scholarly journals Analysis of aircraft and satellite measurements from the Intercontinental Chemical Transport Experiment (INTEX-B) to quantify long-range transport of East Asian sulfur to Canada

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.

2008 ◽  
Vol 8 (1) ◽  
pp. 4017-4057 ◽  
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. Measured sulfate plumes in the free troposphere over British Columbia exceeded 1 μg/m3. We update the global anthropogenic emission inventory in a chemical transport model (GEOS-Chem) and use it to interpret the observations. Trends in 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 63% of the measured sulfate at 600 hPa over British Columbia is due to East Asian sources. Simulation of INTEX-B and May 1985 aircraft measurements off the northwest coast of the United States reveals a 2.4–3.4 fold increase in the relative contribution of East Asian sulfate to the total burden. Campaign-average simulations indicate anthropogenic East Asian sulfur emissions increase mean springtime sulfate in Western Canada at the surface by 0.14–0.19 μg/m3 (~30%) and account for 40% of the overall regional sulfate burden between 1 and 5 km. Mean measured daily surface sulfate concentrations taken in the Vancouver area increase by 0.27 μg/m3 per 10% increase in the simulated fraction of Asian sulfate, suggesting current East Asian emissions degrade local air quality.


2017 ◽  
Author(s):  
Kohei Ikeda ◽  
Hiroshi Tanimoto ◽  
Takafumi Sugita ◽  
Hideharu Akiyoshi ◽  
Yugo Kanaya ◽  
...  

Abstract. We implemented a tagged tracer method of black carbon (BC) into a global chemistry-transport model GEOS-Chem, examined the pathways and efficiency of long-range transport from a variety of anthropogenic and biomass burning emission sources to the Arctic, and quantified the source contributions of individual emissions. Firstly, we evaluated the simulated BC by comparing it with observations at the Arctic sites and found that the simulated seasonal variations were improved by implementing an aging parameterization and reducing the wet scavenging rate by ice clouds. For tagging BC, we added BC tracers distinguished by source types (anthropogenic and biomass burning) and regions; the global domain was divided into 16 and 27 regions for anthropogenic and biomass burning emissions, respectively. Our simulations showed that BC emitted from Europe and Russia was transported to the Arctic mainly in the lower troposphere during winter and spring. In particular, BC transported from Russia was widely spread over the Arctic in winter and spring, leading to a dominant contribution of 62 % to the Arctic BC near the surface as the annual mean. In contrast, BC emitted from East Asia was found to be transported in the middle troposphere into the Arctic mainly over the Okhotsk Sea and East Siberia during winter and spring. We identified an important window area, which allowed a strong incoming of East Asian BC to the Arctic (130°–180° E and 3–8 km altitude at 66° N). The model demonstrated that the contribution from East Asia to the Arctic had a maximum at about 5 km altitude due to uplifting during the long-range transport in early spring. The efficiency of BC transport from East Asia to the Arctic was smaller than that from other large source regions such as Europe, Russia and North America. However, the East Asian contribution was most important for BC in the middle troposphere (41 %) and BC burden over the Arctic (27 %) because of the large emissions from this region. These results suggested that the main sources of the Arctic BC differed with altitude. The contribution of all the anthropogenic sources to Arctic BC concentrations near the surface was dominant (90 %) on an annual basis. The contributions of biomass burning in boreal regions (Siberia, Alaska and Canada) to the annual total BC deposition onto the Arctic were estimated to be 12–15 %, which became the maximum during summer.


2001 ◽  
Vol 106 (D16) ◽  
pp. 18361-18370 ◽  
Author(s):  
I. G. McKendry ◽  
J. P. Hacker ◽  
R. Stull ◽  
S. Sakiyama ◽  
D. Mignacca ◽  
...  

2007 ◽  
Vol 46 (8) ◽  
pp. 1230-1251 ◽  
Author(s):  
George Kallos ◽  
Marina Astitha ◽  
Petros Katsafados ◽  
Chris Spyrou

Abstract During the past 20 years, organized experimental campaigns as well as continuous development and implementation of air-pollution modeling have led to significant gains in the understanding of the paths and scales of pollutant transport and transformation in the greater Mediterranean region (GMR). The work presented in this paper has two major objectives: 1) to summarize the existing knowledge on the transport paths of particulate matter (PM) in the GMR and 2) to illustrate some new findings related to the transport and transformation properties of PM in the GMR. Findings from previous studies indicate that anthropogenically produced air pollutants from European sources can be transported over long distances, reaching Africa, the Atlantic Ocean, and North America. The PM of natural origin, like Saharan dust, can be transported toward the Atlantic Ocean and North America mostly during the warm period of the year. Recent model simulations and studies in the area indicate that specific long-range transport patterns of aerosols, such as the transport from Asia and the Indian Ocean, central Africa, or America, have negligible or at best limited contribution to air-quality degradation in the GMR when compared with the other sources. Also, new findings from this work suggest that the imposed European Union limits on PM cannot be applicable for southern Europe unless the origin (natural or anthropogenic) of the PM is taken into account. The impacts of high PM levels in the GMR are not limited only to air quality, but also include serious implications for the water budget and the regional climate. These are issues that require extensive investigation because the processes involved are complex, and further model development is needed to include the relevant physicochemical processes properly.


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.


2013 ◽  
Vol 13 (15) ◽  
pp. 7511-7529 ◽  
Author(s):  
A. D. Clarke ◽  
S. Freitag ◽  
R. M. C. Simpson ◽  
J. G. Hudson ◽  
S. G. Howell ◽  
...  

Abstract. Airborne aerosol measurements in the central equatorial Pacific during PASE (Pacific Atmospheric Sulfur Experiment) revealed that cloud condensation nuclei (CCN) activated in marine boundary layer (MBL) clouds were strongly influenced by entrainment from the free troposphere (FT). About 65% entered at sizes effective as CCN in MBL clouds, while ~25% entered the MBL too small to activate but subsequently grew via gas to particle conversion. The remaining ~10% were inferred to be sea salt aerosol. FT aerosols at low carbon monoxide (CO) mixing ratios (< 63 ppbv) were mostly volatile at 360 °C with a number mode peak of around 30–40 nm dry diameter and tended to be associated with cloud outflow from distant (3000 km or more) deep convection. Higher CO concentrations were commonly associated with trajectories from South America and the Amazon region (ca. ~10 000 km away) and occurred in layers indicative of combustion sources (biomass burning season) partially scavenged by precipitation. These had number modes near 60–80 nm dry diameter with a large fraction of CCN.2 (those activated at 0.2% supersaturation and representative of MBL clouds) prior to entrainment into the MBL. Flight averaged concentrations of CCN.2 were similar for measurements near the surface, below the inversion and in the FT just above the inversion, confirming that subsidence and entrainment of FT aerosol strongly influenced MBL CCN.2. Concurrent flight-to-flight variations of CCN.2 at all altitudes below 3 km also imply MBL CCN.2 concentrations were in quasi-equilibrium with the FT over a 2–3 day timescale. The observed FT transport over thousands of kilometers indicates teleconnections between MBL CCN and cloud-scavenged sources of both natural and/or residual combustion origin. Nonetheless, in spite of its importance, this source of CCN number is not well represented in most current models and is generally not detectable by satellite because of the low aerosol scattering in such layers as a result of cloud scavenging. In addition, our measurements confirm nucleation in the MBL was not evident during PASE and argue against a localized linear relation in the MBL between dimethyl sulfide (DMS) and CCN suggested by the CLAW hypothesis. However, when the FT is not impacted by long-range transport, sulfate aerosol derived from DMS pumped aloft in the ITCZ (Inter-Tropical Convergence Zone) can provide a source of CCN to the boundary layer via FT teleconnections involving more complex non-linear processes.


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