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1.
During the 1st Lagrangian experiment of the North Atlantic Regional Aerosol Characterisation Experiment (ACE‐2), a parcel of air was tagged by releasing a smart, constant level balloon into it from the Research Vessel Vodyanitskiy . The Meteorological Research Flight's C‐130 aircraft then followed this parcel over a period of 30 h characterising the marine boundary layer (MBL), the cloud and the physical and chemical aerosol evolution. The air mass had originated over the northern North Atlantic and thus was clean and had low aerosol concentrations. At the beginning of the experiment the MBL was over 1500 m deep and made up of a surface mixed layer (SML) underlying a layer containing cloud beneath a subsidence inversion. Subsidence in the free troposphere caused the depth of the MBL to almost halve during the experiment and, after 26 h, the MBL became well mixed throughout its whole depth. Salt particle mass in the MBL increased as the surface wind speed increased from 8 m s−1 to 16 m s−1 and the accumulation mode (0.1μm to 3.0 μm) aerosol concentrations quadrupled from 50 cm−3 to 200 cm−3. However, at the same time the total condensation nuclei (>3 nm) decreased from over 1000 cm−3 to 750 cm−3. The changes in the accumulation mode aerosol concentrations had a significant effect on the observed cloud microphysics. Observational evidence suggests that the important processes in controlling the Aitken mode concentration which, dominated the total CN concentration, included, scavenging of interstitial aerosol by cloud droplets, enhanced coagulation of Aitken mode aerosol and accumulation mode aerosol due to the increased sea salt aerosol surface area, and dilution of the MBL by free tropospheric air.  相似文献   

2.
Measurements of direct solar irradiance were taken employing 4 different sun‐photometers at near infrared wavelengths, suitable for use in atmospheric hygrometry. This technique utilising a set of spectral ratios, in and out of selected water vapour absorption bands, was applied to the measurements to obtain accurate evaluations of precipitable water. For all the hygrometric ratios given by the 4 sun‐photometers used at the 3 stations of Sagres, Monchique and Mt. Foia, during the CLEARCOLUMN experiment, we determined the calibration curves by correcting them for the Rayleigh scattering effects and, then, plotting the natural logarithms of such corrected ratios versus the square root of the water vapour mass present along the atmospheric slant path. The regression lines drawn for the various scatter diagrams were estimated to give evaluations of precipitable water with an uncertainty of less than 5%, 3% and 10% at the 3 stations, respectively. The calibration curves of the sun‐photometer located at the Sagres station were determined using the precipitable water evaluations obtained from the local radiosounding measurements taken on 5 clear‐sky days. Those of the sun‐photometers used at the Monchique and Mt. Foia stations were instead determined through intercomparison between subsets of measurements simultaneously taken with various instruments at Sagres and Mt. Foia. Using these calibration curves, we examined all the field measurements determining the time‐patterns of precipitable water at the 3 stations. During the period from 16 June to 25 July 1997, precipitable water was found to vary between 1.1 and 3.7 g cm−2 at the Sagres station (with an accuracy within ±13%), between 1.0 and 2.8 g cm−2 at Monchique (±11%) and between 0.8 and 3.0 g cm−2 at the top of Mt. Foia (±26%).  相似文献   

3.
During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R2>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R2= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R2=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.  相似文献   

4.
The second Aerosol Characterisation Experiment (ACE‐2) was aimed at investigating the physical, chemical and radiative properties of aerosol and their evolution in the North Atlantic region. In the 2nd "Lagrangian" experiment, an air mass was tracked over a 30‐h period during conditions of extensive stratocumulus cover. Boundary‐layer measurements of the aerosol size distribution obtained with a passive cavity aerosol spectrometer probe (PCASP) during the experiment show a gradual growth in size of particles in the 0.1–0.2 μm diameter mode. Simultaneously, SO2 concentrations were found to decrease sharply from 800 to 20 ppt. The fraction of sulphate in aerosol ionic mass increased from 0.68±0.07 to 0.82±0.09 for small particles (diameter below 1.7 μm) and from 0.21±0.04 to 0.34±0.03 for large particles (diameter above 1.7 μm). The measurements were compared with a multicyclic parcel model of gas phase diffusion into cloud droplets and aqueous phase chemical reactions. The model was able to broadly reproduce the observed transformation in the aerosol spectra and the timescale for the transformation of SO2 to sulphate aerosol. The modelled SO2 concentration in the boundary layer fell to below half its initial value over a 6.5‐h time period due to a combination of the entrainment of cleaner tropospheric air and cloud chemical reactions. NH3 and HCl gas were also found to play an important rôle in cloud processing in the model.  相似文献   

5.
Microphysical measurements performed during 8 flights of the CLOUDYCOLUMN component of ACE‐2, with the Meteo‐France Merlin‐IV, are analyzed in terms of droplet number concentration and size. The droplet concentration is dependent upon the aerosol properties within the boundary layer. Its mean value over a flight varies from 55 cm−3, for the cleanest conditions, to 244 cm−3, for the most polluted one. For each flight, the variability of the concentration, in selected cloud regions that are not affected by mixing with dry air or drizzle scavenging, ranges from 0.5 to 1.5 of the mean value. The mean volume diameter increases with altitude above cloud base according to the adiabatic cloud model. The frequency distribution of mean droplet volume normalized by the adiabatic value, for the selected regions, shows the same dispersion as the distribution of normalized concentration. The values of droplet concentration versus mean volume diameter are then examined in sub‐adiabatic samples to characterize the effects of mixing and drizzle scavenging. Finally, the ratio of mean volume diameter to effective diameter is analyzed and a simple relationship between these 2 crucial parameters is proposed.  相似文献   

6.
The amounts of microbial and root‐respired CO2 in a maize/winter wheat agricultural system in south western Germany were investigated by measurements of the CO2 mixing ratio and the 13C/12C ratio in soil air. CO2 fluxes at the soil surface for the period of investigation (1993–1995) were also determined. Root respired CO2 shows a strong correlation with the plant mass above ground surface of the respective vegetation (R2≥0.88); the maximum CO2 release from roots was in August for the maize (2.0±0.5 mmol m−2 h−1) and in June for winter wheat (1.5±0.5 mmol m−2 h−1). Maximum CO2 production by roots correlate well with the maximum amount of plant root matter. Integrating the CO2 production over the whole growing season and normalizing to the dry root matter yields, the CO2 production per gram dry organic root matter (DORM) of maize was found to be 0.14±0.03 gC (g DORM)−1. At the sites investigated, root‐produced CO2 contributed (16±4)% for maize, and (24±4)% for winter wheat, respectively, to the total annual CO2 production in the soil (450±50 gC m−2 for maize, 210±30 gC m−2 for winter wheat).  相似文献   

7.
Wet‐only rainwater composition, acid‐precursor gas mixing ratios and aerosol loading were determined from weekly‐averaged samples at Petaling Jaya, Malaysia, over the five year period from March 1993 to March 1998. Annual deposition fluxes of acidic sulfur and nitrogen species estimated from these data show this site to be heavily impacted by acidic deposition, with total oxidised sulfur plus nitrogen deposition in the range 277–480 meq m−2 yr−1. Average contributions were 56% as sulfur species, 44% as nitrogen species, with wet deposition in this region of high rainfall accounting for 67% of total deposition. Thus total acid deposition fluxes were equivalent to levels that provided motivation for emissions reduction programs in both Europe and North America. The possibility of adverse environmental effects in Malaysia caused by acid deposition therefore merits serious consideration and assessment.  相似文献   

8.
Long‐range transport of anthropogenic and biogenic CO2 to a remote site in the Arctic is studied. A limited area, off‐line, Eulerian atmospheric transport model is used, and the results are compared to the observed CO2 concentration at the "Ny‐Alesund International Arctic Research and Monitoring Facility". Inventories of anthropogenic CO2 emissions and estimates of biogenic CO2 emissions are used to investigate the respective impact of these emissions on Arctic CO2 variations during 4 winter months. A direct comparison of the modelled and observed concentrations reveals remarkably good timing in the modelled variations as compared to the observed variations for most of the time. The correlation of observed versus modelled CO2 concentration is significant at the 95% confidence level. The biogenic and the anthropogenic CO2 emissions are shown to have approximately equal influence on Arctic CO2 variations during winter. Europe is found to be the dominant source of anthropogenic CO2 at the monitoring station, while Siberia and Northern America have little influence on Arctic CO2, during the months studied. These results contradict Engardt and Holmén whose results indicate that the lower‐Ob region in western Siberia has a large impact on Arctic CO2.  相似文献   

9.
The Hamburg atmospheric general circulation model (AGCM) ECHAM‐4 is used to identify the main source regions of precipitation falling on Greenland and Antarctica. Both water isotopes H218O and HDO are explicitly built into the water cycle of the AGCM, and in addition the capability to trace water from different source regions was added to the model. Present and LGM climate simulations show that water from the most important source regions has an isotopic signature similar to the mean isotope values of the total precipitation amount. But water from other source regions (with very different isotopic signatures) contributes an additional, non‐negligible part of the total precipitation amount on both Greenland and Antarctica. Analyses of the temperature‐isotope‐relations for both polar regions reveal a solely bias of the glacial isotope signal on Greenland, which is caused by a strong change in the seasonal deposition of precipitation originating from nearby polar seas and the northern Atlantic. Although the performed simulations under LGM boundary conditions show a decrease of the δ 18O values in precipitation in agreement with ice core measurements, the AGCM fails to reproduce the observed simultaneous decrease of the deuterium excess signal.  相似文献   

10.
A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr−1. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.  相似文献   

11.
The development of the future atmospheric chemical composition is investigated with respect to NO y and O3 by means of the off‐line coupled dynamic‐chemical general circulation model ECHAM3/CHEM. Two time slice experiments have been performed for the years 1992 and 2015, which include changes in sea surface temperatures, greenhouse gas concentrations, emissions of CFCs, NO x and other species, i.e., the 2015 simulation accounts for changes in chemically relevant emissions and for a climate change and its impact on air chemistry. The 2015 simulation clearly shows a global increase in ozone except for large areas of the lower stratosphere, where no significant changes or even decreases in the ozone concentration are found. For a better understanding of the importance of (A) emissions like NO x and CFCs, (B) future changes of air temperature and water vapour concentration, and (C) other dynamical parameters, like precipitation and changes in the circulation, diabatic circulation, stratosphere‐troposphere‐exchange, the simulation of the future atmosphere has been performed stepwise. This method requires a climate‐chemistry model without interactive coupling of chemical species. Model results show that the direct effect of emissions (A) plays a major rôle for the composition of the future atmosphere, but they also clearly show that climate change (B and C) has a significant impact and strongly reduces the NO y and ozone concentration in the lower stratosphere.  相似文献   

12.
Many researchers have reported the widespread occurrence of excess 210 Po in the global atmosphere and suggested probable sources such as resuspension of top soils, stratospheric aerosols, sea spray of the surface micro‐layer, volcanic emission, and bio‐volatile 210Po species from the productive ocean. We have observed excess 210Po on aerosols in the coastal atmosphere of the Chesapeake and Delaware Bays. On‐board measurements in the Chesapeake Bay atmosphere show that the increase of this excess 210Po is dependent upon wind speed. Simultaneously measured activity ratios of 7Be/210Pb and 210Pb/222Rn argue against either higher altitude air or continental soils as the source of this excess. We hypothesize that the excess 210Po originates mainly from surface waters either by the sea‐spray of the surface microlayer, or more likely, by gas exchange. We conclude gas exchange as the mechanism since the polonium excess increases linearly with wind speed over a threshold of 3 m s−1(mean) similar to other gases (i.e., CO2, SF6 , and DMS). In addition, higher 210Po excess with lower 222Rn is observed in on‐shore marine air at Lewes, DE. This suggests sea‐air exchange of volatile Po along with other bio‐volatile species (i.e., DMS, DMSe, and MMHg) in the coastal productive ocean during high wind speeds.  相似文献   

13.
Global warming simulations are performed with a coupled climate model of reduced complexity to investigate global warming–marine carbon cycle feedbacks. The model is forced by emissions of CO2 and other greenhouse agents from scenarios recently developed by the Intergovernmental Panel on Climate Change and by CO2 stabilization profiles. The uptake of atmospheric CO2 by the ocean is reduced between 7 to 10% by year 2100 compared to simulations without global warming. The reduction is of similar size in the Southern Ocean and in low‐latitude regions (32.5°S‐32.5°N) until 2100, whereas low‐latitude regions dominate on longer time scales. In the North Atlantic the CO2 uptake is enhanced, unless the Atlantic thermohaline circulation completely collapses. At high latitudes, biologically mediated changes enhance ocean CO2 uptake, whereas in low‐latitude regions the situation is reversed. Different implementations of the marine biosphere yield a range of 5 to 16% for the total reduction in oceanic CO2 uptake until year 2100. Modeled oceanic O2 inventories are significantly reduced in global warming simulations. This suggests that the terrestrial carbon sink deduced from atmospheric O2/N2 observations is potentially overestimated if the oceanic loss of O2 to the atmosphere is not considered.  相似文献   

14.
An aerosol dynamics model, AEROFOR2, is developed in the context of the BIOFOR project focussing on boreal forest aerosol. It is the second version of a Lagrangian type box model AEROFOR for investigating the formation and growth of particles under clear sky atmospheric conditions. Particles can consist of soluble and insoluble material and the particle population can be externally or internally mixed. AEROFOR2 includes gas phase chemistry and aerosol dynamics, and calculates the number and composition distributions of particles as functions of time. Observed growth rates of the nucleation mode particles after a typical nucleation event are 2–3 nm/h. The model simulations predict that 3·107 molecules cm−3 of insoluble organic vapour and less than 6·106 molecules cm−3 of soluble vapour condensing onto particles are enough to make them grow in good agreement with the observed growth rates. Then the source rate of the organic vapour must be an order of 105 molecules cm−3 s−1, and its saturation vapour density should be below 106 molecules cm−3. If the aerosol was initially an internal mixture of soluble (70%) and insoluble (30%) constituents it transformed to an externally mixed aerosol during the simulation. By applying the externally‐mixed aerosol based on measured soluble volume fractions, it was concluded that the modelled soluble fraction of the nucleation mode was too low in comparison with the measurements, and thus, a part of the condensable organic vapour must be water soluble.  相似文献   

15.
Boron isotope variations in the atmosphere   总被引：2，自引：0，他引：2  
We report here the first measurements of boron isotope ratios in the maritime atmosphere together with those of precipitation. The δ11B values of atmospheric condensates in the western North Pacific and Japanese coast and snow in Tokyo range from −12.8 to +5.1‰ and from −0.4 to +0.4‰, respectively, which are significantly lower than those of rainwater (+18.9 to +34.7‰) collected mostly over the North Pacific. Since the 11B/10B ratios of the atmosphere are lower than those of volcanic emissions (δ11B=+2.3 to +21.4‰), we must seek sources for atmospheric boron other than volcanism. We postulate that the sea may be an important supplier for atmospheric boron under some dynamic conditions and that boron isotope fractionation during evaporation from seawater and removal from the atmosphere may account for the large variations of 11B/10B ratios observed in the atmosphere and precipitation.  相似文献   

16.
Abstract The spatial and temporal variations of atmospheric CO2 at 8–13 km from April 1993 to April 1999 were observed by measuring CO2 mixing ratios in samples collected biweekly from a commercial airliner between Australia and Japan. The CO2 growth rate showed a considerable interannual variation, with a maximum of about 3 ppm yr−1 during late 1997. This variation is related to the El Niño/Southern Oscillation (ENSO) events. A year-to-year change related to the ENSO events was also found in the latitudinal distribution pattern of the CO2 annual mean between 30°N and 30°S. The averaged CO2 seasonal cycle in the Northern Hemisphere gradually decayed toward the equator, and a relatively complicated variation with a double seasonal maximum appeared in the Southern Hemisphere. A significant yearly change of the seasonal cycle pattern was observed in the Southern Hemisphere. The impact of a tropical biomass-burning injection on the upper tropospheric CO2 was estimated on the basis of the CO data from the same airliner observation.  相似文献   

17.
The dominant sink of atmospheric molecular hydrogen (H2) is its enzymatic destruction in soils. Quantitative estimates of the global sink strength, as derived from bottom-up process studies, are, however, still associated to large uncertainties. Here we present an alternative way to estimate atmosphere-to-soil flux densities, respectively deposition velocities of H2, based on atmospheric H2 and 222Rn observations in the boundary layer. Two and a half years of continuous measurements from a polluted site in the Rhine-Neckar area have been evaluated and night-time flux densities were calculated for situations of strong nocturnal boundary layer inversions using the Radon-Tracer Method. The influences from local anthropogenic combustion sources could be detected and successfully separated by parallel measurements of carbon monoxide. Inferred daily uptake fluxes in the Heidelberg catchment area range from 0.5 to 3 × 10−8 g H2 m−2 s−1 with a mean value of (1.28 ± 0.31) × 10−8 g H2 m−2 s−1. Uptake rates are about 25% larger during summer than during winter, when soil moisture is high, and diffusive transport of H2 into the soil is inhibited. The mean deposition velocity is 3.0 ± 0.7 × 10−2 cm s−1, which is very well in line with direct measurements on similar soil types in Europe and elsewhere.  相似文献   

18.
An atmospheric transport model, NIRE-CTM-96, was evaluated by using measured radon-222 concentrations. The model has 2.5×2.5 degree horizontal resolution and 15 vertical levels. Assimilated global meteorological data for 1990–1996 from the European Centre for Medium Range Weather Forecasts were used to drive the model. We used an emanation rate of radon-222 of 1 atom cm−2 s−1 over mostly ice-free land. Simulated concentrations were compared with measured concentrations for 22 sites worldwide including 10 stations in China. Simulated annual mean concentrations for Freiburg, Germany, and Socorro, New Mexico, and for four stations in northern China were consistent with the measured concentrations. Simulated daily concentrations for Ogasawara-Hahajima, Japan, correlated well with the measured concentrations. Simulated upper tropospheric concentrations for Moffet Field, California, demonstrated the cross-Pacific transport from central Eurasia and India-Indochina area. Simulated concentrations for two stations in southern China were almost half of the measured concentrations. Mixing layer depth in the model was consistent with other estimates which indicates higher emanation rate there. Simulated concentrations for the South Indian Ocean and the Antarctic during summer were significantly lower than the measured concentrations; this difference was accounted for when emanation from the ocean at a rate of 0.01 atom cm−2 s−1 was included in the model. The model failed to simulate amplitudes of high-concentration events at Mauna Loa. These high-concentration events were possibly a result of filament-like horizontal structure or laminated vertical structure. The vertical as well as horizontal resolution of the model were supposed to be insufficient to reproduce these fine structures.  相似文献   

19.
During late austral summer and winter 1998, black carbon (BC) aerosols were monitored with an Aethalometer at 2 sites of La Réunion Island (Indian Ocean): Saint‐Denis, the main city and Sainte‐Rose, a quite uninhabited region situated at the east coast. BC concentration data at Saint‐Denis show a marked diurnal cycle, which may be primarily attributed to traffic. The background data found at night‐time display average BC concentrations, ranging from about 80 to 250 ng/m3 whereas during the day, BC concentrations increase by a factor of at least 4. In comparison, BC concentrations vary in the range of 10 to 60 ng/m3 at Sainte‐Rose. Ozone concentration was also measured at Saint‐Denis using a Dasibi photometer and found to be at significant levels (means: 16.5–23 ppbv in April and 28.5–34 ppbv in September). A noticeable increase of ozone concentrations during the day points out the build‐up of pollutants enhancing photochemical transformations. However, during traffic pollution peaks, ozone concentration displays systematic depletion. The comparison of ozone and BC measurements at both seasons points to some possible effects of heterogeneous interaction of ozone and its precursors with BC particles. These interactions were also simulated with a 0D time‐dependent chemistry model using conditions of a polluted site. The measured ozone concentration characteristics (mean concentration and range of variation) are well simulated in the presence of BC. Our model results show that at La Réunion Island adsorption of ozone and its precursors onto BC aerosol particles could be one of the important steps determining ozone concentration characteristics, especially in absence of photochemistry during night‐time.  相似文献   

20.
The Optical Transient Detector (OTD) lightning data for the 12‐month period of 1996 are used to estimate the seasonal and global distributions of lightning‐produced NO x . The relatively small viewing footprint and the low detection efficiency of the OTD sensor and other difficulties require extrapolations of the OTD data to the actual global flash distributions. Furthermore, available measurements for the ratios of intracloud (IC) to cloud‐to‐ground (CG) flashes have been used to partition lightning counts for IC versus CG flashes from the OTD observations. The resulting lightning distributions are then used to calculate the global and seasonal production of NO x , assuming a NO production rate of 6.2×1025 molecules for each CG flash and 8.7×1024 molecules for each IC flash. Consequently, we find that CG flashes produce more NO x than IC flashes despite fewer CG flashes by a factor of 3 or more. NO x production by lightning varies seasonally in accordance with the global lightning distribution, with the maximum production occurring in the Northern Hemisphere in the local summer. The latitudinal distribution of NO x production exhibits a strong seasonal variation outside the tropics with the production occurring mainly in the summer hemisphere, whereas in the tropics the production is high throughout the year. The annual contribution to NO x production by lightning is higher in the Northern Hemisphere than that in the Southern Hemisphere.  相似文献   

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