Evaluation of the effect of long-range transport of air pollutants on coastal atmospheric monitoring sites in and around Taiwan

Long-range transport of pollution outflow from Asian mainland has been noticed and expected to play a significant role in Pacific background. Since 1993 the Taiwanese Environmental Protection Administration (TEPA) is conducting ground-based observations of various particulate and gaseous pollutants at 74 monitoring stations in Taiwan. One of these stations, Heng-Chun at the south coast of Taiwan can be considered as a background station with only negligible amounts of local pollution, and another one, Wan-Li at the north coast, predominantly receives air that has not passed over Taiwan, so that background air can be analysed by means of sectorisation. In this work, the sectorised 13-year time series of measurements of CO, SO₂, O₃, NO_x and PM₁₀, from the Wan-Li station are presen and compared to data from the Heng-Chun station and another TEPA background station off the coast of mainland China, Ma-Zu. The CO and O₃ measurements are also compared to data from the Yonaguni station, a Pacific island site, part of the Global Atmospheric Watch (GAW) network.The similarity of the sectorised data from the Wan-Li station with the data of the other station indicates that atmospheric measurements from the Wan-Li site can be used to make inferences about trends in western Pacific background air pollution and the effect of long-range transport of pollutants. The measurement time series from 1993 to 2006 do not indicate a significant trend in the monthly mean O₃ concentrations in accordance with other research about ozone in tropical latitudes. An increasing trend in CO concentrations of 2.8% per annum is observed between 1999 and 2006 for long-range transport to northern Taiwan, and a doubling of the SO₂ and NO_x concentrations observed at the Wan-Li and Heng-Chun sites within the period 2001–2006. SO₂ concentrations are found to quadruple at Ma-Zu within the same period. The data suggest that pollution from the Asian mainland enhances significantly the background air pollution over the Pacific.     

The characteristics of ozone and related compounds in the boundary layer of the South China coast: temporal and vertical variations during autumn season

We present measurements of several trace gases made at a subtropical coastal site in Hong Kong in October and November 1997. The gases include O₃, CO, SO₂, and NO_x. The surface measurement data are compared with those from an aircraft study [Kok et al. J. Geophys. Res. 102 (D15) (1997) 19043–19057], and a subset of the latter is used to show the vertical distribution of the trace gases in the boundary layer. During the study period, averaged concentrations at the surface site for O₃, CO, NO_x, and SO₂ were 50, 298, 2.75, and 1.65 ppbv, respectively. Their atmospheric abundance and diurnal pattern are similar to those found in the “polluted” rural areas in North America. The measured trace gases are fairly well mixed in the coastal boundary layer in the warm South China region. Large variability is indicated from the data. Examination of 10-day, isentropic back trajectories shows that the measured trace gases are influenced by maritime air masses, outflow of pollution-laden continental air, and the mixing of the two. The trajectories capture the contrasting chemical features of the large-scale air masses impacting on the study area. CO, NO_x and SO₂ all show higher concentrations in the strong outflow of continental air, as expected, than those in the marine category. Compared with previously reported values for the western Pacific, the much higher levels found in the marine trajectories in our study suggest the impacts of regional and/or sub-regional emissions on the measured trace gases at the study site. The presence of abundant O₃ and other chemically active trace gases in the autumn season, coupled with high solar radiation and warm weather, suggests that the South China Sea is a photochemically active region important for studying the chemical transformation of pollutants emitted from the Asian continent.     

Significant geographic gradients in particulate sulfate over Japan determined from multiple-site measurements and a chemical transport model: Impacts of transboundary pollution from the Asian continent

We found a significant geographic gradient (longitudinal and latitudinal) in the sulfate (SO₄^2?) concentrations measured at multiple sites over the East Asian Pacific Rim region. Furthermore, the observed gradient was well reproduced by a regional chemical transport model. The observed and modeled SO₄^2? concentrations were higher at the sites closer to the Asian continent. The concentrations of SO₄^2? from China as calculated by the model also showed the fundamental features of the longitudinal/latitudinal gradient. The proportional contribution of Chinese SO₄^2? to the total in Japan throughout the year was above 50–70% in the control case, using data for Chinese sulfur dioxide (SO₂) emission from the Regional Emission Inventory in Asia (40–60% in the low Chinese emissions case, using Chinese SO₂ emissions data from the State Environmental Protection Administration of China), with a winter maximum of approximately 65–80%, although the actual concentrations of SO₄^2? from China were highest in summer. The multiple-site measurements and the model analysis strongly suggest that the SO₄^2? concentrations in Japan were influenced by the outflow from the Asian continent, and this influence was greatest in the areas closer to the Asian continent. In contrast, we found no longitudinal/latitudinal gradient in SO₂ concentrations; instead SO₂ concentrations were significantly correlated with local SO₂ emissions. Our results show that large amounts of particulate sulfate are transported over long distances from the East Asian Pacific Rim region, and consequently the SO₄^2? concentrations in Japan are controlled by the transboundary outflow from the Asian continent.     

Transport of SO2 and aerosol over the Yellow sea

Aircraft measurements of air pollutants were made to investigate the characteristic features of long-range transport of sulfur compounds over the Yellow Sea for the periods of 26–27 April and 7–10 November in 1998, and 9–11 April and 19 June in 1999, together with aerosol measurements at the Taean background station in Korea. The overall mean concentrations of SO₂, O₃ and aerosol number in the boundary layer for the observation period ranged 0.1–7.4 ppb 32.1–64.1 ppb and 1.0–143.6 cm⁻³, respectively. It was found that the air mass over the Yellow Sea had a character of both the polluted continental air and clean background air, and the sulfur transport was mainly confined in the atmospheric boundary layer. The median of SO₂ concentration within the boundary layer was about 0.1–2.2 ppb. However, on 8 November, 1998, the mean concentrations of SO₂ and aerosol number increased up to 7.4 ppb and 109.5 cm⁻³, respectively, in the boundary layer, whereas O₃ concentration decreased remarkably. This enhanced SO₂ concentration occurred in low level westerly air stream from China to Korea. Aerosol analyses at the downstream site of Taean in Korea showed 2–3 times higher sulfate concentration than that of other sampling days, indicating a significant amount of SO₂ conversion to non sea-salt sulfate during the long-range transport.     

Transport and transformation of sulfur compounds over East Asia during the TRACE-P and ACE-Asia campaigns

On the basis of the recently estimated emission inventory for East Asia with a resolution of 1×1°, the transport and chemical transformation of sulfur compounds over East Asia during the period of 22 February through 4 May 2001 was investigated by using the Models-3 Community Multi-scale Air Quality (CMAQ) modeling system with meteorological fields calculated by the regional atmospheric modeling system (RAMS). For evaluating the model performance simulated concentrations of sulfur dioxide (SO₂) and aerosol sulfate (SO₄²⁻) were compared with the observations on the ground level at four remote sites in Japan and on board aircraft and vessel during the transport and chemical evolution over the Pacific and Asian Pacific regional aerosol characterization experiment field campaigns, and it was found that the model reproduces many of the important features in the observations, including horizontal and vertical gradients. The SO₂ and SO₄²⁻ concentrations show pronounced variations in time and space, with SO₂ and SO₄²⁻ behaving differently due to the interplay of chemical conversion, removal and transport processes. Analysis of model results shows that emission was the dominant term in regulating the SO₂ spatial distribution, while conversion of SO₂ to SO₄²⁻ in the gas phase and the aqueous phase and wet removal were the primary factors that controlled SO₄²⁻ amounts. The gas phase and the aqueous phase have the same importance in oxidizing SO₂, and about 42% sulfur compounds (25% in SO₂) emitted in the model domain was transported out, while about 57% (35% by wet removal processes) was deposited in the domain during the study period.     

The continuous field measurements of soluble aerosol compositions at the Taipei Aerosol Supersite,Taiwan

The characteristics of ambient aerosols, affected by solar radiation, relative humidity, wind speed, wind direction, and gas–aerosol interaction, changed rapidly at different spatial and temporal scales. In Taipei Basin, dense traffic emissions and sufficient solar radiation for typical summer days favored the formation of secondary aerosols. In winter, the air quality in Taipei Basin was usually affected by the Asian continental outflows due to the long-range transport of pollutants carried by the winter monsoon. The conventional filter-based method needs a long time for collecting aerosols and analyzing compositions, which cannot provide high time-resolution data to investigate aerosol sources, atmospheric transformation processes, and health effects. In this work, the in situ ion chromatograph (IC) system was developed to provide 15-min time-resolution data of nine soluble inorganic species (Cl⁻, NO₂⁻, NO₃⁻, SO₄²⁻, Na⁺, NH₄⁺, K⁺, Mg²⁺ and Ca²⁺). Over 89% of all particles larger than approximately 0.056 μm were collected by the in situ IC system. The in situ IC system is estimated to have a limit of detection lower than 0.3 μg m⁻³ for the various ambient ionic components. Depending on the hourly measurements, the pollutant events with high aerosol concentrations in Taipei Basin were associated with the local traffic emission in rush hour, the accumulation of pollutants in the stagnant atmosphere, the emission of industrial pollutants from the nearby factories, the photochemical secondary aerosol formation, and the long-range transport of pollutants from Asian outflows.     

Seasonal cycle and composition of background fine particles along the west coast of the US

We used aerosol data from 4 sites along the west coast of the U.S. to evaluate the role of transport, seasonal pattern, chemical composition and possible trends in the marine background aerosol for the Pacific Northwest. For the Crater Lake samples, the data have been segregated using 10 day back isentropic trajectories to evaluate the role of transport. Our analysis of the segregated data indicates that the trajectories can successfully separate “locally influenced” from “marine background” aerosol, but are not able to identify a significant difference in the mean concentrations during marine vs Asian transport pathways.The background marine aerosol has an annual mean and median concentrations of 2.0 and 1.5 μg m⁻³, respectively, for particles less than 2.5 μm diameter. There is a seasonal pattern in all components of the aerosol mass, with a summer maximum and winter minimum. This pattern is most likely due to the strong seasonal pattern in precipitation, which peaks in winter, combined with enhanced sources in summer. The Crater Lake marine aerosol composition is dominated by organics (∼40% by mass), with smaller contributions from sulfates, mineral dust and elemental carbon. Analysis of the background marine aerosol found no apparent trend since 1988. This is in contrast to results reported by Prospero et al. (J. Geophys. Res. 108 (2003) 4019) for nss-SO₄²⁻ samples from Midway Island in the North Pacific. Comparison of the mean concentrations for each site shows that the Midway samples are significantly more influenced by Asian industrial sources of sulfur, compared to Crater Lake, which implies a substantial loss of nss-SO₄²⁻ from Asian sources that occurs during transit across the Pacific to Crater Lake due to precipitation scavenging.     

The relationship of sulfur emissions to sulfate in precipitation—II. Gas phase processes

A climatological box model is applied to wet deposition of sulfur in eastern North America using the extreme assumption that all wet-deposited sulfates originate in sulfate aerosol. The measured sulfate in precipitation during 1977–1979 constrains the probability that an SO₂ molecule emitted in the eastern United States is oxidized before deposition or outflow from the region to values greater than 0.5 and more likely near 1.0. This result implies that uniform SO₂ emission reductions will produce nearly proportional reductions in wet sulfates originating in those emissions and deposited on land. A similar result was obtained previously using the more likely assumption that oxidation and removal of SO₂ in precipitating clouds is the major source of wet deposition of sulfur. Therefore, it is argued that uniform regional reductions in annual average SO₂ emissions will produce nearly proportional reductions in wet sulfur deposited on land and originating in those emissions. The amount of wet sulfate deposition is demonstrated to constrain the mean scale of transport along air parcel trajectories for the precursor of wet sulfur, whether SO₂ or sulfate aerosol, to values greater than 900 km. An examination of previous microscopic photochemical models indicates that the sulfate aerosol formation rate is roughly proportional to local SO₂ concentrations, an inference which is consistent with the result of the climatological model.     

Influence of ship emissions on air quality and input of contaminants in southern Alaska National Parks and Wilderness Areas during the 2006 tourist season

The impact of ship emissions on air quality in Alaska National Parks and Wilderness Areas was investigated using the Weather Research and Forecasting model inline coupled with chemistry (WRF/Chem). The visibility and deposition of atmospheric contaminants was analyzed for the length of the 2006 tourist season. WRF/Chem reproduced the meteorological situation well. It seems to have captured the temporal behavior of aerosol concentrations when compared with the few data available. Air quality follows certain predetermined patterns associated with local meteorological conditions and ship emissions. Ship emissions have maximum impacts in Prince William Sound where topography and decaying lows trap pollutants. Along sea-lanes and adjacent coastal areas, NO_x, SO₂, O₃, PAN, HNO₃, and PM_2.5 increase up to 650 pptv, 325 pptv, 900 pptv, 18 pptv, 10 pptv, and 100 ng m^?3. Some of these increases are significant (95% confidence). Enhanced particulate matter concentrations from ship emissions reduce visibility up to 30% in Prince William Sound and 5–25% along sea-lanes.     

Surface ozone at four remote island sites and the preliminary assessment of the exceedances of its critical level in Japan

Analysis of the recent surface ozone data at four remote islands (Rishiri, Oki, Okinawa, and Ogasawara) in Japan indicates that East Asian anthropogenic emissions significantly influence the boundary layer ozone in Japan. Due to these regional-scale emissions, an increase of ozone concentration is observed during fall, winter, and spring when anthropogenically enhanced continental air masses from Siberia/Eurasia arrive at the sites. The O₃ concentrations in the “regionally polluted” continental outflow among sites are as high as 41–46 ppb in winter and 54–61 ppb in spring. Meanwhile, marine air masses from the Pacific Ocean show as low as 13–14 ppb of O₃ at Okinawa and Ogasawara in summer but higher O₃ concentrations, 24–27 ppb, are observed at Oki and Rishiri due to the additional pollution mainly from Japan mainland. The preliminary analysis of the exceedances of ozone critical level using AOT40 and SUM06 exposure indices indicates that the O₃ threshold were exceeded variously among sites and years. The highest AOT40 and SUM06 were observed at Oki in central Japan where the critical levels are distinctly exceeded. In the other years, the O₃ exposures at Oki, Okinawa, and Rishiri are about or slightly higher than the critical levels. The potential risk of crop yields reduction from high level of O₃ exposure in Japan might not be a serious issue during 1990s and at present because the traditional growing season in Japan are during the low O₃ period in summer. However, increases of anthropogenic emission in East Asia could aggravate the situation in the very near future.     

Trans-boundary air pollution over remote islands in Japan: observed data and estimates from a numerical model

Observations of air pollutants were conducted in remote Japanese islands (Oki Island and Okinawa Island) in early spring to clarify the extent of trans-boundary air pollution from the Asian continent. A three-dimensional Eulerian model calculation, which included parameters on emission, transport and transformation of sulfur oxides, nitrogen oxides and ammonia, was performed to compile sulfate isosurface concentrations over the observational sites. Concentrations of non-sea-salt sulfate (nss-SO₄²⁻) of greater than 10 μg m⁻³ were observed at Oki after the northeastward passage of low-pressure systems in the Sea of Japan. At these times, the weather showed a typical winter pattern and air pollutants over China were transported southeastward to Japan with the northwesterly wind. The model calculation reproduced the observed variations of nss-SO₄²⁻ concentration well, except for one case in which the model calculation could not reproduce the extremely low nss-SO₄²⁻ concentration observed on 8 March. In Hedo (Okinawa Island), we observed long-lasting (3 days) medium concentrations of nss-SO₄²⁻ (approximately 5 μg m⁻³). Although the model reproduced these observed medium concentrations well, in general the observed results were reproduced better for Oki than for Hedo. Under the synoptic weather conditions of early spring, high concentrations of nss-sulfate were sometimes transported to these remote Japanese islands from areas of continental Asia with a strong outflow of air pollutants.     

Chemical compositions and radiative properties of dust and anthropogenic air masses study in Taipei Basin, Taiwan, during spring of 2004

Asia is one of the major sources of not only mineral dust but also anthropogenic aerosols. Continental air masses associated with the East Asian winter monsoon always contain high contents of mineral dust and anthropogenic species and transported southeastward to Taiwan, which have significant influences on global atmospheric radiation transfer directly by scattering and absorbing solar radiation in each spring. However, few measurements for the long-range transported aerosol and its optical properties were announced in this area, between the Western Pacific and the southeastern coast of Mainland China. The overall objective of this work is to quantify the optical characteristics of different aerosol types in the Eastern Asian. In order to achieve this objective, meteorological parameters, concentrations of PM₁₀ and its soluble species, and optical property of atmospheric scattering coefficients were measured continuously with 1 h time-resolved from 11 February to 7 April 2004 in Taipei Basin (25°00′N, 121°32′E). In this work, the dramatic changes of meteorological parameters such as temperature and winds were used to determine the influenced period of each air mass. Continental, strong continental, marine, and stagnant air masses defined by the back-trajectory analysis and local meteorology were further characterized as long-range transport pollution, dust, clean marine, and local pollution aerosols, respectively, according to the diagnostic ratios. The aerosol mass scattering efficiency of continental pollution, dust, clean marine, and local pollution aerosols were ranged from 1.3 to 1.6, 0.7 to 1.0, 1.4 and 1.4 to 2.3 m² g⁻¹, respectively. Overall, there are two distinct populations of aerosol mass scattering efficiencies, one for an aerosol chemical composition dominated by dust (<1.0 m² g⁻¹) and the other for an aerosol chemical composition dominated by anthropogenic pollutants (1.3–2.3 m² g⁻¹), which were similar to the previous measurements with high degree of temporal resolution.     

The aging process of naturally emitted aerosol (sea-salt and mineral aerosol) during long range transport

The aging processes of two representative natural aerosol, sea-salt and mineral aerosol, are investigated by using a box model equipped with a thermodynamic module (SCAPE). The model is shown to successfully describe the aging processes between the gas-phase anthropogenic pollutants (SO₂, NO_x, and NH₃) and primary aerosol particles, including self-neutralization process/chlorine depletion in the sea-salt aerosol; formation/dissipation of carbonate and bicarbonate ions in the mineral aerosol; irreversible dynamic deposition of SO₂ and H₂SO₄; and reversible thermodynamic distribution of inorganic volatile species. It is found that SO₂ and H₂SO₄ tend to deposit onto the mode with the largest surface area, and that ammonia deposition is controlled by preceding SO₂/H₂SO₄ deposition. During the SO₂/H₂SO₄ deposition, chloride and carbonate are continuously released from the sea-salt and mineral dust particles, respectively. The findings by the model predictions are consistent with field and observational studies.     

A simulation of sulfur wet deposition and its dependence on the inflow of sulfur species to storms

Numerical precipitation scavenging models are used to investigate the relationship between the inflow concentrations of sulfur species to precipitation systems and the resulting sulfur wet deposition. Simulations have been made for summer and winter seasons using concentration ranges of SO₂, aerosol SO₄²⁻, H₂O₂ and O₃ appropriate for the eastern U.S. summer simulations use one-dimensional timedependent convective cloud and scavenging models; winter simulations use two-dimensional steady-state warm-frontal models. Sulfur scavenging mechanisms include nucleation scavenging of aerosol, aqueous reactions of H₂O₂, O₃ and HCHO with S(IV), and nonreactive S(IV) scavenging. Over the wide range of conditions that have been examined, the relation between sulfur inflow and sulfur wet deposition varies from nearly linear to strongly nonlinear. The degree of nonlinearity is most affected by aerosol SO₄²⁻ levels and relative levels of SO₂ vs H₂O₂. Higher aerosol SO₄²⁻ levels (as found in summer) produce a more linear relation. The greatest nonlinearity occurs when SO₂ exceeds H₂O₂. Winter simulations show more nonlinearity than summer simulations.     

Modeling study of the potential importance of heterogeneous surface reactions for NOx transformations in plumes

A parametric model of gas-particle surface reactions is incorporated into a reactive plume model and used to assess the potential importance of heterogeneous surface reactions on gas phase plume chemistry. Heterogeneous loss of the following species is found to be potentially significant: H₂O₂, PAN, NO₃, N₂O₅, OH, HO₂ and in cold weather HO₂NO₂. This simple model is unable to account for equilibrium/capacity effects in the condensed phase and therefore cannot be used for SO₂ and HNO₃ reaction with aerosol surface.     

Interactions of Sulfur Dioxide with Insoluble Suspended Particulate Matter

A laboratory study was conducted of the heterogeneous catalysis of sulfur dioxide at ppm concentrations in air by insoluble particles of CaCO₂, V₂O₅, Fe₂0₃, flyash from a coal-burning power plant, MnCO₂, activated carbon, and suspended particulate matter from urban air. The investigalion was performed by utilizing a new technique for aerosol stabilization which consists of depositing the aerosol on Teflon beads in a fluidized bed. The Teflon beads with deposited aerosol particles were then packed into a flow reactor. Progress of the chemical reaction of SO₂ with deposited particles was continuously monitored by determining the SO₂ concentrations in the reactor effluent with a microcoulometer.

In this investigation, CaCOg, V₂O₅, and flyash were essentially inert to SO₂ at room temperature. Fe₂O₃, activated carbon, MnO₂, and suspended particulate matter from urban air sorbed SO₂ from air streams with up to 14.4 ppm SO₂ in air. Evidence is presented which suggests that a substantial part of the sorbed SO₂ was physically adsorbed.

Bioassay procedures which utilize pulmonary flow resistance changes in guinea pigs to monitor response to inhaled SO₂-aerosol mixtures in air have indicated the weak or non-potentiating capacity of insoluble aerosols as contrasted to soluble aerosols. Potentiating response of an aerosol appears to be strongly associated with reaction of SO₂ in a water droplet containing aerosol ions and not with physically adsorbed SO₂ on an insoluble aerosol.     

Process analysis of a regional air pollution episode over Pearl River Delta Region,China, using the MM5-CMAQ model

This study focuses on the influences of a warm high-pressure meteorological system on aerosol pollutants, employing the simulations by the Models-3/CMAQ system and the observations collected during October 10–12, 2004, over the Pearl River Delta (PRD) region. The results show that the spatial distributions of air pollutants are generally circular near Guangzhou and Foshan, which are cities with high emissions rates. The primary pollutant is particulate matter (PM) over the PRD. MM5 shows reasonable performance for major meteorological variables (i.e., temperature, relative humidity, wind direction) with normalized mean biases (NMB) of 4.5–38.8% and for their time series. CMAQ can capture one peak of all air pollutant concentrations on October 11, but misses other peaks. The CMAQ model systematically underpredicts the mass concentrations of all air pollutants. Compared with chemical observations, SO₂ and O₃ are predicted well with a correlation coefficient of 0.70 and 0.65. PM_2.5 and NO are significantly underpredicted with an NMB of 43% and 90%, respectively. The process analysis results show that the emission, dry deposition, horizontal transport, and vertical transport are four main processes affecting air pollutants. The contributions of each physical process are different for the various pollutants. The most important process for PM₁₀ is dry deposition, and for NO_x it is transport. The contributions of horizontal and vertical transport processes vary during the period, but these two processes mostly contribute to the removal of air pollutants at Guangzhou city, whose emissions are high. For this high-pressure case, the contributions of the various processes show high correlations in cities with the similar geographical attributes. According to the statistical results, cities in the PRD region are divided into four groups with different features. The contributions from local and nonlocal emission sources are discussed in different groups.

Implications: The characteristics of aerosol pollution episodes are intensively studied in this work using the high-resolution modeling system MM5/SMOKE/CMAQ, with special efforts on examining the contributions of different physical and chemical processes to air concentrations for each city over the PRD region by a process analysis method, so as to provide a scientific basis for understanding the formation mechanism of regional aerosol pollution under the high-pressure system over PRD.     

Field observations of regional and urban impacts on NO2, ozone,UVB, and nitrate radical production rates in the Phoenix air basin

In the May and June of 1998, field measurements were taken at a site near the Usery Pass Recreation Area, ∼27 miles from the downtown Phoenix area, overlooking Phoenix and Mesa, Arizona. This site was selected to examine the impacts of the Phoenix urban plume on the Usery Pass Recreation Area and surrounding regions. Data were obtained for ultraviolet-B (UVB) radiation, nitrogen dioxide (NO₂), peroxyacetyl nitrate (PAN), ozone (O₃), and carbon monoxide (CO). Nocturnal plumes of NO₂ (in tens of ppb), observed near midnight, were correlated with CO and anti-correlated with O₃. This behavior was consistent with the titration of locally generated NO by boundary layer O₃ to form the nighttime NO₂ plumes that were subsequently transported into the Usery Pass Recreation area. Nitrate radical (NO₃) production rates were calculated to be very high on the edges of these nocturnal plumes. Examination of O₃ and PAN data also indicates that Phoenix is being affected by long-range transport of pollutants from the Los Angeles to San Diego areas. A regional smoke episode was observed in May, accompanied by a decrease in UVB of factor of two and a decrease in O₃ and an increase in methyl chloride. Low level back trajectories and chemical evidence confirm that the smoke event originated in northern Mexico and that the reduced O₃ levels observed at Usery Pass could be partially due to reduced photolysis rates caused by carbonaceous soot aerosols transported in the smoke plume. The results are discussed with regard to potential effects of local pollution transport from the Phoenix air basin as well as an assessment of the contributions from long-range transport of pollutants to the background levels in the Phoenix-Usery Pass area.     

A second generation model for regional-scale transport/chemistry/deposition

The regional-scale transport, chemistry and deposition of acidifying compounds, photochemical oxidants, and their precursors are analyzed using a second-generation Eulerian model. The important atmospheric processes are incorporated using chemical, dynamical and thermodynamical parameterizations having sufficient detail to accommodate boundary layer-free troposphere exchange in cloudy and cloud-free environments, and in-cloud and below-cloud wet removal and chemistry. Forty-one species are considered, many of which are also present in the liquid-drop phases. In the regional scale transport, the advected species are NO, NO₂, SO₂, SO⁻²₄, O₃, HNO₃, NH₃, PAN, H₂O₂, HCHO, alkanes, C₂H₄, other olefins, aromatics, RCHO, ROOH, HNO₂, RONO₂ and RO₂NO₂. The model capabilities are illustrated by showing simulations in which non-precipitating clouds are present to absorb gas-phase species, chemically alter these, and then release them to the atmosphere.     

Continuous measurement of peroxyacetyl nitrate (PAN) in suburban and remote areas of western China

Knowledge on atmospheric abundance of peroxyacetyl nitrate (PAN) is important in assessing the severity of photochemical pollution, and for understanding chemical transformation of reactive odd nitrogen and its impact on the budget of tropospheric ozone (O₃). In summer 2006, continuous measurements of PAN were made using an automatic GC–ECD analyzer with an on-line calibrator at a suburban site of Lanzhou (LZ) and a remote site of Mt. Waliguan (WLG) in western China, with concurrent measurements of O₃, total reactive nitrogen (NO_y) and carbon monoxide (CO). At LZ, several photochemical episodes were observed during the study, and the average mixing ratio of PAN (plus or minus standard deviation) was 0.76 (±0.89) ppbv with the maximum value of 9.13 ppbv, compared to an average value of 0.44 (±0.16) ppbv at remote WLG. The PAN mixing ratios in LZ exhibited strong diurnal variations with a maximum at noon, while enhanced concentrations of PAN were observed in the evening and a minimum in the afternoon at WLG. The daily O₃ and PAN concentration maxima showed a strong correlation (r² = 0.91) in LZ, with a regression slope (PAN/O₃) of 0.091 ppbv ppbv^?1. At WLG, six well-identified pollution plumes (lasting 2–8 h) were observed with elevated concentrations of PAN (and other trace gases), and analysis of backward particle release simulation shows that the high-PAN events at WLG were mostly associated with the transport of air masses that had passed over LZ.