| 1. |
- Hamacher-Barth, Evelyne, et al.
(författare)
-
Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008
- 2016
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 16:10, s. 6577-6593
-
Tidskriftsartikel (refereegranskat)abstract
- The representation of aerosol properties and processes in climate models is fraught with large uncertainties. Especially at high northern latitudes a strong underprediction of aerosol concentrations and nucleation events is observed and can only be constrained by in situ observations based on the analysis of individual aerosol particles. To further reduce the uncertainties surrounding aerosol properties and their potential role as cloud condensation nuclei this study provides observational data resolved over size on morphological and chemical properties of aerosol particles collected in the summer high Arctic, north of 80A degrees aEuro-N. Aerosol particles were imaged with scanning and transmission electron microscopy and further evaluated with digital image analysis. In total, 3909 aerosol particles were imaged and categorized according to morphological similarities into three gross morphological groups: single particles, gel particles, and halo particles. Single particles were observed between 15 and 800aEuro-nm in diameter and represent the dominating type of particles (82aEuro-%). The majority of particles appeared to be marine gels with a broad Aitken mode peaking at 70aEuro-nm and accompanied by a minor fraction of ammonium (bi)sulfate with a maximum at 170aEuro-nm in number concentration. Gel particles (11aEuro-% of all particles) were observed between 45 and 800aEuro-nm with a maximum at 154aEuro-nm in diameter. Imaging with transmission electron microscopy allowed further morphological discrimination of gel particles in 'aggregate' particles, 'aggregate with film' particles, and 'mucus-like' particles. Halo particles were observed above 75aEuro-nm and appeared to be ammonium (bi)sulfate (59aEuro-% of halo particles), gel matter (19aEuro-%), or decomposed gel matter (22aEuro-%), which were internally mixed with sulfuric acid, methane sulfonic acid, or ammonium (bi)sulfate with a maximum at 161aEuro-nm in diameter. Elemental dispersive X-ray spectroscopy analysis of individual particles revealed a prevalence of the monovalent ions Na+/K+ for single particles and aggregate particles and of the divalent ions Ca2+/Mg2+ for aggregate with film particles and mucus-like particles. According to these results and other model studies, we propose a relationship between the availability of Na+/K+ and Ca2+/Mg2+ and the length of the biopolymer molecules participating in the formation of the three-dimensional gel networks.
|
|
| 2. |
- Heintzenberg, Jost, et al.
(författare)
-
New particle formation in the Svalbard region 2006-2015
- 2017
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 17:10, s. 6153-6175
-
Tidskriftsartikel (refereegranskat)abstract
- Events of new particle formation (NPF) were analyzed in a 10-year data set of hourly particle size distributions recorded on Mt. Zeppelin, Spitsbergen, Svalbard. Three different types of NPF events were identified through objective search algorithms. The first and simplest algorithm utilizes short-term increases in particle concentrations below 25 nm (PCT (percentiles) events). The second one builds on the growth of the sub-50 nm diameter median (DGR (diameter growth) events) and is most closely related to the classical banana type of event. The third and most complex, multiple-size approach to identifying NPF events builds on a hypothesis suggesting the concurrent production of polymer gel particles at several sizes below ca. 60 nm (MEV (multisize growth) events). As a first and general conclusion, we can state that NPF events are a summer phenomenon and not related to Arctic haze, which is a late winter to early spring feature. The occurrence of NPF events appears to be somewhat sensitive to the available data on precipitation. The seasonal distribution of solar flux suggests some photochemical control that may affect marine biological processes generating particle precursors and/or atmospheric photochemical processes that generate condensable vapors from precursor gases. Notably, the seasonal distribution of the biogenic methanesulfonate (MSA) follows that of the solar flux although it peaks before the maxima in NPF occurrence. A host of ancillary data and findings point to varying and rather complex marine biological source processes. The potential source regions for all types of new particle formation appear to be restricted to the marginal-ice and open-water areas between northeastern Greenland and eastern Svalbard.Depending on conditions, yet to be clarified new particle formation may become visible as short bursts of particles around 20 nm (PCT events), longer events involving condensation growth (DGR events), or extended events with elevated concentrations of particles at several sizes below 100 nm (MEV events). The seasonal distribution of NPF events peaks later than that of MSA and DGR, and in particular than that of MEV events, which reach into late summer and early fall with open, warm, and biologically active waters around Svalbard. Consequently, a simple model to describe the seasonal distribution of the total number of NPF events can be based on solar flux and sea surface temperature, representing environmental conditions for marine biological activity and condensation sink, controlling the balance between new particle nucleation and their condensational growth. Based on the sparse knowledge about the seasonal cycle of gel-forming marine microorganisms and their controlling factors, we hypothesize that the seasonal distribution of DGR and, more so, MEV events reflect the seasonal cycle of the gel-forming phytoplankton.
|
|
| 3. |
- Heintzenberg, J., et al.
(författare)
-
Potential source regions and processes of aerosol in the summer Arctic
- 2015
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:11, s. 6487-6502
-
Tidskriftsartikel (refereegranskat)abstract
- 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.
|
|
| 4. |
- Leck, Caroline, et al.
(författare)
-
Importance of aerosol composition and mixing state for cloud droplet activation over the Arctic pack ice in summer
- 2015
-
Ingår i: Atmospheric Chemistry And Physics. - : Copernicus GmbH. - 1680-7316 .- 1680-7324. ; 15:5, s. 2545-2568
-
Tidskriftsartikel (refereegranskat)abstract
- Concentrations of cloud condensation nuclei (CCN) were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87 degrees N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season, median daily CCN concentrations at 0.2% water vapour supersaturation (SS) were typically in the range of 15 to 30 cm(-3), but concentrations varied by 2 to 3 orders of magnitude over the expedition and were occasionally below 1 cm(-3). The CCN concentrations were highest near the ice edge and fell by a factor of 3 in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again, indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. We inferred the properties of the unexplained non-water soluble aerosol fraction that was necessary for reproducing the observed concentrations of CCN. This was made possible by assuming Kohler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol size ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues that the behaviour of the high Arctic aerosol in CCN-counters operating at water vapour SSs > 0.4% (high relative humidities) may not be properly explained by conventional Kohler theory.
|
|
