Articles | Volume 18, issue 6
https://doi.org/10.5194/acp-18-4329-2018
© 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-18-4329-2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
28 Mar 2018
Research article |
| 28 Mar 2018
| 28 Mar 2018
A revised global ozone dry deposition estimate based on a new two-layer parameterisation for air–sea exchange and the multi-year MACC composition reanalysis
CSIRO Oceans and Atmosphere, Aspendale, 3195, Australia
Matthew T. Woodhouse
CSIRO Oceans and Atmosphere, Aspendale, 3195, Australia
Ian E. Galbally
CSIRO Oceans and Atmosphere, Aspendale, 3195, Australia
Related authors
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
Short summary
Short summary
Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Ashok K. Luhar, Ian E. Galbally, and Matthew T. Woodhouse
Atmos. Chem. Phys., 22, 13013–13033, https://doi.org/10.5194/acp-22-13013-2022, https://doi.org/10.5194/acp-22-13013-2022, 2022
Short summary
Short summary
Recent improvements to global parameterisations of oceanic ozone dry deposition and lightning-generated oxides of nitrogen (LNOx) have consequent impacts on earth's radiative fluxes. Uncertainty in radiative fluxes arising from uncertainty in LNOx is of significant magnitude in comparison with the
present-dayIPCC AR6 anthropogenic effective radiative forcing (ERF) due to ozone. Hence, uncertainty in LNOx needs to be explicitly addressed in relation to the GWP and ERF of anthropogenic methane.
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.
Ashok K. Luhar, David M. Etheridge, Zoë M. Loh, Julie Noonan, Darren Spencer, Lisa Smith, and Cindy Ong
Atmos. Chem. Phys., 20, 15487–15511, https://doi.org/10.5194/acp-20-15487-2020, https://doi.org/10.5194/acp-20-15487-2020, 2020
Short summary
Short summary
With the sharp rise in coal seam gas (CSG) production in Queensland’s Surat Basin, there is much interest in quantifying methane emissions from this area and from unconventional gas production in general. We develop and apply a regional Bayesian inverse model that uses hourly methane concentration data from two sites and modelled backward dispersion to quantify emissions. The model requires a narrow prior and suggests that the emissions from the CSG areas are 33% larger than bottom-up estimates.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Marcus Thatcher
Atmos. Chem. Phys., 17, 3749–3767, https://doi.org/10.5194/acp-17-3749-2017, https://doi.org/10.5194/acp-17-3749-2017, 2017
Short summary
Short summary
Dry deposition of tropospheric ozone relates to its destruction at the Earth’s surface. An improved model scheme for such deposition to the ocean is formulated backed up by field data. It results in the oceanic dry deposition of ozone to be 12 % of the global total, which is much lower than the current model estimate of about 30 %. This result has implications for modelling global tropospheric ozone budget and its radiative forcing, and ozone mixing ratios, especially in the Southern Hemisphere.
Ashok K. Luhar, Anthony C. Jones, and Jonathan M. Wilkinson
Atmos. Chem. Phys., 24, 14005–14028, https://doi.org/10.5194/acp-24-14005-2024, https://doi.org/10.5194/acp-24-14005-2024, 2024
Short summary
Short summary
Nitrate aerosol is often omitted in global chemistry–climate models, partly due to the chemical complexity of its formation process. Using a global model, we show that including nitrate aerosol significantly impacts tropospheric composition fields, such as ozone, and radiation. Additionally, lightning-generated oxides of nitrogen influence both nitrate aerosol mass concentrations and aerosol size distribution, which has important implications for radiative fluxes and indirect aerosol effects.
Sonya L. Fiddes, Matthew T. Woodhouse, Marc D. Mallet, Liam Lamprey, Ruhi S. Humphries, Alain Protat, Simon P. Alexander, Hakase Hayashida, Samuel G. Putland, Branka Miljevic, and Robyn Schofield
EGUsphere, https://doi.org/10.5194/egusphere-2024-3125, https://doi.org/10.5194/egusphere-2024-3125, 2024
Short summary
Short summary
The interaction between natural marine aerosols, clouds and radiation in the Southern Ocean is a major source of uncertainty in climate models. We evaluate the Australian climate model using aerosol observations and find it underestimates aerosol number often by over 50 %. Model changes were tested to improve aerosol concentrations, but some of our changes had severe negative effects on the larger climate system, highlighting issues in aerosol-cloud interaction modelling.
Sonya L. Fiddes, Marc D. Mallet, Alain Protat, Matthew T. Woodhouse, Simon P. Alexander, and Kalli Furtado
Geosci. Model Dev., 17, 2641–2662, https://doi.org/10.5194/gmd-17-2641-2024, https://doi.org/10.5194/gmd-17-2641-2024, 2024
Short summary
Short summary
In this study we present an evaluation that considers complex, non-linear systems in a holistic manner. This study uses XGBoost, a machine learning algorithm, to predict the simulated Southern Ocean shortwave radiation bias in the ACCESS model using cloud property biases as predictors. We then used a novel feature importance analysis to quantify the role that each cloud bias plays in predicting the radiative bias, laying the foundation for advanced Earth system model evaluation and development.
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.
Sonya L. Fiddes, Alain Protat, Marc D. Mallet, Simon P. Alexander, and Matthew T. Woodhouse
Atmos. Chem. Phys., 22, 14603–14630, https://doi.org/10.5194/acp-22-14603-2022, https://doi.org/10.5194/acp-22-14603-2022, 2022
Short summary
Short summary
Climate models have difficulty simulating Southern Ocean clouds, impacting how much sunlight reaches the surface. We use machine learning to group different cloud types observed from satellites and simulated in a climate model. We find the model does a poor job of simulating the same cloud type as what the satellite shows and, even when it does, the cloud properties and amount of reflected sunlight are incorrect. We have a lot of work to do to model clouds correctly over the Southern Ocean.
Ashok K. Luhar, Ian E. Galbally, and Matthew T. Woodhouse
Atmos. Chem. Phys., 22, 13013–13033, https://doi.org/10.5194/acp-22-13013-2022, https://doi.org/10.5194/acp-22-13013-2022, 2022
Short summary
Short summary
Recent improvements to global parameterisations of oceanic ozone dry deposition and lightning-generated oxides of nitrogen (LNOx) have consequent impacts on earth's radiative fluxes. Uncertainty in radiative fluxes arising from uncertainty in LNOx is of significant magnitude in comparison with the
present-dayIPCC AR6 anthropogenic effective radiative forcing (ERF) due to ozone. Hence, uncertainty in LNOx needs to be explicitly addressed in relation to the GWP and ERF of anthropogenic methane.
Sonya L. Fiddes, Matthew T. Woodhouse, Steve Utembe, Robyn Schofield, Simon P. Alexander, Joel Alroe, Scott D. Chambers, Zhenyi Chen, Luke Cravigan, Erin Dunne, Ruhi S. Humphries, Graham Johnson, Melita D. Keywood, Todd P. Lane, Branka Miljevic, Yuko Omori, Alain Protat, Zoran Ristovski, Paul Selleck, Hilton B. Swan, Hiroshi Tanimoto, Jason P. Ward, and Alastair G. Williams
Atmos. Chem. Phys., 22, 2419–2445, https://doi.org/10.5194/acp-22-2419-2022, https://doi.org/10.5194/acp-22-2419-2022, 2022
Short summary
Short summary
Coral reefs have been found to produce the climatically relevant chemical compound dimethyl sulfide (DMS). It has been suggested that corals can modify their environment via the production of DMS. We use an atmospheric chemistry model to test this theory at a regional scale for the first time. We find that it is unlikely that coral-reef-derived DMS has an influence over local climate, in part due to the proximity to terrestrial and anthropogenic aerosol sources.
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.
Sonya L. Fiddes, Matthew T. Woodhouse, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 21, 5883–5903, https://doi.org/10.5194/acp-21-5883-2021, https://doi.org/10.5194/acp-21-5883-2021, 2021
Short summary
Short summary
Coral reefs are known to produce the aerosol precursor dimethyl sulfide (DMS). Currently, this source of coral DMS is unaccounted for in climate modelling, and the impact of coral reef extinction on aerosol and climate is unknown. In this study, we address this problem using a coupled chemistry–climate model for the first time. We find that coral reefs make a minimal contribution to the aerosol population and are unlikely to play a role in climate modulation.
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.
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.
Ashok K. Luhar, David M. Etheridge, Zoë M. Loh, Julie Noonan, Darren Spencer, Lisa Smith, and Cindy Ong
Atmos. Chem. Phys., 20, 15487–15511, https://doi.org/10.5194/acp-20-15487-2020, https://doi.org/10.5194/acp-20-15487-2020, 2020
Short summary
Short summary
With the sharp rise in coal seam gas (CSG) production in Queensland’s Surat Basin, there is much interest in quantifying methane emissions from this area and from unconventional gas production in general. We develop and apply a regional Bayesian inverse model that uses hourly methane concentration data from two sites and modelled backward dispersion to quantify emissions. The model requires a narrow prior and suggests that the emissions from the CSG areas are 33% larger than bottom-up estimates.
Rebecca L. Jackson, Albert J. Gabric, Roger Cropp, and Matthew T. Woodhouse
Biogeosciences, 17, 2181–2204, https://doi.org/10.5194/bg-17-2181-2020, https://doi.org/10.5194/bg-17-2181-2020, 2020
Short summary
Short summary
Coral reefs are a strong source of atmospheric sulfur through stress-induced emissions of dimethylsulfide (DMS). This biogenic sulfur can influence aerosol and cloud properties and, consequently, the radiative balance over the ocean. DMS emissions may therefore help to mitigate coral physiological stress via increased low-level cloud cover and reduced sea surface temperature. The importance of DMS in coral physiology and climate is reviewed and the implications for coral bleaching are discussed.
Melita Keywood, Paul Selleck, Fabienne Reisen, David Cohen, Scott Chambers, Min Cheng, Martin Cope, Suzanne Crumeyrolle, Erin Dunne, Kathryn Emmerson, Rosemary Fedele, Ian Galbally, Rob Gillett, Alan Griffiths, Elise-Andree Guerette, James Harnwell, Ruhi Humphries, Sarah Lawson, Branka Miljevic, Suzie Molloy, Jennifer Powell, Jack Simmons, Zoran Ristovski, and Jason Ward
Earth Syst. Sci. Data, 11, 1883–1903, https://doi.org/10.5194/essd-11-1883-2019, https://doi.org/10.5194/essd-11-1883-2019, 2019
Short summary
Short summary
The Sydney Particle Study increased scientific knowledge of the processes leading to particle formation and transformations in Sydney through two comprehensive observation programs which are described in detail here. The data set and its analysis underpin comprehensive chemical transport modelling tools that can be used to assist in the development of a long-term control strategy for particles in Sydney and thus reduce the impact of particles on human health.
Sonya L. Fiddes, Matthew T. Woodhouse, Zebedee Nicholls, Todd P. Lane, and Robyn Schofield
Atmos. Chem. Phys., 18, 10177–10198, https://doi.org/10.5194/acp-18-10177-2018, https://doi.org/10.5194/acp-18-10177-2018, 2018
Short summary
Short summary
The role of natural aerosol in the climate system is uncertain. A key contributor to marine aerosol is dimethyl sulfide (DMS), released by phytoplankton in the oceans. We study the effect of DMS on clouds and rain using a climate model with a detailed aerosol scheme. We show that DMS acts to reduce rainfall in cloud deck regions, leading to longer lived clouds and a large impact on solar energy reaching the surface. Further study of these areas will improve future climate projections.
Kathryn M. Emmerson, Martin E. Cope, Ian E. Galbally, Sunhee Lee, and Peter F. Nelson
Atmos. Chem. Phys., 18, 7539–7556, https://doi.org/10.5194/acp-18-7539-2018, https://doi.org/10.5194/acp-18-7539-2018, 2018
Short summary
Short summary
We compare the CSIRO in-house biogenic emissions model (ABCGEM) with the Model of Emissions of Gases and Aerosols from Nature (MEGAN), for eucalypt-rich south-east Australia. Differences in emissions are not only due to the emission factors, but also how these emission factors are processed. ABCGEM assumes monoterpenes are not light dependent, whilst MEGAN does. Comparison with observations suggests that Australian monoterpenes may not be as light dependent as other vegetation globally.
Erin Dunne, Ian E. Galbally, Min Cheng, Paul Selleck, Suzie B. Molloy, and Sarah J. Lawson
Atmos. Meas. Tech., 11, 141–159, https://doi.org/10.5194/amt-11-141-2018, https://doi.org/10.5194/amt-11-141-2018, 2018
Short summary
Short summary
A comparison of measurements of 7 volatile organic compounds (VOCs) in urban air by 3 different methods is presented. An uncertainty was calculated for each method and VOCs measured to provide some idea of the reliability of the data. Even when this uncertainty was accounted for, the measurements from the different methods did not agree for 4 of the 7 VOCs. Thus, there is unaccounted uncertainty in VOC measurements which must be considered when utilizing the data and assessing their reliability.
Sarah J. Lawson, Martin Cope, Sunhee Lee, Ian E. Galbally, Zoran Ristovski, and Melita D. Keywood
Atmos. Chem. Phys., 17, 11707–11726, https://doi.org/10.5194/acp-17-11707-2017, https://doi.org/10.5194/acp-17-11707-2017, 2017
Short summary
Short summary
A high-resolution chemical transport model was used to reproduce observed smoke plumes. The model output was highly sensitive to fire emission factors and meteorology, particularly for secondary pollutant ozone. Aged urban air (age = 2 days) was the major source of ozone observed, with minor contributions from the fire. This work highlights the importance of assessing model sensitivity and the use of modelling to determine the contribution from different sources to atmospheric composition.
Clare Paton-Walsh, Élise-Andrée Guérette, Dagmar Kubistin, Ruhi Humphries, Stephen R. Wilson, Doreena Dominick, Ian Galbally, Rebecca Buchholz, Mahendra Bhujel, Scott Chambers, Min Cheng, Martin Cope, Perry Davy, Kathryn Emmerson, David W. T. Griffith, Alan Griffiths, Melita Keywood, Sarah Lawson, Suzie Molloy, Géraldine Rea, Paul Selleck, Xue Shi, Jack Simmons, and Voltaire Velazco
Earth Syst. Sci. Data, 9, 349–362, https://doi.org/10.5194/essd-9-349-2017, https://doi.org/10.5194/essd-9-349-2017, 2017
Short summary
Short summary
The MUMBA campaign provides a detailed snapshot of the atmospheric composition in an urban coastal environment with strong biogenic sources nearby. This campaign involved collaboration between several institutes and was undertaken to provide a case study for atmospheric models in a poorly sampled region of the globe.
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Marcus Thatcher
Atmos. Chem. Phys., 17, 3749–3767, https://doi.org/10.5194/acp-17-3749-2017, https://doi.org/10.5194/acp-17-3749-2017, 2017
Short summary
Short summary
Dry deposition of tropospheric ozone relates to its destruction at the Earth’s surface. An improved model scheme for such deposition to the ocean is formulated backed up by field data. It results in the oceanic dry deposition of ozone to be 12 % of the global total, which is much lower than the current model estimate of about 30 %. This result has implications for modelling global tropospheric ozone budget and its radiative forcing, and ozone mixing ratios, especially in the Southern Hemisphere.
Kathryn M. Emmerson, Ian E. Galbally, Alex B. Guenther, Clare Paton-Walsh, Elise-Andree Guerette, Martin E. Cope, Melita D. Keywood, Sarah J. Lawson, Suzie B. Molloy, Erin Dunne, Marcus Thatcher, Thomas Karl, and Simin D. Maleknia
Atmos. Chem. Phys., 16, 6997–7011, https://doi.org/10.5194/acp-16-6997-2016, https://doi.org/10.5194/acp-16-6997-2016, 2016
Short summary
Short summary
We have tested how a model using a global inventory of plant-based emissions compares with four sets of measurements made in southeast Australia. This region is known for its eucalypt species, which dominate the summertime global inventory. The Australian part of the inventory has been produced using measurements made on eucalypt saplings. The model could not match the measurements, and the inventory needs to be improved by taking measurements of a wider range of Australian plant types and ages.
E. D. Sofen, D. Bowdalo, M. J. Evans, F. Apadula, P. Bonasoni, M. Cupeiro, R. Ellul, I. E. Galbally, R. Girgzdiene, S. Luppo, M. Mimouni, A. C. Nahas, M. Saliba, and K. Tørseth
Earth Syst. Sci. Data, 8, 41–59, https://doi.org/10.5194/essd-8-41-2016, https://doi.org/10.5194/essd-8-41-2016, 2016
Short summary
Short summary
We have brought together all publicly available surface ozone observations from online databases from 1971–2015, with 2200 sites representing regional background conditions appropriate for the evaluation of chemical transport and chemistry-climate models for projects such as the Chemistry-Climate Model Initiative. Gridded data sets of ozone metrics (mean, percentiles, MDA8, SOMO35, etc.) are available from the British Atmospheric Data Centre.
E. W. Butt, A. Rap, A. Schmidt, C. E. Scott, K. J. Pringle, C. L. Reddington, N. A. D. Richards, M. T. Woodhouse, J. Ramirez-Villegas, H. Yang, V. Vakkari, E. A. Stone, M. Rupakheti, P. S. Praveen, P. G. van Zyl, J. P. Beukes, M. Josipovic, E. J. S. Mitchell, S. M. Sallu, P. M. Forster, and D. V. Spracklen
Atmos. Chem. Phys., 16, 873–905, https://doi.org/10.5194/acp-16-873-2016, https://doi.org/10.5194/acp-16-873-2016, 2016
Short summary
Short summary
We estimate the impact of residential emissions (cooking and heating) on atmospheric aerosol, human health, and climate. We find large contributions to annual mean ambient PM2.5 in residential sources regions resulting in significant but uncertain global premature mortality when key uncertainties in emission flux are considered. We show that residential emissions exert an uncertain global radiative effect and suggest more work is needed to characterise residential emissions climate importance.
S. J. Lawson, M. D. Keywood, I. E. Galbally, J. L. Gras, J. M. Cainey, M. E. Cope, P. B. Krummel, P. J. Fraser, L. P. Steele, S. T. Bentley, C. P. Meyer, Z. Ristovski, and A. H. Goldstein
Atmos. Chem. Phys., 15, 13393–13411, https://doi.org/10.5194/acp-15-13393-2015, https://doi.org/10.5194/acp-15-13393-2015, 2015
Short summary
Short summary
Biomass burning (BB) plumes were opportunistically measured at the Cape Grim Baseline Station in Tasmania, Australia. We provide a unique set of trace gas and particle emission factors for temperate Australian coastal heathland fires, and attribute a major short-lived enhancement in emission ratios to a minor rainfall event. The ability of BB particles to act as cloud condensation nuclei, and the contribution of BB emissions to observed particle growth and ozone enhancements are discussed.
R. S. Humphries, R. Schofield, M. D. Keywood, J. Ward, J. R. Pierce, C. M. Gionfriddo, M. T. Tate, D. P. Krabbenhoft, I. E. Galbally, S. B. Molloy, A. R. Klekociuk, P. V. Johnston, K. Kreher, A. J. Thomas, A. D. Robinson, N. R. P. Harris, R. Johnson, and S. R. Wilson
Atmos. Chem. Phys., 15, 13339–13364, https://doi.org/10.5194/acp-15-13339-2015, https://doi.org/10.5194/acp-15-13339-2015, 2015
Short summary
Short summary
An atmospheric new particle formation event that was observed in the pristine East Antarctic pack ice during a springtime voyage in 2012 is characterised in terms of formation and growth rates. Known nucleation mechanisms (e.g. those involving sulfate, iodine and organics) were unable to explain observations; however, correlations with total gaseous mercury were found, leading to the suggestion of a possible mercury-driven nucleation mechanism not previously described.
S. T. Turnock, D. V. Spracklen, K. S. Carslaw, G. W. Mann, M. T. Woodhouse, P. M. Forster, J. Haywood, C. E. Johnson, M. Dalvi, N. Bellouin, and A. Sanchez-Lorenzo
Atmos. Chem. Phys., 15, 9477–9500, https://doi.org/10.5194/acp-15-9477-2015, https://doi.org/10.5194/acp-15-9477-2015, 2015
Short summary
Short summary
We evaluate HadGEM3-UKCA over Europe for the period 1960-2009 against observations of aerosol mass and number, aerosol optical depth (AOD) and surface solar radiation (SSR). The model underestimates aerosol mass and number but is less biased if compared to AOD and SSR. Observed trends in aerosols are well simulated by the model and necessary for reproducing the observed increase in SSR since 1990. European all-sky top of atmosphere aerosol radiative forcing increased by > 3 Wm-2 from 1970 to 2009.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
Short summary
Short summary
Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
M. T. Woodhouse, G. W. Mann, K. S. Carslaw, and O. Boucher
Atmos. Chem. Phys., 13, 2723–2733, https://doi.org/10.5194/acp-13-2723-2013, https://doi.org/10.5194/acp-13-2723-2013, 2013
Related subject area
Subject: Gases | Research Activity: Atmospheric Modelling and Data Analysis | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
Natural emissions of VOC and NOx over Africa constrained by TROPOMI HCHO and NO2 data using the MAGRITTEv1.1 model
Anthropogenic emission controls reduce summertime ozone–temperature sensitivity in the United States
Investigating the response of China's surface ozone concentration to the future changes of multiple factors
Assessing the relative impacts of satellite ozone and its precursor observations to improve global tropospheric ozone analysis using multiple chemical reanalysis systems
Evaluating present-day and future impacts of agricultural ammonia emissions on atmospheric chemistry and climate
Air-pollution-satellite-based CO2 emission inversion: system evaluation, sensitivity analysis, and future research direction
Insights into ozone pollution control in urban areas by decoupling meteorological factors based on machine learning
Quantification of regional net CO2 flux errors in the Orbiting Carbon Observatory-2 (OCO-2) v10 model intercomparison project (MIP) ensemble using airborne measurements
Reactive nitrogen in and around the northeastern and mid-Atlantic US: sources, sinks, and connections with ozone
Preindustrial-to-present-day changes in atmospheric carbon monoxide: agreement and gaps between ice archives and global model reconstructions
Investigating processes influencing simulation of local Arctic wintertime anthropogenic pollution in Fairbanks, Alaska, during ALPACA-2022
Urban ozone formation and sensitivities to volatile chemical products, cooking emissions, and NOx upwind of and within two Los Angeles Basin cities
Causes of growing middle-to-upper tropospheric ozone over the northwest Pacific region
Impact of introducing electric vehicles on ground-level O3 and PM2.5 in the Greater Tokyo Area: yearly trends and the importance of changes in the urban heat island effect
A CO2–Δ14CO2 inversion setup for estimating European fossil CO2 emissions
Maximum ozone concentrations in the southwestern US and Texas: implications of the growing predominance of the background contribution
Derivation of atmospheric reaction mechanisms for volatile organic compounds by the SAPRC mechanism generation system (MechGen)
Seasonal, regional, and vertical characteristics of high-carbon-monoxide plumes along with their associated ozone anomalies, as seen by IAGOS between 2002 and 2019
The potential of drone observations to improve air quality predictions by 4D-Var
Process analysis of elevated concentrations of organic acids at Whiteface Mountain, New York
Ozone source attribution in polluted European areas during summer 2017 as simulated with MECO(n)
Surface ozone trend variability across the United States and the impact of heatwaves (1990–2023)
Opinion: Challenges and needs of tropospheric chemical mechanism development
Tracking daily NOx emissions from an urban agglomeration based on TROPOMI NO2 and a local ensemble transform Kalman filter
The atmospheric oxidizing capacity in China – Part 2: Sensitivity to emissions of primary pollutants
Role of chemical production and depositional losses on formaldehyde in the Community Regional Atmospheric Chemistry Multiphase Mechanism (CRACMM)
Review of source analyses of ambient volatile organic compounds considering reactive losses: methods of reducing loss effects, impacts of losses, and sources
Interpreting summertime hourly variation of NO2 columns with implications for geostationary satellite applications
An investigation into atmospheric nitrous acid (HONO) processes in South Korea
Performance evaluation of UKESM1 for surface ozone across the pan-tropics
Constraining light dependency in modeled emissions through comparison to observed biogenic volatile organic compound (BVOC) concentrations in a southeastern US forest
A global re-analysis of regionally resolved emissions and atmospheric mole fractions of SF6 for the period 2005–2021
Monoterpene oxidation pathways initiated by acyl peroxy radical addition
Tropospheric ozone precursors: global and regional distributions, trends, and variability
Sensitivity of climate effects of hydrogen to leakage size, location, and chemical background
The contribution of transport emissions to ozone mixing ratios and methane lifetime in 2015 and 2050 in the Shared Socioeconomic Pathways (SSPs)
Local and transboundary contributions to nitrogen loadings across East Asia using CMAQ-ISAM and GEMS-informed emissions inventory during the winter-spring transition
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
Chemistry-climate feedback of atmospheric methane in a methane emission flux driven chemistry-climate model
Verifying national inventory-based combustion emissions of CO2 across the UK and mainland Europe using satellite observations of atmospheric CO and CO2
Revisiting the high tropospheric ozone over Southern Africa: overestimated biomass burning and underestimated anthropogenic emissions
Source contribution to ozone pollution during June 2021 in Arizona: Insights from WRF-Chem tagged O3 and CO
Enhanced understanding of atmospheric blocking modulation on ozone dynamics within a high-resolution Earth system model
Estimating the variability of NOx emissions from Wuhan with TROPOMI NO2 data during 2018 to 2023
An improved estimate of inorganic iodine emissions from the ocean using a coupled surface microlayer box model
Technical note: A comparative study of chemistry schemes for volcanic sulfur dioxide in Lagrangian transport simulations: a case study of the 2019 Raikoke eruption
Evaluating tropospheric nitrogen dioxide in UKCA using OMI satellite retrievals over South and East Asia
Impact of improved representation of volatile organic compound emissions and production of NOx reservoirs on modeled urban ozone production
Beata Opacka, Trissevgeni Stavrakou, Jean-François Müller, Isabelle De Smedt, Jos van Geffen, Eloise A. Marais, Rebekah P. Horner, Dylan B. Millet, Kelly C. Wells, and Alex B. Guenther
Atmos. Chem. Phys., 25, 2863–2894, https://doi.org/10.5194/acp-25-2863-2025, https://doi.org/10.5194/acp-25-2863-2025, 2025
Short summary
Short summary
Vegetation releases biogenic volatile organic compounds, while soils and lightning contribute to the natural emissions of nitrogen oxides into the atmosphere. These gases interact in complex ways. Using satellite data and models, we developed a new method to simultaneously optimize these natural emissions over Africa in 2019. Our approach resulted in an increase in natural emissions, supported by independent data indicating that current estimates are underestimated.
Shuai Li, Haolin Wang, and Xiao Lu
Atmos. Chem. Phys., 25, 2725–2743, https://doi.org/10.5194/acp-25-2725-2025, https://doi.org/10.5194/acp-25-2725-2025, 2025
Short summary
Short summary
Summertime ozone–temperature sensitivity has decreased by 50 % from 3.0 ppbv per K in 1990 to 1.5 ppb per K in 2021 in the US. GEOS-Chem simulations show that anthropogenic nitrogen oxide emission reduction is the dominant driver of ozone–temperature sensitivity decline by influencing both temperature direct and temperature indirect processes. Reduced ozone–temperature sensitivity has decreased ozone enhancement from low to high temperatures by an average of 6.8 ppbv across the US.
Jinya Yang, Yutong Wang, Lei Zhang, and Yu Zhao
Atmos. Chem. Phys., 25, 2649–2666, https://doi.org/10.5194/acp-25-2649-2025, https://doi.org/10.5194/acp-25-2649-2025, 2025
Short summary
Short summary
We develop a modeling framework to predict future ozone concentrations (till the 2060s) in China following an IPCC scenario. We evaluate the contributions of climatic, anthropogenic, and biogenic factors by season and region. We find persistent emission controls will alter the nonlinear response of ozone to its precursors and dominate the declining ozone level. The outcomes highlight the importance of human actions, even with a climate penalty on air quality.
Takashi Sekiya, Emanuele Emili, Kazuyuki Miyazaki, Antje Inness, Zhen Qu, R. Bradley Pierce, Dylan Jones, Helen Worden, William Y. Y. Cheng, Vincent Huijnen, and Gerbrand Koren
Atmos. Chem. Phys., 25, 2243–2268, https://doi.org/10.5194/acp-25-2243-2025, https://doi.org/10.5194/acp-25-2243-2025, 2025
Short summary
Short summary
Five global chemical reanalysis datasets were used to assess the relative impacts of assimilating satellite ozone and its precursor measurements on tropospheric ozone analyses for 2010. The multiple reanalysis system comparison allows an evaluation of the dependency of the impacts on different reanalysis systems. The results suggested the importance of satellite ozone and its precursor measurements for improving ozone analysis in the whole troposphere, with varying magnitudes among the systems.
Maureen Beaudor, Didier Hauglustaine, Juliette Lathière, Martin Van Damme, Lieven Clarisse, and Nicolas Vuichard
Atmos. Chem. Phys., 25, 2017–2046, https://doi.org/10.5194/acp-25-2017-2025, https://doi.org/10.5194/acp-25-2017-2025, 2025
Short summary
Short summary
Agriculture is the biggest ammonia (NH3) source, impacting air quality, climate, and ecosystems. Because of food demand, NH3 emissions are projected to rise by 2100. Using a global model, we analyzed the impact of present and future NH3 emissions generated from a land model. Our results show improved ammonia patterns compared to a reference inventory. Future scenarios predict up to 70 % increase in global NH3 burden, with significant changes in radiative forcing that can greatly elevate N2O.
Hui Li, Jiaxin Qiu, and Bo Zheng
Atmos. Chem. Phys., 25, 1949–1963, https://doi.org/10.5194/acp-25-1949-2025, https://doi.org/10.5194/acp-25-1949-2025, 2025
Short summary
Short summary
We conduct a sensitivity analysis with 31 tests on various factors including prior emissions, model resolution, satellite constraint, and other system configurations to assess the vulnerability of emission estimates across temporal, sectoral, and regional dimensions. This reveals the robustness of emissions estimated by this air-pollution-satellite-based CO2 emission inversion system, with relative change between tests and base inversion below 4.0 % for national annual NOx and CO2 emissions.
Yuqing Qiu, Xin Li, Wenxuan Chai, Yi Liu, Mengdi Song, Xudong Tian, Qiaoli Zou, Wenjun Lou, Wangyao Zhang, Juan Li, and Yuanhang Zhang
Atmos. Chem. Phys., 25, 1749–1763, https://doi.org/10.5194/acp-25-1749-2025, https://doi.org/10.5194/acp-25-1749-2025, 2025
Short summary
Short summary
The chemical reactions of ozone (O3) formation are related to meteorology and local emissions. Here, a random forest approach was used to eliminate the effects of meteorological factors (dispersion or transport) on O3 and its precursors. Variations in the sensitivity of O3 formation and the apportionment of emission sources were revealed after meteorological normalization. Our results suggest that meteorological variations should be considered when diagnosing O3 formation.
Jeongmin Yun, Junjie Liu, Brendan Byrne, Brad Weir, Lesley E. Ott, Kathryn McKain, Bianca C. Baier, Luciana V. Gatti, and Sebastien C. Biraud
Atmos. Chem. Phys., 25, 1725–1748, https://doi.org/10.5194/acp-25-1725-2025, https://doi.org/10.5194/acp-25-1725-2025, 2025
Short summary
Short summary
This study quantifies errors in regional net surface–atmosphere CO2 flux estimates from an inverse model ensemble using airborne CO2 measurements. Our results show that flux error estimates based on observations significantly exceed those computed from the ensemble spread of flux estimates in regions with high fossil fuel emissions. This finding suggests the presence of systematic biases in the inversion estimates, associated with errors in the fossil fuel emissions common to all models.
Min Huang, Gregory R. Carmichael, Kevin W. Bowman, Isabelle De Smedt, Andreas Colliander, Michael H. Cosh, Sujay V. Kumar, Alex B. Guenther, Scott J. Janz, Ryan M. Stauffer, Anne M. Thompson, Niko M. Fedkin, Robert J. Swap, John D. Bolten, and Alicia T. Joseph
Atmos. Chem. Phys., 25, 1449–1476, https://doi.org/10.5194/acp-25-1449-2025, https://doi.org/10.5194/acp-25-1449-2025, 2025
Short summary
Short summary
We use model simulations along with multiplatform, multidisciplinary observations and a range of analysis methods to estimate and understand the distributions, temporal changes, and impacts of reactive nitrogen and ozone over the most populous US region that has undergone significant environmental changes. Deposition, biogenic emissions, and extra-regional sources have been playing increasingly important roles in controlling pollutant budgets in this area as local anthropogenic emissions drop.
Xavier Faïn, Sophie Szopa, Vaishali Naïk, Patricia Martinerie, David M. Etheridge, Rachael H. Rhodes, Cathy M. Trudinger, Vasilii V. Petrenko, Kévin Fourteau, and Philip Place
Atmos. Chem. Phys., 25, 1105–1119, https://doi.org/10.5194/acp-25-1105-2025, https://doi.org/10.5194/acp-25-1105-2025, 2025
Short summary
Short summary
Carbon monoxide (CO) plays a crucial role in the atmosphere's oxidizing capacity. In this study, we analyse how historical (1850–2014) [CO] outputs from state-of-the-art global chemistry–climate models over Greenland and Antarctica are able to capture both absolute values and trends recorded in multi-site ice archives. A disparity in [CO] growth rates emerges in the Northern Hemisphere between models and observations from 1920–1975 CE, possibly linked to uncertainties in CO emission factors.
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 Dieudonné, 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
Atmos. Chem. Phys., 25, 1063–1104, https://doi.org/10.5194/acp-25-1063-2025, https://doi.org/10.5194/acp-25-1063-2025, 2025
Short summary
Short summary
Processes influencing dispersion of local anthropogenic pollution in Arctic wintertime are investigated with Lagrangian dispersion modelling. Simulated power plant plume rise that considers temperature inversion layers improves results compared to observations (interior Alaska). Modelled 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.
Chelsea E. Stockwell, Matthew M. Coggon, Rebecca H. Schwantes, Colin Harkins, Bert Verreyken, Congmeng Lyu, Qindan Zhu, Lu Xu, Jessica B. Gilman, Aaron Lamplugh, Jeff Peischl, Michael A. Robinson, Patrick R. Veres, Meng Li, Andrew W. Rollins, Kristen Zuraski, Sunil Baidar, Shang Liu, Toshihiro Kuwayama, Steven S. Brown, Brian C. McDonald, and Carsten Warneke
Atmos. Chem. Phys., 25, 1121–1143, https://doi.org/10.5194/acp-25-1121-2025, https://doi.org/10.5194/acp-25-1121-2025, 2025
Short summary
Short summary
In urban areas, emissions from everyday products like paints, cleaners, and personal care products, along with non-traditional sources such as cooking, are increasingly important and impact air quality. This study uses a box model to evaluate how these emissions impact ozone in the Los Angeles Basin and quantifies the impact of gaseous cooking emissions. Accurate representation of these and other anthropogenic sources in inventories is crucial for informing effective air quality policies.
Xiaodan Ma, Jianping Huang, Michaela I. Hegglin, Patrick Jöckel, and Tianliang Zhao
Atmos. Chem. Phys., 25, 943–958, https://doi.org/10.5194/acp-25-943-2025, https://doi.org/10.5194/acp-25-943-2025, 2025
Short summary
Short summary
Our research explored changes in ozone levels in the northwest Pacific region over 30 years, revealing a significant increase in the middle-to-upper troposphere, especially during spring and summer. This rise is influenced by both stratospheric and tropospheric sources, which affect climate and air quality in East Asia. This work underscores the need for continued study to understand underlying mechanisms.
Hiroo Hata, Norifumi Mizushima, and Tomohiko Ihara
Atmos. Chem. Phys., 25, 1037–1061, https://doi.org/10.5194/acp-25-1037-2025, https://doi.org/10.5194/acp-25-1037-2025, 2025
Short summary
Short summary
The introduction of battery electric vehicles (BEVs) is expected to reduce the primary air pollutants from vehicular exhaust and evaporative emissions while reducing the anthropogenic heat produced by vehicles, ultimately mitigating the urban heat island (UHI) effect. This study revealed the impact of introducing BEVs on the decrease in the UHI effect and the impact of BEVs on the formation of tropospheric ozone and fine particulate matter in the Greater Tokyo Area of Japan.
Carlos Gómez-Ortiz, Guillaume Monteil, Sourish Basu, and Marko Scholze
Atmos. Chem. Phys., 25, 397–424, https://doi.org/10.5194/acp-25-397-2025, https://doi.org/10.5194/acp-25-397-2025, 2025
Short summary
Short summary
In this paper, we test new implementations of our inverse modeling tool to estimate the weekly and regional CO2 emissions from fossil fuels in Europe. We use synthetic atmospheric observations of CO2 and radiocarbon (14CO2) to trace emissions to their sources, while separating the natural and fossil CO2. Our tool accurately estimates fossil CO2 emissions in densely monitored regions like western/central Europe. This approach aids in developing strategies for reducing CO2 emissions.
David D. Parrish, Ian C. Faloona, and Richard G. Derwent
Atmos. Chem. Phys., 25, 263–289, https://doi.org/10.5194/acp-25-263-2025, https://doi.org/10.5194/acp-25-263-2025, 2025
Short summary
Short summary
Observation-based estimates of contributions to maximum ozone (O3) concentrations show that background O3 can exceed the air quality standard of 70 ppb in the southwestern US, precluding standard attainment. Over the past 4 decades, US anthropogenic O3 has decreased by a factor of ~ 6.3, while wildfire contributions have increased, so that the background now dominates maximum concentrations, even in Los Angeles, and the occurrence of maximum O3 has shifted from the eastern to the western US.
William P. L. Carter, Jia Jiang, John J. Orlando, and Kelley C. Barsanti
Atmos. Chem. Phys., 25, 199–242, https://doi.org/10.5194/acp-25-199-2025, https://doi.org/10.5194/acp-25-199-2025, 2025
Short summary
Short summary
This paper describes the scientific basis for gas-phase atmospheric chemical mechanisms derived using the SAPRC mechanism generation system, MechGen. It can derive mechanisms for most organic compounds with C, H, O, or N atoms, including initial reactions of organics with OH, O3, NO3, and O3P or by photolysis, as well as the reactions of the various types of intermediates that are formed. The paper includes a description of areas of uncertainty where additional research and updates are needed.
Thibaut Lebourgeois, Bastien Sauvage, Pawel Wolff, Béatrice Josse, Virginie Marécal, Yasmine Bennouna, Romain Blot, Damien Boulanger, Hannah Clark, Jean-Marc Cousin, Philippe Nedelec, and Valérie Thouret
Atmos. Chem. Phys., 24, 13975–14004, https://doi.org/10.5194/acp-24-13975-2024, https://doi.org/10.5194/acp-24-13975-2024, 2024
Short summary
Short summary
Our study examines intense-carbon-monoxide (CO) pollution events measured by commercial aircraft from the In-service Aircraft for a Global Observing System (IAGOS) research infrastructure. We combine these measurements with the SOFT-IO model to trace the origin of the observed CO. A comprehensive analysis of the geographical origin, source type, seasonal variation, and ozone levels of these pollution events is provided.
Hassnae Erraji, Philipp Franke, Astrid Lampert, Tobias Schuldt, Ralf Tillmann, Andreas Wahner, and Anne Caroline Lange
Atmos. Chem. Phys., 24, 13913–13934, https://doi.org/10.5194/acp-24-13913-2024, https://doi.org/10.5194/acp-24-13913-2024, 2024
Short summary
Short summary
Four-dimensional variational data assimilation allows for the simultaneous optimisation of initial values and emission rates by using trace-gas profiles from drone observations in a regional air quality model. Assimilated profiles positively impact the representation of air pollutants in the model by improving their vertical distribution and ground-level concentrations. This case study highlights the potential of drone data to enhance air quality analyses including local emission evaluation.
Christopher Lawrence, Mary Barth, John Orlando, Paul Casson, Richard Brandt, Daniel Kelting, Elizabeth Yerger, and Sara Lance
Atmos. Chem. Phys., 24, 13693–13713, https://doi.org/10.5194/acp-24-13693-2024, https://doi.org/10.5194/acp-24-13693-2024, 2024
Short summary
Short summary
This work uses chemical transport and box modeling to study the gas- and aqueous-phase production of organic acid concentrations measured in cloud water at the summit of Whiteface Mountain on 1 July 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.
Markus Kilian, Volker Grewe, Patrick Jöckel, Astrid Kerkweg, Mariano Mertens, Andreas Zahn, and Helmut Ziereis
Atmos. Chem. Phys., 24, 13503–13523, https://doi.org/10.5194/acp-24-13503-2024, https://doi.org/10.5194/acp-24-13503-2024, 2024
Short summary
Short summary
Anthropogenic emissions are a major source of precursors of tropospheric ozone. As ozone formation is highly non-linear, we apply a global–regional chemistry–climate model with a source attribution method (tagging) to quantify the contribution of anthropogenic emissions to ozone. Our analysis shows that the contribution of European anthropogenic emissions largely increases during large ozone periods, indicating that emissions from these sectors drive ozone values.
Kai-Lan Chang, Brian C. McDonald, and Owen R. Cooper
EGUsphere, https://doi.org/10.5194/egusphere-2024-3674, https://doi.org/10.5194/egusphere-2024-3674, 2024
Short summary
Short summary
Exposure to high levels of ozone can be harmful to human health. This study shows consistent and robust evidence of decreasing ozone extremes across much of the United States over 1990–2023, previously attributed to ozone precursor emission controls. Nevertheless, we also show that the increasing heatwave frequencies are likely to contribute to additional ozone exceedances, slowing the progress of decreasing the frequency of ozone exceedances.
Barbara Ervens, Andrew Rickard, Bernard Aumont, William P. L. Carter, Max McGillen, Abdelwahid Mellouki, John Orlando, Bénédicte Picquet-Varrault, Paul Seakins, William R. Stockwell, Luc Vereecken, and Timothy J. Wallington
Atmos. Chem. Phys., 24, 13317–13339, https://doi.org/10.5194/acp-24-13317-2024, https://doi.org/10.5194/acp-24-13317-2024, 2024
Short summary
Short summary
Chemical mechanisms describe the chemical processes in atmospheric models that are used to describe the changes in 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 the advances and needs of experimental and theoretical research activities needed to build reliable chemical mechanisms.
Yawen Kong, Bo Zheng, and Yuxi Liu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2996, https://doi.org/10.5194/egusphere-2024-2996, 2024
Short summary
Short summary
Current high-resolution satellite remote sensing technologies provide a unique opportunity to derive timely, high-resolution emission data. We developed an emission inversion system to assimilate satellite NO2 data to obtain daily, kilometer-scale NOx emission inventories. Our results enhance inventory accuracy, allowing us to capture the effects of pollution control policies on daily emissions (e.g., during COVID-19 lockdown) and improve fine-scale air quality modeling.
Jianing Dai, Guy P. Brasseur, Mihalis Vrekoussis, Maria Kanakidou, Kun Qu, Yijuan Zhang, Hongliang Zhang, and Tao Wang
Atmos. Chem. Phys., 24, 12943–12962, https://doi.org/10.5194/acp-24-12943-2024, https://doi.org/10.5194/acp-24-12943-2024, 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 representative winter and summer conditions. The study provides insights into further air quality control in China with reduced primary emissions.
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
Atmos. Chem. Phys., 24, 12903–12924, https://doi.org/10.5194/acp-24-12903-2024, https://doi.org/10.5194/acp-24-12903-2024, 2024
Short summary
Short summary
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, we estimate the cancer risk from inhalation exposure to ambient formaldehyde across the contiguous USA and predict that 40 % of this risk is controllable through reductions in anthropogenic emissions of nitrogen oxides and reactive organic carbon.
Baoshuang Liu, Yao Gu, Yutong Wu, Qili Dai, Shaojie Song, Yinchang Feng, and Philip K. Hopke
Atmos. Chem. Phys., 24, 12861–12879, https://doi.org/10.5194/acp-24-12861-2024, https://doi.org/10.5194/acp-24-12861-2024, 2024
Short summary
Short summary
Reactive loss of volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source analyses. We assess common methods of, and existing issues in, reducing losses, impacts of losses, and sources in current source analyses. We offer a potential supporting role for solving issues of VOC conversion. Source analyses of consumed VOCs that reacted to produce ozone and secondary organic aerosols can play an important role in the effective control of secondary pollution in air.
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
Atmos. Chem. Phys., 24, 12687–12706, https://doi.org/10.5194/acp-24-12687-2024, https://doi.org/10.5194/acp-24-12687-2024, 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 explain the weaker hourly variation in NO2 columns than 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
Atmos. Chem. Phys., 24, 12575–12593, https://doi.org/10.5194/acp-24-12575-2024, https://doi.org/10.5194/acp-24-12575-2024, 2024
Short summary
Short summary
We incorporated each HONO process into the current CMAQ modeling framework to enhance the accuracy of HONO mixing ratio 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 understanding chemical transport models, with implications for better air quality management and environmental protection in the region.
Flossie Brown, Gerd Folberth, Stephen Sitch, Paulo Artaxo, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Matteo Detto, Ninong Komala, Luciana Rizzo, Nestor Rojas, Ines dos Santos Vieira, Steven Turnock, Hans Verbeeck, and Alfonso Zambrano
Atmos. Chem. Phys., 24, 12537–12555, https://doi.org/10.5194/acp-24-12537-2024, https://doi.org/10.5194/acp-24-12537-2024, 2024
Short summary
Short summary
Ozone is a pollutant that is detrimental to human and plant health. Ozone monitoring sites in the tropics are limited, so models are often used to understand ozone exposure. We use measurements from the tropics to evaluate ozone from the UK Earth system model, UKESM1. UKESM1 is able to capture the pattern of ozone in the tropics, except in southeast Asia, although it systematically overestimates it at all sites. This work highlights that UKESM1 can capture seasonal and hourly variability.
Namrata Shanmukh Panji, Deborah F. McGlynn, Laura E. R. Barry, Todd M. Scanlon, Manuel T. Lerdau, Sally E. Pusede, and Gabriel Isaacman-VanWertz
Atmos. Chem. Phys., 24, 12495–12507, https://doi.org/10.5194/acp-24-12495-2024, https://doi.org/10.5194/acp-24-12495-2024, 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 in this parameter for future modifications to models.
Martin Vojta, Andreas Plach, Saurabh Annadate, Sunyoung Park, Gawon Lee, Pallav Purohit, Florian Lindl, Xin Lan, Jens Mühle, Rona L. Thompson, and Andreas Stohl
Atmos. Chem. Phys., 24, 12465–12493, https://doi.org/10.5194/acp-24-12465-2024, https://doi.org/10.5194/acp-24-12465-2024, 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 in the EU, while they are substantially growing in China, leading overall to an increasing global emission trend. The national reports for the USA, EU, 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.
Dominika Pasik, Thomas Golin Almeida, Emelda Ahongshangbam, Siddharth Iyer, and Nanna Myllys
EGUsphere, https://doi.org/10.5194/egusphere-2024-3464, https://doi.org/10.5194/egusphere-2024-3464, 2024
Short summary
Short summary
We used quantum chemistry methods to investigate the oxidation mechanisms of acyl peroxy radicals (APRs) with various monoterpenes. Our findings reveal unique oxidation pathways for different monoterpenes, leading to either chain-terminating products or highly reactive intermediates that can contribute to particle formation in the atmosphere. This research highlights APRs as potentially significant but underexplored atmospheric oxidants, which may influence future approaches to modeling climate.
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.
Ragnhild Bieltvedt Skeie, Marit Sandstad, Srinath Krishnan, Gunnar Myhre, and Maria Sand
EGUsphere, https://doi.org/10.5194/egusphere-2024-3079, https://doi.org/10.5194/egusphere-2024-3079, 2024
Short summary
Short summary
Hydrogen leakages can alter the amount of climate gases in the atmosphere and hence have a climate impact. In this study we investigate, using an atmospheric chemistry model, how this indirect climate effect differs for different amounts of leakages, where the hydrogen leaks and if this effect changes in the future. The effect is largest for emissions far from areas where hydrogen is removed from the atmosphere by the soil, but these are not relevant locations for a future hydrogen economy.
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.
Jincheol Park, Yunsoo Choi, and Sagun Kayastha
EGUsphere, https://doi.org/10.5194/egusphere-2024-3312, https://doi.org/10.5194/egusphere-2024-3312, 2024
Short summary
Short summary
We investigated NOx emissions’ contributions to nitrogen loadings across five regions of East Asia during the 2022 winter-spring transition through chemical transport modeling informed by satellite data. As seasons progress, local contributions within each region to its NOy budget decreased from 32 %–43 % to 23 %–30 %, while transboundary contributions increased from 16 %–33 % to 27 %–37 %, driven by a shift in synoptic settings that allowed pollutants to spread more broadly across the regions.
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.
Laura Stecher, Franziska Winterstein, Patrick Jöckel, Michael Ponater, Mariano Mertens, and Martin Dameris
EGUsphere, https://doi.org/10.5194/egusphere-2024-2938, https://doi.org/10.5194/egusphere-2024-2938, 2024
Short summary
Short summary
Methane, the second most important anthropogenic greenhouse gas, is chemically decomposed in the atmosphere. The chemical sink of atmospheric methane is not constant, but depends on the temperature and on the abundance of its reaction partners. In this study, we use a global chemistry-climate model to assess the feedback of atmospheric methane induced by changes of the chemical sink in a warming climate, and its implications for the chemical composition and the surface air temperature change.
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.
Yufen Wang, Ke Li, Xi Chen, Zhenjiang Yang, Minglong Tang, Pascoal M. D. Campos, Yang Yang, Xu Yue, and Hong Liao
EGUsphere, https://doi.org/10.5194/egusphere-2024-2576, https://doi.org/10.5194/egusphere-2024-2576, 2024
Short summary
Short summary
The impact of biomass burning and anthropogenic emissions on high tropospheric ozone was not well studied in Southern Africa. We combined the model simulation with recent observations at the surface and from space to quantify tropospheric ozone and its main drivers in Southern Africa. Our work focuses on the impact of emissions from different sources at different spatial scales, contributing to a comprehensive understanding of air pollution drivers and their uncertainties in Southern Africa.
Yafang Guo, Mohammad Amin Mirrezaei, Armin Sorooshian, and Avelino F. Arellano
EGUsphere, https://doi.org/10.5194/egusphere-2024-2617, https://doi.org/10.5194/egusphere-2024-2617, 2024
Short summary
Short summary
We assess the contributions of fire and anthropogenic emissions to O3 levels in Phoenix Arizona during a period of intense heat and drought conditions. We find that fire exacerbates O3 pollution and that interactions between weather, climate, and air chemistry are important to consider. This has implications to activities related to formulating emission reduction strategies in areas that are currently under-studied yet becoming relevant due to reports of increasing global aridity.
Wenbin Kou, Yang Gao, Dan Tong, Xiaojie Guo, Xiadong An, Wenyu Liu, Mengshi Cui, Xiuwen Guo, Shaoqing Zhang, Huiwang Gao, and Lixin Wu
EGUsphere, https://doi.org/10.5194/egusphere-2024-2500, https://doi.org/10.5194/egusphere-2024-2500, 2024
Short summary
Short summary
Unlike traditional numerical studies, we apply a high-resolution Earth system model, improving simulations of ozone and large-scale circulations such as atmospheric blocking. In addition to local heatwave effects, we quantify the impact of atmospheric blocking on downstream ozone concentrations, which is closely associated with the blocking position. We identify three major pathways of Rossby wave propagation, stressing the critical role of large-scale circulation play in regional air quality.
Qianqian Zhang, K. Folkert Boersma, Chiel van der Laan, Alba Mols, Bin Zhao, Shengyue Li, and Yuepeng Pan
EGUsphere, https://doi.org/10.5194/egusphere-2024-2641, https://doi.org/10.5194/egusphere-2024-2641, 2024
Short summary
Short summary
Accurate NOx emission estimates are required to better understand air pollution. This study investigates and demonstrates the ability of the superposition column model in combination with TROPOMI tropospheric NO2 column data to estimate city-scale NOx emissions and lifetimes and their variabilities. The results of this work nevertheless confirm the strength of the superposition column model in estimating urban NOx emissions with reasonable accuracy.
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.
Mingzhao Liu, Lars Hoffmann, Jens-Uwe Grooß, Zhongyin Cai, Sabine Grießbach, and Yi Heng
EGUsphere, https://doi.org/10.5194/egusphere-2024-2596, https://doi.org/10.5194/egusphere-2024-2596, 2024
Short summary
Short summary
We studied the transport and chemical decomposition of volcanic SO2, focusing on the 2019 Raikoke event. By comparing two different chemistry modeling schemes, we found that including complex chemical reactions leads to a more accurate prediction of how long SO2 stays in the atmosphere. This research helps improve our understanding of volcanic pollution and its impact on air quality and climate, providing better tools for scientists to track and predict the movement of these pollutants.
Alok K. Pandey, David S. Stevenson, Alcide Zhao, Richard J. Pope, Ryan Hossaini, Krishan Kumar, and Marytn P. Chipperfield
EGUsphere, https://doi.org/10.5194/egusphere-2024-2686, https://doi.org/10.5194/egusphere-2024-2686, 2024
Short summary
Short summary
Nitrogen dioxide is an air pollutant largely controlled by human activity that affects ozone, methane and aerosols. Satellite instruments can quantify column NO2, and by carefully matching the time and location of measurements, enable evaluation of model simulations. NO2 over SE Asia is assessed, showing that the model captures many features of the measurements, but also important differences that suggest model deficiencies in representing several aspects of the atmospheric chemistry of NO2.
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.
Cited articles
Abraham, N. L., Archibald, A. T., Bellouin, N., Boucher, O., Braesicke, P., Bushell, A., Carslaw, K. S., Collins, W., Dalvi, M., Emmerson, K. M., Folberth, G., Haywood, J., Johnson, C., Kipling, Z., Macintyre, H., Mann, G. W., Telford, P. J., Merikanto, J., Morgenstern, O., O'Connor, F., Ordonez, C., Osprey, S., Pringle, K. J., Pyle, J. A., Rae, J. G. L., Reddington, C. L., Savage, D., 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., UK Met Office, Exeter (UK), 74 pp., available at: http://www.ukca.ac.uk/images/b/b1/Umdp_084-umdp84.pdf, 2012.
Bariteau, L., Helmig, D., Fairall, C. W., Hare, J. E., Hueber, J., and Lang, E. K.: Determination of oceanic ozone deposition by ship-borne eddy covariance flux measurements, Atmos. Meas. Tech., 3, 441–455, https://doi.org/10.5194/amt-3-441-2010, 2010.
Bi, D. H., Dix, M., Marsland, S. J., O'Farrell, S., Rashid, H. A., Uotila, P., Hirst, A. C., Kowalczyk, E., Golebiewski, M., Sullivan, A., Yan, H. L., Hannah, N., Franklin, C., Sun, Z. A., Vohralik, P., Watterson, I., Zhou, X. B., Fiedler, R., Collier, M., Ma, Y. M., Noonan, J., Stevens, L., Uhe, P., Zhu, H. Y., Griffies, S. M., Hill, R., Harris, C., and Puri, K.: The ACCESS coupled model: description, control climate and evaluation, Aust. Meteorol. Ocean., 63, 41–64, available at: http://www.bom.gov.au/amm/docs/2013/bi1.pdf, 2013.
Carpenter, L. J. and Nightingale, P. D.: Chemistry and release of gases from the surface ocean, Chem. Rev., 115, 4015–4034, https://doi.org/10.1021/cr5007123, 2015.
Carpenter, L. J., MacDonald, S. M., Shaw, M. D., Kumar, R., Saunders, R. W., Parthipan, R., Wilson, J., and Plane, J. M. C.: Atmospheric iodine levels influenced by sea surface emissions of inorganic iodine, Nat. Geosci., 6, 108–111, https://doi.org/10.1038/NGEO1687, 2013.
Chance, R., Baker, A. R., Carpenter, L., and Jickells, T. D.: The distribution of iodide at the sea surface, Environ. Sci.-Proc. Imp., 16, 1841–1859, https://doi.org/10.1039/c4em00139g, 2014.
Chang, W. N., Heikes, B. G., and Lee, M.: Ozone deposition to the sea surface: Chemical enhancement and wind speed dependence, Atmos. Environ., 38, 1053–1059, https://doi.org/10.1016/j.atmosenv.2003.10.050, 2004.
Coleman, L., Varghese, S., Tripathi, O. P., Jennings, S. G., and O'Dowd, C. D.: Regional-scale ozone deposition to North-East Atlantic waters, Adv. Meteorol., 2010, 243701, https://doi.org/10.1155/2010/243701, 2010.
Dee, D. P., Uppala, S. M., Simmons, A. J., Berrisford, P., Poli, P., Kobayashi, S., Andrae, U., Balmaseda, M. A., Balsamo, G., Bauer, P., Bechtold, P., Beljaars, A. C. M., van de Berg, I., Biblot, J., Bormann, N., Delsol, C., Dragani, R., Fuentes, M., Greer, A. J., Haimberger, L., Healy, S. B., Hersbach, H., Holm, E. V., Isaksen, L., Kallberg, P., Kohler, M., Matricardi, M., McNally, A. P., Mong-Sanz, B. M., Morcette, J.-J., Park, B.-K., Peubey, C., de Rosnay, P., Tavolato, C., Thepaut, J. N., and Vitart, F.: The ERA-Interim reanalysis: Configuration and performance of the data assimilation system, Q. J. Roy. Meteorol. Soc., 137, 553–597, https://doi.org/10.1002/qj.828, 2011.
Emmons, L. K., Walters, S., Hess, P. G., Lamarque, J.-F., Pfister, G. G., Fillmore, D., Granier, C., Guenther, A., Kinnison, D., Laepple, T., Orlando, J., Tie, X., Tyndall, G., Wiedinmyer, C., Baughcum, S. L., and Kloster, S.: Description and evaluation of the Model for Ozone and Related chemical Tracers, version 4 (MOZART-4), Geosci. Model Dev., 3, 43–67, https://doi.org/10.5194/gmd-3-43-2010, 2010.
Fairall, C. W., Hare, J. E., Edson, J. B., and McGillis, W.: Parameterization and micrometeorological measurements of air-sea gas transfer, Bound.-Lay. Meteorol., 96, 63–105, https://doi.org/10.1023/A:1002662826020, 2000.
Fairall, C. W., Helmig, D., Ganzeveld, L., and Hare, J.: Water-side turbulence enhancement of ozone deposition to the ocean, Atmos. Chem. Phys., 7, 443–451, https://doi.org/10.5194/acp-7-443-2007, 2007.
Galbally, I. E. and Roy C. R.: Destruction of ozone at the Earth's surface, Q. J. Roy. Meteor. Soc., 106, 599–620, https://doi.org/10.1002/qj.49710644915, 1980.
Ganzeveld, L., Helmig, D., Fairall, C., Hare, J. E., and Pozzer, A.: Atmosphere-ocean ozone exchange: A global modeling study of biogeochemical, atmospheric and water-side turbulence dependencies, Global Biogeochem. Cy., 23, GB4021, https://doi.org/10.1029/2008GB003301, 2009.
Garland, J. A., Elzerman, A. W., and Penkett, S. A.: The mechanism for dry deposition of ozone to seawater surfaces, J. Geophys. Res., 85, 7488–7492, https://doi.org/10.1029/JC085iC12p07488, 1980.
Gaudel, A., Clark, H., Thouret, V., Jones, L., Inness, A., Flemming, J., Stein, O., Huijnen, V., Eskes, H., Nédélec, P., and Boulanger, D.: On the use of MOZAIC-IAGOS data to assess the ability of the MACC reanalysis to reproduce the distribution of ozone and CO in the UTLS over Europe, Tellus B, 67, 27955, https://doi.org/10.3402/tellusb.v67.27955, 2015.
Geernaert, L. L. S., Geernaert, G. L., Granby, K., and Asman, W. A. H.: Fluxes of soluble gases in the marine atmospheric surface layer, Tellus B, 50, 111–127, https://doi.org/10.1034/j.1600-0889.1998.t01-1-00001.x, 1998.
Giordano, L., Brunner, D., Flemming, J., et al.: Assessment of the MACC reanalysis and its influence as chemical boundary conditions for regional air quality modeling in AQMEII-2, Atmos. Environ., 115, 371–388, https://doi.org/10.1016/j.atmosenv.2015.02.034, 2015.
Hansell, D. A., Carlson, C. A., Repeta, D. J., Schlitzer, R.: Dissolved organic matter in the ocean, Oceanography 22, 202–211, 2009.
Hardacre, C., Wild, O., and Emberson, L.: An evaluation of ozone dry deposition in global scale chemistry climate models, Atmos. Chem. Phys., 15, 6419–6436, https://doi.org/10.5194/acp-15-6419-2015, 2015.
Helmig, D., Lang, E. K., Bariteau, L., Boylan, P., Fairall, C. W., Ganzeveld, L., Hare, J. E., Hueber, J., and Pallandt, M.: Atmosphere-ocean ozone fluxes during the TexAQS 2006, STRATUS 2006, GOMECC 2007, GasEx 2008, and AMMA 2008 cruises, J. Geophys. Res., 117, D04305, https://doi.org/10.1029/2011JD015955, 2012.
Hu, J. H., Shi, Q., Davidovits, P., Worsnop, D. R., Zahniser, M. S., and Kolb, C. E.: Reactive uptake of Cl2(g) and Br2(g) by aqueous surfaces as a function of Br− and I− ion concentration: The effect of chemical reaction at the interface, J. Phys. Chem., 99, 8768–8776, https://doi.org/10.1021/j100021a050, 1995.
Inness, A., Baier, F., Benedetti, A., Bouarar, I., Chabrillat, S., Clark, H., Clerbaux, C., Coheur, P., Engelen, R. J., Errera, Q., Flemming, J., George, M., Granier, C., Hadji-Lazaro, J., Huijnen, V., Hurtmans, D., Jones, L., Kaiser, J. W., Kapsomenakis, J., Lefever, K., Leitão, J., Razinger, M., Richter, A., Schultz, M. G., Simmons, A. J., Suttie, M., Stein, O., Thépaut, J.-N., Thouret, V., Vrekoussis, M., Zerefos, C., and the MACC team: The MACC reanalysis: an 8 yr data set of atmospheric composition, Atmos. Chem. Phys., 13, 4073–4109, https://doi.org/10.5194/acp-13-4073-2013, 2013.
IPCC: Climate Change 2013: The Physical Science Basis, Contribution of Working Group I to the Fifth Assessment Report of the Intergovernmental Panel on Climate Change, edited by: Stocker, T. F., Qin, D., Plattner, G.-K., Tignor, M., Allen, S. K., Boschung, J., Nauels, A., Xia, Y., Bex, V., and Midgley, P. M., Cambridge University Press, Cambridge, UK, New York, NY, USA, 1535 pp., 2013.
Johnson, P. N. and Davis, R. A.: Diffusivity of ozone in water, J. Chem. Eng. Data, 41, 1485–1487, https://doi.org/10.1021/je9602125, 1996.
Katragkou, E., Zanis, P., Tsikerdekis, A., Kapsomenakis, J., Melas, D., Eskes, H., Flemming, J., Huijnen, V., Inness, A., Schultz, M. G., Stein, O., and Zerefos, C. S.: Evaluation of near-surface ozone over Europe from the MACC reanalysis, Geosci. Model Dev., 8, 2299–2314, https://doi.org/10.5194/gmd-8-2299-2015, 2015.
Kerkweg, A., Buchholz, J., Ganzeveld, L., Pozzer, A., Tost, H., and Jöckel, P.: Technical Note: An implementation of the dry removal processes DRY DEPosition and SEDImentation in the Modular Earth Submodel System (MESSy), Atmos. Chem. Phys., 6, 4617–4632, https://doi.org/10.5194/acp-6-4617-2006, 2006.
Kinnison, D. E., Brasseur, G. P., Walters, S., Garcia, R. R., Marsh, D. R., Sassi, F., Harvey, V. L., Randall, C. E., Emmons, L., Lamarque, J. F., Hess, P., Orlando, J. J., Tie, X. X., Randel, W., Pan, L. L., Gettelman, A., Granier, C., Diehl, T., Niemeier, U., and Simmons, A. J.: Sensitivity of chemical tracers to meteorological parameters in the MOZART-3 chemical transport model, J. Geophys. Res., 112, D03303, https://doi.org/10.1029/2008JD010739, 2007.
Lamarque, J.-F., Emmons, L. K., Hess, P. G., Kinnison, D. E., Tilmes, S., Vitt, F., Heald, C. L., Holland, E. A., Lauritzen, P. H., Neu, J., Orlando, J. J., Rasch, P. J., and Tyndall, G. K.: CAM-chem: description and evaluation of interactive atmospheric chemistry in the Community Earth System Model, Geosci. Model Dev., 5, 369–411, https://doi.org/10.5194/gmd-5-369-2012, 2012.
Liu, Q., Schurter, L. M., Muller, C. E., Aloisio, S., Francisco, J. S., and Margerum, D. W.: Kinetics and mechanisms of aqueous ozone reactions with bromide, sulfite, hydrogen sulfite, iodide, and nitrite ions, Inorg. Chem., 40, 4436–4442, https://doi.org/10.1021/ic000919j, 2001.
Luhar, A. K., Galbally, I. E., Woodhouse, M. T., and Thatcher, M.: An improved parameterisation of ozone dry deposition to the ocean and its impact in a global climate–chemistry model, Atmos. Chem. Phys., 17, 3749–767, https://doi.org/10.5194/acp-17-3749-2017, 2017.
MacDonald, S. M., Gómez Martín, J. C., Chance, R., Warriner, S., Saiz-Lopez, A., Carpenter, L. J., and Plane, J. M. C.: A laboratory characterisation of inorganic iodine emissions from the sea surface: dependence on oceanic variables and parameterisation for global modelling, Atmos. Chem. Phys., 14, 5841–5852, https://doi.org/10.5194/acp-14-5841-2014, 2014.
Magi, L., Schweitzer, F., Pallares, C., Cherif, S., Mirabel, P., and George, C.: Investigation of the uptake rate of ozone and methyl hydroperoxide by water surfaces, J. Phys. Chem. A, 101, 4943–4949, https://doi.org/10.1021/jp970646m, 1997.
Mao, J., Paulot, F., Jacob, D. J., Cohen, R. C., Crounse, J. D., Wennberg, P. O., Keller, C. A., Hudman, R. C., Barkley, M. P., and Horowitz, L. W.: Ozone and organic nitrates over the eastern United States: Sensitivity to isoprene chemistry, J. Geophys. Res.-Atmos., 118, 11256–11268, https://doi.org/10.1002/jgrd.50817, 2013.
Massicotte, P., Asmala, E., Stedmon, C., and Markager, S.: Global distribution of dissolved organic matter along the aquatic continuum: Across rivers, lakes and oceans, Sci. Total Environ., 609, 180–191, https://doi.org/10.1016/j.scitotenv.2017.07.076, 2017.
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.
Morris, J. C.: The aqueous solubility of ozone – A review, Ozone news, 1, 14–16, 1988.
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.
Press, W. H., Teukolsky, S. A., Vetterling, W. T., and Flannery, B. P.: Numerical Recipes in Fortran 77, Cambridge University Press, Cambridge, UK, ISBN 0 521 43064 X, 1997.
Sarwar, G., Kang, D., Foley, K., Schwede, D., Gantt, B., and Mathur, R.: Technical note: Examining ozone deposition over seawater, Atmos. Environ., 141, 255–262, https://doi.org/10.1016/j.atmosenv.2016.06.072, 2016.
Soloviev, A. and Lukas, R.: The Near-Surface Layer of the Ocean: Structure, Dynamics and Applications. 2nd edn. Atmospheric and Oceanographic Sciences Library, Springer, Vol. 48, 552 pp., https://doi.org/10.1007/978-94-007-7621-0, 2014.
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., Rodriguez, 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., 111, D08301, https://doi.org/10.1029/2005JD006338, 2006.
Uhe, P. and Thatcher, M.: A spectral nudging method for the ACCESS1.3 atmospheric model, Geosci. Model Dev., 8, 1645–1658, https://doi.org/10.5194/gmd-8-1645-2015, 2015.
von Kuhlmann, R., Lawrence, M. G., Crutzen, P. J., and Rasch, P. J.: A model for studies of tropospheric ozone and nonmethane hydrocarbons: Model description and ozone results, J. Geophys. Res., 108, 4294, https://doi.org/10.1029/2002JD002893, 2003.
Walters, D. N., Williams, K. D., Boutle, I. A., Bushell, A. C., Edwards, J. M., Field, P. R., Lock, A. P., Morcrette, C. J., Stratton, R. A., Wilkinson, J. M., Willett, M. R., Bellouin, N., Bodas-Salcedo, A., Brooks, M. E., Copsey, D., Earnshaw, P. D., Hardiman, S. C., Harris, C. M., Levine, R. C., MacLachlan, C., Manners, J. C., Martin, G. M., Milton, S. F., Palmer, M. D., Roberts, M. J., Rodríguez, J. M., Tennant, W. J., and Vidale, P. L.: The Met Office Unified Model Global Atmosphere 4.0 and JULES Global Land 4.0 configurations, Geosci. Model Dev., 7, 361–386, https://doi.org/10.5194/gmd-7-361-2014, 2014.
Wesely, M.: Parameterization of surface resistances to gaseous dry deposition in regional-scale numerical-models, Atmos. Environ., 23, 1293–1304, https://doi.org/10.1016/0004-6981(89)90153-4, 1989.
Wild, O.: Modelling the global tropospheric ozone budget: exploring the variability in current models, Atmos. Chem. Phys., 7, 2643–2660, https://doi.org/10.5194/acp-7-2643-2007, 2007.
Willmott, C. J.: On the validation of models, Phys. Geography, 2, 184–194, 1981.
Woodhouse, M. T., Luhar, A. K., Stevens, L., Galbally, I., Thatcher, M., Uhe, P., Wolff, H., Noonan, J., and Molloy, S.: Australian reactive-gas emissions in a global chemistry-climate model and initial results, Air Qual. Clim. Change, 49, 31–38, 2015.
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.
Short summary
Dry deposition at the Earth’s surface is an important sink of atmospheric ozone. A new parameterisation for ozone dry deposition to the ocean that accounts for relevant chemical and physical processes is developed and tested. It results in an ocean deposition loss that is only about a third of the current model estimates and corresponds to an increase of 5 % in the tropospheric ozone burden. This is important for tropospheric ozone budget, associated radiative forcing, and ozone mixing ratios.
Dry deposition at the Earth’s surface is an important sink of atmospheric ozone. A new...
Altmetrics
Final-revised paper
Preprint