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.     

An overview of the ACE‐2 CLOUDYCOLUMN closure experiment

CLOUDYCOLUMN is one of the 6 ACE‐2 projects which took place in June‐July 1997, between Portugal and the Canary Islands. It was specifically dedicated to the study of changes of cloud radiative properties resulting from changes in the properties of those aerosols which act as cloud condensation nuclei. This process is also refered to as the aerosol indirect effect on climate. CLOUDYCOLUMN is focused on the contribution of stratocumulus clouds to that process. In addition to the basic aerosol measurements performed at the ground stations of the ACE‐2 project, 5 instrumented aircraft carried out in situ characterization of aerosol physical, chemical and nucleation properties and cloud dynamical and microphysical properties. Cloud radiative properties were also measured remotely with radiometers and a lidar. 11 case studies have been documented, from pure marine to significantly polluted air masses. The simultaneity of the measurements with the multi‐aircraft approach provides a unique data set for closure experiments on the aerosol indirect effect. In particular CLOUDYCOLUMN provided the 1st experimental evidence of the existence of the indirect effect in boundary layer clouds forming in polluted continental outbreacks. This paper describes the objectives of the project, the instrumental setup and the sampling strategy. Preliminary results published in additional papers are briefly summarized.     

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.     

华北中部夏季气溶胶垂直分布及其与云凝结核和云滴转化关系的飞机观测研究

气溶胶的时空分布及其核化成云的转化过程是云降水物理研究的重点,也是气候变化中气溶胶间接效应关注的热点问题。利用2013～2014年期间在华北中部山西地区开展的9架次夏季晴天和积云天气情况下的气溶胶、云凝结核（CCN）及云滴数浓度观测资料,分析研究了气溶胶的垂直分布、谱分布、来源特征及其与云凝结核、云滴数浓度的转化关系。研究结果表明,大气边界层逆温层结对气溶胶、CCN垂直分布有重要影响,不同天气条件下气溶胶谱型在低层差异较大而高层基本一致;垂直方向上CCN数浓度与气溶胶数浓度有较好的相关性,过饱和度0.3%条件下CCN比率（云凝结核/凝结核）与气溶胶有效直径呈线性关系;积云云下气溶胶与云滴的线性拟合方程为y=1.3x?616.3,拟合相关系数为0.96,气溶胶转化为云滴的比率可达到47%。在过饱和度0.3%条件下,云下CCN与云滴的线性拟合方程为y=1.6x?473.8,拟合相关系数也为0.96,CCN转化为云滴的比率可达到69%。     

Microphysical properties of stratocumulus clouds during ACE‐2

Microphysical measurements performed during 8 flights of the CLOUDYCOLUMN component of ACE‐2, with the Meteo‐France Merlin‐IV, are analyzed in terms of droplet number concentration and size. The droplet concentration is dependent upon the aerosol properties within the boundary layer. Its mean value over a flight varies from 55 cm⁻³, for the cleanest conditions, to 244 cm⁻³, for the most polluted one. For each flight, the variability of the concentration, in selected cloud regions that are not affected by mixing with dry air or drizzle scavenging, ranges from 0.5 to 1.5 of the mean value. The mean volume diameter increases with altitude above cloud base according to the adiabatic cloud model. The frequency distribution of mean droplet volume normalized by the adiabatic value, for the selected regions, shows the same dispersion as the distribution of normalized concentration. The values of droplet concentration versus mean volume diameter are then examined in sub‐adiabatic samples to characterize the effects of mixing and drizzle scavenging. Finally, the ratio of mean volume diameter to effective diameter is analyzed and a simple relationship between these 2 crucial parameters is proposed.     

基于航测的云底气溶胶活化率与过饱和度估算

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%。     

Regional aerosol optical depth characteristics from satellite observations: ACE‐1, TARFOX and ACE‐2 results

Analysis of the aerosol properties during 3 recent international field campaigns (ACE‐1, TARFOX and ACE‐2) are described using satellite retrievals from NOAA AVHRR data. Validation of the satellite retrieval procedure is performed with airborne, shipboard, and land‐based sunphotometry during ACE‐2. The intercomparison between satellite and surface optical depths has a correlation coefficient of 0.93 for 630 nm wavelength and 0.92 for 860 nm wavelength. The standard error of estimate is 0.025 for 630 nm wavelength and 0.023 for 860 nm wavelength. Regional aerosol properties are examined in composite analysis of aerosol optical properties from the ACE‐1, TARFOX and ACE‐2 regions. ACE‐1 and ACE‐2 regions have strong modes in the distribution of optical depth around 0.1, but the ACE‐2 tails toward higher values yielding an average of 0.16 consistent with pollution and dust aerosol intrusions. The TARFOX region has a noticeable mode of 0.2, but has significant spread of aerosol optical depth values consistent with the varied continental aerosol constituents off the eastern North American Coast.     

The effect of aerosol representation on cloud microphysical properties in Northeast Asia

This study performed a three-dimensional regional-scale simulation of aerosol and cloud fields using a meso-scale non-hydrostatic model with a bin-based cloud microphysics. The representation of aerosols in the model has been improved to account for more realistic multi-modal size distribution and multiple chemical compositions. Two case studies for shallow stratocumulus over Northeast Asia in March 2005 were conducted with different aerosol conditions to evaluate model performance. Improved condensation nuclei (CN) and cloud condensation nuclei (CCN) are attributable to the newly constructed aerosol size distribution. The simulated results of cloud microphysical properties (cloud droplet effective radius, liquid water path, and optical thickness) with improved CN/CCN number are close to the retrievals from satellite-based observation. The effects of aerosol on the microphysical properties of shallow stratocumulus are investigated by model simulation, in terms of columnar aerosol number concentration. Enhanced aerosol number concentration results in increased liquid water path in humid case, but invariant liquid water path in dry case primarily due to precipitation occurrence. The changes of cloud microphysical properties are more predominant for small aerosol burden than for large aerosol burden with the retarded changes in cloud mass and size due to inactive condensation and collision-coalescence processes. Quantitative evaluation of sensitivity factor between aerosol and cloud microphysical properties indicates a strong aerosol-cloud interaction in Northeast Asian region.     

海洋层积云中的云滴谱宽度及其影响因子

云滴谱宽度对模式中云的光学厚度的参数化、气溶胶间接效应的评估以及降水形成过程的研究至关重要。本文利用美国POST（Physics of Stratocumulus Top）项目2008年7月19日的飞机观测资料，分析了微物理量和云滴谱的垂直分布及微物理过程。结果表明，该云系云滴谱宽度在云底附近较大，这是由低层核化过程导致的；中层凝结增长过程使得云滴谱宽度随高度增加逐渐减小；云顶附近夹卷混合过程导致云滴谱宽度增大。绝热云中垂直速度的增大会促进云凝结核的活化使云滴数浓度增大，促进凝结增长使云滴尺度增大、云滴谱宽度减小，云滴谱宽度与云滴数浓度、云滴尺度呈现负相关关系；云洞中受夹卷混合过程影响，垂直速度减小，云滴蒸发，云滴数浓度和云滴尺度减小、云滴谱宽度增大，且该效应随绝热程度减小而增强。建议云滴谱宽度的参数化将垂直速度、云滴数浓度、云滴尺度和绝热程度等考虑在内。     

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.     

三参数云微物理方案中气溶胶谱函数对云滴谱影响的数值模拟研究

观测和分档方案的数值模拟都证明气溶胶的谱分布特征对云滴谱的演变有直接影响继而作用于降水的发展。目前广泛使用的总体双参数云滴谱方案因为表征云滴谱的预报量不足,在凝结过程中云滴谱呈不正常的拓宽现象。因此在参数化方案中,气溶胶谱对云滴谱的影响未有明确结论。中科学院大气物理研究所(IAP)云降水物理与强风暴重点实验室(LACS)新研发的三参数方案(IAP-LACS)通过增加的预报量克服了云滴谱的拓宽问题,提高了云滴谱模拟的准确性。为了研究在参数化方案中气溶胶谱分布特征对云滴谱的影响,本文采用新方案进行WRF(Weather Research and Forecasting mode)大涡理想性试验,验证了新方案中气溶胶对数正态谱函数中数浓度、几何半径和标准差3个参量对云滴谱演变的影响。针对3个参量的敏感性试验表明新的气溶胶活化方案和三参数云滴凝结增长方案能够描述气溶胶谱对云滴谱演变的影响规律:气溶胶数浓度对云滴谱影响最显著,数浓度越高活化生成的云滴数量越多,云滴半径越小,云滴谱趋向窄谱,气溶胶数浓度低时,云滴数量少、半径大。较大的几何半径使气溶胶谱向大粒径移动,导致大云滴生成,标准差对云滴谱的影响最不显著。     

Evolution of boundary‐layer aerosol particles due to in‐cloud chemical reactions during the 2nd Lagrangian experiment of ACE‐2

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.     

ACE‐2 multiple angle micro‐pulse lidar observations from Las Galletas, Tenerife, Canary Islands

Multiple‐angle micro‐pulse lidar (MPL) observations were made at Las Galletas on Tenerife, Canary Islands during the Aerosol Characterization Experiment‐2 (ACE‐2) conducted June–July, 1997. A principal objective of the MPL observations was to characterize the temporal/spatial distributions of aerosols in the region, particularly to identify and profile elevated Saharan dust layers which occur intermittently during the June–July time period. Vertical and slant angle measurements taken 16 and 17 July characterize such an occurrence, providing aerosol backscatter, extinction, and optical depth profiles of the dust layer between 1 and 5 km above mean sea level (MSL). Additionally, horizontal measurements taken in Las Galletas throughout the 6‐week period provide a time profile of the varying aerosol extinction at the surface. This profile exhibits the alternating periods of clean maritime air and pollution outbreaks that typified the region. Horizontal measurements also provide some evidence suggesting the possible influx of Saharan dust from the free troposphere to the surface. This paper presents estimates of aerosol optical properties retrieved from the multi‐angle MPL measurements in addition to an outline of the methodologies employed to obtain these results.     

巨盐核对云滴活化影响的数值模拟研究

利用包含云凝结核(CCN)与巨核(GCCN)的核化,云滴凝结和碰并增长的分档气块模式模拟研究了不同的CCN数浓度、上升气流速度、CCN中值半径以及云底温度等情况下GCCN对CCN活化的影响,结果表明,在水汽供应相对充足的情况下GCCN对云滴活化数浓度的影响并不明显;而当水汽供应相对不充足时,增加GCCN至1 cm-3的量级以上可以有效减少CCN的活化数浓度.在水汽供应不充分且其他条件相同的情况下,增大CCN的平均直径或是增加云底温度都可以使GCCN对云滴活化的抑制作用增强.对比分析不同的GCCN数浓度对清洁大气和污染大气云底以上300 m高度处粒子谱型的影响可以看出,在水汽供应不充分的条件下加入GCCN,初始时刻CCN的数浓度对GCCN产生的大云滴数目及云滴谱宽的影响较小.在水汽供应相对充足的情况下,GCCN对CCN活化基本没有抑制作用,但此时在高过饱和度峰值下生成的大量小云滴争食水汽,反而导致云滴群凝结增长速度小于水汽供应相对不充足的情况,此时加入的GCCN可以先活化形成大云滴.     

沙尘气溶胶粒子表面变性对云滴形成过程的影响

利用1997年5月14日辽宁省气溶胶和云滴谱航测资料,讨论了沙尘气溶胶粒子表面变性产生的不溶性沙尘粒子外包可溶性硫酸铵层的混合气溶胶粒子作为凝结核的增长规律,计算了由混和核形成的云滴谱特征,并与纯硫酸铵盐核进行对比.结果表明:混和核上初期形成的云滴谱型比纯硫酸铵盐核上初期形成的云滴谱型要宽,更接近实际观测到的云滴谱分布.     

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.     

Ground‐based lidar measurements of aerosols during ACE‐2: instrument description, results, and comparisons with other ground‐based and airborne measurements

A micro‐pulse lidar system (MPL) was used to measure the vertical and horizontal distribution of aerosols during the Aerosol Characterization Experiment 2 (ACE‐2) in June and July of 1997. The MPL measurements were made at the Izaña observatory (IZO), a weather station located on a mountain ridge (28°18' N, 16°30' W, 2367 m asl) near the center of the island of Tenerife, Canary Islands. The MPL was used to acquire aerosol backscatter, extinction, and optical depth profiles for normal background periods and periods influenced by Saharan dust from North Africa. System tests and calibration procedures are discussed, and an analysis of aerosol optical profiles acquired during ACE‐2 is presented. MPL data taken during normal IZO conditions (no dust) showed that upslope aerosols appeared during the day and dissipated at night and that the layers were mostly confined to altitudes a few hundred meters above IZO. MPL data taken during a Saharan dust episode on 17 July showed that peak aerosol extinction values were an order of magnitude greater than molecular scattering over IZO, and that the dust layers extended to 5 km asl. The value of the dust backscatter–extinction ratio was determined to be 0.027±0.007 sr⁻¹. Comparisons of the MPL data with data from other co‐located instruments showed good agreement during the dust episode.     

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。     

气溶胶核化清除的化学效应──Ⅱ：动力学参数对云滴化学非均匀性的影响

运用已建立的气溶胶核化清除的物理化学模式，研究了云的动力学因子（如：气块上升速度、夹卷作用）对云滴化学非均匀性的影响。计算结果表明：较强烈的云发展（较大的气块上升速度）可加强由于气溶胶核化和云滴凝结增长造成的云滴化学的非均匀程度。夹卷作用抑制了云的发展，因而减弱了这种非均匀程度。夹卷作用同时也造成总体液态水中Ｓ（ＶＩ）、Ｈ＋等浓度的增加，在Ｓｍａｘ附近可达１个量级。如果考虑气溶胶粒子的夹卷，则可使气块内云滴污染物浓度随云滴大小的变化更加复杂化，如：不仅云滴污染物浓度随云滴大小而变化，即使对于相同大小的云滴之间，其污染物浓度也可相差很大。     

A physically‐based algorithm for estimating the relationship between aerosol mass and cloud droplet number

In this study, we present a relationship between total accumulation mode aerosol mass concentrations and cloud droplet number concentrations ( N _d). The fundamental aim with the present method is to arrive at a physically‐based conversion algorithm in which each step in the conversion is based on real physical processes that occur and can be observed in the atmosphere, and in which all of the fields involved can be observed or modeled. In the last conversion (the critical part in the algorithm), we use measurements of the size distributions of cloud droplet residual particles for different pollution conditions. This conversion assumes that the size of the residual particles can be described with a lognormal distribution function and uses the Hatch–Choate relationship to convert between residual volume and number. The relatively sparse data set with which we have developed the present algorithm results in a course classification of the aerosol mass field. Consequently, uncertainties need to be recognized when using the algorithm in its present form in model calculations. The algorithm has been used on data from 15 days and the agreement between calculated and observed N _d values is, with one exception, within a factor of 2 and for many of these cases also much better than a factor of 2. In addition to the results of the algorithm itself, we also present a least‐squares fit to the predicted N _d values. To improve the algorithm in the longer‐term requires more data of scavenging fractions, particle chemical composition and density, and residual particle size distributions as a function of aerosol mass loading and cloud type.