Preprints
https://doi.org/10.5194/egusphere-2023-619
https://doi.org/10.5194/egusphere-2023-619
25 Apr 2023
 | 25 Apr 2023

How well are aerosol-cloud interactions represented in climate models? Part 1: Understanding the sulphate aerosol production from the 2014–15 Holuhraun eruption

George Jordan, James Haywood, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, and Anton Laakso

Abstract. For over 6-months, the 2014–2015 effusive eruption at Holuhraun, Iceland injected considerable amounts of sulphur dioxide (SO2) into the lower troposphere with a daily rate of up to one-third of the global emission rate causing extensive air pollution across Europe. The large injection of SO2, which oxidises to form sulphate aerosol (SO42−), provides a natural experiment offering an ideal opportunity to scrutinise state-of-the-art general circulation models (GCMs) representation of aerosol-cloud interactions (ACIs). Here we present Part 1 of a two-part model inter-comparison using the Holuhraun eruption as a framework to analyse ACIs. We use SO2 retrievals from the Infrared Atmospheric Sounding Interferometer (IASI) instrument and ground-based measurements of SO2 and SO42− mass concentrations across Europe in conjunction with trajectory analysis using the Hybrid Single Particle Lagrangian Integrated Trajectory (HYSPLIT) model to assess the spatial and chemical evolution of the volcanic plume as simulated by 5 GCMs and a chemical transport model (CTM). IASI retrievals of plume altitude and SO2 column load reveal that the volcanic perturbation is largely contained within the lower troposphere and that the spatial evolution and vertical variability of the plume is reasonably well captured by the models, although the models underestimate the mean plume altitude. HYSPLIT trajectories are used to attribute to Holuhraun emissions 184 instances of elevated sulphurous surface mass concentrations recorded at 22 air monitoring stations across Europe. Comparisons with the simulated concentrations show that the models underestimate the elevated SO2 concentrations observed at stations closer to Holuhraun whilst overestimating those observed further away. Using a biexponential function to describe the decay of observed surface mass concentration ratios of SO2-to-SO42− with plume age, in-plume gas-phase and aqueous-phase oxidation rates are estimated as 0.031 ± 0.002 h−1 and 0.22 ± 0.16 h−1 respectively with a near-vent ratio of 31 ± 4 [μgm−3 of SO2 / ugm−3 of SO42−]. The derived gas-phase oxidation rates from the models are all lower than the observed estimate, whilst the majority of the aqueous-phase oxidation rates agree with the observed rate. This suggests that the simulated plumes capture the observed chemical behaviour in the young plume (when aqueous-phase oxidation is dominant), yet not in the mature plume (when gas-phase oxidation is dominant). Overall, despite their coarse resolution, the 6 models show reasonable skill in capturing the spatial and chemical evolution of the Holuhraun plume which is essential when exploring the eruption impact on ACIs in the second part of this study.

Journal article(s) based on this preprint

13 Feb 2024
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024,https://doi.org/10.5194/acp-24-1939-2024, 2024
Short summary
George Jordan, James Haywood, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, and Anton Laakso

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-619', Andreas Stohl, 14 Aug 2023
  • RC2: 'Comment on egusphere-2023-619', Anonymous Referee #2, 26 Sep 2023

Interactive discussion

Status: closed

Comment types: AC – author | RC – referee | CC – community | EC – editor | CEC – chief editor | : Report abuse
  • RC1: 'Comment on egusphere-2023-619', Andreas Stohl, 14 Aug 2023
  • RC2: 'Comment on egusphere-2023-619', Anonymous Referee #2, 26 Sep 2023

Peer review completion

AR: Author's response | RR: Referee report | ED: Editor decision | EF: Editorial file upload
AR by George Jordan on behalf of the Authors (20 Nov 2023)  Author's response   Author's tracked changes   Manuscript 
ED: Referee Nomination & Report Request started (29 Nov 2023) by Andreas Petzold
RR by Andreas Stohl (07 Dec 2023)
RR by Anonymous Referee #2 (19 Dec 2023)
ED: Publish subject to minor revisions (review by editor) (20 Dec 2023) by Andreas Petzold
AR by George Jordan on behalf of the Authors (22 Dec 2023)  Author's response   Author's tracked changes   Manuscript 
ED: Publish as is (22 Dec 2023) by Andreas Petzold
AR by George Jordan on behalf of the Authors (02 Jan 2024)  Author's response   Manuscript 

Journal article(s) based on this preprint

13 Feb 2024
How well are aerosol–cloud interactions represented in climate models? – Part 1: Understanding the sulfate aerosol production from the 2014–15 Holuhraun eruption
George Jordan, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, Anton Laakso, and James Haywood
Atmos. Chem. Phys., 24, 1939–1960, https://doi.org/10.5194/acp-24-1939-2024,https://doi.org/10.5194/acp-24-1939-2024, 2024
Short summary
George Jordan, James Haywood, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, and Anton Laakso
George Jordan, James Haywood, Florent Malavelle, Ying Chen, Amy Peace, Eliza Duncan, Daniel G. Partridge, Paul Kim, Duncan Watson-Parris, Toshihiko Takemura, David Neubauer, Gunnar Myhre, Ragnhild Skeie, and Anton Laakso

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Short summary
The 2014−15 Holuhraun eruption caused a huge aerosol plume in an otherwise unpolluted region providing an opportunity to study how aerosol alter cloud properties. This two-part study uses observations and models to quantify this relationship’s impact on the Earth’s energy budget. Part 1 suggests the models capture the observed spatial and chemical evolution of the plume, yet no model plume is exact. Understanding these differences is key for Part 2 where changes to cloud properties are explored.