层状云清除气溶胶的数值模拟

建立了一个一维层状云系的气溶胶清除模式,模式旨在模拟云发展过程中云、雨水中气溶胶浓度的时空演变规律,研究气溶胶粒子的云内清除和云下清除的相对贡献大小及其湿沉降速率等.模拟结果在一定程度上与实测结果相符.     

Chemical composition differences in fog and cloud droplets of different sizes

The distribution of acidity and solute concentration among the various droplet sizes in a fog or cloud and the effect of the evaporation-condensation cycle on the composition and size distribution of atmospheric aerosol is studied. Significant total solute concentration differences can occur in aqueous droplets inside a fog or cloud. For the fog simulated here, during the period of dense fog, the solute concentration in droplets larger than 10 μm diameter increased with size, in such a way that droplets of diameter 20 μm attain a solute concentration that is a factor of 3.6 larger than that in the 10 μm droplets. Droplets on which most of the liquid water condenses have access to most of the reacting medium for in situ S(IV) oxidation and are therefore preferentially enriched in sulfate. The gas and aqueous-phase chemical processes result in an increase of the total solute mass concentration nonuniform over the droplet spectrum for a mature fog. These chemical processes tend to decrease the total solute mass concentration differences among the various droplet sizes. Low cooling rates of the system also tend to decrease these concentration differences while high cooling rates have exactly the opposite effect. The mass/size distribution of the condensation nuclie influences quantitatively, but not qualitatively, the above concentration differences.     

Determining the acidity and chemical composition of fog,haze and cloud droplets in Israel

The chemistry and acidity of individual droplets were analyzed in samples of fog, haze and cloud collected at Tel Aviv University on the Mediterranean seacoast and at the top of Mt Meron and of Mt Carmel in northern Israel. Acidity was measured using pH paper in a cascade impactor. The characteristics of droplets and interstitial particles 0.3–20.0 μm in size were identified using microspot and electron microscopy techniques.The results revealed the following: (1) the aerosols in the micrometer and sub-micrometer range were mostly very acidic droplets, with pH as low as 2.0, caused by the presence of sulfuric acid; (2) lower acidity was associated with an increase in droplet size, due to dilution by condensation or nucleation scavenging of mineral dust, i.e. gypsum, calcite and dolomite; (3) both acidic and alkaline droplets contained significant amounts of sulfur; and (4) the alkaline droplets contained minerals and salt solutions of Na₂SO₄, CaSO₄, or NaCl.     

一次对流过程对气溶胶清除和再生过程的影响

利用中尺度天气预报和研究模式(WRF)对2007年4月23～24日广东省发生的一次飑线过程进行了模拟,研究了水凝物粒子对气溶胶的清除过程、液滴蒸发引起的气溶胶再生过程以及动力输送作用对气溶胶数浓度的影响.结果表明,降水与近地层气溶胶数浓度的变化呈负相关关系.综合对比各水凝物种类的碰撞清除率和核化清除率,发现云滴核化过程...     

Some physical factors influencing scavenging ratios

A better understanding of the causes of scavenging ratio variation is required if one is to use them more precisely for predicting the chemical concentrations in precipitations. For this purpose, a set of 82 rain and associated aerosol samples were obtained during a 1-year sampling program in Paris. Scavenging ratios are calculated for Cl, SO₄²⁻, Na, K, Mg, Ca, Zn, Al, Si and Fe. First, it is shown that scavenging ratios enable us to describe the scavenging processes correctly, even on an urban site: classification of air masses according to back-trajectories indicates similar long range transport impact on both aerosol and precipitation. Scavenging ratios are then shown to vary with the volume of rain: this is interpreted as a dilution effect related to the depletion of the aerosol source. On the other hand, average rain-rate has little effect, if any, on the scavenging parameter. Finally, the role of the cloud mass type (stratiform or convective) is investigated, in relation with differences in nucleation capabilities.     

On the drop and aerosol size dependence of aqueous sulfate formation in a continental cumulus cloud

An entraining air parcel model including microphysical and chemical processes is used to investigate the drop size dependence of pollutant concentrations in a growing cloud under continental background conditions. For the calculation of the chemical processes, the drop size of the cloud drops and their initial dry particle size before activation is taken into account. The size dependence of the pollutant concentration in drops smaller than 8 μm radius is mainly influenced by the activation and fast condensational growth of recently entrained particles. In drops larger than 20 μm radius the main process influencing the drop size dependence of the pollutant concentration is coalescence between drops. The size dependence in drops between 8 and 20 μm radius is determined by the drops activated at the cloud base and the drops growing on particles that are entrained at higher altitudes, the influence of the latter rapidly increasing with height. Drops that are growing on large particles are polluted with initital aerosol matter to such an extent that sulfate production by oxidation is not significant in them. In drops growing on small particles the initial aerosol load has relatively little influence on the chemical processes in the drop. Oxidation of S(IV), especially by ozone, takes place mainly in these drops. The dependence of chemical processes of initial dryk particle size holds throughout the most of the cloud, until coalescence starts playing a role. If the cloud evaporates before producing precipitation-sized drops, the increase of aerosol mass due to cloud chemical processes is found to have taken place in the aerosol accumulation mode. If precipitation-sized drops were produced during the cloud stage, the soluble volume fraction of the aerosol matter has increased throughout the aerosol size distribution, but mainly in the accumulation mode.     

Submicron aerosol size distributions measured over the tropical and South Pacific

Size distributions of aerosol particles in the radius range of 0.006–0.53 μm were measured over the Pacific Ocean along the 150° longitude from about 20°N to 55°S. Throughout the tropical trade wind region, the size distribution of fine particles was relatively stable and exhibited a double-peaked characteristic with one peak at about 0.1 μm and the other in the 0.02–0.04 μm region, separated by a minimum at about 0.06 μm. The total concentrations of particles were in the 150–300 cm⁻³ range with 60–150 cm⁻³ residing in the accumulation mode (0.06<r<0.5 μm). South of the trade wind region, the measured size distributions and meteorological conditions were more diverse. Periods with very low concentrations in the accumulation mode were associated with regions of large-scale precipitation. Large increases in the number of nucleation mode particles were found in air masses with low concentrations of particles in the accumulation mode.     

华南高山背景地区黑碳云内清除特征

基于2020年南岭背景高山地区的3个典型云事件,利用地用逆流虚拟撞击器采集云中颗粒物,结合单颗粒黑碳光度计和激光雾滴谱仪分析黑碳浓度及云参数特征,探讨黑碳云内清除率及其影响因素.结果表明：进入云内的黑碳约占整体的20%,而云中含黑碳云滴的占比（4.67%）则少于含黑碳间隙颗粒的占比（15.31%）;黑碳的分粒径质量清除率和数量清除率接近,变化范围均为28%~59%;高液态含水量和云滴数浓度有利于黑碳云内清除率的增加,而黑碳云内清除率会随黑碳总浓度的增加而降低,各因素对于黑碳云内清除的影响由大到小为：云滴数浓度>液态含水量>总黑碳浓度.     

新疆干旱区气溶胶间接效应区域性分析

利用MODIS气溶胶和云资料以及实测的降水数据,可从宏观角度分析新疆区域气溶胶时空分布特征,研究气溶胶与云和降水之间的相互影响关系.结果表明：近十年来受区域暖-干趋势的转变影响,新疆地区气溶胶光学厚度空间分布呈现显著的区域性和季节性差异;南疆地区气溶胶光学厚度整体高于北疆地区,春、夏高,秋、冬低,整体呈现增加趋势,其中,北疆地区气溶胶光学厚度变化程度相对较为显著;受气候变化和颗粒粒径差异影响,新疆干旱区云光学厚度与气溶胶光学厚度呈负相关变化趋势,相关系数北疆地区高于南疆地区;云水路径受温度、湿度影响较大,对气溶胶光学厚度的变化的敏感程度北疆大于南疆,夏季最高,冬季最低;气溶胶光学厚度与云滴粒子有效半径关系复杂,受水汽影响较大,在云层含水量较低的情况下,云滴粒子有效半径与气溶胶光学厚度呈负相关,说明在干燥地区或季节,气溶胶的增加,抑制云滴粒子的增长;整体来看,新疆干旱区气溶胶的增加抑制了区域降水的形成.     

干旱区云凝结核分布及其影响因子的观测研究

利用DMT CCN仪对宁夏盐池、银川地区地面及高空的云凝结核(CCN)进行实时连续观测.大量资料分析结果表明, CCN日变化明显,受人为因素影响,清晨和傍晚出现高值.夜晚温度与CCN浓度呈正相关,白天相反;强降水对CCN具有一定冲刷作用;沙尘气溶胶没有有效增加盐池地区的CCN浓度.与华北地区比较,银川、盐池地区CCN浓度偏低.此外,研究表明,过饱和度越高,活化CCN浓度越大.根据N=CSK拟合活化谱,银川属于典型大陆性核谱.由于云内清除作用,高空CCN浓度下降明显,但逆温层的存在使得该区CCN浓度累积增加.     

A theoretical determination of the collection rates of aerosol particles by falling ice crystal plates and columns

A theoretical model for the removal of aerosol particles by falling columnar ice crystals is compared to the model results for the removal of aerosol particles by falling planar ice crystals. These results incorporate gravitational, inertial, electrostatic, thermophoretic, diffusiophoretic, and Brownian diffusion mechanisms. Scavenging rates for columnar and planar ice crystals are computed for aerosol particles ranging from 0.001 to 10 μm in radius. The results show that planar ice crystals have greater collection efficiencies than the columnar ice crystals.     

石家庄地区雾霾天气下云滴和云凝结核的分布特征

2009年5~10月在石家庄地区对雾霾天气下的近地面到高空的云雾滴和云凝结核(CCN)进行了7架次飞机探测.利用PMS云粒子测量仪器、机载温湿仪和连续气流纵向热梯度云凝结核仪获得的云雾粒子和云凝结核(CCN)探测资料,分析了层积云(Sc)和高积云(Ac)中云粒子浓度、液态含水量、粒子算术平均直径和粒子有效平均直径的垂直分布特征;分析了CCN垂直和水平分布特征以及谱分布.结果表明雾霾天气状况下,云滴数浓度在102个/cm3量级上.高云粒子粒径总体大于低云粒子.云含水量平均值范围为0.03~0.14g/m3;地面到600 m高度内, CCN值的平均值为3034cm-3(过饱和度S=0.3%).对CCN的活化谱进行拟合表明石家庄属于典型大陆性核谱,云对CCN有消耗作用,逆温层的存在使得该区CCN浓度累积增加.     

南京2007年12月持续雾霾过程的大气消光特性

2007年南京冬季雾外场综合试验期间,雾、霾交替持续的最长时间达100 h以上。利用大气气溶胶粒子和雾滴数浓度尺度谱分布、能见度、相对湿度等同步观测资料,从Mie散射理论出发,研究了雾、霾不同阶段大气消光特征,重点分析了大气气溶胶粒子和雾滴在雾、霾持续和转化过程中的消光作用。结果表明,雾、霾过程不同阶段平均能见度的大小关系为：雾<湿霾<霾~轻雾。平均而言,雾阶段雾滴和气溶胶粒子的消光作用相当,其中,雾滴消光波动幅度大于气溶胶粒子消光,能见度的变化趋势主要由雾滴的消光决定。湿霾、霾和轻雾阶段的消光主要由气溶胶粒子造成。湿霾阶段的低能见度是由于大量积聚模态的气溶胶粒子在较高相对湿度环境中吸湿增长所致。霾阶段气溶胶粒子数浓度达到最大,核模态粒子占总数浓度的80%左右,是导致该阶段能见度较低的主要原因。轻雾阶段气溶胶粒子的消光系数最小,但雾滴可提供10%~15%的消光贡献,导致能见度与霾阶段相当。     

蓬莱19-3原油水下溢油的模拟实验

把握水下溢油时油滴粒径的分布规律是研究溢油行为和归宿的前提,也是水下溢油事故有效应急处置的重要依据。本研究采用自制的1 m×1 m×2 m（长×宽×高）的水下溢油模拟实验装置开展蓬莱19-3原油的水下溢油模拟实验,以油滴体积分布和油滴体积中值粒径为考察指标,评估了水下溢油喷口直径和喷射速度对油滴破碎形成的油滴粒径分布的影响。结果表明,不同粒径油滴体积分布总体上表现为低于100 μm和高于700 μm的油滴粒径体积占比较小,油滴粒径分布主要集中在100 μm~700 μm之间,体积比最高点位置根据喷射条件的不同而有所偏移。喷口直径保持不变时,随着喷射速度增大,小粒径油滴所占体积逐渐增大,大粒径油滴体积比减小。油滴体积中值粒径随喷射速度的增加而减小,相对体积中值粒径与喷射流量经对数变换后呈线性相关关系。本研究结果可为水下溢油行为轨迹的预测提供重要依据。     

嘉兴市冬季不同空气质量等级下大气污染物的分布特征

为研究浙江省嘉兴市冬季PM、污染气体和含碳气溶胶在不同空气质量等级下的分布特征,于2013年11月28日—12月28日使用SHARP测尘仪、热电EMS系统和Sunset在线OCEC分析仪观测了PM（PM₁₀和PM_2.5）、污染气体（SO₂、NO₂、CO和O₃）和含碳气溶胶〔OC（有机碳）、EC（元素碳）和TC（总碳）〕的质量浓度,结合气象数据和HYSPLIT模式,分析了霾污染过程中大气污染物浓度变化、日变化及其来源特征.结果表明:嘉兴市冬季霾天ρ（PM_2.5）、ρ（PM₁₀）、ρ（SO₂）、ρ（NO₂）、ρ（O₃）、ρ（OC）、ρ（EC）、ρ（POC）和ρ（SOC）分别为167.90、248.86、77.79、、97.16、28.50、27.09、7.72、7.50和19.59 μg/m3,ρ（CO）为1.47 mg/m3,分别是空气质量为良时的3.00、2.50、1.29、1.84、0.86、2.59、2.19、2.13、2.82和1.50倍.降雨对不同大气污染物的清除作用不同,对粗粒子的清除作用较大,而对二次产物O₃的影响较小.高ρ（PM）是造成能见度降低的主要原因,随着污染程度的加剧,PM中细粒子占比越来越高,在严重污染过程中ρ（PM_2.5）/ρ（PM₁₀）可达70.31%,比空气质量为良时高14.04%;不同污染气体的日变化不同,OC和EC的来源逐渐趋于一致,ρ（SOC）呈现出积累-爆发-积累-爆发的往复过程,边界层的日变化对污染物浓度的影响逐渐减弱.研究显示,随着霾污染的加剧,SOC气溶胶占比逐渐增加、EC和POC等一次碳气溶胶占比逐渐降低.      

SO2 oxidation in an entraining cloud model with explicit microphysics

A model of the chemical evolution of the droplets in a hill-cap cloud is presented. The chemistry of individual droplets forming on cloud condensation nuclei of differing size and chemical composition is considered, and the take-up of species from the gas phase by the droplets is treated explicity for the droplet population. Oxidation of S(IV) dissolved in cloud droplets is assumed to be dominated by hydrogen peroxide and ozone.Hydrogen peroxide is normally found to be the dominant oxidant for the oxidation of sulphur dioxide (except in the presence of substantial concentrations of ammonia gas, which increases droplet pH and the contribution made by the oxidant ozone). The entrainment of hydrogen peroxide from above the cloud top increases the amount of sulphate produced in conditions where the reaction is otherwise oxidant limited by the availability hydrogen peroxide. These conditions occur when there are high concentrations of sulphur dioxide accompanied by low cloudwater pH values.Within droplets formed on sodium chloride aerosol, reduced levels of acidity lead to an increase in sulphate production as a result of an enhanced reaction between SO₂ and the oxidant ozone. This results in an overall higher increase in cloudwater sulphate than would be expected assuming an even distribution of all reactants amongst the droplets. In addition, concentrations of the hydrogen sulphite ion predicted to occur in the cloudwater can be substantially in excess of those predicted from the bulk cloudwater pH. This is consistent with recent observations.     

Diminished effects of El Chichón on stratospheric aerosols,early 1984 to late 1986

Stratospheric aerosol collections by wire impactors, taken mainly over the western United States from early 1984 to late 1986, show the diminishing effects of El Chichón's 1982 eruption, and provide a set of data for judging subsequent volcanic effects (e.g. Pinatubo). Decrease in sulfate burden during the study time is due to preferential gravitational settling-out of large (> 0.5 μm diameter) sulfate aerosol droplets. As a result of settling from higher levels, lower altitude (12.2–15.2 km) air early in 1984 tends to contain more sulfate than higher level (19.8–21.3 km) air. As of late 1986, however, high- and low-altitude sulfate contents have decreased and are similar, suggesting large-particle settling has been completed. The later sulfate collections also have size distributions that in shape resemble unimodal background spectra, whereas earlier ones are bimodal. Average sulfate load for all altitudes decreases during the period of study from 0.4 to 0.08 μg m⁻³. The latter value is somewhat higher than a volcanically unenriched pre-El Chichón level (0.05 μg m⁻³) suggesting that even as of 1987, stratospheric background had not been obtained.     

天津城区大气气溶胶复折射指数的反演及消光贡献分析

气溶胶的复折射指数是直接影响其散射特性和吸收特性的基本物理量之一.为深入研究城市大气气溶胶的复折射指数特征,引入一种具有高时间分辨率优点的反演方法来反演气溶胶复折射指数.依据辐射传输理论,将天津大气边界层观测站观测到的高精度散射系数、吸收系数和数浓度谱分布数据利用查表法代入Mie理论气溶胶粒子群消光计算公式,对大气气溶胶复折射指数进行反演.结果表明:①天津城区2011年4月观测地点0.55 μm波长处的气溶胶复折射指数实部平均值为1.64,虚部平均值为0.015.②气溶胶复折射指数实部和虚部均有明显日变化规律,实部和虚部均与相对湿度呈正相关,与风速呈负相关.③利用反演得到的复折射指数对不同粒径大气气溶胶的消光特性进行计算发现,对散射特性而言,>0.25~1.00 μm粒子对散射系数的贡献率达86%;对吸收特性而言,>0.25~2.50 μm粒子对吸收系数的贡献率为53%,>2.50~32.00 μm粒子对吸收系数的贡献率为47%.研究显示,>0.25~1.00和>1.00~32.00 μm的粒子对吸收系数的贡献率均较高,但对散射系数而言,>0.25~1.00 μm的粒子贡献率较高,因此综合考虑气溶胶散射系数、吸收系数和消光系数,控制>0.25~1.00 μm的气溶胶粒子数浓度可有效改善大气能见度.      

南京雾过程对大气气溶胶谱分布及化学组成的影响

为探究南京地区雾过程对气溶胶粒子化学组成和尺度分布的影响,在2017年冬季的雾观测中平行收集了3级分档雾水和分粒径气溶胶样品,并对雾微物理量与气溶胶谱分布、3级分档雾水与雾前、雾中、雾后分粒径气溶胶化学组成对比分析。结果表明,2017年冬季南京第1次雾过程的雾滴液态水含量随粒径分布为不对称“V”型,最低值位于7μm处,第2次雾过程的雾滴液态水含量随粒径分布为3峰型,峰值分别位于5,15,21.5μm处。在雾形成、发展阶段,粒径<0.33μm的气溶胶质量浓度降低,粒径0.38μm气溶胶质量浓度升高,雾成熟阶段,气溶胶粒子质量浓度在全粒径段均达到最低,粒径0.38μm的气溶胶质量浓度大幅降低,与雾前相比,雾后气溶胶质量浓度峰值向大粒径方向移动。雾前,气溶胶水溶性离子组分富集在粒径<0.43μm的小粒子中,随着雾过程进行,成核作用和吸湿增长使得水溶性离子向较大粒径段富集。雾中新生成的气溶胶随着雾滴的蒸发被释放,导致雾后NO₃^-、SO₄^2-和NH₄⁺浓度升高。较小粒径的气溶胶中和率更高,雾形成初期的新生雾滴酸性较强,随着雾过程的进行逐渐中和,雾水pH值逐渐升高。     

Modes in the size distributions of atmospheric inorganic aerosol

Ambient aerosol in the size range 0.075–16 μm was sampled with Berner cascade impactors during the summer and fall intensive sampling periods of the Southern California Air Quality Study (SCAQS) of 1987. Deposits on the greased Tedlar stage substrates were extracted with deionized water and analyzed for inorganic anions and cations by ion chromatography. Stage mass data were inverted by a modified version of the Twomey nonlinear iterative algorithm and modes in the inverted size distributions were fitted with lognormal functions. Nine hundred size distributions of ionic species were obtained.Three modes, two submicron and one coarse, were sufficient to fit all of the size distributions. The smallest mode, at 0.2±0.1 μm, aerodynamic diameter, is probably a condensation mode containing gas phase reaction products. A larger mode, at 0.7±0.2 μm, is identified as a droplet mode. Evidence was obtained that the droplet mode grew out of the condensation mode by the addition of water and sulfate. During SCAQS, most of the inorganic particle mass was in the droplet mode except during a period of exceptionally low relative humidity. Nitrate was internally mixed with sulfate in the droplet mode. Since most of the aerosol fine mass is included in the ions analyzed, the observed condensation and droplet modes characterize the overall size distribution in the 0.1–1 μm range, previously described by Whitby as a single accumulation mode.