Correction to “The contribution of ocean‐leaving DMS to the global atmospheric burdens of DMS, MSA, SO2, and NSS SO4=”

Gondwe, Mtinkheni; Krol, Maarten; Gieskes, W.W.C.; Klaassen, Wim; Baar, Hein de

doi:10.1029/2003gb002153

Cited by 11 publications

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“…[31] Analysis of the horizontal spatial distribution of the modeled MSA:nss SO 4 = ratios (Figures 4 and 5a) shows that the highest ratios occur in the Southern Hemisphere throughout the year and that even in the austral winter, the Southern Hemisphere does not relinquish its monopoly of high MSA:nss SO 4 = ratios. This is in agreement with Gondwe et al [2003aGondwe et al [ , 2003b, who found that the contribution of ocean-leaving DMS to the annually averaged atmospheric burdens of DMS oxidation products is greatest in the Southern Hemisphere. Unlike the Southern Hemisphere, the Northern Hemisphere is a region in which the atmospheric sulphur cycle is dominated by anthropogenic inputs throughout the whole year.…”

Section: Ratios Considering All Sulphur Sourcessupporting

confidence: 91%

“…On a hemispheric scale, the highest ratios occur in the Southern Hemisphere, throughout the year, despite multiyear satellite‐deduced primary production showing great concentration of marine phytoplankton at middle to high latitudes in the opposite (Northern) Hemisphere. This is attributed to the fact that the atmospheric DMS burden is also highest in this region [ Gondwe et al , 2003a, 2003b]. Anthropogenic sulphur emissions in the highly industrialized Northern Hemisphere lead to a lower MSA:nss SO 4 = ratio in the Northern Hemisphere.…”

Section: Discussionmentioning

confidence: 99%

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Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis

Gondwe

Krol

Klaassen

et al. 2004

Global Biogeochemical Cycles

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[1] The MSA:nss SO 4 = ratio, which is a measure of the relative marine biogenic contribution to the total atmospheric sulphur burden, has long been measured in various parts of the globe. Transect studies and observations from a network of stations have provided some idea of the spatial and temporal behavior of the ratio in various regions, but gaps in knowledge still exist in other parts of the globe. Here we present results of a global 3-D chemical transport modeling study which complement these measurements and provide a globe-wide picture of the spatial variation and distribution of this ratio.Comparison of modeled versus measured data on the MSA:nss SO 4 = ratio resulting from all sulphur sources considered shows fair model performance (i.e., a general overestimation of 23%; degrees of freedom = 90) in all areas of the globe where actual measurements of the ratio have been made. On the other hand, the model-observation comparisons for the MSA:nss SO 4 = ratio derived solely from the oceanic DMS source are not as satisfactory (an overall overestimation of a factor of 3; degrees of freedom = 50). The MSA:nss SO 4 = ratio that is derived from the oceanic DMS source alone provides information on the relative yields of MSA and SO 4 = from atmospheric DMS oxidation. Our model results are consistent with measurements, showing that the ratio is highest around the polar regions and lowest within the tropics. This spatial trend is attributed to the fact that MSA production occurs best under low temperatures (maximum ambient temperature of 27°C). Despite MSA being preferably produced under low temperatures, observations at high latitudes have consistently shown summer maxima and winter minima in the MSA:nss SO 4 = ratio. This has raised many questions on the robustness of the theory of the MSA production mechanism. Diminished marine biological activity and low seawater DMS conditions in winter have widely been cited as the cause of this observed trend. In this study, we further propose that since photochemical hydroxyl radical (OH) production during the dark winter months at polar latitudes is non-existent, reduced wintertime oxidation of DMS by OH to form MSA results in summer maxima and winter minima in MSA concentrations at these latitudes. Temperature and marine biological activity are, therefore, not the only major determining factors for MSA production at high latitudes on a seasonal scale. Light conditions are also important. Throughout the year, the highest ratios occur in the Southern Hemisphere, where the atmospheric DMS burden is highest. This is in agreement with both short-and long-term measurements in literature.

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Section: Ratios Considering All Sulphur Sourcessupporting

confidence: 91%

Section: Discussionmentioning

confidence: 99%

Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis

Gondwe

Krol

Klaassen

et al. 2004

Global Biogeochemical Cycles

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“…Note that the DMS burdens are slightly higher in C 1 and C 2 than in P 1 and P 2 because the COM cases have different treatments of the DMS‐OH addition adduct formed along the OH‐addition path. Also note that, except for the exceedingly high global DMS burden in Gondwe et al [2003a, 2003b], the MATCH‐based burdens are within a factor of two of the other estimates. The variations among the model estimates result from differences in DMS surface fluxes, OH concentrations, and/or atmospheric circulation patterns.…”

Section: Results and Analysismentioning

confidence: 67%

“… a Other studies: [1], Pham et al [1995]; [2], Chin et al [1996]; [3], Koch et al [1999]; [4], Rasch et al [2000]; [5], Rotstayn and Lohmann [2002]; and [6], Gondwe et al [2003a, 2003b]. All non‐oceanic DMS contributions (e.g., terrestrial DMS, anthropogenic SO 2 , and volcanic SO 2 ) are removed from these estimates using the global annual sulfur budgets contained in these studies.…”

Section: Results and Analysismentioning

confidence: 99%

“…Also, due to their different definitions, there is a two order of magnitude difference between the MATCH burdens and the estimates from the previous studies. As with H 2 SO 4 , these large differences occur because MATCH simulates gas-phase MSA, while the other studies combine MSA in the gas-phase with methanesulfo- Gondwe et al [2003aGondwe et al [ , 2003b. All non-oceanic DMS contributions (e.g., terrestrial DMS, anthropogenic SO 2 , and volcanic SO 2 ) are removed from these estimates using the global annual sulfur budgets contained in these studies.…”

Section: Global Burdensmentioning

confidence: 99%

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Sensitivities of gas‐phase dimethylsulfide oxidation products to the assumed mechanisms in a chemical transport model

Lucas

Prinn

2005

J. Geophys. Res.

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[1] The gas-phase products of dimethylsulfide (DMS) oxidation are simulated in the global 3D Model of Atmospheric Transport and Chemistry (MATCH). The focus is on the sensitivities to the assumed mechanisms of DMS oxidation chemistry in large-scale models, and hence volcanic and anthropogenic sources of SO 2 are ignored. Four representations of DMS chemistry are considered, including two comprehensive mechanisms (about 50 reactions) and two parameterized schemes (four and five reactions). The gas-phase yields of DMS, SO 2 , methanesulfonic acid (MSA) and H 2 SO 4 are compared between these four cases as a measure of the sensitivity to uncertain DMS chemistry. Among the four cases, DMS is largely invariant, while SO 2 using parameterized chemistry is three times higher than its levels using comprehensive chemistry in the tropical upper troposphere. For MSA and H 2 SO 4 , there are order-ofmagnitude inter-mechanistic differences at high and low altitudes in the extratropics, respectively. The differences are attributed to fixed branching yields and the absence of important intermediate species and pathways in the parameterized mechanisms. Regional budgets are also analyzed within the remote Southern Ocean and central tropical Pacific. While the DMS budget varies primarily between the regions, the SO 2 , MSA and H 2 SO 4 budgets vary strongly between the regions and mechanisms. The DMS oxidation products, therefore, are as sensitive to the assumed mechanisms as to the external conditions between the tropics and extratropics. To distinguish between the mechanism cases, the MATCH simulations are also compared to campaign measurements. The simulated values of DMS and SO 2 are found to approximate the observations, but do not provide mechanism differentiation. The gas-phase H 2 SO 4 and MSA simulations differ more extensively from the observations, yet the comprehensive chemistry cases give a better fit to the MSA measurements. Better fits to the MSA observations are also achieved for the two mechanisms that consider dimethylsulfoxide (DMSO) as an MSA precursor.Citation: Lucas, D. D., and R. G. , Sensitivities of gas-phase dimethylsulfide oxidation products to the assumed mechanisms in a chemical transport model,

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Carbonyl sulfide, dimethyl sulfide and carbon disulfide in the Pearl River Delta of southern China: Impact of anthropogenic and biogenic sources

Guo

Simpson

Ding

et al. 2010

Atmospheric Environment

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Reduced sulfur compounds (RSCs) such as carbonyl sulfide (OCS), dimethyl sulfide (DMS) and carbon disulfide (CS 2) impact radiative forcing, ozone depletion, and acid rain. Although Asia is a large source of these compounds, until now a long-term study of their emission patterns has not been carried out. Here we analyze 16 months of RSC data measured at a polluted rural/coastal site in the greater Pearl River Delta (PRD) of southern China. A total of 188 canister air samples were collected from August 2001 to December 2002. The OCS and CS 2 mixing ratios within these samples were higher in autumn/winter and lower in summer due to the influence of Asian monsoon circulations. Comparatively low DMS values observed in this coastal region suggest a relatively low biological productivity during summer months. The springtime OCS levels in the study region (574 AE 40 pptv) were 25% higher than those on other East Asia coasts such Japan, whereas the springtime CS 2 and DMS mixing ratios in the PRD (47 AE 38 pptv and 22 AE 5 pptv, respectively) were 3e30 times lower than elevated values that have been measured elsewhere in East Asia (Japan and Korea) at this time of year. Poor correlations were found among the three RSCs in the whole group of 188 samples, suggesting their complex and variable sources in the region. By means of backward Lagrangian particle release simulations, air samples originating from the inner PRD, urban Hong Kong and South China Sea were identified. The mean mixing ratio of OCS in the inner PRD was significantly higher than that in Hong Kong urban air and South China Sea marine air (p < 0.001), whereas no statistical differences were found for DMS and CS 2 among the three regions (p > 0.05). Using a linear regression method based on correlations with the urban tracer CO, the estimated OCS emission in inner PRD (49.6 AE 4.7 Gg yr À1) was much higher than that in Hong Kong (0.32 AE 0.05 Gg yr À1), whereas the estimated CS 2 and DMS emissions in the study region accounted for a very few percentage of the total CS 2 and DMS emission in China. These findings lay the foundation for better understanding sulfur chemistry in the greater PRD region of southern China.

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Correction to “The contribution of ocean‐leaving DMS to the global atmospheric burdens of DMS, MSA, SO₂, and NSS SO₄⁼”

Cited by 11 publications

References 0 publications

Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis

Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis

Sensitivities of gas‐phase dimethylsulfide oxidation products to the assumed mechanisms in a chemical transport model

Carbonyl sulfide, dimethyl sulfide and carbon disulfide in the Pearl River Delta of southern China: Impact of anthropogenic and biogenic sources

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Correction to “The contribution of ocean‐leaving DMS to the global atmospheric burdens of DMS, MSA, SO2, and NSS SO4=”

Cited by 11 publications

References 0 publications

Comparison of modeled versus measured MSA:nss SO4= ratios: A global analysis

Comparison of modeled versus measured MSA:nss SO4= ratios: A global analysis

Sensitivities of gas‐phase dimethylsulfide oxidation products to the assumed mechanisms in a chemical transport model

Carbonyl sulfide, dimethyl sulfide and carbon disulfide in the Pearl River Delta of southern China: Impact of anthropogenic and biogenic sources

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Product

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Correction to “The contribution of ocean‐leaving DMS to the global atmospheric burdens of DMS, MSA, SO₂, and NSS SO₄⁼”

Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis

Comparison of modeled versus measured MSA:nss SO₄⁼ ratios: A global analysis