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1.
Latitudinal distribution of radon-222 flux from continents   总被引：1，自引：0，他引：1  
Global atmospheric transport models are frequently tested by using 222Rn as a tracer. Generally this tracer is assumed to be emitted at a uniform rate (1 atom cm−2 s−1) from all ice-free land surfaces. The analysis of published data suggests a strong decrease from 30°N northwards to 0.2 atom cm−2 s−1 at 70°N. This could be a result of increasing water tables and proportions of organic soils as indicated by larger proportions of wetlands in northern latitudes.  相似文献   

2.
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   

3.
Terrestrial radon-222 flux density for the Asian continent, integrated over distances of 4500 km, is estimated in two 20° latitudinal bands centred on 48.8°N and 63.2°N. The evaluation is based on three years of wintertime radon measurements at Sado Island, Japan, together with meteorological and trajectory information. A selection of 18% of observations are suitable for evaluation of an analytical expression for the continental surface flux. Various meteorological assumptions are discussed; it is found that there is a substantial effect of increased complexity of the formulation on the flux estimates obtained. The distribution of spatially integrated radon flux over the Asian landmass is reported for the first time. Expressed as geometric means and 1σ-ranges, estimated fluxes are 14.1 mBq m−2 s−1 (1σ-range: 18 mBq m−2 s−1) and 8.4 mBq m−2 s−1 (1σ-range: 10 mBq m−2 s−1) for the lower and higher latitude bands. These results constitute an annual minimum in flux densities for these regions, and are higher than previously reported. The existence of a latitudinal gradient in the continental radon source function is confirmed; the present estimate for Asia (−0.39 mBq m−2 s−1 per degree of latitude) is in agreement with the northern hemisphere terrestrial radon flux gradient proposed previously.  相似文献   

4.
Enclosure measurements have been performed on a bare mineral soil at an experimental field site near Heidelberg, Germany. From observed molecular hydrogen (H2) mixing ratio changes in the enclosure, deposition velocities were calculated ranging from  8.4 × 10−3  to  8.2 × 10−2 cm s−1  and with an annual mean value of  3.1 × 10−2 cm s−1  . In the studied range of  2– 27 °C  , the uptake showed a significant temperature dependence. However, this turned out not to be the primary driving mechanism of the uptake flux. Soil moisture content, co-varying with temperature, was identified as the major parameter being responsible for the diffusive permeability of H2 in the soil and the final rate of H2 uptake. A simple Millington–Quirk diffusion model approach could largely explain this behaviour and yielded a diffusion path length of H2 in the studied soil of only 0.2–1.8 cm, suggesting that total H2 consumption occurs within the first few centimetres of the soil. The diffusion model, when applied to continuous measurements of soil moisture content, atmospheric pressure, temperature and the mixing ratio of H2 in the atmosphere, could largely reproduce the measured deposition flux densities, assuming a mean thickness of the diffusion path length of 0.7 cm.  相似文献   

5.
The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE‐2). Very high cloud droplet number concentrations (almost 3000 cm−3) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150–3000 cm−3. The updraught velocity during the cloud formation was estimated to 2.2 m s−1 by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols.  相似文献   

6.
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   

7.
Concurrent observations of particle number densities and size distributions observed at two different heights (near ocean level and 475 m above sea level) in Ny-Ålesund, Svalbard were studied with respect to the diurnal variation during a summer period in June 2004. The results show that observed variation in particle number density in the Arctic boundary layer may be strongly modulated by vertical mixing and dilution. The particles appeared to be formed in the early morning when solar intensity reached about 30% of the mid-day intensity. Based on differences in the observed number densities at the two heights it appears as if particles are formed in the lower part of the boundary layer. The formation rate of 10 nm diameter particles is estimated to be 0.11 cm−3 s−1 and the growth rate is in a range between 1 and 2 nm h−1.  相似文献   

8.
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   

9.
Physical characterization of aerosol particles during nucleation events   总被引：4，自引：3，他引：4  
Particle concentrations and size distributions have been measured from different heights inside and above a boreal forest during three BIOFOR campaigns (14 April–22 May 1998, 27 July–21 August 1998 and 20 March–24 April 1999) in Hyytiälä, Finland. Typically, the shape of the background distribution inside the forest exhibited 2 dominant modes: a fine or Aitken mode with a geometric number mean diameter of 44 nm and a mean concentration of 1160 cm−3 and an accumulation mode with mean diameter of 154 nm and a mean concentration of 830 cm−3. A coarse mode was also present, extending up to sizes of 20 μm having a number concentration of 1.2 cm−3, volume mean diameter of 2.0 μm and a geometric standard deviation of 1.9. Aerosol humidity was lower than 50% during the measurements. Particle production was observed on many days, typically occurring in the late morning. Under these periods of new particle production, a nucleation mode was observed to form at diameter of the order of 3 nm and, on most occasions, this mode was observed to grow into Aitken mode sizes over the course of a day. Total concentrations ranged from 410–45 000 cm−3, the highest concentrations occurring on particle production days. A clear gradient was observed between particle concentrations encountered below the forest canopy and those above, with significantly lower concentrations occurring within the canopy. Above the canopy, a slight gradient was observed between 18 m and 67 m, with at maximum 5% higher concentration observed at 67 m during the strongest concentration increases.  相似文献   

10.
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   

11.
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   

12.
Ambient CO2 concentration, air temperature and relative humidity were measured intermittently for a 3-year period from the floor to the canopy top of a tropical rainforest in Pasoh, Peninsular Malaysia. Mean diurnal CO2 storage flux ( S c; μmol m−2 s−1) and sensible and latent heat storage fluxes ( Q a and Q w; W m−2) ranged from −12.7 to 3.2 μmol m−2 s−1, −15 to 27 W m−2 and −10 to 20 W m−2, respectively. Small differences in diurnal changes were observed in S c and Q a between the driest and wettest periods. Compared with the ranges of mean diurnal CO2 eddy flux (−14.7 to 4.9 μmol m−2 s−1), sensible eddy flux (−12 to 169 W m−2) and latent eddy flux (0 to 250 W m−2), the contribution of CO2 storage flux was especially large. Comparison with summertime data from a temperate Japanese cypress forest suggested a higher contribution of S c in the tropical rainforest, probably mainly due to the difference in nighttime friction velocity at the sites. On the other hand, differences in Q a and Q w were smaller than the difference in S c, probably because of the smaller nighttime sinks/sources of heat and water vapour.  相似文献   

13.
A set of 152 vertical profiles of aerosol number concentration and size distribution with diameter ranging from 0.12 to 3.0 μm observed by the airborne optical spectrometer probe in Beijing, China, between February 2005 and September 2006 is analysed and discussed. The statistic of aerosol number concentration ( N a) reveals a high aerosol number density in this region with average surface level number concentration ( N 0) of about 6600 cm−3 (0.12–3.0 μm). The average vertical profile of N a approximately satisfies an exponential decline function with a scale height of 1419 m. The N a profiles are influenced by the structures of planetary boundary layer (PBL) significantly and two typical types of N a profile under different conditions of PBL are presented and parametrized in this study. The observations of aerosol size distribution show that, in most cases the aerosol size distributions are not very sensitive to altitude, with effective radii ranging from 0.16 to 0.28 μm. Comparison between aircraft-derived aerosol optical depth (AOD) and Moderate Resolution Imaging Spectroradiometer-derived AOD shows good agreement. The Mie model calculations suggest that the surface level number concentration, the PBL height and the structure of PBL can influence the AOD significantly.  相似文献   

14.
Two airborne campaigns were carried out to measure the tropospheric concentrations and variability of CO2, CO and O3 over Siberia. In order to quantify the influence of remote and regional natural and anthropogenic sources, we analysed a total of 52 vertical profiles of these species collected in April and September 2006, every ∼200 km and up to 7 km altitude. CO2 and CO concentrations were high in April 2006 (respectively 385–390 ppm CO2 and 160–200 ppb CO) compared to background values. CO concentrations up to 220 ppb were recorded above 3.5 km over eastern Siberia, with enhancements in 500–1000 m thick layers. The presence of CO enriched air masses resulted from a quick frontal uplift of a polluted air mass exposed to northern China anthropogenic emissions and to fire emissions in northern Mongolia. A dominant Asian origin for CO above 4 km (71.0%) contrasted with a dominant European origin below this altitude (70.9%) was deduced both from a transport model analysis, and from the contrasted ΔCO/ΔCO2 ratio vertical distribution. In September 2006, a significant O3 depletion (∼–30 ppb) was repeatedly observed in the boundary layer, as diagnosed from virtual potential temperature profiles and CO2 gradients, compared to the free troposphere aloft, suggestive of a strong O3 deposition over Siberian forests.  相似文献   

15.
Long-term measurements of fine particle number-size distributions were carried out over 9.5 yr (May 1997–December 2006), in the urban background atmosphere of Helsinki. The total number of days was 3528 with about 91.9% valid data. A new particle formation event (NPF) is defined if a distinct nucleation mode of aerosol particles is observed below 25 nm for several hours, and it shows a growth pattern. We observed 185 NPF events, 111 d were clear non-events and most of the days (around 83.5%) were undefined. The observed events were regional because they were observed at Hyytiälä (250 km north of Helsinki). The events occurred most frequently during spring and autumn. The observed formation rate was maximum during the spring and summer (monthly median 2.87 cm−3 s−1) and the modal growth rate was maximum during late summer and Autumn (monthly median 6.55 nm h−1). The events were observed around noon, and the growth pattern often continued on the following day. The observation of weak NPF events was hindered due to pre-existing particles from both local sources. It is clear that regional NPF events have a clear influence on the dynamic behaviour of aerosol particles in the urban atmosphere.  相似文献   

16.
In this issue, Ramonet et al. revealed a positive trend in European, atmospheric CO2 concentrations relative to a marine, North Atlantic reference baseline, for the years 2001–2006. The observed build up mainly occurred during the cold season where it reaches a 0.8 ppm yr−1 at low-altitude stations to a 0.3 ppm yr−1 at mid-altitude stations. We explore the cause of this build-up using the mesoscale model CHIMERE. We first model the observed trends, using interannually varying fluxes and transport, then suppress the interannual variability in fluxes or aspects of transport to elucidate the cause. The run with no interannual variability in fluxes still matches observed trends suggesting that transport is the major cause. Separate runs varying either boundary layer height or winds show that changes in boundary layer height explain the trends at low-altitude stations within the continents while changes in wind regimes drive changes elsewhere.  相似文献   

17.
地面风对瓦里关山大气CH4本底浓度的影响分析   总被引：6，自引：1，他引：6       下载免费PDF全文
使用1994年7月至1996年12月大气CH4和地面风现场连续观测资料，分析了瓦里关全球大气本底基准站（36°17′N, 100°54′E，海拔3816 m）地面风变化对大气CH4本底浓度的影响。结果表明，水平风向、风速和垂直风向、风速的变化对大气CH4观测值的影响在春、夏、秋、冬季有明显不同，水平风向NE—ENE—E为CH4测量最主要的局地影响非本底扇区，静风及水平风速大于10 m/s、垂直风速大于±1 m/s对观测结果都有较大影响；由的统计平均还给出了此段期间瓦里关大气CH4在不同季节的浓度分布范围和日变化类型，并分析了可能成因；将地面风数据作为大气CH4本底资料的过滤因子之一，提出了适用于不同使用目的和要求的我国内陆高原大气CH4本底数据筛选方法，本底数据留存率约为原始资料量的50%。  相似文献   

18.
A comparison of large‐scale models simulating atmospheric sulfate aerosols (COSAM) was conducted to increase our understanding of global distributions of sulfate aerosols and precursors. Earlier model comparisons focused on wet deposition measurements and sulfate aerosol concentrations in source regions at the surface. They found that different models simulated the observed sulfate surface concentrations mostly within a factor of two, but that the simulated column burdens and vertical profiles were very different amongst different models. In the COSAM exercise, one aspect is the comparison of sulfate aerosol and precursor gases above the surface. Vertical profiles of SO2, SO2−4, oxidants and cloud properties were measured by aircraft during the North Atlantic Regional Experiment (NARE) experiment in August/September 1993 off the coast of Nova Scotia and during the Second Eulerian Model Evaluation Field Study (EMEFSII), in central Ontario in March/April 1990. While no single model stands out as being best or worst, the general tendency is that those models simulating the full oxidant chemistry tend to agree best with observations although differences in transport and treatment of clouds are important as well.  相似文献   

19.
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   

20.
Concentrations of organic carbon (OC), elemental carbon (EC), selected trace elements and water-soluble (WS) ions were determined for samples collected from August 2004 to February 2005 to assess the aerosol background at two remote sites in China. The OC and EC concentrations in PM10 from near the Tibetan Plateau at Zhuzhang (ZUZ) were comparable with other background sites, averaging 3.1 and 0.34 μg m−3, respectively, with no pronounced seasonality. At Akdala (AKD) on northern margin of the Zhungaer Basin, the average concentrations were similar (mean OC = 2.9 μg m−3 and EC = 0.35 μg m−3), but the concentrations were higher in winter. The aerosol mass at both sites was dominated by OC and SO42−, but a stronger contribution from soil dust was observed at AKD. At ZUZ, NO3− showed a unique weather-related fluctuation in PM10 with a periodicity of ∼1 week. Anthropogenic sources in the Sichuan Basin and southeastern Yunnan Province evidently influence ZUZ in summer and autumn while pollutants from Russia and the China–Mongolia border affect AKD nearly all year. The identification of these upwind sources demonstrates that transboundary transport needs to be taken into account when assessing air quality in remote parts of China.  相似文献   

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