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Potential source regions and processes of aerosol in the summer Arctic

2015, Heintzenberg, J., Leck, C., Tunved, P.

Sub-micrometer particle size distributions measured during four summer cruises of the Swedish icebreaker Oden 1991, 1996, 2001, and 2008 were combined with dimethyl sulfide gas data, back trajectories, and daily maps of pack ice cover in order to investigate source areas and aerosol formation processes of the boundary layer aerosol in the central Arctic. With a clustering algorithm, potential aerosol source areas were explored. Clustering of particle size distributions together with back trajectories delineated five potential source regions and three different aerosol types that covered most of the Arctic Basin: marine, newly formed and aged particles over the pack ice. Most of the pack ice area with < 15% of open water under the trajectories exhibited the aged aerosol type with only one major mode around 40 nm. For newly formed particles to occur, two conditions had to be fulfilled over the pack ice: the air had spent 10 days while traveling over ever more contiguous ice and had traveled over less than 30% open water during the last 5 days. Additionally, the air had experienced more open water (at least twice as much as in the cases of aged aerosol) during the last 4 days before arrival in heavy ice conditions at Oden. Thus we hypothesize that these two conditions were essential factors for the formation of ultrafine particles over the central Arctic pack ice. In a comparison the Oden data with summer size distribution data from Alert, Nunavut, and Mt. Zeppelin, Spitsbergen, we confirmed the Oden findings with respect to particle sources over the central Arctic. Future more frequent broken-ice or open water patches in summer will spur biological activity in surface water promoting the formation of biological particles. Thereby low clouds and fogs and subsequently the surface energy balance and ice melt may be affected.

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Aerosol particle number size distributions and particulate light absorption at the ZOTTO tall tower (Siberia), 2006–2009

2011, Heintzenberg, J., Birmili, W., Otto, R., Andreae, M.O., Mayer, J.-C., Chi, X., Panov, A.

This paper analyses aerosol particle number size distributions, particulate absorption at 570 nm wavelength and carbon monoxide (CO) measured between September 2006 and January 2010 at heights of 50 and 300 m at the Zotino Tall Tower Facility (ZOTTO) in Siberia (60.8° N; 89.35° E). Average number, surface and volume concentrations are broadly comparable to former studies covering shorter observation periods. Fits of multiple lognormal distributions yielded three maxima in probability distribution of geometric mean diameters in the Aitken and accumulation size range and a possible secondary maximum in the nucleation size range below 25 nm. The seasonal cycle of particulate absorption shows maximum concentrations in high winter (December) and minimum concentrations in mid-summer (July). The 90th percentile, however, indicates a secondary maximum in July/August that is likely related to forest fires. The strongly combustion derived CO shows a single winter maximum and a late summer minimum, albeit with a considerably smaller seasonal swing than the particle data due to its longer atmospheric lifetime. Total volume and even more so total number show a more complex seasonal variation with maxima in winter, spring, and summer. A cluster analysis of back trajectories and vertical profiles of the pseudo-potential temperature yielded ten clusters with three levels of particle number concentration: Low concentrations in Arctic air masses (400–500 cm−3), mid-level concentrations for zonally advected air masses from westerly directions between 55° and 65° N (600–800 cm−3), and high concentrations for air masses advected from the belt of industrial and population centers in Siberia and Kazakhstan (1200 cm−3). The observational data is representative for large parts of the troposphere over Siberia and might be particularly useful for the validation of global aerosol transport models.

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The summer aerosol in the central Arctic 1991-2008: Did it change or not?

2012, Heintzenberg, J., Leck, C.

In the course of global warming dramatic changes are taking place in the Arctic and boreal environments. However, physical aerosol data in from the central summer Arctic taken over the course of 18 yr from 1991 to 2008 do not show systematic year-to-year changes, albeit substantial interannual variations. Besides the limited extent of the data several causes may be responsible for these findings. The processes controlling concentrations and particle size distribution of the aerosol over the central Arctic perennial pack ice area, north of 80°, may not have changed substantially during this time. Environmental changes are still mainly effective in the marginal ice zone, the ice-free waters and continental rims and have not propagated significantly into the central Arctic yet where they could affect the local aerosol and its sources. The analysis of meteorological conditions of the four expedition summers reveal substantial variations which we see as main causes of the measured variations in aerosol parameters. With combined lognormal fits of the hourly number size distributions of the four expeditions representative mode parameters for the summer aerosol in the central Arctic have been calculated. The combined aerosol statistics discussed in the present paper provide comprehensive physical data on the summer aerosol in the central Arctic. These data are the only surface aerosol information from this region.

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Infrequent new particle formation over the remote boreal forest of Siberia

2018, Wiedensohler, A., Ma, N., Birmili, W., Heintzenberg, J., Ditas, F., Andreae, M.O., Panov, A.

Aerosol particle number size distributions (PNSD) were investigated to verify, if extremely low-volatility organic vapors (ELVOC) from natural sources alone could induce new particle formation and growth events over the remote boreal forest region of Siberia, hundreds of kilometers away from significant anthropogenic sources. We re-evaluated observations determined at a height of 300 m of the remote observatory ZOTTO (Zotino Tall Tower Observatory, http://www.zottoproject.org). We found that new particle formation events occurred only on 11 days in a 3-year period, suggesting that homogeneous nucleation with a subsequent condensational growth could not be the major process, maintaining the particle number concentration in the planetary boundary layer of the remote boreal forest area of Siberia. © 2018 Elsevier Ltd

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Long-term measurements of aerosol and carbon monoxide at the ZOTTO tall tower to characterize polluted and pristine air in the Siberian taiga

2013, Chi, X., Winderlich, J., Mayer, J.-C., Panov, A.V., Heimann, M., Birmili, W., Heintzenberg, J., Cheng, Y., Andreae, M.O.

Siberia is one of few continental regions in the Northern Hemisphere where the atmosphere may sometimes approach pristine background conditions. We present the time series of aerosol and carbon monoxide (CO) measurements between September 2006 and December 2011 at the Zotino Tall Tower Observatory (ZOTTO) in Central Siberia (61° N; 89° E). We investigate the seasonal, weekly and diurnal variations of aerosol properties (including absorption and scattering coefficients and derived parameters, such as equivalent black carbon (BCe), Ångström exponent, single scattering albedo, and backscattering ratio) and the CO mixing ratios. Criteria were established to distinguish polluted from near-pristine air masses, providing quantitative characteristics for each type. Depending on the season, 23–36% of the sampling time at ZOTTO was found to be representative of a clean atmosphere. The summer pristine data indicate that primary biogenic and secondary organic aerosol formation are quite strong particle sources in the Siberian taiga. The summer seasons 2007–2008 were dominated by an Aitken mode around 80 nm size, whereas the summer 2009 with prevailing easterly winds produced particles in the accumulation mode around 200 nm size. We found these differences to be mainly related to air temperature, through its effect on the production rates of biogenic volatile organic compounds (VOC) precursor gases. In winter, the particle size distribution peaked at 160 nm, and the footprint of clean background air was characteristic for aged particles from anthropogenic sources at great distances from ZOTTO and diluted biofuel burning emissions from domestic heating. The wintertime polluted air originates mainly from large cities south and southwest of the site; these particles have a dominant mode around 100 nm, and the ΔBCe / ΔCO ratio of 7–11 ng m−3 ppb−1 suggests dominant contributions from coal and biofuel burning for heating. During summer, anthropogenic emissions are the dominant contributor to the pollution particles at ZOTTO, while only 12% of the polluted events are classified as biomass-burning-dominated, but then often associated with extremely high CO concentrations and aerosol absorption coefficients. Two biomass-burning case studies revealed different ΔBCe / ΔCO ratios from different fire types, with the agricultural fires in April~2008 yielding a very high ratio of 21 ng m−3 ppb−1. Overall, we find that anthropogenic sources dominate the aerosol population at ZOTTO most of the time, even during nominally clean episodes in winter, and that near-pristine conditions are encountered only in the growing season and then only episodically.

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Size distribution and chemical composition of marine aerosols: A compilation and review

2016, Heintzenberg, J., Covert, D.C., Van Dingenen, R.

Some 30 years of physical and chemical marine aerosol data are reviewed to derive global-size distribution parameters and inorganic particle composition on a coarse 15°×15° grid. There are large gaps in geographical and seasonal coverage and chemical and physical aerosol characterisation. About 28% of the grid cells contain physical data while there are compositional data in some 60% of the cells. The size distribution data were parametrized in terms of 2 submicrometer log-normal distributions. The sparseness of the data did not allow zonal differentiation of the distributions. By segregating the chemical data according to the major aerosol sources, sea salt, dimethylsulfide, crustal material, combustion processes and other anthropogenic sources, much information on mass concentrations and contribution of natural and anthropogenic sources to the marine aerosol can be gleaned from the data base. There are significant meridional differences in the contributions of the different sources to the marine aerosol. Very clearly, we see though that the global marine surface atmosphere is polluted by anthropogenic sulfur. Only in the case of sulfur components did the coverage allow the presentation of very coarse seasonal distributions which reflect the spring blooms in the appropriate parts of the oceans. As an example of the potential value in comparing the marine aerosol data base to chemical transport models, global seasonal meridional MSA distributions were compared to modelled MSA distributions. The general good agreement in mass concentrations is encouraging while some latitudinal discrepancies warrant further investigations covering other aerosol components such as black carbon and metals.