Articles | Volume 23, issue 10
https://doi.org/10.5194/acp-23-5801-2023
© Author(s) 2023. 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-23-5801-2023
© Author(s) 2023. This work is distributed under
the Creative Commons Attribution 4.0 License.
the Creative Commons Attribution 4.0 License.
Research article
| 
24 May 2023
Research article |
| 24 May 2023
| 24 May 2023
Large simulated future changes in the nitrate radical under the CMIP6 SSP scenarios: implications for oxidation chemistry
Scott Archer-Nicholls
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
now at: IT Services, University of Manchester, Manchester, M13 9PL, UK
Rachel Allen
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
Nathan L. Abraham
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
NCAS-Climate, University of Cambridge, Cambridge, CB2 1EW, UK
Paul T. Griffiths
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
NCAS-Climate, University of Cambridge, Cambridge, CB2 1EW, UK
Department of Chemistry, University of Cambridge, Cambridge, CB2 1EW, UK
NCAS-Climate, University of Cambridge, Cambridge, CB2 1EW, UK
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Johana Romero-Alvarez, Aurelia Lupaşcu, Douglas Lowe, Alba Badia, Scott Archer-Nicholls, Steve Dorling, Claire E. Reeves, and Tim Butler
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R. Anthony Cox, Markus Ammann, John N. Crowley, Paul T. Griffiths, Hartmut Herrmann, Erik H. Hoffmann, Michael E. Jenkin, V. Faye McNeill, Abdelwahid Mellouki, Christopher J. Penkett, Andreas Tilgner, and Timothy J. Wallington
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John Staunton-Sykes, Thomas J. Aubry, Youngsub M. Shin, James Weber, Lauren R. Marshall, Nathan Luke Abraham, Alex Archibald, and Anja Schmidt
Atmos. Chem. Phys., 21, 9009–9029, https://doi.org/10.5194/acp-21-9009-2021, https://doi.org/10.5194/acp-21-9009-2021, 2021
Ashok K. Luhar, Ian E. Galbally, Matthew T. Woodhouse, and Nathan Luke Abraham
Atmos. Chem. Phys., 21, 7053–7082, https://doi.org/10.5194/acp-21-7053-2021, https://doi.org/10.5194/acp-21-7053-2021, 2021
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James Keeble, Birgit Hassler, Antara Banerjee, Ramiro Checa-Garcia, Gabriel Chiodo, Sean Davis, Veronika Eyring, Paul T. Griffiths, Olaf Morgenstern, Peer Nowack, Guang Zeng, Jiankai Zhang, Greg Bodeker, Susannah Burrows, Philip Cameron-Smith, David Cugnet, Christopher Danek, Makoto Deushi, Larry W. Horowitz, Anne Kubin, Lijuan Li, Gerrit Lohmann, Martine Michou, Michael J. Mills, Pierre Nabat, Dirk Olivié, Sungsu Park, Øyvind Seland, Jens Stoll, Karl-Hermann Wieners, and Tongwen Wu
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The effect aerosols have on climate can be better understood by studying their vertical and spatial distribution throughout the atmosphere. We use observation data from the ATom campaign and evaluate the vertical profile of aerosol number concentration, sulfur dioxide and condensation sink using the UKESM (UK Earth System Model). We identify uncertainties in key atmospheric processes that help improve their theoretical representation in global climate models.
Paul T. Griffiths, Lee T. Murray, Guang Zeng, Youngsub Matthew Shin, N. Luke Abraham, Alexander T. Archibald, Makoto Deushi, Louisa K. Emmons, Ian E. Galbally, Birgit Hassler, Larry W. Horowitz, James Keeble, Jane Liu, Omid Moeini, Vaishali Naik, Fiona M. O'Connor, Naga Oshima, David Tarasick, Simone Tilmes, Steven T. Turnock, Oliver Wild, Paul J. Young, and Prodromos Zanis
Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, https://doi.org/10.5194/acp-21-4187-2021, 2021
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We analyse the CMIP6 Historical and future simulations for tropospheric ozone, a species which is important for many aspects of atmospheric chemistry. We show that the current generation of models agrees well with observations, being particularly successful in capturing trends in surface ozone and its vertical distribution in the troposphere. We analyse the factors that control ozone and show that they evolve over the period of the CMIP6 experiments.
Peter Sherman, Meng Gao, Shaojie Song, Alex T. Archibald, Nathan Luke Abraham, Jean-François Lamarque, Drew Shindell, Gregory Faluvegi, and Michael B. McElroy
Atmos. Chem. Phys., 21, 3593–3605, https://doi.org/10.5194/acp-21-3593-2021, https://doi.org/10.5194/acp-21-3593-2021, 2021
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The aims here are to assess the role of aerosols in India's monsoon precipitation and to determine the relative contributions from Chinese and Indian emissions using CMIP6 models. We find that increased sulfur emissions reduce precipitation, which is primarily dynamically driven due to spatial shifts in convection over the region. A significant increase in precipitation (up to ~ 20 %) is found only when both Indian and Chinese sulfate emissions are regulated.
Fiona M. O'Connor, N. Luke Abraham, Mohit Dalvi, Gerd A. Folberth, Paul T. Griffiths, Catherine Hardacre, Ben T. Johnson, Ron Kahana, James Keeble, Byeonghyeon Kim, Olaf Morgenstern, Jane P. Mulcahy, Mark Richardson, Eddy Robertson, Jeongbyn Seo, Sungbo Shim, João C. Teixeira, Steven T. Turnock, Jonny Williams, Andrew J. Wiltshire, Stephanie Woodward, and Guang Zeng
Atmos. Chem. Phys., 21, 1211–1243, https://doi.org/10.5194/acp-21-1211-2021, https://doi.org/10.5194/acp-21-1211-2021, 2021
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This paper calculates how changes in emissions and/or concentrations of different atmospheric constituents since the pre-industrial era have altered the Earth's energy budget at the present day using a metric called effective radiative forcing. The impact of land use change is also assessed. We find that individual contributions do not add linearly, and different Earth system interactions can affect the magnitude of the calculated effective radiative forcing.
Gillian Thornhill, William Collins, Dirk Olivié, Ragnhild B. Skeie, Alex Archibald, Susanne Bauer, Ramiro Checa-Garcia, Stephanie Fiedler, Gerd Folberth, Ada Gjermundsen, Larry Horowitz, Jean-Francois Lamarque, Martine Michou, Jane Mulcahy, Pierre Nabat, Vaishali Naik, Fiona M. O'Connor, Fabien Paulot, Michael Schulz, Catherine E. Scott, Roland Séférian, Chris Smith, Toshihiko Takemura, Simone Tilmes, Kostas Tsigaridis, and James Weber
Atmos. Chem. Phys., 21, 1105–1126, https://doi.org/10.5194/acp-21-1105-2021, https://doi.org/10.5194/acp-21-1105-2021, 2021
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We find that increased temperatures affect aerosols and reactive gases by changing natural emissions and their rates of removal from the atmosphere. Changing the composition of these species in the atmosphere affects the radiative budget of the climate system and therefore amplifies or dampens the climate response of climate models of the Earth system. This study found that the largest effect is a dampening of climate change as warmer temperatures increase the emissions of cooling aerosols.
Gillian D. Thornhill, William J. Collins, Ryan J. Kramer, Dirk Olivié, Ragnhild B. Skeie, Fiona M. O'Connor, Nathan Luke Abraham, Ramiro Checa-Garcia, Susanne E. Bauer, Makoto Deushi, Louisa K. Emmons, Piers M. Forster, Larry W. Horowitz, Ben Johnson, James Keeble, Jean-Francois Lamarque, Martine Michou, Michael J. Mills, Jane P. Mulcahy, Gunnar Myhre, Pierre Nabat, Vaishali Naik, Naga Oshima, Michael Schulz, Christopher J. Smith, Toshihiko Takemura, Simone Tilmes, Tongwen Wu, Guang Zeng, and Jie Zhang
Atmos. Chem. Phys., 21, 853–874, https://doi.org/10.5194/acp-21-853-2021, https://doi.org/10.5194/acp-21-853-2021, 2021
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This paper is a study of how different constituents in the atmosphere, such as aerosols and gases like methane and ozone, affect the energy balance in the atmosphere. Different climate models were run using the same inputs to allow an easy comparison of the results and to understand where the models differ. We found the effect of aerosols is to reduce warming in the atmosphere, but this effect varies between models. Reactions between gases are also important in affecting climate.
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
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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.
Sandip S. Dhomse, Graham W. Mann, Juan Carlos Antuña Marrero, Sarah E. Shallcross, Martyn P. Chipperfield, Kenneth S. Carslaw, Lauren Marshall, N. Luke Abraham, and Colin E. Johnson
Atmos. Chem. Phys., 20, 13627–13654, https://doi.org/10.5194/acp-20-13627-2020, https://doi.org/10.5194/acp-20-13627-2020, 2020
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We confirm downward adjustment of SO2 emission to simulate the Pinatubo aerosol cloud with aerosol microphysics models. Similar adjustment is also needed to simulate the El Chichón and Agung volcanic cloud, indicating potential missing removal or vertical redistribution process in models. Important inhomogeneities in the CMIP6 forcing datasets after Agung and El Chichón eruptions are difficult to reconcile. Quasi-biennial oscillation plays an important role in modifying stratospheric warming.
David S. Stevenson, Alcide Zhao, Vaishali Naik, Fiona M. O'Connor, Simone Tilmes, Guang Zeng, Lee T. Murray, William J. Collins, Paul T. Griffiths, Sungbo Shim, Larry W. Horowitz, Lori T. Sentman, and Louisa Emmons
Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, https://doi.org/10.5194/acp-20-12905-2020, 2020
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We present historical trends in atmospheric oxidizing capacity (OC) since 1850 from the latest generation of global climate models and compare these with estimates from measurements. OC controls levels of many key reactive gases, including methane (CH4). We find small model trends up to 1980, then increases of about 9 % up to 2014, disagreeing with (uncertain) measurement-based trends. Major drivers of OC trends are emissions of CH4, NOx, and CO; these will be important for future CH4 trends.
Andrew Orr, J. Scott Hosking, Aymeric Delon, Lars Hoffmann, Reinhold Spang, Tracy Moffat-Griffin, James Keeble, Nathan Luke Abraham, and Peter Braesicke
Atmos. Chem. Phys., 20, 12483–12497, https://doi.org/10.5194/acp-20-12483-2020, https://doi.org/10.5194/acp-20-12483-2020, 2020
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Polar stratospheric clouds (PSCs) are clouds found in the Antarctic winter stratosphere and are implicated in the formation of the ozone hole. These clouds can sometimes be formed or enhanced by mountain waves, formed as air passes over hills or mountains. However, this important mechanism is missing in coarse-resolution climate models, limiting our ability to simulate ozone. This study examines an attempt to include the effects of mountain waves and their impact on PSCs and ozone.
James Weber, Scott Archer-Nicholls, Paul Griffiths, Torsten Berndt, Michael Jenkin, Hamish Gordon, Christoph Knote, and Alexander T. Archibald
Atmos. Chem. Phys., 20, 10889–10910, https://doi.org/10.5194/acp-20-10889-2020, https://doi.org/10.5194/acp-20-10889-2020, 2020
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Highly oxygenated organic molecules (HOMs) are important for aerosol growth and new particle formation, particularly in air masses with less sulphuric acid. This new chemical mechanism reproduces measured [HOM] and [HOM precursors] and is concise enough for use in global climate models. The mechanism also reproduces the observed suppression of HOMs by isoprene, suggesting enhanced emissions may not necessarily lead to more aerosols. Greater HOM importance in the pre-industrial era is also shown.
Cited articles
Archer-Nicholls, S., Abraham, N. L., Shin, Y. M., Weber, J., Russo, M. R., Lowe, D., Utembe, S. R., O'Connor, F. M., Kerridge, B., Latter, B., Siddans, R., Jenkin, M., Wild, O., and Archibald, A. T.:
The Common Representative Intermediates Mechanism Version 2 in the United Kingdom Chemistry and Aerosols Model, J. Adv. Model. Earth Sy., 13, 1–37, https://doi.org/10.1029/2020MS002420, 2021.
Archer-Nicholls, S., Allen, R., Shin, Y., Abraham, N. L., Griffiths, P., and Archibald, A.: UKESM1 diagnostics for CMIP6 ScenarioMIP and CMIP historical experiments, NERC EDS Centre for Environmental Data Analysis [data set], https://doi.org/10.5285/b70e6ae10a9f463d88819eb981cd4d0f, 2023.
Archibald, A. T., Neu, J. L., Elshorbany, Y. F., Cooper, O. R., Young, P. J., Akiyoshi, H., Cox, R. A., Coyle, M., Derwent, R. G., Deushi, M., and Finco, A.:
Tropospheric Ozone Assessment Report: A critical review of changes in the tropospheric ozone burden and budget from 1850 to 2100, Elementa: Science of the Anthropocene, 8, 1–53, https://doi.org/10.1525/elementa.2020.034, 2020a.
Archibald, A. T., O'Connor, F. M., Abraham, N. L., Archer-Nicholls, S., Chipperfield, M. P., Dalvi, M., Folberth, G. A., Dennison, F., Dhomse, S. S., Griffiths, P. T., Hardacre, C., Hewitt, A. J., Hill, R. S., Johnson, C. E., Keeble, J., Köhler, M. O., Morgenstern, O., Mulcahy, J. P., Ordóñez, C., Pope, R. J., Rumbold, S. T., Russo, M. R., Savage, N. H., Sellar, A., Stringer, M., Turnock, S. T., Wild, O., and Zeng, G.:
Description and evaluation of the UKCA stratosphere–troposphere chemistry scheme (StratTrop vn 1.0) implemented in UKESM1, Geosci. Model Dev., 13, 1223–1266, https://doi.org/10.5194/gmd-13-1223-2020, 2020b.
Arneth, A., Niinemets, Ü., Pressley, S., Bäck, J., Hari, P., Karl, T., Noe, S., Prentice, I. C., Serça, D., Hickler, T., Wolf, A., and Smith, B.:
Process-based estimates of terrestrial ecosystem isoprene emissions: incorporating the effects of a direct CO2−isoprene interaction, Atmos. Chem. Phys., 7, 31–53, https://doi.org/10.5194/acp-7-31-2007, 2007.
Arneth, A., Monson, R. K., Schurgers, G., Niinemets, Ü., and Palmer, P. I.:
Why are estimates of global terrestrial isoprene emissions so similar (and why is this not so for monoterpenes)?, Atmos. Chem. Phys., 8, 4605–4620, https://doi.org/10.5194/acp-8-4605-2008, 2008.
Atkinson, R. and Arey, J.:
Gas-phase tropospheric chemistry of biogenic volatile organic compounds: A review, Atmos. Environ., 37, 197–219. https://doi.org/10.1016/S1352-2310(03)00391-1, 2003.
Atkinson, R., Baulch, D. L., Cox, R. A., Hampson, R. F., Kerr Chairman, J. A., and Troe, J.:
Evaluated Kinetic and Photochemical Data for Atmospheric Chemistry: Supplement III, IUPAC Subcommittee on Gas Kinetic Data Evaluation for Atmospheric Chemistry, J. Phys. Chem. Ref. Data, 18, 881–1097, https://doi.org/10.1063/1.555832, 1989.
Bianchi, F., Kurtén, T., Riva, M., Mohr, C., Rissanen, M. P., Roldin, P., Berndt, T., Crounse, J. D., Wennberg, P. O., Mentel, T. F., Wildt, J., Junninen, H., Jokinen, T., Kulmala, M., Worsnop, D. R., Thornton, J. A., Donahue, N., Kjaergaard, H. G., and Ehn, M.:
Highly Oxygenated Organic Molecules (HOM) from Gas-Phase Autoxidation Involving Peroxy Radicals: A Key Contributor to Atmospheric Aerosol, Chem. Rev., 119, 3472–3509, https://doi.org/10.1021/acs.chemrev.8b00395, 2019.
Boyd, C. M., Sanchez, J., Xu, L., Eugene, A. J., Nah, T., Tuet, W. Y., Guzman, M. I., and Ng, N. L.:
Secondary organic aerosol formation from the
Brewer, D. A., Ogliaruso, M. A., Augustsson, T. R., and Levine, J. S.:
The oxidation of isoprene in the troposphere: Mechanism and model calculations, Atmos. Environ. (1967), 18, 2723–2744, https://doi.org/10.1016/0004-6981(84)90338-X, 1984.
Brown, S. S. and Stutz, J.:
Nighttime radical observations and chemistry, Chem. Soc. Rev., 41, 6405–6447, 2012.
Cao, Y., Yue, X., Liao, H., Yang, Y., Zhu, J., Chen, L., Tian, C., Lei, Y., Zhou, H., and Ma, Y.:
Ensemble projection of global isoprene emissions by the end of 21st century using CMIP6 models, Atmos. Environ., 267, 118766, https://doi.org/10.1016/j.atmosenv.2021.118766, 2021.
Ehn, M., Thornton, J. A., Kleist, E., Sipilä, M., Junninen, H., Pullinen, I., Springer, M., Rubach, F., Tillmann, R., Lee, B., Lopez-Hilfiker, F., Andres, S., Acir, I.-H., Rissanen, M., Jokinen, T., Schobesberger, S., Kangasluoma, J., Kontkanen, J., Nieminen, T., and Mentel, T. F.:
A large source of low-volatility secondary organic aerosol, Nature, 506, 476–479, https://doi.org/10.1038/nature13032, 2014.
Ehn, M., Berndt, T., Wildt, J., and Mentel, T.: Highly oxygenated molecules from atmospheric autoxidation of hydrocarbons: a prominent challenge for chemical kinetics studies, Int. J. Chem. Kinet., 49, 821–831, 2017.
Eyring, V., Bony, S., Meehl, G. A., Senior, C. A., Stevens, B., Stouffer, R. J., and Taylor, K. E.:
Overview of the Coupled Model Intercomparison Project Phase 6 (CMIP6) experimental design and organization, Geosci. Model Dev., 9, 1937–1958, https://doi.org/10.5194/gmd-9-1937-2016, 2016.
Faxon, C., Hammes, J., Le Breton, M., Pathak, R. K., and Hallquist, M.: Characterization of organic nitrate constituents of secondary organic aerosol (SOA) from nitrate-radical-initiated oxidation of limonene using high-resolution chemical ionization mass spectrometry, Atmos. Chem. Phys., 18, 5467–5481, https://doi.org/10.5194/acp-18-5467-2018, 2018.
Fish, D. J., Shallcross, D. E., and Jones, R. L.:
The vertical distribution of NO3 in the atmospheric boundary layer, Atmos. Environ., 33, 687–691, https://doi.org/10.1016/S1352-2310(98)00332-X, 1999.
Fry, J. L., Kiendler-Scharr, A., Rollins, A. W., Wooldridge, P. J., Brown, S. S., Fuchs, H., Dubé, W., Mensah, A., dal Maso, M., Tillmann, R., Dorn, H.-P., Brauers, T., and Cohen, R. C.:
Organic nitrate and secondary organic aerosol yield from NO3 oxidation of β-pinene evaluated using a gas-phase kinetics/aerosol partitioning model, Atmos. Chem. Phys., 9, 1431–1449, https://doi.org/10.5194/acp-9-1431-2009, 2009.
Gidden, M. J., Riahi, K., Smith, S. J., Fujimori, S., Luderer, G., Kriegler, E., van Vuuren, D. P., van den Berg, M., Feng, L., Klein, D., Calvin, K., Doelman, J. C., Frank, S., Fricko, O., Harmsen, M., Hasegawa, T., Havlik, P., Hilaire, J., Hoesly, R., Horing, J., Popp, A., Stehfest, E., and Takahashi, K.:
Global emissions pathways under different socioeconomic scenarios for use in CMIP6: a dataset of harmonized emissions trajectories through the end of the century, Geosci. Model Dev., 12, 1443–1475, https://doi.org/10.5194/gmd-12-1443-2019, 2019.
Gordon, H., Kirkby, J., Baltensperger, U., Bianchi, F., Breitenlechner, M., Curtius, J., Dias, A., Dommen, J., Donahue, N. M., Dunne, E. M., Duplissy, J., Ehrhart, S., Flagan, R. C., Frege, C., Fuchs, C., Hansel, A., Hoyle, C. R., Kulmala, M., Kürten, A., and Carslaw, K. S.:
Causes and importance of new particle formation in the present-day and preindustrial atmospheres, J. Geophys. Res.-Atmos., 122, 8739–8760, https://doi.org/10.1002/2017JD026844, 2017.
Griffiths, P. T., Murray, L. T., Zeng, G., Shin, Y. M., Abraham, N. L., Archibald, A. T., Deushi, M., Emmons, L. K., Galbally, I. E., Hassler, B., Horowitz, L. W., Keeble, J., Liu, J., Moeini, O., Naik, V., O'Connor, F. M., Oshima, N., Tarasick, D., Tilmes, S., Turnock, S. T., Wild, O., Young, P. J., and Zanis, P.:
Tropospheric ozone in CMIP6 simulations, Atmos. Chem. Phys., 21, 4187–4218, https://doi.org/10.5194/acp-21-4187-2021, 2021.
Hamilton, J. F., Bryant, D. J., Edwards, P. M., Ouyang, B., Bannan, T. J., Mehra, A., Mayhew, A. W., Hopkins, J. R., Dunmore, R. E., Squires, F. A., Lee, J. D., Newland, M. J., Worrall, S. D., Bacak, A., Coe, H., Percival, C., Whalley, L. K., Heard, D. E., Slater, E. J., Jones, R. L., Cui, T., Surratt, J. D., Reeves, C. E., Mills, G. P., Grimmond, S., Sun, Y., Xu, W., Shi, Z., and Rickard, A. R.: Key Role of NO3 Radicals in the Production of Isoprene Nitrates and Nitrooxyorganosulfates in Beijing,
Environ. Sci. Technol., 55, 842–853,
https://doi.org/10.1021/acs.est.0c05689, 2021.
Hantson, S., Knorr, W., Schurgers, G., Pugh, T. A. M., and Arneth, A.:
Global isoprene and monoterpene emissions under changing climate, vegetation, CO2 and land use, Atmos. Environ., 155, 35–45, https://doi.org/10.1016/j.atmosenv.2017.02.010, 2017.
He, Q., Tomaz, S., Li, C., Zhu, M., Meidan, D., Riva, M., Laskin, A., Brown, S. S., George, C., Wang, X., and Rudich, Y.:
Optical properties of secondary organic aerosol produced by nitrate radical oxidation of biogenic volatile organic compounds, Environ. Sci. Technol., 55, 2878–2889, https://doi.org/10.1021/acs.est.0c06838, 2021.
Hoesly, R. M., Smith, S. J., Feng, L., Klimont, Z., Janssens-Maenhout, G., Pitkanen, T., Seibert, J. J., Vu, L., Andres, R. J., Bolt, R. M., Bond, T. C., Dawidowski, L., Kholod, N., Kurokawa, J.-I., Li, M., Liu, L., Lu, Z., Moura, M. C. P., O'Rourke, P. R., and Zhang, Q.:
Historical (1750–2014) anthropogenic emissions of reactive gases and aerosols from the Community Emissions Data System (CEDS), Geosci. Model Dev., 11, 369–408, https://doi.org/10.5194/gmd-11-369-2018, 2018.
Hoyle, C. R., Boy, M., Donahue, N. M., Fry, J. L., Glasius, M., Guenther, A., Hallar, A. G., Huff Hartz, K., Petters, M. D., Petäjä, T., Rosenoern, T., and Sullivan, A. P.:
A review of the anthropogenic influence on biogenic secondary organic aerosol, Atmos. Chem. Phys., 11, 321–343, https://doi.org/10.5194/acp-11-321-2011, 2011.
Jones, A. C., Hill, A., Remy, S., Abraham, N. L., Dalvi, M., Hardacre, C., Hewitt, A. J., Johnson, B., Mulcahy, J. P., and Turnock, S. T.:
Exploring the sensitivity of atmospheric nitrate concentrations to nitric acid uptake rate using the Met Office's Unified Model, Atmos. Chem. Phys., 21, 15901–15927, https://doi.org/10.5194/acp-21-15901-2021, 2021.
Khan, M. A. H., Cooke, M. C., Utembe, S. R., Archibald, A. T., Derwent, R. G., Xiao, P., Percival, C. J., Jenkin, M. E., Morris, W. C., and Shallcross, D. E.:
Global modeling of the nitrate radical (NO3) for present and pre-industrial scenarios, Atmos. Res., 164–165, 347–357, https://doi.org/10.1016/j.atmosres.2015.06.006, 2015.
Kiendler-Scharr, A., Mensah, A. A., Friese, E., Topping, D., Nemitz, E., Prévôt, A. S., Äijälä, M., Allan, J., Canonaco, F., Canagaratna, M., and Carbone, S.:
Ubiquity of organic nitrates from nighttime chemistry in the European submicron aerosol, Geophys. Res. Lett., 43, 7735–7744, https://doi.org/10.1002/2016GL069239, 2016.
Li, S., Liu, W., Xie, P., Qin, M., and Yang, Y.:
Observation of nitrate radical in the nocturnal boundary layer during a summer field campaign in pearl river delta China, Terr. Atmos. Ocean. Sci., 23, 39–48, https://doi.org/10.3319/TAO.2011.07.26.01(A), 2012.
Mann, G. W., Carslaw, K. S., Spracklen, D. V., Ridley, D. A., Manktelow, P. T., Chipperfield, M. P., Pickering, S. J., and Johnson, C. E.:
Description and evaluation of GLOMAP-mode: a modal global aerosol microphysics model for the UKCA composition-climate model, Geosci. Model Dev., 3, 519–551, https://doi.org/10.5194/gmd-3-519-2010, 2010.
McDuffie, E. E., Fibiger, D. L., Dubé, W. P., Lopez-Hilfiker, F., Lee, B. H., Thornton, J. A.,
Shah, V., Jaeglé, L., Guo, H., Weber, R. J., Reeves, J. M., Weinheimer, A. J., Schroder, J. C., Campuzano-Jost, P., Jimenez, J. L., Dibb, J. E., Veres, P., Ebben, C., Sparks, T. L., Wooldridge, P. J., Cohen, R. C., Hornbrook, R. S., Apel, E. C., Campos, T., Hall, S. R., Ullmann, K., and Brown, S. S.: Heterogeneous N2O5 uptake during winter: Aircraft measurements during the 2015 WINTER campaign and critical evaluation of current parameterizations, J. Geophys. Res.-Atmos., 123, 4345–4372, https://doi.org/10.1002/2018JD028336, 2018.
McGillen, M. R., Carter, W. P. L., Mellouki, A., Orlando, J. J., Picquet-Varrault, B., and Wallington, T. J.:
Database for the kinetics of the gas-phase atmospheric reactions of organic compounds, Earth Syst. Sci. Data, 12, 1203–1216, https://doi.org/10.5194/essd-12-1203-2020, 2020.
Monks, P. S., Archibald, A. T., Colette, A., Cooper, O., Coyle, M., Derwent, R., Fowler, D., Granier, C., Law, K. S., Mills, G. E., Stevenson, D. S., Tarasova, O., Thouret, V., von Schneidemesser, E., Sommariva, R., Wild, O., and Williams, M. L.:
Tropospheric ozone and its precursors from the urban to the global scale from air quality to short-lived climate forcer, Atmos. Chem. Phys., 15, 8889–8973, https://doi.org/10.5194/acp-15-8889-2015, 2015.
Mulcahy, J. P., Johnson, C., Jones, C. G., Povey, A. C., Scott, C. E., Sellar, A., Turnock, S. T., Woodhouse, M. T., Abraham, N. L., Andrews, M. B., Bellouin, N., Browse, J., Carslaw, K. S., Dalvi, M., Folberth, G. A., Glover, M., Grosvenor, D. P., Hardacre, C., Hill, R., Johnson, B., Jones, A., Kipling, Z., Mann, G., Mollard, J., O'Connor, F. M., Palmiéri, J., Reddington, C., Rumbold, S. T., Richardson, M., Schutgens, N. A. J., Stier, P., Stringer, M., Tang, Y., Walton, J., Woodward, S., and Yool, A.:
Description and evaluation of aerosol in UKESM1 and HadGEM3-GC3.1 CMIP6 historical simulations, Geosci. Model Dev., 13, 6383–6423, https://doi.org/10.5194/gmd-13-6383-2020, 2020.
Ng, N. L., Brown, S. S., Archibald, A. T., Atlas, E., Cohen, R. C., Crowley, J. N., Day, D. A., Donahue, N. M., Fry, J. L., Fuchs, H., Griffin, R. J., Guzman, M. I., Herrmann, H., Hodzic, A., Iinuma, Y., Jimenez, J. L., Kiendler-Scharr, A., Lee, B. H., Luecken, D. J., Mao, J., McLaren, R., Mutzel, A., Osthoff, H. D., Ouyang, B., Picquet-Varrault, B., Platt, U., Pye, H. O. T., Rudich, Y., Schwantes, R. H., Shiraiwa, M., Stutz, J., Thornton, J. A., Tilgner, A., Williams, B. J., and Zaveri, R. A.:
Nitrate radicals and biogenic volatile organic compounds: oxidation, mechanisms, and organic aerosol, Atmos. Chem. Phys., 17, 2103–2162, https://doi.org/10.5194/acp-17-2103-2017, 2017.
O'Neill, B. C., Tebaldi, C., van Vuuren, D. P., Eyring, V., Friedlingstein, P., Hurtt, G., Knutti, R., Kriegler, E., Lamarque, J.-F., Lowe, J., Meehl, G. A., Moss, R., Riahi, K., and Sanderson, B. M.:
The Scenario Model Intercomparison Project (ScenarioMIP) for CMIP6, Geosci. Model Dev., 9, 3461–3482, https://doi.org/10.5194/gmd-9-3461-2016, 2016.
Pacifico, F., Folberth, G. A., Jones, C. D., Harrison, S. P., and Collins, W. J.:
Sensitivity of biogenic isoprene emissions to past, present, and future environmental conditions and implications for atmospheric chemistry, J. Geophys. Res.-Atmos., 117, D22302, https://doi.org/10.1029/2012JD018276, 2012.
Pöschl, U.:
Atmospheric aerosols: composition, transformation, climate and health effects, Angew. Chem. Int. Edit., 44, 7520–7540, https://doi.org/10.1002/anie.200501122, 2005.
Pye, H. O. T., Chan, A. W. H., Barkley, M. P., and Seinfeld, J. H.:
Global modeling of organic aerosol: the importance of reactive nitrogen (NOx and NO3), Atmos. Chem. Phys., 10, 11261–11276, https://doi.org/10.5194/acp-10-11261-2010, 2010.
Rao, S., Klimont, Z., Smith, S. J., Van Dingenen, R., Dentener, F., Bouwman, L., Riahi, K., Amann, M., Bodirsky, B. L., van Vuuren, D. P., Aleluia Reis, L., Calvin, K., Drouet, L., Fricko, O., Fujimori, S., Gernaat, D., Havlik, P., Harmsen, M., Hasegawa, T., and Tavoni, M.:
Future air pollution in the Shared Socio-economic Pathways, Glob. Environ. Chang., 42, 346–358, https://doi.org/10.1016/j.gloenvcha.2016.05.012, 2017.
Riemer, N., Vogel, H., Vogel, B., Schell, B., Ackermann, I., Kessler, C., and Hass, H.:
Impact of the heterogeneous hydrolysis of N2O5 on chemistry and nitrate aerosol formation in the lower troposphere under photosmog conditions, J. Geophys. Res., 108, 4144, https://doi.org/10.1029/2002JD002436, 2003.
Sakulyanontvittaya, T., Duhl, T., Wiedinmyer, C., Helmig, D., Matsunaga, S., Potosnak, M., Milford, J., and Guenther, A.:
Monoterpene and sesquiterpene emission estimates for the United States, Environ. Sci. Technol., 42, 1623–1629, https://doi.org/10.1021/es702274e, 2008.
Schwantes, R. H., Charan, S. M., Bates, K. H., Huang, Y., Nguyen, T. B., Mai, H., Kong, W., Flagan, R. C., and Seinfeld, J. H.: Low-volatility compounds contribute significantly to isoprene secondary organic aerosol (SOA) under high-NOx conditions, Atmos. Chem. Phys., 19, 7255–7278, https://doi.org/10.5194/acp-19-7255-2019, 2019.
Schwantes, R. H., Emmons, L. K., Orlando, J. J., Barth, M. C., Tyndall, G. S., Hall, S. R., Ullmann, K., St. Clair, J. M., Blake, D. R., Wisthaler, A., and Bui, T. P. V.:
Comprehensive isoprene and terpene gas-phase chemistry improves simulated surface ozone in the southeastern US, Atmos. Chem. Phys., 20, 3739–3776, https://doi.org/10.5194/acp-20-3739-2020, 2020.
Scott, C. E., Arnold, S. R., Monks, S. A., Asmi, A., Paasonen, P., and Spracklen, D. V.:
Substantial large-scale feedbacks between natural aerosols and climate, Nat. Geosci., 11, 1–6, https://doi.org/10.1038/s41561-017-0020-5, 2017.
Sellar, A. A., Jones, C. G., Mulcahy, J., Tang, Y., Yool, A., Wiltshire, A., O'Connor, F. M., Stringer, M., Hill, R., Palmieri, J., Woodward, S., Mora, L., Kuhlbrodt, T., Rumbold, S., Kelley, D. I., Ellis, R., Johnson, C. E., Walton, J., Abraham, N. L., and Zerroukat, M.:
UKESM1: Description and evaluation of the UK Earth System Model, J. Adv. Model. Earth Sy., 11, 4513–4558, https://doi.org/10.1029/2019ms001739, 2019.
Stevenson, D. S., Zhao, A., Naik, V., O'Connor, F. M., Tilmes, S., Zeng, G., Murray, L. T., Collins, W. J., Griffiths, P. T., Shim, S., Horowitz, L. W., Sentman, L. T., and Emmons, L.: Trends in global tropospheric hydroxyl radical and methane lifetime since 1850 from AerChemMIP, Atmos. Chem. Phys., 20, 12905–12920, https://doi.org/10.5194/acp-20-12905-2020, 2020.
Stone, D., Evans, M. J., Walker, H., Ingham, T., Vaughan, S., Ouyang, B., Kennedy, O. J., McLeod, M. W., Jones, R. L., Hopkins, J., Punjabi, S., Lidster, R., Hamilton, J. F., Lee, J. D., Lewis, A. C., Carpenter, L. J., Forster, G., Oram, D. E., Reeves, C. E., Bauguitte, S., Morgan, W., Coe, H., Aruffo, E., Dari-Salisburgo, C., Giammaria, F., Di Carlo, P., and Heard, D. E.:
Radical chemistry at night: comparisons between observed and modelled HOx, NO3 and N2O5 during the RONOCO project, Atmos. Chem. Phys., 14, 1299–1321, https://doi.org/10.5194/acp-14-1299-2014, 2014.
Tebaldi, C., Debeire, K., Eyring, V., Fischer, E., Fyfe, J., Friedlingstein, P., Knutti, R., Lowe, J., O'Neill, B., Sanderson, B., van Vuuren, D., Riahi, K., Meinshausen, M., Nicholls, Z., Tokarska, K. B., Hurtt, G., Kriegler, E., Lamarque, J.-F., Meehl, G., Moss, R., Bauer, S. E., Boucher, O., Brovkin, V., Byun, Y.-H., Dix, M., Gualdi, S., Guo, H., John, J. G., Kharin, S., Kim, Y., Koshiro, T., Ma, L., Olivié, D., Panickal, S., Qiao, F., Rong, X., Rosenbloom, N., Schupfner, M., Séférian, R., Sellar, A., Semmler, T., Shi, X., Song, Z., Steger, C., Stouffer, R., Swart, N., Tachiiri, K., Tang, Q., Tatebe, H., Voldoire, A., Volodin, E., Wyser, K., Xin, X., Yang, S., Yu, Y., and Ziehn, T.:
Climate model projections from the Scenario Model Intercomparison Project (ScenarioMIP) of CMIP6, Earth Syst. Dynam., 12, 253–293, https://doi.org/10.5194/esd-12-253-2021, 2021.
Tröstl, J., Chuang, W. K., Gordon, H., Heinritzi, M., Yan, C., Molteni, U., Ahlm, L., Frege, C., Bianchi, F., Wagner, R., Simon, M., Lehtipalo, K., Williamson, C., Craven, J. S., Duplissy, J., Adamov, A., Almeida, J., Bernhammer, A.-K., Breitenlechner, M., and Baltensperger, U.:
The role of low-volatility organic compounds in initial particle growth in the atmosphere, Nature, 533, 527–531, https://doi.org/10.1038/nature18271, 2016.
Wayne, R. P., Barnes, I., Biggs, P., Burrows, J. P., Canosa-Mas, C. E., Hjorth, J., Bras, G. L., Moortgat, G. K., Perner, D., Poulet, G., Restelli, G., and Sidebottom, H.:
The Nitrate Radical: Physics, Chemistry, and the Atmosphere, Atmos. Environ., 25A, 1–203, https://doi.org/10.1016/0960-1686(91)90192-A, 1991.
Walters, D., Baran, A. J., Boutle, I., Brooks, M., Earnshaw, P., Edwards, J., Furtado, K., Hill, P., Lock, A., Manners, J., Morcrette, C., Mulcahy, J., Sanchez, C., Smith, C., Stratton, R., Tennant, W., Tomassini, L., Van Weverberg, K., Vosper, S., Willett, M., Browse, J., Bushell, A., Carslaw, K., Dalvi, M., Essery, R., Gedney, N., Hardiman, S., Johnson, B., Johnson, C., Jones, A., Jones, C., Mann, G., Milton, S., Rumbold, H., Sellar, A., Ujiie, M., Whitall, M., Williams, K., and Zerroukat, M.:
The Met Office Unified Model Global Atmosphere 7.0/7.1 and JULES Global Land 7.0 configurations, Geosci. Model Dev., 12, 1909–1963, https://doi.org/10.5194/gmd-12-1909-2019, 2019.
Weber, J., Archer-Nicholls, S., Abraham, N. L., Shin, Y. M., Bannan, T. J., Percival, C. J., Bacak, A., Artaxo, P., Jenkin, M., Khan, M. A. H., Shallcross, D. E., Schwantes, R. H., Williams, J., and Archibald, A. T.:
Improvements to the representation of BVOC chemistry–climate interactions in UKCA (v11.5) with the CRI-Strat 2 mechanism: incorporation and evaluation, Geosci. Model Dev., 14, 5239–5268, https://doi.org/10.5194/gmd-14-5239-2021, 2021.
Yue, M., Wang, M., Guo, J., Zhang, H., Dong, X., and Liu, Y.:
Long-Term Trend Comparison of Planetary Boundary Layer Height in Observations and CMIP6 Models over China, J. Climate, 34, 8237–8256. 2021.
Zhao, D., Pullinen, I., Fuchs, H., Schrade, S., Wu, R., Acir, I.-H., Tillmann, R., Rohrer, F., Wildt, J., Guo, Y., Kiendler-Scharr, A., Wahner, A., Kang, S., Vereecken, L., and Mentel, T. F.:
Highly oxygenated organic molecule (HOM) formation in the isoprene oxidation by NO3 radical, Atmos. Chem. Phys., 21, 9681–9704, https://doi.org/10.5194/acp-21-9681-2021, 2021.
Short summary
The nitrate radical is a major oxidant at nighttime, but much less is known about it than about the other oxidants ozone and OH. We use Earth system model calculations to show how the nitrate radical has changed in abundance from 1850–2014 and to 2100 under a range of different climate and emission scenarios. Depending on the emissions and climate scenario, significant increases are projected with implications for the oxidation of volatile organic compounds and the formation of fine aerosol.
The nitrate radical is a major oxidant at nighttime, but much less is known about it than about...
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