Shortwave cloud radiative forcing on major stratus cloud regions in AMIP-type simulations of CMIP3 and CMIP5 models

Cloud and its radiative effects are major sources of uncertainty that lead to simulation discrepancies in climate models. In this study, shortwave cloud radiative forcing (SWCF) over major stratus regions is evaluated for Atmospheric Models Intercomparison Project (AMIP)-type simulations of models involved in the third and fifth phases of the Coupled Models Intercomparison Project (CMIP3 and CMIP5). Over stratus regions, large deviations in both climatological mean and seasonal cycle of SWCF are found among the models. An ambient field sorted by dynamic (vertical motion) and thermodynamic (inversion strength or stability) regimes is constructed and used to measure the response of SWCF to large-scale controls. In marine boundary layer regions, despite both CMIP3 and CMIP5 models being able to capture well the center and range of occurrence frequency for the ambient field, most of the models fail to simulate the dependence of SWCF on boundary layer inversion and the insensitivity of SWCF to vertical motion. For eastern China, there are large differences even in the simulated ambient fields. Moreover, almost no model can reproduce intense SWCF in rising motion and high stability regimes. It is also found that models with a finer grid resolution have no evident superiority than their lower resolution versions. The uncertainties relating to SWCF in state-of-the-art models may limit their performance in IPCC experiments.     

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.     

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.     

Instrument intercomparison study on cloud droplet size distribution measurements: Holography vs. laser optical particle counter

During the EUROTRAC Ground Based Cloud Experiment (GCE) 1990, a newly developed HODAR (Holographic Droplet and Acrosol Recording) was operated for the first time to measure cloud droplet size distributions by recording Fraunhofer in-line holograms of small cloud sample volumes in situ and analyzing the holographic images in the laboratory.This technical note compares the resulting size distributions with those obtained from two FSSP-100 laser optical particle counters. For all holograms analyzed during the GCE90 field experiment, the size distributions obtained from the two different methods agree well. Additionally, the liquid water contents (LWC) were measured directly by a Gerber particulate volume monitor PVM-100. The LWC calculated from the measured droplet size distributions deviate from the PVM-100 data.     

Effects of prescribed initial cloud droplet spectra on convective cloud and precipitation developments under different thermodynamic conditions: A modeling and observational study

A two-dimensional cloud model with bin microphysics was used to investigate the effects of cloud condensation nuclei (CCN) concentrations and thermodynamic conditions on convective cloud and precipitation developments. Two different initial cloud droplet spectra were prescribed based on the total CCN concentrations of maritime (300 cm^− 3) and continental (1000 cm^− 3) air masses, and the model was run on eight thermodynamic conditions obtained from observational soundings. Six-hourly sounding data and 1-hourly precipitation data from two nearby weather stations in Korea were analyzed for the year 2002 to provide some observational support for the model results.For one small Convective Available Potential Energy (CAPE) ( 300 J kg^− 1) sounding, the maritime and continental differences were incomparably large. The crucial difference was the production of ice phase hydrometeors in the maritime cloud and only water drops in the continental cloud. Ice phase hydrometeors and intrinsically large cloud drops of the maritime cloud eventually lead to significant precipitation. Meanwhile negligible precipitation developed from the continental cloud. For the three other small CAPE soundings, generally weak convective clouds developed but the maritime and continental clouds were of the same phases (both warm or both cold) and their differences were relatively small.Model runs with the four large CAPE ( 3000 J kg^− 1) soundings demonstrated that the depth between the freezing level (FL) and the lifting condensation level (LCL) was crucial to determine whether a cloud becomes a cold cloud or not, which in turn was found to be a crucial factor to enhance cloud invigoration with the additional supply of freezing latent heat. For two large CAPE soundings, FL–LCL was so deep that penetration of FL was prohibitive, and precipitation was only mild in the maritime clouds and negligible in the continental clouds. Two other soundings of similarly large CAPE had small FL–LCL, and both the maritime and continental clouds became cold clouds. Precipitation was strong for both but much more so in the maritime clouds, while the maximum updraft velocity and the cloud top were slightly higher in continental clouds. Although limited to small CAPE cases, more precipitation for smaller FL–LCL for a selected group of precipitation and thermodynamic sounding data from Korea was in support of these model results in its tendency.These results clearly demonstrated that the CCN effects on cloud and precipitation developments critically depended on the given thermodynamic conditions and not just the CAPE but the entire structure of the thermodynamic profiles had to be taken into account.     

云凝结核浓度对南京地区一次冰雹云过程影响的数值研究

采用WRF模式与包含了云凝结核(Cloud Condensation Nuclei,CCN)浓度和霰雹密度预报的NSSL(National Severe Storm Laboratory,国家强风暴实验室)微物理方案,模拟不同CCN初始浓度条件下南京地区的一次冰雹云过程,分析不同CCN初始浓度影响下冰雹云过程的宏微观演变特征,以及对流发展不同阶段的水凝物粒子及流场、温度场的垂直分布特征。研究发现:1)较大的CCN初始浓度虽然抑制了前期对流降水,但对后期对流降水的产生有促进作用;2)CCN初始浓度的增加使得模拟雷达回波的强回波区域(大于40 dBz)缩小,中等强度区域(小于40 dBz)扩张。3)CCN初始浓度增大不利于对流发展初期云雨自动转化过程的发生,但是促进了冰晶与雪的产生,使得冰雹含量峰值出现的时间推迟。4)CCN浓度增大抑制了雨水产生,间接使得霰粒子更倾向于干增长,平均密度更小;5)较大的CCN浓度促使冰雹云单体的发展时间增长。     

云、辐射对中期数值预报影响的数值试验

在国家气象中心引进的EC-T42L9谱模式的基础上，用模式诊断云和模式水汽场（以下简称B方法）代替其中计算辐射时所用的纬向平均的气候云和气候水汽场（以下简称A方法），并减少垂直层以节省计算量，从而发展了一个T42L5谱模式。此外，在计算云和辐射时，还设计了方法C，调整云和辐射计算的“时空”分辩率。该文利用改进的T42L5谱模式，并以EC的1982年7月1日12时（UTC）的客观分析为初始场，进行了A、B、C三种方法的5天中期数值预报试验，较系统地研究了云和辐射在中期数值预报中的作用。数值试验的结果表明:（     

利用毫米波云雷达数据反演层云微物理参数和云内湍流耗散率

利用地基毫米波雷达进行云参数及云内湍流特性的探测和反演。根据云雷达回波的功率谱数据,反演出大气垂直运动速度和云微物理参数,得到云内湍流耗散率ε的大小和分布情况,并进一步研究和分析了云内空气垂直运动与云微物理参数、反射率因子、多普勒速度、速度谱宽变化的关系,更好地了解云的演变情况。对2016年8月8日四川稻城的一次层状云过程的探测和反演表明：1）粒子有效半径随着上升气流的增强而增大,由于碰并聚合的作用,粒子数浓度也呈现相应减小的趋势。2）云内湍流耗散率ε在云底、云顶较大,云内较小,量级在10^-8~10^-2 m²·s^-3,多普勒速度能谱验证了假设雷达探测湍涡的尺度在惯性副区的合理性。3）随着上升气流的增强,云粒子的下沉运动相应减小,速度谱宽相应增大。     

气候模式中云的次网格结构对全球辐射影响的研究

利用一种用于大尺度天气、气候模式的随机云产生器(SCG)和独立气柱近似(ICA)辐射算法,研究了次网格云的水平结构以及垂直重叠结构对全球辐射场的影响.比较了水平非均匀云(IHCLD)和水平均匀云(HCLD)的辐射场差异以及云的最大.随机重叠(MRO)和一般重叠(GenO)的辐射场差异.结果显示,与HCLD相比,IHCLD一方面可增加地面净短波辐射通量,纬向平均最大值(约1W/m~2)和次大值(约0.6 W/m~2)分别位于高纬度低云密集地区和对流旺盛的热带地区;另一方面可增加大气顶的净长波辐射通量,纬向平均最大值(0.3 W/m~2)出现在热带地区.不同的重叠结构对短波和长波辐射收支也有很大的影响.MRO和GenO的短波辐射通量差异在热带辐合带最大.达到30-40W/m~2,在高纬度低云带的纬向平均也可达到5W/m~2左右;长波辐射通量差异具有相似的地区分布,但量值相对较小.不同重叠结构可以造成大气上下层的辐射加热率差异,影响大气热力层结.云的水平和垂直结构对有云区域辐射收支的影响将改变大气热力、动力状况以及水汽条件,从而影响模拟的气候系统的演变.文中采用单向云-辐射计算,排除了与气候系统其他过程复杂的相互作用,从而使其结果具有一定的普适性,可为不同大尺度模式进行次网格云辐射参数化提供参考.     

Comparison of cloud properties between cloudsat retrievals and airplane measurements in mixed-phase cloud layers of weak convective and stratus clouds

Cloud microphysical properties including liquid and ice particle number concentration (NC), liquid water content (LWC), ice water content (IWC) and effective radius (RE) were retrieved from CloudSat data for a weakly convective and a widespread stratus cloud. Within the mixed-phase cloud layers, liquid-phase fractions needed to be assumed in the data retrieval process, and one existing linear (p1) and two exponential (p2 and p3) functions, which estimate the liquid-phase fraction as a function of subfreezing temperature (from -20°C to 0°C), were tested. The retrieved NC, LWC, IWC and RE using p1 were on average larger than airplane measurements in the same cloud layer. Function p2 performed better than p1 or p3 in retrieving the NCs of cloud droplets in the convective cloud, while function p1 performed better in the stratus cloud. Function p3 performed better in LWC estimation in both convective and stratus clouds. The REs of cloud droplets calculated using the retrieved cloud droplet NC and LWC were closer to the values of in situ observations than those retrieved directly using the p1 function. The retrieved NCs of ice particles in both convective and stratus clouds, on the assumption of liquid-phase fraction during the retrieval of liquid droplet NCs, were closer to those of airplane observations than on the assumption of function p1.     

Kinematics, cloud microphysics and spatial structures of tropical cloud clusters: A two-dimensional cloud-resolving modeling study

Kinematics, cloud microphysics and spatial structures of tropical cloud clusters are investigated using hourly outputs from a two-dimensional cloud-resolving model simulation. The model is forced by the large-scale vertical velocity, zonal wind and horizontal advections obtained from Tropical Ocean Global Atmosphere Coupled Ocean–Atmosphere Response Experiment (TOGA COARE). A period of 1600–2300 LST 21 December 1992 is selected for this study when the zonal-mean westerly winds in the lower troposphere intensify while the zonal-mean easterly winds above weaken. Under the vertical-shear environment, there are a westward-propagating cloud cluster, a newly-formed cloud cluster, and four eastward-moving cloud clusters. Two weak eastward-moving cloud clusters merge into strong westward-moving cloud clusters. Merged clouds display notable growth in the eastern edge, indicating that merging processes enhance convection. The development of the new cloud at the western edge of the existing cloud cluster before merging may account for the westward propagation of cloud cluster group, while the advection of the maximum total hydrometeor mixing ratio by the westerly winds after merging may cause the eastward propagation of individual cloud clusters.     

Numerical Investigation of Gas Scavenging by Weak Precipitation

A one-dimensional cloud model with size-resolved microphysics and size-resolved aqueous-phase chemistry, driven by prescribed dynamics, has been used to study gas scavenging by weak precipitation developed from low-level, warm stratiform clouds. The dependence of the gas removal rate on the physical and chemical properties of precipitation has been explored under controlled initial conditions. It is found that the removal of four gaseous species (SO₂, NH₃, H₂O₂ and HNO₃) strongly depends on the total droplet surface area, regardless the mean size of droplets. The removal rates also correlate positively with the precipitation rate, especially for precipitation having a mean radius larger than 20 μm. The dependence of the scavenging coefficients on the total droplet surface area is stronger than on the precipitation rate. The removal rates of SO₂, NH₃ and H₂O₂ by precipitation strongly depend on the others' initial concentrations. When NH₃ (or H₂O₂) concentration is much lower than that of SO₂, the removal rate of SO₂ is then controlled by the concentration of H₂O₂ (or NH₃). The removal of NH₃ (or H₂O₂) also directly depends on the concentration of SO₂. NH₃ and H₂O₂ can also indirectly affect each other's removal rate through interaction with SO₂. The scavenging coefficient of SO₂ increases with the concentration ratio of NH₃ to SO₂ if the ratio is larger than 0.5, while the scavenging coefficient of NH₃ increases with the concentration ratio of SO₂ to NH₃ when the ratio is smaller than 1. The scavenging coefficient of H₂O₂ generally increases with the concentration ratio of SO₂ to H₂O₂. Although the Henry's law equilibrium approach seems to be able to simulate gas scavenging by cloud droplets, it causes large errors when used for simulating the scavenging of soluble gas species by droplets of precipitating sizes.     

Multiphase chemistry and acidity of clouds at Kleiner Feldberg

The chemistry of cloud multiphase systems was studied within the Kleiner Feldberg Cloud Experiment 1990. The clouds encountered during this experimental campaign could be divided into two categories according to the origin of air masses in which the clouds formed. From the chemical point of view, clouds passing the sampling site during the first period of the campaign (26 October-4 November) were characterized by lower pollutant loading and higher pH, as compared to clouds during the final period of the experimental campaign (10–13 November). The study of multiphase partitioning of the main chemical constituents of the cloud systems and of atmospheric acidity within the multiphase systems themselves (gas + interstitial aerosol + liquid droplets) are presented in this paper. A general lack of gaseous NH₃ was found in these cloud systems, which caused a lack of buffer capacity toward acid addition. Evidence supports the hypothesis that the higher acidity of the cloud systems during this final period of the campaign was due to input of HNO₃. Our measurements, however, could not determine whether the observed input was due to scavenging of gaseous HNO₃ from the air feeding into the cloud, or to heterogeneous HNO₃ formation via NO₂ oxidation by O₃ to NO₃ and N₂O₅. Sulfate in cloud droplets mainly originated from aerosol SO ₄ ^2– scavenging, since S(IV) to S(VI) liquid phase conversion was inhibited due to both lack of H₂O₂ and low pH of cloud droplets, which made O₃ and metal catalyzed S(IV) oxidation inefficient.     

利用扫描式红外亮温仪对天空云量的试验观测

利用中国科学院大气物理研究所中层大气与全球环境探测实验室自主开发研制的全自动扫描式天空红外亮温仪,于2007年4-8月在北京市气象局南郊观象台进行了试验观测.利用获得的天空红外亮温数据和南郊观象台(54511站)实时地面气象数据,进行了天空云量的计算.将整点前30 min内观测的云量的平均值作为与观象台观测对应的整点观测云量,分不同情况与观象台目视观测结果进行了对比分析.结果表明:(1)对于中低云,两种观测的云量比较一致,但如果在此期间云消散或增加很快,则差别较大.其主要原因是观测的时间和方式不同所造成的.(2)对于以卷云为主的天空情况,特别是高层薄卷云的情况,两种观测的云量差别较大.原因是受到目前试验所使用的红外传感器低温测量范围的限制(-50℃),以及判定云的阈值算法目前还只对于中低云比较适用,对于卷云的判断能力比较薄弱.(3)对于天空情况比较复杂,以及能见度不好的情况(气象站目视云量记录为10-),两种观测的云量差别也很大.其差别既受到仪器性能的影响,也与观测员视力与经验有关.仪器受到最低测量温度的限制,反演算法也有其不确定性,而观测员在低能见度时的观测局限性亦是一个重要原因.利用SIRIS-1进行云量和云底高度观测的优点是时间分辨率高,且全天时自动化,但对于卷云的判断还较薄弱.     

云滴数浓度影响混合型层状云降水的数值模拟

使用耦合了Morrison双参数微物理方案的中尺度WRF模式V2．2,对2008年1月25-29日发生在我国南方的冰雪天气过程进行了数值试验。在模式准确再现了此次天气过程形势演变特点的基础上,对模式微物理方案中云滴数浓度影响累积降水量的情况进行了敏感性试验,发现云滴数浓度对降水量的影响是复杂和非线性的。对此次天气过程中的微物理量进行了详细的分析,并从各种水成物粒子的发展演变上,讨论了云滴数浓度的增加在暖云和冷云两种降水机制上对降水产生的不同影响。结果表明,云滴数浓度越大,云水混合比就越大,云滴的尺度越小。雨滴对不同云滴数浓度的响应与云滴的情况相反,随着云滴数浓度的增加,雨滴数浓度减小,雨水也减少,暖云降水过程受到了抑制;冰晶和雪晶的数浓度的演变过程没有明显变化,而冰晶和雪晶的混合比是相应增加的,冷云降水过程得到了一定程度的增强。从本文模拟的个例来看,设置不同云滴数浓度所得到的总累计降水量的差异在1％以内。总的来说,增加云滴数浓度,降水量会减少。从比例上来看,增加云滴数浓度对暖云降水过程的抑制作用比对冷云降水过程的增强作用更为显著,但是在本文模拟的个例中,冷云降水过程占主导地位,减少的降水和增加的降水的绝对值在同一个量级上并且数值相近,它们相互抵消后得到的结果是降水量变化的绝对值大大减小了,这解释了增加云滴数浓度后模拟的总累积降水量变化不明显的原因。     

一次积层混合云降水不同尺度结构的数值模拟

利用中尺度数值模式WRF-ARW（V3.2）对2009年4月18-19日发生在张家口地区的一次积层混合云降水进行了模拟,并结合观测资料从不同尺度对这次降水过程进行了对比分析.结果表明：700 hPa西风槽、850 hPa低涡是影响这次降水的主要天气系统,来自南方的暖湿空气和西北内蒙古低涡带来的水汽是这次降水的主要水汽来源,两股水汽在张家口附近低层出现了大尺度辐合,有利于该地区云系的发展、降水的形成;降水云系呈东北-西南向带状分布,带长约1 000 km,带宽300km,在大片的云带中分布着很多个小的高值中心,中心区域一般在几十千米;结合雷达回波可以看到在均匀的回波层中镶嵌着柱状对流回波,具有典型的积层混合云降水回波特征;沿着雷达回波做剖面,发现云中云水含量分布无论是水平方向还是垂直方向都是不均匀的,雨水的大值中心与上层的霰、雪的大值中心相对应,中心水平范围在1020 km.     

云凝结物平流输送对降水云系发展影响的数值模拟研究

大气动力学中"平流输送"是非常重要的宏观动力学过程,云凝结物的平流输送与降水云系的发展演变密切相关,它把宏观动力过程与各种云凝结物粒子的时空演变联系起来,云凝结物的平流输送可以增加或减少局地大气中云凝结物的含量,改变云凝结物的空间分布状况,影响云凝结物的微观物理过程,进而促进或抑制降水云系的发展演变.本文在数值模拟研究中.通过改变云凝结物平流输送的状况来研究宏观动力过程对云微观物理过程的影响,因而利用ARPS模式开展3个分别排除云凝结物水平平流输送、垂直平流输送和三维平流输送的敏感试验,进行关于云凝结物平流输送对降水云系发展演变影响的敏感性数值模拟研究.结果表明,云凝结物的平流输送对水汽比湿的影响很小.云凝结物的三维平流输送有利于增加降水云系中雪和霰的混合比含量,抑制云水、雨水和云冰混合比含量的增长.云凝结物的水平平流输送可以降低降水云系中云水和雨水的混合比含量,增加云冰和雪的混合比含量;云凝结物垂直平流输送的作用是增加降水云系中雨水、雪和霰的混合比含量,减少云与冰混合比含量.云凝结物三维平流输送效应的分析表明,云凝结物的三维平流输送主要通过调整云凝结物的微物理过程源汇项以及降水粒子(雨水、雪和霰)的下落末速项来改变降水云系中云凝结物的垂直结构;另外,雪的三维平流输送对雪本身的分布也有一定影响.     

Modelling of the nighttime nitrogen and sulfur chemistry in size resolved droplets of an orographic cloud

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.     

慕尼黑一次混合型雹暴的数值模拟与成雹机制

利用三维冰雹云模式,对2013年4月29日四川西昌的一次降雹过程进行了数值模拟。模拟结果显示：该例冰雹云存在过冷雨水累积带;霰是冰雹的主要胚胎,雹块主要通过撞冻云水增长,其次是撞冻霰增长;模拟区域内液态降水量和固态降水量分别占地面总降水量的52%和48%,冰雹占固态降水94%;通过对该例雹云中冰晶、雪、霰、冻滴的微物理过程分析发现,在雹云发展的不同阶段,冰雹的形成机制不同。

     

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.