Regional and global trends in sulfate aerosol since the 1980s

Manktelow, P. T.; Mann, G. W.; Carslaw, K. S.; Spracklen, D. V.; Chipperfield, Martyn P.

doi:10.1029/2006gl028668

Cited by 92 publications

(84 citation statements)

References 25 publications

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“…The fraction of SO 2 converted into SO 4 (sulfate production efficiency) lies in the range 0.38-0.51 and, consistent with previous studies, is lowest for W. Europe (Chin et al, 2000;Rasch et al, 2000;Koch et al, 2007;Manktelow et al, 2007) where SO 2 deposition is favored by the slow venting of the boundary layer and where oxidants are more limited than at lower latitudes. The contribution of each region to total (anthropogenic + natural) global SO 4 (SO 4glob ) can be expressed as a fraction of the contribution to total global sulfur emissions, giving a sulfate burden potential (Rasch et al, 2000): (1) where i is the grid box index and reg implies SO 4 originating from regional anthropogenic SO 2 .…”

Section: Regional Aerosol Budgetsupporting

confidence: 72%

“…Our anthropogenic SO 2 emissions are derived from the AEROCOM 2000 inventory (Cofala et al, 2005), while Rasch et al (2000) used the earlier GEIA 1B 1985 emissions (Benkovitz et al, 1996) and Koch et al (2007) used EDGAR 3.2 1995(Olivier and Berdowski, 2001). There are considerable differences in the magnitude of SO 2 emission over Europe, N. America and Asia between each inventory, which will have a significant influence on the behavior of sulfur emitted from each region (Manktelow et al, 2007). Furthermore, each study uses a different set of coordinates to define Europe, N. America and Asia.…”

Section: Regional Aerosol Budgetmentioning

confidence: 99%

“…The Global Model of Aerosol Processes (GLOMAP; Spracklen et al, 2005a, b;Manktelow et al, 2007) is an extension to the TOMCAT offline 3-D global chemical transport model (Chipperfield, 2006). GLOMAP includes the processes of aerosol nucleation, condensation, hygroscopic growth, coagulation, wet and dry deposition, and cloud processing.…”

Section: Model Descriptionmentioning

confidence: 99%

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Variable CCN formation potential of regional sulfur emissions

et al. 2009

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Abstract. Aerosols are short lived so their geographical distribution and impact on climate depends on where they are emitted. Previous model studies have shown that the mass of sulfate aerosol produced per unit sulfur emission (the sulfate burden potential) and the associated direct radiative forcing vary regionally because of differences in meteorology and photochemistry. Using a global model of aerosol microphysics, we show that the total number of aerosol particles produced per unit sulfur emission (the aerosol number potential) has a different regional variation to that of sulfate mass. The aerosol number potential of N. American and Asian emissions is calculated to be a factor of 3 to 4 times greater than that of European emissions, even though Europe has a higher sulfate burden potential. Pollution from N. America and Asia tends to reach higher altitudes than European pollution so forms more new particles through nucleation. Regional differences in particle production and growth mean that sulfur emissions from N. America and E. Asia produce 50 nm diameter cloud condensation nuclei up to 70% more efficiently than Europe. For 80 nm diameter CCN, N. America and Europe produce CCN 2.5 times more efficiently than E. Asia. The impact of regional sulfur emissions on particle concentrations is also much more widely spread than the impact on sulfate mass, due to efficient particle production in the free troposphere during long range transport. These results imply that regional sulfur emissions will have different climate forcing potentials through changes in cloud drop number.

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Section: Regional Aerosol Budgetsupporting

confidence: 72%

Section: Regional Aerosol Budgetmentioning

confidence: 99%

Section: Model Descriptionmentioning

confidence: 99%

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Variable CCN formation potential of regional sulfur emissions

et al. 2009

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“…We used the modal version of the model (GLOMAP-mode) where the aerosol size distribution is treated using a two-moment modal scheme (Manktelow et al, 2007;Mann et al, 2010). We simulated sulfate, sea-salt, Atmos.…”

Section: Glomap Global Aerosol Modelmentioning

confidence: 99%

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

et al. 2011

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Abstract.The budget of atmospheric secondary organic aerosol (SOA) is very uncertain, with recent estimates suggesting a global source of between 12 and 1820 Tg (SOA) a −1 . We used a dataset of aerosol mass spectrometer (AMS) observations from 34 different surface locations to evaluate the GLOMAP global chemical transport model. The standard model simulation (which included SOA from monoterpenes only) underpredicted organic aerosol (OA) observed by the AMS and had little skill reproducing the variability in the dataset. We simulated SOA formation from biogenic (monoterpenes and isoprene), lumped anthropogenic and lumped biomass burning volatile organic compounds (VOCs) and varied the SOA yield from each precursor source to produce the best overall match between model and observations. We assumed that SOA is essentially non-volatile and condenses irreversibly onto existing aerosol. Our best estimate of the SOA source is 140 Tg (SOA) a −1 but with a large uncertainty range which we estimate to be 50-380 Tg (SOA) a −1 . We found the minimum in normalised mean error (NME) between model and the AMS dataset when we assumed a large SOA source (100 Tg (SOA) a −1 ) from sources that spatially matched anthropogenic pollution (which we term antropogenically controlled SOA). We used organic carbon observations compiled by Bahadur et al. (2009) to evaluate our estimated SOA sources. We found that the model with a large anthropogenic SOA source was the most consistent with these observaCorrespondence to: D. V. Spracklen (dominick@env.leeds.ac.uk) tions, however improvement over the model with a large biogenic SOA source (250 Tg (SOA) a −1 ) was small. We used a dataset of 14 C observations from rural locations to evaluate our estimated SOA sources. We estimated a maximum of 10 Tg (SOA) a −1 (10 %) of the anthropogenically controlled SOA source could be from fossil (urban/industrial) sources. We suggest that an additional anthropogenic source is most likely due to an anthropogenic pollution enhancement of SOA formation from biogenic VOCs. Such an anthropogenically controlled SOA source would result in substantial climate forcing. We estimated a global mean aerosol direct effect of −0.26 ± 0.15 Wm −2 and indirect (cloud albedo) effect of −0.6 +0.24 −0.14 Wm −2 from anthropogenically controlled SOA. The biogenic and biomass SOA sources are not well constrained with this analysis due to the limited number of OA observations in regions and periods strongly impacted by these sources. To further improve the constraints by this method, additional OA observations are needed in the tropics and the Southern Hemisphere.

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“…In the atmosphere over remote marine regions, there are two main sources for aerosol nssSO 4 2 : reactions involving either dimethylsulfide (DMS) or primary SO 2 produced through anthropogenic emissions (Stern, 2006;Manktelow et al, 2007). To assess the anthropogenic and/or biogenic influence over the study area, the non sea salt sulphate (nssSO 4 2-) was calculated by assuming Na + as a conservative indicator of marine origin.…”

Section: Latitudinal Variations In Aerosol Composition and Processes mentioning

confidence: 99%

Latitudinal and Size Segregated Compositional Variability of Aerosols over the Indian and Southern Ocean during 2010 Austral Summer

Thakur

Thamban

2014

Aerosol Air Qual. Res.

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To characterize the spatial variations in size segregated aerosols, samples were collected over the Indian and Southern oceans (7°N to 68°S) during the Indian expedition to Southern Ocean (January-February 2010). The chemical and mass concentrations of ions were measured in nine size classes (0.4-> 10 µm) of aerosols through ion-exchange chromatographic system and gravimetric estimates, respectively. Mass concentrations of coarse aerosols increase towards the Antarctic coast which is well correlated with the increasing humidity suggesting growth of particles. The study area was found to be predominately impacted by sea salt aerosols with a sea salt load of 91%. F -, Cl -and NO 3 -reflected anthropogenic impact within the fine mode aerosols but the marine influence dominated the coarse mode. Methanesulphonic (MSA) was predominantly of biogenic origin but a substantially low MSA/nssSO 4 2-ratio suggested that DMS contribution to the total nssSO 4 2-concentration was low. NH 4 + concentrations showed a shift from fine to coarse particles, with a trimodal distribution over the Southern Ocean. Our study reports a significant Cl -depletion in the aerosols and the degree of Cl -deficit was size-dependent, increasing with decreasing particle sizes. The neutralization ratios suggested differential behavior of ions with respect to the prevailing meteorological conditions. The coarse mode aerosols were neutralized by ammonia leading to the formation of NH 4 NO 3 particles. The fine modes were predominately composed of NH 4 HSO 4 and its formation is favored by the high humidity and foggy conditions over the study area. Factor analysis support that the Southern Indian Ocean (10°S to 59°S) had the highest loading of anthropogenic and sea salt aerosols, which lead to the formation of secondary aerosols through gas to particle transformations. The rocky Antarctic coastline, act as a source of coarse crustal aerosols over the Southern Ocean (60°S to 65°S).

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Regional and global trends in sulfate aerosol since the 1980s

Cited by 92 publications

References 25 publications

Variable CCN formation potential of regional sulfur emissions

Variable CCN formation potential of regional sulfur emissions

Aerosol mass spectrometer constraint on the global secondary organic aerosol budget

Latitudinal and Size Segregated Compositional Variability of Aerosols over the Indian and Southern Ocean during 2010 Austral Summer

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