Nucleation of sulfuric acid-water and methanesulfonic acid-water solution particles: Implications for the atmospheric chemistry of organosulfur species

Binary nucleation theory is applied to the formation of aqueous sulfuric acid and aqueous methanesulfonic acid particles and the relative rates of aerosol formation in humid atmospheres are compared. An integral model is presented which describes nucleation of solution particles, aerosol growth, and condensable vapor source and depletion rates. To extend this model, the water activities of the ternary solution, sulfuric acid-methanesulfonic acid-water, are estimated, and growth of the nucleated aerosol by incorporation of both types of acid is considered. Predictions of both forms of the model are compared with the experimental results of Hatakeyama et al. [Atmospheric Environment19, 135–141 (1985)] for the photooxidation of dimethylsulfide in humid air.     

Calculating mean concentrations for steady sources in recirculating wakes by a particle trajectory method

A discrete vortex model of the recirculating flow behind a two-dimensional backward-facing step is used to calculate the trajectories of particles released from a fixed point. By averaging over a large number of such trajectories, an estimate is made of the mean concentration profile associated with a steady source in the wake. These estimates are verified against experimental data for point- and line-sources. The importance of incorporating a ‘random walk’ in calculating the trajectories is demonstrated. The mean flow in the discrete vortex model used appears to be the most critical factor in determining mean concentrations. The poorest predictions appear to be associated with the longest trajectories.Particle ‘recirculation times’ are also briefly examined and it is shown how these are related to the ‘residence times’ of Vincent (1976, Atmospheric Environment11, 765–774) and others. It is suggested that such residence times may not be an appropriate means of quantifying near-wake dispersion if sources are inside the wake. Advantages of a ‘particle trajectory’ method, as against a diffusion equation method, for dealing with dispersion in inhomogeneous flow are finally presented.     

Numerical calculation of flow and stack-gas concentration fluctuation around a cubical building

A numerical simulation model was developed to predict the instantaneous concentration fluctuation of a plume and applied to stack-gas diffusion around a cubical building. The flow field, including an instantaneous velocity component, was predicted using the large eddy simulation (LES) method in the developed numerical model. Then, the instantaneous concentration fluctuation was predicted using the obtained unsteady flow field. Concentration was calculated using the finite difference method, in which the LES is expanded for concentration, and the puff method, in which small volumes of the tracer gas are divided and combined according to the calculation mesh sizes. In order to avoid numerical viscous effects, a puff method and finite difference method were applied separately in the regions near and far from the stack-gas release point, respectively. Then, the flow field around a cubical building and the diffusion of stack-gas, emitted from an elevated point source at an upstream position of the building, were calculated using the model mentioned above. Numerical calculation results were compared with those obtained in wind tunnel experiments in which concentration fluctuation was measured using high-response flame ionization detectors. Although there were some discrepancies in the flow field between the calculated results and those of wind tunnel experiments, e.g., the calculated windward length of a cavity region behind the building, the calculated mean velocity and turbulent intensity showed good agreement with those of the wind tunnel experiments. Furthermore, the calculated concentration fluctuation showed good agreement with that in the wind tunnel, not only regarding the features of fluctuating concentration signals, but also statistic quantities, viz., mean concentration, fluctuation intensity and high-concentration values.     

Flow and dispersion in an urban cubical cavity

Flow and dispersion in an urban cubical cavity are numerically investigated using a Reynolds-averaged Navier–Stokes equations (RANS) model with the renormalization group (RNG) k–? turbulence closure model. The urban cubical cavity is surrounded by flank walls that are parallel to the streamwise direction, called end-walls, as well as upstream and downstream walls. A primary vortex and secondary vortices including end-wall vortices are formed in the cavity. Because of the end-wall drag effect, the averaged mean-flow kinetic energy in the cavity is smaller than that in an urban street canyon that is open in the along-canyon direction. A trajectory analysis shows that the end-wall vortices cause fluid particles to move in the spanwise direction, indicating that flow in the cavity is essentially three-dimensional. The iso-surfaces of the Okubo–Weiss criterion capture cavity vortices well. The pollutant concentration is high near the bottom of the upstream side in the case of continuous pollutant emission, whereas it is high near the center of the primary vortex in the case of instantaneous pollutant emission. To get some insight into the degree of pollutant escape from the cavity according to various meteorological factors, extensive numerical experiments with different ambient wind speeds and directions, inflow turbulence intensities, and cavity-bottom heating intensities are performed. For each experiment, we calculate the time constant, which is defined as the time taken for the pollutant concentration to decrease to e^?1 of its initial value. The time constant decreases substantially with increasing ambient wind speed, and tends to decrease with increasing inflow turbulence intensity and cavity-bottom heating intensity. The time constant increases as the ambient wind direction becomes oblique. High ambient wind speed is found to be the most crucial factor for ventilating the cavity, thus improving air quality in an urban cubical cavity.     

An analytical model for crosswind integrated concentrations released from a continuous source in a finite atmospheric boundary layer

An analytical model for the crosswind integrated concentrations released from a continuous source in a finite atmospheric boundary layer is formulated by considering the wind speed as a power law profile of vertical height above the ground and eddy diffusivity as an explicit function of downwind distance from the source and vertical height. A closed form analytical solution of the resulting advection–diffusion equation for these profiles of wind speed and eddy diffusivity with the physically relevant boundary conditions is derived using the separation of variables technique that leads to a Sturm–Liouville eigen value problem. Various particular cases of the model are deduced.The model is evaluated with the observations obtained from Prairie Grass experiment in various stability classes varying from very unstable to neutral and stable conditions and Hanford diffusion experiment in stable conditions. The agreement is found to be good between the computed and observed concentrations in both the diffusion experiments. For Prairie Grass experiment, the model is predicting 78% cases with in a factor of two and gives a value of NMSE as 0.075. On the other hand, for Hanford observations in stable conditions, it predicts 70% cases with in factor of two. An extensive analysis of statistical measures with the downwind distances from the source reveals that the model is performing well close to the source.     

On the sensitivity of particle size to relative humidity for Los Angeles aerosols

A TDMA system (Tandem Differential Mobility Analyzer; Rader D.J. and McMurry P.H. J. Aerosol Sci. 17, 771–787, 1986) was used to measure the sensitivity of particle size to relative humidity for monodisperse Los Angeles aerosols. Measurements were made at Claremont, CA on 13 days between 19 June and 3 September 1987, in conjunction with the Southern California Air Quality Study (SCAQS). The particle sizes that were studied ranged from 0.05 μm to 0.5 μm diameter at ambient relative humidity (typically 45–65%).The data provide clear evidence that these atmospheric aerosols were externally mixed. Monodisperse ambient aerosols were often found to split into nonhygroscopic (no water uptake) and hygroscopic portions when humidified. An average of 30% of the particles in the 0.2–0.5 μm range were nonhygroscopic. However, the proportion of the particles that was nonhygroscopic varied considerably from day to day and was, on occasion, as high as 70–80% of the particles. There was no clear evidence for nonhygroscopic 0.05 μm particles, but the data are not definitive on this point.The data also show that for the hydrophilic aerosol fraction, the larger particles (0.4–0.5 μm) grew more when humidified than did smaller particles (0.05–0.2 μm). As relative humidities were increased from 50% to 90%, particle diameters grew by average factors of 1.46 ±0.02 (for 0.5 μm particles), 1.49 ± 0.08 (0.4 μm), 1.19 ± 0.08 (0.2 μm) and 1.12 ± 0.05 (0.05 μm). Similarly, when particles were dried from 50% RH to 6–10% RH, particle diameters changed by factors ranging from 0.94 ± 0.03 (0.5 μm) to 0.98 ± 0.01 (0.05 μm).     

Measurement of octanol–air partition coefficients using solid-phase microextraction (SPME)—application to hydroxy alkyl nitrates

Multifunctional organic compounds are thought to constitute a major component of the organic matter found in atmospheric particles. Their partitioning into the organic matter depends on their structure, their chemical properties and the properties of the absorbing matrix. It was recently shown that octanol is a suitable surrogate for organic particles and the octanol–air partition coefficient (K_OA) was suggested as a useful tool for estimating the partitioning of organic compounds into atmospheric particles that contain high organic mass fractions. In this paper, we present a new and simple technique for the determination of K_OA using solid phase microextraction (SPME) relative to a known Henry's law constant. We apply the technique for the determination of K_OA of β-, γ- and δ-C₃–C₅ hydroxy alkyl nitrates. The temperature dependence of K_OA for some of the compounds is also measured. It is shown that the solubility constants of these compounds are higher in octanol than in water and that the solubility in octanol increases with the length of the hydrophobic chain and with increasing distance between the hydroxy and the nitrooxy groups. Partition coefficients between the gas and particulate phase (K_p) are calculated using the determined K_OA values and their atmospheric implications are discussed.     

The effect of humidity and state of water surfaces on deposition of aerosol particles onto a water surface

Deposition processes of particles with dry diameter larger than about 10 μm are dominated by gravitational settling, while molecular diffusion and Brownian motion predominate the deposition processes of particles smaller than 0.1 μm in dry diameter. Many air pollution derived elements exhibit characteristics common to sub-micron particles. The objective of the present study is to examine the effects of meteorological conditions within the turbulent transfer layer on the deposition velocity of particles with dry diameter between 0.1 and 1 μm. It is for these sub-micron particles that particle growth by condensation in the deposition layer, the broken water surface effect and the enhanced transfer process due to atmospheric turbulence in the turbulent transfer layer play important roles in controlling the particle deposition velocity. Results of the present study show that the `dry air’ assumption of Williams’ model is unrealistic. Effects of ambient air relative humidity and water surface temperature cannot be ignored in determining the deposition velocity over a water surface. Neglecting effects of ambient air relative humidity and water surface temperature will result in defining atmospheric stability incorrectly. It is found that the largest effect of air relative humidity on deposition velocity occurs at an air–water temperature difference corresponding to the point of `displaced neutral stability'. For a given wind speed of U=5 m s⁻¹ the additive effects of water surface temperature, T_w, changes from 5 to 25°C and ambient air relative humidity variations from 85 to 60%, respectively, lead to a maximum difference in v_d of about 20%. For a higher wind speed of 10 m s⁻¹, however, the corresponding change in v_d reduces to less than 5%. This is further confirmation that wind speed is one of the strongest variables that governs the magnitude of v_d. The present study also found that the broken surface transfer coefficient, k_bs, given as a multiple of the smooth surface transfer coefficient, k_ss, is physically more meaningful than assigning it a constant value independent of particle size. The method used in this study requires only a single level of atmospheric data coupled with the surface temperature measurement. The present method is applicable for determining deposition velocity not only at the conventional measurement height of 10 m but also at any other heights that are different from the measurement height.     

Morphological and chemical composition characteristics of summertime atmospheric particles collected at Tokchok Island,Korea

Determination of the chemical compositions of atmospheric single particles in the Yellow Sea region is critical for evaluating the environmental impact caused by air pollutants emitted from mainland China and the Korean peninsula. After ambient aerosol particles were collected by the Dekati PM10 cascade impactor on July 17–23, 2007 at Tokchok Island (approximately 50 km west of the Korean coast nearby Seoul), Korea, overall 2000 particles (on stage 2 and 3 with cut-off diameters of 2.5–10 μm and 1.0–2.5 μm, respectively) in 10 samples were determined by using low-Z particle electron probe X-ray microanalysis. X-ray spectral and secondary electron image (SEI) data showed that soil-derived and sea-salt particles which had reacted or were mixed with SO₂ and NO_x (or their acidic products) outnumbered the primary and “genuine” ones (59.2% vs. 19.2% in the stage 2 fraction and 41.3% vs. 9.9% in the stage 3 fraction). Moreover, particles containing nitrate in the secondary soil-derived species greatly outnumbered those containing sulfate. Organic particles, mainly consisting of marine biogenic species, were more abundant in the stage 2 fraction than in the stage 3 fraction (11.6% vs. 5.1%). Their relative abundance was greater than the sum of carbon-rich, K-containing, Fe-containing, and fly ash particles, which exhibited low frequencies in all the samples. In addition, many droplets rich in C, N, O, and S were observed. They tended to be small, exhibiting a dark round shape on SEI, and generally included 8–20 at.% C, 0–12 at.% N, 60–80 at.% O, and 4–10 at.% S (sometimes with <3 at.% Mg and Na). They were attributed to be a mixture of carbonaceous matter, H₂SO₄, and NH₄HSO₄/(NH₄)₂SO₄, mostly from the reaction of atmospheric SO₂ with NH₃ under high relative humidity. The analysis of the relationship between the aerosol particle compositions and 72-h backward air-mass trajectories suggests that ambient aerosols at Tokchok Island are strongly affected not only by seawater from the Yellow Sea but also by anthropogenic pollutants emitted from China and the Seoul–Incheon metropolis, resulting in the dominance of complex secondary aerosol particles.     

Studies of the coarse particle (2.5–10 μm) component in UK urban atmospheres

An analysis is presented of continuous simultaneous measurement data for PM₁₀ and PM_2.5 using TEOM instruments from five sites in the United Kingdom. The results are analysed specifically in relation to the sources and processes influencing the coarse particle fraction (2.5–10 μm). The data show a generally strong correlation between fine and coarse particle concentrations at all sites, with a generally higher proportion of coarse particles in the dryer months of the year. The one rural site shows a notably lower proportion of coarse particles than the urban and suburban sites. Whilst it is possible to disaggregate the coarse particle concentrations into a component which is diluted by increasing windspeed and a component which increases with windspeed and is hence possibly attributable to wind-induced resuspension processes, the latter is only a minor proportion of the total coarse particle concentration. There are appreciable weekday-to-weekend and day-to-night differences between coarse particle concentrations which are most marked at the urban sites indicative of anthropogenic activities being a source of coarse particles. The clearest indication of the likely predominant source of coarse particles arises from an analysis of a data set derived from an urban street canyon site after subtraction of measurements from a nearby urban background location. The data indicate strong relationships of both fine and coarse incremental particle concentrations in the street canyon with incremental NO_x. If incremental fine particles and coarse particles are attributed to exhaust emissions and vehicle-induced resuspension, respectively, then it may be concluded that vehicle-induced resuspension provides a source strength approximately equal to that of exhaust emissions. An analysis of the coarse particle concentration data suggest that episodes of elevated coarse particle concentrations alone very rarely lead to exceedence of the UK air quality standard for PM₁₀ of 50 μg m⁻³ measured as a 24-h running mean.     

Numerical simulation of scalar dispersion downstream of a square obstacle using gradient-transport type models

We present a numerical study of scalar transport released from a line source downstream of a square obstacle to investigate the capabilities and limitations of gradient-transport modeling in predicting atmospheric dispersion. The standard k–? and k–ω models and a Reynolds Stress Transport closure are employed and compared to predict the time-averaged turbulent flow field, while a standard gradient–diffusion model is initially adopted to relate the scalar flux to mean gradients of the concentration field. The analysis of two algebraic closures for turbulent scalar fluxes based on the generalized-gradient–diffusion hypothesis and its quadratic extension is also presented. In spite of the rather simple flow setup, where both the flow and the scalar fields can be assumed homogeneous in the spanwise direction, the analysis clarifies several critical issues concerning gradient-transport type models. We established the dominant role of predicted turbulent kinetic energy on scalar dispersion when a scalar diffusivity is employed, irrespectively of the Reynolds stress closure adopted for the averaged momentum equation. Moreover, the standard gradient–diffusion hypothesis failed to predict the streamwise component of the scalar flux, which is characterized by a counter-gradient-transport mechanism. Although the resulting contribution in the averaged scalar transport equation is small in the present flow configuration, this limitation can become severe for strongly inhomogeneous flows in the presence of point sources, where the spread of the scalar plume is essentially three-dimensional. The predictive capabilities of gradient-transport type modeling are found clearly improved using algebraic closures, which appear to represent a promising tool for predicting atmospheric dispersion in complex flows when unsteady transport mechanisms are not dominant.     

Effects of wind shear on pollution dispersion

Using an accurate numerical method for simulating the advection and diffusion of pollution puffs, it is demonstrated that point releases of pollution grow into a shape reflecting the vertical wind shear profile experienced by the puff within a time scale less than 4 h. For distances beyond several 10 s of kilometers from a release point, shear-related dispersion effects are probably the dominant mechanism affecting the area and magnitude of surface impacts. For assessing long-range pollutant dispersion, the common assumption that pollutants disperse as horizontally spherical “puffs” in the atmosphere is inherently inaccurate since shear-induced horizontal spreading of pollution is not a homogeneous “turbulent-like” diffusion process. A Lagrangian puff model can simulate an area impacted by a pollution puff only if larger shear-dependent horizontal puff dispersions are assumed. However, even if impacted areas are reasonably simulated, peak concentrations will be severely underestimated since atmospheric puffs influenced by even small amounts of wind shear are nonspherical. If horizontal dispersion coefficients in a Lagrangian puff model are adjusted so that peak concentrations are correctly simulated, then the calculated pollution impact area will be severely skewed. In shear environments, no choice of horizontal dispersion coefficients in a single-puff Lagrangian model will yield reasonable correlations with puffs that are skewed into nonspherical shapes by atmospheric wind shear.     

Wind tunnel investigation on the retention of air pollutants in three-dimensional recirculation zones in urban areas

The article discusses an experimental investigation of turbulent dispersion processes in a typical three-dimensional urban geometry, in reduced scale, in neutrally stable conditions. Wind tunnel experiments were carried out for characterizing the flow and the dispersion of a pollutant around a scaled model (1:400) of a group of eight 10-floor buildings surrounding a square. The situation corresponded to the dispersion of fine inertialess particles released from a line source positioned upstream of the urban geometry. After the sudden interruption of the source generation, the particles persisted in the recirculation cavity between the buildings, with the concentration decaying exponentially with time. This is in accordance with previous works on the dispersion process around bluff bodies of different shapes [e.g., Humphries and Vincent, 1976. An experimental investigation of the detention of airborne smoke in the wake bubble behind a disk. Journal of Fluid Mechanics 73, 453–464; Vincent, 1977. Model experiments on the nature of air pollution transport near buildings. Atmospheric Environment 11, 765–774; Fackrell, 1984. Parameters characterizing dispersion in the near wake of buildings. Journal of Wind Engineering and Industrial Aerodynamics 16, 97–118]. The main parameter in the investigation was the characteristic time constant for the concentration decay. The measurements of the variation in the concentration of the fine particles were performed by means of a photo-detection technique based on the attenuation of light. The velocity fields were evaluated with the particle image velocimetry (PIV) technique. The dimensionless residence time H for the particles (H=τU/L, where τ is the time constant for the concentration decay, U the free-stream velocity, and L is a characteristic dimension for the urban geometry, as defined by Humphries and Vincent [1976. An experimental investigation of the detention of airborne smoke in the wake bubble behind a disk. Journal of Fluid Mechanics 73, 453–464] was determined for various locations in the scaled model, in the range of Reynolds numbers (Re) between 8000 and 64,000. H was found to be 6.5±1.0.     

Reactivity between PbSO4 and CaCO3 particles relevant to the modification of mineral particles and chemical forms of Pb in particles sampled at two remote sites during an Asian dust event

During the transboundary transport of anthropogenic heavy metals by mineral particles providing reaction sites, the divalent metal salt PbSO₄ can be converted to PbCO₃ in the presence of water. We carried out laboratory experiments to study the transformation process under various conditions by incorporating test particles comprising CaCO₃ of a particulate mineral component, PbSO₄, and NaCl. After the immersion of PbSO₄ particles in contact with CaCO₃ particles in a water droplet, the conversion of PbSO₄ into PbCO₃ was confirmed by the change in morphology of the original particles to stick or needle form; the percentages of the chemical forms relative to the total Pb were determined by X-ray absorption near edge structure (XANES) analysis. Approximately 60–80% of PbSO₄ was converted to PbCO₃ after 24 h. A small amount of stick particles was detected when NaCl particles attached to PbSO₄/CaCO₃ particles were exposed to air with a relative humidity (RH) of 80–90% for 24 h. XANES measurements of the samples revealed that the molar percentage of PbCO₃ relative to the total Pb content was 4%.Field experiments were also conducted to determine the chemical forms of the Pb particles during the Kosa (Asian dust storm) event. Samples were collected from two remote sites in Japan and Korea. The mass size distribution of Pb aerosols collected in Japan was bimodal with two peaks in the coarse mode; the enrichment factor of Pb suggested that its source was anthropogenic. Pb L3 edge XANES measurements of both samples indicated that they had similar shapes. These measurements also indicated that the major Pb components for the samples collected in Japan were PbO, PbSO₄ PbCl₂, and PbCO₃, with molar percentages of 44%, 30%, 21%, and 5%, respectively. No significant differences were found between the component ratios of the samples collected in Japan and Korea, suggesting that definite transformation did not occur during the transport of the Kosa particles from Korea to Japan. On the basis of these observations, we postulate that the transformation process either occurred mainly before the particles arrived at Korea or did not take place after the particles left continental Asia.     

Stability of two prediction schemes for hourly nitrogen oxide concentrations by a regression model

In a preceding paper (Inoue et al, 1986b, Atmospheric Environment20, 2325–2337), we proposed two prediction schemes for hourly nitrogen oxide (NO) concentration using the regression model with autocorrelated error terms, and applied these schemes to the prediction of NO-concentration at m h later. Data analyses based on the data sets observed at a measurement site for a year showed that these schemes are practical for the predictions 1 h later.In this follow up paper, we apply these schemes to the prediction for other years and/or other measurement sites, and investigate the stability of the assumed regression model and the adopted prediction schemes not only numerically but also theoretically. From these analyses, our prediction schemes are shown to be stable for the prediction of NO-concentration in other years.     

An Analysis of Visual Range in the Eastern United States Under Different Meteorological Regimes

ABSTRACT

The issue of fine particle (PM₂₅) exposures and their potential health effects is a focus of scientific research because of the recently promulgated National Ambient Air Quality Standard for PM_{2 5}. Before final implementation, the health and exposure basis for the standard will be reviewed by the U.S. Environmental Protection Agency within the next five years. As part of this process, it is necessary to understand total particle exposure issues and to determine the relative importance of the origin of PM_{2 5} exposure in various micro-environments. The results presented in this study examine emissions of fine particles from a previously uncharacterized indoor source: the residential vacuum cleaner. Eleven standard vacuum cleaners were tested for the emission rate of fine particles by their individual motors and for their efficiency in collecting laboratory-generated fine particles. An aerosol generator was used to introduce fine potassium chloride (KC1) particles into the vacuum cleaner inlet for the collection efficiency tests. Measurements of the motor emissions, which include carbon, and the KCl aerosol were made using a continuous HIAC/Royco 5130A light-scattering particle detector. All tests were conducted in a metal chamber specifically designed to completely contain the vacuum cleaner and operate it in a stationary position. For the tested vacuum cleaners, fine particle motor emissions ranged from 9.6 x 10⁴ to 3.34 x 10⁸ particles/min, which were estimated to be 0.028 to 176 mg/min for mass emissions, respectively. The vast majority of particles released were in the range of 0.3-0.5 mm in diameter. The lowest particle emission rate was obtained for a vacuum cleaner that had a high efficiency (HEPA) filter placed after the vacuum cleaner bag and the motor within a sealed exhaust system. This vacuum cleaner removed the KC1particles that escaped the vacuum cleaner bag and the particles emitted by the motor. Results obtained for the KC1 collection efficiency tests show >99% of the fine particles were captured by the two vacuum cleaners that used a HEPA filter. A series of tests conducted on two vacuum cleaners found that the motors also emitted ultra-fine particles above 0.01 mm in diameter at rates of greater than 10⁸ ultra-fine particles/CF of air. The model that had the best collection efficiency for fine particles also reduced the ultra-fine particle emissions by a factor of 1 x 10³.     

Applied dispersion modelling based on meteorological scaling parameters

A method for calculating the dispersion of plumes in the atmospheric boundary layer is presented. The method is easy to use on a routine basis. The inputs to the method are fundamental meteorological parameters, which act as distinct scaling parameters for the turbulence. The atmospheric boundary layer is divided into a number of regimes. For each scaling regime we suggest models for the dispersion in the vertical direction. The models directly give the crosswind-integrated concentrations at the ground, x_y, for nonbuoyant releases from a continuous point source. Generally the vertical concentration profile is proposed to be other than Gaussian. The lateral concentration profile is always assumed to be Gaussian, and models for determining the lateral spread σ_y are proposed. The method is limited to horizontally homogeneous conditions and travel distances less than 10km. The method is evaluated against independent tracer experiments over land. The overall agreement between measurements and predictions is very good and better than that found with the traditional Gaussian plume model.     

A photochemical model for air quality assessment: Model description and verification

A hybrid Eulerian-Lagrangian, photochemical model has been developed for the assessment and prediction of the impact of large point sources on air quality. This simple model is based on solving the mass conservation equations which include chemical reaction terms in the cells of a two-dimensional crosswind plane which moves with the air parcel. Testing of the model is done in three ways. First, the chemistry is evaluated using results of smog chamber experiments simulating Melbourne's emissions and meteorological conditions. Second, the accuracy of the emissions inventory is tested using aircraft measurements. Finally the overall performance of the model is evaluated using monitoring station data. In general the model gives good agreement with the measurements, with the predictions for O₃ being somewhat better than those for NO₂. This result was also found in the three-dimensional study of McRae and Seinfeld (1983, Atmospheric Environment17, 501–522) for the Los Angeles area.     

Distribution characteristics of polycyclic aromatic hydrocarbons with particle size in urban aerosols at the roadside in Ho Chi Minh City,Vietnam

The purpose of this study was to characterize size distributions of atmospheric polycyclic aromatic hydrocarbons (PAHs) with 4–6 rings at the roadside in Ho Chi Minh City, Vietnam. Ten PAHs (fluoranthene, pyrene, triphenylene, benzo[a]anthracene, chrysene, benzo[b]fluoranthene, benzo[k]fluoranthene, benzo[a]pyrene, benzo[ghi]perylene and indeno[1,2,3-cd]pyrene) in atmospheric particulate matters (PM) at the roadside were measured in the dry and rainy seasons in 2005 at Ho Chi Minh City, using a low-pressure cascade impactor. The PM were separated into nine fractions by their aerodynamic diameter, i.e. >9.0, 9.0–5.8, 5.8–4.7, 4.7–3.3, 3.3–2.1, 2.1–1.1, 1.1–0.7, 0.7–0.4 and <0.4 μm (a final filter). PAHs were analyzed by high-performance liquid chromatography with fluorescence detection. Total PAHs measured were higher in the rainy season than in the dry season. The mass of coarse particles occupied a higher fraction than that of fine particles in both seasons. Total PAHs were mainly concentrated in particles with aerodynamic diameter smaller than 0.4 μm. The particle size distributions of PAHs investigated were bi-modal with a peak in fine particle mode (<2.1 μm) and another peak in coarse particle mode (>2.1 μm). Generally, 5,6-ring PAHs associated mainly with fine particles and 4-ring PAHs spread out in both fine and coarse particles.     

Sensitivity analysis of source regions to PM2.5 concentration at Fukue Island,Japan

The authors analyze the sensitivities of source regions in East Asia to PM_2.5 (particulate matter with an aerodynamic diameter of ≤2.5 µm) concentration at Fukue Island located in the western part of Japan by using a regional chemical transport model with emission sensitivity simulations for the year 2010. The temporal variations in PM_2.5 concentration are generally reproduced, but the absolute concentration is underestimated by the model. Chemical composition of PM_2.5 in the model is compared with filter sampling data in spring; simulated sulfate, ammonium, and elemental carbon are consistent with observations, but mass concentration of particulate organic matters is underestimated. The relative contribution from each source region shows the seasonal variation, especially in summer. The contribution from central north China (105°E–124°E, 34°N–42°N) accounts for 50–60% of PM_2.5 at Fukue Island except in summer; it significantly decreases in summer (18%). Central south China (105°E–123°E, 26°N–34°N) has the relative contribution of 15–30%. The contribution from the Korean Peninsula is estimated at about 10% except in summer. The domestic contribution accounts for about 7% in spring and autumn and increases to 19% in summer. We also estimate the relative contribution to daily average concentration in high PM_2.5 days (>35 μg m^?3). Central north China has a significant contribution of 60–70% except in summer. The relative contribution from central south China is estimated at 46% in summer and about 30% in the other seasons. The contributions from central north and south China on high PM_2.5 days are generally larger than those of their seasonal mean contributions. The domestic contribution is smaller than the seasonal mean value in every season; it is less than 10% even in summer. These model results suggest that foreign anthropogenic sources have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.

Implications: The contribution from several source regions in East Asia to PM_2.5 concentration at Fukue Island, a remote island located in the western part of Japan and close to the Asian continent, is estimated using a three-dimensional chemical transport model. The model results suggest that PM_2.5 that is attributed to foreign anthropogenic sources have a larger contribution than that of domestic pollution and have a substantial impact on attainment of the atmospheric environmental standard of Japan at Fukue Island.