Articles | Volume 18, issue 10
https://doi.org/10.5194/acp-18-7109-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
https://doi.org/10.5194/acp-18-7109-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
24 May 2018
Research article |
| 24 May 2018
| 24 May 2018
Global modelling of the total OH reactivity: investigations on the “missing” OH sink and its atmospheric implications
Valerio Ferracci
CORRESPONDING AUTHOR
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Lensfield Road, CB2 1EW, UK
now at: Centre for Environmental and Agricultural Informatics,
Cranfield University, College Road, MK43 0AL, UK
Ines Heimann
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Lensfield Road, CB2 1EW, UK
N. Luke Abraham
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Lensfield Road, CB2 1EW, UK
National Centre for Atmospheric Science, University of Cambridge,
Cambridge, UK
John A. Pyle
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Lensfield Road, CB2 1EW, UK
National Centre for Atmospheric Science, University of Cambridge,
Cambridge, UK
Alexander T. Archibald
Centre for Atmospheric Science, Department of Chemistry, University of
Cambridge, Lensfield Road, CB2 1EW, UK
National Centre for Atmospheric Science, University of Cambridge,
Cambridge, UK
Related authors
Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
Short summary
Short summary
The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
Short summary
Short summary
Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
Christa Fittschen, Mohamad Al Ajami, Sebastien Batut, Valerio Ferracci, Scott Archer-Nicholls, Alexander T. Archibald, and Coralie Schoemaecker
Atmos. Chem. Phys., 19, 349–362, https://doi.org/10.5194/acp-19-349-2019, https://doi.org/10.5194/acp-19-349-2019, 2019
Short summary
Short summary
Concentrations of OH, the main oxidant in the atmosphere, were measured in biogenic environments up to a factor of 10 higher than predicted by models. This was interpreted as a major lack in our understanding of biogenic volatile organic compound chemistry. But interferences of unknown origin have also been discovered, and we present experimental and modelling evidence that the interference might be due to the unexpected decomposition of a new class of molecule, ROOOH, in the FAGE instruments.
Paul T. Griffiths, Laura J. Wilcox, Robert J. Allen, Vaishali Naik, Fiona M. O'Connor, Michael J. Prather, Alexander T. Archibald, Florence Brown, Makoto Deushi, William Collins, Stephanie Fiedler, Naga Oshima, Lee T. Murray, Christopher J. Smith, Steven T. Turnock, Duncan Watson-Parris, and Paul J. Young
EGUsphere, https://doi.org/10.5194/egusphere-2024-2528, https://doi.org/10.5194/egusphere-2024-2528, 2024
Short summary
Short summary
The Aerosol Chemistry Model Intercomparison Project (AerChemMIP) aimed to quantify the climate and air quality impacts of aerosols and chemically reactive gases. In this paper, we review its contribution to AR6, and the wider understanding of the role of these species in climate and climate change. We identify remaining challenges concluding with recommendations aimed to improve the utility and uptake of climate model data to address the role of short-lived climate forcers in the Earth system.
Maria Rosa Russo, Sadie L. Bartholomew, David Hassell, Alex M. Mason, Erica Neininger, A. James Perman, David A. J. Sproson, Duncan Watson-Parris, and Nathan Luke Abraham
Geosci. Model Dev. Discuss., https://doi.org/10.5194/gmd-2024-73, https://doi.org/10.5194/gmd-2024-73, 2024
Revised manuscript accepted for GMD
Short summary
Short summary
Observational data and modelling capabilities are expanding in recent years, but there are still barriers preventing these two data sources to be used in synergy. Proper comparison requires generating, storing and handling a large amount of data. This manuscript describes the first step in the development of a new set of software tools, the ‘VISION toolkit’, which can enable the easy and efficient integration of observational and model data required for model evaluation.
Lauren R. Marshall, Anja Schmidt, Andrew P. Schurer, Nathan Luke Abraham, Lucie J. Lücke, Rob Wilson, Kevin Anchukaitis, Gabriele Hegerl, Ben Johnson, Bette L. Otto-Bliesner, Esther C. Brady, Myriam Khodri, and Kohei Yoshida
EGUsphere, https://doi.org/10.5194/egusphere-2024-1322, https://doi.org/10.5194/egusphere-2024-1322, 2024
Short summary
Short summary
Large volcanic eruptions have caused temperature deviations over the past 1000 years, however climate model results and reconstructions of surface cooling using tree-rings do not match. We explore this mismatch using the latest models and find a better match to tree-ring reconstructions for some eruptions. Our results show that the way in which eruptions are simulated in models matters for the comparison to tree-rings, particularly regarding the spatial spread of volcanic aerosol.
Lorrie Simone Denise Jacob, Chiara Giorio, and Alexander Thomas Archibald
Atmos. Chem. Phys., 24, 3329–3347, https://doi.org/10.5194/acp-24-3329-2024, https://doi.org/10.5194/acp-24-3329-2024, 2024
Short summary
Short summary
Recent studies on DMS have provided new challenges to our mechanistic understanding. Here we synthesise a number of recent studies to further develop and extend a state-of-the-art mechanism. Our new mechanism is shown to outperform all existing mechanisms when compared over a wide set of conditions. The development of an improved DMS mechanism will help lead the way to better the understanding the climate impacts of DMS emissions in past, present, and future atmospheric conditions.
Alexander T. Archibald, Bablu Sinha, Maria Russo, Emily Matthews, Freya Squires, N. Luke Abraham, Stephane Bauguitte, Thomas Bannan, Thomas Bell, David Berry, Lucy Carpenter, Hugh Coe, Andrew Coward, Peter Edwards, Daniel Feltham, Dwayne Heard, Jim Hopkins, James Keeble, Elizabeth C. Kent, Brian King, Isobel R. Lawrence, James Lee, Claire R. Macintosh, Alex Megann, Ben I. Moat, Katie Read, Chris Reed, Malcolm Roberts, Reinhard Schiemann, David Schroeder, Tim Smyth, Loren Temple, Navaneeth Thamban, Lisa Whalley, Simon Williams, Huihui Wu, and Ming-Xi Yang
Earth Syst. Sci. Data Discuss., https://doi.org/10.5194/essd-2023-405, https://doi.org/10.5194/essd-2023-405, 2024
Revised manuscript accepted for ESSD
Short summary
Short summary
Here we present an overview of the data generated as part of the North Atlantic Climate System Integrated Studies (ACSIS) programme which are available through dedicated repositories at the Centre for Environmental Data Analysis (CEDA, www.ceda.ac.uk) and the British Oceanographic Data Centre (BODC, bodc.ac.uk). ACSIS data cover the full North Atlantic System comprising: the North Atlantic Ocean, the atmosphere above it including its composition, Arctic Sea Ice and the Greenland Ice Sheet.
Yusuf A. Bhatti, Laura E. Revell, Alex J. Schuddeboom, Adrian J. McDonald, Alex T. Archibald, Jonny Williams, Abhijith U. Venugopal, Catherine Hardacre, and Erik Behrens
Atmos. Chem. Phys., 23, 15181–15196, https://doi.org/10.5194/acp-23-15181-2023, https://doi.org/10.5194/acp-23-15181-2023, 2023
Short summary
Short summary
Aerosols are a large source of uncertainty over the Southern Ocean. A dominant source of sulfate aerosol in this region is dimethyl sulfide (DMS), which is poorly simulated by climate models. We show the sensitivity of simulated atmospheric DMS to the choice of oceanic DMS data set and emission scheme. We show that oceanic DMS has twice the influence on atmospheric DMS than the emission scheme. Simulating DMS more accurately in climate models will help to constrain aerosol uncertainty.
Ben A. Cala, Scott Archer-Nicholls, James Weber, N. Luke Abraham, Paul T. Griffiths, Lorrie Jacob, Y. Matthew Shin, Laura E. Revell, Matthew Woodhouse, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 14735–14760, https://doi.org/10.5194/acp-23-14735-2023, https://doi.org/10.5194/acp-23-14735-2023, 2023
Short summary
Short summary
Dimethyl sulfide (DMS) is an important trace gas emitted from the ocean recognised as setting the sulfate aerosol background, but its oxidation is complex. As a result representation in chemistry-climate models is greatly simplified. We develop and compare a new mechanism to existing mechanisms via a series of global and box model experiments. Our studies show our updated DMS scheme is a significant improvement but significant variance exists between mechanisms.
Ewa M. Bednarz, Ryan Hossaini, N. Luke Abraham, and Martyn P. Chipperfield
Geosci. Model Dev., 16, 6187–6209, https://doi.org/10.5194/gmd-16-6187-2023, https://doi.org/10.5194/gmd-16-6187-2023, 2023
Short summary
Short summary
Development and performance of the new DEST chemistry scheme of UM–UKCA is described. The scheme extends the standard StratTrop scheme by including important updates to the halogen chemistry, thus allowing process-oriented studies of stratospheric ozone depletion and recovery, including impacts from both controlled long-lived ozone-depleting substances and emerging issues around uncontrolled, very short-lived substances. It will thus aid studies in support of future ozone assessment reports.
Nicola J. Warwick, Alex T. Archibald, Paul T. Griffiths, James Keeble, Fiona M. O'Connor, John A. Pyle, and Keith P. Shine
Atmos. Chem. Phys., 23, 13451–13467, https://doi.org/10.5194/acp-23-13451-2023, https://doi.org/10.5194/acp-23-13451-2023, 2023
Short summary
Short summary
A chemistry–climate model has been used to explore the atmospheric response to changes in emissions of hydrogen and other species associated with a shift from fossil fuel to hydrogen use. Leakage of hydrogen results in indirect global warming, offsetting greenhouse gas emission reductions from reduced fossil fuel use. To maximise the benefit of hydrogen as an energy source, hydrogen leakage and emissions of methane, carbon monoxide and nitrogen oxides should be minimised.
Maria Rosa Russo, Brian John Kerridge, Nathan Luke Abraham, James Keeble, Barry Graham Latter, Richard Siddans, James Weber, Paul Thomas Griffiths, John Adrian Pyle, and Alexander Thomas Archibald
Atmos. Chem. Phys., 23, 6169–6196, https://doi.org/10.5194/acp-23-6169-2023, https://doi.org/10.5194/acp-23-6169-2023, 2023
Short summary
Short summary
Tropospheric ozone is an important component of the Earth system as it can affect both climate and air quality. In this work we use observed tropospheric ozone derived from satellite observations and compare it to tropospheric ozone from model simulations. Our aim is to investigate recent changes (2005–2018) in tropospheric ozone in the North Atlantic region and to understand what factors are driving such changes.
Scott Archer-Nicholls, Rachel Allen, Nathan L. Abraham, Paul T. Griffiths, and Alex T. Archibald
Atmos. Chem. Phys., 23, 5801–5813, https://doi.org/10.5194/acp-23-5801-2023, https://doi.org/10.5194/acp-23-5801-2023, 2023
Short summary
Short summary
The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
Ernesto Reyes-Villegas, Douglas Lowe, Jill S. Johnson, Kenneth S. Carslaw, Eoghan Darbyshire, Michael Flynn, James D. Allan, Hugh Coe, Ying Chen, Oliver Wild, Scott Archer-Nicholls, Alex Archibald, Siddhartha Singh, Manish Shrivastava, Rahul A. Zaveri, Vikas Singh, Gufran Beig, Ranjeet Sokhi, and Gordon McFiggans
Atmos. Chem. Phys., 23, 5763–5782, https://doi.org/10.5194/acp-23-5763-2023, https://doi.org/10.5194/acp-23-5763-2023, 2023
Short summary
Short summary
Organic aerosols (OAs), their sources and their processes remain poorly understood. The volatility basis set (VBS) approach, implemented in air quality models such as WRF-Chem, can be a useful tool to describe primary OA (POA) production and aging. However, the main disadvantage is its complexity. We used a Gaussian process simulator to reproduce model results and to estimate the sources of model uncertainty. We do this by comparing the outputs with OA observations made at Delhi, India, in 2018.
Fouzia Fahrin, Daniel C. Jones, Yan Wu, James Keeble, and Alexander T. Archibald
Atmos. Chem. Phys., 23, 3609–3627, https://doi.org/10.5194/acp-23-3609-2023, https://doi.org/10.5194/acp-23-3609-2023, 2023
Short summary
Short summary
We use a machine learning technique called Gaussian mixture modeling (GMM) to classify vertical ozone profiles into groups based on how the ozone concentration changes with pressure. Even though the GMM algorithm was not provided with spatial information, the classes are geographically coherent. We also detect signatures of tropical broadening in UKESM1 future climate scenarios. GMM may be useful for understanding ozone structures in modeled and observed datasets.
Ewa M. Bednarz, Ryan Hossaini, Martyn P. Chipperfield, N. Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 22, 10657–10676, https://doi.org/10.5194/acp-22-10657-2022, https://doi.org/10.5194/acp-22-10657-2022, 2022
Short summary
Short summary
Atmospheric impacts of chlorinated very short-lived substances (Cl-VSLS) over the first two decades of the 21st century are assessed using the UM-UKCA chemistry–climate model. Stratospheric input of Cl from Cl-VSLS is estimated at ~130 ppt in 2019. The use of model set-up with constrained meteorology significantly increases the abundance of Cl-VSLS in the lower stratosphere relative to the free-running set-up. The growth in Cl-VSLS emissions significantly impacted recent HCl and COCl2 trends.
Le Yuan, Olalekan A. M. Popoola, Christina Hood, David Carruthers, Roderic L. Jones, Haitong Zhe Sun, Huan Liu, Qiang Zhang, and Alexander T. Archibald
Atmos. Chem. Phys., 22, 8617–8637, https://doi.org/10.5194/acp-22-8617-2022, https://doi.org/10.5194/acp-22-8617-2022, 2022
Short summary
Short summary
Emission estimates represent a major source of uncertainty in air quality modelling. We developed a novel approach to improve emission estimates from existing inventories using air quality models and routine in situ observations. Using this approach, we derived improved estimates of NOx emissions from the transport sector in Beijing in 2016. This approach has great potential in deriving timely updates of emissions for other pollutants, particularly in regions undergoing rapid emission changes.
Sebastian Landwehr, Michele Volpi, F. Alexander Haumann, Charlotte M. Robinson, Iris Thurnherr, Valerio Ferracci, Andrea Baccarini, Jenny Thomas, Irina Gorodetskaya, Christian Tatzelt, Silvia Henning, Rob L. Modini, Heather J. Forrer, Yajuan Lin, Nicolas Cassar, Rafel Simó, Christel Hassler, Alireza Moallemi, Sarah E. Fawcett, Neil Harris, Ruth Airs, Marzieh H. Derkani, Alberto Alberello, Alessandro Toffoli, Gang Chen, Pablo Rodríguez-Ros, Marina Zamanillo, Pau Cortés-Greus, Lei Xue, Conor G. Bolas, Katherine C. Leonard, Fernando Perez-Cruz, David Walton, and Julia Schmale
Earth Syst. Dynam., 12, 1295–1369, https://doi.org/10.5194/esd-12-1295-2021, https://doi.org/10.5194/esd-12-1295-2021, 2021
Short summary
Short summary
The Antarctic Circumnavigation Expedition surveyed a large number of variables describing the dynamic state of ocean and atmosphere, freshwater cycle, atmospheric chemistry, ocean biogeochemistry, and microbiology in the Southern Ocean. To reduce the dimensionality of the dataset, we apply a sparse principal component analysis and identify temporal patterns from diurnal to seasonal cycles, as well as geographical gradients and
hotspotsof interaction. Code and data are open access.
Anthony C. Jones, Adrian Hill, Samuel Remy, N. Luke Abraham, Mohit Dalvi, Catherine Hardacre, Alan J. Hewitt, Ben Johnson, Jane P. Mulcahy, and Steven T. Turnock
Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, https://doi.org/10.5194/acp-21-15901-2021, 2021
Short summary
Short summary
Ammonium nitrate is hard to model because it forms and evaporates rapidly. One approach is to relate its equilibrium concentration to temperature, humidity, and the amount of nitric acid and ammonia gases. Using this approach, we limit the rate at which equilibrium is reached using various condensation rates in a climate model. We show that ammonium nitrate concentrations are highly sensitive to the condensation rate. Our results will help improve the representation of nitrate in climate models.
James Weber, Scott Archer-Nicholls, Nathan Luke Abraham, Youngsub M. Shin, Thomas J. Bannan, Carl J. Percival, Asan Bacak, Paulo Artaxo, Michael Jenkin, M. Anwar H. Khan, Dudley E. Shallcross, Rebecca H. Schwantes, Jonathan Williams, and Alex T. Archibald
Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, https://doi.org/10.5194/gmd-14-5239-2021, 2021
Short summary
Short summary
The new mechanism CRI-Strat 2 features state-of-the-art isoprene chemistry not previously available in UKCA and improves UKCA's ability to reproduce observed concentrations of isoprene, monoterpenes, and OH in tropical regions. The enhanced ability to model isoprene, the most widely emitted non-methane volatile organic compound (VOC), will allow understanding of how isoprene and other biogenic VOCs affect atmospheric composition and, through biosphere–atmosphere feedbacks, climate change.
John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
Short summary
Short summary
Lightning-generated nitrogen oxides (LNOx) greatly influence tropospheric photochemistry. The most common parameterisation of lightning flash rate used to calculate LNOx in global composition models underestimates measurements over the ocean by a factor of 20–25. We formulate and validate an alternative parameterisation to remedy this problem. The new scheme causes an increase in the ozone burden by 8.5 % and the hydroxyl radical by 13 %, and these have implications for climate and air quality.
Ananth Ranjithkumar, Hamish Gordon, Christina Williamson, Andrew Rollins, Kirsty Pringle, Agnieszka Kupc, Nathan Luke Abraham, Charles Brock, and Ken Carslaw
Atmos. Chem. Phys., 21, 4979–5014, https://doi.org/10.5194/acp-21-4979-2021, https://doi.org/10.5194/acp-21-4979-2021, 2021
Short summary
Short summary
The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
Short summary
Short summary
We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
Short summary
Short summary
The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
Short summary
Short summary
This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126, https://doi.org/10.5194/acp-21-1105-2021, https://doi.org/10.5194/acp-21-1105-2021, 2021
Short summary
Short summary
We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
Short summary
Short summary
This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
James L. France, Prudence Bateson, Pamela Dominutti, Grant Allen, Stephen Andrews, Stephane Bauguitte, Max Coleman, Tom Lachlan-Cope, Rebecca E. Fisher, Langwen Huang, Anna E. Jones, James Lee, David Lowry, Joseph Pitt, Ruth Purvis, John Pyle, Jacob Shaw, Nicola Warwick, Alexandra Weiss, Shona Wilde, Jonathan Witherstone, and Stuart Young
Atmos. Meas. Tech., 14, 71–88, https://doi.org/10.5194/amt-14-71-2021, https://doi.org/10.5194/amt-14-71-2021, 2021
Short summary
Short summary
Measuring emission rates of methane from installations is tricky, and it is even more so when those installations are located offshore. Here, we show the aircraft set-up and demonstrate an effective methodology for surveying emissions from UK and Dutch offshore oil and gas installations. We present example data collected from two campaigns to demonstrate the challenges and solutions encountered during these surveys.
Jane P. Mulcahy, Colin Johnson, Colin G. Jones, Adam C. Povey, Catherine E. Scott, Alistair Sellar, Steven T. Turnock, Matthew T. Woodhouse, Nathan Luke Abraham, Martin B. Andrews, Nicolas Bellouin, Jo Browse, Ken S. Carslaw, Mohit Dalvi, Gerd A. Folberth, Matthew Glover, Daniel P. Grosvenor, Catherine Hardacre, Richard Hill, Ben Johnson, Andy Jones, Zak Kipling, Graham Mann, James Mollard, Fiona M. O'Connor, Julien Palmiéri, Carly Reddington, Steven T. Rumbold, Mark Richardson, Nick A. J. Schutgens, Philip Stier, Marc Stringer, Yongming Tang, Jeremy Walton, Stephanie Woodward, and Andrew Yool
Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, https://doi.org/10.5194/gmd-13-6383-2020, 2020
Short summary
Short summary
Aerosols are an important component of the Earth system. Here, we comprehensively document and evaluate the aerosol schemes as implemented in the physical and Earth system models, HadGEM3-GC3.1 and UKESM1. This study provides a useful characterisation of the aerosol climatology in both models, facilitating the understanding of the numerous aerosol–climate interaction studies that will be conducted for CMIP6 and beyond.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
Short summary
Short summary
We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
Short summary
Short summary
Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
Short summary
Short summary
Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Matt Amos, Paul J. Young, J. Scott Hosking, Jean-François Lamarque, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Ole Kirner, Markus Kunze, Marion Marchand, David A. Plummer, David Saint-Martin, Kengo Sudo, Simone Tilmes, and Yousuke Yamashita
Atmos. Chem. Phys., 20, 9961–9977, https://doi.org/10.5194/acp-20-9961-2020, https://doi.org/10.5194/acp-20-9961-2020, 2020
Short summary
Short summary
We present an updated projection of Antarctic ozone hole recovery using an ensemble of chemistry–climate models. To do so, we employ a method, more advanced and skilful than the current multi-model mean standard, which is applicable to other ensemble analyses. It calculates the performance and similarity of the models, which we then use to weight the model. Calculating model similarity allows us to account for models which are constructed from similar components.
James Keeble, N. Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Paul T. Griffiths, and John A. Pyle
Atmos. Chem. Phys., 20, 7153–7166, https://doi.org/10.5194/acp-20-7153-2020, https://doi.org/10.5194/acp-20-7153-2020, 2020
Short summary
Short summary
The Montreal Protocol was agreed in 1987 to limit and then stop the production of man-made CFCs, which destroy stratospheric ozone. As a result, the atmospheric abundances of CFCs are now declining in the atmosphere. However, the atmospheric abundance of CFC-11 is not declining as expected under complete compliance with the Montreal Protocol. Using the UM-UKCA chemistry–climate model, we explore the impact of future unregulated production of CFC-11 on ozone recovery.
Clara Orbe, David A. Plummer, Darryn W. Waugh, Huang Yang, Patrick Jöckel, Douglas E. Kinnison, Beatrice Josse, Virginie Marecal, Makoto Deushi, Nathan Luke Abraham, Alexander T. Archibald, Martyn P. Chipperfield, Sandip Dhomse, Wuhu Feng, and Slimane Bekki
Atmos. Chem. Phys., 20, 3809–3840, https://doi.org/10.5194/acp-20-3809-2020, https://doi.org/10.5194/acp-20-3809-2020, 2020
Short summary
Short summary
Atmospheric composition is strongly influenced by global-scale winds that are not always properly simulated in computer models. A common approach to correct for this bias is to relax or
nudgeto the observed winds. Here we systematically evaluate how well this technique performs across a large suite of chemistry–climate models in terms of its ability to reproduce key aspects of both the tropospheric and stratospheric circulations.
Alexander T. Archibald, Fiona M. O'Connor, Nathan Luke Abraham, Scott Archer-Nicholls, Martyn P. Chipperfield, Mohit Dalvi, Gerd A. Folberth, Fraser Dennison, Sandip S. Dhomse, Paul T. Griffiths, Catherine Hardacre, Alan J. Hewitt, Richard S. Hill, Colin E. Johnson, James Keeble, Marcus O. Köhler, Olaf Morgenstern, Jane P. Mulcahy, Carlos Ordóñez, Richard J. Pope, Steven T. Rumbold, Maria R. Russo, Nicholas H. Savage, Alistair Sellar, Marc Stringer, Steven T. Turnock, Oliver Wild, and Guang Zeng
Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, https://doi.org/10.5194/gmd-13-1223-2020, 2020
Short summary
Short summary
Here we present a description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in the UK Earth System Model (UKESM1). UKCA StratTrop represents a substantial step forward compared to previous versions of UKCA. We show here that it is fully suited to the challenges of representing interactions in a coupled Earth system model and identify key areas and components for future development that will make it even better in the future.
Conor G. Bolas, Valerio Ferracci, Andrew D. Robinson, Mohammed I. Mead, Mohd Shahrul Mohd Nadzir, John A. Pyle, Roderic L. Jones, and Neil R. P. Harris
Atmos. Meas. Tech., 13, 821–838, https://doi.org/10.5194/amt-13-821-2020, https://doi.org/10.5194/amt-13-821-2020, 2020
Short summary
Short summary
Here we present the iDirac, a new instrument capable of making isoprene measurements in remote and challenging environments. The iDirac is a customisable and rugged field instrument for investigating emissions of volatile organic compounds from vegetation. It has been tested here in a series of experiments to ensure a high degree of technical precision, accuracy and repeatability. This new instrument allows us to ask and answer new questions about the influence of vegetation on the atmosphere.
Ying Chen, Oliver Wild, Edmund Ryan, Saroj Kumar Sahu, Douglas Lowe, Scott Archer-Nicholls, Yu Wang, Gordon McFiggans, Tabish Ansari, Vikas Singh, Ranjeet S. Sokhi, Alex Archibald, and Gufran Beig
Atmos. Chem. Phys., 20, 499–514, https://doi.org/10.5194/acp-20-499-2020, https://doi.org/10.5194/acp-20-499-2020, 2020
Short summary
Short summary
PM2.5 and O3 are two major air pollutants. Some mitigation strategies focusing on reducing PM2.5 may lead to substantial increase in O3. We use statistical emulation combined with atmospheric transport model to perform thousands of sensitivity numerical studies to identify the major sources of PM2.5 and O3 and to develop strategies targeted at both pollutants. Our scientific evidence suggests that regional coordinated emission control is required to mitigate PM2.5 whilst preventing O3 increase.
Yuanhong Zhao, Marielle Saunois, Philippe Bousquet, Xin Lin, Antoine Berchet, Michaela I. Hegglin, Josep G. Canadell, Robert B. Jackson, Didier A. Hauglustaine, Sophie Szopa, Ann R. Stavert, Nathan Luke Abraham, Alex T. Archibald, Slimane Bekki, Makoto Deushi, Patrick Jöckel, Béatrice Josse, Douglas Kinnison, Ole Kirner, Virginie Marécal, Fiona M. O'Connor, David A. Plummer, Laura E. Revell, Eugene Rozanov, Andrea Stenke, Sarah Strode, Simone Tilmes, Edward J. Dlugokencky, and Bo Zheng
Atmos. Chem. Phys., 19, 13701–13723, https://doi.org/10.5194/acp-19-13701-2019, https://doi.org/10.5194/acp-19-13701-2019, 2019
Short summary
Short summary
The role of hydroxyl radical changes in methane trends is debated, hindering our understanding of the methane cycle. This study quantifies how uncertainties in the hydroxyl radical may influence methane abundance in the atmosphere based on the inter-model comparison of hydroxyl radical fields and model simulations of CH4 abundance with different hydroxyl radical scenarios during 2000–2016. We show that hydroxyl radical changes could contribute up to 54 % of model-simulated methane biases.
Kévin Lamy, Thierry Portafaix, Béatrice Josse, Colette Brogniez, Sophie Godin-Beekmann, Hassan Bencherif, Laura Revell, Hideharu Akiyoshi, Slimane Bekki, Michaela I. Hegglin, Patrick Jöckel, Oliver Kirner, Ben Liley, Virginie Marecal, Olaf Morgenstern, Andrea Stenke, Guang Zeng, N. Luke Abraham, Alexander T. Archibald, Neil Butchart, Martyn P. Chipperfield, Glauco Di Genova, Makoto Deushi, Sandip S. Dhomse, Rong-Ming Hu, Douglas Kinnison, Michael Kotkamp, Richard McKenzie, Martine Michou, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Eugene Rozanov, David Saint-Martin, Kengo Sudo, Taichu Y. Tanaka, Daniele Visioni, and Kohei Yoshida
Atmos. Chem. Phys., 19, 10087–10110, https://doi.org/10.5194/acp-19-10087-2019, https://doi.org/10.5194/acp-19-10087-2019, 2019
Short summary
Short summary
In this study, we simulate the ultraviolet radiation evolution during the 21st century on Earth's surface using the output from several numerical models which participated in the Chemistry-Climate Model Initiative. We present four possible futures which depend on greenhouse gases emissions. The role of ozone-depleting substances, greenhouse gases and aerosols are investigated. Our results emphasize the important role of aerosols for future ultraviolet radiation in the Northern Hemisphere.
David C. Wade, Nathan Luke Abraham, Alexander Farnsworth, Paul J. Valdes, Fran Bragg, and Alexander T. Archibald
Clim. Past, 15, 1463–1483, https://doi.org/10.5194/cp-15-1463-2019, https://doi.org/10.5194/cp-15-1463-2019, 2019
Short summary
Short summary
The amount of O2 in the atmosphere may have varied from as little as 10 % to as much as 35 % during the last 541 Myr. These changes are large enough to have led to changes in atmospheric mass, which may alter the radiative budget of the atmosphere. We present the first fully 3-D numerical model simulations to investigate the climate impacts of changes in O2 during different climate states. We identify a complex new mechanism causing increases in surface temperature when O2 levels were higher.
Ewa M. Bednarz, Amanda C. Maycock, Peter Braesicke, Paul J. Telford, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 9833–9846, https://doi.org/10.5194/acp-19-9833-2019, https://doi.org/10.5194/acp-19-9833-2019, 2019
Short summary
Short summary
The atmospheric response to the amplitude of 11-year solar cycle in UM-UKCA is separated into the contributions from changes in direct radiative heating and photolysis rates, and the results compared with a control case with both effects included. We find that while the tropical responses are largely additive, this is not necessarily the case in the high latitudes. We suggest that solar-induced changes in ozone are important for modulating the SH dynamical response to the 11-year solar cycle.
Zainab Q. Hakim, Scott Archer-Nicholls, Gufran Beig, Gerd A. Folberth, Kengo Sudo, Nathan Luke Abraham, Sachin Ghude, Daven K. Henze, and Alexander T. Archibald
Atmos. Chem. Phys., 19, 6437–6458, https://doi.org/10.5194/acp-19-6437-2019, https://doi.org/10.5194/acp-19-6437-2019, 2019
Short summary
Short summary
Surface ozone is an important air pollutant and recent work has calculated that large numbers of people die prematurely because of exposure to high levels of surface ozone in India. However, these calculations require model simulations of ozone as key inputs.
Here we perform the most thorough evaluation of global model surface ozone over India to date. These analyses of model simulations and observations highlight some successes and shortcomings and the need for further process-based studies.
Ewa M. Bednarz, Amanda C. Maycock, Paul J. Telford, Peter Braesicke, N. Luke Abraham, and John A. Pyle
Atmos. Chem. Phys., 19, 5209–5233, https://doi.org/10.5194/acp-19-5209-2019, https://doi.org/10.5194/acp-19-5209-2019, 2019
Short summary
Short summary
Following model improvements, the atmospheric response to the 11-year solar cycle forcing simulated in the UM-UKCA chemistry–climate model is discussed for the first time. In contrast to most previous studies in the literature, we compare the results diagnosed using both a composite and a MLR methodology, and we show that apparently different signals can be diagnosed in the troposphere. In addition, we look at the role of internal atmospheric variability for the detection of the solar response.
Fraser Dennison, James Keeble, Olaf Morgenstern, Guang Zeng, N. Luke Abraham, and Xin Yang
Geosci. Model Dev., 12, 1227–1239, https://doi.org/10.5194/gmd-12-1227-2019, https://doi.org/10.5194/gmd-12-1227-2019, 2019
Short summary
Short summary
Two developments are made to the United Kingdom Chemistry and Aerosols (UKCA) model to improve simulation of stratospheric ozone. The first is the addition of a solar cycle. The influence on ozone from the solar cycle is found to be 1–2 %, which is consistent with other studies. The second is to the heterogeneous chemistry, the most significant change being the addition of reactions involving bromine species. This was shown to reduce ozone biases relative to observations in most regions.
Christa Fittschen, Mohamad Al Ajami, Sebastien Batut, Valerio Ferracci, Scott Archer-Nicholls, Alexander T. Archibald, and Coralie Schoemaecker
Atmos. Chem. Phys., 19, 349–362, https://doi.org/10.5194/acp-19-349-2019, https://doi.org/10.5194/acp-19-349-2019, 2019
Short summary
Short summary
Concentrations of OH, the main oxidant in the atmosphere, were measured in biogenic environments up to a factor of 10 higher than predicted by models. This was interpreted as a major lack in our understanding of biogenic volatile organic compound chemistry. But interferences of unknown origin have also been discovered, and we present experimental and modelling evidence that the interference might be due to the unexpected decomposition of a new class of molecule, ROOOH, in the FAGE instruments.
Samuel R. Hall, Kirk Ullmann, Michael J. Prather, Clare M. Flynn, Lee T. Murray, Arlene M. Fiore, Gustavo Correa, Sarah A. Strode, Stephen D. Steenrod, Jean-Francois Lamarque, Jonathan Guth, Béatrice Josse, Johannes Flemming, Vincent Huijnen, N. Luke Abraham, and Alex T. Archibald
Atmos. Chem. Phys., 18, 16809–16828, https://doi.org/10.5194/acp-18-16809-2018, https://doi.org/10.5194/acp-18-16809-2018, 2018
Short summary
Short summary
Photolysis (J rates) initiates and drives atmospheric chemistry, and Js are perturbed by factors of 2 by clouds. The NASA Atmospheric Tomography (ATom) Mission provides the first comprehensive observations on how clouds perturb Js through the remote Pacific and Atlantic basins. We compare these cloud-perturbation J statistics with those from nine global chemistry models. While basic patterns agree, there is a large spread across models, and all lack some basic features of the observations.
Laura E. Revell, Andrea Stenke, Fiona Tummon, Aryeh Feinberg, Eugene Rozanov, Thomas Peter, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Neal Butchart, Makoto Deushi, Patrick Jöckel, Douglas Kinnison, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke D. Oman, Giovanni Pitari, David A. Plummer, Robyn Schofield, Kane Stone, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 16155–16172, https://doi.org/10.5194/acp-18-16155-2018, https://doi.org/10.5194/acp-18-16155-2018, 2018
Short summary
Short summary
Global models such as those participating in the Chemistry-Climate Model Initiative (CCMI) consistently simulate biases in tropospheric ozone compared with observations. We performed an advanced statistical analysis with one of the CCMI models to understand the cause of the bias. We found that emissions of ozone precursor gases are the dominant driver of the bias, implying either that the emissions are too large, or that the way in which the model handles emissions needs to be improved.
Nathan Luke Abraham, Alexander T. Archibald, Paul Cresswell, Sam Cusworth, Mohit Dalvi, David Matthews, Steven Wardle, and Stuart Whitehouse
Geosci. Model Dev., 11, 3647–3657, https://doi.org/10.5194/gmd-11-3647-2018, https://doi.org/10.5194/gmd-11-3647-2018, 2018
Short summary
Short summary
Using a virtual machine environment, a low-resolution configuration of the United Kingdom Chemistry and Aerosols (UKCA) composition-climate model has been developed. This configuration, while not suitable for long simulations, is an excellent test-bed for new model developments and can be used to train new users in how to use UKCA. This work was motivated by the desire to improve the usability of UKCA, and to encourage more users to become involved with the code development process.
Emre Esentürk, Nathan Luke Abraham, Scott Archer-Nicholls, Christina Mitsakou, Paul Griffiths, Alex Archibald, and John Pyle
Geosci. Model Dev., 11, 3089–3108, https://doi.org/10.5194/gmd-11-3089-2018, https://doi.org/10.5194/gmd-11-3089-2018, 2018
Short summary
Short summary
An integral and expensive part of coupled climate model simulations is the gas-phase chemistry which gives rise to hundreds of coupled differential equations. We propose a method which improves the convergence and robustness properties of commonly used Newton–Raphson solvers. The method is flexible and can be appended to most algorithms. The approach can be useful for a broader community of computational scientists whose interests lie in solving systems with intensive interactive chemistry.
Sandip S. Dhomse, Douglas Kinnison, Martyn P. Chipperfield, Ross J. Salawitch, Irene Cionni, Michaela I. Hegglin, N. Luke Abraham, Hideharu Akiyoshi, Alex T. Archibald, Ewa M. Bednarz, Slimane Bekki, Peter Braesicke, Neal Butchart, Martin Dameris, Makoto Deushi, Stacey Frith, Steven C. Hardiman, Birgit Hassler, Larry W. Horowitz, Rong-Ming Hu, Patrick Jöckel, Beatrice Josse, Oliver Kirner, Stefanie Kremser, Ulrike Langematz, Jared Lewis, Marion Marchand, Meiyun Lin, Eva Mancini, Virginie Marécal, Martine Michou, Olaf Morgenstern, Fiona M. O'Connor, Luke Oman, Giovanni Pitari, David A. Plummer, John A. Pyle, Laura E. Revell, Eugene Rozanov, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Simone Tilmes, Daniele Visioni, Yousuke Yamashita, and Guang Zeng
Atmos. Chem. Phys., 18, 8409–8438, https://doi.org/10.5194/acp-18-8409-2018, https://doi.org/10.5194/acp-18-8409-2018, 2018
Short summary
Short summary
We analyse simulations from the Chemistry-Climate Model Initiative (CCMI) to estimate the return dates of the stratospheric ozone layer from depletion by anthropogenic chlorine and bromine. The simulations from 20 models project that global column ozone will return to 1980 values in 2047 (uncertainty range 2042–2052). Return dates in other regions vary depending on factors related to climate change and importance of chlorine and bromine. Column ozone in the tropics may continue to decline.
James Keeble, Hannah Brown, N. Luke Abraham, Neil R. P. Harris, and John A. Pyle
Atmos. Chem. Phys., 18, 7625–7637, https://doi.org/10.5194/acp-18-7625-2018, https://doi.org/10.5194/acp-18-7625-2018, 2018
Short summary
Short summary
2017 marks the 30th anniversary of the Montreal Protocol, which was implemented to protect the stratospheric ozone layer from the harmful effects of synthetic ozone depleting substances. Since the late 1990s atmospheric concentrations of these species have begun to decline, and as a result ozone concentrations are expected to increase. In this study we use an ensemble of chemistry–climate simulations to investigate recent ozone trends and search for early signs of ozone recovery.
Antara Banerjee, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 18, 2899–2911, https://doi.org/10.5194/acp-18-2899-2018, https://doi.org/10.5194/acp-18-2899-2018, 2018
Short summary
Short summary
This study quantifies the radiative forcing (RF) of future ozone changes. Under climate change, even the sign of the ozone RF can change depending on the greenhouse gas emissions scenario followed. Stratosphere–troposphere exchange plays an important role in driving ozone RF due to reductions in ozone-depleting substances (ODSs) and increases in methane abundance. These could negate the ozone-derived climate benefits of air-quality controls on non-methane ozone precursor emissions.
James Keeble, Ewa M. Bednarz, Antara Banerjee, N. Luke Abraham, Neil R. P. Harris, Amanda C. Maycock, and John A. Pyle
Atmos. Chem. Phys., 17, 13801–13818, https://doi.org/10.5194/acp-17-13801-2017, https://doi.org/10.5194/acp-17-13801-2017, 2017
Short summary
Short summary
In this study we explore the chemical and transport processes controlling ozone abundances in different altitude regions in the tropics for the present day and how these processes may change in the future in order to determine when total-column ozone values in the tropics will recover to pre-1980s values following the implementation of the Montreal Protocol and its subsequent amendments, which imposed bans on the use and emissions of CFCs.
Olaf Morgenstern, Michaela I. Hegglin, Eugene Rozanov, Fiona M. O'Connor, N. Luke Abraham, Hideharu Akiyoshi, Alexander T. Archibald, Slimane Bekki, Neal Butchart, Martyn P. Chipperfield, Makoto Deushi, Sandip S. Dhomse, Rolando R. Garcia, Steven C. Hardiman, Larry W. Horowitz, Patrick Jöckel, Beatrice Josse, Douglas Kinnison, Meiyun Lin, Eva Mancini, Michael E. Manyin, Marion Marchand, Virginie Marécal, Martine Michou, Luke D. Oman, Giovanni Pitari, David A. Plummer, Laura E. Revell, David Saint-Martin, Robyn Schofield, Andrea Stenke, Kane Stone, Kengo Sudo, Taichu Y. Tanaka, Simone Tilmes, Yousuke Yamashita, Kohei Yoshida, and Guang Zeng
Geosci. Model Dev., 10, 639–671, https://doi.org/10.5194/gmd-10-639-2017, https://doi.org/10.5194/gmd-10-639-2017, 2017
Short summary
Short summary
We present a review of the make-up of 20 models participating in the Chemistry–Climate Model Initiative (CCMI). In comparison to earlier such activities, most of these models comprise a whole-atmosphere chemistry, and several of them include an interactive ocean module. This makes them suitable for studying the interactions of tropospheric air quality, stratospheric ozone, and climate. The paper lays the foundation for other studies using the CCMI simulations for scientific analysis.
Nga Lee Ng, Steven S. Brown, Alexander T. Archibald, Elliot Atlas, Ronald C. Cohen, John N. Crowley, Douglas A. Day, Neil M. Donahue, Juliane L. Fry, Hendrik Fuchs, Robert J. Griffin, Marcelo I. Guzman, Hartmut Herrmann, Alma Hodzic, Yoshiteru Iinuma, José L. Jimenez, Astrid Kiendler-Scharr, Ben H. Lee, Deborah J. Luecken, Jingqiu Mao, Robert McLaren, Anke Mutzel, Hans D. Osthoff, Bin Ouyang, Benedicte Picquet-Varrault, Ulrich Platt, Havala O. T. Pye, Yinon Rudich, Rebecca H. Schwantes, Manabu Shiraiwa, Jochen Stutz, Joel A. Thornton, Andreas Tilgner, Brent J. Williams, and Rahul A. Zaveri
Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, https://doi.org/10.5194/acp-17-2103-2017, 2017
Short summary
Short summary
Oxidation of biogenic volatile organic compounds by NO3 is an important interaction between anthropogenic
and natural emissions. This review results from a June 2015 workshop and includes the recent literature
on kinetics, mechanisms, organic aerosol yields, and heterogeneous chemistry; advances in analytical
instrumentation; the current state NO3-BVOC chemistry in atmospheric models; and critical needs for
future research in modeling, field observations, and laboratory studies.
Mingjin Tang, James Keeble, Paul J. Telford, Francis D. Pope, Peter Braesicke, Paul T. Griffiths, N. Luke Abraham, James McGregor, I. Matt Watson, R. Anthony Cox, John A. Pyle, and Markus Kalberer
Atmos. Chem. Phys., 16, 15397–15412, https://doi.org/10.5194/acp-16-15397-2016, https://doi.org/10.5194/acp-16-15397-2016, 2016
Short summary
Short summary
We have investigated for the first time the heterogeneous hydrolysis of ClONO2 on TiO2 and SiO2 aerosol particles at room temperature and at different relative humidities (RHs), using an aerosol flow tube. The kinetic data reported in our current and previous studies have been included in the UKCA chemistry–climate model to assess the impact of TiO2 injection on stratospheric chemistry and stratospheric ozone in particular.
Nicola J. Warwick, Michelle L. Cain, Rebecca Fisher, James L. France, David Lowry, Sylvia E. Michel, Euan G. Nisbet, Bruce H. Vaughn, James W. C. White, and John A. Pyle
Atmos. Chem. Phys., 16, 14891–14908, https://doi.org/10.5194/acp-16-14891-2016, https://doi.org/10.5194/acp-16-14891-2016, 2016
Short summary
Short summary
Methane is an important greenhouse gas. Methane emissions from Arctic wetlands are poorly quantified and may increase in a warming climate. Using a global atmospheric model and atmospheric observations of methane and its isotopologues, we find that isotopologue data are useful in constraining Arctic wetland emissions. Our results suggest that the seasonal cycle of these emissions may be incorrectly simulated in land process models, with implications for our understanding of future emissions.
Ewa M. Bednarz, Amanda C. Maycock, N. Luke Abraham, Peter Braesicke, Olivier Dessens, and John A. Pyle
Atmos. Chem. Phys., 16, 12159–12176, https://doi.org/10.5194/acp-16-12159-2016, https://doi.org/10.5194/acp-16-12159-2016, 2016
Short summary
Short summary
Future trends in springtime Arctic ozone, and its chemical dynamical and radiative drivers, are analysed using a 7-member ensemble of chemistry–climate model integrations, allowing for a detailed assessment of interannual variability. Despite the future long-term recovery of Arctic ozone, there is large interannual variability and episodic reductions in springtime Arctic column ozone. Halogen chemistry will become a smaller but non-negligible driver of Arctic ozone variability over the century.
Ivan Kourtchev, Ricardo H. M. Godoi, Sarah Connors, James G. Levine, Alex T. Archibald, Ana F. L. Godoi, Sarah L. Paralovo, Cybelli G. G. Barbosa, Rodrigo A. F. Souza, Antonio O. Manzi, Roger Seco, Steve Sjostedt, Jeong-Hoo Park, Alex Guenther, Saewung Kim, James Smith, Scot T. Martin, and Markus Kalberer
Atmos. Chem. Phys., 16, 11899–11913, https://doi.org/10.5194/acp-16-11899-2016, https://doi.org/10.5194/acp-16-11899-2016, 2016
R. Hossaini, P. K. Patra, A. A. Leeson, G. Krysztofiak, N. L. Abraham, S. J. Andrews, A. T. Archibald, J. Aschmann, E. L. Atlas, D. A. Belikov, H. Bönisch, L. J. Carpenter, S. Dhomse, M. Dorf, A. Engel, W. Feng, S. Fuhlbrügge, P. T. Griffiths, N. R. P. Harris, R. Hommel, T. Keber, K. Krüger, S. T. Lennartz, S. Maksyutov, H. Mantle, G. P. Mills, B. Miller, S. A. Montzka, F. Moore, M. A. Navarro, D. E. Oram, K. Pfeilsticker, J. A. Pyle, B. Quack, A. D. Robinson, E. Saikawa, A. Saiz-Lopez, S. Sala, B.-M. Sinnhuber, S. Taguchi, S. Tegtmeier, R. T. Lidster, C. Wilson, and F. Ziska
Atmos. Chem. Phys., 16, 9163–9187, https://doi.org/10.5194/acp-16-9163-2016, https://doi.org/10.5194/acp-16-9163-2016, 2016
Peer Johannes Nowack, Nathan Luke Abraham, Peter Braesicke, and John Adrian Pyle
Atmos. Chem. Phys., 16, 4191–4203, https://doi.org/10.5194/acp-16-4191-2016, https://doi.org/10.5194/acp-16-4191-2016, 2016
Short summary
Short summary
Various forms of solar radiation management (SRM) have been proposed to counteract man-made climate change. However, all these countermeasures could have unintended side-effects. We add a novel perspective to this discussion by showing how atmospheric ozone changes under solar geoengineering could affect UV exposure and air pollution. This would have implications for human health and ecology. Atmospheric composition changes are therefore important to consider in the evaluation of any SRM scheme.
Antara Banerjee, Amanda C. Maycock, Alexander T. Archibald, N. Luke Abraham, Paul Telford, Peter Braesicke, and John A. Pyle
Atmos. Chem. Phys., 16, 2727–2746, https://doi.org/10.5194/acp-16-2727-2016, https://doi.org/10.5194/acp-16-2727-2016, 2016
J. R. Pitt, M. Le Breton, G. Allen, C. J. Percival, M. W. Gallagher, S. J.-B. Bauguitte, S. J. O'Shea, J. B. A. Muller, M. S. Zahniser, J. Pyle, and P. I. Palmer
Atmos. Meas. Tech., 9, 63–77, https://doi.org/10.5194/amt-9-63-2016, https://doi.org/10.5194/amt-9-63-2016, 2016
Short summary
Short summary
We present details of an Aerodyne quantum cascade laser absorption spectrometer (QCLAS) used to make airborne measurements of N2O and CH4, including its configuration for use on board an aircraft. Two different methods to correct for the influence of water vapour on the measurements are evaluated. We diagnose a sensitivity of the instrument to changes in pressure, introduce a new calibration procedure to account for this effect, and assess its performance.
M. R. Russo, M. J. Ashfold, N. R. P. Harris, and J. A. Pyle
Atmos. Chem. Phys., 15, 14031–14040, https://doi.org/10.5194/acp-15-14031-2015, https://doi.org/10.5194/acp-15-14031-2015, 2015
Short summary
Short summary
We find a strong regional element to the uplift of CHBr3 from the ocean to the upper troposphere and lower stratosphere. The strongest uplift occurs when the largest emission and the most intense convection are co-located which is over the Maritime Continent in northern winter. Estimates of CHBr3 emissions based on aircraft measurements will be sensitive to where the available aircraft campaigns took place.
J. G. Levine, A. R. MacKenzie, O. J. Squire, A. T. Archibald, P. T. Griffiths, N. L. Abraham, J. A. Pyle, D. E. Oram, G. Forster, J. F. Brito, J. D. Lee, J. R. Hopkins, A. C. Lewis, S. J. B. Bauguitte, C. F. Demarco, P. Artaxo, P. Messina, J. Lathière, D. A. Hauglustaine, E. House, C. N. Hewitt, and E. Nemitz
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acpd-15-24251-2015, https://doi.org/10.5194/acpd-15-24251-2015, 2015
Revised manuscript has not been submitted
Short summary
Short summary
This study explores our ability to simulate atmospheric chemistry stemming from isoprene emissions—a reactive gas emitted from vegetation—in pristine and polluted regions of the Amazon basin. We explore how two contrasting models fare in reproducing recent airborne measurements in the region. Their differing treatments of transport and mixing are found to: profoundly affect their performance; and yield very different pictures of the exposure of the rainforest to harmful ozone concentrations.
H. M. Walker, D. Stone, T. Ingham, S. Vaughan, M. Cain, R. L. Jones, O. J. Kennedy, M. McLeod, B. Ouyang, J. Pyle, S. Bauguitte, B. Bandy, G. Forster, M. J. Evans, J. F. Hamilton, J. R. Hopkins, J. D. Lee, A. C. Lewis, R. T. Lidster, S. Punjabi, W. T. Morgan, and D. E. Heard
Atmos. Chem. Phys., 15, 8179–8200, https://doi.org/10.5194/acp-15-8179-2015, https://doi.org/10.5194/acp-15-8179-2015, 2015
O. J. Squire, A. T. Archibald, P. T. Griffiths, M. E. Jenkin, D. Smith, and J. A. Pyle
Atmos. Chem. Phys., 15, 5123–5143, https://doi.org/10.5194/acp-15-5123-2015, https://doi.org/10.5194/acp-15-5123-2015, 2015
M. J. Ashfold, J. A. Pyle, A. D. Robinson, E. Meneguz, M. S. M. Nadzir, S. M. Phang, A. A. Samah, S. Ong, H. E. Ung, L. K. Peng, S. E. Yong, and N. R. P. Harris
Atmos. Chem. Phys., 15, 3565–3573, https://doi.org/10.5194/acp-15-3565-2015, https://doi.org/10.5194/acp-15-3565-2015, 2015
Short summary
Short summary
We use observations and model calculations to show that "cold surges" occurring during Northern Hemisphere winter can rapidly transport East Asian pollution to equatorial Southeast Asia. As well as affecting atmospheric composition near the surface, we argue that strong convection can subsequently lift the polluted air masses to the tropical upper troposphere. This suggests a potentially important connection between midlatitude pollution sources and the lower stratosphere.
J. Keeble, P. Braesicke, N. L. Abraham, H. K. Roscoe, and J. A. Pyle
Atmos. Chem. Phys., 14, 13705–13717, https://doi.org/10.5194/acp-14-13705-2014, https://doi.org/10.5194/acp-14-13705-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, K. Bower, S. M. Illingworth, J. B. A. Muller, B. T. Jones, C. J. Percival, S. J-B. Bauguitte, M. Cain, N. Warwick, A. Quiquet, U. Skiba, J. Drewer, K. Dinsmore, E. G. Nisbet, D. Lowry, R. E. Fisher, J. L. France, M. Aurela, A. Lohila, G. Hayman, C. George, D. B. Clark, A. J. Manning, A. D. Friend, and J. Pyle
Atmos. Chem. Phys., 14, 13159–13174, https://doi.org/10.5194/acp-14-13159-2014, https://doi.org/10.5194/acp-14-13159-2014, 2014
Short summary
Short summary
This paper presents airborne measurements of greenhouse gases collected in the European Arctic. Regional scale flux estimates for the northern Scandinavian wetlands are derived. These fluxes are found to be in excellent agreement with coincident surface measurements within the aircraft's sampling domain. This has allowed a significant low bias to be identified in two commonly used process-based land surface models.
S. S. Dhomse, K. M. Emmerson, G. W. Mann, N. Bellouin, K. S. Carslaw, M. P. Chipperfield, R. Hommel, N. L. Abraham, P. Telford, P. Braesicke, M. Dalvi, C. E. Johnson, F. O'Connor, O. Morgenstern, J. A. Pyle, T. Deshler, J. M. Zawodny, and L. W. Thomason
Atmos. Chem. Phys., 14, 11221–11246, https://doi.org/10.5194/acp-14-11221-2014, https://doi.org/10.5194/acp-14-11221-2014, 2014
X. Yang, N. L. Abraham, A. T. Archibald, P. Braesicke, J. Keeble, P. J. Telford, N. J. Warwick, and J. A. Pyle
Atmos. Chem. Phys., 14, 10431–10438, https://doi.org/10.5194/acp-14-10431-2014, https://doi.org/10.5194/acp-14-10431-2014, 2014
A. Banerjee, A. T. Archibald, A. C. Maycock, P. Telford, N. L. Abraham, X. Yang, P. Braesicke, and J. A. Pyle
Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, https://doi.org/10.5194/acp-14-9871-2014, 2014
M. S. Mohd Nadzir, S. M. Phang, M. R. Abas, N. Abdul Rahman, A. Abu Samah, W. T. Sturges, D. E. Oram, G. P. Mills, Emma C. Leedham Elvidge, J. A. Pyle, N. R. P. Harris, A. D. Robinson, M. J. Ashfold, M. I. Mead, M. T. Latif, M. F. Khan, A. M. Amiruddin, N. Banan, and M. M. Hanafiah
Atmos. Chem. Phys., 14, 8137–8148, https://doi.org/10.5194/acp-14-8137-2014, https://doi.org/10.5194/acp-14-8137-2014, 2014
M. J. Tang, P. J. Telford, F. D. Pope, L. Rkiouak, N. L. Abraham, A. T. Archibald, P. Braesicke, J. A. Pyle, J. McGregor, I. M. Watson, R. A. Cox, and M. Kalberer
Atmos. Chem. Phys., 14, 6035–6048, https://doi.org/10.5194/acp-14-6035-2014, https://doi.org/10.5194/acp-14-6035-2014, 2014
O. J. Squire, A. T. Archibald, N. L. Abraham, D. J. Beerling, C. N. Hewitt, J. Lathière, R. C. Pike, P. J. Telford, and J. A. Pyle
Atmos. Chem. Phys., 14, 1011–1024, https://doi.org/10.5194/acp-14-1011-2014, https://doi.org/10.5194/acp-14-1011-2014, 2014
F. M. O'Connor, C. E. Johnson, O. Morgenstern, N. L. Abraham, P. Braesicke, M. Dalvi, G. A. Folberth, M. G. Sanderson, P. J. Telford, A. Voulgarakis, P. J. Young, G. Zeng, W. J. Collins, and J. A. Pyle
Geosci. Model Dev., 7, 41–91, https://doi.org/10.5194/gmd-7-41-2014, https://doi.org/10.5194/gmd-7-41-2014, 2014
S. J. O'Shea, G. Allen, M. W. Gallagher, S. J.-B. Bauguitte, S. M. Illingworth, M. Le Breton, J. B. A. Muller, C. J. Percival, A. T. Archibald, D. E. Oram, M. Parrington, P. I. Palmer, and A. C. Lewis
Atmos. Chem. Phys., 13, 12451–12467, https://doi.org/10.5194/acp-13-12451-2013, https://doi.org/10.5194/acp-13-12451-2013, 2013
Z. S. Stock, M. R. Russo, T. M. Butler, A. T. Archibald, M. G. Lawrence, P. J. Telford, N. L. Abraham, and J. A. Pyle
Atmos. Chem. Phys., 13, 12215–12231, https://doi.org/10.5194/acp-13-12215-2013, https://doi.org/10.5194/acp-13-12215-2013, 2013
A. M. Foley, D. Dalmonech, A. D. Friend, F. Aires, A. T. Archibald, P. Bartlein, L. Bopp, J. Chappellaz, P. Cox, N. R. Edwards, G. Feulner, P. Friedlingstein, S. P. Harrison, P. O. Hopcroft, C. D. Jones, J. Kolassa, J. G. Levine, I. C. Prentice, J. Pyle, N. Vázquez Riveiros, E. W. Wolff, and S. Zaehle
Biogeosciences, 10, 8305–8328, https://doi.org/10.5194/bg-10-8305-2013, https://doi.org/10.5194/bg-10-8305-2013, 2013
P. Braesicke, J. Keeble, X. Yang, G. Stiller, S. Kellmann, N. L. Abraham, A. Archibald, P. Telford, and J. A. Pyle
Atmos. Chem. Phys., 13, 10677–10688, https://doi.org/10.5194/acp-13-10677-2013, https://doi.org/10.5194/acp-13-10677-2013, 2013
N. J. Warwick, A. T. Archibald, K. Ashworth, J. Dorsey, P. M. Edwards, D. E. Heard, B. Langford, J. Lee, P. K. Misztal, L. K. Whalley, and J. A. Pyle
Atmos. Chem. Phys., 13, 9183–9194, https://doi.org/10.5194/acp-13-9183-2013, https://doi.org/10.5194/acp-13-9183-2013, 2013
P. J. Young, A. T. Archibald, K. W. Bowman, J.-F. Lamarque, V. Naik, D. S. Stevenson, S. Tilmes, A. Voulgarakis, O. Wild, D. Bergmann, P. Cameron-Smith, I. Cionni, W. J. Collins, S. B. Dalsøren, R. M. Doherty, V. Eyring, G. Faluvegi, L. W. Horowitz, B. Josse, Y. H. Lee, I. A. MacKenzie, T. Nagashima, D. A. Plummer, M. Righi, S. T. Rumbold, R. B. Skeie, D. T. Shindell, S. A. Strode, K. Sudo, S. Szopa, and G. Zeng
Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, https://doi.org/10.5194/acp-13-2063-2013, 2013
P. J. Telford, N. L. Abraham, A. T. Archibald, P. Braesicke, M. Dalvi, O. Morgenstern, F. M. O'Connor, N. A. D. Richards, and J. A. Pyle
Geosci. Model Dev., 6, 161–177, https://doi.org/10.5194/gmd-6-161-2013, https://doi.org/10.5194/gmd-6-161-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Tropospheric ozone precursors: global and regional distributions, trends, and variability
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Ether and ester formation from peroxy radical recombination: a qualitative reaction channel analysis
ACEIC: a comprehensive anthropogenic chlorine emission inventory for China
Impact of methane and other precursor emission reductions on surface ozone in Europe: scenario analysis using the European Monitoring and Evaluation Programme (EMEP) Meteorological Synthesizing Centre – West (MSC-W) model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
The effect of different climate and air quality policies in China on in situ ozone production in Beijing
Enhancing long-term trend simulation of the global tropospheric hydroxyl (TOH) and its drivers from 2005 to 2019: a synergistic integration of model simulations and satellite observations
Intercomparison of GEOS-Chem and CAM-chem tropospheric oxidant chemistry within the Community Earth System Model version 2 (CESM2)
Development of a detailed gaseous oxidation scheme of naphthalene for secondary organic aerosol (SOA) formation and speciation
Large contributions of soil emissions to the atmospheric nitrogen budget and their impacts on air quality and temperature rise in North China
Why did ozone concentrations remain high during Shanghai's static management? A statistical and radical-chemistry perspective
Revising VOC emissions speciation improves the simulation of global background ethane and propane
Changes in South American surface ozone trends: exploring the influences of precursors and extreme events
Evaluating NOx stack plume emissions using a high-resolution atmospheric chemistry model and satellite-derived NO2 columns
NOx emissions in France in 2019–2021 as estimated by the high-spatial-resolution assimilation of TROPOMI NO2 observations
Aggravated surface O3 pollution primarily driven by meteorological variations in China during the 2020 COVID-19 pandemic lockdown period
Identifying decadal trends in deweathered concentrations of criteria air pollutants in Canadian urban atmospheres with machine learning approaches
Evaluation of modelled versus observed non-methane volatile organic compounds at European Monitoring and Evaluation Programme sites in Europe
Constraining non-methane VOC emissions with TROPOMI HCHO observations: impact on summertime ozone simulation in August 2022 in China
Revealing the significant acceleration of hydrofluorocarbon (HFC) emissions in eastern Asia through long-term atmospheric observations
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Interpreting Geostationary Environment Monitoring Spectrometer (GEMS) geostationary satellite observations of the diurnal variation in nitrogen dioxide (NO2) over East Asia
Constraining Light Dependency in Modeled Emissions Through Comparison to Observed BVOC Concentrations in a Southeastern US Forest
An intercomparison of satellite, airborne, and ground-level observations with WRF–CAMx simulations of NO2 columns over Houston, Texas, during the September 2021 TRACER-AQ campaign
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska during ALPACA-2022
Interannual variability of summertime formaldehyde (HCHO) vertical column density and its main drivers at northern high latitudes
The impact of multi-decadal changes in VOC speciation on urban ozone chemistry: a case study in Birmingham, United Kingdom
Technical note: Challenges in detecting free tropospheric ozone trends in a sparsely sampled environment
Combined assimilation of NOAA surface and MIPAS satellite observations to constrain the global budget of carbonyl sulfide
The impact of gaseous degradation on the gas–particle partitioning of methylated polycyclic aromatic hydrocarbons
Technical note: An assessment of the performance of statistical bias correction techniques for global chemistry–climate model surface ozone fields
Interpreting Summertime Hourly Variation of NO2 Columns with Implications for Geostationary Satellite Applications
Opinion: Challenges and needs of tropospheric chemical mechanism development
A better representation of volatile organic compound chemistry in WRF-Chem and its impact on ozone over Los Angeles
High-resolution US methane emissions inferred from an inversion of 2019 TROPOMI satellite data: contributions from individual states, urban areas, and landfills
Summertime tropospheric ozone source apportionment study in the Madrid region (Spain)
CO anthropogenic emissions in Europe from 2011 to 2021: insights from Measurement of Pollution in the Troposphere (MOPITT) satellite data
Constraining long-term NOx emissions over the United States and Europe using nitrate wet deposition monitoring networks
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Analysis of an intense O3 pollution episode on the Atlantic coast of the Iberian Peninsula using photochemical modeling: characterization of transport pathways and accumulation processes
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Atmospheric oxygen as a tracer for fossil fuel carbon dioxide: a sensitivity study in the UK
Source analyses of ambient VOCs considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
MIXv2: a long-term mosaic emission inventory for Asia (2010–2017)
The Atmospheric Oxidizing Capacity in China: Part 2. Sensitivity to emissions of primary pollutants
Process Analysis of Elevated Concentrations of Organic Acids at Whiteface Mountain, New York
Organosulfate produced from consumption of SO3 speeds up sulfuric acid–dimethylamine atmospheric nucleation
Yasin Elshorbany, Jerald R. Ziemke, Sarah Strode, Hervé Petetin, Kazuyuki Miyazaki, Isabelle De Smedt, Kenneth Pickering, Rodrigo J. Seguel, Helen Worden, Tamara Emmerichs, Domenico Taraborrelli, Maria Cazorla, Suvarna Fadnavis, Rebecca R. Buchholz, Benjamin Gaubert, Néstor Y. Rojas, Thiago Nogueira, Thérèse Salameh, and Min Huang
Atmos. Chem. Phys., 24, 12225–12257, https://doi.org/10.5194/acp-24-12225-2024, https://doi.org/10.5194/acp-24-12225-2024, 2024
Short summary
Short summary
We investigated tropospheric ozone spatial variability and trends from 2005 to 2019 and related those to ozone precursors on global and regional scales. We also investigate the spatiotemporal characteristics of the ozone formation regime in relation to ozone chemical sources and sinks. Our analysis is based on remote sensing products of the tropospheric column of ozone and its precursors, nitrogen dioxide, formaldehyde, and total column CO, as well as ozonesonde data and model simulations.
Mariano Mertens, Sabine Brinkop, Phoebe Graf, Volker Grewe, Johannes Hendricks, Patrick Jöckel, Anna Lanteri, Sigrun Matthes, Vanessa S. Rieger, Mattia Righi, and Robin N. Thor
Atmos. Chem. Phys., 24, 12079–12106, https://doi.org/10.5194/acp-24-12079-2024, https://doi.org/10.5194/acp-24-12079-2024, 2024
Short summary
Short summary
We quantified the contributions of land transport, shipping, and aviation emissions to tropospheric ozone; its radiative forcing; and the reductions of the methane lifetime using chemistry-climate model simulations. The contributions were analysed for the conditions of 2015 and for three projections for the year 2050. The results highlight the challenges of mitigating ozone formed by emissions of the transport sector, caused by the non-linearitiy of the ozone chemistry and the long lifetime.
Lauri Franzon, Marie Camredon, Richard Valorso, Bernard Aumont, and Theo Kurtén
Atmos. Chem. Phys., 24, 11679–11699, https://doi.org/10.5194/acp-24-11679-2024, https://doi.org/10.5194/acp-24-11679-2024, 2024
Short summary
Short summary
In this article we investigate the formation of large, sticky molecules from various organic compounds entering the atmosphere as primary emissions and the degree to which these processes may contribute to organic aerosol particle mass. More specifically, we qualitatively investigate a recently discovered chemical reaction channel for one of the most important short-lived radical compounds, peroxy radicals, and discover which of these reactions are most atmospherically important.
Siting Li, Yiming Liu, Yuqi Zhu, Yinbao Jin, Yingying Hong, Ao Shen, Yifei Xu, Haofan Wang, Haichao Wang, Xiao Lu, Shaojia Fan, and Qi Fan
Atmos. Chem. Phys., 24, 11521–11544, https://doi.org/10.5194/acp-24-11521-2024, https://doi.org/10.5194/acp-24-11521-2024, 2024
Short summary
Short summary
This study establishes an inventory of anthropogenic chlorine emissions in China in 2019 with expanded species (HCl, Cl-, Cl2, HOCl) and sources (41 specific sources). The inventory is validated by a modeling study against the observations. This study enhances the understanding of anthropogenic chlorine emissions in the atmosphere, identifies key sources, and provides scientific support for pollution control and climate change.
Willem E. van Caspel, Zbigniew Klimont, Chris Heyes, and Hilde Fagerli
Atmos. Chem. Phys., 24, 11545–11563, https://doi.org/10.5194/acp-24-11545-2024, https://doi.org/10.5194/acp-24-11545-2024, 2024
Short summary
Short summary
Methane in the atmosphere contributes to the production of ozone gas – an air pollutant and greenhouse gas. Our results highlight that simultaneous reductions in methane emissions help avoid offsetting the air pollution benefits already achieved by the already-approved precursor emission reductions by 2050 in the European Monitoring and Evaluation Programme region, while also playing an important role in bringing air pollution further down towards World Health Organization guideline limits.
Tia R. Scarpelli, Paul I. Palmer, Mark Lunt, Ingrid Super, and Arjan Droste
Atmos. Chem. Phys., 24, 10773–10791, https://doi.org/10.5194/acp-24-10773-2024, https://doi.org/10.5194/acp-24-10773-2024, 2024
Short summary
Short summary
Under the Paris Agreement, countries must track their anthropogenic greenhouse gas emissions. This study describes a method to determine self-consistent estimates for combustion emissions and natural fluxes of CO2 from atmospheric data. We report consistent estimates inferred using this approach from satellite data and ground-based data over Europe, suggesting that satellite data can be used to determine national anthropogenic CO2 emissions for countries where ground-based CO2 data are absent.
Ryan J. Pound, Lucy V. Brown, Mat J. Evans, and Lucy J. Carpenter
Atmos. Chem. Phys., 24, 9899–9921, https://doi.org/10.5194/acp-24-9899-2024, https://doi.org/10.5194/acp-24-9899-2024, 2024
Short summary
Short summary
Iodine-mediated loss of ozone to the ocean surface and the subsequent emission of iodine species has a large effect on the troposphere. Here we combine recent experimental insights to develop a box model of the process, which we then parameterize and incorporate into the GEOS-Chem transport model. We find that these new insights have a small impact on the total emission of iodine but significantly change its distribution.
Katherine R. Travis, Benjamin A. Nault, James H. Crawford, Kelvin H. Bates, Donald R. Blake, Ronald C. Cohen, Alan Fried, Samuel R. Hall, L. Gregory Huey, Young Ro Lee, Simone Meinardi, Kyung-Eun Min, Isobel J. Simpson, and Kirk Ullman
Atmos. Chem. Phys., 24, 9555–9572, https://doi.org/10.5194/acp-24-9555-2024, https://doi.org/10.5194/acp-24-9555-2024, 2024
Short summary
Short summary
Human activities result in the emission of volatile organic compounds (VOCs) that contribute to air pollution. Detailed VOC measurements were taken during a field study in South Korea. When compared to VOC inventories, large discrepancies showed underestimates from chemical products, liquefied petroleum gas, and long-range transport. Improved emissions and chemistry of these VOCs better described urban pollution. The new chemical scheme is relevant to urban areas and other VOC sources.
Beth S. Nelson, Zhenze Liu, Freya A. Squires, Marvin Shaw, James R. Hopkins, Jacqueline F. Hamilton, Andrew R. Rickard, Alastair C. Lewis, Zongbo Shi, and James D. Lee
Atmos. Chem. Phys., 24, 9031–9044, https://doi.org/10.5194/acp-24-9031-2024, https://doi.org/10.5194/acp-24-9031-2024, 2024
Short summary
Short summary
The impact of combined air quality and carbon neutrality policies on O3 formation in Beijing was investigated. Emissions inventory data were used to estimate future pollutant mixing ratios relative to ground-level observations. O3 production was found to be most sensitive to changes in alkenes, but large reductions in less reactive compounds led to larger reductions in future O3 production. This study highlights the importance of understanding the emissions of organic pollutants.
Amir H. Souri, Bryan N. Duncan, Sarah A. Strode, Daniel C. Anderson, Michael E. Manyin, Junhua Liu, Luke D. Oman, Zhen Zhang, and Brad Weir
Atmos. Chem. Phys., 24, 8677–8701, https://doi.org/10.5194/acp-24-8677-2024, https://doi.org/10.5194/acp-24-8677-2024, 2024
Short summary
Short summary
We explore a new method of using the wealth of information obtained from satellite observations of Aura OMI NO2, HCHO, and MERRA-2 reanalysis in NASA’s GEOS model equipped with an efficient tropospheric OH (TOH) estimator to enhance the representation of TOH spatial distribution and its long-term trends. This new framework helps us pinpoint regional inaccuracies in TOH and differentiate between established prior knowledge and newly acquired information from satellites on TOH trends.
Haipeng Lin, Louisa K. Emmons, Elizabeth W. Lundgren, Laura Hyesung Yang, Xu Feng, Ruijun Dang, Shixian Zhai, Yunxiao Tang, Makoto M. Kelp, Nadia K. Colombi, Sebastian D. Eastham, Thibaud M. Fritz, and Daniel J. Jacob
Atmos. Chem. Phys., 24, 8607–8624, https://doi.org/10.5194/acp-24-8607-2024, https://doi.org/10.5194/acp-24-8607-2024, 2024
Short summary
Short summary
Tropospheric ozone is a major air pollutant, a greenhouse gas, and a major indicator of model skill. Global atmospheric chemistry models show large differences in simulations of tropospheric ozone, but isolating sources of differences is complicated by different model environments. By implementing the GEOS-Chem model side by side to CAM-chem within a common Earth system model, we identify and evaluate specific differences between the two models and their impacts on key chemical species.
Victor Lannuque and Karine Sartelet
Atmos. Chem. Phys., 24, 8589–8606, https://doi.org/10.5194/acp-24-8589-2024, https://doi.org/10.5194/acp-24-8589-2024, 2024
Short summary
Short summary
Large uncertainties remain in understanding secondary organic aerosol (SOA) formation and speciation from naphthalene oxidation. This study details the development of the first near-explicit chemical scheme for naphthalene oxidation by OH, which includes kinetic and mechanistic data, and is able to reproduce most of the experimentally identified products in both gas and particle phases.
Tong Sha, Siyu Yang, Qingcai Chen, Liangqing Li, Xiaoyan Ma, Yan-Lin Zhang, Zhaozhong Feng, K. Folkert Boersma, and Jun Wang
Atmos. Chem. Phys., 24, 8441–8455, https://doi.org/10.5194/acp-24-8441-2024, https://doi.org/10.5194/acp-24-8441-2024, 2024
Short summary
Short summary
Using an updated soil reactive nitrogen emission scheme in the Unified Inputs for Weather Research and Forecasting coupled with Chemistry (UI-WRF-Chem) model, we investigate the role of soil NO and HONO (Nr) emissions in air quality and temperature in North China. Contributions of soil Nr emissions to O3 and secondary pollutants are revealed, exceeding effects of soil NOx or HONO emission. Soil Nr emissions play an important role in mitigating O3 pollution and addressing climate change.
Jian Zhu, Shanshan Wang, Chuanqi Gu, Zhiwen Jiang, Sanbao Zhang, Ruibin Xue, Yuhao Yan, and Bin Zhou
Atmos. Chem. Phys., 24, 8383–8395, https://doi.org/10.5194/acp-24-8383-2024, https://doi.org/10.5194/acp-24-8383-2024, 2024
Short summary
Short summary
In 2022, Shanghai implemented city-wide static management measures during the high-ozone season in April and May, providing a chance to study ozone pollution control. Despite significant emissions reductions, ozone levels increased by 23 %. Statistically, the number of days with higher ozone diurnal variation types increased during the lockdown period. The uneven decline in VOC and NO2 emissions led to heightened photochemical processes, resulting in the observed ozone level rise.
Matthew J. Rowlinson, Mat J. Evans, Lucy J. Carpenter, Katie A. Read, Shalini Punjabi, Adedayo Adedeji, Luke Fakes, Ally Lewis, Ben Richmond, Neil Passant, Tim Murrells, Barron Henderson, Kelvin H. Bates, and Detlev Helmig
Atmos. Chem. Phys., 24, 8317–8342, https://doi.org/10.5194/acp-24-8317-2024, https://doi.org/10.5194/acp-24-8317-2024, 2024
Short summary
Short summary
Ethane and propane are volatile organic compounds emitted from human activities which help to form ozone, a pollutant and greenhouse gas, and also affect the chemistry of the lower atmosphere. Atmospheric models tend to do a poor job of reproducing the abundance of these compounds in the atmosphere. By using regional estimates of their emissions, rather than globally consistent estimates, we can significantly improve the simulation of ethane in the model and make some improvement for propane.
Rodrigo J. Seguel, Lucas Castillo, Charlie Opazo, Néstor Y. Rojas, Thiago Nogueira, María Cazorla, Mario Gavidia-Calderón, Laura Gallardo, René Garreaud, Tomás Carrasco-Escaff, and Yasin Elshorbany
Atmos. Chem. Phys., 24, 8225–8242, https://doi.org/10.5194/acp-24-8225-2024, https://doi.org/10.5194/acp-24-8225-2024, 2024
Short summary
Short summary
Trends of surface ozone were examined across South America. Our findings indicate that ozone trends in major South American cities either increase or remain steady, with no signs of decline. The upward trends can be attributed to chemical regimes that efficiently convert nitric oxide into nitrogen dioxide. Additionally, our results suggest a climate penalty for ozone driven by meteorological conditions that favor wildfire propagation in Chile and extensive heat waves in southern Brazil.
Maarten Krol, Bart van Stratum, Isidora Anglou, and Klaas Folkert Boersma
Atmos. Chem. Phys., 24, 8243–8262, https://doi.org/10.5194/acp-24-8243-2024, https://doi.org/10.5194/acp-24-8243-2024, 2024
Short summary
Short summary
This paper presents detailed plume simulations of nitrogen oxides and carbon dioxide that are emitted from four large industrial facilities world-wide. Results from the high-resolution simulations that include atmospheric chemistry are compared to nitrogen dioxide observations from satellites. We find good performance of the model and show that common assumptions that are used in simplified models need revision. This work is important for the monitoring of emissions using satellite data.
Robin Plauchu, Audrey Fortems-Cheiney, Grégoire Broquet, Isabelle Pison, Antoine Berchet, Elise Potier, Gaëlle Dufour, Adriana Coman, Dilek Savas, Guillaume Siour, and Henk Eskes
Atmos. Chem. Phys., 24, 8139–8163, https://doi.org/10.5194/acp-24-8139-2024, https://doi.org/10.5194/acp-24-8139-2024, 2024
Short summary
Short summary
This study uses the Community Inversion Framework and CHIMERE model to assess the potential of TROPOMI-S5P PAL NO2 tropospheric column data to estimate NOx emissions in France (2019–2021). Results show a 3 % decrease in average emissions compared to the 2016 CAMS-REG/INS, lower than the 14 % decrease from CITEPA. The study highlights challenges in capturing emission anomalies due to limited data coverage and error levels but shows promise for local inventory improvements.
Zhendong Lu, Jun Wang, Yi Wang, Daven K. Henze, Xi Chen, Tong Sha, and Kang Sun
Atmos. Chem. Phys., 24, 7793–7813, https://doi.org/10.5194/acp-24-7793-2024, https://doi.org/10.5194/acp-24-7793-2024, 2024
Short summary
Short summary
In contrast with past work showing that the reduction of emissions was the dominant factor for the nationwide increase of surface O3 during the lockdown in China, this study finds that the variation in meteorology (temperature and other parameters) plays a more important role. This result is obtained through sensitivity simulations using a chemical transport model constrained by satellite (TROPOMI) data and calibrated with surface observations.
Xiaohong Yao and Leiming Zhang
Atmos. Chem. Phys., 24, 7773–7791, https://doi.org/10.5194/acp-24-7773-2024, https://doi.org/10.5194/acp-24-7773-2024, 2024
Short summary
Short summary
This study investigates long-term trends of criteria air pollutants, including NO2, CO, SO2, O3 and PM2.5, and NO2+O3 measured in 10 Canadian cities during the last 2 to 3 decades. We also investigate associated driving forces in terms of emission reductions, perturbations from varying weather conditions and large-scale wildfires, as well as changes in O3 sources and sinks.
Yao Ge, Sverre Solberg, Mathew R. Heal, Stefan Reimann, Willem van Caspel, Bryan Hellack, Thérèse Salameh, and David Simpson
Atmos. Chem. Phys., 24, 7699–7729, https://doi.org/10.5194/acp-24-7699-2024, https://doi.org/10.5194/acp-24-7699-2024, 2024
Short summary
Short summary
Atmospheric volatile organic compounds (VOCs) constitute many species, acting as precursors to ozone and aerosol. Given the uncertainties in VOC emissions, lack of evaluation studies, and recent changes in emissions, this work adapts the EMEP MSC-W to evaluate emission inventories in Europe. We focus on the varying agreement between modelled and measured VOCs across different species and underscore potential inaccuracies in total and sector-specific emission estimates.
Shuzhuang Feng, Fei Jiang, Tianlu Qian, Nan Wang, Mengwei Jia, Songci Zheng, Jiansong Chen, Fang Ying, and Weimin Ju
Atmos. Chem. Phys., 24, 7481–7498, https://doi.org/10.5194/acp-24-7481-2024, https://doi.org/10.5194/acp-24-7481-2024, 2024
Short summary
Short summary
We developed a multi-air-pollutant inversion system to estimate non-methane volatile organic compound (NMVOC) emissions using TROPOMI formaldehyde retrievals. We found that the inversion significantly improved formaldehyde simulations and reduced NMVOC emission uncertainties. The optimized NMVOC emissions effectively corrected the overestimation of O3 levels, mainly by decreasing the rate of the RO2 + NO reaction and increasing the rate of the NO2 + OH reaction.
Haklim Choi, Alison L. Redington, Hyeri Park, Jooil Kim, Rona L. Thompson, Jens Mühle, Peter K. Salameh, Christina M. Harth, Ray F. Weiss, Alistair J. Manning, and Sunyoung Park
Atmos. Chem. Phys., 24, 7309–7330, https://doi.org/10.5194/acp-24-7309-2024, https://doi.org/10.5194/acp-24-7309-2024, 2024
Short summary
Short summary
We analyzed with an inversion model the atmospheric abundance of hydrofluorocarbons (HFCs), potent greenhouse gases, from 2008 to 2020 at Gosan station in South Korea and revealed a significant increase in emissions, especially from eastern China and Japan. This increase contradicts reported data, underscoring the need for accurate monitoring and reporting. Our findings are crucial for understanding and managing global HFCs emissions, highlighting the importance of efforts to reduce HFCs.
T. Nash Skipper, Emma L. D'Ambro, Forwood C. Wiser, V. Faye McNeill, Rebecca H. Schwantes, Barron H. Henderson, Ivan R. Piletic, Colleen B. Baublitz, Jesse O. Bash, Andrew R. Whitehill, Lukas C. Valin, Asher P. Mouat, Jennifer Kaiser, Glenn M. Wolfe, Jason M. St. Clair, Thomas F. Hanisco, Alan Fried, Bryan K. Place, and Havala O. T. Pye
EGUsphere, https://doi.org/10.5194/egusphere-2024-1680, https://doi.org/10.5194/egusphere-2024-1680, 2024
Short summary
Short summary
Here, we develop the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM) version 2 to improve predictions of formaldehyde in ambient air compared to satellite-, aircraft-, and ground-based observations. With the updated chemistry representation, we then estimate the cancer risk in the contiguous US from exposure to ambient formaldehyde and estimate 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Laura Hyesung Yang, Daniel J. Jacob, Ruijun Dang, Yujin J. Oak, Haipeng Lin, Jhoon Kim, Shixian Zhai, Nadia K. Colombi, Drew C. Pendergrass, Ellie Beaudry, Viral Shah, Xu Feng, Robert M. Yantosca, Heesung Chong, Junsung Park, Hanlim Lee, Won-Jin Lee, Soontae Kim, Eunhye Kim, Katherine R. Travis, James H. Crawford, and Hong Liao
Atmos. Chem. Phys., 24, 7027–7039, https://doi.org/10.5194/acp-24-7027-2024, https://doi.org/10.5194/acp-24-7027-2024, 2024
Short summary
Short summary
The Geostationary Environment Monitoring Spectrometer (GEMS) provides hourly measurements of NO2. We use the chemical transport model to find how emissions, chemistry, and transport drive the changes in NO2 observed by GEMS at different times of the day. In winter, the chemistry plays a minor role, and high daytime emissions dominate the diurnal variation in NO2, balanced by transport. In summer, emissions, chemistry, and transport play an important role in shaping the diurnal variation in NO2.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
EGUsphere, https://doi.org/10.5194/egusphere-2024-1715, https://doi.org/10.5194/egusphere-2024-1715, 2024
Short summary
Short summary
Climate change will bring about changes in parameters that are currently used in global-scale models to calculate biogenic emissions. This study seeks to understand the factors driving these models by comparing long-term datasets of biogenic compounds to modeled emissions. We note that the light-dependent fractions currently used in models do not accurately represent regional observations. We provide evidence for the time-dependent variation of this parameter for future modifications to models.
M. Omar Nawaz, Jeremiah Johnson, Greg Yarwood, Benjamin de Foy, Laura Judd, and Daniel L. Goldberg
Atmos. Chem. Phys., 24, 6719–6741, https://doi.org/10.5194/acp-24-6719-2024, https://doi.org/10.5194/acp-24-6719-2024, 2024
Short summary
Short summary
NO2 is a gas with implications for air pollution. A campaign conducted in Houston provided an opportunity to compare NO2 from different instruments and a model. Aircraft and satellite observations agreed well with measurements on the ground; however, the latter estimated lower values. We find that model-simulated NO2 was lower than observations, especially downtown, suggesting that NO2 sources associated with the urban core of Houston, such as vehicle emissions, may be underestimated.
Natalie Brett, Kathy S. Law, Steve R. Arnold, Javier G. Fochesatto, Jean-Christophe Raut, Tatsuo Onishi, Robert Gilliam, Kathleen Fahey, Deanna Huff, George Pouliot, Brice Barret, Elsa Dieudonne, Roman Pohorsky, Julia Schmale, Andrea Baccarini, Slimane Bekki, Gianluca Pappaccogli, Federico Scoto, Stefano Decesari, Antonio Donateo, Meeta Cesler-Maloney, William Simpson, Patrice Medina, Barbara D'Anna, Brice Temime-Roussel, Joel Savarino, Sarah Albertin, Jingqiu Mao, Becky Alexander, Allison Moon, Peter F. DeCarlo, Vanessa Selimovic, Robert Yokelson, and Ellis S. Robinson
EGUsphere, https://doi.org/10.5194/egusphere-2024-1450, https://doi.org/10.5194/egusphere-2024-1450, 2024
Short summary
Short summary
Processes influencing dispersion of local anthropogenic emissions in Arctic wintertime are investigated with dispersion model simulations. Modelled power plant plume rise that considers surface and elevated temperature inversions improves results compared to observations. Modelled near-surface concentrations are improved by representation of vertical mixing and emission estimates. Large increases in diesel vehicle emissions at temperatures reaching -35 °C are required to reproduce observed NOx.
Tianlang Zhao, Jingqiu Mao, Zolal Ayazpour, Gonzalo González Abad, Caroline R. Nowlan, and Yiqi Zheng
Atmos. Chem. Phys., 24, 6105–6121, https://doi.org/10.5194/acp-24-6105-2024, https://doi.org/10.5194/acp-24-6105-2024, 2024
Short summary
Short summary
HCHO variability is a key tracer in understanding VOC emissions in response to climate change. We investigate the role of methane oxidation and biogenic and wildfire emissions in HCHO interannual variability over northern high latitudes in summer, emphasizing wildfires as a key driver of HCHO interannual variability in Alaska, Siberia and northern Canada using satellite HCHO and SIF retrievals and then GEOS-Chem model. We show SIF is a tool to understand biogenic HCHO variability in this region.
Jianghao Li, Alastair C. Lewis, Jim R. Hopkins, Stephen J. Andrews, Tim Murrells, Neil Passant, Ben Richmond, Siqi Hou, William J. Bloss, Roy M. Harrison, and Zongbo Shi
Atmos. Chem. Phys., 24, 6219–6231, https://doi.org/10.5194/acp-24-6219-2024, https://doi.org/10.5194/acp-24-6219-2024, 2024
Short summary
Short summary
A summertime ozone event at an urban site in Birmingham is sensitive to volatile organic compounds (VOCs) – particularly those of oxygenated VOCs. The roles of anthropogenic VOC sources in urban ozone chemistry are examined by integrating the 1990–2019 national atmospheric emission inventory into model scenarios. Road transport remains the most powerful means of further reducing ozone in this case study, but the benefits may be offset if solvent emissions of VOCs continue to increase.
Kai-Lan Chang, Owen R. Cooper, Audrey Gaudel, Irina Petropavlovskikh, Peter Effertz, Gary Morris, and Brian C. McDonald
Atmos. Chem. Phys., 24, 6197–6218, https://doi.org/10.5194/acp-24-6197-2024, https://doi.org/10.5194/acp-24-6197-2024, 2024
Short summary
Short summary
A great majority of observational trend studies of free tropospheric ozone use sparsely sampled ozonesonde and aircraft measurements as reference data sets. A ubiquitous assumption is that trends are accurate and reliable so long as long-term records are available. We show that sampling bias due to sparse samples can persistently reduce the trend accuracy, and we highlight the importance of maintaining adequate frequency and continuity of observations.
Jin Ma, Linda M. J. Kooijmans, Norbert Glatthor, Stephen A. Montzka, Marc von Hobe, Thomas Röckmann, and Maarten C. Krol
Atmos. Chem. Phys., 24, 6047–6070, https://doi.org/10.5194/acp-24-6047-2024, https://doi.org/10.5194/acp-24-6047-2024, 2024
Short summary
Short summary
The global budget of atmospheric COS can be optimised by inverse modelling using TM5-4DVAR, with the co-constraints of NOAA surface observations and MIPAS satellite data. We found reduced COS biosphere uptake from inversions and improved land and ocean separation using MIPAS satellite data assimilation. Further improvements are expected from better quantification of COS ocean and biosphere fluxes.
Fu-Jie Zhu, Zi-Feng Zhang, Li-Yan Liu, Pu-Fei Yang, Peng-Tuan Hu, Geng-Bo Ren, Meng Qin, and Wan-Li Ma
Atmos. Chem. Phys., 24, 6095–6103, https://doi.org/10.5194/acp-24-6095-2024, https://doi.org/10.5194/acp-24-6095-2024, 2024
Short summary
Short summary
Gas–particle (G–P) partitioning is an important atmospheric behavior for semi-volatile organic compounds (SVOCs). Diurnal variation in G–P partitioning of methylated polycyclic aromatic hydrocarbons (Me-PAHs) demonstrates the possible influence of gaseous degradation; the enhancement of gaseous degradation (1.10–5.58 times) on G–P partitioning is verified by a steady-state G–P partitioning model. The effect of gaseous degradation on G–P partitioning of (especially light) SVOCs is important.
Christoph Staehle, Harald E. Rieder, Arlene M. Fiore, and Jordan L. Schnell
Atmos. Chem. Phys., 24, 5953–5969, https://doi.org/10.5194/acp-24-5953-2024, https://doi.org/10.5194/acp-24-5953-2024, 2024
Short summary
Short summary
Chemistry–climate models show biases compared to surface ozone observations and thus require bias correction for impact studies and the assessment of air quality changes. We compare the performance of commonly used correction techniques for model outputs available via CMIP6. While all methods can reduce model biases, better results are obtained from more complex approaches. Thus, our study suggests broader use of these techniques in studies seeking to inform air quality management and policy.
Deepangsu Chatterjee, Randall V. Martin, Chi Li, Dandan Zhang, Haihui Zhu, Daven K. Henze, James H. Crawford, Ronald C. Cohen, Lok N. Lamsal, and Alexander M. Cede
EGUsphere, https://doi.org/10.5194/egusphere-2024-1401, https://doi.org/10.5194/egusphere-2024-1401, 2024
Short summary
Short summary
We investigate the hourly variation of NO2 columns and surface concentrations by applying the GEOS-Chem model to interpret aircraft and ground-based measurements over the US, and Pandora sun photometer measurements over the US, Europe, and Asia. Corrections to the Pandora columns and finer model resolution improve the modeled representation of the summertime hourly variation of total NO2 columns to enable explaining the weaker hourly variation in NO2 columns than at the surface.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William Stockwell, Luc Vereecken, and Tim Wallington
EGUsphere, https://doi.org/10.5194/egusphere-2024-1316, https://doi.org/10.5194/egusphere-2024-1316, 2024
Short summary
Short summary
Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes of the atmospheric composition. Therefore, accurate chemical mechanisms are necessary to predict the evolution of air pollution and climate change. The article describes all steps that are needed to build chemical mechanisms and discusses advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Qindan Zhu, Rebecca H. Schwantes, Matthew Coggon, Colin Harkins, Jordan Schnell, Jian He, Havala O. T. Pye, Meng Li, Barry Baker, Zachary Moon, Ravan Ahmadov, Eva Y. Pfannerstill, Bryan Place, Paul Wooldridge, Benjamin C. Schulze, Caleb Arata, Anthony Bucholtz, John H. Seinfeld, Carsten Warneke, Chelsea E. Stockwell, Lu Xu, Kristen Zuraski, Michael A. Robinson, J. Andrew Neuman, Patrick R. Veres, Jeff Peischl, Steven S. Brown, Allen H. Goldstein, Ronald C. Cohen, and Brian C. McDonald
Atmos. Chem. Phys., 24, 5265–5286, https://doi.org/10.5194/acp-24-5265-2024, https://doi.org/10.5194/acp-24-5265-2024, 2024
Short summary
Short summary
Volatile organic compounds (VOCs) fuel the production of air pollutants like ozone and particulate matter. The representation of VOC chemistry remains challenging due to its complexity in speciation and reactions. Here, we develop a chemical mechanism, RACM2B-VCP, that better represents VOC chemistry in urban areas such as Los Angeles. We also discuss the contribution of VOCs emitted from volatile chemical products and other anthropogenic sources to total VOC reactivity and O3.
Hannah Nesser, Daniel J. Jacob, Joannes D. Maasakkers, Alba Lorente, Zichong Chen, Xiao Lu, Lu Shen, Zhen Qu, Melissa P. Sulprizio, Margaux Winter, Shuang Ma, A. Anthony Bloom, John R. Worden, Robert N. Stavins, and Cynthia A. Randles
Atmos. Chem. Phys., 24, 5069–5091, https://doi.org/10.5194/acp-24-5069-2024, https://doi.org/10.5194/acp-24-5069-2024, 2024
Short summary
Short summary
We quantify 2019 methane emissions in the contiguous US (CONUS) at a ≈ 25 km × 25 km resolution using satellite methane observations. We find a 13 % upward correction to the 2023 US Environmental Protection Agency (EPA) Greenhouse Gas Emissions Inventory (GHGI) for 2019, with large corrections to individual states, urban areas, and landfills. This may present a challenge for US climate policies and goals, many of which target significant reductions in methane emissions.
David de la Paz, Rafael Borge, Juan Manuel de Andrés, Luis Tovar, Golam Sarwar, and Sergey L. Napelenok
Atmos. Chem. Phys., 24, 4949–4972, https://doi.org/10.5194/acp-24-4949-2024, https://doi.org/10.5194/acp-24-4949-2024, 2024
Short summary
Short summary
This source apportionment modeling study shows that around 70 % of ground-level O3 in Madrid (Spain) is transported from other regions. Nonetheless, emissions from local sources, mainly road traffic, play a significant role, especially under atmospheric stagnation. Local measures during those conditions may be able to reduce O3 peaks by up to 30 % and, thus, lessen impacts from high-O3 episodes in the Madrid metropolitan area.
Audrey Fortems-Cheiney, Gregoire Broquet, Elise Potier, Robin Plauchu, Antoine Berchet, Isabelle Pison, Hugo Denier van der Gon, and Stijn Dellaert
Atmos. Chem. Phys., 24, 4635–4649, https://doi.org/10.5194/acp-24-4635-2024, https://doi.org/10.5194/acp-24-4635-2024, 2024
Short summary
Short summary
We have estimated the carbon monixide (CO) European emissions from satellite observations of the MOPITT instrument at the relatively high resolution of 0.5° for a period of over 10 years from 2011 to 2021. The analysis of the inversion results reveals the challenges associated with the inversion of CO emissions at the regional scale over Europe.
Amy Christiansen, Loretta J. Mickley, and Lu Hu
Atmos. Chem. Phys., 24, 4569–4589, https://doi.org/10.5194/acp-24-4569-2024, https://doi.org/10.5194/acp-24-4569-2024, 2024
Short summary
Short summary
In this work, we provide an additional constraint on emissions and trends of nitrogen oxides using nitrate wet deposition (NWD) fluxes over the United States and Europe from 1980–2020. We find that NWD measurements constrain total NOx emissions well. We also find evidence of NOx emission overestimates in both domains, but especially over Europe, where NOx emissions are overestimated by a factor of 2. Reducing NOx emissions over Europe improves model representation of ozone at the surface.
Kiyeon Kim, Kyung Man Han, Chul Han Song, Hyojun Lee, Ross Beardsley, Jinhyeok Yu, Greg Yarwood, Bonyoung Koo, Jasper Madalipay, Jung-Hun Woo, and Seogju Cho
EGUsphere, https://doi.org/10.5194/egusphere-2024-886, https://doi.org/10.5194/egusphere-2024-886, 2024
Short summary
Short summary
We incoporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratios predictions. These results expand our understanding of HONO photochemistry and identify crucial sources of HONO that impact the total HONO budget in Seoul, South Korea. Through this investigation, we contribute to resolving discrepancies in understading chemical transport models, with implications for better air quality mangement and environmental protection in the region.
Eduardo Torre-Pascual, Gotzon Gangoiti, Ana Rodríguez-García, Estibaliz Sáez de Cámara, Joana Ferreira, Carla Gama, María Carmen Gómez, Iñaki Zuazo, Jose Antonio García, and Maite de Blas
Atmos. Chem. Phys., 24, 4305–4329, https://doi.org/10.5194/acp-24-4305-2024, https://doi.org/10.5194/acp-24-4305-2024, 2024
Short summary
Short summary
We present an analysis of an intense air pollution episode of tropospheric ozone (O3) along the Atlantic coast of the Iberian Peninsula, incorporating both measured and simulated parameters. Our study extends beyond surface-level factors to include altitude-related parameters. These episodes stem from upper-atmosphere O3 accumulation in preceding days, transported to surface layers, causing rapid O3 concentration increase.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyong Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
EGUsphere, https://doi.org/10.5194/egusphere-2024-811, https://doi.org/10.5194/egusphere-2024-811, 2024
Short summary
Short summary
We constrain the global emissions of the very potent greenhouse gas sulfur hexafluoride (SF6) between 2005 and 2021. We show, that SF6 emissions are decreasing in the USA and Europe, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, Europe, and China all underestimated their SF6 emissions. However, stringent mitigation measures can successfully reduce SF6 emissions, as can be seen in the EU emission trend.
Hannah Chawner, Eric Saboya, Karina E. Adcock, Tim Arnold, Yuri Artioli, Caroline Dylag, Grant L. Forster, Anita Ganesan, Heather Graven, Gennadi Lessin, Peter Levy, Ingrid T. Luijkx, Alistair Manning, Penelope A. Pickers, Chris Rennick, Christian Rödenbeck, and Matthew Rigby
Atmos. Chem. Phys., 24, 4231–4252, https://doi.org/10.5194/acp-24-4231-2024, https://doi.org/10.5194/acp-24-4231-2024, 2024
Short summary
Short summary
The quantity of atmospheric potential oxygen (APO), derived from coincident measurements of carbon dioxide (CO2) and oxygen (O2), has been proposed as a tracer for fossil fuel CO2 emissions. In this model sensitivity study, we examine the use of APO for this purpose in the UK and compare our model to observations. We find that our model simulations are most sensitive to uncertainties relating to ocean fluxes and boundary conditions.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
EGUsphere, https://doi.org/10.5194/egusphere-2024-916, https://doi.org/10.5194/egusphere-2024-916, 2024
Short summary
Short summary
Reactive loss of VOCs is a long-term issue yet to be resolved in VOC source analyses. This review assesses the common methods and existing issues of reducing losses, impacts of losses, and sources in current source analyses. We provided a potential supporting role in solving the issues of VOC conversion. Source analyses of consumed VOCs produced by reactions for O3 and secondary organic aerosols can play an important role in effective prevention and control of atmospheric secondary pollution.
Meng Li, Junichi Kurokawa, Qiang Zhang, Jung-Hun Woo, Tazuko Morikawa, Satoru Chatani, Zifeng Lu, Yu Song, Guannan Geng, Hanwen Hu, Jinseok Kim, Owen R. Cooper, and Brian C. McDonald
Atmos. Chem. Phys., 24, 3925–3952, https://doi.org/10.5194/acp-24-3925-2024, https://doi.org/10.5194/acp-24-3925-2024, 2024
Short summary
Short summary
In this work, we developed MIXv2, a mosaic Asian emission inventory for 2010–2017. With high spatial (0.1°) and monthly temporal resolution, MIXv2 integrates anthropogenic and open biomass burning emissions across seven sectors following a mosaic methodology. It provides CO2 emissions data alongside nine key pollutants and three chemical mechanisms. Our publicly accessible gridded monthly emissions data can facilitate long-term atmospheric and climate model analyses.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
EGUsphere, https://doi.org/10.5194/egusphere-2024-693, https://doi.org/10.5194/egusphere-2024-693, 2024
Short summary
Short summary
This paper employs a regional chemical transport model to quantify the sensitivity of air pollutants and photochemical parameters to specified emission reductions in China for conditions of winter and summer as representative. The study provides insights into the further air quality control in China with reduced primary emissions.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
EGUsphere, https://doi.org/10.5194/egusphere-2024-715, https://doi.org/10.5194/egusphere-2024-715, 2024
Short summary
Short summary
This work uses WRF-Chem and chemical box modeling to study the gas and aqueous phase production of organic acid concentrations measured in cloud water the summit of Whiteface Mountain on July 1st, 2018. Isoprene was the major source of formic, acetic, and oxalic acid. Gas phase chemistry greatly underestimated formic and acetic acid, indicating missing sources, while cloud chemistry was a key source of oxalic acid. More studies of organic acids are required to better constrain their sources.
Xiaomeng Zhang, Yongjian Lian, Shendong Tan, and Shi Yin
Atmos. Chem. Phys., 24, 3593–3612, https://doi.org/10.5194/acp-24-3593-2024, https://doi.org/10.5194/acp-24-3593-2024, 2024
Short summary
Short summary
Atmospheric new particle formation (NPF) has a significant influence on the global climate, local air quality and human health. Using a combination of quantum chemical calculations and kinetics modeling, we find that thhe gas-phase organosulfate produced from consumption of SO3 can significantly enhance SA–DMA nucleation in the polluted boundary layer, resulting in non-negligible contributions to NPF. Our findings provide important insights into organic sulfur in atmospheric aerosol formation.
Cited articles
Abraham, N. L., Archibald, A. T., Bellouin, N., Boucher, O., Braesicke, P., Bushell, A., Carslaw, K., Collins, B., Dalvi, M., Emmerson, K., Folberth, G., Haywood, J., Johnson, C., Kipling, Z., Macintyre, H., Mann, G., Telford, P., Merikanto, J., Morgenstern, O., Connor, F. O., Ord, C., Osprey, S., Pringle, K., Pyle, J., Rae, J., Reddington, C., Savage, N., Spracklen, D., Stier, P., and West, R.: Unified Model Documentation Paper No. 84: United Kingdom Chemistry and Aerosol (UKCA) Technical Description MetUM Version 8.4, 84, 74, 2012.
Archibald, A. T., Petit, A. S., Percival, C. J., Harvey, J. N., and Shallcross, D. E.: On the importance of the reaction between OH and RO2 radicals, Atmos. Sci. Lett., 10, 102–108, https://doi.org/10.1002/asl.216, 2009.
Archibald, A. T., Cooke, M. C., Utembe, S. R., Shallcross, D. E., Derwent, R. G., and Jenkin, M. E.: Impacts of mechanistic changes on HOx formation and recycling in the oxidation of isoprene, Atmos. Chem. Phys., 10, 8097–8118, https://doi.org/10.5194/acp-10-8097-2010, 2010.
Archibald, A. T., Levine, J. G., Abraham, N. L., Cooke, M. C., Edwards, P. M., Heard, D. E., Jenkin, M. E., Karunaharan, A., Pike, R. C., Monks, P. S., Shallcross, D. E., Telford, P. J., Whalley, L. K., and Pyle, J. A.: Impacts of HOx regeneration and recycling in the oxidation of isoprene: Consequences for the composition of past, present and future atmospheres, Geophys. Res. Lett., 38, 1–6, https://doi.org/10.1029/2010GL046520, 2011.
Assaf, E., Song, B., Tomas, A., Schoemaecker, C., and Fittschen, C.: Rate Constant of the Reaction between CH3O2 Radicals and OH Radicals Revisited, J. Phys. Chem. A, 120, 8923–8932, 2016.
Assaf, E., Tanaka, S., Kajii, Y., Schoemaecker, C., and Fittschen, C.: Rate constants of the reaction of C2-C4 peroxy radicals with OH radicals, Chem. Phys. Lett., 684, 245–249, https://doi.org/10.1016/j.cplett.2017.06.062, 2017a.
Assaf, E., Sheps, L., Whalley, L. K., Heard, D. E., Tomas, A., Schoemaecker, C., and Fittschen, C.: The Reaction between CH3O2 and OH Radicals: Product Yields and Atmospheric Implications, Environ. Sci. Technol., 51, 2170–2177, 2017b.
Banerjee, A., Archibald, A. T., Maycock, A. C., Telford, P., Abraham, N. L., Yang, X., Braesicke, P., and Pyle, J. A.: Lightning NOx, a key chemistry-climate interaction: impacts of future climate change and consequences for tropospheric oxidising capacity, Atmos. Chem. Phys., 14, 9871–9881, https://doi.org/10.5194/acp-14-9871-2014, 2014.
Bossolasco, A., Faragó, E. P., Schoemaecker, C., and Fittschen, C.: Rate constant of the reaction between CH3O2 and OH radicals, Chem. Phys. Lett., 593, 7–13, https://doi.org/10.1016/j.cplett.2013.12.052, 2014.
Burkholder, J. B., Sander, S. P., Abbatt, J. P. D., Barker, J. R., Huie, R. E., Kolb, C. E., Kurylo, M. J., Orkin, V. L., Wilmouth, D. M., and Wine, P. H.: Chemical Kinetics and Photochemical Data for Use in Atmospheric Studies – Evaluation No. 18, JPL Publication 15–10, Jet Propulsion Laboratory, Pasadena, available at: http://jpldataeval.jpl.nasa.gov (last accessed 18 May 2018), 2015.
Di Carlo, P., Brune, W. H., Martinez, M., Harder, H., Lesher, R., Ren, X., Thornberry, T., Carroll, M. A., Young, V., Shepson, P. B., Riemer, D., Apel, E., and Campbell, C.: Missing OH Reactivity in a Forest: Evidence for Unknown Reactive Biogenic VOCs, Science, 304, 722–725, 2004.
Dolgorouky, C., Gros, V., Sarda-Esteve, R., Sinha, V., Williams, J., Marchand, N., Sauvage, S., Poulain, L., Sciare, J., and Bonsang, B.: Total OH reactivity measurements in Paris during the 2010 MEGAPOLI winter campaign, Atmos. Chem. Phys., 12, 9593–9612, https://doi.org/10.5194/acp-12-9593-2012, 2012.
Edwards, P. M., Evans, M. J., Furneaux, K. L., Hopkins, J., Ingham, T., Jones, C., Lee, J. D., Lewis, A. C., Moller, S. J., Stone, D., Whalley, L. K., and Heard, D. E.: OH reactivity in a South East Asian tropical rainforest during the Oxidant and Particle Photochemical Processes (OP3) project, Atmos. Chem. Phys., 13, 9497–9514, https://doi.org/10.5194/acp-13-9497-2013, 2013.
Ehhalt, D., Prather, M., Dentener, F., Derwent, R., Dlugokencky, E., Holland, E., Isaksen, I., Katima, J., Kirchhoff, V., Matson, P., Midgley, P., and Wang, M.: Atmospheric Chemistry and Greenhouse Gases, in Climate Change 2001: The Scientific Basis, Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change, 239–287, 2001.
Elshorbany, Y. F., Kleffmann, J., Hofzumahaus, A., Kurtenbach, R., Wiesen, P., Brauers, T., Bohn, B., Dorn, H. P., Fuchs, H., Holland, F., Rohrer, F., Tillmann, R., Wegener, R., Wahner, A., Kanaya, Y., Yoshino, A., Nishida, S., Kajii, Y., Martinez, M., Kubistin, D., Harder, H., Lelieveld, J., Elste, T., Plass-Dlmer, C., Stange, G., Berresheim, H., and Schurath, U.: HOx budgets during HOxComp: A case study of HOx chemistry under NOx-limited conditions, J. Geophys. Res.-Atmos., 117, 1–16, https://doi.org/10.1029/2011JD017008, 2012.
Faragó, E. P., Schoemaecker, C., Viskolcz, B., and Fittschen, C.: Experimental determination of the rate constant of the reaction between C2H5O2 and OH radicals, Chem. Phys. Lett., 619, 196–200, https://doi.org/10.1016/j.cplett.2014.11.069, 2015.
Fittschen, C., Whalley, L. K., and Heard, D. E.: The reaction of CH3O2 radicals with OH radicals: A neglected sink for CH3O2 in the remote atmosphere, Environ. Sci. Technol., 48, 7700–7701, https://doi.org/10.1021/es502481q, 2014.
Fuchs, H., Novelli, A., Rolletter, M., Hofzumahaus, A., Pfannerstill, E. Y., Kessel, S., Edtbauer, A., Williams, J., Michoud, V., Dusanter, S., Locoge, N., Zannoni, N., Gros, V., Truong, F., Sarda-Esteve, R., Cryer, D. R., Brumby, C. A., Whalley, L. K., Stone, D., Seakins, P. W., Heard, D. E., Schoemaecker, C., Blocquet, M., Coudert, S., Batut, S., Fittschen, C., Thames, A. B., Brune, W. H., Ernest, C., Harder, H., Muller, J. B. A., Elste, T., Kubistin, D., Andres, S., Bohn, B., Hohaus, T., Holland, F., Li, X., Rohrer, F., Kiendler-Scharr, A., Tillmann, R., Wegener, R., Yu, Z., Zou, Q., and Wahner, A.: Comparison of OH reactivity measurements in the atmospheric simulation chamber SAPHIR, Atmos. Meas. Tech., 10, 4023–4053, https://doi.org/10.5194/amt-10-4023-2017, 2017.
Guenther, A., Karl, T., Harley, P., Wiedinmyer, C., Palmer, P. I., and Geron, C.: Estimates of global terrestrial isoprene emissions using MEGAN (Model of Emissions of Gases and Aerosols from Nature), Atmos. Chem. Phys., 6, 3181–3210, https://doi.org/10.5194/acp-6-3181-2006, 2006.
Hansen, R. F., Griffith, S. M., Dusanter, S., Rickly, P. S., Stevens, P. S., Bertman, S. B., Carroll, M. A., Erickson, M. H., Flynn, J. H., Grossberg, N., Jobson, B. T., Lefer, B. L., and Wallace, H. W.: Measurements of total hydroxyl radical reactivity during CABINEX 2009 – Part 1: field measurements, Atmos. Chem. Phys., 14, 2923–2937, https://doi.org/10.5194/acp-14-2923-2014, 2014.
Hansen, R. F., Blocquet, M., Schoemaecker, C., Léonardis, T., Locoge, N., Fittschen, C., Hanoune, B., Stevens, P. S., Sinha, V., and Dusanter, S.: Intercomparison of the comparative reactivity method (CRM) and pump-probe technique for measuring total OH reactivity in an urban environment, Atmos. Meas. Tech., 8, 4243–4264, https://doi.org/10.5194/amt-8-4243-2015, 2015.
Holzinger, R., Lee, A., Paw, K. T., and Goldstein, U. A. H.: Observations of oxidation products above a forest imply biogenic emissions of very reactive compounds, Atmos. Chem. Phys., 5, 67–75, https://doi.org/10.5194/acp-5-67-2005, 2005.
Ingham, T., Goddard, A., Whalley, L. K., Furneaux, K. L., Edwards, P. M., Seal, C. P., Self, D. E., Johnson, G. P., Read, K. A., Lee, J. D., and Heard, D. E.: A flow-tube based laser-induced fluorescence instrument to measure OH reactivity in the troposphere, Atmos. Meas. Tech., 2, 465–477, https://doi.org/10.5194/amt-2-465-2009, 2009.
Jenkin, M. E., Young, J. C., and Rickard, A. R.: The MCM v3.3.1 degradation scheme for isoprene, Atmos. Chem. Phys., 15, 11433–11459, https://doi.org/10.5194/acp-15-11433-2015, 2015.
Kaiser, J., Skog, K. M., Baumann, K., Bertman, S. B., Brown, S. B., Brune, W. H., Crounse, J. D., de Gouw, J. A., Edgerton, E. S., Feiner, P. A., Goldstein, A. H., Koss, A., Misztal, P. K., Nguyen, T. B., Olson, K. F., St. Clair, J. M., Teng, A. P., Toma, S., Wennberg, P. O., Wild, R. J., Zhang, L., and Keutsch, F. N.: Speciation of OH reactivity above the canopy of an isoprene-dominated forest, Atmos. Chem. Phys., 16, 9349–9359, https://doi.org/10.5194/acp-16-9349-2016, 2016.
Khan, M. A. H., Cooke, M. C., Utembe, S. R., Xiao, P., Derwent, R. G., Jenkin, M. E., Archibald, A. T., Maxwell, P., Morris, W. C., South, N., Percival, C. J., and Shallcross, D. E.: Reassessing the photochemical production of methanol from peroxy radical self and cross reactions using the STOCHEM-CRI global chemistry and transport model, Atmos. Environ., 99, 77–84, https://doi.org/10.1016/j.atmosenv.2014.09.056, 2014.
Kovacs, T. A. and Brune, W. H.: Total OH loss rate measurement, J. Atmos. Chem., 39, 105–122, https://doi.org/10.1023/A:1010614113786, 2001.
Kovacs, T. A., Brune, W. H., Harder, H., Martinez, M., Simpas, J. B., Frost, G. J., Williams, E., Jobson, T., Stroud, C., Young, V., Fried, A., and Wert, B.: Direct measurements of urban OH reactivity during Nashville SOS in summer 1999, J. Environ. Monit., 5, 68–74, https://doi.org/10.1039/b204339d, 2003.
Lawrence, M. G., Jöckel, P., and von Kuhlmann, R.: What does the global mean OH concentration tell us?, Atmos. Chem. Phys., 1, 37–49, https://doi.org/10.5194/acp-1-37-2001, 2001.
Lee, J. D., Young, J. C., Read, K. A., Hamilton, J. F., Hopkins, J. R., Lewis, A. C., Bandy, B. J., Davey, J., Edwards, P., Ingham, T., Self, D. E., Smith, S. C., Pilling, M. J., and Heard, D. E.: Measurement and calculation of OH reactivity at a United Kingdom coastal site, J. Atmos. Chem., 64, 53–76, https://doi.org/10.1007/s10874-010-9171-0, 2009.
Lelieveld, J., Peters, W., Dentener, F. J., and Krol, M. C.: Stability of tropospheric hydroxyl chemistry, J. Geophys. Res.-Atmos., 107, 4715, https://doi.org/10.1029/2002JD002272, 2002.
Lelieveld, J., Gromov, S., Pozzer, A., and Taraborrelli, D.: Global tropospheric hydroxyl distribution, budget and reactivity, Atmos. Chem. Phys., 16, 12477–12493, https://doi.org/10.5194/acp-16-12477-2016, 2016.
Liu, Y., Brito, J., Dorris, M. R., Rivera-Rios, J. C., Seco, R., Bates, K. H., Artaxo, P., Duvoisin, S., Keutsch, F. N., Kim, S., Goldstein, A. H., Guenther, A. B., Manzi, A. O., Souza, R. A. F., Springston, S. R., Watson, T. B., McKinney, K. A., and Martin, S. T.: Isoprene photochemistry over the Amazon rainforest, P. Natl. Acad. Sci. USA, 113, 6125–6130, https://doi.org/10.1073/pnas.1524136113, 2016.
Lou, S., Holland, F., Rohrer, F., Lu, K., Bohn, B., Brauers, T., Chang, C. C., Fuchs, H., Häseler, R., Kita, K., Kondo, Y., Li, X., Shao, M., Zeng, L., Wahner, A., Zhang, Y., Wang, W., and Hofzumahaus, A.: Atmospheric OH reactivities in the Pearl River Delta – China in summer 2006: measurement and model results, Atmos. Chem. Phys., 10, 11243–11260, https://doi.org/10.5194/acp-10-11243-2010, 2010.
Lu, K., Zhang, Y., Su, H., Brauers, T., Chou, C. C., Hofzumahaus, A., Liu, S. C., Kita, K., Kondo, Y., Shao, M., Wahner, A., Wang, J., Wang, X., and Zhu, T.: Oxidant (O3 + NO2) production processes and formation regimes in Beijing, J. Geophys. Res., 115, D07303, https://doi.org/10.1029/2009JD012714, 2010.
Mao, J., Ren, X., Brune, W. H., Olson, J. R., Crawford, J. H., Fried, A., Huey, L. G., Cohen, R. C., Heikes, B., Singh, H. B., Blake, D. R., Sachse, G. W., Diskin, G. S., Hall, S. R., and Shetter, R. E.: Airborne measurement of OH reactivity during INTEX-B, Atmos. Chem. Phys., 9, 163–173, https://doi.org/10.5194/acp-9-163-2009, 2009.
Mao, J., Ren, X., Chen, S., Brune, W. H., Chen, Z., Martinez, M., Harder, H., Lefer, B., Rappenglück, B., Flynn, J., and Leuchner, M.: Atmospheric oxidation capacity in the summer of Houston 2006: Comparison with summer measurements in other metropolitan studies, Atmos. Environ., 44, 4107–4115, https://doi.org/10.1016/j.atmosenv.2009.01.013, 2010.
Mao, J., Ren, X., Zhang, L., Van Duin, D. M., Cohen, R. C., Park, J.-H., Goldstein, A. H., Paulot, F., Beaver, M. R., Crounse, J. D., Wennberg, P. O., DiGangi, J. P., Henry, S. B., Keutsch, F. N., Park, C., Schade, G. W., Wolfe, G. M., Thornton, J. A., and Brune, W. H.: Insights into hydroxyl measurements and atmospheric oxidation in a California forest, Atmos. Chem. Phys., 12, 8009–8020, https://doi.org/10.5194/acp-12-8009-2012, 2012.
Martinez, M., Harder, H., Kubistin, D., Rudolf, M., Bozem, H., Eerdekens, G., Fischer, H., Klüpfel, T., Gurk, C., Königstedt, R., Parchatka, U., Schiller, C. L., Stickler, A., Williams, J., and Lelieveld, J.: Hydroxyl radicals in the tropical troposphere over the Suriname rainforest: airborne measurements, Atmos. Chem. Phys., 10, 3759–3773, https://doi.org/10.5194/acp-10-3759-2010, 2010.
Michoud, V., Hansen, R. F., Locoge, N., Stevens, P. S., and Dusanter, S.: Detailed characterizations of the new Mines Douai comparative reactivity method instrument via laboratory experiments and modeling, Atmos. Meas. Tech., 8, 3537–3553, https://doi.org/10.5194/amt-8-3537-2015, 2015.
Millet, D. B., Jacob, D. J., Custer, T. G., de Gouw, J. A., Goldstein, A. H., Karl, T., Singh, H. B., Sive, B. C., Talbot, R. W., Warneke, C., and Williams, J.: New constraints on terrestrial and oceanic sources of atmospheric methanol, Atmos. Chem. Phys., 8, 6887–6905, https://doi.org/10.5194/acp-8-6887-2008, 2008.
Mogensen, D., Smolander, S., Sogachev, A., Zhou, L., Sinha, V., Guenther, A., Williams, J., Nieminen, T., Kajos, M. K., Rinne, J., Kulmala, M., and Boy, M.: Modelling atmospheric OH-reactivity in a boreal forest ecosystem, Atmos. Chem. Phys., 11, 9709–9719, https://doi.org/10.5194/acp-11-9709-2011, 2011.
Morgenstern, O., Braesicke, P., O'Connor, F. M., Bushell, A. C., Johnson, C. E., Osprey, S. M., and Pyle, J. A.: Evaluation of the new UKCA climate-composition model – Part 1: The stratosphere, Geosci. Model Dev., 2, 43–57, https://doi.org/10.5194/gmd-2-43-2009, 2009.
Müller, J.-F., Liu, Z., Nguyen, V. S., Stavrakou, T., Harvey, J. N., and Peeters, J.: The reaction of methyl peroxy and hydroxyl radicals as a major source of atmospheric methanol, Nature Commun., 7, 13213, https://doi.org/10.1038/ncomms13213, 2016.
Naik, V., Voulgarakis, A., Fiore, A. M., Horowitz, L. W., Lamarque, J.-F., Lin, M., Prather, M. J., Young, P. J., Bergmann, D., Cameron-Smith, P. J., Cionni, I., Collins, W. J., Dalsøren, S. B., Doherty, R., Eyring, V., Faluvegi, G., Folberth, G. A., Josse, B., Lee, Y. H., MacKenzie, I. A., Nagashima, T., van Noije, T. P. C., Plummer, D. A., Righi, M., Rumbold, S. T., Skeie, R., Shindell, D. T., Stevenson, D. S., Strode, S., Sudo, K., Szopa, S., and Zeng, G.: Preindustrial to present-day changes in tropospheric hydroxyl radical and methane lifetime from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), Atmos. Chem. Phys., 13, 5277–5298, https://doi.org/10.5194/acp-13-5277-2013, 2013.
Nakashima, Y., Kato, S., Greenberg, J., Harley, P., Karl, T., Turnipseed, A., Apel, E., Guenther, A., Smith, J., and Kajii, Y.: Total OH reactivity measurements in ambient air in a southern Rocky mountain ponderosa pine forest during BEACHON-SRM08 summer campaign, Atmos. Environ., 85, 1–8, https://doi.org/10.1016/j.atmosenv.2013.11.042, 2014.
Nölscher, A. C., Williams, J., Sinha, V., Custer, T., Song, W., Johnson, A. M., Axinte, R., Bozem, H., Fischer, H., Pouvesle, N., Phillips, G., Crowley, J. N., Rantala, P., Rinne, J., Kulmala, M., Gonzales, D., Valverde-Canossa, J., Vogel, A., Hoffmann, T., Ouwersloot, H. G., Vilà-Guerau de Arellano, J., and Lelieveld, J.: Summertime total OH reactivity measurements from boreal forest during HUMPPA-COPEC 2010, Atmos. Chem. Phys., 12, 8257–8270, https://doi.org/10.5194/acp-12-8257-2012, 2012.
Nölscher, A. C., Yañez-Serrano, A. M., Wolff, S., de Araujo, A. C., Lavrič, J. V, Kesselmeier, J., and Williams, J.: Unexpected seasonality in quantity and composition of Amazon rainforest air reactivity., Nature Commun., 7, 10383, https://doi.org/10.1038/ncomms10383, 2016.
O'Connor, F. M., Johnson, C. E., Morgenstern, O., Abraham, N. L., Braesicke, P., Dalvi, M., Folberth, G. A., Sanderson, M. G., Telford, P. J., Voulgarakis, A., Young, P. J., Zeng, G., Collins, W. J., and Pyle, J. A.: Evaluation of the new UKCA climate-composition model – Part 2: The Troposphere, Geosci. Model Dev., 7, 41–91, https://doi.org/10.5194/gmd-7-41-2014, 2014
Ren, X., Harder, H., Martinez, M., Lesher, R. L., Oliger, A., Shirley, T., Adams, J., Simpas, J. B., and Brune, W. H.: HOx concentrations and OH reactivity observations in New York City during PMTACS-NY2001, Atmos. Environ., 37, 3627–3637, https://doi.org/10.1016/S1352-2310(03)00460-6, 2003a.
Ren, X., Harder, H., Martinez, M., Lesher, R. L., Oliger, A., Simpas, J. B., Brune, W. H., Schwab, J. J., Demerjian, K. L., He, Y., Zhou, X., and Gao, H.: OH and HO2 chemistry in the urban atmosphere of New York City, Atmos. Environ., 37, 3639–3651, https://doi.org/10.1016/S1352-2310(03)00459-X, 2003b.
Ren, X., Brune, W. H., Cantrell, C. A., Edwards, G. D., Shirley, T., Metcalf, A. R., and Lesher, R. L.: Hydroxyl and peroxy radical chemistry in a rural area of central Pennsylvania: Observations and model comparisons, J. Atmos. Chem., 52, 231–257, https://doi.org/10.1007/s10874-005-3651-7, 2005.
Ren, X., Brune, W. H., Mao, J., Mitchell, M. J., Lesher, R. L., Simpas, J. B., Metcalf, A. R., Schwab, J. J., Cai, C., Li, Y., Demerjian, K. L., Felton, H. D., Boynton, G., Adams, A., Perry, J., He, Y., Zhou, X., and Hou, J.: Behavior of OH and HO2 in the winter atmosphere in New York City, Atmos. Environ., 40, 252–263, https://doi.org/10.1016/j.atmosenv.2005.11.073, 2006a.
Ren, X., Brune, W. H., Oliger, A., Metcalf, A. R., Simpas, J. B., Shirley, T., Schwab, J. J., Bai, C., Roychowdhury, U., Li, Y., Cai, C., Demerjian, K. L., He, Y., Zhou, X., Gao, H., and Hou, J.: OH, HO2, and OH reactivity during the PMTACS-NY Whiteface Mountain 2002 campaign: Obervations and model comparison, J. Geophys. Res.-Atmos., 111, 1–12, https://doi.org/10.1029/2005JD006126, 2006b.
Safieddine, S. A., Heald, C. L., and Henderson, B. H.: The global nonmethane reactive organic carbon budget: A modeling perspective, Geophys. Res. Lett., 44, 3897–3906, https://doi.org/10.1002/2017GL072602, 2017.
Shirley, T. R., Brune, W. H., Ren, X., Mao, J., Lesher, R., Cardenas, B., Volkamer, R., Molina, L. T., Molina, M. J., Lamb, B., Velasco, E., Jobson, T., and Alexander, M.: Atmospheric oxidation in the Mexico City Metropolitan Area (MCMA) during April 2003, Atmos. Chem. Phys., 6, 2753–2765, https://doi.org/10.5194/acp-6-2753-2006, 2006.
Sinha, V., Williams, J., Crowley, J. N., and Lelieveld, J.: The Comparative Reactivity Method – a new tool to measure total OH Reactivity in ambient air, Atmos. Chem. Phys., 8, 2213–2227, https://doi.org/10.5194/acp-8-2213-2008, 2008.
Sinha, V., Williams, J., Lelieveld, J., Ruuskanen, T. M., Kajos, M. K., Patokoski, J., Hellen, H., Hakola, H., Mogensen, D., Boy, M., Rinne, J., and Kulmala, M.: OH reactivity measurements within a boreal forest: Evidence for unknown reactive emissions, Environ. Sci. Technol., 44, 6614–6620, https://doi.org/10.1021/es101780b, 2010.
Sinha, V., Williams, J., Diesch, J. M., Drewnick, F., Martinez, M., Harder, H., Regelin, E., Kubistin, D., Bozem, H., Hosaynali-Beygi, Z., Fischer, H., Andrés-Hernández, M. D., Kartal, D., Adame, J. A., and Lelieveld, J.: Constraints on instantaneous ozone production rates and regimes during DOMINO derived using in-situ OH reactivity measurements, Atmos. Chem. Phys., 12, 7269–7283, https://doi.org/10.5194/acp-12-7269-2012, 2012.
Squire, O. J., Archibald, A. T., Griffiths, P. T., Jenkin, M. E., Smith, D., and Pyle, J. A.: Influence of isoprene chemical mechanism on modelled changes in tropospheric ozone due to climate and land use over the 21st century, Atmos. Chem. Phys., 15, 5123–5143, https://doi.org/10.5194/acp-15-5123-2015, 2015.
Stevenson, D. S., Dentener, F. J., Schultz, M. G., Ellingsen, K., van Noije, T. P. C., Wild, O., Zeng, G., Amann, M., Atherton, C. S., Bell, N., Bergmann, D. J., Bey, I., Butler, T., Cofala, J., Collins, W. J., Derwent, R. G., Doherty, R. M., Drevet, J., Eskes, H. J., Fiore, A. M., Gauss, M., Hauglustaine, D. A., Horowitz, L. W., Isaksen, I. S. A., Krol, M. C., Lamarque, J. F., Lawrence, M. G., Montanaro, V., Müller, J. F., Pitari, G., Prather, M. J., Pyle, J. A., Rast, S., Rodriquez, J. M., Sanderson, M. G., Savage, N. H., Shindell, D. T., Strahan, S. E., Sudo, K., and Szopa, S.: Multimodel ensemble simulations of present-day and near-future tropospheric ozone, J. Geophys. Res.-Atmos., 111, D08301, https://doi.org/10.1029/2005JD006338, 2006.
Voulgarakis, A., Naik, V., Lamarque, J.-F., Shindell, D. T., Young, P. J., Prather, M. J., Wild, O., Field, R. D., Bergmann, D., Cameron-Smith, P., Cionni, I., Collins, W. J., Dalsøren, S. B., Doherty, R. M., Eyring, V., Faluvegi, G., Folberth, G. A., Horowitz, L. W., Josse, B., MacKenzie, I. A., Nagashima, T., Plummer, D. A., Righi, M., Rumbold, S. T., Stevenson, D. S., Strode, S. A., Sudo, K., Szopa, S., and Zeng, G.: Analysis of present day and future OH and methane lifetime in the ACCMIP simulations, Atmos. Chem. Phys., 13, 2563–2587, https://doi.org/10.5194/acp-13-2563-2013, 2013.
Whalley, L. K., Stone, D., Bandy, B., Dunmore, R., Hamilton, J. F., Hopkins, J., Lee, J. D., Lewis, A. C., and Heard, D. E.: Atmospheric OH reactivity in central London: observations, model predictions and estimates of in situ ozone production, Atmos. Chem. Phys., 16, 2109–2122, https://doi.org/10.5194/acp-16-2109-2016, 2016.
Yan, C., Kocevska, S., and Krasnoperov, L. N.: Kinetics of the Reaction of CH3O2 Radicals with OH Studied over the 292–526 K Temperature Range, J. Phys. Chem. A, 120, 6111–6121, https://doi.org/10.1021/acs.jpca.6b04213, 2016.
Yang, Y., Shao, M., Wang, X., Nölscher, A. C., Kessel, S., Guenther, A., and Williams, J.: Towards a quantitative understanding of total OH reactivity: A review, Atmos. Environ., 134, 147–161, https://doi.org/10.1016/j.atmosenv.2016.03.010, 2016.
Yang, Y., Shao, M., Keßel, S., Li, Y., Lu, K., Lu, S., Williams, J., Zhang, Y., Zeng, L., Nölscher, A. C., Wu, Y., Wang, X., and Zheng, J.: How the OH reactivity affects the ozone production efficiency: case studies in Beijing and Heshan, China, Atmos. Chem. Phys., 17, 7127–7142, https://doi.org/10.5194/acp-17-7127-2017, 2017.
Young, P. J., Archibald, A. T., Bowman, K. W., Lamarque, J.-F., Naik, V., Stevenson, D. S., Tilmes, S., Voulgarakis, A., Wild, O., Bergmann, D., Cameron-Smith, P., Cionni, I., Collins, W. J., Dalsøren, S. B., Doherty, R. M., Eyring, V., Faluvegi, G., Horowitz, L. W., Josse, B., Lee, Y. H., MacKenzie, I. A., Nagashima, T., Plummer, D. A., Righi, M., Rumbold, S. T., Skeie, R. B., Shindell, D. T., Strode, S. A., Sudo, K., Szopa, S., and Zeng, G.: Pre-industrial to end 21st century projections of tropospheric ozone from the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP), Atmos. Chem. Phys., 13, 2063–2090, https://doi.org/10.5194/acp-13-2063-2013, 2013.
Zannoni, N., Gros, V., Lanza, M., Sarda, R., Bonsang, B., Kalogridis, C., Preunkert, S., Legrand, M., Jambert, C., Boissard, C., and Lathiere, J.: OH reactivity and concentrations of biogenic volatile organic compounds in a Mediterranean forest of downy oak trees, Atmos. Chem. Phys., 16, 1619–1636, https://doi.org/10.5194/acp-16-1619-2016, 2016.
Zannoni, N., Gros, V., Sarda Esteve, R., Kalogridis, C., Michoud, V., Dusanter, S., Sauvage, S., Locoge, N., Colomb, A., and Bonsang, B.: Summertime OH reactivity from a receptor coastal site in the Mediterranean Basin, Atmos. Chem. Phys., 17, 12645–12658, https://doi.org/10.5194/acp-17-12645-2017, 2017.
Short summary
Hydroxyl radicals (OH) control the removal of species emitted in the atmosphere. Field campaigns reported a "missing" OH sink, not included in current atmospheric models. In this work a global model was used to establish the impact of additional OH sinks, based on both observations of the missing sink and newly discovered reactions of OH. Results show modest increases in global atmospheric lifetimes but pronounced regional effects on the abundance of some key species.
Hydroxyl radicals (OH) control the removal of species emitted in the atmosphere. Field campaigns...
Altmetrics
Final-revised paper
Preprint