Influence Of Biomass Burning Emissions Research Articles

Evolution of black carbon and brown carbon during summertime in Southwestern China: An assessment of control measures during the 2023 Chengdu Summer World University Games

The 31st FISU Summer World University Games (SWUG) was held in Chengdu, southwestern China, from July 22 to August 8, 2023. A series of control measures were carried out to ensure good air quality during the SWUG, providing an opportunity to investigate the atmospheric behaviors of light-absorbing aerosols under such a substantial disturbance caused by the control measures. To assess the impacts of emission controls on primary pollutants, a field campaign was conducted at a rural site in Chengdu to investigate the characterization of equivalent black carbon (eBC). The changes of eBC concentrations before, during, and after the SWUG were characterized. The sources of eBC were resolved, and the impacts of atmospheric processes on the absorption capacity were also investigated. During the SWUG, the eBC concentration decreased by 12.1 % and 25.3 % compared with those before and after the SWUG. A fossil fuel combustion (eBCff) and a biomass burning (eBCbb) originated eBC were resolved using the aethalometer model. Both eBCff and eBCbb decreased during the SWUG, indicating the effectiveness of control measures. After the SWUG, the influence of biomass burning emissions became more and more significant, and the contribution of brown carbon (BrC) to light absorption at 370–660 nm increased by 52, 19, 7, 6, and 17 % compared to those during the SWUG. As the biomass burning emitted aerosols aged, the absorption Ångström exponent and babs(BrC370nm) decreased gradually, which was mainly due to the photobleaching of the chromophores during the daytime. eBCff was mainly affected by strong wind, while high eBCbb concentration was mainly attributed to the gradual accumulation of biomass-burning emissions near the observation site. The results show the significant reduction of eBC with the implementation of the air pollution mitigation campaign, and provide insights on the impacts of atmospheric processes on BC optical properties during summertime.

Trends in Seasonal Mean Speciated Aerosol Composition in Remote Areas of the United States From 2000 Through 2021

AbstractLarge reductions in anthropogenic emissions of particulate matter and its precursor emissions have occurred since the enactment of the Clean Air Act Amendments of 1990. The Interagency Monitoring of Protected Visual Environments network has measured PM2.5 gravimetric mass (mass of particles with aerodynamic diameters less than 2.5 μm, also referred to here as fine mass, “FM”) and speciated PM2.5 aerosol composition at remote sites since 1988. Measured species include inorganic anions such as sulfate, nitrate, and chloride, carbonaceous aerosols such as organic (OC) and elemental carbon (EC), and elemental concentrations used to estimate fine dust (FD). Trends in seasonal and annual mean mass concentrations were calculated from 2000 through 2021, a period that includes the largest reductions in emissions. On average, annual mean FM at remote sites in the continental United States has decreased at a rate of −1.8% yr−1. This reduction is largely due to annual mean trends in sulfate (−6.1% yr−1), nitrate (−2.7% yr−1), EC (−2.2% yr−1), FD (−1.3% yr−1), and OC (−0.9% yr−1), although the OC annual mean trend was insignificant. Seasonal and regional mean FM trends varied significantly, with strong reductions in the East in all seasons due to sulfate reductions, and flat and insignificant trends in summer and fall in the West due to the influence of biomass burning emissions on OC trends. Evaluating regional and seasonal mean trends in aerosol composition helps identify sources that continue to adversely impact air quality and hinder progress in FM reductions due to successful regulatory activity.

H2O2 and CH3OOH (MHP) in the Remote Atmosphere: 1. Global Distribution and Regional Influences

AbstractAtmospheric hydroperoxides are a significant component of the atmosphere's oxidizing capacity. Two of the most abundant hydroperoxides, hydrogen peroxide (H2O2) and methyl hydroperoxide (MHP, CH3OOH), were measured in the remote atmosphere using chemical ionization mass spectrometry aboard the NASA DC‐8 aircraft during the Atmospheric Tomography Mission. These measurements present a seasonal investigation into the global distribution of these two hydroperoxides, with near pole‐to‐pole coverage across the Pacific and Atlantic Ocean basins and from the marine boundary layer to the upper troposphere and lower stratosphere. H2O2 mixing ratios are highest between 2 and 4 km altitude in the equatorial region of the Atlantic Ocean basin, where they reach global maximums of 3.6–6.5 ppbv depending on season. MHP mixing ratios reach global maximums of 4.3–8.6 ppbv and are highest between 1 and 3 km altitude, but peak in different regions depending on season. A major factor contributing to the global H2O2 distribution is the influence of biomass burning emissions in the Atlantic Ocean basin, encountered in all four seasons, where the highest H2O2 mixing ratios were found to correlate strongly with increased mixing ratios of the biomass burning tracers hydrogen cyanide (HCN) and carbon monoxide (CO). This biomass burning enhanced H2O2 by a factor of 1.3–2.2, on average, in the Atlantic compared with the Pacific Ocean basin.

Seasonal Variation in Chemical Composition of Size-Segregated Aerosols Over the Northeastern Arabian Sea

Water-soluble species constitute a significant fraction (up to 60–70%) of the total aerosol loading in the marine atmospheric boundary layer (MABL). The “indirect” effects, that is, climate forcing due to modification of cloud properties depend on the water-soluble composition of aerosols. Thus, the characterization of aerosols over the MABL is of greater relevance. Here, we present 1-year long aerosol chemical composition data of PM10 and PM2.5 at a costal location in the northeastern Arabian Sea (Goa; 15.45°N, 73.20°E, 56 m above the sea level). Average water-soluble ionic concentration (sum of anion and cation) is highest (25.5 ± 6.9 and 19.6 ± 5.8 μg·m−3 for PM10 and PM2.5, respectively) during winter season and lowest during post-monsoon (17.3 ± 9.1 and 14.4 ± 8.1 μg·m−3 for PM10 and PM2.5, respectively). Among water-soluble ionic spices, SO42- ion was found to be dominant species in anions and NH4+ is dominant in cations, for both PM10 and PM2.5 during all the seasons. These observations clearly hint to the contribution from anthropogenic emission and significant secondary inorganic species formation. Sea-salt (calculated based on Na+ and Cl−) concentration shows significant temporal variability with highest contribution during summer seasons in both fractions. Sea-salt corrected Ca2+, an indicator of mineral dust is found mostly during summer months, particularly in PM10 samples, indicates contribution from mineral dust emissions from arid/semiarid regions located in the north/northwestern India and southwest Asia. These observations are corroborated with back-trajectory analyses, wherein air parcels were found to derive from the desert area in summer and Indo-Gangetic Plains (a hot spot for anthropogenic emissions) during winter. In addition, we also observe the presence of nss-K+ (sea-salt corrected), for PM2.5, particularly during winter months, indicating influence of biomass burning emissions. The impact on aerosol chemistry is further assessed based on chloride depletion. Chloride depletion is observed very significant during post-monsoon months (October and November), wherein more than 80 up to 100% depletion is found, mediated by excess sulfates highlighting the role of secondary species in atmospheric chemistry. Regional scale characterization of atmospheric aerosols is important for their better parameterization in chemical transport model and estimation of radiative forcing.

Chemical Composition and Light Absorption of PM2.5 Observed at Two Sites near a Busy Road during Summer and Winter

To examine the difference in the major chemical composition of fine particulate matter (PM2.5) between two roadway sites, 24 h integrated PM2.5 samples were simultaneously collected both 15 m (Buk-Ku District Office (BKO) site) and 150 m (Chonnam National University campus (CNU) site) away from busy roads during the summer and winter periods; these samples were taken to determine the concentrations of organic and elemental carbon (OC and EC), water-soluble organic carbon (WSOC), and water-soluble inorganic species. In addition, the real-time aerosol light absorption coefficients (Abs) were measured using a dual-spot seven-wavelength aethalometer at the CNU site to evaluate the influence of traffic and biomass burning (BB) emissions on the concentrations of organic aerosol particles. The hourly NO2 concentration was also observed at an air pollution monitoring network that is about 2 km away from the CNU site. During summer, 24 h PM2.5 concentrations (PM2.5 episode) which exceeded the Korean PM2.5 standard (35 μg/m3) were linked to increases in organic matter (OM) and SO42− concentrations that accounted for on average 35–41% and 26–30%, respectively, of the PM2.5 at the two sites. The increased SO42− concentration was most likely attributable to the inflow of long-range transported aerosols, rather than local production, as demonstrated by both the MODIS (Moderate Resolution Imaging Spectroradiometer) images and transport pathways of air masses reaching the sites. On the other hand, the OM, WSOC, and EC concentrations were directly attributable to traffic emissions at the sampling sites, as supported by the tight correlation between the OC and EC. A small difference between the absorption Ångström exponent (AAE) values calculated at wavelengths of 370–950 nm (AAE370–950nm) and 370–520 nm (AAE370–520nm), and the poor correlation of absorption coefficient by brown carbon (BrC) at 370 nm (AbsBrC370nm) with K+ (R2 = 0.00) also suggest a significant contribution of traffic emissions to OM. However, the wintertime PM2.5 episode was strongly related to the enhanced OM and NO3− concentrations, which contributed 26–28% and 22–23% of the PM2.5 concentration, respectively. It is interesting to note that there were two distinct OC/EC ratios in winter: a lower OC/EC (~3.0), which indicates a significant contribution of traffic emissions to the OC and EC, and a higher OC/EC (~6.5), which suggests an additional influence of BB emissions as well as traffic emissions at the sites. Strong correlations between the OC and EC (R2 = 0.72–0.83) and the enhanced AAE370–520nm values compared to the AAE370–950nm support that BB emissions were also an important contributor to the wintertime OM concentrations as well as traffic emissions at the two sites. A good correlation between the gaseous NO2 and NO3− and meteorological conditions (e.g., low wind speed and high relative humidity) suggest that the heterogeneous oxidation of NO2 on moist particles could be an important contributor to wintertime particulate NO3− formation at the sites. The OC concentrations during summer and winter were higher at the BKO site, with a higher traffic flow and a shorter distance from the roadway than at the CNU site. However, there were slight differences in the concentrations of secondary inorganic species (NO3−, SO42−, and NH4+) between the sites during summer and winter.

Change in characteristics of water-soluble and water-insoluble brown carbon aerosols during a large-scale biomass burning.

Light-absorbing organic aerosol (brown carbon (BrC)) can significantly affect Earth's radiation budget and hydrological cycle. Biomass burning (BB) is among the major sources of atmospheric BrC. In this study, day/night pair (10-h integrated) of ambient PM2.5 were sampled every day before (defined as T1, n = 21), during (T2, n = 36), and after (T3, n = 8) a large-scale paddy-residue burning during October-November over Patiala (30.2° N, 76.3° E, 250m amsl), a site located in the northwestern Indo-Gangetic Plain (IGP). PM2.5 concentration varied from ~ 90 to 500μgm-3 (average ± 1σ standard deviation 230 ± 114) with the average values of 154 ± 57, 271 ± 122, and 156 ± 18μgm-3 during T1, T2, and T3 periods, respectively, indicating the influence of BB emissions on ambient air quality. The absorption coefficient of BrC (babs) is calculated from the high-resolution absorption spectra of water-soluble and methanol-soluble organic carbon measured at 300 to 700nm, and that at 365nm (babs_365) is used as a general measure of BrC. The babs_365_Water and babs_365_Methanol ranged ~ 2 to 112Mm-1 (avg 37 ± 27) and ~ 3 to 457Mm-1 (avg 121 ± 108), respectively, suggesting a considerable presence of water-insoluble BrC. Contrasting differences were also observed in the daytime and nighttime values of babs_365_Water and babs_365_Methanol. Further, the levoglucosan showed a strong correlation with K+ (slope = 0.89 ± 0.06, R = 0.92) during the T2 period. We propose that this slope (~ 0.9) can be used as a typical characteristics of the emissions from paddy-residue burning over the IGP. Absorption Ångström exponent (AAE) showed a clear day/night variability during the T2 period, and lower AAEMethanol compared to AAEWater throughout the sampling period. Further at 365nm, average relative atmospheric radiative forcing (RRF) for BrCWater is estimated to be ~ 17%, whereas that of BrCMethanol ~ 62%with respect to elemental carbon, suggesting that BrC radiative forcing could be largely underestimated by studies those use BrCWater only as a surrogate of total BrC.

Sensitivity of the simulated CO2 concentration to inter-annual variations of its sources and sinks over East Asia

The study on how the variations in CO2 sources and sinks can affect the CO2 concentration over East Asia would be useful to provide information for policymaker concerning carbon emission reduction. In this study, a nested-grid version of global chemical transport model (GEOS-Chem) is employed to assess the impacts of variations in meteorological parameters, terrestrial fluxes, fossil fuel emissions, and biomass burning on inter-annual variations of CO2 concentrations over East Asia in 2004–2012. Simulated CO2 concentrations are compared with observations at 14 surface stations from the World Data Centre for Greenhouse Gases (WDCGG) and satellite-derived CO2 column density (XCO2) from the Gases Observing SATellite (GOSAT). The comparison shows that the simulated CO2 column density is generally higher than that of GOSAT by 1.33 × 10−6 (annual mean point by point biases averaged over East Asia). The model reasonably captures the temporal variations of CO2 concentrations observed at the ground-based stations, but it is likely to underestimate the peaks-to-troughs amplitude of the seasonal cycle by 50% or more. The simulated surface CO2 concentration in East Asia exhibits the largest inter-annual variation in December-January–February (DJF). The regional mean absolute deviation (MAD) values over East Asia are within (4.4–5.0) × 10−6 for all seasons. Model sensitivity simulations indicate that the inter-annual variations of surface CO2 concentrations are mainly driven by variations of meteorological parameters, and partly modulated by the inter-annual variations of terrestrial fluxes and fossil fuel emissions in local regions. The variations of the terrestrial fluxes and fossil fuel emissions may account for ∼28% of the inter-annual variation of surface CO2 concentration in southern China. The inter-annual variations of the peaks-to-troughs amplitude are dependent on variations of meteorological parameters, terrestrial fluxes and fossil fuel emissions in local regions. The influence of biomass burning emissions is relatively weak.

Source apportionment of carbonaceous aerosols in the vicinity of a Mediterranean industrial harbor: A coupled approach based on radiocarbon and molecular tracers

Located in the Mediterranean Basin and close to Marseille (France), Fos-sur-Mer is situated in the vicinity of industrial harbor and agricultural lands. Its location makes it prone to mixed pollution contributions, combining the influence of residential, industrial, agricultural, maritime road and traffic sources. For this study, the origins of carbonaceous particles sampled over several months are investigated by a coupled approach based on analyses of radiocarbon (14C), elemental to total carbon ratio (EC/TC) and various molecular tracers (levoglucosan, methoxyphenols, malic and glyceric acids), giving information about their background origins. Accelerator mass spectrometry with a gas ion source give the opportunity to quantify the fossil and non-fossil fractions for each individual sample, avoiding to pool them. Analyzing 14C in micro-samples (down to a few μg of carbon) complements the approach based on chemical tracers, which are useful to identify sources, but insufficient to quantify accurately the modern and fossil carbon fractions.The measurements in about 30 samples collected during summer and fall/winter 2013, allow the detection of a strong seasonality of the pollution: the fall/winter PM2.5 fraction concentration equals to three times the summer concentration and we observe a significant fluctuation of the relative contributions of fossil and non-fossil fractions (fNF is ≈ 0.83 for fall/winter samples and ≈0.59 for summer samples).Significant correlations between 14C, levoglucosan and different methoxyphenols, allow the identification and quantification of a major influence of biomass burning emissions during fall and winter. Biomass burning organic carbon (OCBB) and elemental carbon (ECBB) contribute to 45% and 8% of the TC, respectively, whereas their total contribution is only 3% in summer samples.Biogenic emissions from the vegetation are the main sources of carbon during summer (≈57%). Significant correlations between summer OCbio and malic acid and DL glyceric acid suggest a secondary origin for this fraction.The total fossil carbon concentration (ECF and OCF) from vehicular, shipping and industrial sources is constant throughout the year, which is compatible with intense road and maritime traffics and industrial activity during both seasons.Overall, our study based on 14C and molecular tracers illustrates the power of a coupled approach in order to both identify and quantify biomass burning, biogenic, traffic and industrial sources of carbonaceous aerosols, forming a complex mix of background PM origins in a typical industrious harbor of the Mediterranean region.

Chemical Characterization of Fine Atmospheric Particles of Water-Soluble Ions and Carbonaceous Species in a Tropical Urban Atmosphere over the Eastern Indo-Gangetic Plain

ABSTRACT Ambient fine aerosols and their sources were evaluated in an eastern Indian megacity, Kolkata (KOL), from September 2010 to August 2011. A submicron aerosol sampler (SAS) with two stage stacked filter units (SFU) was devised for simultaneous but discrete collection of water-soluble inorganic ions (WSII) and carbonaceous aerosols (CA; elemental carbon (EC) and organic carbon (OC)). Characteristics of the WSII and CA were identified using ion chromatography and an OC-EC analyzer, respectively, adopting the Interagency Monitoring of PROtected Visual Environments (IMPROVE-A) protocol. The mean annual concentrations of the WSII showed a predominance of cations (anions), consisting of Ca2+, Mg2+, and Na+ (Cl–, NO3–, and SO42–), with secondary aerosols (NH4+, NO3–, and SO42–) and Ca2+ each constituting 25% and 30%, respectively, of the total WSII (TWSII). The highest mean monthly concentration of SO42– and NO3– was observed during the winter month of February and the summer months of March and May, respectively. A pronounced peak in the monthly mean for the non-sea salt-K+ (nss-K+) concentration was noticed during October and April, implying the strong influence of biomass burning emissions during these months. Among the sea salt (SS), anthropogenic (AN), and dust (DT) sources of the TWSII, a predominant contribution from DT in August and from AN in November, April, and May was inferred. The mean annual concentration of OC was three times higher than that of EC, with 43% of it being secondary OC. Whereas the major sources of OC were inferred to be paved dust, coal combustion, and biomass burning, those of EC were industrial and motor-vehicle non-exhaust emissions, coal combustion, and motor vehicle exhaust.

Observations of particulate matter, NO2, SO2, O3, H2S and selected VOCs at a semi-urban environment in the Amazon region

This research aims to assess air quality in a transitional location between city and forest in the Amazon region. Located downwind of the Manaus metropolitan region, this study is part of the large-scale experiment GoAmazon2014/5. Based on their pollutant potential, inhalable particulate matter (PM2.5), nitrogen dioxide (NO2), sulfur dioxide (SO2), ozone (O3), hydrogen sulfide (H2S), benzene, toluene, ethylbenzene and meta-, orto-, para-xylene (BTEX) were selected for analysis. Sampling took place during the wet season (March–April 2014) and dry season (August–October 2014). The number of forest fires in the surroundings was higher during the dry wet season. Results show significant increase during the dry season in mass concentration (wet: <0.01–10 μg m−3; dry: 9.8–69 μg m−3), NH4+ soluble content (wet: 13–125 μg m−3; dry: 86–323 μg m−3) and K+ soluble content (wet: 11–168 μg m−3; dry 60–356 μg m−3) of the PM2.5, and O3 levels (wet: 1.4–14 μg m−3; dry: 1.0–40 μg m−3), indicating influence of biomass burning emissions. BTEX concentrations were low in both periods, but also increased during the dry season. A weak correlation in the time series of the organic and inorganic gaseous pollutants indicates a combination of different sources in both seasons and NO2 results suggest a spatial heterogeneity in gaseous pollutants levels beyond initial expectations.

Identification of amines in wintertime ambient particulate material using high resolution aerosol mass spectrometry

Significant amounts of amines were detected in fine particulate matter (PM) during ambient wintertime conditions in Yakima, WA, using a high resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). Positive matrix factorization (PMF) of the organic aerosol (OA) signal resulted in a six-factor solution that included two previously unreported amine OA factors. The contributions of the amine factors were strongly episodic, but the concentration of the combined amine factors was as high as 10–15 μg m−3 (2-min average) during those episodes. In one occasion, the Amine-II component was 45% of total OA signal. The Amine-I factor was dominated by spectral peaks at m/z 86 (C5H12N+) and m/z 100 (C6H14N+), while the Amine-II factor was dominated by spectral peaks at m/z 58 (C3H8N+ and C2H6N2+) and m/z 72 (C4H10N+ and C3H8N2+). The ions dominating each amine factor showed distinct time traces, suggesting different sources or formation processes. Investigation into the chemistry of the amine factors suggests a correlation with inorganic anions for Amine-I, but no evidence that the Amine-II was being neutralized by the same inorganic ions. We also excluded the presence of organonitrates (ON) in the OA. The presence of C2H4O2+ at m/z 60 (a levoglucosan fragment) in the Amine-I spectrum suggests some influence of biomass burning emissions (more specifically residential wood combustion) in this PMF factor, but wind direction suggested that the most likely sources of these amines were agricultural activities and feedlots to the S-SW of the site.

Toxic potential of organic constituents of submicron particulate matter (PM1) in an urban road site (Barcelona).

Atmospheric particulate matter (PM) is a recognized risk factor contributing to a number of diseases in human populations and wildlife globally. Organic matter is a major component of PM, but its contribution to overall toxicity of PM has not been thoroughly evaluated yet. In the present work, the biological activity of organic extracts from PM1 (particles with less than 1μm of aerodynamic diameter) collected from an urban road site in the centre of Barcelona (NE Spain) was evaluated using a yeast-based assay (AhR-RYA) and different gene expression markers in zebrafish embryos. Dioxin-like activity of the extracts correlated to primary emissions from local traffic exhausts, reflecting weekday/weekend alternance. Expression levels of cyp1a and of gene markers for key cellular processes and development (ier2, fos) also correlated to vehicle emissions, whereas expression of gene markers related to antioxidant defence and endocrine effects (gstal, hao1, ttr) was strongly reduced in samples with strong contribution from regional air masses with aged secondary organic species or with strong influence of biomass burning emissions. Our data suggest that the toxic potential of PM1 organic chemical constituents strongly depends on the emission sources and on the process of ageing from primary to secondary organic aerosols.

In situ acidity and pH of size-fractionated aerosols during a recent smoke-haze episode in Southeast Asia.

The characterization of aerosol acidity has received increased attention in recent years due to its influence on atmospheric visibility, climate change and human health. Distribution of water soluble inorganic (WSI) ions in 12 different size fractions of aerosols was investigated under two different atmospheric conditions (smoke-haze and non-haze periods) in 2012 using the Micro-Orifice Uniform Deposit Impactor (MOUDI) and nano-MOUDI for the first time in Singapore. To estimate the in situ acidity ([H(+)]Ins) and in situ aerosol pH (pHIS), the Aerosol Inorganic Model version-IV under deliquescent mode of airborne particles was used at prevailing ambient temperature and relative humidity. The study revealed an increase in the levels of airborne particulate matter (PM) mass and concentrations of WSI ions for all size fractions during the smoke-haze period, which was caused by the trans-boundary transport of biomass burning-impacted air masses from Indonesia. A bimodal distribution was observed for concentrations of SO4(2-), NO3(-), Cl(-), K(+) and Na(+), whereas concentrations of NH4(+), Ca(2+) and Mg(2+) showed a single mode distribution. The concentration of WSI ions in PM1.8 during the smoke-haze period increased by 3.8 (for SO4(2-)) to 10.5 (for K(+)) times more than those observed during the non-haze period. The pHIS were observed to be lower during the smoke-haze period than that during the non-haze period for all size fractions of PM, indicating that atmospheric aerosols were more acidic due to the influence of biomass burning emissions. The particles in the accumulation mode were more acidic than those in the coarse mode.

Carbon monoxide and related trace gases and aerosols over the Amazon Basin during the wet and dry seasons

Abstract. We present the results of airborne measurements of carbon monoxide (CO) and aerosol particle number concentration (CN) made during the Balanço Atmosférico Regional de Carbono na Amazônia (BARCA) program. The primary goal of BARCA is to address the question of basin-scale sources and sinks of CO2 and other atmospheric carbon species, a central issue of the Large-scale Biosphere-Atmosphere (LBA) program. The experiment consisted of two aircraft campaigns during November–December 2008 (BARCA-A) and May–June 2009 (BARCA-B), which covered the altitude range from the surface up to about 4500 m, and spanned most of the Amazon Basin. Based on meteorological analysis and measurements of the tracer, SF6, we found that airmasses over the Amazon Basin during the late dry season (BARCA-A, November 2008) originated predominantly from the Southern Hemisphere, while during the late wet season (BARCA-B, May 2009) low-level airmasses were dominated by northern-hemispheric inflow and mid-tropospheric airmasses were of mixed origin. In BARCA-A we found strong influence of biomass burning emissions on the composition of the atmosphere over much of the Amazon Basin, with CO enhancements up to 300 ppb and CN concentrations approaching 10 000 cm−3; the highest values were in the southern part of the Basin at altitudes of 1–3 km. The ΔCN/ΔCO ratios were diagnostic for biomass burning emissions, and were lower in aged than in fresh smoke. Fresh emissions indicated CO/CO2 and CN/CO emission ratios in good agreement with previous work, but our results also highlight the need to consider the residual smoldering combustion that takes place after the active flaming phase of deforestation fires. During the late wet season, in contrast, there was little evidence for a significant presence of biomass smoke. Low CN concentrations (300–500 cm−3) prevailed basinwide, and CO mixing ratios were enhanced by only ~10 ppb above the mixing line between Northern and Southern Hemisphere air. There was no detectable trend in CO with distance from the coast, but there was a small enhancement of CO in the boundary layer suggesting diffuse biogenic sources from photochemical degradation of biogenic volatile organic compounds or direct biological emission. Simulations of CO distributions during BARCA-A using a range of models yielded general agreement in spatial distribution and confirm the important contribution from biomass burning emissions, but the models evidence some systematic quantitative differences compared to observed CO concentrations. These mismatches appear to be related to problems with the accuracy of the global background fields, the role of vertical transport and biomass smoke injection height, the choice of model resolution, and reliability and temporal resolution of the emissions data base.

Levoglucosan enhancement in ambient aerosol during springtime transport events of biomass burning smoke to Southeast China

An intensive field experiment was conducted at an urban and a rural site in Hong Kong to identify the influence of biomass burning emissions transported from distinct regions on ambient aerosol in coastal southeast China. Watersoluble ionic and carbonaceous species, specifically the biomass burning tracer levoglucosan, were analysed. Elevated levoglucosan concentrations with maxima of 91.5 and 133.7 ng m-3 and overall average concentrations of 30 and 36 ng m-3 were observed at the rural and urban sites, respectively. By combining the analysed meteorological data, backward trajectories, fire counts and Aerosol Index from the Earth Probe satellite, southwest China and the northern Philippines, together with the southeast China coast, were identified for the first time as source regions of the transported biomass burning particles at the surface level in rural Hong Kong. Occasional levoglucosan enhancements observed at urban Hong Kong were attributed to local incense and joss paper burning during the Ching-Ming festival period. The contributions of transported biomass burning emissions, especially from the northern Philippines, were estimated to account for 7.5% and 2.9% of OC and PM2.5, respectively.

Chemical composition of mineral dust aerosol during the Saharan Dust Experiment (SHADE) airborne campaign in the Cape Verde region, September 2000

During the Saharan Dust Experiment (SHADE) in September 2000, we collected filter samples on board the Met Office C‐130 aircraft. The main study area was over the Atlantic Ocean between Sal Island and Senegal. Dust was encountered in the altitude range from 0.5–1 to 4–4.5 km. Sublayers with different particle size distributions and different source areas can be distinguished within the main dust plume. Diminution of O3 in anticorrelation with the dust layer suggests removal of O3 by dust particles. Dust loadings containing up to 54 μg m−3 Al (submicron plus supermicron fraction) were measured during particularly intense dust events. Mixing of dust with anthropogenic aerosols, mainly NH4HSO4, was observed in the fine fraction. It was associated with air masses that had originated over Europe and then traveled over North Africa. The ratio of nitrate to non‐sea‐salt sulfate was around 0.3. This argues against any significant influence of biomass burning emissions, which have much higher nitrate. However, we also encountered aged fossil fuel pollution plumes, likely from North America. The geochemical signature of mineral dust was consistent with previous results in the area. Si, Fe, and Ti were not enriched with respect to the soil composition, while other elements, such as Ca and S, were. Ca is prevalently present as calcite in African soils, but it is also found as calcium sulfate in the atmosphere.