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The effect of physical and chemical aerosol properties on warm cloud droplet activation

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The effects of atmospheric aerosol on climate forcing may be very substantial but are quantified poorly at present; in particular, the effects of aerosols on cloud radiative properties, or the 'indirect effects' are credited with the greatest range of uncertainty amongst the known causes of radiative forcing. This manuscript explores the effects that the composition and properties of atmospheric aerosol can have on the activation of droplets in warm clouds, so potentially influencing the magnitude of the indirect effect. The effects of size, composition, mixing state and various derived properties are assessed and a range of these properties provided by atmospheric measurements in a variety of locations is briefly reviewed. The suitability of a range of process-level descriptions to capture these aerosol effects is investigated by assessment of their sensitivities to uncertainties in aerosol properties and by their performance in closure studies. The treatment of these effects within global models is reviewed and suggestions for future investigations are made.
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... The response of cloud characteristics and precipitation processes to increasing anthropogenic aerosol concentrations represents one of the largest areas of uncertainty in the current understanding of climate change. One of the crucial challenges is to determine the ability of aerosol particles to act as CCN under relevant atmospheric conditions, an issue that has received increasing attention over the past years (McFiggans et al. 2006;IAPSAG 2007;IPCC 2007;Andreae and Rosenfeld 2008; and references therein). ...
... By accounting for curvature and solute effects, Köhler theory describes the hygroscopic growth and CCN activation of soluble aerosol particles as a function of relative humidity or water-vapor supersaturation, respectively (Seinfeld and Pandis 1998;Pruppacher and Klett 2000;McFiggans et al. 2006): For a given dry particle diameter, it enables the critical water-vapor supersaturation to be calculated; that is, the minimum supersaturation required to form an aqueous droplet that can freely grow by further condensation (cloud droplet). ...
... The ability of an aerosol particle to act as a CCN ("CCN activity")-that is, its ability to induce water-vapor condensation and cloud droplet formation under a given set of conditions-depends primarily on (a) water-vapor supersaturation, (b) dry particle size, and (c) hygroscopicity (soluble particles) or wettability (insoluble particles) (Seinfeld and Pandis 1998;Pruppacher and Klett 2000;McFiggans et al. 2006;Andreae and Rosenfeld 2008). ...
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... Ainda, é importante salientar que a ativação das partículas de aerossol como CCN no interior das nuvens envolve uma competição pelo vapor de água disponível e, por tanto, o processo é também influenciado pela dinâmica da nuvem e pelos processos cinéticos que intervêm no crescimento por condensação do aerossol. Assim, a quantidade de vapor de água e a velocidade em ascensão da parcela de atmosfera considerada (também chamada de velocidade de updraft), a concentração de número de partículas de aerossol e as diferenças em tamanho e composição das partículas de aerossol, entre outros, afetam a concentração de número de CCN ativado (Farmer et al., 2015;Mcfiggans et al., 2006). Desta forma, o número de aerossóis ativado como CCN dentro de uma nuvem vai depender da supersaturação máxima alcançada, mas também tem um efeito de retroalimentação sobre a mesma. ...
... Estes são: um regime limitado pelo updraft, no qual a ativação é praticamente independente da concentração de aerossóis; um segundo regime limitado pela quantidade de aerossol, no qual a ativação é aproximadamente proporcional à concentração em número de aerossóis; e, por fim, um regime intermediário, sensível tanto ao updraft quanto ao aerossol (Reutter et al., 2009). Além da velocidade de updraft e o CN, a concentração de CCN também é modificada pelos parâmetros da distribuição de tamanho do aerossol, i.e. o diâmetro geométrico médio e o desvio padrão (Mcfiggans et al., 2006;Ward et al., 2010). ...
... Ainda, é importante salientar que a ativação das partículas de aerossol como CCN no interior das nuvens envolve uma competição pelo vapor de água disponível e, por tanto, o processo é também influenciado pela dinâmica da nuvem e pelos processos cinéticos que intervêm no crescimento por condensação do aerossol. Assim, a quantidade de vapor de água e a velocidade em ascensão da parcela de atmosfera considerada (também chamada de velocidade de updraft), a concentração de número de partículas de aerossol e as diferenças em tamanho e composição das partículas de aerossol, entre outros, afetam a concentração de número de CCN ativado (Farmer et al., 2015;Mcfiggans et al., 2006). Desta forma, o número de aerossóis ativado como CCN dentro de uma nuvem vai depender da supersaturação máxima alcançada, mas também tem um efeito de retroalimentação sobre a mesma. ...
... Estes são: um regime limitado pelo updraft, no qual a ativação é praticamente independente da concentração de aerossóis; um segundo regime limitado pela quantidade de aerossol, no qual a ativação é aproximadamente proporcional à concentração em número de aerossóis; e, por fim, um regime intermediário, sensível tanto ao updraft quanto ao aerossol (Reutter et al., 2009). Além da velocidade de updraft e o CN, a concentração de CCN também é modificada pelos parâmetros da distribuição de tamanho do aerossol, i.e. o diâmetro geométrico médio e o desvio padrão (Mcfiggans et al., 2006;Ward et al., 2010). ...
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... Ainda, é importante salientar que a ativação das partículas de aerossol como CCN no interior das nuvens envolve uma competição pelo vapor de água disponível e, por tanto, o processo é também influenciado pela dinâmica da nuvem e pelos processos cinéticos que intervêm no crescimento por condensação do aerossol. Assim, a quantidade de vapor de água e a velocidade em ascensão da parcela de atmosfera considerada (também chamada de velocidade de updraft), a concentração de número de partículas de aerossol e as diferenças em tamanho e composição das partículas de aerossol, entre outros, afetam a concentração de número de CCN ativado (Farmer et al., 2015;Mcfiggans et al., 2006). Desta forma, o número de aerossóis ativado como CCN dentro de uma nuvem vai depender da supersaturação máxima alcançada, mas também tem um efeito de retroalimentação sobre a mesma. ...
... Estes são: um regime limitado pelo updraft, no qual a ativação é praticamente independente da concentração de aerossóis; um segundo regime limitado pela quantidade de aerossol, no qual a ativação é aproximadamente proporcional à concentração em número de aerossóis; e, por fim, um regime intermediário, sensível tanto ao updraft quanto ao aerossol (Reutter et al., 2009). Além da velocidade de updraft e o CN, a concentração de CCN também é modificada pelos parâmetros da distribuição de tamanho do aerossol, i.e. o diâmetro geométrico médio e o desvio padrão (Mcfiggans et al., 2006;Ward et al., 2010). ...
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... The hygroscopicity of atmospheric aerosols, that is, the ability to absorb water vapor, can impact Earth's radiative balance by directly altering the particle optical properties and indirectly influencing cloud formation (McFiggans et al., 2006;Titos et al., 2016). In addition, hygroscopicity affects the formation and alteration of aerosols through aqueous-phase processes in aerosols. ...
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... High values of accumulated precipitation led to anomalously low concentrations of accumulation mode particles. The threshold size for this effect is dependent on the environment (about 60 nm for ATTO, about 40 nm for HYY depending on season, and about 70 nm for ZEP, see also Figure S2 in Supporting Information S1), and influenced by a combination of processes that impact the aerosol size distribution and cloud formation, including the main particle sources, and atmospheric conditions such as updraft velocities and aerosol concentrations (Abdul-Razzak & Ghan, 2000;McFiggans et al., 2006). These conditions affect the ambient supersaturation, which in turn impacts cloud formation, precipitation intensity and type (Figures 2d-2f and Figure S3 in Supporting Information S1). ...
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... The dust aerosol present in the atmosphere during the harmattan season in the northern hemisphere is a common feature of the climate of most parts of West Africa (Akande et al., 2013). The enormous amount of dust and sand particles raised and transported by the harmattan dust haze strongly decreases visibility and are estimated to reach about 6000 m above sea level (Essienimo et al., 2016a;Essienimo et al., 2016b) The hygroscopic growth and the mixing state of aerosol particles play a significant role for various atmospheric effects like the direct aerosol effect on climate, visibility degradation, and cloud formation (Sloane and Wolff, 1985;Pandis et al., 1995;McFiggans et al., 2006). Through the interaction of atmospheric particles and cloud droplets with incoming shortwave radiation, the particle hygroscopic growth is one of the major parameters influencing the terrestrial radiation budget and climate (IPCC, 2007). ...
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