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  • 1. Abdelkader, M.
    et al.
    Metzger, S.
    Mamouri, R. E.
    Astitha, M.
    Barrie, Leonard
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Levin, Z.
    Lelieveld, J.
    Dust-air pollution dynamics over the eastern Mediterranean2015In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 15, no 16, p. 9173-9189Article in journal (Refereed)
    Abstract [en]

    Interactions of desert dust and air pollution over the eastern Mediterranean (EM) have been studied, focusing on two distinct dust transport events on 22 and 28 September 2011. The atmospheric chemistry-climate model EMAC has been used at about 50 km grid spacing, applying an on-line dust emission scheme and calcium as a proxy for dust reactivity. EMAC includes a detailed tropospheric chemistry mechanism, aerosol microphysics and thermodynamics schemes to describe dust aging. The model is evaluated using ground-based observations for aerosol concentrations and aerosol optical depth (AOD) as well as satellite observations. Simulation results and back trajectory analysis show that the development of synoptic disturbances over the EM can enhance dust transport from the Sahara and Arabian deserts in frontal systems that also carry air pollution to the EM. The frontal systems are associated with precipitation that controls the dust removal. Our results show the importance of chemical aging of dust, which increases particle size, dust deposition and scavenging efficiency during transport, overall reducing the lifetime relative to non-aged dust particles. The relatively long travel periods of Saharan dust result in more sustained aging compared to Arabian dust. Sensitivity simulations indicate 3 times more dust deposition of aged relative to pristine dust, which significantly decreases the dust lifetime and loading.

  • 2.
    Chiacchio, Marc
    et al.
    Stockholm University, Faculty of Science, Department of Meteorology .
    Pausata, Francesco S. R.
    Stockholm University, Faculty of Science, Department of Meteorology .
    Messori, Gabriele
    Stockholm University, Faculty of Science, Department of Meteorology .
    Hannachi, Abdel
    Stockholm University, Faculty of Science, Department of Meteorology .
    Chin, Mian
    Onskog, Thomas
    Ekman, Annica M. L.
    Stockholm University, Faculty of Science, Department of Meteorology .
    Barrie, Leonard
    Stockholm University, Faculty of Science, Department of Meteorology .
    On the links between meteorological variables, aerosols, and tropical cyclone frequency in individual ocean basins2017In: Journal of Geophysical Research - Atmospheres, ISSN 2169-897X, E-ISSN 2169-8996, Vol. 122, no 2, p. 802-822Article in journal (Refereed)
    Abstract [en]

    A generalized linear model based on Poisson regression has been used to assess the impact of environmental variables modulating tropical cyclone frequency in six main cyclone development areas: the East Pacific, West Pacific, North Atlantic, North Indian, South Indian, and South Pacific. The analysis covers the period 1980-2009 and focuses on widely used meteorological parameters including wind shear, sea surface temperature, and relative humidity from different reanalyses as well as aerosol optical depth for different compounds simulated by the Goddard Chemistry Aerosol Radiation and Transport model. Circulation indices are also included. Cyclone frequency is obtained from the International Best Track Archive for Climate Stewardship. A strong link is found between cyclone frequency and the relative sea surface temperature, Atlantic Meridional Mode, and wind shear with significant explained log likelihoods in the North Atlantic of 37%, 27%, and 28%, respectively. A significant impact of black carbon and organic aerosols on cyclone frequency is found over the North Indian Ocean, with explained log likelihoods of 27%. A weaker but still significant impact is found for observed dust aerosols in the North Atlantic with an explained log likelihood of 11%. Changes in lower stratospheric temperatures explain 28% of the log likelihood in the North Atlantic. Lower stratospheric temperatures from a subset of Coupled Model Intercomparison Project Phase 5 models properly simulate the warming and subsequent cooling of the lower stratosphere that follows a volcanic eruption but underestimates the cooling by about 0.5 degrees C.

  • 3.
    Freud, Eyal
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Krejci, Radovan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Tunved, Peter
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Leaitch, Richard
    Nguyen, Quynh T.
    Massling, Andreas
    Skov, Henrik
    Barrie, Leonard
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Pan-Arctic aerosol number size distributions: seasonality and transport patterns2017In: Atmospheric Chemistry And Physics, ISSN 1680-7316, E-ISSN 1680-7324, Vol. 17, no 13, p. 8101-8128Article in journal (Refereed)
    Abstract [en]

    The Arctic environment has an amplified response to global climatic change. It is sensitive to human activities that mostly take place elsewhere. For this study, a multi-year set of observed aerosol number size distributions in the diameter range of 10 to 500 nm from five sites around the Arctic Ocean (Alert, Villum Research Station - Station Nord, Zeppelin, Tiksi and Barrow) was assembled and analysed. A cluster analysis of the aerosol number size distributions revealed four distinct distributions. Together with Lagrangian air parcel back-trajectories, they were used to link the observed aerosol number size distributions with a variety of transport regimes. This analysis yields insight into aerosol dynamics, transport and removal processes, on both an intra- and an inter-monthly scale. For instance, the relative occurrence of aerosol number size distributions that indicate new particle formation (NPF) event is near zero during the dark months, increases gradually to similar to 40% from spring to summer, and then collapses in autumn. Also, the likelihood of Arctic haze aerosols is minimal in summer and peaks in April at all sites. The residence time of accumulation-mode particles in the Arctic troposphere is typically long enough to allow tracking them back to their source regions. Air flow that passes at low altitude over central Siberia and western Russia is associated with relatively high concentrations of accumulation-mode particles (N-acc) at all five sites - often above 150 cm(-3). There are also indications of air descending into the Arctic boundary layer after transport from lower latitudes. The analysis of the back-trajectories together with the meteorological fields along them indicates that the main driver of the Arctic annual cycle of N-acc, on the larger scale, is when atmospheric transport covers the source regions for these particles in the 10-day period preceding the observations in the Arctic. The scavenging of these particles by precipitation is shown to be important on a regional scale and it is most active in summer. Cloud processing is an additional factor that enhances the N-acc annual cycle. There are some consistent differences between the sites that are beyond the year-to-year variability. They are the result of differences in the proximity to the aerosol source regions and to the Arctic Ocean sea-ice edge, as well as in the exposure to free-tropospheric air and in precipitation patterns - to mention a few. Hence, for most purposes, aerosol observations from a single Arctic site cannot represent the entire Arctic region. Therefore, the results presented here are a powerful observational benchmark for evaluation of detailed climate and air chemistry modelling studies of aerosols throughout the vast Arctic region.

  • 4. Fu, Pingqing
    et al.
    Kawamura, Kimitaka
    Chen, Jing
    Qin, Mingyue
    Ren, Lujie
    Sun, Yele
    Wang, Zifa
    Barrie, Leonard A.
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Tachibana, Eri
    Ding, Aijun
    Yamashita, Youhei
    Fluorescent water-soluble organic aerosols in the High Arctic atmosphere2015In: Scientific Reports, ISSN 2045-2322, E-ISSN 2045-2322, Vol. 5, article id 9845Article in journal (Refereed)
    Abstract [en]

    Organic aerosols are ubiquitous in the earth's atmosphere. They have been extensively studied in urban, rural and marine environments. However, little is known about the fluorescence properties of water-soluble organic carbon (WSOC) or their transport to and distribution in the polar regions. Here, we present evidence that fluorescent WSOC is a substantial component of High Arctic aerosols. The ratios of fluorescence intensity of protein-like peak to humic-like peak generally increased from dark winter to early summer, indicating an enhanced contribution of protein-like organics from the ocean to Arctic aerosols after the polar sunrise. Such a seasonal pattern is in agreement with an increase of stable carbon isotope ratios of total carbon (delta C-13(TC)) from -26.8 parts per thousand to -22.5 parts per thousand. Our results suggest that Arctic aerosols are derived from a combination of the long-range transport of terrestrial organics and local sea-to-air emission of marine organics, with an estimated contribution from the latter of 8.7-77% (mean 45%).

  • 5. Seguin, Alison Michelle
    et al.
    Norman, Ann-Lise
    Barrie, Leonard
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Evidence of sea ice source in aerosol sulfate loading and size distribution in the Canadian High Arctic from isotopic analysis2014In: J GEOPHYS RES-ATMOS, ISSN 2169-897X, Vol. 119, no 2, p. 1087-1096Article in journal (Refereed)
    Abstract [en]

    The influence of frost flowers and seawater brine on ion chemistry in snow, snowpack, ice cores, and aerosols is detected when a lower sulfate to sodium ratio than in seawater is present in polar regions. This evidence can be masked when large amounts of non-sea-salt sulfate are present from other sources such as biogenic and anthropogenic sulfate. Frost flower delta S-34 values weremeasured for the first time in frost flower sulfates and did not differ significantly from the sea salt delta S-34 values of + 21 parts per thousand. A method using stable isotopes is introduced to determine the limit of contributions from sea salt and sea ice sources (including frost flowers and brine) on sulfate concentrations in aerosol samples from Alert, Canada. Knowledge of the range of values of delta S-34(nss) and the SO4/Na ratio found in sea ice sources (i.e., frost flowers) is used to quantitatively constrain the contributions from frost flowers and sea salt in the Arctic aerosol mass during the onset of winter in 2007 and 2008, allowing for quantification of non-sea-salt sulfate amounts during times when frost flowers are present. Frost flower and/or brine influence was found predominantly in the coarse-mode aerosols (>0.95 mu m). This method to determine the contributions from sea salt and sea ice sources can be carried over to future studies with snow and ice cores.

  • 6. Singh, Dharmendra Kumar
    et al.
    Kawamura, Kimitaka
    Yanase, Ayako
    Barrie, Leonard A.
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Distributions of Polycyclic Aromatic Hydrocarbons, Aromatic Ketones, Carboxylic Acids, and Trace Metals in Arctic Aerosols: Long-Range Atmospheric Transport, Photochemical Degradation/Production at Polar Sunrise2017In: Environmental Science and Technology, ISSN 0013-936X, E-ISSN 1520-5851, Vol. 51, no 16, p. 8992-9004Article in journal (Refereed)
    Abstract [en]

    The distributions, correlations, and source apportionment of aromatic acids, aromatic ketones, polycyclic aromatic hydrocarbons (PAHs), and trace metals were studied in Canadian high Arctic aerosols. Nineteen PAHs including minor sulfur-containing heterocyclic PAH (dibenzothiophene) and major 6 carcinogenic PAHs were detected with a high proportion of fluoranthene followed by benzo[k]fluoranthene, pyrene, and chrysene. However, in the sunlit period of spring, their concentrations significantly declined likely due to photochemical decomposition. During the polar sunrise from mid-March to mid-April, benzo[a]pyrene to benzo[e]pyrene ratios significantly dropped, and the ratios diminished further from late April to May onward. These results suggest that PAHs transported over the Arctic are subjected to strong photochemical degradation at polar sunrise. Although aromatic ketones decreased in spring, concentrations of some aromatic acids such as benzoic and phthalic acids increased during the course of polar sunrise, suggesting that aromatic hydrocarbons are oxidized to result in aromatic acids. However, PAHs do not act as the major source for low molecular weight (LMW) diacids such as oxalic acid that are largely formed at polar sunrise in the arctic atmosphere because PAHs are 1 to 2 orders of magnitude less abundant than LMW diacids. Correlations of trace metals with organics, their sources, and the possible role of trace transition metals are explained.

  • 7.
    Winiger, Patrik
    et al.
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Barrett, T. E.
    Sheesley, R. J.
    Huang, L.
    Sharma, S.
    Barrie, Leonard A.
    Stockholm University, Faculty of Science, Department of Geological Sciences.
    Yttri, K. E.
    Evangeliou, N.
    Eckhardt, S.
    Stohl, A.
    Klimont, Z.
    Heyes, C.
    Semiletov, I. P.
    Dudarev, O.
    Charkin, A.
    Shakhova, N.
    Holmstrand, Henry
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Andersson, August
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Gustafsson, Örjan
    Stockholm University, Faculty of Science, Department of Environmental Science and Analytical Chemistry.
    Source apportionment of circum-Arctic atmospheric black carbon from isotopes and modeling2019In: Science Advances, E-ISSN 2375-2548, Vol. 5, no 2, article id eaau8052Article in journal (Refereed)
    Abstract [en]

    Black carbon (BC) contributes to Arctic climate warming, yet source attributions are inaccurate due to lacking observational constraints and uncertainties in emission inventories. Year-round, isotope-constrained observations reveal strong seasonal variations in BC sources with a consistent and synchronous pattern at all Arctic sites. These sources were dominated by emissions from fossil fuel combustion in the winter and by biomass burning in the summer. The annual mean source of BC to the circum-Arctic was 39 +/- 10% from biomass burning. Comparison of transport-model predictions with the observations showed good agreement for BC concentrations, with larger discrepancies for (fossil/biomass burning) sources. The accuracy of simulated BC concentration, but not of origin, points to misallocations of emissions in the emission inventories. The consistency in seasonal source contributions of BC throughout the Arctic provides strong justification for targeted emission reductions to limit the impact of BC on climate warming in the Arctic and beyond.

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