Microphysics of clouds at Kleiner Feldberg

During a field measuring campaign at Kleiner Feldberg (Taunus) in 1990, microphysical characteristics of clouds have been measured by Forward Scattering Spectrometer Probes (FSSP). The aim was to study the influence of aerosol and meteorological factors on droplet size and number. The results are: More mass in the accumulation size range of the aerosol leads to more droplets in stratocumulus clouds and to higher soluble masses in droplets of stratus clouds. However, the aerosol distribution was coarser in the stratus clouds compared to the stratocumulus clouds. Within the first 200 m from cloud base, the droplets grow while their number decreases. The growth results in a stable size of about 14 µm diameter over a large distance from cloud base in many stratocumulus clouds. Two types of mixing processes were observed: processes with reductions in the number of droplets (inhomogeneous mixing) and with reductions in the size of the droplets (homogeneous mixing).     

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。     

Numerical study of droplet size dependent chemistry in oceanic,wintertime stratus cloud at southern mid-latitudes

Cloud droplet chemistry is modelled for the first 150 m of rise in a wintertime, mid-latitude, marine stratus cloud using observations made at and near the Cape Grim Baseline Station as a source of input parameters. The emphasis in this work was to study the variation in droplet chemistry as a function of both droplet size and nucleus composition, with a particular focus on the way in which oxidation of dissolved sulfur dioxide varied.At 150 m above the condensation level, solute concentration as a function of droplet size was found to increase by as much as 2 to 3 orders of magnitude for only a factor of 2 increase in droplet radius, primarily as a consequence of the 1/r dependence in the droplet growth equation. This type of size dependence exists at all levels in the model cloud, and has a significant influence on oxidation rate of sulfur dioxide in droplets growing on sulfate nuclei, oxidation by ozone being favoured in the smallest droplets, but oxidation by hydrogen peroxide being favoured in the larger droplets. Oxidation by ozone is favoured at all sizes in droplets formed on sea-salt nuclei as a result of the initially high alkalinity of these droplets, and in the cloud overall is calculated to be the more important oxidation pathway. Although based on a simplified chemical scheme, these results suggest that both size-dependent and nucleus-dependent chemistry of cloud droplets may need to be considered explicitly in cloud modelling work.Volume-weighted mean pH values in the range 5 to 6 were predicted from sensitivity studies in which input variables were varied over reasonable ranges, in agreement with two sets of bulk cloud-water pH data obtained by aircraft near Cape Grim.     

不可溶性气溶胶对边界层暖云滴谱离散度影响的模拟研究

基于一维分档MISTRA边界层云模式,模拟研究了内部混有不可溶核的硫酸铵气溶胶对边界层暖云微物理特征的影响。结果表明：边界层内湍流动能通量是影响暖云发展的重要因素。云中液态水含量、过饱和度以及云滴谱离散度均随云中的高度增加而增大。云滴谱标准差是影响云滴谱离散度变化的主要因子。在暖云发展阶段,不可溶性核会增加云中过饱和度,进而导致云滴谱分别向大尺度和小尺度端拓宽,云滴谱标准差增大,云滴谱离散度随时间增加而增大的程度增强;在暖云减弱阶段,不可溶核会造成云中大尺度端云滴数浓度减少,云滴谱变窄,标准差变小,云滴谱离散度逐渐减小的特征减弱。     

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%。     

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.     

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.     

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.     

Impacts of aerosol chemical composition on microphysics and precipitation in deep convection

Aerosols affect precipitation by modifying cloud properties such as cloud droplet number concentration (CDNC). Aerosol effects on CDNC depend on aerosol properties such as number concentration, size spectrum, and chemical composition. This study focuses on the effects of aerosol chemical composition on CDNC and, thereby, precipitation in a mesoscale cloud ensemble (MCE) driven by deep convective clouds. The MCE was observed during the 1997 department of energy's Atmospheric Radiation Measurement (ARM) summer experiment. Double-moment microphysics with explicit nucleation parameterization, able to take into account those three properties of aerosols, is used to investigate the effects of aerosol chemical composition on CDNC and precipitation. The effects of aerosol chemical compositions are investigated for both soluble and insoluble substances in aerosol particles. The effects of soluble substances are examined by varying mass fractions of two representative soluble components of aerosols in the continental air mass: sulfate and organics. The increase in organics with decreasing sulfate lowers critical supersaturation (S_c) and leads to higher CDNC. Higher CDNC results in smaller autoconversion of cloud liquid to rain. This provides more abundant cloud liquid as a source of evaporative cooling, leading to more intense downdrafts, low-level convergence, and updrafts. The resultant stronger updrafts produce more condensation and thus precipitation, as compared to the case of 100% sulfate aerosols. The conventional assumption of sulfate aerosol as a surrogate for the whole aerosol mass can be inapplicable for the case with the strong sources of organics. The less precipitation is simulated when an insoluble substance replaces organics as compared to when it replaces sulfate. When the effects of organics on the surface tension of droplet and solution term in the Köhler curve are deactivated by the insoluble substance, S_c is raised more than when the effects of sulfate on the solution term are deactivated by the insoluble substance. This leads to lower CDNC and, thus, larger autoconversion of cloud liquid to rain, providing less abundant cloud liquid as a source of evaporative cooling. The resultant less evaporative cooling produces less intense downdrafts, weaker low-level convergence, updrafts, condensation and, thereby, less precipitation in the case where organics is replaced by the insoluble substance than in the case where sulfate is replaced by the insoluble substance. The variation of precipitation caused by the change in the mass fraction between the soluble and insoluble substances is larger than that caused by the change in the mass fraction between the soluble substances.     

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.     

Microphysical characteristics of precipitating cumulus cloud based on airborne Ka-band cloud radar and droplet measurements

在积云中,大多数云粒子的直径在7到10微米之间,而在层云中,大多数云粒子的直径不超过2微米.云滴有效半径与云中行星边界层(PBL)及PBL上层的气溶胶数浓度(Na)呈负相关.在1500米以上的高液态水含量区域,云滴浓度(Nc)变化不大,Na含量降低.高雷达反射率对应于大的FCDP云粒子浓度和小的气溶胶粒子浓度.积云中的...     

Cloud condensation nuclei and cloud droplet measurements during ACE‐2

During the 2nd Aerosol Characterization Experiment (ACE‐2), relationships between stratocumulus cloud properties and aerosols were examined. Here, the relevant measurements including the cloud condensation nuclei (CCN) activation spectrum, updraft velocity, cloud microphysical and aerosol properties are presented. It is shown that calculations of droplet concentration based on updraft velocity and the CCN activation spectrum are consistent with direct observations. Also discussed is an apparent disparity among measurements of the CCN activation spectrum, the accumulation mode size distribution, and the composition of the submicrometric aerosol. The observed consistency between CCN, updraft and cloud droplets is a necessary refinement; however, extended analyses of the ACE‐2 data set are needed to guide improvements in model simulations of the interaction between aerosols and cloud microphysics. In particular, there is need for an examination of aerosol size spectra and chemical composition measurements with a view towards validating droplet activation schemes which relate the aerosol and cloud dynamical properties to cloud albedo.     

Aerosol-cloud chemical fractionation: Enrichment factor analysis of cloud water

A field study was conducted at a mountain-top site in northwestern Colorado. Supercooled cloud water, collected as a function of droplet size, was analyzed for anions, cations and trace elements. Enrichment factors (EF) of SO ₄ ^2– , K⁺, Na⁺ and Cl^– relative to crustal and marine reference elements (Al and Na) were calculated to determine whether chemical fractionation of the aerosol occurs during cloud droplet formation. The largest EF's for all ions were found for droplets less than 10–15 µm diameter. Ratios of the small to large droplet mean EF's ranged from 1 to 2, for SO ₄ ^2– relative to both Al and Na⁺, to 10 to 12 for Na⁺, Cl^– and K⁺, relative to Al. EF's of K⁺ and Cl^– in the bulk cloud water were in crustal and marine proportions, respectively. It was concluded that although bulk could chemistry may indicate a lack of enrichment of a species, this may not be true throughout the droplet size distribution. The higher enrichments in small droplets is likely a result of their formation on small aerosol particles whereas the large droplets form on the largest aerosol particles. This may suppress EF's in precipitation relative to the total aerosol.     

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.     

气溶胶核化清除的化学效应 I：云滴化学非均匀性的研究

本文将水汽在云滴上凝结增长的物理过程与气溶胶、气体的化学过程相结合，对气溶胶核化清除的化学效应进行了研究。 计算结果表明:气溶胶的核化清除造成了云滴化学成分随云滴大小分布的非均匀性，这种非均匀性又对云滴内发生的气体吸收、液相氧化产生影响。 本文还比较了不同污染状况下，不同大小的云滴内气溶胶核化清除与液相氧化对云滴化学的相对贡献的差异。 因此，这种云滴化学的非均匀性(云微化学)的研究对于云化学的野外观测及数值模拟都是重要的。     

A Lagrangian Cloud Model for the Study of Marine Fog

A large-eddy simulation model is coupled with a Lagrangian cloud model to study marine fog. In this model, aerosols and droplets are treated from a Lagrangian frame of reference, in contrast to the traditional bulk and bin microphysical models. Droplet growth via condensation is governed by Köhler theory and environmental conditions local to the droplet. Coupling to the vapour and temperature fields of the flow ensures mass, momentum, and energy conservation between the air and droplet phases. Based on the recent C-FOG field campaign, a simulation is performed which highlights the benefits and potential of this type of model. By initializing the simulation with the measured aerosol size distribution and making assumptions about the chemical composition of the multiple peaks, the simulations provide a clear explanation for the observed bimodal droplet distribution during C-FOG: high supersaturation levels cause condensational growth of nearly all coarse-mode aerosols (presumed to be composed of marine salt), as well as a large number of accumulation model aerosols (presumed to be of continental origin with a lower hygroscopicity). The largest peak in the resulting droplet distribution is created from coarse-mode aerosols with high hygroscopicity, while the secondary peak is only possible due to the limited impact of the largest peak on saturation levels inside the fog. Thus, for the simulated levels of supersaturation, it is the limited number of coarse-mode aerosols which is responsible for the emergence of a larger second peak.

     

The Importance of the Shape Parameter in a Bulk Parameterization Scheme to the Evolution of the Cloud Droplet Spectrum during Condensation

The shape parameter of the Gamma size distribution plays a key role in the evolution of the cloud droplet spectrum in the bulk parameterization schemes. However, due to the inaccurate specification of the shape parameter in the commonly used bulk double-moment schemes, the cloud droplet spectra cannot reasonably be described during the condensation process. Therefore, a newly-developed triple-parameter condensation scheme with the shape parameter diagnosed through the number concentration, cloud...     

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 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.     

气溶胶浓度对暖云不同生长阶段物理特征影响的模拟研究

基于云微物理过程完善的TAU2D分档云模式, 模拟研究了用热泡扰动生成的暖云在不同气溶胶数浓度(Na)背景条件下各演变阶段云微物理量的变化特征。结果表明: 在暖云的发展过程中Na越高, 云滴尺度变小, 云滴间的碰并增长发动较晚, 云滴谱因碰并增长而实现的滴谱拓宽变弱, 云滴谱相对较窄, 云滴谱标准差较小, 因此云体发展越缓慢, 云体生命周期越长, 形成降水就越晚; 反之, 云滴尺度越大, 碰并增长发动越早, 云滴谱拓宽更明显, 云滴谱标准差越大, 云体生命周期相对更短, 降水开始时刻越早。高Na背景下, 碰并阶段云滴谱较凝结阶段更宽, 沉降阶段因云体下沉蒸发导致小尺度云滴减少, 使其滴谱较碰并阶段略有拓宽。在凝结阶段, 低气溶胶背景下云滴数浓度(N)和离散度(ε)间呈现正相关关系, 而高气溶胶背景下两者为负相关关系。在碰并阶段, N与ε的相关性关系为负相关, 且随着气溶胶数浓度的增加, 负相关程度降低。在沉降阶段, N和ε间为负相关关系。