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    Cyclones enhance the transport of sea spray aerosols to the high atmosphere in the Southern Ocean
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    Abstract. Cyclones are expected to increase the vertical transport of sea spray aerosols (SSAs), which may significantly impact the climate by increasing the population of cloud condensation nuclei (CCN) and the cloud droplet number concentration (Nd). In this study, a high-time-resolution (1 h) aerosol monitoring was carried out in the middle and high Southern Hemisphere from 23 February to 4 March 2018. The characteristics of SSAs during three cyclones were observed during the cruise. The results showed that SSA level in the low atmosphere did not increase with the wind speed during cyclone processes, which was different from the anticipated scenario that SSA concentration would increase with wind speed. However, the size of SSA particles during cyclones was larger than that in the no-cyclone periods. It seems that the generation of SSAs was enhanced during cyclones, but SSA concentration near the sea surface increased scarcely. The upward-transport proportion was calculated according to the wind stress and sea salt flux between cyclone and non-cyclone periods. It indicated that more than 23.4 % of the SSAs were transported upwards by cyclone processes during event 1, and 36.2 % and 38.9 % were transported upwards in event 2 and event 3, respectively. The upward transport of SSAs was the main reason why SSA concentration did not increase in the low atmosphere. The transport of SSAs to the high atmosphere during cyclones may additionally increase the CCN burden in the marine boundary layer, which may affect the regional climate. This study highlights the importance of SSA transport to the high atmosphere by cyclones and extends the knowledge of SSA generation and the impact factor during the cyclone period in marine atmosphere.
    Keywords:
    Sea spray
    Abstract. We investigate the potential of polarization lidar to provide vertical profiles of aerosol parameters from which cloud condensation nucleus (CCN) and ice nucleating particle (INP) number concentrations can be estimated. We show that height profiles of number concentrations of aerosol particles with radius > 50 nm (APC50, reservoir of favorable CCN) and with radius > 250 nm (APC250, reservoir of favorable INP), as well as profiles of the aerosol particle surface area concentration (ASC, used in INP parameterization) can be retrieved from lidar-derived aerosol extinction coefficients (AEC) with relative uncertainties of a factor of around 2 (APC50), and of about 25–50 % (APC250, ASC). Of key importance is the potential of polarization lidar to identify mineral dust particles and to distinguish and separate the aerosol properties of basic aerosol types such as mineral dust and continental pollution (haze, smoke). We investigate the relationship between AEC and APC50, APC250, and ASC for the main lidar wavelengths of 355, 532 and 1064 nm and main aerosol types (dust, pollution, marine). Our study is based on multiyear Aerosol Robotic Network (AERONET) photometer observations of aerosol optical thickness and column-integrated particle size distribution at Leipzig, Germany, and Limassol, Cyprus, which cover all realistic aerosol mixtures of continental pollution, mineral dust, and marine aerosol. We further include AERONET data from field campaigns in Morocco, Cabo Verde, and Barbados, which provide pure dust and pure marine aerosol scenarios. By means of a simple relationship between APC50 and the CCN-reservoir particles (APCCCN) and published INP parameterization schemes (with APC250 and ASC as input) we finally compute APCCCN and INP concentration profiles. We apply the full methodology to a lidar observation of a heavy dust outbreak crossing Cyprus with dust up to 8 km height and to a case during which anthropogenic pollution dominated.
    AERONET
    Cloud condensation nuclei
    Sea spray
    Effective radius
    Mineral dust
    Haze
    Citations (13)
    Abstract Five years of nearly continuous measurements of aerosol hygroscopicity by a Humidified Tandem Differential Mobility Analyzer (HTDMA) at Mace Head research station are presented, making it the longest aerosol hygroscopicity data set in marine environment and Northeast Atlantic region in particular. The main goal of this work was to examine seasonal patterns of aerosol hygroscopicity and mixing state in a variety of air masses. The entire data set was categorized into clean marine and polluted continental sectors to reveal contrasting physicochemical features. Distinct seasonal patterns were revealed where hygroscopicity of the clean sector aerosol was significantly higher than that of the polluted sector aerosol. The median growth factors (GF) of clean and polluted sectors were 1.67 and 1.31, respectively. Clean sector aerosol median GF reached the lowest values in summer and the highest in winter pointing at an impact of marine biological activity and wind speed driven sea spray production to aerosol hygroscopicity. Conversely, polluted sector aerosol reached the highest median GF of all sizes in summer due to the decrease of anthropogenic emission, enhanced photochemical aging, and secondary inorganic aerosol formation. Wintertime aerosols in both sectors were largely externally mixed, while summertime aerosols were relatively internally mixed. A distinct subset of near‐hydrophobic Aitken mode particles smaller than 50 nm in diameter was observed in the wintertime clean sector which most likely originated in the clean marine atmosphere based on the evolution of air mass back trajectory clustering.
    Sea spray
    Seasonality
    Citations (5)
    Significance Sea spray aerosol, produced through breaking waves, is one of the largest sources of environmental particles. Once in the atmosphere, sea spray aerosol influences cloud formation, serves as microenvironments for multiphase atmospheric chemical reactions, and impacts human health. All of these impacts are affected by aerosol acidity. Here we show that freshly emitted sea spray aerosol particles become highly acidic within minutes as they are transferred across the ocean−air interface. These results have important implications for atmospheric chemistry and climate, including aerosol/gas partitioning, heterogeneous reactions, and chemical speciation at the surface and within sea spray aerosol.
    Sea spray
    Interface (matter)
    Citations (167)
    The aerosol in the coastal environment consists of a complicated mixture of anthropogenic and rural aerosol generated over land, and sea spray aerosol. Also, particles are generate dover sea by physical and chemical processes and the chemical composition may change due to condensation/evaporation of gaseous materials. The actual composition is a function of air mass history and fetch. At the land-sea transition the continental sources cease to exist, and thus the concentrations of land-based particles and gases will gradually decrease. At the same time, sea spray is generated due to the interaction between wind and waves in a developing wave field. A very intense source for sea spray aerosol is the surf zone. Consequently, the aerosol transported over sea in off-shore winds will abruptly charge at the land-sea transition and then gradually loose its continental character, while also the contribution of the surf-generated aerosol will decrease. The latter will be compensated, at least in part, by the production of sea spray aerosol. A Coastal Aerosol Transport model is being developed describing the evolution of the aerosol size distribution in an air column advected from the coast line over sea in off-shore winds. Both removal and production are taken into account. The result are applied to estimate the effect of the changing size distribution on the extinction coefficients. In this contribution, preliminary results are presented from a study of the effects of the surf-generated aerosol and the surface production.
    Sea spray
    Extinction (optical mineralogy)
    Sea breeze
    Fetch
    Sea salt aerosol
    Citations (9)
    Abstract. A range of bubble and sea spray aerosol generators has been tested in the laboratory and compared with ocean measurements. We have shown that the method of generation has a significant influence on the properties of the aerosol particles produced. Hence, the validity of a generation system to mimic atmospheric aerosol is dependent on its capacity of generating bubbles and particulate in a realistic manner. A bubble-bursting aerosol generator consisting in the production of bubbles by the impingement of water jets on seawater was shown to best reproduce the real oceanic bubble and aerosol distributions signatures. Two aeration methods and a plunging-water jet system were tested as bubble-bursting aerosol generators for comparison with a standard nebulizer. The methods for aerosol production were evaluated by analysing the bubble spectrum generated by the bubble-bursting systems and the submicron size distribution, hygroscopicity and cloud condensation nucleus activity of the aerosols generated by the different techniques. Significant differences in the bubble spectrum and aerosol properties were observed when using different aerosol generators. The hygroscopicity and cloud condensation nucleus activity of aerosols generated by the different methods were similar when a sample of purely inorganic salts was used as a parent seawater solution; however, significant differences in the aerosol properties were found when biogenic organics were incorporated in the seawater samples. The presence of organics in the aerosol caused suppression of the growth factor at humidities above 75% RH and an increase in the critical supersaturation when compared with the case without organics. Unequal extent of these effects was observed for aerosols generated by the different methods of particle production. While the highest reductions of the growth factor were observed for the plunging-water jet aerosol, the largest effect on the critical supersaturation was obtained for the atomization-generated particles. The results of this work show that the aerosol generation mechanism affects the particles organic enrichment, thus the behaviour of the produced aerosols strongly depends on the laboratory aerosol generator employed.
    Supersaturation
    Cloud condensation nuclei
    Sea spray
    Bursting
    Citations (7)
    Sea spray aerosol particle is a dominating part of the global aerosol mass load of natural origin. Thus, it strongly influences the atmospheric radiation balance and cloud properties especially over the oceans. Uncertainties of the estimated climate impacts by this aerosol type are partly caused by the uncertainties in the particle size dependent emission fluxes of sea spray aerosol particle. We present simulations with a regional aerosol transport model system in two domains, for three months and compared the model results to measurements at four stations using various sea spray aerosol particle source source functions. Despite these limitations we found the results using different source functions are within the range of most model uncertainties. Especially the model's ability to produce realistic wind speeds is crucial. Furthermore, the model results are more affected by a function correcting the emission flux for the effect of the sea surface temperature than by the use of different source functions.
    Sea spray
    Particle (ecology)
    Abstract. Aerosol samples were collected by aircraft during the summer of 2004 in the Northeastern Pacific and compared to measurements of aerosol hygroscopicity. Chemical speciation analyses of the samples revealed that a significant portion of the marine aerosols was organic, and on average 8% of the total aerosol mass was insoluble organic material, tentatively attributed to natural marine emissions. Two chemical models were explored in an attempt to achieve closure between the marine aerosol chemical and physical properties through reproduction of the observed aerosol growth, both in the subsaturated and supersaturated regimes. Results suggest that at subsaturated relative humidities, the nonideal behavior of water activity with respect to aerosol chemistry has an important effect on aerosol growth. At supersaturations, the underprediction of critical supersaturations by all models suggests the hypothesis that formation of a complete monolayer by the insoluble organics may inhibit the activation of aerosols to form cloud droplets.
    Supersaturation
    Sea spray
    Sea salt aerosol
    Baltic sea
    Citations (34)
    One of the most important natural aerosol systems at the global level is marine aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic marine aerosol, achieved during the EU project MAP (Marine Aerosol Production), comparing them with those reported in the recent literature. Marine aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition trend that is influenced by the oceanic biological activity cycle, in agreement with other observations. Laboratory experiments show that sea‐spray aerosol from biologically active sea water can be highly enriched in organics, and the authors highlight the need for further studies on the atmospheric fate of such primary organics. With regard to the secondary fraction of organic aerosol, the average chemical composition and molecular tracer (methanesulfonic‐acid, amines) distribution could be successfully characterized by adopting a multitechnique analytical approach.
    Primary (astronomy)
    Sea spray
    Methanesulfonic acid
    Citations (191)