Chemical composition of the fine and coarse fraction of aerosols in the northeastern Mediterranean

Two-stage aerosol samples (PM_10–2.5 and PM_2.5) were collected at a coastal rural site located in the northeastern Mediterranean, between April 2001 and 2002. A total of 562 aerosol samples were analyzed for trace elements (Fe, Ti, Mn, Ca, V, Ni, Zn, Cr) and water-soluble ions (Na⁺, NH₄⁺, K⁺, Mg²⁺, Ca²⁺, Cl⁻, Br⁻, NO₃⁻, SO₄²⁻, C₂O₄²⁻ and MS⁻:methane sulfonate). PM₁₀, crustal elements, sea salt aerosols and NO₃⁻ were mainly associated with the coarse mode whereas non-sea salt (nss)SO₄²⁻, C₂O₄²⁻; MS⁻, NH₄⁺, Cr and Ni were found predominantly in the fine fraction. Concentrations of aerosol species exhibited orders of magnitude change from day to day and the aerosol chemical composition is heavily affected by dust events under the influence of airflow from North Africa. During the sampling period, 11 specific mineral dust events of duration varying from 1 day to a week have been identified and their influence on the chemical composition of aerosols has been studied in detail. Ionic balance analysis performed in the coarse and fine aerosol fractions indicated anion and cation deficiency due to CO₃²⁻ and H⁺, respectively. A relationship between nssSO₄²⁻ and NH₄⁺ denoted that sulfate particles were partially neutralized (70%) by ammonium. Excess-K/BC presented two distinct ratios for winter and summer, indicating two different sources: fossil fuel burning in winter and biomass burning in summer.     

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

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

Characteristics of re-suspended road dust and its impact on the atmospheric environment in Beijing

A sampling campaign of re-suspended road dust samples from 53 sites that could cover basically the entire Beijing, soil samples from the source regions of dust storm in August 2003, and aerosol samples from three representative sites in Beijing from December 2001 to September 2003, was carried out to investigate the characteristics of re-suspended road dust and its impact on the atmospheric environment. Ca, S, Cu, Zn, Ni, Pb, and Cd were far higher than its crustal abundances and Ca²⁺, SO₄²⁻, Cl⁻, K⁺, Na⁺, NO₃⁻ were major ions in re-suspended road dust. Al, Ti, Sc, Co, and Mg in re-suspended road dust were mainly originated from crustal source, while Cu, Zn, Ni, and Pb were mainly derived from traffic emissions and coal burning, and Fe, Mn, and Cd were mainly from industrial emissions, coal combustion and oil burning. Ca²⁺ and SO₄²⁻ mainly came from construction activities, construction materials and secondary gas-particle conversions, Cl⁻ and Na⁺ were derived from industrial wastewater disposal and chemical industrial emissions, and NO₃⁻ and K⁺ were from vehicle emissions, photochemical reactions of NO_X, biomass and vegetable burning. The contribution of mineral aerosol from inside Beijing to the total mineral aerosols was ∼30% in spring of 2002, ∼70% in summer of 2002, ∼80% in autumn of 2003, ∼20% in PM₁₀ and ∼50% in PM_2.5, in winter of 2002. The pollution levels of the major pollution species, Ca, S, Cu, Zn, Ni, Pb, Fe, Mn, and Cd in re-suspended road dust reached ∼76%, ∼87%, ∼75%, ∼80%, ∼82%, ∼90%, ∼45%, ∼51%, and ∼94%, respectively. Re-suspended road dust from the traffic and construction activities was one of the major sources of pollution aerosols in Beijing.     

Source identification analysis for the airborne bacteria and fungi using a biomarker approach

Our recent studies have reported the feasibility of employing the 3-hydoxy fatty acids (3-OH FAs) and ergosterol as biomarkers to determine the loading of the airborne endotoxin from the Gram-negative bacteria and fungal biomass in atmospheric aerosols, respectively [Lee, A.K.Y., Chan, C.K., Fang, K., Lau, A.P.S., 2004. The 3-hydroxy fatty acids as biomarkers for quantification and characterization of endotoxins and Gram-negative bacteria in atmospheric aerosols in Hong Kong. Atmospheric Environment 38, 6807–6317; Lau, A.P.S., Lee, A.K.Y., Chan, C.K., Fang, K., 2006. Ergosterol as a biomarker for the quantification of the fungal biomass in atmospheric aerosols. Atmospheric Environment 40, 249–259]. These quantified biomarkers do not, however, provide information on their sources. In this study, the year-long dataset of the endotoxin and ergosterol measured in Hong Kong was integrated with the common water-soluble inorganic ions for source identification through the principal component analysis (PCA) and backward air mass trajectory analysis. In the coarse particles (PM_2.5–10), the bacterial endotoxin is loaded in the same factor group with Ca²⁺ and accounted for about 20% of the total variance of the PCA. This implies the crustal origin for the airborne bacterial assemblage. The fungal ergosterol in the coarse particles (PM_2.5–10) had by itself loaded in a factor group of 10.8% of the total variance in one of the sampling sites with large area of natural vegetative coverage. This suggests the single entity nature of the fungal spores and their independent emission to the ambient air upon maturation of their vegetative growth. In the fine particles (<PM_2.5), the endotoxin and ergosterol associated closely with K⁺ and accounted for 34–38% of the total variance in the two sites studied. The K⁺/Na⁺ ratio is indicative of the possible sources of K⁺, which in turn, provides information on the sources of the associated endotoxin and ergosterol. High K⁺/Na⁺ ratios (>2.0) in the fine particles of the continental air masses imply the microbial source from activities related to biomass burning and industries from the north. The low K⁺/Na⁺ ratios (1.2–1.4) in the fine particles of the mixed air masses suggest microbial sources from the local and regional indoor environment through kitchen emissions and the re-suspension of the road dust due to vehicular exhausts.     

Source apportionment of particulate matter at urban mixed site in Indonesia using PMF

A receptor model of positive matrix factorization (PMF) was used to identify the emission sources of fine and coarse particulates in Bandung, a city located at about 150 km south-east of Jakarta. Total of 367 samples were collected at urban mixed site, Tegalega area, in Bandung City during wet and dry season in the period of 2001–2007. The samples of fine and coarse particulate matter were collected simultaneously using dichotomous samplers and mini-volume samplers. The Samples from dichotomous Samplers were analyzed for black carbon and elements while samples from mini-volume samplers were analyzed for ions. The species analyzed in this study were Na, Mg, Al, Si, K, Ca, Ti, Cr, Mn, Fe, Ni, Cu, Pb, Cl^?, NO₃^?, SO₄^2?, and NH₄⁺. The data were then analyzed using PMF to determine the source factors. Different numbers of source factors were found during dry and wet season. During dry season, the main source factors for fine particles were secondary aerosol (NH₄)₂SO₄, electroplating industry, vehicle emission, and biomass burning, while for coarse particles, the dominant source factors were electroplating industry, followed by aged sea salt, volcanic dust, soil dust, and lime dust. During the wet season, the main source factors for fine particulate matter were vehicle emission and secondary aerosol. Other sources detected were biomass burning, lime dust, soil and volcanic dust. While for coarse particulate matter, the main source factors were sulphate-rich industry, followed by lime dust, soil dust, industrial emission and construction dust.     

Chemical characteristics of atmospheric aerosols over southwest coast of India

Ambient aerosol samples, collected from Mangalore region in the southwest coast of India during the period of late winter (February and March) to early summer (April and May), have been analysed for water-soluble ionic species. Their abundance pattern is dominated by HCO₃⁻, SO₄²⁻, Na⁺, Cl⁻, with minor contribution from NO₃⁻, Ca²⁺, NH₄⁺, K⁺ and Mg²⁺ indicating the contribution from not only sea salt, but also from anthropogenic and dust sources; with pronounced seasonal variability. The suspended particulate matter concentration varied from 35 to 160 μg m⁻³, with consistently higher values during the late winter. Back trajectory analysis suggests the origin of the air masses shifting from Indo-Gangetic Plains (during late winter) to those from the Arabian Sea and the area around Persian Gulf during April–May. Air masses passing over Northern India (Indo-Gangetic Plains) impart characteristic contribution of ionic species from fossil fuel combustion, biomass burning and eolian dust as asserted by the factor analysis. A detailed study on characterisation of aerosols from south Asian region is rather sparse but essential for modelling the effect of tropospheric aerosols on climate.     

Physicochemical variations in atmospheric aerosols recorded at sea onboard the Atlantic–Mediterranean 2008 Scholar Ship cruise (Part I): Particle mass concentrations,size ratios,and main chemical components

We report on ambient atmospheric aerosols present at sea during the Atlantic–Mediterranean voyage of Oceanic II (The Scholar Ship) in spring 2008. A record was obtained of hourly PM₁₀, PM_2.5, and PM₁ particle size fraction concentrations and 24-h filter samples for chemical analysis which allowed for comparison between levels of crustal particles, sea spray, total carbon, and secondary inorganic aerosols. On-board monitoring was continuous from the equatorial Atlantic to the Straits of Gibraltar, across the Mediterranean to Istanbul, and back via Lisbon to the English Channel. Initially clean air in the open Atlantic registered PM₁₀ levels <10 μg m^?3 but became progressively polluted by increasingly coarse PM as the ship approached land. Away from major port cities, the main sources of atmospheric contamination identified were dust intrusions from North Africa (NAF), smoke plumes from biomass burning in sub-Saharan Africa and Russia, industrial sulphate clouds and other regional pollution sources transported from Europe, sea spray during rough seas, and plumes emanating from islands. Under dry NAF intrusions PM₁₀ daily mean levels averaged 40–60 μg m^?3 (30–40 μg m^?3 PM_2.5; c. 20 μg m^?3 PM₁), peaking briefly to >120 μg m^?3 (hourly mean) when the ship passed through curtains of higher dust concentrations amassed at the frontal edge of the dust cloud. PM₁/PM₁₀ ratios ranged from very low during desert dust intrusions (0.3–0.4) to very high during anthropogenic pollution plume events (0.8–1).     

Organic and inorganic components of aerosols over the central Himalayas: winter and summer variations in stable carbon and nitrogen isotopic composition

The aerosol samples were collected from a high elevation mountain site, Nainital, in India (1958 m asl) during September 2006 to June 2007 and were analyzed for water-soluble inorganic species, total carbon, nitrogen, and their isotopic composition (δ¹³C and δ¹⁵N, respectively). The chemical and isotopic composition of aerosols revealed significant anthropogenic influence over this remote free-troposphere site. The amount of total carbon and nitrogen and their isotopic composition suggest a considerable contribution of biomass burning to the aerosols during winter. On the other hand, fossil fuel combustion sources are found to be dominant during summer. The carbon aerosol in winter is characterized by greater isotope ratios (av. ?24.0?‰), mostly originated from biomass burning of C₄ plants. On the contrary, the aerosols in summer showed smaller δ¹³C values (?26.0?‰), indicating that they are originated from vascular plants (mostly of C₃ plants). The secondary ions (i.e., SO₄ ^2?, NH₄ ⁺, and NO₃ ^?) were abundant due to the atmospheric reactions during long-range transport in both seasons. The water-soluble organic and inorganic compositions revealed that they are aged in winter but comparatively fresh in summer. This study validates that the pollutants generated from far distant sources could reach high altitudes over the Himalayan region under favorable meteorological conditions.     

The chemical and strontium isotope composition of atmospheric aerosols over Japan: the contribution of long-range-transported Asian dust (Kosa)

Atmospheric aerosols have been collected at four sites around Japan during 2000. From systematically monitoring the major (Na, Mg, Al, K, Ca, and Fe) and trace (Rb and Sr) elements, along with the Sr isotope composition, we have tried to estimate the contribution of long-range-transported Asian dust (“Kosa”) to the atmospheric aerosols.The results are summarized as follows:(1) The concentration of each element in the aerosols increased during the “Kosa” period. The increase was particularly obvious in samples collected on 8 April 2000, when the “Kosa Phenomenon” was observed at all the sampling sites in Japan, 2 days after a very heavy dust storm had occurred in China.(2) The Rb–Sr isotopic diagram shows a two-component mixing relationship: one with a high ⁸⁷Sr/⁸⁶Sr ratio and a high ⁸⁷Rb/⁸⁶Sr ratio, and the other with a low ⁸⁷Sr/⁸⁶Sr ratio and a low ⁸⁷Rb/⁸⁶Sr ratio. There is a significant difference between that of the expected end member of the Asian dust and that of the reported Asian loess, which is thought to be the possible source of the components of the “Kosa”, although the lower component is consistent with the local component at Wako.(3) Plots of the ⁸⁷Sr/⁸⁶Sr ratio vs the Ca/Al and Sr/Al ratios support a two-component mixing suggested by the Rb–Sr systematics, and they indicate that the contributing continental soil components to the “Kosa” aerosols should be composed of the silicate fraction of Asian loess.(4) The discrepancy in the Rb–Sr systematics between the expected end member and the possible sources may be caused by the dissolution of the Ca-bearing minerals via long-range dust transport, or by a combination of source characteristics and grain size separation.     

Experimental evidence of biomass burning as a source of atmospheric 137Cs,puy de Dôme (1465 m a.s.l.), France

The presence of cesium-137 (¹³⁷Cs) in the environment is mainly due to past nuclear tests and accidental reactor releases. Due to the half-life of ¹³⁷Cs (30.2 y), amounts of this radionuclide releases are in fact still detectable in soils, and at trace levels in the vegetation and the atmosphere. Since the middle of the 1990’s, the presence of ¹³⁷Cs in the atmosphere has long been attributed to the resuspension of terrestrial dust. Recently, modelling studies have demonstrated that an additional and possibly dominant source of this anthropogenic radionuclide is biomass burning. Here, we report the variations of atmospheric ¹³⁷Cs activity levels over a 2-year period at the puy de Dôme (1465 m a.s.l.), France in combination with measurements of the aerosol chemical composition, in particular with indicators for biomass burning (levoglucosan and potassium) and soil dust (calcium). Temporal co-variations of these chemical compounds in addition to back-trajectories are used to identify common source emissions. Significant correlation is found between these compounds. Hence, we experimentally confirm the modelling study highlighting the fact that the atmospheric ¹³⁷Cs is partly released by biomass burning. In addition, we observed that the correlations between the ¹³⁷Cs concentrations and levoglucosan and biomass burning K⁺ differ according to the season. This is in agreement with the temporal evolution of levoglucosan concentration, which has maxima in winter and minima in summer.     

Real-time wet scavenging of major chemical constituents of aerosols and role of rain intensity in Indian region

Real-time simultaneous studies on chemical characteristics of rainwater and PM₁₀ aerosols were carried out to understand the scavenging of major chemical components in Indian region. The concentrations of Ca²⁺, NH₄⁺, SO₄²⁻ and NO₃⁻ were observed to be lower in the aerosol samples collected during rain as compared to before and after rain events. The most significant reduction was noticed for Ca²⁺ (74%) during rain which showed highest scavenging ratio (SR) and indicated that below-cloud scavenging is an effective removal process for Ca²⁺ in Indian region. Among non-sea salt components, Ca²⁺ had highest SR at Hyderabad indicating typical characteristics of crustal influence as abundance of calcium carbonate in soil dust has been reported in India. However, the levels of these major chemical components gradually got build-up in due course of time. After rain events, the levels of SO₄²⁻ aerosols were noticed to be substantially higher (more than double) within 24 h. In general, scavenging ratios for all components (except Ca²⁺, NH₄⁺ and K⁺) were higher over BOB as compared to Hyderabad. The maximum fall in aerosol levels (BR minus AR) was observed during continuous and low intensity rain events that did not allow building up of aerosol concentrations.     

Characterisation for some emission sources in CMB calculation for Mae Moh area, Thailand

Particulate samples of agricultural waste burning, straw burning, forest leaf burning, heavy duty truck emission, paved road dust, soil, agricultural soil, coal, electrostatic precipitator ash, and emission from stack power plant were collected from the Mae Moh area. Chemical compositions of sampling filters were analysed to determine the particulate matter source profiles. The analysis included ICP-MS for elemental compositions, ion chromatography for water soluble ions and CHNS/O for carbon species. In all biomass burning profiles organic carbon (OC) was higher during smouldering phase, while elemental carbon (EC) was higher during flaming phase. Results relating to biomass emission during flaming stage showed increase in K⁺. Organic and elemental carbons were the most abundant in biomass burning and truck exhaust. The abundance of EC was much lower, and the abundance of OC was much higher in biomass burning relative to truck exhaust emission. Al, K, Mg, Ca, and Fe were presented with high abundance in road dust, soil, coal, fly ash and stack samples. The differences in chemical compositions were not sufficient to distinguish geological material and fugitive dust sources. Fly ash profile differed from the others since OC and EC were not detected. Na and Zn were most abundant in stack samples. These findings served as a starting point for source contribution study. For future application of source apportionment using the CMB modelling technique, these source profiles should be appropriately grouped and selected to generate reliable outcomes.     

Distinguishing the relative contribution of fossil fuel and biomass combustion aerosols deposited at Summit,Greenland through isotopic and molecular characterization of insoluble carbon

Quantifying combustion aerosols transported to Summit, Greenland has typically involved the measurement of water-soluble inorganic and organic ions in air, snow, and ice. However, the ubiquitous nature of atmospheric soluble ions makes it difficult to separate the combustion component from the natural component. More specific combustion indicators are therefore needed to accurately quantify inputs from biomass and fossil-fuel burning. This work reports on radiocarbon (¹⁴C) analysis of elemental carbon (EC) and quantification of polycyclic aromatic hydrocarbons (PAHs) of water-insoluble particles from a snowpit excavated at Summit, Greenland in 1996. The ¹⁴C measurements allowed us to quantify the relative contribution of EC from biomass burning and fossil-fuel combustion transported to and deposited at Summit during periods of 1994 and 1995. Specific PAHs associated with conifer combustion helped to identify snowpit layers impacted by forest fires. Our results show that fossil EC was the major component during spring and fall 1994, while biomass EC and fossil EC were present in roughly equal amounts during summer 1994. PAH ratios in spring layers of the snowpit indicate substantial inputs from anthropogenic sources and the ΣPAH depth profile displays springtime maxima that coincided with non-sea-salt sulfate ion maximum concentrations. In other layers, ammonium ion concentrations were independent of the isotopic and molecular carbon measurements. This work demonstrates the utility of radiocarbon techniques to quantify the two different sources of combustion-generated particles at Summit; however, portions of the ¹⁴C results were indeterminate due to large uncertainties that were the result of chemical impurities introduced in the EC isolation technique. Additionally, PAH measurements were successfully performed on as little as 100 ml of snowmelt water, demonstrating the potential for future finer sample resolution.     

Impact of biomass burning on urban air quality estimated by organic tracers: Guangzhou and Beijing as cases

The impacts of biomass burning have not been adequately studied in China. In this work, chemical compositions of volatile organic compounds and particulate organic matters were measured in August 2005 in Beijing and in October 2004 in Guangzhou city. The performance of several possible tracers for biomass burning is compared by using acetonitrile as a reference compound. The correlations between the possible tracers and acetonitrile show that the use of K⁺ as a tracer could result in bias because of the existence of other K⁺ sources in urban areas, while chloromethane is not reliable due to its wide use as industrial chemical. The impact of biomass burning on air quality is estimated using acetonitrile and levoglucosan as tracers. The results show that the impact of biomass burning is ubiquitous in both suburban and urban Guangzhou, and the frequencies of air pollution episodes significantly influenced by biomass burning were 100% for Xinken and 58% for downtown Guangzhou city. Fortunately, the air quality in only 2 out of 22 days was partly impacted by biomass burning in August in Beijing, the month that 2008 Olympic games will take place. The quantitative contribution of biomass burning to ambient PM2.5 concentrations in Guangzhou city was also estimated by the ratio of levoglocusan to PM2.5 in both the ambient air and biomass burning plumes. The results show that biomass burning contributes 3.0–16.8% and 4.0–19.0% of PM2.5 concentrations in Xinken and Guangzhou downtown, respectively.     

Coarse–fine and day–night differences of water-soluble ions in atmospheric aerosols collected in Christchurch and Auckland,New Zealand

The water-soluble ions in fine (PM_<2.5) and coarse (PM_2.5−10) atmospheric aerosols collected in Christchurch during winter 2001, spring 2000 and summer 2001, and in Auckland during winter 2001 have been studied in terms of coarse–fine and day–night differences. Although the chemical characteristics of the coarse particles were similar in both cities, those of the fine particles collected in the Christchurch winter were significantly different, as manifested by higher concentrations of nss-K⁺, nss-Cl⁻, nss-Ca²⁺, nss-SO₄²⁻, NO₃⁻ and NH₄⁺. It was found that nighttime PM₁₀ and nss-K⁺ concentrations were much higher than their daytime concentrations in the Christchurch winter but a clear day–night difference was not apparent in the Auckland winter. Moreover, in the winter, sea-salt ions did not show a day–night difference; however, nss-SO₄²⁻ had opposite day–night variation in the two cities. An ion balance calculation has shown that in most samples, coarse particles can be neutral or alkaline, however, fine particles can be neutral or acidic. The possibility of ammonium salts existing in the fine particles collected in the Christchurch winter is discussed and it is concluded that a variety of ammonium salts were present. Equivalent ratios suggest that the fine particles may be significantly aged in the Christchurch winter.The evidence from our soluble ion study strongly suggests that wood and coal burning and secondary aerosols make a significant contribution to fine particulate mass in the Christchurch atmosphere. Thus, home-heating, a sheltered geographic location and relatively calm atmospheric condition are thought to be the major causes for the serious atmospheric particulate pollution in the Christchurch winter.     

Chemical characterizations of soluble aerosols in southern China

Soluble aerosols are measured at Guangdong and Hainan Provinces of southern China. The measured chemical composition of aerosols includes F-, Cl-, NO3-, SO4=, Na+, NH4+, K+, Ca2+, and Mg2+. The locations of measurements include a mega city (Guangzhou), a medium city along the coastline (Haiko), a small city along the coastline (Shanya), and a remote island site in the South China Sea (Yongxing island). The results reveal that aerosols in this region are complex and heterogeneous. Sulfate aerosol (SO4=) has the highest concentrations in Guangzhou (approximately 41% of total soluble aerosol mass), suggesting that anthropogenic activities (e.g., coal burning) play important roles in controlling aerosol concentrations in Guangzhou. By contrast, the concentrations of chlorine (Cl-) and sodium (Na+) are higher in Yongxing than in Guangzhou, indicating that the sea salt is the dominant aerosol in this marine environment site. In the medium (Haiko) and small (Shanya) city sites, the effects of anthropogenic and marine activities on aerosols fall in between the values in the mega city and the remote island site. The measured ratio of Cl-/Na+ shows that the ratio is less than 1.16 in all observation sites. The ratio in the Guangzhou city, the Haiko city, the Shanya city, and the Yongxing island is 0.52, 0.91, 0.24, and 0.53, respectively, indicating that significantly heterogeneous chemical reactions occur on sea salt particles. Unlike those in Europe and North America, there are high concentrations of calcium (Ca+) in all observation sites. The percentage of calcium mass to the measured total soluble aerosols mass is 21, 32, 34, and 30 at Guangzhou, Haiko, Sanya, and Yongxing, respectively. The calculations show that calcium plays an important role in neutralizing aerosols. The calculated "cation/anion" (summation operator[ion+]/summation operator[ion-]) ratio is 2.5, 2.5, 3.2, and 2.1, at Guangzhou, Haiko, Shanya, and Yongxing, respectively. The high "cation/anion" ratios suggest that SO4=, NO3-, and Cl- are neutralized, and the aerosols as a whole (internally mixed), appear to be in an alkaline mode in this region. However, without taking into account for calcium, the calculated "cation/anion" ratio reduces to 1.2, 0.98, 1.3, and 0.8 at Guangzhou, Haiko, Sanya, and Yongxing, respectively. The property of aerosols switches from an alkaline mode to an acidity mode at the Haiko and Yongxing sites.     

Aerosol transport model evaluation of an extreme smoke episode in Southeast Asia

Biomass burning is one of many sources of particulate pollution in Southeast Asia, but its irregular spatial and temporal patterns mean that large episodes can cause acute air quality problems in urban areas. Fires in Sumatra and Borneo during September and October 2006 contributed to 24-h mean PM₁₀ concentrations above 150 μg m^?3 at multiple locations in Singapore and Malaysia over several days. We use the FLAMBE model of biomass burning emissions and the NAAPS model of aerosol transport and evolution to simulate these events, and compare our simulation results to 24-h average PM₁₀ measurements from 54 stations in Singapore and Malaysia. The model simulation, including the FLAMBE smoke source as well as dust, sulfate, and sea salt aerosol species, was able to explain 50% or more of the variance in 24-h PM₁₀ observations at 29 of 54 sites. Simulation results indicated that biomass burning smoke contributed to nearly all of the extreme PM₁₀ observations during September–November 2006, but the exact contribution of smoke was unclear because the model severely underestimated total smoke emissions. Using regression analysis at each site, the bias in the smoke aerosol flux was determined to be a factor of between 2.5 and 10, and an overall factor of 3.5 was estimated. After application of this factor, the simulated smoke aerosol concentration averaged 20% of observed PM₁₀, and 40% of PM₁₀ for days with 24-h average concentrations above 150 μg m^?3. These results suggest that aerosol transport models can aid analysis of severe pollution events in Southeast Asia, but that improvements are needed in models of biomass burning smoke emissions.     

Effect of biomass burning and regional background aerosols on CCN activity derived from airborne in-situ measurements

Airborne in-situ measurements were analyzed to investigate the effects of biomass burning and regional background aerosols on cloud condensation nuclei (CCN) activity in the Pacific Dust Experiment (PACDEX) during April and May 2007. Airmass trajectories with both horizontal and vertical motions were provided to identify the aerosol sources. In the biomass burning cases, the elevated aerosol layers were clearly observed at dry conditions because of the convection of airmass in the source region. The relative aging of aerosols was supported by the ratios of BC to particles with size ranging from 0.1 to 1.0 μm (N_0.1–1.0) and BC to carbon monoxide. Compared to aerosols in the precedent plume of biomass burning, aged particles in the latter plume were more activated to CCN at 0.4% (CCN_0.4%) than 0.1% supersaturation (CCN_0.1%) due to aerosols chemical modification during the aging process. On the other hand, significant difference of CCN_0.4% and CCN_0.1% at regional background aerosols over the Pacific Ocean was due to the activated particles below 1 μm in diameter. Although higher concentrations of aged particles were observed over the eastern Pacific Ocean, activated aerosols to cloud droplet was comparatively similar in the western Pacific Ocean because of the similar concentrations of N_0.1–1.0 in both cases.     

Mineral aerosols from western India: Temporal variability of coarse and fine atmospheric dust and elemental characteristics

Size-segregated aerosol samples (PM_2.5 and PM₁₀) were collected during Jan–Dec-2007 from a high-altitude site located in a semi-arid region (Mt. Abu, 24.6 °N, 72.7 °E, 1680 m asl) in order to asses the temporal variability in the abundance of atmospheric mineral dust and its elemental composition over western India. The mass concentrations of fine (PM_2.5) and coarse (PM_10–2.5) mode aerosols varied from 1.6 to 46.1 and 2.3 to 102 μg m^?3 respectively over the annual seasonal cycle; with dominant and uniform contribution of mineral dust (60–80%) in the coarse mode relative to large temporal variability (11–75%) observed in the fine mode. The coarse mass fraction shows a characteristic increase with the wind speed during summer months (Mar to Jun); whereas fine aerosol mass and its elemental composition exhibit conspicuous temporal pattern associated with north-easterlies during wintertime (Oct–Feb). The Fe/Al weight ratio in PM_2.5 ranges from 0.5 to 1.0 during winter months. The relative enrichment of Fe in fine mode, compared to the crustal ratio of 0.44, is attributed to the down-wind advective transport of combustion products derived from large-scale biomass burning, industrial and automobile emission sources located in the Indo-Gangetic Plain (northern India). In contrast, Ca/Al and Mg/Al weight ratios show relative enrichment of Ca and Mg in the coarse mode; indicating their dominant contribution from carbonate minerals. This has implication to efficient neutralization of atmospheric acidic species (SO₄^2? and NO₃^?) by mineral dust over western India.     

Elevated nitrogen isotope ratios of tropical Indian aerosols from Chennai: Implication for the origins of aerosol nitrogen in South and Southeast Asia

To better understand the origins of aerosol nitrogen, we measured concentrations of total nitrogen (TN) and its isotope ratios (δ¹⁵N) in tropical Indian aerosols (PM₁₀) collected from Chennai (13.04°N; 80.17°E) on day- and night-time basis in winter and summer 2007. We found high δ¹⁵N values (+15.7 to +31.2‰) of aerosol N (0.3–3.8 μg m^?3), in which NH₄⁺ is the major species (78%) with lesser contribution from NO₃^? (6%). Based on the comparison of δ¹⁵N in Chennai aerosols with those reported for atmospheric aerosols from mid-latitudes and for the particles emitted from point sources (including a laboratory study), as well as the δ¹⁵N ratios of cow-dung samples (this study), we found that the atmospheric aerosol N in Chennai has two major sources; animal excreta and bio-fuel/biomass burning from South and Southeast Asia. We demonstrate that a gas-to-particle conversion of NH₃ to NH₄HSO₄ and (NH₄)₂SO₄ and the subsequent exchange reaction between NH₃ and NH₄⁺ are responsible for the isotopic enrichment of ¹⁵N in aerosol nitrogen.