjamin Ertl, Frank Hase, Omaira García, Farahnaz Khosrawi, Eliezer Sepúlveda, Peter Knippertz, and Peter Braesicke
Earth Syst. Sci. Data, 13, 5273–5292, https://doi.org/10.5194/essd-13-5273-2021, https://doi.org/10.5194/essd-13-5273-2021, 2021
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The joint analysis of different stable water isotopes in water vapour is a powerful tool for investigating atmospheric moisture pathways. This paper presents a novel global and multi-annual dataset of H2O and HDO in mid-tropospheric water vapour by using data from the satellite sensor Metop/IASI. Due to its unique combination of coverage and resolution in space and time, this dataset is highly promising for studying the hydrological cycle and its representation in weather and climate models.
Yu-Wen Chen, Yi-Chun Chen, Charles C.-K. Chou, Hui-Ming Hung, Shih-Yu Chang, Lisa Eirenschmalz, Michael Lichtenstern, Helmut Ziereis, Hans Schlager, Greta Stratmann, Katharina Kaiser, Johannes Schneider, Stephan Borrmann, Florian Obersteiner, Eric Förster, Andreas Zahn, Wei-Nai Chen, Po-Hsiung Lin, Shuenn-Chin Chang, Maria Dolores Andrés Hernández, Pao-Kuan Wang, and John P. Burrows
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2021-788, https://doi.org/10.5194/acp-2021-788, 2021
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By presenting an approach using EMeRGe-Asia airborne field measurements and surface observations, this study shows that the fraction of OH reactivity due to SO2-OH reaction has a significant correlation with the sulfate concentration. Approximately 30 % of sulfate is produced by SO2-OH reaction. Our results underline the importance of SO2-OH gas-phase oxidation in sulfate formation, and demonstrate that the method can be applied to other regions and under different meteorological conditions.
Clara M. Nussbaumer, Uwe Parchatka, Ivan Tadic, Birger Bohn, Daniel Marno, Monica Martinez, Roland Rohloff, Hartwig Harder, Flora Kluge, Klaus Pfeilsticker, Florian Obersteiner, Martin Zöger, Raphael Doerich, John N. Crowley, Jos Lelieveld, and Horst Fischer
Atmos. Meas. Tech., 14, 6759–6776, https://doi.org/10.5194/amt-14-6759-2021, https://doi.org/10.5194/amt-14-6759-2021, 2021
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NO2 plays a central role in atmospheric photochemical processes and requires accurate measurements. This research presents NO2 data obtained via chemiluminescence using a photolytic converter from airborne studies around Cabo Verde and laboratory investigations. We show the limits and error-proneness of a conventional blue light converter in aircraft measurements affected by humidity and NO levels and suggest the use of an alternative quartz converter for more reliable results.
Meike K. Rotermund, Vera Bense, Martyn P. Chipperfield, Andreas Engel, Jens-Uwe Grooß, Peter Hoor, Tilman Hüneke, Timo Keber, Flora Kluge, Benjamin Schreiner, Tanja Schuck, Bärbel Vogel, Andreas Zahn, and Klaus Pfeilsticker
Atmos. Chem. Phys., 21, 15375–15407, https://doi.org/10.5194/acp-21-15375-2021, https://doi.org/10.5194/acp-21-15375-2021, 2021
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Airborne total bromine (Brtot) and tracer measurements suggest Brtot-rich air masses persistently protruded into the lower stratosphere (LS), creating a high Brtot region over the North Atlantic in fall 2017. The main source is via isentropic transport by the Asian monsoon and to a lesser extent transport across the extratropical tropopause as quantified by a Lagrange model. The transport of Brtot via Central American hurricanes is also observed. Lastly, the impact of Brtot on LS O3 is assessed.
Mahesh Kumar Sha, Bavo Langerock, Jean-François L. Blavier, Thomas Blumenstock, Tobias Borsdorff, Matthias Buschmann, Angelika Dehn, Martine De Mazière, Nicholas M. Deutscher, Dietrich G. Feist, Omaira E. García, David W. T. Griffith, Michel Grutter, James W. Hannigan, Frank Hase, Pauli Heikkinen, Christian Hermans, Laura T. Iraci, Pascal Jeseck, Nicholas Jones, Rigel Kivi, Nicolas Kumps, Jochen Landgraf, Alba Lorente, Emmanuel Mahieu, Maria V. Makarova, Johan Mellqvist, Jean-Marc Metzger, Isamu Morino, Tomoo Nagahama, Justus Notholt, Hirofumi Ohyama, Ivan Ortega, Mathias Palm, Christof Petri, David F. Pollard, Markus Rettinger, John Robinson, Sébastien Roche, Coleen M. Roehl, Amelie N. Röhling, Constantina Rousogenous, Matthias Schneider, Kei Shiomi, Dan Smale, Wolfgang Stremme, Kimberly Strong, Ralf Sussmann, Yao Té, Osamu Uchino, Voltaire A. Velazco, Corinne Vigouroux, Mihalis Vrekoussis, Pucai Wang, Thorsten Warneke, Tyler Wizenberg, Debra Wunch, Shoma Yamanouchi, Yang Yang, and Minqiang Zhou
Atmos. Meas. Tech., 14, 6249–6304, https://doi.org/10.5194/amt-14-6249-2021, https://doi.org/10.5194/amt-14-6249-2021, 2021
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This paper presents, for the first time, Sentinel-5 Precursor methane and carbon monoxide validation results covering a period from November 2017 to September 2020. For this study, we used global TCCON and NDACC-IRWG network data covering a wide range of atmospheric and surface conditions across different terrains. We also show the influence of a priori alignment, smoothing uncertainties and the sensitivity of the validation results towards the application of advanced co-location criteria.
Stefan F. Schreier, Tim Bösch, Andreas Richter, Kezia Lange, Michael Revesz, Philipp Weihs, Mihalis Vrekoussis, and Christoph Lotteraner
Atmos. Meas. Tech., 14, 5299–5318, https://doi.org/10.5194/amt-14-5299-2021, https://doi.org/10.5194/amt-14-5299-2021, 2021
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This paper reports on the evaluation of aerosol profiling products retrieved from ground-based MAX-DOAS instruments using the BOREAS algorithm. Aerosol extinction profiles, near-surface aerosol extinction, and aerosol optical depth are compared to measurements collected with ceilometer, sun photometer, and in situ instruments. We show that these MAX-DOAS aerosol profiling products provide useful information to study spatial and temporal variations above the urban area of Vienna.
Lukas Krasauskas, Jörn Ungermann, Peter Preusse, Felix Friedl-Vallon, Andreas Zahn, Helmut Ziereis, Christian Rolf, Felix Plöger, Paul Konopka, Bärbel Vogel, and Martin Riese
Atmos. Chem. Phys., 21, 10249–10272, https://doi.org/10.5194/acp-21-10249-2021, https://doi.org/10.5194/acp-21-10249-2021, 2021
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A Rossby wave (RW) breaking event was observed over the North Atlantic during the WISE measurement campaign in October 2017. Infrared limb sounding measurements of trace gases in the lower stratosphere, including high-resolution 3-D tomographic reconstruction, revealed complex spatial structures in stratospheric tracers near the polar jet related to previous RW breaking events. Backward-trajectory analysis and tracer correlations were used to study mixing and stratosphere–troposphere exchange.
Michael Weimer, Jennifer Buchmüller, Lars Hoffmann, Ole Kirner, Beiping Luo, Roland Ruhnke, Michael Steiner, Ines Tritscher, and Peter Braesicke
Atmos. Chem. Phys., 21, 9515–9543, https://doi.org/10.5194/acp-21-9515-2021, https://doi.org/10.5194/acp-21-9515-2021, 2021
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We show that we are able to directly simulate polar stratospheric clouds formed locally in a mountain wave and represent their effect on the ozone chemistry with the global atmospheric chemistry model ICON-ART. Thus, we show the first simulations that close the gap between directly resolved mountain-wave-induced polar stratospheric clouds and their representation at coarse global resolutions.
Romain Blot, Philippe Nedelec, Damien Boulanger, Pawel Wolff, Bastien Sauvage, Jean-Marc Cousin, Gilles Athier, Andreas Zahn, Florian Obersteiner, Dieter Scharffe, Hervé Petetin, Yasmine Bennouna, Hannah Clark, and Valérie Thouret
Atmos. Meas. Tech., 14, 3935–3951, https://doi.org/10.5194/amt-14-3935-2021, https://doi.org/10.5194/amt-14-3935-2021, 2021
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A lack of information about temporal changes in measurement uncertainties is an area of concern for long-term trend studies of the key compounds which have a direct or indirect impact on climate change. The IAGOS program has measured O3 and CO within the troposphere and lower stratosphere for more than 25 years. In this study, we demonstrated that the IAGOS database can be treated as one continuous program and is therefore appropriate for studies of long-term trends.
Ivan Tadic, Clara M. Nussbaumer, Birger Bohn, Hartwig Harder, Daniel Marno, Monica Martinez, Florian Obersteiner, Uwe Parchatka, Andrea Pozzer, Roland Rohloff, Martin Zöger, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 8195–8211, https://doi.org/10.5194/acp-21-8195-2021, https://doi.org/10.5194/acp-21-8195-2021, 2021
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Although mechanisms of tropospheric ozone (O3) formation are well understood, studies reporting on ozone formation derived from field measurements are challenging and remain sparse in number. We use airborne measurements to quantify nitric oxide (NO) and O3 distributions in the upper troposphere over the Atlantic Ocean and western Africa and compare our measurements to model simulations. Our results show that NO and ozone formation are greatest over the tropical areas of western Africa.
Clara M. Nussbaumer, Ivan Tadic, Dirk Dienhart, Nijing Wang, Achim Edtbauer, Lisa Ernle, Jonathan Williams, Florian Obersteiner, Isidoro Gutiérrez-Álvarez, Hartwig Harder, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 21, 7933–7945, https://doi.org/10.5194/acp-21-7933-2021, https://doi.org/10.5194/acp-21-7933-2021, 2021
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Lightning over continental and coastal areas is frequent and accompanied by deep convection, while lightning over marine areas and particularly in tropical cyclones is rare. This research presents in situ observations of the tropical storm Florence 2018 near Cabo Verde. We show the absence of lightning in the tropical storm despite the occurrence of deep convective processes by atmospheric trace gas measurements of O3, NO, CO, H2O2, DMS and CH2I.
Johannes Schneider, Ralf Weigel, Thomas Klimach, Antonis Dragoneas, Oliver Appel, Andreas Hünig, Sergej Molleker, Franziska Köllner, Hans-Christian Clemen, Oliver Eppers, Peter Hoppe, Peter Hoor, Christoph Mahnke, Martina Krämer, Christian Rolf, Jens-Uwe Grooß, Andreas Zahn, Florian Obersteiner, Fabrizio Ravegnani, Alexey Ulanovsky, Hans Schlager, Monika Scheibe, Glenn S. Diskin, Joshua P. DiGangi, John B. Nowak, Martin Zöger, and Stephan Borrmann
Atmos. Chem. Phys., 21, 989–1013, https://doi.org/10.5194/acp-21-989-2021, https://doi.org/10.5194/acp-21-989-2021, 2021
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During five aircraft missions, we detected aerosol particles containing meteoric material in the lower stratosphere. The stratospheric measurements span a latitude range from 15 to 68° N, and we find that at potential temperature levels of more than 40 K above the tropopause; particles containing meteoric material occur at similar abundance fractions across latitudes and seasons. We conclude that meteoric material is efficiently distributed between high and low latitudes by isentropic mixing.
Stelios Myriokefalitakis, Nikos Daskalakis, Angelos Gkouvousis, Andreas Hilboll, Twan van Noije, Jason E. Williams, Philippe Le Sager, Vincent Huijnen, Sander Houweling, Tommi Bergman, Johann Rasmus Nüß, Mihalis Vrekoussis, Maria Kanakidou, and Maarten C. Krol
Geosci. Model Dev., 13, 5507–5548, https://doi.org/10.5194/gmd-13-5507-2020, https://doi.org/10.5194/gmd-13-5507-2020, 2020
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This work documents and evaluates the detailed tropospheric gas-phase chemical mechanism MOGUNTIA in the three-dimensional chemistry transport model TM5-MP. The Rosenbrock solver, as generated by the KPP software, is implemented in the chemistry code, which can successfully replace the classical Euler backward integration method. The MOGUNTIA scheme satisfactorily simulates a large suite of oxygenated volatile organic compounds (VOCs) that are observed in the atmosphere at significant levels.
Bettina Hottmann, Sascha Hafermann, Laura Tomsche, Daniel Marno, Monica Martinez, Hartwig Harder, Andrea Pozzer, Marco Neumaier, Andreas Zahn, Birger Bohn, Greta Stratmann, Helmut Ziereis, Jos Lelieveld, and Horst Fischer
Atmos. Chem. Phys., 20, 12655–12673, https://doi.org/10.5194/acp-20-12655-2020, https://doi.org/10.5194/acp-20-12655-2020, 2020
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During OMO we observed enhanced mixing ratios of hydroperoxides (ROOH) in the Asian monsoon anticyclone (AMA) relative to the background. The observed mixing ratios are higher than steady-state calculations and EMAC simulations, especially in the AMA, indicating atmospheric transport of ROOH. Uncertainties in the scavenging efficiencies likely cause deviations from EMAC. Longitudinal gradients indicate a pool of ROOH towards the center of the AMA associated with upwind convection over India.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
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Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
Flora Kluge, Tilman Hüneke, Matthias Knecht, Michael Lichtenstern, Meike Rotermund, Hans Schlager, Benjamin Schreiner, and Klaus Pfeilsticker
Atmos. Chem. Phys., 20, 12363–12389, https://doi.org/10.5194/acp-20-12363-2020, https://doi.org/10.5194/acp-20-12363-2020, 2020
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The presented study reports on airborne measurements of formaldehyde, glyoxal, methylglyoxal, and CO over the Amazon basin and lays a special focus on the influence of biomass burning emissions on the atmospheric profiles of these carbonyl compounds within the planetary boundary layer as well as in the free and upper troposphere.
Hirofumi Ohyama, Isamu Morino, Voltaire A. Velazco, Theresa Klausner, Gerry Bagtasa, Matthäus Kiel, Matthias Frey, Akihiro Hori, Osamu Uchino, Tsuneo Matsunaga, Nicholas M. Deutscher, Joshua P. DiGangi, Yonghoon Choi, Glenn S. Diskin, Sally E. Pusede, Alina Fiehn, Anke Roiger, Michael Lichtenstern, Hans Schlager, Pao K. Wang, Charles C.-K. Chou, Maria Dolores Andrés-Hernández, and John P. Burrows
Atmos. Meas. Tech., 13, 5149–5163, https://doi.org/10.5194/amt-13-5149-2020, https://doi.org/10.5194/amt-13-5149-2020, 2020
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Column-averaged dry-air mole fractions of CO2 and CH4 measured by a solar viewing portable Fourier transform spectrometer (EM27/SUN) were validated with in situ profile data obtained during the transfer flights of two aircraft campaigns. Atmospheric dynamical properties based on ERA5 and WRF-Chem were used as criteria for selecting the best aircraft profiles for the validation. The resulting air-mass-independent correction factors for the EM27/SUN data were 0.9878 for CO2 and 0.9829 for CH4.
Cited articles
Amodio, M., de Gennaro, G., Marzocca, A., Trizio, L., and Tutino, M.:
Assessment of Impacts Produced by Anthropogenic Sources in a Little City
near an Important Industrial Area (Modugno, Southern Italy), Sci. World J.,
2013, 1–10, https://doi.org/10.1155/2013/150397, 2013.
Andrés Hernández, M. D., Hilboll, A., Ziereis, H., Förster, E., Krüger, O. O., Kaiser, K., Schneider, J., Barnaba, F., Vrekoussis, M., Schmidt, J., Huntrieser, H., Blechschmidt, A.-M., George, M., Nenakhov, V., Harlass, T., Holanda, B. A., Wolf, J., Eirenschmalz, L., Krebsbach, M., Pöhlker, M. L., Kalisz Hedegaard, A. B., Mei, L., Pfeilsticker, K., Liu, Y., Koppmann, R., Schlager, H., Bohn, B., Schumann, U., Richter, A., Schreiner, B., Sauer, D., Baumann, R., Mertens, M., Jöckel, P., Kilian, M., Stratmann, G., Pöhlker, C., Campanelli, M., Pandolfi, M., Sicard, M., Gómez-Amo, J. L., Pujadas, M., Bigge, K., Kluge, F., Schwarz, A., Daskalakis, N., Walter, D., Zahn, A., Pöschl, U., Bönisch, H., Borrmann, S., Platt, U., and Burrows, J. P.: Overview: On the transport and transformation of pollutants in the outflow of major population centres – observational data from the EMeRGe European intensive operational period in summer 2017, Atmos. Chem. Phys., 22, 5877–5924, https://doi.org/10.5194/acp-22-5877-2022, 2022.
Atkinson, R.: Atmospheric chemistry of VOCs and NOx, Atmos. Environ.,
34, 2063–2101, https://doi.org/10.1016/S1352-2310(99)00460-4, 2000.
Baklanov, A., Lawrence, M., Pandis, S., Mahura, A., Finardi, S., Moussiopoulos, N., Beekmann, M., Laj, P., Gomes, L., Jaffrezo, J.-L., Borbon, A., Coll, I., Gros, V., Sciare, J., Kukkonen, J., Galmarini, S., Giorgi, F., Grimmond, S., Esau, I., Stohl, A., Denby, B., Wagner, T., Butler, T., Baltensperger, U., Builtjes, P., van den Hout, D., van der Gon, H. D., Collins, B., Schluenzen, H., Kulmala, M., Zilitinkevich, S., Sokhi, R., Friedrich, R., Theloke, J., Kummer, U., Jalkinen, L., Halenka, T., Wiedensholer, A., Pyle, J., and Rossow, W. B.: MEGAPOLI: concept of multi-scale modelling of megacity impact on air quality and climate, Adv. Sci. Res., 4, 115–120, doi:10.5194/asr-4-115-2010, 2010.
Baklanov, A., Molina, L. T., and Gauss, M.: Megacities, air quality and
climate, Atmos. Environ., 126, 235–249, https://doi.org/10.1016/j.atmosenv.2015.11.059,
2016.
Brenninkmeijer, C. A. M., Crutzen, P., Boumard, F., Dauer, T., Dix, B., Ebinghaus, R., Filippi, D., Fischer, H., Franke, H., Frieβ, U., Heintzenberg, J., Helleis, F., Hermann, M., Kock, H. H., Koeppel, C., Lelieveld, J., Leuenberger, M., Martinsson, B. G., Miemczyk, S., Moret, H. P., Nguyen, H. N., Nyfeler, P., Oram, D., O'Sullivan, D., Penkett, S., Platt, U., Pupek, M., Ramonet, M., Randa, B., Reichelt, M., Rhee, T. S., Rohwer, J., Rosenfeld, K., Scharffe, D., Schlager, H., Schumann, U., Slemr, F., Sprung, D., Stock, P., Thaler, R., Valentino, F., van Velthoven, P., Waibel, A., Wandel, A., Waschitschek, K., Wiedensohler, A., Xueref-Remy, I., Zahn, A., Zech, U., and Ziereis, H.: Civil Aircraft for the regular investigation of the atmosphere based on an instrumented container: The new CARIBIC system, Atmos. Chem. Phys., 7, 4953–4976, https://doi.org/10.5194/acp-7-4953-2007, 2007.
Brito, J. and Zahn, A.: An unheated permeation device for calibrating atmospheric VOC measurements, Atmos. Meas. Tech., 4, 2143–2152, https://doi.org/10.5194/amt-4-2143-2011, 2011.
Cheng, Y., Lee, S. C., Huang, Y., Ho, K. F., Ho, S. S. H., Yau, P. S.,
Louie, P. K. K., and Zhang, R. J.: Diurnal and seasonal trends of carbonyl
compounds in roadside, urban, and suburban environment of Hong Kong, Atmos.
Environ., 89, 43–51, https://doi.org/10.1016/j.atmosenv.2014.02.014, 2014.
Ciccioli, P., Centritto, M., and Loreto, F.: Biogenic volatile organic
compound emissions from vegetation fires, Plant. Cell Environ., 37,
1810–1825, https://doi.org/10.1111/pce.12336, 2014.
Coggon, M. M., Veres, P. R., Yuan, B., Koss, A., Warneke, C., Gilman, J. B.,
Lerner, B. M., Peischl, J., Aikin, K. C., Stockwell, C. E., Hatch, L. E.,
Ryerson, T. B., Roberts, J. M., Yokelson, R. J., and de Gouw, J. A.:
Emissions of nitrogen-containing organic compounds from the burning of
herbaceous and arboraceous biomass: Fuel composition dependence and the
variability of commonly used nitrile tracers, Geophys. Res. Lett., 43,
9903–9912, https://doi.org/10.1002/2016GL070562, 2016.
Crippa, M., Guizzardi, D., Muntean, M., Schaaf, E., Monforti-Ferrario, F., Banja, M., Pagani, F., and Solazzo, E.: EDGAR v6.1 Global Air Pollutant Emissions, Eur. Comm. Jt. Res. Cent., [data set], https://data.jrc.ec.europa.eu/dataset/df521e05-6a3b-461c-965a-b703fb62313e (last access: 13 January 2023), 2022.
de Gouw, J. A. and Warneke, C.: Measurements of volatile organic compounds in
the earth's atmosphere using proton-transfer-reaction mass spectrometry,
Mass Spectrom. Rev., 26, 223–257, https://doi.org/10.1002/mas.20119, 2007.
de Gouw, J. A., Goldan, P. D., Warneke, C., Kuster, W. C., Roberts, J. M.,
Marchewka, M., Bertman, S. B., Pszenny, A. A. P., and Keene, W. C.:
Validation of proton transfer reaction-mass spectrometry (PTR-MS)
measurements of gas-phase organic compounds in the atmosphere during the New
England Air Quality Study (NEAQS) in 2002, J. Geophys. Res.-Atmos.,
108, 1–18, https://doi.org/10.1029/2003JD003863, 2003a.
de Gouw, J. A., Warneke, C., Karl, T., Eerdekens, G., Van der Veen, C., and
Fall, R.: Sensitivity and specificity of atmospheric trace gas detection by
proton-transfer-reaction mass spectrometry, Int. J. Mass Spectrom.,
223, 365–382, https://doi.org/10.1016/S1387-3806(02)00926-0, 2003b.
de Gouw, J. A., Welsh-Bon, D., Warneke, C., Kuster, W. C., Alexander, L., Baker, A. K., Beyersdorf, A. J., Blake, D. R., Canagaratna, M., Celada, A. T., Huey, L. G., Junkermann, W., Onasch, T. B., Salcido, A., Sjostedt, S. J., Sullivan, A. P., Tanner, D. J., Vargas, O., Weber, R. J., Worsnop, D. R., Yu, X. Y., and Zaveri, R.: Emission and chemistry of organic carbon in the gas and aerosol phase at a sub-urban site near Mexico City in March 2006 during the MILAGRO study, Atmos. Chem. Phys., 9, 3425–3442, https://doi.org/10.5194/acp-9-3425-2009, 2009.
ECMWF: Part IV: Physical Processes IFS Documentation – Cy47r1 Operational
implementation 30 June 2020 Part IV: Physical processes, June,
https://doi.org/10.21957/eyrpir4vj, 2020.
Fischbeck, G.: Mass-spectrometric in-situ measurements of atmospheric
volatile organic compounds onboard passenger and research aircraft, PhD, https://doi.org/10.5445/IR/1000085857, 2017.
Folberth, G. A., Rumbold, S. T., Collins, W. J., and Butler, T. M.: Global
radiative forcing and megacities, Urban Clim., 1, 4–19,
https://doi.org/10.1016/j.uclim.2012.08.001, 2012.
Folberth, G. A., Butler, T. M., Collins, W. J., and Rumbold, S. T.:
Megacities and climate change – A brief overview, Environ. Pollut., 203,
235–242, https://doi.org/10.1016/j.envpol.2014.09.004, 2015.
Gerbig, C., Kley, D., Volz-Thomas, A., Kent, J., Dewey, K., and McKenna, D.
S.: Fast response resonance fluorescence CO measurements aboard the C-130:
Instrument characterization and measurements made during North Atlantic
Regional Experiment 1993, J. Geophys. Res.-Atmos., 101, 29229–29238,
https://doi.org/10.1029/95jd03272, 1996.
Gerbig, C., Schmitgen, S., Kley, D., Volz-Thomas, A., Dewey, K., and Haaks,
D.: An improved fast-response vacuum-UV resonance fluorescence CO
instrument, J. Geophys. Res.-Atmos., 104, 1699–1704,
https://doi.org/10.1029/1998JD100031, 1999.
Guenther, A., Hewitt, C. N., Erickson, D., Fall, R., Geron, C., Graedel, T.,
Harley, P., Klinger, L., Lerdau, M., Mckay, W. A., Pierce, T., Scholes, B.,
Steinbrecher, R., Tallamraju, R., Taylor, J., and Zimmerman, P.: A global
model of natural volatile organic compound emissions, J. Geophys. Res.,
100, 8873, https://doi.org/10.1029/94JD02950, 1995.
Hersbach, H., Bell, B., Berrisford, P., Hirahara, S., Horányi, A.,
Muñoz-Sabater, J., Nicolas, J., Peubey, C., Radu, R., Schepers, D.,
Simmons, A., Soci, C., Abdalla, S., Abellan, X., Balsamo, G., Bechtold, P.,
Biavati, G., Bidlot, J., Bonavita, M., Chiara, G., Dahlgren, P., Dee, D.,
Diamantakis, M., Dragani, R., Flemming, J., Forbes, R., Fuentes, M., Geer,
A., Haimberger, L., Healy, S., Hogan, R. J., Hólm, E., Janisková,
M., Keeley, S., Laloyaux, P., Lopez, P., Lupu, C., Radnoti, G., Rosnay, P.,
Rozum, I., Vamborg, F., Villaume, S., and Thépaut, J.: The ERA5 global
reanalysis, Q. J. R. Meteorol. Soc., 146, 1999–2049,
https://doi.org/10.1002/qj.3803, 2020.
Hüneke, T., Aderhold, O.-A., Bounin, J., Dorf, M., Gentry, E., Grossmann, K., Grooß, J.-U., Hoor, P., Jöckel, P., Kenntner, M., Knapp, M., Knecht, M., Lörks, D., Ludmann, S., Matthes, S., Raecke, R., Reichert, M., Weimar, J., Werner, B., Zahn, A., Ziereis, H., and Pfeilsticker, K.: The novel HALO mini-DOAS instrument: inferring trace gas concentrations from airborne UV/visible limb spectroscopy under all skies using the scaling method, Atmos. Meas. Tech., 10, 4209–4234, https://doi.org/10.5194/amt-10-4209-2017, 2017.
Junge, C. E.: Residence time and variability of tropospheric trace gases,
Tellus, 26, 477–488, https://doi.org/10.3402/tellusa.v26i4.9853, 1974.
Karl, T., Striednig, M., Graus, M., Hammerle, A., and Wohlfahrt, G.: Urban
flux measurements reveal a large pool of oxygenated volatile organic
compound emissions, P. Natl. Acad. Sci. USA, 115, 1186–1191,
https://doi.org/10.1073/pnas.1714715115, 2018.
Khalil, M. A. K. and Rasmussen, R. A.: The global cycle of carbon monoxide:
Trends and mass balance, Chemosphere, 20, 227–242,
https://doi.org/10.1016/0045-6535(90)90098-E, 1990.
Klein Goldewijk, K., Beusen, A., Doelman, J., and Stehfest, E.: Anthropogenic land use estimates for the Holocene – HYDE 3.2, Earth Syst. Sci. Data, 9, 927–953, https://doi.org/10.5194/essd-9-927-2017, 2017.
Kulmala, M., Kokkonen, T. V., Pekkanen, J., Paatero, S., Petäjä, T., Kerminen, V.-M., and Ding, A.: Opinion: Gigacity – a source of problems or the new way to sustainable development, Atmos. Chem. Phys., 21, 8313–8322, https://doi.org/10.5194/acp-21-8313-2021, 2021.
Lindinger, W. and Jordan, A.: Proton-transfer-reaction mass spectrometry (PTR–MS): on-line monitoring of volatile organic compounds at pptv levels, Chem. Soc. Rev., 27, 347, doi:10.1039/a827347z, 1998.
Lindinger, W., Hansel, A., and Jordan, A.: On-line monitoring of volatile
organic compounds at pptv levels by means of Proton-Transfer-Reaction Mass
Spectrometry (PTR-MS) Medical applications, food control and environmental
research, Int. J. Mass Spectrom. Ion Process., 173, 191–241,
https://doi.org/10.1016/s0168-1176(97)00281-4, 1998.
Liu, H., Jacob, D. J., Bey, I., Yantosca, R. M., Duncan, B. N., and Sachse,
G. W.: Transport pathways for Asian pollution outflow over the Pacific:
Interannual and seasonal variations, J. Geophys. Res.-Atmos., 108,
https://doi.org/10.1029/2002jd003102, 2003.
Molina, M. J. and Molina, L. T.: Megacities and atmospheric pollution, J.
Air Waste Manag. Assoc., 54, 644–680,
https://doi.org/10.1080/10473289.2004.10470936, 2004.
Molina, L. T., Madronich, S., Gaffney, J. S., Apel, E., de Foy, B., Fast, J., Ferrare, R., Herndon, S., Jimenez, J. L., Lamb, B., Osornio-Vargas, A. R., Russell, P., Schauer, J. J., Stevens, P. S., Volkamer, R., and Zavala, M.: An overview of the MILAGRO 2006 Campaign: Mexico City emissions and their transport and transformation, Atmos. Chem. Phys., 10, 8697–8760, https://doi.org/10.5194/acp-10-8697-2010, 2010.
Müller, M., Anderson, B. E., Beyersdorf, A. J., Crawford, J. H., Diskin, G. S., Eichler, P., Fried, A., Keutsch, F. N., Mikoviny, T., Thornhill, K. L., Walega, J. G., Weinheimer, A. J., Yang, M., Yokelson, R. J., and Wisthaler, A.: In situ measurements and modeling of reactive trace gases in a small biomass burning plume, Atmos. Chem. Phys., 16, 3813–3824, https://doi.org/10.5194/acp-16-3813-2016, 2016.
NIST Chemistry WebBook: Experimental Proton Affinities,
https://doi.org/10.18434/T4D303, 2022.
re3data.org: HALO database, editing status 2021-11-17, re3data.org –
Registry of Research Data Repositories, [data set],
https://doi.org/10.17616/R39Q0T, 2021.
Savitzky, A. and Golay, M. J. E.: Smoothing and Differentiation of Data by
Simplified Least Squares Procedures., Anal. Chem., 36, 1627–1639,
https://doi.org/10.1021/ac60214a047, 1964.
Schumann, U.: Measurement and model data comparisons for the HALO-FAAM
formation flight during EMeRGe on 17 July 2017,
https://doi.org/10.5281/zenodo.4427965, 2021.
Seidel, D. J., Zhang, Y., Beljaars, A., Golaz, J. C., Jacobson, A. R., and
Medeiros, B.: Climatology of the planetary boundary layer over the
continental United States and Europe, J. Geophys. Res.-Atmos., 117,
1–15, https://doi.org/10.1029/2012JD018143, 2012.
Sindelarova, K., Granier, C., Bouarar, I., Guenther, A., Tilmes, S., Stavrakou, T., Müller, J.-F., Kuhn, U., Stefani, P., and Knorr, W.: Global data set of biogenic VOC emissions calculated by the MEGAN model over the last 30 years, Atmos. Chem. Phys., 14, 9317–9341, https://doi.org/10.5194/acp-14-9317-2014, 2014.
Stohl, A., Forster, C., Frank, A., Seibert, P., and Wotawa, G.: Technical note: The Lagrangian particle dispersion model FLEXPART version 6.2, Atmos. Chem. Phys., 5, 2461–2474, https://doi.org/10.5194/acp-5-2461-2005, 2005.
Stohl, A. and Seibert, P.: Accuracy of trajectories as determined from the
conservation of meteorological tracers, Q. J. Roy. Meteor. Soc., 124,
1465–1484, https://doi.org/10.1256/smsqj.54906, 1998.
Stohl, A., Wotawa, G., Seibert, P., and Kromp-Kolb, H.: Interpolation Errors
in Wind Fields as a Function of Spatial and Temporal Resolution and Their
Impact on Different Types of Kinematic Trajectories, J. Appl. Meteorol.,
34, 2149–2165, https://doi.org/10.1175/1520-0450(1995)034<2149:IEIWFA>2.0.CO;2, 1995.
United Nations: Department of Economic and Social Affairs, Population
Division: The World's Cities in 2018, World's Cities 2018 – Data Bookl.
(ST/ESA/SER.A/417), 34 pp., 2018.
United Nations: Department of Economic and Social Affairs, Population
Division: World Population Prospects 2019, Volume II: Demographic Profiles
(ST/ESA/SER.A/427), II, 1–5,
https://www.un.org/development/desa/publications/2018-revision-of-world-urbanization-prospects.html (last access: 13 January 2023), 2019.
Yuan, B., Koss, A. R., Warneke, C., Coggon, M., Sekimoto, K., and De Gouw, J.
A.: Proton-Transfer-Reaction Mass Spectrometry: Applications in Atmospheric
Sciences, Chem. Rev., 117, 13187–13229,
https://doi.org/10.1021/acs.chemrev.7b00325, 2017.
Zhu, T., Melamed, M., Parrish, D., Gauss, M., Klenner, L. G., Lawrence, M.,
Konare, A., and Liousse, C.: WMO/IGAC Impacts of Megacities on Air Pollution
and Climate, GAW Report., World Meteorological Organization,
https://library.wmo.int/index.php?lvl=notice_display&id=13474 (last access: 13 January 2023), 2012.
Short summary
The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas measurements. We combine measured volatile organic compounds (VOCs) with trajectory-modelled emission uptakes to identify potential source regions of pollution. We also characterise the chemical fingerprints (e.g. biomass burning and anthropogenic signatures) of the probed air masses to corroborate the contributing source regions. Our approach is the first large-scale study of VOCs originating from megacities.
The airborne megacity campaign EMeRGe provided an unprecedented amount of trace gas...
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