Articles | Volume 15, issue 12
23 Jun 2015
Research article | 23 Jun 2015
Chlorine isotope composition in chlorofluorocarbons CFC-11, CFC-12 and CFC-113 in firn, stratospheric and tropospheric air
S. J. Allin et al.
No articles found.
Liubov Poshyvailo-Strube, Rolf Müller, Stephan Fueglistaler, Michaela I. Hegglin, Johannes C. Laube, C. Michael Volk, and Felix Ploeger
Atmos. Chem. Phys., 22, 9895–9914,Short summary
Brewer–Dobson circulation (BDC) controls the composition of the stratosphere, which in turn affects radiation and climate. As the BDC cannot be measured directly, it is necessary to infer its strength and trends indirectly. In this study, we test in the
model worlddifferent methods for estimating the mean age of air trends based on a combination of stratospheric water vapour and methane data. We also provide simple practical advice of a more reliable estimation of the mean age of air trends.
Josué Bock, Jan Kaiser, Max Thomas, Andreas Bott, and Roland von Glasow
Geosci. Model Dev., 15, 5807–5828,Short summary
MISTRA-v9.0 is an atmospheric boundary layer chemistry model. The model includes a detailed particle description with regards to the microphysics, gas–particle interactions, and liquid phase chemistry within particles. Version 9.0 is the first release of MISTRA as an open-source community model. This paper presents a thorough description of the model characteristics and components. We show some examples of simulations reproducing previous studies with MISTRA with good consistency.
Hossein Maazallahi, Antonio Delre, Charlotte Scheutz, Anders M. Fredenslund, Stefan Schwietzke, Hugo Denier van der Gon, and Thomas Röckmann
Atmos. Meas. Tech. Discuss.,
Preprint under review for AMTShort summary
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.
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,Short summary
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,Short summary
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,Short summary
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.
Michael P. Hemming, Jan Kaiser, Jacqueline Boutin, Liliane Merlivat, Karen J. Heywood, Dorothee C. E. Bakker, Gareth A. Lee, Marcos Cobas García, David Antoine, and Kiminori Shitashima
Ocean Sci. Discuss.,
Revised manuscript accepted for OSShort summary
An underwater glider mission was carried out in spring 2016 near a mooring in the northwestern Mediterranean Sea. The glider deployment served as a test of a prototype ion-sensitive field-effect transistor pH sensor. Mean net community production rates were estimated from glider and buoy measurements of dissolved oxygen and inorganic carbon concentrations before and during the spring bloom. Incorporating advection is important for accurate mass budgets. Unexpected metabolic quotients were found.
Juhi Nagori, Narcisa Nechita-Bândă, Sebastian Oscar Danielache, Masumi Shinkai, Thomas Röckmann, and Maarten Krol
Atmos. Chem. Phys. Discuss.,
Revised manuscript has not been submittedShort summary
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.
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 Discuss.,
Revised manuscript accepted for ESSDShort summary
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.
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys. Discuss.,
Revised manuscript under review for ACPShort summary
We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). The modelling study showed that this newly tested photochemistry produces more H2 over densely forested areas were is also removed more strongly compared to the rest of the world. The results highlight that other processes, like emissions or sinks, that contribute to atmospheric H2 levels should be studied further.
Truls Andersen, Marcel de Vries, Jaroslaw Necki, Justyna Swolkien, Malika Menoud, Thomas Röckmann, Anke Roiger, Andreas Fix, Wouter Peters, and Huilin Chen
Atmos. Chem. Phys. Discuss.,
Preprint under review for ACPShort summary
The Upper Silesian Coal Basin, Poland is one of the hot spots of methane emissions in Europe. Using an unmanned 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.
Merve Polat, Jesper Baldtzer Liisberg, Morten Krogsbøll, Thomas Blunier, and Matthew S. Johnson
Atmos. Meas. Tech., 14, 8041–8067,Short summary
We have designed a process for removing methane from a gas stream so that nitrous oxide can be measured without interference. These are both key long-lived greenhouse gases frequently studied in relation to ice cores, plants, water treatment and so on. However, many researchers are not aware of the problem of methane interference, and in addition there have not been good methods available for solving the problem. Here we present and evaluate such a method.
Tom Hull, Naomi Greenwood, Antony Birchill, Alexander Beaton, Matthew Palmer, and Jan Kaiser
Biogeosciences, 18, 6167–6180,Short summary
The shallow shelf seas play a large role in the global cycling of CO2 and also support large fisheries. We use an autonomous underwater vehicle in the central North Sea to measure the rates of change in oxygen and nutrients. Using these data we determine the amount of carbon dioxide taken out of the atmosphere by the sea and measure how productive the region is. These observations will be useful for improving our predictive models and help us predict and adapt to a changing ocean.
Benjamin Loveday, Timothy Smyth, Anıl Akpinar, Tom Hull, Mark Inall, Jan Kaiser, Bastien Queste, Matt Tobermann, Charlotte Williams, and Matthew Palmer
Earth Syst. Sci. Data Discuss.,
Revised manuscript accepted for ESSDShort summary
Using a new approach to combine autonomous underwater glider data and satellite Earth observations, we have generated a 19-month time-series of North Sea net primary productivity – the rate at which phytoplankton absorbs carbon dioxide, minus that lost through respiration. This time-series, which spans 13 gliders, allows for new investigations into small-scale, high-frequency variability in the biogeochemical processes that underpin the carbon cycle and coastal marine ecosystems in shelf seas.
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,Short summary
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,Short summary
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.
Felix Ploeger, Mohamadou Diallo, Edward Charlesworth, Paul Konopka, Bernard Legras, Johannes C. Laube, Jens-Uwe Grooß, Gebhard Günther, Andreas Engel, and Martin Riese
Atmos. Chem. Phys., 21, 8393–8412,Short summary
We investigate the global stratospheric circulation (Brewer–Dobson circulation) in the new ECMWF ERA5 reanalysis based on age of air simulations, and we compare it to results from the preceding ERA-Interim reanalysis. Our results show a slower stratospheric circulation and higher age for ERA5. The age of air trend in ERA5 over the 1989–2018 period is negative throughout the stratosphere, related to multi-annual variability and a potential contribution from changes in the reanalysis system.
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,Short summary
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.
Luca Possenti, Ingunn Skjelvan, Dariia Atamanchuk, Anders Tengberg, Matthew P. Humphreys, Socratis Loucaides, Liam Fernand, and Jan Kaiser
Ocean Sci., 17, 593–614,Short summary
A Seaglider was deployed for 8 months in the Norwegian Sea mounting an oxygen and, for the first time, a CO2 optode and a chlorophyll fluorescence sensor. The oxygen and CO2 data were used to assess the spatial and temporal variability and calculate the net community production, N(O2) and N(CT). The dataset was used to calculate net community production from inventory changes, air–sea flux, diapycnal mixing and entrainment.
Max Thomas, James France, Odile Crabeck, Benjamin Hall, Verena Hof, Dirk Notz, Tokoloho Rampai, Leif Riemenschneider, Oliver John Tooth, Mathilde Tranter, and Jan Kaiser
Atmos. Meas. Tech., 14, 1833–1849,Short summary
We describe the Roland von Glasow Air-Sea-Ice Chamber, a laboratory facility for studying ocean–sea-ice–atmosphere interactions. We characterise the technical capabilities of our facility to help future users plan and perform experiments. We also characterise the sea ice grown in the facility, showing that the extinction of photosynthetically active radiation, the bulk salinity, and the growth rate of our artificial sea ice are within the range of natural values.
Shamil Maksyutov, Tomohiro Oda, Makoto Saito, Rajesh Janardanan, Dmitry Belikov, Johannes W. Kaiser, Ruslan Zhuravlev, Alexander Ganshin, Vinu K. Valsala, Arlyn Andrews, Lukasz Chmura, Edward Dlugokencky, László Haszpra, Ray L. Langenfelds, Toshinobu Machida, Takakiyo Nakazawa, Michel Ramonet, Colm Sweeney, and Douglas Worthy
Atmos. Chem. Phys., 21, 1245–1266,Short summary
In order to improve the top-down estimation of the anthropogenic greenhouse gas emissions, a high-resolution inverse modelling technique was developed for applications to global transport modelling of carbon dioxide and other greenhouse gases. A coupled Eulerian–Lagrangian transport model and its adjoint are combined with surface fluxes at 0.1° resolution to provide high-resolution forward simulation and inverse modelling of surface fluxes accounting for signals from emission hot spots.
Andreas Plach, Bo M. Vinther, Kerim H. Nisancioglu, Sindhu Vudayagiri, and Thomas Blunier
Clim. Past, 17, 317–330,Short summary
In light of recent large-scale melting of the Greenland ice sheet (GrIS), e.g., in the summer of 2012 several days with surface melt on the entire ice sheet (including elevations above 3000 m), we use computer simulations to estimate the amount of melt during a warmer-than-present period of the past. Our simulations show more extensive melt than today. This is important for the interpretation of ice cores which are used to reconstruct the evolution of the ice sheet and the climate.
Bette L. Otto-Bliesner, Esther C. Brady, Anni Zhao, Chris M. Brierley, Yarrow Axford, Emilie Capron, Aline Govin, Jeremy S. Hoffman, Elizabeth Isaacs, Masa Kageyama, Paolo Scussolini, Polychronis C. Tzedakis, Charles J. R. Williams, Eric Wolff, Ayako Abe-Ouchi, Pascale Braconnot, Silvana Ramos Buarque, Jian Cao, Anne de Vernal, Maria Vittoria Guarino, Chuncheng Guo, Allegra N. LeGrande, Gerrit Lohmann, Katrin J. Meissner, Laurie Menviel, Polina A. Morozova, Kerim H. Nisancioglu, Ryouta O'ishi, David Salas y Mélia, Xiaoxu Shi, Marie Sicard, Louise Sime, Christian Stepanek, Robert Tomas, Evgeny Volodin, Nicholas K. H. Yeung, Qiong Zhang, Zhongshi Zhang, and Weipeng Zheng
Clim. Past, 17, 63–94,Short summary
The CMIP6–PMIP4 Tier 1 lig127k experiment was designed to address the climate responses to strong orbital forcing. We present a multi-model ensemble of 17 climate models, most of which have also completed the CMIP6 DECK experiments and are thus important for assessing future projections. The lig127ksimulations show strong summer warming over the NH continents. More than half of the models simulate a retreat of the Arctic minimum summer ice edge similar to the average for 2000–2018.
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,Short summary
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,Short summary
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,Short summary
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.
James E. Lee, Edward J. Brook, Nancy A. N. Bertler, Christo Buizert, Troy Baisden, Thomas Blunier, V. Gabriela Ciobanu, Howard Conway, Dorthe Dahl-Jensen, Tyler J. Fudge, Richard Hindmarsh, Elizabeth D. Keller, Frédéric Parrenin, Jeffrey P. Severinghaus, Paul Vallelonga, Edwin D. Waddington, and Mai Winstrup
Clim. Past, 16, 1691–1713,Short summary
The Roosevelt Island ice core was drilled to investigate climate from the eastern Ross Sea, West Antarctica. We describe the ice age-scale and gas age-scale of the ice core for 0–763 m (83 000 years BP). Old ice near the bottom of the core implies the ice dome existed throughout the last glacial period and that ice streaming was active in the region. Variations in methane, similar to those used as evidence of early human influence on climate, were observed prior to significant human populations.
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,Short summary
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,Short summary
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.
Anders Svensson, Dorthe Dahl-Jensen, Jørgen Peder Steffensen, Thomas Blunier, Sune O. Rasmussen, Bo M. Vinther, Paul Vallelonga, Emilie Capron, Vasileios Gkinis, Eliza Cook, Helle Astrid Kjær, Raimund Muscheler, Sepp Kipfstuhl, Frank Wilhelms, Thomas F. Stocker, Hubertus Fischer, Florian Adolphi, Tobias Erhardt, Michael Sigl, Amaelle Landais, Frédéric Parrenin, Christo Buizert, Joseph R. McConnell, Mirko Severi, Robert Mulvaney, and Matthias Bigler
Clim. Past, 16, 1565–1580,Short summary
We identify signatures of large bipolar volcanic eruptions in Greenland and Antarctic ice cores during the last glacial period, which allows for a precise temporal alignment of the ice cores. Thereby the exact timing of unexplained, abrupt climatic changes occurring during the last glacial period can be determined in a global context. The study thus provides a step towards a full understanding of elements of the climate system that may also play an important role in the future.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Edward J. Dlugokencky, Ray L. Langenfelds, Michel Ramonet, Doug Worthy, and Bo Zheng
Atmos. Chem. Phys., 20, 9525–9546,Short summary
The hydroxyl radical (OH), which is the dominant sink of methane (CH4), plays a key role in closing the global methane budget. This study quantifies how uncertainties in the hydroxyl radical can influence top-down estimates of CH4 emissions based on 4D Bayesian inversions with different OH fields and the same surface observations. We show that uncertainties in CH4 emissions driven by different OH fields are comparable to the uncertainties given by current bottom-up and top-down estimations.
Charles J. R. Williams, Maria-Vittoria Guarino, Emilie Capron, Irene Malmierca-Vallet, Joy S. Singarayer, Louise C. Sime, Daniel J. Lunt, and Paul J. Valdes
Clim. Past, 16, 1429–1450,Short summary
Computer simulations of the geological past are an important tool to improve our understanding of climate change. We present results from two simulations using the latest version of the UK's climate model, the mid-Holocene (6000 years ago) and Last Interglacial (127 000 years ago). The simulations reproduce temperatures consistent with the pattern of incoming radiation. Model–data comparisons indicate that some regions (and some seasons) produce better matches to the data than others.
Getachew Agmuas Adnew, Thijs L. Pons, Gerbrand Koren, Wouter Peters, and Thomas Röckmann
Biogeosciences, 17, 3903–3922,Short summary
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).
Marielle Saunois, Ann R. Stavert, Ben Poulter, Philippe Bousquet, Josep G. Canadell, Robert B. Jackson, Peter A. Raymond, Edward J. Dlugokencky, Sander Houweling, Prabir K. Patra, Philippe Ciais, Vivek K. Arora, David Bastviken, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Kimberly M. Carlson, Mark Carrol, Simona Castaldi, Naveen Chandra, Cyril Crevoisier, Patrick M. Crill, Kristofer Covey, Charles L. Curry, Giuseppe Etiope, Christian Frankenberg, Nicola Gedney, Michaela I. Hegglin, Lena Höglund-Isaksson, Gustaf Hugelius, Misa Ishizawa, Akihiko Ito, Greet Janssens-Maenhout, Katherine M. Jensen, Fortunat Joos, Thomas Kleinen, Paul B. Krummel, Ray L. Langenfelds, Goulven G. Laruelle, Licheng Liu, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Joe McNorton, Paul A. Miller, Joe R. Melton, Isamu Morino, Jurek Müller, Fabiola Murguia-Flores, Vaishali Naik, Yosuke Niwa, Sergio Noce, Simon O'Doherty, Robert J. Parker, Changhui Peng, Shushi Peng, Glen P. Peters, Catherine Prigent, Ronald Prinn, Michel Ramonet, Pierre Regnier, William J. Riley, Judith A. Rosentreter, Arjo Segers, Isobel J. Simpson, Hao Shi, Steven J. Smith, L. Paul Steele, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Francesco N. Tubiello, Aki Tsuruta, Nicolas Viovy, Apostolos Voulgarakis, Thomas S. Weber, Michiel van Weele, Guido R. van der Werf, Ray F. Weiss, Doug Worthy, Debra Wunch, Yi Yin, Yukio Yoshida, Wenxin Zhang, Zhen Zhang, Yuanhong Zhao, Bo Zheng, Qing Zhu, Qiuan Zhu, and Qianlai Zhuang
Earth Syst. Sci. Data, 12, 1561–1623,Short summary
Understanding and quantifying the global methane (CH4) budget is important for assessing realistic pathways to mitigate climate change. We have established a consortium of multidisciplinary scientists under the umbrella of the Global Carbon Project to synthesize and stimulate new research aimed at improving and regularly updating the global methane budget. This is the second version of the review dedicated to the decadal methane budget, integrating results of top-down and bottom-up estimates.
Stephen J. Harris, Jesper Liisberg, Longlong Xia, Jing Wei, Kerstin Zeyer, Longfei Yu, Matti Barthel, Benjamin Wolf, Bryce F. J. Kelly, Dioni I. Cendón, Thomas Blunier, Johan Six, and Joachim Mohn
Atmos. Meas. Tech., 13, 2797–2831,Short summary
The latest commercial laser spectrometers have the potential to revolutionize N2O isotope analysis. However, to do so, they must be able to produce trustworthy data. Here, we test the performance of widely used laser spectrometers for ambient air applications and identify instrument-specific dependencies on gas matrix and trace gas concentrations. We then provide a calibration workflow to facilitate the operation of these instruments in order to generate reproducible and accurate data.
Kévin Fourteau, Laurent Arnaud, Xavier Faïn, Patricia Martinerie, David M. Etheridge, Vladimir Lipenkov, and Jean-Marc Barnola
Earth Syst. Sci. Data, 12, 1171–1177,Short summary
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,Short summary
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 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,Short summary
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.
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,Short summary
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,Short summary
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,
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,Short summary
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,Short summary
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.
Roger J. Francey, Jorgen S. Frederiksen, L. Paul Steele, and Ray L. Langenfelds
Atmos. Chem. Phys., 19, 14741–14754,Short summary
25-year composites of interhemispheric baseline CO2 differences demonstrate close agreement between 4 monitoring networks. Variability from monthly to multiyear time frames mostly reflects variability in upper troposphere dynamical indices chosen to represent eddy and mean transport interhemispheric exchange. Monthly interhemispheric atmospheric fluxes are much larger than air–surface terrestrial exchanges. The composite differences offer unusual constraints on transport in global carbon models.
Laurie Menviel, Emilie Capron, Aline Govin, Andrea Dutton, Lev Tarasov, Ayako Abe-Ouchi, Russell N. Drysdale, Philip L. Gibbard, Lauren Gregoire, Feng He, Ruza F. Ivanovic, Masa Kageyama, Kenji Kawamura, Amaelle Landais, Bette L. Otto-Bliesner, Ikumi Oyabu, Polychronis C. Tzedakis, Eric Wolff, and Xu Zhang
Geosci. Model Dev., 12, 3649–3685,Short summary
As part of the Past Global Changes (PAGES) working group on Quaternary Interglacials, we propose a protocol to perform transient simulations of the penultimate deglaciation for the Paleoclimate Modelling Intercomparison Project (PMIP4). This design includes time-varying changes in orbital forcing, greenhouse gas concentrations, continental ice sheets as well as freshwater input from the disintegration of continental ice sheets. Key paleo-records for model-data comparison are also included.
Charel Wohl, David Capelle, Anna Jones, William T. Sturges, Philip D. Nightingale, Brent G. T. Else, and Mingxi Yang
Ocean Sci., 15, 925–940,Short summary
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.
Tobias Erhardt, Emilie Capron, Sune Olander Rasmussen, Simon Schüpbach, Matthias Bigler, Florian Adolphi, and Hubertus Fischer
Clim. Past, 15, 811–825,Short summary
The cause of the rapid warming events documented in proxy records across the Northern Hemisphere during the last glacial has been a long-standing puzzle in paleo-climate research. Here, we use high-resolution ice-core data from to cores in Greenland to investigate the progression during the onset of these events on multi-annual timescales to test their plausible triggers. We show that atmospheric circulation changes preceded the warming in Greenland and the collapse of the sea ice by a decade.
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,Short summary
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.
Mai Winstrup, Paul Vallelonga, Helle A. Kjær, Tyler J. Fudge, James E. Lee, Marie H. Riis, Ross Edwards, Nancy A. N. Bertler, Thomas Blunier, Ed J. Brook, Christo Buizert, Gabriela Ciobanu, Howard Conway, Dorthe Dahl-Jensen, Aja Ellis, B. Daniel Emanuelsson, Richard C. A. Hindmarsh, Elizabeth D. Keller, Andrei V. Kurbatov, Paul A. Mayewski, Peter D. Neff, Rebecca L. Pyne, Marius F. Simonsen, Anders Svensson, Andrea Tuohy, Edwin D. Waddington, and Sarah Wheatley
Clim. Past, 15, 751–779,Short summary
We present a 2700-year timescale and snow accumulation history for an ice core from Roosevelt Island, Ross Ice Shelf, Antarctica. We observe a long-term slightly decreasing trend in accumulation during most of the period but a rapid decline since the mid-1960s. The latter is linked to a recent strengthening of the Amundsen Sea Low and the expansion of regional sea ice. The year 1965 CE may thus mark the onset of significant increases in sea-ice extent in the eastern Ross Sea.
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,Short summary
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,Short summary
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.
Ann R. Stavert, Rachel M. Law, Marcel van der Schoot, Ray L. Langenfelds, Darren A. Spencer, Paul B. Krummel, Scott D. Chambers, Alistair G. Williams, Sylvester Werczynski, Roger J. Francey, and Russell T. Howden
Atmos. Meas. Tech., 12, 1103–1121,Short summary
The Southern Ocean is a key sink of carbon dioxide (CO2), but efforts to study trends in and the variability of the sink have been hindered by the limited number of CO2 measurements in this region. Here we describe a set of new in situ continuous (minutely) atmospheric CO2 observations. We show that this new record better captures long-term changes and seasonality than traditional 2-weekly flask records. As such, this data set will provide key insights into the changing Southern Ocean sink.
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,Short summary
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,
Jonas Beck, Michael Bock, Jochen Schmitt, Barbara Seth, Thomas Blunier, and Hubertus Fischer
Biogeosciences, 15, 7155–7175,Short summary
Ice core concentration and stable isotope measurements of atmospheric CH4 give valuable insights into the CH4 cycle of the past. New carbon and hydrogen stable isotope CH4 data measured on ice from both Greenland and Antarctica over the Holocene allow us to draw conclusions on the methane emission processes. In particular, our results cast doubt on a hypothesis proposing early human land use to be responsible for the atmospheric methane concentration increase in the second half of the Holocene.
Laurie Menviel, Emilie Capron, Aline Govin, Andrea Dutton, Lev Tarasov, Ayako Abe-Ouchi, Russell Drysdale, Philip Gibbard, Lauren Gregoire, Feng He, Ruza Ivanovic, Masa Kageyama, Kenji Kawamura, Amaelle Landais, Bette L. Otto-Bliesner, Ikumi Oyabu, Polychronis Tzedakis, Eric Wolff, and Xu Zhang
Clim. Past Discuss.,
Preprint withdrawnShort summary
The penultimate deglaciation (~ 138–128 ka), which represents the transition into the Last Interglacial period, provides a framework to investigate the climate and environmental response to large changes in boundary conditions. Here, as part of the PAGES-PMIP working group on Quaternary Interglacials, we propose a protocol to perform transient simulations of the penultimate deglaciation as well as a selection of paleo records for upcoming model-data comparisons.
Alexis Burr, Clément Ballot, Pierre Lhuissier, Patricia Martinerie, Christophe L. Martin, and Armelle Philip
The Cryosphere, 12, 2481–2500,Short summary
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.
Reiner Onken, Heinz-Volker Fiekas, Laurent Beguery, Ines Borrione, Andreas Funk, Michael Hemming, Jaime Hernandez-Lasheras, Karen J. Heywood, Jan Kaiser, Michaela Knoll, Baptiste Mourre, Paolo Oddo, Pierre-Marie Poulain, Bastien Y. Queste, Aniello Russo, Kiminori Shitashima, Martin Siderius, and Elizabeth Thorp Küsel
Ocean Sci., 14, 321–335,Short summary
In June 2014, high-resolution oceanographic data were collected in the western Mediterranean Sea by two research vessels, 11 gliders, moored instruments, drifters, and one profiling float. The objective of this article is to provide an overview of the data set which is utilised by various ongoing studies, focusing on (i) water masses and circulation, (ii) operational forecasting, (iii) data assimilation, (iv) variability of the ocean, and (v) new payloads for gliders.
Marco de Bruine, Maarten Krol, Twan van Noije, Philippe Le Sager, and Thomas Röckmann
Geosci. Model Dev., 11, 1443–1465,Short summary
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,
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,
Emma 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,Short summary
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,Short summary
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.
Nancy A. N. Bertler, Howard Conway, Dorthe Dahl-Jensen, Daniel B. Emanuelsson, Mai Winstrup, Paul T. Vallelonga, James E. Lee, Ed J. Brook, Jeffrey P. Severinghaus, Taylor J. Fudge, Elizabeth D. Keller, W. Troy Baisden, Richard C. A. Hindmarsh, Peter D. Neff, Thomas Blunier, Ross Edwards, Paul A. Mayewski, Sepp Kipfstuhl, Christo Buizert, Silvia Canessa, Ruzica Dadic, Helle A. Kjær, Andrei Kurbatov, Dongqi Zhang, Edwin D. Waddington, Giovanni Baccolo, Thomas Beers, Hannah J. Brightley, Lionel Carter, David Clemens-Sewall, Viorela G. Ciobanu, Barbara Delmonte, Lukas Eling, Aja Ellis, Shruthi Ganesh, Nicholas R. Golledge, Skylar Haines, Michael Handley, Robert L. Hawley, Chad M. Hogan, Katelyn M. Johnson, Elena Korotkikh, Daniel P. Lowry, Darcy Mandeno, Robert M. McKay, James A. Menking, Timothy R. Naish, Caroline Noerling, Agathe Ollive, Anaïs Orsi, Bernadette C. Proemse, Alexander R. Pyne, Rebecca L. Pyne, James Renwick, Reed P. Scherer, Stefanie Semper, Marius Simonsen, Sharon B. Sneed, Eric J. Steig, Andrea Tuohy, Abhijith Ulayottil Venugopal, Fernando Valero-Delgado, Janani Venkatesh, Feitang Wang, Shimeng Wang, Dominic A. Winski, V. Holly L. Winton, Arran Whiteford, Cunde Xiao, Jiao Yang, and Xin Zhang
Clim. Past, 14, 193–214,Short summary
Temperature and snow accumulation records from the annually dated Roosevelt Island Climate Evolution (RICE) ice core show that for the past 2 700 years, the eastern Ross Sea warmed, while the western Ross Sea showed no trend and West Antarctica cooled. From the 17th century onwards, this dipole relationship changed. Now all three regions show concurrent warming, with snow accumulation declining in West Antarctica and the eastern Ross Sea.
Malte Winther, David Balslev-Harder, Søren Christensen, Anders Priemé, Bo Elberling, Eric Crosson, and Thomas Blunier
Biogeosciences, 15, 767–780,Short summary
Nitrous oxide (N2O) is an important and strong greenhouse gas in the atmosphere and part of climate. N2O is produced by microbes in terrestrial and aquatic ecosystems. The properties of each specific molecule can be used to determine the source. We implemented continuous measurements of N2O during incubation of denitrifying bacteria and believe that similar experiments will lead to a better understanding of N2O turnover and on the biotic mechanisms behind greenhouse gas exchange of the globe.
Chris J. Curtis, Jan Kaiser, Alina Marca, N. John Anderson, Gavin Simpson, Vivienne Jones, and Erika Whiteford
Biogeosciences, 15, 529–550,Short summary
Few studies have investigated the atmospheric deposition of nitrate in the Arctic or its impacts on Arctic ecosystems. We collected late-season snowpack from three regions in western Greenland from the coast to the edge of the ice sheet. We found major differences in nitrate concentrations (lower at the coast) and deposition load (higher). Nitrate in snowpack undergoes losses and isotopic enrichment which are greatest in inland areas; hence deposition impacts may be greatest at the coast.
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,Short summary
We measured the three chlorofluorocarbons (CFCs) CFC-13, CFC-114, and CFC-115 in the atmosphere because they are important in stratospheric ozone depletion. These compounds should have decreased in the atmosphere because they are banned by the Montreal Protocol but we find the opposite. Emissions over the last decade have not declined on a global scale. We use inverse modeling and our observations to find that a large part of the emissions originate in the Asian region.
Kelley C. Wells, Dylan B. Millet, Nicolas Bousserez, Daven K. Henze, Timothy J. Griffis, Sreelekha Chaliyakunnel, Edward J. Dlugokencky, Eri Saikawa, Gao Xiang, Ronald G. Prinn, Simon O'Doherty, Dickon Young, Ray F. Weiss, Geoff S. Dutton, James W. Elkins, Paul B. Krummel, Ray Langenfelds, and L. Paul Steele
Atmos. Chem. Phys., 18, 735–756,Short summary
This paper uses three different frameworks to derive nitrous oxide (N2O) emissions based on global surface observations. One of these frameworks employs a new approach that allows for fast computation and explores a larger solution space than other methods. Our results point to a few conclusions about the global N2O budget, including a larger contribution from tropical sources, an overestimate of natural soil emissions, and an underestimate of agricultural sources particularly in springtime.
Kévin Fourteau, Xavier Faïn, Patricia Martinerie, Amaëlle Landais, Alexey A. Ekaykin, Vladimir Ya. Lipenkov, and Jérôme Chappellaz
Clim. Past, 13, 1815–1830,Short summary
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,Short summary
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.
Michaela Knoll, Ines Borrione, Heinz-Volker Fiekas, Andreas Funk, Michael P. Hemming, Jan Kaiser, Reiner Onken, Bastien Queste, and Aniello Russo
Ocean Sci., 13, 889–904,Short summary
The hydrography and circulation west of Sardinia, observed in June 2014 during REP14-MED by means of various measuring platforms, are presented and compared with previous knowledge. So far, the circulation of this area is not well-known and the hydrography is subject to long-term changes. The different water masses are characterized and temporal changes are emphasized. The observed eddies are specified and geostrophic transports in the upper ocean are presented.
Bette L. Otto-Bliesner, Pascale Braconnot, Sandy P. Harrison, Daniel J. Lunt, Ayako Abe-Ouchi, Samuel Albani, Patrick J. Bartlein, Emilie Capron, Anders E. Carlson, Andrea Dutton, Hubertus Fischer, Heiko Goelzer, Aline Govin, Alan Haywood, Fortunat Joos, Allegra N. LeGrande, William H. Lipscomb, Gerrit Lohmann, Natalie Mahowald, Christoph Nehrbass-Ahles, Francesco S. R. Pausata, Jean-Yves Peterschmitt, Steven J. Phipps, Hans Renssen, and Qiong Zhang
Geosci. Model Dev., 10, 3979–4003,Short summary
The PMIP4 and CMIP6 mid-Holocene and Last Interglacial simulations provide an opportunity to examine the impact of two different changes in insolation forcing on climate at times when other forcings were relatively similar to present. This will allow exploration of the role of feedbacks relevant to future projections. Evaluating these simulations using paleoenvironmental data will provide direct out-of-sample tests of the reliability of state-of-the-art models to simulate climate changes.
David E. Oram, Matthew J. Ashfold, Johannes C. Laube, Lauren J. Gooch, Stephen Humphrey, William T. Sturges, Emma 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,Short summary
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.
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Ray Weiss, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Atmos. Chem. Phys., 17, 11135–11161,Short summary
Following the Global Methane Budget 2000–2012 published in Saunois et al. (2016), we use the same dataset of bottom-up and top-down approaches to discuss the variations in methane emissions over the period 2000–2012. The changes in emissions are discussed both in terms of trends and quasi-decadal changes. The ensemble gathered here allows us to synthesise the robust changes in terms of regional and sectorial contributions to the increasing methane emissions.
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,Short summary
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.
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,Short summary
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.
Michael P. Hemming, Jan Kaiser, Karen J. Heywood, Dorothee C.E. Bakker, Jacqueline Boutin, Kiminori Shitashima, Gareth Lee, Oliver Legge, and Reiner Onken
Ocean Sci., 13, 427–442,Short summary
Underwater gliders are useful platforms for monitoring the world oceans at a high resolution. An experimental pH sensor was attached to an underwater glider in the Mediterranean Sea, which is an important carbon sink region. Comparing measurements from the glider with those obtained from a ship indicated that there were issues with the experimental pH sensor. Correcting for these issues enabled us to look at pH variability in the area related to biomass abundance and physical water properties.
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,Short summary
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,Short summary
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.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Ed Dlugokencky, Angel J. Gomez-Pelaez, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, Jgor Arduini, Francesco Apadula, Christoph Gerbig, Dietrich G. Feist, Rigel Kivi, Yukio Yoshida, and Wouter Peters
Geosci. Model Dev., 10, 1261–1289,Short summary
In this study, we found that the average global methane emission for 2000–2012, estimated by the CTE-CH4 model, was 516±51 Tg CH4 yr-1, and the estimates for 2007–2012 were 4 % larger than for 2000–2006. The model estimates are sensitive to inputs and setups, but according to sensitivity tests the study suggests that the increase in atmospheric methane concentrations during 21st century was due to an increase in emissions from the 35S-EQ latitudinal bands.
Imke Grefe, Sophie Fielding, Karen J. Heywood, and Jan Kaiser
Revised manuscript not accepted
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,Short summary
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.
Bastiaan Jonkheid, Thomas Röckmann, Norbert Glatthor, Christof Janssen, Gabriele Stiller, and Thomas von Clarmann
Atmos. Meas. Tech., 9, 6069–6079,
Marielle Saunois, Philippe Bousquet, Ben Poulter, Anna Peregon, Philippe Ciais, Josep G. Canadell, Edward J. Dlugokencky, Giuseppe Etiope, David Bastviken, Sander Houweling, Greet Janssens-Maenhout, Francesco N. Tubiello, Simona Castaldi, Robert B. Jackson, Mihai Alexe, Vivek K. Arora, David J. Beerling, Peter Bergamaschi, Donald R. Blake, Gordon Brailsford, Victor Brovkin, Lori Bruhwiler, Cyril Crevoisier, Patrick Crill, Kristofer Covey, Charles Curry, Christian Frankenberg, Nicola Gedney, Lena Höglund-Isaksson, Misa Ishizawa, Akihiko Ito, Fortunat Joos, Heon-Sook Kim, Thomas Kleinen, Paul Krummel, Jean-François Lamarque, Ray Langenfelds, Robin Locatelli, Toshinobu Machida, Shamil Maksyutov, Kyle C. McDonald, Julia Marshall, Joe R. Melton, Isamu Morino, Vaishali Naik, Simon O'Doherty, Frans-Jan W. Parmentier, Prabir K. Patra, Changhui Peng, Shushi Peng, Glen P. Peters, Isabelle Pison, Catherine Prigent, Ronald Prinn, Michel Ramonet, William J. Riley, Makoto Saito, Monia Santini, Ronny Schroeder, Isobel J. Simpson, Renato Spahni, Paul Steele, Atsushi Takizawa, Brett F. Thornton, Hanqin Tian, Yasunori Tohjima, Nicolas Viovy, Apostolos Voulgarakis, Michiel van Weele, Guido R. van der Werf, Ray Weiss, Christine Wiedinmyer, David J. Wilton, Andy Wiltshire, Doug Worthy, Debra Wunch, Xiyan Xu, Yukio Yoshida, Bowen Zhang, Zhen Zhang, and Qiuan Zhu
Earth Syst. Sci. Data, 8, 697–751,Short summary
An accurate assessment of the methane budget is important to understand the atmospheric methane concentrations and trends and to provide realistic pathways for climate change mitigation. The various and diffuse sources of methane as well and its oxidation by a very short lifetime radical challenge this assessment. We quantify the methane sources and sinks as well as their uncertainties based on both bottom-up and top-down approaches provided by a broad international scientific community.
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,
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,Short summary
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,Short summary
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.
Bette L. Otto-Bliesner, Pascale Braconnot, Sandy P. Harrison, Daniel J. Lunt, Ayako Abe-Ouchi, Samuel Albani, Patrick J. Bartlein, Emilie Capron, Anders E. Carlson, Andrea Dutton, Hubertus Fischer, Heiko Goelzer, Aline Govin, Alan Haywood, Fortunat Joos, Allegra N. Legrande, William H. Lipscomb, Gerrit Lohmann, Natalie Mahowald, Christoph Nehrbass-Ahles, Jean-Yves Peterschmidt, Francesco S.-R. Pausata, Steven Phipps, and Hans Renssen
Clim. Past Discuss.,
Olivier Eicher, Matthias Baumgartner, Adrian Schilt, Jochen Schmitt, Jakob Schwander, Thomas F. Stocker, and Hubertus Fischer
Clim. Past, 12, 1979–1993,Short summary
A new high-resolution total air content record over the NGRIP ice core, spanning 0.3–120 kyr is presented. In agreement with Antarctic ice cores, we find a strong local insolation signature but also 3–5 % decreases in total air content as a local response to Dansgaard–Oeschger events, which can only partly be explained by changes in surface pressure and temperature. Accordingly, a dynamic response of firnification to rapid climate changes on the Greenland ice sheet must have occurred.
Emma J. Stone, Emilie Capron, Daniel J. Lunt, Antony J. Payne, Joy S. Singarayer, Paul J. Valdes, and Eric W. Wolff
Clim. Past, 12, 1919–1932,Short summary
Climate models forced only with greenhouse gas concentrations and orbital parameters representative of the early Last Interglacial are unable to reproduce the observed colder-than-present temperatures in the North Atlantic and the warmer-than-present temperatures in the Southern Hemisphere. Using a climate model forced also with a freshwater amount derived from data representing melting from the remnant Northern Hemisphere ice sheets accounts for this response via the bipolar seesaw mechanism.
Amaelle Landais, Valérie Masson-Delmotte, Emilie Capron, Petra M. Langebroek, Pepijn Bakker, Emma J. Stone, Niklaus Merz, Christoph C. Raible, Hubertus Fischer, Anaïs Orsi, Frédéric Prié, Bo Vinther, and Dorthe Dahl-Jensen
Clim. Past, 12, 1933–1948,Short summary
The last lnterglacial (LIG; 116 000 to 129 000 years before present) surface temperature at the upstream Greenland NEEM deposition site is estimated to be warmer by +7 to +11 °C compared to the preindustrial period. We show that under such warm temperatures, melting of snow probably led to a significant surface melting. There is a paradox between the extent of the Greenland ice sheet during the LIG and the strong warming during this period that models cannot solve.
Matthias Egger, Peter Kraal, Tom Jilbert, Fatimah Sulu-Gambari, Célia J. Sapart, Thomas Röckmann, and Caroline P. Slomp
Biogeosciences, 13, 5333–5355,Short summary
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,Short summary
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,Short summary
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.
Aki Tsuruta, Tuula Aalto, Leif Backman, Janne Hakkarainen, Ingrid T. van der Laan-Luijkx, Maarten C. Krol, Renato Spahni, Sander Houweling, Marko Laine, Marcel van der Schoot, Ray Langenfelds, Raymond Ellul, and Wouter Peters
Geosci. Model Dev. Discuss.,
Revised manuscript has not been submittedShort summary
In this study, we found that methane emission estimates, driven by the CTE-CH4 model, depend on model setups and inputs, especially for regional estimates. An optimal setup makes the estimates stable, but inputs, such as emission estimates from inventories, and observations, also play significant role. The results can be used for an extended analysis on relative contributions of methane emissions to atmospheric methane concentration changes in recent decades.
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,Short summary
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,Short summary
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.
Malte Winther, David Balslev-Harder, Søren Christensen, Anders Priemé, Bo Elberling, Eric Crosson, and Thomas Blunier
Revised manuscript not acceptedShort summary
Nitrous oxide (N2O) is an important and strong greenhouse gas in the atmosphere and part of climate. N2O is produced by microbes in terrestrial and aquatic ecosystems. The properties of each specific molecule can be used to determine the source. We implemented continuous measurements of N2O during incubation of denitrifying bacteria and believe that similar experiments will lead to a better understanding of N2O turnover and on the biotic mechanisms behind greenhouse gas exchange of the Globe.
Rachael H. Rhodes, Xavier Faïn, Edward J. Brook, Joseph R. McConnell, Olivia J. Maselli, Michael Sigl, Jon Edwards, Christo Buizert, Thomas Blunier, Jérôme Chappellaz, and Johannes Freitag
Clim. Past, 12, 1061–1077,Short summary
Local artifacts in ice core methane data are superimposed on consistent records of past atmospheric variability. These artifacts are not related to past atmospheric history and care should be taken to avoid interpreting them as such. By investigating five polar ice cores from sites with different conditions, we relate isolated methane spikes to melt layers and decimetre-scale variations as "trapping signal" associated with a difference in timing of air bubble closure in adjacent firn layers.
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,Short summary
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,Short summary
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.
L. M. T. Joelsson, J. A. Schmidt, E. J. K. Nilsson, T. Blunier, D. W. T. Griffith, S. Ono, and M. S. Johnson
Atmos. Chem. Phys., 16, 4439–4449,Short summary
We present experimental kinetic isotope effects (KIE) for the OH oxidation of CH3D and 13CH3D and their temperature dependence. Our determination of the 13CH3D + OH KIE is novel and we find no "clumped" isotope effect within the experimental uncertainty.
Lucie Bazin, Amaelle Landais, Emilie Capron, Valérie Masson-Delmotte, Catherine Ritz, Ghislain Picard, Jean Jouzel, Marie Dumont, Markus Leuenberger, and Frédéric Prié
Clim. Past, 12, 729–748,Short summary
We present new measurements of δO2⁄N2 and δ18Oatm performed on well-conserved ice from EDC covering MIS5 and between 380 and 800 ka. The combination of the observation of a 100 ka periodicity in the new δO2⁄N2 record with a MIS5 multi-site multi-proxy study has revealed a potential influence of local climatic parameters on δO2⁄N2. Moreover, we propose that the varying delay between d18Oatm and precession for the last 800 ka is affected by the occurrence of ice sheet discharge events.
Dominika Lewicka-Szczebak, Jens Dyckmans, Jan Kaiser, Alina Marca, Jürgen Augustin, and Reinhard Well
Biogeosciences, 13, 1129–1144,Short summary
Oxygen isotopic signatures of N2O are formed in complex multistep enzymatic reactions and depend on isotopic fractionation during enzymatic reduction of nitrate to N2O and on the oxygen isotope exchange with soil water. We propose a new method for quantification of oxygen isotope exchange, with simultaneous determination of oxygen isotopic signatures, to decipher the mechanism of oxygen isotopic fractionation. We indicate the differences between fractionation mechanisms by various pathways.
Tom Hull, Naomi Greenwood, Jan Kaiser, and Martin Johnson
Biogeosciences, 13, 943–959,Short summary
We explore the estimation of NCP using an oxygen time series from a surface mooring located in the River Thames plume. Our study site is identified as a region of net heterotrophy with strong seasonal variability. Short-term daily variability in oxygen and horizontal advection is demonstrated to make accurate estimates challenging. The effects of bubble-induced supersaturation is shown to have a large influence on cumulative annual estimates.
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,Short summary
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,Short summary
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,Short summary
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,Short summary
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.
T. Kobashi, T. Ikeda-Fukazawa, M. Suwa, J. Schwander, T. Kameda, J. Lundin, A. Hori, H. Motoyama, M. Döring, and M. Leuenberger
Atmos. Chem. Phys., 15, 13895–13914,Short summary
We find that argon/nitrogen ratios of trapped air in the GISP2 ice core on “gas ages” are significantly negatively correlated with accumulation rate changes over the past 6000 years. Lines of evidence indicate that changes in overloading pressure at bubble closeoff depths induced the gas fractionation in closed bubbles. Further understanding of the fractionation processes may lead to a new proxy for the past temperature and accumulation rate.
J. Gloël, C. Robinson, G. H. Tilstone, G. Tarran, and J. Kaiser
Ocean Sci., 11, 947–952,Short summary
We assess benzalkonium chloride (BAC) as alternative to mercuric chloride (HgCl2) for preservation of seawater samples. BAC concentrations of 50mg dm–3 inhibited microbial activity for at least 3 days in samples tested with chlorophyll a concentrations up to 1mg m–3. With fewer risks to health and environment, and lower waste disposal costs, BAC could be a short-term alternative to HgCl2, but cannot replace it for oxygen triple isotope samples, which require storage over weeks to months.
Q. Chen, M. E. Popa, A. M. Batenburg, and T. Röckmann
Atmos. Chem. Phys., 15, 13003–13021,Short summary
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.
C. Reutenauer, A. Landais, T. Blunier, C. Bréant, M. Kageyama, M.-N. Woillez, C. Risi, V. Mariotti, and P. Braconnot
Clim. Past, 11, 1527–1551,Short summary
Isotopes of atmospheric O2 undergo millennial-scale variations during the last glacial period, and systematically increase during Heinrich stadials. Such variations are mostly due to vegetation and water cycle processes. Our modeling approach reproduces the main observed features of Heinrich stadials in terms of climate, vegetation and rainfall. It highlights the strong role of hydrology on O2 isotopes, which can be seen as a global integrator of precipitation changes over vegetated areas.
K. C. Wells, D. B. Millet, N. Bousserez, D. K. Henze, S. Chaliyakunnel, T. J. Griffis, Y. Luan, E. J. Dlugokencky, R. G. Prinn, S. O'Doherty, R. F. Weiss, G. S. Dutton, J. W. Elkins, P. B. Krummel, R. Langenfelds, L. P. Steele, E. A. Kort, S. C. Wofsy, and T. Umezawa
Geosci. Model Dev., 8, 3179–3198,Short summary
This paper introduces a new inversion framework for N2O using GEOS-Chem and its adjoint, which we employed in a series of observing system simulation experiments to evaluate the source and sink constraints provided by surface and aircraft-based N2O measurements. We also applied a new approach for estimating a posteriori uncertainty for high-dimensional inversions, and used it to quantify the spatial and temporal resolution of N2O emission constraints achieved with the current observing network.
S. Pandey, S. Houweling, M. Krol, I. Aben, and T. Röckmann
Atmos. Chem. Phys., 15, 8615–8629,Short summary
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.,
Revised manuscript not acceptedShort summary
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,
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,Short summary
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.
F. Parrenin, L. Bazin, E. Capron, A. Landais, B. Lemieux-Dudon, and V. Masson-Delmotte
Geosci. Model Dev., 8, 1473–1492,Short summary
This manuscript describes a probabilistic model which aims at optimizing the chronology of ice cores by combining different sources of information.
C. Martín, R. Mulvaney, G. H. Gudmundsson, and H. Corr
Clim. Past, 11, 547–557,
J. A. Fisher, S. R. Wilson, G. Zeng, J. E. Williams, L. K. Emmons, R. L. Langenfelds, P. B. Krummel, and L. P. Steele
Atmos. Chem. Phys., 15, 3217–3239,Short summary
The Southern Hemisphere (SH) serves as an important test bed for evaluating our understanding of the processes that drive the composition of the clean background atmosphere. Using data from two aircraft campaigns, combined with four atmospheric chemistry models, we find a large sensitivity in the remote SH to biogenic emissions and their subsequent chemistry and transport. Future model evaluation and measurement campaigns should prioritize reducing uncertainties in these processes.
F. A. Stap, O. P. Hasekamp, and T. Röckmann
Atmos. Meas. Tech., 8, 1287–1301,Short summary
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,Short summary
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,
E. 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,
D. J. Mrozek, C. van der Veen, M. Kliphuis, J. Kaiser, A. A. Wiegel, and T. Röckmann
Atmos. Meas. Tech., 8, 811–822,Short summary
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.
E. C. Leedham Elvidge, S.-M. Phang, W. T. Sturges, and G. Malin
Biogeosciences, 12, 387–398,
A. Fraser, P. I. Palmer, L. Feng, H. Bösch, R. Parker, E. J. Dlugokencky, P. B. Krummel, and R. L. Langenfelds
Atmos. Chem. Phys., 14, 12883–12895,Short summary
Satellite measurements of CO2 and CH4 can be subject to regional systematic errors that can consequently compromise their ability to infer robust flux estimates of these two gases. We develop a method to use retrieved ratios of CH4 and CO2 that are less affected by systematic error. We show that additional in situ data are needed to anchor these observed ratios so they can simultaneously infer fluxes of CO2 and CH4. We argue the ratio data will provide a more faithful description of true fluxes.
M. Guillevic, L. Bazin, A. Landais, C. Stowasser, V. Masson-Delmotte, T. Blunier, F. Eynaud, S. Falourd, E. Michel, B. Minster, T. Popp, F. Prié, and B. M. Vinther
Clim. Past, 10, 2115–2133,
M. F. Loutre, T. Fichefet, H. Goosse, P. Huybrechts, H. Goelzer, and E. Capron
Clim. Past, 10, 1541–1565,
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, E. C. Leedham, 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,
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
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Related subject area
Subject: Isotopes | Research Activity: Laboratory Studies | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)Quantifying the nitrogen isotope effects during photochemical equilibrium between NO and NO2: implications for δ15N in tropospheric reactive nitrogenTemporal variation in 129I and 127I in aerosols from Xi'an, China: influence of East Asian monsoon and heavy haze eventsHigh time-resolved measurement of stable carbon isotope composition in water-soluble organic aerosols: method optimization and a case study during winter haze in eastern ChinaDependence between the photochemical age of light aromatic hydrocarbons and the carbon isotope ratios of atmospheric nitrophenolsEvidence for a major missing source in the global chloromethane budget from stable carbon isotopesAtmospheric Δ17O(NO3−) reveals nocturnal chemistry dominates nitrate production in Beijing hazeMass spectrometric measurement of hydrogen isotope fractionation for the reactions of chloromethane with OH and ClStable carbon isotope ratios of ambient aromatic volatile organic compoundsKinetic isotope effects of 12CH3D + OH and 13CH3D + OH from 278 to 313 KInvestigation of post-depositional processing of nitrate in East Antarctic snow: isotopic constraints on photolytic loss, re-oxidation, and source inputsNOx cycle and the tropospheric ozone isotope anomaly: an experimental investigationFractionation of sulfur isotopes during heterogeneous oxidation of SO2 on sea salt aerosol: a new tool to investigate non-sea salt sulfate production in the marine boundary layerSulfur isotope fractionation during oxidation of sulfur dioxide: gas-phase oxidation by OH radicals and aqueous oxidation by H2O2, O3 and iron catalysisMolecular hydrogen (H2) emissions and their isotopic signatures (H/D) from a motor vehicle: implications on atmospheric H2Isotope effect in the formation of H2 from H2CO studied at the atmospheric simulation chamber SAPHIRPressure dependence of the deuterium isotope effect in the photolysis of formaldehyde by ultraviolet light
Jianghanyang Li, Xuan Zhang, John Orlando, Geoffrey Tyndall, and Greg Michalski
Atmos. Chem. Phys., 20, 9805–9819,Short summary
Nitrogen isotopic compositions of atmospheric reactive nitrogen are widely used to infer their sources. However, the reactions between NO and NO2 strongly impact their isotopes, which was not well understood. We conducted a series of experiments in an atmospheric simulation chamber to determine the isotopic effects of (1) direct isotopic exchange between NO and NO2 and (2) the isotopic fractionations during NOx photochemistry, then developed an equation to quantify the overall isotopic effect.
Luyuan Zhang, Xiaolin Hou, Sheng Xu, Tian Feng, Peng Cheng, Yunchong Fu, and Ning Chen
Atmos. Chem. Phys., 20, 2623–2635,Short summary
To trace the long-range transport of air pollutants and understand the atmospheric effect of iodine, the daily-resolution temporal variations of 129I and 127I in aerosols from a monsoonal city indicate the East Asian monsoon and fossil fuel combustion plays crucial roles on transport of 129I from Europe to East Asia and on elevated 127I concentrations. Through linking iodine isotopes with five major air pollutants, this study proposes the possible role of iodine in urban air pollution.
Wenqi Zhang, Yan-Lin Zhang, Fang Cao, Yankun Xiang, Yuanyuan Zhang, Mengying Bao, Xiaoyan Liu, and Yu-Chi Lin
Atmos. Chem. Phys., 19, 11071–11087,Short summary
A novel method to determine the concentration and the isotopes of WSOC in aerosols is established and applied in the analysis of a severe haze in eastern China. The results show that the studied site is affected by the photochemical aging, biomass burning and dust aerosols in different episodes during the sampling period. The analysis of WSOC and its isotopes offers a great potential to better understand the source emission, the atmospheric aging and the secondary production of WSOC.
Marina Saccon, Anna Kornilova, Lin Huang, and Jochen Rudolph
Atmos. Chem. Phys., 19, 5495–5509,Short summary
As compound are emitted into the atmosphere, they can undergo chemical reactions to produce secondary products. This paper investigates the relations of compounds' unique chemical characteristics to the processes that formed them from emissions in the atmosphere. A model is applied to help with this investigation. The complexity of the atmosphere, including mixing of air masses and variability in precursor reactivity, is taken into consideration, and results are presented.
Enno Bahlmann, Frank Keppler, Julian Wittmer, Markus Greule, Heinz Friedrich Schöler, Richard Seifert, and Cornelius Zetzsch
Atmos. Chem. Phys., 19, 1703–1719,Short summary
Chloromethane is the most important natural carrier of chlorine to the stratosphere. From a newly determined carbon isotope effect of −11.2 ‰ for the tropospheric loss of CH3Cl we derive a tropical rainforest CH3Cl source of 670 ± 200 Gg a−1, 60 % smaller than previous estimates. A revision of previous bottom-up estimates using above-ground biomass instead of rainforest area strongly supports this lower estimate. Our results suggest a large unknown tropical value of 1530 ± 200 Gg a−1.
Pengzhen He, Zhouqing Xie, Xiyuan Chi, Xiawei Yu, Shidong Fan, Hui Kang, Cheng Liu, and Haicong Zhan
Atmos. Chem. Phys., 18, 14465–14476,Short summary
We present the first observations of the oxygen-17 excess of atmospheric nitrate (Δ17O(NO−3)) collected in Beijing haze to reveal the relative importance of different nitrate formation pathways. We found that nocturnal pathways (N2O5 + H2O/Cl– and NO3 + HC) dominated nitrate production during polluted days (PM2.5 ≥ 75 μg m–3), with a mean possible fraction of 56–97 %.
Frank Keppler, Enno Bahlmann, Markus Greule, Heinz Friedrich Schöler, Julian Wittmer, and Cornelius Zetzsch
Atmos. Chem. Phys., 18, 6625–6635,Short summary
Chloromethane is involved in stratospheric ozone depletion, but detailed knowledge of its global budget is missing. In this study stable hydrogen isotope analyses were performed to investigate the dominant loss process for atmospheric chloromethane with photochemically produced hydroxyl radicals. The findings might have significant implications for the use of stable isotope signatures in elucidation of global chloromethane cycling.
Anna Kornilova, Lin Huang, Marina Saccon, and Jochen Rudolph
Atmos. Chem. Phys., 16, 11755–11772,Short summary
The photochemical oxidation of organic compounds in the atmosphere results in the formation of important secondary pollutants such as ozone and fine particles. The extent of oxidation the organic compounds have been subjected too since there emissions is essential is key for understanding the formation of secondary pollutants. This paper demonstrates that measurements of the carbon isotope ratios allow determining the extent of photochemical processing for individual compounds.
L. M. T. Joelsson, J. A. Schmidt, E. J. K. Nilsson, T. Blunier, D. W. T. Griffith, S. Ono, and M. S. Johnson
Atmos. Chem. Phys., 16, 4439–4449,Short summary
We present experimental kinetic isotope effects (KIE) for the OH oxidation of CH3D and 13CH3D and their temperature dependence. Our determination of the 13CH3D + OH KIE is novel and we find no "clumped" isotope effect within the experimental uncertainty.
G. Shi, A. M. Buffen, M. G. Hastings, C. Li, H. Ma, Y. Li, B. Sun, C. An, and S. Jiang
Atmos. Chem. Phys., 15, 9435–9453,Short summary
We evaluate isotopic composition of NO3- in different environments across East Antarctica. At high snow accumulation sites, isotopic ratios are suggestive of preservation of NO3- deposition. At low accumulation sites, isotopes are sensitive to both the loss of NO3- due to photolysis and secondary formation of NO3- within the snow. The imprint of post-depositional alteration is not uniform with depth, making it difficult to predict the isotopic composition at depth from near-surface data alone.
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Atmos. Chem. Phys., 12, 407–423,
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Atmos. Chem. Phys., 10, 5343–5357,
E. J. K. Nilsson, V. F. Andersen, H. Skov, and M. S. Johnson
Atmos. Chem. Phys., 10, 3455–3462,
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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.
Stratospheric ozone protects life on Earth from harmful UV-B radiation. Chlorofluorocarbons...