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4.2 Aerosol Production and Transport in the Marine Atmosphere

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Sea Spray Aerosol (SSA) consists of a suspension in air of particles that originate directly at the sea surface (de Leeuw et al.2011a). The review by de Leeuw et al. 2011a) included material published in the peer-reviewed literature up to early 2010. Atlantic results were confirmed by measurements in the South Atlantic Ocean on Amsterdam Island (Sciare et al.2009).

Charlson et al.1987) and is one of the main oxidation products of dimethyl sulfide (DMS), a plankton waste gas. Grousset and Biscaye 2005) with the exception of the Greenland region, which is dominated by Asian dust (Bory et al. 2003).

Puyeheu (Chile)

Ash plume

Nevertheless, both sesquiterepenes (Bonn and Moortgat2003) and isoprene (Claeys et al. 2004) have been identified as important precursor sources. The detailed characterization of the vast array of OA compounds is beyond the capabilities of most analytical techniques (Kroll et al. 2011). The conversion of dust during atmospheric transport mainly leads to coating by sulfates or nitrates (Formenti et al.2011).

POA/ SOA

Thus, diurnal oxidant cycling includes a significant diurnal variation of OA composition with more oxidized OA in the afternoon (Aiken et al. 2008; Hildebrandt et al. 2010; Adler et al. 2011). Aging processes in the atmosphere, resulting in further oxidation and oligopolymerization of the organic compounds, eventually transform them into highly oxidized macromolecular material such as humic substances (HULIS) (Holmes and Petrucci 2006; Hallquist et al. 2009). For example, inorganic sulfate or nitrate aerosols are usually coated or aggregated with organic particles, forming organic sulfate or organic nitrate aerosols (Surratt et al. 2007; Froyd et al. 2010; Hawkins et al. 2010; Li and Shao 2010 ).

Consequently, some recent studies aim to identify organic species or find a metric that can be used as a tracer of organic aging, such as determination of molecular markers (eg Claeys et al.2010), mass. Despite this extreme chemical complexity, it appears that organic matter produced by pollutants in urban atmospheres, by biogenic emissions, or by terpenes exposed to photochemical reactions in smog chambers, is processed into particulate organic matter with similar oxidation states, hygroscopicity, volatility and the mole. - mass lar (Jimenez et al.2009). In other words, organic aerosols of very different origins are observed to evolve in the atmosphere into particles with similar chemical and physical properties (Jimenez et al.2009; Ng et al.2010).

Sulfate/nitrate coating is the result of various heterogeneous chemical processes, such as the uptake of gaseous SO2 or HNO3 (and/or NOx) onto the particle surface and their subsequent conversion to SO42 and NO3 (Dentener et al. 1996; Kim). and Park 2001; Usher et al. 2002) and collision/coalescence between dust and ammonium sulfate or nitrate aerosol (Mori et al. 1998; Sullivan et al. 2007; Suzuki et al. 2010). Heterogeneous processes responsible for mixing sulfate with dust may depend on the season with the dominance of the coagulation process in summer and SO2 uptake in spring (Suzuki et al. 2010). Recent observations of strong internal mixing of dust with nitrate or sulfate in mesoscale convective clouds during the AMMA campaign (Crumeyrolle et al. 2008;

2010a) suggest cloud processing involving aqueous phase oxidation of NOx/SO2, as previously hypothesized by Levin and Ganor (1996) and Liu et al.

OOA i

OOA ii

OOA j

OOA jj

Direct Radiative Effects (DRE)

Second, the decrease in sea ice extent due to climate change leads to an increase in sea salt production (Bellouin et al.2011). Marine aerosols lack elemental oxides of carbon and iron and therefore absorb poorly in the shortwave spectrum (Irshad et al.2009). The size distribution of marine aerosols, especially sea salt, covers both the sub- and super-micron ranges (Dubovik et al. 2002).

In the longwave spectrum, marine DRE is positive at the top of the atmosphere because the aerosol layer is typically cooler than the surface (Reddy et al. 2005). Satellite products also include information on the aerosol size distribution, through the A˚ ngstro¨m coefficient or fine-mode optical depth (Anderson et al. 2005). Ground-based sun-photometer networks provide single-distribution albedo (Schuster et al. 2005) and size distribution (Dubovik et al. 2002) retrievals.

Coastal and island locations and ship cruises are useful to locally characterize marine aerosols (Smirnov et al. 2011). The vertical profile of the aerosol is available from ground- and space-based lidars (Winker et al.2010). In a comparison of global numerical aerosol modeling (Kinne et al. 2006), the median optical depth of sea salt is 0.030 by 0.55 μm on a global average, 24% of the total optical aerosol depth.

However, evidence for a major role of organic compounds in the atmospheric aerosol cycle is growing (Kirkby et al. 2011).

Effects on Cloud Formation and Indirect Radiative Effects

They find the global mean shortwave DRE of sea salt at the top of the cloud-free atmosphere. Sea salt is the second largest contaminant after sulfate, which itself includes an unspecified marine component. The variation among participating models is large and the fraction of sea salt in the optical depth varies between 18% and reports the optical depth of sea salt and natural sulfate (mainly contributed by the ocean) at 0.55 μm 0.040, which is a third of the global total aerosol optics. depth.

The contribution of sea salt is greater in the simulations with the Hadley Center climate model described by Bellouin et al. At cloud-free longwave, the sea salt DRE is +0.4 Wm 2 , half the total DRE in that spectrum. There is a factor of 5 between model simulations of sea salt dry mass (Kinne et al. 2006), and improvements in the parameterization of sea salt production as a function of wind speed may reduce that range, although changes in wind speed simulated wind will certainly remain.

Sea salt and sulfate from DMS oxidation are the only aerosols produced at the ocean–atmosphere interface in current atmosphere–ocean general circulation models. Despite this, Latham and Smith (1990) postulated that sea salt could be involved in a wind speed-related negative feedback system whereby zonal wind speeds with increasing global temperatures would increase, leading to increased sea salt CCN generation, increased cloud droplet concentrations, and ultimately increased cloud albedo. Their measurements were based on the existence of sea salt CCN down to sizes of ~0.2μm radius.

1993) demonstrated through combined measurement and modeling studies that there was significant competition between sea salt and nss sulfate nuclei and that under certain conditions the addition of a small number of sea salt nuclei under moderately low entrainment velocity conditions led to a reduction in cloud droplet concentrations as this nucleus cloud was preferred over sulfate nuclei is activated, leading to a suppression of the peak supersaturation reached in clouds.

Deposition of Aerosol Particles to the Ocean Surface and Impacts

Therefore, atmospheric deposition may play a decisive role in supplying new iron to the surface ocean (Fung et al. 2000). Not all forms of iron are thought to be equally bioavailable (Jickells and Spokes 2001; Mahowald et al. 2009). Zhu et al. 1997 ), although this can be very sensitive to the mineralogical composition of aerosol ( Journet et al. 2008 ).

Because of the large phosphorus reservoir in the oceans, atmospheric deposition is not thought to be a dominant control on global ocean productivity (Krishnamurthy et al. 2010). While released into the atmosphere as a gas, about half of reactive nitrogen is deposited as aerosols (Adams et al. 1999). Indeed, dust deposition events can temporarily increase the concentration of dissolved inorganic P in the surface waters of the LNLC Mediterranean Sea (Pulido-Villena et al.2010).

The use of such indirect approaches has in many cases led to the misattribution of cause (aerosol deposition) and effect (altered ocean biogeochemistry via aerosol- and iron-mediated phytoplankton blooms) (Boyd et al. 2010). However, other studies, such as SERIES in the NE Subarctic Pacific, did not observe such an increase in DMS until the end of the bloom (Boyd et al. 2007). Heavy dust deposition (delivery of 2 mg L 1 aerosols to the upper mixed layer) can release about 2 nM Fe (Bonnet and Guieu 2004; Mills et al. 2004).

Numbers in each panel: (1) Fe*, the relative magnitude of Fe input to macronutrient input (Parekh et al.2005);. Similarly, bacterial production was found to increase by a factor of 8 during dust addition experiments in the eastern Mediterranean microcosm (Herut et al.2005). Mahowald et al.2009), several ocean modeling studies have explored its potential impact on marine biogeochemistry.

Summary and Outlook

De Leeuw et al. 2011a) concluded that the uncertainties in the production flows are still very large. Albert MFMA, Schaap M, Scannell C, O'Dowd CD, de Leeuw G (2012) Uncertainties in determining the organic fraction of global sub-micron sea spray emissions. Covert DS, Kapustin VN, Bates TS, Quinn PK (1992) New particle formation in the marine boundary layer.

Dulac F, Bergametti G, Losno R, Remoudaki E, Gomes L et al (1992) Dry deposition of mineral aerosol particles in the marine atmosphere: importance of the large fraction. Hunter KA, Boyd PW (2007) Iron-binding ligands and their role in ocean iron biogeochemistry. Koc¸ak M, Mihalopoulos N, Kubilay N (2007) Chemical composition of fine and coarse aerosol fractions in the northeastern Mediterranean.

Pirjola L, O'Dowd CD, Brooks IM, Kulmala M (2000) Can new particle formation occur in the clear marine boundary layer. L'Helguen S, Pujo-Pay M (2011) Nutrient control of N2 fixation in the oligotrophic Mediterranean Sea and the impact of Saharan dust events. Russell LM, Pandis SN, Seinfeld JH (1994) Aerosol production and growth in the marine boundary layer.

Ternon E, Guieu C, Loy¨e-Pilot MD, Leblond N, Bosc E, Gasser B, Martin J, Miquel JC (2010) The impact of dust from the Sahara on particulate export in the water column of the northwestern Mediterranean. Uematsu M, Duce RA, Prospero JM (1985) Deposition of atmospheric mineral particles in the North Pacific. Vogt R, Crutzen PJ, Sander R (1996) A mechanism for the release of halogen from sea salt aerosol in the remote marine boundary layer.

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