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1.
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
2.
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
3.
《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
4.
We studied the effect of supercooled cloud droplets on the diffusional growth rate of isolated ice plates and ice columns by approximating the shape of a plate as an oblate spheroid and a column as a prolate spheroid. This work is an extension of the pioneering work of Marshall and Palmer [Marshall, J.S. and Langleben, M.P., A theory of snow-crystal habit and growth, J. Met., 11, 104–120, 1954] who studied the influence of cloud droplets on the growth rate of spherical ice crystals. The vapour density field for oblate and prolate spheroids was obtained by solving Helmholtz's equation with the assumption that the vapour at the ice surface had the equilibrium value. As result, it was possible to calculate separately the temporal evolution of the axis length and the mass of the snow crystals.The results indicate that the presence of cloud droplets around the snow crystal can increase by around 10% of the ice growth rate relative to an environment free of cloud droplets. The magnitude of the growth enhancement is proportional to the liquid water content. The results also corroborate the importance of the shape and aspect ratio on the crystal growth. A general mass growth rate equation for diffusional growth was found, which incorporates effects of cloud droplets and crystal shape through the size and aspect ratio of the snow crystal. 相似文献
5.
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
6.
将DeMott冰核浓度参数化方案引入到WRF中尺度数值模式中,模拟了新疆阿克苏地区一次多单体型强对流风暴,并对背景大气条件和沙尘条件下气溶胶作为冰核,对云中微物理结构和降水变化的影响进行了敏感性试验和对比分析,结果显示:在背景大气条件和沙尘条件下增加冰核浓度对降水中心强度影响较小,并且总体上看降水分布变化不大,但是降水局部的变化量较明显;不同背景条件下IN（Ice Nuclei）浓度的增加使得冰晶和雪的质量混合比和数浓度均有较大幅度的增加,其中雪的主要源项为凝华增长过程,而霰增长主要来源于冰相粒子碰并过冷云滴,并且在背景大气和沙尘条件下增加IN都使得霰的数浓度增加,尺度减少。 相似文献
7.
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
8.
本文利用“太行山东麓人工增雨防雹作业技术试验”的飞机和地面雷达观测数据,重点研究分析了2018年5月21日一次典型西风槽天气系统影响下的层状云微物理特征。结果表明,?5°C层的过冷水含量低于0.05 g m?3,冰粒子数浓度量级101～102 L?1。冰粒子数浓度高值区主要以针状和柱状冰晶为主。这可能低层是Hallett-Mossop机制和其他冰晶繁生机制共同作用下所产生的冰晶碎片在冰面过饱和条件下凝华增长所形成的。冰粒子数浓度低值区的冰晶形状基本以片状或枝状为主。?5°C层的冰雪晶增长主要以凝华和聚并增长为主,凇附过程很弱。零度层附近云水含量峰值区的液态水占比达到70%以上。云水含量峰值区的粒子主要以直径10～50 μm的云滴为主,伴随着少量聚合状冰晶。零度层其他区域的过冷水含量维持在0.05 g m?3左右,冰晶形态主要以聚合状、凇附状及霰粒子为主。液水层则主要以球形液滴及半融化状态的冰粒子为主。垂直探测表明:零度层以上的冰雪晶数浓度呈现随高度递增的趋势。在发展稳定的层状云内,混合层的过冷水含量很低,冰粒子主要通过凝华和聚并过程增长,云体冰晶化程度较高。而在发展较为旺盛的层状云区里过冷水含量也较高,大量液滴的存在也表明混合层冰-液相之间的转化不充分。不同温度层的粒子谱显示,冷水含量高值区的冰粒子平均浓度比过冷水低值区高,但平均直径比过冷水低值区小。 相似文献
9.
对流云对大气气溶胶和相对湿度变化响应的数值模拟 总被引：6，自引：3，他引：3
利用二维面对称分档云模式研究了气溶胶颗粒物浓度和尺度谱分布对混合相对流云微物理过程和降水的影响, 并重点讨论了气溶胶效应随环境相对湿度的变化。结果表明, 在初始热力和动力条件相同的情况下, 相对清洁的海洋性云在发展和成熟阶段能更有效地产生雨滴、 冰晶和霰粒, 形成更强的雷达反射率。随着气溶胶浓度增加, 比如在本文模拟的污染大陆性云中, 气溶胶粒子数浓度的增加限制云滴增长, 不利于降水粒子的形成。模拟结果也发现, 环境相对湿度对气溶胶效应有显著影响, 即当地面相对湿度从50%增大到70%时, 所模拟的云从浅对流泡发展为深对流云; 气溶胶对云微物理特性和降水的影响在干空气中较小, 但在湿空气中表现非常显著, 这与前人结果一致。随着相对湿度的增加, 冰相粒子出现的时间提前, 增长加快, 云砧范围扩大, 但相对来说, 降水起始时间对相对湿度的变化比气溶胶更敏感。 相似文献
10.
11.
2016年11月13日在北京地区上空存在持续稳定的层状云天气背景下,利用飞机开展气溶胶粒径谱、化学组成、云滴谱等参量的垂直观测,研究该个例云底气溶胶的活化能力。结果表明:探测期间北京地区为轻度污染天气,地面气溶胶浓度(0.11~3 μm)达到4600 cm-3。云层高度为800~1200 m,云底气溶胶数浓度相对于近地面大幅度降低,有效粒径显著增大(0.3~0.6 μm)。同时,近地面气溶胶中疏水性的一次有机气溶胶贡献显著,而云底气溶胶中一次有机气溶胶的贡献大幅降低,无机组分和二次有机气溶胶的贡献明显增大,造成吸湿性参数κ由0.25(地面)增大至0.32(云底)。云中气溶胶和云滴的谱分布衔接较好,且两者的数浓度之和与云底气溶胶浓度一致,可分别代表未活化和已活化的粒子。基于云底气溶胶粒径谱和吸湿性参数计算得到不同过饱和比下云凝结核的活化率,通过与云中观测结果对比,反推得到云底过饱和度约为0.048%。 相似文献
12.
Wolfram Wobrock Andrea I. Flossmann Marie Monier Jean-Marc Pichon Laurent Cortez Jean-Franois Fournol Alfons Schwarzenbck Stephan Mertes Jost Heintzenberg Paolo Laj Giordano Orsi Loretta Ricci Sandro Fuzzi Harry Ten Brink Piet Jongejan Ren Otjes 《Atmospheric Research》2001,58(4):7907
The second field campaign of the Cloud Ice Mountain Experiment (CIME) project took place in February 1998 on the mountain Puy de Dôme in the centre of France. The content of residual aerosol particles, of H2O2 and NH3 in cloud droplets was evaluated by evaporating the drops larger than 5 μm in a Counterflow Virtual Impactor (CVI) and by measuring the residual particle concentration and the released gas content. The same trace species were studied behind a round jet impactor for the complementary interstitial aerosol particles smaller than 5 μm diameter. In a second step of experiments, the ambient supercooled cloud was converted to a mixed phase cloud by seeding the cloud with ice particles by the gas release from pressurised gas bottles. A comparison between the physical and chemical characteristics of liquid drops and ice particles allows a study of the fate of the trace constituents during the presence of ice crystals in the cloud.In the present paper, an overview is given of the CIME 98 experiment and the instrumentation deployed. The meteorological situation during the experiment was analysed with the help of a cloud scale model. The microphysics processes and the behaviour of the scavenged aerosol particles before and during seeding are analysed with the detailed microphysical model ExMix. The simulation results agreed well with the observations and confirmed the assumption that the Bergeron–Findeisen process was dominating during seeding and was influencing the partitioning of aerosol particles between drops and ice crystals. The results of the CIME 98 experiment give an insight on microphysical changes, redistribution of aerosol particles and cloud chemistry during the Bergeron–Findeisen process when acting also in natural clouds. 相似文献
13.
A. Gelencsér A. Hoffer G. Kiss E. Tombácz R. Kurdi L. Bencze 《Journal of Atmospheric Chemistry》2003,45(1):25-33
Current climate models seem to underestimate the flux of solar energy absorbed by the global troposphere. All of these models are constrained with the assumption that cloud droplets consist of pure water. Here we demonstrate in a simple laboratory experiment that aromatic hydroxy-acids which are found in continental fine aerosol can react with hydroxyl radicals under typical conditions prevalent in cloud water influenced by biomass burning. The reactions yield colored organic species which do absorb solar radiation. We also suggest that the products of such reactions may be humic-like substances whose presence in continental aerosol has been confirmed but their source mechanisms are still much sought after. We also attempt to give a first order estimate of the enhancement of water absorption at a visible wavelength under atmospheric conditions. 相似文献
14.
15.
K. N. Bower T. W. Choularton M. W. Gallagher R. N. Colvile K. M. Beswick D. W. F. Inglis C. Bradbury B. G. Martinsson E. Swietlicki O. H. Berg S. -I. Cederfelt G. Frank J. Zhou J. N. Cape M. A. Sutton G. G. McFadyen C. Milford W. Birmili B. A. Yuskiewicz A. Wiedensohler F. Stratmann M. Wendisch A. Berner P. Ctyroky Z. Galambos S. H. Mesfin U. Dusek C. J. Dore D. S. Lee S. A. Pepler M. Bizjak B. Divjak 《Atmospheric Research》1999,50(3-4)
During March and April of 1995 a major international field project was conducted at the UMIST field station site on Great Dun Fell in Cumbria, Northern England. The hill cap cloud which frequently envelopes this site was used as a natural flow through reactor to examine the sensitivity of the cloud microphysics to the aerosol entering the cloud and also to investigate the effects of the cloud in changing the aerosol size distribution, chemical composition and associated optical properties. To investigate these processes, detailed measurements of the cloud water chemistry (including the chemistry of sulphur compounds, organic and inorganic oxidised nitrogen and ammonia), cloud microphysics and properties of the aerosol and trace gas concentrations upwind and downwind of the cap cloud were undertaken. It was found that the cloud droplet number was generally strongly correlated to aerosol number concentration, with up to 2000 activated droplets cm−3 being observed in the most polluted conditions. In such conditions it was inferred that hygroscopic organic compounds were important in the activation process. Often, the size distribution of the aerosol was substantially modified by the cloud processing, largely due to the aqueous phase oxidation of S(IV) to sulphate by hydrogen peroxide, but also through the uptake and fixing of gas phase nitric acid as nitrate, increasing the calculated optical scattering of the aerosol substantially (by up to 24%). New particle formation was also observed in the ultrafine aerosol mode (at about 5 nm) downwind of the cap cloud, particularly in conditions of low total aerosol surface area and in the presence of ammonia and HCl gases. This was seen to occur at night as well as during the day via a mechanism which is not yet understood. The implications of these results for parameterising aerosol growth in Global Climate Models are explored. 相似文献
16.
气溶胶与云的垂直分布特征是气溶胶间接气候效应关注的重点。基于2018年7—8月华北中部6架次飞机观测数据,研究气溶胶和云滴的垂直和水平分布特征。结果表明:华北中部780~5687 m高度内气溶胶数浓度( Na )平均值为821.36 cm-3,最大量级可达到104 cm-3,云中气溶胶数浓度(Nacc)占总颗粒浓度的80%以上,表明细颗粒占大多数,气溶胶粒子算术平均直径( Dm )平均值为0.12~0.52 μm;大气层结对气溶胶垂直分布影响较大,逆温阻挡气溶胶垂直输送,高空(高度2000 m以上) Dm 的垂直分布受到相对湿度影响较大; Na 和 Dm 在垂直方向波动较大,水平方向波动较小;低层云中云滴数浓度(Nc)较大、液态水含量(L)较小,而中层和高层云中Nc较小、L较大,Nc和云滴有效半径(Re)的概率密度函数均为双峰型分布,L的概率密度函数为单峰型分布;气溶胶数浓度谱基本呈现多峰型分布,而云滴数浓度谱多呈现单峰型分布。 相似文献
17.
Brett A. Yuskiewicz F. Stratmann W. Birmili A. Wiedensohler E. Swietlicki O. Berg J. Zhou 《Atmospheric Research》1999,50(3-4)
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
18.
Numerical Simulation of Macro- and Micro-structures of Intense Convective Clouds with a Spectral Bin Microphysics Model 总被引：1，自引：0，他引：1
By use of a three-dimensional compressible non-hydrostatic convective cloud
model with detailed microphysics featuring spectral bins of cloud
condensation nuclei (CCN), liquid droplets, ice crystals, snow and graupel
particles, the spatial and temporal distributions of hydrometeors in a
supercell observed by the (Severe Thunderstorm Electrification and
Precipitation Study) STEPS triple-radar network are simulated and analyzed.
The bin model is also employed to study the effect of CCN concentration on
the evolution characteristics of the supercell. It is found that the CCN
concentration not only affects the concentration and spectral distribution
of water droplets, but also influences the characteristics of ice crystals
and graupel particles. With a larger number of CCN, more water droplets and
ice crystals are produced and the growth of graupel is restrained. With a
small quantity of CCN the production of large size water droplets are
promoted by initially small concentrations of water droplets and ice
crystals, leading to earlier formation of small size graupel and restraining
the recycling growth of graupel, and thus inhibiting the formation of large
size graupel (or small size hail). It can be concluded that both the macroscopic
airflow and microphysical processes influence the formation and growth of large
size graupel (or small size hail). In regions with heavy pollution, a high
concentration of CCN may restrain the formation of graupel and hail, and in
extremely clean regions, excessively low concentrations of CCN may also limit
the formation of large size graupel (hail). 相似文献
19.
为全面了解水汽在气溶胶影响雷暴云电过程中的作用,本研究在已有的二维雷暴云起、放电模式基础上,通过改变相对湿度和气溶胶初始浓度（文中气溶胶浓度均指气溶胶数浓度）进行敏感性数值模拟试验。结果表明:（1）随着气溶胶浓度升高,雷暴云产生更多的小云滴,降水过程受到抑制。而当水汽含量升高时,云滴数浓度的增长速度更快,雨滴数浓度升高,缓解了降水变弱的趋势。（2）水汽含量较低时,随着气溶胶浓度升高,更多小云滴被带入冻结层形成大量小冰晶,霰粒含量升高,雷暴云起电过程增强。气溶胶浓度升高至一定的量级（3000 cm?3）时,冰晶尺度减小和雨滴浓度降低抑制霰粒生长,雷暴云起电过程受到削弱。感应起电和非感应起电过程随气溶胶浓度升高呈先增强后减弱的趋势。水汽含量的升高促进了冰相粒子的增长,起电过程呈现持续增强的趋势,气溶胶浓度为3000 cm?3时起电率达到极值,电荷密度的增幅扩大。（3）水汽含量较低时,雷暴云难以发展成深厚的系统,气溶胶浓度变化对其影响不明显,电荷结构由三极性发展,在消散期演变为偶极性电荷结构;水汽含量较高时,雷暴云迅速发展成深厚的系统,随着气溶胶浓度升高,在雷暴发展旺盛阶段电荷分布表现为多层复杂结构。研究显示水汽含量在气溶胶浓度变化对雷暴云微物理、起电过程及电荷结构的作用中扮演重要角色。 相似文献
20.
热带深对流云砧数值模拟及云凝结核数浓度对其影响的初步试验 总被引：2，自引：6，他引：2
利用中国科学院大气物理研究所发展的三维强风暴模式，对Egrett Microphysics Experiment with Radiation Lidar and Dynamics（EMERALD）试验期间的一次长寿命热带深对流个例进行对流产生、发展、消亡过程以及云砧的数值模拟，并与实测资料［包括C波段双线偏振雷达图像资料、机载云粒子成像仪（CPI）探测的云砧卷云微物理特性以及激光雷达探测的云砧宏观特性资料］进行了细致的对比，然后通过改变模式中最大云滴数浓度进行有关云凝结核数浓度影响云砧卷云冰晶含水量和数浓度的敏感性试验。模式较好地模拟出系统的一些重要宏观特征，如爆发性增长阶段、各高度雷达水平反射率因子的最大值、对流云主体移动方向、云砧底部和顶部高度。对云砧冰相粒子含水量、数浓度以及平均直径等微观特征的模拟结果与实测也比较接近。对于本文个例而言，异质核化为冰晶形成的最主要方式，其次为过冷云滴的均质核化。敏感性试验结果表明:当云凝结核数浓度增加时，爆发性增长阶段的垂直速度减小，使得对流云从中低层向高层的水物质输送量减少，从而使云砧卷云冰晶的数量减少。 相似文献