Aerosols play a key role in the radiation balance of the atmosphere. Here, we present evidence that the European boreal region is a substantial source of both aerosol mass and aerosol number. The investigation supplies a straightforward relation between emissions of monoterpenes and gas-to-particle formation over regions substantially lacking in anthropogenic aerosol sources. Our results show that the forest provides an aerosol population of 1000 to 2000 particles of climatically active sizes per cubic centimeter during the late spring to early fall period. This has important implications for radiation budget estimates and relevancy for the evaluation of feedback loops believed to determine our future climate.

In this study we present a qualitative and quantitative assessment of more than 10 yr of aerosol number size distribution data observed in the Arctic environment (Mt. Zeppelin (78°56' N, 11°53' E, 474 m a.s.l.), Ny Ålesund, Svalbard). We provide statistics on both seasonal and diurnal characteristics of the aerosol observations and conclude that the Arctic aerosol number size distribution and related parameters such as integral mass and surface area exhibit a very pronounced seasonal variation. This seasonal variation seems to be controlled by both dominating source as well as meteorological conditions. Three distinctly different periods can be identified during the Arctic year: the haze period characterized by a dominating accumulation mode aerosol (March–May), followed by the sunlit summer period with low abundance of accumulation mode particles but high concentration of small particles which are likely to be recently and locally formed (June–August). The rest of the year is characterized by a comparably low concentration of accumulation mode particles and negligible abundance of ultrafine particles (September–February). A minimum in aerosol mass and number concentration is usually observed during September/October.

We further show that the transition between the different regimes is fast, suggesting rapid change in the conditions defining their appearance. A source climatology based on trajectory analysis is provided, and it is shown that there is a strong seasonality of dominating source areas, with Eurasia dominating during the Autumn–Winter period and dominance of North Atlantic air during the summer months. We also show that new-particle formation events are rather common phenomena in the Arctic during summer, and this is the result of photochemical production of nucleating/condensing species in combination with low condensation sink. It is also suggested that wet removal may play a key role in defining the Arctic aerosol year, via the removal of accumulation mode size particles, which in turn have a pivotal role in facilitating the conditions favorable for new-particle formation events. In summary the aerosol Arctic year seems to be at least qualitatively predictable based on the knowledge of seasonality of transport paths and associated source areas, meteorological conditions and removal processes

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.

Abstract. As a part of the IPY project POLARCAT (Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate Chemistry, Aerosols and Transport), this paper studies the sources of equivalent black carbon (EBC), sulphate, light-scattering aerosols and ozone measured at the Arctic stations Zeppelin, Alert, Barrow and Summit during the years 2000-2007. These species are important pollutants and climate forcing agents, and sulphate and EBC are main components of Arctic haze. To determine where these substances originate, the measurement data were combined with calculations using FLEXPART, a Lagrangian particle dispersion model. The climatology of atmospheric transport from surrounding regions on a twenty-day time scale modelled by FLEXPART shows that the stations Zeppelin, Alert and Barrow are highly sensitive to surface emissions in the Arctic and to emissions in high-latitude Eurasia in winter. Emission sensitivities over southern Asia and southern North America are small throughout the year. The high-altitude station Summit is an order of magnitude less sensitive to surface emissions in the Arctic whereas emissions in the southern parts of the Northern Hemisphere continents are more influential relative to the other stations. Our results show that for EBC and sulphate measured at Zeppelin, Alert and Barrow, northern Eurasia is the dominant Correspondence to: D. Hirdman (dhi@nilu.no) source region. For sulphate, Eastern Europe and the metal smelting industry in Norilsk are particularly important. For EBC, boreal forest fires also contribute in summer. No evidence for any substantial contribution to EBC from sources in southern Asia is found. European air masses are associated with low ozone concentrations in winter due to titration by nitric oxides, but are associated with high ozone concentrations in summer due to photochemical ozone formation. There is also a strong influence of ozone depletion events in the Arctic boundary layer on measured ozone concentrations in spring and summer. These results will be useful for developing emission reduction strategies for the Arctic.

We present an estimate of net ecosystem exchange (NEE) of CO₂ in Europe for the years 2001 through 2007. It is derived with a data assimilation that uses a large set of atmospheric CO₂ mole fraction observations (<70 000) to guide relatively simple descriptions of terrestrial and oceanic net exchange, while fossil fuel and fire emissions are prescribed. Weekly terrestrial sources and sinks are optimized (i.e., a flux inversion) for a set of 18 large ecosystems across Europe in which prescribed climate, weather, and surface characteristics introduce finer scale gradients. We find that the terrestrial biosphere in Europe absorbed a net average of 2212165 TgC yr22121 over the period considered. This uptake is predominantly in non-EU countries, and is found in the northern coniferous (221294 TgC/yr) and mixed forests (221230 TgC yr22121) as well as the forest/field complexes of eastern Europe (221285 TgC yr22121). An optimistic uncertainty estimate derived using three biosphere models suggests the uptake to be in a range of 2212122 to 2212258 TgC yr22121, while a more conservative estimate derived from the a-posteriori covariance estimates is 2212165±437 TgC yr22121. Note however that uncertainties are hard to estimate given the nature of the system and are likely to be significantly larger than this. Interannual variability in NEE includes a reduction in uptake due to the 2003 drought followed by three years of more than average uptake. The largest anomaly of NEE occurred in 2005 concurrent with increased seasonal cycles of observed CO₂. We speculate these changes to result from the strong negative phase of the North Atlantic Oscillation in 2005 that lead to favorable summer growth conditions, and altered horizontal and vertical mixing in the atmosphere. All our results are available through http://www.carbontracker.e

In situ observations of the microphysical properties of upper-tropospheric contrails and cirrus clouds have been performed during more than 15 airborne missions over central Europe. Experimental and technical aspects concerning in situ characterization of ice clouds with the help of optical and nonoptical detection methods (preferably FSSP-300 and Hallet-type replicator) are addressed. The development of contrails into cirrus clouds on the timescale of 1 h is discussed in terms of a representative set of number densities, and size distributions and surface area distributions of aerosols and cloud elements, with special emphasis on small ice crystals (diameter Ͻ20 m). Contrails are dominated by high concentrations (Ͼ100 cm Ϫ3) of nearly spherical ice crystals with mean diameters in the range 1-10 m. Young cirrus clouds, which mostly contain small regularly shaped ice crystals in the range 10-20-m diameter and typical concentrations 2-5 cm Ϫ3 , have been observed. Measurement results are compared to simple parcel model calculations to identify parameters relevant for the contrail-cirrus transition. Observations and model estimates suggest that contrail growth is only weakly, if at all, affected by preexisting cirrus clouds.

Abstract. Sea-spray aerosols (SSA) are an important part of the climate system because of their effects on the global radiative budget -both directly as scatterers and absorbers of solar and terrestrial radiation, and indirectly as cloud condensation nuclei (CCN) influencing cloud formation, lifetime, and precipitation. In terms of their global mass, SSA have the largest uncertainty of all aerosols. In this study we review 21 SSA source functions from the literature, several of which are used in current climate models. In addition, we propose a new function. Even excluding outliers, the global annual SSA mass produced spans roughly 3-70 Pg yr −1 for the different source functions, for particles with dry diameter D p < 10 µm, with relatively little interannual variability for a given function. The FLEXPART Lagrangian particle dispersion model was run in backward mode for a large global set of observed SSA concentrations, comprised of several station networks and ship cruise measurement campaigns. FLEX-PART backward calculations produce gridded emission sensitivity fields, which can subsequently be multiplied with gridded SSA production fluxes in order to obtain modeled SSA concentrations. This allowed us to efficiently and simultaneously evaluate all 21 source functions against the measurements. Another advantage of this method is that sourceregion information on wind speed and sea surface temperatures (SSTs) could be stored and used for improving the SSA source function parameterizations. The best source functions reproduced as much as 70 % of the observed SSA concentration variability at several stations, which is comparable with "state of the art" aerosol models. The main driver of SSA production is wind, and we found that the best fit to the observation data could be obtained when the SSA production is proportional to U 3.5 10 , where U 10 is the source region averaged 10 m wind speed. A strong influence of SST on SSA production, with higher temperatures leading to higher production, could be detected as well, although the underlying physical mechanisms of the SST influence remains unclear. Our new source function with wind speed and temperature dependence gives a global SSA production for particles smaller than D p < 10 µm of 9 Pg yr −1 , and is the best fit to the observed concentrations.

[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.