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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.
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   

3.
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   

4.
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   

5.
A closed-cell marine stratocumulus case during the Aerosol and Cloud Experiments in the Eastern North Atlantic (ACE-ENA) aircraft field campaign is selected to examine the heterogeneities of cloud and drizzle microphysical properties and the aerosol-cloud-precipitation interactions. The spatial and vertical variabilities of cloud and drizzle microphysics are found in two different sets of flight legs: Leg-1 and Leg-2, which are parallel and perpendicular to the cloud propagation, respectively. The cloud along Leg-2 was close to adiabatic, where cloud-droplet effective radius and liquid water content linearly increase from cloud base to cloud top with less drizzle. The cloud along Leg-1 was sub-adiabatic with lower cloud-droplet number concentration and larger cloud-droplet effective, but higher drizzle droplet number concentration, larger drizzle droplet median diameter and drizzle liquid water content. The heavier drizzle frequency and intensity on Leg-1 were enhanced by the collision-coalescence processes within cloud due to strong turbulence. The sub-cloud precipitation rate on Leg-1 was significantly higher than that along Leg-2. As a result, the sub-cloud accumulation mode aerosols and CCN on Leg-1 were depleted, but the coarse model aerosols increased. This further leads to a counter-intuitive phenomenon that the CCN is less than cloud-droplet number concentration for Leg-1. The average CCN loss rates are ?3.89 \begin{document}$\mathrm{c}{\mathrm{m}}^{-3}\;{\mathrm{h}}^{-1}$\end{document} and ?0.77 \begin{document}$\mathrm{c}{\mathrm{m}}^{-3}\;{\mathrm{h}}^{-1}$\end{document} on Leg-1 and Leg-2, respectively. The cloud and drizzle heterogeneities inside the same stratocumulus can significantly alter the sub-cloud aerosols and CCN budget. Hence it should be treated with caution in the aircraft assessment of aerosol-cloud-precipitation interactions.  相似文献   

6.
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   

7.
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   

8.
In this study, we present a relationship between total accumulation mode aerosol mass concentrations and cloud droplet number concentrations ( N d). The fundamental aim with the present method is to arrive at a physically‐based conversion algorithm in which each step in the conversion is based on real physical processes that occur and can be observed in the atmosphere, and in which all of the fields involved can be observed or modeled. In the last conversion (the critical part in the algorithm), we use measurements of the size distributions of cloud droplet residual particles for different pollution conditions. This conversion assumes that the size of the residual particles can be described with a lognormal distribution function and uses the Hatch–Choate relationship to convert between residual volume and number. The relatively sparse data set with which we have developed the present algorithm results in a course classification of the aerosol mass field. Consequently, uncertainties need to be recognized when using the algorithm in its present form in model calculations. The algorithm has been used on data from 15 days and the agreement between calculated and observed N d values is, with one exception, within a factor of 2 and for many of these cases also much better than a factor of 2. In addition to the results of the algorithm itself, we also present a least‐squares fit to the predicted N d values. To improve the algorithm in the longer‐term requires more data of scavenging fractions, particle chemical composition and density, and residual particle size distributions as a function of aerosol mass loading and cloud type.  相似文献   

9.
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   

10.
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   

11.
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   

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.
The evolution of cloud droplet size spectra is calculated using an adiabatic condensational growth model. Broadness (e.g., standard deviation of diameter) of cloud droplet spectra in adiabatic cloud parcels was determined to be critically dependent on cloud supersaturation. Although droplet spectra become narrower as growth continues, the rate of narrowing is slower when cloud supersaturation is lower. This actually leads to broader droplet spectra for more continental clouds or for weaker updrafts because both of these conditions are associated with lower cloud supersaturations. More continental type clouds, which have higher concentrations of smaller droplets, were indeed found to have larger dispersions (standard deviation of diameter/mean diameter of cloud droplets). Some of these results were consistent with observations, but the larger dispersions that were much more commonly observed for continental compared to maritime clouds were due almost exclusively to smaller droplets rather than broader droplet distributions. Contrary to the model calculations, typical observations show that cleaner clouds usually have broader droplet spectra. The gaps in magnitude between theory and observations of broadness are significant in all clouds. When cloud parcels that had ascended under different updraft conditions were compared at a constant cloud altitude, parcels with lower updrafts were predicted to have broader droplet spectra with larger mean diameters. This trend of apparent spectral broadening was consistent with observations for some near-adiabatic cloud parcels.  相似文献   

14.
Climate sensitivity to cloud optical properties   总被引：1，自引：0，他引：1  
A radiative–convective model was developed to investigate the sensitivity of climate to cloud optical properties and the related feedback processes. This model demonstrates that the Earth's surface temperature increases with cloud optical depth when the clouds are very thin but decreases with cloud optical depth when the cloud shortwave (solar) radiative forcing is larger than the cloud longwave (terrestrial) radiative forcing. When clouds are included in the model, the magnitude of the greenhouse effect due to a doubling of the CO2 concentration varies with the cloudoptical depth: the thicker the clouds, the weaker the greenhouse warming. In addition, a small variation in the cloud droplet size has a larger impact on the equilibrium state temperature in the lower atmosphere than the warming caused by a doubling of the CO2 concentration: a 2% increase in the average cloud droplet size per degree increase in temperature doubles the warming caused by the doubling of the CO2 concentration. These findings suggest that physically reliable correlations between the cloud droplet size and macrophysical meteorological variables such as temperature, wind and water vapor fields are needed on a global climate scale to assess the climate impact of increases in greenhouse gases.  相似文献   

15.
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   

16.
基于飞机观测资料的降水粒子反射率因子阈值分析   总被引：2，自引：0，他引：2       下载免费PDF全文
降水粒子对云的生消和演化有非常重要的影响。毫米波雷达适合观测非降水云和弱降水云。利用毫米波雷达数据判断云内降水粒子生成与否有很高的实用价值。本文利用飞机观测的云滴谱数据计算云的反射率因子。将其与雷达探测值进行比对,发现两者有较好的一致性。因此利用滴谱计算的降水粒子反射率因子阈值可以作为雷达判断降水粒子生成的指标。通过分析滴谱计算云滴和降水粒子的反射率因子的概率密度函数可以得到用于区分云滴和降水粒子的反射率因子阈值。通常,云滴的反射率因子不超过-5dBz,降水粒子的反射率因子高于-20dBz,-15~-12dBz可作为判断降水粒子出现的阈值。  相似文献   

17.
The present work summarises the results of a 2‐year study of wet‐only sequential deposition in 2 rural areas (Alcan¯iz and Morella) located at different distances from a large coal‐fired power station. Precipitation chemistry was characterised by relatively high , Ca2+ and average concentrations. Sequential study of single precipitation events showed that concentrations of most of the ions studied decreased exponentially throughout single precipitation events, with a sharper decrease in concentrations at the beginning of the event. Usually, 40 to 80% of the wet‐only deposition of major ions occurred in the first 2 mm. pH measurements, ranging from 5.6 to 8.1, showed a decrease in the pH values throughout a precipitation event. Deposition levels of Ca2+ and accounted for the neutralisation of major acidic species in the precipitation events except in 5 rain episodes sampled at Morella. The sequential study of the evolution of the ratio during a single precipitation allowed us to identify potential acidic rainfall fractions after an initial volume of precipitation, after most of the Ca2+ in atmospheric particles had been scavenged. A higher neutralisation capacity was deduced for Alcan¯iz owing to the higher atmospheric levels of natural carbonates and .  相似文献   

18.
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   

19.
The atmospheric sulfur cycle of the remote Arctic marine boundary layer is studied using trajectories and measurements of sulfur compounds from the International Arctic Ocean Expedition 1991, along with a pseudo-Lagrangian approach and an analytical model. The dimethyl sulfide [DMS(g)] turnover time was  h. Only  % of DMS(g) followed reaction paths to sulfur dioxide [SO2(g)], sub-micrometre aerosol non-seasalt sulfate (nss-SO42−) or methane sulfonate (MSA). During the first 3 d of transport over the pack ice, fog deposition and drizzle resulted in short turnover times;  h for SO2(g),  h for MSA and  h for nss-SO42−. Therefore, DMS(g) will, owing to its origin along or south of the ice edge and longer turnover time, survive the original sub-micrometre sulfur aerosol mass and gradually replace it with new biogenic sulfur aerosol mass. The advection of DMS(g) along with heat and moisture will influence the clouds and fogs over the Arctic pack ice through the formation of cloud condensation nuclei (CCN). If the pack ice cover were to decrease owing to a climate change, the total Arctic Ocean DMS production would change, and potentially there could be an ice–DMS–cloud–albedo climate feedback effect, but it would be accompanied by changes in the fog aerosol sink.  相似文献   

20.
The POLDER instrument is devoted to global observations of the solar radiation reflected by the Earth–atmosphere system. The airborne version of the instrument was operated during the ACE‐2 experiment, more particularly as a component of the CLOUDYCOLUMN project of ACE‐2 that was conducted in summer 1997 over the subtropical northeastern Atlantic ocean. CLOUDYCOLUMN is a coordinated project specifically dedicated to the study of the indirect effect of aerosols. In this context, the airborne POLDER was assigned to remote measurements of the cloud optical and radiative properties, namely the cloud optical thickness and the cloud albedo. This paper presents the retrievals of those 2 cloud parameters for 2 golden days of the campaign 26 June and 9 July 1997. Coincident spaceborne ADEOS‐POLDER data from 2 orbits over the ACE‐2 area on 26 June are also analyzed. 26 June corresponds to a pure air marine case and 9 July is a polluted air case. The multidirectional viewing capability of airborne POLDER is here demonstrated to be very useful to estimate the effective radius of cloud droplet that characterizes the observed stratocumulus clouds. A 12 μm cloud droplet size distribution appears to be a suitable cloud droplet model in the pure marine cloud case study. For the polluted case the mean retrieved effective droplet radius is of the order of 6–10 μm. This only preliminary result can be interpreted as a confirmation of the indirect effect of aerosols. It is consistent with the significant increase in droplet concentration measured in polluted marine clouds compared to clean marine ones. Further investigations and comparisons to in‐situ microphysical measurements are now needed.  相似文献   

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