B. C. Nguyen

Seasonal variation of atmospheric dimethylsulfide at Amsterdam Island in the southern Indian Ocean

Daily measurements of atmospheric concentrations of dimethylsulfide (DMS) were carried out for two years in a marine site at remote area: the Amsterdam Island (37°50′S–77°31′E) located in the southern Indian Ocean. DMS concentrations were also measured in seawater. A seasonal variation is observed for both DMS in the atmosphere and in the sea-surface. The monthly averages of DMS concentrations in the surface coastal seawater and in the atmosphere ranged, respectively, from 0.3 to 2.0 nmol l-1 and from 1.4 to 11.3 nmol m-3 (34 to 274 pptv), with the highest values in summer. The monthly variation of sea-to-air flux of DMS from the southern Indian Ocean ranges from 0.7 to 4.4 μmol m-2 d-1. A factor of 2.3 is observed between summer and winter with mean DMS fluxes of 3.0 and 1.3 μmol m-2 d-1, respectively.

Seasonal variations of atmospheric sulfur dioxide and dimethylsulfide concentrations at Amsterdam Island in the southern Indian Ocean

Daily measurements of atmospheric sulfur dioxide (SO2) concentrations were performed from March 1989 to January 1991 at Amsterdam Island (37°50′ S–77°30′ E), a remote site located in the southern Indian Ocean. Long-range transport of continental air masses was studied using Radon (222Rn) as continental tracer. Average monthly SO2 concentrations range from less than 0.2 to 3.9 nmol m-3 (annual average = 0.7 nmol m-3) and present a seasonal cycle with a minimum in winter and a maximum in summer, similar to that described for atmospheric DMS concentrations measured during the same period. Clear diel correlation between atmospheric DMS and SO2 concentrations is also observed during summer. A photochemical box model using measured atmospheric DMS concentrations as input data reproduces the seasonal variations in the measured atmospheric SO2 concentrations within ±30%. Comparing between computed and measured SO2 concentrations allowed us to estimate a yield of SO2 from DMS oxidation of about 70%.

Dimethylsulfide, aerosols, and condensation nuclei over the tropical northeastern Atlantic Ocean

Concentration of dimethylsuifide (DMS) in seawater, concentrations of DMS and sulfur dioxide (SO2) in the atmosphere, concentrations of methanesulfonate (MSA) and non-sea-salt sulfate (nss-SO42−) in size-segregated aerosols, and number concentration of condensation nuclei (CN) were measured during September and October 1991 in the northern tropical Atlantic Ocean in order to assess the role of DMS in CN production over this oceanic area. Radon-222 activity and aerosol ionic composition were used to distinguish air masses with oceanic, continental, and/or polluted characters. No obvious covariation appeared between DMS and its oxidation products (SO2, H2SO4, and MSA) over the whole period of the experiment. However, the division of data into subsets according to continental tracer information allowed us to show that SO2 and nss-SO4 concentrations correlated with DMS concentration in unpolluted air masses. MSA and nss-SO42− were found to be mainly concentrated in particles with diameters < of 0.6 μm. Daily mean nss-SO42− in the <0.6-μm-diameter range and CN concentration were correlated (R = 0.91, n = 17, P < 0.001), which suggests that H2SO4 is an important CN precursor. Atmospheric DMS and CN number daily mean concentrations also correlated (R = 0.82, n = 21, P < 0.001). However, the CN population was strongly influenced by continental inputs less than 500 km downwind of Africa, whereas DMS seemed to be able to affect the CN number concentration at about 1500 km from this continent.

The oceanic source of carbonyl sulfide (COS)

Abstract Carbonyl sulfide (COS) concentrations both in sea water and in the marine atmospheric boundary layer have been measured for 2 years at Amsterdam Island, as well as during oceanographic cruises in regions of different productivity (coastal areas, upwelling areas and open ocean) in the Indian Ocean and Mediterranean Sea. Surface waters of the Indian Ocean and Mediterranean Sea were found to be supersaturated with respect to the atmosphere. The supersaturation of surface coastal sea water in COS displays a diurnal cycle with a midday/midnight ratio of approximately 4, and in addition a seasonal cycle with maximum values during summer and a summer/winter ratio of 2. The supersaturation of open ocean surface sea water is 3 times lower than that of the coastal areas. Taking into account the diurnal, seasonal and geographical variations of the sea water supersaturation in COS, along with the seasonal variation of the sea-air exchange coefficient and the Henrys law coefficient, a global oceanic flux of COS of 0.43 (0.30 to 0.60)Tg COS per year is estimated.

Field study of dimethylsulfide oxibation in the boundary layer: Variations of dimethylsulfide, methanesulfonic acid, sulfur dioxide, non-sea-salt sulfate and aitken nuclei at a coastal site

Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO2), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO42-) were monitored during the period June 9–26, 1989 at a coastal site in Brittany. As indicated by the radon (Rn-222) activities and the high concentrations of NOx the air masses, for most of the experiment, were continental in origin. The observed concentrations range from 1.9 to 65 nmol/m3 for DMS (n=157), 0.6 to 94.2 nmol/m3 for SO2 (n=50), 0.6 to 11.6 nmol/m3 for MSA (n=44) and 42 to 350 nmol/m3 for nss-SO42- (n=44). Aitken nuclei reached values as high as 4.5 × 105 particles/m3. When continental conditions predominated, the measured SO2 concentrations were lower than those expected from a consideration of the observed DMS concentrations and the existence of SO2 background of the continental air masses. Similarly, compared to the MSA/DMS ratio in the marine atmosphere, higher concentrations of MSA were observed than those expected from the measured levels of DMS. The presence of enhanced levels of MSA was also endorsed by the observation that the measured mean MSA/nss-SO42- ratio of 6±3% was similar to the mean value of 6.9% observed in the marine atmosphere. These above observations are in line with recent laboratory findings by Barnes et al. (1988), which show an increase of the MSA/DMS yield with a simultaneous decrease of the SO2/DMS yield in the presence of NOx.

Summertime Seawater Concentrations of Dimethylsulfide in the Western Indian Ocean: Reconciliation of Fluxes and Spatial Variability with Long-Term Atmospheric Observations

Dimethylsulfide (DMS) measurements in the seawater of the subtropical and the temperate western Indian Ocean were conducted for the first time from 3 December to 20 December 1997. In total, 443 surface seawater DMS determinations were performed between 24°–49° S and 50° E–77° E with a frequency of 1 sample every 10 km. An important spatial variability was observed in seawater DMS concentrations with values ranging from 0.9 to 35.8 nM. DMS maxima coincided in most cases with thermal fronts and were in reasonable agreement with mean pigment figures obtained from satellite observations. The deduced DMS fluxes are consistent with long-term observations of atmospheric DMS and rainwater concentrations of nss- SO4= and MSA measured at Amsterdam island (37° S, 77° E); then account for the differences observed in atmospheric DMS concentrations between Amsterdam island and Cape Grim, Indian Ocean monitoring stations.

Annual variation of atmospheric carbonyl sulfide in the marine atmosphere in the Southern Indian Ocean

Measurements of the concentrations of carbonyl sulfide (COS) in the marine atmosphere were made over a period of two years in the southern Indian Ocean (Amsterdam Island, 37°50′ S–77°31′ E; March 1987–February 1988 and April 1989–February 1990). The mean atmospheric COS concentration for the whole period was 475±48 pptv (n=544). Atmospheric COS concentrations show no significant seasonal variation with a summer to winter ratio of 1.05. Taking into account the observed variability of the atmospheric COS concentration (10%), a value of 1.4 yr is estimated as a lower limit for the atmospheric COS lifetime. A comparison of the COS data at Amsterdam Island with those obtained in the Southern Hemisphere in the past 12 yr does not reveal any significant trend in the tropospheric background COS mixing ratio.

Spatial and temporal variability of dissolved sulfur compounds in European estuaries

The spatial and temporal distribution of Dimethylsulfide (DMS),Dimethylsulfoniopropionate (DMSP) – its precursor –,Dimethylsulfoxyde (DMSO) – one of its oxidation products –Carbonyl sulfide (COS) and Carbonyl disulfide (CS2) wereinvestigated during nine oceanographic cruises carried out in six majortidal European estuaries between July 1996 and May 1998. Low levels ofDMS were recorded (mean of 0.6 nM, standard deviation (σ) 0.3 nM)during these 9 cruises. Positive correlations between DMS and salinitywere frequently observed, with the highest DMS concentrations in theplume of estuaries, which could be explained by change in phytoplanktonspeciation from estuarine to shelf waters. Strong correlation betweenDMSP and DMS was reported for most of the estuaries denoting a simpleconservative mixing of riverine and marine waters controlled by tide. Incontrast to DMS, significant levels of COS and CS2 with meanconcentrations of 220 ± 150 (pM; pM =10−12 M) and 25 ± 6 pM respectively wererecorded in four estuaries, indicating that estuaries could be asignificant source of these compounds.

Seasonal variation of dimethylsulfoxide in rainwater at Amsterdam Island in the Southern Indian Ocean : Implications on the biogenic sulfur cycle

A continuous record of dimethylsulfoxide (DMSO) in rainwater was performed at Amsterdam island (37°S 77°E) from December 1995 to February 1997. Eighty one rainwater samples were collected. DMSO, methanesulfonic acid (MSA), the major anions, and cations were analyzed. DMSO concentrations ranged from 7.0 to 369 nM, with a distinct seasonal variation. The mean concentrations during the summer and the winter periods were 90 nM and 25.6 nM respectively. The observed DMSO seasonal cycle is in line with the observations of DMS in the atmosphere and MSA in rainwater, measured simultaneously during the reported period. However, the summer to winter ratio of DMSO is significantly lower than that observed for DMS and MSA. The DMSO to MSA ratio and its observed seasonal variability are also presented. The implications on the biogenic sulfur cycle are discussed.

Carbonyl sulfide emissions from biomass burning in the tropics

Carbonyl sulfide emissions from biomass burning have been studied during field experiments conducted both in an African savanna area (Ivory Coast) and rice fields, central highland pine forest and savanna areas in Viet-Nam. During these experiments CO2, CO and C2H2 or CH4 have also been also monitored. COS values range from 0.6 ppbv outside the fires to 73 ppbv in the plumes. Significant correlations have been observed between concentrations of COS and CO (R2=0.92,n=25) and COS and C2H2 (R2=0.79,n=26) indicating a COS production during the smoldering combustion. COS/CO2 emission factors (ΔCOS/ΔCO2) during field experiments ranged from 1.2 to 61×10−6 (11.4×10−6 mean value). COS emission by biomass burning was estimated to be up to 0.05 Tg S/yr in tropics and up to 0.07 Tg S/yr on a global basis, contributing thus about 10% to the global COS flux. Based on the S/C ratio measured in the dry plant biomass and the ΔCOS/ΔCO2 emission factor, COS can account for only about 7% of the sulfur emitted in the atmosphere by biomass burning.