Aerosol spectra and new particle formation observed in various seasons in Nanjing

The aerosol number spectrum and gas pollutants were measured and the new particle formation （NPF） events were discussed in Nanjing. The results showed that the size distributions of aerosol number concen- trations exhibited distinct seasonal variations, implying the relations of particle sizes and their sources and sinks. The number concentrations of particles in the nuclei mode （10-30 nm）, Aitken mode （30-100 nm）, accumulation mode （100 -1000 nm） and coarse mode （〉1μm） varied in the order of summer 〉 spring 〉 autumn, summer 〉 autumn 〉 spring, autumn 〉 summer 〉 spring, and spring 〉 autumn 〉summer, re- spectively. The diurnal variation of total aerosol number concentrations showed three peaks in all observed periods, which corresponded to two rush hours and the photochemistry period at noon. In general, the NPF in summer occurred under the conditions of east winds and dominant air masses originating from marine areas with high relative humidity （50%-70%） and strong solar radiations （400 -700 W m-2）. In spring, the NPF were generally accompanied by low relative humidity （14%-30%） and strong solar radiations （400-600 W m-2）. The new particle growth rates （GR） were higher in the summertime in the range of 10- 16 nm h-1. In spring, the GR were 6.8-8.3 nm h-1. Under polluted air conditions, NPF events were seldom captured in autumn in Nanjing. During NPF periods, positive correlations between 10- 30 nm particles and 03 were detected, particularly in spring, indicating that NPF can be attributed to photochemical reactions.     

Relevance of ion-induced nucleation of sulfuric acid and water in the lower troposphere over the boreal forest at northern latitudes

The relevance of ion-induced nucleation of sulfuric acid and water (IINSW) in the troposphere over the boreal forest at northern latitudes is investigated by combining two existing and previously published models (MALTE — model to predict new aerosol formation in the lower troposphere; PARNUC — a parameterized steady-state model of neutral and ion-induced nucleation of sulfuric acid and water for atmospheric conditions). Simulations were performed for 4 days with observed new particle formation at ground level by using input data from the SMEAR II station in Hyytiälä, Finland. The selected days were chosen to cover a wide range of values of the parameters most relevant for IINSW. The results showed that ion-induced nucleation of sulfuric acid and water can contribute up to 15% to the total amount of newly formed particles in the size range of 3–10 nm inside the mixed layer at the Hyytiälä site. The importance of IINSW seemed to increase in the free troposphere above the boundary layer, however, lack of measurements in the vertical structure of the input parameters suggest that the model results are burdened with high uncertainties.     

MEASUREMENTS OF PARTICLE NUMBER SIZE DISTRIBUTIONS AND NEW PARTICLE FORMATION EVENTS DURING WINTER IN THE PEARL RIVER DELTA REGION, CHINA

Particle number size distribution(PNSD) between 10 nm and 20 μm were measured in the Pearl River Delta(PRD) region in winter 2011.The average particle number concentration of the nucleation mode(10-20 nm),Aitken mode(20-100 nm),accumulation mode(100 nm-1μm) and coarse mode(1-20 μm) particles were 1 552,7 470,4 012,and 19 cm-3,respectively.The volume concentration of accumulation mode particles with peak at 300 nm accounted for over 70% of the total volume concentration.Diurnal variations and dependencies on meteorological parameters of PNSD were investigated.The diurnal variation of nucleation mode particles was mainly influenced by new particle formation events,while the diurnal variation of Aitken mode particles correlated to the traffic emission and the growth process of nucleation mode particles.When the PRD region was controlled by a cold high pressure,conditions of low relative humidity,high wind speed and strong radiation are favorable for the occurrence of new particle formation(NPF) events.The frequency of occurrence of NPF events was 21.3% during the whole measurement period.Parameters describing NPF events,including growth rate(GR) and source rate of condensable vapor(Q),were slightly larger than those in previous literature.This suggests that intense photochemical and biological activities may be the source of condensable vapor for particle growth,even during winter in the PRD.     

Atmospheric variability and binary homogeneous nucleation: A parametrisation and conditions required for a significant effect

The binary water–sulphuric acid nucleation has long been considered an important path for new particle formation in the atmosphere. The formation rate depends nonlinearly on temperature and vapour concentrations. We aim to find out if atmospheric small scale and mesoscale spatial and temporal variability can increase the nucleation rate significantly. Simultaneous and separate effects of variation in temperature, humidity and sulphuric acid concentration on the mean nucleation rate have been modelled. We have assumed that the distributions of variables are Gaussian and compare the mean of simulated nucleation rates with the nucleation rate in mean conditions without variation. According to our studies the atmospheric variability can increase the mean nucleation rate by orders of magnitude but the significant effect is limited to specific conditions. The effect seems to be more important in the lower troposphere than in the upper troposphere, where temperature and sulphuric acid concentrations are lower. In addition, our model simulations indicate that the atmospheric variability can only explain part of the difference between measured and theoretically required sulphuric acid concentrations in conditions where particle formation has been observed. We have parametrised the effect of atmospheric variability as a simple correction factor for the effect of temperature and humidity variation.     

Humidity fluctuations in the marine boundary layer measured at a coastal site with an infrared humidity sensor

An extensive set of humidity turbulence data has been analyzed from 22-m height in the marine boundary layer. Fluctuations of humidity were measured by an OPHIR, an infrared humidity sensor with a 10 Hz scanning frequency and humidity spectra were produced. The shapes of the normalized spectra follow the established similarity functions. However the 10-min time averaged measurements underestimate the value of the absolute humidity. The importance of the humidity flux contribution in a marine environment in calculating the Obukhov stability length has been studied. Deviations from Monin-Obukhov similarity theory seem to be connected to a low correlation between humidity and temperature.     

Size-Resolved Aerosol Characterization for a Polluted Episode at the IfT Research Station Melpitz in Autumn 1997

Inorganic ions, organic carbon (OC), elemental carbon (EC) and a variety of organic single species in airborne particles have been determined at the research station of the Leibniz – Institut für Troposphärenforschung (IfT) in Melpitz (Germany) in autumn 1997.Samples of eight selected measurement events were divided in two groups in order to investigate differences in the chemical composition of particles originating from southwesterly (SW – developed EU countries) or from easterly directions (E – less developed eastern countries). Differences between these two groups were tested statistically by Student's t-test.Five stage cascade impactor samples show nitrate as most abundant in the accumulation mode in the SW group. EC and sulphate show the most abundant mass fractions in the E group. That can be considered as a consequence of domestic coal heating and coal-fired power plant emissions in the region of westerly Poland, northern Czech Republic and easterly Germany. Higher nitrate concentrations in the SW group can be explained by stronger NO _x emissions caused by the leeward plume of the conurbation of Leipzig, as well as by the still higher traffic density in western Germany.The methane sulphonic acid (MSA) mass fraction was higher for SW air masses in accumulation mode particles, probably indicating marine origin. Succinic acid also showed higher mass fractions for the SW group. This could be caused by primary emission in automobile exhaust gases and photochemical formation during transport from SW. Indeed, during SW sampling, solar radiation intensity was higher than during E sampling.The observed differences in the particle composition are an expression of the still existing technology gradient in Europe. Future campaigns could show the development to a joint economy with smaller differences in anthropogenic emissions.     

湛江地区一次冷锋型海雾微物理特征

利用2010年3月31日—4月2日冷锋天气系统影响下湛江海雾综合观测资料,分析了海雾的微物理特征及海雾过程中气溶胶粒子谱的演变特征。结果表明,海雾的生消与风场密切相关,海雾生成和发展与较强的ESE气流相联系,而弱的NE气流则会促使海雾减弱或消散。湛江海雾的雾滴数浓度为100~102cm-3,液态含水量为0.001~0.232 g·m-3,雾滴平均半径小于10μm,雾滴峰值半径多位于1.4μm。海雾雾滴谱分布以单调递减谱为主,谱宽超过20μm,且雾发展过程中雾滴谱谱宽存在突然增宽和迅速减小的现象。海雾过程中雾滴数浓度的变化主要是由半径小于5μm的雾滴数密度变化引起的。海雾过程对气溶胶粒子的湿清除效果并不显著,雾过程中粒径小于0.1μm和大于4μm的气溶胶粒子数密度显著减少,但在雾消散后又迅速恢复到雾发生前的水平。     

华东高海拔地区夏季气溶胶数浓度及谱分布特征

利用2014年7月黄山光明顶观测获得的气溶胶数浓度、气溶胶数谱数据,对黄山夏季气溶胶数浓度及谱分布特征进行分析,并在此基础上对气溶胶数谱进行了对数正态分布拟合。研究结果表明:黄山夏季气溶胶平均数浓度约为3 518.27 cm~(-3),主要集中在爱根核模态;气溶胶平均数浓度日变化呈双峰分布,峰值浓度的出现伴随着小粒子的增多。气溶胶数浓度与相对湿度和风速成负相关,高浓度的气溶胶多出现在较弱的东南风时;积聚模态气溶胶数浓度受风向影响显著。不同气团背景下气溶胶数谱差异集中在小于100 nm和500~1 000 nm粒径范围。爱根核模态气溶胶在高湿的西南气团影响下数浓度最低、谱较窄,而高温、低湿的东南气团对应的气溶胶数浓度最高、谱最宽,北方气团对应的气溶胶数浓度和谱宽居中;500~1 000 nm粒径范围气溶胶数谱分布特征与之相反。不同背景的气溶胶数谱和体积谱均可采用爱根模态、积聚模态1和积聚模态2三个模态进行对数正态分布拟合,但不同气团背景下的各模态谱型参数差异较大。     

Charging state of atmospheric nanoparticles during the nucleation burst events

In this work, the charging state of atmospheric nanoparticles was estimated through simultaneous measurements of aerosol size distribution and air ions mobility distribution with the aim to elucidate the formation mechanisms of atmospheric aerosols. The measurements were performed as a part of the QUEST 2 campaign at a boreal forest station in Finland. The overlapping part of the measurement ranges of the particle size spectrometers and air ion mobility spectrometers in the mass diameter interval of 2.6–40 nm was used to assess the percentage of charged particles (charging probability). This parameter was obtained as the slope of the linear regression line on the scatterplot of the measured concentrations of total (neutral + charged) and charged particles for the same diameter interval. Charging probabilities as a function of particle diameter were calculated for different days and were compared with the steady state charging probabilities of the particles in the bipolar ion atmosphere. For the smallest particles detectable by the particle size spectrometers (2.6–5 nm), the high percentages of negatively charged particles were found during the nanometer particle concentration bursts. These values considerably exceeded the values for the steady charging state and it was concluded that negative cluster ions preferably act as condensation nuclei. This effect was found to be the highest in the case of comparatively weak nucleation bursts of nanoparticles, when the rate of the homogeneous nucleation and the concentration of freshly nucleated particles were low. The nucleation burst days were classified according to the concentration of the generated smallest detectable new particles (weak and strong bursts). Approximately the same classification was obtained based on the charge asymmetry on particles with respect to the charge sign (polarity). The probabilities of negative and positive charge on the particles with the diameter of 5–20 nm were found to be nearly equal and they approximately agree with the values corresponding to the steady state charge distribution for negative particles known from lab experiments. It means that the steady charging state was reached during the growing time of particles up to 5 nm. The natural charging state of particles with a diameter between 2.5 and 4.5 nm was estimated by means of a special DMPS setup. Results were found to be in good correlation with the data by the particle size spectrometers and air ion mobility spectrometers.     

Transformation of Aerosol Chemical Properties due to Transport Over a City

The change of the chemical composition of the near-ground level atmospheric aerosol was studied during two summer episodes by a Lagrangian type of experimental approach. Bulk and single-particle chemical analyses of ions and elements in the particulate phase were deployed. N(-III) and N(V) components were also measured in the gas-phase. The measurements were completed by particle size distributions.Secondary inorganic aerosols (SIA) and fine particles of ≈0.2–0.4 μm size were still elevated 50 km downwind of the city. The direct comparison of transport over the city in contrast to transport over the surrounding areas showed that SIA was formed from emission from the city within less than 3 h. Relative increases, i.e., enrichment during transport were observed for primary and secondary aerosol components. The degree of mixing on the individual particle level increased significantly during transport in the area. In particular, newly emitted carbonaceous particles became internally mixed within hours with pre-existing sulphate particles. Mostly due to secondary aerosol formation the average particle size (mass median diameter) of major constituents of the aerosol was significantly decreased while being transported over 13 h. Given recent insights which link fine particles number and mass concentrations with health risks, the results suggest that rural populations in areas which frequently are located within an urban plume might run an elevated health risk relative to populations in areas not affected by urban plumes.     

Growth Rates of Fine Aerosol Particles at a Site near Beijing in June 2013

Growth of fine aerosol particles is investigated during the Aerosol–CCN–Cloud Closure Experiment campaign in June2013 at an urban site near Beijing. Analyses show a high frequency(~ 50%) of fine aerosol particle growth events, and show that the growth rates range from 2.1 to 6.5 nm h~(-1) with a mean value of ~ 5.1 nm h~(-1). A review of previous studies indicates that at least four mechanisms can affect the growth of fine aerosol particles: vapor condensation, intramodal coagulation,extramodal coagulation, and multi-phase chemical reaction. At the initial stage of fine aerosol particle growth, condensational growth usually plays a major role and coagulation efficiency generally increases with particle sizes. An overview of previous studies shows higher growth rates over megacity, urban and boreal forest regions than over rural and oceanic regions. This is most likely due to the higher condensational vapor, which can cause strong condensational growth of fine aerosol particles.Associated with these multiple factors of influence, there are large uncertainties for the aerosol particle growth rates, even at the same location.     

一次霾天气条件下石家庄上空大气气溶胶数浓度的飞行探测与特征分析

利用2010年8月30日河北省石家庄一次霾天气条件下的气溶胶飞行探测资料,分析了石家庄地区上空658—6933 m高度范围内大气气溶胶粒子平均数浓度、平均直径的垂直分布特征和9个水平飞行高度上的谱分布特征。结果表明:轻度霾天气条件下的气溶胶平均数浓度为325个/cm3,平均直径为0.169μm。在约1000 m高度以下,气溶胶平均数浓度随高度的增加呈线性减少趋势。粒径也随高度增加而减小,由0.187μm减小至0.164μm。1000 m高度以上,气溶胶平均数浓度随高度减少趋势变缓,粒子平均直径在0.167~0.171μm范围内波动。9个不同高度上的谱分布都呈单峰型,随着高度增加,谱宽变小,峰值向小尺度方向移动。后向轨迹计算分析表明:污染气团的远距离输送可能是导致大气1500 m高度层气溶胶数浓度突增的原因。     

Chemical characterization of cloud episodes at a ridge site in Tuscan Appennines, Italy

Cloudwater samples were collected from November 1992 to March 1995 in Vallombrosa, a mountain site of the Tuscan Apennines (central Italy). Chemical analyses show that all examined inorganic ions contributed significantly to the total ionic content (TIC). The ratio SO₄²⁻/NO₄⁻ ranged from 0.92 to 3.46 and was >1 for 86% of samples. There is a wide range in the chemical composition of the cloudwater. The total ionic content ranged from 640 to 7476 μeq l⁻¹ and pH from 3.17 to 6.22. The liquid water content (LWC) ranged from 0.06 to 0.94 g m⁻³ and electrical conductivity from 47 to 485 μΩ⁻¹. The total ionic content decreases while the liquid water content increases. Also analyzed were soluble trace metals (Fe, Pb, Cu, Mn, Cd, Al), synthetic anionic surfactants and the methanesulphonic acid. Chemical analyses evidenced in some cases a high concentration of organic matter. The meteorological analysis for a few samples of individual passages was carried out for the possibility of establishing a correspondence between meteorological events and chemical composition. The sources (marine, crustal and anthropogenic) of chemical components were deduced.     

Atmospheric concentrations of nonmethane hydrocarbons at a North European coastal site

Two years of individual nonmethane hydrocarbon (NMHC) measurements at a rural site close to the south coast of Norway show that there was a distinct annual cycle with a late winter maximum and late summer minimum in the slowly reacting NMHCs acetylene, ethane, propane and i- and n-butane. The average January—March concentrations were a factor 2–4 higher than the July-September concentrations. Also ethene, propene and the pentanes show a similar annual cycle, but the individual scatter in the measurements in particular of propene, is large. The highest concentrations of NMHC were found in winter for easterly transport on a regional scale (out to 1500 km from the site), and for southeasterly transport in the summer.     

中国超大城市综合实验:京、沪、穗气溶胶理化和吸湿特性

气溶胶对环境、气象和人体健康都有较大影响,这些影响与气溶胶理化特性(粒子尺度谱、化学组分、混合状态等)密切相关。为了深入研究气溶胶的环境和气候效应,发展了一套气溶胶在线综合观测系统。本文介绍了利用该系统在北京、上海、广州三个超大城市开展的综合观测实验结果。通过对比分析发现,广州气溶胶数浓度最高,其粒子尺度谱分布特征与北京特征相似,均以核模态为主,上海气溶胶数浓度则整体较低。对比三个超大城市的新粒子生成(New Particle Formation,NPF)特征发现,北京NPF的发生频率低于广州,主要由于北京地区大气中大粒径气溶胶更多,较高的碰并汇抑制了NPF的发生和发展。研究发现,观测期间北京和上海站点气溶胶的吸湿性强于广州,人为一次性排放气溶胶吸湿性较弱。气溶胶吸湿性日变化特征与人为活动、气溶胶老化程度密切相关。此外,三个超大城市中气溶胶光吸收系数的日变化特征存在明显差别,北京站点的气溶胶吸收系数呈现白天高、夜间低的特点,而广州站点气溶胶的吸收系数呈现相反的日变化趋势,这可能是由观测站周边的环境差异及大气边界层的变化特征差异造成的。     

Elemental and Single Particle Aerosol Characterisation at a Background Station in Kazakhstan

Aerosol sampling in Kazakhstan was performed at a remote astronomical observatory in the Tien Shan mountain region. The background character of the site was considered by comparing the elemental concentrations, obtained by Energy Dispersive X-Ray Fluorescence (EDXRF), with those reported for other remote stations. On the basis of the variability of the elemental concentrations and the source of origin, the elements could be classified into two main groups. These findings, complemented with enrichment factor calculations revealed the first group of elements to be originating mainly from local sources, and the second group to be related to long-range transport of anthropogenic aerosol. Automated individual particle analysis by electron probe X-ray microanalysis (EPXMA) and subsequent cluster analysis resulted in the identification of 12 distinct aerosol particle types. Relative particle type abundances were converted to absolute abundances by estimating the particle number concentrations for the detected particles, exploring the seasonal particle variation. Based on the absolute abundances, a strong seasonal pattern was found for Si-Al-Fe-, Si-, Ca-S-Si-, Ca-Si-, Fe-Si- and Ti-Si-rich particles. These particle types can mainly be attributed to the local soil source. For most of the remaining particle types, a completely different seasonal trend was found, which can be related to anthropogenic emissions. Their abundance in winter can be related to long-range transport of anthropogenic aerosols. As a result, these data can be representative for the Tien Shan site and may be useful to climate modellers and environmentalists.     

New aerosol particle formation via certain ion driven processes

Ions can speed up the formation of aerosol particles. The former studies have mainly concerned on the role of the ion charge itself. We have studied the possible (additional) role of the actual small air ion spectrum shape, and the quantitative role of ion–ion recombination pathway. By means of our ion evolution model, formation of new species (H₂SO₄)_n(NH₃)_m(HNO₃)_k via ion–ion recombination was investigated. The model shows how the generation rate of the new species depends on the concentrations of H₂SO₄ and NH₃, and how it depends on the tropospheric background aerosol situation. The rate can be up to a few new neutral complexes per cubic centimeter and per second. New particle generation via ion–ion recombination provides an extra channel, especially for the clean atmosphere. Former results have shown that such situations are often present in Antarctica. Our aerosol spectrum measurements reveal a number of similar non-Antarctic results. Sometimes, such situations are followed by aerosol bursts, which may be (partly) due to an ion–ion recombination channel.     

GPM卫星DPR和GMI探测的2018年5月重庆超级单体云团降水结构特征分析

目前人们对超级单体云团降水回波结构的认知仍有限。本文采用GPM (Global Precipitation Measurement)卫星搭载的测雨雷达DPR (Dual-frequency Precipitation Radar)和微波成像仪GMI (GPM Microwave Imager)的探测结果,结合FY-4A静止卫星多通道扫描成像辐射计(AGRI)的热红外10.8μm通道观测结果、探空站的温湿风观测结果及欧洲天气预报中心再分析数据,利用雷达回波剖面和回波反射率因子概率密度随高度分布的方法,分析了2018年5月重庆地区超级单体云团的降水结构特征。结果表明:该超级单体云团由西北向东南运动的冷空气与暖湿空气交汇而引发;超级单体云团内存在对流降水和层状降水等次尺度系统;强降水区位于云贵高原与四川盆地交界处至盆地的西南部;超级单体暴雨云中冰相粒子多;对流降水的回波顶高度超过12 km,且最大回波强度多数位于地面上空4—5 km;对流降水比层状降水拥有更高的降水粒子浓度,而粒子大小却小于后者;对流降水的粒子尺度随着高度下降而明显增大,反映了其明显碰并增长过程。     

北京乡村地区分粒径气溶胶OC及EC分析

利用北京上甸子区域大气本底站2004年观测的分粒径大气气溶胶资料,分析了气溶胶中有机碳 (OC) 及元素碳 (EC) 的质量浓度水平、季节变化、尺度分布特征、OC与EC比值及其相关性。结果显示:上甸子站总悬浮颗粒物 (TSP) 中OC平均质量浓度为7.5~31.5 μg·m-3,EC质量浓度为1.4~6.6 μg·m-3;PM_2.1(粒径小于2.1 μm) 中OC质量浓度为4.0~19.1 μg·m-3,EC质量浓度大约为0.8~4.3 μg·m-3。冬季OC及EC质量浓度明显高于其他季节,其中冬、夏、秋季OC及EC峰值粒径出现为0.65~2.1 μm,但在春季峰值粒径移至2.1~4.7 μm。观测期间,OC与EC质量浓度比值平均为4~6,该比值略高于文献报道的我国一些城市地区的观测结果。     

Analysis and numerical simulation of the meteorological observations at a tropical coastal site Chennai in India

Meteorological measurements were carried out at North Chennai semi rural area during pre-monsoon period as a part of an air quality study program. Analysis of the data showed the effects of coastal terrain namely the land-sea breeze circulation, temperature cooling during the sea breeze, difference in onset times at these sites etc. Sea breeze onset was observed with a sharp turning of the wind from westerly to south easterly associated with rise in wind speed. Advection speed of the front was about 2.0 m s^− 1. A simple mesoscale meteorological model (MAM-I) developed at Kalpakkam for coastal atmospheric dispersion estimation was used to simulate the observed characteristics. All the major features observed could be simulated by the model while significant difference was noticed in sea breeze frontal movement. MAM results were also inter-compared with MM5. There were no significant differences in the estimate of mean parameters by both the models. It is concluded that the simple model, which takes less run time in a desktop PC, is adequate enough for practical application of providing wind field for plume dispersion models at coastal sites.