Long-term assessment of particulate matter using CHIMERE model

Particulate matter (PM) and aerosols have became a critical pollutant and object of several research applications, due to their increasing levels, especially in urban areas, causing air pollution problems and thus effects on human health. The main purpose of this study is to perform a first long-term air quality assessment for Portugal, regarding aerosols and PM pollution. The CHIMERE chemistry-transport model, forced by the MM5 meteorological fields, was applied over Portugal for 2001 year, with 10 km horizontal resolution, using an emission inventory obtained from a spatial top-down disaggregation of the 2001 national inventory database. The evaluation model exercise shows a model trend to overestimate particulate pollution episodes (peaks) at urban sites, especially in winter season. This could be due to an underprediction of the winter model vertical mixing and also to an overestimation of PM emissions. Simulated inorganic components (ammonium and sulfate) and secondary organic aerosols (SOA) were compared to measurements taken at Aveiro (northwest coast of Portugal). An underestimation of the three components was verified. However, the model is able to predict their seasonal variation. Nevertheless, as a first approach, and despite the complex topography and coastal location of Portugal affected by sea salt natural aerosols emissions, the results obtained show that the model reproduces the PM levels, temporal evolution, and spatial patterns. The concentration maps reveal that the areas with high PM values are covered by the air quality monitoring network.     

Long-term simulations of photo oxidant pollution over Portugal using the CHIMERE model

This work examines the performance of the CHIMERE photochemical model in simulating ozone and nitrogen dioxide in Portugal over a long-term summer period. The analysis focuses on comparisons against the available measurements during the 2001 summer season. The meteorological forcing of the model is given by the European Centre for Medium-Range Weather Forecasts (ECMWF), and the emission inventory used was obtained with a top-down methodology updated for the simulation year.Despite the coarse resolution of the meteorological data, the complex topography and coastal location of Portugal, the results obtained show that the modelling system is able to reproduce the nitrogen dioxide and ozone episodes that occurred during the simulated summer period. Mean error and correlation improve when considering the sum of photo oxidant instead of individual pollutants, indicating that a significant part of the model error is due to either the lack of representativeness of monitoring stations or to inaccuracies in the emission inventory.     

Evaluation of the MODIS aerosol optical depth retrieval over different ecosystems in China during EAST-AIRE

The accuracy of the Moderate Resolution Imaging Spectroradiometer's (MODIS) aerosol products is still uncertain in China, due to a lack of validation by long-term and large-scale ground-based observations. In this paper, the MODIS aerosol optical depth (AOD) product is evaluated using Chinese Sun Hazemeter Network (CSHNET) data as ground truths over different ecological regions in China during the East Asian Study of Tropospheric Aerosols—an International Regional Experiment (EAST-AIRE). The evaluation results show very large differences in the MODIS AOD retrieval between different ecosystems and geographic locations. The most agreement between the MODIS data and that of the CSHNET was in farmland sites in central-southern China, where high correlation (R>0.82) and large percentages (R2>72%) within the expected error lines issued by NASA were found. In temperate forest, coastal regions, and northeast and central farmlands, there appeared moderate agreement, with R∼0.64–0.80 and 45–73% of retrieval data falling within the expected errors. The poorest agreement existed in northern arid and semiarid regions, in remote northeast farmlands, in the Tibetan and Loess Plateau, and in southern forests, with 13–54% of retrieval data falling within the expected errors. In addition, the MODIS AOD retrievals were significantly overestimated in the northern arid and semiarid regions and underestimated in remote northeast farmlands and southern forests.     

A size-segregated particle dry deposition scheme for an atmospheric aerosol module

A parameterization of particle dry deposition has been developed for the Canadian Aerosol Module (CAM).This parameterization calculates particle dry deposition velocities as a function of particle size and density as well as relevant meteorological variables. It includes deposition processes, such as, turbulent transfer, Brownian diffusion, impaction, interception, gravitational settling and particle rebound. Particle growth under humid conditions is also considered. Sensitivity tests show that the parameterization provides deposition velocities comparable with recent field observations, especially for sub-micron particles. The present parameterization has also been evaluated using two empirical bulk resistance models, which were originally developed from field observations. The present parameterization has been implemented in CAM, with meteorological input provided by the Canadian Regional Climate Model (RCM) to the eastern North America. A comparison of the modelled dry deposition velocities to a variety of recent measurements that have been reported in the literature demonstrated that the current parameterization produces reasonable results. The main improvement of the current parameterization compared to earlier size-dependent particle dry deposition models is that the current one produces more realistic deposition velocities for sub-micron particles and agrees better with recently published field measurements.     

Modelling aerosol number distributions from a vehicle exhaust with an aerosol CFD model

Vehicular traffic contributes significantly to the aerosol number concentrations at the local scale by emitting primary soot particles and forming secondary nucleated nanoparticles. Because of their potential health effects, more attention is paid to the traffic induced aerosol number distributions.The aim of this work is to explain the phenomenology leading to the formation and the evolution of the aerosol number distributions in the vicinity of a vehicle exhaust using numerical modelling. The emissions are representative of those of a light-duty diesel truck without a diesel particle filter. The atmospheric flow is modelled with a computational fluid dynamics (CFD) code to describe the dispersion of pollutants at the local scale. The CFD code, coupled to a modal aerosol model (MAM) describing the aerosol dynamics, is used to model the tailpipe plume of a vehicle with emissions corresponding to urban driving conditions. On the basis of available measurements in Schauer et al. (1999), three surrogate species are chosen to treat the semi-volatile organic compounds in the emissions.The model simulates the formation of the aerosol distribution in the exhaust plume of a vehicle as follows. After emission to the atmosphere, particles are formed by nucleation of sulphuric acid and water vapour depending strongly on the thermodynamic state of the atmosphere and on the dilution conditions. The semi-volatile organic compounds are critical for the rapid growth of nanoparticles through condensation. The semi-volatile organic compounds are also important for the evolution of primary soot particles and can contribute substantially to their chemical composition.The most influential parameters for particle formation are the sulphur fuel content, the semi-volatile organic emissions and also the mass and initial diameter of the soot particles emitted. The model is able to take into account the complex competition between nucleation, condensation and dilution, as well as the interactions among the different aerosol modes. This type of model is a useful tool to better understand the dynamics leading to the formation of traffic induced aerosol distributions. However, some key issues such as the turbulence in the exhaust plume and in the wake of the car, the magnitude and chemical composition of semi-volatile organic emissions and the possible nucleation of organic species need to be investigated further to improve our understanding of ultrafine particle formation.     

The sensitivity of the CHIMERE model to emissions reduction scenarios on air quality in Northern Italy

The sensitivity of the CHIMERE model to emission reduction scenarios on particulate matter PM2.5 and ozone (O₃) in Northern Italy is studied. The emissions of NO_x, PM2.5 SO₂, VOC or NH₃ were reduced by 50% for different source sectors for the Lombardy region, together with 5 additional scenarios to estimate the effect of local measures on improving the air quality for the Po valley area. Firstly, we evaluate the model performance by comparing calculated surface aerosol concentrations for the standard case (no emission reductions) with observations for January and June 2005. Calculated monthly mean PM10 concentrations are in general underestimated. For June, modelled PM10 concentrations slightly overestimate the measurements. Calculated monthly mean SO₄, NO₃^?, NH₄⁺ concentrations are in good agreement with the observations for January and June. Secondly, the model sensitivity of emission reduction scenarios on PM2.5 and O₃ calculated concentrations for the Po valley area is evaluated. The most effective scenarios to abate PM2.5 concentration are based on the SNAP2 (non-industrial combustion plants) and SNAP7 (road traffic) sectors, for which the NO_x and PM2.5 emissions are reduced by 50%. The number of days that the 2015 PM2.5 limit value of 25 μg m^?3 in Milan is exceeded by reducing primary PM2.5 and NO_x emissions for SNAP2 and 7 by 50%, does not change in January when compared to the standard case for the Milan area. It appears that 40% of the PM2.5 concentration in the greater Milan area is caused by the emissions surrounding the Lombardy region and from the model boundary conditions.This study also showed that a more effective pollutant reduction (emissions) per ton of pollutant reduced (concentrations) for the greater Milan area is obtained by reducing the primary PM2.5 emissions for SNAP7 by 50%. The most effective scenario on PM2.5 decrease for which precursor emissions are reduced is achieved by reducing SO₂ emissions by 50% for SNAP7.Our study showed that during summer time, the largest reductions in O₃ concentrations are achieved for SNAP7 emission reductions, when volatile organic compounds (VOCs) are reduced by 50%.     

Influence of aerosol optical properties on surface temperatures computed with a radiative-convective model

Calculations on the effects of aerosols (i.e. suspended particles) have been shown to lead to heating or cooling in atmospheric models, depending on the size distribution of the aerosols, the height of the aerosol layer, and nature of the underlying surface. This work reports a study of the influence of different aerosol optical properties on surface temperature.The calculated surface temperatures are shown to be relatively insensitive to the real part of the refractive index and to the aerosol size distribution assumed. The sensitivity to surface albedo is similar for three aerosol types characteristic of marine aerosols, continental aerosols and stratospheric aerosols. For an aerosol composed of limonite or silicate, an increase in the absorptive component of the refractive index n₂ increases the calculated surface temperature for a constant global average airborne aerosol density as shown below. Surface albedo Surface temperature change for 0.1 increase in n₂ 0.07 (oceans) 0.4 K 0.60 (snow and ice) 1.0 K It can be seen that the heating is increased 2–3 times as the surface albedo is increased by an order of magnitude. A 0.1 increase in n₂, corresponds very roughly to a factor of two increase in the percentage of solar absorption by an average particle.It would be useful to be able to determine from the results of this study, if global average aerosols heat or cool the atmosphere. Unfortunately our knowledge of the actual global aerosol distribution, optical properties and optical density is inadequate to make this determination.     

Transferring the heterogeneity of surface emissions to variability in pollutant concentrations over urban areas through a chemistry-transport model

Horizontal resolution of grid-based chemistry-transport models is limited to a few square kilometers which has been proved insufficient for assessing human exposure and health impact. We propose a general methodology, applicable on any kind of grid-based air-quality model, that combines subgrid scale information on emission and land-use data in order to disaggregate the grid-averaged emission flux into a set of source-specific components (subgrid-environments). Different subgrid concentrations are calculated inside each one of these environments providing a direct estimate of pollutant variability along with the ‘standard’ grid-averaged model output. The method was first validated over a controlled emissions case by comparing concentrations modeled in the subgrid-environments with concentrations modeled directly at higher model resolution and next over a real case-study, where subgrid concentrations were compared with monitor data from sites representing different types of urban environments (i.e. roads and residential blocks). It was shown that the method is capable to yield accurate estimates of small scale pollutant variability.     

Trends in aerosol optical depth for cities in India

Recent analysis of trends in global short-wave radiation measured with pyranometers in major cities in India support a decrease in solar radiation in many of those cities since 1990. Since direct and diffuse radiation measurements include cloud effects, spring and summer dust and the variable summer monsoon rains, we concentrate in this paper on wintertime (November–February) aerosol optical depth measurements. The aerosol optical depth is derived from cloud-free turbidity measurements beginning in the 1960s and more recent sun photometer direct aerosol optical depth measurements. We compare the sun photometer derived trends with the pyranometer-derived trends using a radiative transfer model. These results are then compared to total ozone mapping spectrometer (TOMS) satellite-derived regional aerosol optical depths from 1980 to 2000. The results show that inclusion of the earlier turbidity measurements helps to establish an increasing regional turbidity trend. However, most of the increasing trend is confined to the larger cities in the Ganges River Basin of India (mainly Calcutta and New Delhi) with other cities showing a much less increase. Regional satellite data show that there is an increasing trend in aerosol off the coast of India and over the Ganges River Basin. The increase over the Ganges River Basin is consistent with population trends over the region during 1980–2000.     

Link between aerosol optical,microphysical and chemical measurements in an underground railway station in Paris

Measurements carried out in Paris Magenta railway station in April–May 2006 underlined a repeatable diurnal cycle of aerosol concentrations and optical properties. The average daytime PM₁₀ and PM_2.5 concentrations in such a confined space were approximately 5–30 times higher than those measured in Paris streets. Particles are mainly constituted of dust, with high concentrations of iron and other metals, but are also composed of black and organic carbon. Aerosol levels are linked to the rate at which rain and people pass through the station. Concentrations are also influenced by ambient air from the nearby streets through tunnel ventilation. During daytime approximately 70% of aerosol mass concentrations are governed by coarse absorbing particles with a low Angström exponent (～0.8) and a low single-scattering albedo (～0.7). The corresponding aerosol density is about 2 g cm^?3 and their complex refractive index at 355 nm is close to 1.56–0.035 i. The high absorption properties are linked to the significant proportion of iron oxides together with black carbon in braking systems. During the night, particles are mostly submicronic, thus presenting a greater Angström exponent (～2). The aerosol density is lower (1.8 g cm^?3) and their complex refractive index presents a lower imaginary part (1.58–0.013 i), associated to a stronger single-scattering albedo (～0.85–0.90), mostly influenced by the ambient air. For the first time we have assessed the emission (deposition) rates in an underground station for PM₁₀, PM_2.5 and black carbon concentrations to be 3314 ± 781(?1164 ± 160), 1186 ± 358(?401 ± 66) and 167 ± 46(?25 ± 9) μg m^?2 h^?1, respectively.     

Seasonal variability of aerosol optical properties over Beijing

The knowledge of aerosol properties at local and regional scale is important in understanding of the global climate change. In this study, the aerosol optical properties over Beijing have been presented from the Aerosol Robotic Network (AERONET) measurements during 2002–2007. The aerosol optical depth (AOD) showed a distinct seasonal variation with high values in spring (March–May) and summer (June–August). The magnitude of Ångström exponent (α) was found to be relatively high throughout the year and the highest values (1.27) occurred in summer and the lowest (1.0) in spring. The water vapor retrieved from AERONET was found to be highest (2.60 cm) in summer. The fine modes of aerosol volume size distributions showed the highest peak around radius 0.15 μm in spring, autumn (September–November) and winter (December–February), and radius 0.19 μm in summer. The coarse modes showed the maxima peak at radius 3.0 μm in all seasons. The asymmetry factor (g) has considered as 0.65 at 440, 675, 870 and 1020 nm over Beijing in climate and radiation models. The average values of the single scattering albedo (SSA) at the four wavelengths were taken as 0.89, 0.91, 0.87 and 0.86 in spring, summer, autumn and winter, respectively. Both real and imaginary parts of the refractive index showed low wavelength dependence. The highest averages of real (1.52) and imaginary parts (0.0165) were found in spring and winter respectively in the wavelength range of 440–1020 nm. The aerosol properties over Beijing were found to highly dependent on season, and changes in aerosol properties were mainly attributed to the presence of dust as the main component during the spring season and the dominance of anthropogenic pollutants during the winter season.     

An absorption model of the gas/aerosol partitioning involved in the formation of secondary organic aerosol

A partitioning model is developed to allow the modeling of the dynamics of secondary organic aerosol (SOA) formation. The gas/aerosol partitioning is assumed to be governed by equilibrium partitioning into an absorptive, well-mixed liquid (or at least amorphous) organic matter (om) phase. The model is represented using a set of coupled linear equations. It may be especially applicable when photochemical smog is being formed in the summer. The model permits (indeed, it requires) partitioning of a given compound i to occur even when i is present at a level below its saturation vapor pressure. During early periods of SOA formation, to determine the partitioning for each compound of interest, the model must be solved iteratively for each time and location of interest. Iteration is required because the partitioning is assumed to be governed by mole fraction concentrations in the om phase, and because prior to solving the problem, one does not know the total number of mols of condensed compounds in the om phase. During later stages of SOA formation, if the amount and general composition of the SOA begin to become constant, the partitioning coefficient of each of the compounds will also stabilize, and an iterative solution will be less needed.     

A preliminary study on the correlation between TOMS aerosol index and ground-based measured aerosol optical depth

The aim of this work is to study the correlation between ground-based measured aerosol optical depth (AOD) and TOMS Aerosol Index. For this reason, two AOD data-sets have been analysed. The first set of measurements has been obtained in a desert plateau in Namibia during July 1998, while the second one has been collected in Tito Scalo (Italy), a very small industrial zone surrounded by a large rural area, in June–July 2000. The AOD has been computed in the spectral range 400–870 nm with a resolution of 3 nm by measuring the direct solar irradiance. The used spectroradiometer is an Optical Spectrum Analyser, equipped with a continuously rotating diffraction grating. Successively, a correlation between the Earth Probe TOMS Aerosol Index, whose definition uses backscattered radiances at 331 and 360 nm, and the AOD in the visible range was searched for. A satisfying correlation was found, whose Pearson correlation coefficient R² values range from 0.64 to 0.91.     

Evaluation of secondary organic aerosol formation in winter

Three different methods are used to predict secondary organic aerosol (SOA) concentrations in the San Joaquin Valley of California during the winter of 1995–1996 [Integrated Monitoring Study, (IMS95)]. The first of these methods estimates SOA by using elemental carbon as a tracer of primary organic carbon. The second method relies on a Lagrangian trajectory model that simulates the formation, transport, and deposition of secondary organic aerosol. The model includes a recently developed gas–particle partitioning mechanism. Results from both methods are in good agreement with the chemical speciation of organic aerosol during IMS95 and suggest that most of the OC measured during IMS95 is of primary origin. Under suitable conditions (clear skies, low winds, low mixing heights) as much as 15–20 μg C m⁻³ of SOA can be produced, mainly due to oxidation of aromatics. The low mixing heights observed during the winter in the area allow accumulation of SOA precursors and the acceleration of SOA formation. Clouds and fog slow down the production of secondary compounds, reducing their concentrations by a factor of two or three from the above maximum levels. In addition, it appears that there is significant diurnal variation of SOA concentration. A strong dependence of SOA concentrations on temperature is observed, along with the existence of an optimal temperature for SOA formation.     

New particle formation in the presence of an aerosol

Condensable molecules generated in the gas phase by chemical reaction can either form new panicles or condense on existing aerosol particles. Experiments were carried out to study the effect of a preexisting aerosol on aerosol dynamics in such systems. Secondary sulfate aerosol was produced by photochemical reactions in the SO₂-NO_x-propylene system. A new theory which predicts the rate at which new particles of a given size are formed is also presented. Scavenging of molecular clusters by surrounding aerosols can be important, and is incorporated in the theory. Measured rates of new particle formation are compared with predicted rates, taking into account the minimum particle size detected experimentally. Agreement between theory and experiment is within experimental error. Based on the theoretical analysis, a criterion for determining whether or not new particle formation is important in such systems is established.     

Study on the aerosol optical properties and their relationship with aerosol chemical compositions over three regional background stations in China

The special and temporal characteristics of aerosol optical depth (AOD) and Angstrom wavelength exponent (Alpha) and their relationship with aerosol chemical compositions were analyzed by using the data of CE318 sun-photometer and aerosol sampling instruments at Lin'an, Shangdianzi and Longfengshan regional atmospheric background stations. Having the highest AOD among the three stations, Lin'an shows two peaks in a year. The AOD at Shangdianzi station shows a single annual peak with an obvious seasonal variation. The AOD at Longfengshan station has obvious seasonal variation which peaks in spring. The Alpha analysis suggests that the aerosol sizes in Lin'an, Longfengshan and Shangdianzi change from fine to coarse categories. The relationship between the aerosol optical depths of the Lin'an and Longfengshan stations and their chemical compositions is not significant, which suggests that there is not a simple linear relationship between column aerosol optical depth and the near surface chemical compositions of atmospheric aerosols. The aerosol optical depth may be affected by the chemical composition, the particle size and the shape of aerosol as well as the water vapor in the atmosphere.     

Signs of a negative trend in the MODIS aerosol optical depth over the Southern Balkans

A negative trend is being revealed in the MODIS aerosol optical depth [AOD] observed over the Southern Balkan/Eastern Mediterranean region. Collection 005 MODIS/Terra and MODIS/Aqua AOD at 470 nm measurements were evaluated against Brewer ground-based measurements over Thessaloniki, Greece and CIMEL ground-based measurements of AOD over Heraklion, Crete. A detailed study of the monthly, seasonal and inter-annual variability of the MODIS/Terra and MODIS/Aqua AOD values over selected locations around the Balkan Peninsula showed that the higher mean AOD values occurred in the spring and summer months, whereas the lowest were found in the winter-time. For all seasons, the highest AODs were observed for the northern-most latitudes with a marked decrease towards the southern-most sites. A statistically significant decreasing trend in aerosol load in the region over all sites as derived from the MODIS/Terra measurements gave the highest per annum change seen for the summer months to be ?4.09 ± 2.34%, and the lowest for the winter months as ?2.55 ± 4.36%, which also shows the higher variability.     

Correlation between PM concentrations and aerosol optical depth in eastern China

Using one year of Aerosol Optical Depth (AOD) derived from Moderate Resolution Imaging Spectroradiometer (MODIS) on the Terra satellite and particular matter (PM) contents measured at eleven sites located mostly in the eastern China in 2007, the relationship between columnar AOD and hourly and daily average (DA) PM were established. The peak AOD observed from MODIS was generally consistent with the surface PM measurements in eastern China, where Zhengzhou had the maximum annual mean PM₁₀ of 182.1 μg m^?3, while Longfengshan had the minimum annual mean of 38.1 μg m^?3. Ground level observations indicated that PM concentration varies widely across different regions, which was mainly due to the difference in weather conditions and anthropogenic emissions. The coarse particles accounted for the main air pollution in Zhengzhou and Benxi whiles the fine particles, however, were the main constituents in other sites. Results showed that MODIS AOD (averaged over the box of 5 × 5 and 3 × 3 pixels) had a better positive correlation with the coincident hourly average (HA) PM concentration than with DA due to diurnal variation in PM mass measurements. After correcting AOD for relative humidity (RH), the correlation did not improve significantly, suggesting that the RH was not the main factor affecting the correlation of PM with AOD. The statistical regression analysis between MODIS AOD and PM mass suggested that the satellite-derived AOD is a useful tool for mapping PM distribution over large spatial domains.