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1.
Individual bacterial cells occur in many samples that were collected at Cape Grim, Tasmania and during the Lagrangian “B” experiment of the Aerosol Characterization Experiment 1 (ACE-1) campaign that was conducted above the Southern Ocean. They are present in samples from altitudes as high as 5.4 km. Morphologically, almost all bacteria are rod-shaped, about 1 μm long or smaller, have one polar flagellum, and contain inclusions that are rich in P and K. Their morphological features suggest that these bacteria are motile, marine species. It seems likely that the cells became airborne by the same bubble-bursting mechanism that ejects sea-salt aerosol particles into the atmosphere; however, the bacteria and sea-salt particles are typically not aggregated with one another. The estimated number ratio of bacteria and the dominant aerosol species, sea salt, varies in the samples and averages about 1%. The aerosol bacteria seem to represent an important atmospheric reservoir of P and organic compounds; on the other hand, since they are externally mixed with sea salt, they are unlikely to be effective as cloud condensation nuclei.  相似文献   

2.
High-volume aerosol filters, exposed in maritime air masses at Cape Grim since late 1976, were analysed for excess sulfate (not of seasalt origin) and methanesulfonate. The mean concentrations (standard errors) of 2.80(0.59) and 0.176(0.027) nmole/m3 respectively are about half those reported in a recent study of aerosol samples from various locations in the Atlantic and Pacific oceans.Methanesulfonate concentration varied seasonally by at least an order of magnitude with a summer maximum and winter minimum. No comparable cycle was found for excess sulfate.  相似文献   

3.
Aerosol samples were collected in the Atlantic marine boundary layer between the English Channel and Antarctica during November–December 1999. The composition of coarse (aerodynamic diameter 1–3 μm) individual aerosol particles was studied using the SEM/EDX method. The major particle types observed were fresh sea salt, sea-salt particles reacted partly or totally with sulphuric acid or nitric acid, Mg-sulphate, Ca-sulphate, mixed aluminosilicates and sea salt, aluminosilicates, Ca-rich particles and Fe-rich particles. The relative fractions of sea-salt particles with moderate or strong Cl depletion were high near the coasts of Europe (65–74%) and Northern Africa (44–87%), low far from the coast of Western Africa (10–20%) and very low in remote sea areas between Africa and Antarctica (1%). The Cl depletion was strongest when air masses arrived from the direction of anthropogenic pollution sources. The fractions of Mg-sulphate particles were high (18–25%) in 2 samples near Europe. The Mg-sulphate particles were probably formed as a result of fractional recrystallization of sea-salt particles in which Cl was substituted by sulphate. It remained unclear whether these particles were formed in the atmosphere or during and after sampling. The relative fractions of particles from continental sources were quite low (10–15%) near Europe, very high (25–78%) near the coast of Northwestern Africa and very low in the remote sea areas (0–2%). Most of the continental particles were aluminosilicates and some of them were internally mixed with sea salt. Near the coast of Northwestern Africa, the main source of aluminosilicates was Saharan dust, and near the Gulf of Guinea, emissions from biomass burning were also mixed with aluminosilicates and sea salt.  相似文献   

4.
There are large uncertainties in identifying and quantifying the natural and anthropogenic sources of chloromethanes – methyl chloride (CH3Cl), chloroform (CHCl3) and dichloromethane (CH2Cl2), which are responsible for about 15% of the total chlorine in the stratosphere. We report two years of in situ observations of these species from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41° S, 145° E). The average background levels of CH3Cl, CHCl3 and CH2Cl2 during 1998–2000 were 551± 8, 6.3± 0.2 and 8.9± 0.2 ppt (dry air mole fractions expressed in parts per 1012) respectively, with a two-year average amplitude of the seasonal cycles in background air of 25, 1.1 and 1.5 ppt respectively. The CH3Cl and CHCl3 records at Cape Grim show clear episodes of elevated mixing ratios up to 1300 ppt and 55 ppt respectively, which are highly correlated, suggesting common source(s). Trajectory analyses show that the sources of CH3Cl and CHCl3 that are responsible for these elevated observations are located in coastal-terrestrial and/or coastal-seawater regions in Tasmania and the south-eastern Australian mainland. Elevated levels of CH2Cl2 (up to 70 ppt above background) are associated mainly with emissions from the Melbourne/Port Phillip region, a large urban/industrial complex (population 3.5 million) 300 km north of Cape Grim.Now at the Centre for Atmospheric ChemistryNow at School of Environmental Sciences  相似文献   

5.
There are large uncertainties in identifying and quantifying the globally significant sources and sinks of methyl bromide (CH3Br) and methyl iodide (CH3I). Long-term, quasi-continuous observations can provide valuable information about their regional sources, which may be significant in the global context. We report 3 years of in situobservations of these trace gases from the AGAGE (Advanced Global Atmospheric Gas Experiment) program at Cape Grim, Tasmania (41 °S, 145 °E). The average background levels of CH3Br and CH3I during March 1998–March 2001 were 8.05 and 1.39 ppt (dry air mole fractions expressed in parts per 1012), respectively. The CH3Br background data showed little seasonal variability. Trajectory analyses reveal that air masses showing elevated CH3Br levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater and/or urban source regions. The CH3I background data showed a seasonal cycle with a 3-year average amplitude of 0.47 ppt and maximum concentrations in summer, suggesting that the Southern Ocean is a significant source.Trajectory analyses reveal that air masses showing highly elevated CH3I levels at Cape Grim have had significant contact with coastal-terrestrial and/or coastal-seawater regions and/or the open-ocean regions of Bass Strait and the Tasman Sea.  相似文献   

6.
Atmospheric mixing ratios of methyl iodide (CH3I) and other methyl halides have been measured at Cape Grim, Tasmania (41°S, 145°E), since early 1998 as part of the Advanced Global Atmospheric Gases Experiment (AGAGE). This paper analyses about 1700 ambient air CH3I measurements from the 14-month period (March 1998–April 1999). Mixing ratios peaked during the summer, despite faster photolytic loss, suggesting local oceanic emissions were about 2.2–3.6 times stronger in summer than in winter. Back trajectories show that CH3I levels are strongly dependent on air mass origin, with highest mixing ratios in air from the Tasman Sea/Bass Strait region and lowest levels in air originating from the Southern Ocean at higher latitudes. CH3I mixing ratios were not well correlated with other methyl halides in unpolluted marine air. The large variations with season and air mass origin suggest that high frequency, continuous data from key locations will make a significant contribution to the understanding of sources and sinks of this important short-lived atmospheric species.  相似文献   

7.
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   

8.
The concentration of gas-phase peroxides has been measured almost continuously at the Cape Grim baseline station (41° S) over a period of 393 days (7702 h of on-line measurements) between February 1991 and March 1992. In unpolluted marine air a distinct seasonal cycle in concentration was evident, from a monthly mean value of>1.4 ppbv in summer (December) to <0.2 ppbv in winter (July). In the summer months a distinct diurnal cycle in peroxides was also observed in clean marine air, with a daytime build-up in concentration and decay overnight. Both the seasonal and diurnal cycles of peroxides concentration were anticorrelated with ozone concentration, and were largely explicable using a simple photochemical box model of the marine boundary layer in which the central processes were daytime photolytic destruction of ozone, transfer of reactive oxygen into the peroxides under the low-NOx ambient conditions that favour self-reaction between peroxy radicals, and continuous heterogeneous removal of peroxides at the ocean surface. Additional factors affecting peroxides concentrations at intermediate timescales (days to a week) were a dependence on air mass origin, with air masses arriving at Cape Grim from higher latitudes having lower peroxides concentrations, a dependence on local wind speed, with higher peroxides concentrations at lower wind speeds, and a systematic decrease in peroxides concentration during periods of rainfall. Possible physical mechanisms for these synoptic scale dependencies are discussed.  相似文献   

9.
Nitrous oxide (N2O) fluxes for south-easternAustralia have been estimated using a combination ofthe in situ N2O and radon (Rn) measurementsmade at the Cape Grim Baseline Air Pollution Station,in north-west Tasmania. The average N2O fluxesfrom the south-eastern mainland of Australia and fromTasmania over the nine years of record analysed (1985–1993) have beenfound to be 130 ± 30 kgN km-2yr-1 and 160 ± 45 kgN km-2yr-1respectively. These fluxes are larger than expectedand a significant dependence of the flux on rainfallis observed, with greater fluxes in the spring (October–December) andduring periods of positive SouthernOscillation Index. A large flux (1,300 ± 500kgN km-2 yr-1) from a nearby island (KingIsland) was also estimated from the data record,indicating a strong source, although the small size ofthe island means that it is not a significant sourcefor Australia.  相似文献   

10.
The sub-monthly evolution of the interannual variations of absorbing aerosols and related hydrometeorology over South Asia in the pre-monsoon period is investigated from the analysis of pentad-resolution observational datasets.It is shown that pre-monsoon (late April–early May) variations are characterized by increased aerosols, reduced cloudiness and precipitation, and increased downward shortwave radiation. Lead-lag regressions indicate the significant influence of synoptic scale advection (and related vertical motion) in simultaneously shaping the aerosol distribution and associated significant hydroclimate (precipitation, cloudiness, surface shortwave radiation, and 2-m air temperature) over the Indo-Gangetic Plain.The above findings can be interpreted as a manifestation of the aerosol “semi-direct” effect if one is not mindful of the prevailing circulation anomalies and their concurrent impact on aerosol and hydroclimate. The complex interplay among aerosols, dynamics and precipitation also shows the challenge of extracting the aerosol impact from an observational analysis. Finally, the analysis points to the pitfalls of a columnar, circulation-blind framework in investigating aerosol–monsoon interactions, a concern of relevance in analyses of the impact of long-term aerosol trends, as well.  相似文献   

11.
Measurements of the stable carbon isotope ratio in atmospheric CO2 permit a distinction between variations resulting from biospheric and oceanic exchange. In situ extraction of CO2 from Cape Grim air (41°S) for isotopic analysis commenced in 1977; however difficulties with technique reliability were experienced until 1982. Since 1982, 2.6 years of relatively consistent values have accumulated.For a preliminary assessment of the latter data, estimates of the isotopic behaviour from the global transport and inter-reservoir exchange model of Pearman and Hyson (1985) have been employed. The assessment demonstrates the precision requirements of a carbon isotope monitoring program and the relevance of the isotope measurements as a constraint on parameterization of the model.Clear evidence of the changes due to fossil fuel combustion is seen in the year-to-year differences in 13C, with the mean and standard error of the overall trend being –0.025±0.005 yr-1. A significant seasonal variation in 13C is apparent, despite considerable inter-annual variability possibly associated with the 1982/83 ENSO phenomena. The average peak-to-peak amplitude is 0.055±0.014 with a maximum on day 85±15 (approx. 26 March).There is some evidence for a complex seasonal inter-relationship between concentration and isotope ratio, both in the Cape Grim data and in Mook et al. (1983) South Pole data, but with marked differences between the stations, and with both different from the model estimates.In particular, the Cape Grim results suggest that exchange with Southern Hemisphere biosphere is the main contributor to the seasonal variation in isotope ratio at this latitude.  相似文献   

12.
Results of more than 800 new measurements of methane (CH4) concentrations in the Southern Hemisphere troposphere (34–41° S, 130–150° E) are reported. These were obtained between September 1980 and March 1983 from the surface at Cape Grim, Tasmania, through the middle (3.5–5.5 km) to the upper troposphere (7–10 km). The concentration of CH4 increased throughout the entire troposphere over the measurement period, adding further support to the view that CH4 concentrations are currently increasing on a global scale. For data averaged vertically through the troposphere the rate of increase found was 20 ppbv/yr or 1.3%/yr at December 1981. In the surface CH4 data a seasonal cycle with a peak to peak amplitude of approximately 28 ppbv is seen, with the minimum concentration occurring in March and the maximum in September–October. A cycle with the same phase as that seen at the surface, but with a significantly decreased amplitude, is apparent in the mid troposphere but no cycle is detected in the upper tropospheric data. The phase and amplitude of the cycle are qualitatively in agreement with the concept that the major sink for methane is oxidation by hydroxyl radicals. Also presented is evidence of a positive vertical gradient in methane, with a suggestion that the magnitude of this gradient has changed over the period of measurements.  相似文献   

13.
Mid-latitude winter atmospheric variability in the South Indian Ocean and southwest Pacific Ocean regions of the circum-Antarctic are reconstructed using sea-salt aerosol concentrations measured in the high resolution Law Dome (DSS) ice core from East Antarctica. The sea-salt aerosol concentration data, as sodium (Na), were measured at approximately monthly resolution spanning the past 700 years. Analyses of covariations between Na concentrations in Law Dome ice, and mean sea-level pressure (MSLP) and wind field data were conducted to define the mid-latitude and sub-Antarctic atmospheric circulation patterns associated with variations in Na delivery. High Na concentrations in Law Dome snow are associated with increased meridional aerosol transport from mid-latitude sources. The seasonal average Na concentration for early winter (May, June, July (MJJ)) is strongly correlated to the mid-latitude MSLP field in the South Indian and southwest Pacific Oceans, and southern Australian regions. In addition, the average MJJ Na concentrations display a strong association with the stationary Rossby wave number 3 circulation, and are anti-correlated to the Southern Annular Mode (SAM) index of climate variability: high (low) Na concentrations occurring during negative (positive) SAM phases. This observed relationship is used to derive a proxy record for early-winter MSLP anomalies and the SAM in the South Indian and southwest Pacific Ocean regions over the period 1300–1995 AD. The proxy SAM index from 1300 to 1995 AD shows pronounced decadal-scale variability throughout. The period after 1500 AD is marked by a tendency toward slower variations and a weakly-positive mean SAM (enhanced westerlies in the 50° to 65°S zone) compared to the early part of the record.  相似文献   

14.
Characterizations of urban and regional sources of particulate matter (PM) were performed in the Milan area (North of Italy) during Föhn and stagnant (non-Föhn) conditions. The measurements were performed at two different places: in an urban area North of Milan (Bresso) and in a regional area at the EMEP-GAW station in Ispra (about 65 km NW from Milan) during the winter periods of the years 2002–2007. Particle size distributions and chemical bulk analysis of aerosols are combined with single particle mass spectrometry to obtain information about the chemical content of the particles and their mixing state. Föhn conditions are characterized by extremely clean background air from which background aerosol is scavenged, and consequently local sources (here defined as sources between the sampling sites and the mountain range top about 100–150 km away depending on the wind direction) determine the aerosol properties.It was observed that during Föhn events the accumulation mode in the size range 50 nm < d < 300 nm practically disappears and that the size fraction below 50 nm dominates the total number distribution. The significant change in the number size distribution and the large decrease in PM10 mass during Föhn events are accompanied by a significant change in the chemical composition of the particles. Results from bulk chemical analysis showed high amounts of carbonaceous compounds and very low concentrations of ammonium nitrate (as indicator for secondary chemistry) during Föhn episodes, in contrast to stagnant conditions, when secondary components are dominating the aerosol composition. Single particle measurements confirm the high contribution of carbonaceous compounds in locally emitted particles.It was concluded that particles that originated in the urban area come mainly from combustion processes, especially direct traffic emissions, domestic heating and industrial activities, whereas the regionally emitted particles are different with much less traffic contribution.We estimate that under prevailing (non-Föhn) winter conditions, about 50–65% of the aerosol mass load in the city of Milan are caused by local emissions, and about 35–50% come from regional background. This finding suggests that in order to improve air quality in a big city like Milan, it is important to combine local traffic restriction interventions with other long-term regional scale air-quality-measures.  相似文献   

15.
The microphysical structure, chemical composition and prehistory of aerosol are related to the aerosol optical properties and radiative effect in the UV spectral range. The aim of this work is the statistical mapping of typical aerosol scenarios and adjustment of regional aerosol parameters. The investigation is based on the in situ measurements in Preila (55.55° N, 21.00° E), Lithuania, and the AERONET data from the Gustav Dalen Tower (58 N, 17 E), Sweden.Clustering of multiple characteristics enabled to distinguish three aerosol types for clear-sky periods: 1) clean maritime–continental aerosol; 2) moderately polluted maritime–continental aerosol; 3) polluted continental aerosol. Differences between these types are due to significant differences in aerosol number and volume concentration, effective radius of volume distribution, content of SO4− ions and Black Carbon, as well as different vertical profiles of atmospheric relative humidity. The UV extinction, aerosol optical depth (AOD) and the Ångstrom coefficient α increased with the increasing pollution. The value α = 1.96 was observed in the polluted continental aerosol that has passed over central and eastern Europe and southern Russia. Reduction of the clear-sky UV index against the aerosol-free atmosphere was of 4.5%, 27% and 41% for the aerosol types 1, 2 and 3, respectively.  相似文献   

16.
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.  相似文献   

17.
Individual aerosol particles collected in the Negev desert in Israel during a summer and winter campaign in 1996–1997 were analysed by scanning electron microscopy with energy-dispersive X-ray analysis. Hierarchical cluster analysis was performed to interpret the data on the basis of particle diameter and composition. Eleven particle classes (groups) provided clues on sources and/or particle formation. The summer samples were enriched in sulphates and mineral dusts; the winter samples contained more sea salts, aged sea salts, and industrial particles. The fine size fraction below 1 m diameter was enriched in secondary particles and showed evidence of atmospheric processing. The secondary sulphate particles were mainly attributed to long-range transport. A regional conversion from calcite to calcium sulphate occurred during summer. Industrial particles originating from local pollution appeared during winter.  相似文献   

18.
Cloud droplet chemistry is modelled for the first 150 m of rise in a wintertime, mid-latitude, marine stratus cloud using observations made at and near the Cape Grim Baseline Station as a source of input parameters. The emphasis in this work was to study the variation in droplet chemistry as a function of both droplet size and nucleus composition, with a particular focus on the way in which oxidation of dissolved sulfur dioxide varied.At 150 m above the condensation level, solute concentration as a function of droplet size was found to increase by as much as 2 to 3 orders of magnitude for only a factor of 2 increase in droplet radius, primarily as a consequence of the 1/r dependence in the droplet growth equation. This type of size dependence exists at all levels in the model cloud, and has a significant influence on oxidation rate of sulfur dioxide in droplets growing on sulfate nuclei, oxidation by ozone being favoured in the smallest droplets, but oxidation by hydrogen peroxide being favoured in the larger droplets. Oxidation by ozone is favoured at all sizes in droplets formed on sea-salt nuclei as a result of the initially high alkalinity of these droplets, and in the cloud overall is calculated to be the more important oxidation pathway. Although based on a simplified chemical scheme, these results suggest that both size-dependent and nucleus-dependent chemistry of cloud droplets may need to be considered explicitly in cloud modelling work.Volume-weighted mean pH values in the range 5 to 6 were predicted from sensitivity studies in which input variables were varied over reasonable ranges, in agreement with two sets of bulk cloud-water pH data obtained by aircraft near Cape Grim.  相似文献   

19.
The potential resources on the ion-stimulated syntheses effects of aerosol particles of lower troposphere in test sites in the arctic, mountain, arid and forest areas as the function of irradiation time and gas-precursor concentration were experimentally and theoretically evaluated. The dust-free outdoor air was irradiated with an ionization current of 10− 6 A by α-rays from isotope 239Pu. The total output of radiolytic aerosols (RA) with a diameter of 3–1000 nm was found to be 0.05–0.1 molecules per 1 eV of absorbed radiation, while the physical upper limit is 0.25–0.4 molecules/eV. In an interval of exposition time from 6 to 800 s (adsorbed energy is 3 · 1012–1014 eV/cm3) the RA mass concentration at different sites was increased from 1–10 to 50–500 μg/m3. According to the liquid chromatography data the major RA material is the H2O/HNO3 solution with acid concentration  25%. The used physical model presents new aerosols as a product from small and intermediate ion association through formation of neutral clusters and describes adequately some of the peculiarities in field experiment data. Introducing SO2, NH3, and also hydrochloric, nitric and sulphuric acid vapours with concentration 0.1–1 mg/m3 in the irradiated air stimulated an increase of mass aerosol concentration by a factor of 8–30. The mean size also decreased by a factor of 3–5. These facts allowed us to expect that the chemical composition of radiolytic aerosols generated in outdoor air would noticeably differ after addition of the gas-precursors.  相似文献   

20.
In situ AGAGE GC-MS measurements of methyl bromide (CH3Br) and methyl chloride (CH3Cl) at Mace Head, Ireland and Cape Grim, Tasmania (1998–2001) reveal a complex pattern of sources. At Mace Head both gases have well-defined seasonal cycles with similar average annual decreases of 3.0% yr−1 (CH3Br) and 2.6% yr−1 (CH3Cl), and mean northern hemisphere baseline mole fractions of 10.37 ± 0.05 ppt and 535.7 ± 2.2 ppt, respectively. We have used a Lagrangian dispersion model and local meteorological data to segregate the Mace Head observations into different source regions, and interpret the results in terms of the known sources and sinks of these two key halocarbons. At Cape Grim CH3Br and CH3Cl also show annual decreases in their baseline mixing ratios of 2.5% yr−1 and 1.5% yr−1, respectively. Mean baseline mole fractions were 7.94 ± 0.03 ppt (CH3Br) and 541.3 ± 1.1 ppt (CH3Cl). Although CH3Cl has astrong seasonal cycle there is no well-defined seasonal cycle in the Cape Grim CH3Br record. The fact that both gases are steadily decreasing in the atmosphere at both locations implies that a change has occurred which is affecting a common, major source of both gases (possibly biomass burning) and/or their major sink process (destruction by hydroxyl radical).  相似文献   

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