Articles | Volume 17, issue 5
Atmos. Chem. Phys., 17, 3749–3767, 2017
https://doi.org/10.5194/acp-17-3749-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Atmos. Chem. Phys., 17, 3749–3767, 2017
https://doi.org/10.5194/acp-17-3749-2017
© Author(s) 2017. This work is distributed under
the Creative Commons Attribution 3.0 License.
the Creative Commons Attribution 3.0 License.
Research article
17 Mar 2017
Research article
| 17 Mar 2017
An improved parameterisation of ozone dry deposition to the ocean and its impact in a global climate–chemistry model
Ashok K. Luhar et al.
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Ashok K. Luhar, Ian E. Galbally, and Matthew T. Woodhouse
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-275, https://doi.org/10.5194/acp-2022-275, 2022
Revised manuscript accepted for ACP
Short summary
Short summary
This study shows that recent improvements to global parameterisations of oceanic ozone dry deposition and lightning-generated NOx (LNOx) impact Earth’s radiative fluxes. These radiation changes are larger in magnitude in the tropics and are dominated by the LNOx parameterisation change. Uncertainty in radiative fluxes arising from reported uncertainty in LNOx is estimated to be significant in comparison with the ‘present-day’ IPCC AR6 anthropogenic effective radiative forcing due to ozone.
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
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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
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With the sharp rise in coal seam gas (CSG) production in Queensland’s Surat Basin, there is much interest in quantifying methane emissions from this area and from unconventional gas production in general. We develop and apply a regional Bayesian inverse model that uses hourly methane concentration data from two sites and modelled backward dispersion to quantify emissions. The model requires a narrow prior and suggests that the emissions from the CSG areas are 33% larger than bottom-up estimates.
Ashok K. Luhar, Matthew T. Woodhouse, and Ian E. Galbally
Atmos. Chem. Phys., 18, 4329–4348, https://doi.org/10.5194/acp-18-4329-2018, https://doi.org/10.5194/acp-18-4329-2018, 2018
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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.
Ashok K. Luhar, Ian E. Galbally, and Matthew T. Woodhouse
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-275, https://doi.org/10.5194/acp-2022-275, 2022
Revised manuscript accepted for ACP
Short summary
Short summary
This study shows that recent improvements to global parameterisations of oceanic ozone dry deposition and lightning-generated NOx (LNOx) impact Earth’s radiative fluxes. These radiation changes are larger in magnitude in the tropics and are dominated by the LNOx parameterisation change. Uncertainty in radiative fluxes arising from reported uncertainty in LNOx is estimated to be significant in comparison with the ‘present-day’ IPCC AR6 anthropogenic effective radiative forcing due to ozone.
Sonya L. Fiddes, Alain Protat, Marc D. Mallet, Simon P. Alexander, and Matthew T. Woodhouse
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-259, https://doi.org/10.5194/acp-2022-259, 2022
Revised manuscript under review for ACP
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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 correct cloud type and even when it does, the cloud properties and amount of reflected sunlight is incorrect. We have a lot of work to do to model clouds correctly over the Southern Ocean.
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
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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
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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
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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
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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
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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.
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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
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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
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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
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Ashok K. Luhar, Matthew T. Woodhouse, and Ian E. Galbally
Atmos. Chem. Phys., 18, 4329–4348, https://doi.org/10.5194/acp-18-4329-2018, https://doi.org/10.5194/acp-18-4329-2018, 2018
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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.
Erin Dunne, Ian E. Galbally, Min Cheng, Paul Selleck, Suzie B. Molloy, and Sarah J. Lawson
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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.
Hannah M. Horowitz, Rebecca M. Garland, Marcus Thatcher, Willem A. Landman, Zane Dedekind, Jacobus van der Merwe, and Francois A. Engelbrecht
Atmos. Chem. Phys., 17, 13999–14023, https://doi.org/10.5194/acp-17-13999-2017, https://doi.org/10.5194/acp-17-13999-2017, 2017
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Africa is a major source of particles (or aerosols) from dust and fires, which impact climate. Models used to predict impacts of future climate change have not been well tested for aerosols over Africa. In this study we evaluate aerosols in the CCAM climate model against observations across Africa and surrounding regions. We find the model generally captures observed variability but overestimates dust in northern Africa, which has implications for its representation of climate feedbacks.
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
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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
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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.
Mathew J. Lipson, Melissa A. Hart, and Marcus Thatcher
Geosci. Model Dev., 10, 991–1007, https://doi.org/10.5194/gmd-10-991-2017, https://doi.org/10.5194/gmd-10-991-2017, 2017
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City-scale models describing the surface energy balance have difficulties representing heat storage in urban materials. This paper proposes an alternative method to discretise heat conduction through urban materials. We compare the new method with an approach commonly used in urban models and find the new method better matches exact solutions to heat transfer for a wide variety of urban material compositions. We also find the new method improves the bulk energy flux response of an urban model.
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
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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
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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
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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
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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
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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
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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.
P. Uhe and M. Thatcher
Geosci. Model Dev., 8, 1645–1658, https://doi.org/10.5194/gmd-8-1645-2015, https://doi.org/10.5194/gmd-8-1645-2015, 2015
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We describe a spectral nudging technique to constrain the large spatial structures of an atmospheric general circulation model (ACCESS1.3) towards an observational product (ERA-Interim). This has a number of applications for model development and scientific studies. This paper shows potential benefits of using the spectral nudging over the traditional Newtonian relaxation method.
S. J. Lawson, P. W. Selleck, I. E. Galbally, M. D. Keywood, M. J. Harvey, C. Lerot, D. Helmig, and Z. Ristovski
Atmos. Chem. Phys., 15, 223–240, https://doi.org/10.5194/acp-15-223-2015, https://doi.org/10.5194/acp-15-223-2015, 2015
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Glyoxal and methylglyoxal are short-lived organic trace gases and important precursors of secondary organic aerosol. Measurements over oceans are sparse. We present the first in situ glyoxal and methylglyoxal observations over remote temperate oceans, alongside observations of precursor gases. Precursor gases cannot explain observed mixing ratios, highlighting an unknown source. We show a large discrepancy between calculated vertical column densities of glyoxal and those retrieved by satellite.
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
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Subject: Gases | Research Activity: Atmospheric Modelling | Altitude Range: Troposphere | Science Focus: Chemistry (chemical composition and reactions)
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Surface ozone impacts on major crop production in China from 2010 to 2017
Enhanced summertime ozone and SOA from biogenic volatile organic compound (BVOC) emissions due to vegetation biomass variability during 1981–2018 in China
Pyruvic acid, an efficient catalyst in SO3 hydrolysis and effective clustering agent in sulfuric-acid-based new particle formation
Tropospheric ozone changes and ozone sensitivity from the present day to the future under shared socio-economic pathways
An integrated analysis of contemporary methane emissions and concentration trends over China using in situ and satellite observations and model simulations
Maria Paula Pérez-Peña, Jenny A. Fisher, Dylan B. Millet, Hisashi Yashiro, Ray L. Langenfelds, Paul B. Krummel, and Scott H. Kable
Atmos. Chem. Phys., 22, 12367–12386, https://doi.org/10.5194/acp-22-12367-2022, https://doi.org/10.5194/acp-22-12367-2022, 2022
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We used two atmospheric models to test the implications of previously unexplored aldehyde photochemistry on the atmospheric levels of molecular hydrogen (H2). We showed that the new photochemistry from aldehydes produces more H2 over densely forested areas. Compared to the rest of the world, it is over these forested regions where the produced H2 is more likely to be removed. The results highlight that other processes that contribute to atmospheric H2 levels should be studied further.
Flossie Brown, Gerd A. Folberth, Stephen Sitch, Susanne Bauer, Marijn Bauters, Pascal Boeckx, Alexander W. Cheesman, Makoto Deushi, Inês Dos Santos Vieira, Corinne Galy-Lacaux, James Haywood, James Keeble, Lina M. Mercado, Fiona M. O'Connor, Naga Oshima, Kostas Tsigaridis, and Hans Verbeeck
Atmos. Chem. Phys., 22, 12331–12352, https://doi.org/10.5194/acp-22-12331-2022, https://doi.org/10.5194/acp-22-12331-2022, 2022
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Surface ozone can decrease plant productivity and impair human health. In this study, we evaluate the change in surface ozone due to climate change over South America and Africa using Earth system models. We find that if the climate were to change according to the worst-case scenario used here, models predict that forested areas in biomass burning locations and urban populations will be at increasing risk of ozone exposure, but other areas will experience a climate benefit.
Therese S. Carter, Colette L. Heald, Jesse H. Kroll, Eric C. Apel, Donald Blake, Matthew Coggon, Achim Edtbauer, Georgios Gkatzelis, Rebecca S. Hornbrook, Jeff Peischl, Eva Y. Pfannerstill, Felix Piel, Nina G. Reijrink, Akima Ringsdorf, Carsten Warneke, Jonathan Williams, Armin Wisthaler, and Lu Xu
Atmos. Chem. Phys., 22, 12093–12111, https://doi.org/10.5194/acp-22-12093-2022, https://doi.org/10.5194/acp-22-12093-2022, 2022
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Fires emit many gases which can contribute to smog and air pollution. However, the amount and properties of these chemicals are not well understood, so this work updates and expands their representation in a global atmospheric model, including by adding new chemicals. We confirm that this updated representation generally matches measurements taken in several fire regions. We then show that fires provide ~15 % of atmospheric reactivity globally and more than 75 % over fire source regions.
Etienne Terrenoire, Didier A. Hauglustaine, Yann Cohen, Anne Cozic, Richard Valorso, Franck Lefèvre, and Sigrun Matthes
Atmos. Chem. Phys., 22, 11987–12023, https://doi.org/10.5194/acp-22-11987-2022, https://doi.org/10.5194/acp-22-11987-2022, 2022
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Aviation NOx emissions not only have an impact on global climate by changing ozone and methane levels in the atmosphere, but also contribute to the deterioration of local air quality. The LMDZ-INCA global model is applied to re-evaluate the impact of aircraft NOx and aerosol emissions on climate. We investigate the impact of present-day and future (2050) aircraft emissions on atmospheric composition and the associated radiative forcings of climate for ozone, methane and aerosol direct forcings.
Aurelia Lupaşcu, Noelia Otero, Andrea Minkos, and Tim Butler
Atmos. Chem. Phys., 22, 11675–11699, https://doi.org/10.5194/acp-22-11675-2022, https://doi.org/10.5194/acp-22-11675-2022, 2022
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Ground-level ozone is an important air pollutant that affects human health, ecosystems, and climate. Ozone is not emitted directly but rather formed in the atmosphere through chemical reactions involving two distinct precursors. Our results provide detailed information about the origin of ozone in Germany during two peak ozone events that took place in 2015 and 2018, thus improving our understanding of ground-level ozone.
Hervé Petetin, Dene Bowdalo, Pierre-Antoine Bretonnière, Marc Guevara, Oriol Jorba, Jan Mateu Armengol, Margarida Samso Cabre, Kim Serradell, Albert Soret, and Carlos Pérez Garcia-Pando
Atmos. Chem. Phys., 22, 11603–11630, https://doi.org/10.5194/acp-22-11603-2022, https://doi.org/10.5194/acp-22-11603-2022, 2022
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This study investigates the extent to which ozone forecasts provided by the Copernicus Atmospheric Monitoring Service (CAMS) can be improved using surface observations and state-of-the-art statistical methods. Through a case study over the Iberian Peninsula in 2018–2019, it unambiguously demonstrates the value of these methods for improving the raw CAMS O3 forecasts while at the same time highlighting the complexity of improving the detection of the highest O3 concentrations.
Megan Jeramaz Lickley, John S. Daniel, Eric L. Fleming, Stefan Reimann, and Susan Solomon
Atmos. Chem. Phys., 22, 11125–11136, https://doi.org/10.5194/acp-22-11125-2022, https://doi.org/10.5194/acp-22-11125-2022, 2022
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Halocarbons contained in equipment continue to be emitted after production has ceased. These
banksmust be carefully accounted for in evaluating compliance with the Montreal Protocol. We extend a Bayesian model to the suite of regulated chemicals subject to banking. We find that banks are substantially larger than previous estimates, and we identify banks by chemical and equipment type whose future emissions will contribute to global warming and delay ozone-hole recovery if left unrecovered.
Yawen Kong, Bo Zheng, Qiang Zhang, and Kebin He
Atmos. Chem. Phys., 22, 10769–10788, https://doi.org/10.5194/acp-22-10769-2022, https://doi.org/10.5194/acp-22-10769-2022, 2022
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We developed a Bayesian atmospheric inversion system based on the 4D local ensemble transform Kalman filter (4D-LETKF) algorithm coupled with GEOS-Chem from the latest Orbiting Carbon Observatory-2 (OCO-2) V10r XCO2 retrievals. This is the first adaptation of 4D-LETKF to an OCO-2-based global carbon inversion system. We inferred global gridded carbon fluxes and investigated their magnitudes, variations, and partitioning schemes to understand the global and regional carbon budgets for 2015–2020.
Shanshan Ouyang, Tao Deng, Run Liu, Jingyang Chen, Guowen He, Jeremy Cheuk-Hin Leung, Nan Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 10751–10767, https://doi.org/10.5194/acp-22-10751-2022, https://doi.org/10.5194/acp-22-10751-2022, 2022
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A record-breaking severe O3 pollution episode occurred under the influence of a Pacific subtropical high followed by Typhoon Mitag in the Pearl River Delta (PRD) in early Autumn 2019. Through WRF-CMAQ model simulations, we propose that the enhanced photochemical production of O3 during the episode is a major cause of the most severe O3 pollution year since the official O3 observation started in the PRD in 2006.
Luke M. Western, Alison L. Redington, Alistair J. Manning, Cathy M. Trudinger, Lei Hu, Stephan Henne, Xuekun Fang, Lambert J. M. Kuijpers, Christina Theodoridi, David S. Godwin, Jgor Arduini, Bronwyn Dunse, Andreas Engel, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Michela Maione, Jens Mühle, Simon O'Doherty, Hyeri Park, Sunyoung Park, Stefan Reimann, Peter K. Salameh, Daniel Say, Roland Schmidt, Tanja Schuck, Carolina Siso, Kieran M. Stanley, Isaac Vimont, Martin K. Vollmer, Dickon Young, Ronald G. Prinn, Ray F. Weiss, Stephen A. Montzka, and Matthew Rigby
Atmos. Chem. Phys., 22, 9601–9616, https://doi.org/10.5194/acp-22-9601-2022, https://doi.org/10.5194/acp-22-9601-2022, 2022
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The production of ozone-destroying gases is being phased out. Even though production of one of the main ozone-depleting gases, called HCFC-141b, has been declining for many years, the amount that is being released to the atmosphere has been increasing since 2017. We do not know for sure why this is. A possible explanation is that HCFC-141b that was used to make insulating foams many years ago is only now escaping to the atmosphere, or a large part of its production is not being reported.
Eva Gorrochategui, Isabel Hernandez, and Romà Tauler
Atmos. Chem. Phys., 22, 9111–9127, https://doi.org/10.5194/acp-22-9111-2022, https://doi.org/10.5194/acp-22-9111-2022, 2022
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A multiway methodology is proposed to handle complex and incomplete atmospheric data sets, providing concise and easily interpretable results. Changes in air quality by NO2, O3 and PM10 in 8 sampling stations located in Catalonia during the COVID-19 lockdown with respect to previous years (2018 and 2019) are investigated. Simultaneous analysis of the 3 contaminants among the 8 stations and for the 3 years allows the evaluation of correlations among the pollutants, even when having missing data.
Christopher D. Holmes
Atmos. Chem. Phys., 22, 9011–9015, https://doi.org/10.5194/acp-22-9011-2022, https://doi.org/10.5194/acp-22-9011-2022, 2022
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Cloud water and ice enable reactions that lead to acid rain and alter atmospheric oxidants, among other impacts. This work develops and evaluates an efficient method of simulating cloud chemistry within global and regional atmospheric models in order to better understand the role of clouds in atmospheric chemistry.
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
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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.
Angharad C. Stell, Michael Bertolacci, Andrew Zammit-Mangion, Matthew Rigby, Paul J. Fraser, Christina M. Harth, Paul B. Krummel, Xin Lan, Manfredi Manizza, Jens Mühle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, Dickon Young, and Anita L. Ganesan
EGUsphere, https://doi.org/10.5194/egusphere-2022-513, https://doi.org/10.5194/egusphere-2022-513, 2022
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Nitrous oxide is a potent greenhouse gas and ozone depleting substance, whose atmospheric abundance has risen throughout the contemporary record. In this work, we carry out the first global hierarchical Bayesian inversion to solve for nitrous oxide emissions. We derive increasing global nitrous oxide emissions, which are mainly driven by emissions between 0° and 30° N, with the highest emissions recorded in 2020.
Kaixiang Song, Run Liu, Yu Wang, Tao Liu, Liyan Wei, Yanxing Wu, Junyu Zheng, Boguang Wang, and Shaw Chen Liu
Atmos. Chem. Phys., 22, 8403–8416, https://doi.org/10.5194/acp-22-8403-2022, https://doi.org/10.5194/acp-22-8403-2022, 2022
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We developed an observation-based method to investigate the sensitivity of ozone formation to precursors during two elevated ozone episodes observed at 77 stations in Guangdong, China. We found approximately 67 % of the station days exhibit ozone formation sensitivity to NOx, 20 % of the station days are in the transitional regime sensitive to both NOx and volatile organic compounds (VOCs), and only 13 % of the station days are sensitive to VOCs.
Xiang Weng, Grant L. Forster, and Peer Nowack
Atmos. Chem. Phys., 22, 8385–8402, https://doi.org/10.5194/acp-22-8385-2022, https://doi.org/10.5194/acp-22-8385-2022, 2022
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We use machine learning to quantify the meteorological drivers behind surface ozone variations in China between 2015 and 2019. Our novel approaches show improved performance when compared to previous analysis methods. We highlight that nonlinearity in driver relationships and the impacts of large-scale meteorological phenomena are key to understanding ozone pollution. Moreover, we find that almost half of the observed ozone trend between 2015 and 2019 might have been driven by meteorology.
Zhaojun Tang, Jiaqi Chen, and Zhe Jiang
Atmos. Chem. Phys., 22, 7815–7826, https://doi.org/10.5194/acp-22-7815-2022, https://doi.org/10.5194/acp-22-7815-2022, 2022
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We provide a comparative analysis to explore the effects of satellite and surface measurements on atmospheric CO in data assimilations in 2015–2020 over East Asia. We find possible overestimated enhancements of atmospheric CO by assimilating surface CO measurements due to model representation errors, and a large discrepancy in the derived trends of CO columns due to different vertical sensitivities of satellite and surface observations to lower and free troposphere.
Yue Jia, Birgit Quack, Robert D. Kinley, Ignacio Pisso, and Susann Tegtmeier
Atmos. Chem. Phys., 22, 7631–7646, https://doi.org/10.5194/acp-22-7631-2022, https://doi.org/10.5194/acp-22-7631-2022, 2022
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In this study, we assessed the potential risks of bromoform released from Asparagopsis farming near Australia for the stratospheric ozone layer by analyzing different cultivation scenarios. We conclude that the intended operation of Asparagopsis seaweed cultivation farms with an annual yield to meet the needs of 50 % of feedlots and cattle in either open-ocean or terrestrial cultures in Australia will not impact the ozone layer under normal operating conditions.
Min Huang, James H. Crawford, Gregory R. Carmichael, Kevin W. Bowman, Sujay V. Kumar, and Colm Sweeney
Atmos. Chem. Phys., 22, 7461–7487, https://doi.org/10.5194/acp-22-7461-2022, https://doi.org/10.5194/acp-22-7461-2022, 2022
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This study demonstrates that ozone dry-deposition modeling can be improved by revising the model's dry-deposition parameterizations to better represent the effects of environmental conditions including the soil moisture fields. Applying satellite soil moisture data assimilation is shown to also have added value. Such advancements in coupled modeling and data assimilation can benefit the assessments of ozone impacts on human and vegetation health.
Shidong Fan and Ying Li
Atmos. Chem. Phys., 22, 7331–7351, https://doi.org/10.5194/acp-22-7331-2022, https://doi.org/10.5194/acp-22-7331-2022, 2022
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We investigated the mechanisms by which marine-emitted halogens influence the OH radical, which is not considered in air quality forecasting model systems. The atmospheric OH radical has a complicated response to halogen emissions by species through both physical and chemical processes. Over ocean, inorganic iodine is the controlling species and chemistry is more important. Over land, the physics of sea salt aerosols are more important. The mechanism is applicable to other circumstances.
Zhongjing Jiang and Jing Li
Atmos. Chem. Phys., 22, 7273–7285, https://doi.org/10.5194/acp-22-7273-2022, https://doi.org/10.5194/acp-22-7273-2022, 2022
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This study investigates the changes of tropospheric ozone in China associated with EP and CP El Niño, using satellite observations and the GEOS-Chem model. We found that El Niño generally leads to lower tropospheric ozone (LTO) decrease over most parts of China; La Niña acts the opposite. The difference between LTO changes during EP and CP El Niño primarily lies in southern China. Regional transport and chemical processes play the leading and secondary roles in driving the LTO changes.
Peter Huszar, Jan Karlický, Lukáš Bartík, Marina Liaskoni, Alvaro Patricio Prieto Perez, and Kateřina Šindelářová
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-337, https://doi.org/10.5194/acp-2022-337, 2022
Revised manuscript accepted for ACP
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Urbanization turns the rural land-cover into an artificial one while due to human activities, it introduces a great amount of emissions. We attempt to quantify the impact of urbanization on the final air-pollutant levels by looking at not only these emissions, but also on the way how the urban land-cover influences the meteorological conditions, how the removal of pollutants changes due to urban land-cover and finally, how emissions from vegetation change due to less vegetation in urban areas.
Linda Smoydzin and Peter Hoor
Atmos. Chem. Phys., 22, 7193–7206, https://doi.org/10.5194/acp-22-7193-2022, https://doi.org/10.5194/acp-22-7193-2022, 2022
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Our study presents a detailed analysis of the spatial and temporal distribution of elevated CO level in the upper troposphere over the Pacific using 20 years of MOPITT data. We create a climatology of severe pollution episodes and use trajectory calculations to link each particular pollution event detected in MOPITT satellite data with a distinct source region. Additionally, we analyse uplift mechanisms such as WCB-related upward transport.
Michael Sitwell, Mark W. Shephard, Yves Rochon, Karen Cady-Pereira, and Enrico Dammers
Atmos. Chem. Phys., 22, 6595–6624, https://doi.org/10.5194/acp-22-6595-2022, https://doi.org/10.5194/acp-22-6595-2022, 2022
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Observations of ammonia made using the satellite-borne CrIS instrument were used to improve the ammonia emissions used in the GEM-MACH model. These observations were used to refine estimates of the monthly mean ammonia emissions over North America for May to August 2016. The updated ammonia emissions reduced biases of GEM-MACH surface ammonia fields with surface observations and showed some improvements in the forecasting of species involved in inorganic particulate matter formation.
Yiwen Hu, Zengliang Zang, Xiaoyan Ma, Yi Li, Yanfei Liang, Wei You, Xiaobin Pan, and Zhijin Li
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-301, https://doi.org/10.5194/acp-2022-301, 2022
Revised manuscript accepted for ACP
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This study developed a four-dimensional variational assimilation (4DVAR) system based on WRF-Chem to optimize SO2 emissions. The system was applied to investigate the changes in SO2 emission in China during the COVID-19 lockdown, with special focus on Central China, by assimilating surface hourly SO2 observations. The results showed that the 4DVAR system can effectively optimize the emissions to describe the actual change in SO2 emissions during special events and improve the forecast skill.
Dimitris Akritidis, Andrea Pozzer, Johannes Flemming, Antje Inness, Philippe Nédélec, and Prodromos Zanis
Atmos. Chem. Phys., 22, 6275–6289, https://doi.org/10.5194/acp-22-6275-2022, https://doi.org/10.5194/acp-22-6275-2022, 2022
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We perform a process-oriented evaluation of Copernicus Atmosphere Monitoring Service (CAMS) reanalysis (CAMSRA) O3 over Europe using WOUDC (World Ozone and Ultraviolet Radiation Data Centre) ozonesondes and IAGOS (In-service Aircraft for a Global Observing System) aircraft measurements. Chemical data assimilation assists CAMSRA to reproduce the observed O3 increases in the troposphere during the examined folding events, but it mostly results in O3 overestimation in the upper troposphere.
Maximilian Herrmann, Moritz Schöne, Christian Borger, Simon Warnach, Thomas Wagner, Ulrich Platt, and Eva Gutheil
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-334, https://doi.org/10.5194/acp-2022-334, 2022
Revised manuscript accepted for ACP
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Ozone depletion events (ODEs) are a common occurence in the boundary layer during Arctic spring. Ozone is depleted by bromine species in an auto-catalytic reaction cycle. Previous modeling studies assumed an infinite bromine source at the ground. An alternative emission scheme is presented in which a finite amount of bromide in the snow is tracked over time. The Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) is used to study ODEs in the Arctic from February to May 2019.
Mike J. Newland, Camille Mouchel-Vallon, Richard Valorso, Bernard Aumont, Luc Vereecken, Michael E. Jenkin, and Andrew R. Rickard
Atmos. Chem. Phys., 22, 6167–6195, https://doi.org/10.5194/acp-22-6167-2022, https://doi.org/10.5194/acp-22-6167-2022, 2022
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Alkene ozonolysis produces Criegee intermediates, which can act as oxidants or decompose to give a range of closed-shell and radical products, including OH. Therefore it is essential to accurately represent the chemistry of Criegee intermediates in atmospheric models in order to understand their impacts on atmospheric composition. Here we provide a mechanism construction protocol by which the central features of alkene ozonolysis chemistry can be included in an automatic mechanism generator.
Guus J. M. Velders, John S. Daniel, Stephen A. Montzka, Isaac Vimont, Matthew Rigby, Paul B. Krummel, Jens Muhle, Simon O'Doherty, Ronald G. Prinn, Ray F. Weiss, and Dickon Young
Atmos. Chem. Phys., 22, 6087–6101, https://doi.org/10.5194/acp-22-6087-2022, https://doi.org/10.5194/acp-22-6087-2022, 2022
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The emissions of hydrofluorocarbons (HFCs) have increased significantly in the past as a result of the phasing out of ozone-depleting substances. Observations indicate that HFCs are used much less in certain refrigeration applications than previously projected. Current policies are projected to reduce emissions and the surface temperature contribution of HFCs from 0.28–0.44 °C to 0.14–0.31 °C in 2100. The Kigali Amendment is projected to reduce the contributions further to 0.04 °C in 2100.
Joe McNorton, Nicolas Bousserez, Anna Agustí-Panareda, Gianpaolo Balsamo, Luca Cantarello, Richard Engelen, Vincent Huijnen, Antje Inness, Zak Kipling, Mark Parrington, and Roberto Ribas
Atmos. Chem. Phys., 22, 5961–5981, https://doi.org/10.5194/acp-22-5961-2022, https://doi.org/10.5194/acp-22-5961-2022, 2022
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Concentrations of atmospheric methane continue to grow, in recent years at an increasing rate, for unknown reasons. Using newly available satellite observations and a state-of-the-art weather prediction model we perform global estimates of emissions from hotspots at high resolution. Results show that the system can accurately report on biases in national inventories and is used to conclude that the early COVID-19 slowdown period (March–June 2020) had little impact on global methane emissions.
Cynthia H. Whaley, Rashed Mahmood, Knut von Salzen, Barbara Winter, Sabine Eckhardt, Stephen Arnold, Stephen Beagley, Silvia Becagli, Rong-You Chien, Jesper Christensen, Sujay Manish Damani, Xinyi Dong, Konstantinos Eleftheriadis, Nikolaos Evangeliou, Gregory Faluvegi, Mark Flanner, Joshua S. Fu, Michael Gauss, Fabio Giardi, Wanmin Gong, Jens Liengaard Hjorth, Lin Huang, Ulas Im, Yugo Kanaya, Srinath Krishnan, Zbigniew Klimont, Thomas Kühn, Joakim Langner, Kathy S. Law, Louis Marelle, Andreas Massling, Dirk Olivié, Tatsuo Onishi, Naga Oshima, Yiran Peng, David A. Plummer, Olga Popovicheva, Luca Pozzoli, Jean-Christophe Raut, Maria Sand, Laura N. Saunders, Julia Schmale, Sangeeta Sharma, Ragnhild Bieltvedt Skeie, Henrik Skov, Fumikazu Taketani, Manu A. Thomas, Rita Traversi, Kostas Tsigaridis, Svetlana Tsyro, Steven Turnock, Vito Vitale, Kaley A. Walker, Minqi Wang, Duncan Watson-Parris, and Tahya Weiss-Gibbons
Atmos. Chem. Phys., 22, 5775–5828, https://doi.org/10.5194/acp-22-5775-2022, https://doi.org/10.5194/acp-22-5775-2022, 2022
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Air pollutants, like ozone and soot, play a role in both global warming and air quality. Atmospheric models are often used to provide information to policy makers about current and future conditions under different emissions scenarios. In order to have confidence in those simulations, in this study we compare simulated air pollution from 18 state-of-the-art atmospheric models to measured air pollution in order to assess how well the models perform.
Ruochong Xu, Joel A. Thornton, Ben H. Lee, Yanxu Zhang, Lyatt Jaeglé, Felipe D. Lopez-Hilfiker, Pekka Rantala, and Tuukka Petäjä
Atmos. Chem. Phys., 22, 5477–5494, https://doi.org/10.5194/acp-22-5477-2022, https://doi.org/10.5194/acp-22-5477-2022, 2022
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Monoterpenes are emitted into the atmosphere by vegetation and by the use of certain consumer products. Reactions of monoterpenes in the atmosphere lead to low-volatility products that condense to grow particulate matter or participate in new particle formation and, thus, affect air quality and climate. We use a model of atmospheric chemistry and transport to evaluate the global-scale importance of recent updates to our understanding of monoterpene chemistry in particle formation and growth.
Wei Ma, Zemin Feng, Junlei Zhan, Yongchun Liu, Pengfei Liu, Chengtang Liu, Qingxin Ma, Kang Yang, Yafei Wang, Hong He, Markku Kulmala, Yujing Mu, and Junfeng Liu
Atmos. Chem. Phys., 22, 4841–4851, https://doi.org/10.5194/acp-22-4841-2022, https://doi.org/10.5194/acp-22-4841-2022, 2022
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The influence of photochemical loss of volatile organic compounds (VOCS) on O3 formation is investigated using an observation-based model. The sensitivity regime of ozone formation might be misdiagnosed due to the photochemical loss of VOCs in the atmosphere. The contribution of local photochemistry is underestimated regarding O3 pollution when one does not consider the photochemical loss of VOCs.
Pinya Wang, Yang Yang, Huimin Li, Lei Chen, Ruijun Dang, Daokai Xue, Baojie Li, Jianping Tang, L. Ruby Leung, and Hong Liao
Atmos. Chem. Phys., 22, 4705–4719, https://doi.org/10.5194/acp-22-4705-2022, https://doi.org/10.5194/acp-22-4705-2022, 2022
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China is now suffering from both severe ozone (O3) pollution and heat events. We highlight that North China Plain is the hot spot of the co-occurrences of extremes in O3 and high temperatures in China. Such coupled extremes exhibit an increasing trend during 2014–2019 and will continue to increase until the middle of this century. And the coupled extremes impose more severe health impacts to human than O3 pollution occurring alone because of elevated O3 levels and temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O’Connor, and Steven T. Turnock
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-196, https://doi.org/10.5194/acp-2022-196, 2022
Revised manuscript accepted for ACP
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Weaknesses in process representation in chemistry-climate models lead to biases in simulating surface ozone and to uncertainty in projections of future ozone change. We develop a deep learning model to demonstrate the feasibility of ozone bias correction, and show the capability of providing improved assessments of the impacts of climate and emission changes on future air quality, along with valuable information to guide future model development.
Glenn M. Wolfe, Thomas F. Hanisco, Heather L. Arkinson, Donald R. Blake, Armin Wisthaler, Tomas Mikoviny, Thomas B. Ryerson, Ilana Pollack, Jeff Peischl, Paul O. Wennberg, John D. Crounse, Jason M. St. Clair, Alex Teng, L. Gregory Huey, Xiaoxi Liu, Alan Fried, Petter Weibring, Dirk Richter, James Walega, Samuel R. Hall, Kirk Ullmann, Jose L. Jimenez, Pedro Campuzano-Jost, T. Paul Bui, Glenn Diskin, James R. Podolske, Glen Sachse, and Ronald C. Cohen
Atmos. Chem. Phys., 22, 4253–4275, https://doi.org/10.5194/acp-22-4253-2022, https://doi.org/10.5194/acp-22-4253-2022, 2022
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Smoke plumes are chemically complex. This work combines airborne observations of smoke plume composition with a photochemical model to probe the production of ozone and the fate of reactive gases in the outflow of a large wildfire. Model–measurement comparisons illustrate how uncertain emissions and chemical processes propagate into simulated chemical evolution. Results provide insight into how this system responds to perturbations, which can help guide future observation and modeling efforts.
Nikos Daskalakis, Laura Gallardo, Maria Kanakidou, Johann Rasmus Nüß, Camilo Menares, Roberto Rondanelli, Anne M. Thompson, and Mihalis Vrekoussis
Atmos. Chem. Phys., 22, 4075–4099, https://doi.org/10.5194/acp-22-4075-2022, https://doi.org/10.5194/acp-22-4075-2022, 2022
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Forest fires emit carbon monoxide (CO) that can be transported into the atmosphere far from the sources and reacts to produce ozone (O3) that affects climate, ecosystems and health. O3 is also produced in the stratosphere and can be transported downwards. Using a global numerical model, we found that forest fires can affect CO and O3 even in the South Pacific, the most pristine region of the global ocean, but transport from the stratosphere is a more important O3 source than fires in the region.
Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Acher-Nicholls, Steve R. Dorling, Claire E. Reeves, and Tim Butler
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-173, https://doi.org/10.5194/acp-2022-173, 2022
Revised manuscript accepted for ACP
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As ozone can be transported across countries, efficient air quality management and regulatory policies rely on the assessment of local ozone production vs. transport. In our study, we investigate the origin of surface ozone in the UK and the contribution of the different source regions to regulatory ozone metrics. It is shown that emissions controls over western Europe would be necessary to improve health-related metrics and over larger areas to reduce impacts on ecosystems.
Le Cao, Linjie Fan, Simeng Li, and Shuangyan Yang
Atmos. Chem. Phys., 22, 3875–3890, https://doi.org/10.5194/acp-22-3875-2022, https://doi.org/10.5194/acp-22-3875-2022, 2022
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We analyzed the observational data and used models to discover the impact of the total ozone column (TOC) on the occurrence of tropospheric ozone depletion events (ODE) in the Antarctic. The results suggest that the decrease of TOC favors the occurrence of ODE. When TOC varies the rates of major ODE accelerating reactions are substantially altered but the rates of major ODE decelerating reactions remain unchanged. As a result, the occurrence of ODE negatively depends on the TOC.
Sarah E. Benish, Jesse O. Bash, Kristen M. Foley, K. Wyat Appel, Christian Hogrefe, Robert Gilliam, and George Pouliot
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-201, https://doi.org/10.5194/acp-2022-201, 2022
Revised manuscript accepted for ACP
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We assess CMAQ model simulations of nitrogen and sulfur deposition over US climate regions to evaluate the model ability to reproduce long-term deposition trends and total deposition budgets. A measurement-model fusion technique is found to improve estimates of wet deposition. Emission controls set by the Clean Air Act successfully decreased oxidized nitrogen deposition across the US and we find increasing amounts of reduced nitrogen to the total nitrogen budget over the simulation time period.
Henry Bowman, Steven Turnock, Susanne E. Bauer, Kostas Tsigaridis, Makoto Deushi, Naga Oshima, Fiona M. O'Connor, Larry Horowitz, Tongwen Wu, Jie Zhang, Dagmar Kubistin, and David D. Parrish
Atmos. Chem. Phys., 22, 3507–3524, https://doi.org/10.5194/acp-22-3507-2022, https://doi.org/10.5194/acp-22-3507-2022, 2022
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A full understanding of ozone in the troposphere requires investigation of its temporal variability over all timescales. Model simulations show that the northern midlatitude ozone seasonal cycle shifted with industrial development (1850–2014), with an increasing magnitude and a later summer peak. That shift reached a maximum in the mid-1980s, followed by a reversal toward the preindustrial cycle. The few available observations, beginning in the 1970s, are consistent with the model simulations.
Peter Bergamaschi, Arjo Segers, Dominik Brunner, Jean-Matthieu Haussaire, Stephan Henne, Michel Ramonet, Tim Arnold, Tobias Biermann, Huilin Chen, Sebastien Conil, Marc Delmotte, Grant Forster, Arnoud Frumau, Dagmar Kubistin, Xin Lan, Markus Leuenberger, Matthias Lindauer, Morgan Lopez, Giovanni Manca, Jennifer Müller-Williams, Simon O’Doherty, Bert Scheeren, Martin Steinbacher, Pamela Trisolino, Gabriela Vítková, and Camille Yver Kwok
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-118, https://doi.org/10.5194/acp-2022-118, 2022
Revised manuscript accepted for ACP
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We present a novel high-resolution inverse modelling system ("FLEXVAR") and its application for the inverse modelling of European CH4 emissions in 2018. The new FLEXVAR system combines high spatial resolution of 7 km x 7 km with a variational data assimilation technique, which allows to optimize CH4 emissions from individual model grid cells. The high resolution allows to better reproduce the observations, while the derived emissions show overall good consistency with two existing models.
Jason Schroeder, Chenxia Cai, Jin Xu, David Ridley, Jin Lu, Nancy Bui, Fang Yan, and Jeremy Avise
Atmos. Chem. Phys. Discuss., https://doi.org/10.5194/acp-2022-178, https://doi.org/10.5194/acp-2022-178, 2022
Revised manuscript accepted for ACP
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Ozone, a key component of smog, has plagued the Los Angeles region for decades. Ozone is created by complex chemical reactions that can be greatly impacted by anthropogenic emissions. This study makes use of the COVID-19 period to study the sensitivity of ozone chemistry in LA to certain anthropogenic emissions, notably from vehicles. We find that vehicular emissions of key pollutants dropped by up to 25 % during COVID-19, which caused a fundamental shift in ozone chemistry in the region.
Jingwei Zhang, Chaofan Lian, Weigang Wang, Maofa Ge, Yitian Guo, Haiyan Ran, Yusheng Zhang, Feixue Zheng, Xiaolong Fan, Chao Yan, Kaspar R. Daellenbach, Yongchun Liu, Markku Kulmala, and Junling An
Atmos. Chem. Phys., 22, 3275–3302, https://doi.org/10.5194/acp-22-3275-2022, https://doi.org/10.5194/acp-22-3275-2022, 2022
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This study added six potential HONO sources to the WRF-Chem model, evaluated their impact on HONO and O3 concentrations, including surface and vertical concentrations. The simulations extend our knowledge on atmospheric HONO sources, especially for nitrate photolysis. The study also explains the HONO difference in O3 formation on clean and hazy days, and reveals key potential HONO sources to O3 enhancements in haze-aggravating processes with a co-occurrence of high PM2.5 and O3 concentrations.
Lei Hu, Stephen A. Montzka, Fred Moore, Eric Hintsa, Geoff Dutton, M. Carolina Siso, Kirk Thoning, Robert W. Portmann, Kathryn McKain, Colm Sweeney, Isaac Vimont, David Nance, Bradley Hall, and Steven Wofsy
Atmos. Chem. Phys., 22, 2891–2907, https://doi.org/10.5194/acp-22-2891-2022, https://doi.org/10.5194/acp-22-2891-2022, 2022
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The unexpected increase in CFC-11 emissions between 2012 and 2017 resulted in concerns about delaying the stratospheric ozone recovery. Although the subsequent decline of CFC-11 emissions indicated a mitigation in part to this problem, the regions fully responsible for these large emission changes were unclear. Here, our new estimate, based on atmospheric measurements from two global campaigns and from NOAA, suggests Asia primarily contributed to the global CFC-11 emission rise during 2012–2017.
Dianyi Li, Drew Shindell, Dian Ding, Xiao Lu, Lin Zhang, and Yuqiang Zhang
Atmos. Chem. Phys., 22, 2625–2638, https://doi.org/10.5194/acp-22-2625-2022, https://doi.org/10.5194/acp-22-2625-2022, 2022
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In this study, we applied chemical transport model simulation with the latest annual anthropogenic emission inventory to study the long-term trend of ozone-induced crop production losses from 2010 to 2017 in China. We find that overall the ozone-induced crop production loss in China is significant and the annual average economic losses for wheat, rice, maize, and soybean in China are USD 9.55 billion, USD 8.53 billion, USD 2.23 billion, and USD 1.16 billion respectively, over the 8 years.
Jing Cao, Shuping Situ, Yufang Hao, Shaodong Xie, and Lingyu Li
Atmos. Chem. Phys., 22, 2351–2364, https://doi.org/10.5194/acp-22-2351-2022, https://doi.org/10.5194/acp-22-2351-2022, 2022
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Based on localized emission factors and high-resolution vegetation data, we simulated the impacts of BVOC emissions on O3 and SOA during 1981–2018 in China. The interannual variation of BVOC emissions caused by increasing leaf biomass resulted in O3 and SOA concentrations increasing at average annual rates of 0.11 ppb and 0.008 μg m−3, respectively. The results show different variations which can be attributed to the different changing trends of leaf biomass by region and vegetation type.
Narcisse Tsona Tchinda, Lin Du, Ling Liu, and Xiuhui Zhang
Atmos. Chem. Phys., 22, 1951–1963, https://doi.org/10.5194/acp-22-1951-2022, https://doi.org/10.5194/acp-22-1951-2022, 2022
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This study explores the effect of pyruvic acid (PA) both in the SO3 hydrolysis and in sulfuric-acid-based aerosol formation. Results show that in dry and polluted areas, PA-catalyzed SO3 hydrolysis is about 2 orders of magnitude more efficient at forming sulfuric acid than the water-catalyzed reaction. Moreover, PA can effectively enhance the ternary SA-PA-NH3 particle formation rate by up to 4.7×102 relative to the binary SA-NH3 particle formation rate at cold temperatures.
Zhenze Liu, Ruth M. Doherty, Oliver Wild, Fiona M. O'Connor, and Steven T. Turnock
Atmos. Chem. Phys., 22, 1209–1227, https://doi.org/10.5194/acp-22-1209-2022, https://doi.org/10.5194/acp-22-1209-2022, 2022
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Tropospheric ozone is important to future air quality and climate, and changing emissions and climate influence ozone. We investigate the evolution of ozone and ozone sensitivity from the present day (2004–2014) to the future (2045–2055) and explore the main drivers of ozone changes from global and regional perspectives. This helps guide suitable emission control strategies to mitigate ozone pollution.
Haiyue Tan, Lin Zhang, Xiao Lu, Yuanhong Zhao, Bo Yao, Robert J. Parker, and Hartmut Boesch
Atmos. Chem. Phys., 22, 1229–1249, https://doi.org/10.5194/acp-22-1229-2022, https://doi.org/10.5194/acp-22-1229-2022, 2022
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Methane is the second most important anthropogenic greenhouse gas. Understanding methane emissions and concentration growth over China in the past decade is important to support its mitigation. This study analyzes the contributions of methane emissions from different regions and sources over the globe to methane changes over China in 2007–2018. Our results show strong international transport influences and emphasize the need of intensive methane measurements covering eastern China.
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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 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.
Dry deposition of tropospheric ozone relates to its destruction at the Earth’s surface. An...
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