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1.
Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation. 相似文献
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L. Bourcier K. Sellegri P. Chausse J. M. Pichon P. Laj 《Journal of Atmospheric Chemistry》2012,69(1):47-66
The size-segregated chemical composition of aerosol particles was investigated during 1?year at the puy de D?me (1,465?m?a.s.l.), France. These measurements aimed to a better understanding of the influence of the air mass origin on the size-segregated chemical composition of the aerosol at an altitude site. Mountain site measurements are important because they are representative of long range transport and useful for model validation. PM1 mass concentration exhibits a seasonal variability with a summer maximum. The composition of PM1 did not change significantly in terms of relative contribution of water soluble inorganic ions but is rather variable in term of total mass concentrations. For the PM10-1, a different seasonal behaviour was found with maxima concentrations in autumn-winter. Aerosols were classified into four different categories according to their air mass origin: marine, marine modified, continental and Mediterranean. The PM10 aerosol mass at 50?% relative humidity was close to 2.5???g?m?3 in the marine, 4.3???g?m?3 in the marine modified, 10.3???g?m?3 in the continental and 7.7???g?m?3 in the Mediterranean sectors. We noted that the influence of the air mass origin (on the chemical properties) could be seen especially on the PM10-1. A significant PM10-1 mode was found in marine, modified marine, and Mediterranean air masses, and PM1 dominated in the continental air masses samples. As a result, the aerosol chemical composition variability at the puy de D?me is a function of both the season and air mass type and we provide a chemical composition of the aerosol as a function of each of these environmental factors. 相似文献
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Alan L. Dick 《Journal of Atmospheric Chemistry》1990,11(1-2):179-196
A model has been set up to investigate the wet and dry aerosol removal processes which occur in clean air over the Antarctic Peninsula. Input for the model was obtained from bulk chemical analysis and scanning electron microscopy of aerosol and snow samples collected simultaneously at remote sites around the Peninsula. The model predicts that sulphate and sea-salt aerosol will be removed mainly in-cloud by riming of falling snow and ice crystals. Crustal aerosol is principally removed by acting as nuclei for these crystals and by impaction on falling snow. For the largest, locally-generated aerosol dry deposition is indicated as the major removal process. These findings suggest a possible mechanism for the observed air/snow fractionation. 相似文献
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Anthony J. Dore Douglas W. Johnson Simon R. Osborne Thomas W. Choularton Keith N. Bower Meinrat O. Andreae Brian J. Bandy 《Tellus. Series B, Chemical and physical meteorology》2000,52(2):452-462
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
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I. Garbariene K. Kvietkus J. ?akalys J. Ovadnevait? D. ?eburnis 《Journal of Atmospheric Chemistry》2012,69(2):159-174
An Aerodyne quadruple aerosol mass spectrometer (Q-AMS) has been used to provide on-line measurements of size dependent chemical composition of fine aerosol particles (PM1) at the Air Pollution Research Station in Preila, Lithuania, representing the east Baltic region. The size dependent chemical composition measurements by AMS have revealed that in marine air masses 118?nm mode organics-containing particles were fresher compared to sulfate-containing particles (295?nm), likely originated as secondary aerosol from forest emissions or produced by primary sea spray over the Baltic Sea. In polluted continental air masses sulfate and organics were highly internally mixed and aged. The mass spectral results indicated that the major components of organic compounds were oxygenated organic species with strong signals at m/z 18, 43, 44 with several specific features. Positive matrix factorization (PMF) of AMS organic mass spectral data has identified three factors: aged oxygenated low-volatility organic aerosol (LV-OOA), less oxygenated semi-volatile organic aerosol (SV-OOA), and biogenic organic aerosol (BGOA) of either terrestrial or marine origin. The measurements were compared with a real-time particulate matter Beta Absorption Monitor (Thermo ESM Andersen) and Micro Orifice Uniform Deposit Impactor (MOUDI) data. The intercomparison showed a good correlation and a stable ratio between PM1 and PM2.5 concentrations. A comparison of the on-line Q-AMS data and the off-line MOUDI fine particle (<1???m) data yielded a reasonable agreement in size distributions but not the absolute mass concentrations due to sampling conditions, evaporation of acidic species from sampling substrates and bounce of the particles in the MOUDI. 相似文献
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GUILÉNE GÉRÉMY WOLFRAM WOBROCK REA I. FLOSSMANN ALFONS SCHWARZENBÖCK STEPHAN MERTES 《Tellus. Series B, Chemical and physical meteorology》2000,52(3):959-979
During February 1997, one of the 2 observational periods of CIME ( c loud i ce m ountain e xperiment), a joint field experiment funded by the European Commission, took place on the summit of the Puy de Dōme in the centre of France. During this experiment the droplet spectra were measured with an FSSP and the aerosol particles in the drops and in the interstitial particle phase were measured with a counterflow virtual impactor and a round jet impactor inside a windtunnel. Very low aerosol particle and drop concentrations were observed and particles as small as 25 nm in diameter were found to activate. Two datasets obtained on 15 February and 17 February were used to study the activation of the small Aitken‐mode particles and the spectral form of the droplet spectrum and the scavenging fraction. Numerous sensitivity studies were performed investigating the rôle of the number density and chemical composition of the aerosol particles. The rôle of mixing inside the orographic cloud was studied by using a new technique. It considers the fact that the air arriving on the summit of the Puy de Dôme is a mixture of air of different origins. Thus, it weighs the results of a spectral scavenging model (DESCAM or EXMIX) calculated along a number of individual trajectories. The weighing function is derived from tracer and trajectory studies with a 3‐dimensional mesoscale model. The model was able to reproduce the activation of aerosol particles as small as 25 nm. It was caused by the low aerosol particle number concentrations. In general, we can conclude that the variability found in the sensitivity tests of the dynamical and chemical factors allows to reproduce the shape of the observed results. As too many free parameters exit at the moment we cannot quantify the contribution of each factor studied to the observed scavenging fraction, however, it seems that dynamics dominates. 相似文献
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Stefaan Hoornaert Ricardo Henrique Moreton Godoi René Van Grieken 《Journal of Atmospheric Chemistry》2003,46(3):271-293
In the framework of the 2nd Aerosol Characterization Experiment (ACE-2), in June and July 1997, size segregated samples were collected for single particle analysis on the island of Tenerife, in both the marine boundary layer (MBL) and the free troposphere (FT), to study the characteristics of the North Atlantic aerosol. A systematic assessment was made of the aerosol under background conditions and when the environment was perturbed by European emissions and/or Saharan dust. The aerosol particles were analysed by automated and manual SEM-EDX, followed by cluster analysis to identify the different particle types and their abundance. Basing on back trajectory calculations, particle numbers and volume concentrations, different periods can be identified regarding the origin of the sampled air masses. In the FT, the air masses were classified as clean Atlantic, Saharan dust from Africa or pollution from Europe. In the MBL, air masses were classified as clean, polluted or perturbed by emissions from Europe. For both the FT and MBL samples, the main changes in chemical composition were observed between the fine and coarse mode aerosol. The FT fine mode aerosol is dominated by S-poor aluminosilicates (62%) in the event of the dust samples or sulphates, carbonaceous particles (20%) and S-rich aluminosilicates (46%) in the polluted samples. For the larger fractions, a strong decreasing trend was observed for the sulphates (less than 20%) and carbonaceous particles (10%) in the polluted samples. The MBL fine mode was completely dominated by S-rich particles (polluted 55% and perturbed 59%), and to a lesser extent, carbonaceous and aged sea salt particles. In the coarse mode, the polluted air mass is dominated by sea salt particles (62%). Contrary to the fine fraction, the polluted air mass in the coarse fraction contained 5.3% of S-rich particles. The combined interpretation of the data from the analysis of size-fractioned particles and the calculated backward trajectories for air masses coming from Europe, Africa and the Atlantic, results in better insights on aerosol chemistry, especially for the comparison of the particle composition in the FT and the MBL. 相似文献
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Admir C. Targino Kevin J. Noone Frank Drewnick Johannes Schneider Radovan Krejci Gustavo Olivares Silke Hings Stephan Borrmann 《Atmospheric Research》2007,86(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
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《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
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Aerosol particles are of particular importance because of their impacts on cloud development and precipitation processes over land and ocean. Aerosol properties as well as meteorological observations from the Department of Energy Atmospheric Radiation Measurement(ARM) platform situated in the Southern Great Plains(SGP) are utilized in this study to illustrate the dependence of continental cloud condensation nuclei(CCN) number concentration(NCCN) on aerosol type and transport pathways. ARM-SGP observations from the 2011 Midlatitude Continental Convective Clouds Experiment field campaign are presented in this study and compared with our previous work during the 2009–10 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer field campaign over the current ARM Eastern North Atlantic site. Northerly winds over the SGP reflect clean, continental conditions with aerosol scattering coefficient(σ_(sp)) values less than 20 Mm~(-1) and NCCNvalues less than 100 cm~(-3). However, southerly winds over the SGP are responsible for the observed moderate to high correlation(R)among aerosol loading(σ_(sp) 60 Mm~(-1)) and NCCN, carbonaceous chemical species(biomass burning smoke), and precipitable water vapor. This suggests a common transport mechanism for smoke aerosols and moisture via the Gulf of Mexico,indicating a strong dependence on air mass type. NASA MERRA~(-2) reanalysis aerosol and chemical data are moderately to highly correlated with surface ARM-SGP data, suggesting that this facility can represent surface aerosol conditions in the SGP, especially during strong aerosol loading events that transport via the Gulf of Mexico. Future long-term investigations will help to understand the seasonal influences of air masses on aerosol, CCN, and cloud properties over land in comparison to over ocean. 相似文献
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利用2014年7月黄山光明顶观测获得的气溶胶数浓度、气溶胶数谱数据,对黄山夏季气溶胶数浓度及谱分布特征进行分析,并在此基础上对气溶胶数谱进行了对数正态分布拟合。研究结果表明:黄山夏季气溶胶平均数浓度约为3 518.27 cm~(-3),主要集中在爱根核模态;气溶胶平均数浓度日变化呈双峰分布,峰值浓度的出现伴随着小粒子的增多。气溶胶数浓度与相对湿度和风速成负相关,高浓度的气溶胶多出现在较弱的东南风时;积聚模态气溶胶数浓度受风向影响显著。不同气团背景下气溶胶数谱差异集中在小于100 nm和500~1 000 nm粒径范围。爱根核模态气溶胶在高湿的西南气团影响下数浓度最低、谱较窄,而高温、低湿的东南气团对应的气溶胶数浓度最高、谱最宽,北方气团对应的气溶胶数浓度和谱宽居中;500~1 000 nm粒径范围气溶胶数谱分布特征与之相反。不同背景的气溶胶数谱和体积谱均可采用爱根模态、积聚模态1和积聚模态2三个模态进行对数正态分布拟合,但不同气团背景下的各模态谱型参数差异较大。 相似文献
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Maud Leriche R. Lyana Curier Laurent Deguillaume Dimitri Caro Karine Sellegri Nadine Chaumerliac 《Journal of Atmospheric Chemistry》2007,57(3):281-297
The Model of Multiphase Cloud Chemistry M2C2 has recently been extended to account for nucleation scavenging of aerosol particles in the cloud water chemical composition. This extended version has been applied to multiphase measurements available at the Puy de Dôme station for typical wintertime anthropogenic air masses. The simulated ion concentrations in cloud water are in reasonable agreement with the experimental data. The analysis of the sources of the chemical species in cloud water shows an important contribution from nucleation scavenging of particles which prevails for nitrate, sulphate and ammonium. Moreover, the simulation shows that iron, which comes only from the dissolution of aerosol particles in cloud water, has a significant contribution in the hydroxyl radical production. Finally, the simulated phase partitioning of chemical species in cloud are compared with measurements. Numerical results show an underestimation of interstitial particulate phase fraction with respect to the measurements, which could be due to an overestimation of activated mass by the model. However, the simulated number scavenging efficiency of particles agrees well with the measured value of 40% of total number of aerosol particles activated in cloud droplets. Concerning the origin of chemical species in cloud water, the model reproduces quite well the contribution of gas and aerosol scavenging estimated from measurements. In addition, the simulation provides the contribution of in-cloud chemical reactivity to cloud water concentrations. 相似文献
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Aerosol properties and air pollutants over an urban area 总被引：2，自引：0，他引：2
For a better understanding of urban aerosols, sun/sky photometry has been undertaken at the Kinki University campus in Higashi-Osaka as a NASA/AERONET station since 2002. A new instrument, the SPM-613D (Kimoto Electric), has been taking measurements at the same site since March 15, 2004. The relationship between aerosol properties obtained from radiometry with AERONET and the SPM measurements is examined. It is found that there is a linear correlation between SPM concentrations and aerosol properties, which indicates that aerosol characteristics can be estimated from SPM data, and vice versa.It is also shown that the air quality of the Higashi-Osaka site is poor due to not only the anthropogenic particles by local emissions, such as diesel vehicles and chemical industries, but also due to the dust particles coming from continental desert areas by large scale climatic conditions. 相似文献
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《Atmospheric Research》2007,83(3-4):643-651
For a better understanding of urban aerosols, sun/sky photometry has been undertaken at the Kinki University campus in Higashi-Osaka as a NASA/AERONET station since 2002. A new instrument, the SPM-613D (Kimoto Electric), has been taking measurements at the same site since March 15, 2004. The relationship between aerosol properties obtained from radiometry with AERONET and the SPM measurements is examined. It is found that there is a linear correlation between SPM concentrations and aerosol properties, which indicates that aerosol characteristics can be estimated from SPM data, and vice versa.It is also shown that the air quality of the Higashi-Osaka site is poor due to not only the anthropogenic particles by local emissions, such as diesel vehicles and chemical industries, but also due to the dust particles coming from continental desert areas by large scale climatic conditions. 相似文献
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Doug W. Johnson Simon Osborne Robert Wood Karsten Suhre Patricia K. Quinn Tim Bates M. O. Andreae Kevin J. Noone Paul Glantz Brian Bandy J. Rudolph Colin O'Dowd 《Tellus. Series B, Chemical and physical meteorology》2000,52(2):348-374
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