New approach using lidar measurements to characterize spatiotemporal aerosol mass distribution in an underground railway station in Paris

For the first time eye safe lidar measurements were performed at 355 nm simultaneously to in situ measurements in an underground station so as to test the potential interest of active remote sensing measurements to follow the spatiotemporal evolution of aerosol content inside such a confined microenvironment. The purpose of this paper is to describe different methods enabling the conversion of lidar-derived aerosol extinction coefficient into aerosol mass concentrations (PM_2.5 and PM₁₀). A theoretical method based on a well marked linear regression between mass concentrations simulated from the size distribution and extinction coefficients retrieved from Mie calculations provides averaged mass to optics' relations over the campaign for traffic (6.47 × 10⁵ μg m^?2) or no traffic conditions (3.73 × 10⁵ μg m^?2). Two empirical methods enable to significantly reduce CPU time. The first one is based upon the knowledge of size distribution measurements and scattering coefficients from nephelometer and allows retrieving mass to optics' relations for well determined periods or particular traffic conditions, like week-ends, with a good accuracy. The second method, that is more direct, is simply based on the ratio between TEOM concentrations and extinction coefficients obtained from nephelometer. This method is easy to set up but is not suitable for nocturnal measurements where PM stabilization time is short. Lidar signals thus converted into PM concentrations from those approaches with a fine accuracy (30%) provide a spatiotemporal distribution of concentrations in the station. This highlights aerosol accumulation in one side of the station, which can be explained by air displacement from the tunnel entrance. Those results allow expecting a more general use of lidar measurement to survey indoor air quality.     

Properties and sources of individual particles and some chemical species in the aerosol of a metropolitan underground railway station

Aerosol samples in PM_10–2.0 and PM_2.0 size fractions were collected on the platform of a metropolitan underground railway station in central Budapest. Individual aerosol particles were studied using atomic force microscopy, scanning electron microscopy and transmission electron microscopy with energy-dispersive X-ray spectrometry and electron diffraction. The bulk aerosol samples were investigated by ⁵⁷Fe Mössbauer spectroscopy, and they were subjected to chemical speciation analysis for Cr. The particles were classified into groups of iron oxides and iron, carbonates, silicates, quartz and carbonaceous debris. Electron micrographs showed that the Fe-rich particles in the PM_2.0 size fraction typically consisted of aggregates of nano-sized hematite crystals that were randomly oriented, had round shapes and diameters of 5–15 nm. In addition to hematite, a minor fraction of the iron oxide particles also contained magnetite. In addition, the PM_2.0-fraction particles typically had a rugged surface with layered or granular morphologies. Mössbauer spectroscopy suggested that hematite was a major Fe-bearing species in the PM_10–2.0 size fraction; its mass contribution to the Fe was 36%. Further constituents (ferrite, carbides and FeOOH) were also identified. The water soluble amounts of Cr for the underground railway station and city center were similar. In the PM_10–2.0 size fraction, practically all dissolved Cr had an oxidation state of three, which corresponds to ambient conditions. In the PM_2.0 size fraction, however, approximately 7% of the dissolved Cr was present as Cr(VI), which was different from that for the urban aerosol. It is suggested that the increased adverse health effects of aerosol particles in metros with respect to ambient outdoor particles is linked to the differences in the oxidation states, surface properties or morphologies.     

Time-resolved mass concentration,composition and sources of aerosol particles in a metropolitan underground railway station

Aerosol samples were collected using a stacked filter unit (SFU) for PM10-2.0 and PM2.0 size fractions on the platform of a metropolitan underground railway station in downtown Budapest. Temporal variations in the PM10 mass concentration and wind speed and direction were determined with time resolutions of 30 and 4 s using a tapered-element oscillating microbalance (TEOM) and a wind monitor, respectively. Sample analysis involved gravimetry for particulate mass, and particle-induced X-ray emission spectrometry (PIXE) for elemental composition. Diurnal variation of the PM10 mass concentration exhibited two peaks, one at approximately 07:00 h and the other at approximately 17:00 h. The mean±SD PM10 mass concentration for working hours was 155±55 μg m⁻³. Iron, Mn, Ni, Cu, and Cr concentrations were higher than in outdoor air by factors between 5 and 20, showing substantial enrichment compared to both the average crustal rock composition and the average outdoor aerosol composition. Iron accounted for 40% and 46% of the PM10-2.0 and PM2.0 masses, respectively, and 72% of the PM10 mass was associated with the PM10-2.0 size fraction. The aerosol composition in the metro station (in particular the abundance of the metals mentioned above) is quite different from the average outdoor downtown composition. Mechanical wear and friction of electric conducting rails and bow sliding collectors, ordinary rails and wheels, as well as resuspension, were identified as the primary sources. Possible health implications based on comparison to various limit values and to data available for other underground railways are discussed.     

On the relation between the size and chemical composition of aerosol particles and their optical properties

The light scattering and absorption coefficients of fine atmospheric aerosol particles were recorded in Hungary under rural conditions in 1998–1999 by an integrating nephelometer and particle soot absorption photometer, respectively. In some cases optical properties in the fine size range were compared to those in the coarse particles. Results obtained indicate, as expected, that fine particles control the scattering and absorption caused by the aerosol. In 1999 the size distribution of aerosol particles was also monitored by means of an electric low pressure impactor (ELPI). This makes it possible the study of the relationship between the number, surface and mass concentration in the size range of 0.1–1.0 μm and the optical characteristics by also considering the chemical composition of the particles.     

Organic aerosol characterization by complementary measurements of chemical bonds and molecular fragments

Organic aerosol chemical markers from normalized concentrations of independent measurements of mass fragments (using Aerosol Mass Spectrometry, AMS) are compared to bond-based functional groups (from Fourier Transform Infrared spectroscopy, FTIR) during eight field projects in the western hemisphere. Several field projects show weak correlations between alcohol group fractions and m/z 60 fractions, consistent with the organic hydroxyl groups and the fragmentation of saccharides, but the weakness of the correlations indicate chemical differences among the relationships for ambient aerosols in different regions. Carboxylic acid group fractions and m/z 44 fractions are correlated weakly for three projects, with correlations expected for aerosols dominated by di-acid compounds since their fragmentation is typically dominated by m/z 44. Despite differences for three projects with ratios of m/z 44 to m/z 57 fragments less than 10, five projects showed a linear trend between the project-average m/z 44 to m/z 57 ratio and the ratio of acid and alkane functional groups. While this correlation explains only a fraction of the fragment and bond variability measured, the consistency of this relationship at multiple sites indicates a general agreement with the interpretation of the relative amount of m/z 44 as a carboxylic acid group marker and m/z 57 as an alkane group marker.     

Columnar optical properties of tropospheric aerosol by combined lidar and sunphotometer measurements at Taipei,Taiwan

Vertical extinction profiles and columnar optical properties (optical depth, Angstrom exponent, lidar ratio, and particle depolarization) of aerosols were obtained by simultaneous measurements with a depolarization lidar and a sunphotometer at Taipei, Taiwan from February 2004 to January 2006. Columnar optical depths are high in Feb–Apr (0.61–0.75) by sunphotometer measurements. Lidar measurements show the contribution of aerosols in the free atmosphere on columnar optical depths are about 44–50% in Feb–Apr and about 26–37% in other months. Back-trajectory analyses and depolarization measurements show almost all of non-spherical aerosols originated from Northwest China which indicate Asian dusts frequently transported to Taipei from dust source regions in the free atmosphere. Aerosols with depolarization lower than 5% are found mostly originated from South China or Southeast Asia. Good correlations between columnar lidar ratio, particle depolarization, and Angstrom exponent are found for cases that columnar water vapor less than 1.5 cm. The effect of water vapor on particle depolarization is briefly discussed.     

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.     

Airborne electrical and microphysical measurements in clouds in maritime and urban environments

A study by Khemani and Ramana Murty (1973) has indicated significant increases of rainfall downwind of the urban industrial complex at Bombay during the period of increased industrialisation. In order to understand the physical processes responsible for the observed increases in rainfall, aircraft measurements of cloud electrical and microphysical parameters and of free-air temperatures were made in the maritime (upwind) and urban (downwind) regions at Bombay.The study has pointed out differences in the electrical and microphysical state of clouds in maritime and urban environments. In the maritime clouds the electric field was both positive and negative and the cloud droplet charges were positive. In urban clouds the electric field was negative and the droplet charge was also negative. The cloud condensation nuclei and the total measured droplet concentrations were higher in the urban environment. In urban clouds the droplet spectra showed a multimodal distribution and in maritime clouds it was unimodal. Also, the concentration of large droplets of diameter 50 μm and above, and the integrated cloud droplet liquid water content were more in the urban environment. The tail of the droplet spectra extended to higher sizes in urban clouds. The free air temperature in the urban environment was higher by about 1°C.     

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.     

Airborne electrical and microphysical observations in the environment of a thermal power station

Using aircraft, electrical and microphysical observations were made, on a few occasions within 15 km upwind and downwind of a thermal power station under cloud-free and in-cloud conditions. The values of the parameters measured were found to be systematically higher in the downwind region than in the upwind. Under cloud-free conditions, the concentrations of the cloud condensation nuclei and the computed cloud droplets were higher up to two times, the atmospheric electric field was higher up to seven times and the air temperature up to 2.3°C. Under in-cloud conditions, the values of the electric field and droplet charge were higher up to two times, the measured droplet concentration was higher by one and a half times, the cloud air temperature up to 1.5°C and the liquid water content up to four times. However, these differences were in general within the spatial variability found outside the plume affected area.     

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.     

Extensive aerosol optical properties and aerosol mass related measurements during TRAMP/TexAQS 2006 – Implications for PM compliance and planning

Extensive aerosol optical properties, particle size distributions, and Aerodyne quadrupole aerosol mass spectrometer measurements collected during TRAMP/TexAQS 2006 were examined in light of collocated meteorological and chemical measurements. Much of the evident variability in the observed aerosol-related air quality is due to changing synoptic meteorological situations that direct emissions from various sources to the TRAMP site near the center of the Houston-Galveston-Brazoria (HGB) metropolitan area. In this study, five distinct long-term periods have been identified. During each of these periods, observed aerosol properties have implications that are of interest to environmental quality management agencies. During three of the periods, long range transport (LRT), both intra-continental and intercontinental, appears to have played an important role in producing the observed aerosol. During late August 2006, southerly winds brought super-micron Saharan dust and sea salt to the HGB area, adding mass to fine particulate matter (PM_2.5) measurements, but apparently not affecting secondary particle growth or gas-phase air pollution. A second type of LRT was associated with northerly winds in early September 2006 and with increased ozone and sub-micron particulate matter in the HGB area. Later in the study, LRT of emissions from wildfires appeared to increase the abundance of absorbing aerosols (and carbon monoxide and other chemical tracers) in the HGB area. However, the greatest impacts on Houston PM_2.5 air quality are caused by periods with low-wind-speed sea breeze circulation or winds that directly transport pollutants from major industrial areas, i.e., the Houston Ship Channel, into the city center.     

Optical and chemical properties of marine boundary-layer aerosol around Japan determined from shipboard measurements in 2002

Shipboard measurements of the optical and chemical properties of marine boundary-layer aerosol were made around Japan over the period from 28 August to 25 September 2002. Measurements were conducted aboard the Research Vessel (R/V) Shirase along cruise tracks beginning from Yokosuka, and proceeding on to Hakodate, Sakata, Sasebo, Naha, Kure, and Yokkaichi. This paper describes the results of optical measurements using an Optical Particle Counter (OPC), an Integrating Nephelometer (IN), and a Particle Soot/Absorption Photometer (PSAP), as well as chemical analyses of water-soluble aerosol particles collected by impactor and filter systems. Coulter Multisizer measurements were used for water-insoluble aerosol particles. The complex refractive index (CRI), scattering and absorption coefficients, and size distribution of aerosols were estimated from combined measurements made using OPC, IN, and PSAP. Contrasting aerosol characteristics were observed during different stages of the cruise. Discussion on these differences focuses mainly on two legs: Leg-1 from Yokosuka to Hakodate and Leg-4 from Sasebo to Naha. Backward trajectory analyses indicate that the air sampled during Leg-1 originated from the Pacific Ocean, whereas the air sampled during Leg-4 originated from the Chinese Continent via the Korean Peninsula. For the first half of Leg-1, the number concentration was low and larger particles were relatively predominant. The real and imaginary parts of the CRI were estimated to be 1.38–1.40 and close to zero, respectively. This estimation is consistent with the results of chemical analyses, which show that the sea salt is rich in aerosols sourced from remote ocean areas. In contrast, small particles were predominant during Leg-4, and the real and imaginary parts of the CRI were estimated to be 1.52–1.59 and approximately −0.002, respectively. These findings are also consistent with chemical analyses that reveal a mixture of mineral dust and sulfate aerosol likely transported from China and Korea. The Coulter Multisizer measurements conducted during Leg-4 reveal abundant water-insoluble particles with a mode radius of 1.35 μm.     

Evaluation of an aerosol optical scheme in the chemistry-transport model CHIMERE

This paper presents an aerosol optical scheme developed in the chemistry-transport model CHIMERE dedicated to calculate optical properties of particles. Such developments are very helpful as they complement the usual validation with PM (Particulate Matter) ground-based measurements by using surface (AERONET/PHOTONS network) and satellite (MODIS) remote sensing observations. To reach this goal, Aerosol Optical Thickness (AOT), column-averaged Single Scattering Albedo (SSA) and asymmetry parameter (g) are calculated at 440 nm, 675 nm, 870 nm and 1020 nm (AERONET wavelengths) under three hypotheses on the particle mixing state (external, internally homogeneous and core-shell). Furthermore and in addition to optical calculations, an original development has been made to estimate column volume size distributions in CHIMERE, directly comparable with AERONET retrievals. Comparisons between simulations and observations are made over Western Europe for the year 2003 but also for one specific case focused on ammonium nitrate aerosols. Observed AOT display a seasonal cycle (with highest values during summer) rather well reproduced by the model but biases with observational data have been found depending on seasons. In fall, winter and early spring, modeled AOT values agree well with AERONET retrievals with small negative biases. Focus on a pollution episode of ammonium nitrate origin during March 2003 reveals that CHIMERE is able to well reproduce the fine mode volume size distribution retrieved by AERONET, leading to good agreements between modeled and observed AOT. In late spring and summer, AERONET AOT values are underpredicted by the model, which could be due to uncertainties in modeling secondary species.     

Radiative heating rates and some optical properties of the St. Louis aerosol,as inferred from Aircraft measurements

Radiative heating rates were determined from measurements made aboard an aircraft flying within and above the St. Louis boundary layer during the Regional Air Pollution Study (RAPS; 1975–1976). In the mean, heating rates tor both solar and infrared radiation were found to diminish steadily from a maximum near the surface to nearly zero above the mixing layer. Similarly, there was a mean decrease in large particle aerosol concentrations and in extinction coefficient with height to insignificant values above the mixing layer. Over the entire mixing depth, there was an average net solar warming and an average net longwave cooling due to the presence of aerosol. When normalized for a 24 h period the solar warming was found to be very slightly less than the magnitude of the long-wave cooling, although the former somewhat exceeded the latter during midday. Derived values of the asymmetry parameter and single scattered albedo were large, the value for each averaging close to 0.9. The ratio of backscatter to absorption for the aerosol was approximately unity.Thus the arosol was not a strongly absorbing material and. consequently, the aerosol healing or cooling rates were not very large within the St. Louis mixing layer and the total (solar + IR) effect of the temperature changes on the atmospheric motions were likely to have been insignificant.     

Optical and microphysical properties of severe haze and smoke aerosol measured by integrated remote sensing techniques in Gwangju,Korea

Aerosol optical and microphysical parameters from severe haze events observed in October 2005 at Gwangju, Korea (35.10°N, 126.53°E) were determined from the ground using a multi-wavelength Raman lidar, a sunphotometer, and a real-time carbon particle analyzer and from space using satellite retrievals. Two different aerosol types were identified based on the variability of optical characteristics for different air mass conditions. Retrievals of microphysical properties of the haze from the Raman lidar indicated distinct light-absorbing characteristics for different haze aerosols originating from eastern and northern China (haze) and eastern Siberia (forest-fire smoke). The haze transported from the west showed moderately higher absorbing characteristics (SSA = 0.90 ± 0.03, 532 nm) than from the northern direction (SSA = 0.96 ± 0.02). The organic/elemental carbon (OC/EC) ratio varied between 2.5 ± 0.4 and 4.1 ± 0.7.     

Correction in aerosol mass concentration measurements with humidity difference between ambient and instrumental conditions

The influence of humidity is considered on the concentration of the suspended particulate matter (SPM) measured with a β-ray counter. The humidity condition inside a small observatory where the counter is located is, in general, different from the ambient condition outside the observatory. From the measured values, the ambient SPM concentration is derived considering the hygroscopic effect of common aerosol species of sea salt (SS), (NH₄)₂SO₄, NH₄NO₃ and NaNO₃. In a case study conducted during September 2005, temperature and humidity were measured both inside and outside the observatory. The average value of the relative humidity is 48% for inside and 78% for outside, resulting in approximately 53% larger SPM mass concentration after the correction. Accordingly, the value of mass extinction efficiency, which is given by the ratio between the optically measured extinction coefficient and the mass concentration, becomes lower after the correction.     

Contrasting seasonal pattern between ground-based PM2.5 and MODIS satellite-based aerosol optical depth (AOD) at an urban site in Hanoi,Vietnam

Environmental Science and Pollution Research - This study investigated the seasonal variations of the ground-based PM2.5 concentration measured at an urban site and Terra MODIS satellite-based...