Abstract. The April-May, 2010 volcanic eruptions of Eyjafjallajökull, Iceland caused significant economic and social disruption in Europe whilst state of the art measurements and ash dispersion forecasts were heavily criticized by the aviation industry. Here we demonstrate for the first time that large improvements can be made in quantitative predictions of the fate of volcanic ash emissions, by using an inversion scheme that couples a priori source information and the output of a Lagrangian dispersion model with satellite data to estimate the volcanic ash source strength as a function of altitude and time. From the inversion, we obtain a total fine ash emission of the eruption of 8.3±4.2 Tg for particles in the size range of 2.8-28 µm diameter. We evaluate the results of our model results with a posteriori ash emissions using independent ground-based, airborne and space-borne measurements both in case studies and statistically. Subsequently, we estimate the area over Europe affected by volcanic ash above certain concentration thresholds relevant for the aviation industry. We find that during three episodes in April and May, volcanic ash concentrations at some altitude in the atmosphere exceeded the limits for the "Normal" flying zone in up to 14 % (6-16 %), 2 % (1-3 %) and 7 % (4-11 %), respecCorrespondence to: A. Stohl (ast@nilu.no) tively, of the European area. For a limit of 2 mg m −3 only two episodes with fractions of 1.5 % (0.2-2.8 %) and 0.9 % (0.1-1.6 %) occurred, while the current "No-Fly" zone criterion of 4 mg m −3 was rarely exceeded. Our results have important ramifications for determining air space closures and for real-time quantitative estimations of ash concentrations. Furthermore, the general nature of our method yields better constraints on the distribution and fate of volcanic ash in the Earth system.

The Lagrangian particle dispersion model FLEX-PART in its original version in the mid-1990s was designed for calculating the long-range and mesoscale dispersion of hazardous substances from point sources, such as those released after an accident in a nuclear power plant. Over the past decades, the model has evolved into a comprehensive tool for multi-scale atmospheric transport modeling and analysis and has attracted a global user community. Its application fields have been extended to a large range of atmospheric gases and aerosols, e.g., greenhouse gases, short-lived climate forcers like black carbon and volcanic ash, and it has also been used to study the atmospheric branch of the water cycle. Given suitable meteorological input data, it can be used for scales from dozens of meters to global. In particular, inverse modeling based on source-receptor relationships from FLEXPART has become widely used. In this paper, we present FLEXPART version 10.4, which works with meteorological input data from the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecast System (IFS) and data from the United States National Cen-ters of Environmental Prediction (NCEP) Global Forecast System (GFS). Since the last publication of a detailed FLEX-PART description (version 6.2), the model has been improved in different aspects such as performance, physicochemical parameterizations, input/output formats, and available preprocessing and post-processing software. The model code has also been parallelized using the Message Passing Interface (MPI). We demonstrate that the model scales well up to using 256 processors, with a parallel efficiency greater than 75 % for up to 64 processes on multiple nodes in runs with very large numbers of particles. The deviation from 100 % efficiency is almost entirely due to the remaining nonparallelized parts of the code, suggesting large potential for further speedup. A new turbulence scheme for the convective boundary layer has been developed that considers the skewness in the vertical velocity distribution (updrafts and downdrafts) and vertical gradients in air density. FLEXPART is the only model available considering both effects, making it highly accurate for small-scale applications, e.g., to quantify dispersion in the vicinity of a point source. The wet deposi-Published by Copernicus Publications on behalf of the European Geosciences Union. 4956 I. Pisso et al.: FLEXPART version 10.4tion scheme for aerosols has been completely rewritten and a new, more detailed gravitational settling parameterization for aerosols has also been implemented. FLEXPART has had the option of running backward in time from atmospheric concentrations at receptor locations for many years, but this has now been extended to also work for deposition values and may become useful, for instance, for the interpretation of ice core measurements. To our knowledge, to date FLEX-PART is the only model with that capability. Furthermore, the temporal variation and temperature dependence of chemical reactions with ...

An analytical inversion method is used to estimate the vertical profile of sulfur dioxide (SO2) emissions from the major 2008 eruption of Kasatochi Volcano, located on the Aleutian Arc, Alaska. The method uses satellite‐observed total SO2 columns from the Global Ozone Monitoring Experiment‐2 (GOME‐2), Ozone Monitoring Instrument (OMI), and Atmospheric InfraRed Sounder (AIRS) during the first 2 days after the eruption, and an atmospheric transport model, FLEXPART, to calculate the vertical emission profile. The inversion yields an emission profile with two large emission maxima near 7 km above sea level (asl) and around 12 km asl, with smaller emissions up to 20 km. The total mass of SO2 injected into the atmosphere by the eruption is estimated to 1.7 Tg, with ∼1 Tg reaching the stratosphere (above 10 km asl). The estimated vertical emission profile is robust against changes of the assumed eruption time, meteorological input data, and satellite data used. Using the vertical emission profile, a simulation of the transport extending for 1 month after the eruption is performed. The simulated cloud agrees very well with SO2 columns observed by GOME‐2, OMI, and AIRS until 6 days after the eruption, and the altitudes agree with both Cloud‐Aerosol Lidar and Infrared Pathfinder Satellite Observation measurements and ground‐based lidar observations to within 1 km. The method is computationally very fast. It is therefore suitable for implementation within an operational environment, such as the Volcanic Ash Advisory Centers, to predict the threat posed by volcanic emissions for air traffic.

[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.

[1] The requirement to forecast volcanic ash concentrations was amplified as a response to the 2010 Eyjafjallajökull eruption when ash safety limits for aviation were introduced in the European area. The ability to provide accurate quantitative forecasts relies to a large extent on the source term which is the emissions of ash as a function of time and height. This study presents source term estimations of the ash emissions from the Eyjafjallajökull eruption derived with an inversion algorithm which constrains modeled ash emissions with satellite observations of volcanic ash. The algorithm is tested with input from two different dispersion models, run on three different meteorological input data sets. The results are robust to which dispersion model and meteorological data are used. Modeled ash concentrations are compared quantitatively to independent measurements from three different research aircraft and one surface measurement station. These comparisons show that the models perform reasonably well in simulating the ash concentrations, and simulations using the source term obtained from the inversion are in overall better agreement with the observations (rank correlation = 0.55, Figure of Merit in Time (FMT) = 25-46%) than simulations using simplified source terms (rank correlation = 0.21, FMT = 20-35%). The vertical structures of the modeled ash clouds mostly agree with lidar observations, and the modeled ash particle size distributions agree reasonably well with observed size distributions. There are occasionally large differences between simulations but the model mean usually outperforms any individual model. The results emphasize the benefits of using an ensemble-based forecast for improved quantification of uncertainties in future ash crises.

Abstract. A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for MediumRange Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity.Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) 137 Cs released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles.Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 µm diameter and a few hours for 10 µm particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85 % of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000 m (52 % of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here.For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.

Mount Kelut (Indonesia) erupted explosively around 15:50 UT on 13 February 2014 sending ash and gases into the stratosphere. Satellite ash retrievals and dispersion transport modeling are combined within an inversion framework to estimate the volcanic ash source term and to study ash transport. The estimated source term suggests that most of the ash was injected to altitudes of 16–17 km, in agreement with space‐based lidar data. Modeled ash concentrations along the flight track of a commercial aircraft that encountered the ash cloud indicate that it flew under the main ash cloud and encountered maximum ash concentrations of 9 ± 3 mg m−3, mean concentrations of 2 ± 1 mg m−3over a period of 10–11 min of the flight, giving a dosage of 1.2 ± 0.3 g s m−3. Satellite data could not be used directly to observe the ash cloud encountered by the aircraft, whereas inverse modeling revealed its presence.

[1] The dangers to people living near a volcano due to lava and pyroclastic flows, and, on glacier-or snow-covered volcanoes, jökulhlaups, are well known. The level of risk to human health due to high concentrations of ash from direct emission and resuspension from the ground is, however, not as well known. The eruption at Eyjafjallajökull, 14 April to 20 May 2010, produced abundant particulate matter due to its explosive eruption style. Even after the volcanic activity ceased, high particulate matter (PM) concentrations were still measured on several occasions, due to resuspended ash. The 24 hour mean concentration of PM 10 in the small town of Vík, 38 km SE of the volcano, reached 1230 mg m À3 , which is about 25 times the health limit, on 7 May 2010, with 10 min average values over 13,000 mg m À3 . Even after the eruption ceased, values as high as 8000 mg m À3 (10 min), and 900 mg m À3 (24 h), were measured because of resuspension of freshly deposited fine ash. In Reykjavík, 125 km WNW of the volcano, the PM 10 concentration reached over 2000 mg m À3 (10 min) during an ash storm on 4 June 2010, which should have warranted airport closure. Summarizing, our study reveals the importance of ash resuspension compared to direct volcanic ash emissions. This likely has implications for air quality but could also have detrimental effects on the quality of ash dispersion model predictions, which so far generally do not include this secondary source of volcanic ash.