Tracers for evaluating computational models of atmospheric transport and oxidation at regional to global scales

P.G. Simmonds*, P. I. Palmer, M. Rigby, A. McCulloch, S. O’Doherty, A.J. Manning

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)peer-review

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Abstract

Atmospheric tracers are effective tools for characterizing dispersion and for testing computational models of atmospheric transport. Atmospheric trace gas measurements are now used widely to infer geographical surface flux distributions. However, robust flux estimates critically rely on well-validated knowledge of atmospheric chemistry, loss processes and transport, without which we are not fully realizing the potential of atmospheric measurements collected on the ground, or from aircraft and satellites. This challenge has taken on renewed importance in the shadow of the Paris Agreement that will likely take advantage of atmospheric trace gas measurements to help improve national and global greenhouse gas emission budgets. We describe a wide range of existing and new potential atmospheric tracers for improving our understanding of atmospheric dispersion. We consider the investigation of atmospheric transport over two scales: 1) short-to-medium length scale (on the order of 1-1000 km) to improve our understanding of convection and boundary layer transport processes, and 2) hemisphere-to-global length scale (on the order of 1,000-10,000 km), where large-scale mixing, cross hemisphere transport and stratosphere-troposphere exchange are important. Although we note the possibility of using “tracers of opportunity,” our primary focus is on deliberate-release tracers, and we explore the use of cyclic perfluorocarbons, hydrofluorocarbons, hydrochlorofluorocarbons, hydrofluoroethers and novel tracers of deuterium-substituted halocarbons. We examine how we might exploit existing instrumentation already deployed at remote global monitoring sites as well as requirements for new instrumentation. To guide the discussion, we provide example scenarios for how experiments might be set up, covering regional to global spatial scales for the evaluation and improvement of atmospheric transport models. However, we stress that appropriate three-dimensional modelling studies and preliminary experiments would need to be carried out to determine the specific details of any real-world experiment.
Original languageEnglish
Article number118074
JournalAtmospheric Environment
Volume246
Early online date21 Nov 2020
DOIs
Publication statusPublished - 1 Feb 2021

Bibliographical note

Funding Information:
This study was supported by various grants from the Department for Business, Energy & Industrial Strategy , R100415-101 (BEIS, UK formerly the Department of Energy and Climate Change ( DECC )) , the National Aeronautical and Space Administration , NNX16AC98G (NASA, USA.). P. Palmer is supported by the EU H2020 . We specifically acknowledge the cooperation and support of the AGAGE community, and constructive inputs from the TransCom community. We thank Dr Steve Montzka for providing detailed information on NOAA flask sampling programmes. We also thank Dr Richard Derwent for valuable discussions on certain aspects of the paper.

Publisher Copyright:
© 2020 Elsevier Ltd

Keywords

  • Deliberate-release tracers. Atmospheric transport
  • dispersion and oxidation

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