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1.
The Petryanov air filters combined into half-year sets were analyzed for the presence of 40K, 137Cs and 22Na by means of low-background gamma rays spectrometry. Each sample contains aerosols from more than 1 Mm3 of air. Samples were collected in ground level air at Kraków (Southern Poland) from 1996 to 2002. Activity concentrations of 40K are almost constant with the mean of 14.7± 4.5 Bq m–3. Activity concentrations of 137Cs, which are on the level of single Bq m– 3 show exponential decrease with effective half-life time of 7.07± 0.77 years. The cosmogenic 22Na shows a strong seasonal variation with significant different mean values activity concentration between 0.333± 0.095 Bq m–3 and 0.137± 0.045 Bq m–3, for summer and winter, respectively. Moreover, the activity ratio for two cosmogenic radionuclides: 22Na and measured previously 7Be show also changes with statistically significant seasonal differences. The lower values were found during winters. The mechanisms which might govern this ratio are discussed. The conclusion is that transport of 22Na during summer seems to be so much effective, that results in kind of relative depletion of stratosphere of this nuclide.  相似文献   

2.
Weekly bulk aerosol samples collected at Funafuti, Tuvalu (8°30S, 179°12E), American Samoa (14°15S, 170°35W), and Rarotonga (21°15S, 159°45W), from 1983 through most of 1987 have been analyzed for nitrate and other constituents. The mean nitrate concentration is about 0.11 g m–3 at each of these stations: 0.107±0.011 g m–3 at Funafuti; 0.116±0.008 at American Samoa; and 0.117±0.010 at Rarotonga. Previous measurements of mineral aerosol and trace metal concentrations at American Samoa are among the lowest ever recorded for the near-surface troposphere and indicate that this region is minimally affected by transport of soil material and pollutants from the continents. Consequently, the nitrate concentration of 0.11 g m–3 can be regarded as the natural level for the remote marine boundary layer of the tropical South Pacific Ocean. In contrast, over the tropical North Pacific which is significantly impacted by the transport of material from Asia and North America, the mean nitrate concentrations are about three times higher, 0.29 and 0.36 g m–3 at Midway and Oahu, respectively. The major sources of the nitrate over the tropical South Pacific are still very uncertain. A very significant correlation between the nitrate concentrations at American Samoa and the concentrations of 210Pb suggests that transport from continental sources might be important. This continental source could be lightning, which occurs most frequently over the tropical continents. A near-zero correlation with 7Be indicates that the stratosphere and upper troposphere are probably not the major sources. A significant biogenic source would be consistent with the higher mean nitrate concentrations, 0.16 to 0.17 g m–3, found over the equatorial Pacific at Fanning Island (3°55N, 159°20W) and Nauru (0°32S, 166°57E). The lack of correlation between nitrate and nss sulfate at American Samoa does not necessarily preclude an important role for marine biogenic sources.  相似文献   

3.
Rain and air of Florence have been collected in a continuous way andanalysed by flow analysis spectrofluorimetric methods for formaldehydeand hydrogen peroxide. Diurnal and seasonal variations were observed;the mean/maximum concentrations of all data (as gm–3) are 3.3/23.4 for HCHO and 0.4/4.93 forH2O2. The effect of external sources and ofphotochemical reactions produces periods of positive and negativecorrelations for these compounds. The mean/maximum rain concentration ofall data are 98/443 g l–1 for HCHO and 84/685 g l–1 for H2O2. Concentrationratios rain/air and discrepancies to Henry's Law equilibrium arediscussed.  相似文献   

4.
We present the first application of a multi-stage impactor to study volcanic particle emissions to the troposphere from Masaya volcano, Nicaragua. Concentrations of soluble SO4 2–,Cl–, F–, NO3 –, K+, Na+,NH4 +, Ca2+ and Mg2+ were determined in 11 size bins from 0.07 m to >25.5 m. The near-source size distributions showed major modes at 0.5m (SO4 2–, H+,NH4 +); 0.2 m and 5.0 m (Cl–) and 2.0–5.0 m(F–). K+ and Na+ mirrored the SO4 2– size-resolvedconcentrations closely, suggesting that these were transported primarily asK2SO4 and Na2SO4 in acidic solution, while Mg2+ andCa2+ presented modes in both <1 m and >1 m particles. Changes in relative humidity were studied by comparing daytime (transparent plume) and night-time (condensed plume) results. Enhanced particle growth rates were observed in the night-time plume as well as preferential scavenging of soluble gases, such as HCl, by condensed water. Neutralisation of the acidic aerosol by background ammonia was observed at the crater rim and to a greater extent approximately 15 km downwind of the active crater. We report measurements of re-suspended near-source volcanic dust, which may form a component of the plume downwind. Elevated levels ofSO4 2–, Cl–, F–,H+, Na+, K+ and Mg2+ were observed around the 10 m particle diameter in this dust. The volcanic SO4 2– flux leaving the craterwas 0.07 kg s–1.  相似文献   

5.
Radiative Heat Transfer and Hydrostatic Stability in Nocturnal Fog   总被引：1，自引：0，他引：1  
We have performed a one-dimensional and transient radiative heat transfer analysis in order to investigate interaction between atmospheric radiation and convective instability within a nocturnal fog. The radiation element method using the Ray Emission Model (REM2), which is a generalized numerical method, in conjunction with a line-by-line (LBL) method, is employed to attain high spectral resolution calculations for anisotropically scattering fog. The results show that the convective instability has a strong dependence on radiative properties of the fog. For the condition of a 20-m droplet diameter and liquid water content of 0.1 × 10–3 kg m–3;, the temperature profile within the fog becomes S shaped, and a convective instability layer forms in the middle or lower level of the fog. However, for the same water content and a 40-m diameter droplet, no strong convective instability layer forms, whereas for a 10-m diameter droplet a strong convective instability is observed.  相似文献   

6.
During April 1986, as part of an international arctic air chemistry study (AGASP-2), ground level observations of aerosol trace elements, oxides of sulphur and nitrogen and particle number size distribution were made at Alert Canada (82.5N, 62.3W). Pollution haze was evident as indicated by daily aerosol number (size > 0.15 m diameter) and SO4 = concentrations in the range 125 – 260 cm–3 and 1.6 – 4.5 g m–3, respectively. Haze and associated acidic gases tended to increase throughout the period. SO2 and peroxyacetylnitrate (PAN) mixing ratios were in the range 140 – 480 and 370 – 590 ppt(v), respectively. About 88% of the total end-product nitrogen was in the form of PAN. In air dried to 2% relative humidity by warming to room temperature, the aerosol mass size distribution had a major mode at 0.3 m diameter and a minor one at 2.5 m. Aerosol mass below 1.5 m was well correlated with SO4 =, K+ and PAN. There was a steady increase in the oxidized fraction of total airborne sulphur and nitrogen oxide throughout April as the sun rose above the horizon and remained above. The mean oxidation rate of SO2 between Eurasia and Alert was estimated as 0.25 – 0.5% h–1. The molar ratio of total nitrogen oxide to total sulphur oxide in the arctic atmosphere (0.67±0.17) was comparable to that in European emissions. A remarkably strong inverse correlation of filterable Br and O3 led to the conclusion that O3 destruction and filterable Br production below the Arctic surface radiation inversion is associated with tropospheric photochemical reactions involving naturally occurring gaseous bromine compounds.  相似文献   

7.
Aerosol chemical composition and trace gas measurements were made at twolocations on the northeastern peninsula of Tenerife during the ACE-2HILLCLOUD experiment, between 28 June and 23 July 1997. Measurementswere made of coarse (#gt;2.5 m aerodynamic diameter) and fine (#lt; 2.5m) aerosol Cl–, NO3 –,SO4 2–, non-sea saltSO4 2– (NSSS),CH3SO3 – (MSA) andNH4 +, and gas phase dimethylsulphide (DMS), HCl,HNO3, SO2, CH3COOH, HCOOH andNH3. Size distributions were measured using a cascadeimpactor. Results show that in marine air masses NSSS and MSA wereformed via DMS oxidation, with additional NSSS present in air massescontaining a continental component. Using a Eulerian box model approachfor aerosols transported between upwind and downwind sites, a mean NSSSproduction rate of 4.36 × 10–4 gm–3 s–1 was calculated for daytimeclear sky periods (highest insolation), with values for cloudy periodsduring daytime and nighttime of 3.55 × 10–4 and2.40 × 10–4 g m–3s–1, respectively. The corresponding rates for MSA were6.23 × 10–6, 8.49 × 10–6and 6.95 × 10–6 g m–3s–1, respectively. Molar concentration ratios forMSA/NSSS were 8.7% (1.8–18.2%) and 1.9%(1.3–3.5%) in clean and polluted air masses, respectively.Reactions occurring within clouds appeared to have a greater influenceon rates of MSA production, than of NSSS, while conversely daytime gasphase reactions were more important for NSSS. For MSA, nighttimein-cloud oxidation rates exceeded rates of daytime gas phase productionvia OH oxidation of DMS. NSSS, MSA and ammonium had trimodal sizedistributions, with modes at 0.3, 4.0 and >10.0 m (NSSS andNH4 +), and 0.3, 1.5 and 4.0 m (MSA). Nosignificant production of other aerosol species was observed, with theexception of ammonium, which was formed at variable rates dependent onneutralisation of the aerosol with ammonia released from spatiallynon-uniform surface sources. Seasalt components were mainly present incoarse particles, although sub-micrometre chloride was also measured.Losses by deposition exceeded calculated expectations for all species,and were highest for the seasalt fraction and nitrate.  相似文献   

8.
Summary The relationships between smoke concentrations, measured at two monitoring stations in Athens by the ASTM (American Society for Testing and Materials) and the OECD (Organization for Economic Co-Operation and Development) methods are studied by using a sample of 738 mean daily values of simultaneous measurements during the period 1984–1986. It is shown that an exponential model, different for each monitoring station, with smoke concentrations in COH (coefficient of haze) as the independent variable and smoke concentrations in gr/m3 as the dependent variable, was the most appropriate for transforming smoke data from COH to gr/m3. Also it is shown that the transformation models can be applied independent of the prevailing meteorological conditions. Finally some tentative conclusions are derived concerning the long term variations of smoke concentrations in gr/m3 for the period 1977–1990 and 1973–1990 at the two monitoring stations respectively. The trend analysis has shown that pollution abatement efforts resulted in an about 10% per year decreasing trend in smoke concentrations, during the period 1986–1990, at these two Athenian stations.With 4 Figures  相似文献   

9.
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   

10.
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.  相似文献   

11.
Summary The performance of evaporation schemes with and approach and their combination within resistance representation of evaporation from bare soil surface is discussed. For this purpose nine schemes, based on different functions of or , on the ratio of the volumetric soil moisture content and its saturated value are used.The quality of the chosen schemes has been evaluated using the results of time integration by the coupled soil moisture and surface temperature prediction model, BARESOIL, using in situ data. A sensitivity analysis was made using two sets of data derived from the volumetric soil moisture content of the top soil layer. One with values below the wilting point (0.17 m3m–3) and the second with values above 0.20m3m–3. Data sets were obtained at the experimental site Rimski anevi, Yugoslavia, from the bare surface of a chernozem soil.With 4 Figures  相似文献   

12.
On the determination of the height of the Ekman boundary layer   总被引：1，自引：1，他引：1  
The heighth of the Ekman turbulent boundary layer determined by the momentum flux profile is estimated with the aid of considerations of similarity and an analysis of the dynamic equations. Asymptotic formulae have been obtained showing that, with increasing instability,h increases as ¦¦1/2 (where is the non-dimensional stratification parameter); with increasing stability, on the other hand,h decreases as –1/2. For comparison, a simple estimate of the boundary-layer heighth u determined by the velocity profile is given. As is shown, in unstable stratification,h u behaves asymptotically as ¦¦–1, i.e., in a manner entirely different from that ofh .  相似文献   

13.
Emission of nitrous oxide from temperate forest soils into the atmosphere   总被引：5，自引：0，他引：5  
N2O emission rates were measured during a 13-month period from July 1981 till August 1982 with a frequency of once every two weeks at six different forest sites in the vicinity of Mainz, Germany. The sites were selected on the basis of soil types typical for many of the Central European forest ecosystems. The individual N2O emission rates showed a high degree of temporal and spatial variabilities which, however, were not significantly correlated to variabilities in soil moisture content or soil temperatures. However, the N2O emission rates followed a general seasonal trend with relatively high values during spring and fall. These maxima coincided with relatively high soil moisture contents, but may also have been influenced by the leaf fall in autumn. In addition, there was a brief episode of relatively high N2O emission rates immediately after thawing of the winter snow. The individual N2O emission rates measured during the whole season ranged between 1 and 92 g N2O-N m–2 h–1. The average values were in the range of 3–11 g N2O-N m–2 h–1 and those with a 50% probability were in the range of 2–8 g N2O-N m–2 h–1. The total source strength of temperate forest soils for atmospheric N2O may be in the range of 0.7–1.5 Tg N yr–1.  相似文献   

14.
Summary The influence of agricultural management on the CO2 budget of a typical subalpine grassland was investigated at the Swiss CARBOMONT site at Rigi-Seebodenalp (1025m a.s.l.) in Central Switzerland. Eddy covariance flux measurements obtained during the first growing season from the mid of spring until the first snow fall (17 Mai to 25 September 2002) are reported. With respect to the 10-year average 1992–2001, we found that this growing season had started 10 days earlier than normal, but was close to average temperature with above-normal precipitation (100–255% depending on month). Using a footprint model we found that a simple approach using wind direction sectors was adequate to classify our CO2 fluxes as being controlled by either meadow or pasture. Two significantly different light response curves could be determined: one for periods with external interventions (grass cutting, cattle grazing) and the other for periods without external interventions. Other than this, meadow and pasture were similar, with a net carbon gain of –128±17g Cm–2 on the undisturbed meadow, and a net carbon loss of 79±17g Cm–2 on the managed meadow, and 270±24g Cm–2 on the pasture during 131 days of the growing season, respectively. The grass cut in June reduced the gross CO2 uptake of the meadow by 50±2% until regrowth of the vegetation. Cattle grazing reduced gross uptake over the whole vegetation period (37±2%), but left respiration at a similar level as observed in the meadow.  相似文献   

15.
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   

16.
Although extensive areas of forests and grasslands are burned in the tropics, relatively little scientific attention has been focused on this phenomenon. In order to determine the land area burned and estimate the charcoal (elemental or graphitic carbon) produced, I monitored agricultural burning in a 1145 km2 area in central Panama during the 1981 dry season. Over 10% of the land surface was burned in that year. Charcoal concentrations in the aerosol were also measured and reached values of 3.1 gC/m3 during the peak in burning. Off-peak values of aerosol charcoal are less than 1 gC/m3. The high charcoal concentration reflects the massive amounts of vegetational burning occurring in the area.The charcoal advected by the air mass flowing over the area has been estimated using a box model. Assuming an average aerosol concentration of charcoal of 1 gC/m3 for a three-month burning period, a 2 km atmospheric mixed layer, a 14 km/h wind velocity to the south, and a 150 km wide zone across the western Gulf of Panama watershed, I estimate that, during the dry season, 9×109 g charcoal are mobilized by the troposphere. If 4.1×1012 g phytomass are annually burned in this region, then the charcoal emission factor to the troposphere is 2.2×10–3.  相似文献   

17.
Henry's law constants KH (mol kg–1 atm–1) for the reaction HOCl(g)=HOCl(aq) near room temperature, literature data for the associated enthalpy change, and solubilities of HOCl in aqueous H2SO4 (46 to 60 wt%) at temperatures relevant to the stratosphere (200 KT230 K) are shown to be thermodynamically consistent. Effective Henry's law constants [H*=mHOCl/pHOCl, in mol kg–1 atm–1] of HOCl in aqueous H2SO4 are given by: ln(H*)=6.4946–mH2SO4(–0.04107+54.56/T)–5862 (1/To–1/T) where T(K) is temperature and To=298.15K. The activity coefficient of HOCl in aqueous H2SO4 has a simple Setchenow-type dependence upon H2SO4 molality.  相似文献   

18.
Henry's law constants KH (mol kg-1 atm-1) have been measured between 278.15 K and 308.15 K for the following organic acids: CH2FCOOH (ln(KH[298.15 K]) = 11.3 ± 0.2), CH2ClCOOH (11.59 ± 0.14), CH2BrCOOH (11.94 ± 0.21), CHF2COOH (10.32 ± 0.10), CHCl2COOH (11.69 ± 0.11), CHBr2COOH (12.33 ± 0.29), CBr3COOH (12.61 ± 0.21), and CClF2COOH (10.11 ± 0.12). The variation of KH with temperature was determined for all acids except CH2FCOOH and CBr3COOH, with r H° for the dissolution reaction ranging from –85.2 ± 2.6 to –57.1 ± 2.5 kJ mol-1, meaning that their solubility is generally more sensitive to temperature than is the case for the simple carboxylic acids. The Henry's law constants show consistent trends with halogen substitution and, together with their high solubility compared to the parent (acetic) acid (ln(KH[298.15 K]) = 8.61), present a severe test of current predictive models based upon molecular structure. The solubility of haloacetic acids and strong dissociation at normal pH mean that they will partition almost entirely into cloud and fog in the atmosphere (0.05–1.0 g H2O m-3), but can reside in both phases for the liquid water contents typical of aerosols (10-5-10-4 g H2O m-3).  相似文献   

19.
Use of an airborne quartz crystal microbalance cascade impactor instrument together with a correlation spectrometer has allowed the flux of particles and their size distribution to be determined at Mount Erebus. The plume contributes 21±3 metric tomnes/day of aerosol particles to the Antarctic upper troposphere. The aerosol particles consist of larger (5–25 m) particles of elemental sulfur and silica, a middle sized group of iron oxides and smaller particles (less than 1 m) of complex liquids. Unlike many volcanic plumes, the Erebus plume has only a small amount of sulfate particles. The concentrations of particles in the Erebus plumes was 70–370 m/m3. Limited sampling of the Antarctic atmosphere at 8 km altitude but hundreds of km away from Erebus obtained a few large particles of sulfur and silicates, suggesting a similarity with the Erebus plume. The fallout of these particles occurs slowly over a broad area of the Antarctic continent.  相似文献   

20.
A technique was developed that allows the determination of the stable carbon isotope ratio of isoprene in air. The method was used for a limited number of ambient measurements as well as laboratory studies of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis), including the light and temperature dependence. The mean stable carbon isotope ratio ( 13C) of isoprene emitted from Velvet Bean (Mucana pruriens L. var. utilis) for all our measurements is –27.7 ± 2.0 (standard deviation for 23 data points). Our results indicate a small dependence of the stable carbon isotope ratios on leaf temperature and photosynthetic photon flux density (PPFD). The light dependence is 0.0026 ± 0.0012/( mol of photons m–2 s–1) for the studied range from 400 to 1700 mol of photons m–2 s–1. The temperature dependence is 0.16 ± 0.09/K. On average, the emitted isoprene is 2.6 ± 0.9 lighter than the leaf carbon. An uncertainty analysis of the possibility to use stable carbon isotope ratio measurements of isoprene for estimates of its mean photochemical age suggests that meaningful results can be obtained. This is supported by the results of a small number of measurements of the stable carbon isotope composition of ambient isoprene at different locations. The results range from approximately –29 to –16. They are consistent with vegetation emissions of isoprene that is slightly depleted in 13C relative to the plant material and enrichment of 13C in the atmosphere due to isotope fractionation associated with the reaction with OH-radicals. The stable carbon isotope ratio of ambient isoprene at locations directly influenced by isoprene emissions is very close to the values we found in our emission studies, whereas at sites located remote from isoprene emitting vegetation we find substantial enrichment of 13C. This suggests that stable carbon isotope ratio measurements will be a valuable, quantitative method to determine the extent of photochemical processing of isoprene in ambient air.  相似文献   

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