Highlights of fifty years of atmospheric aerosol research at Mace Head

This paper summarises the development and principal results of fifty years of research on aerosols in the marine atmosphere at Mace Head Atmospheric Research Station on the west coast of Ireland. It concentrates on the sources, physico-chemical properties, number and mass concentrations, size range, volatility and chemical composition of aerosols in different air masses. It also examines optical properties of the aerosols and their long-range transport.     

Highlights of fifty years of atmospheric aerosol research at Mace Head

This paper summarises the development and principal results of fifty years of research on aerosols in the marine atmosphere at Mace Head Atmospheric Research Station on the west coast of Ireland. It concentrates on the sources, physico-chemical properties, number and mass concentrations, size range, volatility and chemical composition of aerosols in different air masses. It also examines optical properties of the aerosols and their long-range transport.     

Continental origin and industrial sources of trace metals in the Northwest Atlantic troposphere

Trace metals (Mn, Fe, Ni, Cu, Zn, Cd, Pb and stable lead isotopes) have been analyzed in precipitation and total aerosols collected in the northwest Atlantic troposphere in April and November 1989. According to stable lead isotope signatures we encountered two main air mass sources, Mediterranean easterlies (206Pb/207Pb=1.131) and US westerlies (206Pb/207Pb=1.195–1.205). The phasing out of leaded gasoline has been invoked to explain the decrease of the 206Pb/207Pb ratios from 1.22 to 1.20 for the past 10 years in North America. Based on trajectory analyses, intermediate 206Pb/207Pb ratios are explained by a mixing of pure US westerlies with Canadian air masses (206Pb/207Pb=1.190–1.195) or Mediterranean air masses (206Pb/207Pb=1.18–1.19). Isentropic trajectories are very useful in explaining the variability of trace metal concentrations, a result of the fluctuating transport range of anthropogenic aerosols to remote marine areas of the North Atlantic. Lead concentrations appear to be closely correlated to the air mass transport patterns as defined from the meteorological analyses. For instance oceanic air masses transported over remote marine areas for more than three days were characterized by lead concentrations 2 to 10 times lower (Pb=0.5 to 2 ng/scm) than coastal air masses (Pb=3 to 10 ng/scm).Anthropogenic trace metal concentrations are generally in good agreement with the air mass signatures which display Pb and Cu, Ni, Zn concentrations higher than 2 and 10 ng/scm respectively in aerosol samples for the US source. Trace metal elemental ratios and soil enrichment factors were used to define industrial sources. Aerosol originating from the US exhibits the distinct industrial signature of Cu/Ni production and coal-oil combustion, while steel metallurgy could account for more than 50% of the overall Mn input into the Northwest Atlantic ocean.     

Occurrence of water soluble organic nitrogen in aerosols at a coastal area

Aerosol samples (205) were collected from January 2005 to November 2006 at a coastal site at Keelung City (Taiwan), on the southern East China Sea. The atmospheric concentrations of major ions indicated that the area was dominated by different air masses at different times of the year: continental Asia from January to May and November to December; air masses from Indonesia and surrounding islands (south-eastern region) dominated during early-summer (July 2005 and June 2006), and air masses directly from the adjacent ocean dominated during late-summer (July to August 2006) and early-autumn (September to October 2005). The atmospheric concentrations of water soluble organic nitrogen (WSON) corresponded to the different sources and weather conditions. The results of a factor analysis of combined major ions, water soluble inorganic nitrogen (WSIN) and WSON indicated that a fossil fuel combustion source and biomass burning were the two major controlling factors during the sampling period. We discuss the correlations between WSON, WSIN and major anthropogenic ions in relation to the different formation mechanisms for the various sources. We propose a mechanism whereby biomass burning is the major input of aerosols derived from mainland China. Fossil fuel combustion was found to be important during periods when aerosols were derived from the south-eastern area. Our data indicate that WSON was predominantly associated with aerosols derived from biomass burning when the origin of the air mass was mainland China.     

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。     

Optical Properties and Source Analysis of Aerosols over a Desert Area in Dunhuang,Northwest China

Aerosol observational data for 2012 obtained from Dunhuang Station of CARE-China(Campaign on Atmospheric Aerosol Research Network of China) were analyzed to achieve in-depth knowledge of aerosol optical properties over Dunhuang region. The results showed that the annual average aerosol optical depth(AOD) at 500 nm was 0.32 ± 0.06, and the ?ngstr?m exponent(α) was 0.73 ± 0.27. Aerosol optical properties revealed significant seasonal characteristics. Frequent sandstorms in MAM(March–April–May) resulted in the seasonal maximum AOD, 0.41 ± 0.04, and a relatively smaller αvalue, 0.44 ± 0.04. The tourism seasons, JJA(June–July–August) and SON(September–October–November) coincide with serious emissions of small anthropogenic aerosols. While in DJF(December–January–February), the composition of the atmosphere was a mixture of dust particles and polluted aerosols released by domestic heating; the average AOD and αwere 0.29 ± 0.02 and 0.66 ± 0.17, respectively. Different air masses exhibited different degrees of influence on the aerosol concentration over Dunhuang in different seasons. During MAM, ranges of AOD(0.11–1.18) and α(0.06–0.82) were the largest under the dust influence of northwest-short-distance air mass in the four trajectories. Urban aerosols transported by northwest-short-distance air mass accounted for a very large proportion in JJA and the mixed aerosols observed in SON were mainly conveyed by air masses from the west. In DJF, the similar ranges of AOD and α under the three air mass demonstrated the analogous diffusion effects on regional pollutants over Dunhuang.     

Geochemistry of regional background aerosols in the Western Mediterranean

The chemical composition of regional background aerosols, and the time variability and sources in the Western Mediterranean are interpreted in this study. To this end 2002–2007 PM speciation data from an European Supersite for Atmospheric Aerosol Research (Montseny, MSY, located 40 km NNE of Barcelona in NE Spain) were evaluated, with these data being considered representative of regional background aerosols in the Western Mediterranean Basin. The mean PM₁₀, PM_2.5 and PM₁ levels at MSY during 2002–2007 were 16, 14 and 11 µg/m³, respectively. After compiling data on regional background PM speciation from Europe to compare our data, it is evidenced that the Western Mediterranean aerosol is characterised by higher concentrations of crustal material but lower levels of OM + EC and ammonium nitrate than at central European sites. Relatively high PM_2.5 concentrations due to the transport of anthropogenic aerosols (mostly carbonaceous and sulphate) from populated coastal areas were recorded, especially during winter anticyclonic episodes and summer midday PM highs (the latter associated with the transport of the breeze and the expansion of the mixing layer). Source apportionment analyses indicated that the major contributors to PM_2.5 and PM₁₀ were secondary sulphate, secondary nitrate and crustal material, whereas the higher load of the anthropogenic component in PM_2.5 reflects the influence of regional (traffic and industrial) emissions. Levels of mineral, sulphate, sea spray and carbonaceous aerosols were higher in summer, whereas nitrate levels and Cl/Na were higher in winter. A considerably high OC/EC ratio (14 in summer, 10 in winter) was detected, which could be due to a combination of high biogenic emissions of secondary organic aerosol, SOA precursors, ozone levels and insolation, and intensive recirculation of aged air masses. Compared with more locally derived crustal geological dusts, African dust intrusions introduce relatively quartz-poor but clay mineral-rich silicate PM, with more kaolinitic clays from central North Africa in summer, and more smectitic clays from NW Africa in spring.     

Concentrations of metallic elements in long-range-transported aerosols measured simultaneously at three coastal sites in China and Japan

To determine the effects of long-range transport of aerosols from an upwind area in East Asia to a downwind area in Japan, we chemically analyzed aerosols collected simultaneously on Tuoji Island (Shandong Province, China), Fukue Island (Nagasaki Prefecture, Japan), and Cape Hedo (Okinawa Prefecture, Japan). We focused on changes in the metallic composition of PM_2.5 aerosols during long-range transport. The average mass concentrations of PM_2.5 at the three sites decreased in the order Tuoji Island > Fukue Island ≈ Cape Hedo (48.3 ± 4.5, 13.9 ± 1.5, and 13.2 ± 0.9 μg/m³, respectively). The fraction of coarse particles in total suspended particles estimated by (1–PM_2.5/TSP) was highest on Cape Hedo, indicating that the contribution of sea salts was increased by long-range transport of the aerosols over the ocean. Enrichment factor analysis revealed that at all three sites, Al, K, Ca, Mn, Fe, Co, Sr, and Ba originated from soil; whereas Cr, Ni, Cu, Zn, As, Mo, Ag, Cd, Sn, Sb, Tl, and P appeared to be of anthropogenic origin. Na was the most abundant element on Cape Hedo, indicating the addition of sea salts during aerosol transport. The V concentration was highest at Fukue Island, which was ascribed to V emission from ships. Sixty-one percent of the V on Fukue Island and 62% of the V on Cape Hedo were determined to have originated from ships, implicating of data obtained on dates during which backward trajectory analysis indicated that the same air mass passed over Tuoji Island, Fukue Island, and Cape Hedo in that order.     

宁波地区空气质量及大气自净能力海陆差异对比

以镇海、奉化分别作为宁波沿海和内陆空气质量代表站。基于代表站2013-2017年污染物资料和2015年12月至2017年2月冬季激光雷达资料,对比分析宁波地区沿海和内陆站点的空气质量差异;利用NCEP的GDAS(Global Data Assimilation System)资料和ERA-Interim高分辨率再分析资料评估两地气溶胶来源及大气自净能力差异。结果表明:宁波沿海和内陆地区中度及以上污染主要集中于冬季,冬季首要污染物以PM2.5为主;镇海NO2浓度较奉化显著偏高,而两地PM2.5 和PM10 浓度差异较小。冬季镇海和奉化3km以下都存在消光系数大的气溶胶集中层,镇海3km内消光系数平均值较奉化偏高约40%。两地中度及以上污染时,镇海和奉化的气溶胶粒子主要来自宁波西北方向的内陆地区,比例分别为90%和63%,镇海地区其余10%左右来自近距离低空偏东气流的输送,而奉化地区有37%来自浙江西南部的短距离输送。冬季当宁波地区出现区域性优和中度以上污染时,浙江北部沿海分别盛行东北风和西北风,空气质量优时混合层内平均风速大于中度以上污染时。浙江省大气自净能力比值呈自西北向东南减小,宁波地区优等空气质量大气自净能力约为中度以上污染的 1.5倍。大气自净能力在不同空气质量等级下差异显著,可作为大气污染发生、发展和消退判定的参考依据。     

泰山PM10及其中化学成分变化特征

为研究华北平原区域背景气溶胶成分及其变化特征,2010年6月至2011年7月在泰山顶采集了64个PM10滤膜样品,分析了样品的PM10及其中无机盐离子和有机碳（OC）、元素碳（EC）的质量浓度,并对各成分相关性等进行了分析。泰山PM10年均质量浓度约为68.4 mg/m³,其中无机盐离子约占总质量的64.8%,碳气溶胶约占17.4%。无机盐离子的质量浓度从春季逐渐增大,夏季达到峰值,秋季下降,冬季最小;OC质量浓度从春季至秋季逐渐增高,冬季最低,EC变化类似,但夏秋两季差别不大。二次有机碳（SOC）与OC的比值四季均在50%以上,年均值约为58.5%。通过后向轨迹聚类分析发现,在经过城市的较短轨迹以及南方较短混合轨迹的影响下,泰山PM10质量浓度较高,而西北长距离传输气团PM10浓度均较低。     

An experimental investigation of Arctic haze at Alert,N.W.T., March 1985

Abstract

Arctic haze has been attributed to industrial pollution released at mid‐latitudes. Our current understanding has been pieced together from routine meteorological data, ground‐based air chemistry observations and limited aircraft measurements. This study investigates the relationship between synoptic boundary‐layer meteorology and the composition of the near‐surface atmosphere during the polar sunrise at Alert, N.W.T. A secondary objective is to characterize the influence of local activity on the atmospheric composition at a site for a new baseline monitoring station and at a location where aerosol chemistry and grab‐flask samples for CO₂ have been made for many years. Detailed measurements of the vertical distribution of aerosols were obtained from an upward‐looking lidar to complement the ground‐based measurements. Meteorological profiles of the near‐surface boundary layer were obtained from both free‐flying and tethered balloons. Near‐surface measurements were made of aerosol physical and chemical properties, O₃, NO₂, NO/NO_x, Peroxyacetylnitrate (PAN) and hydrocarbons.

The study period was characterized by prolonged periods with strong surface inversions, which were broken up occasionally by intrusions of cold air into the warmer air aloft. Lidar observations showed that ice crystals often accompanied aerosols and were responsible for reducing visibility below 30–40 km. There was a strong correlation between aerosol mass in the diameter size range 0.15 to 1.5 μm and total SO₄ ⁼ . PAN found at concentrations of about 200 ppt(v) was the main carrier of atmospheric nitrogen. Aerosol trace elements were divisible into anthropogenic soil, mixed soil/anthropogenic sea salt and halogens. Vertical transport in the surface boundary layer, as regulated by the strength of the surface radiation inversion, may play an important role in influencing the chemical composition of the air at the ground. The location of the new baseline monitoring laboratory was found to be generally windier and warmer than the lower altitude weather station, and the influence of local activity was found to be minimal.     

Simulation of the radiative effect of black carbon aerosols and the regional climate responses over China

As part of the development work of the Chinese new regional climate model (RIEMS), the radiative process of black carbon (BC) aerosols has been introduced into the original radiative procedures of RIEMS,and the transport model of BC aerosols has also been established and combined with the RIEMS model.Using the new model system, the distribution of black carbon aerosols and their radiative effect over the China region are investigated. The influences of BC aerosole on the atmospheric radiative transfer and on the air temperature, land surface temperature, and total rainfall are analyzed. It is found that BC aerosols induce a positive radiative forcing at the top of the atmosphere (TOA), which is dominated by shortwave radiative forcing. The maximum radiative forcing occurs in North China in July and in South China in April. At the same time, negative radiative forcing is observed on the surface. Based on the radiative forcing comparison between clear sky and cloudy sky, it is found that cloud can enforce the TOA positive radiative forcing and decrease the negative surface radiative forcing. The responses of the climate system in July to the radiative forcing due to BC aerosols are the decrease in the air temperature in the middle and lower reaches of the Changjiang River and Huaihe area and most areas of South China, and the weak increase or decrease in air temperature over North China. The total rainfall in the middle and lower reaches of the Changjiang River area is increased, but it decreased in North China in July.     

Episode Simulation of Asian Dust Storms with an Air Quality Modeling System

A dust deflation module was developed and coupled with the air quality modeling system RAMS-CMAQ to simultaneously treat all the major tropospheric aerosols（i.e.,organic and black carbons,sulfate,nitrate, ammonia,soil dust,and sea salt）.Then the coupled system was applied to East Asia to simulate Asian dust aerosol generation,transport and dry/wet removal processes during 14-25 March 2002 when two strong dust storms occurred consecutively.To evaluate model performance and to analyze the observed features of dust aerosols over the East Asian region,model results were compared to concentrations of suspended particulate matter of 10μm or less(PM₁₀;1-h intervals) at four remote Japanese stations and daily air pollution index （API） values for PM₁₀ at four large Chinese cities.The modeled values were generally in good agreement with observed data,and the model reasonably reproduced two dust storm outbreaks and generally predicted the dust onset and cessation times at each observation site.In addition,hourly averaged values of aerosol optical thickness（AOT） were calculated and compared with observations at four Aerosol Robotic Network （AERONET） stations to assess the model’s capability of estimating dust aerosol column burden.Analysis shows that modeled and observed AOT values were generally comparable and that the contribution of dust aerosols to AOT was significant only with regard to their source regions and their transport paths.     

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.     

秸秆燃烧对北京秋季气溶胶浓度和短波辐射影响的模拟研究

利用地面细颗粒物（PM2.5）浓度和气象常规观测资料、地基 AERONET观测资料、GFED生物质燃烧排放清单和大气化学—天气耦合模式WRF-Chem,模拟研究了华北地区2014年10月气象要素和大气污染物的时空演变,重点关注北京10月7～11日的一次重霾事件及其天气形势、边界层气象特征、输送路径、PM2.5及其化学成分浓度变化等特征,以及秸秆燃烧对华北和北京地区细颗粒物浓度和地面短波辐射的影响。与观测资料的对比结果显示,模式可以很好地模拟北京地区地面气象要素和PM2.5质量浓度,考虑秸秆燃烧排放源可以明显改进北京PM2.5浓度模拟的准确性,但在重度污染情况下,模式总体上低估气溶胶光学厚度和高估地面短波辐射。10月7～11日北京地区重霾事件主要是不利气象条件下人为污染物累积和区域输送造成,也受到华北地区南部秸秆燃烧的影响。河南北部、河北南部和山东西部大面积秸秆燃烧释放的气态污染物和颗粒物在南风的作用下输送至北京,秸秆燃烧对北京地区地面PM2.5、有机碳（OC）、硝酸盐、铵盐、硫酸盐和黑碳（BC）的平均贡献率分别为24.6%、36.8%、23.2%、22.6%、7.1%和19.8%,秸秆燃烧产生的气溶胶可以导致北京地面平均短波辐射最大减小超过20 W m－2,约占总气溶胶导致地表短波辐射变化的24%。     

Analysis of dust events in 2008 and 2009 using the lidar network, surface observations and the CFORS model

The Asian dust events in 2008 (May 24–June 4 in 2008) and in 2009 (March 12–25, October 13–26, and December 15–28 in 2009) were analyzed with the lidar network observations, surface observations in China, Korea, Japan, and Mongolia, and with the chemical transport model CFORS. Transport of Asian dust and mixing of dust with air pollution aerosols were studied. The event of May 24 to June 4 in 2008 was a significant event unusually late in the spring dust season. The dust event of March 12–25, 2009 was an interesting example of elevated dust layer, and transport of dust from the elevated dust layer to the ground by the boundary layer activity was observed with the lidars and surface observations in Japan. The concentration of air pollution aerosols was relatively high during the dust event, and the results suggest that vertical structure as well as transport path is important for the mixing of dust and air pollution aerosols. The dust events in October and December 2009 were examples of dust events in autumn and winter. The online mode CFORS reproduced the observation data generally well, except for the event of May 24 to June 4 in 2008. The results of the fourdimensional variational assimilation of the lidar network data reproduced the dust concentration in Korea and Japan reasonably in that event.     

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.     

Atmospheric circulation as a factor for air temperatures in Bulgaria

The research period is 1950–2012, and includes data for air temperatures in 21 Bulgarian stations. Two circulation indices, covering the same period and showing west–east or south–north directions of transport of air masses, were calculated. Statistical methods were used in the study. The results show a significant positive trend in average annual air temperatures in almost the entire territory of Bulgaria with the exception of its eastern-northeastern part. The warming occurs mainly in March, June and July, with some stations having significant positive values also in January, May and August. The zonal index reveals an insignificant increase of western transport of air masses in the cold half of the year (October–April) and strengthening of the eastern transport in the rest of the year. The meridional index shows an increase of the northern transport of air masses over the entire year and this is particularly visible in March, June, August and September. Correlation coefficients indicate that atmospheric circulation has leading role in determination of air temperatures during the period from November to April. Western transport of air masses leads to higher temperatures in spring, autumn and winter and to lower temperatures in summer. The influence of ENSO on atmospheric circulation over Bulgaria is weak, with a time lag of 2 months. El Niño is associated with increased western and northern transport of air masses, while La Niña is associated with increased eastern and southern transport of air masses over southeastern Europe.     

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.