The Evolution of Visibility Deterioration and Aerosol Spectra in the St. Louis Urban Plume

Under the auspices of Project METROMEX, studies of visibility de-teoration downwind of St. Louis were conducted during July-August 1974-1975. Estimates of horizontal visual range, standard meteorological data, and aerosol characteristics within the mixing layer were acquired upwind, over, and downwind of the metropolitan area by means of airborne transects. Aerosol number, surface, and volume distributions for particles between 0.025-2.5 µm were generated from the airborne measurement of Aitken nucleus concentrations, cloud condensation nuclei, and aerosols detected in situ with optical probes. Visibility reduction amounting to 50% of prevailing regional upwind visibilities consistently occurs at a distance corresponding to 2-3 hours travel time downwind for an air parcel moving with the mean transport wind. The regions of visibility minimum do not coincide with locations of maximum Aitken nucleus concentrations, but rather correspond in space and time to increased values of cloud condensation nuclei and increased numbers of particles in the 0.1-2.5 µm diameter range. Comparisons of observed aerosol evolution with similar laboratory studies suggest that most of the light scattering aerosols are of secondary origin.     

The Nature and Sources of Haze in the Shenandoah Valley/Blue Ridge Mountains Area

In order to investigate the nature and sources of regional haze, the General Motors mobile Atmospheric Research Laboratory was used in the summer of 1980 to monitor ambient air quality in the Shenandoah Valley of northern Virginia. On the average, 92% of the total light extinction was due to scattering by particles; the remainder was due to scattering by gases and absorption by gases and particles. Sulfate aerosols were the most Important visibility-reducing species. Averaging 55% of the fine participate mass, sulfates (and associated water) accounted for 78% of the total light extinction. The second most abundant fine particulate, accounting for 29% of the fine mass, was carbon—most of which was organic. Most of the remaining particulate mass and extinction were due to crustal materials. It is estimated that 78–86% of the total light extinction was caused by anthropogenic aerosol, most of which originated in major source areas of the midwest.     

On the optical properties of the polluted Athens atmosphere,during May 1995

Using ground-based spectral solar extinction data taken over the Athens atmosphere, reduced (total minus Rayleigh) and aerosol (Angstrom) spectral optical depths of the atmosphere, have been retrieved, under different polluted conditions. The results suggest that the optical depth, on days with relatively low pollution, exhibits slight variation with wavelength denoting that aerosols deplete all wavelengths almost equally. In contrast, under dense pollution, small particles scattering and trace gases absorption, are the dominant processes, resulting in steeper optical depth’s slopes, mainly in the ultraviolet domain. The Angstrom’s parameters β and α were determined through a least-squares fitting method. The turbidity β coefficient always shows a temporal pattern with high values in the morning and afternoon and low values midday.     

Relationship of extinction coefficient, air pollution, and meteorological parameters in an urban area during 2007 to 2009

Light extinction, which is the extent of attenuation of light signal for every distance traveled by light in the absence of special weather conditions (e.g., fog and rain), can be expressed as the sum of scattering and absorption effects of aerosols. In this paper, diurnal and seasonal variations of the extinction coefficient are investigated for the urban areas of Tehran from 2007 to 2009. Cases of visibility impairment that were concurrent with reports of fog, mist, precipitation, or relative humidity above 90 % are filtered. The mean value and standard deviation of daily extinction are 0.49 and 0.39 km^?1, respectively. The average is much higher than that in many other large cities in the world, indicating the rather poor air quality over Tehran. The extinction coefficient shows obvious diurnal variations in each season, with a peak in the morning that is more pronounced in the wintertime. Also, there is a very slight increasing trend in the annual variations of atmospheric extinction coefficient, which suggests that air quality has regressed since 2007. The horizontal extinction coefficient decreased from January to July in each year and then increased between July and December, with the maximum value in the winter. Diurnal variation of extinction is often associated with small values for low relative humidity (RH), but increases significantly at higher RH. Annual correlation analysis shows that there is a positive correlation between the extinction coefficient and RH, CO, PM₁₀, SO₂, and NO₂ concentration, while negative correlation exists between the extinction and T, WS, and O₃, implying their unfavorable impact on extinction variation. The extinction budget was derived from multiple regression equations using the regression coefficients. On average, 44 % of the extinction is from suspended particles, 3 % is from air molecules, about 5 % is from NO₂ absorption, 0.35 % is from RH, and approximately 48 % is unaccounted for, which may represent errors in the data as well as contribution of other atmospheric constituents omitted from the analysis. Stronger regression equation is achieved in the summer, meaning that the extinction is more predictable in this season using pollutant concentrations.     

Optical properties of tropospheric aerosols based on measurements of lidar,sun-photometer,and visibility at Chung-Li (25°N, 121°E)

We have used lidar, sun-photometer, and the visibility measurements to investigate the optical properties of aerosols in the lower air. The observations were performed at Chung-Li (25°N, 121°E) during the period of February 2002–May 2004. Combined data indicate that 40–50% of total extinction in the column air contributed by aerosols in 1–5 km. Seasonally, spring time extinction is higher than other seasons. However, the summer extinction is the highest below about 2 km. Sources for aerosols are determined by using satellite imageries and back trajectories. Aerosols backscattering ratio and depolarization ratio are then categorized based on their sources. We found that the largest optical thickness is biomass burning aerosols originated in Southeast Asia. The aerosols generated from Northern China transported by the high-pressure system in spring are usually dust with depolarization ratios in the range of 0.1–0.3, but varying backscattering coefficients. The aerosols optical characteristics will be useful for future understanding about their environmental and climate effects.     

Seasonal characteristics of chemically apportioned aerosol optical properties at Seoul and Gosan,Korea

Seasonal variations of aerosol optical properties in Seoul (polluted urban site) and Gosan (coastal background site), Korea, with an emphasis on the relative humidity were investigated using ground-based aerosol measurements and optical model calculations. The mass fraction of elemental carbon was 9–20%, but the optical contribution of these particles to light extinction was higher, up to 33–55% in Seoul. In Gosan, the contribution of non-sea-salt water-soluble aerosols on extinction was 81–93% due to the high mass fraction of these particles. Based on daily MODIS datasets, our analysis showed that the aerosol optical depths at Seoul and Gosan were highest in spring due to the influence of dust particles. The aerosol water content at Gosan, calculated using a thermodynamic equilibrium model, was higher than that at Seoul; this was attributed to the high relative humidity and high fraction of water-soluble aerosols at Gosan. At Seoul, despite abundant water vapors in summer, the possibility of hygroscopic growth of water-soluble aerosols was not more significant than that at Gosan.     

A case study of optical and chemical ground apportionment for urban aerosols in Thessaloniki

Urban aerosol characterization gathering ground-based in situ and sunphotometer measurements have been performed for the city of Thessaloniki for two specific days: the 12th and 13th of June 1997. A representative aerosol model for Thessaloniki aerosols was tentatively constructed for each day. Four components have been selected from our chemical measurements: black carbon (BC), particulate organic matter (POM), inorganic fine water soluble particles (WS) and a residue coarse component which mainly contains coarse dust and sea-salt particles (CC). Size distribution and complex refractive index for (WS) and (CC) components were determined from published data. (CC) has been shown to have a small optical effect compared to the submicron components. Size distribution for carbonaceous particles was obtained from sensitivity tests on particulate number and visible Angström exponent. The impact of relative humidity on extinction and scattering coefficients has been calculated on 13 June with Mie theory and Hänel relationships. Parameters needed for this calculation were well known for WS particles only. For POM particles we have used the experimental curve of hygroscopic factors obtained by Hobbs et al. (1997) for urban aerosols sampled on the East coast of United States to determine the hydrophilic dependency of POM particles. Relative humidity has been shown to be an important parameter even for values lower than 50%. Optical apportionment calculation has been realized pointing out that more than 45% of the total extinction coefficient is due to (POM) particles and about 20 and 30% to (WS) and (BC), respectively.     

Retrieval of the aerosol size distribution in the complex anomalous diffraction approximation

This contribution reports some recently achieved results in aerosol size distribution retrieval in the complex anomalous diffraction approximation (ADA) to MIE scattering theory. This approximation is valid for spherical particles that are large compared to the wavelength and have a refractive index close to 1.The ADA kernel is compared with the exact MIE kernel. Despite being a simple approximation, the ADA seems to have some practical value for the retrieval of the larger modes of tropospheric and lower stratospheric aerosols.The ADA has the advantage over MIE theory that an analytic inversion of the associated Fredholm integral equation becomes possible. In addition, spectral inversion in the ADA can be formulated as a well-posed problem. In this way, a new inverse formula was obtained, which allows the direct computation of the size distribution as an integral over the spectral extinction function. This formula is valid for particles that both scatter and absorb light and it also takes the spectral dispersion of the refractive index into account.Some details of the numerical implementation of the inverse formula are illustrated using a modified gamma test distribution. Special attention is given to the integration of spectrally truncated discrete extinction data with errors.     

Assessing the Relative Contribution of Biogenic and Fossil Processes to Visibility-Scattering Aerosols Found in Remote Areas: Near-Term Organic Research Program

Abstract

Organic carbon has been found to be a significant component of aerosols that impair visibility in remote areas across the country. Organic aerosols are particularly important in western areas of the United States and contribute roughly equally with sulfate aerosols and dust in the total extinction budget. Potential visibility enhancement resulting from various future energy management options that reduce volatile organic carbon and particulate material emissions from fossil-energy-related processes hinges on the relative contribution of the fossil-fuel-derived organic component to the extinction budget. Thus, additional studies are needed to quantify the partitioning of organic carbon between biogenic and fossil sources. Relative humidity (RH) also plays an important role in visibility impairment. It is well known that water soluble aerosol species, such as sulfate and nitrate, can increase light-scattering efficiencies of fine particles by more than an order of magnitude as RH is increased from 20-30% to 90-95%. Organic carbon aerosol has been found to be a mixture of more soluble and less soluble components, but few studies have been performed to evaluate the RH response function of aerosols composed of these components, either separately or in combination, especially at high relative humidities. The purpose of this paper is to describe some experiments that could address the major uncertainties of biogenic and fossil carbon contributions to the fine particle extinction budget and visibility impairment.     

Vertical distributions of aerosols under different weather conditions: Analysis of in-situ aircraft measurements in Beijing,China

In this study, aerosol vertical distributions of 17 in-situ aircraft measurements during 2005 and 2006 springs are analyzed. The 17 flights are carefully selected to exclude dust events, and the analyses are focused on the vertical distributions of aerosol particles associated with anthropogenic activities. The results show that the vertical distributions of aerosol particles are strongly affected by weather and meteorological conditions, and 3 different types of aerosol vertical distributions corresponding to different weather systems are defined in this study. The measurement with a flat vertical gradient and low surface aerosol concentrations is defined as type-1; a gradual decrease of aerosols with altitudes and modest surface aerosol concentrations is defined as type-2; a sharp vertical gradient (aerosols being strongly depressed in the PBL) with high surface aerosol concentrations is defined as type-3. The weather conditions corresponding to the 3 different aerosol types are high pressure, between two high pressures, and low pressure systems (frontal inversions), respectively. The vertical mixing and horizontal transport for the 3 different vertical distributions are analyzed. Under the type-1 condition, the vertical mixing and horizontal transport were rapid, leading to strong dilution of aerosols in both vertical and horizontal directions. As a result, the aerosol concentrations in PBL (planetary boundary layer) were very low, and the vertical distribution was flat. Under the type-2 condition, the vertical mixing was strong and there was no strong barrier at the PBL height. The horizontal transport (wind flux) was modest. As a result, the aerosol concentrations were gradually reduced with altitude, with modest surface aerosol concentrations. Under the type-3 condition, there was a cold front near the region. As a result, a frontal inversion associated with weak vertical mixing appeared at the top of the inversion layer, forming a very strong barrier to prevent aerosol particles being exchanged from the PBL height to the free troposphere. As a result, the aerosol particles were strongly depressed in the PBL height, producing high surface aerosol concentrations. The measured vertical aerosol distributions have important implications for studying the effects of aerosols on photochemistry. The J[O₃] values are reduced by 11%, 48%, and 50%, under the type-1, type-2, and type-3 conditions, respectively. This result reveals that atmospheric oxidant capacity (OH concentrations) is modestly reduced under the type-1 condition, but is significantly reduced under the type-2 and type-3 conditions. This result also suggests that the effect of aerosol particles on surface solar flux is an integrated column effect, and detailed vertical distributions of aerosol particles are very important for assessing the impacts of aerosol on photochemistry.     

Fine particulate chemical composition and light extinction at Meadview, AZ

The concentration of fine particulate nitrate, sulfate, and carbonaceous material was measured for 12-hr day-night samples using diffusion denuder samplers during the Project Measurement of Haze and Visibility Effects (MOHAVE) July to August 1992 Summer Intensive study at Meadview, AZ, just west of Grand Canyon National Park. Organic material was measured by several techniques. Only the diffusion denuder method measured the semivolatile organic material. Fine particulate sulfate and nitrate (using denuder technology) determined by various groups agreed. Based on the various collocated measurements obtained during the Project MOHAVE study, the precision of the major fine particulate species was +/- 0.6 microg/m3 organic material, +/- 0.3 microg/m3 ammonium sulfate, and +/- 0.07 microg/m3 ammonium nitrate. Data were also available on fine particulate crustal material, fine and coarse particulate mass from the Interagency Monitoring of Protected Visual Environments sampling system, and relative humidity (RH), light absorption, particle scattering, and light extinction measurements from Project MOHAVE. An extinction budget was obtained using mass scattering coefficients estimated from particle size distribution data. Literature data were used to estimate the change in the mass scattering coefficients for the measured species as a function of RH and for the absorption of light by elemental carbon. Fine particulate organic material was the principal particulate contributor to light extinction during the study period, with fine particulate sulfate as the second most important contributor. During periods of highest light extinction, contributions from fine particulate organic material, sulfate, and light-absorbing carbon dominated the extinction of light by particles. Particle light extinction was dominated by sulfate and organic material during periods of lowest light extinction. Combination of the extinction data and chemical mass balance analysis of sulfur oxides sources in the region indicate that the major anthropogenic contributors to light extinction were from the Los Angeles, CA, and Las Vegas, NV, urban areas. Mohave Power Project associated secondary sulfate was a negligible contributor to light extinction.     

Sulphur in the arctic environment (2): results of multi-medium regional mapping.

The regional distribution patterns of S in terrestrial moss and in the O-, B-, and C-horizon of podzols have been studied in a 188,000 km2 area in Arctic Europe with both, large natural (marine aerosols) and anthropogenic gradients of S-input. Although the existence of a pollution source is visible in the S-maps for moss, the S-deposition gradient is not depicted. The concentration of S in moss is not at all influenced by input of marine aerosols. In contrast, the O-horizon of podzols shows a coastal enrichment of S but does not reflect the anthropogenic input. Even the coastal pattern visible in the map of S in the O-horizon is, however, not linked to the input of SO4(2-) via sea spray but is rather caused by low litter decomposition rates due to low temperature, increasing total S and decreasing mobile S near coast. S-concentrations as observed in the deeper soil horizons are only locally influenced by both anthropogenic and marine input of S. These results suggest that in undisturbed terrestrial environments no mechanism exists for enriching an additional input of S from anthropogenic or natural sources. A very high local variability in the four sample materials points to small-scale local processes being most important for the observed S-concentrations.     

Aerosol composition as a function of haze and humidity levels in the Southwestern U.S.

The observed composition of visibility-reducing aerosols in the Grand Canyon region is summarized in climatological terms. Observations are from SCENES, a measurement program extending from 1984 to 1989. Results are presented as average mass balances stratified by various factors.Aerosols were found to exhibit substantial seasonal variation, but little systematic diurnal variation. Crustal material was a dynamic component, and peaked during springtime. Aerosol composition, but not total concentration, depended strongly on ambient relative humidity, with crustal material augmented at low humidities and sulfates augmented at high humidities. Total fine-particle concentrations correlated strongly with light scattering, as expected; however, little association between chemical composition and light scattering was observed.     

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.     

Atmospheric turbidity over Kathmandu valley

The atmosphere of Kathmandu Valley has been investigated by using Sunphotometer and Nephelometer during the pre-monsoon period of 1999. The atmospheric turbidity parameters (extinction coefficient for 500 nm wavelength τ_AG and Angstrom coefficient β) are found high in the morning and show decreasing trends from morning to late afternoon on average. Vertical dispersion of pollutants and increasing pollutant flushing rate by increasing wind speed from morning to late afternoon is the cause for this decreasing trend of turbidity over the valley. Being surrounded by high hills all around the valley, horizontal exit of pollutants without vertical dispersion is not possible. The scattering coefficient b_scat of aerosols in ground level troposphere is also found high in the morning, which decreases and becomes minimum during afternoon. During late afternoon, b_scat again shows a slightly increasing trend. The reason is the increasing vehicular emission during late afternoon rush period. The average values of Angstrom exponent α, β, τ_AG and b_scat are found to be 0.624±0.023, 0.299±0.009, 0.602±0.022 and 0.353±0.014 km⁻¹, respectively. About 76.8% of the observed values of β lie above 0.2 indicating heavy particulate pollution in the valley. A comparison of observed values of turbidity parameters with other major cities of the world shows that Kathmandu is as polluted as cities like Jakarta, Kansas, Beijing, Vienna, etc.     

Fine Particulate Chemical Composition and Light Extinction at Meadview,AZ

Abstract

The concentration of fine particulate nitrate, sulfate, and carbonaceous material was measured for 12-hr day-night samples using diffusion denuder samplers during the Project Measurement of Haze and Visibility Effects (MOHAVE) July to August 1992 Summer Intensive study at Meadview, AZ, just west of Grand Canyon National Park. Organic material was measured by several techniques. Only the diffusion denuder method measured the semivolatile organic material. Fine particulate sulfate and nitrate (using denuder technology) determined by various groups agreed. Based on the various collocated measurements obtained during the Project MOHAVE study, the precision of the major fine particulate species was ±0.6 μg/m³ organic material, ±0.3 μg/m³ ammonium sulfate, and ±0.07 μg/m³ ammonium nitrate. Data were also available on fine particulate crustal material, fine and coarse particulate mass from the Interagency Monitoring of Protected Visual Environments sampling system, and relative humidity (RH), light absorption, particle scattering, and light extinction measurements from Project MOHAVE. An extinction budget was obtained using mass scattering coefficients estimated from particle size distribution data. Literature data were used to estimate the change in the mass scattering coefficients for the measured species as a function of RH and for the absorption of light by elemental carbon. Fine particulate organic material was the principal particulate contributor to light extinction during the study period, with fine particulate sulfate as the second most important contributor. During periods of highest light extinction, contributions from fine particulate organic material, sulfate, and light-absorbing carbon dominated the extinction of light by particles. Particle light extinction was dominated by sulfate and organic material during periods of lowest light extinction. Combination of the extinction data and chemical mass balance analysis of sulfur oxides sources in the region indicate that the major anthropogenic contributors to light extinction were from the Los Angeles, CA, and Las Vegas, NV, urban areas. Mohave Power Project associated secondary sulfate was a negligible contributor to light extinction.     

Measurements of aerosol optical properties in central Tokyo during summertime using cavity ring-down spectroscopy: Comparison with conventional techniques

A highly sensitive cavity ring-down spectrometer (CRDS) was used to monitor the aerosol extinction coefficient at 532 nm. The performance of the spectrometer was evaluated using measurements of nearly monodisperse polystyrene particles with diameters between 150 and 500 nm. By comparing the observed results with those determined using Mie theory, the accuracy of the CRDS instrument was determined to be >97%, while the upper limit for the precision of the instrument was estimated to be 0.6–3.5% (typically 2%), depending on the particle number concentration, which was in the range of 30–2300 particles cm^?3. Simultaneous measurements of the extinction (b_ext), scattering (b_sca) and absorption (b_abs) coefficients of ambient aerosols were performed in central Tokyo from 14 August to 2 September 2007 using the CRDS instrument, two nephelometers and a particle/soot absorption photometer (PSAP), respectively. The value of b_ext measured using the CRDS instrument was compared with the sum of the b_sca and b_abs values measured with a nephelometer and a PSAP, respectively. Good agreement between the b_ext and b_sca + b_abs values was obtained except for data on days when high ozone mixing ratios (>130 ppbv) were observed. During the high-O₃ days, the values for b_sca + b_abs were ～7% larger than the value for b_ext, possibly because the value for b_abs measured by the PSAP was overestimated due to interference from coexisting non-absorbing aerosols such as secondary organic aerosols.     

APCA Financial Statements for FY 1979-80

The U.S. Environmental Protection Agency (EPA) has proposed a new secondary standard based on visibility in urban areas. The proposed standard will be based on light extinction, calculated from 24-hr averaged measurements. It would be desirable to base the standard on a shorter averaging time to better represent human perception of visibility. This could be accomplished by either an estimation of extinction from semicontinuous particulate matter (PM) data or direct measurement of scattering and absorption. To this end we have compared 1-hr measurements of fine plus coarse particulate scattering using a nephelometer, along with an estimate of absorption from aethalometer measurements. The study took place in Lindon, UT, during February and March 2012. The nephelometer measurements were corrected for coarse particle scattering and compared to the Filter Dynamic Measurement System (FDMS) tapered element oscillating microbalance monitor (TEOM) PM_2.5 measurements. The two measurements agreed with a mass scattering coefficient of 3.3 ± 0.3 m²/g at relative humidity below 80%. However, at higher humidity, the nephelometer gave higher scattering results due to water absorbed by ammonium nitrate and ammonium sulfate in the particles. This particle-associated water is not measured by the FDMS TEOM. The FDMS TEOM data could be corrected for this difference using appropriate IMPROVE protocols if the particle composition is known. However, a better approach may be to use a particle measurement system that allows for semicontinuous measurements but also measures particle bound water. Data are presented from a 2003 study in Rubidoux, CA, showing how this could be accomplished using a Grimm model 1100 aerosol spectrometer or comparable instrument.

Implications: Visibility is currently based on 24-hr averaged PM mass and composition. A metric that captures diurnal changes would better represent human perception. Furthermore, if the PM measurement included aerosol bound water, this would negate the need to know particulate composition and relative humidity (RH), which is currently used to estimate visibility. Methods are outlined that could accomplish both of these objectives based on use of a PM monitor that includes aerosol-bound water. It is recommended that these techniques, coupled with appropriate measurements of light scattering and absorption by aerosols, be evaluated for potential use in the visibility based secondary standard.     

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.