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.

Abstract. In spring 2006, the European Arctic was abnormally warm, setting new historical temperature records. During this warm period, smoke from agricultural fires in Eastern Europe intruded into the European Arctic and caused the most severe air pollution episodes ever recorded there. This paper confirms that biomass burning (BB) was indeed the source of the observed air pollution, studies the transport of the smoke into the Arctic, and presents an overview of the observations taken during the episode. Fire detections from the MODIS instruments aboard the Aqua and Terra satellites were used to estimate the BB emissions. The FLEX-PART particle dispersion model was used to show that the smoke was transported to Spitsbergen and Iceland, which was confirmed by MODIS retrievals of the aerosol optical depth (AOD) and AIRS retrievals of carbon monoxide (CO) total columns. Concentrations of halocarbons, carbon dioxide and CO, as well as levoglucosan and potassium, measured at Zeppelin mountain near NyÅlesund, were used to further corroborate the BB source of the smoke at Spitsbergen. The ozone (O 3 ) and CO concentrations were the highest ever observed at the Zeppelin station, and gaseous elemental mercury was also elevated. A new O 3 record was also set at a station on Iceland. The smoke was strongly absorbingblack carbon concentrations were the highest ever recorded Correspondence to: A. Stohl (ast@nilu.no) at Zeppelin -and strongly perturbed the radiation transmission in the atmosphere: aerosol optical depths were the highest ever measured at NyÅlesund. We furthermore discuss the aerosol chemical composition, obtained from filter samples, as well as the aerosol size distribution during the smoke event. Photographs show that the snow at a glacier on Spitsbergen became discolored during the episode and, thus, the snow albedo was reduced. Samples of this polluted snow contained strongly elevated levels of potassium, sulphate, nitrate and ammonium ions, thus relating the discoloration to the deposition of the smoke aerosols. This paper shows that, to date, BB has been underestimated as a source of aerosol and air pollution for the Arctic, relative to emissions from fossil fuel combustion. Given its significant impact on air quality over large spatial scales and on radiative processes, the practice of agricultural waste burning should be banned in the future.

[1] During summer of 2004, about 2.7 million hectare of boreal forest burned in Alaska, the largest annual area burned on record, and another 3.1 million hectare burned in Canada. This study explores the impact of emissions from these fires on light absorbing aerosol concentration levels, aerosol optical depths (AOD), and albedo at the Arctic stations Barrow (Alaska), Alert (Canada), Summit (Greenland), and Zeppelin/Ny Å lesund on Spitsbergen (Norway). The Lagrangian particle dispersion model FLEXPART was run backward from these sites to identify periods that were influenced by forest fire pollution plumes. It is shown that the fires led to enhanced values of particle light absorption coefficients (s ap ) at all of these sites. Barrow, about 1000 km away from the fires, was affected by several fire pollution plumes, one leading to spectacularly high 3-hour mean s ap values of up to 32 Mm À1 , more than the highest values measured in Arctic Haze. AOD measurements for a wavelength of 500 nm saturated but were estimated at above 4-5 units, unprecedented in the station records. Fire plumes were transported through the atmospheric column over Summit continuously for 2 months, during which all measured AOD values were enhanced, with maxima up to 0.4-0.5 units. Equivalent black carbon concentrations at the surface at Summit were up to 600 ng m À3 during two major episodes, and Alert saw at least one event with enhanced s ap values. FLEXPART results show that Zeppelin was located in a relatively unaffected part of the Arctic. Nevertheless, there was a 4-day period with daily mean s ap > 0.3 Mm À1 , the strongest episode of the summer half year, and enhanced AOD values. Elevated concentrations of the highly source-specific compound levoglucosan positively confirmed that biomass burning was the source of the aerosols at Zeppelin. In summary, this paper shows that boreal forest fires can lead to elevated concentrations of light absorbing aerosols throughout the entire Arctic. Enhanced AOD values suggest a substantial impact of these plumes on radiation transmission in the Arctic atmosphere. During the passage of the largest fire plume, a pronounced drop of the albedo of the snow was observed at Summit. We suggest that this is due to the deposition of light absorbing particles on the snow, with further potentially important consequences for the Arctic radiation budget.

[1] Large sets of filtered actinometer, filtered pyrheliometer and Sun photometer measurements have been carried out over the past 30 years by various groups at different Arctic and Antarctic sites and for different time periods. They were examined to estimate ensemble average, long-term trends of the summer background aerosol optical depth AOD(500 nm) in the polar regions (omitting the data influenced by Arctic haze and volcanic eruptions). The trend for the Arctic was estimated to be between À1.6% and À2.0% per year over 30 years, depending on location. No significant trend was observed for Antarctica. The time patterns of AOD(500 nm) and Å ngström's parameters a and b measured with Sun photometers during the last 20 years at various Arctic and Antarctic sites are also presented. They give a measure of the large variations of these parameters due to El Chichon, Pinatubo, and Cerro Hudson volcanic particles, Arctic haze episodes most frequent in winter and spring, and the transport of Asian dust and boreal smokes to the Arctic region. Evidence is also shown of marked differences between the aerosol optical parameters measured at coastal and high-altitude sites in Antarctica. In situ optical and chemical composition parameters of aerosol particles measured at Arctic and Antarctic sites are also examined to achieve more complete information on the multimodal size distribution shape parameters and their radiative properties. A characterization of aerosol radiative parameters is also defined by plotting the daily mean values of a as a function of AOD(500 nm), separately for the two polar regions, allowing the identification of different clusters related to fifteen aerosol classes, for which the spectral values of complex refractive index and single scattering albedo were evaluated. Citation: Tomasi, C., et al. (2007), Aerosols in polar regions: A historical overview based on optical depth and in situ observations,

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.

The eruption of the Icelandic volcano Eyjafjallajökull in April- May 2010 represents a "natural experiment" to study the impact of volcanic emissions on a continental scale. For the first time, quantitative data about the presence, altitude, and layering of the volcanic cloud, in conjunction with optical information, are available for most parts of Europe derived from the observations by the European Aerosol Research Lidar NETwork (EARLINET). Based on multi-wavelength Raman lidar systems, EARLINET is the only instrument worldwide that is able to provide dense time series of high-quality optical data to be used for aerosol typing and for the retrieval of particle microphysical properties as a function of altitude. In this work we show the four-dimensional (4-D) distribution of the Eyjafjallajökull volcanic cloud in the troposphere over Europe as observed by EARLINET during the entire volcanic event (15 April-26 May 2010). All optical properties directly measured (backscatter, extinction, and particle linear depolarization ratio) are stored in the EARLINET database available at http://www.earlinet.org. A specific relational database providing the volcanic mask over Europe, realized ad hoc for this specific event, has been developed and is available on request at http://www.earlinet.org.During the first days after the eruption, volcanic particles were detected over Central Europe within a wide range of altitudes, from the upper troposphere down to the local planetary boundary layer (PBL). After 19 April 2010, volcanic particles were detected over southern and south-eastern Europe. During the first half of May (5-15 May), material emitted by the Eyjafjallajökull volcano was detected over Spain and Portugal and then over the Mediterranean and the Balkans. The last observations of the event were recorded until 25 May in Central Europe and in the Eastern Mediterranean area.The 4-D distribution of volcanic aerosol layering and optical properties on European scale reported here provides an unprecedented data set for evaluating satellite data and aerosol dispersion models for this kind of volcanic events

Abstract. In this study we have analyzed whether tourist cruise ships have an influence on measured sulfur dioxide (SO2), ozone (O3), Aitken mode particle and equivalent black carbon (EBC) concentrations at Ny Ålesund and Zeppelin Mountain on Svalbard in the Norwegian Arctic during summer. We separated the measurement data set into periods when ships were present and periods when ships were not present in the Kongsfjord area, according to a long-term record of the number of passengers visiting Ny Ålesund. We show that when ships with more than 50 passengers cruise in the Kongsfjord, measured daytime mean concentrations of 60 nm particles and EBC in summer show enhancements of 72 and 45%, respectively, relative to values when ships are not present. Even larger enhancements of 81 and 72% were found for stagnant conditions. In contrast, O3 concentrations were 5% lower on average and 7% lower under stagnant conditions, due to titration of O3 with the emitted nitric oxide (NO). The differences between the two data subsets are largest for the highest measured percentiles, while relatively small differences were found for the median concentrations, indicating that ship plumes are sampled relatively infrequently even when ships are present although they carry high pollutant concentrations. We estimate that the ships increased the total summer mean concentrations of SO2, 60 nm particles and EBC by 15, 18 and 11%, respectively. Our findings have two important implications. Firstly, even at such a remote Arctic observatory as Zeppelin, the measurements can be influenced by tourist ship emissions. Careful data screening is recommended before summertime Zeppelin data is used for data analysis or for comparison with global chemistry transport models. However, Zeppelin remains as one of the most valuable Arctic observatories, as most other Arctic observatories face even larger local pollution problems. Secondly, given landing statistics of tourist ships on Svalbard, it is suspected that large parts of the Svalbard archipelago are affected by cruise ship emissions. Thus, our results may be taken as a warning signal of future pan-Arctic conditions if Arctic shipping becomes more frequent and emission regulations are not strict enough.

[1] Within the framework of the Network for the Detection of Stratospheric Change (NDSC), an intercomparison campaign of ground-based zenith-sky viewing UV-visible spectrometers was held at the Andøya Rocket Range (69°N, 16°E) at Andenes, Norway, from February 12 to March 8, 2003. The chosen site is classified as a complementary NDSC site. Eight groups from seven countries participated in the campaign which focused on the measurements of slant columns of NO 2 , BrO, and OClO. This first campaign publication concentrates on measurements of the NO 2 slant columns. Different analysis criteria were investigated during the campaign. These included the use of fitting parameters as chosen by each group to provide what they considered to be optimized retrievals. Additional sets of parameters, imposed for all the groups, were also used, including the wavelength interval, absorption cross sections, and species fitted. Each instrument's results were compared to the measurements of selected reference instruments, whose choice was based on a technique combining regression analysis and examination of the residuals with solar zenith angle. Considering the data obtained during the whole campaign for solar zenith angles between 75°and 95°, all instruments agreed within 5% in the case of NO 2 with imposed analysis parameters in the 425-450 nm region. Measurements agree less well when retrieving the NO 2 slant columns in the 400-418 nm region or when using parameters optimized by each investigator for their instrument.