Unique measurements of vertical size-resolved aerosol particle concentrations, trace gas concentrations and meteorological data were obtained during the Arctic Summer Cloud Ocean Study (ASCOS, ...www.ascos.se), an International Polar Year project aimed at establishing the processes responsible for formation and evolution of low-level clouds over the high Arctic summer pack ice. The experiment was conducted from on board the Swedish icebreaker Oden, and provided both ship- and helicopter-based measurements. This study focuses on the vertical helicopter profiles and onboard measurements obtained during a three-week period when Oden was anchored to a drifting ice floe, and sheds light on the characteristics of Arctic aerosol particles and their distribution throughout the lower atmosphere. Distinct differences in aerosol particle characteristics within defined atmospheric layers are identified. Within the lowermost couple hundred metres, transport from the marginal ice zone (MIZ), condensational growth and cloud processing develop the aerosol population. During two of the four representative periods defined in this study, such influence is shown. At altitudes above about 1 km, long-range transport occurs frequently. However, only infrequently does large-scale subsidence descend such air masses to become entrained into the mixed layer in the high Arctic, and therefore long-range transport plumes are unlikely to directly influence low-level stratiform cloud formation. Nonetheless, such plumes can influence the radiative balance of the planetary boundary layer (PBL) by influencing formation and evolution of higher clouds, as well as through precipitation transport of particles downwards. New particle formation was occasionally observed, particularly in the near-surface layer. We hypothesize that the origin of these ultrafine particles could be in biological processes, both primary and secondary, within the open leads between the pack ice and/or along the MIZ. In general, local sources, in combination with upstream boundary-layer transport of precursor gases from the MIZ, are considered to constitute the origin of cloud condensation nuclei (CCN) particles and thus be of importance for the formation of interior Arctic low-level clouds during summer, and subsequently, through cloud influences, for the melting and freezing of sea ice.
Measurements of submicron aerosol chemical composition were made over the central Arctic Ocean from 5 August to 8 September 2008 as a part of the Arctic Summer Cloud Ocean Study (ASCOS) using an ...aerosol mass spectrometer (AMS). The median levels of sulphate and organics for the entire study were 0.051 and 0.055 μ g m−3, respectively. Positive matrix factorisation was performed on the entire mass spectral time series and this enabled marine biogenic and continental sources of particles to be separated. These factors accounted for 33% and 36% of the sampled ambient aerosol mass, respectively, and they were both predominantly composed of sulphate, with 47% of the sulphate apportioned to marine biogenic sources and 48% to continental sources, by mass. Within the marine biogenic factor, the ratio of methane sulphonate to sulphate was 0.25 ± 0.02, consistent with values reported in the literature. The organic component of the continental factor was more oxidised than that of the marine biogenic factor, suggesting that it had a longer photochemical lifetime than the organics in the marine biogenic factor. The remaining ambient aerosol mass was apportioned to an organic-rich factor that could have arisen from a combination of marine and continental sources. In particular, given that the factor does not correlate with common tracers of continental influence, we cannot rule out that the organic factor arises from a primary marine source.
Abstract
The largest uncertainty in the historical radiative forcing of climate is caused by changes in aerosol particles due to anthropogenic activity. Sophisticated aerosol microphysics processes ...have been included in many climate models in an effort to reduce the uncertainty. However, the models are very challenging to evaluate and constrain because they require extensive in situ measurements of the particle size distribution, number concentration, and chemical composition that are not available from global satellite observations. The Global Aerosol Synthesis and Science Project (GASSP) aims to improve the robustness of global aerosol models by combining new methodologies for quantifying model uncertainty, to create an extensive global dataset of aerosol in situ microphysical and chemical measurements, and to develop new ways to assess the uncertainty associated with comparing sparse point measurements with low-resolution models. GASSP has assembled over 45,000 hours of measurements from ships and aircraft as well as data from over 350 ground stations. The measurements have been harmonized into a standardized format that is easily used by modelers and nonspecialist users. Available measurements are extensive, but they are biased to polluted regions of the Northern Hemisphere, leaving large pristine regions and many continental areas poorly sampled. The aerosol radiative forcing uncertainty can be reduced using a rigorous model–data synthesis approach. Nevertheless, our research highlights significant remaining challenges because of the difficulty of constraining many interwoven model uncertainties simultaneously. Although the physical realism of global aerosol models still needs to be improved, the uncertainty in aerosol radiative forcing will be reduced most effectively by systematically and rigorously constraining the models using extensive syntheses of measurements.
We present direct eddy covariance measurements of aerosol number fluxes, dominated by sub-50 nm particles, at the edge of an ice floe drifting in the central Arctic Ocean. The measurements were made ...during the ice-breaker borne ASCOS (Arctic Summer Cloud Ocean Study) expedition in August 2008 between 2°–10° W longitude and 87°–87.5° N latitude. The median aerosol transfer velocities over different surface types (open water leads, ice ridges, snow and ice surfaces) ranged from 0.27 to 0.68 mm s−1 during deposition-dominated episodes. Emission periods were observed more frequently over the open lead, while the snow behaved primarily as a deposition surface. Directly measured aerosol fluxes were compared with particle deposition parameterizations in order to estimate the emission flux from the observed net aerosol flux. Finally, the contribution of the open lead particle source to atmospheric variations in particle number concentration was evaluated and compared with the observed temporal evolution of particle number. The direct emission of aerosol particles from the open lead can explain only 5–10% of the observed particle number variation in the mixing layer close to the surface.
Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic ...Summer Cloud Ocean Study (ASCOS). The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS) that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of unknown composition and source. In general, the study suffered from low counting statistics due to the overall small number of particles found in this pristine environment, the small sizes of the prevailing aerosol below the detection limit of the ATOFMS, and its low hit rate. To our knowledge, this study reports on the first in situ single-particle mass-spectrometric measurements in the marine boundary layer of the high-Arctic pack ice region.
We present results of measurements of black carbon (BC) from ground-based wet-only rainwater (RW) and cloud-water (CW) sampling at a mountain field station, Sinhagad, situated in south western India ...during the period from June 2008 to October 2010. The amount of BC in the sample was determined by photometry at a wavelength of 528 nm after a procedure including the filtration through a 0.4 μm polycarbonate membrane filter. Water soluble concentrations of major anions in RW and CW were also determined. The average concentration of BC in RW (16 μmol dm−3) is higher by at least a factor 2 than that found in similar studies reported from other parts of the world. On the other hand, the average concentration of BC in CW (47 μmol dm−3) is lower by about a factor of 2 than that found at other sites. The ratio between the average concentrations in CW and RW varies from 2 (K+) to 7 (SO42−). The ratio for BC was about 3. No significant difference was observed for pH. Analysis of air mass back trajectories and of correlations between the various components indicates that long range transport of pollutants and dust from East Africa and Southern part of the Arabian peninsula might contribute to the high concentrations of BC and some of the ionic constituents at Sinhagad during the monsoon season.
•First observations of black carbon in cloud-water from South Asia.•Avg. concentration of BC was 3 times higher in cloud-water than in rain.•Biomass burning is an important source of BC in cloud-water.
We present an aerosol – cloud condensation nuclei (CCN) closure study on summer high Arctic aerosol based on measurements that were carried out in 2008 during the Arctic Summer Cloud Ocean Study ...(ASCOS) on board the Swedish ice breaker Oden. The data presented here were collected during a three-week time period in the pack ice (>85° N) when the icebreaker Oden was moored to an ice floe and drifted passively during the most biological active period into autumn freeze up conditions. CCN number concentrations were obtained using two CCN counters measuring at different supersaturations. The directly measured CCN number concentration was then compared with a CCN number concentration calculated using both bulk aerosol mass composition data from an aerosol mass spectrometer (AMS) and aerosol number size distributions obtained from a differential mobility particle sizer, assuming κ-Köhler theory, surface tension of water and an internally mixed aerosol. The last assumption was supported by measurements made with a hygroscopic tandem differential mobility analyzer (HTDMA) for particles >70 nm. For the two highest measured supersaturations, 0.73 and 0.41%, closure could not be achieved with the investigated settings concerning hygroscopicity and density. The calculated CCN number concentration was always higher than the measured one for those two supersaturations. This might be caused by a relative larger insoluble organic mass fraction of the smaller particles that activate at these supersaturations, which are thus less good CCN than the larger particles. On average, 36% of the mass measured with the AMS was organic mass. At 0.20, 0.15 and 0.10% supersaturation, closure could be achieved with different combinations of hygroscopic parameters and densities within the uncertainty range of the fit. The best agreement of the calculated CCN number concentration with the observed one was achieved when the organic fraction of the aerosol was treated as nearly water insoluble (κorg=0.02), leading to a mean total κ, κtot, of 0.33 ± 0.13. However, several settings led to closure and κorg=0.2 is found to be an upper limit at 0.1% supersaturation. κorg≤0.2 leads to a κtot range of 0.33 ± 013 to 0.50 ± 0.11. Thus, the organic material ranges from being sparingly soluble to effectively insoluble. These results suggest that an increase in organic mass fraction in particles of a certain size would lead to a suppression of the Arctic CCN activity.
Observations made during late summer in the central Arctic Ocean, as part of the Arctic Summer Cloud Ocean Study (ASCOS), are used to evaluate cloud and vertical temperature structure in the Met ...Office Unified Model (MetUM). The observation period can be split into 5 regimes; the first two regimes had a large number of frontal systems, which were associated with deep cloud. During the remainder of the campaign a layer of low-level cloud occurred, typical of central Arctic summer conditions, along with two periods of greatly reduced cloud cover. The short-range operational NWP forecasts could not accurately reproduce the observed variations in near-surface temperature. A major source of this error was found to be the temperature-dependant surface albedo parameterisation scheme. The model reproduced the low-level cloud layer, though it was too thin, too shallow, and in a boundary-layer that was too frequently well-mixed. The model was also unable to reproduce the observed periods of reduced cloud cover, which were associated with very low cloud condensation nuclei (CCN) concentrations (<1 cm−3). As with most global NWP models, the MetUM does not have a prognostic aerosol/cloud scheme but uses a constant CCN concentration of 100 cm−3 over all marine environments. It is therefore unable to represent the low CCN number concentrations and the rapid variations in concentration frequently observed in the central Arctic during late summer. Experiments with a single-column model configuration of the MetUM show that reducing model CCN number concentrations to observed values reduces the amount of cloud, increases the near-surface stability, and improves the representation of both the surface radiation fluxes and the surface temperature. The model is shown to be sensitive to CCN only when number concentrations are less than 10–20 cm−3.
Arctic clouds are sensitive to atmospheric particles since these are sometimes in such low concentrations that clouds cannot always form under supersaturated water vapor conditions. This is ...especially true in the late summer, when aerosol concentrations are generally very low in the high Arctic. The environment changes rapidly around freeze‐up as the open waters close and snow starts accumulating on ice. We investigated droplet formation during eight significant fog events in the central Arctic Ocean, north of 80°, from August 12 to 19 September 2018 during the Arctic Ocean 2018 expedition onboard the icebreaker Oden. Calculated hygroscopicity parameters (κ) for the entire study were very high (up to κ = 0.85 ± 0.13), notably after freeze‐up, suggesting that atmospheric particles were very cloud condensation nuclei (CCN)‐active. At least one of the events showed that surface clouds were able to form and persist for at least a couple hours at aerosol concentrations less than 10 cm−3, which was previously suggested to be the minimum for cloud formation. Among these events that were considered limited in CCN, effective radii were generally larger than in the high CCN cases. In some of the fog events, droplet residuals particles did not reactivate under supersaturations up to 0.95%, suggesting either in‐droplet reactions decreased hygroscopicity, or an ambient supersaturation above 1%. These results provide insight into droplet formation during the clean late‐summer and fall of the high Arctic with limited influence from continental sources.
Plain Language Summary
The Arctic atmosphere can be very clean in the summer, to the point that clouds cannot form because there are insufficient particles present for the water vapor to condense upon. This has important implications for the radiation budget, which is highly dependent on clouds. As part of the Arctic Ocean 2018 expedition in the central Arctic Ocean near the North Pole, we investigated the ability of particles to turn into droplets throughout the whole cruise (August 12 to 19 September 2018), and during eight significant fog events. Overall, we found that after the sea ice started to freeze, the particles were more capable of turning into cloud droplets. During one fog event, we observed fog droplets forming when the particle concentrations were lower than the limit that past studies had suggested that fog/cloud could be sustained. During several fog events, the dried fog droplets did not always re‐form droplets when exposed to cloud‐like conditions, which suggests that the original droplets must have formed under extreme conditions. Our results show that in the summer/fall in the high Arctic, liquid droplets sometimes form under unusual circumstances that are likely not always considered in models.
Key Points
Aerosol hygroscopicity was greater after surface water freeze‐up than before
Hygroscopicity of Aitken mode particles was generally greater than accumulation mode particles
Cloud droplet effective radii during aerosol‐limited periods were larger generally than periods with higher aerosol concentrations
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