Coarse Aerosol Research Articles

Bias induced by the AOD representation time scale in long-term solar radiation calculations. Part 1: Sensitivity of the AOD distribution to the representation time scale

The temporal resolution of aerosol optical depth (AOD) affects the prediction of surface irradiance and hence impacts solar resource assessments. Most current global AOD databases used for solar radiation estimation span from monthly to yearly time scales, which are much coarser than the typical hourly or sub-hourly time step used for irradiance calculations. The relative variation of the AOD’s mean and standard deviation (SD) calculated from data at monthly and daily temporal resolutions is assumed here as a proxy for the expected differences in the calculated long-term average of solar irradiance when using monthly and daily AOD data. This is specifically analyzed in Part 2 of this study. In this Part 1, the changes in the mean and SD of AOD caused by an alteration of the time scale from daily to monthly time resolution are investigated first. A database from 214 AERONET sites with long historical record series is used, as well as data from worldwide multi-year evaluations of AOD from a numerical weather model coupled with an aerosol transport model. The AERONET AOD data is fitted to the log-normal distribution and the results are separately analyzed for multiple AOD representation time scales from daily to monthly, and for sites with prevalence of coarse, mixed or fine aerosols. When the averaging period is increased from one to 30days, three effects are noticed regardless of the aerosol regime: (i) the range of possible AOD values narrows; (ii) the probability around the modal AOD increases; and (iii) the AOD distribution’s mode moves toward higher values. On average, the mean AOD at sites dominated by coarse or mixed aerosols does not significantly vary (it does by only less than 1%) when the averaging time increases from one day to 30days, although with significant dispersion from site to site (≈±5%). In contrast, again on average, it declines ≈4% at the fine aerosol sites. Conversely, the SD decays exponentially fast at all sites—faster at the fine aerosol sites—on average. For an averaging period of 30days, the SD of AOD over Europe and inland areas of Asia can be as low as 40% of the daily SD, while for most other land areas it stays at ≈60% of the daily SD. The impact that this change in the AOD SD has on the prediction of surface irradiance is investigated in this study’s Part 2.

Validation of Aqua-MODIS C051 and C006 Operational Aerosol Products Using AERONET Measurements Over Pakistan

The aim of this study was to evaluate the performance of the Aqua-MODIS (MYD04) collections 5.1 (C051) and 6 (C006) operational aerosol products over Pakistan. These include the Dark Target (DT) and the Deep Blue (DB) C051/C006 aerosol optical depth (AOD) observations at 10-km spatial resolution, and which were validated using 7 years (2007–2013) AOD measurements from two AERONET stations located in Pakistan’s two largest cities, Lahore and Karachi. Lahore is an inland city, consisting of built-up areas and agricultural land and dominated by mainly fine aerosol particles. Karachi is an urban-coastal city with built-up areas and bare land, and mainly affected by coarse aerosol particles. The retrieval uncertainties and accuracy were evaluated using the expected error over land ( ${\text{EE}}:\, \pm {{0}}.{{05}} + {{15}}\% $ ), the root-mean-square error (RMSE), the mean absolute error (MAE), and the relative mean bias (RMB). It was found that the DT C051 AOD retrievals were significantly overestimated over both AERONET sites with mean overestimation of 21% and 31% for Lahore and Karachi, respectively. On the other hand, the DB C051 retrievals were underestimated by 10% and 35% for both cities. Similar to the DT C051, the C006 AOD retrievals were overestimated over Lahore, but significantly improved over Karachi, as the mean overestimation reduced from 31% ( ${\text{RMB}} = {{1}}.{{31}}$ ) to 4% ( ${\text{RMB}} = {{1}}.{{04}}$ ) and the percentage of retrievals within the EE increased from 38.46% to 63.33%. However, the DB C006 AOD retrievals have similar errors (RMSE and MAE) and the percentage of retrievals within the EE over both cities as C051, but they have more mean underestimations. Spatio-temporal distributions showed that the DT and DB C006 were well correlated with Karachi and Lahore AERONET measurements, respectively. Therefore, these results recommend the use of the DT C006 algorithm over Karachi and the DB C006 over Lahore for qualitative regional air quality applications due to differences in land cover characteristics and aerosol types.

Validation of MODIS 3 km Resolution Aerosol Optical Depth Retrievals Over Asia

This study evaluates the new Aqua MODIS Dark Target (DT) Collection 6 (C6) Aerosol Optical Depth (AOD) (MYD04_3K) retrieval algorithm at 3 km resolution over Asian countries that have recently experienced severe and increasing air pollution. Retrievals showed generally low accuracy compared with the AErosol RObotic NETwork (AERONET), with only 55% of retrievals within the expected error (EE). The uncertainty appears mainly due to systematic overestimation at both low and high AOD levels. This is attributed to under-prediction of surface reflectance, similar to, but more severe than, the C6 DT product at 10-km resolution. This is because MYD04_3K observes more noise in the surface reflectance computations, due to retention of some bright pixels in the retrieval window which would be discarded at 10 km. Greatest uncertainty was observed at urban sites, especially those dominated by coarse aerosols. Results suggest that the DT at 3 km is less reliable than MODIS C6 AOD products at 10 km.

Effects of data assimilation on the global aerosol key optical properties simulations

We present the one month results of global aerosol optical properties for April 2006, using the Spectral Radiation Transport Model for Aerosol Species (SPRINTARS) coupled with the Non-hydrostatic ICosahedral Atmospheric Model (NICAM), by assimilating Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) with Local Ensemble Transform Kalman Filter (LETKF). The simulated AOD, Ångström Exponent (AE) and single scattering albedo (SSA) are validated by independent Aerosol Robotic Network (AERONET) observations over the global sites. The data assimilation has the strongest positive effect on the AOD simulation and slight positive influences on the AE and SSA simulations. For the time-averaged globally spatial distribution, the data assimilation increases the model skill score (S) of AOD, AE, and SSA from 0.55, 0.92, and 0.75 to 0.79, 0.94, and 0.80, respectively. Over the North Africa (NAF) and Middle East region where the aerosol composition is simple (mainly dust), the simulated AODs are best improved by the data assimilation, indicating the assimilation correctly modifies the wrong dust burdens caused by the uncertainties of the dust emission parameterization. Assimilation also improves the simulation of the temporal variations of the aerosol optical properties over the AERONET sites, with improved S at 60 (62%), 45 (55%) and 11 (50%) of 97, 82 and 22 sites for AOD, AE and SSA. By analyzing AOD and AE at five selected sites with best S improvement, this study further indicates that the assimilation can reproduce short duration events and ratios between fine and coarse aerosols more accurately.

Lidar-Radiometer Inversion Code (LIRIC) for the retrieval of vertical aerosol properties from combined lidar/radiometer data: development and distribution in EARLINET

Abstract. This paper presents a detailed description of LIRIC (LIdar-Radiometer Inversion Code) algorithm for simultaneous processing of coincident lidar and radiometric (sun photometric) observations for the retrieval of the aerosol concentration vertical profiles. As the lidar/radiometric input data we use measurements from European Aerosol Research Lidar Network (EARLINET) lidars and collocated sun-photometers of Aerosol Robotic Network (AERONET). The LIRIC data processing provides sequential inversion of the combined lidar and radiometric data. The algorithm starts with the estimations of column-integrated aerosol parameters from radiometric measurements followed by the retrieval of height dependent concentrations of fine and coarse aerosols from lidar signals using integrated column characteristics of aerosol layer as a priori constraints. The use of polarized lidar observations allows us to discriminate between spherical and non-spherical particles of the coarse aerosol mode.The LIRIC software package was implemented and tested at a number of EARLINET stations. Intercomparison of the LIRIC-based aerosol retrievals was performed for the observations by seven EARLINET lidars in Leipzig, Germany on 25 May 2009. We found close agreement between the aerosol parameters derived from different lidars that supports high robustness of the LIRIC algorithm. The sensitivity of the retrieval results to the possible reduction of the available observation data is also discussed.

Observational evidence for the convective transport of dust over the Central United States

AbstractBulk aerosol composition and aerosol size distributions measured aboard the DC‐8 aircraft during the Deep Convective Clouds and Chemistry Experiment mission in May/June 2012 were used to investigate the transport of mineral dust through nine storms encountered over Colorado and Oklahoma. Measurements made at low altitudes (<5 km mean sea level (MSL)) in the storm inflow region were compared to those made in cirrus anvils (altitude > 9 km MSL). Storm mean outflow Ca2+ mass concentrations and total coarse (1 µm < diameter < 5 µm) aerosol volume (Vc) were comparable to mean inflow values as demonstrated by average outflow/inflow ratios greater than 0.5. A positive relationship between Ca2+, Vc, ice water content, and large (diameter > 50 µm) ice particle number concentrations was not evident; thus, the influence of ice shatter on these measurements was assumed small. Mean inflow aerosol number concentrations calculated over a diameter range (0.5 µm < diameter < 5.0 µm) relevant for proxy ice nuclei (NPIN) were ~15–300 times higher than ice particle concentrations for all storms. Ratios of predicted interstitial NPIN (calculated as the difference between inflow NPIN and ice particle concentrations) and inflow NPIN were consistent with those calculated for Ca2+ and Vc and indicated that on average less than 10% of the ingested NPIN were activated as ice nuclei during anvil formation. Deep convection may therefore represent an efficient transport mechanism for dust to the upper troposphere where these particles can function as ice nuclei cirrus forming in situ.

Effects of mineral dust on global atmospheric nitrate concentrations

Abstract. This study assesses the chemical composition and global aerosol load of the major inorganic aerosol components, focusing on mineral dust and aerosol nitrate. The mineral dust aerosol components (i.e., Ca2+, Mg2+, K+, Na+) and their emissions are included in the ECHAM5/MESSy Atmospheric Chemistry model (EMAC). Gas/aerosol partitioning is simulated using the ISORROPIA-II thermodynamic equilibrium model that considers K+, Ca2+, Mg2+, NH4+, Na+, SO42−, NO3−, Cl−, and H2O aerosol components. Emissions of mineral dust are calculated online by taking into account the soil particle size distribution and chemical composition of different deserts worldwide. Presence of metallic ions can substantially affect the nitrate partitioning into the aerosol phase due to thermodynamic interactions. The model simulates highest fine aerosol nitrate concentration over urban and industrialized areas (1–3 µg m−3), while coarse aerosol nitrate is highest close to deserts (1–4 µg m−3). The influence of mineral dust on nitrate formation extends across southern Europe, western USA, and northeastern China. The tropospheric burden of aerosol nitrate increases by 44 % when considering interactions of nitrate with mineral dust. The calculated global average nitrate aerosol concentration near the surface increases by 36 %, while the coarse- and fine-mode concentrations of nitrate increase by 53 and 21 %, respectively. Other inorganic aerosol components are affected by reactive dust components as well (e.g., the tropospheric burden of chloride increases by 9 %, ammonium decreases by 41 %, and sulfate increases by 7 %). Sensitivity tests show that nitrate aerosol is most sensitive to the chemical composition of the emitted mineral dust, followed by the soil size distribution of dust particles, the magnitude of the mineral dust emissions, and the aerosol state assumption.

Long-term (2002–2012) investigation of Saharan dust transport events at Mt. Cimone GAW global station, Italy (2165 m a.s.l.)

Mineral dust transport from North Africa towards the Mediterranean basin and Europe was monitored over an 11-y period (2002–2012) using the continuous observations made at Mt. Cimone WMO/GAW global station (CMN). CMN is in a strategic position for investigating the impact of mineral dust transported from northern Africa on the atmospheric composition of the Mediterranean basin and southern Europe. The identification of “dusty days” is based on coupling the measured in situ coarse aerosol particle number concentration with an analysis of modeled back trajectories tracing the origin of air masses from North Africa. More than 400 episodes of mineral dust transport were identified, accounting for 15.7% of the investigated period. Our analysis points to a clear seasonal cycle, with the highest frequency from spring to autumn, and a dust-induced variation of the coarse particle number concentration larger than 123% on a seasonal basis. In addition, FLEXTRA 10-d back trajectories showed that northwestern and central Africa are the major mineral dust source regions. Significant inter-annual variability of dust outbreak frequency and related mineral dust loading were detected and during spring the NAO index was positively correlated (R2 = 0.32) with dust outbreak frequency. Lastly, the impact of transported mineral dust on the surface O3 mixing ratio was quantified over the 11-y investigation period. Evidence of a non-linear and negative correlation between mineral dust and ozone concentrations was found, resulting in an average spring and summer decrease of the O3 mixing ratio down to 7%.

Tracing the Sources of Atmospheric Phosphorus Deposition to a Tropical Rain Forest in Panama Using Stable Oxygen Isotopes.

Atmospheric dust deposition can be a significant source of phosphorus (P) in some tropical forests, so information on the origins and solubility of atmospheric P is needed to understand and predict patterns of forest productivity under future climate scenarios. We characterized atmospheric dust P across a seasonal cycle in a tropical lowland rain forest on Barro Colorado Nature Monument (BCNM), Republic of Panama. We traced P sources by combining remote sensing imagery with the first measurements of stable oxygen isotopes in soluble inorganic phosphate (δ(18)OP) in dust. In addition, we measured soluble inorganic and organic P concentrations in fine (<1 μm) and coarse (>1 μm) aerosol fractions and used this data to estimate the contribution of P inputs from dust deposition to the forest P budget. Aerosol dry mass was greater in the dry season (December to April, 5.6-15.7 μg m(-3)) than the wet season (May to November, 3.1-7.1 μg m(-3)). In contrast, soluble P concentrations in the aerosols were lower in the dry season (980-1880 μg P g(-1)) than the wet season (1170-3380 μg P g(-1)). The δ(18)OP of dry-season aerosols resembled that of nearby forest soils (∼19.5‰), suggesting a local origin. In the wet season, when the Trans-Atlantic Saharan dust belt moves north close to Panama, the δ(18)OP of aerosols was considerably lower (∼15.5‰), suggesting a significant contribution of long-distance dust P transport. Using satellite retrieved aerosol optical depth (AOD) and the P concentrations in aerosols we sampled in periods when Saharan dust was evident we estimate that the monthly P input from long distance dust transport during the period with highest Saharan dust deposition is 88 ± 31 g P ha(-1) month(-1), equivalent to between 10 and 29% of the P in monthly litter fall in nearby forests. These findings have important implications for our understanding of modern nutrient budgets and the productivity of tropical forests in the region under future climate scenarios.

Combining AOT, Angstrom Exponent and PM concentration data, with PSCF model, to distinguish fine and coarse aerosol intrusions in Southern France

In this paper, a cluster analysis of backward air mass trajectories, arriving in Avignon (Southern France), was combined with a Potential Source Contribution Function (PSCF) model on a 0.5°×0.5° resolution grid, in order to indicate possible aerosol intrusions. A strict triple criterion was constructed from Aerosol Optical Thickness (AOT), Angstrom Exponent (AE), and PM (PM10 and PM2.5) concentration measurements, aiming to distinguish more effectively Episodes of Fine, Coarse and Overall Aerosols (FAE, CAE and OAE respectively). Large fractions of FAE (60.0%) and CAE (40.6%) were strongly attributed to the prevalence of Eastern and South–Southwest (S–SW) airflows respectively, whereas these distinct trajectory clusters also gathered large fractions of OAE (90.2% cumulatively). According to PSCF results, FAE events were strongly associated with the influence of air masses traveling over North Italy and Southern Germany, hence the impact of urban and industrial combustion was emerged. Main sources of coarse aerosols were principally isolated over the Mediterranean, thus the import of sea spray and dust from the Sahara desert is presumed. Satellite AOT observations were used for a more detailed identification of an intense 5-day intrusion of coarse aerosols. Short range slow moving air mass trajectories, were proven to be a clear marker of atmospheric stagnation, based on a wind speed analysis, triggering the accumulation of locally emitted anthropogenic aerosols (mainly PM2.5) and lack of city ventilation.

Chemical characterization and mass closure of PM10 and PM2.5 at an urban site in Karachi – Pakistan

Abstract A mass balance method is applied to assess main source contributions to PM2.5 and PM10 levels in Karachi. Carbonaceous species (elemental carbon, organic carbon, carbonate carbon), soluble ions (Ca++, Mg++, Na+, K+, NH4+, Cl − , NO3 − , SO4 − ), saccharides (levoglucosan, galactosan, mannosan, sucrose, fructose, glucose, arabitol and mannitol) were determined in atmospheric fine (PM2.5) and coarse (PM10) aerosol samples collected under pre-monsoon conditions (March–April 2009) at an urban site in Karachi (Pakistan). The concentrations of PM2.5 and PM10 were found to be 75 μg/m3 and 437 μg/m3 respectively. The large difference between PM10 and PM2.5 originated predominantly from mineral dust. “Calcareous dust” and „siliceous dust” were the over all dominating material in PM, with 46% contribution to PM2.5 and 78% to PM10–2.5. Combustion particles and secondary organics (EC + OM) comprised 23% of PM2.5 and 6% of PM10–2.5. EC, as well as OC ambient levels were higher (59% and 56%) in PM10–2.5 than in PM2.5. Biomass burning contributed about 3% to PM2.5, and had a share of about 13% of “EC + OM” in PM2.5. The impact of bioaerosol (fungal spores) was minor and had a share of 1 and 2% of the OC in the PM2.5 and PM10–2.5 size fractions. In case of secondary inorganic aerosols, ammonium sulphate (NH4)2SO4 contributes 4.4% to PM2.5 and no detectable quantity were found in fraction PM10–2.5. The sea salt contribution is about 2% both to PM2.5 and PM10–2.5.

Comparison of physicochemical properties between fine (PM2.5) and coarse airborne particles at cold season in Korea

Although it has been well-known that atmospheric aerosols affect negatively the local air quality, human health, and climate changes, the chemical and physical properties of atmospheric aerosols are not fully understood yet. This study experimentally measured the physiochemical characteristics of fine and coarse aerosol particles at the suburban area to evaluate relative contribution to environmental pollution in consecutive seasons of autumn and winter, 2014–2015, using XRD, SEM–EDX, XNI, ICP-MS, and TOF-SIMS. For these experimental works, the fine and coarse aerosols were collected by the high volume air sampler for 7days each season. The fine particles contain approximately 10μgm−3 of carbonaceous aerosols consisting of 90% organic and 10% elemental carbon. The spherical-shape carbonaceous particles were observed for the coarse samples as well. Interestingly, the coarse particles in winter showed the increased frequency of carbon-rich particles with high contents of heavy metals. These results suggest that, for the cold season, the coarse particles could contribute relatively more to the conveyance of toxic contaminants compared to the fine particles in the study area. However, the fine particles showed acidic properties so that their deposition to surface may cause facilitate the increase of mobility for toxic heavy metals in soil and groundwater environments. The fine and coarse particulate matters, therefore, should be monitored separately with temporal variation to evaluate the impact of atmospheric aerosols to environmental pollution and human health.

On the Importance of Aerosol Composition for Estimating Incoming Solar Radiation: Focus on the Western African Stations of Dakar and Niamey during the Dry Season

The article investigates the impact of aerosol composition on the estimation of the downwelling surface shortwave flux (DSSF). This initiative forms part of the efforts to improve the DSSF distributed by the Land Surface Analysis Satellite Application Facility (LSA-SAF). This operational product assumes invariant aerosol properties under clear sky conditions, which can be inaccurate for some regions of the world. This is the case of West Africa, where aerosol activity is not only highly variable due to frequent dust storms but also rich because of the coexistence of different aerosol species. This study was carried out over the West African stations of Dakar and Niamey, which represent different aerosol scenarios. Several dates during the dry season of 2006 were selected and classified into four different day types according to aerosol activity: standard, clean, mixture and dusty days. The diurnal evolution of DSSF and its direct and diffuse components were estimated for the selected dates by the current LSA-SAF algorithm and two other approaches using aerosol measurements from the Aerosol Robotic Network (AERONET) as input. The first alternative approach took the diurnal evolution of the total aerosol optical depth (AOD) into account, assuming a default desert aerosol type. Experiments with this method showed a significant improvement in the estimated DSSF compared to the current LSA-SAF algorithm. For example, root mean square error (RMSE) improved from 170 W/m2 to 50 W/m2 for dusty days in Dakar and from 73 W/m2 to 21 W/m2 for mixture days in Niamey. This improvement resulted from the consideration of a time-varying AOD, which accounted for the rapidly changing aerosol load for these two day types. The second alternative approach tested included consideration of the diurnal variation of the aerosol load and composition. Again, this was done using AERONET data on the fine and coarse aerosol modes, which may be associated with different sized dust particles, sea salt, or soot from biomass burning (depending on the date). This enhanced consideration of the aerosol composition greatly improved the estimation of the diffuse component of the DSSF, further reducing the RMSE during mixture days from 50 W/m2 to less than 10 W/m2. This improvement mainly came from consideration of the right scattering properties of the aerosol particles, which may be significantly different for each aerosol type.

Characteristics of aerosols over Beijing and Kanpur derived from the AERONET dataset

Beijing and Kanpur are two cities identified as high aerosol optical thickness (AOT) and complex composition of aerosols in Asian monsoon regions. Detail knowledge of key aerosol types in these two countries would be helpful for clarifying the mechanisms of aerosol radiative forcing and improving the accuracy of satellite remote sensing in these two countries. This study examines the characteristics of aerosol types over Beijing and Kanpur derived from a 12-year dataset from Aerosol Robotic Network (AERONET) stations and compares them via cluster analysis of optical and microphysical properties. Aerosols in Beijing are more complex than in Kanpur. Four fine-size dominated aerosol types (including two types of moderately absorbing aerosols, one highly absorbing aerosol type and one non-absorbing aerosol type) and one coarse-size dominated aerosol type are identified over Beijing. In Kanpur, two fine-sized dominated aerosol types (one high absorbing aerosol type and one non-absorbing aerosol type) and one coarse-sized dominated aerosol type are obtained. Compared to Beijing, the average SSAs of non-absorbing and high-absorbing aerosols are lower for the four wavelengths (440 nm, 676 nm, 869 nm, 1020 nm) in Kanpur. High absorbing aerosols usually occur in the months December to February (DJF) for both sites. The proportion in Kanpur (14%) is about twice that in Beijing (7%). Non-absorbing aerosols are usually observed in the months June to August (JJA) for both sites. Their proportion in Kanpur (31%) is ∼3 times larger than that in Beijing (11%). Coarse aerosols are frequently observed in the months March to May (MAM) for both sites. Their proportion in Kanpur (54%) is two times larger than in Beijing (21%).

Potential source identification for aerosol concentrations over a site in Northwestern India

The collocated measurements of aerosols size distribution (ASD) and aerosol optical thickness (AOT) are analyzed simultaneously using Grimm aerosol spectrometer and MICROTOP II Sunphotometer over Jaipur, capital of Rajasthan in India. The contrast temperature characteristics during winter and summer seasons of year 2011 are investigated in the present study. The total aerosol number concentration (TANC, 0.3–20μm) during winter season was observed higher than in summer time and it was dominated by fine aerosol number concentration (FANC<2μm). Particles smaller than 0.8μm (at aerodynamic size) constitute ~99% of all particles in winter and ~90% of particles in summer season. However, particles greater than 2μm contribute ~3% and ~0.2% in summer and winter seasons respectively. The aerosols optical thickness shows nearly similar AOT values during summer and winter but corresponding low Angstrom Exponent (AE) values during summer than winter, respectively. In this work, Potential Source Contribution Function (PSCF) analysis is applied to identify locations of sources that influenced concentrations of aerosols over study area in two different seasons. PSCF analysis shows that the dust particles from Thar Desert contribute significantly to the coarse aerosol number concentration (CANC). Higher values of the PSCF in north from Jaipur showed the industrial areas in northern India to be the likely sources of fine particles. The variation in size distribution of aerosols during two seasons is clearly reflected in the log normal size distribution curves. The log normal size distribution curves reveals that the particle size less than 0.8μm is the key contributor in winter for higher ANC.

Atmospheric particulate mercury at the urban and forest sites in central Poland.

Particulate mercury concentrations were investigated during intensive field campaigns at the urban and forest sites in central Poland, between April 2013 and October 2014. For the first time, quantitative determination of total particulate mercury in coarse (PHg2.2) and fine (PHg0.7) aerosol samples was conducted in Poznań and Jeziory. The concentrations in urban fine and coarse aerosol fractions amounted to <MDL ± 77.1 pg m−3 and <MDL ± 604.9 pg m−3, respectively. Aerosol samples collected during the whole study period showed statistically significant differences for particulate mercury concentrations. A strong impact of meteorological conditions (wind velocity, air mass direction, air temperature, and precipitation amount) on particulate mercury concentrations was also observed. In particular, higher variation and concentration range of PHg0.7 and PHg2.2 was reported for wintertime measurements. An increase in atmospheric particulate mercury during the cold season in the study region indicated that coal combustion, i.e., residential and industrial heating, is the main contribution factor for the selected particle size modes. Coarse particulate Hg at the urban site during summer was mainly attributed to anthropogenic sources, with significant contribution from resuspension processes and long-range transport. The highest values of PHg0.7 and PHg2.2 were found during westerly and southerly wind events, reflecting local emission from highly polluted areas. The period from late fall to spring showed that advection from the southern part of Poland was the main factor responsible for elevated Hg concentrations in fine and coarse particles in the investigated region. Moreover, September 2013 could be given as an example of the influence of additional urban activities which occurred approx. 10 m from the sampling site—construction works connected with replacement of the road surface, asphalting, etc. The concentrations of particulate Hg (>600.0 pg m−3) were much higher than during the following months when any similar situation did not occur. Our investigations confirmed that Hg in urban aerosol samples was predominantly related to local industrial and commercial emissions, whereas the main source of Hg in particulate matter collected at the forest site was connected with regional anthropogenic processes. This paper provides the results of the first long-term measurements of size-fractionated particulate mercury conducted in central Poland, which could be an important insight into atmospheric Hg processes within such a scarcely investigated part of Europe.

Characterization of aerosols in Beijing during severe aerosol loadings

Severe aerosol pollutions in China significantly impact radiative forcing of climate at regional and global scales. Until now, the uncertainties in net climate forcing from severe aerosol pollutions in China are substantial, largely due to the lack of detailed knowledge of radiative properties of severe aerosol pollutions. Here the characteristics of aerosols under severe aerosol pollution days (APs) in Beijing are studied by analyzing the ground-based radiance measurements during the period from 2002 to 2014. We show that the mean single scattering albedo (SSA) values increase by 0.03–0.06 (7%) in APs, and the mean asymmetry (ASY) parameter values increase by 0.03–0.04 (6%) for the four wavelengths of 440–1020 nm. The atmospheric forcing of the APs is 2 times higher than that in other days. Contrary to the RF values, the radiative forcing efficiencies in the APs are 38% lower than those in the other days. Larger values of SSA and ASY under APs represent larger presence of more scattering aerosols and irregular-sized aerosols such as dust and non-absorbing fine mode particles. These particles are also verified by the much lower radiative forcing efficiency values. Analyses are applied on the dataset of the APs over Beijing, to group them into four discrete clusters. The two fine-size absorbing aerosols show larger mean atmospheric radiative forcing values (152.5 W/m2 and 184.5 W/m2 respectively) and forcing efficiency values (83.5 W/m2 and 108.5 W/m2 respectively). The non-absorbing aerosols and coarse aerosols exert large planetary cooling (−86.7 W/m2 and −77.3 W/m2) and low atmospheric heating effect.

Seasonal dynamics of coarse atmospheric particulate matter between 2.5 μm and 80 μm in Beijing and the impact of 2008 Olympic Games

Beijing is well known as a megacity facing severe atmospheric pollution problems. One very important kind of pollution is the high amount of particles in Beijing's atmosphere. Numerous studies investigated the dynamics of fine particles smaller 10 μm. Less information is available on the coarse particle fraction larger 10 μm, although geogenic dusts, which often are composed by those coarser particles, frequently affect the air quality in Beijing. Therefore, systematic sampling and analysis of size fractionated particulate matter between 2.5 and 80 μm was performed in Beijing from April 2005 till October 2009. Atmospheric particles were collected in the North-West of Beijing using a cost-effective passive sampling method called Sigma-2. Altogether, 200 weeks could be analysed and assessed. Concentrations and size distribution of atmospheric coarse particles were determined by automated microscopic single particle analysis. Seasonal variability of the total mass of different size fractions was identified as follows: spring > winter > autumn > summer. High concentrations of transparent mineral particles indicate the activity of geogenic sources in spring and winter time, due to asian dust events and resuspension of soil from local bare land during dry and windy periods. The percentage of opaque particle components differs seasonally with relatively high values in winter, confirming combustion of fossil fuels for heating purposes as a predominant pollution source in this season. The influence of meteorological conditions on concentrations and size distribution of atmospheric particulate matter between 2.5 and 80 μm is demonstrated for the whole sampling period. Lowest pollution by coarse aerosols occurred during the period of the 2008 Olympic Summer Games. A general trend of decreasing total coarse particle mass concentrations was observed. Due to frequently observed high total coarse particle mass concentrations of several 100 μg·m−³ it is strongly recommended to enhance research and observation regarding these air pollutants to gain a better understanding of their dynamics, health effects, well being impacts on Beijing inhabitants and the effectiveness of mitigation measures.

Retrieval of aerosol microphysical properties from AERONET photopolarimetric measurements: 1. Information content analysis

AbstractThis paper is the first part of a two‐part study that aims to retrieve aerosol particle size distribution (PSD) and refractive index from the multispectral and multiangular polarimetric measurements taken by the new‐generation Sun photometer as part of the Aerosol Robotic Network (AERONET). It provides theoretical analysis and guidance to the companion study in which we have developed an inversion algorithm for retrieving 22 aerosol microphysical parameters associated with a bimodal PSD function from real AERONET measurements. Our theoretical analysis starts with generating the synthetic measurements at four spectral bands (440, 675, 870, and 1020 nm) with a Unified Linearized Vector Radiative Transfer Model for various types of spherical aerosol particles. Subsequently, the quantitative information content for retrieving aerosol parameters is investigated in four observation scenarios, i.e., I1, I2, P1, and P2. Measurements in the scenario (I1) comprise the solar direct radiances and almucantar radiances that are used in the current AERONET operational inversion algorithm. The other three scenarios include different additional measurements: (I2) the solar principal plane radiances, (P1) the solar principal plane radiances and polarization, and (P2) the solar almucantar polarization. Results indicate that adding polarization measurements can increase the degree of freedom for signal by 2–5 in the scenario P1, while not as much of an increase is found in the scenarios I2 and P2. Correspondingly, smallest retrieval errors are found in the scenario P1: 2.3% (2.9%) for the fine‐mode (coarse‐mode) aerosol volume concentration, 1.3% (3.5%) for the effective radius, 7.2% (12%) for the effective variance, 0.005 (0.035) for the real‐part refractive index, and 0.019 (0.068) for the single‐scattering albedo. These errors represent a reduction from their counterparts in scenario I1 of 79% (57%), 76% (49%), 69% (52%), 66% (46%), and 49% (20%), respectively. We further investigated those retrieval errors over a variety of aerosol loading and fine‐/coarse‐mode prevalence, which indicates that observations in scenario P1 can yield the retrieval of refractive index and single‐scattering albedo for both fine and coarse aerosol modes, when aerosol optical depth at 440 nm is larger than 0.2 and 870/1020 nm Ångström exponent ranges between 0.7 and 1.6.

Aerosol Type Identification Using PARASOL Multichannel Polarized Data

AbstractPARASOL (Polarization & Anisotropy of Reflectances for Atmospheric Sciences coupled with Observations from a Lidar) multi-channel and multi-directional polarized data for different aerosol types were compared. The PARASOL polarized radiance data at 490 nm, 670 nm, and 865 nm increased with aerosol optical thickness (AOT) for fine-mode aerosols; however, the polarized radiances at 490 nm and 670 nm decreased as AOT increased for coarse dust aerosols. Thus, the variation of the polarized radiance with AOT can be used to identify fine or coarse particle-dominated aerosols. Polarized radiances at three wavelengths for fine- and coarse-mode aerosols were analyzed and fitted by linear regression. The slope of the line for 670 nm and 490 nm wavelength pairs is less than 0.35 for dust aerosols. However, the value for fine-mode aerosols is greater than 0.60. The Support Vector Machine method (SVM) based on 12 vector features was used to discriminate clear sky, coarse dust aerosols, fine-mode aerosols, and ...