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。     

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。     

气溶胶粒子的降水清除

讨论了雨滴在云下对气溶胶粒子的清除,考虑了气溶胶粒子和雨滴之间的碰并系数,雨滴谱以及气溶胶粒子谱对清除系数的影响。在０１＜ ｒ＜ １０ μｍ 范围内,利用不同的碰并系数表达式算得的降雨对该区间内气溶胶粒子的清除系数相差很大,但对总质量清除系数影响不大;雨滴谱的改变对总质量清除系数有很大影响;不同的气溶胶粒子谱对总质量清除也有一定影响。雨滴谱用Ｍａｒｓｈａｌｌ－ Ｐａｌｍ ｅｒ 分布;气溶胶粒子谱用Ｊｕｎｇｅ 分布ｎ（ｒ）＝ ａｒｂ 算得清除系数与雨强关系为Λ＝ ０５１Ｉ０７８,而气溶胶粒子谱改用三参数分布（ｒ）＝ ａｒｂｅ－ ｃｒ得到清除系数与雨强的关系为Λ＝ ０２５Ｉ０７７。     

积云的清除作用与其酸化的数值模拟

一维时变参数化积云模式与污染物浓度连续方程相结合，根据积云内外SO2和HNO3浓度、云水S(VI)浓度、H2O2和O3的氧化速率以及地面雨水S(VI)浓度的时空变化，分别讨论核化清除、液相氧化、云下气溶胶清除、碱性气溶胶、云外污染物的夹卷以及SO2初始分布等因子的重要性。     

南京北郊冬季大气气溶胶及其湿清除特征研究

利用WPS(宽范围颗粒粒径谱仪)、雨滴潜仪和雾滴谱仪测量了2007～2008年冬季南京北郊大气气溶胶数浓度谱分布和降水强度,分析了气溶胶粒子的分布特征以及气溶胶粒径与湿清除系数的关系.结果表明:气溶胶粒子具有明显的双峰型R变化特征,数浓度主要集中在0.02～O.2μm粒径范围内,受汽车尾气排放、混合层高度变化以及颗粒物水平输送的影响较大.降雨、降雪和雾过程都对气溶胶粒子有不同程度的清除,降雨和浓雾对核模态和粗模态的气溶胶粒子的清除能力显著,降雪对粒径小于0.03μm的气溶胶粒子的清除能力较强.     

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。     

从反射太阳光谱反演大气气溶胶体积谱分布的理论研究

由大气顶射出太阳辐射的形式解出发,结合球形粒子的米散射理论,由反射太阳光谱推导获得了反演整层大气气溶胶粒子体积谱分布的权重函数。在权重函数特征分析的基础上,根据一个简单的线性反演算法,利用大气辐射传输计算模拟的大气顶反射太阳光谱,反演获得了不同气溶胶浓度和复折射率条件下的气溶胶粒子体积谱。结果表明,初步建立了一套自洽的大气气溶胶体积谱分布的反演方法。通过米散射计算获得的反演参数考虑了波长对粒子半径的权重特征,使气溶胶体积谱的反演具有了明确的物理依据;同目前常用的查算表方法相比,简化了反演方案中参数化的复杂程度。     

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.     

大气气溶胶的粒度谱分布函数及其随高度的变化

本文对用光学粒子计数器在飞机上测量的大气气溶胶数密度-粒度谱分布进行了分析研究.根据对气溶胶谱形成过程的分析,指出大气气溶胶是四种气溶胶体系的混合物,需要用四个正态分布函数的和来描述大气气溶胶的体积-粒度谱分布.用非线性最小二乘法计算了谱分布函数的经验参数;研究了粒子浓度、体积、及粒度谱分布函数随高度的变化.观测资料表明,在大气温度和湿度水平均匀、层结稳定的情况下,气溶胶粒子浓度水平分布不均匀,而且垂直方向上也并不随高度单调递减.     

南京冬季大气气溶胶的物理特征

根据１９９３年１１月１５日－１２月－１０日南京北部的大气气溶胶粒子的连续观测资料，分析了大气气溶胶粒子的浓度，日变化，日际变化，谱分布以及降水对大气气溶胶粒子的湿沉降清除。     

Temporal and spatial variations of marine aerosols over the Atlantic Ocean

Aerosol samples, collected daily were analyzed with electron microscopy for particle concentration and size distribution. The chemical compositions of individual particles were determined with X-ray energy spectrometry and specific morphological tests. The results demonstrated clear and significant dependencies of aerosol properties on air trajectories computed from a backtrack model. Air parcels, such as American air pollution and Sahara dust, were identified. Their physical mixing and chemical reactions with marine aerosols as well as aerosol wet deposition are discussed.     

Anthropogenic Aerosol Pollution over the Eastern Slope of the Tibetan Plateau

In this study, a combination of satellite observations and reanalysis datasets is used to analyze the spatiotemporal distribution, classification and source of pollutants over the eastern slope of the Tibetan Plateau(ESTP). The aerosol optical depth(AOD) over the ESTP is extremely large and even larger than some important industrialized regions and deserts. The main aerosol component over the ESTP is sulfate, followed by carbonaceous and dust aerosols. Local emissions related to human activity directly contribute to the accumulation of sulfate and carbonaceous aerosols over the Sichuan Basin. In addition, in spring, abundant carbonaceous aerosols emitted from forest, grassland and savanna fires in Southeast Asia can be transported by the prevailing southwesterly wind to southern China and the ESTP. The dust AOD over the ESTP peaks in spring because of the transport from the Taklimakan and Gobi deserts. Additionally, the high aerosol loading over the ESTP is also directly related to the meteorological background. Due to the special topography, the terrain-driven circulation can trap aerosols in the Sichuan Basin and these aerosols can climb along the ESTP due to the perennial updraft. The aerosol loading is lowest in summer because of effective wet deposition induced by the strong precipitation and better dispersion conditions due to the larger vertical temperature gradients and ascending air movement enhanced by the plateau heat pump effect. In contrast,the aerosol loading is greatest in winter. Abundant anthropogenic aerosols over the ESTP may generate some climatic and environmental risks and consequently greatly influence the downstream regions.     

华北中部夏季气溶胶和云分布特征

气溶胶与云的垂直分布特征是气溶胶间接气候效应关注的重点。基于2018年7—8月华北中部6架次飞机观测数据,研究气溶胶和云滴的垂直和水平分布特征。结果表明:华北中部780~5687 m高度内气溶胶数浓度( N_a )平均值为821.36 cm-3,最大量级可达到104 cm-3,云中气溶胶数浓度(N_acc)占总颗粒浓度的80%以上,表明细颗粒占大多数,气溶胶粒子算术平均直径( D_m )平均值为0.12~0.52 μm;大气层结对气溶胶垂直分布影响较大,逆温阻挡气溶胶垂直输送,高空(高度2000 m以上) D_m 的垂直分布受到相对湿度影响较大; N_a 和 D_m 在垂直方向波动较大,水平方向波动较小;低层云中云滴数浓度(N_c)较大、液态水含量(L)较小,而中层和高层云中N_c较小、L较大,N_c和云滴有效半径(R_e)的概率密度函数均为双峰型分布,L的概率密度函数为单峰型分布;气溶胶数浓度谱基本呈现多峰型分布,而云滴数浓度谱多呈现单峰型分布。     

On the effect of the chemical composition of atmospheric aerosol particles on nucleation scavenging and the formation of a cloud interstitial aerosol

Nucleation scavenging and the formation of a cloud interstitial aerosol (CIA) were theoretically studied in terms of the chemical composition of atmospheric aerosol particles. For this study, we used our air-parcel cloud model, which includes the entrainment of air and detailed microphysics, for determining the growth and interaction of aerosol particles and drops. Maritime and remote continental aerosol particle spectrums were used whose size distributions were superpositions of three log-normal distributions, each of a prescribed chemical composition. Our results show (1) that the CIA exhibits a size distribution with a distinctive cut-off at a specific radius of the dry as well as of the wet particle size distribution. All particles above this limiting size become activated to cloud drops and, thus, are not present in the CIA spectrum. This limiting size was found to be independent of the chemical composition of the particles and only dependent on the prevailing supersaturation. Below this specific size, the CIA spectrum becomes depleted of dry aerosol particles in a manner which does depend on their chemical composition and on the supersaturation in the air. (2) The number of aerosol particles nucleated to cloud drops depends critically on the chemical composition of the particles and on the prevailing supersaturation.     

南京地区冬季大气冰核特征及其与气溶胶关系的研究

2011年11月15日～12月2日期间对南京地区近地面大气气溶胶和冰核进行了同步观测,综合分析了 冰核浓度的特征及其与气溶胶粒子浓度的关系。结果表明:活化温度T_a为-20℃,水面过饱和度为1%时,南京地区冰核浓度N_IN为0.352 L-1,与0.01～10 μm气溶胶数浓度比值仅为4×10-8。冰核活化温度越低,湿度越大,冰核浓度越高。雾和降雨对冰核都有明显的清除作用。对比不同气团对南京地区冰核的影响发现,偏东方向的污染气团中冰核以及气溶胶的浓度最高,但是来自西北地区的气团中冰核占气溶胶的比例最高,这可能是由于冰相核化能力较强的沙尘气溶胶导致的。分析冰核与不同粒径段气溶胶的相关性发现,较大粒径气溶胶的表面积浓度与冰核相关性更高,本文也得到了由活化温度T_a和粒径大于0.5 μm气溶胶数浓度N_{0.5～10 μm}共同计算冰核浓度的经验公式。     

气溶胶辐射效应对边界层结构及夹卷特征影响的观测分析

2017年12月22日至2018年1月18日利用无人机携带温、湿和颗粒物浓度探测仪对南京地区灰霾污染条件下大气边界层垂直结构开展加密观测。通过比较不同灰霾污染条件下温度、湿度和PM_2.5（直径小于2.5微米的颗粒物）浓度的垂直结构差异,结合地面热通量、2米空气温度、相对湿度、风速、风向及主要大气污染物（如臭氧和PM_2.5）浓度,定量评估了气溶胶辐射效应对边界层和夹卷过程的影响。分析表明,灰霾或气溶胶削弱到达地表太阳辐射,减小地表感热通量,延迟边界层发展,增加近地层大气稳定度,降低边界层高度,并加重灰霾污染。灰霾污染物在混合层顶处累积,导致PM_2.5浓度最大变化出现在边界层顶部而不是近地层。气溶胶辐射效应对夹卷特征及其特征参数有重要影响。灰霾浓度升高时,夹卷区厚度增加;无量纲化夹卷速度随对流理查逊数的变化不再符合负1次方幂函数关系,与大涡模拟结果一致。本研究进一步指出,为提高重霾污染条件下天气和空气质量数值预报水平,必须考虑气溶胶辐射效应对边界层和夹卷参数化的影响。     

Effects of air masses and synoptic weather on aerosol formation in the continental boundary layer

Nucleation of near nm sized aerosol particles and subsequent growth to ∼100 nm in 1–2 days has in recent years been frequently observed in the continental boundary layer at several European locations. In 1998–99, this was the focus of the BIOFOR experiment in Hyytiälä in the boreal Finnish forest. Nucleation occurred in arctic and to some extent in polar air masses, with a preference for maritime air in transition to continental air masses, and never in sub‐tropical air. The air masses originated north of the BIOFOR experiment by paths from the southwest to northeast sector. The nucleation was also associated with cold air advection behind cold fronts, never warm air advection. This may relate to low pre‐existing aerosol concentration, low cloudiness and large diurnal amplitudes in the continental boundary layer associated with cold air advection and clear skies. Arctic and polar air together with cold air advection did not always lead to nucleation. The most important limiting meteorological factors were cold front passages and high cloudiness, probably through reduced photochemistry and wet scavenging of precursor gases and new aerosol particles. The preference for nucleation to occur in arctic air masses, which seldom form in the summer, suggests a meteorological explanation for the annual cycle of nucleation, which has a minimum in summer. The connection to cold‐air outbreaks suggests that the maximum in nucleation events during spring and autumn may be explained by the larger latitudinal temperature gradients and higher cyclone activity at that time of the year. Nucleation was observed on the same days over large parts (1000‐km distance) of the same air mass. This suggests that the aerosol nucleation spans from the microphysical scale to the synoptic scale, perhaps connected through boundary layer and mesoscale processes.