Airborne Observations of Cloud Condensation Nuclei Spectra and Aerosols over East Inner Mongolia

A set of vertical profiles of aerosol number concentrations, size distributions and cloud condensation nuclei(CCN)spectra was observed using a passive cloud and aerosol spectrometer(PCASP) and cloud condensation nuclei counter, over the Tongliao area, East Inner Mongolia, China. The results showed that the average aerosol number concentration in this region was much lower than that in heavily polluted areas. Monthly average aerosol number concentrations within the boundary layer reached a maximum in May and a minimum in September, and the variations in CCN number concentrations at different supersaturations showed the same trend. The parameters c and k of the empirical function N = c S~kwere 539 and1.477 under clean conditions, and their counterparts under polluted conditions were 1615 and 1.42. Measurements from the airborne probe mounted on a Yun-12(Y12) aircraft, together with Hybrid Single-Particle Lagrangian Integrated Trajectory model backward trajectories indicated that the air mass from the south of Tongliao contained a high concentration of aerosol particles(1000–2500 cm~(-3)) in the middle and lower parts of the troposphere. Moreover, detailed intercomparison of data obtained on two days in 2010 indicated that the activation efficiency in terms of the ratio of NCCNto N_a(aerosols measured from PCASP) was 0.74(0.4 supersaturations) when the air mass mainly came from south of Tongliao, and this value increased to 0.83 on the relatively cleaner day. Thus, long-range transport of anthropogenic pollutants from heavily polluted mega cities,such as Beijing and Tianjin, may result in slightly decreasing activation efficiencies.     

Vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai

A comparative study on the vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai was conducted based on the data obtained from a micro pulse lidar.There was a distinct difference in layer thickness and extinction coefficient under the two types of weather conditions.Aerosols were concentrated below 1 km and the aerosol extinction coefficients ranged from 0.25 to 1.50km^-1 on haze days.In contrast,aerosols with smaller extinction coefficients(0.20 0.35 km^-1) accumulated mainly from the surface to 2 km on floating dust days.The seasonal variations of extinction and aerosol optical depth（AOD） for both haze and floating dust cases were similar greatest in winter,smaller in spring,and smallest in autumn.More than 85%of the aerosols appeared in the atmosphere below 1 km during severe haze and floating dust weather.The diurnal variation of the extinction coefficient of haze exhibited a bimodal shape with two peaks in the morning or at noon,and at nightfall,respectively.The aerosol extinction coefficient gradually increased throughout the day during floating dust weather.Case studies showed that haze aerosols were generated from the surface and then lifted up,but floating dust aerosols were transported vertically from higher altitude to the surface.The AOD during floating dust weather was higher than that during haze.The boundary layer was more stable during haze than during floating dust weather.     

Spectral dependence on the correction factor of erythemal UV for cloud,aerosol, total ozone,and surface properties: A modeling study

Radiative transfer model simulations were used to investigate the erythemal ultraviolet(EUV) correction factors by separating the UV-A and UV-B spectral ranges. The correction factor was defined as the ratio of EUV caused by changing the amounts and characteristics of the extinction and scattering materials. The EUV correction factors(CFEUV) for UV-A[CFEUV(A)] and UV-B [CFEUV(B)] were affected by changes in the total ozone, optical depths of aerosol and cloud, and the solar zenith angle. The differences between CFEUV(A) and CFEUV(B) were also estimated as a function of solar zenith angle, the optical depths of aerosol and cloud, and total ozone. The differences between CFEUV(A) and CFEUV(B) ranged from-5.0% to 25.0% for aerosols, and from-9.5% to 2.0% for clouds in all simulations for different solar zenith angles and optical depths of aerosol and cloud. The rate of decline of CFEUV per unit optical depth between UV-A and UV-B differed by up to 20% for the same aerosol and cloud conditions. For total ozone, the variation in CFEUV(A) was negligible compared with that in CFEUV(B) because of the effective spectral range of the ozone absorption band. In addition, the sensitivity of the CFEUVs due to changes in surface conditions(i.e., surface albedo and surface altitude) was also estimated by using the model in this study. For changes in surface albedo, the sensitivity of the CFEUVs was 2.9%–4.1% per 0.1 albedo change,depending on the amount of aerosols or clouds. For changes in surface altitude, the sensitivity of CFEUV(B) was twice that of CFEUV(A), because the Rayleigh optical depth increased significantly at shorter wavelengths.     

Characteristics of Aerosol Activation Efficiency and Aerosol and CCN Vertical Distributions in North China

By analyzing airborne observations over North China from 30 flights during spring and autumn of 2005-2007, characteristics of the vertical distributions of aerosol and cloud condensation nuclei (CCN) at 0.3% supersaturation in various locations of North China are investigated. The measurement samplings were conducted over different surfaces such as plains, plateau, and sea. The results show that the number concentration of accumulation mode aerosols was greater in autumn than in spring, but the reverse is true for CCN. This means that more aerosols with diameters smaller than 100 nm could be activated as CCN in spring, and this could induce higher aerosol activation efficiency. The aerosol activation efficiency over the plains near the Taihang Mountain was greater in spring than in autumn, and it was greater over sea than over land. The aerosol activation efficiency above the boundary layer over the Bashang Plateau was very low. Based on a fit of the negative exponential vertical distributions of aerosol and CCN, a spatial parameterization model of aerosol and CCN as well as aerosol activation efficiency over North China was proposed. The results show that aerosol activation efficiency was not clearly dependent on altitude because it was mainly affected by regional physical and chemical characteristics of aerosols and the ambient atmospheric conditions. The mean aerosol activation efficiency is 0.66, with values of 0.70 and 0.53 in spring and autumn,respectively.     

Some physical aspects of summer monsoon clouds—comparison of cloud model results with observations

The physical characteristics of the summer monsoon clouds were investigated. The results of a simple cloud mod-el were compared with the aircraft cloud physical observations collected during the summer monsoon seasons of 1973,1974,1976 and 1981 in the Deccan Plateau region.The model predicted profiles of cloud liquid water content (LWC) are in agreement with the observed profiles. There is reasonable agreement between the model predicted cloud vertical thickness and observed rainfall.The observed cloud-drop spectra were found to be narrow and the concentration of drops with diameter >20μm is either low or absent on many occasions. In such clouds the rain-formation cannot take place under natural atmos-pheric conditions due to the absence of collision-coalescence process. A comparison of the model predicted and ob-served rainfall suggested that the precipitation efficiency in cumulus clouds of small vertical thickness could be as low as 20 per cent.The clouds forming in the Deccan Plateau region during the summer monsoon are, by and large, cumulus and strato-cumulus type. The vertical thickness of the cumulus clouds is in the range of 1.0-2.0 km. The LWC is found to be more in the region between 1.6-1.9 km A. S. L., which corresponds to the level at almost 3 / 4 th of the total verti-cal thickness of the cloud and thereafter the LWC sharply decreased. Nearly 98 per cent of the tops of the low clouds in the region are below freezing level and the most frequent range of occurrence of these cloud-tops is in the range of 2.0-3.0 km A. S. L.. The dominant physical mechanism of rain-formation in these summer monsoon clouds it the col-lision-coalescence process.     

Aerosol Microphysical and Radiative Effects on Continental Cloud Ensembles

Aerosol–cloud–radiation interactions represent one of the largest uncertainties in the current climate assessment. Much of the complexity arises from the non-monotonic responses of clouds, precipitation and radiative fluxes to aerosol perturbations under various meteorological conditions. In this study, an aerosol-aware WRF model is used to investigate the microphysical and radiative effects of aerosols in three weather systems during the March 2000 Cloud Intensive Observational Period campaign at the US Southern Great Plains. Three simulated cloud ensembles include a low-pressure deep convective cloud system, a collection of less-precipitating stratus and shallow cumulus, and a cold frontal passage. The WRF simulations are evaluated by several ground-based measurements. The microphysical properties of cloud hydrometeors, such as their mass and number concentrations, generally show monotonic trends as a function of cloud condensation nuclei concentrations.Aerosol radiative effects do not influence the trends of cloud microphysics, except for the stratus and shallow cumulus cases where aerosol semi-direct effects are identified. The precipitation changes by aerosols vary with the cloud types and their evolving stages, with a prominent aerosol invigoration effect and associated enhanced precipitation from the convective sources. The simulated aerosol direct effect suppresses precipitation in all three cases but does not overturn the aerosol indirect effect. Cloud fraction exhibits much smaller sensitivity(typically less than 2%) to aerosol perturbations, and the responses vary with aerosol concentrations and cloud regimes. The surface shortwave radiation shows a monotonic decrease by increasing aerosols, while the magnitude of the decrease depends on the cloud type.     

All-Sky Direct Radiative Effects of Urban Aerosols in Beijing and Shanghai,China

Aerosol particles can directly alter the radiation balance by scattering and absorbing incident solar radiation, thus decreasing the amount of light reaching the surface and increasing the fraction of diffuse radiation—the so-called ‘aerosol direct radiative effect'. Using the Moderate Resolution Imaging Spectroradiometer aerosol products, the aerosol direct radiative effects under all-sky conditions in Beijing and Shanghai in 2007 were explored in this study. The total shortwave radiation was calculated using the Fu-Liou radiative transfer model, with the influence of clouds taken into account through sunshine-duration data, and the diffuse radiation was calculated with radiation decomposition models. Good correlation between measured and calculated total radiation was obtained at both cities, with an R greater than 0.9, and thus this calculation method was adopted to derive aerosol direct radiative effects. The presence of aerosols caused the mean total and diffuse solar radiation reaching the surface to change by-19.9% and +27.4% in Beijing, respectively, and by-18.4% and +6.5% in Shanghai. It was also found that, despite the strong negative correlation between aerosol optical depth and total radiation change, the diffuse radiation changes were determined predominantly by clouds. The effects of such changes induced by aerosols on plant productivity should be further studied.     

Some Physical Aspects of Summer Monsoon Clouds-Comparison of Cloud Model Results with Observations

The physical characteristics of the summer monsoon clouds were investigated. The results of a simple cloud model were compared with the aircraft cloud physical observations collected during the summer monsoon seasons of 1973, 1974, 1976 and 1981 in the Deccan Plateau region.The model predicted profiles of cloud liquid water content (LWC) are in agreement with the observed profiles. There is reasonable agreement between the model predicted cloud vertical thickness and observed rainfall.The observed cloud-drop spectra were found to be narrow and the concentration of drops with diameter > 20um is either low or absent on many occasions. In such clouds the rain-formation cannot take place under natural atmospheric conditions due to the absence of collision-coalescence process. A comparison of the model predicted and observed rainfall suggested that the precipitation efficiency in cumulus clouds of small vertical thickness could be as low as 20 per cent.The clouds forming in the Deccan Plateau region during t     

Characteristics of Solar Radiation and the Impact of Clouds at Yangbajing, Tibet

Yangbajing (YBJ) is located in the Tibetan Plateau, China. The characteristics of solar radiation and its relationship with clouds at YBJ from April 2009 to April 2010 were analyzed in this paper. The annual mean solar radiation was 478.4 W m 2 , and the annual mean transmittance was 0.713. The atmospheric mean trans- mittance of clear skies reaches 0.828 when the solar elevation angle (SEA) is greater than 10 degrees. Comparisons with numerical simulations show that the atmosphere of YBJ is clean. Impacts from atmospheric conditions on solar radiation are similar for clear skies during the year because the standard deviation of transmittance in clear skies was less than 0.05 when the SEA was greater than 10 degrees. It is important to understand the impact of clouds on solar radiation without considering other impact factors. In the last part of this article, the authors analyzed and established a statistical quantitative relationship between surface solar radiation and cloud fraction.     

Relationship between cloud characteristics and radar reflectivity based on aircraft and cloud radar co-observations

Cloud properties were investigated based on aircraft and cloud radar co-observation conducted at Yitong, Jilin, Northeast China. The aircraft provided in situ measurements of cloud droplet size distribution, while the millimeter-wavelength cloud radar vertically scanned the same cloud that the aircraft penetrated. The reflectivity factor calculated from aircraft measurements was compared in detail with simultaneous radar observations. The results showed that the two reflectivities were comparable in warm clouds, but in ice cloud there were more differences, which were probably associated with the occurrence of liquid water. The acceptable agreement between reflectivities obtained in water cloud confirmed that it is feasible to derive cloud properties by using aircraft data, and hence for cloud radar to remotely sense cloud properties. Based on the dataset collected in warm clouds, the threshold of reflectivity to diagnose drizzle and cloud particles was studied by analyses of the probability distribution function of reflectivity from cloud particles and drizzle drops. The relationship between reflectivity factor (Z) and cloud liquid water content (LWC) was also derived from data on both cloud particles and drizzle. In comparison with cloud droplets, the relationship for drizzle was blurred by many scatter points and thus was less evident. However, these scatters could be partly removed by filtering out the drop size distribution with a large ratio of reflectivity and large extinction coefficient but small effective radius. Empirical relationships of Z-LWC for both cloud particles and drizzle could then be derived.     

华北地区一次气溶胶与浅积云微物理特性的飞机观测研究

2014年8月15日,山西省人工降雨防雹办公室在山西忻州开展了气溶胶和浅积云的飞机观测,本文利用机载云物理资料,详细分析了华北地区气溶胶、云凝结核（CCN）和浅积云微物理特性及其相互影响。主要结论有:（1）此次过程的边界层高度约为3600 m,不同层结情况下,0.1～3 μm尺度范围内的气溶胶粒子浓度N_a、有效直径D_a和CCN数浓度的垂直廓线明显不同,近地面N_a可达2500 cm?3。（2）CCN的主要来源为积聚模态、爱根模态或者核模态的气溶胶颗粒,0.2%过饱和度下,气溶胶活化率（AR）在各高度层的结果变化不大;0.4%过饱和度下,AR随着高度增加而降低。（3）后向轨迹模式分析表明,2 km以下的气溶胶主要来自于当地城市排放,由细颗粒污染物组成;2 km以上的气溶胶主要来源于中国西北和蒙古地区的沙漠,由亚微米沙尘组成,溶解度相对较低,可作为潜在的冰核。（4）本文细致分析了两块相邻浅积云（Cu-1和Cu-2）的云物理特性。Cu-1云底高度约4500 m,云厚约600 m,云体松散,夹卷较多;云中液态含水量（LWC）基本保持在0.5 g m?3,云粒子浓度N_c平均值为278.3 cm?3,云滴有效直径D_c整体在15 μm以内;毛毛雨滴粒子浓度最大值为0.002 cm?3,云中几乎无降水粒子;粒子谱宽随着高度增加而增大,主要集中在30 μm以内。Cu-2云底高度约3900 m,云厚约1200 m,云体密实;云中过冷水丰沛,LWC有多个超过1 g m?3的区域,云顶附近出现冰晶,云中粒子从凝结增长状态直接进入到混合相态;积云内部粒子水平分布不均,同一高度N_c相差较大,最大可达1240 cm?3。D_c随着高度增加而增大;粒子谱宽随着高度增加而拓展,最大可达1100 μm,谱型由单峰向多峰转变;降水粒子和冰晶图像大多为霰粒子、针状和板状。     

A Study of Shallow Cumulus Cloud Droplet Dispersion by Large Eddy Simulations

Cloud droplet dispersion is an important parameter in estimating aerosol indirect effect on climate in general circulation models (GCMs). This study investigates droplet dispersion in shallow cumulus clouds under different aerosol conditions using three-dimensional large eddy simulations (LES). It is found that cloud droplet mean radius, standard deviation, and relative dispersion generally decrease as aerosol mixing ratio increases from 25 mg⁻¹ (clean case) to 100 mg⁻¹ (moderate case), and to 2000 mg⁻¹ (polluted case). Under all the three simulated aerosol conditions, cloud droplet mean radius and standard deviation increase with height. However, droplet relative dispersion increases with height only in the polluted case, and does not vary with height in the clean and moderate cases.     

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.     

Validation of very high cloud droplet number concentrations in air masses transported thousands of kilometres over the ocean

The microstructure of orographic clouds related to the aerosol present was studied during the second Aerosol Characterisation Experiment (ACE‐2). Very high cloud droplet number concentrations (almost 3000 cm⁻³) were observed. These high concentrations occurred when clouds formed on a hill slope at Tenerife in polluted air masses originating in Europe that had transported the order of 1000 km over the Atlantic Ocean. The validity of the measured droplet number concentrations was investigated by comparing with measurements of the aerosol upstream of the cloud and cloud interstitial aerosol. Guided by distributions of the ratios between the measurements, three criteria of typically 30% in maximum deviation were applied to the measurements to test their validity. Agreement was found for 88% of the cases. The validated data set spans droplet number concentrations of 150–3000 cm⁻³. The updraught velocity during the cloud formation was estimated to 2.2 m s⁻¹ by model calculations, which is typical of cumuliform clouds. The results of the present study are discussed in relation to cloud droplet number concentrations previously reported in the literature. The importance of promoting the mechanistic understanding of the aerosol/cloud interaction and the use of validation procedures of cloud microphysical parameters is stressed in relation to the assessment of the indirect climatic effect of aerosols.     

The chemical fractionation of atmospheric aerosol as a result of snow crystal formation and growth

The relationships between the physical and chemical properties of mixed-phase clouds were investigated at Storm Peak Laboratory (3220m MSL) located near the continental divide in northwestern Colorado. Interstitial aerosol particles, cloud droplets and snow crystals were concurrently collected when the laboratory was enveloped by a precipitating cloud. All samples were analyzed for trace elements, soluble anions, electrical conductivity and acidity.The results show average trace constituent concentration ratios of cloud water to snow water range from 0.4 to 26. All but six of the 32 elements and ions measured had ratios greater than one. This result suggests a chemical species dependency of in-cloud aerosol particle scavenging processes. Evidence of a decrease of in-cloud aerosol particle scavenging efficiency by snow due to increases in aerosol concentration is also presented.Differences between the chemical composition of cloud water and snow water are manifested most strongly when snow crystals grow by vapor deposition. In-cloud scavenging efficiencies by snow crystals for most aerosol particle chemical species are dependent on the growth of the snow crystals by accretion of cloud droplets. This chemical fractionation of the atmospheric aerosol by snow crystal formation and growth should be most active where narrow, continental cloud droplet size distributions and low liquid water contents are prevalent, enhancing the probability of snow crystal growth by diffusion.     

Cloud optical thickness and albedo retrievals from bidirectional reflectance measurements of POLDER instruments during ACE‐2

The POLDER instrument is devoted to global observations of the solar radiation reflected by the Earth–atmosphere system. The airborne version of the instrument was operated during the ACE‐2 experiment, more particularly as a component of the CLOUDYCOLUMN project of ACE‐2 that was conducted in summer 1997 over the subtropical northeastern Atlantic ocean. CLOUDYCOLUMN is a coordinated project specifically dedicated to the study of the indirect effect of aerosols. In this context, the airborne POLDER was assigned to remote measurements of the cloud optical and radiative properties, namely the cloud optical thickness and the cloud albedo. This paper presents the retrievals of those 2 cloud parameters for 2 golden days of the campaign 26 June and 9 July 1997. Coincident spaceborne ADEOS‐POLDER data from 2 orbits over the ACE‐2 area on 26 June are also analyzed. 26 June corresponds to a pure air marine case and 9 July is a polluted air case. The multidirectional viewing capability of airborne POLDER is here demonstrated to be very useful to estimate the effective radius of cloud droplet that characterizes the observed stratocumulus clouds. A 12 μm cloud droplet size distribution appears to be a suitable cloud droplet model in the pure marine cloud case study. For the polluted case the mean retrieved effective droplet radius is of the order of 6–10 μm. This only preliminary result can be interpreted as a confirmation of the indirect effect of aerosols. It is consistent with the significant increase in droplet concentration measured in polluted marine clouds compared to clean marine ones. Further investigations and comparisons to in‐situ microphysical measurements are now needed.     

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.     

华北中部夏季气溶胶和云分布特征

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( N_a )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(N_acc)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( D_m )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) D_m 的垂直分布受到相对湿度影响较大; N_a 和 D_m 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(N_c)较大、液态水含量(L)较小,而中层和高层云中N_c较小、L较大,N_c和云滴有效半径(R_e)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。     

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.