Impact of Changes in Future Anthropogenic Aerosol Emissions on Northern Hemispheric Regional Air Quality and Climate

Maureen Lei1,3, Elizabeth Duval2, and Mian Chin4 Abstract

Student1, Teacher2: Montgomery Blair High School, 51 East Boulevard, Silver Spring, MD, 20901
Intern3, Mentor/Professor4: NASA Goddard Space Flight Center, 8800 Greenbelt Rd., Greenbelt,Maryland 20771

ACCELERATED ARTICLE

Anthropogenic* aerosols play important roles in climate change, air quality, and human health and visibility. To better understand the impact of changes in future anthropogenic emissions, we analyzed output from the NASA Goddard Chemistry Aerosol Radiation Transport(GOCART) Global Model for present (year 2001) and future (years 2030 and 2050) emission scenarios with a focus on northern hemispheric air quality and climate. GOCART uses assimilated meteorological fields from the NASA Goddard Earth Observing System Data Assimilation System (GEOS DAS version 4). In this study, which is part of a comprehensive project coordinated by the United Nations Task Force on Hemispheric Transport of Air Pollution (HTAP), anthropogenic sulfur aerosols, black carbon (BC), and particulate organic matter (POM) were analyzed for surface concentration, column load and deposition over time, source attribution, source-receptor relationships, and Relative Annual Intercontinental Response (RAIR). The analysis used five tagged regions, including four major anthropogenic source (and also receptor) regions of East Asia, Europe, North America, and South Asia, and one climatically sensitive receptor region of the Arctic. This study reveals a sensitivity of North American air quality and climate to Asian anthropogenic emissions, and an Arctic vulnerability to Asian and European emissions. Our results suggest that intercontinental transport is a critical element to be considered in the development of emission control strategies for northern hemispheric air quality and climate.

Introduction

Aerosols, also referred to as particulate matter (PM), are liquid or solid particles suspended in the air that affect climate, air quality, and human health and visibility20. Atmospheric aerosols originate from both anthropogenic (such as fossil fuel combustion, oil drilling, and agriculture) and natural (such as desert *caused or produced by humans

storms, volcanoes, vegetation, and wildfires) sources. Anthropogenic activities have become a significant source of atmospheric aerosols, including sulfate, nitrate, black carbon (BC), and particulate organic matter (POM), among others. Aerosols generated by anthropogenic emissions consist mostly of finemode particles (less than 2.5 m in diameter) that can be harmful to human health12. The principal aerosol components are sulfate and POM, which reflect solar radiation to space and therefore cool the atmosphere5. BC is only a minor contributor to aerosol mass but is of great climatic concern as an absorber of solar radiation both in the atmosphere and after deposition to snow, thus contributing to atmospheric warming, and the melting of snow and ice16. Anthropogenic aerosols have relatively short atmospheric lifetimes (several days). In spite of their short lifetimes, aerosols originating in one region can travel long distances to affect the environments of downwind regions5, demonstrating the hemispheric to global scale of aerosol influence. In the northern hemisphere, specific source-receptor relationships have been identified. Model experiments suggest the regular outflow of Asian air pollution over the Pacific to North America through conveyer belt activity21. This mechanism has been confirmed through the Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission11. Further, Asia has been shown to be influential over most of the northern hemisphere, except for in the North Atlantic and the tropics4. Intercontinental transport from Europe has also been studied. Europe lacks mechanisms to effectively transport aerosols across the Atlantic Ocean17. Instead, European outflow tends to travel North to the Arctic, contributing to Arctic haze15. European emissions, however, are capable of reaching other northern hemispheric regions by traveling eastward across Asia and the Pacific to reach North America. Because these aerosols tend to mix with Asian emissions, they are difficult to detect4. Anthropogenic emissions in the industrial period greatly increased the amount of aerosols in

Maureen Lei, Elizabeth Duval, and Mian Chin the northern hemisphere13. As a result of economic development, and emission control policies and technologies, anthropogenic emissions from the major northern hemispheric source regions will continue to change in the coming decades, as projected by the future emission scenarios developed for the 5th Intergovernmental Panel on Climate Change (IPCC) assessment report14. Even though local and regional emissions are primarily responsible for pollution, hemispheric transport of air pollution (HTAP) can intensify air quality issues caused by local and regional emissions19. To understand the impact of changes in future anthropogenic emissions, we analyzed anthropogenic northern hemispheric emissions, intercontinental transport, and source-receptor relationships in present(year 2001) and future (years 2030 and 2050) emission scenarios. Intercontinental transport was studied among five tagged regions: East Asia, Europe, North America, South Asia, and the Arctic (Fig. 1) using the Goddard Chemistry Aerosol Radiation Transport (GOCART) Global Model. The Arctic is strictly a receptor region. Its air quality can be influenced by anthropogenic emissions from outside regions, but it produces few anthropogenic emissions of its own to influence outside air quality. The other four regions are source and receptor regions. In this paper, we present the model and emission scenarios, aerosol concentration behavior over time, source attribution of aerosol species, sourcereceptor relationships amongst tagged regions, and Relative Annual Intercontinental Response (RAIR). Our results show that North American surface concentration and column load, which are relevant to air quality and climate change respectively, are sensitive to Asian anthropogenic emissions; and Arctic column load is sensitive to Asian and European emissions. These findings demonstrate the importance of intercontinental transport in air quality and climate. The implications of these findings on future air quality, climate, human health, and policy are discussed.

Page 2 of 8

Figure 1. Source and receptor regions designated in this study. The map shows the tagged regions that were used in the GOCART Global Model runs. EA (East Asia), EU (Europe), NA (North America), and SA (South Asia), each boxed and highlighted in color, are all source and receptor regions. AR (Arctic, latitudes > 66.5N) is only a receptor region.

Materials and Methods

GOCART global model experiments were carried out to address source attribution and source-receptor relationships in present and future emission scenarios for sulfate, BC, and POM. GOCART is used to simulate major aerosol species and their precursors in the troposphere including sulfur, dust, BC, sea

salt, and POM1,2,3,4,7,8. The model uses assimilated meteorological fields from the NASA Goddard Earth Observing System Data Assimilation System with a horizontal resolution of 2 latitude by 2.5 longitude, and 30 vertical layers. Processes included are emissions from anthropogenic, biomass burning and natural sources, transport, chemistry, and dry and wet removal. Using GOCART, we examined three anthropogenic emission scenarios specified by HTAP: SR1 (2001), FE1 (2030), and FE2 (2050). Figure 2 shows changes in global anthropogenic emissions. The 2001 simulation uses present-day emissions, whereas 2030 uses Representative Concentration Pathway (RCP) 8.5-like emissions (high non-anthropogenic greenhouse gas emissions, low methane) and 2050 uses RCP2.6-like emissions (low nonanthropogenic greenhouse gas emissions, low methane)14. The year 2030 and year 2050 simulations are driven by 2001 meteorological fields. Both RCP emission scenarios were assigned by the United Nations Task Force on the Hemispheric Transport of Air Pollutants. Table 1 lists the anthropogenic emissions of SO2, BC, and POM in 2001, 2030, and 2050 in the four major source regions of North America, Europe, East Asia, and South Asia. East Asian and South Asian anthropogenic emissions increase by 5% and 47%, respectively, from 2001 to 2030, while other regions decrease (Table 1, 2001 and 2030). From 2030 to 2050, anthropogenic emissions decrease in all four tagged regions (Table 1, 2030 and 2050). With each scenario, five global model experiments were conducted: one with all emissions

Maureen Lei, Elizabeth Duval, and Mian Chin

Page 3 of 8

Figure 2. Anthropogenic emission changes over time. The sum of emissions of anthropogenic aerosol (sulfur species, or BC, or POM) from all source regions in a year is represented by a bar. 2001, 2030, and 2050 are represented by the black, light gray, and dark gray bars, respectively. TgM=TgS for sulfur species, TgC for BC and POM.

a region due to a 20% decrease in emissions in all four regions19. For example, RAIR for North America is calculated as follows: N/F, where N = changes in North American aerosol in response to a 20% reduction in East Asian, European, and South Asian anthropogenic emissions and T = changes in North American aerosol in response to 20% reductions in anthropogenic emissions of all four source regions. RAIR ranges from 0%, indicating no intercontinental influence, to 100%, indicating complete domination by intercontinental sources. It is a measure of how much a region may benefit from emission reductions in other regions if reductions occur on the northern hemispheric scale.

(including natural and anthropogenic), and the other four with anthropogenic emissions reduced by 20% in each of the major source regions. To quantify the intercontinental influence of changes in anthropogenic emissions, we examine source attribution, sourcereceptor relationships, and RAIR among these regions. For our analysis, we calculated source attribution values, which represent the percent of aerosols in a region that can be attributed to anthropogenic emissions from a single source region. They are calculated by finding the ratio between the amount of aerosol from anthropogenic emissions in a specified source region and the total amount of aerosol in a specified receptor region (A/T, where A = aerosols attributed to a specified source region and T = total aerosol in receptor region). Source-receptor relationship values were also calculated. They represent the percent reduction in concentrations or depositions of a receptor region in response to a 20% reduction in anthropogenic emissions of a source region19. Source-receptor relationship values are calculated as follows: (OR)/O, where O = original receptor region concentration, and R = receptor region concentration after 20% reduction in source regions anthropogenic emissions. They describe the sensitivity of concentrations or depositions of a receptor to changes in emissions from a source. RAIR is the sum of changes in the annual, regionally averaged concentration in a region due to a 20% decrease in emissions in the three other regions, divided by the sum of changes in concentration within

Table 1. Anthropogenic emissions in source regions for years 2001, 2030, and 2050. SO2, BC, and POM emissions used in GOCART Global Model runs in 2001, 2030, and 2050 emission scenario are shown in the top, middle and bottom sub-tables, respectively. SO2 instead of SO4 emissions were used because most anthropogenic SO4 comes from converted SO2. EA: East Asia. EU: Europe. NA: North America. SA: South Asia.

Results

Northern hemispheric aerosols selectively decrease in future emission scenarios: With changes in anthropogenic emissions from 2001 to 2050, there were paralleled changes in total northern hemispheric pollutant concentrations and depositions. Increases and decreases in surface concentrations, column loads, and depositions (Fig. 3) generally matched increases and decreases in regional anthropogenic emissions (Table 1). North American and European anthropogenic emissions steadily decreased, as shown in Table 1. With these decreases, we see decreases in surface concentrations, column loads, and depositions

Maureen Lei, Elizabeth Duval, and Mian Chin

Page 4 of 8

in both regions (Fig. 3). North America exhibited the most dramatic reductions of all sulfate surface concentrations over the East Coast (Fig. 3, top row). They fall from a peak of 2.0-3.0 gS/m3 in 2001 (Fig. 3, top row, left map) to a peak 0.30-0.40 gS/m3 (Fig. 3, top row, right map) in 2050. North American East Coast BC column load levels drop as well, but over a significantly smaller range (Fig. 3, middle row). The highest 2001 levels registered at 0.701.0mgC/m2 (Fig. 3, middle row, left map) and the highest 2050 levels registered at 0.30-0.40mgC/m2 (Fig. 3, middle row, right map). There are also reductions in sulfate deposition over the same region (Fig. 3, bottom row). In 2001, 1.0-2.0 mgS/m2/day at most are deposited over the North American East Coast (Fig. 3, bottom row, left map), but in 2050, 0.20-0.30 mgS/m2/day at most are deposited (Fig. 3, bottom row, right map). Similarly, the changes in amount of aerosols in East Asia and South Asia matched changes in regional anthropogenic emissions. East Asian and South Asian distributions increase from 2001 to 2030 and decrease from 2030 to 2050 (Fig. 3), consistent with the fluctuation of emission changes (Table 1). In terms of absolute amount, East Asia is consistently home to the highest amounts of aerosols out of all the tagged regions. In 2001 and 2030, East Asias sulfate surface concentrations are as high as 5.0-7.0 gS/m3, while the sulfate surface concentrations of other tagged regions peak at 3.0-5.0 gS/m3 (Fig. 3, top row, left and middle map). By 2050, East Asias sulfate surface concentrations peak at 1.0-2.0 gS/m3, while those of other tagged regions always fall below 0.50 gS/m3 (Fig. 3, top row, right map). Also, East Asias 2001 and 2030 BC column loads are as high as 3.0-5.0 mgC/m2, compared to the less than 1.0 mgC/m2 column loads of the rest of the tagged regions (Fig. 3, middle row, left and middle map). Its 2050 BC column loads are as high as 1.0-2.0 mgC/m2, outdoing the BC column loads of the rest of the tagged regions, which largely register below 1.0 mgC/m2 (Fig. 3, middle row, right map). Lastly, East Asian sulfate depositions in 2001 and 2030 register as high as 3.0-5.0 mgS/m2/day, outdoing the less than 2.0 mgS/m2/day sulfate depositions in the rest of the world (Fig. 3, bottom row, left and middle map). In 2050, sulfate is deposited over East Asia in quantities as high as 1.0-2.0 mgS/m2/day; the most deposited over other regions is 0.50 mgS/m2/day (Fig. 3, bottom row, right map).Intercontinental transport exerts influence in regional air quality and climate in future emission scenarios: In evaluating the source attribution of aerosols in all source regions, it is evident that local emissions are the most significant individual contributor to local concentrations (Figs. 4, 5, and 6). In most cases, the amount of aerosols in a region is controlled more by local anthropogenic emissions than outside anthropogenic emissions. The impact of intercontinental transport Figure 3. Northern hemispheric anthropogenic aerosol distributions in from outside tagged regions, however, is still 2001, 2030, and 2050. Sulfate surface concentration, BC column load and sulfate deposition in tagged areas (North America: 125W-60W, 15N-55N, noteworthy. North America is the most significant Europe: 10W-50E, 25N-65N, South Asia: 50E-95E, 5N-35N, East Asia: contributor to its own air quality. Its surface 95E-160E, 15N-50N, and Arctic: 180W-180E, 66.5N-90N) are shown in the the top, middle and bottom row, In concentration from 2001 to 2050 is dominated by maps inand right map show distributions inrespectively. and each row, the left, middle, 2001, 2030, 2050, respectively. its own anthropogenic emissions for all aerosol Color changes in tagged regions indicate changes in aerosol amounts. The
color key assigns a range of aerosol concentrations to a specific color.

Maureen Lei, Elizabeth Duval, and Mian Chin species (Fig. 4). At their highest, aerosols from North American anthropogenic emissions constitute nearly 90% of North American BC (Fig. 4, B). East Asia is the second most significant contributor to North American pollutants, but its anthropogenic emissions account for less than 20% of North American surface concentration (Fig. 4, D and E). By 2050, however, there is a decrease in how much of North Americas surface concentration can be attributed to its own anthropogenic emissions (Fig. 4, G, H, and I). The most extreme example is the decrease in sulfate attributions. In 2001, North America controls nearly 80% of its own sulfate surface concentrations (Fig. 4, A). By 2050, North American anthropogenic emissions will be responsible for less than 40% of the regions own sulfate pollution (Fig. 4, G). However, anthropogenic emissions from other source regions also have very little impact. East Asian anthropogenic emissions, again the second most significant contributor, are responsible for at most 5% of North American sulfate (Fig. 4, G). North American column load, which is relevant to climate change, is sensitive to intercontinental transport (Fig. 5). In 2030, North Americas BC column load is atypically sensitive to anthropogenic South Asian and East Asian emissions (Fig. 5, E). For all of 2030, anthropogenic North American BC

Page 5 of 8

emissions are completely overtaken by at least one other region in determining North American BC column loads. Anthropogenic East Asian BC emissions are responsible for a greater percentage of North American BC column loads than anthropogenic North American BC emissions for the entire year, and anthropogenic South Asian BC emissions are responsible for a greater percentage than anthropogenic North American BC emissions in the spring and fall months (Fig. 5, E). North Americas response to anthropogenic East Asian and South Asian BC emissions in the 2001 and 2050 emission scenarios is not as dramatic. However, East Asia and South Asia are consistently the second and third most significant contributors to North American column loads (Fig. 5, B and H). Although total BC column loads are the most dramatic example of North America developing sensitivity to outside sources, sulfate (Fig. 5, A, D, and G) and POM (Fig. 5, C, F and I) column loads also demonstrate vulnerability to anthropogenic emissions from other tagged regions. From 2001 to 2030, North American control of its own sulfate column load drops from a peak of 75% (Fig. 5, A) to a peak of 40% (Fig. 5, D). East Asian influence also increases from 2001 to 2030, becoming more influential relative to North American emissions. In 2030, anthropogenic East Asian sulfate emissions are the
Figure 4. North American surface concentration source attribution in years 2001, 2030, and 2050. Yaxis in each graph: percent of North American surface concentration attributed to anthropogenic emissions from four source regions (EA: East Asia, EU: Europe, NA: North America, SA: South Asia). Each source region is represented by a colored line. X-axis in each graph: months of the year. The left (A, B, C), middle (D, E, F), and right (G, H, I) columns are for source attribution in years 2001, 2030, and 2050, respectively. The top (A, D, G), middle (B, E, H), and bottom (C, F, I) rows are for source attribution of sulfate, BC, and POM, respectively.

Maureen Lei, Elizabeth Duval, and Mian Chin

Figure 5. (Top) North American column load source attribution in years 2001, 2030, and 2050. Y-axis in each graph: percent of North American column load attributed to anthropogenic emissions from four source regions (EA: East Asia, EU: Europe, NA: North America, SA: South Asia). Each source region is represented by a colored line. X-axis in each graph: months of the year. The left (A, B, C), middle (D, E, F), and right (G, H, I) columns are for source attribution in years 2001, 2030, and 2050, respectively. The top (A, D, G), middle (B, E, H), and bottom (C, F, I) rows are for source attribution of sulfate, BC, and POM, respectively. Figure 6. (Bottom) Arctic column load source attribution in years 2001, 2030, and 2050. Y-axis in each graph: percent of Arctic column load attributed to anthropogenic emissions from four source regions (EA: East Asia, EU: Europe, NA: North America, SA: South Asia). Each source region is represented by a colored line. X-axis in each graph: months of the year. The left (A, B, C), middle (D, E, F), and right (G, H, I) columns are for source attribution in years 2001, 2030, and 2050, respectively. The top (A, D, G), middle (B, E, H), and bottom (C, F, I) rows are for source attribution of sulfate, BC, and POM, respectively.

Page 6 of 8

second-most significant anthropogenic contributor to North American sulfate column loads. For the first three months of 2030 in particular, East Asian contributions trail North American contributions, consistently falling less than 5% below anthropogenic North American contributions (Fig. 5, D). North American POM column loads are less sensitive to outside anthropogenic sources, but anthropogenic sources in general are relatively minor contributors. The sum of POM column load attributed to outside anthropogenic sources is less than 20% of total POM column load in 2001 and 2050 (Fig. 5, C and I). In 2030, the influence of intercontinental transport peaks (Fig. 5, F). For all of 2030, less than 20% of POM column load can be attributed to North American anthropogenic emissions. However, at least 5% of POM column load can be attributed to East Asia and South Asia. Most notably, in October of 2030, South Asian and North American contributions are equal (Fig. 5, F).

Discussion

Our analysis reveals significant decreases in surface concentrations, column loads, and depositions across the northern hemisphere in future emission scenarios (Fig. 3). This finding suggests that intercontinental coordination of emission reductions could lead to across the board decreases in amounts of aerosols. Because of the contributions of local emissions and intercontinental transport, a balance of local and hemispheric regulation may be necessary. Furthermore, a targeted approach may prove useful in controlling northern hemispheric air quality in the future. In particular, regulation of North American climate (particularly for BC column loads) may require coordination between North American and East Asian governments. This argument is supported by several findings of this study: Source attribution between the two regions shows

Maureen Lei, Elizabeth Duval, and Mian Chin a significant portion of North American aerosols coming from anthropogenic East Asian emissions (Figs. 4 and 5), RAIR calculations reveal high sensitivity of North American air quality to intercontinental transport (Table 3, Appendix), and source-receptor calculations demonstrate sensitivity of North American air quality to anthropogenic East Asian emissions in particular (Table 2, Appendix). Although fluctuations in anthropogenic East Asian emissions will not guarantee proportional fluctuations in North American air quality, other outcomes are unlikely because of the confirmed path of air pollutants from Asia to North America11. Because East Asia is in a continual state of economic development, further fluctuations in its anthropogenic emissions are almost guaranteed. Therefore, North America will do itself a disservice if it neglects to negotiate anthropogenic emission regulations with East Asia; it may end up having little control over its own air quality and climate, and the health of its citizenry. In addition to North America, Arctic climate may also benefit from special attention. Concerns regarding the Arctic are not directed towards direct impacts on human health, but rather, the chain reaction on global climate that may be set off by changes in Arctic climate. Although a uniform, northern hemispheric reduction in anthropogenic emissions will likely reduce intercontinental transport to the Arctic, reductions in anthropogenic East Asian and European emissions may prove especially beneficial, especially because of the confirmed northward path taken by European emissions18. We conducted a novel investigation to gauge the consequences of changes in future anthropogenic aerosol emissions on northern hemispheric air quality and climate. Different regions displayed varying degrees of sensitivity to intercontinental transport. In particular, North America and the Arctic (judged by source attribution, source-receptor relationships, and RAIR) demonstrate vulnerability to intercontinental transport. North American air quality shows sensitivity to anthropogenic East Asian emissions. Significant portions of North American aerosols have been attributed to anthropogenic East Asian emissions (Figs. 4 and 5), and source receptor calculations for North America demonstrated heightened sensitivity to changes in anthropogenic East Asian emissions (Table

Page 7 of 8

2, Appendix). Further, RAIR calculations for North America demonstrated a high level of dependence of local air quality on all intercontinental sources (Table 3, Appendix). Arctic climate was also revealed to be sensitive to outside sources. In particular, Arctic climate is influenced by anthropogenic East Asian and European emissions (Fig. 6). These results suggest that the effective way to control local climate, especially for North America and the Arctic, is to coordinate emission reductions on a larger scale, whether global or hemispheric. For these two regions in particular, targeted reductions in emissions of key source regions and regulation of intercontinental transport may prove necessary to control local air quality. Previous observatory and modeling studies5,11,18,21 for the present day have reached similar conclusions, including long range transport of pollutants from Asia to North America11,21, from Asia to the Arctic17, and from Europe to the Arctic5. The trends in intercontinental transport in our study were consistent with the trends identified in past studies. Our study, however, provides a projection into the future. To further solidify the results of this model run, the same emission scenarios will need to be tested in other models. Multiple model runs with future emissions scenarios will prove useful in planning ahead for policy recommendations to manage the impacts of future anthropogenic emission fluctuation.

References

1. Chin, M., Rood, R. B., Lin, S. J., Muller, J. F., and Thompson, A. M.: Atmospheric sulfur cycle simulated in the global model GOCART: Model description and global properties, Journal of Geophysical ResearchAtmospheres, 105, 24671-24687, 2000a. 2. Chin, M., Savoie, D. L., Huebert, B. J., Bandy, A. R., Thornton, D. C., Bates, T. S., Quinn, P. K., Saltzman, E. S., and De Bruyn, W. J.: Atmospheric sulfur cycle simulated in the global model GOCART: Comparison with field observations and regional budgets, Journal of Geophysical Research-Atmospheres, 105, 2468924712, 2000b. 3.Chin, M., Ginoux, P., Kinne, S., Torres, O., Holben, B. N., Duncan, B. N., Martin, R. V., Logan, J. A., Higurashi, A., and Nakajima, T.: Tropospheric aerosol optical thickness from the GOCART model and comparisons with satellite and Sun photometer measurements, Journal of the Atmospheric Sciences, 59, 461-483, 2002.

Maureen Lei, Elizabeth Duval, and Mian Chin

Page 8 of 8

4. Chin, M., Diehl, T., Ginoux, P., and Malm, W.: Intercontinental transport of pollution and dust aerosols: implications for regional air quality, Atmospheric Chemistry and Physics, 7, 5501-5517, 2007. 5. Fiore, A., Holloway, T., and Hastings, M.: A global perspective on air quality: intercontinental transport and linkages with climate, EM-PittsburghAir and Waste Management Association, 13-22, 2003. 6. Flanner, M. G., Zender, C. S., Randerson, J. T., and Rasch, P. J.: Present-day climate forcing and response from black carbon in snow, Journal of Geophysical Research-Atmospheres, 112, 2007. 7. Ginoux, P., Chin, M., Tegen, I., Prospero, J. M., Holben, B., Dubovik, O., and Lin, S. J.: Sources and distributions of dust aerosols simulated with the GOCART model, Journal of Geophysical ResearchAtmospheres, 106, 20255-20273, , 2001. 8. Ginoux, P., Prospero, J. M., Torres, O., and Chin, M.: Long-term simulation of global dust distribution with the GOCART model: correlation with North Atlantic Oscillation, Environmental Modelling & Software, 19, 113-128, 2004. 9. Goldstein, A. H., Millet, D. B., McKay, M., Jaegl, L., Horowitz, L., Cooper, O., Hudman, R., Jacob, D. J., Oltmans, S., and Clarke, A.: Impact of Asian emissions on observations at Trinidad Head, California, during ITCT 2K2, Journal of Geophysical Research- Atmospheres, 109, 13, 2004. 10. Hogrefe, C., Lynn, B., Civerolo, K., Ku, J. Y., Rosenthal, J., Rosenzweig, C., Goldberg, R., Gaffin, S., Knowlton, K., and Kinney, P. L.: Simulating changes in regional air pollution over the eastern United States due to changes in global and regional climate and emissions, Journal of Geophysical ResearchAtmospheres, 109, 2004. 11. Jacob, D. J., Crawford, J. H., Kleb, M. M., Connors, V. S., Bendura, R. J., Raper, J. L., Sachse, G. W., Gille, J. C., Emmons, L., and Heald, C. L.: Transport and Chemical Evolution over the Pacific (TRACE-P) aircraft mission: Design, execution, and first results, Journal of Geophysical Research, 108, 2003. 12. Kulle, T. J., Sauder, L. R., Shanty, F., Kerr, H. D., Farrell, B. P., Miller, W. R., and Milman, J. H.: Sulfurdioxide and ammonium-sulfate effects on pulmonaryfunction and bronchial reactivity in human-subjects, American Industrial Hygiene Association Journal, 45,

156- 161, 1984. 13. Le Treut, H., Somerville, R., Cubasch, U., Ding, Y., Mauritzen, C., Mokssit, A., Peterson, T., and Prather, M.: Historical Overview of Climate Change. in: Climate Change 2007: The Physical Science Basis. Contribution of Working Group I to the Fourth Assessment Report of the Intergovernmental Panel on Climate Change [Solomon, S., Qin, D., Manning, M., Chen, Z., Marquis, M., Averyt, K. B., Tignor, M., and Miller, H. L. (eds.)]. Cambridge University Press, Cambridge, United Kingdom and New York, NY, USA, 2007. 14. Moss, R. H., Babiker, M., Brinkman, S., Calvo, E., Carter, T., Edmonds, J. A., Elgizouli, I., Emori, S., Lin, E., and Hibbard, K.: Towards new scenarios for analysis of emissions, climate change, impacts, and response strategies, Pacific Northwest National Laboratory (PNNL), Richland, WA (US), 2008. 15. Raatz, W. E.: An anticyclonic point of view on low-level tropospheric long-range transport, Atmospheric Environment, 23, 2501-2504, 1989. 16. Ramanathan, V., and Carmichael, G.: Global and regional climate changes due to black carbon, Nature Geoscience, 1, 221-227, 2008. 17. Stohl, A.: A 1-year Lagrangian climatology of airstreams in the Northern Hemisphere troposphere and lowermost stratosphere, Journal of Geophysical Research-Atmospheres, 106, 7263-7279, 2001. 18. Stohl, A.: Intercontinental transport of air pollution, Springer Verlag, 2004. 19. West, J. J., Emberson, L., Ainsworth, E., Anenberg, S. C., Arnold, S., Ashmore, M., Atkinson, R., Bellouin, N., Cohen, R., Collins, B., Delmelle, P., Doherty, R., Farah, N., Fuhrer, J., Hicks, K., Holloway, T., Kobayashi, K., Liu, J. F., Mauzerall, D., Mercado, L., Mills, J., Sanderson, M., Shindell, D., Sitch, S., Stevenson, D., Tuovinen, J., van Dingenen, R., Wang, J., Yu, H. B., and Zdanowicz, C.: Chapter A5: Impacts on Health, Ecosystems and Climate, in: Hemispheric Transport of Air Pollution 2010, Part A: Ozone and Particulate Matter, Air Pollution Studies No. 17, 278pp. [F. Dentener, T. Keating, and H. Akimoto (eds)], United Nations, Economic Commission for Europe, 2011. 20. World Health Organization, NIS Environment Strategy background paper Pollution Prevention and Control, WHO Regional Office for Europe, 2002. 21. Yienger, J. J., Galanter, M., Holloway, T. A., Phadnis, M. J., Guttikunda, S. K., Carmichael, G. R., Moxim, W. J., and Levy, H.: The episodic nature of air pollution transport from Asia to North America, Journal of Geophysical Research-Atmospheres, 105, 26931-26945, 2000.

APPENDIX
2001 Emissions Source: EA

Species SO2 (mgS/m2 /year) BC (mgC/m2 /year) POM (mgC/m2 /year)

EU

NA 358.51 17.03 26.26

NA 147.74 6.33 17.35 NA 18.84 6.15 21.54

SA 277.55 40.93 104.54

SA 443.81 50.52 127.26 SA 143.33 24.83 80.20

597.49 742.24 71.02 33.30 99.48 37.55 2030 Emissions

Source: EA EU 362.07 13.96 14.06 EU 75.09 7.82 25.67

Species SO2 (mgS/m2 /year) BC (mgC/m2 /year) POM (mgC/m2 /year)

Species SO2 (mgS/m2 /year) BC (mgC/m2 /year) POM (mgC/m2 /year)

638.57 74.55 89.54 2050 Emissions Source: EA 90.41 20.68 62.74

Table 1. Anthropogenic emissions in source regions for years 2001, 2030, and 2050. SO2, BC, and POM emissions used in GOCART Global Model runs in 2001, 2030, and 2050 emission scenario are shown in the top, middle and bottom sub-tables, respectively. SO2 instead of SO4 emissions were used because most anthropogenic SO4 comes from converted SO2. EA: East Asia. EU: Europe. NA: North America. SA: South Asia.

Receptor: SO4 BC POM SO4 BC POM SO4 BC POM

2001 RAIR EA EU NA 10.00 3.16 4.13 7.11 5.30 5.68

SA

Receptor: SO4 BC POM SO4 BC POM SO4 BC POM

2030 RAIR EA EU 7.12 2.65 4.72 18.67 16.61 26.35 9.27 7.45 9.52 9.01 10.75 13.19 26.69 54.79 64.07 7.51 8.79 8.65

NA 16.62 21.56 10.46 45.01 71.56 56.25 8.86 18.98 14.38

SA 11.27 7.79 4.36 16.22 15.74 8.36 18.53 16.78 9.10

Receptor: SO4 BC POM SO4 BC POM SO4 BC POM

2050 RAIR EA EU 8.32 4.85 4.92 26.25 26.85 26.11 11.74 12.31 11.30 6.22 9.24 6.18 20.55 48.99 41.27 5.60 14.30 9.41

NA 14.94 8.83 6.52 49.40 48.42 41.61 14.88 18.04 12.24

SA 5.05 5.51 5.68 8.17 11.64 11.19 4.35 8.30 7.74

Surface Concentration Response (%)

10.20 22.25 9.62 11.67 7.82 6.68

Surface Concentration Response (%)

Surface Concentration Response (%)

Column Load Response (%)

23.29 20.35 27.74 32.89 17.33 34.12 47.10 22.72 22.58 39.43 45.62 12.89 9.27 7.45 9.52 9.52 8.79 8.65 8.86 18.53 18.98 16.78 14.38 9.10

Column Load Response (%)

Column Load Response (%)

Deposition Response (%)

Deposition Response (%)

Deposition Response (%)

Table 3. Relative Annual Intercontinental Response (RAIR) in 2001, 2030, and 2050. Each sub-table shows RAIR for surface concentration, column load, and deposition for four tagged regions in 2001, 2030, and 2050, respectively. Each number represents the percent of concentrations or depositions of an aerosol (specified on the left of each sub-table) influenced by intercontinental sources (specified on the top of each sub-table). For example, North American BC column load (boxed in red) is 71.56% dependent on intercontinental sources. EA: East Asia. EU: Europe. NA: North America. SA: South Asia. AR: Arctic. 1

! !

A 2001 Surface Concentration Source-Receptor

Receptor SO4 BC POM
EU (% reduction)

Source:

EA

EU

NA

SA

2001 Column Load Source-Receptor Source: EA EU NA Receptor

EA (% reduction)

SA 0.86 1.83 1.36 0.35 1.60 1.06 0.46 1.91 1.01 8.46 10.21 6.51

2001 Deposition Source-Receptor Source: EA EU NA Receptor

EA (% reduction)

SA 0.50 0.87 0.69 0.12 0.29 0.17 0.10 0.56 0.21 12.95 12.22 7.60

EA (% reduction)

11.02 17.06 9.85 0.25 0.35 0.16 0.78 1.03 0.26 1.25 1.10 0.47

0.78 0.19 0.08 13.62 16.65 8.08 0.65 0.30 0.06 2.02 0.60 0.12

0.14 0.05 0.03 0.65 0.33 0.18 13.47 14.93 5.18 0.21 0.08 0.02

0.31 0.31 0.32 0.14 0.25 0.15 0.10 0.26 0.12 12.15 13.51 8.68

SO4 BC POM
EU (% reduction)

8.92 12.36 5.60 0.85 2.19 0.83 1.77 3.74 1.08 1.17 1.83 0.67

1.45 0.53 0.17 10.90 9.88 3.79 1.16 0.65 0.16 2.64 0.94 0.22

0.39 0.23 0.10 1.59 1.33 0.58 8.82 7.08 2.67 0.33 0.23 0.07

SO4 BC POM
EU (% reduction)

11.38 15.27 7.62 0.24 0.59 0.22 0.66 1.79 0.35 1.33 1.68 0.61

0.55 0.27 0.08 13.27 15.53 7.09 0.60 0.55 0.10 1.48 0.67 0.12

0.11 0.09 0.03 0.72 0.62 0.29 13.95 12.37 3.91 0.14 0.11 0.03

SO4 BC POM
NA (% reduction)

SO4 BC POM
NA (% reduction)

SO4 BC POM
NA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM

SO4 BC POM

SO4 BC POM

B 2030 Surface Concentration Source-Receptor

Receptor SO4 BC POM
EU (% reduction)

Source:

EA

EU

NA

SA

2030 Column Load Source-Receptor Source: EA EU NA SA Receptor

EA (% reduction)

2030 Deposition Source-Receptor Source: EA EU NA Receptor

EA (% reduction)

SA 0.80 1.05 0.87 0.33 0.70 0.26 0.30 1.17 0.27 14.83 13.52 8.67

EA (% reduction)

11.46 17.25 9.32 0.46 0.74 0.19 1.51 2.06 0.25 1.03 1.01 0.39

0.34 0.07 0.03 12.60 13.52 3.94 0.49 0.23 0.03 0.72 0.21 0.04

0.05 0.02 0.02 0.40 0.25 0.16 11.48 10.54 3.76 0.06 0.03 0.01

0.50 0.38 0.41 0.39 0.64 0.24 0.29 0.61 0.16 14.26 14.71 9.77

SO4 BC POM
EU (% reduction)

9.54 12.64 5.15 1.42 3.37 0.86 2.70 5.01 1.01 1.08 1.77 0.57

0.63 0.21 0.06 8.78 5.79 1.56 0.69 0.33 0.06 1.05 0.34 0.07

0.14 0.08 0.07 0.89 0.72 0.44 5.45 3.33 1.85 0.10 0.08 0.05

1.42 2.23 1.71 0.88 2.93 1.48 1.07 3.05 1.30 11.49 11.72 7.55

SO4 BC POM
EU (% reduction)

11.67 15.47 7.10 0.44 1.20 0.26 1.30 3.11 0.34 1.06 1.56 0.51

0.23 0.11 0.03 12.72 12.00 3.32 0.46 0.36 0.04 0.51 0.24 0.04

0.03 0.03 0.02 0.44 0.44 0.25 11.83 7.61 2.77 0.04 0.04 0.02

SO4 BC POM
NA (% reduction)

SO4 BC POM
NA (% reduction)

SO4 BC POM
NA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM

SO4 BC POM

SO4 BC POM

C 2050 Surface Concentration Source-Receptor

Receptor SO4 BC POM
EU (% reduction)

Source:

EA

EU

NA

SA

EA (% reduction)

6.12 13.15 7.65 0.13 0.32 0.11 0.45 0.64 0.17 0.33 0.48 0.34

1 0.14 0.11 0.06

0.01 0.05 0.03 0.13 0.37 0.17 5.27 11.57 4.50 0.02 0.04 0.02

0.40 0.51 0.30 0.37 0.48 0.13 0.24 0.33 0.10 13.04 12.41 7.53

2050 Column Load Source-Receptor Source: EA EU NA Receptor EA (% reduction) 1 SO4 3.42 0.23 0.03 BC 7.35 0.24 0.17 POM 4.03 0.13 0.09
EU (% reduction)

SA 0.95 2.29 1.20 0.56 2.15 0.90 0.57 2.07 0.83 7.89 9.25 5.54

2050 Deposition Source-Receptor Source: EA EU NA Receptor EA (% reduction) 1 SO4 5.63 0.09 0.01 BC 10.48 0.14 0.07 POM 5.66 0.07 0.03
EU (% reduction)

SA 0.64 1.26 0.62 0.33 0.52 0.15 0.25 0.69 0.17 13.50 11.26 6.53

SO4 BC POM
NA (% reduction)

9.33 11.50 6.36 0.23 0.14 0.05 0.34 0.20 0.10

SO4 BC POM
NA (% reduction)

0.30 1.41 0.58 0.51 1.93 0.72 0.28 0.79 0.47

4.17 4.81 2.85 0.21 0.25 0.11 0.40 0.30 0.16

0.21 1.06 0.52 1.29 4.53 2.33 0.02 0.12 0.07

SO4 BC POM
NA (% reduction)

0.12 0.50 0.16 0.37 1.04 0.23 0.36 0.74 0.43

9.93 9.98 5.50 0.22 0.24 0.07 0.25 0.22 0.09

0.14 0.65 0.27 4.84 8.92 3.36 0.01 0.06 0.03

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM
SA (% reduction)

SO4 BC POM

SO4 BC POM

SO4 BC POM

Table 2. Source-receptor relationships among tagged regions in 2001, 2030, and 2050. Each number in this table represents the percent reduction in the receptor region (specified on the left of each sub-table) to a 20% reduction in 1 emissions from the source1(specified on the top of each sub-table). For example, East Asian sulfate surface 1 concentration decreases 11.02% in response to a 20% decrease in its own anthropogenic emissions (A, boxed in red). The sub-tables in the left (A, B, C), central (D, E, F), and right (G, H, I) columns show source-receptor relationships in year 2001, 2030 and 2050, respectively. The sub-tables in the top (A, D, G), middle (B, E, H), and bottom (C, F, I) rows show source-receptor relationships for surface concentration, column load, and deposition, respectively. EA: East Asia. EU: Europe. NA: North America. SA: South Asia.