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1.
The interpretation of the physico-chemical processes in clouds is facilitated by segregating in situ cloud elements from their carrier gas and small particles (interstitial aerosol). Thus, the present study focuses on the quantitative phase segregation of interstitial air from cloud phase by two complementary samplers with microphysical on-line analysis of the separated phases. An improved counterflow virtual impactor (CVI) was developed for the collection and subsequent evaporation of the condensed phase, releasing dissolved gaseous material and residual particles. This sampler operates in the size range of few micrometers up to 50 μm in cloud element diameter and is matched by an interstitial Round Jet Impactor sampling the gas phase with interstitial particles. Calibrations of both samplers verified the calculated cut sizes D50 of 4, 5, and 6 μm and quantified the slope of the collection efficiency curves. Until this study no direct CVI measurements of the residual particle sizes far below the diameter of 0.1 μm were available. For the first time a CVI was connected to a Differential Mobility Particle Sizer (DMPS) scanning between 25 nm and 850 nm, thus, including the entire Aitken mode in the residual size analysis. Cloud studies on the Puy de Dôme, France, revealed residual particle sizes including Aitken mode (diameter D<100 nm) and accumulation mode (D>100 nm). A major feature of the CVI data is expressed by the fact that despite incomplete incorporation of accumulation mode particles in cloud elements there are contributions of particles with diameters smaller than 0.1 μm to the number of residual particles. Cloud entrainment from height levels above the maximum supersaturation as wells as the size-dependent chemical composition of the aerosol population most likely produced the S-shaped size-dependent partitioning of residual particles. Compared to earlier studies the 50% partitioning diameters dropped significantly below 100 nm to roughly 70 nm.  相似文献   

2.
Direct physical measurements of particle mass and number concentration indicate an increase in overall aerosol mass resulting from cloud processing, most likely through aqueous-phase chemistry (e.g., SO2 oxidation). Measurements conducted in the Pennines of Northern England reveal an average increase of 14 to 20% in dry aerosol mass (0.003<particle diameter<0.9 μm) after aerosol passage through an orographic cloud. The rate of in-cloud mass production is most sensitive to changes in upwind particle size distributions, SO2 concentration, and cloud water acidity. Newly-formed mass appears in size range between 200 and 600 nm and enhances the bimodality of the particle number distribution after cloud processing. Furthermore, the cloud-produced mass is estimated to increase total light scattering, bsp, by 18 to 24%. The scattering efficiency of the dry, cloud-generated aerosol is 5.0±0.3 m2 g−1 and increases to 7.4±0.7 m2 g−1 when adjusted to 90% relative humidity by incorporating particle hygroscopicity data.  相似文献   

3.
In November 2004–January 2005, a micro orifice uniform deposit impactor (MOUDI) and a Nanometer (nanometer)-MOUDI were used in the center of Taiwan to measure particle size (18 nm particle size 18 μm) distributions of atmospheric aerosols at a traffic site during the winter period. The average Mass in Media Aerodynamic Diameter (MMAD) of suspended particles is 0.99 μm this study. As for the ultra fine and nanometer (nanometer) particle mode, the composition order for these major ions species was SO42− NH4+ NO3− Mg2+ Ca2+ Na+ K+ Cl−. An ion Chromatography (DIONEX-100) was used to analyze major anion species, Cl−, NO3−, SO42− and cation species, NH4+Na+, K+, Ca2+Mg2+. Their concentrations were also extracted from various particles size modes (nanometer (nanometer), ultra fine, fine and coarse). The results obtained in this study also indicated that the average portions for the major ionic species (SO42−, NH4+ and Mg2+) in the nanometer (nanometer), ultra fine, fine and coarse particulate modes are about 34%, 37%, 63% and 30%, respectively at this traffic sampling site during the winter period.  相似文献   

4.
Size segregated sampling of aerosol particles at the coal-fired power station Šoštanj, Slovenia was performed by a newly developed system. In addition, simultaneous sampling of particles was performed at two locations, Velenje and Veliki vrh, chosen on the basis of long term monitoring of SO2 in the influential area of power plant. The signature of the power plant (e.g. characteristic size distributions of some typical trace elements) was identified. For elements, like As, Mo, Cd and Ga, which are typical for coal combustion, the highest concentrations were observed in the size range between 1 and 4 μm. For Se and sometimes for Ga two modes were identified, first between 0.1 and 0.5 μm and second between 1 and 4 μm. Ratios between the average concentrations of selected elements in fine and coarse particles collected at Veliki vrh (the most influenced location) and Velenje (usually not influenced by the thermo power station) were significantly higher than 1 in the case of Mo and Se for coarse and fine size range, while for As the ratio was higher than 1 for the coarse fraction. Consequently, Mo, Se and As were found as the most important tracers for the emissions from the investigated source. On the basis of the ratios between the concentrations of elements measured in particles at low and high SO2 concentrations at Veliki vrh, Cd was shown to be a typical tracer as well. Our results definitely showed that size segregated measurements of particles at the source and in the influenced area give more precise information on the influence of source to the surrounding region. It was found that patterns of size distributions for typical trace elements observed at the source are found also in the influenced area, i.e. Veliki vrh.  相似文献   

5.
Radar parameters including radar reflectivity,Doppler velocity,and Doppler spectrum width were obtained from Doppler spectrum moments.The Doppler spectrum moment is the convolution of both the particle spectrum and the mean air vertical motion.Unlike strong precipitation,the motion of particles in cirrus clouds is quite close to the air motion around them.In this study,a method of Doppler moments was developed and used to retrieve cirrus cloud microphysical properties such as the mean air vertical velocity,mass-weighted diameter,effective particle size,and ice content.Ice content values were retrieved using both the Doppler spectrum method and classic Z-IWC(radar reflectivity-ice water content) relationships;however,the former is a more reasonable method.  相似文献   

6.
南京霾天颗粒物数浓度特征及其受气象条件影响分析   总被引：5，自引：3，他引：2  
2013年12月,我国中东部地区爆发持续性霾污染过程。本研究利用空气动力学粒径谱仪和气溶胶粒径谱仪在线观测这次霾污染过程中13.6~20 000 nm颗粒物数浓度,结合气象参数和颗粒物化学组分对南京霾天颗粒物数浓度分布特征,及其与气象条件相关性进行分析。结果表明,霾天颗粒物主要分布在积聚模态,且500~1 000 nm和1 000~2 500 nm粒径段颗粒物数浓度的增多是造成霾天能见度低的主要原因;随着相对湿度的增大,13.6~100 nm粒径段颗粒物数浓度逐渐降低,而大于100 nm颗粒物数浓度升高;500~1 000 nm和1 000~2 500 nm粒径段颗粒物数浓度受相对湿度的影响尤为明显,并且这2个粒径段颗粒物受气态污染物(SO2,NOX)的二次转化影响较大。霾污染期间南京大气颗粒物主要来自南京东南和西北方向的污染源排放,颗粒物数浓度总体上与风速呈负相关关系;温度对颗粒物数浓度的影响主要集中在13.6~100 nm粒径段;边界层的高度与粒径100 nm颗粒物呈负相关性,边界层的抬升反而利于超细粒子的生成和增长;逆温层的强度对超细粒子的作用更为明显。  相似文献   

7.
In this study the possible conditions for new aerosol particle formation in a background area of Helsinki have been analysed. The measurements of aerosol particle size distribution, main gaseous pollutant compounds, UV spectra and meteorological parameters were performed during April–May 1993. The main interest was concentrated on the investigations of photochemical OH radical formation, the oxidation of gas phase SO2 to H2SO4 and the formation of H2SO4---H2O aerosol particles. The measurements were analysed using a model for OH radical formation and aerosol dynamics. The analysis of aerosol size distributions was carried out using positive matrix factorization. The main conclusion is that based on our model analysis no evidence of new particle formation in the vicinity of the measurement station was found. However, the high concentrations of aerosol particles in the ultrafine size range indicate that some other particle formation pathways are to be considered.  相似文献   

8.
机载光阵探头探测时,云粒子(液态和固态)进入二维光阵探头的采样区前,会因与探头探测臂发生机械碰撞,或者与探头外壳产生的湍流和风切变相互作用而破碎。破碎程度与粒子类型、大小、粒子密度、探头入口设计以及飞行空速等有关。利用2008年7~9月探测飞机(Y-12)在山西省太原地区的航测资料并对飞机采样期间的云粒子破碎现象进行介绍和分析,分析结果表明,粒子到达时间间隔分布具有双模态特征:长时间模态是粒子空间分布的真实结构,短时间模态则是云粒子破碎的结果。提出用粒子到达时间间隔阈值作为粒子破碎的判定标准,给出适用于2008年太原地区航测资料的粒子破碎识别阈值,其中适合于探头云粒子成像仪(CIP)的阈值是2×10-5 s,而探头降水粒子成像仪(PIP)的阈值是1×10-4 s。所提的阈值对于以Y-12为机载探测平台,以CIP和PIP探头为探测仪器所获取的其它航次云微物理图像资料的粒子破碎处理也是有一定的参考使用价值。  相似文献   

9.
The changing chemical composition of cloud water and precipitation in the Western Sudety Mountains are discussed against the background of air-pollution changes in the Black Triangle since the 1980s until September 2004. A marked reduction of sulphur dioxide emissions between the early 1990's and the present (from almost 2 million tons to around 0.2 million tons) has been observed, with a substantial decline of sulphate and hydrogen concentration in cloud water (SO42− from more than 200 to around 70 μmol l− 1; H+ from 150 to 50 μmol l− 1) and precipitation (SO42− from around 80 to 20–30 μmol l− 1; H+ from around 60 to 10–15 μmol l− 1) samples. At some sites, where fog/cloud becomes the major source of pollutants, deposition hot spots are still observed where, for example, nitrogen deposition can exceed 20 times the relevant critical load. The results show that monitoring of cloud water chemistry can be a sensitive indicator of pollutant emissions.  相似文献   

10.
A multifunctional HTDMA system with a robust temperature control   总被引：3，自引：0，他引：3  
The hygroscopicity of atmospheric aerosols significantly influences their size distribution, cloud condensation nuclei ability, atmospheric residence time, and climate forcing. In order to investigate the hygroscopic behavior of aerosol particles and serious haze in China, a Hygroscopic Tandem Differential Mobility Analyzers (HTDMA) system was designed and constructed at Fudan University. It can function as a scanning mobility particle sizing system to measure particle size distribution in the range of 20--1000 nm in diameter, as well as a hygroscopicity analyzer for aerosol particles with diameters between 20--400 nm in the range of 20%--90% RH (relative humidity). It can also measure the effect of uptake of inorganic acids or semi-VOCs on the hygroscopic behavior of aerosols, such as typical inorganic salts in atmospheric dust or their mixtures. The performance tests show that the system measured particle size of the standard polystyrene latex spheres (PSLs) is 197 nm, which is in excellent agreement with the certified diameter D=199±6 nm, as well as a standard deviation of the repeated runs SD=8.9x10-4. In addition, the measured hygroscopic growth factors of the model compounds, (NH4)2SO4 and NaNO3, agree with the Kohler theoretical curves. The results indicate that the HTDMA system is an excellent and powerful tool for studying the hygroscopic behavior of submicron aerosols and meets the demand required for laboratory research and fieldwork on atmospheric aerosols in China.  相似文献   

11.
A model with spectral microphysics was developed to describe the scavenging of nitrate aerosol particles and HNO3 gas. This model was incorporated into the dynamic framework of an entraining air parcel model with which we computed the uptake of nitrate by cloud drops whose size distribution changes with time because of condensation, collision-coalescence and break-up. Significant differences were found between the scavenging behavior of nitrate and our former results on the scavenging behavior of sulfate. These reflect the following chemical and microphysical differences between the two systems:
  1. nitrate particles occur in a larger size range than sulfate particles.
  2. HNO3 has a much greater solubility than SO2 and is taken up irreversibly inside the drops in contrast to SO2.
  3. nitric acid in the cloud water is formed directly on uptake of HNO3 gas whereas on uptake of SO2 sulfuric acid is formed only after the reaction with oxidizing agents such as e.g., H2O2 or O3.
  4. nitrate resulting from uptake of HNO3 is confined mainly to small drops, whereas sulfate resulting from uptake of SO2 is most concentrated in the largest, oldest drops, which have had the greatest time for reaction.
Sensitivity studies showed that the nitrate concentration of small drops is significantly affected by the mass accommodation coefficient.  相似文献   

12.
A closure study of sub-micrometer aerosol particle hygroscopic behaviour   总被引：2，自引：0，他引：2  
The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.  相似文献   

13.
The chemical removal of SO2 in the presence of different aerosol systems has been investigated in laboratory experiments using a dynamic flow reactor. The aerosols consisted of wetted particles containing one of the following substances: MnCl2, Mn(NO3)2, MnSO4, CuCl2, Cu(NO3)2, CuSO4, FeCl3, NaCl. The SO2 removal rate R was measured as a function of the SO2 gas phase concentration (SO2)g, the spatial metal concentration CMe, and the relative humidity rH in the reactor. A first-order dependence with regard to (SO2)g was observed for each type of aerosol. For the Mn(II) and Cu(II) aerosols R was found to be a non-linear function of CMe except for MnSO4 and Cu(NO3)2 particles. The removal rate showed a significant increase with the relative humidity particularly when rH was close to the deliquescence point of the wetted particles. Among the Mn(II) and Cu(II) aerosols investigated Mn(NO3)2 was found to be most efficient for the chemical removal of SO2 at atmospheric background conditions, especially in haze and fog droplets. The results further indicate that the catalytic oxidation of S(IV) in such aerosol systems may be as efficient as its oxidation by H2O2 in cloud water.  相似文献   

14.
In November 1993 an airborne field study was performed in order to investigate the microphysical and radiative properties of cooling tower water clouds initiated by water vapour emissions and polluted by the exhaust from coal-fired power plants. The number-median diameter of the droplet size distributions of these artificial clouds was in the range of 13 μm. The concentration of smaller droplets (diameters dD < 10 μm) increased with height and horizontal distance from the cooling towers. Close to the cooling towers, bimodal spectra were found with a second mode at 19 μm. The liquid water content (LWC) ranged between 2 and 5 g/m3 and effective droplet radii (Re) between 6 and 9 μm were measured. LWC and Re decreased with altitude, whereas the droplet concentration (ND) remained approximately constant (about 2000 cm−3 ). An enrichment of interstitial aerosol particles with particle diameters (dp) smaller 0.2 μm compared to the power plant plume in the vicinity of the clouds was observed. Particle activation for dm > 0.3 μm. was evident, especially in cooling tower clouds further apart and separated from their sources. Furthermore, radiation measurements were performed, which revealed differences in the vertical profiles of downwelling solar and UV radiation flux densities inside the clouds.The effective droplet radius Re was parameterized in terms of LWC and ND using equations known from literature. The close agreement between measured and parameterized Re indicates a similar coupling of Re, LWC and ND as in natural clouds.By means of Mie calculations, volume scattering coefficients and asymmetry factors are derived for both the cloud droplets and the aerosol particles. For the cloud droplets, the optical parameters were described by parameterizations from the literature. The results show, that the link between radiative and microphysical properties of natural clouds is not changed by the extreme pollution of the artificial clouds.  相似文献   

15.
This work attempts to characterize metallic elements associated with atmospheric particulate matter on a dry deposition plate, a TE-PUF high-volume air sampler and a universal air sampler. Dry deposition fluxes of particulates and concentrations of total suspended particulate, fine (PM2.5) and coarse (PM2.5–10) particulate matters were collected at Taichung harbor sampling sites from August 2004 to January 2005. Chemical analyses of metallic elements were made using a flame atomic absorption spectrophotometer coupled with hollow cathode lamps. Concentrations of metal elements in the forms of coarse particles and fine particles as well as the coarse/fine particulate ratios were presented. Statistical methods such as correlation analysis, principal component analysis and enrichment factor analysis were performed to compare the chemical components and identify possible emission sources at the sampling sites. Metallic elements of Cu, Zn, Pb, Cr, Ni and Mg had higher EFcrust ratios in winter and spring than in summer and autumn. Diurnal and nocturnal variations of metallic element concentrations in fine and coarse particles were also discussed.  相似文献   

16.
The chemical conversion of emitted SO2 and SO3 to gaseous H2SO4 in nascent aircraft exhaust plumes and subsequent adsorption of the fully oxidized sulfur species on the surfaces of emitted combustion aerosols (soot) is investigated. Results are presented for the mass fractions of SO3 and H2SO4 acquired per soot particle early in the plume, suggesting that sulfur-induced activation is an efficient pathway to increase the ability of exhaust soot emitted at altitude to host heterogeneous chemical reactions and to trigger the formation of cirrus clouds.  相似文献   

17.
《Atmospheric Research》2008,87(3-4):225-240
During June and July 2003 the Sources and Origins of Atmospheric Cloud Droplets experiment (SOACED) was carried out on a mountain-top site in central Sweden. The main objective of the experiment was to characterise the microphysical and chemical properties of cloud droplet residuals and interstitial aerosol particles in continental clouds and to understand the processes controlling cloud properties at this location.Interstitial and residual aerosol size distributions, cloud liquid water content and species- and size-resolved aerosol mass concentrations are the main variables employed to address questions pertaining to the cloud droplet number concentration and scavenging efficiency during a stratocumulus cloud event observed on July 28, 2003. In this cloud event, about 56% of the aerosol mass was associated with organic species, whilst SO4 accounted for 23% and NH4 for 14%. NO3 and Cl made up about 7% of the total mass.The partitioning of the aerosol particles between cloud droplets and interstitial air has been studied in terms of their microphysical properties. The scavenging efficiency, defined as the fraction of particles activated into cloud elements compared to the total amount of particles, was investigated as a function of size. The scavenging efficiency curves displayed different shapes during the cloud event, from an S-shaped curve, with low scavenging efficiency in the Aitken mode and larger scavenging efficiency in the accumulation mode, to more unusual shapes where Aitken-mode particles were either solely activated or activated in addition to accumulation-mode particles.This study suggests that alterations of the aerosol chemical composition occurred during the measurement period, changing the hygroscopic nature of the CCN and decreasing their activation diameter. It is also hypothesized that entrainment of drier air aloft may have introduced inhomogeneities in the supersaturation field and modified the S-shaped scavenging curves.  相似文献   

18.
During June and July 2003 the Sources and Origins of Atmospheric Cloud Droplets experiment (SOACED) was carried out on a mountain-top site in central Sweden. The main objective of the experiment was to characterise the microphysical and chemical properties of cloud droplet residuals and interstitial aerosol particles in continental clouds and to understand the processes controlling cloud properties at this location.Interstitial and residual aerosol size distributions, cloud liquid water content and species- and size-resolved aerosol mass concentrations are the main variables employed to address questions pertaining to the cloud droplet number concentration and scavenging efficiency during a stratocumulus cloud event observed on July 28, 2003. In this cloud event, about 56% of the aerosol mass was associated with organic species, whilst SO4 accounted for 23% and NH4 for 14%. NO3 and Cl made up about 7% of the total mass.The partitioning of the aerosol particles between cloud droplets and interstitial air has been studied in terms of their microphysical properties. The scavenging efficiency, defined as the fraction of particles activated into cloud elements compared to the total amount of particles, was investigated as a function of size. The scavenging efficiency curves displayed different shapes during the cloud event, from an S-shaped curve, with low scavenging efficiency in the Aitken mode and larger scavenging efficiency in the accumulation mode, to more unusual shapes where Aitken-mode particles were either solely activated or activated in addition to accumulation-mode particles.This study suggests that alterations of the aerosol chemical composition occurred during the measurement period, changing the hygroscopic nature of the CCN and decreasing their activation diameter. It is also hypothesized that entrainment of drier air aloft may have introduced inhomogeneities in the supersaturation field and modified the S-shaped scavenging curves.  相似文献   

19.
为加深对南京地区重霾天气过程纳米尺度气溶胶物理特征的了解,对2017年12月21—25日的一次重霾天气过程进行了综合探测,利用宽范围粒径谱仪观测了此次过程中10～1 000 nm颗粒物数浓度,并结合能见度等气象要素,对重霾期间纳米气溶胶谱分布进行了分析。结果表明:此次霾重污染过程出现在低温、高湿、气压上升期间;与非重污染时期相比,重污染期间N_(10-20)与N_(20-100)降低,N_(100-1000)升高;重污染期间气溶胶粒子平均数浓度为17 035个/cm~3,低于非重污染期间粒子数浓度,N_(100-1000)占总数浓度的55.05%;重霾发生期间纳米气溶胶数浓度谱为单峰结构,峰值在100 nm附近,随着污染加重,纳米气溶胶峰值粒径向大粒径偏移,粒子向大粒径段集中;不同温度对不同粒径粒子数浓度的影响不同,20～100 nm粒径段气溶胶与数浓度与温度呈反相关性,100～500 nm粒子数浓度与温度呈正相关性.  相似文献   

20.
A chemistry module has been incorporated into a Lagrangian type model that computes the dynamics and microphysics of an orographical cloud formed in moist air flowing over the summit of Great Dun Fell (GDF) in England. The cloud droplets grow on a maritime aerosol which is assumed to be an external mixture of sea-salt particles and ammonium-sulfate particles. The dry particle radii are in the range 10 nm<r<1 µm. The gas-phase chemical reaction scheme considers reactions of nitrogen compounds that are important at night. The treatment of scavenging of gases into the aqueous phase in the model takes into account the different solubilities and accommodation coefficients. The chemistry in the aqueous phase focusses on the oxidation of S(IV) via different pathways.Sensitivity analyses have been performed to investigate deviations from gas-liquid equilibria according to Henry's law and also to study the influence of iron and of nitrogen compounds on the aqueous-phase oxidation of dissolved SO2. When addressing these questions, special attention has been given to the dependence on the droplet size distribution and on the chemical composition of the cloud condensation nuclei on which the droplets have formed. It was found that the oxidation of S(IV) via a chain reaction of sulfur radicals can be important under conditions where H2O2 is low. However, major uncertainties remain with respect to the interaction of iron with the radical chain. It was shown that mixing of individual cloud droplets, which are not in equilibrium according to Henry's law, can result in a bulk sample in equilibrium with the ambient air. The dependence of the aqueous-phase concentrations on the size of the cloud droplets is discussed for iron, chloride and NO3.  相似文献   

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