Single Particle Characterisation of the Aerosol in the Marine Boundary Layer and Free Troposphere over Tenerife, NE Atlantic, during ACE-2

In the framework of the 2nd Aerosol Characterization Experiment (ACE-2), in June and July 1997, size segregated samples were collected for single particle analysis on the island of Tenerife, in both the marine boundary layer (MBL) and the free troposphere (FT), to study the characteristics of the North Atlantic aerosol. A systematic assessment was made of the aerosol under background conditions and when the environment was perturbed by European emissions and/or Saharan dust. The aerosol particles were analysed by automated and manual SEM-EDX, followed by cluster analysis to identify the different particle types and their abundance. Basing on back trajectory calculations, particle numbers and volume concentrations, different periods can be identified regarding the origin of the sampled air masses. In the FT, the air masses were classified as clean Atlantic, Saharan dust from Africa or pollution from Europe. In the MBL, air masses were classified as clean, polluted or perturbed by emissions from Europe. For both the FT and MBL samples, the main changes in chemical composition were observed between the fine and coarse mode aerosol. The FT fine mode aerosol is dominated by S-poor aluminosilicates (62%) in the event of the dust samples or sulphates, carbonaceous particles (20%) and S-rich aluminosilicates (46%) in the polluted samples. For the larger fractions, a strong decreasing trend was observed for the sulphates (less than 20%) and carbonaceous particles (10%) in the polluted samples. The MBL fine mode was completely dominated by S-rich particles (polluted 55% and perturbed 59%), and to a lesser extent, carbonaceous and aged sea salt particles. In the coarse mode, the polluted air mass is dominated by sea salt particles (62%). Contrary to the fine fraction, the polluted air mass in the coarse fraction contained 5.3% of S-rich particles. The combined interpretation of the data from the analysis of size-fractioned particles and the calculated backward trajectories for air masses coming from Europe, Africa and the Atlantic, results in better insights on aerosol chemistry, especially for the comparison of the particle composition in the FT and the MBL.     

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.     

基于航测的珠三角气溶胶垂直分布及活化特性

2017年9月14—27日在珠江三角洲地区开展了6个架次飞机观测试验。利用飞行获取的气溶胶、云凝结核、云滴及常规气象探头观测资料,结合天气形势、气象条件及气团后向轨迹分析,研究了珠江三角洲地区深圳气溶胶数浓度及其谱的垂直分布特征,配合不同过饱和度条件下云凝结核浓度观测,分析了气溶胶活化特性。结果表明:在不同天气条件下,深圳低层气溶胶数浓度变化范围为500~9000 cm-3;边界层内气溶胶分布相对均匀,谱型随高度变化与气象条件相关。将6个架次气溶胶观测资料根据数浓度及谱型分为3种类型:类型Ⅰ为海洋型气溶胶,数浓度小,粒子尺度大,谱型呈双峰分布;类型Ⅲ为大陆型气溶胶,数浓度高,粒子尺度小,谱宽较宽且呈三峰分布;类型Ⅱ为海洋大陆影响型气溶胶,即受海洋和大陆共同影响,数浓度低于类型Ⅲ高于类型Ⅰ,谱型为双峰分布。拟合了包含海洋型及大陆型气溶胶的3个架次近地面云凝结核活化谱,计算了气溶胶在不同过饱和度条件下的活化效率。     

Cloud condensation nuclei measurements at Mace Head, Ireland, over the period 1994–2002

Analyses of cloud condensation nuclei (CCN) number concentrations (cm^− 3) measured at the Mace Head Atmospheric Research Station, near Carna, County Galway, Ireland, using a DH Associates Model M1 static thermal diffusion cloud chamber over the period from March 1994 to September 2002 are presented in this work. Air masses are defined as being ‘marine’ if they originate from a wind direction of 180–300° and ‘continental’ air masses are defined as originating from a wind direction of 45–135°. Air masses without such filtering were classified as ‘undefined’ air masses. Air masses were found to be dominated by marine sector air, re-affirming Mace Head as a baseline atmospheric research station. CCN levels for specific air masses at Mace Head were found to be comparable with earlier studies both at Mace Head and elsewhere. Monthly averaged clean marine (wind direction of 180–300° and black carbon absorption coefficient < 1.425 Mm^− 1) CCN and marine CCN varied between 15–247 cm^− 3 and 54–670 cm^− 3, respectively. As expected, significant increases in number concentration were found in continentally sourced CCN over that of marine CCN and were found to follow a log-normal distribution significantly tighter than that of clean marine air masses. No significant trend was found for CCN over the 9-year period. While polluted continental air masses showed a slight increase in CCN concentrations over the winter months, most likely due to increased fuel usage and a lower mixed boundary layer, the dominance of marine sector air arriving at Mace Head, which generally consists of background CCN concentrations, reduced seasonal differences for polluted air. Marine air showed a distinct seasonal pattern, with elevated values occurring over the spring and summer seasons. This is thought to be due to enhanced biogenic aerosol production as a result of phytoplankton bloom activity in the North Atlantic.     

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.     

Cloud condensation nuclei (CCN) concentration in the Brazilian northeast semi-arid region: the influence of local circulation

Ground-based aerosol instrumentation covering particle size diameters from 25 nm to 32 µm was deployed to determine aerosol concentration and cloud condensation nuclei (CCN)-activation properties at water vapor supersaturations in the range of S = 0.20–1.50 % in the remote Brazilian northeast semi-arid region (NEB) in coastal (maritime) and continental (inland) regimes. The instruments measured aerosol number concentration and activation spectra for CCN and revealed that aerosol properties are sensitive with respect to the sources as a function of the local wind circulation system. The observations show that coastal aerosol total number concentrations are above 3,000 cm^?3 on average, exhibiting concentration peaks depending on the time of the day in a consistent daily pattern. The variation on aerosol concentration has also influences on the fraction of particles active as CCN. At 1.0 % water vapor supersaturation, the fraction can reach as high as 80 %. Inland aerosol total concentrations were about 1,800–1,900 cm^?3 and did not show much diurnal variation. The fraction of particles active as CCN observed inland depend on the history of the air masses, and was much higher when air masses were originated over the sea. It was found that (NH₄)₂SO₄ and NaCl are the major soluble inorganic fraction of the aerosols at the coast. The major fraction of NaCl was present in the coarse mode, while ammonium sulfate dominates the inorganic fraction at the submicron range, with about 10 % of the total aerosol mass at 0.32 µm. Inorganic compounds are almost absent in particles with sizes around 0.1 μm. The study suggests that the air masses with high concentration of CCN originate at the sea. The feasible explanation lies in the fact that the NEB’s beaches have a particular morphology that produces a wide surf zone and creates a large load of aerosols when combined with strong and permanent winds of the region.     

Investigation of aerosol indirect effects on simulated flash-flood heavy rainfall over Korea

This study investigates aerosol indirect effects on the development of heavy rainfall near Seoul, South Korea, on 12 July 2006, focusing on precipitation amount. The impact of the aerosol concentration on simulated precipitation is evaluated by varying the initial cloud condensation nuclei (CCN) number concentration in the Weather Research and Forecasting (WRF) Double-Moment 6-class (WDM6) microphysics scheme. The simulations are performed under clean, semi-polluted, and polluted conditions. Detailed analysis of the physical processes that are responsible for surface precipitation, including moisture and cloud microphysical budgets shows enhanced ice-phase processes to be the primary driver of increased surface precipitation under the semi-polluted condition. Under the polluted condition, suppressed auto-conversion and the enhanced evaporation of rain cause surface precipitation to decrease. To investigate the role of environmental conditions on precipitation response under different aerosol number concentrations, a set of sensitivity experiments are conducted with a 5?% decrease in relative humidity at the initial time, relative to the base simulations. Results show ice-phase processes having small sensitivity to CCN number concentration, compared with the base simulations. Surface precipitation responds differently to CCN number concentration under the lower humidity initial condition, being greatest under the clean condition, followed by the semi-polluted and polluted conditions.     

Cloud Condensation Nuclei over the Bay of Bengal during the Indian Summer Monsoon

The first measurements of cloud condensation nuclei(CCN) at five supersaturations were carried out onboard the research vessel "Sagar Kanya"(cruise SK-296) from the south to the head-bay of the Bay of Bengal as part of the Continental Tropical Convergence Zone(CTCZ) Project during the Indian summer monsoon of 2012. In this paper, we assess the diurnal variation in CCN distributions at supersaturations from 0.2% to 1%(in steps of 0.2%) and the power-law fit at supersaturation of 1%.The diurnal pattern shows peaks in CCN concentration(NCCN) at supersaturations from 0.2% to 1% between 0600 and 0700 LST(local standard time, UTC+0530), with relatively low concentrations between 1200 and 1400 LST, followed by a peak at around 1800 LST. The power-law fit for the CCN distribution at different supersaturation levels relates the empirical exponent(k) of supersaturation(%) and the NCCNat a supersaturation of 1%. The NCCNat a supersaturation of 0.4% is observed to vary from 702 cm~(-3) to 1289 cm~(-3), with a mean of 961 ± 161 cm~(-3)(95% confidence interval), representing the CCN activity of marine air masses. Whereas, the mean NCCNof 1628 ± 193 cm~(-3) at a supersaturation of 1% is higher than anticipated for the marine background. When the number of CCN spectra is 1293, the value of k is 0.57 ± 0.03(99% confidence interval)and its probability distribution shows cumulative counts significant at k ≈ 0.55 ± 0.25. The results are found to be better at representing the features of the marine environment(103 cm~(-3) and k ≈ 0.5) and useful for validating CCN closure studies for Indian sea regions.     

天空辐射计观测反演北京城区气溶胶光学特性

利用2018年10月—2019年9月天空辐射计观测数据反演北京城区气溶胶光学特性参数,重点分析污染过程中气溶胶光学特性与气象条件的相关性。结果表明:500 nm气溶胶光学厚度在2—7月较大,最高值出现在6月,为0.71。单次散射反照率最高值出现在8月,为0.96;最低值出现在5月,为0.89。440~870 nm ?ngstr?m波长指数最高值出现在夏季,为1.11;最低值出现在春季,为0.89。统计发现污染日数仅占总日数的17%,其中62%为轻度污染;污染和清洁天气条件下PM_2.5浓度分别为107.22 μg·m-3和47.16 μg·m-3,500 nm气溶胶光学厚度分别为0.85和0.49,单次散射反照率分别为0.96和0.92;冬季?ngstr?m波长指数在污染天气条件下（1.02）大于清洁天气（0.91）,春季相反。结合天空辐射计、激光雷达和气象数据分析2019年1月一次污染事件,可知低风速与高湿度等不利气象条件、气溶胶粒子的吸湿增长和二次转化、污染物局地排放及区域输送共同导致污染事件发生。     

Cloud condensation nuclei from biomass burning during the Amazonian dry-to-wet transition season

Aircraft measurements of cloud condensation nuclei (CCN) during the Large-Scale Biosphere–Atmosphere Experiment in Amazonia (LBA) were conducted over the Southwestern Amazon region in September–October 2002, to emphasize the dry-to-wet transition season. The CCN concentrations were measured for values within the range 0.1–1.0% of supersaturation. The CCN concentration inside the boundary layer revealed a general decreasing trend during the transition from the end of the dry season to the onset of the wet season. Clean and polluted areas showed large differences. The differences were not so strong at high levels in the troposphere and there was evidence supporting the semi-direct aerosol effect in suppressing convection through the evaporation of clouds by aerosol absorption. The measurements also showed a diurnal cycle following biomass burning activity. Although biomass burning was the most important source of CCN, it was seen as a source of relatively efficient CCN, since the increase was significant only at high supersaturations.     

Size‐segregated chemical, gravimetric and number distribution‐derived mass closure of the aerosol in Sagres, Portugal during ACE‐2

During the ACE‐2 field campaign in the summer of 1997 an intensive, ground‐based physical and chemical characterisation of the clean marine and continentally polluted aerosol was performed at Sagres, Portugal. Number size distributions of the dry aerosol in the size range 3–10 000 nm were continuously measured using DMPS and APS systems. Impactor samples were regularly taken at 60% relative humidity (RH) to obtain mass size distributions by weighing the impactor foils, and to derive a chemical mass balance by ion and carbon analysis. Hygroscopic growth factors of the metastable aerosol at 60% RH were determined to estimate the number size distribution at a relative humidity of 60%. A size segregated 3‐way mass closure study was performed in this investigation for the first time. Mass size distributions at 60% RH derived from number size distribution measurements and impactors samples (weighing and chemical analysis) are compared. A good agreement was found for the comparison of total gravimetrically‐determined mass with both number distribution‐derived (slope=1.23/1.09; R²>0.97; depending on the parameters humidity growth and density) and chemical mass concentration (slope=1.02; R²= 0.79) for particles smaller than 3 μm in diameter. Except for the smallest impactor size range relatively good correlations (slope=0.86–1.42) with small deviations (R²=0.76–0.98) for the different size fractions were found. Since uncertainties in each of the 3 methods are about 20% the observed differences in the size‐segregated mass fractions can be explained by the measurement uncertainties. However, the number distribution‐derived mass is mostly higher than the chemically and gravimetrically determined mass, which can be explained by sampling losses of the impactor, but as well with measurement uncertainties as, e.g., the sizing of the DMPS/APS.     

基于气象要素的气溶胶吸湿增长分析:以浙江省为例

气溶胶粒子的吸湿增长对区域环境、气象与辐射收支都有巨大影响,精确的气溶胶吸湿特性观测对描述气溶胶吸湿增长特性,以及研究气溶胶对气候环境影响,拓展卫星气溶胶产品的应用有非常重要的意义。本研究提出一种基于常规气象观测（能见度、相对湿度）和空气质量观测（PM2.5浓度,即空气动力学当量直径小于等于2.5 μm的颗粒物浓度）相结合的气溶胶吸湿增长估算方法,在此基础上对浙江地区气溶胶吸湿特性的时空变化影响因素进行了探讨。研究发现,沿海的温州瓯海站的吸湿增长能力最高,长三角典型城市环境的杭州和睦小学站的吸湿增长能力次之,而地处较为洁净内陆的衢州实验学校站的吸湿增长能力最低。在时间变化中,同一站点不同湿度条件的吸湿增长变化趋势相同,温州瓯海站的吸湿性变化最为剧烈,杭州和睦小学站的吸湿性变化次之,衢州实验学校站变化较为平缓。本研究表明,浙江地区的气溶胶吸湿增长特性存在较大的时空差异,基于本方法能够在较大的时空范围内描述气溶胶的吸湿增长特性,为有限的精密观测提供重要补充。     

A closure study of sub-micrometer aerosol particle hygroscopic behaviour

The hygroscopic properties of sub-micrometer aerosol particles were studied in connection with a ground-based cloud experiment at Great Dun Fell, in northern England in 1995. Hygroscopic diameter growth factors were measured with a Tandem Differential Mobility Analyser (TDMA) for dry particle diameters between 35 and 265 nm at one of the sites upwind of the orographic cloud. An external mixture consisting of three groups of particles, each with different hygroscopic properties, was observed. These particle groups were denoted less-hygroscopic, more-hygroscopic and sea spray particles and had average diameter growth factors of 1.11–1.15, 1.38–1.69 and 2.08–2.21 respectively when taken from a dry state to a relative humidity of 90%. Average growth factors increased with dry particle size. A bimodal hygroscopic behaviour was observed for 74–87% of the cases depending on particle size. Parallel measurements of dry sub-micrometer particle number size distributions were performed with a Differential Mobility Particle Sizer (DMPS). The inorganic ion aerosol composition was determined by means of ion chromatography analysis of samples collected with Berner-type low pressure cascade impactors at ambient conditions. The number of ions collected on each impactor stage was predicted from the size distribution and hygroscopic growth data by means of a model of hygroscopic behaviour assuming that only the inorganic substances interacted with the ambient water vapour. The predicted ion number concentration was compared with the actual number of all positive and negative ions collected on the various impactor stages. For the impactor stage which collected particles with aerodynamic diameters between 0.17–0.53 μm at ambient relative humidity, and for which all pertinent data was available for the hygroscopic closure study, the predicted ion concentrations agreed with the measured values within the combined measurement and model uncertainties for all cases but one. For this impactor sampling occasion, the predicted ion concentration was significantly higher than the measured. The air mass in which this sample was taken had undergone extensive photochemical activity which had probably produced hygroscopically active material other than inorganic ions, such as organic oxygenated substances.     

Hygroscopic growth of aerosol particles and its influence on nucleation scavenging in cloud: Experimental results from Kleiner Feldberg

The hygroscopic growth of individual aerosol particles has been measured with a Tandem Differential Mobility Analyser. The hygroscopic growth spectra were analysed in terms of diameter change with increasing RH from 20% to 85%. The measurements were carried out during the GCE cloud experiment at Kleiner Feldberg, Taunus, Germany in October and November 1990.Two groups of particles with different hygroscopic growth were observed. The less-hygroscopic group had average growth factors of 1.11, 1.04 and 1.02 for particle diameters of 50, 150 and 300 nm, respectively. The more-hygroscopic group had average growth factors of 1.34, 1.34, and 1.37 for the same particle diameters. The average fraction of less-hygroscopic particles was about 50%. Estimates of the soluble fractions of the particles belonging to the two groups are reported.Hygroscopic growth spectra for total aerosol, interstitial aerosol and cloud drop residuals were measured. A comparison of these hygroscopic growths of individual aerosol particles provides clear evidence for the importance of hygroscopic growth in nucleation scavenging. The measured scavenged fraction of particles as a function of diameter can be explained by the hygroscopic growth spectra.     

The effect of clouds on aerosol growth in the rural atmosphere

Measurements of accumulation mode aerosol in the atmospheric boundary layer under cloudy and cloud-free conditions, and in the lower free troposphere under cloud-free conditions, were conducted over the rural northwest of England. Normalised size distributions in the cloud-free boundary layer (CFBL) and the cloud-free free troposphere (CFFT) exhibited almost identical spectral similarities with both size distributions possessing a concentration peak mode-radius of ≈0.05 μm or less. By comparison, aerosol distributions observed in cloudy air exhibited a distinctive log-normal distribution with mode-radii occurring at ≈0.1 μm concomitant with a local minimum at ≈0.05 μm. The consistent and noticeable difference in spectral features observed between cloudy and cloud-free conditions suggest that a greater amount of gas-to-particle conversion occurs on cloudy days, presumably through in-cloud aqueous phase oxidation processes, leading to larger sized accumulation mode particles. Apart from the distinct difference between cloudy and cloud-free aerosol spectra on cloudy days, aerosol concentration and mass were observed to be significantly enhanced above that of the ambient background in the vicinity of clouds. Volatility analysis during one case of cloud processing indicated an increase in the relative contribution of aerosol mass volatile at temperatures characteristic of sulphuric acid, along with a smaller fraction of more volatile material (possibly nitric acid and/or organic aerosol). Growth-law analysis of possible growth mechanisms point to aqueous phase oxidation of aerosol precursors in cloud droplets as being the only feasible mechanism capable of producing the observed growth. The effect of cloud processing is to alter the cloud condensation nuclei (CCN) supersaturation spectrum in a manner which increases the availability of CCN at lower cloud supersaturations.     

A GIS based approach to back trajectory analysis for the source apportionment of aerosol constituents and its first application

A new method has been developed to combine back trajectory statistics with a detailed land cover analysis. It provides numeric proxies for the residence times of sampled air masses above certain land cover classes (marine, natural vegetation, agricultural lands, urban areas, and bare areas), as well as further meteorological parameters (mean trajectory length, solar radiation along trajectory, and local height of the boundary mixing layer). The method has been implemented into a GIS-enabled database system to allow for an efficient processing of large datasets with low computational demands. A principal component analysis was performed on a dataset including the modelled residence times, the modelled meteorological parameters, some measured meteorological parameters (wind speed and temperature), and the concentrations of 10 particle constituents (inorganic ions and organic and elemental carbon) in 5 particle size ranges for 29 winter- and summertime samples at an urban background site in Leipzig, Germany. Six principal components could be extracted which together explained about 80% of the total variance in the dataset. The factors could be attributed to the influence of meteorology to continental background pollution, secondary formation processes in polluted air masses, wood burning, aged sea-salt, local traffic, and long-range transported crustal material. The modelled residence times and the meteorological parameters were generally consistent with the existing knowledge of specific particle sources and thereby facilitated and strengthened the interpretation of the factors. Moreover, they allowed for a clear distinction between continental background pollution and secondary formation processes, which has not been possible in previous source apportionment studies. The results demonstrate that the combined usage of back trajectory, land cover, and meteorological data by the presented method yields valuable additional information on the history of sampled air masses, which can improve the quality of source apportionment of atmospheric aerosol constituents.     

Oscillation of Surface PM<Subscript>2.5</Subscript> Concentration Resulting from an Alternation of Easterly and Southerly Winds in Beijing: Mechanisms and Implications

We used simultaneous measurements of surface PM_2.5 concentration and vertical profiles of aerosol concentration, temperature, and humidity, together with regional air quality model simulations, to study an episode of aerosol pollution in Beijing from 15 to 19 November 2016. The potential effects of easterly and southerly winds on the surface concentrations and vertical profiles of the PM_2.5 pollution were investigated. Favorable easterly winds produced strong upward motion and were able to transport the PM_2.5 pollution at the surface to the upper levels of the atmosphere. The amount of surface PM_2.5 pollution transported by the easterly winds was determined by the strength and height of the upward motion produced by the easterly winds and the initial height of the upward wind. A greater amount of PM_2.5 pollution was transported to upper levels of the atmosphere by upward winds with a lower initial height. The pollutants were diluted by easterly winds from clean ocean air masses. The inversion layer was destroyed by the easterly winds and the surface pollutants and warm air masses were then lifted to the upper levels of the atmosphere, where they re-established a multi-layer inversion. This region of inversion was strengthened by the southerly winds, increasing the severity of pollution. A vortex was produced by southerly winds that led to the convergence of air along the Taihang Mountains. Pollutants were transported from southern–central Hebei Province to Beijing in the boundary layer. Warm advection associated with the southerly winds intensified the inversion produced by the easterly winds and a more stable boundary layer was formed. The layer with high PM_2.5 concentration became dee-per with persistent southerly winds of a certain depth. The polluted air masses then rose over the northern Taihang Mountains to the northern mountainous regions of Hebei Province.     

Aerosol Properties and Their Impacts on Surface CCN at the ARM Southern Great Plains Site during the 2011 Midlatitude Continental Convective Clouds Experiment

Aerosol particles are of particular importance because of their impacts on cloud development and precipitation processes over land and ocean. Aerosol properties as well as meteorological observations from the Department of Energy Atmospheric Radiation Measurement(ARM) platform situated in the Southern Great Plains(SGP) are utilized in this study to illustrate the dependence of continental cloud condensation nuclei(CCN) number concentration(NCCN) on aerosol type and transport pathways. ARM-SGP observations from the 2011 Midlatitude Continental Convective Clouds Experiment field campaign are presented in this study and compared with our previous work during the 2009–10 Clouds, Aerosol, and Precipitation in the Marine Boundary Layer field campaign over the current ARM Eastern North Atlantic site. Northerly winds over the SGP reflect clean, continental conditions with aerosol scattering coefficient(σ_(sp)) values less than 20 Mm~(-1) and NCCNvalues less than 100 cm~(-3). However, southerly winds over the SGP are responsible for the observed moderate to high correlation(R)among aerosol loading(σ_(sp) 60 Mm~(-1)) and NCCN, carbonaceous chemical species(biomass burning smoke), and precipitable water vapor. This suggests a common transport mechanism for smoke aerosols and moisture via the Gulf of Mexico,indicating a strong dependence on air mass type. NASA MERRA~(-2) reanalysis aerosol and chemical data are moderately to highly correlated with surface ARM-SGP data, suggesting that this facility can represent surface aerosol conditions in the SGP, especially during strong aerosol loading events that transport via the Gulf of Mexico. Future long-term investigations will help to understand the seasonal influences of air masses on aerosol, CCN, and cloud properties over land in comparison to over ocean.     

Highly Biased Hygroscopicity Derived from Size-Resolved Cloud Condensation Nuclei Activation Ratios without Data Inversion

The impact of aerosols on the climate and atmospheric environment depends on the water uptake ability of particles; namely, hygroscopic growth and acti- vation into cloud condensation nuclei （CCN）. The size-resolved activation ratios （SRAR）, characterizing the fraction of aerosol particles that act as CCN at different particle sizes and supersaturations, can be measured using a combination of differential mobility analyzers （DMA） and particle counters. DMA-based measurements are in- fluenced by the multiply charged particles and the quasi-mono-dispersed particles （effect of DMA transfer function） selected for each prescribed particle size. A theoretical study, assuming different particle number size distributions and hygroscopicity of aerosols, is performed to study the effects of the DMA transfer function and multiple charging on the measured SRAR and the derived hygroscopicity. Results show that the raw SRAR can be significantly skewed and hygroscopicity may be highly biased from the true value if the data are not corrected. The effect of the transfer function is relatively small and depends on the sample to sheath flow ratio. Multiply charged particles, however, can lead to large biases of the SRAR. These results emphasize that the inversion algo- rithm, which is used to correct the effects of the DMA transfer function and multiple charging, is necessary for accurate measurement of the SRAR.     

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.