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

• Published in: Atmospheric chemistry and physics 2024-02, Vol.24 (3), p.1939-1960
• Main Authors: Jordan, George, Malavelle, Florent, Chen, Ying, Peace, Amy, Duncan, Eliza, Partridge, Daniel G, Kim, Paul, Watson-Parris, Duncan, Takemura, Toshihiko, Neubauer, David, Myhre, Gunnar, Skeie, Ragnhild, Laakso, Anton, Haywood, James
• Format: Article
• Language: English
• Subjects: Aerosol production; Aerosol-cloud interactions; Aerosols; Air pollution; Algorithms; Altitude; Atmospheric models; Atmospheric sounding; Chemical evolution; Chemical transport; Climate models; Clouds; Constants; Earthquakes; Emissions; Eruptions; Evolution; Exponential functions; General circulation models; Infrared analysis; Infrared interferometers; Jupiter; Lower troposphere; Mass; Outdoor air quality; Oxidation; Oxidation rate; Perturbation; Plumes; Rate constants; Remote sensing; Representations; Satellite observation; Satellites; Simulation; Spacecraft recovery; Sulfates; Sulfur; Sulfur dioxide; Sulphur; Sulphur dioxide; Trajectory analysis; Troposphere; Volcanic eruption effects; Volcanic plumes
• ISSN: 1680-7324; 1680-7316; 1680-7324
• DOI: 10.5194/acp-24-1939-2024

For over 6 months, the 2014–2015 effusive eruption at Holuhraun, Iceland, injected considerable amounts of sulfur 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 sulfate 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 a 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 five 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. Compared to the satellite observations, the models capture the spatial evolution and vertical variability of the plume reasonably well, although the models often overestimate the plume altitude. HYSPLIT trajectories are used to attribute to Holuhraun emissions 111 instances of elevated sulfurous surface mass concentrations recorded at European Monitoring and Evaluation Programme (EMEP) stations during September and October 2014. Comparisons with the simulated concentrations show that the modelled ratio of SO2 to SO42- during these pollution episodes is often underestimated and overestimated for the young and mature plume, respectively. Models with finer vertical resolutions near the surface are found to better capture these elevated sulfurous ground-level concentrations. Using an exponential function to describe the decay of observed surface mass concentration ratios of SO2 to SO42- with plume age, the in-plume oxidation rate constant is estimated as 0.032 ± 0.002 h−1 (1.30 ± 0.08 d e-folding time), with a near-vent ratio of 25 ± 5 (µg m−3 of SO2 / µg m−3 of SO42-). The majority of the corresponding derived modelled oxidation rate constants are lower than the observed estimate. This suggests that the representation of the oxidation pathway/s in the simulated pl