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 degree 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.
Sea spray is one of the largest natural aerosol sources and plays an important role in the Earth's radiative budget. These particles are inherently hygroscopic, that is, they take-up moisture from ...the air, which affects the extent to which they interact with solar radiation. We demonstrate that the hygroscopic growth of inorganic sea salt is 8-15% lower than pure sodium chloride, most likely due to the presence of hydrates. We observe an increase in hygroscopic growth with decreasing particle size (for particle diameters <150 nm) that is independent of the particle generation method. We vary the hygroscopic growth of the inorganic sea salt within a general circulation model and show that a reduced hygroscopicity leads to a reduction in aerosol-radiation interactions, manifested by a latitudinal-dependent reduction of the aerosol optical depth by up to 15%, while cloud-related parameters are unaffected. We propose that a value of κ
=1.1 (at RH=90%) is used to represent the hygroscopicity of inorganic sea salt particles in numerical models.
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.
Observations from the Arctic Summer Cloud Ocean Study (ASCOS), in the central Arctic sea-ice pack in late summer 2008, provide a detailed view of cloud–atmosphere–surface interactions and vertical ...mixing processes over the sea-ice environment. Measurements from a suite of ground-based remote sensors, near-surface meteorological and aerosol instruments, and profiles from radiosondes and a helicopter are combined to characterize a week-long period dominated by low-level, mixed-phase, stratocumulus clouds. Detailed case studies and statistical analyses are used to develop a conceptual model for the cloud and atmosphere structure and their interactions in this environment. Clouds were persistent during the period of study, having qualities that suggest they were sustained through a combination of advective influences and in-cloud processes, with little contribution from the surface. Radiative cooling near cloud top produced buoyancy-driven, turbulent eddies that contributed to cloud formation and created a cloud-driven mixed layer. The depth of this mixed layer was related to the amount of turbulence and condensed cloud water. Coupling of this cloud-driven mixed layer to the surface boundary layer was primarily determined by proximity. For 75% of the period of study, the primary stratocumulus cloud-driven mixed layer was decoupled from the surface and typically at a warmer potential temperature. Since the near-surface temperature was constrained by the ocean–ice mixture, warm temperatures aloft suggest that these air masses had not significantly interacted with the sea-ice surface. Instead, back-trajectory analyses suggest that these warm air masses advected into the central Arctic Basin from lower latitudes. Moisture and aerosol particles likely accompanied these air masses, providing necessary support for cloud formation. On the occasions when cloud–surface coupling did occur, back trajectories indicated that these air masses advected at low levels, while mixing processes kept the mixed layer in equilibrium with the near-surface environment. Rather than contributing buoyancy forcing for the mixed-layer dynamics, the surface instead simply appeared to respond to the mixed-layer processes aloft. Clouds in these cases often contained slightly higher condensed water amounts, potentially due to additional moisture sources from below.
Sea spray aerosol particles are an integral part of the Earth's radiation budget. To date, the inorganic composition of nascent sea spray aerosol particles has widely been assumed to be equivalent to ...the inorganic composition of seawater. Here we challenge this assumption using a laboratory sea spray chamber containing both natural and artificial seawater, as well as with ambient aerosol samples collected over the central Arctic Ocean during summer. We observe significant enrichment of calcium in submicrometer (<1 μm in diameter) sea spray aerosol particles when particles are generated from both seawater sources in the laboratory as well as in the ambient aerosols samples. We also observe a tendency for increasing calcium enrichment with decreasing particle size. Our results suggest that calcium enrichment in sea spray aerosol particles may be environmentally significant with implications for our understanding of sea spray aerosol, its impact on Earth's climate, as well as the chemistry of the marine atmosphere.
Key Points
We observe significant enrichment of calcium in submicrometer sea spray aerosol particles
We observe increasing calcium enrichment with decreasing particle size that is independent of seawater organic carbon content
We observe this behavior in laboratory‐generated aerosols using natural and artificial seawater as well as in ambient aerosol samples
Loss of summertime Arctic sea ice will lead to a large increase in the emission of aerosols and precursor gases from the ocean surface. It has been suggested that these enhanced emissions will exert ...substantial aerosol radiative forcings, dominated by the indirect effect of aerosol on clouds. Here, we investigate the potential for these indirect forcings using a global aerosol microphysics model evaluated against aerosol observations from the Arctic Summer Cloud Ocean Study (ASCOS) campaign to examine the response of Arctic cloud condensation nuclei (CCN) to sea-ice retreat. In response to a complete loss of summer ice, we find that north of 70° N emission fluxes of sea salt, marine primary organic aerosol (OA) and dimethyl sulfide increase by a factor of ~ 10, ~ 4 and ~ 15 respectively. However, the CCN response is weak, with negative changes over the central Arctic Ocean. The weak response is due to the efficient scavenging of aerosol by extensive drizzling stratocumulus clouds. In the scavenging-dominated Arctic environment, the production of condensable vapour from oxidation of dimethyl sulfide grows particles to sizes where they can be scavenged. This loss is not sufficiently compensated by new particle formation, due to the suppression of nucleation by the large condensation sink resulting from sea-salt and primary OA emissions. Thus, our results suggest that increased aerosol emissions will not cause a climate feedback through changes in cloud microphysical and radiative properties.
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.
An Arctic CCN-limited cloud-aerosol regime Mauritsen, T.; Sedlar, J.; Tjernström, M. ...
Atmospheric chemistry and physics,
01/2011, Volume:
11, Issue:
1
Journal Article
Peer reviewed
Open access
On average, airborne aerosol particles cool the Earth's surface directly by absorbing and scattering sunlight and indirectly by influencing cloud reflectivity, life time, thickness or extent. Here we ...show that over the central Arctic Ocean, where there is frequently a lack of aerosol particles upon which clouds may form, a small increase in aerosol loading may enhance cloudiness thereby likely causing a climatologically significant warming at the ice-covered Arctic surface. Under these low concentration conditions cloud droplets grow to drizzle sizes and fall, even in the absence of collisions and coalescence, thereby diminishing cloud water. Evidence from a case study suggests that interactions between aerosol, clouds and precipitation could be responsible for attaining the observed low aerosol concentrations.
Climate models generally simulate a unidirectional, positive liquid water path (LWP) response to increasing aerosol number concentration. However, satellite observations and large‐eddy simulations ...show that the LWP may either increase or decrease with increasing aerosol concentration, influencing the overall magnitude of the aerosol indirect effect (AIE). We use large‐eddy simulation to investigate the LWP response of a marine stratocumulus cloud and its dependence on different parameterizations for obtaining cloud droplet number concentration (CDNC). The simulations confirm that the LWP response is not always positive—regardless of CDNC treatment. However, the AIE simulated with the model version with prescribed CDNC is almost 3 times larger compared to the version with prognostic CDNC. The reason is that the CDNC in the prognostic scheme varies in time due to supersaturation fluctuations, collection, and other microphysical processes. A substantial spread in simulated AIE may thus arise simply due to the CDNC treatment.
Plain Language Summary
Our poor understanding of aerosol‐cloud‐radiation interactions (aerosol indirect effects) results in a major uncertainty in estimates of anthropogenic aerosol forcing. In climate models, the cloud water response to an increased aerosol number concentration may be especially uncertain as models simplify, or do not account for, processes that affect the cloud droplet number concentration and the total amount of cloud water. In this study, we employ large‐eddy simulation to explore how different model descriptions for obtaining the number concentration of cloud droplets influences the cloud water response of a marine stratocumulus cloud and thus the simulated aerosol indirect effect. Our simulations show a qualitatively similar cloud water response regardless of model description: the total amount of cloud water increases first and then decreases with increasing aerosol concentration. However, the simulated aerosol indirect effect is almost 3 times as large when the number concentration of cloud droplets is prescribed compared to when it is dependent on the calculated supersaturation and other microphysical processes such as collisions between cloud droplets. Our findings show that a relatively simple difference in the treatment of the number concentration of cloud droplets in climate models may result in a significant spread in the simulated aerosol indirect effect.
Key Points
We use large‐eddy simulation to investigate the response of a marine stratocumulus cloud to increasing aerosol concentration
The aerosol indirect effect is almost 3 times as large when the cloud droplet concentration is prescribed instead of prognostic
Time variations in supersaturation and collection influence the overall cloud droplet number and aerosol indirect effect
Understanding the rapidly changing climate in the Arctic is limited by a lack of understanding of underlying strong feedback mechanisms that are specific to the Arctic. Progress in this field can ...only be obtained by process-level observations; this is the motivation for intensive ice-breaker-based campaigns such as the Arctic Summer Cloud-Ocean Study (ASCOS), described here. However, detailed field observations also have to be put in the context of the larger-scale meteorology, and short field campaigns have to be analysed within the context of the underlying climate state and temporal anomalies from this. To aid in the analysis of other parameters or processes observed during this campaign, this paper provides an overview of the synoptic-scale meteorology and its climatic anomaly during the ASCOS field deployment. It also provides a statistical analysis of key features during the campaign, such as key meteorological variables, the vertical structure of the lower troposphere and clouds, and energy fluxes at the surface. In order to assess the representativity of the ASCOS results, we also compare these features to similar observations obtained during three earlier summer experiments in the Arctic Ocean: the AOE-96, SHEBA and AOE-2001 expeditions. We find that these expeditions share many key features of the summertime lower troposphere. Taking ASCOS and the previous expeditions together, a common picture emerges with a large amount of low-level cloud in a well-mixed shallow boundary layer, capped by a weak to moderately strong inversion where moisture, and sometimes also cloud top, penetrate into the lower parts of the inversion. Much of the boundary-layer mixing is due to cloud-top cooling and subsequent buoyant overturning of the cloud. The cloud layer may, or may not, be connected with surface processes depending on the depths of the cloud and surface-based boundary layers and on the relative strengths of surface-shear and cloud-generated turbulence. The latter also implies a connection between the cloud layer and the free troposphere through entrainment at cloud top.
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