A modelling study of aerosol processing by stratocumulus clouds and its impact on general circulation model parameterisations of cloud and aerosol

A model of the aqueous phase processing of an aerosol population undergoing multiple cycling through a stratocumulus (Sc) cloud layer is presented. Results indicate that a significant modification of the aerosol properties is achieved following the first cycle through cloud. In a polluted atmosphere, further modification in subsequent cycles is seen to be hydrogen peroxide limited unless there is a flux of ammonia entering the system through cloud base (CB). The modification of the aerosol population is seen to have little effect on the microphysics (specifically the cloud droplet concentration and effective radius) of the processing cloud. However, it enables processed aerosols to subsequently act as efficient cloud condensation nuclei (CCN) in less vigorous clouds (as a result of reducing the critical supersaturation required to activate them). The effects of variations in the internal mixture of soluble components of aerosols on the microphysics of clouds forming on them are also investigated using the cloud model. A (K2) parameterisation of the effects of variations in internally mixed nitrate loadings on the cloud droplet number concentration is presented. The effects of applying this K2 correction to the droplet number (derived from a parameterisation based on sulphate) for the presence of nitrate in aerosol have been investigated using the HadAM3 version of the Hadley Centre General Circulation Model (GCM). The effect on global annual mean simulations of the indirect forcing and effective radius is small, but more pronounced regionally. Suggestions (based on model results and observations) for parameterising the size distribution and in-cloud growth of aerosols for use in GCMs are presented.     

The effect of clouds on aerosol growth in the rural atmosphere

Measurements of accumulation mode aerosol in the atmospheric boundary layer under cloudy and cloud-free conditions, and in the lower free troposphere under cloud-free conditions, were conducted over the rural northwest of England. Normalised size distributions in the cloud-free boundary layer (CFBL) and the cloud-free free troposphere (CFFT) exhibited almost identical spectral similarities with both size distributions possessing a concentration peak mode-radius of ≈0.05 μm or less. By comparison, aerosol distributions observed in cloudy air exhibited a distinctive log-normal distribution with mode-radii occurring at ≈0.1 μm concomitant with a local minimum at ≈0.05 μm. The consistent and noticeable difference in spectral features observed between cloudy and cloud-free conditions suggest that a greater amount of gas-to-particle conversion occurs on cloudy days, presumably through in-cloud aqueous phase oxidation processes, leading to larger sized accumulation mode particles. Apart from the distinct difference between cloudy and cloud-free aerosol spectra on cloudy days, aerosol concentration and mass were observed to be significantly enhanced above that of the ambient background in the vicinity of clouds. Volatility analysis during one case of cloud processing indicated an increase in the relative contribution of aerosol mass volatile at temperatures characteristic of sulphuric acid, along with a smaller fraction of more volatile material (possibly nitric acid and/or organic aerosol). Growth-law analysis of possible growth mechanisms point to aqueous phase oxidation of aerosol precursors in cloud droplets as being the only feasible mechanism capable of producing the observed growth. The effect of cloud processing is to alter the cloud condensation nuclei (CCN) supersaturation spectrum in a manner which increases the availability of CCN at lower cloud supersaturations.     

东亚夏季气溶胶—云—降水分布特征及其相互影响的资料分析

东亚季风气候受到自然因素和人类活动的共同影响,而人类活动因子中气溶胶的作用尤为关键,采用诊断分析的手段研究东亚地区气溶胶的特征及其与云和降水的相互关系具有重要的科学意义。本文利用MODIS(moderate-resolution imaging spectroradiometer)气溶胶和云资料以及TRMM(Tropical Rainfall Measuring Mission)降水数据,分析了东亚夏季气溶胶、云、降水的时空分布特征,研究了气溶胶与云和降水的相互关系。结果表明:中国四个典型地区(珠三角、长三角、四川盆地、京津唐)2001～2011年夏季(6～8月)平均气溶胶光学厚度(Aerosol Optical Depth, AOD)变化范围为0.40～0.68,云光学厚度平均值为18.7～23.6,水云云滴有效粒子半径在20.2～25.6 μm,冰云有效粒子半径在12.9～15.3 μm,云水路径为222.2～243.8 g m-2,降水强度平均值3.6～8.6 mm d-1;珠三角气溶胶光学厚度有显著降低趋势,年倾向为-3.31%,四川盆地云滴有效粒子半径(冰云、水云)和云水路径年变化趋势为-0.42%、-0.49%和-1.26%,京津唐夏季降水量年增幅为3.24%。气溶胶光学厚度和云光学厚度呈正相关,相关系数最大为0.77;在相对湿度较低(30%～50%)情况下,气溶胶光学厚度与云滴有效粒子半径呈负相关;气溶胶光学厚度与云水路径呈正相关,相关系数最大为0.92;相对于低污染情况(AOD<0.5),高污染情况(AOD>0.5)下出现大雨(>10 mm d-1)的频率增加了6.6%～19.1%,小雨(<1 mm d-1)的频率减少了0.72%～7.3%。在水汽含量较少的情况下,气溶胶的增加导致云滴有效粒子半径的减少;气溶胶增强了南方地区的对流性降水,抑制了北方地区层云降水。     

Numerical quantification of sources and phase partitioning of chemical species in cloud: application to wintertime anthropogenic air masses at the Puy de Dôme station

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.     

Computer modelling of clouds at Kleiner Feldberg

The airflow, cloud microphysics and gas- and aqueous-phase chemistry on Kleiner Feldberg have been modelled for the case study of the evening of 1 November 1990, in order to calculate parameters that are not easily measured in the cloud and thus to aid the interpretation of the GCE experimental data-set. An airflow model has been used to produce the updraught over complex terrain for the cloud model, with some care required to ensure realistic modelling of the strong stable stratification of the atmosphere. An extensive set of measurements has been made self-consistent and used to calculate gas and aerosol input parameters for the model. A typical run of the cloud model has calculated a peak supersaturation of 0.55% which occurs about 20 s after entering cloud where the updraught is 0.6 m s^–1. This figure has been used to calculate the efficiency with which aerosol particles were scavenged; it is higher than that calculated by other methods, and produces a cloud with slightly too many droplets. A broad cloud droplet size spectrum has been produced by varying the model inputs to simulate turbulent mixing and fluctuations in cloud parameters in space and time, and the ability of mixing processes near cloud-base to produce a lower peak supersaturation is discussed. The scavenging of soluble gases by cloud droplets has been observed and departures from Henry's Law in bulk cloud-water samples seen to be caused by variation of pH across the droplet spectrum and the inability of diffusion to adjust initial distributions of highly soluble substances across the spectrum in the time available. Aqueous-phase chemistry has been found to play a minor role in the cloud as modelled, but circumstances in which these processes would be more important are identified.     

基于TUV模式的银川光化辐射通量特征及其影响因子

利用TUV模式计算分析了银川光化辐射通量变化特征,探讨了云、气溶胶、臭氧柱浓度、NO₂柱浓度等因子对银川光化辐射通量的影响。结果表明：2019年7—9月银川月平均光化辐射通量分别为6.5E+16光子数·cm^-2·s^-1、5.6E+16光子数·cm^-2·s^-1和4.7E+16光子数·cm^-2·s^-1,日最大值出现在13:00;波长小于325 nm时,光化辐射通量随波长增加缓慢上升,波长在325—480 nm之间时,光化辐射通量迅速升高,波长大于480 nm时,光化辐射通量随波长增加变化较小,此特征在中午前后较早晚表现更明显;云光学厚度和气溶胶光学厚度对光化辐射通量的衰减作用具有明显的“U”型日变化特征,比较而言,气溶胶光学厚度对光化辐射通量衰减作用的“U”型波形更为宽广;光化辐射通量衰减率对较低的云光学厚度的变化更敏感;光化辐射通量随气溶胶光学厚度增加而减小的变率要比随云光学厚度增加而减小的变率小;光化辐射通量对单次散射反照比大于0.6...     

Case study of cloud physical and chemical processes in low clouds at Mt. Brocken

Frequency distributions of cloud base height and cloud type of low clouds observed between May and October 1998 at Mt. Brocken (Germany) have been derived from ceilometer measurements and synoptic observations. The summit at 1142 m a.s.l. was about 50% of that time in cloud. During daytime, Stratus clouds were the dominant cloud type (65%), whereas Cumulus clouds amounted to 27% and Stratocumulus clouds to 8%. Evidence was found that the increase of the cloud base height observed at Mt. Brocken continues since the end of the 1980s. An example for a clear anticorrelation between the liquid water content (LWC) of the cloud and the height above cloud base is shown. Other results of this detailed case study of a cloud event on October 8, 1998 concerning phase partitioning of water-soluble inorganic compounds, black carbon (BC) and organic carbon (OC) between the liquid and the interstitial phase will also be presented. The observed ion-specific increase in the solute mass per cubic meter of air with decrease of the distance between sampling position and cloud base was caused mainly by entrainment of air from the below-cloud layer. As expected, for sulfate, ammonia and nitrate, high scavenging coefficients (>0.8) were found. OC exhibits a high scavenging fraction of between 0.4 and 0.7; the value for black carbon (0.2–0.4) implies that soot was possibly to some extent internally mixed in the cloud condensation nuclei (CCN). Simultaneous measurements during a cloud event of HNO₂ and HNO₃ in the gas phase and N(III) and N(V) in the liquid phase were made for the first time.     

海盐气溶胶和硫酸盐气溶胶在云微物理过程中的作用

利用大气气溶胶和云分档模式研究海盐气溶胶和硫酸盐气溶胶在云微物理过程中的作用, 计算结果表明:云中液态水含量随高度的分布并不随海盐、硫酸盐的数目以及云团上升速度的变化而变化; 随着云滴数目的增加, 云滴的有效半径会减小; 硫酸盐对云滴数目影响起主导作用, 海盐在水汽相对充足情况下增加了云滴数目, 在水汽相对不足的情况下减少了云滴数目; 硫酸盐粒子浓度特别强的情况下 (人类活动污染比较严重时), 如果水汽相对不足, 云滴数目会明显小于硫酸盐粒子浓度; 而海盐粒子的存在, 加剧了水汽的供应不足, 从而可以在很大程度上进一步降低云滴数目。也就是说, 在有些情况下, 如果不考虑海盐气溶胶的作用, 硫酸盐气溶胶对云特性的影响会被过高估计。     

气溶胶对北京中尺度对流系统影响的数值试验

利用可分辨云模式(WRF),模拟研究了不同气溶胶浓度对北京地区2001年8月23日一次产生强降水和冰雹的对流天气的影响。结果表明,气溶胶浓度的增加不利于对流云的发展,导致地面降水减小,但是对降水结构没有明显影响。气溶胶浓度增加导致云中水成物数浓度和质量浓度均发生变化,其中云水、冰晶和雪含量增加,而雨水、霰和雹含量减小。从云微物理学分析发现,气溶胶浓度减小有利于高层云的形成,云滴有效半径随着气溶胶浓度增加而减小。     

气溶胶对北京地区不同类型云降水影响的数值模拟

利用耦合Milbrandt双参数显式云方案的WRF模式,在大陆型和海洋型气溶胶浓度背景下,对北京地区暴雨、中雨和微量降水等3次云降水过程进行了数值模拟研究。结果表明,气溶胶的增加对北京地区云降水有多方面的影响：（1）影响地面降水量。随着气溶胶浓度的增加,北京地区的暴雨、中雨和微量降水平均累计降水量分别减少了23.8%,...     

2014年春季华北两次降水过程的人工增雨催化数值模拟研究

在WRF中尺度模式中耦合了中国气象科学研究院发展的CAMS（Chinese Academy of Meteorological Sciences）云微物理方案,并在CAMS方案中增加了直接播撒冰晶（S1方案）和播撒碘化银催化剂（S2方案）两种云催化方案。利用此模式,对2014年我国华北干旱期间开展飞机增雨作业的两次降水过程（个例1:5月9～10日;个例2:5月10～11日）进行了云催化数值模拟研究,分析了催化对降水和云物理量场影响,对比了S1和S2方案催化效果的异同。结果表明,在云层适当部位播撒催化剂,两种催化方案均会达到增雨效果,催化会引起云中各水凝物的明显变化,并导致催化区域温度、垂直速度的变化。个例1中,S2方案的催化影响范围要大于S1方案,在播撒区下游地区,S2方案催化效果要强于S1方案;而个例2中两方案催化效果没有表现出显著差异。S1和S2方案的催化效果在不同个例中表现不同,其重要原因在于两种催化方案的催化机制差异以及云系动力条件、水汽条件的不同。通过采用适当的催化剂量,在其他催化设置条件相同的情况下,S1和S2方案可以取得相似的催化效果,但需注意由于二者催化机制的差异,在一些具体云系条件下,二者的催化效果会有一定差异。当实际人工增雨作业采用碘化银催化剂时,相应的催化模拟研究使用S2方案更为适合。     

Role of organic acids (formic, acetic, pyruvic and oxalic) in the formation of cloud condensation nuclei (CCN): a review

Although it is believed that organic aerosols play a key role in cloud nucleation and make an important contribution to the cloud condensation nuclei (CCN) population, their specific species remain poorly characterized. This paper reviews the current knowledge of organic acids (mainly formic, acetic, pyruvic and oxalic acids). Without specification, organic acids in this paper refer to these four organic acids in the gas and aerosol phases. This paper analyzes the extent to which organic acids act as CCN and compares the physical and chemical properties of organic acids with those of CCN. The results show that aerosol formate and acetate concentrations range from 0.02 to 5.3 nmol m⁻³ and from 0.03 to 12.4 nmol m⁻³, respectively, and that between 34 to 77% of formate and between 21 to 66% of acetate are present in the fine fraction of aerosols. It was found that although most (98–99%) of these volatile organic acids are present in the gas phase, their concentrations in the aerosol particles are sufficient to make them a good candidate for CCN. The results also show that organic acids may make an important contribution to the formation of CCN in some special sources such as vegetation emissions and biomass-burning. Organic acids are expected to contribute significantly to the estimates of indirect (cloud-mediated) forcing due to aerosols.     

层积云覆盖的海洋边界层云详细微物理过程的数值模拟

文中建立了一个含显式分档的云微物理模式和辐射传输模式的一维 3阶湍流闭合模式 ,该模式可用于研究海洋边界层云中气溶胶和云的相互作用过程 ,同时提出了一种新的动力模式和微物理模式耦合方法 ,该方法可使动力模式中液态水相关项可以直接由微物理模式变量计算得到。作为模式的初步应用模拟了 2 0 0 1年APEX/ACE Asia在西太平洋上所观测到的一个个例。模拟结果和观测资料比较表明该模式基本上模拟出层积云覆盖的海洋边界层的基本结构     

35GHz云雷达反射率因子数据的质量控制

大气非云粒子(气溶胶、昆虫、悬浮物)以及雷达元器件固有噪声,是影响云雷达定量探测大气云层宏观以及微观产品的重要因素。为了剔除云雷达基数据中的散点噪声对数据质量的影响,本文利用新一代多普勒偏振8.6 mm云雷达资料,基于模糊逻辑识别地物的方法分析雷达散点噪声、气溶胶以及大气云粒子的反射率因子回波的统计特征,通过统计的特征值对反射率因子进行分类,保留正常回波数据。结果表明:该方法能较好区分云粒子回波和非云粒子回波,提高云雷达反射率因子的数据质量。     

不同水汽条件下气溶胶对雷暴云电过程影响的数值模拟研究

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...     

气溶胶影响混合相对流云降水的数值模拟研究

利用一种新的异质冰相核化参数化方案,研究了当气溶胶同时作为云凝结核和冰核时,在不同高度输送对混合相对流云和降水的影响。结果发现,对于本文研究的理想混合相对流云,气溶胶在边界层的输送导致液滴数浓度明显增加,有效半径减小,霰粒的生长受到抑制,引起霰粒质量浓度降低;而气溶胶在对流层中层4～6km输送时,导致冰晶和霰粒数浓度明显增加。由于较多的冰晶引起更加快速的贝吉隆过程,使霰粒的质量浓度增加;气溶胶在对流层中层2～4km高度输送时冰相形成作用相对较弱,并引起霰粒的数浓度略微增加,由于霰粒的有效半径减小导致其质量浓度下降。气溶胶在不同高度的输送都导致液态和固态降水率降低,随着背景气溶胶数浓度的增加,气溶胶在0～2km、2～4km以及4～6km的输送分别导致累积降水量减少28％～64％、4％～44％和3％～46％,并且对降水的抑制效应及所在高度不同引起的降水差异随着背景气溶胶数浓度的增加而减小。     

The scavenging of nitrate by clouds and precipitation

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.     

The Cloud Ice Mountain Experiment (CIME) 1998: experiment overview and modelling of the microphysical processes during the seeding by isentropic gas expansion

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.     

气溶胶影响云和降水的机理和观测研究进展

气溶胶对云和降水的影响,对于气候系统、大气环境以及水循环至关重要。气溶胶粒子作为云凝结核和大气冰核影响云的微物理过程,进而影响雨、雪、雹和其他形式的降水。近年来,在理解气溶胶的化学成分,气溶胶微物理特性以及气溶胶作为云凝结核和大气冰核影响云降水等方面已取得重大进展。本文对于气溶胶的概念、来源以及气溶胶的直接和间接效应进行了简要概述,重点总结了国内外在气溶胶影响云和降水的机理研究方面的成果,回顾了近年来利用卫星、地面观测设备、机载探测设备等对气溶胶和云进行遥感观测和直接观测所获得的观测事实并讨论了其可能的物理机制,在总结前人研究成果的基础上对未来的研究方向进行了讨论。     

Kinetic limitations on cloud droplet formation and impact on cloud albedo

Under certain conditions mass transfer limitations on the growth of cloud condensation nuclei (CCN) may have a significant impact on the number of droplets that can form in a cloud. The assumption that particles remain in equilibrium until activated may therefore not always be appropriate for aerosol populations existing in the atmosphere. This work identifies three mechanisms that lead to kinetic limitations, the effect of which on activated cloud droplet number and cloud albedo is assessed using a one‐dimensional cloud parcel model with detailed microphysics for a variety of aerosol size distributions and updraft velocities. In assessing the effect of kinetic limitations, we have assumed as cloud droplets not only those that are strictly activated (as dictated by classical Köhler theory), but also unactivated drops large enough to have an impact on cloud optical properties. Aerosol number concentration is found to be the key parameter that controls the significance of kinetic effects. Simulations indicate that the equilibrium assumption leads to an overprediction of droplet number by less than 10% for marine aerosol; this overprediction can exceed 40% for urban type aerosol. Overall, the effect of kinetic limitations on cloud albedo can be considered important when equilibrium activation theory consistently overpredicts droplet number by more than 10%. The maximum change in cloud albedo as a result of kinetic limitations is less than 0.005 for cases such as marine aerosol; however albedo differences can exceed 0.1 under more polluted conditions. Kinetic limitations are thus not expected to be climatically significant on a global scale, but can regionally have a large impact on cloud albedo.