Exposure to ambient fine particulate matter (PM) is a leading risk factor for the global burden of disease. However, uncertainty remains about PM sources. We use a global chemical transport model (GEOS-Chem) simulation for 2014, constrained by satellite-based estimates of PM to interpret globally dispersed PM mass and composition measurements from the ground-based surface particulate matter network (SPARTAN). Measured site mean PM composition varies substantially for secondary inorganic aerosols (2.4-19.7 μg/m), mineral dust (1.9-14.7 μg/m), residual/organic matter (2.1-40.2 μg/m), and black carbon (1.0-7.3 μg/m). Interpretation of these measurements with the GEOS-Chem model yields insight into sources affecting each site. Globally, combustion sectors such as residential energy use (7.9 μg/m), industry (6.5 μg/m), and power generation (5.6 μg/m) are leading sources of outdoor global population-weighted PM concentrations. Global population-weighted organic mass is driven by the residential energy sector (64%) whereas population-weighted secondary inorganic concentrations arise primarily from industry (33%) and power generation (32%). Simulation-measurement biases for ammonium nitrate and dust identify uncertainty in agricultural and crustal sources. Interpretation of initial PM mass and composition measurements from SPARTAN with the GEOS-Chem model constrained by satellite-based PM provides insight into sources and processes that influence the global spatial variation in PM composition.
[1] Aerosols from the Sarychev Peak volcano entered the Arctic region less than a week after the strongest SO 2 eruption on June 15 and 16, 2009 and had, by the first week in July, spread out over the entire Arctic region. These predominantly stratospheric aerosols were determined to be sub-micron in size and inferred to be composed of sulphates produced from the condensation of SO 2 gases emitted during the eruption. Average (500 nm) Sarychev-induced stratospheric optical depths (SOD) over the Polar Environmental Atmospheric Research Laboratory (PEARL) at Eureka (Nunavut, Canada) were found to be between 0.03 and 0.05 during the months of July and August, 2009. This estimate, derived from sunphotometry and integrated lidar backscatter profiles was consistent with averages derived from lidar estimates over Ny-Ålesund (Spitsbergen). The Sarychev SOD e-folding time at Eureka, deduced from lidar profiles, was found to be approximately 4 months relative to a regression start date of July 27. These profiles initially revealed the presence of multiple Sarychev plumes between the tropopause and about 17 km altitude. After about two months, the complex vertical plume structures had collapsed into fewer, more homogeneous plumes located near the tropopause. It was found that the noisy character of daytime backscatter returns induced an artifactual minimum in the temporal, pan-Arctic, CALIOP SOD response to Sarychev sulphates. A depolarization ratio discrimination criterion was used to separate the CALIOP stratospheric layer class into a low depolarization subclass which was more representative of Sarychev sulphates. Post-SAT (post Sarychev Arrival Time) retrievals of the fine mode effective radius (r eff,f ) and the logarithmic standard deviation for two Eureka sites and Thule (Greenland) were all close to 0.25 mm and 1.6 respectively. The stratospheric analogue to the columnar r eff,f average was estimated to be r eff,f (+) = 0.29 mm for Eureka data. Stratospheric, Raman lidar retrievals at Ny-Ålesund, yielded a post-SAT average of r eff,f (+) = 0.27 mm. These results are $50% larger than the background stratospheric-aerosol value. They are also about a factor of two larger than modeling values used in recent publications or about a factor of five larger in terms of (per particle) backscatter cross section.
Globally consistent measurements of airborne metal concentrations in fine particulate matter (PM2.5) are important for understanding potential health impacts, prioritizing air pollution mitigation strategies, and enabling global chemical transport model development. PM2.5 filter samples (N ~ 800 from 19 locations) collected from a globally distributed surface particulate matter sampling network (SPARTAN) between January 2013 and April 2019 were analyzed for particulate mass and trace metals content. Metal concentrations exhibited pronounced spatial variation, primarily driven by anthropogenic activities. PM2.5 levels of lead, arsenic, chromium, and zinc were significantly enriched at some locations by factors of 100–3000 compared to crustal concentrations. Levels of metals in PM2.5 and PM10 exceeded health guidelines at multiple sites. For example, Dhaka and Kanpur sites exceeded the US National Ambient Air 3-month Quality Standard for lead (150 ng m−3). Kanpur, Hanoi, Beijing and Dhaka sites had annual mean arsenic concentrations that approached or exceeded the World Health Organization’s risk level for arsenic (6.6 ng m−3). The high concentrations of several potentially harmful metals in densely populated cites worldwide motivates expanded measurements and analyses.
Abstract. We present the results of total column measurements of CO, C2H6 and fine-mode aerosol optical depth (AOD) during the "Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites" (BORTAS-B) campaign over eastern Canada. Ground-based observations, using Fourier transform spectrometers (FTSs) and sun photometers, were carried out in July and August 2011. These measurements were taken in Halifax, Nova Scotia, which is an ideal location to monitor the outflow of boreal fires from North America, and also in Toronto, Ontario. Measurements of fine-mode AOD enhancements were highly correlated with enhancements in coincident trace gas (CO and C2H6) observations between 19 and 21 July 2011, which is typical for a smoke plume event. In this paper, we focus on the identification of the origin and the transport of this smoke plume. We use back trajectories calculated by the Canadian Meteorological Centre as well as FLEXPART forward trajectories to demonstrate that the enhanced CO, C2H6 and fine-mode AOD seen near Halifax and Toronto originated from forest fires in northwestern Ontario that occurred between 17 and 19 July 2011. In addition, total column measurements of CO from the satellite-borne Infrared Atmospheric Sounding Interferometer (IASI) have been used to trace the smoke plume and to confirm the origin of the CO enhancement. Furthermore, the enhancement ratio – that is, in this case equivalent to the emission ratio (ERC2H6/CO) – was estimated from these ground-based observations. These C2H6 emission results from boreal fires in northwestern Ontario agree well with C2H6 emission measurements from other boreal regions, and are relatively high compared to fires from other geographical regions. The ground-based CO and C2H6 observations were compared with outputs from the 3-D global chemical transport model GEOS-Chem, using the Fire Locating And Modeling of Burning Emissions (FLAMBE) inventory. Agreement within the stated measurement uncertainty (~3% for CO and ~8% for C2H6) was found for the magnitude of the enhancement of the CO and C2H6 total columns between the measured and modelled results. However, there is a small shift in time (of approximately 6 h) of arrival of the plume over Halifax between the results.
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