Articles | Volume 9, issue 11
https://doi.org/10.5194/amt-9-5265-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
https://doi.org/10.5194/amt-9-5265-2016
© Author(s) 2016. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
31 Oct 2016
Research article |
| 31 Oct 2016
A versatile, refrigerant- and cryogen-free cryofocusing–thermodesorption unit for preconcentration of traces gases in air
Florian Obersteiner
CORRESPONDING AUTHOR
Institute for Atmospheric and Environmental Science, Goethe
University Frankfurt, Frankfurt, Germany
Harald Bönisch
Institute of Meteorology and Climate Research, KIT, Karlsruhe,
Germany
Timo Keber
Institute for Atmospheric and Environmental Science, Goethe
University Frankfurt, Frankfurt, Germany
Simon O'Doherty
School of Chemistry, University of Bristol, Bristol, UK
Andreas Engel
Institute for Atmospheric and Environmental Science, Goethe
University Frankfurt, Frankfurt, Germany
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Rodrigo J. Seguel, Charlie Opazo, Yann Cohen, Owen R. Cooper, Laura Gallardo, Björn-Martin Sinnhuber, Florian Obersteiner, Andreas Zahn, Peter Hoor, and Susanne Rohs
EGUsphere, https://doi.org/10.5194/egusphere-2024-3719, https://doi.org/10.5194/egusphere-2024-3719, 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.
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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.
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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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
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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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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
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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
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Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 9, 179–194, https://doi.org/10.5194/amt-9-179-2016, https://doi.org/10.5194/amt-9-179-2016, 2016
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We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument, with focus on quantitative analysis of halocarbons in air samples. The applicability of the TOFMS technique, e.g. to form the basis of a "digital air archieve", is supported by the findings of this work: very high sensitivity, high measurement precision, a large dynamical range and an open data format which allows in-depth analysis of the data.
J. Hoker, F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 8, 2195–2206, https://doi.org/10.5194/amt-8-2195-2015, https://doi.org/10.5194/amt-8-2195-2015, 2015
Rodrigo J. Seguel, Charlie Opazo, Yann Cohen, Owen R. Cooper, Laura Gallardo, Björn-Martin Sinnhuber, Florian Obersteiner, Andreas Zahn, Peter Hoor, and Susanne Rohs
EGUsphere, https://doi.org/10.5194/egusphere-2024-3719, https://doi.org/10.5194/egusphere-2024-3719, 2024
This preprint is open for discussion and under review for Atmospheric Chemistry and Physics (ACP).
Short summary
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We explored differences in ozone levels between the Northern and Southern Hemispheres in the Stratosphere-troposphere exchange region. Using unique data from a research aircraft, we found significantly lower ozone levels (with stratospheric character) in the Southern Hemisphere, especially during years of severe ozone depletion. A Sudden Stratospheric Warming event in 2019 increased Southern Hemisphere ozone levels, highlighting the relationship between atmospheric events and ozone distribution.
Tanja J. Schuck, Johannes Degen, Timo Keber, Katharina Meixner, Thomas Wagenhäuser, Mélanie Ghysels, Georges Durry, Nadir Amarouche, Alessandro Zanchetta, Steven van Heuven, Huilin Chen, Johannes C. Laube, Sophie Baartman, Carina van der Veen, Maria Elena Popa, and Andreas Engel
EGUsphere, https://doi.org/10.5194/egusphere-2024-3279, https://doi.org/10.5194/egusphere-2024-3279, 2024
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A balloon was launched in 2021 in the Arctic to carry instruments for trace gase measurements up to 32 km. One purpose was to compare measurement techniques. We focus on the major greenhouse gases. To measure these, air was sampled with the AirCore technique and with flask sampling and analysed after the flight. In flight, observations were done with an optical method. In a companion paper we report on observations of chlorine and bromine containing trace gases.
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.
Patrick Konjari, Christian Rolf, Michaela Imelda Hegglin, Susanne Rohs, Yun Li, Andreas Zahn, Harald Bönisch, Martina Krämer, and Andreas Petzold
EGUsphere, https://doi.org/10.5194/egusphere-2024-2360, https://doi.org/10.5194/egusphere-2024-2360, 2024
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This study introduces a new method to deriving adjusted water vapor (H2O) climatologies for the upper tropopshere and lower statosphere (UT/LS) using data from 60,000 flights under the IAGOS program. Biases in the IAGOS water vapor dataset are adjusted, based on the more accurate IAGOS-CARIBIC data. The resulting highly resolved H2O climatologies will contribute to a better understanding of the H2O variability in the UT/LS and its connection to various transport and mixing processes.
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
EGUsphere, https://doi.org/10.5194/egusphere-2024-2117, https://doi.org/10.5194/egusphere-2024-2117, 2024
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We present a 17-year stratospheric age of air dataset derived from ACE-FTS satellite measurements of sulfur hexafluoride. This is the longest continuous, global, and vertically resolved age of air time series available to date. In this paper, we show that this dataset agrees well with age of air datasets based on measurements from other instruments. We also present trends in the midlatitude lower stratosphere that indicate changes in the global circulation that are predicted by climate models.
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.
Dafina Kikaj, Edward Chung, Alan D. Griffiths, Scott D. Chambers, Grant Foster, Angelina Wenger, Penelope Pickers, Chris Rennick, Simon O'Doherty, Joseph Pitt, Kieran Stanley, Dickon Young, Leigh S. Fleming, Karina Adcock, and Tim Arnold
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-54, https://doi.org/10.5194/amt-2024-54, 2024
Revised manuscript accepted for AMT
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We present a protocol to enhance confidence in reported atmospheric radon measurements, enabling direct comparisons between sites and integration with GHG measurements. Radon, a natural atmospheric tracer, provides an independent evaluation of transport model performance. The standardized approach ensures radon's use as a metric for model evaluation. Applicable beyond UK observatories, this protocol can benefit larger networks like ICOS or GAW, advancing atmospheric studies worldwide.
Felicia Kolonjari, Patrick E. Sheese, Kaley A. Walker, Chris D. Boone, David A. Plummer, Andreas Engel, Stephen A. Montzka, David E. Oram, Tanja Schuck, Gabriele P. Stiller, and Geoffrey C. Toon
Atmos. Meas. Tech., 17, 2429–2449, https://doi.org/10.5194/amt-17-2429-2024, https://doi.org/10.5194/amt-17-2429-2024, 2024
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The Canadian Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS) satellite instrument is currently providing the only vertically resolved chlorodifluoromethane (HCFC-22) measurements from space. This study assesses the most current ACE-FTS HCFC-22 data product in the upper troposphere and lower stratosphere, as well as modelled HCFC-22 from a 39-year run of the Canadian Middle Atmosphere Model (CMAM39) in the same region.
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.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
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We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
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The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
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.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
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The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
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.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
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Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
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.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
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Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
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.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
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Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
Thomas Wagenhäuser, Markus Jesswein, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 23, 3887–3903, https://doi.org/10.5194/acp-23-3887-2023, https://doi.org/10.5194/acp-23-3887-2023, 2023
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A common assumption to derive mean age from trace gas observations is that all air enters the stratosphere through the tropical tropopause. Using SF6 as an age tracer, this leads to negative mean age values close to the Northern Hemispheric extra-tropical tropopause. Our improved method also considers extra-tropical input into the stratosphere. More realistic values are derived using this method. Interhemispheric differences in mean age are found when comparing data from two aircraft campaigns.
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.
Eric Förster, Harald Bönisch, Marco Neumaier, Florian Obersteiner, Andreas Zahn, Andreas Hilboll, Anna B. Kalisz Hedegaard, Nikos Daskalakis, Alexandros Panagiotis Poulidis, Mihalis Vrekoussis, Michael Lichtenstern, and Peter Braesicke
Atmos. Chem. Phys., 23, 1893–1918, https://doi.org/10.5194/acp-23-1893-2023, https://doi.org/10.5194/acp-23-1893-2023, 2023
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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.
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.
Markus Jesswein, Rafael P. Fernandez, Lucas Berná, Alfonso Saiz-Lopez, Jens-Uwe Grooß, Ryan Hossaini, Eric C. Apel, Rebecca S. Hornbrook, Elliot L. Atlas, Donald R. Blake, Stephen Montzka, Timo Keber, Tanja Schuck, Thomas Wagenhäuser, and Andreas Engel
Atmos. Chem. Phys., 22, 15049–15070, https://doi.org/10.5194/acp-22-15049-2022, https://doi.org/10.5194/acp-22-15049-2022, 2022
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This study presents the global and seasonal distribution of the two major brominated short-lived substances CH2Br2 and CHBr3 in the upper troposphere and lower stratosphere based on observations from several aircraft campaigns. They show similar seasonality for both hemispheres, except in the respective hemispheric autumn lower stratosphere. A comparison with the TOMCAT and CAM-Chem models shows good agreement in the annual mean but larger differences in the seasonal consideration.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
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We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
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Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Marcel Zauner-Wieczorek, Martin Heinritzi, Manuel Granzin, Timo Keber, Andreas Kürten, Katharina Kaiser, Johannes Schneider, and Joachim Curtius
Atmos. Chem. Phys., 22, 11781–11794, https://doi.org/10.5194/acp-22-11781-2022, https://doi.org/10.5194/acp-22-11781-2022, 2022
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We present measurements of ambient ions in the free troposphere and lower stratosphere over Europe in spring 2020. We observed nitrate and hydrogen sulfate, amongst others. From their ratio, the number concentrations of gaseous sulfuric acid were inferred. Nitrate increased towards the stratosphere, whilst sulfuric acid was slightly decreased there. The average values for sulfuric acid were 1.9 to 7.8 × 105 cm-3. Protonated pyridine was identified in an altitude range of 4.6 to 8.5 km.
Praveen Kumar Pothapakula, Amelie Hoff, Anika Obermann-Hellhund, Timo Keber, and Bodo Ahrens
Earth Syst. Dynam. Discuss., https://doi.org/10.5194/esd-2022-24, https://doi.org/10.5194/esd-2022-24, 2022
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The Vb-cyclones simulated with a coupled regional climate model with two different driving data sets are compared against each other in historical period, thereafter the future climate predictions were analyzed. The Vb-cyclones in two simulations agree well in terms of their occurrence, intensity and track in two simulations, though there are discrepancies in seasonal cycles and their process linking Mediterranean Sea in historical period. So significant changes were observed in the future.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
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.
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.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
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.
Haklim Choi, Mi-Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, and Sunyoung Park
Atmos. Chem. Phys., 22, 5157–5173, https://doi.org/10.5194/acp-22-5157-2022, https://doi.org/10.5194/acp-22-5157-2022, 2022
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We observed 12-year continuous CH3Br pollution signals at Gosan and estimated anthropogenic CH3Br emissions in eastern China. The analysis revealed a significant discrepancy between top-down estimates and the bottom-up emissions from the fumigation usage reported to the United Nations Environment Programme, likely due to unreported or inaccurately reported fumigation usage. This result provides information to monitor international compliance with the Montreal Protocol.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
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Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
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.
Jens Mühle, Lambert J. M. Kuijpers, Kieran M. Stanley, Matthew Rigby, Luke M. Western, Jooil Kim, Sunyoung Park, Christina M. Harth, Paul B. Krummel, Paul J. Fraser, Simon O'Doherty, Peter K. Salameh, Roland Schmidt, Dickon Young, Ronald G. Prinn, Ray H. J. Wang, and Ray F. Weiss
Atmos. Chem. Phys., 22, 3371–3378, https://doi.org/10.5194/acp-22-3371-2022, https://doi.org/10.5194/acp-22-3371-2022, 2022
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Emissions of the strong greenhouse gas perfluorocyclobutane (c-C4F8) into the atmosphere have been increasing sharply since the early 2000s. These c-C4F8 emissions are highly correlated with the amount of hydrochlorofluorocarbon-22 produced to synthesize polytetrafluoroethylene (known for its non-stick properties) and related chemicals. From this process, c-C4F8 by-product is vented to the atmosphere. Avoiding these unnecessary c-C4F8 emissions could reduce the climate impact of this industry.
Dominique Rust, Ioannis Katharopoulos, Martin K. Vollmer, Stephan Henne, Simon O'Doherty, Daniel Say, Lukas Emmenegger, Renato Zenobi, and Stefan Reimann
Atmos. Chem. Phys., 22, 2447–2466, https://doi.org/10.5194/acp-22-2447-2022, https://doi.org/10.5194/acp-22-2447-2022, 2022
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Artificial halocarbons contribute to ozone layer depletion and to global warming. We measured the atmospheric concentrations of halocarbons at the Beromünster tower, modelled the Swiss emissions, and compared the results to the internationally reported Swiss emissions inventory. For most of the halocarbons, we found good agreement, whereas one refrigerant might be overestimated in the inventory. In addition, we present first emission estimates of the newest types of halocarbons.
Markus Jesswein, Heiko Bozem, Hans-Christoph Lachnitt, Peter Hoor, Thomas Wagenhäuser, Timo Keber, Tanja Schuck, and Andreas Engel
Atmos. Chem. Phys., 21, 17225–17241, https://doi.org/10.5194/acp-21-17225-2021, https://doi.org/10.5194/acp-21-17225-2021, 2021
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This study presents and compares inorganic chlorine (Cly) derived from observations with the HALO research aircraft in the Antarctic late winter–early fall 2019 and the Arctic winter 2015–2016. Trend-corrected correlations from the Northern Hemisphere show excellent agreement with those from the Southern Hemisphere. After observation allocation inside and outside the vortex based on N2O measurements, results of the two campaigns reveal substantial differences in Cly within the respective vortex.
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.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
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We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
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.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
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This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
Ruth E. Hill-Pearce, Aimee Hillier, Eric Mussell Webber, Kanokrat Charoenpornpukdee, Simon O'Doherty, Joachim Mohn, Christoph Zellweger, David R. Worton, and Paul J. Brewer
Atmos. Meas. Tech., 14, 5447–5458, https://doi.org/10.5194/amt-14-5447-2021, https://doi.org/10.5194/amt-14-5447-2021, 2021
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There is currently a need for gas reference materials with well-characterised delta values for monitoring N2O amount fractions. We present work towards the preparation of gas reference materials for calibration of in-field monitoring equipment, which target the WMO-GAW data quality objectives for comparability of amount fraction and demonstrate the stability of δ15Nα, δ15Nβ and δ18O values with pressure and effects of cylinder passivation.
Fides Lefrancois, Markus Jesswein, Markus Thoma, Andreas Engel, Kieran Stanley, and Tanja Schuck
Atmos. Meas. Tech., 14, 4669–4687, https://doi.org/10.5194/amt-14-4669-2021, https://doi.org/10.5194/amt-14-4669-2021, 2021
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Synthetic halocarbons can contribute to stratospheric ozone depletion or to climate change. In many applications they have been replaced over the last years. The presented non-target analysis shows an application approach to quantify those replacements retrospectively, using recorded data of air measurements with gas chromatography coupled to time-of-flight mass spectrometry. We focus on the retrospective analysis of the fourth-generation halocarbons, detected at Taunus Observatory in Germany.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412, https://doi.org/10.5194/acp-21-8393-2021, https://doi.org/10.5194/acp-21-8393-2021, 2021
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We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
Thomas Wagenhäuser, Andreas Engel, and Robert Sitals
Atmos. Meas. Tech., 14, 3923–3934, https://doi.org/10.5194/amt-14-3923-2021, https://doi.org/10.5194/amt-14-3923-2021, 2021
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AirCore samplers are increasingly deployed to weather balloons to collect continuous atmospheric samples. We introduce a technique that can be used in situ to evaluate different data processing methods that are required to derive vertical trace gas profiles from AirCore measurements after sample recovery. Results from two test flights with a specific AirCore configuration provide evidence for systematic deviations in altitude attribution for the upper levels, which can be empirically corrected.
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.
Daniel Say, Alistair J. Manning, Luke M. Western, Dickon Young, Adam Wisher, Matthew Rigby, Stefan Reimann, Martin K. Vollmer, Michela Maione, Jgor Arduini, Paul B. Krummel, Jens Mühle, Christina M. Harth, Brendan Evans, Ray F. Weiss, Ronald G. Prinn, and Simon O'Doherty
Atmos. Chem. Phys., 21, 2149–2164, https://doi.org/10.5194/acp-21-2149-2021, https://doi.org/10.5194/acp-21-2149-2021, 2021
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Perfluorocarbons (PFCs) are potent greenhouse gases with exceedingly long lifetimes. We used atmospheric measurements from a global monitoring network to track the accumulation of these gases in the atmosphere. In the case of the two most abundant PFCs, recent measurements indicate that global emissions are increasing. In Europe, we used a model to estimate regional PFC emissions. Our results show that there was no significant decline in northwest European PFC emissions between 2010 and 2019.
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.
Rachel L. Tunnicliffe, Anita L. Ganesan, Robert J. Parker, Hartmut Boesch, Nicola Gedney, Benjamin Poulter, Zhen Zhang, Jošt V. Lavrič, David Walter, Matthew Rigby, Stephan Henne, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 20, 13041–13067, https://doi.org/10.5194/acp-20-13041-2020, https://doi.org/10.5194/acp-20-13041-2020, 2020
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This study quantifies Brazil’s emissions of a potent atmospheric greenhouse gas, methane. This is in the field of atmospheric modelling and uses remotely sensed data and surface measurements of methane concentrations as well as an atmospheric transport model to interpret the data. Because of Brazil’s large emissions from wetlands, agriculture and biomass burning, these emissions affect global methane concentrations and thus are of global significance.
Martin Heinritzi, Lubna Dada, Mario Simon, Dominik Stolzenburg, Andrea C. Wagner, Lukas Fischer, Lauri R. Ahonen, Stavros Amanatidis, Rima Baalbaki, Andrea Baccarini, Paulus S. Bauer, Bernhard Baumgartner, Federico Bianchi, Sophia Brilke, Dexian Chen, Randall Chiu, Antonio Dias, Josef Dommen, Jonathan Duplissy, Henning Finkenzeller, Carla Frege, Claudia Fuchs, Olga Garmash, Hamish Gordon, Manuel Granzin, Imad El Haddad, Xucheng He, Johanna Helm, Victoria Hofbauer, Christopher R. Hoyle, Juha Kangasluoma, Timo Keber, Changhyuk Kim, Andreas Kürten, Houssni Lamkaddam, Tiia M. Laurila, Janne Lampilahti, Chuan Ping Lee, Katrianne Lehtipalo, Markus Leiminger, Huajun Mai, Vladimir Makhmutov, Hanna Elina Manninen, Ruby Marten, Serge Mathot, Roy Lee Mauldin, Bernhard Mentler, Ugo Molteni, Tatjana Müller, Wei Nie, Tuomo Nieminen, Antti Onnela, Eva Partoll, Monica Passananti, Tuukka Petäjä, Joschka Pfeifer, Veronika Pospisilova, Lauriane L. J. Quéléver, Matti P. Rissanen, Clémence Rose, Siegfried Schobesberger, Wiebke Scholz, Kay Scholze, Mikko Sipilä, Gerhard Steiner, Yuri Stozhkov, Christian Tauber, Yee Jun Tham, Miguel Vazquez-Pufleau, Annele Virtanen, Alexander L. Vogel, Rainer Volkamer, Robert Wagner, Mingyi Wang, Lena Weitz, Daniela Wimmer, Mao Xiao, Chao Yan, Penglin Ye, Qiaozhi Zha, Xueqin Zhou, Antonio Amorim, Urs Baltensperger, Armin Hansel, Markku Kulmala, António Tomé, Paul M. Winkler, Douglas R. Worsnop, Neil M. Donahue, Jasper Kirkby, and Joachim Curtius
Atmos. Chem. Phys., 20, 11809–11821, https://doi.org/10.5194/acp-20-11809-2020, https://doi.org/10.5194/acp-20-11809-2020, 2020
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With experiments performed at CLOUD, we show how isoprene interferes in monoterpene oxidation via RO2 termination at atmospherically relevant concentrations. This interference shifts the distribution of highly oxygenated organic molecules (HOMs) away from C20 class dimers towards C15 class dimers, which subsequently reduces both biogenic nucleation and early growth rates. Our results may help to understand the absence of new-particle formation in isoprene-rich environments.
Marius Hauck, Harald Bönisch, Peter Hoor, Timo Keber, Felix Ploeger, Tanja J. Schuck, and Andreas Engel
Atmos. Chem. Phys., 20, 8763–8785, https://doi.org/10.5194/acp-20-8763-2020, https://doi.org/10.5194/acp-20-8763-2020, 2020
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This study features an extended inversion method that includes transport across the extratropical tropopause to derive age spectra in the lowermost stratosphere from in situ trace gas measurements. The refined method is validated in a model setup and applied to data gained with the HALO research aircraft. Results are congruent with the findings of previous studies so that the method provides a promising toolset for the analysis of stratospheric dynamics based on observations in the future.
Frauke Fritsch, Hella Garny, Andreas Engel, Harald Bönisch, and Roland Eichinger
Atmos. Chem. Phys., 20, 8709–8725, https://doi.org/10.5194/acp-20-8709-2020, https://doi.org/10.5194/acp-20-8709-2020, 2020
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We test two methods to derive age of air as a diagnostic of the Brewer–Dobson circulation from non-linear increasing trace gases such as SF6 using a chemistry-climate model and observations. Both the model and the observations show systematic variation of the age of air trend dependent on the chosen assumptions that are required when deriving age of air from measurements. This provides insight into the differences in age of air trends of observations and models.
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623, https://doi.org/10.5194/essd-12-1561-2020, https://doi.org/10.5194/essd-12-1561-2020, 2020
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Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Moya L. Macdonald, Jemma L. Wadham, Dickon Young, Chris R. Lunder, Ove Hermansen, Guillaume Lamarche-Gagnon, and Simon O'Doherty
Atmos. Chem. Phys., 20, 7243–7258, https://doi.org/10.5194/acp-20-7243-2020, https://doi.org/10.5194/acp-20-7243-2020, 2020
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Climate change has caused glaciers in the Arctic to shrink, uncovering new soils. We used field measurements to study the exchange of a group of gases involved in ozone destruction, called halocarbons, between these new soils and the atmosphere. We found that mats of cyanobacteria, early colonisers of soils, are linked to a larger-than-expected exchange of halocarbons with the atmosphere. We also found that gases which are commonly thought to be marine in origin were released from these soils.
Luke M. Western, Zhe Sha, Matthew Rigby, Anita L. Ganesan, Alistair J. Manning, Kieran M. Stanley, Simon J. O'Doherty, Dickon Young, and Jonathan Rougier
Geosci. Model Dev., 13, 2095–2107, https://doi.org/10.5194/gmd-13-2095-2020, https://doi.org/10.5194/gmd-13-2095-2020, 2020
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Assessments of greenhouse gas emissions using atmospheric measurements and meteorological models, or
top-downmethods, are important to verify national inventories or produce a stand-alone estimate where no inventory exists. We present a novel top-down method to estimate emissions. This approach uses a fast method called an integrated nested Laplacian approximation to estimate how these emissions are correlated with other emissions in different locations and at different times.
Elise S. Droste, Karina E. Adcock, Matthew J. Ashfold, Charles Chou, Zoë Fleming, Paul J. Fraser, Lauren J. Gooch, Andrew J. Hind, Ray L. Langenfelds, Emma C. Leedham Elvidge, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Marios Panagi, Claire E. Reeves, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 20, 4787–4807, https://doi.org/10.5194/acp-20-4787-2020, https://doi.org/10.5194/acp-20-4787-2020, 2020
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We update the tropospheric trends and emissions of six perfluorocarbon (PFC) gases, including separate isomers. Trends for these strong greenhouse gases are still increasing, but at slower rates than previously. The lack of natural sinks results in the global accumulation of 833 million metric tonnes of CO2 equivalent for these six PFCs by 2017. Modelling results indicate potential source regions and types in East Asia, but we find that many emissions are unaccounted for in emission reports.
Timo Keber, Harald Bönisch, Carl Hartick, Marius Hauck, Fides Lefrancois, Florian Obersteiner, Akima Ringsdorf, Nils Schohl, Tanja Schuck, Ryan Hossaini, Phoebe Graf, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 20, 4105–4132, https://doi.org/10.5194/acp-20-4105-2020, https://doi.org/10.5194/acp-20-4105-2020, 2020
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In this paper we summarize observations of short-lived halocarbons in the tropopause region. We show that, especially during winter, the levels of short-lived bromine gases at the extratropical tropopause are higher than at the tropical tropopause. We discuss the impact of the distributions on stratospheric bromine levels and compare our observations to two models with four different emission scenarios.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
Angelina Wenger, Katherine Pugsley, Simon O'Doherty, Matt Rigby, Alistair J. Manning, Mark F. Lunt, and Emily D. White
Atmos. Chem. Phys., 19, 14057–14070, https://doi.org/10.5194/acp-19-14057-2019, https://doi.org/10.5194/acp-19-14057-2019, 2019
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We present 14CO2 observations at a background site in Ireland and a tall tower site in the UK. These data have been used to calculate the contribution of fossil fuel sources to atmospheric CO2 mole fractions from the UK and Ireland. 14CO2 emissions from nuclear industry sites in the UK cause a higher uncertainty in the results compared to observations in other locations. The observed ffCO2 at the site was not significantly different from simulated values based on the bottom-up inventory.
Maxime Prignon, Simon Chabrillat, Daniele Minganti, Simon O'Doherty, Christian Servais, Gabriele Stiller, Geoffrey C. Toon, Martin K. Vollmer, and Emmanuel Mahieu
Atmos. Chem. Phys., 19, 12309–12324, https://doi.org/10.5194/acp-19-12309-2019, https://doi.org/10.5194/acp-19-12309-2019, 2019
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Hydrochlorofluorocarbons (HCFCs) are the first, but temporary, substitution products for the strong ozone-depleting chlorofluorocarbons (CFCs). In this work, we present and validate an improved method to retrieve the most abundant HCFC in the atmosphere, allowing its evolution to be monitored independently in the troposphere and stratosphere. These kinds of contributions are fundamental for scrutinizing the fulfilment of the Montreal Protocol on Substances that Deplete the Ozone Layer.
Andreas Marsing, Tina Jurkat-Witschas, Jens-Uwe Grooß, Stefan Kaufmann, Romy Heller, Andreas Engel, Peter Hoor, Jens Krause, and Christiane Voigt
Atmos. Chem. Phys., 19, 10757–10772, https://doi.org/10.5194/acp-19-10757-2019, https://doi.org/10.5194/acp-19-10757-2019, 2019
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We study the partitioning of inorganic chlorine into active (ozone-depleting) and reservoir species in the lowermost stratosphere of the Arctic polar vortex, using novel in situ aircraft measurements in winter 2015/2016. We observe a change in recovery pathways of the reservoirs HCl and ClONO2 with increasing potential temperature. A comparison with the CLaMS model relates the observations to the vortex-wide evolution and confirms unresolved discrepancies in the mid-winter HCl distribution.
Ann R. Stavert, Simon O'Doherty, Kieran Stanley, Dickon Young, Alistair J. Manning, Mark F. Lunt, Christopher Rennick, and Tim Arnold
Atmos. Meas. Tech., 12, 4495–4518, https://doi.org/10.5194/amt-12-4495-2019, https://doi.org/10.5194/amt-12-4495-2019, 2019
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Under the UK GAUGE project, two new greenhouse gas observation sites were established in the 2013/2014 winter at two telecommunications towers. A combination of spectroscopic and chromatographic instrumentation was used to measure CO2, CH4, CO, N2O and SF6. The advantages and disadvantages of two CRDS sample drying strategies, Nafion(R) and empirical water correction, were also examined.
Jens Mühle, Cathy M. Trudinger, Luke M. Western, Matthew Rigby, Martin K. Vollmer, Sunyoung Park, Alistair J. Manning, Daniel Say, Anita Ganesan, L. Paul Steele, Diane J. Ivy, Tim Arnold, Shanlan Li, Andreas Stohl, Christina M. Harth, Peter K. Salameh, Archie McCulloch, Simon O'Doherty, Mi-Kyung Park, Chun Ok Jo, Dickon Young, Kieran M. Stanley, Paul B. Krummel, Blagoj Mitrevski, Ove Hermansen, Chris Lunder, Nikolaos Evangeliou, Bo Yao, Jooil Kim, Benjamin Hmiel, Christo Buizert, Vasilii V. Petrenko, Jgor Arduini, Michela Maione, David M. Etheridge, Eleni Michalopoulou, Mike Czerniak, Jeffrey P. Severinghaus, Stefan Reimann, Peter G. Simmonds, Paul J. Fraser, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 19, 10335–10359, https://doi.org/10.5194/acp-19-10335-2019, https://doi.org/10.5194/acp-19-10335-2019, 2019
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We discuss atmospheric concentrations and emissions of the strong greenhouse gas perfluorocyclobutane. A large fraction of recent emissions stem from China, India, and Russia, probably as a by-product from the production of fluoropolymers and fluorochemicals. Most historic emissions likely stem from developed countries. Total emissions are higher than what is being reported. Clearly, more measurements and better reporting are needed to understand emissions of this and other greenhouse gases.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Christina Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys., 19, 9865–9885, https://doi.org/10.5194/acp-19-9865-2019, https://doi.org/10.5194/acp-19-9865-2019, 2019
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Despite its emergence as a global economic power, very little information exists regarding India's halocarbon (CFC, HCFC, HFC and chlorocarbon) emissions. We report atmospheric measurements of these gases from above India, and use them to estimate India's emissions. Our results are consistent with the emissions profile of a developing country, with large emissions of HCFCs, HFCs and chlorocarbons not regulated under the Montreal Protocol, but little evidence for ongoing CFC consumption.
David D. Parrish, Richard G. Derwent, Simon O'Doherty, and Peter G. Simmonds
Atmos. Meas. Tech., 12, 3383–3394, https://doi.org/10.5194/amt-12-3383-2019, https://doi.org/10.5194/amt-12-3383-2019, 2019
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We present a flexible method that employs a power series expansion and Fourier series analysis to characterize the average long-term change and seasonal cycle, respectively, from a time series of observations of a trace atmospheric species. This approach maximizes the statistically significant information derived, including non-linear aspects of the long-term trends, without over fitting the data. Generally, a small set of parameter values (e.g., 7 or 8) provides this characterization.
Felix Ploeger, Bernard Legras, Edward Charlesworth, Xiaolu Yan, Mohamadou Diallo, Paul Konopka, Thomas Birner, Mengchu Tao, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 19, 6085–6105, https://doi.org/10.5194/acp-19-6085-2019, https://doi.org/10.5194/acp-19-6085-2019, 2019
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We analyse the change in the circulation of the middle atmosphere based on current generation meteorological reanalysis data sets. We find that long-term changes from 1989 to 2015 are similar for the chosen reanalyses, mainly resembling the forced response in climate model simulations to climate change. For shorter periods circulation changes are less robust, and the representation of decadal variability appears to be a major uncertainty for modelling the circulation of the middle atmosphere.
Marius Hauck, Frauke Fritsch, Hella Garny, and Andreas Engel
Atmos. Chem. Phys., 19, 5269–5291, https://doi.org/10.5194/acp-19-5269-2019, https://doi.org/10.5194/acp-19-5269-2019, 2019
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The paper presents a modified method to invert mixing ratios of chemically active tracers into stratospheric age spectra. It features an imposed seasonal cycle to include transport seasonality into the spectra. An idealized set of tracers from a model is used as proof of concept and results are in good agreement with the model reference, except for the lowermost stratosphere. Applicability is studied with focus on number of tracers and error tolerance, providing a starting point for future work.
Emily D. White, Matthew Rigby, Mark F. Lunt, T. Luke Smallman, Edward Comyn-Platt, Alistair J. Manning, Anita L. Ganesan, Simon O'Doherty, Ann R. Stavert, Kieran Stanley, Mathew Williams, Peter Levy, Michel Ramonet, Grant L. Forster, Andrew C. Manning, and Paul I. Palmer
Atmos. Chem. Phys., 19, 4345–4365, https://doi.org/10.5194/acp-19-4345-2019, https://doi.org/10.5194/acp-19-4345-2019, 2019
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Understanding carbon dioxide (CO2) fluxes from the terrestrial biosphere on a national scale is important for evaluating land use strategies to mitigate climate change. We estimate emissions of CO2 from the UK biosphere using atmospheric data in a top-down approach. Our findings show that bottom-up estimates from models of biospheric fluxes overestimate the amount of CO2 uptake in summer. This suggests these models wrongly estimate or omit key processes, e.g. land disturbance due to harvest.
Carole Helfter, Neil Mullinger, Massimo Vieno, Simon O'Doherty, Michel Ramonet, Paul I. Palmer, and Eiko Nemitz
Atmos. Chem. Phys., 19, 3043–3063, https://doi.org/10.5194/acp-19-3043-2019, https://doi.org/10.5194/acp-19-3043-2019, 2019
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We present a novel approach to estimate the annual budgets of carbon dioxide (881.0 ± 128.5 Tg) and methane (2.55 ± 0.48 Tg) of the British Isles from shipborne measurements taken over a 3-year period (2015–2017). This study brings independent verification of the emission budgets estimated using alternative products and investigates the seasonality of these emissions, which is usually not possible.
Daniel Say, Anita L. Ganesan, Mark F. Lunt, Matthew Rigby, Simon O'Doherty, Chris Harth, Alistair J. Manning, Paul B. Krummel, and Stephane Bauguitte
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1287, https://doi.org/10.5194/acp-2018-1287, 2019
Publication in ACP not foreseen
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India is a potentially significant source of chlorocarbons, gases typically used as solvents and feedstocks. Given the potential for these species to deplete stratospheric ozone, understanding their sources is important. We use flask measurements collected from an aircraft to infer India's chlorocarbon emissions. We link emissions of carbon tetrachloride to the industrial production of other chloromethanes, and provide evidence for rapid growth in India's emissions of dichloromethane.
Roland Eichinger, Simone Dietmüller, Hella Garny, Petr Šácha, Thomas Birner, Harald Bönisch, Giovanni Pitari, Daniele Visioni, Andrea Stenke, Eugene Rozanov, Laura Revell, David A. Plummer, Patrick Jöckel, Luke Oman, Makoto Deushi, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 19, 921–940, https://doi.org/10.5194/acp-19-921-2019, https://doi.org/10.5194/acp-19-921-2019, 2019
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To shed more light upon the changes in stratospheric circulation in the 21st century, climate projection simulations of 10 state-of-the-art global climate models, spanning from 1960 to 2100, are analyzed. The study shows that in addition to changes in transport, mixing also plays an important role in stratospheric circulation and that the properties of mixing vary over time. Furthermore, the influence of mixing is quantified and a dynamical framework is provided to understand the changes.
Sarah Connors, Alistair J. Manning, Andrew D. Robinson, Stuart N. Riddick, Grant L. Forster, Anita Ganesan, Aoife Grant, Stephen Humphrey, Simon O'Doherty, Dave E. Oram, Paul I. Palmer, Robert L. Skelton, Kieran Stanley, Ann Stavert, Dickon Young, and Neil R. P. Harris
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2018-1187, https://doi.org/10.5194/acp-2018-1187, 2018
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Methane is an important greenhouse gas & reducing its emissions is a vital part of climate change mitigation to limit global temperature increase to 1.5 °C or 2.0 °C. This paper explains a way to estimate emitted methane over a sub-national area by combining measurements & computer dispersion modelling in a so-called
inversiontechnique. Compared with the current national inventory, our results show lower emissions for Cambridgeshire, possibly due to waste sector emission differences.
Tanja J. Schuck, Fides Lefrancois, Franziska Gallmann, Danrong Wang, Markus Jesswein, Jesica Hoker, Harald Bönisch, and Andreas Engel
Atmos. Chem. Phys., 18, 16553–16569, https://doi.org/10.5194/acp-18-16553-2018, https://doi.org/10.5194/acp-18-16553-2018, 2018
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We present the first results of regular halocarbon measurements at Taunus Observatory, Germany. Halogenated gases contribute to stratospheric ozone depletion and to radiative forcing. Time-of-flight mass spectrometry allows one to assess a large number of compounds; the measurements are expected to provide better constraints for European emission estimates. CFC-11 and CFC-12 show small unexpected differences regarding outlier occurrence and seasonality, indicating ongoing emissions of CFC-11.
Simon Chabrillat, Corinne Vigouroux, Yves Christophe, Andreas Engel, Quentin Errera, Daniele Minganti, Beatriz M. Monge-Sanz, Arjo Segers, and Emmanuel Mahieu
Atmos. Chem. Phys., 18, 14715–14735, https://doi.org/10.5194/acp-18-14715-2018, https://doi.org/10.5194/acp-18-14715-2018, 2018
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Mean age of stratospheric air is computed for the period 1989–2015 with a kinematic transport model which uses surface pressure and wind fields from five reanalyses: ERA-I, MERRA-2, MERRA, CFSR, JRA-55. The spread between the resulting datasets is as large as in climate model intercomparisons; the age trends have large disagreement and depend strongly on the considered period. We highlight the need for similar studies using diabatic transport models which also use temperature and heating rates.
Tim Arnold, Alistair J. Manning, Jooil Kim, Shanlan Li, Helen Webster, David Thomson, Jens Mühle, Ray F. Weiss, Sunyoung Park, and Simon O'Doherty
Atmos. Chem. Phys., 18, 13305–13320, https://doi.org/10.5194/acp-18-13305-2018, https://doi.org/10.5194/acp-18-13305-2018, 2018
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Emissions of carbon tetrafluoride CF4, NF3 and CHF3 in east Asia have been calculated using atmospheric measurements and an atmospheric transport model. We calculate emissions of CF4 to be quite constant between the years 2008 and 2015 for both China and South Korea, with 2015 emissions calculated at 4.33 ± 2.65 Gg yr-1 and 0.36 ± 0.11 Gg yr-1, respectively. Emission estimates of NF3 from South Korea could be made with relatively small uncertainty at 0.6 ± 0.07 Gg yr-1 in 2015.
Franz Slemr, Andreas Weigelt, Ralf Ebinghaus, Johannes Bieser, Carl A. M. Brenninkmeijer, Armin Rauthe-Schöch, Markus Hermann, Bengt G. Martinsson, Peter van Velthoven, Harald Bönisch, Marco Neumaier, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 18, 12329–12343, https://doi.org/10.5194/acp-18-12329-2018, https://doi.org/10.5194/acp-18-12329-2018, 2018
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Total and elemental mercury were measured in the upper troposphere and lower stratosphere onboard a passenger aircraft. Their concentrations in the upper troposphere were comparable implying low concentrations of oxidized mercury in this region. Large scale seasonally dependent influence of emissions from biomass burning was also observed. Their distributions in the lower stratosphere implies a long stratospheric lifetime, which precludes significant mercury oxidation by ozone.
Sunyoung Park, Shanlan Li, Jens Mühle, Simon O'Doherty, Ray F. Weiss, Xuekun Fang, Stefan Reimann, and Ronald G. Prinn
Atmos. Chem. Phys., 18, 11729–11738, https://doi.org/10.5194/acp-18-11729-2018, https://doi.org/10.5194/acp-18-11729-2018, 2018
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Multi-year, real-time atmospheric carbon tetrachloride (CCl4) record obtained at Gosan station (33° N, 126° E) presents evidence of significant unreported emissions of this first-generation ozone-depleting substance. The missing emissions (~ 19 Gg yr−1) for China contribute to approximately 54 % of global emissions and are most likely related to CCl4 escape occurring during the production of chlorinated compounds and their usage as feedstocks and process agents in chemical manufacturing industries.
Sören Johansson, Wolfgang Woiwode, Michael Höpfner, Felix Friedl-Vallon, Anne Kleinert, Erik Kretschmer, Thomas Latzko, Johannes Orphal, Peter Preusse, Jörn Ungermann, Michelle L. Santee, Tina Jurkat-Witschas, Andreas Marsing, Christiane Voigt, Andreas Giez, Martina Krämer, Christian Rolf, Andreas Zahn, Andreas Engel, Björn-Martin Sinnhuber, and Hermann Oelhaf
Atmos. Meas. Tech., 11, 4737–4756, https://doi.org/10.5194/amt-11-4737-2018, https://doi.org/10.5194/amt-11-4737-2018, 2018
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We present two-dimensional cross sections of temperature, HNO3, O3, ClONO2, H2O and CFC-12 from measurements of the GLORIA infrared limb imager during the POLSTRACC/GW-LCYCLE/SALSA aircraft campaigns in the Arctic winter 2015/2016. GLORIA sounded the atmosphere between 5 and 14 km with vertical resolutions of 0.4–1 km. Estimated errors are in the range of 1–2 K (temperature) and 10 %–20 % (trace gases). Comparisons to in situ instruments onboard the aircraft and to Aura/MLS are shown.
Ronald G. Prinn, Ray F. Weiss, Jgor Arduini, Tim Arnold, H. Langley DeWitt, Paul J. Fraser, Anita L. Ganesan, Jimmy Gasore, Christina M. Harth, Ove Hermansen, Jooil Kim, Paul B. Krummel, Shanlan Li, Zoë M. Loh, Chris R. Lunder, Michela Maione, Alistair J. Manning, Ben R. Miller, Blagoj Mitrevski, Jens Mühle, Simon O'Doherty, Sunyoung Park, Stefan Reimann, Matt Rigby, Takuya Saito, Peter K. Salameh, Roland Schmidt, Peter G. Simmonds, L. Paul Steele, Martin K. Vollmer, Ray H. Wang, Bo Yao, Yoko Yokouchi, Dickon Young, and Lingxi Zhou
Earth Syst. Sci. Data, 10, 985–1018, https://doi.org/10.5194/essd-10-985-2018, https://doi.org/10.5194/essd-10-985-2018, 2018
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We present the data and accomplishments of the multinational global atmospheric measurement program AGAGE (Advanced Global Atmospheric Gases Experiment). At high frequency and at multiple sites, AGAGE measures all the important chemicals in the Montreal Protocol for the protection of the ozone layer and the non-carbon-dioxide gases assessed by the Intergovernmental Panel on Climate Change. AGAGE uses these data to estimate sources and sinks of all these gases and has operated since 1978.
Simone Dietmüller, Roland Eichinger, Hella Garny, Thomas Birner, Harald Boenisch, Giovanni Pitari, Eva Mancini, Daniele Visioni, Andrea Stenke, Laura Revell, Eugene Rozanov, David A. Plummer, John Scinocca, Patrick Jöckel, Luke Oman, Makoto Deushi, Shibata Kiyotaka, Douglas E. Kinnison, Rolando Garcia, Olaf Morgenstern, Guang Zeng, Kane Adam Stone, and Robyn Schofield
Atmos. Chem. Phys., 18, 6699–6720, https://doi.org/10.5194/acp-18-6699-2018, https://doi.org/10.5194/acp-18-6699-2018, 2018
Jens Krause, Peter Hoor, Andreas Engel, Felix Plöger, Jens-Uwe Grooß, Harald Bönisch, Timo Keber, Björn-Martin Sinnhuber, Wolfgang Woiwode, and Hermann Oelhaf
Atmos. Chem. Phys., 18, 6057–6073, https://doi.org/10.5194/acp-18-6057-2018, https://doi.org/10.5194/acp-18-6057-2018, 2018
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We present tracer measurements of CO and N2O measured during the POLSTRACC aircraft campaign in winter 2015–2016. We found enhanced CO values relative to N2O in the polar lower stratosphere in addition to the ageing of this region during winter. By using model simulations it was possible to link this enhancement to an increased mixing of the tropical tropopause. We thus conclude that the polar lower stratosphere in late winter is strongly influenced by quasi-isentropic mixing from the tropics.
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Martin K. Vollmer, Stephan Henne, Jens Mühle, Simon O'Doherty, Alistair J. Manning, Paul B. Krummel, Paul J. Fraser, Dickon Young, Ray F. Weiss, Peter K. Salameh, Christina M. Harth, Stefan Reimann, Cathy M. Trudinger, L. Paul Steele, Ray H. J. Wang, Diane J. Ivy, Ronald G. Prinn, Blagoj Mitrevski, and David M. Etheridge
Atmos. Chem. Phys., 18, 4153–4169, https://doi.org/10.5194/acp-18-4153-2018, https://doi.org/10.5194/acp-18-4153-2018, 2018
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Recent measurements of the potent greenhouse gas HFC-23, a by-product of HCFC-22 production, show a 28 % increase in the atmospheric mole fraction from 2009 to 2016. A minimum in the atmospheric abundance of HFC-23 in 2009 was attributed to abatement of HFC-23 emissions by incineration under the Clean Development Mechanism (CDM). Our results indicate that the recent increase in HFC-23 emissions is driven by failure of mitigation under the CDM to keep pace with increased HCFC-22 production.
Fabian Schoenenberger, Stephan Henne, Matthias Hill, Martin K. Vollmer, Giorgos Kouvarakis, Nikolaos Mihalopoulos, Simon O'Doherty, Michela Maione, Lukas Emmenegger, Thomas Peter, and Stefan Reimann
Atmos. Chem. Phys., 18, 4069–4092, https://doi.org/10.5194/acp-18-4069-2018, https://doi.org/10.5194/acp-18-4069-2018, 2018
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Anthropogenic halocarbon emissions contribute to stratospheric ozone depletion and global warming. We measured atmospheric halocarbons for 6 months on Crete to extend the coverage of the existing observation network to the Eastern Mediterranean. The derived emission estimates showed a contribution of 16.8 % (13.6–23.3 %) and 53.2 % (38.1–84.2 %) of this region to the total HFC and HCFC emissions of the analyzed European domain and a reduction of the underlying uncertainties by 40–80 %.
Kieran M. Stanley, Aoife Grant, Simon O'Doherty, Dickon Young, Alistair J. Manning, Ann R. Stavert, T. Gerard Spain, Peter K. Salameh, Christina M. Harth, Peter G. Simmonds, William T. Sturges, David E. Oram, and Richard G. Derwent
Atmos. Meas. Tech., 11, 1437–1458, https://doi.org/10.5194/amt-11-1437-2018, https://doi.org/10.5194/amt-11-1437-2018, 2018
Emma C. Leedham Elvidge, Harald Bönisch, Carl A. M. Brenninkmeijer, Andreas Engel, Paul J. Fraser, Eileen Gallacher, Ray Langenfelds, Jens Mühle, David E. Oram, Eric A. Ray, Anna R. Ridley, Thomas Röckmann, William T. Sturges, Ray F. Weiss, and Johannes C. Laube
Atmos. Chem. Phys., 18, 3369–3385, https://doi.org/10.5194/acp-18-3369-2018, https://doi.org/10.5194/acp-18-3369-2018, 2018
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Chemical species measured in stratospheric air can be used as proxies for stratospheric circulation changes which cannot be measured directly. A range of tracers is important to understand changing stratospheric dynamics. We demonstrate the suitability of PFCs and HFCs as tracers and support recent work that reduces the current stratospheric lifetime of SF6. Updates to policy-relevant parameters (e.g. stratospheric lifetime) linked to this change are provided for O3-depleting substances.
Peter Bergamaschi, Ute Karstens, Alistair J. Manning, Marielle Saunois, Aki Tsuruta, Antoine Berchet, Alexander T. Vermeulen, Tim Arnold, Greet Janssens-Maenhout, Samuel Hammer, Ingeborg Levin, Martina Schmidt, Michel Ramonet, Morgan Lopez, Jost Lavric, Tuula Aalto, Huilin Chen, Dietrich G. Feist, Christoph Gerbig, László Haszpra, Ove Hermansen, Giovanni Manca, John Moncrieff, Frank Meinhardt, Jaroslaw Necki, Michal Galkowski, Simon O'Doherty, Nina Paramonova, Hubertus A. Scheeren, Martin Steinbacher, and Ed Dlugokencky
Atmos. Chem. Phys., 18, 901–920, https://doi.org/10.5194/acp-18-901-2018, https://doi.org/10.5194/acp-18-901-2018, 2018
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European methane (CH4) emissions are estimated for 2006–2012 using atmospheric in situ measurements from 18 European monitoring stations and 7 different inverse models. Our analysis highlights the potential significant contribution of natural emissions from wetlands (including peatlands and wet soils) to the total European emissions. The top-down estimates of total EU-28 CH4 emissions are broadly consistent with the sum of reported anthropogenic CH4 emissions and the estimated natural emissions.
Martin K. Vollmer, Dickon Young, Cathy M. Trudinger, Jens Mühle, Stephan Henne, Matthew Rigby, Sunyoung Park, Shanlan Li, Myriam Guillevic, Blagoj Mitrevski, Christina M. Harth, Benjamin R. Miller, Stefan Reimann, Bo Yao, L. Paul Steele, Simon A. Wyss, Chris R. Lunder, Jgor Arduini, Archie McCulloch, Songhao Wu, Tae Siek Rhee, Ray H. J. Wang, Peter K. Salameh, Ove Hermansen, Matthias Hill, Ray L. Langenfelds, Diane Ivy, Simon O'Doherty, Paul B. Krummel, Michela Maione, David M. Etheridge, Lingxi Zhou, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Peter G. Simmonds
Atmos. Chem. Phys., 18, 979–1002, https://doi.org/10.5194/acp-18-979-2018, https://doi.org/10.5194/acp-18-979-2018, 2018
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We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere because they are important in stratospheric ozone depletion. These compounds should have decreased in the atmosphere because they are banned by the Montreal Protocol but we find the opposite. Emissions over the last decade have not declined on a global scale. We use inverse modeling and our observations to find that a large part of the emissions originate in the Asian region.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756, https://doi.org/10.5194/acp-18-735-2018, https://doi.org/10.5194/acp-18-735-2018, 2018
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This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Andreas Engel, Harald Bönisch, Jennifer Ostermöller, Martyn P. Chipperfield, Sandip Dhomse, and Patrick Jöckel
Atmos. Chem. Phys., 18, 601–619, https://doi.org/10.5194/acp-18-601-2018, https://doi.org/10.5194/acp-18-601-2018, 2018
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We present a new method to derive equivalent effective stratospheric chlorine (EESC), which is based on an improved formulation of the propagation of trends of species with chemical loss from the troposphere to the stratosphere. EESC calculated with the new method shows much better agreement with model-derived ESC. Based on this new formulation, we expect the halogen impact on midlatitude stratospheric ozone to return to 1980 values about 10 years later, then using the current formulation.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Ray Weiss, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Atmos. Chem. Phys., 17, 11135–11161, https://doi.org/10.5194/acp-17-11135-2017, https://doi.org/10.5194/acp-17-11135-2017, 2017
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Following the Global Methane Budget 2000–2012 published in Saunois et al. (2016), we use the same dataset of bottom-up and top-down approaches to discuss the variations in methane emissions over the period 2000–2012. The changes in emissions are discussed both in terms of trends and quasi-decadal changes. The ensemble gathered here allows us to synthesise the robust changes in terms of regional and sectorial contributions to the increasing methane emissions.
Dominik Brunner, Tim Arnold, Stephan Henne, Alistair Manning, Rona L. Thompson, Michela Maione, Simon O'Doherty, and Stefan Reimann
Atmos. Chem. Phys., 17, 10651–10674, https://doi.org/10.5194/acp-17-10651-2017, https://doi.org/10.5194/acp-17-10651-2017, 2017
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Hydrofluorocarbons (HFCs) and SF6 are industrially produced gases with a large greenhouse-gas warming potential. In this study, we estimated the emissions of HFCs and SF6 over Europe by combining measurements at three background stations with four different model systems. We identified significant differences between our estimates and nationally reported numbers, but also found that the network of only three sites in Europe is insufficient to reliably attribute emissions to individual countries.
Ellen Eckert, Thomas von Clarmann, Alexandra Laeng, Gabriele P. Stiller, Bernd Funke, Norbert Glatthor, Udo Grabowski, Sylvia Kellmann, Michael Kiefer, Andrea Linden, Arne Babenhauserheide, Gerald Wetzel, Christopher Boone, Andreas Engel, Jeremy J. Harrison, Patrick E. Sheese, Kaley A. Walker, and Peter F. Bernath
Atmos. Meas. Tech., 10, 2727–2743, https://doi.org/10.5194/amt-10-2727-2017, https://doi.org/10.5194/amt-10-2727-2017, 2017
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We retrieved vertical profiles of CCl4 from MIPAS Envisat IMK/IAA data. A detailed description of all characteristics is included in the paper as well as comparisons with historical measurements and comparisons with collocated measurements of instruments covering the same time span as MIPAS Envisat. A particular focus also lies on the usage of a new CCl4 spectroscopic dataset introduced recently, which leads to more realistic CCl4 volume mixing ratios.
Olivier Membrive, Cyril Crevoisier, Colm Sweeney, François Danis, Albert Hertzog, Andreas Engel, Harald Bönisch, and Laurence Picon
Atmos. Meas. Tech., 10, 2163–2181, https://doi.org/10.5194/amt-10-2163-2017, https://doi.org/10.5194/amt-10-2163-2017, 2017
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A new high-resolution AirCore system is presented. This system flown with stratospheric balloons allows us to sample atmospheric air during the descent. The analysis of trace gases (CO2 and CH4 in this case) in the collected air sample provides information on the vertical distribution along the atmospheric column. The continuous vertical profiles retrieved may contribute to several research topics concerning the observation of greenhouse gases and, more generally, carbon cycle studies.
Andreas Engel, Harald Bönisch, Markus Ullrich, Robert Sitals, Olivier Membrive, Francois Danis, and Cyril Crevoisier
Atmos. Chem. Phys., 17, 6825–6838, https://doi.org/10.5194/acp-17-6825-2017, https://doi.org/10.5194/acp-17-6825-2017, 2017
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AirCore is new technique for sampling stratospheric air. We present new observations of CO2 and CH4 using AirCore and derive stratospheric transport time, called the mean age of air. The purpose of using AirCore is to provide a cost-effective tool for deriving mean age. Mean age may serve as a proxy to investigate changes in stratospheric circulation. We show that there is no statistically significant trend in our 40-year time series of mean age, which is now extended using AirCore.
Malte Meinshausen, Elisabeth Vogel, Alexander Nauels, Katja Lorbacher, Nicolai Meinshausen, David M. Etheridge, Paul J. Fraser, Stephen A. Montzka, Peter J. Rayner, Cathy M. Trudinger, Paul B. Krummel, Urs Beyerle, Josep G. Canadell, John S. Daniel, Ian G. Enting, Rachel M. Law, Chris R. Lunder, Simon O'Doherty, Ron G. Prinn, Stefan Reimann, Mauro Rubino, Guus J. M. Velders, Martin K. Vollmer, Ray H. J. Wang, and Ray Weiss
Geosci. Model Dev., 10, 2057–2116, https://doi.org/10.5194/gmd-10-2057-2017, https://doi.org/10.5194/gmd-10-2057-2017, 2017
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Climate change is primarily driven by human-induced increases of greenhouse gas (GHG) concentrations. Based on ongoing community efforts (e.g. AGAGE and NOAA networks, ice cores), this study presents historical concentrations of CO2, CH4, N2O and 40 other GHGs from year 0 to year 2014. The data is recommended as input for climate models for pre-industrial, historical runs under CMIP6. Global means, but also latitudinal by monthly surface concentration fields are provided.
Peter G. Simmonds, Matthew Rigby, Archie McCulloch, Simon O'Doherty, Dickon Young, Jens Mühle, Paul B. Krummel, Paul Steele, Paul J. Fraser, Alistair J. Manning, Ray F. Weiss, Peter K. Salameh, Chris M. Harth, Ray H. J. Wang, and Ronald G. Prinn
Atmos. Chem. Phys., 17, 4641–4655, https://doi.org/10.5194/acp-17-4641-2017, https://doi.org/10.5194/acp-17-4641-2017, 2017
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This paper reports how long-term atmospheric measurements demonstrate that the Montreal Protocol has been effective in controlling production and consumption of the hydrochlorofluorocarbons, a group of industrial chemicals that have detrimental effects on the ozone layer and also contribute to global warming as greenhouse gases and their hydrofluorocarbon substitutes which are also potent greenhouse gases but do not materially affect the ozone layer.
Mohamadou Diallo, Bernard Legras, Eric Ray, Andreas Engel, and Juan A. Añel
Atmos. Chem. Phys., 17, 3861–3878, https://doi.org/10.5194/acp-17-3861-2017, https://doi.org/10.5194/acp-17-3861-2017, 2017
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We construct a new monthly zonal mean CO2 distribution from the upper troposphere to the stratosphere over the 2000–2010 period. The main features of the CO2 distribution are consistent with expected variability due to the transport of long-lived trace gases by the Brewer–Dobson circulation. The method used to construct this CO2 product is unique and should be useful for model and satellite validation in the upper troposphere and stratosphere.
Jennifer Ostermöller, Harald Bönisch, Patrick Jöckel, and Andreas Engel
Atmos. Chem. Phys., 17, 3785–3797, https://doi.org/10.5194/acp-17-3785-2017, https://doi.org/10.5194/acp-17-3785-2017, 2017
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We analysed the temporal evolution of fractional release factors (FRFs) from EMAC model simulations for several halocarbons and nitrous oxide. The current formulation of FRFs yields values that depend on the tropospheric trend of the species. This is a problematic issue for the application of FRF in the calculation of steady-state quantities (e.g. ODP). Including a loss term in the calculation, we develop a new formulation of FRF and find that the time dependence can almost be compensated.
Whitney Bader, Benoît Bovy, Stephanie Conway, Kimberly Strong, Dan Smale, Alexander J. Turner, Thomas Blumenstock, Chris Boone, Martine Collaud Coen, Ancelin Coulon, Omaira Garcia, David W. T. Griffith, Frank Hase, Petra Hausmann, Nicholas Jones, Paul Krummel, Isao Murata, Isamu Morino, Hideaki Nakajima, Simon O'Doherty, Clare Paton-Walsh, John Robinson, Rodrigue Sandrin, Matthias Schneider, Christian Servais, Ralf Sussmann, and Emmanuel Mahieu
Atmos. Chem. Phys., 17, 2255–2277, https://doi.org/10.5194/acp-17-2255-2017, https://doi.org/10.5194/acp-17-2255-2017, 2017
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An increase of 0.31 ± 0.03 % year−1 of atmospheric methane is reported using 10 years of solar observations performed at 10 ground-based stations since 2005. These trend agree with a GEOS-Chem-tagged simulation that accounts for the contribution of each emission source and one sink in the total methane. The GEOS-Chem simulation shows that anthropogenic emissions from coal mining and gas and oil transport and exploration have played a major role in the increase methane since 2005.
Garlich Fischbeck, Harald Bönisch, Marco Neumaier, Carl A. M. Brenninkmeijer, Johannes Orphal, Joel Brito, Julia Becker, Detlev Sprung, Peter F. J. van Velthoven, and Andreas Zahn
Atmos. Chem. Phys., 17, 1985–2008, https://doi.org/10.5194/acp-17-1985-2017, https://doi.org/10.5194/acp-17-1985-2017, 2017
Martyn P. Chipperfield, Qing Liang, Matthew Rigby, Ryan Hossaini, Stephen A. Montzka, Sandip Dhomse, Wuhu Feng, Ronald G. Prinn, Ray F. Weiss, Christina M. Harth, Peter K. Salameh, Jens Mühle, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Paul B. Krummel, Paul J. Fraser, L. Paul Steele, James D. Happell, Robert C. Rhew, James Butler, Shari A. Yvon-Lewis, Bradley Hall, David Nance, Fred Moore, Ben R. Miller, James W. Elkins, Jeremy J. Harrison, Chris D. Boone, Elliot L. Atlas, and Emmanuel Mahieu
Atmos. Chem. Phys., 16, 15741–15754, https://doi.org/10.5194/acp-16-15741-2016, https://doi.org/10.5194/acp-16-15741-2016, 2016
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Carbon tetrachloride (CCl4) is a compound which, when released into the atmosphere, can cause depletion of the stratospheric ozone layer. Its emissions are controlled under the Montreal Protocol, and its atmospheric abundance is slowly decreasing. However, this decrease is not as fast as expected based on estimates of its emissions and its atmospheric lifetime. We have used an atmospheric model to look at the uncertainties in the CCl4 lifetime and to examine the impact on its atmospheric decay.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751, https://doi.org/10.5194/essd-8-697-2016, https://doi.org/10.5194/essd-8-697-2016, 2016
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An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
Francesco Graziosi, Jgor Arduini, Paolo Bonasoni, Francesco Furlani, Umberto Giostra, Alistair J. Manning, Archie McCulloch, Simon O'Doherty, Peter G. Simmonds, Stefan Reimann, Martin K. Vollmer, and Michela Maione
Atmos. Chem. Phys., 16, 12849–12859, https://doi.org/10.5194/acp-16-12849-2016, https://doi.org/10.5194/acp-16-12849-2016, 2016
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Carbon tetrachloride is an ozone-depleting greenhouse gas banned under the Montreal Protocol. Measurements of atmospheric levels combined with global transport models indicate that it is still being emitted, in contrast to what is reported. In order to help solve the "mystery of carbon tetrachloride", we estimated European emissions during 2006–2014 using atmospheric observations and models. We identified emission hot spots and showed inconsistencies in national emission declarations.
Cathy M. Trudinger, Paul J. Fraser, David M. Etheridge, William T. Sturges, Martin K. Vollmer, Matt Rigby, Patricia Martinerie, Jens Mühle, David R. Worton, Paul B. Krummel, L. Paul Steele, Benjamin R. Miller, Johannes Laube, Francis S. Mani, Peter J. Rayner, Christina M. Harth, Emmanuel Witrant, Thomas Blunier, Jakob Schwander, Simon O'Doherty, and Mark Battle
Atmos. Chem. Phys., 16, 11733–11754, https://doi.org/10.5194/acp-16-11733-2016, https://doi.org/10.5194/acp-16-11733-2016, 2016
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Perfluorocarbons (PFCs) are potent, long-lived and mostly man-made greenhouse gases released to the atmosphere mainly during aluminium production and semiconductor manufacture. Here we present the first continuous histories of three PFCs from 1800 to 2014, derived from measurements of these PFCs in the atmosphere and in air bubbles in polar ice. The records show how human actions have affected these important greenhouse gases over the past century.
Stefan Müller, Peter Hoor, Heiko Bozem, Ellen Gute, Bärbel Vogel, Andreas Zahn, Harald Bönisch, Timo Keber, Martina Krämer, Christian Rolf, Martin Riese, Hans Schlager, and Andreas Engel
Atmos. Chem. Phys., 16, 10573–10589, https://doi.org/10.5194/acp-16-10573-2016, https://doi.org/10.5194/acp-16-10573-2016, 2016
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In situ airborne measurements performed during TACTS/ESMVal 2012 were analysed to investigate the chemical compostion of the upper troposphere and lower stratosphere. N2O, CO and O3 data show an increase in tropospherically affected air masses within the extratropical stratosphere from August to September 2012, which originate from the Asian monsoon region. Thus, the Asian monsoon anticyclone significantly affected the chemical composition of the extratropical stratosphere during summer 2012.
E. Eckert, A. Laeng, S. Lossow, S. Kellmann, G. Stiller, T. von Clarmann, N. Glatthor, M. Höpfner, M. Kiefer, H. Oelhaf, J. Orphal, B. Funke, U. Grabowski, F. Haenel, A. Linden, G. Wetzel, W. Woiwode, P. F. Bernath, C. Boone, G. S. Dutton, J. W. Elkins, A. Engel, J. C. Gille, F. Kolonjari, T. Sugita, G. C. Toon, and K. A. Walker
Atmos. Meas. Tech., 9, 3355–3389, https://doi.org/10.5194/amt-9-3355-2016, https://doi.org/10.5194/amt-9-3355-2016, 2016
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We investigate the accuracy, precision and long-term stability of the MIPAS Envisat IMK/IAA CFC-11 (CCl3F) and CFC-12 (CCl2F2) products.
For comparisons we use several data products from satellite, airplane and balloon-borne instruments as well as ground-based data.
MIPAS Envisat CFC-11 has a slight high bias at the lower end of the profile.
CFC-12 agrees well with other data products.
The temporal stability is good up to ~ 30 km, but still leaves room for improvement.
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Joe McNorton, Martyn P. Chipperfield, Manuel Gloor, Chris Wilson, Wuhu Feng, Garry D. Hayman, Matt Rigby, Paul B. Krummel, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, Ed Dlugokencky, and Steve A. Montzka
Atmos. Chem. Phys., 16, 7943–7956, https://doi.org/10.5194/acp-16-7943-2016, https://doi.org/10.5194/acp-16-7943-2016, 2016
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Methane (CH4) is an important greenhouse gas. The growth of atmospheric CH4 stalled from 1999 to 2006, with current explanations focussed mainly on changing surface fluxes. We combine models with observations and meteorological data to assess the atmospheric contribution to CH4 changes. We find that variations in mean atmospheric hydroxyl concentration can explain part of the stall in growth. Our study highlights the role of multi-annual variability in atmospheric chemistry in global CH4 trends.
M. Chirkov, G. P. Stiller, A. Laeng, S. Kellmann, T. von Clarmann, C. D. Boone, J. W. Elkins, A. Engel, N. Glatthor, U. Grabowski, C. M. Harth, M. Kiefer, F. Kolonjari, P. B. Krummel, A. Linden, C. R. Lunder, B. R. Miller, S. A. Montzka, J. Mühle, S. O'Doherty, J. Orphal, R. G. Prinn, G. Toon, M. K. Vollmer, K. A. Walker, R. F. Weiss, A. Wiegele, and D. Young
Atmos. Chem. Phys., 16, 3345–3368, https://doi.org/10.5194/acp-16-3345-2016, https://doi.org/10.5194/acp-16-3345-2016, 2016
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HCFC-22 global distributions from MIPAS measurements for 2005 to 2012 are presented. Tropospheric trends are in good agreement with ground-based observations. A layer of enhanced HCFC-22 in the upper tropospheric tropics and northern subtropics is identified to come from Asian sources uplifted in the Asian monsoon. Stratospheric distributions provide show seasonal, semi-annual, and QBO-related variations. Hemispheric asymmetries of trends hint towards a change in the stratospheric circulation.
Andreas Engel, Harald Bönisch, Tim Schwarzenberger, Hans-Peter Haase, Katja Grunow, Jana Abalichin, and Stephan Sala
Atmos. Meas. Tech., 9, 1051–1062, https://doi.org/10.5194/amt-9-1051-2016, https://doi.org/10.5194/amt-9-1051-2016, 2016
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We present a validation of MIPAS-ENVISAT vertical profiles (ESA operational retrieval version 6.0) of N2O, CH4, CFC-12, and CFC-11. The geophysical validation is performed using data from a balloon-borne cryogenic whole air sampler and trajectory matching. We show that the validation results are different for the period prior to 2005 compared to the post 2005 period. N2O, CH4, and CFC-12 show partly good agreement while CFC-11 data from this retrieval cannot be used for scientific studies.
F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 9, 179–194, https://doi.org/10.5194/amt-9-179-2016, https://doi.org/10.5194/amt-9-179-2016, 2016
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We present the characterization and application of a new gas chromatography time-of-flight mass spectrometry instrument, with focus on quantitative analysis of halocarbons in air samples. The applicability of the TOFMS technique, e.g. to form the basis of a "digital air archieve", is supported by the findings of this work: very high sensitivity, high measurement precision, a large dynamical range and an open data format which allows in-depth analysis of the data.
P. G. Simmonds, M. Rigby, A. J. Manning, M. F. Lunt, S. O'Doherty, A. McCulloch, P. J. Fraser, S. Henne, M. K. Vollmer, J. Mühle, R. F. Weiss, P. K. Salameh, D. Young, S. Reimann, A. Wenger, T. Arnold, C. M. Harth, P. B. Krummel, L. P. Steele, B. L. Dunse, B. R. Miller, C. R. Lunder, O. Hermansen, N. Schmidbauer, T. Saito, Y. Yokouchi, S. Park, S. Li, B. Yao, L. X. Zhou, J. Arduini, M. Maione, R. H. J. Wang, D. Ivy, and R. G. Prinn
Atmos. Chem. Phys., 16, 365–382, https://doi.org/10.5194/acp-16-365-2016, https://doi.org/10.5194/acp-16-365-2016, 2016
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We report regional and global emissions estimates of HFC-152a using high frequency measurements from 11 observing sites and archived air samples dating back to 1978 together with atmospheric transport models. The "bottom-up" emissions of HFC-152a reported to the UNFCCC appear to significantly underestimate those reported here from observations. This discrepancy we suggest arises from largely underestimated USA and undeclared Asian emissions.
A. Laeng, J. Plieninger, T. von Clarmann, U. Grabowski, G. Stiller, E. Eckert, N. Glatthor, F. Haenel, S. Kellmann, M. Kiefer, A. Linden, S. Lossow, L. Deaver, A. Engel, M. Hervig, I. Levin, M. McHugh, S. Noël, G. Toon, and K. Walker
Atmos. Meas. Tech., 8, 5251–5261, https://doi.org/10.5194/amt-8-5251-2015, https://doi.org/10.5194/amt-8-5251-2015, 2015
S. T. Lennartz, G. Krysztofiak, C. A. Marandino, B.-M. Sinnhuber, S. Tegtmeier, F. Ziska, R. Hossaini, K. Krüger, S. A. Montzka, E. Atlas, D. E. Oram, T. Keber, H. Bönisch, and B. Quack
Atmos. Chem. Phys., 15, 11753–11772, https://doi.org/10.5194/acp-15-11753-2015, https://doi.org/10.5194/acp-15-11753-2015, 2015
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Marine-produced short-lived trace gases such as halocarbons and DMS significantly impact atmospheric chemistry. To assess this impact on ozone depletion and the radiative budget, it is critical that their marine emissions in atmospheric chemistry models are quantified as accurately as possible. We show that calculating emissions online with an interactive atmosphere improves the agreement with current observations and should be employed regularly in models where marine sources are important.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198, https://doi.org/10.5194/gmd-8-3179-2015, https://doi.org/10.5194/gmd-8-3179-2015, 2015
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This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
A. L. Ganesan, A. J. Manning, A. Grant, D. Young, D .E. Oram, W. T. Sturges, J. B. Moncrieff, and S. O'Doherty
Atmos. Chem. Phys., 15, 6393–6406, https://doi.org/10.5194/acp-15-6393-2015, https://doi.org/10.5194/acp-15-6393-2015, 2015
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The UK is one of several countries to enact legislation to reduce its greenhouse gas emissions. We present top-down emissions of methane and nitrous oxide for the UK and Ireland over 2012-2014. We inferred average UK emissions of 2.09Tg/yr CH4 and 0.101Tg/yr N2O and used sectoral distributions to determine whether these discrepancies can be attributed to specific source sectors. We found the agricultural sector likely to be overestimated in the bottom-up emissions inventories of both gases.
J. Hoker, F. Obersteiner, H. Bönisch, and A. Engel
Atmos. Meas. Tech., 8, 2195–2206, https://doi.org/10.5194/amt-8-2195-2015, https://doi.org/10.5194/amt-8-2195-2015, 2015
P. Bergamaschi, M. Corazza, U. Karstens, M. Athanassiadou, R. L. Thompson, I. Pison, A. J. Manning, P. Bousquet, A. Segers, A. T. Vermeulen, G. Janssens-Maenhout, M. Schmidt, M. Ramonet, F. Meinhardt, T. Aalto, L. Haszpra, J. Moncrieff, M. E. Popa, D. Lowry, M. Steinbacher, A. Jordan, S. O'Doherty, S. Piacentino, and E. Dlugokencky
Atmos. Chem. Phys., 15, 715–736, https://doi.org/10.5194/acp-15-715-2015, https://doi.org/10.5194/acp-15-715-2015, 2015
M. Kaufmann, J. Blank, T. Guggenmoser, J. Ungermann, A. Engel, M. Ern, F. Friedl-Vallon, D. Gerber, J. U. Grooß, G. Guenther, M. Höpfner, A. Kleinert, E. Kretschmer, Th. Latzko, G. Maucher, T. Neubert, H. Nordmeyer, H. Oelhaf, F. Olschewski, J. Orphal, P. Preusse, H. Schlager, H. Schneider, D. Schuettemeyer, F. Stroh, O. Suminska-Ebersoldt, B. Vogel, C. M. Volk, W. Woiwode, and M. Riese
Atmos. Meas. Tech., 8, 81–95, https://doi.org/10.5194/amt-8-81-2015, https://doi.org/10.5194/amt-8-81-2015, 2015
M. Maione, F. Graziosi, J. Arduini, F. Furlani, U. Giostra, D. R. Blake, P. Bonasoni, X. Fang, S. A. Montzka, S. J. O'Doherty, S. Reimann, A. Stohl, and M. K. Vollmer
Atmos. Chem. Phys., 14, 9755–9770, https://doi.org/10.5194/acp-14-9755-2014, https://doi.org/10.5194/acp-14-9755-2014, 2014
S. O'Doherty, M. Rigby, J. Mühle, D. J. Ivy, B. R. Miller, D. Young, P. G. Simmonds, S. Reimann, M. K. Vollmer, P. B. Krummel, P. J. Fraser, L. P. Steele, B. Dunse, P. K. Salameh, C. M. Harth, T. Arnold, R. F. Weiss, J. Kim, S. Park, S. Li, C. Lunder, O. Hermansen, N. Schmidbauer, L. X. Zhou, B. Yao, R. H. J. Wang, A. J. Manning, and R. G. Prinn
Atmos. Chem. Phys., 14, 9249–9258, https://doi.org/10.5194/acp-14-9249-2014, https://doi.org/10.5194/acp-14-9249-2014, 2014
A. Tilgner, L. Schöne, P. Bräuer, D. van Pinxteren, E. Hoffmann, G. Spindler, S. A. Styler, S. Mertes, W. Birmili, R. Otto, M. Merkel, K. Weinhold, A. Wiedensohler, H. Deneke, R. Schrödner, R. Wolke, J. Schneider, W. Haunold, A. Engel, A. Wéber, and H. Herrmann
Atmos. Chem. Phys., 14, 9105–9128, https://doi.org/10.5194/acp-14-9105-2014, https://doi.org/10.5194/acp-14-9105-2014, 2014
S. N. Vardag, S. Hammer, S. O'Doherty, T. G. Spain, B. Wastine, A. Jordan, and I. Levin
Atmos. Chem. Phys., 14, 8403–8418, https://doi.org/10.5194/acp-14-8403-2014, https://doi.org/10.5194/acp-14-8403-2014, 2014
S. Sala, H. Bönisch, T. Keber, D. E. Oram, G. Mills, and A. Engel
Atmos. Chem. Phys., 14, 6903–6923, https://doi.org/10.5194/acp-14-6903-2014, https://doi.org/10.5194/acp-14-6903-2014, 2014
R. L. Thompson, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, P. K. Patra, P. Bergamaschi, F. Chevallier, E. Dlugokencky, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, A. Vermeulen, Y. Tohjima, A. Jordan, L. Haszpra, M. Steinbacher, S. Van der Laan, T. Aalto, F. Meinhardt, M. E. Popa, J. Moncrieff, and P. Bousquet
Atmos. Chem. Phys., 14, 6177–6194, https://doi.org/10.5194/acp-14-6177-2014, https://doi.org/10.5194/acp-14-6177-2014, 2014
R. L. Thompson, P. K. Patra, K. Ishijima, E. Saikawa, M. Corazza, U. Karstens, C. Wilson, P. Bergamaschi, E. Dlugokencky, C. Sweeney, R. G. Prinn, R. F. Weiss, S. O'Doherty, P. J. Fraser, L. P. Steele, P. B. Krummel, M. Saunois, M. Chipperfield, and P. Bousquet
Atmos. Chem. Phys., 14, 4349–4368, https://doi.org/10.5194/acp-14-4349-2014, https://doi.org/10.5194/acp-14-4349-2014, 2014
A. L. Ganesan, M. Rigby, A. Zammit-Mangion, A. J. Manning, R. G. Prinn, P. J. Fraser, C. M. Harth, K.-R. Kim, P. B. Krummel, S. Li, J. Mühle, S. J. O'Doherty, S. Park, P. K. Salameh, L. P. Steele, and R. F. Weiss
Atmos. Chem. Phys., 14, 3855–3864, https://doi.org/10.5194/acp-14-3855-2014, https://doi.org/10.5194/acp-14-3855-2014, 2014
S. Tegtmeier, K. Krüger, B. Quack, E. Atlas, D. R. Blake, H. Boenisch, A. Engel, H. Hepach, R. Hossaini, M. A. Navarro, S. Raimund, S. Sala, Q. Shi, and F. Ziska
Atmos. Chem. Phys., 13, 11869–11886, https://doi.org/10.5194/acp-13-11869-2013, https://doi.org/10.5194/acp-13-11869-2013, 2013
R. Hossaini, H. Mantle, M. P. Chipperfield, S. A. Montzka, P. Hamer, F. Ziska, B. Quack, K. Krüger, S. Tegtmeier, E. Atlas, S. Sala, A. Engel, H. Bönisch, T. Keber, D. Oram, G. Mills, C. Ordóñez, A. Saiz-Lopez, N. Warwick, Q. Liang, W. Feng, F. Moore, B. R. Miller, V. Marécal, N. A. D. Richards, M. Dorf, and K. Pfeilsticker
Atmos. Chem. Phys., 13, 11819–11838, https://doi.org/10.5194/acp-13-11819-2013, https://doi.org/10.5194/acp-13-11819-2013, 2013
A. L. Ganesan, A. Chatterjee, R. G. Prinn, C. M. Harth, P. K. Salameh, A. J. Manning, B. D. Hall, J. Mühle, L. K. Meredith, R. F. Weiss, S. O'Doherty, and D. Young
Atmos. Chem. Phys., 13, 10633–10644, https://doi.org/10.5194/acp-13-10633-2013, https://doi.org/10.5194/acp-13-10633-2013, 2013
P. D. Hamer, V. Marécal, R. Hossaini, M. Pirre, N. Warwick, M. Chipperfield, A. A. Samah, N. Harris, A. Robinson, B. Quack, A. Engel, K. Krüger, E. Atlas, K. Subramaniam, D. Oram, Emma C. Leedham Elvidge, G. Mills, K. Pfeilsticker, S. Sala, T. Keber, H. Bönisch, L. K. Peng, M. S. M. Nadzir, P. T. Lim, A. Mujahid, A. Anton, H. Schlager, V. Catoire, G. Krysztofiak, S. Fühlbrügge, M. Dorf, and W. T. Sturges
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-13-20611-2013, https://doi.org/10.5194/acpd-13-20611-2013, 2013
Revised manuscript not accepted
J. C. Laube, A. Keil, H. Bönisch, A. Engel, T. Röckmann, C. M. Volk, and W. T. Sturges
Atmos. Chem. Phys., 13, 2779–2791, https://doi.org/10.5194/acp-13-2779-2013, https://doi.org/10.5194/acp-13-2779-2013, 2013
Related subject area
Subject: Gases | Technique: Laboratory Measurement | Topic: Instruments and Platforms
High-precision oxygen isotope (δ18O) measurements of atmospheric dioxygen using optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS)
Water vapor stable isotope memory effects of common tubing materials
Evaluation of a reduced-pressure chemical ion reactor utilizing adduct ionization for the detection of gaseous organic and inorganic species
Ammonium CI-Orbitrap: a tool for characterizing the reactivity of oxygenated organic molecules
A high-accuracy dynamic dilution method for generating reference gas mixtures of carbonyl sulfide at sub-nanomole-per-mole levels for long-term atmospheric observation
Optimizing the iodide-adduct chemical ionization mass spectrometry (CIMS) quantitative method for toluene oxidation intermediates: experimental insights into functional-group differences
Simultaneous measurement of greenhouse gases (CH4, CO2 and N2O) at atmospheric levels using a gas chromatography system
A new portable sampler of atmospheric methane for radiocarbon measurements
Characterization of a new Teflon chamber and on-line analysis of isomeric multifunctional photooxidation products
A versatile water vapor generation module for vapor isotope calibration and liquid isotope measurements
Extraction, purification, and clumped isotope analysis of methane (Δ13CDH3 and Δ12CD2H2) from sources and the atmosphere
Response of protonated, adduct, and fragmented ions in Vocus proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS)
Absorption of volatile organic compounds (VOCs) by polymer tubing: implications for indoor air and use as a simple gas-phase volatility separation technique
A flexible device to produce a gas stream with a precisely controlled water vapour mixing ratio and isotope composition based on microdrop dispensing technology
Revision of an open-split-based dual-inlet system for elemental and isotope ratio mass spectrometers with a focus on clumped-isotope measurements
Characterisation of gaseous iodine species detection using the multi-scheme chemical ionisation inlet 2 with bromide and nitrate chemical ionisation methods
A novel inlet for enriching concentrations of reactive organic gases in low sampling flows
Characterizing the automatic radon flux transfer standard system Autoflux: laboratory calibration and field experiments
Influence of ozone and humidity on PTR-MS and GC-MS VOC measurements with and without a Na2S2O3 ozone scrubber
Laser-induced sublimation extraction for centimeter-resolution multi-species greenhouse gas analysis on ice cores
Ozone reactivity measurement of biogenic volatile organic compound emissions
Comparison of two photolytic calibration methods for nitrous acid
Measurement of enantiomer percentages for five monoterpenes from six conifer species by cartridge-tube-based passive sampling adsorption–thermal desorption (ps-ATD)
Identification, monitoring, and reaction kinetics of reactive trace species using time-resolved mid-infrared quantum cascade laser absorption spectroscopy: development, characterisation, and initial results for the CH2OO Criegee intermediate
Air pollution monitoring: development of ammonia (NH3) dynamic reference gas mixtures at nanomoles per mole levels to improve the lack of traceability of measurements
Formaldehyde and glyoxal measurement deploying a selected ion flow tube mass spectrometer (SIFT-MS)
Fragmentation inside proton-transfer-reaction-based mass spectrometers limits the detection of ROOR and ROOH peroxides
MULTICHARME: a modified Chernin-type multi-pass cell designed for IR and THz long-path absorption measurements in the CHARME atmospheric simulation chamber
Silicone tube humidity generator
A source for the continuous generation of pure and quantifiable HONO mixtures
Photochemical method for removing methane interference for improved gas analysis
A simulation chamber for absorption spectroscopy in planetary atmospheres
An automated system for trace gas flux measurements from plant foliage and other plant compartments
Simultaneous measurement of δ13C, δ18O and δ17O of atmospheric CO2 – performance assessment of a dual-laser absorption spectrometer
Measurement of iodine species and sulfuric acid using bromide chemical ionization mass spectrometers
A method for resolving changes in atmospheric He ∕ N2 as an indicator of fossil fuel extraction and stratospheric circulation
Application of chemical derivatization techniques combined with chemical ionization mass spectrometry to detect stabilized Criegee intermediates and peroxy radicals in the gas phase
Atomic emission detector with gas chromatographic separation and cryogenic pre-concentration (CryoTrap–GC–AED) for atmospheric trace gas measurements
New technique for high-precision, simultaneous measurements of CH4, N2O and CO2 concentrations; isotopic and elemental ratios of N2, O2 and Ar; and total air content in ice cores by wet extraction
High-precision laser spectrometer for multiple greenhouse gas analysis in 1 mL air from ice core samples
A thermal-dissociation–cavity ring-down spectrometer (TD-CRDS) for the detection of organic nitrates in gas and particle phases
Interference from alkenes in chemiluminescent NOx measurements
Calibration of an airborne HOx instrument using the All Pressure Altitude-based Calibrator for HOx Experimentation (APACHE)
Measurement of ammonia, amines and iodine compounds using protonated water cluster chemical ionization mass spectrometry
An instrument for in situ measurement of total ozone reactivity
Portable calibrator for NO based on the photolysis of N2O and a combined NO2∕NO∕O3 source for field calibrations of air pollution monitors
A new instrument for time-resolved measurement of HO2 radicals
Investigation of adsorption and desorption behavior of small-volume cylinders and its relevance for atmospheric trace gas analysis
Towards an understanding of surface effects: testing of various materials in a small volume measurement chamber and its relevance for atmospheric trace gas analysis
Stability of halocarbons in air samples stored in stainless- steel canisters
Clément Piel, Daniele Romanini, Morgane Farradèche, Justin Chaillot, Clémence Paul, Nicolas Bienville, Thomas Lauwers, Joana Sauze, Kévin Jaulin, Frédéric Prié, and Amaëlle Landais
Atmos. Meas. Tech., 17, 6647–6658, https://doi.org/10.5194/amt-17-6647-2024, https://doi.org/10.5194/amt-17-6647-2024, 2024
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This paper introduces a new optical gas analyzer based on an optical-feedback cavity-enhanced absorption spectroscopy (OF-CEAS) technique enabling high-temporal-resolution and high-precision measurements of oxygen isotopes (δ18O) and dioxygen (O2) concentration of atmospheric O2 (respectively 0.06 ‰ and 0.002 % over 10 min integration). The results underscore the good agreement with isotope ratio mass spectrometry measurements and the ability of the instrument to monitor biological processes.
Alexandra L. Meyer and Lisa R. Welp
Atmos. Meas. Tech., 17, 6193–6212, https://doi.org/10.5194/amt-17-6193-2024, https://doi.org/10.5194/amt-17-6193-2024, 2024
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Water molecules stick to air intake tubing wall surfaces, smoothing measurements of fast isotopic variability in the atmosphere. We tested this stickiness and saw small differences in isotopic signal speed between materials, tubing inner dimensions, and isotopic switch direction, although no consistent temperature effects. Researchers can confidently compare measurements across observation systems using different commonly used tubing materials and plan for optimal inlet designs of new systems.
Matthieu Riva, Veronika Pospisilova, Carla Frege, Sebastien Perrier, Priyanka Bansal, Spiro Jorga, Patrick Sturm, Joel A. Thornton, Urs Rohner, and Felipe Lopez-Hilfiker
Atmos. Meas. Tech., 17, 5887–5901, https://doi.org/10.5194/amt-17-5887-2024, https://doi.org/10.5194/amt-17-5887-2024, 2024
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We present a newly designed reduced-pressure chemical ionization reactor for detection of gas-phase organic and inorganic species. The system operates through the combined use of vacuum ultraviolet ionization and photosensitizers to generate numerous adduct ionization schemes. As a result, it offers the ability to simultaneously measure a wide variety of organic and inorganic species in terms of compound volatility and functionality, while being largely independent of changes in sample humidity.
Dandan Li, Dongyu Wang, Lucia Caudillo, Wiebke Scholz, Mingyi Wang, Sophie Tomaz, Guillaume Marie, Mihnea Surdu, Elias Eccli, Xianda Gong, Loic Gonzalez-Carracedo, Manuel Granzin, Joschka Pfeifer, Birte Rörup, Benjamin Schulze, Pekka Rantala, Sébastien Perrier, Armin Hansel, Joachim Curtius, Jasper Kirkby, Neil M. Donahue, Christian George, Imad El-Haddad, and Matthieu Riva
Atmos. Meas. Tech., 17, 5413–5428, https://doi.org/10.5194/amt-17-5413-2024, https://doi.org/10.5194/amt-17-5413-2024, 2024
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Due to the analytical challenges of measuring organic vapors, it remains challenging to identify and quantify organic molecules present in the atmosphere. Here, we explore the performance of the Orbitrap chemical ionization mass spectrometer (CI-Orbitrap) using ammonium ion chemistry. This study shows that ammonium-ion-based chemistry associated with the high mass resolution of the Orbitrap mass analyzer can measure almost all inclusive compounds.
Hideki Nara, Takuya Saito, Taku Umezawa, and Yasunori Tohjima
Atmos. Meas. Tech., 17, 5187–5200, https://doi.org/10.5194/amt-17-5187-2024, https://doi.org/10.5194/amt-17-5187-2024, 2024
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We have developed a high-accuracy dynamic dilution system for generating reference gas mixtures containing carbonyl sulfide (COS). Although COS at ambient levels generally has poor storage stability, our approach involves the dilution of a gas mixture containing micromole-per-mole levels of COS, the stability of which was validated for more than 1 decade. The developed system has excellent dilution performance and will facilitate accurate instrumental calibration for atmospheric COS observation.
Mengdi Song, Shuyu He, Xin Li, Ying Liu, Shengrong Lou, Sihua Lu, Limin Zeng, and Yuanhang Zhang
Atmos. Meas. Tech., 17, 5113–5127, https://doi.org/10.5194/amt-17-5113-2024, https://doi.org/10.5194/amt-17-5113-2024, 2024
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We introduce detailed and improved quantitation and semi-quantitation methods of iodide-adduct time-of-flight chemical ionization mass spectrometry (I-CIMS) to measure toluene oxidation intermediates. We assess the experimental sensitivity of various functional group species and their binding energy with iodide ions in I-CIMS. A novel classification approach was introduced to significantly enhance the accuracy of semi-quantitative methods (improving R2 values from 0.52 to beyond 0.88).
Michal Bucha, Dominika Lewicka-Szczebak, and Piotr Wójtowicz
EGUsphere, https://doi.org/10.5194/egusphere-2024-2125, https://doi.org/10.5194/egusphere-2024-2125, 2024
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Manuscript presents new method for determination of GHG’s (CH4, CO2 and N2O) at ambient levels using chromatographic system with barrier ion discharge detector (BID) and Carboxen 1010 column. System is omitting the need for an electron capture detector (ECD) containing radiogenic components for N2O analysis and a flame ionisation detector (FID) with a methaniser for CO2 samples. This simplification reduces analytical costs, facilitates instrument maintenance and improves measurement robustness.
Giulia Zazzeri, Lukas Wacker, Negar Haghipour, Philip Gautchi, Thomas Laemmel, Sönke Szidat, and Heather Graven
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amt-2024-123, https://doi.org/10.5194/amt-2024-123, 2024
Revised manuscript accepted for AMT
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Radiocarbon (14C) is an optimal tracer of methane (CH4) emissions, as 14C measurements enable distinguishing fossil from biogenic methane. However, these measurements are particularly challenging, mainly due to technical difficulties in the sampling procedure. With this work we made the sample extraction much simpler and time efficient, providing a new technology that can be used by any research group, with the goal of expanding 14C measurements for an improved understanding of methane sources.
Finja Löher, Esther Borrás, Amalia Muñoz, and Anke Christine Nölscher
Atmos. Meas. Tech., 17, 4553–4579, https://doi.org/10.5194/amt-17-4553-2024, https://doi.org/10.5194/amt-17-4553-2024, 2024
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We constructed and characterized a new indoor Teflon atmospheric simulation chamber. We evaluated wall losses, photolysis rates, and secondary reactions of multifunctional photooxidation products in the chamber. To measure these products on-line, we combined chromatographic and mass spectrometric analyses to obtain both isomeric information and a high temporal resolution. For method validation, we studied the formation yields of the main ring-retaining products of toluene.
Hans Christian Steen-Larsen and Daniele Zannoni
Atmos. Meas. Tech., 17, 4391–4409, https://doi.org/10.5194/amt-17-4391-2024, https://doi.org/10.5194/amt-17-4391-2024, 2024
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The water vapor generation module is completely scalable, allowing autonomous calibrations to use N standards and providing integration times only restricted by sample availability. We document improved reproducibility in 17O-excess liquid measurements. This module makes spectroscopy measurements comparable to mass spectrometry. We document that the vapor generation module can be used to analyze instrument performance and for vapor isotope calibration during field campaign measurements.
Malavika Sivan, Thomas Röckmann, Carina van der Veen, and Maria Elena Popa
Atmos. Meas. Tech., 17, 2687–2705, https://doi.org/10.5194/amt-17-2687-2024, https://doi.org/10.5194/amt-17-2687-2024, 2024
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We have set up a measurement system for methane-clumped isotopologues. We have built an extraction and purification system to extract pure methane for these measurements, for samples of various origins, including atmospheric air, for which we need to process about 1000 L of air for one measurement. We report here the technical setup for extraction and measurements, as well as the calibration, and we give an overview of the samples measured so far.
Fangbing Li, Dan Dan Huang, Linhui Tian, Bin Yuan, Wen Tan, Liang Zhu, Penglin Ye, Douglas Worsnop, Ka In Hoi, Kai Meng Mok, and Yong Jie Li
Atmos. Meas. Tech., 17, 2415–2427, https://doi.org/10.5194/amt-17-2415-2024, https://doi.org/10.5194/amt-17-2415-2024, 2024
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The responses of protonated, adduct, and fragmented ions of 21 volatile organic compounds (VOCs) were investigated with varying instrument settings and relative humidity (RH) in a Vocus proton-transfer-reaction mass spectrometer (PTR-MS). The protonated ions of most VOCs studied show < 15 % variation in sensitivity, except for some long-chain aldehydes. The relationship between sensitivity and PTR rate constant is complicated by the influences from ion transmission and protonated ion fraction.
Melissa A. Morris, Demetrios Pagonis, Douglas A. Day, Joost A. de Gouw, Paul J. Ziemann, and Jose L. Jimenez
Atmos. Meas. Tech., 17, 1545–1559, https://doi.org/10.5194/amt-17-1545-2024, https://doi.org/10.5194/amt-17-1545-2024, 2024
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Polymer absorption of volatile organic compounds (VOCs) is important to characterize for atmospheric sampling setups (as interactions cause sampling delays) and indoor air quality. Here we test different polymer materials and quantify their absorptive capacities through modeling. We found the main polymers in carpets to be highly absorptive, acting as large reservoirs for indoor pollution. We also demonstrated how polymer tubes can be used as a low-cost gas separation technique.
Harald Sodemann, Alena Dekhtyareva, Alvaro Fernandez, Andrew Seidl, and Jenny Maccali
Atmos. Meas. Tech., 16, 5181–5203, https://doi.org/10.5194/amt-16-5181-2023, https://doi.org/10.5194/amt-16-5181-2023, 2023
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We describe a device that allows one to produce a continuous stream of water vapour with a specified level of humidity. As a main innovation, we can mix waters with different water isotope composition. Through a series of tests we show that the performance characteristics of the device are in line with specifications. We present two laboratory applications where the device proves useful, first in characterizing instruments, and second for the analysis of water contained in stalagmites.
Stephan Räss, Peter Nyfeler, Paul Wheeler, Will Price, and Markus Christian Leuenberger
Atmos. Meas. Tech., 16, 4489–4505, https://doi.org/10.5194/amt-16-4489-2023, https://doi.org/10.5194/amt-16-4489-2023, 2023
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Due to technological advances clumped-isotope studies have gained importance in recent years. Typically, these studies are performed with high-resolution isotope ratio mass spectrometers (IRMSs) along with a changeover-valve-based dual-inlet system (DIS). We are taking a different approach, namely performing clumped-isotope measurements with a compact low-resolution IRMS with an open-split-based DIS. Currently, we are working with pure-oxygen gas for which we are providing a proof of concept.
Xu-Cheng He, Jiali Shen, Siddharth Iyer, Paxton Juuti, Jiangyi Zhang, Mrisha Koirala, Mikko M. Kytökari, Douglas R. Worsnop, Matti Rissanen, Markku Kulmala, Norbert M. Maier, Jyri Mikkilä, Mikko Sipilä, and Juha Kangasluoma
Atmos. Meas. Tech., 16, 4461–4487, https://doi.org/10.5194/amt-16-4461-2023, https://doi.org/10.5194/amt-16-4461-2023, 2023
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In this study, the upgraded multi-scheme chemical ionisation inlet 2 is presented. Sulfuric acid, hypoiodous acid, iodine, sulfur dioxide, and hydroperoxyl radicals are calibrated, and the improved ion optics allow us to detect sulfuric acid and iodine-containing molecules at as low as a few parts per quadrillion by volume. Additionally, we confirm the reliable detection of iodic acid using both the nitrate and bromide chemical ionisation methods under atmospherically relevant conditions.
Namrata Shanmukh Panji and Gabriel Isaacman-VanWertz
Atmos. Meas. Tech., 16, 4319–4330, https://doi.org/10.5194/amt-16-4319-2023, https://doi.org/10.5194/amt-16-4319-2023, 2023
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Measuring volatile organic compounds (VOCs) in the atmosphere is crucial for understanding air quality and environmental impact. Since these compounds are present in low concentrations, preconcentration of samples is often necessary for accurate detection. To address this issue, we have developed a novel inlet that uses selective permeation to concentrate organic gases in small sample flows. This device offers a promising approach for accurately detecting low levels of VOCs in the atmosphere.
Claudia Grossi, Daniel Rabago, Scott Chambers, Carlos Sáinz, Roger Curcoll, Peter P. S. Otáhal, Eliška Fialová, Luis Quindos, and Arturo Vargas
Atmos. Meas. Tech., 16, 2655–2672, https://doi.org/10.5194/amt-16-2655-2023, https://doi.org/10.5194/amt-16-2655-2023, 2023
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The automatic and low-maintenance radon flux system Autoflux, completed with environmental soil and atmosphere sensors, has been theoretically and experimentally characterized and calibrated under laboratory conditions to be used as transfer standard for in situ measurements. It will offer for the first time long-term measurements to validate radon flux maps used by the climate and the radiation protection communities for assessing the radon gas emissions in the atmosphere.
Lisa Ernle, Monika Akima Ringsdorf, and Jonathan Williams
Atmos. Meas. Tech., 16, 1179–1194, https://doi.org/10.5194/amt-16-1179-2023, https://doi.org/10.5194/amt-16-1179-2023, 2023
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Atmospheric ozone can induce artefacts in volatile organic compound measurements. Laboratory tests were made using GC-MS and PTR-MS aircraft systems under tropospheric and stratospheric conditions of humidity and ozone, with and without sodium thiosulfate filter scrubbers. Ozone in dry air produces some carbonyls and degrades alkenes. The scrubber lifetime depends on ozone concentration, flow rate and humidity. For the troposphere with scrubber, no significant artefacts were found over 14 d.
Lars Mächler, Daniel Baggenstos, Florian Krauss, Jochen Schmitt, Bernhard Bereiter, Remo Walther, Christoph Reinhard, Béla Tuzson, Lukas Emmenegger, and Hubertus Fischer
Atmos. Meas. Tech., 16, 355–372, https://doi.org/10.5194/amt-16-355-2023, https://doi.org/10.5194/amt-16-355-2023, 2023
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We present a new method to extract the gases from ice cores and measure their greenhouse gas composition. The ice is sublimated continuously with a near-infrared laser, releasing the gases, which are then analyzed on a laser absorption spectrometer. The main advantage over previous efforts is a low effective resolution of 1–2 cm. This capability is crucial for the analysis of highly thinned ice, as expected from ongoing drilling efforts to extend ice core history further back in time.
Detlev Helmig, Alex Guenther, Jacques Hueber, Ryan Daly, Wei Wang, Jeong-Hoo Park, Anssi Liikanen, and Arnaud P. Praplan
Atmos. Meas. Tech., 15, 5439–5454, https://doi.org/10.5194/amt-15-5439-2022, https://doi.org/10.5194/amt-15-5439-2022, 2022
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This research demonstrates a new method for determination of the chemical reactivity of volatile organic compounds that are emitted from the leaves and needles of trees. These measurements allow elucidating if and how much of these emissions and their associated reactivity are captured and quantified by currently applicable chemical analysis methods.
Andrew J. Lindsay and Ezra C. Wood
Atmos. Meas. Tech., 15, 5455–5464, https://doi.org/10.5194/amt-15-5455-2022, https://doi.org/10.5194/amt-15-5455-2022, 2022
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Nitrous acid (HONO) is an important source of the main atmospheric oxidant – the hydroxyl radical (OH). Advances in nitrous acid measurement techniques and calibration methods therefore improve our understanding of atmospheric oxidation processes. In this paper, we present two calibration methods based on photo-dissociating water vapor. These calibration methods are useful alternatives to conventional calibrations that involve a reacting hydrogen chloride vapor with sodium nitrite.
Ying Wang, Wentai Luo, Todd N. Rosenstiel, and James F. Pankow
Atmos. Meas. Tech., 15, 4651–4661, https://doi.org/10.5194/amt-15-4651-2022, https://doi.org/10.5194/amt-15-4651-2022, 2022
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A rapid, sensitive, and precise analytical method was developed for measuring the fractional amounts of the (−) and (+) forms of chiral enantiomeric forms of monoterpenes in air containing biogenic plant emissions. The method uses passive air sampling onto adsorption–thermal desorption (ATD) gas sampling cartridge tubes; this is followed by automatable thermal desorption onto a chiral gas chromatography (GC) column, followed by detection with mass spectrometry (MS).
Zara S. Mir, Matthew Jamieson, Nicholas R. Greenall, Paul W. Seakins, Mark A. Blitz, and Daniel Stone
Atmos. Meas. Tech., 15, 2875–2887, https://doi.org/10.5194/amt-15-2875-2022, https://doi.org/10.5194/amt-15-2875-2022, 2022
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In this work we describe the development and characterisation of an experiment using laser flash photolysis coupled with time-resolved mid-infrared (mid-IR) quantum cascade laser (QCL) absorption spectroscopy, with initial results reported for measurements of the infrared spectrum, kinetics, and product yields for the reaction of the CH2OO Criegee intermediate with SO2. This work has significance for the identification and measurement of reactive trace species in complex systems.
Tatiana Macé, Maitane Iturrate-Garcia, Céline Pascale, Bernhard Niederhauser, Sophie Vaslin-Reimann, and Christophe Sutour
Atmos. Meas. Tech., 15, 2703–2718, https://doi.org/10.5194/amt-15-2703-2022, https://doi.org/10.5194/amt-15-2703-2022, 2022
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LNE developed, with the company 2M PROCESS, a gas reference generator to dynamically generate NH3 reference gas mixtures in the air at very low fractions between 1 and 400 nmol/mol. The procedure defined by LNE for calibrating NH3 analyzers used for monitoring air quality guarantees relative expanded uncertainties lower than 2 % for this measurement range. The results of a comparison organized between METAS and LNE allowed the validation of LNE's reference generator and calibration procedure.
Antonia G. Zogka, Manolis N. Romanias, and Frederic Thevenet
Atmos. Meas. Tech., 15, 2001–2019, https://doi.org/10.5194/amt-15-2001-2022, https://doi.org/10.5194/amt-15-2001-2022, 2022
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We emphasize the application of SIFT-MS to detect two important atmospheric pollutants, i.e., formaldehyde (FM) and glyoxal (GL). FM and GL are secondary products formed by volatile organic compound oxidation in indoor and outdoor environments and play a key role in air quality and climate. We show that SIFT-MS is able to monitor these species selectively and in real time, overcoming the limitations of other, classical analytical techniques used to monitor these species in the atmosphere.
Haiyan Li, Thomas Golin Almeida, Yuanyuan Luo, Jian Zhao, Brett B. Palm, Christopher D. Daub, Wei Huang, Claudia Mohr, Jordan E. Krechmer, Theo Kurtén, and Mikael Ehn
Atmos. Meas. Tech., 15, 1811–1827, https://doi.org/10.5194/amt-15-1811-2022, https://doi.org/10.5194/amt-15-1811-2022, 2022
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This work evaluated the potential for PTR-based mass spectrometers to detect ROOR and ROOH peroxides both experimentally and through computations. Laboratory experiments using a Vocus PTR observed only noisy signals of potential dimers during α-pinene ozonolysis and a few small signals of dimeric compounds during cyclohexene ozonolysis. Quantum chemical calculations for model ROOR and ROOH systems showed that most of these peroxides should fragment partially following protonation.
Jean Decker, Éric Fertein, Jonas Bruckhuisen, Nicolas Houzel, Pierre Kulinski, Bo Fang, Weixiong Zhao, Francis Hindle, Guillaume Dhont, Robin Bocquet, Gaël Mouret, Cécile Coeur, and Arnaud Cuisset
Atmos. Meas. Tech., 15, 1201–1215, https://doi.org/10.5194/amt-15-1201-2022, https://doi.org/10.5194/amt-15-1201-2022, 2022
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We present a multiple pass system developed for the CHamber for Atmospheric Reactivity and Metrology of the Environment. This multi-pass cell allows monitoring of atmospheric species at trace levels by high-resolution spectroscopy with long interaction path lengths in the IR and for the first time in the terahertz range. Interesting prospects are highlighted in this frequency domain, such as a high degree of selectivity or the possibility to monitor in real-time atmospheric processes.
Robert F. Berg, Nicola Chiodo, and Eric Georgin
Atmos. Meas. Tech., 15, 819–832, https://doi.org/10.5194/amt-15-819-2022, https://doi.org/10.5194/amt-15-819-2022, 2022
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We made a humidity generator that adds water vapor to a flowing gas. Its range of humidity is useful for calibrating balloon-borne probes to the Earth's stratosphere. The generator’s novel feature is a saturator that comprises 5 m of silicone tubing immersed in water. The length was enough to ensure that the saturator’s output was independent of the dimensions and permeability of the tube. This simple, low-cost design provides an accuracy that is acceptable for many applications.
Guillermo Villena and Jörg Kleffmann
Atmos. Meas. Tech., 15, 627–637, https://doi.org/10.5194/amt-15-627-2022, https://doi.org/10.5194/amt-15-627-2022, 2022
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A continuous source for the generation of pure HONO mixtures was developed and characterized, which is based on the Henry's law solubility of HONO in acidic aqueous solutions. The source shows a fast time response and an excellent long-term stability and can be easily adjusted to HONO mixing ratios in the range 0.05–500 ppb. A general equation based on Henry's law is developed, whereby the HONO concentration of the source can be absolutely calculated with an accuracy of better than 10 %.
Merve Polat, Jesper Baldtzer Liisberg, Morten Krogsbøll, Thomas Blunier, and Matthew S. Johnson
Atmos. Meas. Tech., 14, 8041–8067, https://doi.org/10.5194/amt-14-8041-2021, https://doi.org/10.5194/amt-14-8041-2021, 2021
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We have designed a process for removing methane from a gas stream so that nitrous oxide can be measured without interference. These are both key long-lived greenhouse gases frequently studied in relation to ice cores, plants, water treatment and so on. However, many researchers are not aware of the problem of methane interference, and in addition there have not been good methods available for solving the problem. Here we present and evaluate such a method.
Marcel Snels, Stefania Stefani, Angelo Boccaccini, David Biondi, and Giuseppe Piccioni
Atmos. Meas. Tech., 14, 7187–7197, https://doi.org/10.5194/amt-14-7187-2021, https://doi.org/10.5194/amt-14-7187-2021, 2021
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A novel simulation chamber, PASSxS (Planetary Atmosphere Simulation System for Spectroscopy), has been developed for absorption measurements with a Fourier transform spectrometer (FTS) and possibly a cavity ring-down (CRD) spectrometer, with a sample temperature ranging from 100 K up to 550 K, while the pressure of the gas can be varied up to 60 bar. These temperature and pressure ranges cover a significant part of the planetary atmospheres in the solar system and possibly extrasolar planets.
Lukas Kohl, Markku Koskinen, Tatu Polvinen, Salla Tenhovirta, Kaisa Rissanen, Marjo Patama, Alessandro Zanetti, and Mari Pihlatie
Atmos. Meas. Tech., 14, 4445–4460, https://doi.org/10.5194/amt-14-4445-2021, https://doi.org/10.5194/amt-14-4445-2021, 2021
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We present ShoTGa-FluMS, a measurement system designed for continuous and automated measurements of trace gas and volatile organic compound (VOC) fluxes from plant shoots. ShoTGa-FluMS uses transparent shoot enclosures equipped with cooling elements, automatically replaces fixated CO2, and removes transpired water from the enclosure, thus solving multiple technical problems that have so far prevented automated plant shoot trace gas flux measurements.
Pharahilda M. Steur, Hubertus A. Scheeren, Dave D. Nelson, J. Barry McManus, and Harro A. J. Meijer
Atmos. Meas. Tech., 14, 4279–4304, https://doi.org/10.5194/amt-14-4279-2021, https://doi.org/10.5194/amt-14-4279-2021, 2021
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For understanding the sources and sinks of atmospheric CO2, measurement of stable isotopes has proven to be highly valuable. We present a new method using laser absorption spectroscopy to simultaneously conduct measurements of three CO2 isotopes, directly on dry-air samples. This new method reduces sample preparation time significantly, compared to the conventional method in which measurements are conducted on pure CO2, and avoids measurement biases introduced by CO2 extraction.
Mingyi Wang, Xu-Cheng He, Henning Finkenzeller, Siddharth Iyer, Dexian Chen, Jiali Shen, Mario Simon, Victoria Hofbauer, Jasper Kirkby, Joachim Curtius, Norbert Maier, Theo Kurtén, Douglas R. Worsnop, Markku Kulmala, Matti Rissanen, Rainer Volkamer, Yee Jun Tham, Neil M. Donahue, and Mikko Sipilä
Atmos. Meas. Tech., 14, 4187–4202, https://doi.org/10.5194/amt-14-4187-2021, https://doi.org/10.5194/amt-14-4187-2021, 2021
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Atmospheric iodine species are often short-lived with low abundance and have thus been challenging to measure. We show that the bromide chemical ionization mass spectrometry, compatible with both the atmospheric pressure and reduced pressure interfaces, can simultaneously detect various gas-phase iodine species. Combining calibration experiments and quantum chemical calculations, we quantify detection sensitivities to HOI, HIO3, I2, and H2SO4, giving detection limits down to < 106 molec. cm-3.
Benjamin Birner, William Paplawsky, Jeffrey Severinghaus, and Ralph F. Keeling
Atmos. Meas. Tech., 14, 2515–2527, https://doi.org/10.5194/amt-14-2515-2021, https://doi.org/10.5194/amt-14-2515-2021, 2021
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The atmospheric helium-to-nitrogen ratio is a promising indicator for circulation changes in the upper atmosphere and fossil fuel burning by humans. We present a very precise analysis method to determine changes in the helium-to-nitrogen ratio of air samples. The method relies on stabilizing the gas flow to a mass spectrometer and continuous removal of reactive gases. These advances enable new insights and monitoring possibilities for anthropogenic and natural processes.
Alexander Zaytsev, Martin Breitenlechner, Anna Novelli, Hendrik Fuchs, Daniel A. Knopf, Jesse H. Kroll, and Frank N. Keutsch
Atmos. Meas. Tech., 14, 2501–2513, https://doi.org/10.5194/amt-14-2501-2021, https://doi.org/10.5194/amt-14-2501-2021, 2021
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We have developed an online method for speciated measurements of organic peroxy radicals and stabilized Criegee intermediates using chemical derivatization combined with chemical ionization mass spectrometry. Chemical derivatization prevents secondary radical reactions and eliminates potential interferences. Comparison between our measurements and results from numeric modeling shows that the method can be used for the quantification of a wide range of atmospheric radicals and intermediates.
Einar Karu, Mengze Li, Lisa Ernle, Carl A. M. Brenninkmeijer, Jos Lelieveld, and Jonathan Williams
Atmos. Meas. Tech., 14, 1817–1831, https://doi.org/10.5194/amt-14-1817-2021, https://doi.org/10.5194/amt-14-1817-2021, 2021
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A gas measurement device was developed to measure trace gases (ppt level) in the air based on an atomic emission detector. It combines a cryogenic pre-concentrator (CryoTrap), a gas chromatograph (GC), and a new high-resolution atomic emission detector (AED). The CryoTrap–GC–AED instrumental setup, limits of detection, and elemental performance are presented and discussed. Two measurement case studies are reported: one in a Finnish boreal forest and the other based on an aircraft campaign.
Ikumi Oyabu, Kenji Kawamura, Kyotaro Kitamura, Remi Dallmayr, Akihiro Kitamura, Chikako Sawada, Jeffrey P. Severinghaus, Ross Beaudette, Anaïs Orsi, Satoshi Sugawara, Shigeyuki Ishidoya, Dorthe Dahl-Jensen, Kumiko Goto-Azuma, Shuji Aoki, and Takakiyo Nakazawa
Atmos. Meas. Tech., 13, 6703–6731, https://doi.org/10.5194/amt-13-6703-2020, https://doi.org/10.5194/amt-13-6703-2020, 2020
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Air in polar ice cores provides information on past atmosphere and climate. We present a new method for simultaneously measuring eight gases (CH4, N2O and CO2 concentrations; isotopic ratios of N2 and O2; elemental ratios between N2, O2 and Ar; and total air content) from single ice-core samples with high precision.
Bernhard Bereiter, Béla Tuzson, Philipp Scheidegger, André Kupferschmid, Herbert Looser, Lars Mächler, Daniel Baggenstos, Jochen Schmitt, Hubertus Fischer, and Lukas Emmenegger
Atmos. Meas. Tech., 13, 6391–6406, https://doi.org/10.5194/amt-13-6391-2020, https://doi.org/10.5194/amt-13-6391-2020, 2020
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The record of past greenhouse gas composition from ice cores is crucial for our understanding of global climate change. Deciphering this archive requires highly accurate and spatially resolved analysis of the very small amount of gas that is trapped in the ice. This is achieved with a mid-IR laser absorption spectrometer that provides simultaneous, high-precision measurements of CH4, N2O, CO2, and δ13C(CO2) and which will be coupled to a quantitative sublimation extraction method.
Natalie I. Keehan, Bellamy Brownwood, Andrey Marsavin, Douglas A. Day, and Juliane L. Fry
Atmos. Meas. Tech., 13, 6255–6269, https://doi.org/10.5194/amt-13-6255-2020, https://doi.org/10.5194/amt-13-6255-2020, 2020
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This paper describes a new instrument (a thermal-dissociation–cavity ring-down spectrometer, TD-CRDS) for the measurement of key atmospheric gaseous and particle-phase molecules containing the nitrate functional group. Several operational considerations affecting the measurements are described, as well as several characterization experiments comparing the TD-CRDS measurements to analogous measurements from other instruments. Examples are given using a TD-CRDS for ambient and laboratory studies.
Mohammed S. Alam, Leigh R. Crilley, James D. Lee, Louisa J. Kramer, Christian Pfrang, Mónica Vázquez-Moreno, Milagros Ródenas, Amalia Muñoz, and William J. Bloss
Atmos. Meas. Tech., 13, 5977–5991, https://doi.org/10.5194/amt-13-5977-2020, https://doi.org/10.5194/amt-13-5977-2020, 2020
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We report on the interference arising in measurements of nitrogen oxides (NOx) from the presence of a range of alkenes in sampled air when using the most widespread air quality monitoring technique for chemiluminescence detection. Interferences of up to 11 % are reported, depending upon the alkene present and conditions used. Such interferences may be of substantial importance for the interpretation of ambient NOx data, particularly for high volatile organic compound and low NOx environments.
Daniel Marno, Cheryl Ernest, Korbinian Hens, Umar Javed, Thomas Klimach, Monica Martinez, Markus Rudolf, Jos Lelieveld, and Hartwig Harder
Atmos. Meas. Tech., 13, 2711–2731, https://doi.org/10.5194/amt-13-2711-2020, https://doi.org/10.5194/amt-13-2711-2020, 2020
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In this study, a calibration device for OH and HO2 instruments is characterized at pressures of 275 to 1000 mbar, allowing instrument pressure sensitivity to be quantified to an accuracy of 22 % (1σ). Computational fluid dynamic simulations supporting the understanding of interactions between generated HOx and the instrument inlet led to enhanced determination of factors affecting instrument sensitivity.
Joschka Pfeifer, Mario Simon, Martin Heinritzi, Felix Piel, Lena Weitz, Dongyu Wang, Manuel Granzin, Tatjana Müller, Steffen Bräkling, Jasper Kirkby, Joachim Curtius, and Andreas Kürten
Atmos. Meas. Tech., 13, 2501–2522, https://doi.org/10.5194/amt-13-2501-2020, https://doi.org/10.5194/amt-13-2501-2020, 2020
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Ammonia is an important atmospheric trace gas that affects secondary aerosol formation and, together with sulfuric acid, the formation of new particles. A measurement technique is presented that uses high-resolution mass spectrometry and protonated water clusters for the ultrasensitive detection of ammonia at single-digit parts per trillion by volume levels. The instrument is further capable of measuring amines and a suite of iodine compounds at sub-parts per trillion by volume levels.
Roberto Sommariva, Louisa J. Kramer, Leigh R. Crilley, Mohammed S. Alam, and William J. Bloss
Atmos. Meas. Tech., 13, 1655–1670, https://doi.org/10.5194/amt-13-1655-2020, https://doi.org/10.5194/amt-13-1655-2020, 2020
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Ozone is a key atmospheric pollutant formed through chemical processing of natural and anthropogenic emissions and removed by reaction with organic compounds emitted by plants. We describe a new instrument – the
Total Ozone Reactivity Systemor TORS – that measures the total loss of ozone in the troposphere. The objective of the TORS instrument is to provide an estimate of the organic compounds emitted by plants which are not measured and thus to improve our understanding of the ozone budget.
John W. Birks, Andrew A. Turnipseed, Peter C. Andersen, Craig J. Williford, Stanley Strunk, Brian Carpenter, and Christine A. Ennis
Atmos. Meas. Tech., 13, 1001–1018, https://doi.org/10.5194/amt-13-1001-2020, https://doi.org/10.5194/amt-13-1001-2020, 2020
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We describe a portable calibration source of nitric oxide (NO) based on the photolysis of nitrous oxide. Combining this with a previous photolytic ozone (O3) source yields a calibrator that produces known mixing ratios of NO, O3, and nitrogen dioxide (NO2); NO2 is produced by the reaction of NO with O3. This portable
NO2/NO/O3 calibration source requires no external gas cylinders and can be used as a standard to calibrate O3 and NOx air pollution monitors in the field.
Thomas H. Speak, Mark A. Blitz, Daniel Stone, and Paul W. Seakins
Atmos. Meas. Tech., 13, 839–852, https://doi.org/10.5194/amt-13-839-2020, https://doi.org/10.5194/amt-13-839-2020, 2020
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OH and HO2 radicals are important trace constituents of the atmosphere that are closely coupled via several types of reaction. This paper describes a new laboratory method to simultaneously determine OH kinetics and HO2 yields from chemical processes. The instrument also provides some time resolution on HO2 detection allowing one to separate HO2 produced from the target reaction from HO2 arising from secondary chemistry. Examples of applications are presented.
Ece Satar, Peter Nyfeler, Bernhard Bereiter, Céline Pascale, Bernhard Niederhauser, and Markus Leuenberger
Atmos. Meas. Tech., 13, 101–117, https://doi.org/10.5194/amt-13-101-2020, https://doi.org/10.5194/amt-13-101-2020, 2020
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Good-quality measurements of atmospheric trace gases are only possible with regular calibrations and stable measurements from the standard cylinders. This study investigates instabilities due to surface effects on newly built aluminum and steel cylinders. We present measurements over a set of temperature and pressure ranges for the amount fractions of CO2, CO, CH4 and H2O using a commercial and a novel laser spectroscopic analyzer.
Ece Satar, Peter Nyfeler, Céline Pascale, Bernhard Niederhauser, and Markus Leuenberger
Atmos. Meas. Tech., 13, 119–130, https://doi.org/10.5194/amt-13-119-2020, https://doi.org/10.5194/amt-13-119-2020, 2020
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To ensure the best preparation and measurement conditions for trace gases, usage of coated materials is in demand in gas metrology and atmospheric measurement communities. In this article, the previously introduced aluminum measurement chamber is used to investigate materials such as glass, aluminum, copper, brass, steel and three different commercially available coatings. Our measurements focus on temperature and pressure dependencies for the species CO2, CO, CH4 and H2O using a CRDS analyzer.
Tanja J. Schuck, Ann-Katrin Blank, Elisa Rittmeier, Jonathan Williams, Carl A. M. Brenninkmeijer, Andreas Engel, and Andreas Zahn
Atmos. Meas. Tech., 13, 73–84, https://doi.org/10.5194/amt-13-73-2020, https://doi.org/10.5194/amt-13-73-2020, 2020
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Air sample collection aboard aircraft is a tool to measure atmospheric trace gas mixing ratios at altitude. We present results on the stability of 28 halocarbons during storage of air samples collected in stainless-steel flasks inside an automated air sampling unit which is part of the CARIBIC instrument package. Selected fluorinated compounds grew during the experiments while short-lived compounds were depleted. Individual substances were additionally influenced by high mixing ratios of ozone.
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Short summary
The analysis of trace gases in ambient air requires a preconcentration technique, in many cases to make the species of interest detectable and quantifiable. In this paper, such a preconcentration set-up is presented. Target species are trapped on adsorptive material cooled by a Stirling cooler which allows for a very low adsorption temperature but only requires electrical power. A simple and lightweight mechanical design guarantees very good suitability for remote-site field operation.
The analysis of trace gases in ambient air requires a preconcentration technique, in many cases...
