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Abstract. Temporal variations in the amount of radionuclides released into the atmosphere during the Fukushima Daiichi Nuclear Power Station (FNPS1) accident and their atmospheric and marine dispersion are essential to evaluate the environmental impacts and resultant radiological doses to the public. In this paper, we estimate the detailed atmospheric releases during the accident using a reverse estimation method which calculates the release rates of radionuclides by comparing measurements of air concentration of a radionuclide or its dose rate in the environment with the ones calculated by atmospheric and oceanic transport, dispersion and deposition models. The atmospheric and oceanic models used are WSPEEDI-II (Worldwide version of System for Prediction of Environmental Emergency Dose Information) and SEA-GEARN-FDM (Finite difference oceanic dispersion model), both developed by the authors. A sophisticated deposition scheme, which deals with dry and fog-water depositions, cloud condensation nuclei (CCN) activation, and subsequent wet scavenging due to mixed-phase cloud microphysics (in-cloud scavenging) for radioactive iodine gas (I2 and CH3I) and other particles (CsI, Cs, and Te), was incorporated into WSPEEDI-II to improve the surface deposition calculations. The results revealed that the major releases of radionuclides due to the FNPS1 accident occurred in the following periods during March 2011: the afternoon of 12 March due to the wet venting and hydrogen explosion at Unit 1, midnight of 14 March when the SRV (safety relief valve) was opened three times at Unit 2, the morning and night of 15 March, and the morning of 16 March. According to the simulation results, the highest radioactive contamination areas around FNPS1 were created from 15 to 16 March by complicated interactions among rainfall, plume movements, and the temporal variation of release rates. The simulation by WSPEEDI-II using the new source term reproduced the local and regional patterns of cumulative surface deposition of total 131I and 137Cs and air dose rate obtained by airborne surveys. The new source term was also tested using three atmospheric dispersion models (Modèle Lagrangien de Dispersion de Particules d'ordre zéro: MLDP0, Hybrid Single Particle Lagrangian Integrated Trajectory Model: HYSPLIT, and Met Office's Numerical Atmospheric-dispersion Modelling Environment: NAME) for regional and global calculations, and the calculated results showed good agreement with observed air concentration and surface deposition of 137Cs in eastern Japan.

[1] During the 2010 eruption of Eyjafjallajökull, improvements were made to the modeling procedure at the Met Office, UK, enabling peak ash concentrations within the volcanic cloud to be estimated. In this paper we describe the ash concentration forecasting method, its rationale and how it evolved over time in response to new information and user requirements. The change from solely forecasting regions of ash to also estimating peak ash concentrations required consideration of volcanic ash emission rates, the fraction of ash surviving near-source fall-out, and the relationship between predicted mean and local peak ash concentrations unresolved by the model. To validate the modeling procedure, predicted peak ash concentrations are compared against observations obtained by ground-based and research aircraft instrumentation. This comparison between modeled and observed peak concentrations highlights the many sources of error and the uncertainties involved. Despite the challenges of predicting ash concentrations, the ash forecasting method employed here is found to give useful guidance on likely ash concentrations. Predicted peak ash concentrations lie within about one and a half orders of magnitude of the observed peak concentrations. A significant improvement in the agreement between modeled and observed values is seen if a buffer zone, accounting for positional errors in the predicted ash cloud, is used. Sensitivity of the predicted ash concentrations to the source properties (e.g., the plume height and the vertical distribution of ash at the source) is assessed and in some cases, seemingly minor uncertainties in the source specification have a large effect on predicted ash concentrations.

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.

[1] The Eyjafjallajökull volcano in Iceland erupted explosively on 14 April 2010, emitting a plume of ash into the atmosphere. The ash was transported from Iceland toward Europe where mostly cloud-free skies allowed ground-based lidars at Chilbolton in England and Leipzig in Germany to estimate the mass concentration in the ash cloud as it passed overhead. The UK Met Office's Numerical Atmospheric-dispersion Modeling Environment (NAME) has been used to simulate the evolution of the ash cloud from the Eyjafjallajökull volcano during the initial phase of the ash emissions, 14-16 April 2010. NAME captures the timing and sloped structure of the ash layer observed over Leipzig, close to the central axis of the ash cloud. Relatively small errors in the ash cloud position, probably caused by the cumulative effect of errors in the driving meteorology en route, result in a timing error at distances far from the central axis of the ash cloud. Taking the timing error into account, NAME is able to capture the sloped ash layer over the UK. Comparison of the lidar observations and NAME simulations has allowed an estimation of the plume height time series to be made. It is necessary to include in the model input the large variations in plume height in order to accurately predict the ash cloud structure at long range. Quantitative comparison with the mass concentrations at Leipzig and Chilbolton suggest that around 3% of the total emitted mass is transported as far as these sites by small (<100 mm diameter) ash particles. , et al. (2011), Evaluating the structure and magnitude of the ash plume during the initial phase of the 2010 Eyjafjallajökull eruption using lidar observations and NAME simulations,