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.     

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.     

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.     

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.     

Aircraft Measurements of Cloud–Aerosol Interaction over East Inner Mongolia

To investigate the potential effects of aerosols on the microphysical properties of warm clouds, airborne observational data collected from 2009 to 2011 in Tongliao, Inner Mongolia, China, were statistically analyzed in this study. The results demonstrated that the vertical distribution of the aerosol number concentration(N_a) was similar to that of the clean rural continent. The average aerosol effective diameter(D_e) was maintained at approximately 0.4 μm at all levels. The data obtained during cloud penetrations showed that there was a progressive increase in the cloud droplet concentration(N_c) and liquid water content(LWC) from outside to inside the clouds, while the Nawas negatively related to the Ncand LWC at the same height. The fluctuation of the N_a, Ncand LWC during cloud penetration was more obvious under polluted conditions(Type 1) than under clean conditions(Type 2). Moreover, the wet scavenging of cloud droplets had a significant impact on the accumulation mode of aerosols, especially on particles with diameters less than 0.4 μm. The minimum wet scavenging coefficient within the cloud was close to 0.02 under Type 1 conditions, while it increased to 0.1 under Type 2 conditions,which proved that the cloud wet scavenging effect under Type 1 conditions was stronger than that under Type 2 conditions.Additionally, cloud droplet spectra under Type 1 conditions were narrower, and their horizontal distributions were more homogeneous than those under Type 2 conditions.     

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.     

Lagrangian air mass tracking with smart balloons during ACE‐2

A 3rd‐generation smart balloon designed at National Oceanic and Atmospheric Administration, Air Resources Laboratory Field Research Division, in collaboration with the University of Hawaii, was released from ship‐board during the recent Second Aerosol Characterization Experiment (ACE‐2) to provide Lagrangian air‐mass tracking data. ACE‐2 is the 3rd in a series of field experiments designed to study the chemical, physical, and radiative properties and processes of atmospheric aerosols and their role in climate and is organized by the international global atmospheric chemistry (IGAC) program. The adjective smart in the title of this paper refers to the fact that the buoyancy of the balloon automatically adjusts through the act of pumping air into or releasing air from the ballast portion of the balloon when it travels vertically outside a barometric pressure range set prior to release. The smart balloon design provides GPS location, barometric pressure, temperature, relative humidity, and other data via a transponder to a C130 research aircraft flying in the vicinity of the balloon. The addition of 2‐way communication allows interactive control of the balloon operating parameters by an observer. A total of 3 cloudy Lagrangian experiments were conducted during the ACE‐2 field program which lasted from 16 June through 26 July 1997. This paper reviews the design and capability of the smart balloons and their performance during the ACE‐2 Lagrangian experiments. Future development and applications of the technology are discussed.     

Clear‐sky closure studies of lower tropospheric aerosol and water vapor during ACE‐2 using airborne sunphotometer, airborne in‐situ, space‐borne, and ground‐based measurements

We report on clear‐sky column closure experiments (CLEARCOLUMN) performed in the Canary Islands during the second Aerosol Characterization Experiment (ACE‐2) in June/July 1997. We present CLEARCOLUMN results obtained by combining airborne sunphotometer and in‐situ (optical particle counter, nephelometer, and absorption photometer) measurements taken aboard the Pelican aircraft, space‐borne NOAA/AVHRR data and ground‐based lidar and sunphotometer measurements. During both days discussed here, vertical profiles flown in cloud‐free air masses revealed 3 distinctly different layers: a marine boundary layer (MBL) with varying pollution levels, an elevated dust layer, and a very clean layer between the MBL and the dust layer. A key result of this study is the achievement of closure between extinction or layer aerosol optical depth (AOD) computed from continuous in‐situ aerosol size‐distributions and composition and those measured with the airborne sunphotometer. In the dust, the agreement in layer AOD (λ=380–1060 nm) is 3–8%. In the MBL there is a tendency for the in‐situ results to be slightly lower than the sunphotometer measurements (10–17% at λ=525 nm), but these differences are within the combined error bars of the measurements and computations.     

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.     

The 2nd Aerosol Characterization Experiment (ACE‐2): meteorological and chemical context

A review is given of the climatological and actual meteorological conditions in the sub‐tropical northeast Atlantic, during June–July 1997, when the 2nd Aerosol Characterization Experiment (ACE‐2) took place. Surface pressure maps, trajectory calculations and in‐situ measurements show how the outflow of European pollution into the marine boundary layer of this area is determined by the location of the Azores high pressure cell. Observations during ACE‐2 and 3 preceding summers show that pollution outbreaks both from the Iberian peninsula and from northern or central Europe can occur during such situations. During ACE‐2, an unusually low number of strong North African dust outbreaks were recorded at the free tropospheric station of Izaña (Tenerife, 2360 m asl), although dust was recorded aloft the station.     

硫酸盐气溶胶间接效应对中国东部冬季气候的影响

气溶胶间接效应通过对云的作用来影响气候,其过程复杂且不确定性较大。本研究利用美国国家大气研究中心（NCAR）的公共大气模式CAM5.1,通过改变模式中硫酸盐气溶胶转化为云凝结核数浓度的数量,设计了硫酸盐气溶胶间接效应的敏感性试验,通过与控制试验对比来研究其间接效应对中国东部地区冬季云、降水和季风强度的影响。结果表明：在东亚地区云凝结核形成过程中,硫酸盐气溶胶占绝对的主导地位。硫酸盐气溶胶间接效应导致中国东部地区冬季云凝结核和云滴数浓度显著增加,海洋和陆地低层的云滴有效半径减小和总云液水路径的增加,导致了云反照率的增加。引起的负辐射强迫使地表和大气降温,海平面气压升高,增加的海陆气压梯度导致中国南方地区东亚冬季风增强,总降水率减少。硫酸盐气溶胶间接效应可能不是东亚冬季风在20世纪80年代中期年际变率减弱的原因。     

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.     

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.     

Boundary layer and aerosol evolution during the 3rd Lagrangian experiment of ACE‐2

Aircraft measurements are presented of the Lagrangian evolution of a marine boundary layer over a 30‐h period during the ACE‐2 field campaign. At the start of the observational period, a 500‐m deep polluted marine internal boundary layer (MIBL) was overlain by the remnants of a polluted continental boundary layer extending to around 2 km below a clean, dry free troposphere. The MIBL grew rapidly to a thickness of 900–1000 m in response to increasing sea surface temperatures. No significant aerosol spectral evolution was observed in the boundary layer. Low concentrations of SO₂ were observed in the MIBL suggesting that the air mass contained relatively aged aerosol. Aerosol spectra show a broad mode with a modal diameter of around 0.1μm. The polluted layer between the MIBL and the unpolluted free troposphere was only weakly and intermittently turbulent which prevented significant entrainment of clean air into the polluted layer from aloft. The polluted layer depth was thus controlled mainly by subsidence which as a result becomes shallower, decreasing from over 2000 m to around 1200 m during the observational period. The aerosol characteristics of the polluted layer were similar to those in the MIBL and so although the MIBL entrained considerable amounts of air from above the MIBL the aerosol characteristics underwent no significant change. This has important implications for the rate at which a polluted continental air mass is converted to a clean marine one. The dataset should prove useful in the validation of the modelling of continental pollution outbreaks.     

Measurements of aerosol optical depth above 3570 m asl in the North Atlantic free troposphere: results from ACE‐2

As part of the 2nd A erosol C haracterisation E xperiment (ACE‐2), conducted during summer 1997 in the North Atlantic region between the Canary Islands and Portugal, we measured aerosol optical depths (AOD) at a mid‐tropospheric site, near the top of the volcanic mountain "El Teide"(28°16'N, 16°36' W, 3570 m asl). Our instrument was located at the highest altitude in a network of sunphotometers that extended down to sea level. Clear conditions dominated the ACE‐2 period, and, although suggested by back‐trajectories at 300 hPa, no evidence of anthropogenic pollution was found in our data. Three distinct dust episodes were observed. Vertical soundings and back trajectories suggested mineral dust from the Sahel region as a source. During these episodes, AOD increased an order of magnitude with respect to background conditions (from 0.017 up to 0.19 at λ=500 nm). A shift towards neutrality of the extinction spectral dependence (Ångstrom exponent α down to 0.13), indicated that the coarse mode (particle diameter >2 μm) dominated the aerosol size distribution. For 6 days during the episodes of mineral dust, a monomodal size distribution between 2 and 20 μm diameter was obtained from Mie based size distribution calculations. Estimates, at 500 nm, of the single scattering albedo ω₀(0.87–0.96), and the aerosol asymmetry parameter g (0.72–0.73) suggest that the dust layer causes a net cooling forcing at the top of the atmosphere.     

Observations of the evolution of the aerosol, cloud and boundary‐layer characteristics during the 1st ACE‐2 Lagrangian experiment

During the 1st Lagrangian experiment of the North Atlantic Regional Aerosol Characterisation Experiment (ACE‐2), a parcel of air was tagged by releasing a smart, constant level balloon into it from the Research Vessel Vodyanitskiy . The Meteorological Research Flight's C‐130 aircraft then followed this parcel over a period of 30 h characterising the marine boundary layer (MBL), the cloud and the physical and chemical aerosol evolution. The air mass had originated over the northern North Atlantic and thus was clean and had low aerosol concentrations. At the beginning of the experiment the MBL was over 1500 m deep and made up of a surface mixed layer (SML) underlying a layer containing cloud beneath a subsidence inversion. Subsidence in the free troposphere caused the depth of the MBL to almost halve during the experiment and, after 26 h, the MBL became well mixed throughout its whole depth. Salt particle mass in the MBL increased as the surface wind speed increased from 8 m s⁻¹ to 16 m s⁻¹ and the accumulation mode (0.1μm to 3.0 μm) aerosol concentrations quadrupled from 50 cm⁻³ to 200 cm⁻³. However, at the same time the total condensation nuclei (>3 nm) decreased from over 1000 cm⁻³ to 750 cm⁻³. The changes in the accumulation mode aerosol concentrations had a significant effect on the observed cloud microphysics. Observational evidence suggests that the important processes in controlling the Aitken mode concentration which, dominated the total CN concentration, included, scavenging of interstitial aerosol by cloud droplets, enhanced coagulation of Aitken mode aerosol and accumulation mode aerosol due to the increased sea salt aerosol surface area, and dilution of the MBL by free tropospheric air.     

Dimethylsulphide production in the subantarctic southern ocean under enhanced greenhouse conditions

Dimethylsulphide (DMS) is an important sulphur‐containing trace gas produced by enzymatic cleavage of its precursor compound, dimethylsulphoniopropionate (DMSP), which is released by marine phytoplankton in the upper ocean. After ventilation to the atmosphere, DMS is oxidised to form sulphate aerosols which in the unpolluted marine atmosphere are a major source of cloud condensation nuclei (CCN). Because the micro‐physical properties of clouds relevant to climate change are sensitive to CCN concentration in air, it has been postulated that marine sulphur emissions may play a rôle in climate regulation. The Subantarctic Southern Ocean (41–53°S) is relatively free of anthropogenic sulphur emissions, thus sulphate aerosols will be mainly derived from the biogenic source of DMS, making it an ideal region in which to evaluate the DMS‐climate regulation hypothesis. We have extended a previous modelling analysis of the DMS cycle in this region by employing a coupled general circulation model (CGCM) which has been run in transient mode to provide a more realistic climate scenario. The CGCM output provided meteorological data under the IPCC/IS92a radiative forcing scenario. A DMS production model has been forced with the CGCM climate data to simulate the trend in the sea‐to‐air DMS flux for the period 1960 to 2080, corresponding to equivalent CO₂ tripling relative to pre‐industrial levels. The results confirm a minor but non‐negligible increase in DMS flux in this region, in the range +1% to +6% predicted over the period simulated. Uncertainty analysis of the DMS model predictions have confirmed the positive sign for the change in DMS flux, that is a negative DMS feedback on warming.     

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.     

Investigation of aerosol–cloud interactions using a chemical transport model constrained by satellite observations

This study simulates optical depth of marine warm clouds for year 2001 based on interactively predicted aerosol concentrations with a global chemical transport model (CTM) driven by the ERA-40 re-analysis meteorological data. The simulated aerosol and cloud droplet number concentrations (CDNC) largely reproduce the variations between polluted and pristine marine environment as revealed by surface and aircraft measurements. By constraining cloud liquid water path (CLWP) with satellite microwave measurements, the simulated global and southern hemispheric aerosol optical depth (AOD) and cloud optical depth (COD) are well within 10% of the observed values. As a result of larger anthropogenic aerosol loadings over the northern oceans, the simulated CDNC and COD are, respectively, by 51 and 18% higher than those over the southern oceans, while the column-averaged droplet effective radius is 13% smaller. These simulated interhemispheric differences, while qualitatively consistent with satellite observations, are larger than the observations. Inclusion of drizzle effect improved the disparities but not entirely. The constrained CTM generally captures the seasonality in AOD and CLWP observations, and demonstrates that annual cycle of COD is dominated by CLWP. During winter monsoon the simulated and observed COD correlate more strongly with changes in AOD over the N. Indian Ocean.     

辽宁层状云微物理结构的水平变化特征

根据1997年在辽宁利用机载粒子测量系统(PMS)获取的探测资料,探讨了层状云中云滴谱、粒子数浓度在水平方向上的分布变化,并分析了温度、粒子含水量在水平方向上的变化特征。研究表明:云滴数浓度和云滴半径在水平方向上存在着较强的起伏性变化;层状云中温度在水平方向上总体变化不大;云中的云滴谱结构在水平方向上的起伏较大,存在3种变化规律;云中含水量在水平方向上的变化大,且与粒子数浓度存在正相关。