Articles | Volume 14, issue 8
https://doi.org/10.5194/amt-14-5447-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/amt-14-5447-2021
© Author(s) 2021. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
09 Aug 2021
Research article |
| 09 Aug 2021
| 09 Aug 2021
Characterisation of gas reference materials for underpinning atmospheric measurements of stable isotopes of nitrous oxide
Ruth E. Hill-Pearce
CORRESPONDING AUTHOR
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Aimee Hillier
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Eric Mussell Webber
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Kanokrat Charoenpornpukdee
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Atmospheric Chemistry Research Group, University of Bristol, Bristol, United Kingdom
Simon O'Doherty
Atmospheric Chemistry Research Group, University of Bristol, Bristol, United Kingdom
Joachim Mohn
Empa, Swiss Federal Laboratories for Materials Science and
Technology, Laboratory for Air Pollution/ Environmental Technology,
Dübendorf, Switzerland
Christoph Zellweger
Empa, Swiss Federal Laboratories for Materials Science and
Technology, Laboratory for Air Pollution/ Environmental Technology,
Dübendorf, Switzerland
David R. Worton
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Paul J. Brewer
National Physical Laboratory, Hampton Road, Teddington, TW11 0LW,
United Kingdom
Related authors
No articles found.
Kane Stone, Candice Chen, Susan Solomon, Luke M. Western, Paul B. Krummel, Gabrielle Pétron, Jens Mühle, and Simon O'Doherty
Atmos. Chem. Phys., 26, 10241–10253, https://doi.org/10.5194/acp-26-10241-2026, https://doi.org/10.5194/acp-26-10241-2026, 2026
Short summary
Short summary
There is growing interest in hydrogens impact on atmospheric chemistry and climate. Here, the seasonality of hydrogen oxidation and loss to microbial activity in soils are investigated using information from the hydrofluorocarbon, HFC-152a. A large seasonal range of the soil sink, over twice that of hydroxyl loss, is seen in the Northern latitudes peaking in the late summer, while the Southern latitudes show a much lower range. This will be useful for validating model hydrogen cycles.
Joseph R. Pitt, Dominique Rust, Anita Ganesan, Luke M. Western, Martin K. Vollmer, Jens Mühle, Tobias Bühlmann, Christina M. Harth, Stephen A. Montzka, Brad D. Hall, Isaac J. Vimont, Alistair J. Manning, Alison L. Redington, Stephan Henne, Daniela B. Melo, Saurabh Annadate, Lionel Constantin, Brendan M. Murphy, Matthew Rigby, Dickon Young, Simon O'Doherty, Angelina Wenger, Chris R. Lunder, Ove Hermansen, Thomas Wagenhäuser, Andreas Engel, Jgor Arduini, Michela Maione, Jaegeun Yun, Blagoj Mitrevski, Paul B. Krummel, Paul J. Fraser, Jooil Kim, Ray H. J. Wang, Tae Siek Rhee, Peter K. Salameh, T. Gerard Spain, Stefan Reimann, Ronald G. Prinn, Ray F. Weiss, and Kieran M. Stanley
Atmos. Chem. Phys., 26, 10167–10195, https://doi.org/10.5194/acp-26-10167-2026, https://doi.org/10.5194/acp-26-10167-2026, 2026
Short summary
Short summary
1,2‑Dichloroethane (DCE) can contribute to the depletion of the stratospheric ozone layer. Whether DCE reaches the stratosphere depends on where and when it is emitted. We present the ongoing measurements of DCE from the Advanced Global Atmospheric Gases Experiment (AGAGE) and National Oceanic and Atmospheric Administration (NOAA) global monitoring networks. For the period 2017–2023, our modelled average global emissions based on these observations align with another study, while regional estimates differ. This suggests remaining uncertainty in the geographical distribution of emissions.
Hélène De Longueville, Daniela B. Melo, Alison L. Redington, Alice Ramsden, Alexandre Danjou, Peter Andrews, Joseph Pitt, Brendan Murphy, Lionel Constantin, Kieran M. Stanley, Simon O'Doherty, Angelina Wenger, Dickon Young, Andreas Engel, Tanja Schuck, Katharina Meixner, Thomas Wagenhaeuser, Fides Gad, Martin K. Vollmer, Stefan Reimann, Michela Maoine, Jgor Arduini, Chris Lunder, Norbert Schmidtbauer, László Haszpra, Mihály Molnár, Arnoud Frumau, Cedric Couret, Matthew Rigby, Stephan Henne, Alistair Manning, and Anita L. Ganesan
Atmos. Chem. Phys., 26, 7647–7675, https://doi.org/10.5194/acp-26-7647-2026, https://doi.org/10.5194/acp-26-7647-2026, 2026
Short summary
Short summary
This study estimates emissions of hydrofluorocarbons, potent greenhouse gases, in north-western Europe using atmospheric observations and atmospheric modelling. The estimates are compared with nationally reported emissions submitted to the United Nations. Overall, our results are consistent with reported values, although differences are found for some gases and countries. The findings indicate that emissions in north-western Europe are declining, reflecting the effects of climate regulations.
Julius C. Havsteen, Mehr Fatima, Simone Brunamonti, Andrea Pogány, Thomas Hausmaninger, Benjamin Wolf, Reinhard Well, and Joachim Mohn
Atmos. Meas. Tech., 19, 3557–3580, https://doi.org/10.5194/amt-19-3557-2026, https://doi.org/10.5194/amt-19-3557-2026, 2026
Short summary
Short summary
We present a new correction and calibration protocol to improve the accuracy of nitrous oxide isotope measurements obtained using laser spectroscopy. Through laboratory experiments, spectral simulations, and an automated MATLAB (Matrix Laboratory) reduction scheme, we identify and correct biases caused by matrix gas composition, spectral interferences and instrument variability. This protocol enables researchers to produce more reliable isotope data and supports standardised isotope analyses across laboratories.
Emmal Safi, Joe Pitt, Grant Forster, Chris Rennick, Simon O’Doherty, Dickon Young, Kanokrat Charoenpornpukdee, Nick Garrard, Dafina Kikaj, Andrew Manning, Gerard Spain, Damien Martin, Morgan Lopez, Michel Ramonet, and Kieran Stanely
EGUsphere, https://doi.org/10.5194/egusphere-2026-1802, https://doi.org/10.5194/egusphere-2026-1802, 2026
This preprint is open for discussion and under review for Atmospheric Measurement Techniques (AMT).
Short summary
Short summary
We compared whole and synthetic-air reference materials (RMs) for investigating offsets in greenhouse gas measurements so data from different sites/networks can be trusted when combined. By sending whole and synthetic-air (RMs) to six sites and measuring under routine field conditions, we found whole-air gives the most precise results, especially for carbon dioxide and nitrous oxide. Synthetic-air worked fairly well for methane but synthetic-air RMs needs lower uncertainty before wide use.
Martin K. Vollmer, Joseph R. Pitt, Dickon Young, Stephan Henne, Blagoj Mitrevski, Jens Mühle, Anita Ganesan, Jgor Arduini, Alistair J. Manning, Thomas Wagenhäuser, Alison L. Redington, Daniela B. Melo, Brendan Murphy, Ray Gluckmann, Kieran M. Stanley, Paul B. Krummel, Chris R. Lunder, Jaegeun Yun, Dominique Rust, Angelina Wenger, Myriam Guillevic, Jooil Kim, Ray H. J. Wang, Tae Siek Rhee, Lionel Constantin, Arnoud Frumau, Christina M. Harth, Peter K. Salameh, Ove Hermansen, Matthew Rigby, Luke M. Western, Andreas Engel, Simon O'Doherty, Sunyoung Park, Michela Maione, Paul J. Fraser, Ronald G. Prinn, Ray F. Weiss, and Stefan Reimann
Atmos. Chem. Phys., 26, 6993–7012, https://doi.org/10.5194/acp-26-6993-2026, https://doi.org/10.5194/acp-26-6993-2026, 2026
Short summary
Short summary
Halogenated olefins (HFOs) are newly emerging compounds in the atmosphere. They are in reach of the definition of PFAS (Per- and polyfluoroalkyl substances) and some decay to the eternal chemical trifluoroacetate (TFA). We provide atmospheric measurements of three HFOs from the large Advanced Global Atmospheric Gases Experiment (AGAGE) network and estimate emissions for Northwest Europe for the first time. We find a quasi-ubiquitous presence in the atmosphere and rapidly increasing emissions.
Leonie Bernet, Benjamin T. Brem, Nicolas Bukowiecki, Stephan Henne, Jörg Klausen, Mathew Mutuku, David Njiru, Patricia Nying'uro, Christoph Zellweger, and Martin Steinbacher
Atmos. Chem. Phys., 26, 6741–6762, https://doi.org/10.5194/acp-26-6741-2026, https://doi.org/10.5194/acp-26-6741-2026, 2026
Short summary
Short summary
Long-term atmospheric measurements are crucial to understanding climate change but remain scarce across Africa. We monitored atmospheric species at Mt. Kenya from 2020 to 2024. Our data reveal equatorial seasonal and daily variability and show that models miss local patterns. Emissions at Mt. Kenya mainly come from households, industry, and agriculture, though with large uncertainties. These findings stress the need for more ground stations to improve climate models and emission estimates.
Noémy Chénier, Paul M. Magyar, Jakob Zopfi, Claudia Frey, Thomas Kuhn, Moritz F. Lehmann, and Joachim Mohn
EGUsphere, https://doi.org/10.5194/egusphere-2026-1824, https://doi.org/10.5194/egusphere-2026-1824, 2026
Short summary
Short summary
N₂O is a greenhouse gas produced by microbes during nitrogen cycling. We studied two bacterial species and found that the isotope signatures of the N₂O they produced changed strongly depending on growth conditions and cell activity. Early during growth, the distribution of N isotopes within the N₂O molecule also changed unexpectedly. These results show that N₂O isotope signatures are more variable than previously assumed and depend strongly on physiology.
Paul M. Magyar, Nico Kueter, Simone Brunamonti, Naizhong Zhang, Ivan Prokhorov, Noémy Chénier, Lukas Emmenegger, Béla Tuzson, and Joachim Mohn
EGUsphere, https://doi.org/10.5194/egusphere-2026-874, https://doi.org/10.5194/egusphere-2026-874, 2026
Short summary
Short summary
Human activity drives increases in atmospheric nitrous oxide. Stable isotopes help trace the pathways involved. We developed a reliable way to calibrate measurements of rare isotopic variants of nitrous oxide so results from different labs can be compared. By heating nitrous oxide with a catalyst, the molecules reach well-defined equilibrium patterns suitable as a reference. To measure these isotopic variants quickly and precisely, we improved a laser-based measurement approach.
Alice Emily Ramsden, Anita Ganesan, Matthew Rigby, Chris Rennick, Tim Arnold, Emmal Safi, Edward Chung, Dafina Kikaj, Cameron Yeo, Dave Lowry, Pete Levy, Simon O'Doherty, Kieran Stanley, Dickon Young, Joe Pitt, Damien Martin, Morgan Lopez, Michel Ramonet, Grant Forster, Arnoud Frumau, and Alistair Manning
EGUsphere, https://doi.org/10.5194/egusphere-2026-779, https://doi.org/10.5194/egusphere-2026-779, 2026
Short summary
Short summary
Methane is emitted from a range of anthropogenic and natural sources, each with a characteristic isotope ratio signature. We present a method for estimating emissions from multiple sources using isotopic signatures and observations of atmospheric methane isotope ratios. We show the importance of considering isotopic signature uncertainty and demonstrate how our current understanding of these signatures may be limiting this method’s ability to reduce uncertainties in emissions estimates.
Hannes Keck, Laurence Strubbe, Paul M. Magyar, Adriano Joss, Andreas Froemelt, André Kupferschmid, Klaus-Holger Knorr, and Joachim Mohn
EGUsphere, https://doi.org/10.5194/egusphere-2026-857, https://doi.org/10.5194/egusphere-2026-857, 2026
Short summary
Short summary
We monitored nitrous oxide in a pilot wastewater treatment plant in real time to understand how microbes produce and remove this greenhouse gas. We designed and tested a laser-based analytical setup, with which we were able to show that denitrification is the main source of nitrous oxide emissions and that low oxygen concentrations enhances nitrous oxide removal. Our approach offers a new way to monitor the wastewater treatment processes and to cut climate-relevant nitrous oxide emissions.
Benjamin Püschel, Martin Vojta, Luise Kandler, Molly Crotwell, Andreas Engel, Paul B. Krummel, Chris R. Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Thomas Wagenhäuser, Ray F. Weiss, Dickon Young, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2025-5656, https://doi.org/10.5194/egusphere-2025-5656, 2025
Short summary
Short summary
We present global and regionally resolved emissions of the two highly potent greenhouse gases CF4 and C2F6 from 2006 to 2023, based on atmospheric measurements and transport modeling. In nearly all regions studied, our results show that national reports and industry-based data underestimate emissions. While emissions in Europe and the U.S. declined, we find rising emissions in South, Southeast, and East Asia. China and India are the major contributors to global emissions in recent years.
Luke M. Western, Stephen Bourguet, Molly Crotwell, Lei Hu, Paul B. Krummel, Hélène De Longueville, Alistair J. Manning, Jens Mühle, Dominique Rust, Isaac Vimont, Martin K. Vollmer, Minde An, Jgor Arduini, Andreas Engel, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Chris Lunder, Michela Maione, Stephen A. Montzka, David Nance, Simon O'Doherty, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Roland Schmidt, Kieran M. Stanley, Thomas Wagenhäuser, Dickon Young, Matt Rigby, Ronald G. Prinn, and Ray F. Weiss
Atmos. Chem. Phys., 25, 17761–17778, https://doi.org/10.5194/acp-25-17761-2025, https://doi.org/10.5194/acp-25-17761-2025, 2025
Short summary
Short summary
We used atmospheric measurements to estimate emissions of two hydrochlorofluorocarbon (HCFC) gases, called HCFC-123 and HCFC-124, that harm the ozone layer. Despite international regulation to stop their production, their emissions have not fallen. This may be linked to how they are used to make other chemicals. Our findings show that some banned substances are still reaching the atmosphere, likely through leaks during chemical production, which could slow the recovery of the ozone layer.
Luke M. Western, Matthew Rigby, Jens Mühle, Paul B. Krummel, Chris R. Lunder, Simon O'Doherty, Stefan Reimann, Martin K. Vollmer, Dickon Young, Ben Adam, Paul J. Fraser, Anita L. Ganesan, Christina M. Harth, Ove Hermansen, Jooil Kim, Ray L. Langenfelds, Zoë M. Loh, Blagoj Mitrevski, Joseph R. Pitt, Peter K. Salameh, Roland Schmidt, Kieran Stanley, Ann R. Stavert, Hsiang-Jui Wang, Ray F. Weiss, and Ronald G. Prinn
Earth Syst. Sci. Data, 17, 6557–6582, https://doi.org/10.5194/essd-17-6557-2025, https://doi.org/10.5194/essd-17-6557-2025, 2025
Short summary
Short summary
We used global measurements and an atmospheric model to estimate how emissions and abundances of 42 chemically and radiatively important trace gases have changed over time. These gases affect the Earth's radiative balance and the ozone layer. Our data sets help track progress in reducing emissions of these gases to the atmosphere. This work supports international efforts to protect the environment by providing clear, long-term, consistent data on how these gases are changing in the atmosphere.
Martin Vojta, Andreas Plach, Rona L. Thompson, Pallav Purohit, Kieran Stanley, Simon O'Doherty, Dickon Young, Joe Pitt, Jgor Arduini, Xin Lan, and Andreas Stohl
Atmos. Chem. Phys., 25, 15197–15243, https://doi.org/10.5194/acp-25-15197-2025, https://doi.org/10.5194/acp-25-15197-2025, 2025
Short summary
Short summary
We determine European emissions of the highly potent greenhouse gas sulfur hexafluoride from 2005 to 2021 – focusing on high-emitting countries and the aggregated EU-27 emissions. Emissions declined in most regions, likely due to EU F-gas regulations. However, our results reveal that most studied countries underestimate their emissions in their national reports. Our sensitivity tests highlight the importance of dense observational networks for reliable inversion-based emission estimates.
Kirstin Gerrand, Elena Fillola, Alistair J. Manning, Jgor Arduini, Paul B. Krummel, Chris R. Lunder, Jens Mühle, Simon O'Doherty, Sunyoung Park, Ronald G. Prinn, Stefan Reimann, Dickon Young, and Matthew Rigby
EGUsphere, https://doi.org/10.5194/egusphere-2025-4137, https://doi.org/10.5194/egusphere-2025-4137, 2025
Short summary
Short summary
To analyse long-term trends in atmospheric trace gas concentrations, it is important to identify data points minimally affected by local pollution sources or air masses carried from other latitudes or altitudes. Traditional methods for detecting these “baselines” are computationally expensive or lack a basis in physical principles. This paper introduces a machine-learning method that uses meteorological data and offers significantly lower computational costs compared to physics-based techniques.
Antti Laitinen, Hermanni Aaltonen, Christoph Zellweger, Aki Tsuruta, Tuula Aalto, and Juha Hatakka
Atmos. Meas. Tech., 18, 3109–3133, https://doi.org/10.5194/amt-18-3109-2025, https://doi.org/10.5194/amt-18-3109-2025, 2025
Short summary
Short summary
This paper presents long-term observations of atmospheric CO2 and CH4 mole fractions and a comparison of two permanent and two mobile measurement systems located in Northern Finland. Furthermore, the observed mole fractions are compared against the mean marine boundary layer product for the Northern Hemisphere. The comparisons of all the systems show good agreement in relation to the World Meteorological Organization/Global Atmosphere Watch network compatibility goal limits for CO2 and CH4.
Dafina Kikaj, Edward Chung, Alan D. Griffiths, Scott D. Chambers, Grant Forster, Angelina Wenger, Penelope Pickers, Chris Rennick, Simon O'Doherty, Joseph Pitt, Kieran Stanley, Dickon Young, Leigh S. Fleming, Karina Adcock, Emmal Safi, and Tim Arnold
Atmos. Meas. Tech., 18, 151–175, https://doi.org/10.5194/amt-18-151-2025, https://doi.org/10.5194/amt-18-151-2025, 2025
Short summary
Short summary
We present a protocol to improve confidence in atmospheric radon measurements, enabling site comparisons and integration with greenhouse gas data. As a natural tracer, radon provides an independent check of transport model performance. This standardized method enhances radon’s use as a metric for model evaluation. Beyond UK observatories, it can support broader networks like ICOS and WMO/GAW, advancing global atmospheric research.
Emily Dowd, Alistair J. Manning, Bryn Orth-Lashley, Marianne Girard, James France, Rebecca E. Fisher, Dave Lowry, Mathias Lanoisellé, Joseph R. Pitt, Kieran M. Stanley, Simon O'Doherty, Dickon Young, Glen Thistlethwaite, Martyn P. Chipperfield, Emanuel Gloor, and Chris Wilson
Atmos. Meas. Tech., 17, 1599–1615, https://doi.org/10.5194/amt-17-1599-2024, https://doi.org/10.5194/amt-17-1599-2024, 2024
Short summary
Short summary
We provide the first validation of the satellite-derived emission estimates using surface-based mobile greenhouse gas surveys of an active gas leak detected near Cheltenham, UK. GHGSat’s emission estimates broadly agree with the surface-based mobile survey and steps were taken to fix the leak, highlighting the importance of satellite data in identifying emissions and helping to reduce our human impact on climate change.
Rona L. Thompson, Stephen A. Montzka, Martin K. Vollmer, Jgor Arduini, Molly Crotwell, Paul B. Krummel, Chris Lunder, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Stefan Reimann, Isaac Vimont, Hsiang Wang, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 24, 1415–1427, https://doi.org/10.5194/acp-24-1415-2024, https://doi.org/10.5194/acp-24-1415-2024, 2024
Short summary
Short summary
The hydroxyl radical determines the atmospheric lifetimes of numerous species including methane. Since OH is very short-lived, it is not possible to directly measure its concentration on scales relevant for understanding its effect on other species. Here, OH is inferred by looking at changes in hydrofluorocarbons (HFCs). We find that OH levels have been fairly stable over our study period (2004 to 2021), suggesting that OH is not the main driver of the recent increase in atmospheric methane.
Leonard Kirago, Örjan Gustafsson, Samuel Mwaniki Gaita, Sophie L. Haslett, Michael J. Gatari, Maria Elena Popa, Thomas Röckmann, Christoph Zellweger, Martin Steinbacher, Jörg Klausen, Christian Félix, David Njiru, and August Andersson
Atmos. Chem. Phys., 23, 14349–14357, https://doi.org/10.5194/acp-23-14349-2023, https://doi.org/10.5194/acp-23-14349-2023, 2023
Short summary
Short summary
This study provides ground-observational evidence that supports earlier suggestions that savanna fires are the main emitters and modulators of carbon monoxide gas in Africa. Using isotope-based techniques, the study has shown that about two-thirds of this gas is emitted from savanna fires, while for urban areas, in this case Nairobi, primary sources approach 100 %. The latter has implications for air quality policy, suggesting primary emissions such as traffic should be targeted.
Ioannis Katharopoulos, Dominique Rust, Martin K. Vollmer, Dominik Brunner, Stefan Reimann, Simon J. O'Doherty, Dickon Young, Kieran M. Stanley, Tanja Schuck, Jgor Arduini, Lukas Emmenegger, and Stephan Henne
Atmos. Chem. Phys., 23, 14159–14186, https://doi.org/10.5194/acp-23-14159-2023, https://doi.org/10.5194/acp-23-14159-2023, 2023
Short summary
Short summary
The effectiveness of climate change mitigation needs to be scrutinized by monitoring greenhouse gas (GHG) emissions. Countries report their emissions to the UN in a bottom-up manner. By combining atmospheric observations and transport models someone can independently validate emission estimates in a top-down fashion. We report Swiss emissions of synthetic GHGs based on kilometer-scale transport and inverse modeling, highlighting the role of appropriate resolution in complex terrain.
Hyeri Park, Jooil Kim, Haklim Choi, Sohyeon Geum, Yeaseul Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Kieran M. Stanley, Simon O'Doherty, Paul J. Fraser, Peter G. Simmonds, Paul B. Krummel, Ray F. Weiss, Ronald G. Prinn, and Sunyoung Park
Atmos. Chem. Phys., 23, 9401–9411, https://doi.org/10.5194/acp-23-9401-2023, https://doi.org/10.5194/acp-23-9401-2023, 2023
Short summary
Short summary
Based on atmospheric HFC-23 observations, the first estimate of post-CDM HFC-23 emissions in eastern Asia for 2008–2019 shows that these emissions contribute significantly to the global emissions rise. The observation-derived emissions were much larger than the bottom-up estimates expected to approach zero after 2015 due to national abatement activities. These discrepancies could be attributed to unsuccessful factory-level HFC-23 abatement and inaccurate quantification of emission reductions.
Alison L. Redington, Alistair J. Manning, Stephan Henne, Francesco Graziosi, Luke M. Western, Jgor Arduini, Anita L. Ganesan, Christina M. Harth, Michela Maione, Jens Mühle, Simon O'Doherty, Joseph Pitt, Stefan Reimann, Matthew Rigby, Peter K. Salameh, Peter G. Simmonds, T. Gerard Spain, Kieran Stanley, Martin K. Vollmer, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 23, 7383–7398, https://doi.org/10.5194/acp-23-7383-2023, https://doi.org/10.5194/acp-23-7383-2023, 2023
Short summary
Short summary
Chlorofluorocarbons (CFCs) were used in Europe pre-1990, damaging the stratospheric ozone layer. Legislation has controlled production and use, and global emissions have decreased sharply. The global rate of decline in CFC-11 recently slowed and was partly attributed to illegal emission in eastern China. This study concludes that emissions of CFC-11 in western Europe have not contributed to the unexplained part of the global increase in CFC-11 observed in the last decade.
Elena Fillola, Raul Santos-Rodriguez, Alistair Manning, Simon O'Doherty, and Matt Rigby
Geosci. Model Dev., 16, 1997–2009, https://doi.org/10.5194/gmd-16-1997-2023, https://doi.org/10.5194/gmd-16-1997-2023, 2023
Short summary
Short summary
Lagrangian particle dispersion models are used extensively for the estimation of greenhouse gas (GHG) fluxes using atmospheric observations. However, these models do not scale well as data volumes increase. Here, we develop a proof-of-concept machine learning emulator that can produce outputs similar to those of the dispersion model, but 50 000 times faster, using only meteorological inputs. This works demonstrates the potential of machine learning to accelerate GHG estimations across the globe.
David R. Worton, Sergi Moreno, Kieran O'Daly, and Rupert Holzinger
Atmos. Meas. Tech., 16, 1061–1072, https://doi.org/10.5194/amt-16-1061-2023, https://doi.org/10.5194/amt-16-1061-2023, 2023
Short summary
Short summary
Proton-transfer-reaction mass spectrometry is widely used in the environmental, health, and food and beverage sectors. As a result, there is a need for accurate and comparable measurements. In this work we have developed a 20-component gravimetrically prepared traceable primary reference material (gas standard in a high-pressure cylinder) to enable quantitative and comparable measurements. The accuracy of all components was better than 3 %–10 % with stabilities of better than 1–2 years.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O'Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys., 22, 13243–13268, https://doi.org/10.5194/acp-22-13243-2022, https://doi.org/10.5194/acp-22-13243-2022, 2022
Short summary
Short summary
We present a novel high-resolution inverse modelling system, "FLEXVAR", and its application for the inverse modelling of European CH4 emissions in 2018. The new system combines a high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows CH4 emissions to be optimized from individual model grid cells. The high resolution allows the observations to be better reproduced, while the derived emissions show overall good consistency with two existing models.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
Atmos. Chem. Phys., 22, 12945–12960, https://doi.org/10.5194/acp-22-12945-2022, https://doi.org/10.5194/acp-22-12945-2022, 2022
Short summary
Short summary
Nitrous oxide is a potent greenhouse gas and ozone-depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions over 2011–2020, which are mainly driven by emissions between 0° and 30°N, with the highest emissions recorded in 2020.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
Short summary
Short summary
The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
Short summary
Short summary
The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Haklim Choi, Mi-Kyung Park, Paul J. Fraser, Hyeri Park, Sohyeon Geum, Jens Mühle, Jooil Kim, Ian Porter, Peter K. Salameh, Christina M. Harth, Bronwyn L. Dunse, Paul B. Krummel, Ray F. Weiss, Simon O'Doherty, Dickon Young, and Sunyoung Park
Atmos. Chem. Phys., 22, 5157–5173, https://doi.org/10.5194/acp-22-5157-2022, https://doi.org/10.5194/acp-22-5157-2022, 2022
Short summary
Short summary
We observed 12-year continuous CH3Br pollution signals at Gosan and estimated anthropogenic CH3Br emissions in eastern China. The analysis revealed a significant discrepancy between top-down estimates and the bottom-up emissions from the fumigation usage reported to the United Nations Environment Programme, likely due to unreported or inaccurately reported fumigation usage. This result provides information to monitor international compliance with the Montreal Protocol.
Alice E. Ramsden, Anita L. Ganesan, Luke M. Western, Matthew Rigby, Alistair J. Manning, Amy Foulds, James L. France, Patrick Barker, Peter Levy, Daniel Say, Adam Wisher, Tim Arnold, Chris Rennick, Kieran M. Stanley, Dickon Young, and Simon O'Doherty
Atmos. Chem. Phys., 22, 3911–3929, https://doi.org/10.5194/acp-22-3911-2022, https://doi.org/10.5194/acp-22-3911-2022, 2022
Short summary
Short summary
Quantifying methane emissions from different sources is a key focus of current research. We present a method for estimating sectoral methane emissions that uses ethane as a tracer for fossil fuel methane. By incorporating variable ethane : methane emission ratios into this model, we produce emissions estimates with improved uncertainty characterisation. This method will be particularly useful for studying methane emissions in areas with complex distributions of sources.
Jens Mühle, Lambert J. M. Kuijpers, Kieran M. Stanley, Matthew Rigby, Luke M. Western, Jooil Kim, Sunyoung Park, Christina M. Harth, Paul B. Krummel, Paul J. Fraser, Simon O'Doherty, Peter K. Salameh, Roland Schmidt, Dickon Young, Ronald G. Prinn, Ray H. J. Wang, and Ray F. Weiss
Atmos. Chem. Phys., 22, 3371–3378, https://doi.org/10.5194/acp-22-3371-2022, https://doi.org/10.5194/acp-22-3371-2022, 2022
Short summary
Short summary
Emissions of the strong greenhouse gas perfluorocyclobutane (c-C4F8) into the atmosphere have been increasing sharply since the early 2000s. These c-C4F8 emissions are highly correlated with the amount of hydrochlorofluorocarbon-22 produced to synthesize polytetrafluoroethylene (known for its non-stick properties) and related chemicals. From this process, c-C4F8 by-product is vented to the atmosphere. Avoiding these unnecessary c-C4F8 emissions could reduce the climate impact of this industry.
Dominique Rust, Ioannis Katharopoulos, Martin K. Vollmer, Stephan Henne, Simon O'Doherty, Daniel Say, Lukas Emmenegger, Renato Zenobi, and Stefan Reimann
Atmos. Chem. Phys., 22, 2447–2466, https://doi.org/10.5194/acp-22-2447-2022, https://doi.org/10.5194/acp-22-2447-2022, 2022
Short summary
Short summary
Artificial halocarbons contribute to ozone layer depletion and to global warming. We measured the atmospheric concentrations of halocarbons at the Beromünster tower, modelled the Swiss emissions, and compared the results to the internationally reported Swiss emissions inventory. For most of the halocarbons, we found good agreement, whereas one refrigerant might be overestimated in the inventory. In addition, we present first emission estimates of the newest types of halocarbons.
Mark F. Lunt, Alistair J. Manning, Grant Allen, Tim Arnold, Stéphane J.-B. Bauguitte, Hartmut Boesch, Anita L. Ganesan, Aoife Grant, Carole Helfter, Eiko Nemitz, Simon J. O'Doherty, Paul I. Palmer, Joseph R. Pitt, Chris Rennick, Daniel Say, Kieran M. Stanley, Ann R. Stavert, Dickon Young, and Matt Rigby
Atmos. Chem. Phys., 21, 16257–16276, https://doi.org/10.5194/acp-21-16257-2021, https://doi.org/10.5194/acp-21-16257-2021, 2021
Short summary
Short summary
We present an evaluation of the UK's methane emissions between 2013 and 2020 using a network of tall tower measurement sites. We find emissions that are consistent in both magnitude and trend with the UK's reported emissions, with a declining trend driven by a decrease in emissions from England. The impact of various components of the modelling set-up on these findings are explored through a number of sensitivity studies.
Alistair J. Manning, Alison L. Redington, Daniel Say, Simon O'Doherty, Dickon Young, Peter G. Simmonds, Martin K. Vollmer, Jens Mühle, Jgor Arduini, Gerard Spain, Adam Wisher, Michela Maione, Tanja J. Schuck, Kieran Stanley, Stefan Reimann, Andreas Engel, Paul B. Krummel, Paul J. Fraser, Christina M. Harth, Peter K. Salameh, Ray F. Weiss, Ray Gluckman, Peter N. Brown, John D. Watterson, and Tim Arnold
Atmos. Chem. Phys., 21, 12739–12755, https://doi.org/10.5194/acp-21-12739-2021, https://doi.org/10.5194/acp-21-12739-2021, 2021
Short summary
Short summary
This paper estimates UK emissions of important greenhouse gases (hydrofluorocarbons (HFCs)) using high-quality atmospheric observations and atmospheric modelling. We compare these estimates with those submitted by the UK to the United Nations. We conclude that global concentrations of these gases are still increasing. Our estimates for the UK are 73 % of those reported and that the UK emissions are now falling, demonstrating an impact of UK government policy.
Cited articles
BIPM, IEC, IFCC, ILAC, ISO, IUPAC, IUPAP, and OIML: Evaluation of measurement data – guide to the expression of uncertainty in measurement, International Bureau of Weights and Measures/Bureau International des Poids et Measures, Working group 1 of the Joint Committee for Guides in Metrology (JCGM 100: 2008, GUM 1995 with minor corrections), available at: http://www.bipm.org/utils/common/documents/jcgm/JCGM 100 2008 E.pdf (last access: 20 January 2021), 2008.
Brewer, P. J., Brown, R. J., Mussell Webber, E. B., van Aswegen, S., Ward,
M. K., Hill-Pearce, R. E., and Worton, D. R.: Breakthrough in Negating the
Impact of Adsorption in Gas Reference Materials, Anal. Chem., 91,
5310–5315, https://doi.org/10.1021/acs.analchem.9b00175, 2019a.
Brewer, P. J., Kim, J. S., Lee, S., Tarasova, O. A., Viallon, J., Flores,
E., Wielgosz, R. I., Shimosaka, T., Assonov, S., and Allison, C. E.:
Advances in reference materials and measurement techniques for greenhouse
gas atmospheric observations, Metrologia, 56, 034006,
https://doi.org/10.1088/1681-7575/ab1506, 2019b.
Brown, A.: GravCalc2 (version 2.3.0) User Guide, National Physical
Laboratory (NPL), Teddington, UK, 2009.
Denk, T. R., Mohn, J., Decock, C., Lewicka-Szczebak, D., Harris, E.,
Butterbach-Bahl, K., Kiese, R., and Wolf, B.: The nitrogen cycle: A review
of isotope effects and isotope modeling approaches, Soil Biol.
Biochem., 105, 121–137, https://doi.org/10.1016/j.soilbio.2016.11.015, 2017.
Erler, D. V., Duncan, T., Murray, R., Maher, D. T., Santos, I. R., Gatland,
J., Mangion, P., and Eyre, B. D.: Applying cavity ring-down spectroscopy for
the measurement of dissolved nitrous oxide concentrations and bulk nitrogen
isotopic composition in aquatic systems: Correcting for interferences and
field application, Limnol. Oceanogr.-Meth., 13, 391–401,
https://doi.org/10.1002/lom3.10032, 2015.
Flores, E., Viallon, J., Moussay, P., Griffith, D. W., and Wielgosz, R. I.:
Calibration strategies for FT-IR and other isotope ratio infrared
spectrometer instruments for accurate δ13C and δ18O measurements of CO2 in air, Anal. Chem., 89,
3648–3655, https://doi.org/10.1021/acs.analchem.6b05063, 2017.
Ganesan, A. L., Chatterjee, A., Prinn, R. G., Harth, C. M., Salameh, P. K., Manning, A. J., Hall, B. D., Mühle, J., Meredith, L. K., Weiss, R. F., O'Doherty, S., and Young, D.: The variability of methane, nitrous oxide and sulfur hexafluoride in Northeast India, Atmos. Chem. Phys., 13, 10633–10644, https://doi.org/10.5194/acp-13-10633-2013, 2013.
Griffith, D. W. T., Deutscher, N. M., Caldow, C., Kettlewell, G., Riggenbach, M., and Hammer, S.: A Fourier transform infrared trace gas and isotope analyser for atmospheric applications, Atmos. Meas. Tech., 5, 2481–2498, https://doi.org/10.5194/amt-5-2481-2012, 2012.
Hall, B., Dutton, G., and Elkins, J.: The NOAA nitrous oxide standard scale
for atmospheric observations, J. Geophys. Res.-Atmos.,
112, D09305, https://doi.org/10.1029/2006JD007954, 2007.
Harris, S. J., Liisberg, J., Xia, L., Wei, J., Zeyer, K., Yu, L., Barthel, M., Wolf, B., Kelly, B. F. J., Cendón, D. I., Blunier, T., Six, J., and Mohn, J.: N2O isotopocule measurements using laser spectroscopy: analyzer characterization and intercomparison, Atmos. Meas. Tech., 13, 2797–2831, https://doi.org/10.5194/amt-13-2797-2020, 2020.
Hill-Pearce, R. E., Resner, K. V., Worton, D. R., and Brewer, P. J.:
Synthetic Zero Air Reference Material for High Accuracy Greenhouse Gas
Measurements, Anal. Chem., 91, 1974–1979,
https://doi.org/10.1021/acs.analchem.8b04297, 2018.
ISO: 6142-1: Gas analysis-Preparation of calibration gas mixtures – Part 1:
Gravimetric method for Class I mixtures, Geneva, Switzerland, 2015.
Kantnerová, K., Tuzson, B., Emmenegger, L., Bernasconi, S. M., and Mohn,
J.: Quantifying isotopic signatures of N2O using quantum cascade laser
absorption spectroscopy, CHIMIA, 73,
232–238, https://doi.org/10.2533/chimia.2019.232, 2019.
Lewicka-Szczebak, D., Well, R., Köster, J. R., Fuß, R., Senbayram,
M., Dittert, K., and Flessa, H.: Experimental determinations of isotopic
fractionation factors associated with N2O production and reduction
during denitrification in soils, Geochim. Cosmochim. Ac., 134,
55–73, https://doi.org/10.1016/j.gca.2014.03.010, 2014.
Lim, J. S., Lee, J., Moon, D., Kim, J. S., Lee, J., and Hall, B. D.:
Gravimetric standard gas mixtures for global monitoring of atmospheric
SF6, Anal. Chem., 89, 12068–12075,
https://doi.org/10.1021/acs.analchem.7b02545, 2017.
Lopez, M., Schmidt, M., Ramonet, M., Bonne, J.-L., Colomb, A., Kazan, V., Laj, P., and Pichon, J.-M.: Three years of semicontinuous greenhouse gas measurements at the Puy de Dôme station (central France), Atmos. Meas. Tech., 8, 3941–3958, https://doi.org/10.5194/amt-8-3941-2015, 2015.
Lushozi, S., Tshilongo, J., and Chimuka, L.: Verification of nitrous oxide
primary standard gas mixtures by gas chromatography and cavity ring-down
spectroscopy for ambient measurements in South Africa, Accredit.
Qual. Assur., 24, 203–214, https://doi.org/10.1007/s00769-019-01375-x, 2019.
Mohn, J., Wolf, B., Toyoda, S., Lin, C. T., Liang, M. C., Brüggemann,
N., Wissel, H., Steiker, A. E., Dyckmans, J., and Szwec, L.: Interlaboratory
assessment of nitrous oxide isotopomer analysis by isotope ratio mass
spectrometry and laser spectroscopy: current status and perspectives, Rapid
Commun. Mass Sp., 28, 1995–2007, https://doi.org/10.1002/rcm.6982,
2014.
Myhre, G., Shindell, D., Bréon, F., Collins, W., Fuglestvedt, J., Huang,
J., Koch, D., Lamarque, J., Lee, D., and Mendoza, B.: Anthropogenic and
Natural Radiative Forcing, Climate Change 2013: The Physical Science Basis.
Contribution of Working Group I to the Fifth Assessment Report of the
Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S.
K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P. M., Cambridge University Press, Cambridge, UK and New York, NY, USA, 659–740,
https://doi.org/10.1017/CBO9781107415324.018, 2013.
Nara, H., Tanimoto, H., Tohjima, Y., Mukai, H., Nojiri, Y., Katsumata, K., and Rella, C. W.: Effect of air composition (N2, O2, Ar, and H2O) on CO2 and CH4 measurement by wavelength-scanned cavity ring-down spectroscopy: calibration and measurement strategy, Atmos. Meas. Tech., 5, 2689–2701, https://doi.org/10.5194/amt-5-2689-2012, 2012.
NOAA/ESRL: Nitrous oxide (N2O) WMO scale: https://www.esrl.noaa.gov/gmd/ccl/n2o_scale.html (last access: 21 December 2020), 2011.
Ostrom, N. E. and Ostrom, P. H.: Mining the isotopic complexity of nitrous
oxide: a review of challenges and opportunities, Biogeochemistry, 132,
359–372, https://doi.org/10.1007/s10533-017-0301-5, 2017.
Ostrom, N. E., Gandhi, H., Coplen, T. B., Toyoda, S., Böhlke, J. K.,
Brand, W. A., Casciotti, K. L., Dyckmans, J., Giesemann, A., and Mohn, J.:
Preliminary assessment of stable nitrogen and oxygen isotopic composition of
USGS51 and USGS52 nitrous oxide reference gases and perspectives on
calibration needs, Rapid Commun. Mass Sp., 32, 1207–1214,
https://doi.org/10.1002/rcm.8157, 2018.
Picarro: δ15N and δ18O Isotopic and Nitrous Oxide
Gas Concentration Analyzer, available at: https://www.picarro.com/support/library/documents/g5131i_analyzer_datasheet (last access: 20 January 2021), 2017.
Platonov, I., Rodinkov, O., Gorbacheva, A., Moskvin, L., and Kolesnichenko,
I.: Methods and devices for the preparation of standard gas mixtures,
J. Anal. Chem., 73, 109–127, https://doi.org/10.1134/S1061934818020090,
2018.
Snider, D. M., Venkiteswaran, J. J., Schiff, S. L., and Spoelstra, J.: From
the ground up: Global nitrous oxide sources are constrained by stable
isotope values, PloS one, 10, e0118954, https://doi.org/10.1371/journal.pone.0118954,
2015.
Tohjima, Y., Katsumata, K., Morino, I., Mukai, H., Machida, T., Akama, I.,
Amari, T., and Tsunogai, U.: Theoretical and experimental evaluation of the
isotope effect of NDIR analyzer on atmospheric CO2 measurement, J. Geophys. Res.-Atmos., 114, D13302, https://doi.org/10.1029/2009JD011734, 2009.
Toyoda, S. and Yoshida, N.: Determination of nitrogen isotopomers of nitrous
oxide on a modified isotope ratio mass spectrometer, Anal. Chem.,
71, 4711–4718, https://doi.org/10.1021/ac9904563, 1999.
Toyoda, S., Yoshida, N., and Koba, K.: Isotopocule analysis of biologically
produced nitrous oxide in various environments, Mass Spectrom. Rev.,
36, 135–160, https://doi.org/10.1002/mas.21459, 2017.
van der Schoot, M., Langenfelds, R., Fraser, P., Krummel, P., Ward, J., and
Somerville, N.: The WMO/GAW Cape Grim Baseline Air Pollution Station Air
Archive, Asia-Pacific GAW on Greenhouse Gases, Korea Metrological Administration (KMA), vol. 6. 13–20, 2015.
Winther, M., Balslev-Harder, D., Christensen, S., Priemé, A., Elberling, B., Crosson, E., and Blunier, T.: Continuous measurements of nitrous oxide isotopomers during incubation experiments, Biogeosciences, 15, 767–780, https://doi.org/10.5194/bg-15-767-2018, 2018.
WMO: 20th WMO/IAEA Meeting on Carbon Dioxide, Other Greenhouse Gases and
Related Tracers Measurement Techniques (GGMT-2019), World Meteorological
Organization, Geneva, Switzerland, 2019a.
WMO: Greenhouse Gas Bulletin (GHG Bulletin) – No. 15: The State of Greenhouse Gases in the Atmosphere Based on Global Observations through 2018,
World Meteorological Organization, Geneva, Switzerland, available at:
https://public.wmo.int/en/resources/library/wmo-greenhouse-gas-bulletin-no-15 (last access: 13 January 2021), 2019b.
WMO: Carbon dioxide levels continue at record levels, despite COVID-19
lockdown, available at: https://public.wmo.int/en/media/press-release/carbon-dioxide- levels-continue-record-levels-despite-covid-19-lockdown (last access: 13 January 2021), 2020.
Short summary
There is currently a need for gas reference materials with well-characterised delta values for monitoring N2O amount fractions. We present work towards the preparation of gas reference materials for calibration of in-field monitoring equipment, which target the WMO-GAW data quality objectives for comparability of amount fraction and demonstrate the stability of δ15Nα, δ15Nβ and δ18O values with pressure and effects of cylinder passivation.
There is currently a need for gas reference materials with well-characterised delta values for...
