Characterization of organic aerosols in Beijing using an aerodyne high-resolution aerosol mass spectrometer

Fine particle of organic aerosol(OA), mostly arising from pollution, are abundant in Beijing. To achieve a better understanding of the difference in OA in summer and autumn, a high-resolution time-of-flight aerosol mass spectrometer(HRTo F-AMS, Aerodyne Research Inc., USA) was deployed in urban Beijing in August and October 2012. The mean OA mass concentration in autumn was 30 ± 30 μg m-3, which was higher than in summer(13 ± 6.9 μg m-3). The elemental analysis found that OA was more aged in summer(oxygen-to-carbon(O/C) ratios were 0.41 and 0.32 for summer and autumn,respectively). Positive matrix factorization(PMF) analysis identified three and five components in summer and autumn, respectively. In summer, an oxygenated OA(OOA), a cooking-emission-related OA(COA), and a hydrocarbon-like OA(HOA)were indentified. Meanwhile, the OOA was separated into LV-OOA(low-volatility OOA) and SV-OOA(semi-volatile OOA);and in autumn, a nitrogen-containing OA(NOA) was also found. The SOA(secondary OA) was always the most important OA component, accounting for 55% of the OA in the two seasons. Back trajectory clustering analysis found that the origin of the air masses was more complex in summer. Southerly air masses in both seasons were associated with the highest OA loading, while northerly air masses were associated with the lowest OA loading. A preliminary study of OA components,especially the POA(primary OA), in different periods found that the HOA and COA all decreased during the National Day holiday period, and HOA decreased at weekends compared with weekdays.     

Effects of additional HONO sources on visibility over the North China Plain

The objective of the present study was to better understand the impacts of the additional sources of nitrous acid （HONO） on visibility, which is an aspect not considered in current air quality models. Simulations of HONO contributions to visibility over the North China Plain （NCP） during August 2007 using the fully coupled Weather Research and Forecasting/Chemistry （WRF/Chem） model were performed, including three additional HONO sources： （1） the reaction of photo-excited nitrogen dioxide （NO~） with water vapor; （2） the NO2 heterogeneous reaction on aerosol surfaces; and （3） HONO emissions. The model generally reproduced the spatial patterns and diurnal variations of visibility over the NCP well. When the additional HONO sources were included in the simulations, the visibility was occasionally decreased by 20%-30% （3-4 km） in local urban areas of the NCP. Monthly-mean concentrations of NO3, NH＋, SO]- and PM2.5 were increased by 20%-52% （3-11μg m-3）, 10%-38%, 6%-10%, and 6%-11% （9-17 μg m-3）, respectively; and in urban areas, monthly-mean accumulation- mode number concentrations （AMNC） and surface concentrations of aerosols were enhanced by 15%-20% and 10%-20%, respectively. Overall, the results suggest that increases in concentrations of PM2.5, its hydrophilic components, and AMNC, are key factors for visibility degradation. A proposed conceptual model for the impacts of additional HONO sources on visibility also suggests that visibility estimation should consider the heterogeneous reaction on aerosol surfaces and the enhanced atmospheric oxidation capacity due to additional HONO sources, especially in areas with high mass concentrations of NOx and aerosols.     

2014-2017年华北平原PM2.5组分消光与能见度对比研究

华北平原大气污染与低能见度状况一直是人们关切的问题.本文通过分析2014-2017年PM2.5化学成分的浓度和消光效果,研究了华北平原典型城市保定市的大气污染特征.结果表明,PM2.5组分的年均浓度显示下降趋势,水溶性无机离子,碳质气溶胶和金属元素分别减少了11 μg m-3,23μgm-3和1796 ng m-3.NH4+,NO3-和SO42-是PM2.5污染的主要污染物,三者之和占总离子浓度的82.9％.基于IMPROVE方程对细颗粒物进行重构,在观测期间PM2.5质量浓度平均为93±69μgm-3,春季,夏季,秋季和冬季的消光系数分别为373.8±233.6 M m-1,405.3±300.1 M m-1,554.3±378.2 M m-1和1005.2±750.3 M m-1.硫酸铵,硝酸铵和有机物对消光的贡献最大,不同季节下占比达55％～77％.通过PM2.5组分进行重构,利用IMPROVE算法计算得到Rbsca,用能见度测量值转换得到Vbsca,二者具有较高的相关性(r2=0.84);但存在Vbsca的高值被低估,Vbsca的低值被高估的现象;特别是当Rbsca＞1123 M m-1(对应能见度约小于2.0 km)时,Vbsca的值被低估了17.6％.高浓度PM2.5和高湿度对IMPROVE算法结果有显著的影响.     

Ground-Based In Situ Measurements of Near-Surface Aerosol Mass Concentration over Anantapur: Heterogeneity in Source Impacts

Surface measurements of aerosol physical properties were made at Anantapur(14.62°N,77.65 °E,331 m a.s.l),a semiarid rural site in India,during August 2008-July 2009.Measurements included the segregated sizes of aerosolsas as well as total mass concentration and size distributions of aerosols measured at low relative humidity(RH<75%) using a Quartz Crystal Microbalance(QCM) in the 25-0.05 μm aerodynamic diameter range.The hourly average total surface aerosol mass concentration in a day varied from 15 to 70 μg m-3,with a mean value of 34.02±9.05μgm-3 for the entire study period.A clear diurnal pattern appeared in coarse,accumulation and nucleation-mode particle concentrations,with two local maxima occurring in early morning and late evening hours.The concentration of coarse-mode particles was high during the summer season,with a maximum concentration of 11.81±0.98μgm-3 in the month of April,whereas accumulationmode concentration was observed to be high in the winter period contributed >68% to the total aerosol mass concentration.Accumulation aerosol mass fraction,A f(=Ma/Mt) was highest during winter(mean value of Af～0.80) and lowest(Af～0.64) during the monsoon season.The regression analysis shows that both R eff and R m are dependent on coarse-mode aerosols.The relationship between the simultaneous measurements of daily mean aerosol optical depth at 500 nm(AOD500) and PM 2.5 mass concentration([PM2.5]) shows that surface-level aerosol mass concentration increases with the increase in columnar aerosol optical depth over the observation period.     

Observation-based Estimation of Aerosol-induced Reduction of Planetary Boundary Layer Height

Radiative aerosols are known to influence the surface energy budget and hence the evolution of the planetary boundary layer. In this study, we develop a method to estimate the aerosol-induced reduction in the planetary boundary layer height(PBLH) based on two years of ground-based measurements at a site, the Station for Observing Regional Processes of the Earth System(SORPES), at Nanjing University, China, and radiosonde data from the meteorological station of Nanjing. The observations show that increased aerosol loads lead to a mean decrease of 67.1 W m-2for downward shortwave radiation(DSR) and a mean increase of 19.2 W m-2for downward longwave radiation(DLR), as well as a mean decrease of 9.6W m-2for the surface sensible heat flux(SHF) in the daytime. The relative variations of DSR, DLR and SHF are shown as a function of the increment of column mass concentration of particulate matter(PM2.5). High aerosol loading can significantly increase the atmospheric stability in the planetary boundary layer during both daytime and nighttime. Based on the statistical relationship between SHF and PM2.5column mass concentrations, the SHF under clean atmospheric conditions(same as the background days) is derived. In this case, the derived SHF, together with observed SHF, are then used to estimate changes in the PBLH related to aerosols. Our results suggest that the PBLH decreases more rapidly with increasing aerosol loading at high aerosol loading. When the daytime mean column mass concentration of PM2.5reaches 200 mg m-2, the decrease in the PBLH at 1600 LST(local standard time) is about 450 m.     

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%。     

Spatio-temporal variations of optical properties of aerosols in East Asia measured by MODIS and relation to the ground-based mass concentrations observed in central Korea during 2001∼2010

Long-term variations and trends of atmospheric aerosols in the East Asian region were analyzed by using aerosol optical depth (AOD or τ), and ångström exponent (AE or α) obtained from the Moderate Resolution Imaging Spectroradiometer (MODIS) from 2001 to 2010. The increased emission of anthropogenic fine aerosols in east China resulted in the high AOD in this region during summer. The steady increasing emission of anthropogenic fine aerosols caused an increasing trend of AOD in east China, and the large-scale transport of sandstorms and smoke plume caused by forest fires affected intense inter-annual variations of AOD in the East Asian region. While in the central part of South Korea, located in the lee side of the East Asian continent, AE tended to rise to a level higher than in east China, the ground-based mass concentrations continued to decline. A noticeable decrease of PM10 mass concentration in spring and winter in central Korea is most likely attributable to decreases in sandstorms in the source region of East Asia. However, the ratio of PM2.5 mass concentration to PM10 increases overall with a high level in summer. Aerosol types were classified into dust, smoke plume, and sulphate by using satellite data over Cheongwon in central Korea. The columnar AOD, with different aerosol types, was compared with the ground-based mass concentrations at Cheongwon, and the relatively high level of the correlations presented between PM2.5 and AOD produced in sulphate. Growth and increases of fine hygroscopic aerosols generated as gas-to-particle conversion particularly in summer contribute to increases of columnar AOD in the East Asian region.     

Comparison of Two Air Pollution Episodes over Northeast China in Winter 2016/17 Using Ground-Based Lidar

This study analyzes and compares aerosol properties and meteorological conditions during two air pollution episodes in 19–22 (E1) and 25–26 (E2) December 2016 in Northeast China. The visibility, particulate matter (PM) mass concentration, and surface meteorological observations were examined, together with the planetary boundary layer (PBL) properties and vertical profiles of aerosol extinction coefficient and volume depolarization ratio that were measured by a ground-based lidar in Shenyang of Liaoning Province, China during December 2016–January 2017. Results suggest that the low PBL height led to poor pollution dilution in E1, while the high PBL accompanied by low visibility in E2 might have been due to cross-regional and vertical air transmission. The PM mass concentration decreased as the PBL height increased in E1 while these two variables were positively correlated in E2. The enhanced winds in E2 diffused the pollutants and contributed largely to the aerosol transport. Strong temperature inversion in E1 resulted in increased PM_2.5 and PM₁₀ concentrations, and the winds in E2 favoured the southwesterly transport of aerosols from the North China Plain into the region surrounding Shenyang. The large extinction coefficient was partially attributed to the local pollution under the low PBL with high ground-surface PM mass concentrations in E1, whereas the cross-regional transport of aerosols within a high PBL and the low PM mass concentration near the ground in E2 were associated with severe aerosol extinction at high altitudes. These results may facilitate better understanding of the vertical distribution of aerosol properties during winter pollution events in Northeast China.     

Profiles and Source Apportionment of Nonmethane Volatile Organic Compounds in Winter and Summer in Xi’an,China, based on the Hybrid Environmental Receptor Model

Summer and winter campaigns for the chemical compositions and sources of nonmethane hydrocarbons(NMHCs)and oxygenated volatile organic compounds(OVOCs)were conducted in Xi’an.Data from 57 photochemical assessment monitoring stations for NMHCs and 20 OVOC species were analyzed.Significant seasonal differences were noted for total VOC(TVOC,NMHCs and OVOCs)concentrations and compositions.The campaign-average TVOC concentrations in winter(85.3±60.6 ppbv)were almost twice those in summer(47.2±31.6 ppbv).Alkanes and OVOCs were the most abundant category in winter and summer,respectively.NMHCs,but not OVOCs,had significantly higher levels on weekends than on weekdays.Total ozone formation potential was higher in summer than in winter(by 50%)because of the high concentrations of alkenes(particularly isoprene),high temperature,and high solar radiation levels in summer.The Hybrid Environmental Receptor Model(HERM)was used to conduct source apportionment for atmospheric TVOCs in winter and summer,with excellent accuracy.HERM demonstrated its suitability in a situation where only partial source profile data were available.The HERM results indicated significantly different seasonal source contributions to TVOCs in Xi’an.In particular,coal and biomass burning had contributions greater than half in winter(53.4%),whereas traffic sources were prevalent in summer(53.1%).This study’s results highlight the need for targeted and adjustable VOC control measures that account for seasonal differences in Xi’an;such measures should target not only the severe problem with VOC pollution but also the problem of consequent secondary pollution(e.g.,from ozone and secondary organic aerosols).     

Identification of Aerosol Types and Their Optical Properties in the North China Plain Based on Long-Term AERONET Data

Characterization of aerosols is required to reduce uncertainties in satellite retrievals of global aerosols and for modeling the effects of these aerosols on climate.Aerosols in the North China Plain(NCP) are complex,which provides a good opportunity to study key aerosol optical properties for various aerosol types.A cluster analysis of key optical properties obtained from Aerosol Robotic Network(AERONET) data in Beijing and Xianghe during 2001-11 was performed to identify dominant aerosol types and their associated optical properties.Five dominant aerosol types were identified.The results show that the urban/industrial aerosol of moderate absorption was dominant in the region and that this type varied little with season.Urban/industrial aerosol of weak absorption was the next most common type and mainly occurs in summer,followed by that strong aerosols occurring mainly in winter.All were predominantly fine mode particles.Mineral dust(MD) and polluted dust(PD) occurred mainly in spring,followed by winter,and their absorption decreased with wavelength.In addition,aerosol dynamics and optical parameters such as refractive index and asymmetry factor were examined.Results show that the size of coarse mode particles decreased with AOD indicating the domination of external mixing between aerosols.     

Satellite and ground-based remote sensing of aerosols during intense haze event of October 2013 over lahore,Pakistan

Due to increase in population and economic development, the mega-cities are facing increased haze events which are causing important effects on the regional environment and climate. In order to understand these effects, we require an in-depth knowledge of optical and physical properties of aerosols in intense haze conditions. In this paper an effort has been made to analyze the microphysical and optical properties of aerosols during intense haze event over mega-city of Lahore by using remote sensing data obtained from satellites (Terra/Aqua Moderate-resolution Imaging Spectroradiometer (MODIS) and Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO)) and ground based instrument (AErosol RObotic NETwork (AERONET)) during 6-14 October 2013. The instantaneous highest value of Aerosol Optical Depth (AOD) is observed to be 3.70 on 9 October 2013 followed by 3.12 on 8 October 2013. The primary cause of such high values is large scale crop residue burning and urban-industrial emissions in the study region. AERONET observations show daily mean AOD of 2.36 which is eight times higher than the observed values on normal day. The observed fine mode volume concentration is more than 1.5 times greater than the coarse mode volume concentration on the high aerosol burden day. We also find high values (~0.95) of Single Scattering Albedo (SSA) on 9 October 2013. Scatter-plot between AOD (500 nm) and Angstrom exponent (440-870 nm) reveals that biomass burning/urban-industrial aerosols are the dominant aerosol type on the heavy aerosol loading day over Lahore. MODIS fire activity image suggests that the areas in the southeast of Lahore across the border with India are dominated by biomass burning activities. A Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model backward trajectory showed that the winds at 1000 m above the ground are responsible for transport from southeast region of biomass burning to Lahore. CALIPSO derived sub-types of aerosols with vertical profile taken on 10 October 2013 segregates the wide spread aerosol burden as smoke, polluted continental and dust aerosols.     

非洲地区大气气溶胶光学厚度时空变化及亚速尔高压对沙尘越大西洋传输的影响

研究了非洲地区大气气溶胶光学厚度（AOD）的时空变化及沙尘气溶胶越大西洋海区的传输。结果表明：1）源于撒哈拉沙漠的沙尘及其随赤道东风向西输送使得沙尘气溶胶成为非洲沙漠地区和紧邻的大西洋海区的主要气溶胶组分;AOD高值区和沙尘气溶胶光学厚度高值区在1—7月随赤道辐合带北移同步向北移动,而在8—12月则向南回撤。2）刚果盆地大气气溶胶主要为热带雨林和稀树草原排放的有机碳（OC）和黑碳（BC）气溶胶;其中与生物质燃烧源排放有关的OC、BC高值主要集中在干季（6—9月）的后半段（8—9月）;而生物源OC排放全年连续,其排放峰值出现于雨季开始时;生物质燃烧排放高值期与生物源排放高值期前后相继,形成干季（尤其是后半段）时期的OC、BC光学厚度高值。3）亚马逊河入海口地区主要气溶胶组分为海盐气溶胶,9—11月该区风力输送增强,风向由东南风转变为东风,海盐进入亚马逊河入海口处,形成AOD和海盐气溶胶光学厚度高值区。4）撒哈拉沙漠沙尘气溶胶向大西洋传输的偏北月份为7—9月、偏南月份为1—3月;2000—2016年海区沙尘气溶胶的传输路径存在向南移动的变化趋势,与同期亚速尔高压的增强和沙尘传输路径以北北风分量的增强以及赤道辐合带的移动一致。上述研究结果揭示了利用大气气溶胶时空变化特征反映区域大气环流和气候变化的可能性。     

中国大陆黑碳气溶胶排放清单

The detailed high-resolution emission inventory of black carbon (BC) from China in the year 2000 was calculated. The latest fuel consumption data including fossil and biomass fuels, and socio-economic statistics used were obtained from government agencies, mostly at the county level, and some new emission factors (Efs) from local measurements were also used. National and regional summaries of emissions were presented at 0.2°×0.2°resolution. Total BC emission was 1499.4 Gg in 2000, mainly due to the burning of coal and biomass. The BC emission estimated here is higher than those in previous studies, mainly because the emissions from coal burning by rural industries and residences were previously underestimated. More BC aerosols were emitted from eastern China than western China. A strong seasonal dependence was observed for BC emissions, with peaks in January and December and low emissions in July and August; and this seasonality is mainly due to patterns in residential heating and the open burning of crop residues.     

ROx Budgets and O3 Formation during Summertime at Xianghe Suburban Site in the North China Plain

Photochemical smog characterized by high concentrations of ozone (O3) is a serious air pollution issue in the North China Plain (NCP) region, especially in summer and autumn. For this study, measurements of O3, nitrogen oxides (NOx), volatile organic compounds (VOCs), carbon monoxide (CO), nitrous acid (HONO), and a number of key physical parameters were taken at a suburban site, Xianghe, in the NCP region during the summer of 2018 in order to better understand the photochemical processes leading to O3 formation and find an optimal way to control O3 pollution. Here, the radical chemistry and O3 photochemical budget based on measurement data from 1-23 July using a chemical box model is investigated. The daytime (0600-1800 LST) average production rate of the primary radicals referred to as ROx (OH + HO2+ RO2) is 3.9 ppbv h-1. HONO photolysis is the largest primary ROx source (41％). Reaction of NO2 + OH is the largest contributor to radical termination (41％), followed by reactions of RO2 + NO2 (26％). The average diurnal maximum O3 production and loss rates are 32.9 ppbv h-1 and 4.3 ppbv h-1, respectively. Sensitivity tests without the HONO constraint lead to decreases in daytime average primary ROx production by 55％ and O3 photochemical production by 42％, highlighting the importance of accurate HONO measurements when quantifying the ROx budget and O3 photochemical production. Considering heterogeneous reactions of trace gases and radicals on aerosols, aerosol uptake of HO2 contributes 11％ to ROx sink, and the daytime average O3 photochemical production decreases by 14％. The O3-NOx-VOCs sensitivity shows that the O3 production at Xianghe during the investigation period is mainly controlled by VOCs.     

Characteristics of biomass burning aerosol and its impact on regional air quality in the summer of 2003 at Gwangju, Korea

The main objective of this study is to investigate the chemical characteristics of biomass burning aerosol and its impact on regional air quality during an agricultural waste burning period in early summer in the rural areas of Korea. A 12-h integrated intensive sampling of biomass burning aerosol in the fine and coarse modes was conducted on 2–20 June 2003 in Gwangju, Korea. The collected samples were analyzed for concentrations of mass, ionic, elemental, and carbonaceous species. Average concentrations of fine and coarse mass were measured to be 67.9 and 18.7 μg m^− 3 during the biomass burning period, 41.9 and 18.8 μg m^− 3 during the haze period, and 35.6 and 13.3 μg m^− 3 during the normal period, respectively. An exceptionally high PM_2.5 concentration of 110.3 μg m^− 3 with a PM_2.5/PM₁₀ ratio of 0.79 was observed on 6 June 2003 during the biomass burning period. The potassium ratio method was used to identify biomass burning samples. The average ratio of potassium in the fine mode to the coarse mode (FK/CK) was 23.8 during the biomass burning period, 6.0 during the haze period, and 4.7 during the normal period, respectively. A FK/CK ratio above 9.2 was considered a criterion for biomass burning event in this study. Particulate matter from the open field burning of agricultural waste has an adverse impact on visibility, human health, and regional air quality.     

Sources and Transport of Urban and Biomass Burning Aerosol Black Carbon at the South–West Atlantic Coast

The total extent of the atmospheric impacts associated to the aerosol black carbon (BC) emissions from South America is not completed described. This work presents results of BC monitored during three scientific expeditions (2002, 2003 and 2004) on board of a Brazilian oceanographic vessel Ary Rongel that covered the South–West Atlantic coast between 22–62°S. This latitudinal band encloses major urban regions of South America and the outflow region of the SACZ (South Atlantic Convergent Zone), which is an important mechanism of advective transport of heat, moisture, minor gases and aerosols from the South America continental land to the Southern Atlantic Ocean. Our results showed that aerosol BC enhanced concentrations from urban/industrial origin can be transported to the South–West Atlantic Ocean due to the migration of sub-polar fronts that frequently reach tropical/subtropical regions. Despite the decrease of aerosol BC concentrations southwards (from ∼1,200 ng m⁻³ at latitude 22°S to ∼10 ng m⁻³ at latitude 62°S), several observed peak events were attributed to regional urban activities. Most of such events could be explained by the use of air mass back trajectories analysis. In addition, a global model simulation is presented (Goddard Institute for Space Studies – GISS GCM BC simulation) to explore the origins of aerosol BC in the South–West Atlantic. The model allowed isolating the biomass emissions from South America and Africa and industrial (non-biomass) pollution from other regions of the globe. This model suggests that the apportionment of about half of the aerosol BC at the South–West Atlantic may derive from South American biomass burning.     

耦合气溶胶气候模式FGOALS-f3-L模拟青藏高原地区气溶胶特性

基于新耦合气溶胶气候模式FGOALS-f3-L模拟分析了2002-2011年青藏高原地区气溶胶时空分布特征.结果表明:青藏高原地区,沙尘,硫酸盐,碳质气溶胶(包括黑碳,有机碳和混合碳)地表质量浓度分别占比为53.6％,32.2％,14.2％;在拉萨站点,模拟的气溶胶地表质量浓度被低估,尤其是黑碳和有机碳气溶胶;模拟的气溶胶光学厚度(AOD)时空分布与卫星观测结果较为一致,均方根误差和偏差分别为0.081和0.036;由于模式中沙尘排放参数化的不确定性,模式对AOD的模拟效果在夏季和秋季优于春季.     

CALIOP对一次秸秆焚烧后气溶胶光学特性的探测分析

采用星载激光雷达(Cloud - Aerosol LIdar with Orthogonal Polarization,CALIOP)资料研究了2008年6月2日华东秸秆焚烧排放气溶胶的光学特性,并与2006～2008年统计结果进行了对比.结果表明:1)CALIOP能够有效探测到气溶胶层,探测结果符合生物质燃烧气溶胶的...     

Source attribution of urban smog episodes caused by coal combustion

Stable weather conditions together with extensive use of coal combustion often lead to severe smog episodes in certain urban environments, especially in Eastern Europe. In order to identify the specific sources that cause the smog episodes in such environments, and to better understand the mixing state and atmospheric processing of aerosols, both single particle and bulk chemical characterization analysis of aerosols were performed in Krakow, Poland, during winter 2005.Real-time measurements of the bulk PM10 aerosol during a severe smog episode (PM10 mass > 400 µg m^− 3) showed a stable concentration of black carbon in the aerosol, and an increase in the sulphate and chlorine mass contributions towards the end of the episode. Chemical characterization of single particles further helped to identify residential coal burning as the main source that caused this severe smog episode, consisting of single particles with major signals for carbon with simultaneous absence of sulphate, chlorine and calcium. Particles from industrial coal combustion gained importance towards the end of that episode, after residential coal combustion was switched off, indicated by an increase of the percentage of sulphate and chlorine containing particles. Traffic was not a significant source during the severe smog episode. During a lighter smog episode, residential and industrial coal combustion was still predominant, with an increased contribution of traffic and processed/aged aerosols. On a clean day, particle classes containing nitrate were the most abundant. In addition, the aerosol was more internally mixed showing that there were more sources contributing to the total aerosol population.     

Modeling Study of the Impact of Heterogeneous Reactions on Dust Surfaces on Aerosol Optical Depth and Direct Radiative Forcing over East Asia in Springtime

The spatial distributions and interannual variations of aerosol concentrations,aerosol optical depth(AOD) ,aerosol direct radiative forcings,and their responses to heterogeneous reactions on dust surfaces over East Asia in March 2006-10 were investigated by utilizing a regional coupled climate-chemistry/aerosol model. Anthropogenic aerosol concentrations(inorganic+carbonaceous) were higher in March 2006 and 2008,whereas soil dust reached its highest levels in March 2006 and 2010,resulting in stronger aerosol radiative forcings in these periods.The domain and five-year(2006-10) monthly mean concentrations of anthropogenic and dust aerosols,AOD,and radiative forcings at the surface(SURF) and at the top of the atmosphere(TOA) in March were 2.4μg m-3,13.1μg m-3,0.18,-19.0 W m-2,and-7.4 W m-2,respectively.Heterogeneous reactions led to an increase of total inorganic aerosol concentration;however,the ambient inorganic aerosol concentration decreased,resulting in a smaller AOD and weaker aerosol radiative forcings.In March 2006 and 2010,the changes in ambient inorganic aerosols,AOD,and aerosol radiative forcings were more evident.In terms of the domain and five-year averages,the total inorganic aerosol concentrations increased by 13.7%(0.17μg m-3) due to heterogeneous reactions,but the ambient inorganic aerosol concentrations were reduced by 10.5%(0.13μg m-3) .As a result,the changes in AOD,SURF and TOA radiative forcings were estimated to be-3.9%(-0.007) ,-1.7%(0.34 W m-2) ,and-4.3%(0.34 W m-2) ,respectively,in March over East Asia.