Articles | Volume 14, issue 3
https://doi.org/10.5194/acp-14-1463-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Special issue:
https://doi.org/10.5194/acp-14-1463-2014
© Author(s) 2014. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
| 
10 Feb 2014
Research article |
| 10 Feb 2014
Reconstruction of Northern Hemisphere 1950–2010 atmospheric non-methane hydrocarbons
D. Helmig
Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
V. Petrenko
Department of Earth and Environmental Sciences, University of Rochester, Rochester, USA
Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
P. Martinerie
UJF-Grenoble/CNRS, Laboratory for Glaciology and Geophysics of the Environment, Grenoble, France
E. Witrant
UJF-Grenoble/CNRS, Grenoble Image Parole Signal Automatique, St. Martin d'Hères, France
T. Röckmann
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, the Netherlands
A. Zuiderweg
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, the Netherlands
R. Holzinger
Institute for Marine and Atmospheric Research Utrecht, Utrecht University, the Netherlands
J. Hueber
Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
C. Thompson
Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
J. W. C. White
Institute of Arctic and Alpine Research, University of Colorado, Boulder, USA
W. Sturges
School of Environmental Sciences, University of East Anglia, Norwich, UK
Max Planck Institute for Chemistry, Mainz, Germany
T. Blunier
Niels Bohr Institute, University of Copenhagen, Denmark
D. Etheridge
Centre for Australian Weather and Climate Research, CSIRO Marine and Atmospheric Research, Aspendale, Australia
M. Rubino
Centre for Australian Weather and Climate Research, CSIRO Marine and Atmospheric Research, Aspendale, Australia
P. Tans
Global Monitoring Division, Earth Systems Research Laboratory, NOAA, Boulder, USA
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S. Preunkert, M. Legrand, M. M. Frey, A. Kukui, J. Savarino, H. Gallée, M. King, B. Jourdain, W. Vicars, and D. Helmig
Atmos. Chem. Phys., 15, 6689–6705, https://doi.org/10.5194/acp-15-6689-2015, https://doi.org/10.5194/acp-15-6689-2015, 2015
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K. Dzepina, C. Mazzoleni, P. Fialho, S. China, B. Zhang, R. C. Owen, D. Helmig, J. Hueber, S. Kumar, J. A. Perlinger, L. J. Kramer, M. P. Dziobak, M. T. Ampadu, S. Olsen, D. J. Wuebbles, and L. R. Mazzoleni
Atmos. Chem. Phys., 15, 5047–5068, https://doi.org/10.5194/acp-15-5047-2015, https://doi.org/10.5194/acp-15-5047-2015, 2015
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Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
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S. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20117-2014, https://doi.org/10.5194/acpd-14-20117-2014, 2014
Revised manuscript not accepted
P. Boylan, D. Helmig, and J.-H. Park
Atmos. Meas. Tech., 7, 1231–1244, https://doi.org/10.5194/amt-7-1231-2014, https://doi.org/10.5194/amt-7-1231-2014, 2014
B. Zhang, R. C. Owen, J. A. Perlinger, A. Kumar, S. Wu, M. Val Martin, L. Kramer, D. Helmig, and R. E. Honrath
Atmos. Chem. Phys., 14, 2267–2287, https://doi.org/10.5194/acp-14-2267-2014, https://doi.org/10.5194/acp-14-2267-2014, 2014
A. Kumar, S. Wu, M. F. Weise, R. Honrath, R. C. Owen, D. Helmig, L. Kramer, M. Val Martin, and Q. Li
Atmos. Chem. Phys., 13, 12537–12547, https://doi.org/10.5194/acp-13-12537-2013, https://doi.org/10.5194/acp-13-12537-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
L. Hu, D. B. Millet, S. Y. Kim, K. C. Wells, T. J. Griffis, E. V. Fischer, D. Helmig, J. Hueber, and A. J. Curtis
Atmos. Chem. Phys., 13, 3379–3392, https://doi.org/10.5194/acp-13-3379-2013, https://doi.org/10.5194/acp-13-3379-2013, 2013
Julien Westhoff, Johannes Freitag, Anaïs Orsi, Patricia Martinerie, Ilka Weikusat, Michael Dyonisius, Xavier Faïn, Kevin Fourteau, and Thomas Blunier
The Cryosphere, 18, 4379–4397, https://doi.org/10.5194/tc-18-4379-2024, https://doi.org/10.5194/tc-18-4379-2024, 2024
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Andrew O. Langford, Raul J. Alvarez II, Kenneth C. Aikin, Sunil Baidar, W. Alan Brewer, Steven S. Brown, Matthew M. Coggan, Patrick D. Cullis, Jessica Gilman, Georgios I. Gkatzelis, Detlev Helmig, Bryan J. Johnson, K. Emma Knowland, Rajesh Kumar, Aaron D. Lamplugh, Audra McClure-Begley, Brandi J. McCarty, Ann M. Middlebrook, Gabriele Pfister, Jeff Peischl, Irina Petropavlovskikh, Pamela S. Rickley, Andrew W. Rollins, Scott P. Sandberg, Christoph J. Senff, and Carsten Warneke
EGUsphere, https://doi.org/10.5194/egusphere-2024-1938, https://doi.org/10.5194/egusphere-2024-1938, 2024
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High ozone (O3) formed by reactions of nitrogen oxides (NOx) and volatile organic compounds (VOCs) can harm human health and welfare. High O3 is usually associated with hot summer days, but under certain conditions, high O3 can also form under winter conditions. In this study, we describe a high O3 event that occurred in Colorado during the COVID-19 quarantine that was caused in part by the decrease in traffic, and in part by a shallow inversion created by descent of stratospheric air.
Romilly Harris Stuart, Amaëlle Landais, Laurent Arnaud, Christo Buizert, Emilie Capron, Marie Dumont, Quentin Libois, Robert Mulvaney, Anaïs Orsi, Ghislain Picard, Frédéric Prié, Jeffrey Severinghaus, Barbara Stenni, and Patricia Martinerie
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Ice core δO2/N2 records are useful dating tools due to their local insolation pacing. A precise understanding of the physical mechanism driving this relationship, however, remain ambiguous. By compiling data from 15 polar sites, we find a strong dependence of mean δO2/N2 on accumulation rate and temperature in addition to the well-documented insolation dependence. Snowpack modelling is used to investigate which physical properties drive the mechanistic dependence on these local parameters.
Hossein Maazallahi, Foteini Stavropoulou, Samuel Jonson Sutanto, Michael Steiner, Dominik Brunner, Mariano Mertens, Patrick Jöckel, Antoon Visschedijk, Hugo Denier van der Gon, Stijn Dellaert, Nataly Velandia Salinas, Stefan Schwietzke, Daniel Zavala-Araiza, Sorin Ghemulet, Alexandru Pana, Magdalena Ardelean, Marius Corbu, Andreea Calcan, Stephen A. Conley, Mackenzie L. Smith, and Thomas Röckmann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2135, https://doi.org/10.5194/egusphere-2024-2135, 2024
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This article provide insights from airborne in-situ measurements during the ROMEO campaign with support from two model simulations. The results from the evaluations performed for this article are independently consistent with the results from previously published article which was based on ground-based measurements during the ROMEO campaign. The results show that reported methane emissions from oil and gas industry in Romania are largely under-reported to UNFCCC in 2019.
Maitane Iturrate-Garcia, Thérèse Salameh, Paul Schlauri, Annarita Baldan, Martin K. Vollmer, Evdokia Stratigou, Sebastian Dusanter, Jianrong Li, Stefan Persijn, Anja Claude, Rupert Holzinger, Christophe Sutour, Tatiana Macé, Yasin Elshorbany, Andreas Ackermann, Céline Pascale, and Stefan Reimann
EGUsphere, https://doi.org/10.5194/egusphere-2024-2236, https://doi.org/10.5194/egusphere-2024-2236, 2024
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Accurate and comparable measurements of oxygenated organic compounds (OVOCs) are crucial to assess tropospheric ozone burdens and trends. However, monitoring of many OVOCs remains challenging because of their low atmospheric abundance and lack of stable and traceable calibration standards. This research describes the calibration standards developed for selected OVOCs at low amount of substance fractions (<100 nmol mol-1) to transfer traceability to the international system of units to the field.
Vasilii V. Petrenko, Segev BenZvi, Michael Dyonisius, Benjamin Hmiel, Andrew M. Smith, and Christo Buizert
The Cryosphere, 18, 3439–3451, https://doi.org/10.5194/tc-18-3439-2024, https://doi.org/10.5194/tc-18-3439-2024, 2024
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This manuscript presents the concept for a new proxy for past variations in the galactic cosmic ray flux (GCR). Past variations in GCR flux are important to understand for interpretation of records of isotopes produced by cosmic rays; these records are used for reconstructing solar variations and past land ice extent. The proxy involves using measurements of 14CO in ice cores, which should provide an uncomplicated and precise estimate of past GCR flux variations for the past few thousand years.
Benjamin Hmiel, Vasilii V. Petrenko, Christo Buizert, Andrew M. Smith, Michael N. Dyonisius, Philip Place, Bin Yang, Quan Hua, Ross Beaudette, Jeffrey P. Severinghaus, Christina Harth, Ray F. Weiss, Lindsey Davidge, Melisa Diaz, Matthew Pacicco, James A. Menking, Michael Kalk, Xavier Faïn, Alden Adolph, Isaac Vimont, and Lee T. Murray
The Cryosphere, 18, 3363–3382, https://doi.org/10.5194/tc-18-3363-2024, https://doi.org/10.5194/tc-18-3363-2024, 2024
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The main aim of this research is to improve understanding of carbon-14 that is produced by cosmic rays in ice sheets. Measurements of carbon-14 in ice cores can provide a range of useful information (age of ice, past atmospheric chemistry, past cosmic ray intensity). Our results show that almost all (>99 %) of carbon-14 that is produced in the upper layer of ice sheets is rapidly lost to the atmosphere. Our results also provide better estimates of carbon-14 production rates in deeper ice.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
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Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Hella van Asperen, Thorsten Warneke, Alessandro Carioca de Araújo, Bruce Forsberg, Sávio José Filgueiras Ferreira, Thomas Röckmann, Carina van der Veen, Sipko Bulthuis, Leonardo Ramos de Oliveira, Thiago de Lima Xavier, Jailson da Mata, Marta de Oliveira Sá, Paulo Ricardo Teixeira, Julie Andrews de França e Silva, Susan Trumbore, and Justus Notholt
Biogeosciences, 21, 3183–3199, https://doi.org/10.5194/bg-21-3183-2024, https://doi.org/10.5194/bg-21-3183-2024, 2024
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Carbon monoxide (CO) is regarded as an important indirect greenhouse gas. Soils can emit and take up CO, but, until now, uncertainty remains as to which process dominates in tropical rainforests. We present the first soil CO flux measurements from a tropical rainforest. Based on our observations, we report that tropical rainforest soils are a net source of CO. In addition, we show that valley streams and inundated areas are likely additional hot spots of CO in the ecosystem.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
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The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Katrine A. Gorham, Sam Abernethy, Tyler R. Jones, Peter Hess, Natalie M. Mahowald, Daphne Meidan, Matthew S. Johnson, Maarten M. J. W. van Herpen, Yangyang Xu, Alfonso Saiz-Lopez, Thomas Röckmann, Chloe A. Brashear, Erika Reinhardt, and David Mann
Atmos. Chem. Phys., 24, 5659–5670, https://doi.org/10.5194/acp-24-5659-2024, https://doi.org/10.5194/acp-24-5659-2024, 2024
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Rapid reduction in atmospheric methane is needed to slow the rate of global warming. Reducing anthropogenic methane emissions is a top priority. However, atmospheric methane is also impacted by rising natural emissions and changing sinks. Studies of possible atmospheric methane removal approaches, such as iron salt aerosols to increase the chlorine radical sink, benefit from a roadmapped approach to understand if there may be viable and socially acceptable ways to decrease future risk.
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.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Phillip Place
EGUsphere, https://doi.org/10.5194/egusphere-2024-653, https://doi.org/10.5194/egusphere-2024-653, 2024
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Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry-climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
Alina Fiehn, Maximilian Eckl, Julian Kostinek, Michał Gałkowski, Christoph Gerbig, Michael Rothe, Thomas Röckmann, Malika Menoud, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Mila Stanisavljević, Justyna Swolkień, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 23, 15749–15765, https://doi.org/10.5194/acp-23-15749-2023, https://doi.org/10.5194/acp-23-15749-2023, 2023
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During the CoMet mission in the Upper Silesian Coal Basin (USCB) ground-based and airborne air samples were taken and analyzed for the isotopic composition of CH4 to derive the mean signature of the USCB and source signatures of individual coal mines. Using δ2H signatures, the biogenic emissions from the USCB account for 15 %–50 % of total emissions, which is underestimated in common emission inventories. This demonstrates the importance of δ2H-CH4 observations for methane source apportionment.
John D. Patterson, Murat Aydin, Andrew M. Crotwell, Gabrielle Pétron, Jeffery P. Severinghaus, Paul B. Krummel, Ray L. Langenfelds, Vasilii V. Petrenko, and Eric S. Saltzman
Clim. Past, 19, 2535–2550, https://doi.org/10.5194/cp-19-2535-2023, https://doi.org/10.5194/cp-19-2535-2023, 2023
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Atmospheric levels of molecular hydrogen (H2) can impact climate and air quality. Constraining past changes to atmospheric H2 is useful for understanding how H2 cycles through the Earth system and predicting the impacts of increasing anthropogenic emissions under the
hydrogen economy. Here, we use the aging air found in the polar snowpack to reconstruct H2 levels over the past 100 years. We find that H2 levels increased by 30 % over Greenland and 60 % over Antarctica during the 20th century.
Robbert P. J. Moonen, Getachew A. Adnew, Oscar K. Hartogensis, Jordi Vilà-Guerau de Arellano, David J. Bonell Fontas, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5787–5810, https://doi.org/10.5194/amt-16-5787-2023, https://doi.org/10.5194/amt-16-5787-2023, 2023
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Isotope fluxes allow for net ecosystem gas exchange fluxes to be partitioned into sub-components like plant assimilation, respiration and transpiration, which can help us better understand the environmental drivers of each partial flux. We share the results of a field campaign isotope fluxes were derived using a combination of laser spectroscopy and eddy covariance. We found lag times and high frequency signal loss in the isotope fluxes we derived and present methods to correct for both.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
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This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Xavier Faïn, David M. Etheridge, Kévin Fourteau, Patricia Martinerie, Cathy M. Trudinger, Rachael H. Rhodes, Nathan J. Chellman, Ray L. Langenfelds, Joseph R. McConnell, Mark A. J. Curran, Edward J. Brook, Thomas Blunier, Grégory Teste, Roberto Grilli, Anthony Lemoine, William T. Sturges, Boris Vannière, Johannes Freitag, and Jérôme Chappellaz
Clim. Past, 19, 2287–2311, https://doi.org/10.5194/cp-19-2287-2023, https://doi.org/10.5194/cp-19-2287-2023, 2023
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We report on a 3000-year record of carbon monoxide (CO) levels in the Southern Hemisphere's high latitudes by combining ice core and firn air measurements with modern direct atmospheric samples. Antarctica [CO] remained stable (–835 to 1500 CE), decreased during the Little Ice Age, and peaked around 1985 CE. Such evolution reflects stable biomass burning CO emissions before industrialization, followed by growth from CO anthropogenic sources, which decline after 1985 due to improved combustion.
Marie Bouchet, Amaëlle Landais, Antoine Grisart, Frédéric Parrenin, Frédéric Prié, Roxanne Jacob, Elise Fourré, Emilie Capron, Dominique Raynaud, Vladimir Ya Lipenkov, Marie-France Loutre, Thomas Extier, Anders Svensson, Etienne Legrain, Patricia Martinerie, Markus Leuenberger, Wei Jiang, Florian Ritterbusch, Zheng-Tian Lu, and Guo-Min Yang
Clim. Past, 19, 2257–2286, https://doi.org/10.5194/cp-19-2257-2023, https://doi.org/10.5194/cp-19-2257-2023, 2023
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A new federative chronology for five deep polar ice cores retrieves 800 000 years of past climate variations with improved accuracy. Precise ice core timescales are key to studying the mechanisms linking changes in the Earth’s orbit to the diverse climatic responses (temperature and atmospheric greenhouse gas concentrations). To construct the chronology, new measurements from the oldest continuous ice core as well as glaciological modeling estimates were combined in a statistical model.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech., 16, 5051–5073, https://doi.org/10.5194/amt-16-5051-2023, https://doi.org/10.5194/amt-16-5051-2023, 2023
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Measurement methods are increasingly deployed to verify reported methane emissions of gas leaks. This study describes unique advantages and limitations of three methods. Two methods are rapidly deployed, but uncertainties and biases exist for some leak locations. In contrast, the suction method could accurately determine leak rates in principle. However, this method, which provides data for the German emission inventory, creates an overall low bias in our study due to non-random site selection.
Tim René de Groot, Anne Margriet Mol, Katherine Mesdag, Pierre Ramond, Rachel Ndhlovu, Julia Catherine Engelmann, Thomas Röckmann, and Helge Niemann
Biogeosciences, 20, 3857–3872, https://doi.org/10.5194/bg-20-3857-2023, https://doi.org/10.5194/bg-20-3857-2023, 2023
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This study investigates methane dynamics in the Wadden Sea. Our measurements revealed distinct variations triggered by seasonality and tidal forcing. The methane budget was higher in warmer seasons but surprisingly high in colder seasons. Methane dynamics were amplified during low tides, flushing the majority of methane into the North Sea or releasing it to the atmosphere. Methanotrophic activity was also elevated during low tide but mitigated only a small fraction of the methane efflux.
Foteini Stavropoulou, Katarina Vinković, Bert Kers, Marcel de Vries, Steven van Heuven, Piotr Korbeń, Martina Schmidt, Julia Wietzel, Pawel Jagoda, Jaroslav M. Necki, Jakub Bartyzel, Hossein Maazallahi, Malika Menoud, Carina van der Veen, Sylvia Walter, Béla Tuzson, Jonas Ravelid, Randulph Paulo Morales, Lukas Emmenegger, Dominik Brunner, Michael Steiner, Arjan Hensen, Ilona Velzeboer, Pim van den Bulk, Hugo Denier van der Gon, Antonio Delre, Maklawe Essonanawe Edjabou, Charlotte Scheutz, Marius Corbu, Sebastian Iancu, Denisa Moaca, Alin Scarlat, Alexandru Tudor, Ioana Vizireanu, Andreea Calcan, Magdalena Ardelean, Sorin Ghemulet, Alexandru Pana, Aurel Constantinescu, Lucian Cusa, Alexandru Nica, Calin Baciu, Cristian Pop, Andrei Radovici, Alexandru Mereuta, Horatiu Stefanie, Alexandru Dandocsi, Bas Hermans, Stefan Schwietzke, Daniel Zavala-Araiza, Huilin Chen, and Thomas Röckmann
Atmos. Chem. Phys., 23, 10399–10412, https://doi.org/10.5194/acp-23-10399-2023, https://doi.org/10.5194/acp-23-10399-2023, 2023
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In this study, we quantify CH4 emissions from onshore oil production sites in Romania at source and facility level using a combination of ground- and drone-based measurement techniques. We show that the total CH4 emissions in our studied areas are much higher than the emissions reported to UNFCCC, and up to three-quarters of the detected emissions are related to operational venting. Our results suggest that oil and gas production infrastructure in Romania holds a massive mitigation potential.
Brandon Bottorff, Michelle M. Lew, Youngjun Woo, Pamela Rickly, Matthew D. Rollings, Benjamin Deming, Daniel C. Anderson, Ezra Wood, Hariprasad D. Alwe, Dylan B. Millet, Andrew Weinheimer, Geoff Tyndall, John Ortega, Sebastien Dusanter, Thierry Leonardis, James Flynn, Matt Erickson, Sergio Alvarez, Jean C. Rivera-Rios, Joshua D. Shutter, Frank Keutsch, Detlev Helmig, Wei Wang, Hannah M. Allen, Johnathan H. Slade, Paul B. Shepson, Steven Bertman, and Philip S. Stevens
Atmos. Chem. Phys., 23, 10287–10311, https://doi.org/10.5194/acp-23-10287-2023, https://doi.org/10.5194/acp-23-10287-2023, 2023
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The hydroxyl (OH), hydroperoxy (HO2), and organic peroxy (RO2) radicals play important roles in atmospheric chemistry and have significant air quality implications. Here, we compare measurements of OH, HO2, and total peroxy radicals (XO2) made in a remote forest in Michigan, USA, to predictions from a series of chemical models. Lower measured radical concentrations suggest that the models may be missing an important radical sink and overestimating the rate of ozone production in this forest.
Farhan R. Nursanto, Roy Meinen, Rupert Holzinger, Maarten C. Krol, Xinya Liu, Ulrike Dusek, Bas Henzing, and Juliane L. Fry
Atmos. Chem. Phys., 23, 10015–10034, https://doi.org/10.5194/acp-23-10015-2023, https://doi.org/10.5194/acp-23-10015-2023, 2023
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Particulate matter (PM) is a harmful air pollutant that depends on the complex mixture of natural and anthropogenic emissions into the atmosphere. Thus, in different regions and seasons, the way that PM is formed and grows can differ. In this study, we use a combined statistical analysis of the chemical composition and particle size distribution to determine what drives particle formation and growth across seasons, using varying wind directions to elucidate the role of different sources.
Andreas Forstmaier, Jia Chen, Florian Dietrich, Juan Bettinelli, Hossein Maazallahi, Carsten Schneider, Dominik Winkler, Xinxu Zhao, Taylor Jones, Carina van der Veen, Norman Wildmann, Moritz Makowski, Aydin Uzun, Friedrich Klappenbach, Hugo Denier van der Gon, Stefan Schwietzke, and Thomas Röckmann
Atmos. Chem. Phys., 23, 6897–6922, https://doi.org/10.5194/acp-23-6897-2023, https://doi.org/10.5194/acp-23-6897-2023, 2023
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Large cities emit greenhouse gases which contribute to global warming. In this study, we measured the release of one important green house gas, methane, in Hamburg. Multiple sources that contribute to methane emissions were located and quantified. Methane sources were found to be mainly caused by human activity (e.g., by release from oil and gas refineries). Moreover, potential natural sources have been located, such as the Elbe River and lakes.
Truls Andersen, Zhao Zhao, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys., 23, 5191–5216, https://doi.org/10.5194/acp-23-5191-2023, https://doi.org/10.5194/acp-23-5191-2023, 2023
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The Upper Silesian Coal Basin, Poland, is one of the hot spots of methane emissions in Europe. Using an uncrewed aerial vehicle (UAV), we performed atmospheric measurements of methane concentrations downwind of five ventilation shafts in this region and determined the emission rates from the individual shafts. We found a strong correlation between quantified shaft-averaged emission rates and hourly inventory data, which also allows us to estimate the methane emissions from the entire region.
Christo Buizert, Sarah Shackleton, Jeffrey P. Severinghaus, William H. G. Roberts, Alan Seltzer, Bernhard Bereiter, Kenji Kawamura, Daniel Baggenstos, Anaïs J. Orsi, Ikumi Oyabu, Benjamin Birner, Jacob D. Morgan, Edward J. Brook, David M. Etheridge, David Thornton, Nancy Bertler, Rebecca L. Pyne, Robert Mulvaney, Ellen Mosley-Thompson, Peter D. Neff, and Vasilii V. Petrenko
Clim. Past, 19, 579–606, https://doi.org/10.5194/cp-19-579-2023, https://doi.org/10.5194/cp-19-579-2023, 2023
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It is unclear how different components of the global atmospheric circulation, such as the El Niño effect, respond to large-scale climate change. We present a new ice core gas proxy, called krypton-86 excess, that reflects past storminess in Antarctica. We present data from 11 ice cores that suggest the new proxy works. We present a reconstruction of changes in West Antarctic storminess over the last 24 000 years and suggest these are caused by north–south movement of the tropical rain belt.
David R. Worton, Sergi Moreno, Kieran O'Daly, and Rupert Holzinger
Atmos. Meas. Tech., 16, 1061–1072, https://doi.org/10.5194/amt-16-1061-2023, https://doi.org/10.5194/amt-16-1061-2023, 2023
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Proton-transfer-reaction mass spectrometry is widely used in the environmental, health, and food and beverage sectors. As a result, there is a need for accurate and comparable measurements. In this work we have developed a 20-component gravimetrically prepared traceable primary reference material (gas standard in a high-pressure cylinder) to enable quantitative and comparable measurements. The accuracy of all components was better than 3 %–10 % with stabilities of better than 1–2 years.
Michael N. Dyonisius, Vasilii V. Petrenko, Andrew M. Smith, Benjamin Hmiel, Peter D. Neff, Bin Yang, Quan Hua, Jochen Schmitt, Sarah A. Shackleton, Christo Buizert, Philip F. Place, James A. Menking, Ross Beaudette, Christina Harth, Michael Kalk, Heidi A. Roop, Bernhard Bereiter, Casey Armanetti, Isaac Vimont, Sylvia Englund Michel, Edward J. Brook, Jeffrey P. Severinghaus, Ray F. Weiss, and Joseph R. McConnell
The Cryosphere, 17, 843–863, https://doi.org/10.5194/tc-17-843-2023, https://doi.org/10.5194/tc-17-843-2023, 2023
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Cosmic rays that enter the atmosphere produce secondary particles which react with surface minerals to produce radioactive nuclides. These nuclides are often used to constrain Earth's surface processes. However, the production rates from muons are not well constrained. We measured 14C in ice with a well-known exposure history to constrain the production rates from muons. 14C production in ice is analogous to quartz, but we obtain different production rates compared to commonly used estimates.
Bryce F. J. Kelly, Xinyi Lu, Stephen J. Harris, Bruno G. Neininger, Jorg M. Hacker, Stefan Schwietzke, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Carina van der Veen, Malika Menoud, and Thomas Röckmann
Atmos. Chem. Phys., 22, 15527–15558, https://doi.org/10.5194/acp-22-15527-2022, https://doi.org/10.5194/acp-22-15527-2022, 2022
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This study explores using the composition of methane of in-flight atmospheric air samples for greenhouse gas inventory verification. The air samples were collected above one of the largest coal seam gas production regions in the world. Adjacent to these gas fields are coal mines, Australia's largest cattle feedlot, and over 1 million grazing cattle. The results are also used to identify methane mitigation opportunities.
Vanessa Selimovic, Damien Ketcherside, Sreelekha Chaliyakunnel, Catherine Wielgasz, Wade Permar, Hélène Angot, Dylan B. Millet, Alan Fried, Detlev Helmig, and Lu Hu
Atmos. Chem. Phys., 22, 14037–14058, https://doi.org/10.5194/acp-22-14037-2022, https://doi.org/10.5194/acp-22-14037-2022, 2022
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Arctic warming has led to an increase in plants that emit gases in response to stress, but how these gases affect regional chemistry is largely unknown due to lack of observational data. Here we present the most comprehensive gas-phase measurements for this area to date and compare them to predictions from a global transport model. We report 78 gas-phase species and investigate their importance to atmospheric chemistry in the area, with broader implications for similar plant types.
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.
Malika Menoud, Carina van der Veen, Dave Lowry, Julianne M. Fernandez, Semra Bakkaloglu, James L. France, Rebecca E. Fisher, Hossein Maazallahi, Mila Stanisavljević, Jarosław Nęcki, Katarina Vinkovic, Patryk Łakomiec, Janne Rinne, Piotr Korbeń, Martina Schmidt, Sara Defratyka, Camille Yver-Kwok, Truls Andersen, Huilin Chen, and Thomas Röckmann
Earth Syst. Sci. Data, 14, 4365–4386, https://doi.org/10.5194/essd-14-4365-2022, https://doi.org/10.5194/essd-14-4365-2022, 2022
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Emission sources of methane (CH4) can be distinguished with measurements of CH4 stable isotopes. We present new measurements of isotope signatures of various CH4 sources in Europe, mainly anthropogenic, sampled from 2017 to 2020. The present database also contains the most recent update of the global signature dataset from the literature. The dataset improves CH4 source attribution and the understanding of the global CH4 budget.
Albane Barbero, Roberto Grilli, Markus M. Frey, Camille Blouzon, Detlev Helmig, Nicolas Caillon, and Joël Savarino
Atmos. Chem. Phys., 22, 12025–12054, https://doi.org/10.5194/acp-22-12025-2022, https://doi.org/10.5194/acp-22-12025-2022, 2022
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The high reactivity of the summer Antarctic boundary layer results in part from the emissions of nitrogen oxides produced during photo-denitrification of the snowpack, but its underlying mechanisms are not yet fully understood. The results of this study suggest that more NO2 is produced from the snowpack early in the photolytic season, possibly due to stronger UV irradiance caused by a smaller solar zenith angle near the solstice.
Xavier Faïn, Rachael H. Rhodes, Philip Place, Vasilii V. Petrenko, Kévin Fourteau, Nathan Chellman, Edward Crosier, Joseph R. McConnell, Edward J. Brook, Thomas Blunier, Michel Legrand, and Jérôme Chappellaz
Clim. Past, 18, 631–647, https://doi.org/10.5194/cp-18-631-2022, https://doi.org/10.5194/cp-18-631-2022, 2022
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Carbon monoxide (CO) is a regulated pollutant and one of the key components determining the oxidizing capacity of the atmosphere. In this study, we analyzed five ice cores from Greenland at high resolution for CO concentrations by coupling laser spectrometry with continuous melting. By combining these new datasets, we produced an upper-bound estimate of past atmospheric CO abundance since preindustrial times for the Northern Hemisphere high latitudes, covering the period from 1700 to 1957 CE.
Stephen M. Platt, Øystein Hov, Torunn Berg, Knut Breivik, Sabine Eckhardt, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Markus Fiebig, Rebecca Fisher, Georg Hansen, Hans-Christen Hansson, Jost Heintzenberg, Ove Hermansen, Dominic Heslin-Rees, Kim Holmén, Stephen Hudson, Roland Kallenborn, Radovan Krejci, Terje Krognes, Steinar Larssen, David Lowry, Cathrine Lund Myhre, Chris Lunder, Euan Nisbet, Pernilla B. Nizzetto, Ki-Tae Park, Christina A. Pedersen, Katrine Aspmo Pfaffhuber, Thomas Röckmann, Norbert Schmidbauer, Sverre Solberg, Andreas Stohl, Johan Ström, Tove Svendby, Peter Tunved, Kjersti Tørnkvist, Carina van der Veen, Stergios Vratolis, Young Jun Yoon, Karl Espen Yttri, Paul Zieger, Wenche Aas, and Kjetil Tørseth
Atmos. Chem. Phys., 22, 3321–3369, https://doi.org/10.5194/acp-22-3321-2022, https://doi.org/10.5194/acp-22-3321-2022, 2022
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Here we detail the history of the Zeppelin Observatory, a unique global background site and one of only a few in the high Arctic. We present long-term time series of up to 30 years of atmospheric components and atmospheric transport phenomena. Many of these time series are important to our understanding of Arctic and global atmospheric composition change. Finally, we discuss the future of the Zeppelin Observatory and emerging areas of future research on the Arctic atmosphere.
Charel Wohl, Anna E. Jones, William T. Sturges, Philip D. Nightingale, Brent Else, Brian J. Butterworth, and Mingxi Yang
Biogeosciences, 19, 1021–1045, https://doi.org/10.5194/bg-19-1021-2022, https://doi.org/10.5194/bg-19-1021-2022, 2022
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We measured concentrations of five different organic gases in seawater in the high Arctic during summer. We found higher concentrations near the surface of the water column (top 5–10 m) and in areas of partial ice cover. This suggests that sea ice influences the concentrations of these gases. These gases indirectly exert a slight cooling effect on the climate, and it is therefore important to measure the levels accurately for future climate predictions.
Rupert Holzinger, Oliver Eppers, Kouji Adachi, Heiko Bozem, Markus Hartmann, Andreas Herber, Makoto Koike, Dylan B. Millet, Nobuhiro Moteki, Sho Ohata, Frank Stratmann, and Atsushi Yoshida
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-95, https://doi.org/10.5194/acp-2022-95, 2022
Revised manuscript not accepted
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In spring 2018 the research aircraft Polar 5 conducted flights in the Arctic atmosphere. The flight operation was from Station Nord in Greenland, 1700 km north of the Arctic Circle (81°43'N, 17°47'W). Using a mass spectrometer we measured more than 100 organic compounds in the air. We found a clear signature of natural organic compounds that are transported from forests to the high Arctic. These compounds have the potential to change the cloud cover and energy budget of the Arctic region.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-68, https://doi.org/10.5194/acp-2022-68, 2022
Publication in ACP not foreseen
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The sulfur isotopes (32S and 34S) were studied to understand the sources, sinks and processes of carbonyl sulphide (COS) in the atmosphere. COS is an important source of sulfur aerosol in the stratosphere (SSA). Few measurements of COS and SSA exist, but with our 1D model, we were able to match them and show the importance of COS to sulfate formation. Moreover, we are able to highlight some important processes for the COS budget and where measurements may fill a gap in current knowledge.
Sarah Shackleton, James A. Menking, Edward Brook, Christo Buizert, Michael N. Dyonisius, Vasilii V. Petrenko, Daniel Baggenstos, and Jeffrey P. Severinghaus
Clim. Past, 17, 2273–2289, https://doi.org/10.5194/cp-17-2273-2021, https://doi.org/10.5194/cp-17-2273-2021, 2021
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In this study, we measure atmospheric noble gases trapped in ice cores to reconstruct ocean temperature during the last glaciation. Comparing the new reconstruction to other climate records, we show that the ocean reached its coldest temperatures before ice sheets reached maximum volumes and atmospheric CO2 reached its lowest concentrations. Ocean cooling played a major role in lowering atmospheric CO2 early in the glaciation, but it only played a minor role later.
Hélène Angot, Connor Davel, Christine Wiedinmyer, Gabrielle Pétron, Jashan Chopra, Jacques Hueber, Brendan Blanchard, Ilann Bourgeois, Isaac Vimont, Stephen A. Montzka, Ben R. Miller, James W. Elkins, and Detlev Helmig
Atmos. Chem. Phys., 21, 15153–15170, https://doi.org/10.5194/acp-21-15153-2021, https://doi.org/10.5194/acp-21-15153-2021, 2021
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After a multidecadal global decline in atmospheric abundance of ethane and propane (precursors of tropospheric ozone and aerosols), previous work showed a reversal of this trend in 2009–2015 in the Northern Hemisphere due to the growth in oil and natural gas production in North America. Here we show a temporary pause in the growth of atmospheric ethane and propane in 2015–2018 and highlight the critical need for additional top-down studies to further constrain ethane and propane emissions.
Malika Menoud, Carina van der Veen, Jaroslaw Necki, Jakub Bartyzel, Barbara Szénási, Mila Stanisavljević, Isabelle Pison, Philippe Bousquet, and Thomas Röckmann
Atmos. Chem. Phys., 21, 13167–13185, https://doi.org/10.5194/acp-21-13167-2021, https://doi.org/10.5194/acp-21-13167-2021, 2021
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Using measurements of methane isotopes in ambient air and a 3D atmospheric transport model, in Krakow, Poland, we mainly detected fossil-fuel-related sources, coming from coal mining in Silesia and from the use of natural gas in the city. Emission inventories report large emissions from coal mine activity in Silesia, which is in agreement with our measurements. However, methane sources in the urban area of Krakow related to the use of fossil fuels might be underestimated in the inventories.
Xinyi Lu, Stephen J. Harris, Rebecca E. Fisher, James L. France, Euan G. Nisbet, David Lowry, Thomas Röckmann, Carina van der Veen, Malika Menoud, Stefan Schwietzke, and Bryce F. J. Kelly
Atmos. Chem. Phys., 21, 10527–10555, https://doi.org/10.5194/acp-21-10527-2021, https://doi.org/10.5194/acp-21-10527-2021, 2021
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Many coal seam gas (CSG) facilities in the Surat Basin, Australia, are adjacent to other sources of methane, including agricultural, urban, and natural seeps. This makes it challenging to estimate the amount of methane being emitted into the atmosphere from CSG facilities. This research demonstrates that measurements of the carbon and hydrogen stable isotopic composition of methane can distinguish between and apportion methane emissions from CSG facilities, cattle, and many other sources.
Max Thomas, Johannes C. Laube, Jan Kaiser, Samuel Allin, Patricia Martinerie, Robert Mulvaney, Anna Ridley, Thomas Röckmann, William T. Sturges, and Emmanuel Witrant
Atmos. Chem. Phys., 21, 6857–6873, https://doi.org/10.5194/acp-21-6857-2021, https://doi.org/10.5194/acp-21-6857-2021, 2021
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CFC gases are destroying the Earth's life-protecting ozone layer. We improve understanding of CFC destruction by measuring the isotopic fingerprint of the carbon in the three most abundant CFCs. These are the first such measurements in the main region where CFCs are destroyed – the stratosphere. We reconstruct the atmospheric isotope histories of these CFCs back to the 1950s by measuring air extracted from deep snow and using a model. The model and the measurements are generally consistent.
Vasilii V. Petrenko, Andrew M. Smith, Edward M. Crosier, Roxana Kazemi, Philip Place, Aidan Colton, Bin Yang, Quan Hua, and Lee T. Murray
Atmos. Meas. Tech., 14, 2055–2063, https://doi.org/10.5194/amt-14-2055-2021, https://doi.org/10.5194/amt-14-2055-2021, 2021
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This paper presents an improved methodology for measurements of atmospheric concentration of carbon-14-containing carbon monoxide (14CO), as well as a 1-year dataset that demonstrates the methodology. Atmospheric 14CO concentration measurements are useful for improving the understanding of spatial and temporal variability of hydroxyl radical concentrations. Key improvements over prior methods include a greatly reduced air sample size and accurate procedural blank characterization.
Jakob B. Pernov, Rossana Bossi, Thibaut Lebourgeois, Jacob K. Nøjgaard, Rupert Holzinger, Jens L. Hjorth, and Henrik Skov
Atmos. Chem. Phys., 21, 2895–2916, https://doi.org/10.5194/acp-21-2895-2021, https://doi.org/10.5194/acp-21-2895-2021, 2021
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Volatile organic compounds (VOCs) are an important constituent in the Arctic atmosphere due to their effect on aerosol and ozone formation. However, an understanding of their sources is lacking. This research presents a multiseason high-time-resolution dataset of VOCs in the Arctic and details their temporal characteristics and source apportionment. Four sources were identified: biomass burning, marine cryosphere, background, and Arctic haze.
Ashok K. Luhar, David M. Etheridge, Zoë M. Loh, Julie Noonan, Darren Spencer, Lisa Smith, and Cindy Ong
Atmos. Chem. Phys., 20, 15487–15511, https://doi.org/10.5194/acp-20-15487-2020, https://doi.org/10.5194/acp-20-15487-2020, 2020
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With the sharp rise in coal seam gas (CSG) production in Queensland’s Surat Basin, there is much interest in quantifying methane emissions from this area and from unconventional gas production in general. We develop and apply a regional Bayesian inverse model that uses hourly methane concentration data from two sites and modelled backward dispersion to quantify emissions. The model requires a narrow prior and suggests that the emissions from the CSG areas are 33% larger than bottom-up estimates.
Hélène Angot, Katelyn McErlean, Lu Hu, Dylan B. Millet, Jacques Hueber, Kaixin Cui, Jacob Moss, Catherine Wielgasz, Tyler Milligan, Damien Ketcherside, M. Syndonia Bret-Harte, and Detlev Helmig
Biogeosciences, 17, 6219–6236, https://doi.org/10.5194/bg-17-6219-2020, https://doi.org/10.5194/bg-17-6219-2020, 2020
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We report biogenic volatile organic compounds (BVOCs) ambient levels and emission rates from key vegetation species in the Alaskan arctic tundra, providing a new data set to further constrain isoprene chemistry under low NOx conditions in models. We add to the growing body of evidence that climate-induced changes in the vegetation composition will significantly affect the BVOC emission potential of the tundra, with implications for atmospheric oxidation processes and climate feedbacks.
Hossein Maazallahi, Julianne M. Fernandez, Malika Menoud, Daniel Zavala-Araiza, Zachary D. Weller, Stefan Schwietzke, Joseph C. von Fischer, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 14717–14740, https://doi.org/10.5194/acp-20-14717-2020, https://doi.org/10.5194/acp-20-14717-2020, 2020
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Methane accounts for ∼ 25 % of current climate warming. The current lack of methane measurements is a barrier for tracking major sources, which are key for near-term climate mitigation. We use mobile measurements to identify and quantify methane emission sources in Utrecht (NL) and Hamburg (DE) with a focus on natural gas pipeline leaks. The measurements resulted in fixing the major leaks by the local utility, but coordinated efforts are needed at national levels for further emission reductions.
Joram J. D. Hooghiem, Maria Elena Popa, Thomas Röckmann, Jens-Uwe Grooß, Ines Tritscher, Rolf Müller, Rigel Kivi, and Huilin Chen
Atmos. Chem. Phys., 20, 13985–14003, https://doi.org/10.5194/acp-20-13985-2020, https://doi.org/10.5194/acp-20-13985-2020, 2020
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Wildfires release a large quantity of pollutants that can reach the stratosphere through pyro-convection events. In September 2017, a stratospheric plume was accidentally sampled during balloon soundings in northern Finland. The source of the plume was identified to be wildfire smoke based on in situ measurements of carbon monoxide (CO) and stable isotope analysis of CO. Furthermore, the age of the plume was estimated using backwards transport modelling to be ~24 d, with its origin in Canada.
Alina Fiehn, Julian Kostinek, Maximilian Eckl, Theresa Klausner, Michał Gałkowski, Jinxuan Chen, Christoph Gerbig, Thomas Röckmann, Hossein Maazallahi, Martina Schmidt, Piotr Korbeń, Jarosław Neçki, Pawel Jagoda, Norman Wildmann, Christian Mallaun, Rostyslav Bun, Anna-Leah Nickl, Patrick Jöckel, Andreas Fix, and Anke Roiger
Atmos. Chem. Phys., 20, 12675–12695, https://doi.org/10.5194/acp-20-12675-2020, https://doi.org/10.5194/acp-20-12675-2020, 2020
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A severe reduction of greenhouse gas emissions is necessary to fulfill the Paris Agreement. We use aircraft- and ground-based in situ observations of trace gases and wind speed from two flights over the Upper Silesian Coal Basin, Poland, for independent emission estimation. The derived methane emission estimates are within the range of emission inventories, carbon dioxide estimates are in the lower range and carbon monoxide emission estimates are slightly higher than emission inventory values.
Wei Wang, Laurens Ganzeveld, Samuel Rossabi, Jacques Hueber, and Detlev Helmig
Atmos. Chem. Phys., 20, 11287–11304, https://doi.org/10.5194/acp-20-11287-2020, https://doi.org/10.5194/acp-20-11287-2020, 2020
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Trees exchange with the atmosphere nitrogen oxides and ozone, affecting the tropospheric composition and consequently air quality and ecosystem health. We examined the leaf-level gas exchanges for four typical tree species (pine, maple, oak, aspen) found in northern Michigan, US. The leaves largely absorb the gases, showing little evidence of emission. We measured the uptake rates that can be used to improve model studies of the source and sink processes controlling these gases in forests.
Patrick Dewald, Jonathan M. Liebmann, Nils Friedrich, Justin Shenolikar, Jan Schuladen, Franz Rohrer, David Reimer, Ralf Tillmann, Anna Novelli, Changmin Cho, Kangming Xu, Rupert Holzinger, François Bernard, Li Zhou, Wahid Mellouki, Steven S. Brown, Hendrik Fuchs, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 20, 10459–10475, https://doi.org/10.5194/acp-20-10459-2020, https://doi.org/10.5194/acp-20-10459-2020, 2020
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We present direct measurements of NO3 reactivity resulting from the oxidation of isoprene by NO3 during an intensive simulation chamber study. Measurements were in excellent agreement with values calculated from measured isoprene amounts and the rate coefficient for the reaction of NO3 with isoprene. Comparison of the measurement with NO3 reactivities from non-steady-state and model calculations suggests that isoprene-derived RO2 and HO2 radicals account to ~ 50 % of overall NO3 losses.
Jordi Vilà-Guerau de Arellano, Patrizia Ney, Oscar Hartogensis, Hugo de Boer, Kevin van Diepen, Dzhaner Emin, Geiske de Groot, Anne Klosterhalfen, Matthias Langensiepen, Maria Matveeva, Gabriela Miranda-García, Arnold F. Moene, Uwe Rascher, Thomas Röckmann, Getachew Adnew, Nicolas Brüggemann, Youri Rothfuss, and Alexander Graf
Biogeosciences, 17, 4375–4404, https://doi.org/10.5194/bg-17-4375-2020, https://doi.org/10.5194/bg-17-4375-2020, 2020
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The CloudRoots field experiment has obtained an open comprehensive observational data set that includes soil, plant, and atmospheric variables to investigate the interactions between a heterogeneous land surface and its overlying atmospheric boundary layer, including the rapid perturbations of clouds in evapotranspiration. Our findings demonstrate that in order to understand and represent diurnal variability, we need to measure and model processes from the leaf to the landscape scales.
Johannes C. Laube, Emma C. Leedham Elvidge, Karina E. Adcock, Bianca Baier, Carl A. M. Brenninkmeijer, Huilin Chen, Elise S. Droste, Jens-Uwe Grooß, Pauli Heikkinen, Andrew J. Hind, Rigel Kivi, Alexander Lojko, Stephen A. Montzka, David E. Oram, Steve Randall, Thomas Röckmann, William T. Sturges, Colm Sweeney, Max Thomas, Elinor Tuffnell, and Felix Ploeger
Atmos. Chem. Phys., 20, 9771–9782, https://doi.org/10.5194/acp-20-9771-2020, https://doi.org/10.5194/acp-20-9771-2020, 2020
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We demonstrate that AirCore technology, which is based on small low-cost balloons, can provide access to trace gas measurements such as CFCs at ultra-low abundances. This is a new way to quantify ozone-depleting, and related, substances in the stratosphere, which is largely inaccessible to aircraft. We show two potential uses: (a) tracking the stratospheric circulation, which is predicted to change, and (b) assessing three common meteorological reanalyses driving a global stratospheric model.
Dean Howard, Yannick Agnan, Detlev Helmig, Yu Yang, and Daniel Obrist
Biogeosciences, 17, 4025–4042, https://doi.org/10.5194/bg-17-4025-2020, https://doi.org/10.5194/bg-17-4025-2020, 2020
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The Arctic tundra represents a vast store of carbon that may be broken down by microbial activity into greenhouse gases such as CO2 and CH4. Though microbes are less active in winter, the long duration of the cold season makes this period very important for carbon cycling. We show that, under conditions of warmer winter air temperatures and greater snowfall, deeper soils can remain warm enough to sustain significantly enhanced CH4 emission. This could have large implications for future climates.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922, https://doi.org/10.5194/bg-17-3903-2020, https://doi.org/10.5194/bg-17-3903-2020, 2020
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We measured the effect of photosynthesis, the largest flux in the carbon cycle, on the triple oxygen isotope composition of atmospheric CO2 at the leaf level during gas exchange using three plant species. The main factors that limit the impact of land vegetation on the triple oxygen isotope composition of atmospheric CO2 are identified, characterized and discussed. The effect of photosynthesis on the isotopic composition of CO2 is commonly quantified as discrimination (ΔA).
Kévin Fourteau, Laurent Arnaud, Xavier Faïn, Patricia Martinerie, David M. Etheridge, Vladimir Lipenkov, and Jean-Marc Barnola
Earth Syst. Sci. Data, 12, 1171–1177, https://doi.org/10.5194/essd-12-1171-2020, https://doi.org/10.5194/essd-12-1171-2020, 2020
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Measurements of the porosity of three polar firns were conducted in the 1990s by Jean-Marc Barnola using the method of gas pycnometry. From these data, a parametrization of firn pore closure was produced and used in different published articles. However, the data have not been published in their own right yet. We have made the data publicly accessible on the PANGAEA database and here propose describing how they were obtained and used to produce the pore closure parametrization.
Charel Wohl, Ian Brown, Vassilis Kitidis, Anna E. Jones, William T. Sturges, Philip D. Nightingale, and Mingxi Yang
Biogeosciences, 17, 2593–2619, https://doi.org/10.5194/bg-17-2593-2020, https://doi.org/10.5194/bg-17-2593-2020, 2020
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The oceans represent a poorly understood source of organic carbon to the atmosphere. In this paper, we present ship-based measurements of specific compounds in ambient air and seawater of the Southern Ocean. We present fluxes of these gases between air and sea at very high resolution. The data also contain evidence for day and night variations in some of these compounds. These measurements can be used to better understand the role of the Southern Ocean in the cycling of these compounds.
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.
Ryan J. Pound, Tomás Sherwen, Detlev Helmig, Lucy J. Carpenter, and Mat J. Evans
Atmos. Chem. Phys., 20, 4227–4239, https://doi.org/10.5194/acp-20-4227-2020, https://doi.org/10.5194/acp-20-4227-2020, 2020
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Ozone is an important pollutant with impacts on health and the environment. Ozone is lost to plants, land and the oceans. Loss to the ocean is slow compared to all other types of land cover and has not received as much attention. We build on previous work to more accurately model ozone loss to the ocean. We find changes in the concentration of ozone over the oceans, notably the Southern Ocean, which improves model performance.
Jia Chen, Florian Dietrich, Hossein Maazallahi, Andreas Forstmaier, Dominik Winkler, Magdalena E. G. Hofmann, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Chem. Phys., 20, 3683–3696, https://doi.org/10.5194/acp-20-3683-2020, https://doi.org/10.5194/acp-20-3683-2020, 2020
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We demonstrate for the first time that large festivals can be significant methane sources, though they are not included in emission inventories. We combined in situ measurements with a Gaussian plume model to determine the Oktoberfest emissions and show that they are not due solely to human biogenic emissions, but are instead primarily fossil fuel related. Our study provides the foundation to develop reduction policies for such events and new pathways to mitigate fossil fuel methane emissions.
Kévin Fourteau, Patricia Martinerie, Xavier Faïn, Alexey A. Ekaykin, Jérôme Chappellaz, and Vladimir Lipenkov
Clim. Past, 16, 503–522, https://doi.org/10.5194/cp-16-503-2020, https://doi.org/10.5194/cp-16-503-2020, 2020
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We quantify how the greenhouse gas records of East Antarctic ice cores (which are the oldest ice cores) might differ from the actual atmosphere history. It is required to properly interpret ice core data. For this, we measured the methane of five new East Antarctic ice core sections using a high-resolution technique. We found that in these very old ice cores, one can retrieve concentration variations occurring in only a few centuries, allowing climatologists to study climate's fast dynamics.
Stefan Lossow, Charlotta Högberg, Farahnaz Khosrawi, Gabriele P. Stiller, Ralf Bauer, Kaley A. Walker, Sylvia Kellmann, Andrea Linden, Michael Kiefer, Norbert Glatthor, Thomas von Clarmann, Donal P. Murtagh, Jörg Steinwagner, Thomas Röckmann, and Roland Eichinger
Atmos. Meas. Tech., 13, 287–308, https://doi.org/10.5194/amt-13-287-2020, https://doi.org/10.5194/amt-13-287-2020, 2020
Detlev Helmig, Daniel Liptzin, Jacques Hueber, and Joel Savarino
The Cryosphere, 14, 199–209, https://doi.org/10.5194/tc-14-199-2020, https://doi.org/10.5194/tc-14-199-2020, 2020
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We present 15 months of trace gas observations from air withdrawn within the snowpack and from above the snow at Concordia Station in Antarctica. The data show occasional positive spikes, indicative of pollution from the station generator. The pollution signal can be seen in snowpack air shortly after it is observed above the snow surface, and lasting for up to several days, much longer than above the surface.
Kévin Fourteau, Patricia Martinerie, Xavier Faïn, Christoph F. Schaller, Rebecca J. Tuckwell, Henning Löwe, Laurent Arnaud, Olivier Magand, Elizabeth R. Thomas, Johannes Freitag, Robert Mulvaney, Martin Schneebeli, and Vladimir Ya. Lipenkov
The Cryosphere, 13, 3383–3403, https://doi.org/10.5194/tc-13-3383-2019, https://doi.org/10.5194/tc-13-3383-2019, 2019
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Understanding gas trapping in polar ice is essential to study the relationship between greenhouse gases and past climates. New data of bubble closure, used in a simple gas-trapping model, show inconsistency with the final air content in ice. This suggests gas trapping is not fully understood. We also use a combination of high-resolution measurements to investigate the effect of polar snow stratification on gas trapping and find that all strata have similar pores, but that some close in advance.
Marco de Bruine, Maarten Krol, Jordi Vilà-Guerau de Arellano, and Thomas Röckmann
Geosci. Model Dev., 12, 5177–5196, https://doi.org/10.5194/gmd-12-5177-2019, https://doi.org/10.5194/gmd-12-5177-2019, 2019
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An aerosol scheme with multiple aerosol species is introduced in the Dutch Atmospheric Large-Eddy Simulation model (DALES) and focused to simulate the feedback of aerosol–cloud interaction (ACI) on the aerosol population. Cloud aerosol processing is found to be sensitive to the numerical method, while removal by precipitation is more stable. How ACI increases or decreases the mean aerosol size depends on the balance between the evaporation of clouds/rain and ultimate removal by precipitation.
Rupert Holzinger, W. Joe F. Acton, William J. Bloss, Martin Breitenlechner, Leigh R. Crilley, Sébastien Dusanter, Marc Gonin, Valerie Gros, Frank N. Keutsch, Astrid Kiendler-Scharr, Louisa J. Kramer, Jordan E. Krechmer, Baptiste Languille, Nadine Locoge, Felipe Lopez-Hilfiker, Dušan Materić, Sergi Moreno, Eiko Nemitz, Lauriane L. J. Quéléver, Roland Sarda Esteve, Stéphane Sauvage, Simon Schallhart, Roberto Sommariva, Ralf Tillmann, Sergej Wedel, David R. Worton, Kangming Xu, and Alexander Zaytsev
Atmos. Meas. Tech., 12, 6193–6208, https://doi.org/10.5194/amt-12-6193-2019, https://doi.org/10.5194/amt-12-6193-2019, 2019
Martin Jiskra, Jeroen E. Sonke, Yannick Agnan, Detlev Helmig, and Daniel Obrist
Biogeosciences, 16, 4051–4064, https://doi.org/10.5194/bg-16-4051-2019, https://doi.org/10.5194/bg-16-4051-2019, 2019
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The tundra plays a pivotal role in Arctic mercury cycling by storing atmospheric mercury deposition and shuttling it to the Arctic Ocean. We used the isotopic fingerprint of mercury to investigate the processes controlling atmospheric mercury deposition. We found that the uptake of atmospheric mercury by vegetation was the major deposition source. Direct deposition to snow or soils only played a minor role. These results improve our understanding of Arctic mercury cycling.
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.
James A. Menking, Edward J. Brook, Sarah A. Shackleton, Jeffrey P. Severinghaus, Michael N. Dyonisius, Vasilii Petrenko, Joseph R. McConnell, Rachael H. Rhodes, Thomas K. Bauska, Daniel Baggenstos, Shaun Marcott, and Stephen Barker
Clim. Past, 15, 1537–1556, https://doi.org/10.5194/cp-15-1537-2019, https://doi.org/10.5194/cp-15-1537-2019, 2019
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An ice core from Taylor Glacier, Antarctica, spans a period ~ 70 000 years ago when Earth entered the last ice age. Chemical analyses of the ice and air bubbles allow for an independent determination of the ages of the ice and gas bubbles. The difference between the age of the ice and the bubbles at any given depth, called ∆age, is unusually high in the Taylor Glacier core compared to the Taylor Dome ice core situated to the south. This implies a dramatic accumulation gradient between the sites.
Charel Wohl, David Capelle, Anna Jones, William T. Sturges, Philip D. Nightingale, Brent G. T. Else, and Mingxi Yang
Ocean Sci., 15, 925–940, https://doi.org/10.5194/os-15-925-2019, https://doi.org/10.5194/os-15-925-2019, 2019
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In this paper we present a gas equilibrator that can be used to equilibrate gases continuously or in discrete samples from seawater into a carrier gas. The headspace is analysed by a commercially available proton-transfer-reaction mass spectrometer. This allows for the measurement of a broad range of dissolved gases up to a very high solubility in seawater. The main advantage of this equilibrator is its unique design and ease of reproducibility.
Isaac J. Vimont, Jocelyn C. Turnbull, Vasilii V. Petrenko, Philip F. Place, Colm Sweeney, Natasha Miles, Scott Richardson, Bruce H. Vaughn, and James W. C. White
Atmos. Chem. Phys., 19, 8547–8562, https://doi.org/10.5194/acp-19-8547-2019, https://doi.org/10.5194/acp-19-8547-2019, 2019
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Stable isotopes of Carbon Monoxide (CO) and radiocarbon carbon dioxide were measured over three summers at Indianapolis, Indiana, US, and for 1 year at a site thought to be strongly influenced by CO from oxidized volatile organic compounds (VOCs) in South Carolina, US. The Indianapolis results were used to provide an estimate of the carbon and oxygen isotopic signatures of CO produced from oxidized VOCs. This updated estimate agrees well with the data from South Carolina during the summer.
Mauro Rubino, David M. Etheridge, David P. Thornton, Russell Howden, Colin E. Allison, Roger J. Francey, Ray L. Langenfelds, L. Paul Steele, Cathy M. Trudinger, Darren A. Spencer, Mark A. J. Curran, Tas D. van Ommen, and Andrew M. Smith
Earth Syst. Sci. Data, 11, 473–492, https://doi.org/10.5194/essd-11-473-2019, https://doi.org/10.5194/essd-11-473-2019, 2019
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The scientific community uses numerical models to predict future atmospheric levels of greenhouse gases causing global warming. This study presents the history of atmospheric concentration of the major greenhouse gases over the last 2000 years measured in ice core bubbles from the site of Law Dome (East Antarctica). The associated dataset is useful to test climate models and help provide accurate predictions of future climate change.
Martin K. Vollmer, François Bernard, Blagoj Mitrevski, L. Paul Steele, Cathy M. Trudinger, Stefan Reimann, Ray L. Langenfelds, Paul B. Krummel, Paul J. Fraser, David M. Etheridge, Mark A. J. Curran, and James B. Burkholder
Atmos. Chem. Phys., 19, 3481–3492, https://doi.org/10.5194/acp-19-3481-2019, https://doi.org/10.5194/acp-19-3481-2019, 2019
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We have discovered a new compound in the atmosphere, octafluorooxolane (c-C4F8O), from measurements in archived air samples. From our laboratory studies, we find that c-C4F8O is a very powerful greenhouse gas thereby contributing to global warming, and that it has a very long atmospheric lifetime of more than 3500 years. Based on our measurements we could reconstruct its atmospheric evolution over more than 4 decades. Based on this, we could estimate the global emissions of c-C4F8O.
Iris N. Dekker, Sander Houweling, Sudhanshu Pandey, Maarten Krol, Thomas Röckmann, Tobias Borsdorff, Jochen Landgraf, and Ilse Aben
Atmos. Chem. Phys., 19, 3433–3445, https://doi.org/10.5194/acp-19-3433-2019, https://doi.org/10.5194/acp-19-3433-2019, 2019
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During November 2017, very high pollution levels were measured in the northern part of India. In this study, satellite (TROPOMI) data and model (WRF) data on carbon monoxide (CO) are studied to investigate the main sources of the CO pollution over the Indo-Gangetic Plain. We found that residential and commercial combustion was a much more important source of CO than the post-monsoon crop burning during this period. Meteorology was found important in the accumulation and ventilation of CO.
Naomi J. Farren, Rachel E. Dunmore, Mohammed Iqbal Mead, Mohd Shahrul Mohd Nadzir, Azizan Abu Samah, Siew-Moi Phang, Brian J. Bandy, William T. Sturges, and Jacqueline F. Hamilton
Atmos. Chem. Phys., 19, 1537–1553, https://doi.org/10.5194/acp-19-1537-2019, https://doi.org/10.5194/acp-19-1537-2019, 2019
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During the winter monsoon, air quality on the east coast of Peninsular Malaysia is influenced by local emissions and aged emissions transported from highly polluted East Asian regions. Atmospheric particulate matter has been sampled at a rural coastal location, and ion chromatography has been used to make time-resolved measurements of the major atmospheric ions present. Analysis of aerosol composition and back trajectories has provided an insight into common sources and formation pathways.
Dušan Materić, Elke Ludewig, Kangming Xu, Thomas Röckmann, and Rupert Holzinger
The Cryosphere, 13, 297–307, https://doi.org/10.5194/tc-13-297-2019, https://doi.org/10.5194/tc-13-297-2019, 2019
Shaojie Song, Hélène Angot, Noelle E. Selin, Hubert Gallée, Francesca Sprovieri, Nicola Pirrone, Detlev Helmig, Joël Savarino, Olivier Magand, and Aurélien Dommergue
Atmos. Chem. Phys., 18, 15825–15840, https://doi.org/10.5194/acp-18-15825-2018, https://doi.org/10.5194/acp-18-15825-2018, 2018
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Mercury is a trace metal with adverse health effects on human and wildlife. Its unique property makes it undergo long-range transport, and even remote Antarctica receives significant inputs. This paper presents the first model that aims to understand mercury behavior over the Antarctic Plateau. We find that mercury is quickly cycled between snow and air in the sunlit period, likely driven by bromine chemistry, and that several uncertain processes contribute to its behavior in the dark period.
Georgios I. Gkatzelis, Thorsten Hohaus, Ralf Tillmann, Iulia Gensch, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Zhujun Yu, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Chem. Phys., 18, 12969–12989, https://doi.org/10.5194/acp-18-12969-2018, https://doi.org/10.5194/acp-18-12969-2018, 2018
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Defining the fundamental parameters that distribute organic molecules between the gas and particle phases is essential to understand their impact on the atmosphere. In this work, gas to particle partitioning of major biogenic oxidation products from monoterpenes and real plant emissions was investigated. While measurement results and theoretical calculation for most semi-volatile compounds are in good agreement, significant deviations are found for intermediate volatile organic compounds.
Alexis Burr, Clément Ballot, Pierre Lhuissier, Patricia Martinerie, Christophe L. Martin, and Armelle Philip
The Cryosphere, 12, 2481–2500, https://doi.org/10.5194/tc-12-2481-2018, https://doi.org/10.5194/tc-12-2481-2018, 2018
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Three-dimensional imaging of the pore network of polar firn from Antarctica was realized in order to relate the morphological evolution of pores with their progressive closure with depth. Evaluating the closed porosity was found to be very dependent on the size of samples and image reconstructions. A connectivity index, which is a parameter less dependent on such issues, was proposed and proved to accurately predict the close-off depths and densities of two polar sites.
Yannick Agnan, Thomas A. Douglas, Detlev Helmig, Jacques Hueber, and Daniel Obrist
The Cryosphere, 12, 1939–1956, https://doi.org/10.5194/tc-12-1939-2018, https://doi.org/10.5194/tc-12-1939-2018, 2018
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In this study, we investigated mercury dynamics in an interior arctic tundra at Toolik Field Station (200 km from the Arctic Ocean) during two full snow seasons. We continuously measured atmospheric, snow gas phase, and soil pores mercury concentrations. We observed consistent concentration declines from the atmosphere to snowpack to soils, indicating that soils are continuous sinks of mercury. We suggest that interior arctic snowpacks may be negligible sources of mercury.
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465, https://doi.org/10.5194/gmd-11-1443-2018, https://doi.org/10.5194/gmd-11-1443-2018, 2018
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Precipitation evaporation (PE) and subsequent aerosol resuspension (AR) are currently ignored or implemented only crudely in GCMs. This research introduces PE to Earth system model EC-Earth and explores ways to treat AR and the impact on global aerosol burden. Simple 1:1 scaling of AR with PE leads to an increase (+8 to 15.9 %). Taking into account raindrop size distribution and/or accounting for in-rain aerosol processing decreases aerosol burden -1.5 to 6.2 % and -10 to -11 %, respectively.
Karina E. Adcock, Claire E. Reeves, Lauren J. Gooch, Emma C. Leedham Elvidge, Matthew J. Ashfold, Carl A. M. Brenninkmeijer, Charles Chou, Paul J. Fraser, Ray L. Langenfelds, Norfazrin Mohd Hanif, Simon O'Doherty, David E. Oram, Chang-Feng Ou-Yang, Siew Moi Phang, Azizan Abu Samah, Thomas Röckmann, William T. Sturges, and Johannes C. Laube
Atmos. Chem. Phys., 18, 4737–4751, https://doi.org/10.5194/acp-18-4737-2018, https://doi.org/10.5194/acp-18-4737-2018, 2018
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.
Georgios I. Gkatzelis, Ralf Tillmann, Thorsten Hohaus, Markus Müller, Philipp Eichler, Kang-Ming Xu, Patrick Schlag, Sebastian H. Schmitt, Robert Wegener, Martin Kaminski, Rupert Holzinger, Armin Wisthaler, and Astrid Kiendler-Scharr
Atmos. Meas. Tech., 11, 1481–1500, https://doi.org/10.5194/amt-11-1481-2018, https://doi.org/10.5194/amt-11-1481-2018, 2018
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This manuscript presents an intercomparison of state-of-the-art online and in situ particle sampling techniques connected to proton transfer reaction time-of-flight mass spectrometry (PTR-ToF-MS). Collection and vaporization of aerosol combined with soft ionization mass spectrometry offers the advantage of detailed chemical characterization of SOA species. The benefits of these techniques are highlighted through their consistency in providing the chemical composition of biogenic SOA.
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.
Taku Umezawa, Carl A. M. Brenninkmeijer, Thomas Röckmann, Carina van der Veen, Stanley C. Tyler, Ryo Fujita, Shinji Morimoto, Shuji Aoki, Todd Sowers, Jochen Schmitt, Michael Bock, Jonas Beck, Hubertus Fischer, Sylvia E. Michel, Bruce H. Vaughn, John B. Miller, James W. C. White, Gordon Brailsford, Hinrich Schaefer, Peter Sperlich, Willi A. Brand, Michael Rothe, Thomas Blunier, David Lowry, Rebecca E. Fisher, Euan G. Nisbet, Andrew L. Rice, Peter Bergamaschi, Cordelia Veidt, and Ingeborg Levin
Atmos. Meas. Tech., 11, 1207–1231, https://doi.org/10.5194/amt-11-1207-2018, https://doi.org/10.5194/amt-11-1207-2018, 2018
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Isotope measurements are useful for separating different methane sources. However, the lack of widely accepted standards and calibration methods for stable carbon and hydrogen isotopic ratios of methane in air has caused significant measurement offsets among laboratories. We conducted worldwide interlaboratory comparisons, surveyed the literature and assessed them systematically. This study may be of help in future attempts to harmonize data sets of isotopic composition of atmospheric methane.
Julia Schmale, Silvia Henning, Stefano Decesari, Bas Henzing, Helmi Keskinen, Karine Sellegri, Jurgita Ovadnevaite, Mira L. Pöhlker, Joel Brito, Aikaterini Bougiatioti, Adam Kristensson, Nikos Kalivitis, Iasonas Stavroulas, Samara Carbone, Anne Jefferson, Minsu Park, Patrick Schlag, Yoko Iwamoto, Pasi Aalto, Mikko Äijälä, Nicolas Bukowiecki, Mikael Ehn, Göran Frank, Roman Fröhlich, Arnoud Frumau, Erik Herrmann, Hartmut Herrmann, Rupert Holzinger, Gerard Kos, Markku Kulmala, Nikolaos Mihalopoulos, Athanasios Nenes, Colin O'Dowd, Tuukka Petäjä, David Picard, Christopher Pöhlker, Ulrich Pöschl, Laurent Poulain, André Stephan Henry Prévôt, Erik Swietlicki, Meinrat O. Andreae, Paulo Artaxo, Alfred Wiedensohler, John Ogren, Atsushi Matsuki, Seong Soo Yum, Frank Stratmann, Urs Baltensperger, and Martin Gysel
Atmos. Chem. Phys., 18, 2853–2881, https://doi.org/10.5194/acp-18-2853-2018, https://doi.org/10.5194/acp-18-2853-2018, 2018
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Collocated long-term observations of cloud condensation nuclei (CCN) number concentrations, particle number size distributions and chemical composition from 12 sites are synthesized. Observations cover coastal environments, the Arctic, the Mediterranean, the boreal and rain forest, high alpine and continental background sites, and Monsoon-influenced areas. We interpret regional and seasonal variability. CCN concentrations are predicted with the κ–Köhler model and compared to the measurements.
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.
Kévin Fourteau, Xavier Faïn, Patricia Martinerie, Amaëlle Landais, Alexey A. Ekaykin, Vladimir Ya. Lipenkov, and Jérôme Chappellaz
Clim. Past, 13, 1815–1830, https://doi.org/10.5194/cp-13-1815-2017, https://doi.org/10.5194/cp-13-1815-2017, 2017
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We measured methane concentrations from a polar ice core to quantify the differences between the ice record and the past true atmospheric conditions. Two effects were investigated by combining data analysis and modeling: the stratification of polar snow before gas enclosure driving chronological hiatuses in the record and the gradual formation of bubbles in the ice attenuating fast atmospheric variations. This study will contribute to improving future climatic interpretations from ice archives.
Iris N. Dekker, Sander Houweling, Ilse Aben, Thomas Röckmann, Maarten Krol, Sara Martínez-Alonso, Merritt N. Deeter, and Helen M. Worden
Atmos. Chem. Phys., 17, 14675–14694, https://doi.org/10.5194/acp-17-14675-2017, https://doi.org/10.5194/acp-17-14675-2017, 2017
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This study estimates carbon monoxide emissions from the city of Madrid using MOPITT satellite data. There are two methods used and reviewed in this paper: a method that can only estimate a trend in the emission and a newly developed method that also includes model data from WRF to quantify the emissions. We find Madrid CO emissions to be lower by 48 % for 2002 and by 17 % for 2006 compared with the EdgarV4.2 emission inventory, but uncertainty (20 to 50 %) remains.
Yaoxian Huang, Shiliang Wu, Louisa J. Kramer, Detlev Helmig, and Richard E. Honrath
Atmos. Chem. Phys., 17, 14661–14674, https://doi.org/10.5194/acp-17-14661-2017, https://doi.org/10.5194/acp-17-14661-2017, 2017
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A global chemical transport model (GEOS-Chem) was employed to simulate surface ozone and its precursors at Summit, Greenland in the Arctic and compare them with 2-year in situ surface observations. The model performed well in simulating certain species (such as carbon monoxide and propane), but some significant discrepancies were identified for other species (e.g., nitrogen oxides, ethane, PAN, and ozone). We further investigated the exact causes for model–data biases.
Heather Graven, Colin E. Allison, David M. Etheridge, Samuel Hammer, Ralph F. Keeling, Ingeborg Levin, Harro A. J. Meijer, Mauro Rubino, Pieter P. Tans, Cathy M. Trudinger, Bruce H. Vaughn, and James W. C. White
Geosci. Model Dev., 10, 4405–4417, https://doi.org/10.5194/gmd-10-4405-2017, https://doi.org/10.5194/gmd-10-4405-2017, 2017
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Modelling of carbon isotopes 13C and 14C in land and ocean components of Earth system models provides opportunities for new insights and improved understanding of global carbon cycling, and for model evaluation. We compiled existing historical datasets to define the annual mean carbon isotopic composition of atmospheric CO2 for 1850–2015 that can be used in CMIP6 and other modelling activities.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma C. Leedham Elvidge, Grant L. Forster, Neil R. P. Harris, Mohammed Iqbal Mead, Azizan Abu Samah, Siew Moi Phang, Chang-Feng Ou-Yang, Neng-Huei Lin, Jia-Lin Wang, Angela K. Baker, Carl A. M. Brenninkmeijer, and David Sherry
Atmos. Chem. Phys., 17, 11929–11941, https://doi.org/10.5194/acp-17-11929-2017, https://doi.org/10.5194/acp-17-11929-2017, 2017
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We have observed large amounts of man-made chlorine compounds in E and SE Asia and in the upper tropical troposphere. These relatively short-lived compounds are not controlled by the Montreal Protocol, but if significant quantities were able to reach the stratosphere, the long-term recovery of stratospheric ozone would be delayed. We have also identified an important atmospheric transport mechanism that can rapidly transport these chemicals from E Asia to the upper troposphere via the tropics.
Jason Roberts, Andrew Moy, Christopher Plummer, Tas van Ommen, Mark Curran, Tessa Vance, Samuel Poynter, Yaping Liu, Joel Pedro, Adam Treverrow, Carly Tozer, Lenneke Jong, Pippa Whitehouse, Laetitia Loulergue, Jerome Chappellaz, Vin Morgan, Renato Spahni, Adrian Schilt, Cecilia MacFarling Meure, David Etheridge, and Thomas Stocker
Clim. Past Discuss., https://doi.org/10.5194/cp-2017-96, https://doi.org/10.5194/cp-2017-96, 2017
Preprint withdrawn
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Here we present a revised Law Dome, Dome Summit South (DSS) ice core age model (denoted LD2017) that significantly improves the chronology over the last 88 thousand years. An ensemble approach was used, allowing for the computation of both a median age and associated uncertainty as a function of depth. We use a non-linear interpolation between age ties and unlike previous studies, we made an independent estimate of the snow accumulation rate, where required, for the use of gas based age ties.
Daniel Baggenstos, Thomas K. Bauska, Jeffrey P. Severinghaus, James E. Lee, Hinrich Schaefer, Christo Buizert, Edward J. Brook, Sarah Shackleton, and Vasilii V. Petrenko
Clim. Past, 13, 943–958, https://doi.org/10.5194/cp-13-943-2017, https://doi.org/10.5194/cp-13-943-2017, 2017
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We present measurements of the gas composition in trapped air bubbles in ice samples taken from Taylor Glacier, Antarctica. We can show that ice from the entire last glacial cycle (125 000 years ago to the present) is exposed at the surface of this glacier and that the atmospheric record contained in the air bubbles is well preserved. Taylor Glacier therefore provides an easily accessible archive of ancient ice that allows for studies of trace components that require large ice volumes.
Mike J. Newland, Patricia Martinerie, Emmanuel Witrant, Detlev Helmig, David R. Worton, Chris Hogan, William T. Sturges, and Claire E. Reeves
Atmos. Chem. Phys., 17, 8269–8283, https://doi.org/10.5194/acp-17-8269-2017, https://doi.org/10.5194/acp-17-8269-2017, 2017
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We report increasing levels of alkyl nitrates in the Northern Hemisphere atmosphere between 1960 and the mid-1990s. These increases are symptomatic of large-scale changes to the chemical composition of the atmosphere, particularly with regards to the amounts of short-lived, reactive species. The observed increases are likely driven by increasing levels of nitrogen oxides. These changes have direct implications for the lifetimes of climate-relevant species in the atmosphere, such as methane.
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.
Carl Meusinger, Ulrike Dusek, Stephanie M. King, Rupert Holzinger, Thomas Rosenørn, Peter Sperlich, Maxime Julien, Gerald S. Remaud, Merete Bilde, Thomas Röckmann, and Matthew S. Johnson
Atmos. Chem. Phys., 17, 6373–6391, https://doi.org/10.5194/acp-17-6373-2017, https://doi.org/10.5194/acp-17-6373-2017, 2017
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Isotope studies can constrain budgets of secondary organic aerosol (SOA) that is pivotal to air pollution and climate. SOA from α-pinene ozonolysis was found to be enriched in 13C relative to the precursor. The observed difference in 13C between the gas and particle phases may arise from isotope-dependent changes in branching ratios. Alternatively, some gas-phase products involve carbon atoms from highly enriched and depleted sites, giving a non-kinetic origin to the observed fractionations.
Célia J. Sapart, Natalia Shakhova, Igor Semiletov, Joachim Jansen, Sönke Szidat, Denis Kosmach, Oleg Dudarev, Carina van der Veen, Matthias Egger, Valentine Sergienko, Anatoly Salyuk, Vladimir Tumskoy, Jean-Louis Tison, and Thomas Röckmann
Biogeosciences, 14, 2283–2292, https://doi.org/10.5194/bg-14-2283-2017, https://doi.org/10.5194/bg-14-2283-2017, 2017
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The Arctic Ocean, especially the Siberian shelves, overlays large areas of subsea permafrost that is degrading. We show that methane with a biogenic origin is emitted from this permafrost. At locations where bubble plumes have been observed, methane can escape oxidation in the surface sediment and rapidly migrate through the very shallow water column of this region to escape to the atmosphere, generating a positive radiative feedback.
Markella Prokopiou, Patricia Martinerie, Célia J. Sapart, Emmanuel Witrant, Guillaume Monteil, Kentaro Ishijima, Sophie Bernard, Jan Kaiser, Ingeborg Levin, Thomas Blunier, David Etheridge, Ed Dlugokencky, Roderik S. W. van de Wal, and Thomas Röckmann
Atmos. Chem. Phys., 17, 4539–4564, https://doi.org/10.5194/acp-17-4539-2017, https://doi.org/10.5194/acp-17-4539-2017, 2017
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Nitrous oxide is the third most important anthropogenic greenhouse gas with an increasing mole fraction. To understand its natural and anthropogenic sources
we employ isotope measurements. Results show that while the N2O mole fraction increases, its heavy isotope content decreases. The isotopic changes observed underline the dominance of agricultural emissions especially at the early part of the record, whereas in the later decades the contribution from other anthropogenic sources increases.
Ulrike Dusek, Regina Hitzenberger, Anne Kasper-Giebl, Magdalena Kistler, Harro A. J. Meijer, Sönke Szidat, Lukas Wacker, Rupert Holzinger, and Thomas Röckmann
Atmos. Chem. Phys., 17, 3233–3251, https://doi.org/10.5194/acp-17-3233-2017, https://doi.org/10.5194/acp-17-3233-2017, 2017
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Measurements of the radioactive carbon isotope 14C allow to identify the sources of aerosol carbon. We report an extensive 14C source apportionment record in the Netherlands with samples covering a whole year. We discovered that long-range transport has a large influence on aerosol carbon levels. Fossil fuel carbon is least influenced by long-range transport and more regional in origin. Biomass burning seems to be a minor source of aerosol carbon in the Netherlands.
Pearse J. Buchanan, Richard J. Matear, Andrew Lenton, Steven J. Phipps, Zanna Chase, and David M. Etheridge
Clim. Past, 12, 2271–2295, https://doi.org/10.5194/cp-12-2271-2016, https://doi.org/10.5194/cp-12-2271-2016, 2016
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We quantify the contributions of physical and biogeochemical changes in the ocean to enhancing ocean carbon storage at the Last Glacial Maximum. We find that simulated circulation and surface conditions cannot explain changes in carbon storage or other major biogeochemical fields that existed during the glacial climate. Key modifications to the functioning of the biological pump are therefore required to explain the glacial climate and improve model–proxy agreement for all fields.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079, https://doi.org/10.5194/amt-9-6069-2016, https://doi.org/10.5194/amt-9-6069-2016, 2016
Johannes C. Laube, Norfazrin Mohd Hanif, Patricia Martinerie, Eileen Gallacher, Paul J. Fraser, Ray Langenfelds, Carl A. M. Brenninkmeijer, Jakob Schwander, Emmanuel Witrant, Jia-Lin Wang, Chang-Feng Ou-Yang, Lauren J. Gooch, Claire E. Reeves, William T. Sturges, and David E. Oram
Atmos. Chem. Phys., 16, 15347–15358, https://doi.org/10.5194/acp-16-15347-2016, https://doi.org/10.5194/acp-16-15347-2016, 2016
Dorota Janina Mrozek, Carina van der Veen, Magdalena E. G. Hofmann, Huilin Chen, Rigel Kivi, Pauli Heikkinen, and Thomas Röckmann
Atmos. Meas. Tech., 9, 5607–5620, https://doi.org/10.5194/amt-9-5607-2016, https://doi.org/10.5194/amt-9-5607-2016, 2016
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Stratospheric Air Sub-sampler (SAS) is a device to collect and to store the stratospheric profile of air collected with an AirCore (Karion et al., 2010) in numerous sub-samples. The sub-samples (each of 25 mL at ambient temperature and pressure) can be later introduced to the continuous flow systems to measure for example the isotopic composition of CO2. The performance of the coupled system is demonstrated for a set of air samples from an AirCore flight in November 2014 near Sodankylä, Finland.
Beatriz Sayuri Oyama, Maria de Fátima Andrade, Pierre Herckes, Ulrike Dusek, Thomas Röckmann, and Rupert Holzinger
Atmos. Chem. Phys., 16, 14397–14408, https://doi.org/10.5194/acp-16-14397-2016, https://doi.org/10.5194/acp-16-14397-2016, 2016
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Vehicular emissions have a strong impact on air pollution in big cities; hence, the study was performed in São Paulo city, where light- (LDVs) and heavy-duty vehicles (HDVs) run on different fuels. We find that organic aerosol emission from LDVs and HDVs is a complex process involving oxidation of fuel constituents, NOx chemistry, and condensation of unburned fuel hydrocarbons on new or existing particles. The obtained emission patterns can be used to study processing of young aerosol in Brazil.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355, https://doi.org/10.5194/bg-13-5333-2016, https://doi.org/10.5194/bg-13-5333-2016, 2016
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By combining detailed geochemical analyses with diagenetic modeling, we provide new insights into how methane dynamics may strongly overprint burial records of iron, sulfur and phosphorus in marine systems subject to changes in organic matter loading or water column salinity. A better understanding of these processes will improve our ability to read ancient sediment records and thus to predict the potential consequences of global warming and human-enhanced inputs of nutrients to the ocean.
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.
Thomas Röckmann, Simon Eyer, Carina van der Veen, Maria E. Popa, Béla Tuzson, Guillaume Monteil, Sander Houweling, Eliza Harris, Dominik Brunner, Hubertus Fischer, Giulia Zazzeri, David Lowry, Euan G. Nisbet, Willi A. Brand, Jaroslav M. Necki, Lukas Emmenegger, and Joachim Mohn
Atmos. Chem. Phys., 16, 10469–10487, https://doi.org/10.5194/acp-16-10469-2016, https://doi.org/10.5194/acp-16-10469-2016, 2016
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A dual isotope ratio mass spectrometric system (IRMS) and a quantum cascade laser absorption spectroscopy (QCLAS)-based technique were deployed at the Cabauw experimental site for atmospheric research (CESAR) in the Netherlands and performed in situ, high-frequency (approx. hourly) measurements for a period of more than 5 months, yielding a combined dataset with more than 2500 measurements of both δ13C and δD.
Peter Sperlich, Nelly A. M. Uitslag, Jürgen M. Richter, Michael Rothe, Heike Geilmann, Carina van der Veen, Thomas Röckmann, Thomas Blunier, and Willi A. Brand
Atmos. Meas. Tech., 9, 3717–3737, https://doi.org/10.5194/amt-9-3717-2016, https://doi.org/10.5194/amt-9-3717-2016, 2016
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Isotope measurements in atmospheric CH4 are performed since more than 3 decades. However, standard gases to harmonize global measurements are not available to this day. We designed two methods to calibrate a suite of 8 CH4 gases with a wide range in isotopic composition to the VPDB and VSMOW scales with high precision and accuracy. Synthetic air mixtures with ~2 ppm of calibrated CH4 can be provided to the community by the ISOLAB of the Max Planck Institute for Biogeochemistry in Jena, Germany.
Theo Manuel Jenk, Mauro Rubino, David Etheridge, Viorela Gabriela Ciobanu, and Thomas Blunier
Atmos. Meas. Tech., 9, 3687–3706, https://doi.org/10.5194/amt-9-3687-2016, https://doi.org/10.5194/amt-9-3687-2016, 2016
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Atmospheric CO2 and δ13C-CO2 records from polar ice cores provide important constraints on the natural carbon cycle variability. Still, data exist only from a limited number of sampling sites and time periods due to demanding analytical challenges. Additional analytical state-of-the-art resources are desirable. This study describes such a new facility. Its analytical performance and new approaches for dealing with procedural blank contribution and analytical outliers are discussed in detail.
Makoto Inoue, Isamu Morino, Osamu Uchino, Takahiro Nakatsuru, Yukio Yoshida, Tatsuya Yokota, Debra Wunch, Paul O. Wennberg, Coleen M. Roehl, David W. T. Griffith, Voltaire A. Velazco, Nicholas M. Deutscher, Thorsten Warneke, Justus Notholt, John Robinson, Vanessa Sherlock, Frank Hase, Thomas Blumenstock, Markus Rettinger, Ralf Sussmann, Esko Kyrö, Rigel Kivi, Kei Shiomi, Shuji Kawakami, Martine De Mazière, Sabrina G. Arnold, Dietrich G. Feist, Erica A. Barrow, James Barney, Manvendra Dubey, Matthias Schneider, Laura T. Iraci, James R. Podolske, Patrick W. Hillyard, Toshinobu Machida, Yousuke Sawa, Kazuhiro Tsuboi, Hidekazu Matsueda, Colm Sweeney, Pieter P. Tans, Arlyn E. Andrews, Sebastien C. Biraud, Yukio Fukuyama, Jasna V. Pittman, Eric A. Kort, and Tomoaki Tanaka
Atmos. Meas. Tech., 9, 3491–3512, https://doi.org/10.5194/amt-9-3491-2016, https://doi.org/10.5194/amt-9-3491-2016, 2016
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In this study, we correct the biases of GOSAT XCO2 and XCH4 using TCCON data. To evaluate the effectiveness of our correction method, uncorrected/corrected GOSAT data are compared to independent XCO2 and XCH4 data derived from aircraft measurements. Consequently, we suggest that this method is effective for reducing the biases of the GOSAT data. We consider that our work provides GOSAT data users with valuable information and contributes to the further development of studies on greenhouse gases.
Patrick Schlag, Astrid Kiendler-Scharr, Marcus Johannes Blom, Francesco Canonaco, Jeroen Sebastiaan Henzing, Marcel Moerman, André Stephan Henry Prévôt, and Rupert Holzinger
Atmos. Chem. Phys., 16, 8831–8847, https://doi.org/10.5194/acp-16-8831-2016, https://doi.org/10.5194/acp-16-8831-2016, 2016
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This work provides chemical composition data of atmospheric aerosols acquired during 1 year in the rural site of Cabauw, the Netherlands. In some periods, we found unexpected high particle mass concentrations exceeding the WHO limits. Using these composition data, we found that reducing ammonia emissions in this region would largely reduce the main aerosol component ammonium nitrate, whereas the local mitigation of the organics turned out to be difficult due to the lack of a designated source.
Hélène Angot, Olivier Magand, Detlev Helmig, Philippe Ricaud, Boris Quennehen, Hubert Gallée, Massimo Del Guasta, Francesca Sprovieri, Nicola Pirrone, Joël Savarino, and Aurélien Dommergue
Atmos. Chem. Phys., 16, 8249–8264, https://doi.org/10.5194/acp-16-8249-2016, https://doi.org/10.5194/acp-16-8249-2016, 2016
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While the Arctic has been extensively monitored, there is still much to be learned from the Antarctic continent regarding the processes that govern the budget of atmospheric mercury species. We report here the first year-round measurements of gaseous elemental mercury (Hg(0)) in the atmosphere and in snowpack interstitial air on the East Antarctic ice sheet. The striking reactivity observed on the Antarctic plateau most likely influences the cycle of atmospheric mercury on a continental scale.
Michel Legrand, Susanne Preunkert, Joël Savarino, Markus M. Frey, Alexandre Kukui, Detlev Helmig, Bruno Jourdain, Anna E. Jones, Rolf Weller, Neil Brough, and Hubert Gallée
Atmos. Chem. Phys., 16, 8053–8069, https://doi.org/10.5194/acp-16-8053-2016, https://doi.org/10.5194/acp-16-8053-2016, 2016
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Surface ozone, the most abundant atmospheric oxidant, has been measured since 2004 at the coastal East Antarctic site of Dumont d’Urville, and since 2007 at the Concordia station located on the high East Antarctic plateau. Long-term changes, seasonal and diurnal cycles, as well as inter-annual summer variability observed at these two East Antarctic sites are discussed. Influences like sea ice extent and outflow from inland Antarctica are discussed.
Anna Karion, Colm Sweeney, John B. Miller, Arlyn E. Andrews, Roisin Commane, Steven Dinardo, John M. Henderson, Jacob Lindaas, John C. Lin, Kristina A. Luus, Tim Newberger, Pieter Tans, Steven C. Wofsy, Sonja Wolter, and Charles E. Miller
Atmos. Chem. Phys., 16, 5383–5398, https://doi.org/10.5194/acp-16-5383-2016, https://doi.org/10.5194/acp-16-5383-2016, 2016
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Northern high-latitude carbon sources and sinks, including those resulting from degrading permafrost, are thought to be sensitive to the rapidly warming climate. Here we use carbon dioxide and methane measurements from a tower near Fairbanks AK to investigate regional Alaskan fluxes of CO2 and CH4 for 2012–2014.
Sudhanshu Pandey, Sander Houweling, Maarten Krol, Ilse Aben, Frédéric Chevallier, Edward J. Dlugokencky, Luciana V. Gatti, Emanuel Gloor, John B. Miller, Rob Detmers, Toshinobu Machida, and Thomas Röckmann
Atmos. Chem. Phys., 16, 5043–5062, https://doi.org/10.5194/acp-16-5043-2016, https://doi.org/10.5194/acp-16-5043-2016, 2016
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This study investigates the constraint provided by measurements of Xratio (XCH4/XCO2) from space on surface fluxes of CH4 and CO2. We apply the ratio inversion method described in Pandey et al. (2015) to Xratio retrievals from the GOSAT with the TM5-4DVAR inverse modeling system, to constrain the surface fluxes of CH4 and CO2 for 2009 and 2010. The results are compared to proxy CH4 inversions using model-derived-XCO2 mixing ratios from CarbonTracker and MACC.
Reinhard Drews, Joel Brown, Kenichi Matsuoka, Emmanuel Witrant, Morgane Philippe, Bryn Hubbard, and Frank Pattyn
The Cryosphere, 10, 811–823, https://doi.org/10.5194/tc-10-811-2016, https://doi.org/10.5194/tc-10-811-2016, 2016
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The thickness of ice shelves is typically inferred using hydrostatic equilibrium which requires knowledge of the firn density. Here, we infer density from wide-angle radar using a novel algorithm including traveltime inversion and ray tracing. We find that firn is denser inside a 2 km wide ice-shelf channel which is confirmed by optical televiewing of two boreholes. Such horizontal density variations must be accounted for when using the hydrostatic ice thickness for determining basal melt rate.
Armin Rauthe-Schöch, Angela K. Baker, Tanja J. Schuck, Carl A. M. Brenninkmeijer, Andreas Zahn, Markus Hermann, Greta Stratmann, Helmut Ziereis, Peter F. J. van Velthoven, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3609–3629, https://doi.org/10.5194/acp-16-3609-2016, https://doi.org/10.5194/acp-16-3609-2016, 2016
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The flying laboratory CARIBIC onboard a passenger aircraft measured trace gases and aerosol particles in the upper tropospheric Indian summer monsoon anticyclone in summer 2008. We used the measurements together with meteorological analyses to investigate the chemical signature of the northern and southern part of the monsoon, the source regions from where the air was entrained into the monsoon and which parts of the world received polluted air that had been chemically processed in the monsoon.
Narendra Ojha, Andrea Pozzer, Armin Rauthe-Schöch, Angela K. Baker, Jongmin Yoon, Carl A. M. Brenninkmeijer, and Jos Lelieveld
Atmos. Chem. Phys., 16, 3013–3032, https://doi.org/10.5194/acp-16-3013-2016, https://doi.org/10.5194/acp-16-3013-2016, 2016
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We compare simulations of ozone and carbon monoxide using a regional chemistry transport model (WRF-Chem) with aircraft observations from CARIBIC program over India during monsoon period. Sensitivity simulations are conducted to assess the influences of regional emissions and long-range transport.
S. Eyer, B. Tuzson, M. E. Popa, C. van der Veen, T. Röckmann, M. Rothe, W. A. Brand, R. Fisher, D. Lowry, E. G. Nisbet, M. S. Brennwald, E. Harris, C. Zellweger, L. Emmenegger, H. Fischer, and J. Mohn
Atmos. Meas. Tech., 9, 263–280, https://doi.org/10.5194/amt-9-263-2016, https://doi.org/10.5194/amt-9-263-2016, 2016
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We present a newly developed field-deployable, autonomous platform simultaneously measuring the three most abundant isotopologues of methane using mid-infrared laser absorption spectroscopy.
The instrument consists of a compact quantum cascade laser absorption spectrometer (QCLAS) coupled to a preconcentration unit, called TRace gas EXtractor (TREX).
The performance of this new in situ technique was investigated during a 2-week measurement campaign and compared to other techniques.
N. Bândă, M. Krol, M. van Weele, T. van Noije, P. Le Sager, and T. Röckmann
Atmos. Chem. Phys., 16, 195–214, https://doi.org/10.5194/acp-16-195-2016, https://doi.org/10.5194/acp-16-195-2016, 2016
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We quantify the processes responsible for methane growth rate variability in the period 1990 to 1995, a period with variations in climate and radiation due to the Pinatubo eruption. We find significant contributions from changes in the methane emission from wetlands, and in the methane removal by OH caused by stratospheric aerosols, by the decrease in temperature and water vapour, by stratospheric ozone depletion and by changes in emissions of CO and NMVOC.
S. Walter, A. Kock, T. Steinhoff, B. Fiedler, P. Fietzek, J. Kaiser, M. Krol, M. E. Popa, Q. Chen, T. Tanhua, and T. Röckmann
Biogeosciences, 13, 323–340, https://doi.org/10.5194/bg-13-323-2016, https://doi.org/10.5194/bg-13-323-2016, 2016
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Oceans are a source of H2, an indirect greenhouse gas. Measurements constraining the temporal and spatial patterns of oceanic H2 emissions are sparse and although H2 is assumed to be produced mainly biologically, direct evidence for biogenic marine production was lacking. By analyzing the H2 isotopic composition (δD) we were able to constrain the global H2 budget in more detail, verify biogenic production and point to additional sources. We also showed that current models are reasonably working.
S. L. Pathirana, C. van der Veen, M. E. Popa, and T. Röckmann
Atmos. Meas. Tech., 8, 5315–5324, https://doi.org/10.5194/amt-8-5315-2015, https://doi.org/10.5194/amt-8-5315-2015, 2015
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CO is established as an important indirect greenhouse gas, as it is the major sink for the OH∙. We have developed a fully automated system for the determination of δ13C and δ18O in atmospheric CO. The blank signal of the Schütze reagent is 1-3 % of the typical sample size. The repeatability is 0.1 ‰ for δ13C and 0.2 ‰ for δ18O. The analytical repeatability for the mole fraction is ~0.7 nmol mol-1 for 100 mL of ambient air (185.4 nmol mol-1 of CO). A single measurement is performed in 18 min.
S. X. Fang, P. P. Tans, M. Steinbacher, L. X. Zhou, and T. Luan
Atmos. Meas. Tech., 8, 5301–5313, https://doi.org/10.5194/amt-8-5301-2015, https://doi.org/10.5194/amt-8-5301-2015, 2015
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The identification of atmospheric CO2 observation data which are minimally influenced by very local emissions/removals is essential for trend analysis and for the estimation of regional sources and sinks. We compared four data filtering regimes based on the observation records at Lin'an station in China, and found that the use of meteorological parameters was the most favorable. This conclusion will aid regional data selection at the Lin'an station.
J. M. Barlow, P. I. Palmer, L. M. Bruhwiler, and P. Tans
Atmos. Chem. Phys., 15, 13739–13758, https://doi.org/10.5194/acp-15-13739-2015, https://doi.org/10.5194/acp-15-13739-2015, 2015
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The major results from our analysis include (1) a significant revision to previously reported estimates of phase changes in the seasonal cycle atmospheric CO2, which are more closely related to changes in the terrestrial biosphere; and (2) an indirect observation that is consistent with high northern latitude ecosystems progressively taking up more CO2 during spring and early summer.
J. Timkovsky, A. W. H. Chan, T. Dorst, A. H. Goldstein, B. Oyama, and R. Holzinger
Atmos. Meas. Tech., 8, 5177–5187, https://doi.org/10.5194/amt-8-5177-2015, https://doi.org/10.5194/amt-8-5177-2015, 2015
C. Le Quéré, R. Moriarty, R. M. Andrew, J. G. Canadell, S. Sitch, J. I. Korsbakken, P. Friedlingstein, G. P. Peters, R. J. Andres, T. A. Boden, R. A. Houghton, J. I. House, R. F. Keeling, P. Tans, A. Arneth, D. C. E. Bakker, L. Barbero, L. Bopp, J. Chang, F. Chevallier, L. P. Chini, P. Ciais, M. Fader, R. A. Feely, T. Gkritzalis, I. Harris, J. Hauck, T. Ilyina, A. K. Jain, E. Kato, V. Kitidis, K. Klein Goldewijk, C. Koven, P. Landschützer, S. K. Lauvset, N. Lefèvre, A. Lenton, I. D. Lima, N. Metzl, F. Millero, D. R. Munro, A. Murata, J. E. M. S. Nabel, S. Nakaoka, Y. Nojiri, K. O'Brien, A. Olsen, T. Ono, F. F. Pérez, B. Pfeil, D. Pierrot, B. Poulter, G. Rehder, C. Rödenbeck, S. Saito, U. Schuster, J. Schwinger, R. Séférian, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, I. T. van der Laan-Luijkx, G. R. van der Werf, S. van Heuven, D. Vandemark, N. Viovy, A. Wiltshire, S. Zaehle, and N. Zeng
Earth Syst. Sci. Data, 7, 349–396, https://doi.org/10.5194/essd-7-349-2015, https://doi.org/10.5194/essd-7-349-2015, 2015
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Accurate assessment of anthropogenic carbon dioxide emissions and their redistribution among the atmosphere, ocean, and terrestrial biosphere is important to understand the global carbon cycle, support the development of climate policies, and project future climate change. We describe data sets and a methodology to quantify all major components of the global carbon budget, including their uncertainties, based on a range of data and models and their interpretation by a broad scientific community.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021, https://doi.org/10.5194/acp-15-13003-2015, https://doi.org/10.5194/acp-15-13003-2015, 2015
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We investigated soil production and uptake of H2 and associated isotope effects. Uptake and emission of H2 occurred simultaneously at all sampling sites, with strongest emission where N2 fixing legume was present. The fractionation constant during soil uptake was about 0.945 and it did not show positive correlation with deposition velocity. The isotopic composition of H2 emitted from soil with legume was about -530‰, which is less deuterium-depleted than isotope equilibrium between H2O and H2.
R. Holzinger
Atmos. Meas. Tech., 8, 3903–3922, https://doi.org/10.5194/amt-8-3903-2015, https://doi.org/10.5194/amt-8-3903-2015, 2015
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629, https://doi.org/10.5194/acp-15-8615-2015, https://doi.org/10.5194/acp-15-8615-2015, 2015
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This study attempts to determine the feasibility of a new assimilation method of satellite measurements of CH4 and CO2 for optimization of their surface fluxes in a synthetic environment. Instead of their absolute concentrations, we assimilate the ratios of their concentrations (CH4/CO2) in our inversion. Doing so helps us to reduce the effect of atmospheric scattering on the measurements in our system. However, assimilation of the ratios makes the inversion non-linear.
K. Ishijima, M. Takigawa, K. Sudo, S. Toyoda, N. Yoshida, T. Röckmann, J. Kaiser, S. Aoki, S. Morimoto, S. Sugawara, and T. Nakazawa
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-19947-2015, https://doi.org/10.5194/acpd-15-19947-2015, 2015
Revised manuscript not accepted
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We developed an atmospheric N2O isotopocule model based on a chemistry-coupled atmospheric general circulation model and a simple method to optimize the model, and estimated the isotopic signatures of surface sources at the hemispheric scale. Data obtained from ground-based observations, measurements of firn air, and balloon and aircraft flights were used to optimize the long-term trends, interhemispheric gradients, and photolytic fractionation, respectively, in the model.
B. Lemieux-Dudon, L. Bazin, A. Landais, H. Toyé Mahamadou Kele, M. Guillevic, P. Kindler, F. Parrenin, and P. Martinerie
Clim. Past, 11, 959–978, https://doi.org/10.5194/cp-11-959-2015, https://doi.org/10.5194/cp-11-959-2015, 2015
S. J. Allin, J. C. Laube, E. Witrant, J. Kaiser, E. McKenna, P. Dennis, R. Mulvaney, E. Capron, P. Martinerie, T. Röckmann, T. Blunier, J. Schwander, P. J. Fraser, R. L. Langenfelds, and W. T. Sturges
Atmos. Chem. Phys., 15, 6867–6877, https://doi.org/10.5194/acp-15-6867-2015, https://doi.org/10.5194/acp-15-6867-2015, 2015
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Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons (CFCs) are man-made compounds which act to destroy this barrier.
This paper presents (1) the first measurements of the stratospheric δ(37Cl) of CFCs -11 and -113; (2) the first quantification of long-term trends in the tropospheric δ(37Cl) of CFCs -11, -12 and -113.
This study provides a better understanding of source and sink processes associated with these destructive compounds.
L. J. Kramer, D. Helmig, J. F. Burkhart, A. Stohl, S. Oltmans, and R. E. Honrath
Atmos. Chem. Phys., 15, 6827–6849, https://doi.org/10.5194/acp-15-6827-2015, https://doi.org/10.5194/acp-15-6827-2015, 2015
L. K. Emmons, S. R. Arnold, S. A. Monks, V. Huijnen, S. Tilmes, K. S. Law, J. L. Thomas, J.-C. Raut, I. Bouarar, S. Turquety, Y. Long, B. Duncan, S. Steenrod, S. Strode, J. Flemming, J. Mao, J. Langner, A. M. Thompson, D. Tarasick, E. C. Apel, D. R. Blake, R. C. Cohen, J. Dibb, G. S. Diskin, A. Fried, S. R. Hall, L. G. Huey, A. J. Weinheimer, A. Wisthaler, T. Mikoviny, J. Nowak, J. Peischl, J. M. Roberts, T. Ryerson, C. Warneke, and D. Helmig
Atmos. Chem. Phys., 15, 6721–6744, https://doi.org/10.5194/acp-15-6721-2015, https://doi.org/10.5194/acp-15-6721-2015, 2015
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Eleven 3-D tropospheric chemistry models have been compared and evaluated with observations in the Arctic during the International Polar Year (IPY 2008). Large differences are seen among the models, particularly related to the model chemistry of volatile organic compounds (VOCs) and reactive nitrogen (NOx, PAN, HNO3) partitioning. Consistency among the models in the underestimation of CO, ethane and propane indicates the emission inventory is too low for these compounds.
S. Preunkert, M. Legrand, M. M. Frey, A. Kukui, J. Savarino, H. Gallée, M. King, B. Jourdain, W. Vicars, and D. Helmig
Atmos. Chem. Phys., 15, 6689–6705, https://doi.org/10.5194/acp-15-6689-2015, https://doi.org/10.5194/acp-15-6689-2015, 2015
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During two austral summers HCHO was investigated in air, snow, and interstitial air at the Concordia site located on the East Antarctic Plateau. Snow emission fluxes were estimated to be around 1 to 2 and 3 to 5 x 10^12 molecules m-2 s-1 at night and at noon, respectively. Shading experiments suggest that the photochemical HCHO production in the snowpack at Concordia remains negligible. The mean HCHO level of 130pptv observed at 1m above the surface is quite well reproduced by 1-D simulations.
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.
C. Le Quéré, R. Moriarty, R. M. Andrew, G. P. Peters, P. Ciais, P. Friedlingstein, S. D. Jones, S. Sitch, P. Tans, A. Arneth, T. A. Boden, L. Bopp, Y. Bozec, J. G. Canadell, L. P. Chini, F. Chevallier, C. E. Cosca, I. Harris, M. Hoppema, R. A. Houghton, J. I. House, A. K. Jain, T. Johannessen, E. Kato, R. F. Keeling, V. Kitidis, K. Klein Goldewijk, C. Koven, C. S. Landa, P. Landschützer, A. Lenton, I. D. Lima, G. Marland, J. T. Mathis, N. Metzl, Y. Nojiri, A. Olsen, T. Ono, S. Peng, W. Peters, B. Pfeil, B. Poulter, M. R. Raupach, P. Regnier, C. Rödenbeck, S. Saito, J. E. Salisbury, U. Schuster, J. Schwinger, R. Séférian, J. Segschneider, T. Steinhoff, B. D. Stocker, A. J. Sutton, T. Takahashi, B. Tilbrook, G. R. van der Werf, N. Viovy, Y.-P. Wang, R. Wanninkhof, A. Wiltshire, and N. Zeng
Earth Syst. Sci. Data, 7, 47–85, https://doi.org/10.5194/essd-7-47-2015, https://doi.org/10.5194/essd-7-47-2015, 2015
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Carbon dioxide (CO2) emissions from human activities (burning fossil fuels and cement production, deforestation and other land-use change) are set to rise again in 2014.
This study (updated yearly) makes an accurate assessment of anthropogenic CO2 emissions and their redistribution between the atmosphere, ocean, and terrestrial biosphere in order to better understand the global carbon cycle, support the development of climate policies, and project future climate change.
K. Dzepina, C. Mazzoleni, P. Fialho, S. China, B. Zhang, R. C. Owen, D. Helmig, J. Hueber, S. Kumar, J. A. Perlinger, L. J. Kramer, M. P. Dziobak, M. T. Ampadu, S. Olsen, D. J. Wuebbles, and L. R. Mazzoleni
Atmos. Chem. Phys., 15, 5047–5068, https://doi.org/10.5194/acp-15-5047-2015, https://doi.org/10.5194/acp-15-5047-2015, 2015
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Aerosol was sampled at the Pico Mountain Observatory located at 2.2km amsl on Pico Island of the North Atlantic Azores archipelago. Two aerosol samples characterized by ultrahigh resolution mass spectrometry had biomass burning and marine emissions origins, as corroborated by collocated gas- and particle-phase measurements, air masses analyses and satellites. The paper presents the first molecular characterization of aged and processed aerosol intercepted at a remote lower free troposphere
A. P. Ballantyne, R. Andres, R. Houghton, B. D. Stocker, R. Wanninkhof, W. Anderegg, L. A. Cooper, M. DeGrandpre, P. P. Tans, J. B. Miller, C. Alden, and J. W. C. White
Biogeosciences, 12, 2565–2584, https://doi.org/10.5194/bg-12-2565-2015, https://doi.org/10.5194/bg-12-2565-2015, 2015
R. J. Matear, A. Lenton, D. Etheridge, and S. J. Phipps
Clim. Past Discuss., https://doi.org/10.5194/cpd-11-1093-2015, https://doi.org/10.5194/cpd-11-1093-2015, 2015
Revised manuscript has not been submitted
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Global climate models provide an important tool for simulating the earth's climate. Here we present a simulation of the climate of the Last Glacial Maximum, which was obtained by setting atmospheric greenhouse gas concentrations and the earth's orbital parameters to the 21 000 years before present values. We simulate an ocean behaviour that agrees with paleoclimate reconstructions supporting our ability to model the climate system and use the model to explore the impacts on the carbon cycle.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301, https://doi.org/10.5194/amt-8-1287-2015, https://doi.org/10.5194/amt-8-1287-2015, 2015
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We present the capability of an aerosol retrieval algorithm, intended for multi-angle, multi-wavelength photopolarimetric measurements, to intrinsically screen for sub-pixel liquid water cloud contamination.
The screening is based on goodness-of-fit criteria. The algorithm has been applied to a synthetic data set of partially clouded scenes and (non-cloud-screened) POLDER3/PARASOL observations.
A. Ghosh, P. K. Patra, K. Ishijima, T. Umezawa, A. Ito, D. M. Etheridge, S. Sugawara, K. Kawamura, J. B. Miller, E. J. Dlugokencky, P. B. Krummel, P. J. Fraser, L. P. Steele, R. L. Langenfelds, C. M. Trudinger, J. W. C. White, B. Vaughn, T. Saeki, S. Aoki, and T. Nakazawa
Atmos. Chem. Phys., 15, 2595–2612, https://doi.org/10.5194/acp-15-2595-2015, https://doi.org/10.5194/acp-15-2595-2015, 2015
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Atmospheric CH4 increased from 900ppb to 1800ppb during the period 1900–2010 at a rate unprecedented in any observational records. We use bottom-up emissions and a chemistry-transport model to simulate CH4. The optimized global total CH4 emission, estimated from the model–observation differences, increased at fastest rate during 1940–1990. Using δ13C of CH4 measurements we attribute this emission increase to biomass burning. Total CH4 lifetime is shortened by 4% over the simulation period.
S. J. Sutanto, G. Hoffmann, R. A. Scheepmaker, J. Worden, S. Houweling, K. Yoshimura, I. Aben, and T. Röckmann
Atmos. Meas. Tech., 8, 999–1019, https://doi.org/10.5194/amt-8-999-2015, https://doi.org/10.5194/amt-8-999-2015, 2015
Emma C. Leedham Elvidge, D. E. Oram, J. C. Laube, A. K. Baker, S. A. Montzka, S. Humphrey, D. A. O'Sullivan, and C. A. M. Brenninkmeijer
Atmos. Chem. Phys., 15, 1939–1958, https://doi.org/10.5194/acp-15-1939-2015, https://doi.org/10.5194/acp-15-1939-2015, 2015
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822, https://doi.org/10.5194/amt-8-811-2015, https://doi.org/10.5194/amt-8-811-2015, 2015
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Our analytical system is a promising tool for investigating the triple oxygen isotope composition of CO2 from stratospheric air samples of volumes 100ml and smaller. The method is designed for measuring air samples with CO2 mole fractions between 360 and 400ppm, and it is the first fully automated analytical system that uses CeO2 as the isotope exchange medium.
Emma C. Leedham Elvidge, S.-M. Phang, W. T. Sturges, and G. Malin
Biogeosciences, 12, 387–398, https://doi.org/10.5194/bg-12-387-2015, https://doi.org/10.5194/bg-12-387-2015, 2015
R. Ahmadov, S. McKeen, M. Trainer, R. Banta, A. Brewer, S. Brown, P. M. Edwards, J. A. de Gouw, G. J. Frost, J. Gilman, D. Helmig, B. Johnson, A. Karion, A. Koss, A. Langford, B. Lerner, J. Olson, S. Oltmans, J. Peischl, G. Pétron, Y. Pichugina, J. M. Roberts, T. Ryerson, R. Schnell, C. Senff, C. Sweeney, C. Thompson, P. R. Veres, C. Warneke, R. Wild, E. J. Williams, B. Yuan, and R. Zamora
Atmos. Chem. Phys., 15, 411–429, https://doi.org/10.5194/acp-15-411-2015, https://doi.org/10.5194/acp-15-411-2015, 2015
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High 2013 wintertime O3 pollution events associated with oil/gas production within the Uinta Basin are studied using a 3D model. It's able quantitatively to reproduce these events using emission estimates of O3 precursors based on ambient measurements (top-down approach), but unable to reproduce them using a recent bottom-up emission inventory for the oil/gas industry. The role of various physical and meteorological processes, chemical species and pathways contributing to high O3 are quantified.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
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Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
K. A. Masarie, W. Peters, A. R. Jacobson, and P. P. Tans
Earth Syst. Sci. Data, 6, 375–384, https://doi.org/10.5194/essd-6-375-2014, https://doi.org/10.5194/essd-6-375-2014, 2014
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Observation Package (ObsPack) is a framework designed to bring together atmospheric greenhouse gas measurements from a variety of sampling platforms, prepare them with specific applications in mind, and package and distribute them in a self-consistent and well-documented product. The framework includes a unique distribution stategy designed to improve communication between product users and data providers. The concepts presented are general and may be easily applied to other scientific data.
M. Inoue, I. Morino, O. Uchino, Y. Miyamoto, T. Saeki, Y. Yoshida, T. Yokota, C. Sweeney, P. P. Tans, S. C. Biraud, T. Machida, J. V. Pittman, E. A. Kort, T. Tanaka, S. Kawakami, Y. Sawa, K. Tsuboi, and H. Matsueda
Atmos. Meas. Tech., 7, 2987–3005, https://doi.org/10.5194/amt-7-2987-2014, https://doi.org/10.5194/amt-7-2987-2014, 2014
L. Bruhwiler, E. Dlugokencky, K. Masarie, M. Ishizawa, A. Andrews, J. Miller, C. Sweeney, P. Tans, and D. Worthy
Atmos. Chem. Phys., 14, 8269–8293, https://doi.org/10.5194/acp-14-8269-2014, https://doi.org/10.5194/acp-14-8269-2014, 2014
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, Emma C. Leedham Elvidge, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
S. J. Sutanto, B. van den Hurk, P. A. Dirmeyer, S. I. Seneviratne, T. Röckmann, K. E. Trenberth, E. M. Blyth, J. Wenninger, and G. Hoffmann
Hydrol. Earth Syst. Sci., 18, 2815–2827, https://doi.org/10.5194/hess-18-2815-2014, https://doi.org/10.5194/hess-18-2815-2014, 2014
S. J. Oltmans, A. Karion, R. C. Schnell, G. Pétron, C. Sweeney, S. Wolter, D. Neff, S. A. Montzka, B. R. Miller, D. Helmig, B. J. Johnson, and J. Hueber
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-14-20117-2014, https://doi.org/10.5194/acpd-14-20117-2014, 2014
Revised manuscript not accepted
U. Dusek, M. Monaco, M. Prokopiou, F. Gongriep, R. Hitzenberger, H. A. J. Meijer, and T. Röckmann
Atmos. Meas. Tech., 7, 1943–1955, https://doi.org/10.5194/amt-7-1943-2014, https://doi.org/10.5194/amt-7-1943-2014, 2014
A. J. van Beelen, G. J. H. Roelofs, O. P. Hasekamp, J. S. Henzing, and T. Röckmann
Atmos. Chem. Phys., 14, 5969–5987, https://doi.org/10.5194/acp-14-5969-2014, https://doi.org/10.5194/acp-14-5969-2014, 2014
C. Le Quéré, G. P. Peters, R. J. Andres, R. M. Andrew, T. A. Boden, P. Ciais, P. Friedlingstein, R. A. Houghton, G. Marland, R. Moriarty, S. Sitch, P. Tans, A. Arneth, A. Arvanitis, D. C. E. Bakker, L. Bopp, J. G. Canadell, L. P. Chini, S. C. Doney, A. Harper, I. Harris, J. I. House, A. K. Jain, S. D. Jones, E. Kato, R. F. Keeling, K. Klein Goldewijk, A. Körtzinger, C. Koven, N. Lefèvre, F. Maignan, A. Omar, T. Ono, G.-H. Park, B. Pfeil, B. Poulter, M. R. Raupach, P. Regnier, C. Rödenbeck, S. Saito, J. Schwinger, J. Segschneider, B. D. Stocker, T. Takahashi, B. Tilbrook, S. van Heuven, N. Viovy, R. Wanninkhof, A. Wiltshire, and S. Zaehle
Earth Syst. Sci. Data, 6, 235–263, https://doi.org/10.5194/essd-6-235-2014, https://doi.org/10.5194/essd-6-235-2014, 2014
O. Peltola, A. Hensen, C. Helfter, L. Belelli Marchesini, F. C. Bosveld, W. C. M. van den Bulk, J. A. Elbers, S. Haapanala, J. Holst, T. Laurila, A. Lindroth, E. Nemitz, T. Röckmann, A. T. Vermeulen, and I. Mammarella
Biogeosciences, 11, 3163–3186, https://doi.org/10.5194/bg-11-3163-2014, https://doi.org/10.5194/bg-11-3163-2014, 2014
H. F. Zhang, B. Z. Chen, I. T. van der Laan-Luijk, T. Machida, H. Matsueda, Y. Sawa, Y. Fukuyama, R. Langenfelds, M. van der Schoot, G. Xu, J. W. Yan, M. L. Cheng, L. X. Zhou, P. P. Tans, and W. Peters
Atmos. Chem. Phys., 14, 5807–5824, https://doi.org/10.5194/acp-14-5807-2014, https://doi.org/10.5194/acp-14-5807-2014, 2014
P. Boylan, D. Helmig, and J.-H. Park
Atmos. Meas. Tech., 7, 1231–1244, https://doi.org/10.5194/amt-7-1231-2014, https://doi.org/10.5194/amt-7-1231-2014, 2014
S. Houweling, M. Krol, P. Bergamaschi, C. Frankenberg, E. J. Dlugokencky, I. Morino, J. Notholt, V. Sherlock, D. Wunch, V. Beck, C. Gerbig, H. Chen, E. A. Kort, T. Röckmann, and I. Aben
Atmos. Chem. Phys., 14, 3991–4012, https://doi.org/10.5194/acp-14-3991-2014, https://doi.org/10.5194/acp-14-3991-2014, 2014
B. Ringeval, S. Houweling, P. M. van Bodegom, R. Spahni, R. van Beek, F. Joos, and T. Röckmann
Biogeosciences, 11, 1519–1558, https://doi.org/10.5194/bg-11-1519-2014, https://doi.org/10.5194/bg-11-1519-2014, 2014
S. X. Fang, L. X. Zhou, P. P. Tans, P. Ciais, M. Steinbacher, L. Xu, and T. Luan
Atmos. Chem. Phys., 14, 2541–2554, https://doi.org/10.5194/acp-14-2541-2014, https://doi.org/10.5194/acp-14-2541-2014, 2014
B. Zhang, R. C. Owen, J. A. Perlinger, A. Kumar, S. Wu, M. Val Martin, L. Kramer, D. Helmig, and R. E. Honrath
Atmos. Chem. Phys., 14, 2267–2287, https://doi.org/10.5194/acp-14-2267-2014, https://doi.org/10.5194/acp-14-2267-2014, 2014
A. E. Andrews, J. D. Kofler, M. E. Trudeau, J. C. Williams, D. H. Neff, K. A. Masarie, D. Y. Chao, D. R. Kitzis, P. C. Novelli, C. L. Zhao, E. J. Dlugokencky, P. M. Lang, M. J. Crotwell, M. L. Fischer, M. J. Parker, J. T. Lee, D. D. Baumann, A. R. Desai, C. O. Stanier, S. F. J. De Wekker, D. E. Wolfe, J. W. Munger, and P. P. Tans
Atmos. Meas. Tech., 7, 647–687, https://doi.org/10.5194/amt-7-647-2014, https://doi.org/10.5194/amt-7-647-2014, 2014
M. E. Popa, M. K. Vollmer, A. Jordan, W. A. Brand, S. L. Pathirana, M. Rothe, and T. Röckmann
Atmos. Chem. Phys., 14, 2105–2123, https://doi.org/10.5194/acp-14-2105-2014, https://doi.org/10.5194/acp-14-2105-2014, 2014
A. Kumar, S. Wu, M. F. Weise, R. Honrath, R. C. Owen, D. Helmig, L. Kramer, M. Val Martin, and Q. Li
Atmos. Chem. Phys., 13, 12537–12547, https://doi.org/10.5194/acp-13-12537-2013, https://doi.org/10.5194/acp-13-12537-2013, 2013
B. W. LaFranchi, G. Pétron, J. B. Miller, S. J. Lehman, A. E. Andrews, E. J. Dlugokencky, B. Hall, B. R. Miller, S. A. Montzka, W. Neff, P. C. Novelli, C. Sweeney, J. C. Turnbull, D. E. Wolfe, P. P. Tans, K. R. Gurney, and T. P. Guilderson
Atmos. Chem. Phys., 13, 11101–11120, https://doi.org/10.5194/acp-13-11101-2013, https://doi.org/10.5194/acp-13-11101-2013, 2013
J. Timkovsky, P. Gankema, R. Pierik, and R. Holzinger
Atmos. Meas. Tech. Discuss., https://doi.org/10.5194/amtd-6-9005-2013, https://doi.org/10.5194/amtd-6-9005-2013, 2013
Preprint withdrawn
R. Holzinger, A. H. Goldstein, P. L. Hayes, J. L. Jimenez, and J. Timkovsky
Atmos. Chem. Phys., 13, 10125–10141, https://doi.org/10.5194/acp-13-10125-2013, https://doi.org/10.5194/acp-13-10125-2013, 2013
M. Inoue, I. Morino, O. Uchino, Y. Miyamoto, Y. Yoshida, T. Yokota, T. Machida, Y. Sawa, H. Matsueda, C. Sweeney, P. P. Tans, A. E. Andrews, S. C. Biraud, T. Tanaka, S. Kawakami, and P. K. Patra
Atmos. Chem. Phys., 13, 9771–9788, https://doi.org/10.5194/acp-13-9771-2013, https://doi.org/10.5194/acp-13-9771-2013, 2013
F. A. Haumann, A. M. Batenburg, G. Pieterse, C. Gerbig, M. C. Krol, and T. Röckmann
Atmos. Chem. Phys., 13, 9401–9413, https://doi.org/10.5194/acp-13-9401-2013, https://doi.org/10.5194/acp-13-9401-2013, 2013
M. von Hobe, S. Bekki, S. Borrmann, F. Cairo, F. D'Amato, G. Di Donfrancesco, A. Dörnbrack, A. Ebersoldt, M. Ebert, C. Emde, I. Engel, M. Ern, W. Frey, S. Genco, S. Griessbach, J.-U. Grooß, T. Gulde, G. Günther, E. Hösen, L. Hoffmann, V. Homonnai, C. R. Hoyle, I. S. A. Isaksen, D. R. Jackson, I. M. Jánosi, R. L. Jones, K. Kandler, C. Kalicinsky, A. Keil, S. M. Khaykin, F. Khosrawi, R. Kivi, J. Kuttippurath, J. C. Laube, F. Lefèvre, R. Lehmann, S. Ludmann, B. P. Luo, M. Marchand, J. Meyer, V. Mitev, S. Molleker, R. Müller, H. Oelhaf, F. Olschewski, Y. Orsolini, T. Peter, K. Pfeilsticker, C. Piesch, M. C. Pitts, L. R. Poole, F. D. Pope, F. Ravegnani, M. Rex, M. Riese, T. Röckmann, B. Rognerud, A. Roiger, C. Rolf, M. L. Santee, M. Scheibe, C. Schiller, H. Schlager, M. Siciliani de Cumis, N. Sitnikov, O. A. Søvde, R. Spang, N. Spelten, F. Stordal, O. Sumińska-Ebersoldt, A. Ulanovski, J. Ungermann, S. Viciani, C. M. Volk, M. vom Scheidt, P. von der Gathen, K. Walker, T. Wegner, R. Weigel, S. Weinbruch, G. Wetzel, F. G. Wienhold, I. Wohltmann, W. Woiwode, I. A. K. Young, V. Yushkov, B. Zobrist, and F. Stroh
Atmos. Chem. Phys., 13, 9233–9268, https://doi.org/10.5194/acp-13-9233-2013, https://doi.org/10.5194/acp-13-9233-2013, 2013
P. M. Edwards, C. J. Young, K. Aikin, J. deGouw, W. P. Dubé, F. Geiger, J. Gilman, D. Helmig, J. S. Holloway, J. Kercher, B. Lerner, R. Martin, R. McLaren, D. D. Parrish, J. Peischl, J. M. Roberts, T. B. Ryerson, J. Thornton, C. Warneke, E. J. Williams, and S. S. Brown
Atmos. Chem. Phys., 13, 8955–8971, https://doi.org/10.5194/acp-13-8955-2013, https://doi.org/10.5194/acp-13-8955-2013, 2013
P. Sperlich, C. Buizert, T. M. Jenk, C. J. Sapart, M. Prokopiou, T. Röckmann, and T. Blunier
Atmos. Meas. Tech., 6, 2027–2041, https://doi.org/10.5194/amt-6-2027-2013, https://doi.org/10.5194/amt-6-2027-2013, 2013
V. V. Petrenko, P. Martinerie, P. Novelli, D. M. Etheridge, I. Levin, Z. Wang, T. Blunier, J. Chappellaz, J. Kaiser, P. Lang, L. P. Steele, S. Hammer, J. Mak, R. L. Langenfelds, J. Schwander, J. P. Severinghaus, E. Witrant, G. Petron, M. O. Battle, G. Forster, W. T. Sturges, J.-F. Lamarque, K. Steffen, and J. W. C. White
Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, https://doi.org/10.5194/acp-13-7567-2013, 2013
L. Bazin, A. Landais, B. Lemieux-Dudon, H. Toyé Mahamadou Kele, D. Veres, F. Parrenin, P. Martinerie, C. Ritz, E. Capron, V. Lipenkov, M.-F. Loutre, D. Raynaud, B. Vinther, A. Svensson, S. O. Rasmussen, M. Severi, T. Blunier, M. Leuenberger, H. Fischer, V. Masson-Delmotte, J. Chappellaz, and E. Wolff
Clim. Past, 9, 1715–1731, https://doi.org/10.5194/cp-9-1715-2013, https://doi.org/10.5194/cp-9-1715-2013, 2013
D. Veres, L. Bazin, A. Landais, H. Toyé Mahamadou Kele, B. Lemieux-Dudon, F. Parrenin, P. Martinerie, E. Blayo, T. Blunier, E. Capron, J. Chappellaz, S. O. Rasmussen, M. Severi, A. Svensson, B. Vinther, and E. W. Wolff
Clim. Past, 9, 1733–1748, https://doi.org/10.5194/cp-9-1733-2013, https://doi.org/10.5194/cp-9-1733-2013, 2013
P. I. Palmer, M. Parrington, J. D. Lee, A. C. Lewis, A. R. Rickard, P. F. Bernath, T. J. Duck, D. L. Waugh, D. W. Tarasick, S. Andrews, E. Aruffo, L. J. Bailey, E. Barrett, S. J.-B. Bauguitte, K. R. Curry, P. Di Carlo, L. Chisholm, L. Dan, G. Forster, J. E. Franklin, M. D. Gibson, D. Griffin, D. Helmig, J. R. Hopkins, J. T. Hopper, M. E. Jenkin, D. Kindred, J. Kliever, M. Le Breton, S. Matthiesen, M. Maurice, S. Moller, D. P. Moore, D. E. Oram, S. J. O'Shea, R. C. Owen, C. M. L. S. Pagniello, S. Pawson, C. J. Percival, J. R. Pierce, S. Punjabi, R. M. Purvis, J. J. Remedios, K. M. Rotermund, K. M. Sakamoto, A. M. da Silva, K. B. Strawbridge, K. Strong, J. Taylor, R. Trigwell, K. A. Tereszchuk, K. A. Walker, D. Weaver, C. Whaley, and J. C. Young
Atmos. Chem. Phys., 13, 6239–6261, https://doi.org/10.5194/acp-13-6239-2013, https://doi.org/10.5194/acp-13-6239-2013, 2013
X. Faïn, D. Helmig, J. Hueber, D. Obrist, and M. W. Williams
Biogeosciences, 10, 3793–3807, https://doi.org/10.5194/bg-10-3793-2013, https://doi.org/10.5194/bg-10-3793-2013, 2013
Emma C. Leedham Elvidge, C. Hughes, F. S. L. Keng, S.-M. Phang, G. Malin, and W. T. Sturges
Biogeosciences, 10, 3615–3633, https://doi.org/10.5194/bg-10-3615-2013, https://doi.org/10.5194/bg-10-3615-2013, 2013
Y. Miyamoto, M. Inoue, I. Morino, O. Uchino, T. Yokota, T. Machida, Y. Sawa, H. Matsueda, C. Sweeney, P. P. Tans, A. E. Andrews, and P. K. Patra
Atmos. Chem. Phys., 13, 5265–5275, https://doi.org/10.5194/acp-13-5265-2013, https://doi.org/10.5194/acp-13-5265-2013, 2013
J. Schmitt, B. Seth, M. Bock, C. van der Veen, L. Möller, C. J. Sapart, M. Prokopiou, T. Sowers, T. Röckmann, and H. Fischer
Atmos. Meas. Tech., 6, 1425–1445, https://doi.org/10.5194/amt-6-1425-2013, https://doi.org/10.5194/amt-6-1425-2013, 2013
S. Walter, A. Kock, and T. Röckmann
Biogeosciences, 10, 3391–3403, https://doi.org/10.5194/bg-10-3391-2013, https://doi.org/10.5194/bg-10-3391-2013, 2013
M. Guillevic, L. Bazin, A. Landais, P. Kindler, A. Orsi, V. Masson-Delmotte, T. Blunier, S. L. Buchardt, E. Capron, M. Leuenberger, P. Martinerie, F. Prié, and B. M. Vinther
Clim. Past, 9, 1029–1051, https://doi.org/10.5194/cp-9-1029-2013, https://doi.org/10.5194/cp-9-1029-2013, 2013
E. Capron, A. Landais, D. Buiron, A. Cauquoin, J. Chappellaz, M. Debret, J. Jouzel, M. Leuenberger, P. Martinerie, V. Masson-Delmotte, R. Mulvaney, F. Parrenin, and F. Prié
Clim. Past, 9, 983–999, https://doi.org/10.5194/cp-9-983-2013, https://doi.org/10.5194/cp-9-983-2013, 2013
H. Chen, A. Karion, C. W. Rella, J. Winderlich, C. Gerbig, A. Filges, T. Newberger, C. Sweeney, and P. P. Tans
Atmos. Meas. Tech., 6, 1031–1040, https://doi.org/10.5194/amt-6-1031-2013, https://doi.org/10.5194/amt-6-1031-2013, 2013
L. Hu, D. B. Millet, S. Y. Kim, K. C. Wells, T. J. Griffis, E. V. Fischer, D. Helmig, J. Hueber, and A. J. Curtis
Atmos. Chem. Phys., 13, 3379–3392, https://doi.org/10.5194/acp-13-3379-2013, https://doi.org/10.5194/acp-13-3379-2013, 2013
S. C. Biraud, M. S. Torn, J. R. Smith, C. Sweeney, W. J. Riley, and P. P. Tans
Atmos. Meas. Tech., 6, 751–763, https://doi.org/10.5194/amt-6-751-2013, https://doi.org/10.5194/amt-6-751-2013, 2013
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
A. Karion, C. Sweeney, S. Wolter, T. Newberger, H. Chen, A. Andrews, J. Kofler, D. Neff, and P. Tans
Atmos. Meas. Tech., 6, 511–526, https://doi.org/10.5194/amt-6-511-2013, https://doi.org/10.5194/amt-6-511-2013, 2013
N. Bândă, M. Krol, M. van Weele, T. van Noije, and T. Röckmann
Atmos. Chem. Phys., 13, 2267–2281, https://doi.org/10.5194/acp-13-2267-2013, https://doi.org/10.5194/acp-13-2267-2013, 2013
C. M. Trudinger, I. G. Enting, P. J. Rayner, D. M. Etheridge, C. Buizert, M. Rubino, P. B. Krummel, and T. Blunier
Atmos. Chem. Phys., 13, 1485–1510, https://doi.org/10.5194/acp-13-1485-2013, https://doi.org/10.5194/acp-13-1485-2013, 2013
J.-H. Park, A. H. Goldstein, J. Timkovsky, S. Fares, R. Weber, J. Karlik, and R. Holzinger
Atmos. Chem. Phys., 13, 1439–1456, https://doi.org/10.5194/acp-13-1439-2013, https://doi.org/10.5194/acp-13-1439-2013, 2013
Related subject area
Subject: Gases | Research Activity: Field Measurements | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Consistency evaluation of tropospheric ozone from ozonesonde and IAGOS (In-service Aircraft for a Global Observing System) observations: vertical distribution, ozonesonde types, and station–airport distance
CO2 and CO temporal variability over Mexico City from ground-based total column and surface measurements
Investigating carbonyl compounds above the Amazon rainforest using a proton-transfer-reaction time-of-flight mass spectrometer (PTR-ToF-MS) with NO+ chemical ionization
Measurement report: In-flight and ground-based measurements of nitrogen oxide emissions from latest-generation jet engines and 100 % sustainable aviation fuel
Measurement report: Sources, sinks, and lifetime of NOx in a suburban temperate forest at night
Measurement report: Urban ammonia and amines in Houston, Texas
Biomass-burning sources control ambient particulate matter, but traffic and industrial sources control volatile organic compound (VOC) emissions and secondary-pollutant formation during extreme pollution events in Delhi
Multi-year observations of variable incomplete combustion in the New York megacity
Observations of the vertical distributions of summertime atmospheric pollutants in Nam Co: OH production and source analysis
Measurement report: Elevated atmospheric ammonia may promote particle pH and HONO formation – insights from the COVID-19 pandemic
Measurement report: Vertical and temporal variability in the near-surface ozone production rate and sensitivity in an urban area in the Pearl River Delta region, China
Elevated oxidized mercury in the free troposphere: analytical advances and application at a remote continental mountaintop site
Using observed urban NOx sinks to constrain VOC reactivity and the ozone and radical budget in the Seoul Metropolitan Area
Real-world emission characteristics of VOCs from typical cargo ships and their potential contributions to secondary organic aerosol and O3 under low-sulfur fuel policies
NO3 reactivity during a summer period in a temperate forest below and above the canopy
The role of oceanic ventilation and terrestrial outflow in atmospheric non-methane hydrocarbons over the Chinese marginal seas
Concentration and source changes of nitrous acid (HONO) during the COVID-19 lockdown in Beijing
Characteristics and sources of nonmethane volatile organic compounds (NMVOCs) and O3–NOx–NMVOC relationships in Zhengzhou, China
Seasonal Air Concentration Variability, Gas/Particle Partitioning, Precipitation Scavenging, and Air-Water Equilibrium of Organophosphate Esters in Southern Canada
Measurement report: Surface exchange fluxes of HONO during the growth process of paddy fields in the Huaihe River Basin, China
Characterization of biogenic volatile organic compounds and their oxidation products at a stressed pine forest close to a biogas power plant
On the dynamics of ozone depletion events at Villum Research Station in the High Arctic
Deciphering anthropogenic and biogenic contributions to selected non-methane volatile organic compound emissions in an urban area
Emission characteristics of reactive organic gases (ROGs) from industrial volatile chemical products (VCPs) in the Pearl River Delta (PRD), China
Measurement report: Enhanced photochemical formation of formic and isocyanic acids in urban regions aloft – insights from tower-based online gradient measurements
Sources of organic gases and aerosol particles and their roles in nighttime particle growth at a rural forested site in southwest Germany
Surface snow bromide and nitrate at Eureka, Canada, in early spring and implications for polar boundary layer chemistry
Molecular and seasonal characteristics of organic vapors in urban Beijing: insights from Vocus-PTR measurements
Opinion: Strengthening research in the Global South – atmospheric science opportunities in South America and Africa
Analysis of ozone vertical profile day-to-day variability in the lower troposphere during the Paris-2022 ACROSS campaign
Shipping and algae emissions have a major impact on ambient air mixing ratios of non-methane hydrocarbons (NMHCs) and methanethiol on Utö Island in the Baltic Sea
Measurement report: Long-term measurements of ozone concentrations in semi-natural African ecosystems
Contribution of cooking emissions to the urban volatile organic compounds in Las Vegas, NV
Reanalysis of NOAA H2 observations: implications for the H2 budget
A large role of missing volatile organic compound reactivity from anthropogenic emissions in ozone pollution regulation
Measurement report: Insights into the chemical composition and origin of molecular clusters and potential precursor molecules present in the free troposphere over the southern Indian Ocean: observations from the Maïdo Observatory (2150 m a.s.l., Réunion)
Ozone deposition measurements over wheat fields in the North China Plain: variability and related factors of deposition flux and velocity
Production of oxygenated volatile organic compounds from the ozonolysis of coastal seawater
Comment on “Transport of substantial stratospheric ozone to the surface by a dying typhoon and shallow convection” by Chen et al. (2022)
Observations of cyanogen bromide (BrCN) in the global troposphere and their relation to polar surface O3 destruction
Individual coal mine methane emissions constrained by eddy covariance measurements: low bias and missing sources
The variations of VOCs based on the policy change of Omicron in polluted winter in traffic-hub city, China
Discovery of reactive chlorine, sulphur and nitrogen containing ambient volatile organic compounds in the megacity of Delhi during both clean and extremely polluted seasons
Measurement report: Observations of ground-level ozone concentration gradients perpendicular to the Lake Ontario shoreline
Measurement report: The Palau Atmospheric Observatory and its ozonesonde record – continuous monitoring of tropospheric composition and dynamics in the tropical western Pacific
Quantifying SO2 oxidation pathways to atmospheric sulfate using stable sulfur and oxygen isotopes: laboratory simulation and field observation
Influences of downward transport and photochemistry on surface ozone over East Antarctica during austral summer: in situ observations and model simulations
Iodine oxoacids and their roles in sub-3 nm particle growth in polluted urban environments
Intensive photochemical oxidation in the marine atmosphere: evidence from direct radical measurements
Diurnal variations in oxygen and nitrogen isotopes of atmospheric nitrogen dioxide and nitrate: implications for tracing NOx oxidation pathways and emission sources
Honglei Wang, David W. Tarasick, Jane Liu, Herman G. J. Smit, Roeland Van Malderen, Lijuan Shen, Romain Blot, and Tianliang Zhao
Atmos. Chem. Phys., 24, 11927–11942, https://doi.org/10.5194/acp-24-11927-2024, https://doi.org/10.5194/acp-24-11927-2024, 2024
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In this study, we identify 23 suitable pairs of sites from World Ozone and Ultraviolet Radiation Data Centre (WOUDC) and In-service Aircraft for a Global Observing System (IAGOS) datasets (1995 to 2021), compare the average vertical distributions of tropospheric O3 from ozonesonde and aircraft measurements, and analyze the differences based on ozonesonde type and station–airport distance.
Noémie Taquet, Wolfgang Stremme, María Eugenia González del Castillo, Victor Almanza, Alejandro Bezanilla, Olivier Laurent, Carlos Alberti, Frank Hase, Michel Ramonet, Thomas Lauvaux, Ke Che, and Michel Grutter
Atmos. Chem. Phys., 24, 11823–11848, https://doi.org/10.5194/acp-24-11823-2024, https://doi.org/10.5194/acp-24-11823-2024, 2024
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We characterize the variability in CO and CO2 emissions over Mexico City from long-term time-resolved Fourier transform infrared spectroscopy solar absorption and surface measurements from 2013 to 2021. Using the average intraday CO growth rate from total columns, the average CO / CO2 ratio and TROPOMI data, we estimate the interannual variability in the CO and CO2 anthropogenic emissions of Mexico City, highlighting the effect of an unprecedented drop in activity due to the COVID-19 lockdown.
Akima Ringsdorf, Achim Edtbauer, Bruna Holanda, Christopher Poehlker, Marta O. Sá, Alessandro Araújo, Jürgen Kesselmeier, Jos Lelieveld, and Jonathan Williams
Atmos. Chem. Phys., 24, 11883–11910, https://doi.org/10.5194/acp-24-11883-2024, https://doi.org/10.5194/acp-24-11883-2024, 2024
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We show the average height distribution of separately observed aldehydes and ketones over a day and discuss their rainforest-specific sources and sinks as well as their seasonal changes above the Amazon. Ketones have much longer atmospheric lifetimes than aldehydes and thus different implications for atmospheric chemistry. However, they are commonly observed together, which we overcome by measuring with a NO+ chemical ionization mass spectrometer for the first time in the Amazon rainforest.
Theresa Harlass, Rebecca Dischl, Stefan Kaufmann, Raphael Märkl, Daniel Sauer, Monika Scheibe, Paul Stock, Tiziana Bräuer, Andreas Dörnbrack, Anke Roiger, Hans Schlager, Ulrich Schumann, Magdalena Pühl, Tobias Schripp, Tobias Grein, Linda Bondorf, Charles Renard, Maxime Gauthier, Mark Johnson, Darren Luff, Paul Madden, Peter Swann, Denise Ahrens, Reetu Sallinen, and Christiane Voigt
Atmos. Chem. Phys., 24, 11807–11822, https://doi.org/10.5194/acp-24-11807-2024, https://doi.org/10.5194/acp-24-11807-2024, 2024
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Emissions from aircraft have a direct impact on our climate. Here, we present airborne and ground-based measurement data of nitrogen oxides that were collected in the exhaust of an Airbus aircraft. We study the impact of burning fossil and sustainable aviation fuel on nitrogen oxide emissions at different engine settings related to combustor temperature, pressure and fuel flow. Further, we compare observations with engine emission models.
Simone T. Andersen, Max R. McGillen, Chaoyang Xue, Tobias Seubert, Patrick Dewald, Gunther N. T. E. Türk, Jan Schuladen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Abdelwahid Mellouki, Lucy J. Carpenter, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 11603–11618, https://doi.org/10.5194/acp-24-11603-2024, https://doi.org/10.5194/acp-24-11603-2024, 2024
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Using measurements of various trace gases in a suburban forest near Paris in the summer of 2022, we were able to gain insight into the sources and sinks of NOx (NO+NO2) with a special focus on their nighttime chemical and physical loss processes. NO was observed as a result of nighttime soil emissions when O3 levels were strongly depleted by deposition. NO oxidation products were not observed at night, indicating that soil and/or foliar surfaces are an efficient sink of reactive N.
Lee Tiszenkel, James H. Flynn, and Shan-Hu Lee
Atmos. Chem. Phys., 24, 11351–11363, https://doi.org/10.5194/acp-24-11351-2024, https://doi.org/10.5194/acp-24-11351-2024, 2024
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Ammonia and amines are important ingredients for aerosol formation in urban environments, but the measurements of these compounds are extremely challenging. Our observations show that urban ammonia and amines in Houston are emitted from urban sources, and diurnal variations in their concentrations are likely governed by gas-to-particle conversion and emissions.
Arpit Awasthi, Baerbel Sinha, Haseeb Hakkim, Sachin Mishra, Varkrishna Mummidivarapu, Gurmanjot Singh, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Vinayak Sinha, and Madhavan N. Rajeevan
Atmos. Chem. Phys., 24, 10279–10304, https://doi.org/10.5194/acp-24-10279-2024, https://doi.org/10.5194/acp-24-10279-2024, 2024
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We use 111 volatile organic compounds (VOCs), PM10, and PM2.5 in a positive matrix factorization (PMF) model to resolve 11 pollution sources validated with chemical fingerprints. Crop residue burning and heating account for ~ 50 % of the PM, while traffic and industrial emissions dominate the gas-phase VOC burden and formation potential of secondary organic aerosols (> 60 %). Non-tailpipe emissions from compressed-natural-gas-fuelled commercial vehicles dominate the transport sector's PM burden.
Luke D. Schiferl, Cong Cao, Bronte Dalton, Andrew Hallward-Driemeier, Ricardo Toledo-Crow, and Róisín Commane
Atmos. Chem. Phys., 24, 10129–10142, https://doi.org/10.5194/acp-24-10129-2024, https://doi.org/10.5194/acp-24-10129-2024, 2024
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Carbon monoxide (CO) is an air pollutant and an important indicator of the incomplete combustion of fossil fuels in cities. Using 4 years of winter and spring observations in New York City, we found that both the magnitude and variability of CO from the metropolitan area are greater than expected. Transportation emissions cannot explain the missing and variable CO, which points to energy from buildings as a likely underappreciated source of urban air pollution and greenhouse gas emissions.
Chengzhi Xing, Cheng Liu, Chunxiang Ye, Jingkai Xue, Hongyu Wu, Xiangguang Ji, Jinping Ou, and Qihou Hu
Atmos. Chem. Phys., 24, 10093–10112, https://doi.org/10.5194/acp-24-10093-2024, https://doi.org/10.5194/acp-24-10093-2024, 2024
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We identified the contributions of ozone (O3) and nitrous acid (HONO) to the production rates of hydroxide (OH) in vertical space on the Tibetan Plateau (TP). A new insight was offered: the contributions of HONO and O3 to the production rates of OH on the TP are even greater than in lower-altitudes areas. This study enriches the understanding of vertical distribution of atmospheric components and explains the strong atmospheric oxidation capacity (AOC) on the TP.
Xinyuan Zhang, Lingling Wang, Nan Wang, Shuangliang Ma, Shenbo Wang, Ruiqin Zhang, Dong Zhang, Mingkai Wang, and Hongyu Zhang
Atmos. Chem. Phys., 24, 9885–9898, https://doi.org/10.5194/acp-24-9885-2024, https://doi.org/10.5194/acp-24-9885-2024, 2024
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This study highlights the importance of the redox reaction of NO2 with SO2 based on actual atmospheric observations. The particle pH in future China is expected to rise steadily. Consequently, this reaction could become a significant source of HONO in China. Therefore, it is crucial to coordinate the control of SO2, NOx, and NH3 emissions to avoid a rapid increase in the particle pH.
Jun Zhou, Chunsheng Zhang, Aiming Liu, Bin Yuan, Yan Wang, Wenjie Wang, Jie-Ping Zhou, Yixin Hao, Xiao-Bing Li, Xianjun He, Xin Song, Yubin Chen, Suxia Yang, Shuchun Yang, Yanfeng Wu, Bin Jiang, Shan Huang, Junwen Liu, Yuwen Peng, Jipeng Qi, Minhui Deng, Bowen Zhong, Yibo Huangfu, and Min Shao
Atmos. Chem. Phys., 24, 9805–9826, https://doi.org/10.5194/acp-24-9805-2024, https://doi.org/10.5194/acp-24-9805-2024, 2024
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In-depth understanding of the near-ground vertical variability in photochemical ozone (O3) formation is crucial for mitigating O3 pollution. Utilizing a self-built vertical observation system, a direct net photochemical O3 production rate detection system, and an observation-based model, we diagnosed the vertical distributions and formation mechanism of net photochemical O3 production rates and sensitivity in the Pearl River Delta region, one of the most O3-polluted areas in China.
Eleanor J. Derry, Tyler R. Elgiar, Taylor Y. Wilmot, Nicholas W. Hoch, Noah S. Hirshorn, Peter Weiss-Penzias, Christopher F. Lee, John C. Lin, A. Gannet Hallar, Rainer Volkamer, Seth N. Lyman, and Lynne E. Gratz
Atmos. Chem. Phys., 24, 9615–9643, https://doi.org/10.5194/acp-24-9615-2024, https://doi.org/10.5194/acp-24-9615-2024, 2024
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Mercury (Hg) is a globally distributed neurotoxic pollutant. Atmospheric deposition is the main source of Hg in ecosystems. However, measurement biases hinder understanding of the origins and abundance of the more bioavailable oxidized form. We used an improved, calibrated measurement system to study air mass composition and transport of atmospheric Hg at a remote mountaintop site in the central US. Oxidized Hg originated upwind in the low to middle free troposphere under clean, dry conditions.
Benjamin A. Nault, Katherine R. Travis, James H. Crawford, Donald R. Blake, Pedro Campuzano-Jost, Ronald C. Cohen, Joshua P. DiGangi, Glenn S. Diskin, Samuel R. Hall, L. Gregory Huey, Jose L. Jimenez, Kyung-Eun Min, Young Ro Lee, Isobel J. Simpson, Kirk Ullmann, and Armin Wisthaler
Atmos. Chem. Phys., 24, 9573–9595, https://doi.org/10.5194/acp-24-9573-2024, https://doi.org/10.5194/acp-24-9573-2024, 2024
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Ozone (O3) is a pollutant formed from the reactions of gases emitted from various sources. In urban areas, the density of human activities can increase the O3 formation rate (P(O3)), thus impacting air quality and health. Observations collected over Seoul, South Korea, are used to constrain P(O3). A high local P(O3) was found; however, local P(O3) was partly reduced due to compounds typically ignored. These observations also provide constraints for unmeasured compounds that will impact P(O3).
Fan Zhang, Binyu Xiao, Zeyu Liu, Yan Zhang, Chongguo Tian, Rui Li, Can Wu, Yali Lei, Si Zhang, Xinyi Wan, Yubao Chen, Yong Han, Min Cui, Cheng Huang, Hongli Wang, Yingjun Chen, and Gehui Wang
Atmos. Chem. Phys., 24, 8999–9017, https://doi.org/10.5194/acp-24-8999-2024, https://doi.org/10.5194/acp-24-8999-2024, 2024
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Mandatory use of low-sulfur fuel due to global sulfur limit regulations means large uncertainties in volatile organic compound (VOC) emissions. On-board tests of VOCs from nine cargo ships in China were carried out. Results showed that switching from heavy-fuel oil to diesel increased emission factor VOCs by 48 % on average, enhancing O3 and the secondary organic aerosol formation potential. Thus, implementing a global ultra-low-sulfur oil policy needs to be optimized in the near future.
Patrick Dewald, Tobias Seubert, Simone T. Andersen, Gunther N. T. E. Türk, Jan Schuladen, Max R. McGillen, Cyrielle Denjean, Jean-Claude Etienne, Olivier Garrouste, Marina Jamar, Sergio Harb, Manuela Cirtog, Vincent Michoud, Mathieu Cazaunau, Antonin Bergé, Christopher Cantrell, Sebastien Dusanter, Bénédicte Picquet-Varrault, Alexandre Kukui, Chaoyang Xue, Abdelwahid Mellouki, Jos Lelieveld, and John N. Crowley
Atmos. Chem. Phys., 24, 8983–8997, https://doi.org/10.5194/acp-24-8983-2024, https://doi.org/10.5194/acp-24-8983-2024, 2024
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In the scope of a field campaign in a suburban forest near Paris in the summer of 2022, we measured the reactivity of the nitrate radical NO3 towards biogenic volatile organic compounds (BVOCs; e.g. monoterpenes) mainly below but also above the canopy. NO3 reactivity was the highest during nights with strong temperature inversions and decreased strongly with height. Reactions with BVOCs were the main removal process of NO3 throughout the diel cycle below the canopy.
Jian Wang, Lei Xue, Qianyao Ma, Feng Xu, Gaobin Xu, Shibo Yan, Jiawei Zhang, Jianlong Li, Honghai Zhang, Guiling Zhang, and Zhaohui Chen
Atmos. Chem. Phys., 24, 8721–8736, https://doi.org/10.5194/acp-24-8721-2024, https://doi.org/10.5194/acp-24-8721-2024, 2024
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This study investigated the distribution and sources of non-methane hydrocarbons (NMHCs) in the lower atmosphere over the marginal seas of China. NMHCs, a subset of volatile organic compounds (VOCs), play a crucial role in atmospheric chemistry. Derived from systematic atmospheric sampling in coastal cities and marginal sea regions, this study offers valuable insights into the interaction between land and sea in shaping offshore atmospheric NMHCs.
Yusheng Zhang, Feixue Zheng, Zemin Feng, Chaofan Lian, Weigang Wang, Xiaolong Fan, Wei Ma, Zhuohui Lin, Chang Li, Gen Zhang, Chao Yan, Ying Zhang, Veli-Matti Kerminen, Federico Bianch, Tuukka Petäjä, Juha Kangasluoma, Markku Kulmala, and Yongchun Liu
Atmos. Chem. Phys., 24, 8569–8587, https://doi.org/10.5194/acp-24-8569-2024, https://doi.org/10.5194/acp-24-8569-2024, 2024
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The nitrous acid (HONO) budget was validated during a COVID-19 lockdown event. The main conclusions are (1) HONO concentrations showed a significant decrease from 0.97 to 0.53 ppb during lockdown; (2) vehicle emissions accounted for 53 % of nighttime sources, with the heterogeneous conversion of NO2 on ground surfaces more important than aerosol; and (3) the dominant daytime source shifted from the homogenous reaction between NO and OH (51 %) to nitrate photolysis (53 %) during lockdown.
Dong Zhang, Xiao Li, Minghao Yuan, Yifei Xu, Qixiang Xu, Fangcheng Su, Shenbo Wang, and Ruiqin Zhang
Atmos. Chem. Phys., 24, 8549–8567, https://doi.org/10.5194/acp-24-8549-2024, https://doi.org/10.5194/acp-24-8549-2024, 2024
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The increasing concentration of O3 precursors and unfavorable meteorological conditions are key factors in the formation of O3 pollution in Zhengzhou. Vehicular exhausts (28 %), solvent usage (27 %), and industrial production (22 %) are identified as the main sources of NMVOCs. Moreover, O3 formation in Zhengzhou is found to be in an anthropogenic volatile organic compound (AVOC)-limited regime. Thus, to reduce O3 formation, a minimum AVOCs / NOx reduction ratio ≥ 3 : 1 is recommended.
Yuening Li, Faqiang Zhan, Chubashini Shunthirasingham, Ying Duan Lei, Jenny Oh, Amina Ben Chaaben, Zhe Lu, Kelsey Lee, Frank A. P. C. Gobas, Hayley Hung, and Frank Wania
EGUsphere, https://doi.org/10.5194/egusphere-2024-1883, https://doi.org/10.5194/egusphere-2024-1883, 2024
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Organophosphate esters are important man-made trace contaminants. Measuring them in the atmospheric gas phase, particles, precipitation and surface water from Canada, we explore seasonal concentration variability, gas/particle partitioning, precipitation scavenging, and air-water equilibrium. Whereas higher concentrations in summer and efficient precipitation scavenging conform with expectations, the lack of a relationship between compound volatility and gas-particle partitioning is puzzling.
Fanhao Meng, Baobin Han, Min Qin, Wu Fang, Ke Tang, Dou Shao, Zhitang Liao, Jun Duan, Yan Feng, Yong Huang, Ting Ni, and Pinhua Xie
EGUsphere, https://doi.org/10.5194/egusphere-2024-2127, https://doi.org/10.5194/egusphere-2024-2127, 2024
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Comprehensive observations of HONO and NOx fluxes were first performed over paddy fields in the Huaihe River Basin. The consecutive peaks in HONO flux and NO flux demonstrated a potentially enhanced release of HONO and NO due to soil tillage, whereas higher WFPS (~80 %) inhibited microbial processes following irrigation. Notably, the biological processes and light-driven NO2 reactions on the surface could both be sources of HONO and influence the local HONO budget during rotary tillage.
Junwei Song, Georgios I. Gkatzelis, Ralf Tillmann, Nicolas Brüggemann, Thomas Leisner, and Harald Saathoff
EGUsphere, https://doi.org/10.5194/egusphere-2024-1768, https://doi.org/10.5194/egusphere-2024-1768, 2024
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VOCs and organic aerosol (OA) particles were measured online at an European stressed pine forest site. Higher temperatures can enhance the forest emissions of biogenic VOCs exceeding their photochemical consumption during daytime. Weakly oxidized monoterpene products dominated the VOCs during nighttime. Moreover, increasing relative humidity can promote the gas-to-particle partitioning of these weakly oxidized monoterpene products, leading to increased OA mass.
Jakob Boyd Pernov, Jens Liengaard Hjorth, Lise Lotte Sørensen, and Henrik Skov
EGUsphere, https://doi.org/10.5194/egusphere-2024-1676, https://doi.org/10.5194/egusphere-2024-1676, 2024
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Arctic ozone depletion events (ODEs) occurs every spring and have vast implications for the oxidizing capacity, radiative balance, and mercury oxidation. In this study, we analyze ozone, ODEs, and their connection to meteorological and air mass history variables through statistical analyses, back-trajectories, and machine learning (ML) at Villum Research Station. ODEs are favorable under sunny, calm conditions with air masses arriving from northerly wind directions with sea ice contact.
Arianna Peron, Martin Graus, Marcus Striednig, Christian Lamprecht, Georg Wohlfahrt, and Thomas Karl
Atmos. Chem. Phys., 24, 7063–7083, https://doi.org/10.5194/acp-24-7063-2024, https://doi.org/10.5194/acp-24-7063-2024, 2024
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The anthropogenic fraction of non-methane volatile organic compound (NMVOC) emissions associated with biogenic sources (e.g., terpenes) is investigated based on eddy covariance observations. The anthropogenic fraction of terpene emissions is strongly dependent on season. When analyzing volatile chemical product (VCP) emissions in urban environments, we caution that observations from short-term campaigns might over-/underestimate their significance depending on local and seasonal circumstances.
Sihang Wang, Bin Yuan, Xianjun He, Ru Cui, Xin Song, Yubin Chen, Caihong Wu, Chaomin Wang, Yibo Huangfu, Xiao-Bing Li, Boguang Wang, and Min Shao
Atmos. Chem. Phys., 24, 7101–7121, https://doi.org/10.5194/acp-24-7101-2024, https://doi.org/10.5194/acp-24-7101-2024, 2024
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Emissions of reactive organic gases from industrial volatile chemical product sources are measured. There are large differences among these industrial sources. We show that oxygenated species account for significant contributions to reactive organic gas emissions, especially for industrial sources utilizing water-borne chemicals.
Qing Yang, Xiao-Bing Li, Bin Yuan, Xiaoxiao Zhang, Yibo Huangfu, Lei Yang, Xianjun He, Jipeng Qi, and Min Shao
Atmos. Chem. Phys., 24, 6865–6882, https://doi.org/10.5194/acp-24-6865-2024, https://doi.org/10.5194/acp-24-6865-2024, 2024
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Online vertical gradient measurements of formic and isocyanic acids were made based on a 320 m tower in a megacity. Vertical variations and sources of the two acids were analyzed in this study. We find that formic and isocyanic acids exhibited positive vertical gradients and were mainly contributed by photochemical formations. The formation of formic and isocyanic acids was also significantly enhanced in urban regions aloft.
Junwei Song, Harald Saathoff, Feng Jiang, Linyu Gao, Hengheng Zhang, and Thomas Leisner
Atmos. Chem. Phys., 24, 6699–6717, https://doi.org/10.5194/acp-24-6699-2024, https://doi.org/10.5194/acp-24-6699-2024, 2024
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This study presents concurrent online measurements of organic gas and particles (VOCs and OA) at a forested site in summer. Both VOCs and OA were largely contributed by oxygenated organic compounds. Semi-volatile oxygenated OA and organic nitrate formed from monoterpenes and sesquiterpenes contributed significantly to nighttime particle growth. The results help us to understand the causes of nighttime particle growth regularly observed in summer in central European rural forested environments.
Xin Yang, Kimberly Strong, Alison S. Criscitiello, Marta Santos-Garcia, Kristof Bognar, Xiaoyi Zhao, Pierre Fogal, Kaley A. Walker, Sara M. Morris, and Peter Effertz
Atmos. Chem. Phys., 24, 5863–5886, https://doi.org/10.5194/acp-24-5863-2024, https://doi.org/10.5194/acp-24-5863-2024, 2024
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This study uses snow samples collected from a Canadian high Arctic site, Eureka, to demonstrate that surface snow in early spring is a net sink of atmospheric bromine and nitrogen. Surface snow bromide and nitrate are significantly correlated, indicating the oxidation of reactive nitrogen is accelerated by reactive bromine. In addition, we show evidence that snow photochemical release of reactive bromine is very weak, and its emission flux is much smaller than the deposition flux of bromide.
Zhaojin An, Rujing Yin, Xinyan Zhao, Xiaoxiao Li, Yi Yuan, Junchen Guo, Yuyang Li, Xue Li, Dandan Li, Yaowei Li, Dongbin Wang, Chao Yan, Kebin He, Douglas R. Worsnop, Frank N. Keutsch, and Jingkun Jiang
EGUsphere, https://doi.org/10.5194/egusphere-2024-1325, https://doi.org/10.5194/egusphere-2024-1325, 2024
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Online Vocus-PTR measurements show the compositions and seasonal variations of organic vapors in urban Beijing. With enhanced sensitivity and mass resolution, various sub-ppt level species and organics with multiple oxygens (≥3) were discovered. The fast photooxidation process in summer leads to an increase in both concentration and proportion of organics with multiple oxygens. While in other seasons, the variations of them could be influenced by primary emissions.
Rebecca M. Garland, Katye E. Altieri, Laura Dawidowski, Laura Gallardo, Aderiana Mbandi, Nestor Y. Rojas, and N'datchoh E. Touré
Atmos. Chem. Phys., 24, 5757–5764, https://doi.org/10.5194/acp-24-5757-2024, https://doi.org/10.5194/acp-24-5757-2024, 2024
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This opinion piece focuses on two geographical areas in the Global South where the authors are based that are underrepresented in atmospheric science. This opinion provides context on common challenges and constraints, with suggestions on how the community can address these. The focus is on the strengths of atmospheric science research in these regions. It is these strengths, we believe, that highlight the critical role of Global South researchers in the future of atmospheric science research.
Gerard Ancellet, Camille Viatte, Anne Boynard, François Ravetta, Jacques Pelon, Cristelle Cailteau-Fischbach, Pascal Genau, Julie Capo, Axel Roy, and Philippe Nédélec
EGUsphere, https://doi.org/10.5194/egusphere-2024-892, https://doi.org/10.5194/egusphere-2024-892, 2024
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Characterization of ozone pollution in urban areas has benefited from a measurement campaign in summer 2022 in the Paris region. The analysis is based on 21 days of lidar and aircraft observations. The main objective is a sensitivity analysis of ozone pollution to first the micrometeorological processes in the urban atmospheric boundary layer, and second, the transport of regional pollution. The paper also discuss to what extent satellite observations can track the observed ozone plumes.
Heidi Hellén, Rostislav Kouznetsov, Kaisa Kraft, Jukka Seppälä, Mika Vestenius, Jukka-Pekka Jalkanen, Lauri Laakso, and Hannele Hakola
Atmos. Chem. Phys., 24, 4717–4731, https://doi.org/10.5194/acp-24-4717-2024, https://doi.org/10.5194/acp-24-4717-2024, 2024
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Mixing ratios of C2-C5 NMHCs and methanethiol were measured on an island in the Baltic Sea using an in situ gas chromatograph. Shipping emissions were found to be an important source of ethene, ethyne, propene, and benzene. High summertime mixing ratios of methanethiol and dependence of mixing ratios on seawater temperature and height indicated the biogenic origin to possibly be phytoplankton or macroalgae. These emissions may have a strong impact on SO2 production and new particle formation.
Hagninou Elagnon Venance Donnou, Aristide Barthélémy Akpo, Money Ossohou, Claire Delon, Véronique Yoboué, Dungall Laouali, Marie Ouafo-Leumbe, Pieter Gideon Van Zyl, Ousmane Ndiaye, Eric Gardrat, Maria Dias-Alves, and Corinne Galy-Lacaux
EGUsphere, https://doi.org/10.5194/egusphere-2024-284, https://doi.org/10.5194/egusphere-2024-284, 2024
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Ozone is a secondary air pollutant that is detrimental to human and plant health. A better understanding of its chemical evolution is a challenge for Africa, where it is still under-sampled. Out of 14 sites examined (1995–2020), high levels of O3 are reported in southern Africa. The dominant chemical processes leading to O3 formation are identified. A decrease in O3 is observed at Katibougou (Mali) and Banizoumbou (Niger), and an increase at Zoétélé (Cameroon) and Skukuza (South Africa).
Matthew M. Coggon, Chelsea E. Stockwell, Lu Xu, Jeff Peischl, Jessica B. Gilman, Aaron Lamplugh, Henry J. Bowman, Kenneth Aikin, Colin Harkins, Qindan Zhu, Rebecca H. Schwantes, Jian He, Meng Li, Karl Seltzer, Brian McDonald, and Carsten Warneke
Atmos. Chem. Phys., 24, 4289–4304, https://doi.org/10.5194/acp-24-4289-2024, https://doi.org/10.5194/acp-24-4289-2024, 2024
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Residential and commercial cooking emits pollutants that degrade air quality. Here, ambient observations show that cooking is an important contributor to anthropogenic volatile organic compounds (VOCs) emitted in Las Vegas, NV. These emissions are not fully presented in air quality models, and more work may be needed to quantify emissions from important sources, such as commercial restaurants.
Fabien Paulot, Gabrielle Pétron, Andrew M. Crotwell, and Matteo B. Bertagni
Atmos. Chem. Phys., 24, 4217–4229, https://doi.org/10.5194/acp-24-4217-2024, https://doi.org/10.5194/acp-24-4217-2024, 2024
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New data from the National Oceanic and Atmospheric Administration show that hydrogen (H2) concentrations increased from 2010 to 2019, which is consistent with the simulated increase in H2 photochemical production (mainly from methane). But this cannot be reconciled with the expected decrease (increase) in H2 anthropogenic emissions (soil deposition) in the same period. This shows gaps in our knowledge of the H2 biogeochemical cycle that must be resolved to quantify the impact of higher H2 usage.
Wenjie Wang, Bin Yuan, Hang Su, Yafang Cheng, Jipeng Qi, Sihang Wang, Wei Song, Xinming Wang, Chaoyang Xue, Chaoqun Ma, Fengxia Bao, Hongli Wang, Shengrong Lou, and Min Shao
Atmos. Chem. Phys., 24, 4017–4027, https://doi.org/10.5194/acp-24-4017-2024, https://doi.org/10.5194/acp-24-4017-2024, 2024
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This study investigates the important role of unmeasured volatile organic compounds (VOCs) in ozone formation. Based on results in a megacity of China, we show that unmeasured VOCs can contribute significantly to ozone fomation and also influence the determination of ozone control strategy. Our results show that these unmeasured VOCs are mainly from human sources.
Romain Salignat, Matti Rissanen, Siddharth Iyer, Jean-Luc Baray, Pierre Tulet, Jean-Marc Metzger, Jérôme Brioude, Karine Sellegri, and Clémence Rose
Atmos. Chem. Phys., 24, 3785–3812, https://doi.org/10.5194/acp-24-3785-2024, https://doi.org/10.5194/acp-24-3785-2024, 2024
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Using mass spectrometry data collected at the Maïdo Observatory (2160 m a.s.l., Réunion), we provide the first detailed analysis of molecular cluster chemical composition specifically in the marine free troposphere. The abundance of the identified species is related both to in situ meteorological parameters and air mass history, which also provide insight into their origin. Our work makes an important contribution to documenting the chemistry and physics of the marine free troposphere.
Xiaoyi Zhang, Wanyun Xu, Weili Lin, Gen Zhang, Jinjian Geng, Li Zhou, Huarong Zhao, Sanxue Ren, Guangsheng Zhou, Jianmin Chen, and Xiaobin Xu
EGUsphere, https://doi.org/10.5194/egusphere-2024-643, https://doi.org/10.5194/egusphere-2024-643, 2024
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Ozone (O3) deposition is a key process removing surface O3, affecting air quality, ecosystem and climate change. This study conducted an O3 deposition measurement over wheat canopy using a newly relaxed eddy accumulation flux system. Large variabilities of O3 deposition were detected mainly determined by crop growth and modulated by various environmental factors. More O3 deposition observations over different surfaces are needed for exploring deposition mechanism, model optimization.
Delaney B. Kilgour, Gordon A. Novak, Megan S. Claflin, Brian M. Lerner, and Timothy H. Bertram
Atmos. Chem. Phys., 24, 3729–3742, https://doi.org/10.5194/acp-24-3729-2024, https://doi.org/10.5194/acp-24-3729-2024, 2024
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Laboratory experiments with seawater mimics suggest ozone deposition to the surface ocean can be a source of reactive carbon to the marine atmosphere. We conduct both field and laboratory measurements to assess abiotic VOC composition and yields from ozonolysis of real surface seawater. We show that C5–C11 aldehydes contribute to the observed VOC emission flux. We estimate that VOCs generated by the ozonolysis of surface seawater are competitive with biological VOC production and emission.
Xiangdong Zheng, Wen Yang, Yuting Sun, Chunmei Geng, Yingying Liu, and Xiaobin Xu
Atmos. Chem. Phys., 24, 3759–3768, https://doi.org/10.5194/acp-24-3759-2024, https://doi.org/10.5194/acp-24-3759-2024, 2024
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Chen et al. (2022) attributed the nocturnal ozone enhancement (NOE) during the night of 31 July 2021 in the North China Plain (NCP) to "the direct stratospheric intrusion to reach the surface". We analyzed in situ data from the NCP. Our results do not suggest that there was a significant impact from the stratosphere on surface ozone during the NOE. We argue that the NOE was not caused by stratospheric intrusion but originated from fresh photochemical production in the lower troposphere.
James M. Roberts, Siyuan Wang, Patrick R. Veres, J. Andrew Neuman, Michael A. Robinson, Ilann Bourgeois, Jeff Peischl, Thomas B. Ryerson, Chelsea R. Thompson, Hannah M. Allen, John D. Crounse, Paul O. Wennberg, Samuel R. Hall, Kirk Ullmann, Simone Meinardi, Isobel J. Simpson, and Donald Blake
Atmos. Chem. Phys., 24, 3421–3443, https://doi.org/10.5194/acp-24-3421-2024, https://doi.org/10.5194/acp-24-3421-2024, 2024
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We measured cyanogen bromide (BrCN) in the troposphere for the first time. BrCN is a product of the same active bromine chemistry that destroys ozone and removes mercury in polar surface environments and is a previously unrecognized sink for active Br compounds. BrCN has an apparent lifetime against heterogeneous loss in the range 1–10 d, so it serves as a cumulative marker of Br-radical chemistry. Accounting for BrCN chemistry is an important part of understanding polar Br cycling.
Kai Qin, Wei Hu, Qin He, Fan Lu, and Jason Blake Cohen
Atmos. Chem. Phys., 24, 3009–3028, https://doi.org/10.5194/acp-24-3009-2024, https://doi.org/10.5194/acp-24-3009-2024, 2024
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We compute CH4 emissions and uncertainty on a mine-by-mine basis, including underground, overground, and abandoned mines. Mine-by-mine gas and flux data and 30 min observations from a flux tower located next to a mine shaft are integrated. The observed variability and bias correction are propagated over the emissions dataset, demonstrating that daily observations may not cover the range of variability. Comparisons show both an emissions magnitude and spatial mismatch with current inventories.
Bowen Zhang, Dong Zhang, Zhe Dong, Xinshuai Song, Ruiqin Zhang, and Xiao Li
EGUsphere, https://doi.org/10.5194/egusphere-2024-575, https://doi.org/10.5194/egusphere-2024-575, 2024
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Continuous online VOCs monitoring was carried out at an urban site in a traffic-hub city for two months during the Omicron-infected stage. The characteristics and variations of VOCs in different periods were studied, and their impact on the formation of SOA were evaluated. The work in this manuscript evaluated the influence of the policy variation on VOCs pollution, which will provide some basis for VOCs pollution research and control of pollution sources.
Sachin Mishra, Vinayak Sinha, Haseeb Hakkim, Arpit Awasthi, Sachin D. Ghude, Vijay Kumar Soni, Narendra Nigam, Baerbel Sinha, and Madhavan N. Rajeevan
EGUsphere, https://doi.org/10.5194/egusphere-2024-500, https://doi.org/10.5194/egusphere-2024-500, 2024
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We quantified 111 gases using extended volatility mass spectrometry to understand how changes in seasonality and emissions lead from clean air in monsoon to extremely polluted air in the post-monsoon season in Delhi. Averaged total mass concentrations (260 µgm-3) were >4 times in polluted periods, driven by biomass burning emissions and reduced atmospheric ventilation. Reactive gaseous nitrogen, chlorine and sulphur compounds hitherto un-reported from such a polluted environment were discovered.
Yao Yan Huang and D. James Donaldson
Atmos. Chem. Phys., 24, 2387–2398, https://doi.org/10.5194/acp-24-2387-2024, https://doi.org/10.5194/acp-24-2387-2024, 2024
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Ground-level ozone interacts at the lake–land boundary; this is important to our understanding and modelling of atmospheric chemistry and air pollution in the lower atmosphere. We show that a steep ozone gradient occurs year-round moving inland up to 1 km from the lake and that this gradient is influenced by seasonal factors on the local land environment, where more rural areas are more greatly affected seasonally.
Katrin Müller, Jordis S. Tradowsky, Peter von der Gathen, Christoph Ritter, Sharon Patris, Justus Notholt, and Markus Rex
Atmos. Chem. Phys., 24, 2169–2193, https://doi.org/10.5194/acp-24-2169-2024, https://doi.org/10.5194/acp-24-2169-2024, 2024
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The Palau Atmospheric Observatory is introduced as an ideal site to detect changes in atmospheric composition and dynamics above the remote tropical western Pacific. We focus on the ozone sounding program from 2016–2021, including El Niño 2016. The year-round high convective activity is reflected in dominant low tropospheric ozone and high relative humidity. Their seasonal distributions are unique compared to other tropical sites and are modulated by the Intertropical Convergence Zone.
Ziyan Guo, Keding Lu, Pengxiang Qiu, Mingyi Xu, and Zhaobing Guo
Atmos. Chem. Phys., 24, 2195–2205, https://doi.org/10.5194/acp-24-2195-2024, https://doi.org/10.5194/acp-24-2195-2024, 2024
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The formation of secondary sulfate needs to be further explored. In this work, we simultaneously measured sulfur and oxygen isotopic compositions to gain an increased understanding of specific sulfate formation processes. The results indicated that secondary sulfate was mainly ascribed to SO2 homogeneous oxidation by OH radicals and heterogeneous oxidation by H2O2 and Fe3+ / O2. This study is favourable for deeply investigating the sulfur cycle in the atmosphere.
Imran A. Girach, Narendra Ojha, Prabha R. Nair, Kandula V. Subrahmanyam, Neelakantan Koushik, Mohammed M. Nazeer, Nadimpally Kiran Kumar, Surendran Nair Suresh Babu, Jos Lelieveld, and Andrea Pozzer
Atmos. Chem. Phys., 24, 1979–1995, https://doi.org/10.5194/acp-24-1979-2024, https://doi.org/10.5194/acp-24-1979-2024, 2024
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We investigate surface ozone variability in East Antarctica based on measurements and EMAC global model simulations during austral summer. Nearly half of the surface ozone is found to be of stratospheric origin. The east coast of Antarctica acts as a stronger sink of ozone than surrounding regions. Photochemical loss of ozone is counterbalanced by downward transport of ozone. The study highlights the intertwined role of chemistry and dynamics in governing ozone variations over East Antarctica.
Ying Zhang, Duzitian Li, Xu-Cheng He, Wei Nie, Chenjuan Deng, Runlong Cai, Yuliang Liu, Yishuo Guo, Chong Liu, Yiran Li, Liangduo Chen, Yuanyuan Li, Chenjie Hua, Tingyu Liu, Zongcheng Wang, Jiali Xie, Lei Wang, Tuukka Petäjä, Federico Bianchi, Ximeng Qi, Xuguang Chi, Pauli Paasonen, Yongchun Liu, Chao Yan, Jingkun Jiang, Aijun Ding, and Markku Kulmala
Atmos. Chem. Phys., 24, 1873–1893, https://doi.org/10.5194/acp-24-1873-2024, https://doi.org/10.5194/acp-24-1873-2024, 2024
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This study conducts a long-term observation of gaseous iodine oxoacids in two Chinese megacities, revealing their ubiquitous presence with peak concentrations (up to 0.1 pptv) in summer. Our analysis suggests a mix of terrestrial and marine sources for iodine. Additionally, iodic acid is identified as a notable contributor to sub-3 nm particle growth and particle survival probability.
Guoxian Zhang, Renzhi Hu, Pinhua Xie, Changjin Hu, Xiaoyan Liu, Liujun Zhong, Haotian Cai, Bo Zhu, Shiyong Xia, Xiaofeng Huang, Xin Li, and Wenqing Liu
Atmos. Chem. Phys., 24, 1825–1839, https://doi.org/10.5194/acp-24-1825-2024, https://doi.org/10.5194/acp-24-1825-2024, 2024
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Comprehensive observation of HOx radicals was conducted at a coastal site in the Pearl River Delta. Radical chemistry was influenced by different air masses in a time-dependent way. Land mass promotes a more active photochemical process, with daily averages of 7.1 × 106 and 5.2 × 108 cm−3 for OH and HO2 respectively. The rapid oxidation process was accompanied by a higher diurnal HONO concentration, which influences the ozone-sensitive system and eventually magnifies the background ozone.
Sarah Albertin, Joël Savarino, Slimane Bekki, Albane Barbero, Roberto Grilli, Quentin Fournier, Irène Ventrillard, Nicolas Caillon, and Kathy Law
Atmos. Chem. Phys., 24, 1361–1388, https://doi.org/10.5194/acp-24-1361-2024, https://doi.org/10.5194/acp-24-1361-2024, 2024
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This study reports the first simultaneous records of oxygen (Δ17O) and nitrogen (δ15N) isotopes in nitrogen dioxide (NO2) and nitrate (NO3−). These data are combined with atmospheric observations to explore sub-daily N reactive chemistry and quantify N fractionation effects in an Alpine winter city. The results highlight the necessity of using Δ17O and δ15N in both NO2 and NO3− to avoid biased estimations of NOx sources and fates from NO3− isotopic records in urban winter environments.
Cited articles
Ambrose, D. and Tsonopoulos, C.: Vapor-liquid critical properties of elements and compounds. 2. Normal-alkanes, J. Chem. Eng. Data, 40, 531–546, https://doi.org/10.1021/je00019a001, 1995.
Andreae, M. O. and Merlet, P.: Emission of trace gases and aerosols from biomass burning, Global Biogeochem. Cy., 15, 955–966, 2001.
Atkinson, R.: Kinetics of the gas-phase reactions of OH radicals with alkanes and cycloalkanes, Atmos. Chem. Phys., 3, 2233–2307, https://doi.org/10.5194/acp-3-2233-2003, 2003.
Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F., Hynes, R. G., Jenkin, M. E., Rossi, M. J., and Troe, J.: Evaluated kinetic and photochemical data for atmospheric chemistry: Volume I – gas phase reactions of Ox, HOx, NOx and SOx species, Atmos. Chem. Phys., 4, 1461-1738, https://doi.org/10.5194/acp-4-1461-2004, 2004.
Aydin, M., Williams, M. B., and Saltzman, E. S.: Feasibility of reconstructing paleoatmospheric records of selected alkanes, methyl halides, and sulfur gases from Greenland ice cores, J. Geophys. Res.-Atmos., 112, D07312, https://doi.org/10.1029/2006jd008027, 2007.
Aydin, M., Verhulst, K. R., Saltzman, E. S., Battle, M. O., Montzka, S. A., Blake, D. R., Tang, Q., and Prather, M. J.: Recent decreases in fossil-fuel emissions of ethane and methane derived from firn air, Nature, 476, 198–201, https://doi.org/10.1038/nature10352, 2011.
Baker, A. K., Slemr, F., and Brenninkmeijer, C. A. M.: Analysis of non-methane hydrocarbons in air samples collected aboard the CARIBIC passenger aircraft, Atmos. Meas. Tech., 3, 311–321, https://doi.org/10.5194/amt-3-311-2010, 2010.
Battle, M., Bender, M., Sowers, T., Tans, P. P., Butler, J. H., Elkins, J. W., Ellis, J. T., Conway, T., Zhang, N., Lang, P., and Clarke, A. D.: Atmospheric gas concentrations over the past century measured in air from firn at the South Pole, Nature, 383, 231–235, https://doi.org/10.1038/383231a0, 1996.
Broadgate, W. J., Liss, P. S., and Penkett, S. A.: Seasonal emissions of isoprene and other reactive hydrocarbon gases from the ocean, Geophys. Res. Lett., 24, 2675–2678, https://doi.org/10.1029/97gl02736, 1997.
Buizert, C., Martinerie, P., Petrenko, V. V., Severinghaus, J. P., Trudinger, C. M., Witrant, E., Rosen, J. L., Orsi, A. J., Rubino, M., Etheridge, D. M., Steele, L. P., Hogan, C., Laube, J. C., Sturges, W. T., Levchenko, V. A., Smith, A. M., Levin, I., Conway, T. J., Dlugokencky, E. J., Lang, P. M., Kawamura, K., Jenk, T. M., White, J. W. C., Sowers, T., Schwander, J., and Blunier, T.: Gas transport in firn: multiple-tracer characterisation and model intercomparison for NEEM, Northern Greenland, Atmos. Chem. Phys., 12, 4259–4277, https://doi.org/10.5194/acp-12-4259-2012, 2012.
Carpenter, L. J., Monks, P. S., Bandy, B. J., Penkett, S. A., Galbally, I. E., and Meyer, C. P.: A study of peroxy radicals and ozone photochemistry at coastal sites in the northern and southern hemispheres, J. Geophys. Res.-Atmos., 102, 25417–25427, https://doi.org/10.1029/97jd02242, 1997.
Chen, N. H. and Othmer, D. F.: New generalized equation for gas diffusion coefficient, J. Chem. Eng. Data, 7, 37–41, 1962.
Daubert, T. E.: Vapor-liquid critical properties of elements and compounds. 5. Branched alkanes and cycloalkanes, J. Chem. Eng. Data, 41, 365–372, https://doi.org/10.1021/je9501548, 1996.
Eckhardt, S., Stohl, A., Beirle, S., Spichtinger, N., James, P., Forster, C., Junker, C., Wagner, T., Platt, U., and Jennings, S. G.: The North Atlantic Oscillation controls air pollution transport to the Arctic, Atmos. Chem. Phys., 3, 1769–1778, https://doi.org/10.5194/acp-3-1769-2003, 2003.
Ehhalt, D. H., Rudolph, J., Meixner, F., and Schmidt, U.: Measurements of selected C2-C5 hydrocarbons in the background troposphere – vertical and latitudinal variations, J. Atmos. Chem., 3, 29–52, https://doi.org/10.1007/bf00049367, 1985.
Etiope, G. and Ciccioli, P.: Earth's Degassing: A Missing Ethane and Propane Source, Science, 323, 478–478, https://doi.org/10.1126/science.1165904, 2009.
Gautrois, M., Brauers, T., Koppmann, R., Rohrer, F., Stein, O., and Rudolph, J.: Seasonal variability and trends of volatile organic compounds in the lower polar troposphere, J. Geophys. Res.-Atmos., 108, 4393, https://doi.org/10.1029/2002jd002765, 2003.
Gilman, J. B., Burkhart, J. F., Lerner, B. M., Williams, E. J., Kuster, W. C., Goldan, P. D., Murphy, P. C., Warneke, C., Fowler, C., Montzka, S. A., Miller, B. R., Miller, L., Oltmans, S. J., Ryerson, T. B., Cooper, O. R., Stohl, A., and de Gouw, J. A.: Ozone variability and halogen oxidation within the Arctic and sub-Arctic springtime boundary layer, Atmos. Chem. Phys., 10, 10223–10236, https://doi.org/10.5194/acp-10-10223-2010, 2010.
Gilman, J. B., Lerner, B. M., Kuster, W. C., and de Gouw, J. A.: Source Signature of Volatile Organic Compounds from Oil and Natural Gas Operations in Northeastern Colorado, Environ. Sci. Technol., 47, 1297–1305, https://doi.org/10.1021/es304119a, 2013.
Graedel, T. E. and Keene, W. C.: Tropospheric budget of reactive chlorine, Global Biogeochem. Cy., 9, 47–77, https://doi.org/10.1029/94gb03103, 1995.
Helmig, D., Oltmans, S. J., Morse, T. O., and Dibb, J. E.: What is causing high ozone at Summit, Greenland?, Atmos. Environ., 41, 5031–5043, https://doi.org/10.1016/j.atmosenv.2006.05.084, 2007.
Helmig, D., Tanner, D. M., Honrath, R. E., Owen, R. C., and Parrish, D. D.: Nonmethane hydrocarbons at Pico Mountain, Azores: 1. Oxidation chemistry in the North Atlantic region, J. Geophys. Res.-Atmos., 113, D20S91, https://doi.org/10.1029/2007jd008930, 2008.
Helmig, D., Bottenheim, J., Galbally, I. E., Lewis, A., Milton, M. J. T., Penkett, S., Plass-Duelmer, C., Reimann , S., Tans, P., and Theil, S.: Volatile Organic Compounds in the Global Atmosphere, Eos Trans. AGU, 90, 2009.
Helmig, D., Stephens, C., Carmore, J., and Hueber, J.: Seasonal cycle of non-methane hydrocarbons in the atmosphere and firn air at Summit, Greenland, Atmos. Environ., 85, 234–246, 2014.
Jobson, B. T., Niki, H., Yokouchi, Y., Bottenheim, J., Hopper, F., and Leaitch, R.: Measurements of C2–C6 hydrocarbons during the polar sunrise 1992 experiment – evidence of Cl atom and Br atom chemistry, J. Geophys. Res.-Atmos., 99, 25355–25368, 1994.
Kahl, J. D. W., Martinez, D. A., Kuhns, H., Davidson, C. I., Jaffrezo, J. L., and Harris, J. M.: Air mass trajectories to Summit, Greenland: A 44-year climatology and some episodic events, J. Geophys. Res.-Oceans, 102, 26861–26875, https://doi.org/10.1029/97jc00296, 1997.
Kleinman, L., Lee, Y. N., Springston, S. R., Lee, J. H., Nunnermacker, L., Weinsteinlloyd, J., Zhou, X. L., and Newman, L.: Peroxy radical concentration and ozone formation rate at a rural site in the southeastern united-states, J. Geophys. Res.-Atmos., 100, 7263–7273, https://doi.org/10.1029/95jd00215, 1995.
Klonecki, A., Hess, P., Emmons, L., Smith, L., Orlando, J., and Blake, D.: Seasonal changes in the transport of pollutants into the Arctic troposphere-model study, J. Geophys. Res.-Atmos., 108, 8367, https://doi.org/10.1029/2002jd002199, 2003.
Lamarque, J. F., Hess, P., Emmons, L., Buja, L., Washington, W., and Granier, C.: Tropospheric ozone evolution between 1890 and 1990, J. Geophys. Res.-Atmos., 110, D08304, https://doi.org/10.1029/2004JD005537, 2005.
Lamarque, J.-F., Bond, T. C., Eyring, V., Granier, C., Heil, A., Klimont, Z., Lee, D., Liousse, C., Mieville, A., Owen, B., Schultz, M. G., Shindell, D., Smith, S. J., Stehfest, E., Van Aardenne, J., Cooper, O. R., Kainuma, M., Mahowald, N., McConnell, J. R., Naik, V., Riahi, K., and van Vuuren, D. P.: Historical (1850–2000) gridded anthropogenic and biomass burning emissions of reactive gases and aerosols: methodology and application, Atmos. Chem. Phys., 10, 7017–7039, https://doi.org/10.5194/acp-10-7017-2010, 2010.
Lewis, A. C., Carpenter, L. J., and Pilling, M. J.: Nonmethane hydrocarbons in Southern Ocean boundary layer air, J. Geophys. Res.-Atmos., 106, 4987–4994, https://doi.org/10.1029/2000jd900634, 2001.
Lukas, M. A.: Strong robust generalized cross-validation for choosing the regularization parameter, Inverse Probl., 24, 034006, https://doi.org/10.1088/0266-5611/24/3/034006, 2008.
Mahieu, E., Duchatelet, P., Zander, R., Demoulin, P., Servais, C., Rinsland, C. P., Chipperfield, M. P., and De Maziere, M.: The evolution of inorganic chlorine above the Jungfraujoch station: an update, Proceedings of the 20th Quadrennial Ozone Symposium, 2, 997–998, 2004.
Masarie, K. A. and Tans, P. P.: Extension and integration of atmospheric carbon dioxide data into a globally consistent measurement record, J. Geophys. Res. 100, 11593–11610, 1995.
Mielke, L. H., Furgeson, A., and Osthoff, H. D.: Observation of CINO2 in a Mid-Continental Urban Environment, Environ. Sci. Technol., 45, 8889–8896, https://doi.org/10.1021/es201955u, 2011.
Montzka, S. A., Spivakovsky, C. M., Butler, J. H., Elkins, J. W., Lock, L. T., and Mondeel, D. J.: New observational constraints for atmospheric hydroxyl on global and hemispheric scales, Science, 288, 500–503, https://doi.org/10.1126/science.288.5465.500, 2000.
Montzka, S. A., Krol, M., Dlugokencky, E., Hall, B., Jockel, P., and Lelieveld, J.: Small Interannual Variability of Global Atmospheric Hydroxyl, Science, 331, 67–69, https://doi.org/10.1126/science.1197640, 2011.
Ohara, T., Akimoto, H., Kurokawa, J., Horii, N., Yamaji, K., Yan, X., and Hayasaka, T.: An Asian emission inventory of anthropogenic emission sources for the period 1980–2020, Atmos. Chem. Phys., 7, 4419–4444, https://doi.org/10.5194/acp-7-4419-2007, 2007.
Parrish, D. D., Hahn, C. J., Williams, E. J., Norton, R. B., Fehsenfeld, F. C., Singh, H. B., Shetter, J. D., Gandrud, B. W., and Ridley, B. A.: Indications of photochemical histories of pacific air masses from measurements of atmospheric trace species at point arena, california, J. Geophys. Res.-Atmos., 97, 15883–15901, 1992.
Parrish, D. D., Trainer, M., Young, V., Goldan, P. D., Kuster, W. C., Jobson, B. T., Fehsenfeld, F. C., Lonneman, W. A., Zika, R. D., Farmer, C. T., Riemer, D. D., and Rodgers, M. O.: Internal consistency tests for evaluation of measurements of anthropogenic hydrocarbons in the troposphere, J. Geophys. Res.-Atmos., 103, 22339–22359, https://doi.org/10.1029/98jd01364, 1998.
Petrenko, V. V., Martinerie, P., Novelli, P., Etheridge, D. M., Levin, I., Wang, Z., Blunier, T., Chappellaz, J., Kaiser, J., Lang, P., Steele, L. P., Hammer, S., Mak, J., Langenfelds, R. L., Schwander, J., Severinghaus, J. P., Witrant, E., Petron, G., Battle, M. O., Forster, G., Sturges, W. T., Lamarque, J.-F., Steffen, K., and White, J. W. C.: A 60 yr record of atmospheric carbon monoxide reconstructed from Greenland firn air, Atmos. Chem. Phys., 13, 7567–7585, https://doi.org/10.5194/acp-13-7567-2013, 2013.
Pollmann, J., Helmig, D., Hueber, J., Plass-Dülmer, C., and Tans, P.: Sampling, storage, and analysis of C2–C7 non-methane hydrocarbons from the US National Oceanic and Atmospheric Administration Cooperative Air Sampling Network glass flasks, J. Chromatogr. A, 1188, 75–87, 2008.
Pozzer, A., Pollmann, J., Taraborrelli, D., Jöckel, P., Helmig, D., Tans, P., Hueber, J., and Lelieveld, J.: Observed and simulated global distribution and budget of atmospheric C2-C5 alkanes, Atmos. Chem. Phys., 10, 4403–4422, https://doi.org/10.5194/acp-10-4403-2010, 2010.
Prinn, R. G., Cunnold, D., Simmonds, P., Alyea, F., Boldi, R., Crawford, A., Fraser, P., Gutzler, D., Hartley D., Rosen, R., and Rasmussen, R.: Global average concentration and trend for hydroxyl radicals deduced from ALE/GAGE trichloroethane (methyl chloroform) data for 1978–1990, J. Geophys. Res., 97, 2445–2461, 1992.
Prinn, R. G., Huang, J., Weiss, R. F., Cunnold, D. M., Fraser, P. J., Simmonds, P. G., McCulloch, A., Harth, C., Reimann, S., Salameh, P., O'Doherty, S., Wang, R. H. J., Porter, L. W., Miller, B. R., and Krummel, P. B.: Evidence for variability of atmospheric hydroxyl radicals over the past quarter century, Geophys. Res. Lett., 32, L07809, https://doi.org/10.1029/2004gl022228, 2005.
Rasmussen, R. A. and Khalil, M. A. K.: Atmospheric trace gases – trends and distributions over the last decade, Science, 232, 1623–1624, https://doi.org/10.1126/science.232.4758.1623, 1986.
Rommelaere, V., Arnaud, L., and Barnola, J. M.: Reconstructing recent atmospheric trace gas concentrations from polar firn and bubbly ice data by inverse methods, J. Geophys. Res.-Atmos., 102, 30069–30083, https://doi.org/10.1029/97jd02653, 1997.
Ross, S. M.: Peirce's criterion for the elimination of suspect experimental data, J. Eng. Technol., 20, 38–41, 2003.
Sapart, C. J., Martinerie, P., Witrant, E., Chappellaz, J., van de Wal, R. S. W., Sperlich, P., van der Veen, C., Bernard, S., Sturges, W. T., Blunier, T., Schwander, J., Etheridge, D., and Röckmann, T.: Can the carbon isotopic composition of methane be reconstructed from multi-site firn air measurements?, Atmos. Chem. Phys., 13, 6993–7005, https://doi.org/10.5194/acp-13-6993-2013, 2013.
Schwander, J., Barnola, J. M., Andrie, C., Leuenberger, M., Ludin, A., Raynaud, D., and Stauffer, B.: The age of the air in the firn and the ice at summit, greenland, J. Geophys. Res.-Atmos., 98, 2831–2838, https://doi.org/10.1029/92jd02383, 1993.
Sillman, S., Logan, J. A., and Wofsy, S. C.: The sensitivity of ozone to nitrogen-oxides and hydrocarbons in regional ozone episodes, J. Geophys. Res.-Atmos., 95, 1837–1851, https://doi.org/10.1029/JD095iD02p01837, 1990.
Simpson, I. J., Andersen, M. P. S., Meinardi, S., Bruhweiler, L., Blake, N. J., Helmig, D., Rowland, F. S., and Blake, D. R.: Long-term decline of global atmospheric ethane concentrations and implications for methane, Nature, 488, 490–494, 2012.
Singh, H. B., Viezee, W., and Salas, L. J.: Measurements of selected C2-C5 hydrocarbons in the troposphere – latitudinal, vertical, and temporal variations, J. Geophys. Res.-Atmos., 93, 15861–15878, https://doi.org/10.1029/JD093iD12p15861, 1988.
Stohl, A.: Characteristics of atmospheric transport into the Arctic troposphere, J. Geophys. Res.-Atmos., 111, D11306, https://doi.org/10.1029/2005jd006888, 2006.
Tanaka, P. L., Oldfield, S., Neece, J. D., Mullins, C. B., and Allen, D. T.: Anthropogenic sources of chlorine and ozone formation in urban atmospheres, Environ. Sci. Technol., 34, 4470–4473, https://doi.org/10.1021/es991380v, 2000.
Tanaka, P. L., Riemer, D. D., Chang, S. H., Yarwood, G., McDonald-Buller, E. C., Apel, E. C., Orlando, J. J., Silva, P. J., Jimenez, J. L., Canagaratna, M. R., Neece, J. D., Mullins, C. B., and Allen, D. T.: Direct evidence for chlorine-enhanced urban ozone formation in Houston, Texas, Atmos. Environ., 37, 1393–1400, https://doi.org/10.1016/s1352-2310(02)01007-5, 2003.
Tanner, D., Helmig, D., Hueber, J., and Goldan, P.: Gas chromatography system for the automated, unattended, and cryogen-free monitoring of C2 to C6 non-methane hydrocarbons in the remote troposphere, J. Chromatogr. A, 1111, 76–88, 2006.
Thompson, C. R., Helmig, D., Park, J. H., and Hueber, J.: Evidence for radical oxidation of non-methane hydrocarbons within a continental seasonal snowpack, in preparation, 2014.
Thoning, K. W., Tans, P. P., and Komhyr, W. D.: Atmospheric carbon-dioxide at mauna loa observatory. 2. Analysis of the NOAA GMCC data, 1974–1985, J. Geophys. Res.-Atmos., 94, 8549–8565, https://doi.org/10.1029/JD094iD06p08549, 1989.
Thornton, J. A., Kercher, J. P., Riedel, T. P., Wagner, N. L., Cozic, J., Holloway, J. S., Dube, W. P., Wolfe, G. M., Quinn, P. K., Middlebrook, A. M., Alexander, B., and Brown, S. S.: A large atomic chlorine source inferred from mid-continental reactive nitrogen chemistry, Nature, 464, 271–274, https://doi.org/10.1038/nature08905, 2010.
von Schneidemesser, E., Monks, P. S., and Plass-Duelmer, C.: Global comparison of VOC and CO observations in urban areas, Atmos. Environ., 44, 5053–5064, https://doi.org/10.1016/j.atmosenv.2010.09.010, 2010.
Wang, Z., Chappellaz, J., Martinerie, P., Park, K., Petrenko, V., Witrant, E., Emmons, L. K., Blunier, T., Brenninkmeijer, C. A. M., and Mak, J. E.: The isotopic record of Northern Hemisphere atmospheric carbon monoxide since 1950: implications for the CO budget, Atmos. Chem. Phys., 12, 4365–4377, https://doi.org/10.5194/acp-12-4365-2012, 2012.
Warneke, C., de Gouw, J. A., Holloway, J. S., Peischl, J., Ryerson, T. B., Atlas, E., Blake, D., Trainer, M., and Parrish, D. D.: Multiyear trends in volatile organic compounds in Los Angeles, California: Five decades of decreasing emissions, J. Geophys. Res.-Atmos., 117, D00v17, https://doi.org/10.1029/2012jd017899, 2012.
Witrant, E. and Martinerie, P.: Input Estimation from Sparse Measurements in LPV Systems and Isotopic Ratios in Polar Firns, Proc. of the 5th IFAC Symposium on System Structure and Control, https://doi.org/10.3182/20130204-3-FR-2033.00201, 659–664, 2013.
Witrant, E., Martinerie, P., Hogan, C., Laube, J. C., Kawamura, K., Capron, E., Montzka, S. A., Dlugokencky, E. J., Etheridge, D., Blunier, T., and Sturges, W. T.: A new multi-gas constrained model of trace gas non-homogeneous transport in firn: evaluation and behaviour at eleven polar sites, Atmos. Chem. Phys., 12, 11465–11483, https://doi.org/10.5194/acp-12-11465-2012, 2012.
Worton, D. R., Sturges, W. T., Reeves, C. E., Newland, M. J., Penkett, S. A., Atlas, E., Stroud, V., Johnson, K., Schmidbauer, N., Solberg, S., Schwander, J., and Barnola, J.-M.: Evidence from firn air for recent decreases in non-methane hydrocarbons and a 20th century increase in nitrogen oxides in the northern hemisphere, Atmos. Environ., 54, 592–602, 2012.
Zuiderweg, A., Holzinger, R., and Röckmann, T.: Analytical system for stable carbon isotope measurements of low molecular weight (C2-C6) hydrocarbons, Atmos. Meas. Tech., 4, 1161–1175, https://doi.org/10.5194/amt-4-1161-2011, 2011.
Zuiderweg, A., Holzinger, R., Martinerie, P., Schneider, R., Kaiser, J., Witrant, E., Etheridge, D., Petrenko, V., Blunier, T., and Röckmann, T.: Extreme 13C depletion of CCl2F2 in firn air samples from NEEM, Greenland, Atmos. Chem. Phys., 13, 599–609, https://doi.org/10.5194/acp-13-599-2013, 2013.
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