Analysis of long-range transport of aerosols for Portugal using 3D chemical transport model and satellite measurements

2013 ◽  
Vol 64 ◽  
pp. 229-241 ◽  
Author(s):  
O. Tchepel ◽  
J. Ferreira ◽  
A.P. Fernandes ◽  
S. Basart ◽  
J.M. Baldasano ◽  
...  
2010 ◽  
Vol 10 (2) ◽  
pp. 4673-4717 ◽  
Author(s):  
D. Durnford ◽  
A. Dastoor ◽  
D. Figueras-Nieto ◽  
A. Ryjkov

Abstract. This study is the most extensive study to date on the transport of mercury to the Arctic. Moreover, it is the first such study to use a fully-coupled, online chemical transport model, Environment Canada's Global/Regional Atmospheric Heavy Metals model (GRAHM), where the meteorology and mercury processes are fully integrated. It is also the only study to date on the transport of mercury across Canada. We determined source attribution from Asia, North America, Russia and Europe at six arctic verification stations, as well as three subarctic and eight midlatitude Canadian stations. We have found that Asia, despite having transport efficiencies that were almost always lower than those of North America and often lower than those of Russia, was the dominant source of gaseous atmospheric mercury at all verification stations: it contributed the most mercury (29–37% at all stations, seasons and levels considered), its concentrations frequently explained nearly 100% of the variability in the concentrations produced by the simulation performed with full global emissions, particularly in the absence of local sources, and it generated the most long range transport (LRT) events, causing 43%, 67% and 75% of the events at the arctic, subarctic and midlatitude stations, respectively. For the Arctic, Russian transport efficiencies tended to be the strongest, as expected, while European and Asian efficiencies were lower and higher, respectively, than those found in the literature. This disagreement is likely produced by mercury's long lifetime relative to that of other pollutants. The accepted springtime preference for the trans-Pacific transport of Asian pollution was evident only in the midlatitude group of stations, being masked in the arctic and subarctic groups by the occurrence of atmospheric mercury depletion events. Some neighbouring arctic stations recorded dissimilar numbers of LRT events; despite their proximity, the behaviour of mercury at these stations was governed by different dynamics and transport pathways. The column burden of GEM in the lowest 5 km of the Northern Hemisphere was largest in summer from Asia, North America and Russia, but in winter from Europe. In the vertical, transport of mercury from all source regions occurred principally in the mid-troposphere.


2008 ◽  
Vol 8 (4) ◽  
pp. 16335-16379 ◽  
Author(s):  
D. R. Reidmiller ◽  
D. A. Jaffe ◽  
D. Chand ◽  
S. Strode ◽  
P. Swartzendruber ◽  
...  

Abstract. Interannual variations in background tropospheric trace gases (such as carbon monoxide, CO) are largely driven by variations in emissions (especially wildfires), transport pathways and tropospheric oxidizing capacity. Understanding this variability is essential to quantify the intercontinental contribution to US air quality. We investigate the interannual variability of long-range transport of Asian pollutants to the Northeast Pacific via measurements from the Mt. Bachelor Observatory (MBO: 43.98° N, 121.69° W; 2.7 km above sea level) and GEOS-Chem chemical transport model simulations in spring 2005 vs. the INTEX-B campaign during spring 2006. Measurements of CO at MBO were significantly enhanced during spring 2005 relative to the same time in 2006 (the INTEX-B study period); a monthly mean decline in CO of 41 ppbv was observed between April 2005 and April 2006. Meteorological indices show that long-range transport of CO from the heavily industrialized region of East Asia was significantly greater in 2005 than in 2006. In addition, spring 2005 was an anomalously strong biomass burning season in Southeast Asia. Data presented by Yurganov et al. (2008) using MOPITT satellite retrievals from this area reveal an average CO burden anomaly (referenced to March 2000–February 2002 mean values) between October 2004 through April 2005 of 2.6 Tg CO vs. 0.6 Tg CO for the same period a year later. The Naval Research Laboratory's global aerosol transport model shows that emissions from these fires were efficiently transported to MBO throughout April 2005. Asian dust transport, however, was substantially greater in 2006 than 2005, particularly in May. Monthly mean aerosol light scattering coefficient at 532 nm (σsp) at MBO more than doubled from 2.7 Mm−1 in May 2005 to 6.2 Mm−1 in May 2006. We also evaluate CO interannual variability throughout the western US via Earth System Research Laboratory ground site data and throughout the Northern Hemisphere via MOPITT and TES satellite observations. Both in the Northeast Pacific and on larger scales, we reveal a significant decrease (from 2–21%) in springtime maximum CO between 2005 and 2006, evident in all platforms and the GEOS-Chem model. We attribute this to (a) anomalously strong biomass burning in Southeast Asia during winter 2004 through spring 2005, and (b) the transport pattern in 2006 which limited the inflow of Asian pollution to the lower free troposphere over western North America.


2009 ◽  
Vol 9 (2) ◽  
pp. 557-572 ◽  
Author(s):  
D. R. Reidmiller ◽  
D. A. Jaffe ◽  
D. Chand ◽  
S. Strode ◽  
P. Swartzendruber ◽  
...  

Abstract. Interannual variations in background tropospheric trace gases (such as carbon monoxide, CO) are largely driven by variations in emissions (especially wildfires) and transport pathways. Understanding this variability is essential to quantify the intercontinental contribution to US air quality. We investigate the interannual variability of long-range transport of Asian pollutants to the Northeast Pacific via measurements from the Mt. Bachelor Observatory (MBO: 43.98° N, 121.69° W; 2.7 km a.s.l.) and GEOS-Chem chemical transport model simulations in spring 2005 vs. the INTEX-B campaign during spring 2006. Measurements of CO at MBO were significantly enhanced during spring 2005 relative to the same time in 2006 (the INTEX-B study period); a decline in monthly mean CO of 41 ppbv was observed between April 2005 and April 2006. A backtrajectory-based meteorological index shows that long-range transport of CO from the heavily industrialized region of East Asia was significantly greater in early spring 2005 than in 2006. In addition, spring 2005 was an anomalously strong biomass burning season in Southeast Asia. Data presented by Yurganov et al. (2008) using MOPITT satellite retrievals from this area reveal an average CO burden anomaly (referenced to March 2000–February 2002 mean values) between October 2004 through April 2005 of 2.6 Tg CO vs. 0.6 Tg CO for the same period a year later. The Naval Research Laboratory's global aerosol transport model, as well as winds from NCEP reanalysis, show that emissions from these fires were efficiently transported to MBO throughout April 2005. Asian dust transport, however, was substantially greater in 2006 than 2005, particularly in May. Monthly mean aerosol light scattering coefficient at 532 nm (σsp) at MBO more than doubled from 2.7 Mm−1 in May 2005 to 6.2 Mm−1 in May 2006. We also evaluate CO interannual variability throughout the western US via Earth System Research Laboratory ground site data and throughout the Northern Hemisphere via MOPITT and TES satellite observations. Both in the Northeast Pacific and on larger scales, we reveal a significant decrease (from 2–21%) in springtime maximum CO between 2005 and 2006, evident in all platforms and the GEOS-Chem model. We attribute this to (a) anomalously strong biomass burning in Southeast Asia during winter 2004 through spring 2005, and (b) the transport pattern in March and April 2006 which limited the inflow of Asian pollution to the lower free troposphere over western North America.


2010 ◽  
Vol 10 (13) ◽  
pp. 6063-6086 ◽  
Author(s):  
D. Durnford ◽  
A. Dastoor ◽  
D. Figueras-Nieto ◽  
A. Ryjkov

Abstract. This study is the most extensive study to date on the transport of mercury to the Arctic. Moreover, it is the first such study to use a fully-coupled, online chemical transport model, Environment Canada's Global/Regional Atmospheric Heavy Metals model (GRAHM), where the meteorology and mercury processes are fully integrated. It is also the only study to date on the transport of mercury across Canada. We estimated source attribution from Asia, North America, Russia and Europe at six arctic verification stations, as well as three subarctic and eight midlatitude Canadian stations. We have found that Asia, despite having transport efficiencies that were almost always lower than those of North America and often lower than those of Russia, was the dominant source of gaseous atmospheric mercury at all verification stations: it contributed the most mercury (29–37% at all stations, seasons and levels considered), its concentrations frequently explained nearly 100% of the variability in the concentrations produced by the simulation performed with full global emissions, particularly in the absence of local sources, and it generated the most long range transport (LRT) events, causing 43%, 67% and 75% of the events at the arctic, subarctic and midlatitude stations, respectively. For the Arctic, Russian transport efficiencies tended to be the strongest, as expected, while European and Asian efficiencies were lower and higher, respectively, than those found in the literature. This disagreement is likely produced by mercury's long lifetime relative to that of other pollutants. The accepted springtime preference for the trans-Pacific transport of Asian pollution was evident only in the midlatitude group of stations, being masked in the arctic and subarctic groups by the occurrence of atmospheric mercury depletion events. Some neighbouring arctic stations recorded dissimilar numbers of LRT events; despite their proximity, the behaviour of mercury at these stations was governed by different dynamics and transport pathways. The column burden of GEM in the lowest 5 km of the Northern Hemisphere was largest in summer from Asia, North America and Russia, but in winter from Europe. In the vertical, transport of mercury from all source regions occurred principally in the mid-troposphere.


2008 ◽  
Vol 8 (11) ◽  
pp. 2999-3014 ◽  
Author(s):  
A. van Donkelaar ◽  
R. V. Martin ◽  
W. R. Leaitch ◽  
A. M. Macdonald ◽  
T. W. Walker ◽  
...  

Abstract. We interpret a suite of satellite, aircraft, and ground-based measurements over the North Pacific Ocean and western North America during April–May 2006 as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign to understand the implications of long-range transport of East Asian emissions to North America. The Canadian component of INTEX-B included 33 vertical profiles from a Cessna 207 aircraft equipped with an aerosol mass spectrometer. Long-range transport of organic aerosols was insignificant, contrary to expectations. Measured sulfate plumes in the free troposphere over British Columbia exceeded 2 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Aerosol Optical Depth (AOD) retrieved from two satellite instruments (MISR and MODIS) for 2000–2006 are analyzed with GEOS-Chem to estimate an annual growth in Chinese sulfur emissions of 6.2% and 9.6%, respectively. Analysis of aircraft sulfate measurements from the NASA DC-8 over the central Pacific, the NSF C-130 over the east Pacific and the Cessna over British Columbia indicates most Asian sulfate over the ocean is in the lower free troposphere (800–600 hPa), with a decrease in pressure toward land due to orographic effects. We calculate that 56% of the measured sulfate between 500–900 hPa over British Columbia is due to East Asian sources. We find evidence of a 72–85% increase in the relative contribution of East Asian sulfate to the total burden in spring off the northwest coast of the United States since 1985. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.31 μg/m3 (~30%) and account for 50% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.32 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, and suggest current East Asian emissions episodically degrade local air quality by more than 1.5 μg/m3.


2010 ◽  
Vol 10 (12) ◽  
pp. 5739-5748 ◽  
Author(s):  
C. Paton-Walsh ◽  
L. K. Emmons ◽  
S. R. Wilson

Abstract. In this paper we describe a new method for estimating trace gas emissions from large vegetation fires using satellite measurements of aerosol optical depth (AOD) at 550 nm, combined with an atmospheric chemical transport model. The method uses a threshold value to screen out normal levels of AOD that may be caused by raised dust, sea salt aerosols or diffuse smoke transported from distant fires. Using this method we infer an estimated total emission of 15±5 Tg of carbon monoxide, 0.05±0.02 Tg of hydrogen cyanide, 0.11±0.03 Tg of ammonia, 0.25±0.07 Tg of formaldehyde, 0.03±0.01 of acetylene, 0.10±0.03 Tg of ethylene, 0.03±0.01 Tg of ethane, 0.21±0.06 Tg of formic acid and 0.28±0.09 Tg of methanol released to the atmosphere from the Canberra fires of 2003. An assessment of the uncertainties in the new method is made and we show that our estimate agrees (within expected uncertainties) with estimates made using current conventional methods of multiplying together factors for the area burned, fuel load, the combustion efficiency and the emission factor for carbon monoxide. A simpler estimate derived directly from the satellite AOD measurements is also shown to be in agreement with conventional estimates, suggesting that the method may, under certain meteorological conditions, be applied without the complication of using a chemical transport model. The new method is suitable for estimating emissions from distinct large fire episodes and although it has some significant uncertainties, these are largely independent of the uncertainties inherent in conventional techniques. Thus we conclude that the new method is a useful additional tool for characterising emissions from vegetation fires.


2007 ◽  
Vol 7 (6) ◽  
pp. 1549-1564 ◽  
Author(s):  
X. Davoine ◽  
M. Bocquet

Abstract. The reconstruction of the Chernobyl accident source term has been previously carried out using core inventories, but also back and forth confrontations between model simulations and activity concentration or deposited activity measurements. The approach presented in this paper is based on inverse modelling techniques. It relies both on the activity concentration measurements and on the adjoint of a chemistry-transport model. The location of the release is assumed to be known, and one is looking for a source term available for long-range transport that depends both on time and altitude. The method relies on the maximum entropy on the mean principle and exploits source positivity. The inversion results are mainly sensitive to two tuning parameters, a mass scale and the scale of the prior errors in the inversion. To overcome this hardship, we resort to the statistical L-curve method to estimate balanced values for these two parameters. Once this is done, many of the retrieved features of the source are robust within a reasonable range of parameter values. Our results favour the acknowledged three-step scenario, with a strong initial release (26 to 27 April), followed by a weak emission period of four days (28 April–1 May) and again a release, longer but less intense than the initial one (2 May–6 May). The retrieved quantities of iodine-131, caesium-134 and caesium-137 that have been released are in good agreement with the latest reported estimations. Yet, a stronger apportionment of the total released activity is ascribed to the first period and less to the third one. Finer chronological details are obtained, such as a sequence of eruptive episodes in the first two days, likely related to the modulation of the boundary layer diurnal cycle. In addition, the first two-day release surges are found to have effectively reached an altitude up to the top of the domain (5000 m).


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