Estimating the impact of Saharan dust on the year 2001 PM10 record of Rome,Italy

This paper evaluates the role of Saharan dust advection in the exceeding of the PM₁₀ thresholds in the city of Rome, Italy. To this purpose, a series of observations and model forecasts recorded in the year 2001 are analysed and discussed. Lidar profiles collected over 168 days of the year are employed to both assess the presence and magnitude of Saharan dust layers over the city and to evaluate the depth of the planetary boundary layer. Backtrajectories are used to verify the Saharan origin of the lidar-sounded air masses. Model predictions of the presence of Saharan dust over the area are employed to fill the time gaps between lidar observations. PM₁₀ and carbon monoxide records of both a city background (Villa Ada) and a heavy traffic station (Magna Grecia) are cross-analysed with the dust events record and meteorological data. The analysis shows that: (1) Saharan dust was advected over Rome on about 30% of the days of 2001; (2) mean contribution of Saharan dust transport events to daily PM₁₀ levels was of the order of 20 μg m⁻³; (3) at the urban background station of Villa Ada, the Saharan contribution caused the surpassing of the maximum number of days in excess of 50 μg m⁻³ fixed by the current legislation (35 per year). Conversely, at the heavy traffic station of Magna Grecia the Saharan contribution was not determinant at causing the observed large exceeding of that limit, as well as of the maximum yearly average of 40 μg m⁻³; (4) 25% of the Saharan advection days (of the order of 100/year at Rome) led to a PM₁₀ increase >30 μg m⁻³, 4% caused an increase >50 μg m⁻³, thus leading on their own to surpassing the 50 μg m⁻³ daily limit.     

Influence of air mass trajectories on the chemical composition of precipitation in India

Chemical composition of precipitation was measured with wet-only samplers at a rural site at Bhubaneswar in eastern India during 1997–1998. All rain events were compared with trajectories and precipitation fields from the ECMWF. The pH and ionic concentrations were found to vary systematically with the origin of air and the amount of rainfall along the trajectory. A seasonal cycle for pH was found with a monthly median pH below 5.0 during October–December. The highest monthly median concentration of Ca²⁺ was found in May with 20 μmol l⁻¹ and for SO₄²⁻ in January with 52 μmol l⁻¹. Samples with trajectories within 400 km from Bhubaneswar during the last 5 days were found to have a median pH slightly below 5.0 as an average. These samples also had the highest concentration for all measured ions, indicating large pollution sources within the region. Samples with continental origin showed a decrease of ∼70% in concentration if there had been rain during >50% of the last 5 days compared to rain during <50% of the last 5 days. High concentrations of Na⁺ and Cl⁻ were also found in continental samples. Resuspension of previously deposited sea salt is believed to be the reason. The data were compared with data from three other sites in western India and higher concentrations of almost all ions (NH₄⁺ being the exception) compared to Bhubaneswar were found at the west coast in monsoon samples.     

SPM and fungal spores in the ambient air of west Korea during the Asian dust (Yellow sand) period

The relationship between suspended particulate matter (SPM) and fungal spore was investigated in Seosan, a rural county along the west coast of Korea, in the spring of 2000. SPM concentrations in the air were 199.8 μg m⁻³ in the first Asian dust period (23–24 March), 249.4 μg m⁻³ in the second Asian dust period (7–9 April) and 98.9 μg m⁻³ in the non-Asian dust period (12–16 May), respectively. The majority of the total SPM were composed of coarse particles sized about 5 μm during the two Asian dust periods. Four molds genera grown from airborne fungal spores were identified in colonies grown from SPM samples taken during the Asian dust periods. All the genera found, Fusarium, Aspergillus, Penicillium and Basipetospora, are hyphomycetes in the division Deuteromycota. Morphologically, more diversified mycelia of hyphomycetes were grown on the sample captured from 1.1 to 2.1 μm sized SPM than on the other sized samples gathered in the dust periods. On the other hand, no mold was observed on the sample of 1.1–2.1 μm sized SPM in the non-Asian dust period. From these results, it seems evident that several sorts of fine sized fungal spores were suspended in the atmospheric environment of this study area during Asian dust periods.     

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.     

Chemical composition of snowfall in the high Arctic: 1990–1994

From 1990 to 1994 at Alert, Nunavut, Canada, weekly snow samples were collected under low wind conditions to avoid contamination by blowing snow. They were analysed for major ions, Br⁻, and the organic ions methylsulphonate, formate, acetate and propionate. In the Arctic, where annual precipitation is low and blowing snow is common, these observations are unique. On an equivalent weight basis, acids and sea salt in snowfall are mixed approximately equally from December to January but from March to May acids dominate. The acidity of snowfall increases progressively throughout the winter to a May peak of ∼16 μeq l⁻¹. SO₄²⁻, Br⁻, and the organic acids acetate, and propionate peak in snowfall after polar sunrise indicate the influence of enhanced photochemical reactions. The greater enrichment of halides relative to sea salt Na⁺ in snow compared to aerosols indicates that gaseous uptake by snowflakes is important in the removal of these substances from the atmosphere and their deposition on to the Earth's surface. There is a marked difference between the seasonal variation of enrichment of Cl⁻ and Br⁻ in snow. The latter show a marked increase after polar sunrise while the former does not. These results provide valuable baseline information on the ionic content of fresh snowfall to be used in understanding the results of snowpack chemistry and post-depositional process studies conducted in the high Arctic.     

Aerosol scattering properties in northern China

The aerosol scattering properties were investigated at two continental sites in northern China in 2004. Aerosol light scattering coefficient (σ_sp) at 525 nm, PM₁₀, and aerosol mass scattering efficiencies (α) at Dunhuang had a mean value of 165.1±148.8 M m⁻¹, 157.6±270.0 μg m⁻³, and 2.30±3.41 m² g⁻¹, respectively, while these values at Dongsheng were, respectively, 180.2±151.9 M m⁻¹, 119.0±112.9 μg m⁻³, and 1.87±1.41 m² g⁻¹. There existed a seasonal variability of aerosol scattering properties. In spring, at Dunhuang PM₁₀, σ_sp, and α were 184.1±211.548 μg m⁻³, 126.3±89.6 M m⁻¹, and 1.05±0.97 m² g⁻¹, respectively, and these values at Dongsheng were 146.4±142.1 μg m⁻³, 183.4±81.7 M m⁻¹, and 1.98±1.52 m² g⁻¹, respectively. However, in winter at Dunhuang PM₁₀, σ_sp, and α were 158.1±261.4 μg m⁻³, 303.3±165.2 M m⁻¹, and 3.17±1.93 m² g⁻¹, respectively, and these values at Dongsheng were 155.7±170.1 μg m⁻³, 304.4±158.1 M m⁻¹, and 2.90±1.72 m² g⁻¹, respectively. σ_sp and α in winter were higher than that in spring at both the sites, which coincides with the characteristics of dust aerosol and pollution aerosol. Overall, the dominant aerosol types in spring and winter at both sites in northern China are dust aerosol and pollution aerosol, respectively.     

PM2.5 particles and size-segregated ionic species measured during fall season in three urban sites in Korea

Twelve hours integrated fine particles (PM_2.5) and 24-h average size-segregated particles were collected to investigate the chemical characteristics and to determine the size distribution of ionic species during October–December 1999 in three cities of different urban scale; Chongju, Kwangju, and Seoul, Korea. Concentrations of 5-min PM_2.5 black carbon (BC) and hourly criteria air pollutants (PM₁₀, CO, NO_x, SO₂, and O₃) were also measured using the Aethalometer and ambient air monitoring system, respectively.Highest PM_2.5 mass concentrations at Chongju, Kwangju, and Seoul sites were 63.0, 77.9, and 143.7 μg m⁻³, respectively. For the time period when highest PM_2.5 mass occurred, BC level out of PM_2.5 chemical species was highest at both Chongju and Kwangju, and highest NO₃⁻ (23.6 μg m⁻³) followed by BC (23.1 μg m⁻³) were observed at Seoul site, indicating that highest PM_2.5 pollution is closely associated with the traffic emissions. Strong relationships of Fe with BC and Zn at both Kwangju and Seoul sites support that the Fe and Zn measured there are originated partly from same source as BC, i.e. diesel traffics. However, it is suggested that the Fe measured at Chongju is most likely derived from dispersion of soil dust.The size distributions of SO₄²⁻, NO₃⁻, and NH₄⁺ ionic species indicated similar unimodal distributions at all sampling sites. However, different unimodal patterns in the accumulation mode size range with a peak in the smaller size (0.28–0.53 μm, condensation mode) in both Kwangju and Seoul, and in the relatively larger size (0.53–1.0 μm, droplet mode) in Chongju, were found. The potassium ion under the study sites dominates in the fine mode, and its size distribution showed unimodal character with a maximum in the size range 0.56–1.0 μm.     

Chemical composition of aerosols during a major biomass burning episode over northern Europe in spring 2006: Experimental and modelling assessments

The long-range transported smokes emitted by biomass burning had a strong impact on the PM_2.5 mass concentrations in Helsinki over the 12 days period in April and May 2006. To characterize aerosols during this period, the real-time measurements were done for PM_2.5, PM_2.5–10, common ions and black carbon. Moreover, the 24-h PM₁ filter samples were analysed for organic and elemental carbon (OC and EC), water-soluble organic carbon (WSOC), ions and levoglucosan. The Finnish emergency and air quality modelling system SILAM was used for the forecast of the PM_2.5 concentration generated by biomass burning. According to the real-time PM_2.5 data, the investigated period was divided into four types of PM situations: episode 1 (EPI-1; 25–29 April), episode 2 (EPI-2; 1–5 May), episode 3 (EPI-3; 5–6 May) and a reference period (REF; 24 March–24 April). EPI-3 included a local warehouse fire and therefore it is discussed separately. The PM₁ mass concentrations of biomass burning tracers—levoglucosan, potassium and oxalate—increased during the two long-range transport episodes (EPI-1 and EPI-2). The most substantial difference between the episodes was exhibited by the sulphate concentration, which was 4.9 (±1.4) μg m⁻³ in EPI-2 but only 2.4 (±0.31) μg m⁻³ in EPI-1 being close to that of REF (1.8±0.54 μg m⁻³). The concentration of particulate organic matter in PM₁ was clearly higher during EPI-1 (11±3.3 μg m⁻³) and EPI-2 (9.7±4.0 μg m⁻³) than REF (1.3±0.45 μg m⁻³). The long-range transported smoke had only a minor impact on the WSOC-to-OC ratio. According to the model simulations, MODIS detected the fires that caused the first set of concentration peaks (EPI-1) and the local warehouse fire (EPI-3), but missed the second one (EPI-2) probably due to dense frontal clouds.     

Glaciochemical records from a Mt. Everest ice core: relationship to atmospheric circulation over Asia

Glaciochemical records recovered from an 80.4 m ice core in the East Rongbuk (ER) Glacier (elevation: 6450 m) on the northern slope of Mt. Everest provide a reconstructing of past climate for the period AD 1846–1997. Empirical orthogonal function (EOF) analysis on the eight major ion (SO₄²⁻, Mg²⁺, Ca²⁺, Na⁺, Cl⁻, NH₄⁺, K⁺, and NO₃⁻) time-series reveals inter-species relations and common structure within the ER glaciochemical data. The first two EOF series (EOF1-ions and EOF2-ions) are compared with instrumental data of sea level pressure (SLP) to demonstrate that the EOF-ions series display strong connections to winter (January) and summer (July) SLP over the Mongolian region. The positive relationship between EOF1-ions and the Mongolian High (MongHi) series suggests that enhanced winter MongHi strengthens the transport of dust aerosols southward from arid regions over central Asia to Mt. Everest. The close correspondence between EOF2-ions and the summer Mongolian Low (MongLow) indicates that the deeper MongLow, which is related to the stronger Indian Monsoon, contributes to a decrease in summer dust aerosols. Therefore, the ER ice core record comprises two assemblages of crustal species, each transported from different source regions during different seasons. EOF1-ions represents the majority of the crustal species and is related to winter atmospheric circulation patterns. These species are mainly transported from arid regions of central Asia during the winter dry season. EOF2-ions represents crustal species transported by summer atmospheric circulation from local/regional sources in the northern and southern Himalayas.     

Atmospheric concentrations of ammonia and ammonium at an agricultural site in the southeast United States

In this study, we present ∼1 yr (October 1998–September 1999) of 12-hour mean ammonia (NH₃), ammonium (NH₄⁺), hydrochloric acid (HCl), chloride (Cl⁻), nitrate (NO₃⁻), nitric acid (HNO₃), nitrous acid (HONO), sulfate (SO₄²⁻), and sulfur dioxide (SO₂) concentrations measured at an agricultural site in North Carolina's Coastal Plain region. Mean gas concentrations were 0.46, 1.21, 0.54, 5.55, and 4.15 μg m⁻³ for HCl, HNO₃, HONO, NH₃, and SO₂, respectively. Mean aerosol concentrations were 1.44, 1.23, 0.08, and 3.37 μg m⁻³ for NH₄⁺, NO₃⁻, Cl⁻, and SO₄²⁻, respectively. Ammonia, NH₄⁺, HNO₃, and SO₄²⁻ exhibit higher concentrations during the summer, while higher SO₂ concentrations occur during winter. A meteorology-based multivariate regression model using temperature, wind speed, and wind direction explains 76% of the variation in 12-hour mean NH₃ concentrations (n=601). Ammonia concentration increases exponentially with temperature, which explains the majority of variation (54%) in 12-hour mean NH₃ concentrations. Dependence of NH₃ concentration on wind direction suggests a local source influence. Ammonia accounts for >70% of NH_x (NH_x=NH₃+NH₄⁺) during all seasons. Ammonium nitrate and sulfate aerosol formation does not appear to be NH₃ limited. Sulfate is primarily associated ammonium sulfate, rather than bisulfate, except during the winter when the ratio of NO₃⁻–NH₄⁺ is ∼0.66. The annual average NO₃⁻–NH₄⁺ ratio is ∼0.25.     

Aerosol radiative forcing over the Indo-Gangetic plains during major dust storms

Indo-Gangetic (IG) alluvial plains, one of the largest river basins in the world, suffers from the long range transport of mineral dust from the western arid and desert regions of Africa, Arabia and Rajasthan during the summer (pre-monsoon season, April–June). These dust storms influence the aerosol optical depth (AOD) across the IG plains. The Kanpur AERONET (Aerosol Robotic Network) station and Moderate Resolution Imaging Spectro-radiometer (MODIS) data show pronounced effect on the aerosol optical properties and aerosol size distribution during major dust storm events over the IG plains that have significant effect on the aerosol radiative forcing (ARF). The multi-band AOD, from AERONET and MODIS, show contrasting changes in wavelength dependency over dust affected regions. A time collocated (±30 min) validation of AERONET AOD with MODIS Terra (level 2 swath product) over Kanpur, at a common wavelength of 550 nm for the period 2001–2005 show moderate correlation (R²∼0.6) during the summer season. The average surface forcing is found to change by −23 W m⁻² during dust events and the top of the atmosphere (TOA) forcing change by −11 W m⁻² as compared to the non-dusty clear-sky days. A strong correlation is found between AOD at 500 nm and the ARF. At surface, the correlation coefficient between AOD and ARF is found to be high (R²=0.925) and is found to be moderate (R²=0.628) at the TOA. The slope of the regression line gives the aerosol forcing efficiency at 500 nm of about −46±2.6 W m⁻² and −17±2.5 W m⁻² at the surface and the TOA, respectively. The ARF is found to increase with the advance of the dry season in conjunction with the gradual rise in AOD (at 500 nm) from April (0.4–0.5) to June (0.6–0.7) over the IG plains.     

Characterization,identification of road dust PAHs in central Shanghai areas,China

Road dust samples were collected from central Shanghai in winter (January) and summer (August), respectively. Sixteen polycyclic aromatic hydrocarbons (PAHs) in the United States Environmental Protection Agency (USEPA) priority-controlled list were determined by GC/MS. Total PAH (t-PAH) concentrations in winter samples ranged from 9176 to 32,573 ng g⁻¹ with a mean value of 20,648 ng g⁻¹, while they varied from 6875 to 27,766 ng g⁻¹ in summer with an average of 14,098 ng g⁻¹. Spatial variation showed that city park (CP) samples had the lowest t-PAH concentration, while industrial area (ID) and traffic area (TR) and commercial area (CO) were the most polluted, in both seasons. PAH homologues concentrations were getting higher with the more rings and higher molecular weight (HMW) in all areas. The study of effective factors showed that grain size was only a minor factor influencing the accumulation of PAHs, whereas total organic carbon (TOC) was found to be closely correlated with t-PAH concentration. Prevailing winds could directly affect on the spatial distribution of PAHs. Chemical source apportionment studies took the form of principal component analysis (PCA), followed by compositional analysis. It was demonstrated that road dust PAHs in central Shanghai mainly came from the mixing of traffic and coal combustion. The contribution percentages of pyrogenic and petrogenic sources were respectively 71.0% and 11.4% in winter, while they were, 64.9% and 14.1% in summer, respectively. Road dust PAHs in Shanghai city mostly came from local sources.     

Transport and evolution of a winter-time Yellow sand observed in Korea

Long-range transport of mineral dust such as Yellow sand (YS) is not restricted to the springtime periods in Northeast Asia. A YS phenomenon was observed during 25–27 January 1999, which was a remarkably distinctive episode in the occurrence time and intensity that had ever observed in the wintertime in Korea. This YS event was traced to be originated from the arid region of central and eastern Asia; the Gobi desert and Loess plateau. The traveling speed of the dust storm was found to be about 70 km h⁻¹ with it's horizontal size of larger than the whole Korean peninsula during this episode. Aerosol mass loadings changed by an order of magnitude within a few hours. The dominant ion components were SO₄²⁻, NO₃⁻, Ca²⁺ and Na⁺ during the passage of YS. The mode diameter of these compounds of YS was around 4 μm, compared to 0.4–0.9 μm after the passage of YS. SO₄²⁻ and NO₃⁻ concentrations were found to be well correlated with Ca²⁺ concentration in the coarse mode during the YS event, whereas they were well correlated with NH₄⁺ concentration during the non-YS period, indicating a significant amount of SO₄²⁻ and NO₃⁻ formations on the Ca²⁺-rich coarse aerosol during the long-range transport of YS.     

An analysis of seasonal surface dust aerosol concentrations in the western US (2001–2004): Observations and model predictions

Long-term surface observations indicate that soil dust represents over 30% of the annual fine (particle diameter less than 2.5 μm) particulate mass in many areas of the western US; in spring and summer, it represents an even larger fraction. There are numerous dust-producing playas in the western US, but surface dust aerosol concentrations in this region are also influenced by dust of Asian origin. This study examines the seasonality of surface soil dust concentrations at 15 western US sites using observations from the Interagency Monitoring of PROtected Visual Environments (IMPROVE) network from 2001 to 2004. Average soil concentrations in particulate matter less than 10 μm in diameter (PM₁₀) were lowest in winter and peaked during the summer months at these sites; however, episodic higher-concentration events (>10 μg m⁻³) occurred in the spring, the time of maximum Asian dust transport to the western US. Simulated surface dust concentrations from the Navy Aerosol Analysis and Prediction System (NAAPS) suggested that long-range transport from Asia dominates surface dust concentrations in the western US in the spring, and that, although some long-range transport does occur throughout the year (1–2 μg m⁻³), locally generated dust plays a larger role in the region in summer and fall. However, NAAPS simulated some anomalously high concentrations (>50 μg m⁻³) of local dust in the fall and winter months over portions of the western US. Differences between modeled and observed dust concentrations were attributed to overestimation of total observed soil dust concentrations by the assumptions used to convert IMPROVE measurements into PM₁₀ soil concentrations, lack of inhibition of model dust production in snow-covered regions, and lack of seasonal agricultural sources in the model.     

Denuder measurements of gas and aerosol species above Arctic snow surfaces at Alert 2000

Gas and aerosol measurements were made during the Polar Sunrise Experiment 2000 at Alert, Nunavut (Canada), using two independent denuder/filter systems for sampling and subsequent analysis by ion chromatography. Twelve to forty-eight hour samples were taken during a winter (9–21 February 2000) and a spring (17 April–5 May 2000) campaign. During the spring campaign, samples were taken at two different heights above the snow surface to investigate concentration differences. Total particulate NO₃⁻ is the most abundant inorganic nitrogen compound during Arctic springtime (mean 137.4 ng m⁻³). The NO₃⁻ fluxes were calculated above the snow surface to help identify processes that control snow–atmosphere exchange of reactive nitrogen compounds. We suggest that the observed fluxes of coarse particle NO₃⁻ via snow deposition may contribute to the nitrogen inventory in the snow surface. Measurements of surface snow provide experimental data that constrain the contribution of dry deposition of coarse particle NO₃⁻ to <7%. Wet deposition in falling snow appears to be the major contributor to the nitrate input to the snow.     

PM2.5–10, PM2.5 and associated water-soluble inorganic species at a coastal urban site in the metropolitan region of Rio de Janeiro

The concentrations of PM_2.5−10, PM_2.5 and associated water-soluble inorganic species (WSIS) were determined in a coastal site of the metropolitan region of Rio de Janeiro, Southeastern Brazil, from October 1998 to September 1999 (n=50). Samples were dissolved in water and analyzed for major inorganic ions. The mean (± standard deviation; median) concentrations of PM_2.5−10 and PM_2.5 were, respectively, 26 (± 16; 21) μg m⁻³ and 17 (± 13; 14) μg m⁻³. Their mean concentrations were 1.7–1.8 times higher in dry season (May–October) than in rainy season (November–April). The WSIS comprised, respectively, 34% and 28% of the PM_2.5−10 and PM_2.5 masses. Chloride, Na⁺ and Mg²⁺ were the predominant ions in PM_2.5−10, indicating a significant influence of sea-salt aerosols. In PM_2.5, SO₄²⁻ (∼97% nss-SO₄²⁻) and NH₄⁺ were the most abundant ions and their equivalent concentration ratio (SO₄²⁻/NH₄⁺ ∼1.0) suggests that they were present as (NH₄)₂SO₄ particles. The mean concentration of (NH₄)₂SO₄ was 3.4 μg m⁻³. The mean equivalent PM_2.5 NO₃⁻ concentration was eight times smaller than those of SO₄²⁻ and NH₄⁺. The PM_2.5 NO₃⁻ concentration in dry season was three times higher than in rainy season, probably due to reaction of NaCl (sea salt) with HNO₃ as a result of higher levels of NO_y during the dry season and/or reduced volatilization of NH₄NO₃ due to lower wintertime temperature. Chloride depletion was observed in both size ranges, although more pronouncely in PM_2.5.     

Nitric acid and the origin and size segregation of aerosol nitrate aloft during BRACE 2002

As part of the BRACE 2002 May field intensive, the NOAA Twin Otter flew 21 missions over terrestrial, marine, and mixed terrestrial and marine sites in the greater Tampa, Florida, airshed including over Tampa Bay and the Gulf of Mexico. Aerosols were collected with filter packs and their inorganic fractions analyzed post hoc with ion chromatography. Anion mass dominated both the fine- (particle diameters ⩽2.5 μm) and coarse-mode (particle diameters 10.0–2.5 μm) inorganic fractions: SO₄²⁻in the fine fraction, 3.7 μg m⁻³ on average and Cl⁻ and NO₃⁻ in the coarse fraction, 0.6 μg m⁻³ on average and 1.4 μg m⁻³ on average, respectively. Ammonium ion dominated the inorganic fine-mode cation mass, averaging 1.2 μg m⁻³, presumably in association with SO₄². Coarse-mode cation mass was dominated by Na⁺, but the concentrations of Ca²⁺ and K⁺ together often equaled or exceeded the Na⁺ mass which was, on average, 0.6 μg m⁻³. Nitrate appeared predominantly in the coarse rather than the fine fraction, as expected, and the fine fraction never contributed >15% of the total NO₃ concentration. Nitric acid dominated the NO₃⁻ contribution from both aerosol size fractions, and constituted at least 45% of the total NO₃ in all samples. Coarse-mode Cl⁻ depletion, and hence NO₃⁻ replacement, reached 100% within the first 4 h of plume travel from the urban core in some samples, although it was most often less than 100% and slightly below the expected 1:1 ratio with coarse-mode NO₃⁻ concentration: the slope of the regression line of NO₃⁻ concentration to Cl⁻ depletion was 0.9 in the coarse fraction. In addition, terrestrial samples were markedly lower in Cl⁻ depletion, and thus in substituted NO₃^–, than were marine and mixed samples: 15–25% depletion in terrestrial samples vs. 50–65% in marine samples with the same air mass age. Thus, we conclude that NO₃⁻ and its progenitor compound HNO₃ were present in the Tampa airshed in insufficient amounts to titrate fully the slightly alkaline coarse-mode particles there, and to replace completely the Cl⁻ from the coarse-mode NaCl.     

Long-term measurements of SO2 dry deposition over Gansu Province,China

Potassium carbonate sulfation plates, monitored monthly for 11 years from 48 sites in 11 cities in Gansu Province, China, provide a crude estimate of cumulative SO₂ dry depositions. Measured SO₂ dry deposition rates were 1.6–472 mg m⁻² day⁻¹ and had seasonal variations with maxima in winter and minima mainly during summer as a result of higher winter and lower summer SO₂ concentrations. The 11-year monthly average SO₂ dry deposition rates are 23.2–248.97 and 11.7–175.6 mg m⁻² day⁻¹ in the eleven cities in winter and summer, respectively. A monthly average SO₂ deposition velocity was also estimated from 0.06 to 9.72 cm s⁻² in the 11 cities studied with a 11-year average maximum value of about 1.1–2.7 cm s⁻² in April and July and a 11-year average minimum value of about 0.2–1.0 cm s⁻¹ in January. The SO₂ dry deposition velocity also exhibits an increasing with wind speed in basins of less than 500 mm annual precipitation. In contrast, due to influences of the relative humidity in valleys of more than 500 mm annual precipitation, it shows a decreasing trend with wind speed increasing.     

The impact of transpacific transport of mineral dust in the United States

We use a global chemical transport model (GEOS-Chem) to estimate the impact of transpacific transport of mineral dust on aerosol concentrations in North America during 2001. We have implemented two dust mobilization schemes in the model (GOCART and DEAD) and find that the best simulation of North American surface observations with GEOS-Chem is achieved by combining the topographic source used in GOCART with the entrainment scheme used in DEAD. This combination restricts dust emissions to year-round arid areas but includes a significant wind threshold for dust mobilization. The model captures the magnitude and seasonal cycle of observed surface dust concentrations over the northern Pacific. It simulates the free tropospheric outflow of dust from Asia observed in the TRACE-P and ACE-Asia aircraft campaigns of spring 2001. It reproduces the timing and distribution of Asian dust outbreaks in North America during April–May. Beyond these outbreaks we find persistent Asian fine dust (averaging 1.2 μg m⁻³) in surface air over the western United States in spring, with much weaker influence (0.25 μg m⁻³) in summer and fall. Asian influence over the eastern United States is 30–50% lower. We find that transpacific sources accounted for 41% of the worst dust days in the western United States in 2001.     

Characteristics of regional nucleation events in urban East St. Louis

Continuous measurements of aerosol size distributions (3 nm–2 μm) were carried out over a 26 month period (1 April 2001–31 May 2003; 650 days with valid data) in urban East St. Louis, IL, as a part of the US Environmental Protection Agency's Supersite program. This paper analyzes data for the 155 days on which “regional nucleation events” were observed during this study. Such events were observed during every month of the study except January 2003. We observed some differences, however, between events in the summer (defined here as April–September) and winter (December–February). Regional nucleation events were observed more frequently in summer months (36±13% of days) than in winter (8±7%), and nucleated particles grew faster in the summer (6.7±4.8 nm h⁻¹) than in winter (1.8±1.9 nm h⁻¹). The daily maximum in the number concentration of nanoparticles formed by nucleation (4.8±3.5×10⁴ cm⁻³) was highly variable and showed no clear seasonal dependence. Particle formation increased particle concentrations by an average factor of 3.1±2.8. Maximum daily rates of 3 nm particle production (17±20 cm⁻³ s⁻¹) were also highly variable and without a clear seasonal dependence. During these events, particle formation rates were typically near their maxima at 08:00–09:00 a.m., but particle production sometimes persisted at diminishing rates until late in the afternoon (15:00–16:00 p.m.).