Correlations among combustion effluent species at Barrow,Alaska: Aerosol black carbon,carbon dioxide,and methane

As part of the second Arctic Gas and Aerosol Sampling Program (AGASP II) continuous measurements of atmospheric aerosol black carbon (BC) were made at the NOAA/GMCC observatory at Barrow, Alaska (71°19N, 156°36W) during the period March 21–April 22, 1986. Black carbon is produced only by incomplete combustion of carbonaceous materials and so is a particularly useful atmospheric indicator of anthropogenic activities. The BC data have been analyzed together with the concurrent measurements of carbon dioxide (CO₂), methane (CH₄), and condensation nuclei (CN) that are routinely made at the observatory. All four species showed elevated and highly variable concentrations due to local human activities, principally in the township of Barrow, 7 km to the southwest, and at the DEW Line radar installation 1 km to the northwest. We distinguish between those periods of the record that are affected by local activities and those that are not, on the basis of the short-term (periods of up to 1 hour) variability of the continuous CO₂ and CN records, with large short-term variabilities indicating local sources. We identified seven periods of time (events) with durations ranging from 13 to 37 hours when the BC, CO₂, and CH₄ concentrations changed smoothly over time, were highly correlated with each other, and were not influenced by local activities. These events had BC/CO₂ ratios in the range (50–103)×10^–6. These ratios are dimensionless since we convert the CO₂ concentrations to units of ng m^–3 of carbon. Such values of BC/CO₂ are characteristic of the combustion effluent from large installations burning heavy fuel oil or coal, automobiles, and domestic-scale natural gas usage. We conclude that these events are indicative of air masses that have been polluted with combustion emissions in a distant location and then transported to the Arctic. In the absence of species-selective loss mechanisms, these air masses will maintain their combustion effluent signatures during the transport. The BC/CO₂ ratios found for the local combustion activities are consistent with those expected from known combustion processes.     

Measurement of Carbon Dioxide Emissions Plumes from Prudhoe Bay, Alaska Oil Fields

Large carbon dioxide plumes with concentrations up to 45 ppm aboveambient levels were measured about 15 km downwind of the Prudhoe Bay, Alaskamajor oil production facilities, located at 70° N Lat. above the ArcticCircle. The measured emissions were 1.3 × 10³ metrictons (C) hour^-1 (11.4× 10⁶ metric tons(C) year^-1), six times greater than the combustion emissionsassumed by Jaffe and coworkers in J. Atmos. Chem. 20 (1995), 213–227,based on 1989 reported Prudhoe Bay oil facility fuel consumption data, andfour times greater than the total C emissions reported by the oil facilitiesfor the same months as the measurement time periods. Variations in theemissions were estimated by extrapolating the observed emissions at a singlealtitude for all tundra research transect flights conducted downwind of theoil fields. These 30 flights yielded an average emission rate of1.02 × 10³ metric tons (C) hour^-1 with astandard deviation of 0.33 × 10³. These quantity ofemissions are roughly equivalent to the carbon dioxide emissions of7–10 million hectares of arctic tussock tundra (Oechel and Vourlitis,Trends in Ecol. Evolution 9 (1994), 324–329).     

A model investigation of the impact of increases in anthropogenic NO x emissions between 1967 and 1980 on tropospheric ozone

Recent observations suggest that the abundance of ozone between 2 and 8 km in the Northern Hemisphere mid-latitudes has increased by about 12% during the period from 1970 to 1981. Earlier estimates were somewhat more conservative suggesting increases at the rate of 7% per decade since the start of regular observations in 1967. Previous photochemical model studies have indicated that tropospheric ozone concentrations would increase with increases in emissions of CO, CH₄ and NO _x . This paper presents an analysis of tropospheric ozone which suggests that a significant portion of its increase may be attributed to the increase in global anthropogenic NO _x emissions during this period while the contribution of CH₄ to the increase is quite small. Two statistical models are presented for estimating annual global anthropogenic emissions of NO _x and are used to derive the trend in the emissions for the years 1966–1980. These show steady increase in the emissions during this interval except for brief periods of leveling off after 1973 and 1978. The impact of this increase in emissions on ozone is estimated by calculations with a onedimensional (latitudinal) model which includes coupled tropospheric photochemistry and diffusive meridional transport. Steady-state photochemical calculations with prescribed NO _x emissions appropriate for 1966 and 1980 indicate an ozone increase of 8–11% in the Northern Hemisphere, a result which is compatible with the rise in ozone suggested by the observations.     

Nitrogen compound emission from biomass burning in tropical African savanna FOS/DECAFE 1991 experiment (Lamto,Ivory Coast)

Gaseous nitrogen compounds (NO _x , NO _y , NH₃, N₂O) were measured at ground level in smoke plumes of prescribed savanna fires in Lamto, in the southern Ivory Coast, during the FOS/DECAFE experiment in January 1991. During the flaming phase, the linear regression between [NO _x ] and [CO₂] (differences in concentration between smoke plumes and atmosheric background) results volumic emission ratio [NO _x ]/[CO₂]=1.37×10^–3 with only slight differences between heading and backing fires. Nearly 90% of the nitrogen oxides are emitted as NO. Average emission ratios of other compounds are: 1.91, 0.047, and 0.145×10^–3 for NO _y , NH₃ and N₂O, respectively. The emission ratios obtained during this field experiment are compred with corresponding values measured during former experiments with the same plant species in combustion chambers. An accurate determination of both the biomass actually burned and of the plant nitrogen content, allows an assessment of emission fluxes of N-compounds from Guinean savanna burns. Preliminary results dealing with the influence of fire on biogenic emissions from soils are also reported.     

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 (R ²=0.92,n=25) and COS and C₂H₂ (R ²=0.79,n=26) indicating a COS production during the smoldering combustion. COS/CO₂ emission factors (COS/CO₂) 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 COS/CO₂ emission factor, COS can account for only about 7% of the sulfur emitted in the atmosphere by biomass burning.     

A discharge flow mass-spectrometric study of the reaction between the NO3 radical and isoprene

The kinetics and mechanism of the reactionNO₃+CH₂=C(CH₃)–CH=CH₂productswere studied in two laboratories at 298 K in the pressure range 0.7–3 torr using the discharge-flow mass-spectrometric method. The rate constant obtained under pseudo-first-order conditions with excess of either NO₃ or isoprene was: k ₁=(7.8±0.6)×10^–13 cm³ molecule^–1 s^–1. The product analysis indicated that the primary addition of NO₃ occurred on both -bonds of the isprene molecule.     

In-situ measurements of the aerosol size distributions,physicochemistry and light absorption properties of Arctic haze

Thermal and optical techniques were used at Barrow, Alaska during AGASP II (3/20/86–4/7/86) to measure in-situ variability of major aerosol components present in Arctic Haze. The experiment provided continuous data on the concentration, size distribution and relative proportions of sulfate species and refractory aerosol for particle diameters of 0.15 to 5 m. Filter samples were also taken for determination of aerosol optical absorption due to soot (EC-elemental carbon). Although pronounced haze events were absence during this period the haze aerosol present varied in concentration between 2 and 6 g/m³ but showed little change in relative constituents. Apart from local influences, the optical data indicated a persistent fine-mode sulfate aerosol with a NH₄ ⁺/SO₄ ^– molar ratio of about 0.4 and a refractory component of somewhat less than 10% by mass. A preliminary comparison of soot estimates determined from the light absorption data with the size distributions of refractory aerosol observed independently by the optical particle counter showed good agreement during the sample period. In the absence of local pollution, values of single scatter albedo derived from light scattering and light absorption showed similar variation about the average value of 0.86 found by us during flights north of Barrow three years earlier during AGASP I.     

GREENHOUSE GASES FROM DEFORESTATION IN BRAZILIAN AMAZONIA: NET COMMITTED EMISSIONS

Deforestation in Brazilian Amazonia is a significant source of greenhouse gases today and, with almost 90% of the originally forested area still uncleared, is a very large potential source of future emissions. The 1990 rate of loss of forest (13.8 × 10³ km²/year) and cerrado savanna (approximately 5 × 10³ km²/year) was responsible for releasing approximately 261 × 10⁶ metric tons of carbon (10⁶ t C) in the form of CO2, or 274–285 × 10⁶ t of CO2-equivalent C considering IPCC 1994 global warming potentials for trace gases over a 100-year horizon. These calculations consider conversion to a landscape of agriculture, productive pasture, degraded pasture, secondary forest, and regenerated forest in the proportions corresponding to the equilibrium condition implied by current land-use patterns. Emissions are expressed as net committed emissions, or the gases released over a period of years as the carbon stock in each hectare deforested approaches a new equilibrium in the landscape that replaces the original forest. For low and high trace gas scenarios, respectively, 1990 clearing produced net committed emissions (in 10⁶ t of gas) of 957–958 for CO2, 1.10–1.42 for CH₄, 28–35 for CO, 0.06–0.16 for N₂O, 0.74–0.74 for NO_x and 0.58–1.16 for non-methane hydrocarbons.     

Measurements of trace gases emitted by Australian savanna fires during the 1990 dry season

During 18–23 July 1990, 31 smoke samples were collected from an aircraft flying at low altitudes through the plumes of tropical savanna fires in the Northern Territory, Australia. The excess (above background) mixing ratios of 17 different trace gases including CO₂, CO, CH₄, several non-methane hydrocarbons (NMHC), CH₃CHO, NO _x (– NO + NO₂), NH₃, N₂O, HCN and total unspeciated NMHC and sulphur were measured. Emissionratios relative to excess CO₂ and CO, and emissionfactors relative to the fuel carbon, nitrogen or sulphur content are determined for each measured species. The emission ratios and factors determined here for carbon-based gases, NO _x , and N₂O are in good agreement with those reported from other biomass burning studies. The ammonia data represent the first such measurements from savanna fires, and indicate that NH₃ emissions are more than half the strength of NO _x emissions. The emissions of NO _x , NH₃, N₂O and HCN together represent only 27% of the volatilised fuel N, and are primarily NO _x (16%) and NH₃ (9%). Similarly, only 56% of the volatilised fuel S is accounted for by our measurements of total unspeciated sulphur.     

Kinetics of the Gas-Phase Reactions of OH Radicals, NO3 Radicals and O3 with Three C7-Carbonyls Formed From The Atmospheric Reactions of Myrcene, Ocimene and Terpinolene

Rate constants for the gas-phase reactions of OH radicals, NO₃ radicals and O₃ with the C₇-carbonyl compounds 4-methylenehex-5-enal [CH₂=CHC(=CH₂)CH₂CH₂CHO], (3Z)- and (3E)-4-methylhexa-3,5-dienal [CH₂=CHC(CH₃)=CHCH₂CHO] and 4-methylcyclohex-3-en-1-one, which are products of the atmospheric degradations of myrcene, Z- and E-ocimene and terpinolene, respectively, have been measured at 296 ± 2 K and atmospheric pressure of air using relative rate methods. The rate constants obtained (in cm³ molecule^–1 s^–1 units) were: for 4-methylenehex-5-enal, (1.55 ± 0.15) × 10^–10, (4.75 ± 0.35) × 10^–13 and (1.46 ± 0.12) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; for (3Z)-4-methylhexa-3,5-dienal: (1.61 ± 0.35) × 10^–10, (2.17 ± 0.30) × 10^–12, and (4.13 ± 0.81) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; for (3E)-4-methylhexa-3,5-dienal: (2.52 ± 0.65) × 10^–10, (1.75 ± 0.27) × 10^–12, and (5.36 ± 0.28) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively; and for 4-methylcyclohex-3-en-1-one: (1.10 ± 0.19) × 10^–10, (1.81 ± 0.35) × 10^–12, and (6.98 ± 0.40) × 10^–17 for the OH radical, NO₃ radical and O₃ reactions, respectively. These carbonyl compounds are all reactive in the troposphere, with daytime reaction with the OH radical and nighttime reaction with the NO₃ radical being predicted to dominate as loss processes and with estimated lifetimes of about an hour or less.     

Atmospheric CO2 variations at Barrow,Alaska, 1973–1982

The first 10 years (1973–1982) of atmospheric CO₂ measurements at Barrow, Alaska, by the NOAA/GMCC program are described. The paper updates and extends the Barrow CO₂ record presented in Tellus (1982). The data are given in final form, based on recent calibrations of the Scripps Institution of Oceanography, with selected values identified as representative of large, spacescale conditions. Analyses of the data show: (1) a long-term CO₂ average increase of 1.3 ppm per year, but with large year-to-year variations in that growth rate; (2) a suggestion, not statistically significant, of a secular increase in the amplitude of the annual cycle, presumably a reflection of global-scale biospheric variability; and (3) good absolute agreement between the Barrow results and those from four neighboring high latitude sites between 50 and 82°N.     

Relations between Light Hydrocarbon, Carbon Monoxide, and Carbon Dioxide Concentrations in the Plume from the Combustion of Plant Material in a Furnace

To systematically explain relations between light hydrocarbons, CO, and CO₂ concentrations/emissions of biomassburning, we measured concentrations/emissions of carbon gases – CO,CO₂, light hydrocarbons (CH₄, C₂H₆,C₂H₄, C₂H₂, C₃H₈, C₃H₆,n-C₄H₁₀, i-C₄H₁₀, n-C₅H₁₂,i-C₅H₁₂), and THC (total hydrocarbon) – in the burning of dead plant material, mainly Imperata grass, byclosed-chamber experiments and by time-series analyses of gas concentrations in combustion plumes in relatively efficient and inefficient combustion situations. Concentrations of hydrocarbons measured were well correlated to [CO] although [C₂H₂] was exceptionally well correlated to[CO₂]. The phase diagrams (relation between [CO]/ [CO₂] and [hydrocarbon]/ [CO₂]) obtained by the time-seriesexperiments well illustrated the variation in the overall emission rates of the closed-chamber experiments. The higher rates of decrease in hydrocarbon concentration with increasing carbon number in the efficient case compared with the inefficient case probably reflected the rate of oxidation and the amount of radicals. The overall concentrations (or emissions) of C₂H₄ and C₃H₆ were higher thanthose of C₂H₆ and C₃H₈, suggesting a linkage to mechanisms in whichthe predominant path of hydrocarbon oxidation is through the degradation of alkyl radicals, which can be immediately converted into or formed from alkenes. For C₃ and C₄ species, normal-chain species hadhigher emissions than iso-chain species under lower combustion efficiency. This may be attributable to the presence of tertiary C–H bonds in iso-species,which show more reactivity in the abstraction of H than secondary C–H bonds unless the carbon number is large.     

Airborne measurements of savanna fire emissions and the regional distributio of pyrogenic pollutants over Western Africa

We measured CO₂, CO, CH₄, H₂, and NO₂ in air masses polluted by savanna fires over Côte d'Ivoire, western Africa. Elevated concentrations of these trace gases were found in fire plumes and also in extensive haze layers. Trace gas mixing ratios ranged as high as 605 ppmv for CO₂, 14.8 ppmv for CO, 2.7 ppmv for CH₄, 4.2 ppmv for H₂, and 25 ppbv for NO₂. We compare our emission ratios to those obtained in previous field and laboratory studies. The emission ratios, expressed as an average and as a range or as an average only, were: dCO/dCO₂ 5.3×10^–2 (3–18×10^–2); dCH₄/dCO 5.3×10^–2; dH₂/dCO 2.4×10^–1 and dNO₂/dCO₂ 1.8×10^–4 (1.5–2.2×10^–4). The values found match those found during similar measurements, though our results point to rather vigorous burning in the savanna of western Africa.     

Field studies of methane emission from termite nests into the atmosphere and measurements of methane uptake by tropical soils

The flux of CH₄ and CO₂ from termite nests into the atmosphere has been measured in a broad-leafed-type savannah in South Africa. Measurements were carried out on nests of species of six genera, i.e., Hodotermes, Macrotermes, Odontotermes, Trinervitermes, Cubitermes, and Amitermes. The flux rates of CH₄ relative to the flux rate of CO₂ in terms of carbon obtained for the individual species showed ratios of 2.9×10^-3, 7.0×10^-4, 6.7×10^-5, 8.7×10^-3, 2.0×10^-3 and 4.2×10^-3, respectively. Using data published on the assimulation efficiencies of termites, the flux of carbon as CH₄ accounts for 6.0×10^-5 to 2.6×10^-3 of the carbon ingested which results in a global CH₄ emission by termites of 2 to 5×10¹² g/yr. Methane is decomposed in the soil with average decomposition rates of 52 g/m²/h. The annual CH₄ consumption in the tropics and subtropics is estimated to be 21×10¹² g which exceeds the CH₄ emission rate by termites.     

Biomass burning in the tropical savannas of Ivory Coast: An overview of the field experiment Fire of Savannas (FOS/DECAFE 91)

FOS/DECAFE 91 (Fire of Savannas/Dynamique et Chimie Atmosphérique en Forêt Equatoriale) was the first multidisciplinary experiment organized in Africa to determine gas and aerosol emissions by prescribed savanna fires. The humid savanna of Lamto in Ivory Coast was chosen for its ecological characteristics representative of savannas with a high biomass density (900 g m^–2 dry matter). Moreover the vegetation and the climate of Lamto have been studied for more than twenty years. The emission ratios (X/CO₂) of the carbon compounds (CO₂, CO, NMHC, CH₄, PAH, organic acids and aerosols), nitrogen compounds (NO_x, N₂O, NH₃ and soluble aerosols) and sulfur compounds (SO₂, COS and aerosols) were experimentally determined by ground and aircraft measurements. To perform this experiment, 4 small plots (100×100 m) and 2 large areas (10×10 km) were prepared and burnt in January 1991 during the period of maximum occurrence of fires in this type of savanna. The detailed ecological study shows that the carbon content of the vegetation is constant within 1% (42 g C for 100 g of vegetal dry matter), the nitrogen content (0.29 g N for 100 g of dry matter) may vary by 10% and the sulfur content (0.05 g S/100 d.m.) by 20%. These variations of the biomass chemical content do not constitute an important factor in the variation of the gas and particle emission levels. With the emission ratios characteristic of humid savanna and flaming conditions (CO/CO₂ of 6.1% at the ground and 8% for airborne measurements), we propose a set of new emission factors, taking into account the burning efficiency which is about 80%: 74.4% of the carbon content of the savanna biomass is released to the atmosphere in the form of CO₂, 4.6% as CO, 0.2% as CH₄, 0.5% as NMHC and 0.7% as aerosols. 17.2% of the nitrogen content of the biomass is released as NO_x, 3.5% as N₂O, 0.6% as NH₃ and 0.5% as soluble aerosols.     

Trace gas measurements at the monitoring station cape point,South Africa,between 1978 and 1988

Since 1978, a measuring station has been operated at Cape Point (34°21 S, 18°29 E). In this article, results of measurements of CO, CFCl₃, CCl₄, O₃, N₂O and CH₄ are presented as monthly means and analyzed with respect to long-term trends and seasonal variations. For CO and CH₄, very similar seasonal variations have been observed, indicating strong interrelations between these two gases. For CO and O₃, no significant changes of the mean annual concentrations can be established for the observation periods of 10 and 5 years, respectively. The measurements yield a growth rate of 9.1 pptv yr^-1 for CFCl₃ (1980–1987) and 0.6 ppbv yr^-1 for N₂O (1983–1987). The concentration increases of CH₄ (10.3 ppbv yr^-1 for 1983–1987) and of CCl₄ (2.1 pptv yr^-1 for 1980–1988) are analyzed for temporal changes during the last years.Presented at the Second Conference on Baseline Observations in Atmospheric Chemistry (SABOAC II) in Melbourne, Australia, November 1988.     

Carbon dioxide and methane in the Arctic atmosphere

Fifty flask air samples were taken during April 1986 from a NOAA WP-3D Orion aircraft which flew missions across a broad region of the Arctic as part of the second Arctic Gas and Aerosol Sampling Program (AGASP II). The samples were subsequently analyzed for both carbon dioxide (CO₂) and methane (CH₄). The samples were taken in well-defined layers of Arctic haze, in the background troposphere where no haze was detected, and from near the surface to the lower stratosphere. Vertical profiles were specifically measured in the vicinity of Barrow, Alaska to enable comparisons with routine surface measurements made at the NOAA/GMCC observatory. Elevated levels of both methane and carbon dioxide were found in haze layers. For samples taken in the background troposphere we found negative vertical gradients (lower concentrations aloft) for both gases. For the entire data set (including samples collected in the haze layers) we found a strong positive correlation between the methane and carbon dioxide concentrations, with a linear regression slope of 17.5 ppb CH₄/ppm CO₂, a standard error of 0.6, and a correlation coefficient (r²) of 0.95. This correlation between the two gases seen in the aircraft samples was corroborated by in situ surface measurements of these gases made at the Barrow observatory during March and April 1986. We also find a similar relationship between methane and carbon dioxide measured concurrenty for a short period in the moderately polluted urban atmosphere of Boulder, Colorado. We suggest that the strong correlation between methane and carbon dioxide concentrations reflects a common source region for both, with subsequent long-range transport of the polluted air to the Arctic.     

Vertical distribution of dimethylsulfide,sulfur dioxide,aerosol ions,and radon over the Northeast Pacific Ocean

Dimethylsulfide (DMS), sulfur dioxide (SO₂), methanesulfonate (MSA), nonsea-salt sulfate (nss-SO₄ ^2–), sodium (Na⁺), ammonium (NH₄ ⁺), and nitrate (NO₃ ^–) were determined in samples collected by aircraft over the open ocean in postfrontal maritime air masses off the northwest coast of the United States (3–12 May 1985). Measurements of radon daughter concentrations and isentropic trajectory calculations suggested that these air masses had been over the Pacific for 4–8 days since leaving the Asian continent. The DMS and MSA profiles showed very similar structures, with typical concentrations of 0.3–1.2 and 0.25–0.31 nmol m^–3 (STP) respectively in the mixed layer, decreasing to 0.01–0.12 and 0.03–0.13 nmol m^–3 (STP) at 3.6 km. These low atmospheric DMS concentrations are consistent with low levels of DMS measured in the surface waters of the northeastern Pacific during the study period.The atmospheric SO₂ concentrations always increased with altitude from <0.16–0.25 to 0.44–1.31 nmol m^–3 (STP). The nonsea-salt sulfate (ns-SO₄ ^2–) concentrations decreased with altitude in the boundary layer and increased again in the free troposphere. These data suggest that, at least under the conditions prevailing during our flights, the production of SO₂ and nss-SO₄ ^2– from DMS oxidation was significant only within the boundary layer and that transport from Asia dominated the sulfur cycle in the free troposphere. The existence of a sea-salt inversion layer was reflected in the profiles of those aerosol components, e.g., Na⁺ and NO₃ ^–, which were predominantly present as coarse particles. Our results show that long-range transport at mid-tropospheric levels plays an important role in determining the chemical composition of the atmosphere even in apparently remote northern hemispheric regions.     

Seasonal variation of gaseous HNO3 and NH3 at a Tropical Savannah site

Gaseous nitric acid and ammonia were sampled with annular denuders at a forest savannah site from April to December 1987. The analysis of the extract was made spectrophotometrically and by a selective electrode for NO₃ ^– and NH₄ ⁺, respectively. Higher concentrations were observed during the vegetation burning period at the end of the dry season. In the studied savannah area, large soil emissions of NO occur during the rainy season, although very low concentrations of HNO₃ (0.035 ppb) and also of particulate NO₃ ^– (0.43 g m^-3) were observed; it is likely that NO_x are lost by fast vertical transport to the upper troposphere. During the nonburning period, the average concentration of NH₃ was 2.7 ppb, which is much lower than values given in the literature for the tropical America atmosphere. The concentrations of HNO₃ and NH₃ were always below the values needed to produce ammonium nitrate aerosols.     

Spatial, Temporal and Interannual Variability of Methanesulfonate and Non-Sea-Salt Sulfate in Rainwater in the Southern Indian Ocean (Amsterdam, Crozet and Kerguelen Islands)

Methanesulfonate (MS^–) and non-sea-salt sulfate (nss-SO ₄ ^2– ), two of the major oxidation products of atmospheric dimethylsulfide (DMS), have been continuously measured in rainwater at three remote islands in the Southern Indian Ocean: Amsterdam since 1991, Crozet since 1992, and Kerguelen since 1993. The annual volume weighted mean (VWM) concentrations of nss-SO ₄ ^2– in rainwater were 3.19, 3.04 and 4.57 eq l^–1 at Amsterdam, Crozet, and Kerguelen, respectively while the VWM of MS^– were 0.24, 0.15 and 0.30 eq l^–1, respectively. At all three islands, MS^– presented a well-distinguished seasonal variation with a maximum during summer whereas the seasonal variation of nss-SO ₄ ^2– was less pronounced, possibly due to the increased anthropogenic influence during the winter period. Furthermore, MS^– presented significant interannual variations, in particular at Amsterdam and Crozet, which is closely related to the sea-surface temperature (SST) anomalies). Finally, the nss-SO ₄ ^2– deposition at Crozet Island presented a decreasing interannual trend, reflecting probably reductions in sulfur emissions from Southern Africa. On the contrary no interannual tendency was observed in the nss-SO ₄ ^2– concentrations at Amsterdam Island, indicating that the biogeochemical sulfur cycle at this area is mainly influenced by biogenic emissions.