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.     

Role of the volatile fraction of submicron marine aerosol on its hygroscopic properties

The hygroscopic growth factor (HGF) of 85 nm and 20 nm marine aerosol particles was measured during January 2006 for a three-week period within the frame of the EU FP6 project MAP (Marine Aerosol Production) winter campaign at the coastal site of Mace Head, using the TDMA technique. The results are compared to aerosol particles produced in a simulation tank by bubbling air through sea water sampled near the station, and through synthetic sea water (inorganic salts). This simulation is assimilated to primary production. Aitken and mode particles (20 nm) and accumulation mode particles (85 nm) both show HGF of 1.92 and 2.01 for particles generated through bubbling in natural and artificial sea water respectively. In the Aitken mode, the marine particles sampled in the atmosphere shows a monomodal HGF slightly lower than the one measured for sea salt particles artificially produced by bubble bursting in natural sea water (HGF = 1.83). This is also the case for the more hygroscopic mode of accumulation mode particles. In addition, the HGF of 85 nm particles observed in the atmosphere during clean marine sectors exhibits half of its population with a 1.4 HGF. An external mixture of the accumulation mode marine particles indicates a secondary source of this size of particles, a partial processing during transport, or an inhomogeneity of the sea water composition. A gentle 90 °C thermo-desorption results in a significant decrease of the number fraction of moderately hygroscopic (HGF = 1.4) particles in the accumulation mode to the benefit of the seasalt mode, pointing to the presence of semi-volatile compounds with pronounced hydrophobic properties. The thermo-desorption has no effect on the HGF of bubble generated aerosols, neither for synthetic or natural sea water, nor on the atmospheric Aitken mode, indicating that these hydrophobic compounds are secondarily integrated in the particulate phase. No difference between night and day samples is observed on the natural marine aerosols regarding hygroscopicity, but a more pronounced sensitivity to volatilization of the 1.4 HGF mode in the accumulation mode is observed during the day.     

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.     

黄山夏季气溶胶多尺度吸湿性的参数化方案构建研究

利用2014年7月在黄山光明顶观测的气溶胶吸湿性参数（κ）和气溶胶离子化学组分、有机碳（OC,organic carbon）数据,对多尺度气溶胶吸湿性参数进行分析,并在此基础上建立了多尺度κ的参数化方案。研究结果表明,影响黄山夏季气溶胶来源的主要气团包括西南气团、北方气团以及东南气团。黄山夏季κ的变化范围为0.2-0.48,且随粒径增大成先增大后减小的分布特征;气溶胶粒径在0.15-1.1 μm的强吸湿段,κ>0.3,而在粒径小于0.15 μm和粒径大于1.1 μm弱吸湿段,κκ分布不同,气溶胶粒子在小于1.1 μm的粒径段,当受西南气团影响时,κ值最大,而受东南气团影响时,κ值最小;在气溶胶粒径大于1.1 μm时,κ在两个气团背景下呈现与气溶胶粒径小于1.1 μm时相反的分布特征。影响粒径小于1.1 μm气溶胶吸湿能力的主要水溶性化学组分为NH4+、SO42-、水溶性有机碳（WSOC,water soluble organic carbon）,而影响大于1.1 μm粒径范围气溶胶吸湿能力的主要水溶性化学组分为NH4+、SO42-、NO3-、WSOC和Ca2+。由气溶胶多尺度离子化学组分和WSOC构建的气溶胶κ的参数化方案,在小于1.1 μm和大于1.1 μm的粒径范围内的表达式分别为κreg=0.12+0.45fNH4++0.63fSO42-+0.18fWSOC和κreg=0.01+0.78fNH4++0.76fNO3-+0.8fSO42--0.28fCa2++0.14fWSOC（f为对应组分的质量份数）。两个参数化方案均能较好地预报κ,预报值κreg与κ的计算值间存在较好的相关关系,相关系数通过了置信度99%的显著性检验,且预报误差在30%范围内。      

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。     

黄山地区气溶胶吸湿增长特性数值模拟研究

应用多种化学组分气溶胶的绝热气块分档模式,对2008年春季黄山地区气溶胶吸湿增长特性进行了模拟分析.结果表明:黄山地区气溶胶吸湿增长因子f的大小与粒子半径、相对湿度、粒子化学组分、上升速度及上升高度密切相关,且小粒子吸湿增长比大粒子显著.吸湿增长因子与相对湿度呈正相关,相对湿度越接近粒子的临界饱和比,吸湿增长因子变化越显著.可溶性有机气溶胶,通过增加溶液中溶质的百分比来影响临界饱和比,使吸湿增长因子增大.若不考虑不可溶粒子的成核作用,会高估粒子的吸湿性.随着上升速度增大,吸湿增长因子降低,降低程度与粒子初始高度的相对湿度有关.上升高度通过改变气块相对湿度的变化来影响气溶胶吸湿增长因子.     

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.     

A study of aerosol particle sizes in the atmosphere of Athens, Greece, retrieved from solar spectral measurements

This work aims at determining the aerosol particle radii in the atmosphere of Athens. Such a work is carried out in Athens for the first time. For this purpose, solar spectral direct-beam irradiance measurements were used in the spectral range 310–575 nm. To estimate the particle radius from aerosol optical depth retrieval, a minimization technique was employed based on the golden-section search of the difference between experimental and theoretical values of the aerosol optical depth. The necessary Mie computations were performed based on the algorithm LVEC.In this study, the mean particle radius of a given distribution was calculated every 30 min during cloudless days in the period November 1996 to September 1997. The largest particles were observed in the summer and the smallest during winter. The result was verified by the increased values of the aerosol optical depth and the turbidity factors calculated in the summer. The differences in the diurnal variation from season to season are attributed to the prevailing wind regime, pollutant emission and sink rates in the atmosphere of Athens.     

基于地基观测的成都彭州气溶胶光学特性研究

利用2017年成都市彭州地区CE318型太阳分光光度计的观测数据,反演了该地区的气溶胶光学厚度(Aerosol Optical Depth,AOD)、Angstr?m指数(α)和大气浑浊度(β),分析了AOD与α、β以及可吸入颗粒物(PM₁₀、PM_(2. 5))之间的关系。结果表明:AOD表现出冬季>春季>夏季>秋季的季节变化特征,高值主要出现在冬、春季,低值主要出现在夏、秋季。Angstr?m指数在全年的波动不大,月平均值为1. 22±0. 19,低值出现在春季,高值出现在夏季。除了冬季,在其他季节观察到和Angstr?m指数具有相同的月变化趋势。AOD与β之间具有较强的相关性,但与PM₁₀、PM_(2. 5)的正相关关系表现偏弱。该地区气溶胶光学特性受北方沙尘的影响并不明显,但受到人类活动的影响显著,该地区主控态气溶胶是以细粒子为主的城市—工业型气溶胶类型。     

华东地区气溶胶分布和变化特征研究

利用中分辨率光谱仪(MODIS)获得的气溶胶光学厚度(AOD)、细粒子比例(FMF)和臭氧检测仪(OMI)获得的气溶胶指数(AI)统计分析了2005—2014年我国华东地区气溶胶光学性质的时空分布特征,同时利用潜在源分析(PSCF)模型对我国华东地区AOD和AI的潜在源区进行分析。研究结果表明:华东地区的AOD、FMF和AI时空分布存在较大的差异,2005—2014年AOD和AI的平均值高值主要分布在华东地区北部,FMF的高值区则分布在华东南部地区;10 a间华东地区AOD呈现出先升高后降低的趋势,FMF波动幅度不明显,AI值有所上升;整个华东地区AOD的季节变化较为明显,春夏两季AOD明显高于秋冬两季。华东北部和中部地区夏季由于较高的相对湿度,AOD最大可达0.8以上。而在华东南部地区,夏季受到降水的影响,AOD维持在0.2~0.4之间。FMF季节变化趋势与AOD不同,夏季最大达到0.58,春季最小仅为0.26。AI平均值在冬季最大高达0.63,夏季最小,为0.27。PSCF分析显示华东地区AOD主要源区以局地排放为主,同时也存在由河南、湖北和湖南等周边省市近距离输送影响;AI以局地和北方远距离输送为主,同时也受到河南、湖北等周边省市近距离输送的影响。     

不同水汽条件下气溶胶对雷暴云电过程影响的数值模拟研究

为全面了解水汽在气溶胶影响雷暴云电过程中的作用,本研究在已有的二维雷暴云起、放电模式基础上,通过改变相对湿度和气溶胶初始浓度(文中气溶胶浓度均指气溶胶数浓度)进行敏感性数值模拟试验.结果表明:(1)随着气溶胶浓度升高,雷暴云产生更多的小云滴,降水过程受到抑制.而当水汽含量升高时,云滴数浓度的增长速度更快,雨滴数浓度升高...     

气溶胶对北京中尺度对流系统影响的数值试验

利用可分辨云模式(WRF),模拟研究了不同气溶胶浓度对北京地区2001年8月23日一次产生强降水和冰雹的对流天气的影响。结果表明,气溶胶浓度的增加不利于对流云的发展,导致地面降水减小,但是对降水结构没有明显影响。气溶胶浓度增加导致云中水成物数浓度和质量浓度均发生变化,其中云水、冰晶和雪含量增加,而雨水、霰和雹含量减小。从云微物理学分析发现,气溶胶浓度减小有利于高层云的形成,云滴有效半径随着气溶胶浓度增加而减小。     

FY-3A/MERSI、MODIS C5.1和C6气溶胶光学厚度产品在中国区域与地面观测站点的对比分析

准确获取气溶胶光学厚度对于气候变化研究和大气环境监测具有重要意义。通过波长插值和时空匹配方法,利用气溶胶自动观测站网（AERONET）观测的气溶胶光学厚度（AOD）对风云3A/中分辨率光谱成像仪（FY-3A/MERSI）、Terra（Aqua）/MODIS的C5.1（Collections 5.1）和C6（Collections 6）气溶胶光学厚度产品在中国区域的反演精度进行验证分析。结合一次发生在中国境内的沙尘天气与一次严重雾霾天气个例,分析上述卫星气溶胶光学厚度的分布特征。研究结果表明,（1）FY-3A/MERSI AOD的反演精度较高（R=0.887,RMSE=0.234）,其值低于AERONET的观测值（Bias=-0.293）。（2）在不同的下垫面下,各种卫星暗像元算法AOD产品反演精度有差异,植被覆盖情况越好,反演精度越高,而植被很少的地区,即亮地表甚至没有反演值。（3）MODIS C5.1深蓝算法产品能在亮地表地区反演AOD,但效果不佳。MODIS C6中的深蓝算法产品在不同下垫面的反演精度都很高（RMSE为0.096-0.127）。（4）在不同季节的对比中,各种卫星AOD产品在夏季的反演精度最差,而反演最好的季节各有不同。（5）在一次沙尘天气污染与一次严重雾霾天气个例中,中国西部与北部区域,MODIS C6深蓝算法AOD的监测效果优于其他算法AOD;MERSI AOD产品在此区域的分布不连续。总体而言,MODIS C6 AOD分布比MODIS C5.1产品连续,MODIS 3 km产品在相同区域的AOD值高于其他产品。以上结论可为卫星AOD产品在中国区域的使用提供参考。      

基于离子配对法的黄山地区云凝结核闭合研究

为了对黄山地区云凝结核(Cloud Condensation Nuclei,CCN)进行闭合研究,2014年6月30日至7月28日在黄山光明顶对大气气溶胶理化性质和CCN数浓度进行观测,分析了气溶胶化学组分、谱分布以及CCN数浓度随时间变化的特征,通过κ-K?hler理论并使用离子配对法计算得到CCN数浓度与观测得到的...     

卫星气溶胶光学厚度资料同化对灰霾预报改进个例研究

面对日益严峻的大气污染形势,针对卫星气溶胶光学厚度（AOD）资料在灰霾数值预报领域的合理有效利用问题,使用WRF-Chem（WRF coupled with Chemistry）大气化学模式以及GSI（Gridpoint Statistical Interpolation）三维变分同化系统,利用MODIS和FY-3A/MERSI AOD资料,对一次灰霾天气过程进行了同化预报试验。试验结果显示,同化卫星AOD资料有效改善了模式初始场,MODIS和MERSI同化试验分别在AOD分析场的中心强度和空间分布各具优势,且对PM_2.5和PM₁₀的后续预报改进明显;从统计分析上看,同化试验的预报效果整体上好于控制试验,同化试验中PM_2.5和PM₁₀预报值的平均值、中值、平均偏差、均方根误差等指标均明显优于控制试验,且MODIS和MERSI同化试验分别在PM_2.5和PM₁₀预报统计结果中体现出了优势;卫星AOD资料同化能明显降低污染事件的空报率和漏报率,提高预报的TS评分和ETS评分。不同卫星AOD资料的差异对分析场中AOD的分布和强度产生了相应影响,进而影响了模式的灰霾预报效果;本次试验中,MODIS和MERSI AOD同化试验分别在PM_2.5和PM₁₀预报的评分上表现更佳。结果表明,卫星AOD资料同化对数值预报产生了积极的效果。      

区域站和基准站气溶胶的分析

文章讨论了秋季（1994年10月）和冬季（1995年1月）在中国西部青海省共和县瓦里关山（36°17′N,100°54′E,海拔3816 m）基准站和中国东北黑龙江省五常县的龙凤山（44°44′N,127°36′E,海拔331 m）及中国东南沿海的浙江省临安县的横畈乡（30°18′N,119°44′E,海拔131 m）两个区域本底站（上述3站均属WMO）所采集的气溶胶样品的质量浓度、可溶性离子浓度的时空分布特征和变化规律。初步得出：气溶胶质量浓度和可溶性离子浓度以临安为最高。其次是龙凤山,而瓦里关山为最低     

基于卫星观测的我国北方地区紫外吸收性气溶胶的时空分布研究

利用气溶胶指数(Aerosol Index,AI)资料研究了东亚地区紫外吸收性气溶胶的时空分布特征,主要得出以下结论:1)雨云七号卫星(Nimbus 7,N7)和地球探测卫星(Earth Probe,EP)搭载的臭氧总量测绘光谱仪(Total Ozone Mapping Spectrometer,TOMS)以及臭氧监测仪(Ozone Monitoring Instrument,OMI)反演的AI数据在东亚大陆具有较好的一致性,但EP/TOMS-OMI AI的连续性较好,而N7/TOMS-EP/TOMS AI的连续性较差;2)东亚地区紫外吸收性气溶胶主要位于塔克拉玛干沙漠及其东部周边的库姆塔格、柴达木盆地沙漠、古尔班通古特沙漠、内蒙古中西部、蒙古国南部以及我国东北、华北地区;3)紫外吸收性气溶胶具有明显的月际变化特征;4)旋转正交经验函数分析不仅能分离紫外吸收性气溶胶的源区范围,还能给出源强相对大小的定性信息。     

测量NO气体吸收截面的方法

差分吸收光谱技术(DOAS)已经被广泛用于各种污染气体浓度的测量,其中影响其测量精度的主要因素就是气体吸收截面的测量.利用Lambert Beer 吸收定律以及自主设计的测量装置对大气的主要污染气体NO的吸收截面进行了测量,并采用多项式拟合的方法提高了测量的精度,根据所测得的吸收截面反演了NO气体的浓度值,取得了良好的效果.     

冰冻圈资源可持续利用探讨

冰冻圈资源是寒区旱区社会经济发展的重要物质基础,在气候变化背景下受到了深刻的影响。在人类需求日益增长、冰冻圈资源稀缺性不断加剧的情况下,如何妥善开发利用冰冻圈资源已成为保证区域可持续发展的核心问题之一。基于“资源—资产—资本”视角的冰冻圈资源可持续利用路径为这一问题提供了新的思路,探讨了以资源资产化、资产资本化为核心的冰冻圈资源运营管理过程,并基于这一视角进行了冰冻圈服务过程的讨论,分析了中国冰冻圈流量资产效用潜力空间格局与三种潜力之间的协调程度。结果表明,东北地区大部、新疆自治区西部与藏南地区为人口与经济效用高等级流域聚集区,华北、东北、新疆西部、藏南及青藏高原东缘等地区为高潜力协调度流域聚集区。这种基于“人口-经济-生态”三大系统的效用潜力识别,有利于冰冻圈资源“提质”与“增效”两个目标的达成,进而促进冰冻圈资源可持续利用的实现。