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1.
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.  相似文献   

2.
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°50S–77°31E) 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 mol 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 mol m-2 d-1, respectively.  相似文献   

3.
Simultaneous shipboard measurements of atmospheric dimethylsulfide and hydrogen sulfide were made on three cruises in the Gulf of Mexico and the Caribbean. The cruise tracks include both oligotrophic and coastal waters and the air masses sampled include both remote marine air and air masses heavily influenced by terrestrial or coastal inputs. Using samples from two north-south Caribbean transects which are thought to represent remote subtropical Atlantic air, mean concentrations of DMS and H2S were found to be 57 pptv (74 ng S m-3, =29 pptv, n=48) and 8.5 pptv (11 ng S m-3, =5.3 pptv, n=36), respectively. The ranges of measured concentrations for all samples were 0–800 pptv DMS and 0–260 pptv H2S. Elevated concentrations were found in coastal regions and over some shallow waters. Statistical analysis reveals slight nighttime maxima in the concentrations of both DMS and H2S in the remote marine atmosphere. The diurnal nature of the H2S data is only apparent after correcting the measurements for interference due to carbonyl sulfide. Calculations using the measured ratio of H2S to DMS in remote marine air suggest that the oxidation of H2S contributes only about 11% to the excess (non-seasalt) sulfate in the marine boundary layer.  相似文献   

4.
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%.  相似文献   

5.
A global three-dimensional model of the tropospheric sulfur cycle   总被引：9，自引：0，他引：9  
The tropospheric part of the atmospheric sulfur cycle has been simulated in a global three-dimensional model. The model treats the emission, transport, chemistry, and removal processes for three sulfur components; DMS (dimethyl sulfide), SO2 and SO4 2– (sulfate). These processes are resolved using an Eulerian transport model, the MOGUNTIA model, with a horizontal resolution of 10° longitude by 10° latitude and with 10 layers in the vertical between the surface and 100 hPa. Advection takes place by climatological monthly mean winds. Transport processes occurring on smaller space and time scales are parameterized as eddy diffusion except for transport in deep convective clouds which is treated separately. The simulations are broadly consistent with observations of concentrations in air and precipitation in and over polluted regions in Europe and North America. Oxidation of DMS by OH radicals together with a global emission of 16 Tg DMS-S yr–1 from the oceans result in DMS concentrations consistent with observations in the marine boundary layer. The average turn-over times were estimated to be 3, 1.2–1.8, and 3.2–6.1 days for DMS, SO2, and SO4 2– respectively.  相似文献   

6.
DMS emissions and fluxes from the Australasian sector of the Antarctic and Subantarctic Oceans, bound by 46–68° S and 65.5–142.6° E, were determined from a limited number of samples (n=32) collected during three summer resupply voyages to Australian Antarctic continental research bases between November 1988 and January 1989 (a 92 day period). The maximum DMS emission from this sector of the Antarctic Ocean was in an area near the Antarctic Divergence (60–63° S) and the minimum DMS emission was from the Antarctic coastal and offshelf waters. The greatest emission of DMS from this sector of the Southern Ocean was from the Subantarctic waters. DMS flux from the Australasian Antarctic Ocean was 64.3×106 (±115) mol d–1 or 5.9 (±10.6)×109 mol based on an emission of 10.9 (±19.5) µmol m–2 d–1 (n=26). The flux of DMS from the Australasian sector of the Subantarctic Ocean was probably twice the flux of DMS from the adjacent Antarctic Ocean.  相似文献   

7.
Dimethylsulfide (DMS) in surface seawater and the air, methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2–) in aerosol, and radon-222 (Rn-222) were measured in the northern North Pacific, including the Bering Sea, during summer (13 July – 6 September 1997). The mean atmospheric DMS concentrations in the eastern region (21.0 ± 5.8 nmole/m3 (mean ± S.D.), n=30) and Bering Sea (19.9 ± 9.8 nmole/m3, n=10) were higher than that in the western region (11.1 ± 6.4 nmole/m3, n=31) (p<0.05), although these regions did not significantly differ in the mean DMS concentration in surface seawater. Mean sea-to-air DMS flux in the eastern region (21.0 ± 10.4 mole/m2/day, n=19) was larger than those in the western region (11.3 ± 16.9 mole /m2/day, n=22) and Bering Sea (11.2 ± 7.8 mole/m2/day, n=7) (p<0.05). This suggests that the longitudinal difference in atmospheric DMS was produced by that in DMS flux owing to wind speed, while the possible causes of the higher DMS concentrations in the Bering Sea include (1) later DMS oxidation rates, (2) lower heights of the marine boundary layer, and (3) more inactive convection. The mean MSA concentrations in the eastern region (1.18 ± 0.84 nmole/m3, n=35) and Bering Sea (1.17 ± 0.87 nmole/m3, n=13) were higher than that in the western region (0.49 ± 0.25 nmole/m3, n=28) (p < 0.05). Thus the distribution of MSA was similar to that of DMS, while the nss-SO4 2– concentrations were higher near the continent. This suggests that nss-SO4 2– concentrations were regionally influenced by anthropogenic sulfur input, because the distribution of nss-SO4 2– was similar to that of Rn-222 used as a tracer of continental air masses.  相似文献   

8.
A one-month experiment was performed at Amsterdam Island in January 1998, to investigate the factors controlling the short-term variations of atmospheric dimethylsulfide (DMS) and its oxidation products in the mid-latitudes remote marine atmosphere. High mixing ratios of DMS, sulfur dioxide (SO2) and dimethylsulfoxide (DMSO) have been observed during this experiment, with mean concentrations of 395 parts per trillion by volume (pptv) (standard deviation, = 285, n = 500), 114 pptv ( = 125, n = 12) and 3 pptv ( = 1.2, n = 167), respectively. Wind speed and direction were identified as the major factors controlling atmospheric DMS levels. Changes in air temperature/air masses origin were found to strongly influence the dimethylsulfoxide (DMSO)/DMS and SO2/DMS molar ratios, in line with recent laboratory data. Methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2–) mean concentrations in aerosols during this experiment were 12.2± 6.5 pptv (1, n=47) and 59 ± 33 pptv (1, n=47), respectively. Evidence of vertical entrainment was reported following frontal passages, with injection of moisture-poor, ozone-rich air. High MSA/ nss-SO4 2– molar ratios (mean 0.44) were calculated during these events. Finally following frontal passages, few spots in condensation nuclei (CN) concentration were also observed.  相似文献   

9.
A box model, involving simple heterogeneous reaction processes associated with the production of non-sea-salt sulfate (nss-SO 4 2– ) particles, is used to investigate the oxidation processes of dimethylsulfide (DMS or CH3SCH3) in the marine atmosphere. The model is applied to chemical reactions in the atmospheric surface mixing layer, at intervals of 15 degrees latitude between 60° N and 60° S. Given that the addition reaction of the hydroxyl radical (OH) to the sulfur atom in the DMS molecule is faster at lower temperature than at higher temperature and that it is the predominant pathway for the production of methanesulfonic acid (MSA or CH3SO3H), the results can well explain both the increasing tendency of the molar ratio of MSA to nss-SO 4 2– toward higher latitudes and the uniform distribution with latitude of sulfur dioxide (SO2). The predicted production rate of MSA increases with increasing latitude due to the elevated rate constant of the addition reaction at lower temperature. Since latitudinal distributions of OH concentration and DMS reaction rate with OH are opposite, a uniform production rate of SO2 is realized over the globe. The primary sink of DMS in unpolluted air is caused by the reaction with OH. Reaction of DMS with the nitrate radical (NO3) also reduces DMS concentration but it is less important compared with that of OH. Concentrations of SO2, MSA, and nss-SO 4 2– are almost independent of NO x concentration and radiation field. If dimethylsulfoxide (DMSO or CH3S(O)CH3) is produced by the addition reaction and further converted to sulfuric acid (H2SO4) in an aqueous solution of cloud droplets, the oxidation process of DMSO might be important for the production of aerosol particles containing nss-SO 4 2– at high latitudes.  相似文献   

10.
During a cruise of RV Polarstern over the Atlantic in September/October 1988, C2–C4 hydrocarbons were measured in surface sea water. The ship passed through three different ocean regions divided by divergences at 8° N and 3° S. Hydrocarbon concentrations differed considerably in these regions. The highest values were obtained for ethene with mean concentrations of 246 pMol/l between 35° N and 8° N, 165 pMol/l between 8° N and 3° S, and 63 pMol/l between 3° S and 30° S. Low values were found for i- and n-butane and acetylene between 32 pMol/l and 1 pMol/l. The alkene concentrations were in general higher than the concentrations of their saturated homologs. Concentrations decreased with increasing carbon numbers. The various alkenes were well correlated with one another as were the various alkanes. Oceanic emission rates of the light hydrocarbons were calculated from their sea water concentrations using an ocean atmosphere exchange model. The averaged fluxes ranged from about 108 molec cm-2 s-1 for the alkenes and ethane to less than 107 molec cm-2 s-1 for the C4 alkanes. Acetylene emissions were below 3×106 molec cm-2 s-1. Based upon these rates budget estimates of NMHC in the ocean surface layer were made with a simple model considering production and destruction processes in the water. The emissions to the atmosphere appear to be the dominant loss process between 35° N and 8° N, whereas destruction in the water seems to be dominant in the latitude ranges 8° N-3° S and 3° S-30° S.  相似文献   

11.
C2-C6 Nonmethane hydrocarbon (NMHC) concentrations in the atmospheric boundary layer and in surface seawater were simultaneously measured during an oceanographic cruise in the intertropical Indian Ocean. NMHC were found to be mainly C2-C4 alkenes and C2-C3 alkanes. Their concentrations ranged from 1 to 30×10–9 l/l in the seawater and 0.1 to 15 ppbv in the atmosphere. Seawater appeared to be a source because the C2-C6 NMHC were supersaturated with respect to the atmosphere by 2 or 3 orders of magnitude.After a selection of the pure marine atmospheric samples, performed with the help of stable and radioactive continental tracers, we found an identical composition in NMHC of surface air and seawater. This observation enabled us to establish that the gas transfer between sea and air occurred according to nonsteady state processes, and that the fluxes cannot be deduced only from atmospheric measurements. An order of magnitude value of the oceanic source for the different NMHC is however derived from the comparison of their sea water concentrations to that of propane and an independent evluation of the marine source of this last compound.  相似文献   

12.
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.  相似文献   

13.
The major components of the marine boundary layer biogeochemical sulfur cycle were measured simultaneously onshore and off the coast of Washington State, U.S.A. during May 1987. Seawater dimethylsulfide (DMS) concentrations on the continental shelf were strongly influenced by coastal upwelling. Concentration further offshore were typical of summer values (2.2 nmol/L) at this latitude. Although seawater DMS concentrations were high on the biologically productive continental shelf (2–12 nmol/L), this region had no measurable effect on atmospheric DMS concentrations. Atmospheric DMS concentrations (0.1–12 nmol/m3), however, were extremely dependent upon wind speed and boundary layer height. Although there appeared to be an appreciable input of non-sea-salt sulfate to the marine boundary layer from the free troposphere, the local flux of DMS from the ocean to the atmosphere was sufficient to balance the remainder of the sulfur budget.  相似文献   

14.
A photochemical box model is used to simulate seasonal variations in concentrations of sulfur compounds at latitude 40° S. It is assumed that the hydroxyl radical (OH) addition reaction to sulfur in the dimethyl sulfide (DMS) molecule is the predominant pathway for methanesulfonic acid (MSA) production, and that the rate constant increases as the air temperature decreases. Concentration of the nitrate radical (NO3) is a function of the DMS flux, because the reaction of DMS with NO3 is the most important loss mechanism of NO3. While the diurnally averaged concentration of OH in winter is a factor of about 8 smaller than in summer, due to the weak photolysis process, the diurnally averaged concentration of NO3 in winter is a factor of about 4–5 larger than in summer, due to the decrease of DMS flux. Therefore, at middle and high latitudes in winter, atmospheric DMS is mainly oxidized by the reaction with NO3. The calculated ratio of the MSA to SO2 production rates is smaller in winter than in summer, and the MSA to non-sea-salt sulfate (nssSO4 2-) molar ratio varies seasonally. This result agrees with data on the seasonal variation of the MSA/nssSO4 2- molar ratio obtained at middle and high latitudes. The calculations indicate that during winter the reaction of DMS with NO3 is likely to be a more important sink of NOx (NO+NO2) than the reaction of NO2 with OH, and to serve as a significant pathway of the HNO3 production. If dimethyl sulfoxide (DMSO) is produced through the OH addition reaction and is heterogeneously oxidized in aqueous solutions, half of the nssSO4 2- produced in summer may be through the oxidation process of DMSO. It is necessary to further investigate the oxidation products by the reaction of DMS with OH, and the possibility of the reaction of DMS with NO3 during winter.  相似文献   

15.
Measurements of atmospheric dimethylsulfide (DMS) and its oxidation products, sulfur dioxide (SO2), methanesulfonic acid (MSA) and non-sea-salt sulfate (nss-SO4 2-) 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-SO4 2- (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-SO4 2- 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.  相似文献   

16.
Simultaneous measurements of rain acidity and dimethyl sulfide (DMS) at the ocean surface and in the atmosphere were performed at Amsterdam Island over a 4 year period. During the last 2 years, measurements of sulfur dioxide (SO2) in the atmosphere and of methane sulfonic acid (MSA) and non-sea-salt-sulfate (nss-SO4 2-) in rainwater were also performed. Covariations are observed between the oceanic and atmospheric DMS concentrations, atmospheric SO2 concentrations, wet deposition of MSA, nss-SO4 2-, and rain acidity. A comparable summer to winter ratio of DMS and SO2 in the atmosphere and MSA in precipitation were also observed. From the chemical composition of precipitation we estimate that DMS oxidation products contribute approximately 40% of the rain acidity. If we consider the acidity in excess, then DMS oxidation products contribute about 55%.  相似文献   

17.
Measurements of Hg (total gas-phase, precipitation-phase andparticulate-phase), aerosol mass, particulate 210Pb and7Be and precipitation 210Pb were made at an atmosphericcollection station located in a near remote area of northcentral Wisconsin,U.S.A. (46°10N, 89°50W) during the summers of 1993, 1994and 1995. Total Hg and 210Pb were observed to correlate strongly(slope = 0.06 ± 0.03 ng mBq-1; r 2 =0.72) in rainwater. Mercury to 210Pb ratios in particulate matter(0.03 ± 0.02 ng mBq-1; r 2 = 0.06) wereconsistent with the ratio in rain. Enrichment of the Hg/mass ratio (approx.5–50×) relative to soil and primary pollutant aerosols indicatedthat gas-to-particle conversion had taken place during transport. Comparisonof these results with models for the incorporation of Hg into precipitationindicates that atmospheric particles deliver more Hg to precipitation than canbe explained by the presence of soot. A lack of correlation between totalgas-phase Hg (TGM) and a 7Be/210Pb function suggests novertical concentration gradient within the troposphere, and allows an estimateof TGM residence time of 1.5 ± 0.6 yr be made based on surface airsamples.  相似文献   

18.
The daytime boundary-layer heating process and the air-land heat budget were investigated over the coastal sea-breeze region by means of observations over the Sendai plain in Japan during the summer. In this area, the onset of the sea breeze begins at the coast around 0900 LST, intruding about 35 km inland by late afternoon. The cold sea breeze creates a temperature difference of over 10°C between the coastal and inland areas in the afternoon. On the other hand, warm air advection due to the combination of the counter-sea breeze and land-to-sea synoptic wind occurs in the layer above the cold sea breeze in the coastal region. Owing to this local warm air advection, there is no significant difference in the daytime heating rate over the entire atmospheric boundary layer between the coastal and inland areas. The sensible heat flux from the land surface gradually decreases as distance from the coastline increases, being mainly attributed to the cold sea breeze. The daytime mean cold air advection due to the sea breeze is estimated asQ adv local =–29 W m–2 averaged over the sea breeze region (035 km from the coastline). This value is 17% of the surface sensible heat fluxH over the same region. The results of a two-dimensional numerical model show that the value ofQ adv local /H is strongly affected by the upper-level synoptic wind direction. The absolute value ofQ adv local /H becomes smaller when the synoptic wind has the opposite direction of the sea breeze. This condition occurred during the observations used in the present study.  相似文献   

19.
Low-level temperature inversions are a common feature of the wintertime troposphere in the Arctic and Antarctic. Inversion strength plays an important role in regulating atmospheric processes including air pollution, ozone destruction, cloud formation, and negative longwave feedback mechanisms that shape polar climate response to anthropogenic forcing. The Atmospheric Infrared Sounder (AIRS) instrument provides reliable measures of spatial patterns in mean wintertime inversion strength when compared with available radiosonde observations and reanalysis products. Here, we examine the influence of sea ice concentration on inversion strength in the Arctic and Antarctic. Correlation of inversion strength with mean annual sea ice concentration, likely a surrogate for the effective thermal conductivity of the wintertime ice pack, yields strong, linear relationships in the Arctic (r?=?0.88) and Antarctic (r?=?0.86). We find a substantially greater (stronger) linear relationship between sea ice concentration and surface air temperature than with temperature at 850?hPa, lending credence to the idea that sea ice controls inversion strength through modulation of surface heat fluxes. As such, declines in sea ice in either hemisphere may imply weaker mean inversions in the future. Comparison of mean inversion strength in AIRS and global climate models (GCMs) suggests that many GCMs poorly characterize mean inversion strength at high latitudes.  相似文献   

20.
Measurements of various sulphur gases in a coastal marine environment   总被引：4，自引：0，他引：4  
Measurements of several sulphur gases have been made in coastal seawaters (including microlayers) and marine air off Great Yarmouth, U.K., and in a freshwater lake. The results show dimethyl sulphide to be the dominant sulphur gas in all the waters examined, with lesser amounts of carbonyl sulphide and carbon disulphide. For the marine air and water samples carbonyl sulphide showed no significant seasonal variation in concentration. The seawater was always supersaturated with respect to the carbonyl sulphide concentration in the air; the mean saturation value being 4.6. Likewise the seawater was always supersaturated with dimethyl sulphide, but for this gas the concentrations in the water showed substantial seasonal variation (× 40), with a maximum value of about 500 ng(S) l-1 in late June, approximately contemporaneous with the second plankton bloom in the region.Sea surface microlayers harvested cryogenically showed a mean enrichment of 2.4 relative to subsurface water for carbonyl sulphide. Some part of the observed microlayer enrichment for this gas may be due to freezing-on of atmospheric carbonyl sulphide onto the frozen microlayer sample. In general, microlayer samples did not exhibit a significant enrichment for dimethyl sulphide. However, under conditions of high biological production, enrichments of several-fold were found, but may be attributable, at least in part, to biological production of dimethyl sulphide in the microlayer water in the period between collection and analysis.  相似文献   

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