Primary marine aerosols are an important component of the climate system, especially in the remote marine environment. With diminishing sea-ice cover, better understanding of the role of sea spray aerosol on climate in the polar regions is required. As for Arctic Ocean water, laboratory experiments with NaCl water confirm that a few degrees change in the water temperature (<i>T</i>_w) gives a large change in the number of primary particles. Smaller particles with a dry diameter between 0.01 μm and 0.25 μm dominate the aerosol number density, but their relative dominance decreases with increasing water temperature from 0 °C where they represent 85–90% of the total aerosol number to 60–70% of the total aerosol number at 10 °C water temperature. This effect is most likely related to a change in physical properties and not to modification of sea water chemistry. A change of salinity between 15 g kg⁻¹ and 35 g kg⁻¹ showed no influence on the relative shape of a particle number size distribution, nor did a change in water temperature between 0 °C and 16 °C. An experiment where succinic acid was added to a NaCl water solution showed, that the number concentration of particles with <i>D</i>_p < 0.312 μm decreased by 43% when the succinic acid concentration in NaCl water at <i>T</i>_w = 0 °C was increased from 0 μmol l⁻¹ to 2446 μmol l⁻¹. Different organic constituents and perhaps inorganic substances resulted in a particle number shift towards larger particle sizes, when comparing a size distribution resulting from pure NaCl water to size distributions resulting from Arctic Ocean water and resulting from NaCl water with a succinic acid concentration of 2446 μmol l⁻¹

Abstract. Primary marine aerosol fluxes were measured using eddy covariance (EC), a condensation particle counter (CPC) and an optical particle counter (OPC) with a heated inlet. The later was used to discriminate between sea salt and total aerosol. Measurements were made from the 25 m tower at the research station Mace Head at the Irish west coast, May to September 2002. The aerosol fluxes were dominated by upward fluxes, sea spray from bubble bursting at the ocean surface. The sea salt aerosol number emissions increased two orders of magnitude with declining diameter from 1 to 0.1 μm where it peaked at values of 105 to 107 particles m−2s−1. The sea salt emissions increased at all sizes in the wind range 4 to 22 ms−1, in consistency with a power function of the wind speed. The sea salt emission data were compared to three recent sub micrometer sea salt source parameterisations. The best agreement was with Mårtensson et al. (2003), which appear to apply from 0.1 to 1.1 μm diameters in temperate water (12°C) as well as tropical water (25°C). The total aerosol emissions were independent of the wind speed below 10 ms−1, but increased with the wind above 10 ms−1. The aerosol volume emissions were larger for the total aerosol than for the sea salt at all wind speeds, while the sea salt number emissions approached the total number emissions at 15 ms−1. It is speculated that this is caused by organic carbon in the surface water that is depleted at high wind speeds. The data are consistent with an internal aerosol mixture of sea salt, organic carbon and water. Using the aerosol model by Ellison et al. (1999) (a mono-layer of organic carbon surrounding a water-sea-salt brine) we show that the total and sea salt aerosol emissions are consistent. This predict that the organic carbon fraction increase with decreasing diameter from a few % at 1 μm over 50% at about 0.5 μm to about 90% at 0.1 μm, in consistency with simultaneous chemical data by Cavalli et al. (2004). The combined models of Mårtensson et al. (2003) and Ellison et al. (1999) reproduce the observed total aerosol emissions and offer an approach to model the organic sea spray fraction.

Aerosol nucleation events occurring in the continental boundary layer over the boreal forest region in Finland, during the BIOFOR experiment, have been examined to elucidate the rôle of micrometeorology in promoting such events. Invariably, during the spring campaign of 1999, nucleation events occurred in Arctic and polar air masses during cold air outbreaks. Under clear‐sky conditions, typical of these synoptic meteorological patterns, the boundary layer evolution was characterized by the rapid growth of a mixed layer, convection and strong entrainment, first from the residual later and later from the free troposphere. It was found that the freshly nucleated particles were detected within two hours from the onset of strong turbulent kinetic energy, independent of how fast the boundary layer evolved. When considering the growth time from cluster size of ≈ 1 nm to detectable sizes of 3 nm, the nucleation and onset of strong turbulence coincided almost exactly. The most likely site for nucleation to take place was the mixed layer or the entrainment zone, while the forest canopy and the free troposphere could be excluded as the nucleation region. There are several possible explanations for the correlation between the onset of turbulence and nucleation: (1) new aerosols or clusters may have been entrained from the residual layer into the mixed layer where they then (in the case of clusters) underwent growth to detectable sizes; (2) two or more precursor gases may have been mixed with each other over the entrainment zone; (3) the adiabatic cooling in the rising convective plumes and the turbulent fluctuation in temperature and vapors by the entrainment flux may have enhanced aerosol formation; (4) a sudden decrease in preexisting aerosol due to dilution of the mixed layer aerosol by entrained air may have reduced the vapor sink enough to initiate nucleation. However, the lack of vertical profile measurements of nucleation mode aerosols, precursor vapors and turbulent fluctuations throughout and above the mixed‐layer results in it remaining an open question as to which one of these processes dominates.

Understanding Arctic climate change requires knowledge of both the external and the local drivers of Arctic climate as well as local feedbacks within the system. An Arctic feedback mechanism relating changes in sea ice extent to an alteration of the emission of sea salt aerosol and the consequent change in radiative balance is examined. A set of idealized climate model simulations were performed to quantify the radiative effects of changes in sea salt aerosol emissions induced by prescribed changes in sea ice extent. The model was forced using sea ice concentrations consistent with present day conditions and projections of sea ice extent for 2100. Sea salt aerosol emissions increase in response to a decrease in sea ice, the model results showing an annual average increase in number emission over the polar cap (70–90° N) of 86×10⁶ m⁻² s⁻¹ (mass emission increase of 23 μg m⁻² s⁻¹). This in turn leads to an increase in the natural aerosol optical depth of approximately 23%. In response to changes in aerosol optical depth, the natural component of the aerosol direct forcing over the Arctic polar cap is estimated to be between −0.2 and −0.4 W m⁻² for the summer months, which results in a negative feedback on the system. The model predicts that the change in first indirect aerosol effect (cloud albedo effect) is approximately a factor of ten greater than the change in direct aerosol forcing although this result is highly uncertain due to the crude representation of Arctic clouds and aerosol-cloud interactions in the model. This study shows that both the natural aerosol direct and first indirect effects are strongly dependent on the surface albedo, highlighting the strong coupling between sea ice, aerosols, Arctic clouds and their radiative effects

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