A modelling study of the atmospheric chemistry of DMS using the global model, STOCHEM-CRI

Khan, M. Anwar H.; Gillespie, Simon; Razis, Benjamin; Xiao, Peng; Davies‐Coleman, Michael T.; Percival, Carl J.; Derwent, R.G.; Dyke, John M.; Ghosh, Mariana; Lee, E.P.F.; Shallcross, Dudley E.

doi:10.1016/j.atmosenv.2015.12.028

Cited by 36 publications

(49 citation statements)

References 53 publications

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“…Largescale models of atmospheric chemistry typically contain very simplified DMS chemistry and often ignore potentially important reaction intermediates. Most of these models include oxidation of DMS by OH and NO 3 radicals, directly producing SO 2 and MSA, and ignore the formation of dimethyl sulfoxide (DMSO: CH 3 SOCH 3 ) and methane sulphinic acid (MSIA: CH 3 SO 2 H) intermediates (Chin et al, 1996(Chin et al, , 2000Gondwe et al, 2003;Berglen et al, 2004;Kloster et al, 2006). Nevertheless, previous large-scale modeling studies have suggested that BrO could be an important sink for DMS globally (up to 30 %), especially in the remote MBL where BrO mixing ratios can reach ppt levels (Boucher et al, 2003;von Glasow et al, 2004;Breider et al, 2010;Khan et al, 2016).…”

Section: Introductionmentioning

confidence: 99%

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

et al. 2018

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Abstract. The oxidation of dimethyl sulfide (DMS) in the troposphere and subsequent chemical conversion into sulfur dioxide (SO2) and methane sulfonic acid (MSA) are key processes for the formation and growth of sulfur-containing aerosol and cloud condensation nuclei (CCN), but are highly simplified in large-scale models of the atmosphere. In this study, we implement a series of gas-phase and multiphase sulfur oxidation mechanisms into the Goddard Earth Observing System-Chemistry (GEOS-Chem) global chemical transport model – including two important intermediates, dimethyl sulfoxide (DMSO) and methane sulphinic acid (MSIA) – to investigate the sulfur cycle in the global marine troposphere. We found that DMS is mainly oxidized in the gas phase by OH (66 %), NO3 (16 %) and BrO (12 %) globally. DMS + BrO is important for the model's ability to reproduce the observed seasonality of surface DMS mixing ratio in the Southern Hemisphere. MSA is mainly produced from multiphase oxidation of MSIA by OH(aq) (66 %) and O3(aq) (30 %) in cloud droplets and aerosols. Aqueous-phase reaction with OH accounts for only 12 % of MSA removal globally, and a higher MSA removal rate is needed to reproduce observations of the MSA ∕ nssSO42- ratio. The modeled conversion yield of DMS into SO2 and MSA is 75 % and 15 %, respectively, compared to 91 % and 9 % in the standard model run that includes only gas-phase oxidation of DMS by OH and NO3. The remaining 10 % of DMS is lost via deposition of intermediates DMSO and MSIA. The largest uncertainties for modeling sulfur chemistry in the marine boundary layer (MBL) are unknown concentrations of reactive halogens (BrO and Cl) and OH(aq) concentrations in cloud droplets and aerosols. To reduce uncertainties in MBL sulfur chemistry, we should prioritize observations of reactive halogens and OH(aq).

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Section: Introductionmentioning

confidence: 99%

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

et al. 2018

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“…The western Pacific warm pool (WPWP) is a coral-reefdense region located to the north-east of Australia, where SST reaches an upper limit of ∼ 30 • C due to regular pulses of low-level cloud (LLC) cover which closely follow the tidal cycle (Kleypas et al, 2008;Takahashi et al, 2010;Ramanathan and Collins, 1991). It has been posited that coral-reef DMS emissions contribute to the formation of this "ocean thermostat", acting to suppress ocean temperatures below coral thermal tolerance thresholds, resulting in few coral bleaching events over the past 25 years (Kleypas et al, 2008; Takahashi et al, 2010).…”

Section: Influence On Low-level Clouds Sea Surface Temperature and Smentioning

confidence: 99%

Dimethylsulfide (DMS), marine biogenic aerosols and the ecophysiology of coral reefs

et al. 2020

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Abstract. Global climate change and the impacts of ocean warming, ocean acidification and declining water quality are adversely affecting coral-reef ecosystems. This is of great concern, as coral reefs provide numerous ecosystem, economic and social services. Corals are also recognised as being amongst the strongest individual sources of natural atmospheric sulfur, through stress-induced emissions of dimethylsulfide (DMS). In the clean marine boundary layer, biogenic sulfates contribute to new aerosol formation and the growth of existing particles, with important implications for the radiative balance over the ocean. Evidence suggests that DMS is not only directly involved in the coral stress response, alleviating oxidative stress, but also may create an “ocean thermostat” which suppresses sea surface temperature through changes to aerosol and cloud properties. This review provides a summary of the current major threats facing coral reefs and describes the role of dimethylated sulfur compounds in coral ecophysiology and the potential influence on climate. The role of coral reefs as a source of climatically important compounds is an emerging topic of research; however the window of opportunity to understand the complex biogeophysical processes involved is closing with ongoing degradation of the world's coral reefs. The greatest uncertainty in our estimates of radiative forcing and climate change is derived from natural aerosol sources, such as marine DMS, which constitute the largest flux of oceanic reduced sulfur to the atmosphere. Given the increasing frequency of coral bleaching events, it is crucial that we gain a better understanding of the role of DMS in local climate of coral reefs.

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“…The lifetime of DMS in the atmosphere with respect to the primary oxidant OH is around 1.3 days (reaction rate = 7.8 × 10 −12 cm 3 molec −1 s −1 , [OH] = 1.1 × 10 6 molec/cm 3 (Albu et al, 2006)). In some regions of the marine boundary layer, BrO may also contribute to the oxidation of DMS leading to shorter DMS lifetimes (Breider et al, 2010;Khan et al, 2016;Barnes et al, 2006). The high and variable levels of DMS encountered during the Arabian Sea crossing suggest that DMS mixing ratios are influenced by local variation of the sources (i.e.…”

Section: Atmospheric Lifetimes Of Dms Dmso 2 and Msammentioning

confidence: 99%

A new marine biogenic emission: methane sulfonamide (MSAM), DMS and DMSO2 measured in air over the Arabian Sea

Edtbauer

Stönner

Pfannerstill

et al. 2020

Preprint

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Abstract. We present the first ambient measurements of a new marine emission methane sulfonamide (MSAM), along with dimethyl sulfide (DMS) and dimethyl sulfone (DMSO2) over the Arabian Sea. Two shipborne transects (W to E, E to W) were made during the AQABA (Air Quality and Climate Change in the Arabian Basin) measurement campaign. DMS mixing ratios were in the range 0.3&#8211;0.5&#8201;ppb during the first traverse of the Arabian Sea (first leg) and 0.1 to 0.3&#8201;ppb in the second leg. In the first leg DMSO2 was always below 0.04&#8201;ppb and MSAM was close to the limit of detection. During the second leg DMSO2 was between 0.04&#8211;0.12&#8201;ppb and MSAM was mostly in the range 0.02&#8211;0.05&#8201;ppb with maximum values of 0.06&#8201;ppb. An analysis of HYSPLIT back trajectories combined with calculations of the exposure of these trajectories to chlorophyll a content in the water revealed that most MSAM originates from the Somalia upwelling region, known for its high biological activity. This new marine emission is of particular interest as it contains both sulfur and nitrogen, making it potentially relevant to marine nutrient cycling and particle formation.

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A modelling study of the atmospheric chemistry of DMS using the global model, STOCHEM-CRI

Cited by 36 publications

References 53 publications

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

Dimethylsulfide (DMS), marine biogenic aerosols and the ecophysiology of coral reefs

A new marine biogenic emission: methane sulfonamide (MSAM), DMS and DMSO<sub>2</sub> measured in air over the Arabian Sea

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A modelling study of the atmospheric chemistry of DMS using the global model, STOCHEM-CRI

Cited by 36 publications

References 53 publications

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

DMS oxidation and sulfur aerosol formation in the marine troposphere: a focus on reactive halogen and multiphase chemistry

Dimethylsulfide (DMS), marine biogenic aerosols and the ecophysiology of coral reefs

A new marine biogenic emission: methane sulfonamide (MSAM), DMS and DMSO&lt;sub&gt;2&lt;/sub&gt; measured in air over the Arabian Sea

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Product

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A new marine biogenic emission: methane sulfonamide (MSAM), DMS and DMSO<sub>2</sub> measured in air over the Arabian Sea