Quasi‐Lagrangian investigation into dimethyl sulfide oxidation in maritime air using a combination of measurements and model

James, Jonathan; Harrison, Roy M.; Savage, Nick; Allen, Andrew G.; Grenfell, John Lee; Allan, B. J.; Plane, J. M. C.; Hewitt, C. N.; Davison, Brian; Robertson, Lennart

doi:10.1029/2000jd900375

Cited by 19 publications

(20 citation statements)

References 48 publications

(15 reference statements)

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“…It is assumed that the only end product of DMS oxidation is SO 2 , thus ignoring the relatively small yield of methanesulphonic acid (MSA) and other oxidation products. Following the suggestion that an additional (unknown) oxidant is required to obtain reasonable agreement between observed and modelled DMS concentrations (Chin et al 1996, James et al 2000, we increase the reaction rate between DMS and OH by a factor of two, relative to the original rate given by Hynes et al (1986). This is smaller than the factor of 3.3 needed by James et al (2000) to enable their model to reproduce measurements at Mace Head Research Station in Ireland.…”

Section: Numerical Experimentsmentioning

confidence: 93%

Global simulations of the impact on contemporary climate of a perturbation to the sea-to-air flux of dimethylsulfide

Gabric¹,

Qu²,

Rotstayn³

et al. 2013

AMOJ

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The sea-to-air flux of the biogenic sulfur (S) compound dimethylsulfide (DMS) is thought to constitute an important radiative impact on climate, especially in remote marine areas. Previous biogeochemical modelling analyses simulate medium to large changes in the sea-to-air flux of DMS in polar regions under warming scenarios. Here we assess the global radiative impact of such a prescribed change in DMS flux on contemporary climate using a low-resolution atmospheric general circulation model. This impact operates through the atmospheric oxidation of DMS to radiatively-active sulfate aerosols, which are known to both reflect incoming short-wave radiation and to affect the microphysical properties of clouds, for example, through an increase in cloud albedo. We use an atmospheric GCM with incorporated sulfur cycle, coupled to a mixed-layer ('q-flux') ocean, to estimate the climatic response to a prescribed meridionally-variable change in zonal DMS flux, as simulated in a previous modelling analysis. We compare baseline sulfur emissions (contemporary anthropogenic S and contemporary DMS sea-to-air flux), with contemporary anthropogenic S and a perturbed DMS flux. Our results indicate that the global mean DMS vertically integrated concentration increases by about 41 per cent. The relative increase in DMS annual emission is around 17 per cent in 70-80°N, although the most significant increase is in 50-70°S, up to 70 per cent. However, concentrations of atmospheric SO 2 and SO 4 2-increase by only about eight per cent. The oxidation of DMS by OH increases by about 20 per cent. Oxidation of SO 2 to SO 4 2 by H 2 O 2 increases seven per cent. The oxidation of SO 2 by O 3 increases around six per cent. Overall sulfur emissions increase globally by around 4.6 per cent.Global mean aerosol optical depth (AOD) increases by 3.5 per cent. Global mean surface temperature decreases by 0.6 K. There is a notable difference between the impacts in the southern and northern hemispheres. In general, most processes and chemical species related to the sulfur cycle show a larger increase in the southern hemisphere, except SO 2 and the oxidation of DMS by NO 3 . The global mean direct radiative forcing due to the DMS change is -0.05 Wm -2 with total forcing (direct + indirect effects) of -0.48 Wm -2 . This perturbation on DMS flux leads to a mean surface temperature decrease in the southern hemisphere of around 0.8 K, compared with a decrease of 0.4 K in the northern hemisphere.

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Section: Numerical Experimentsmentioning

confidence: 93%

Global simulations of the impact on contemporary climate of a perturbation to the sea-to-air flux of dimethylsulfide

Gabric¹,

Qu²,

Rotstayn³

et al. 2013

AMOJ

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“…It is assumed that the only end product of DMS oxidation is SO 2 , thus ignoring the relatively small yield of methane sulfonic acid (MSA) and other oxidation products. A modification to the treatment of DMS oxidation used in ECHAM4 is introduced, following other authors who have argued that an additional (unknown) oxidant is required to obtain reasonable agreement between observed and modeled DMS concentrations [ Chin et al , 1996; James et al , 2000]. We increase the reaction rate between DMS and OH by a factor of two, relative to the original rate given by Hynes et al [1986].…”

Section: Model Descriptionmentioning

confidence: 99%

Simulation of the tropospheric sulfur cycle in a global model with a physically based cloud scheme

Rotstayn

Lohmann

2002

J. Geophys. Res.

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[1] The treatment of the sulfur cycle in the CSIRO global climate model (GCM) is described. It is substantially based on the scheme developed previously for the European Center/Hamburg (ECHAM) model, but the treatment of wet scavenging has been completely rewritten to better reflect the different properties of liquid and frozen precipitation, and the treatment of these in the model's cloud microphysical scheme. The model is able to reproduce the observed finding that wet deposition of sulfur over Europe and North America is larger in summer than in winter, but the seasonal cycle of sulfate over Europe is not well simulated. The latter is improved when the amplitude of the seasonal cycle of European emissions is increased. Below-cloud scavenging makes an important contribution in our scheme: On omitting it, the global sulfate burden increases from 0.67 to 0.93 Tg S. On reverting to the less efficient scavenging treatment used in ECHAM, the global sulfate burden again increases from 0.67 to 0.93 Tg S, and excessive sulfate concentrations are obtained in Europe and North America. Some deficiencies in the simulation are investigated via further sensitivity tests. In particular, during the Arctic winter, the modeled sulfur dioxide (SO 2 ) concentrations are too large, and the modeled sulfate concentrations are too small (as in most global sulfur-cycle models). Recent laboratory experiments suggest that SO 2 oxidation in ice clouds is nonnegligible. We obtain a much improved Arctic simulation when a simple treatment of SO 2 oxidation in ice clouds is included.

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“…DMS oxidation by halogen oxides in the gas phase [12][13][14][15], and via heterogeneous reactions [16], for example, with aqueous phase ozone (O 3 ) [17,18], may also be important. Some model calculations over predict the concentration of DMS in the marine boundary layer (MBL), suggesting that there may be a missing sink [19]. In addition to looking for a new DMS sink, there has been much interest in examining the reactions that are known sinks for DMS, including reaction with OH [20].…”

Section: Introductionmentioning

confidence: 99%

Theoretical study of adducts of dimethyl sulfide with hydroperoxyl and hydroxyl radicals

Aloisio¹

2006

Chemical Physics

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Structures and energies of complexes of dimethyl sulfide (DMS) with hydroxyl (OH) and hydroperoxyl (HO 2 ) radicals have been studied using ab initio and density functional theory. Two isomers of the complex between OH and DMS were found, one dipole-dipole complex and one 3e À /2c complex. The binding energies (D 0 ) of these two complexes have been found to be consistent with previous studies. This is the first reported study of the complex between DMS and HO 2 . One structure was found for this complex, and the binding energy (D 0 ) has been determined to be 9.0 kcal mol À1 using the fully optimized MP2/6-311++G(3df,3pd) level of theory. Vibrational and rotational constants are also presented for all of complexes calculated. Thermodynamic parameters and equilibrium constants for the formation of these complexes from the monomers have been calculated. The results have been related to laboratory experiments studying these reactions, and some implications to oxidation of DMS in the atmosphere have been discussed.

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Quasi‐Lagrangian investigation into dimethyl sulfide oxidation in maritime air using a combination of measurements and model

Cited by 19 publications

References 48 publications

Global simulations of the impact on contemporary climate of a perturbation to the sea-to-air flux of dimethylsulfide

Global simulations of the impact on contemporary climate of a perturbation to the sea-to-air flux of dimethylsulfide

Simulation of the tropospheric sulfur cycle in a global model with a physically based cloud scheme

Theoretical study of adducts of dimethyl sulfide with hydroperoxyl and hydroxyl radicals

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