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Abstract. Volcanic sulfate aerosols in the stratosphere produce significant long-term solar and infrared radiative perturbations in the Earth's atmosphere and at the surface, which cause a response of the climate system. Here we study the fundamental process of the development of this volcanic radiative forcing, focusing on the eruption of Mount Pinatubo in the Philippines on June 15, 1991. We develop a spectral-, space-, and time-dependent set of aerosol parameters for 2 years after the Pinatubo eruption using a combination of SAGE II aerosol extinctions and UARS-retrieved effective radii, supported by SAM II, AVHRR, lidar and balloon observations. Using these data, we calculate the aerosol radiative forcing with the ECHAM4 general circulation model (GCM) for cases with climatological and observed sea surface temperature (SST), as well as with and without climate response. We find that the aerosol radiative forcing is not sensitive to the climate variations caused by SST or the atmospheric response to the aerosols, except in regions with varying dense cloudiness. The solar forcing in the near infrared contributes substantially to the total stratospheric heating. A complete formulation of radiative forcing should include not only changes of net fluxes at the tropopause but also the vertical distribution of atmospheric heating rates and the change of downward thermal and net solar radiative fluxes at the surface. These forcing and aerosol data are available for GCM experiments with any spatial and spectral resolution.

The 2014-2015 Bárðarbunga-Veiðivötn fissure eruption at Holuhraun produced about 1.5 km 3 of lava, making it the largest eruption in Iceland in more than 200 years. Over the course of the eruption, daily volcanic sulfur dioxide (SO 2 ) emissions exceeded daily SO 2 emissions from all anthropogenic sources in Europe in 2010 by at least a factor of 3. We present surface air quality observations from across Northern Europe together with satellite remote sensing data and model simulations of volcanic SO 2 for September 2014. We show that volcanic SO 2 was transported in the lowermost troposphere over long distances and detected by air quality monitoring stations up to 2750 km away from the source. Using retrievals from the Ozone Monitoring Instrument (OMI) and the Infrared Atmospheric Sounding Interferometer (IASI), we calculate an average daily SO 2 mass burden of 99 ± 49 kilotons (kt) of SO 2 from OMI and 61 ± 18 kt of SO 2 from IASI for September 2014. This volcanic burden is at least a factor of 2 greater than the average SO 2 mass burden between 2007 and 2009 due to anthropogenic emissions from the whole of Europe. Combining the observational data with model simulations using the United Kingdom Met Office's Numerical Atmospheric-dispersion Modelling Environment model, we are able to constrain SO 2 emission rates to up to 120 kilotons per day (kt/d) during early September 2014, followed by a decrease to 20-60 kt/d between 6 and 22 September 2014, followed by a renewed increase to 60-120 kt/d until the end of September 2014. Based on these fluxes, we estimate that the eruption emitted a total of 2.0 ± 0.6 Tg of SO 2 during September 2014, in good agreement with ground-based remote sensing and petrological estimates. Although satellite-derived and model-simulated vertical column densities of SO 2 agree well, the model simulations are biased low by up to a factor of 8 when compared to surface observations of volcanic SO 2 on 6-7 September 2014 in Ireland. These biases are mainly due to relatively small horizontal and vertical positional errors in the simulations of the volcanic plume occurring over transport distances of thousands of kilometers. Although the volcanic air pollution episodes were transient and lava-dominated volcanic eruptions are sporadic events, the observations suggest that (i) during an eruption, volcanic SO 2 measurements should be assimilated for near real-time air quality forecasting and (ii) existing air quality monitoring networks should be retained or extended to monitor SO 2 and other volcanic pollutants.