Paper to be submitted to Environmental Science & Technology May, 2000 Haze Trends over the United States, 1980-1995 Rudolf B. Husara, Bret A. Schichtela and William E. Wilsonb aCenter for Air Pollution Impact and Trend Analysis, Washington University, St. Louis, MO, USA Center for Environmental Assessment, US EPA, Research Triangle Park, NC, USA bNational Abstract This is an update of the haze pattern over the U.S. for the period 1980-95, based on human visual range observations at 260 synoptic meteorological stations. There has been a significant (~10%) decline in haziness over the 15 year period. The reductions were evident throughout the eastern US domain as well as over the hazy air basins of California. During the same period, the eastern U.S. sulfur emissions have also declined by about 10%. However, a causality has not been established. 1. Introduction The spatial and temporal trends as well as the man-made causes of atmospheric haze have received considerable attention from North American researchers since the late 1960s. (e.g. Elridge, 1966, Miller et al., 1972; Munn, 1973; Husar et al., 1976; Weiss et al. 1977; Husar et al. 1979; Leaderer et al., 1979; Ferman, 1981; Husar et al., 1981; Robinson and Valente, 1982; Sloane, 1982; Sloane, 1982; Trijonis, 1982; Wolff et al., 1982; Sloane, 1983; Sloane, 1984; Husar and Patterson, 1986; Husar and Wilson, 1993). Much of the recent literature deals with physico-chemical properties of haze, with the aim of understanding its sources and formation mechanisms (NAPAP, 1990). This report is an update of the haze trend research at Washington University's Center for Air Pollution Impact and Trend Analysis that was initiated in 1976. 2. Haze trend data sets The data set used for the visibility trend analysis consist of hourly prevailing daytime (noon) visibility, V, recorded at synoptic weather stations by human observers. The observed visual range (km) is used to calculate the extinction coefficient, bext (km-1) via the Koschmieder relationship bext=K/V (Koschmieder, 1926). The value of K is 1 determined by the threshold sensitivity of the human eye, by the contrast of the visible objects against the horizon sky and by the available visual targets. In this report, we use K=1.9 in accordance with the data by Griffing (1980). The extinction coefficient is in units of km-1 and is proportional to the concentration of light scattering and absorbing aerosols and gases (NAPAP, 1990). The terms extinction coefficient and haze are used here synonymously. For purposes of spatial-temporal trend analysis, the raw visibility observations were summarized as quarterly averages of noontime light extinction coefficient. For each quarter and station, three different extinction coefficients were calculated. The first set included all visibility data regardless of weather and pollutant conditions (BX). The second group (FX) is composed of extinction coefficients excluding precipitation and fog. For the third group (RH) a relative humidity correction was performed to compensate for water vapor effects. This latter parameter is closely related to the dry fine particle aerosol mass concentration. The extinction coefficient calculated from the visual range is influenced by both haze aerosol and natural obstructions to vision, such as rain, fog, and snow. The role of these natural obstructions can be eliminated by discarding the values that occur when these meteorological phenomena occur. The specific parameter that is plotted for the haze maps is the 75th percentile. While this is unconventional, it constitutes the safest approach in that it does not require any extrapolation or other adjustments to the data. A significant problem with airport visual range observations is that there is a furthest marker beyond which the visual range is not resolved (Husar and Wilson, 1993). More conventional statistical measures, e.g. the mean can be estimated as follows: from previous research, e.g. Husar et al. (1979), the extinction coefficient is roughly lognormally distributed with typical logarithmic standard deviation of 2.5. For such a distribution, the 50th percentile is 0.5 times the 75th percentile, and the mean is 0.76 times the 75th percentile. The spatial patterns are presented on contour maps. The contours were derived from the station-point observations using a spatial extrapolation scheme, described previously (Husar et al., 1994) 3. National seasonal trend maps The U.S. haze patterns and trends since 1980 are shown in 12 seasonal maps covering 5-year periods, centered at 1983, 1988, and 1993. (Figure 1). The seasons are defined by calendar quarter. The overall national view shows two large contiguous haze regions, one over the eastern U.S. and another one along the Pacific coast. In between the 2 two haze regions lies a haze free territory that spans from the Rocky Mountains to the Sierra-Cascade mountain ranges. This general pattern was preserved over the past 30year period (Husar and Wilson, 1993). However, notable trends have occurred over both the western and the eastern haze regions. The eastern U.S. shows significant seasonal variation and there is also a significant trend over the past 30 years. The maps in Figure 1 (1980-1995) show that over the eastern U.S., the RH corrected dry extinction coefficient is highest during the summer season (Quarter 3). The highest extinction coefficient (bext>0.2 km-1) is observed adjacent to the Appalachian Mountains in Tennessee and the Carolinas. It is observed, that on the periphery of the eastern U.S. (Maine, Florida, Texas, North Dakota) the summer-time extinction coefficient is less than half (bext<0.1 km-1) of the values near the center of the eastern U.S. The dry extinction coefficient over the eastern U.S. during the cold season, Quarters 1 and 4, is shown on the top and bottom row of maps. In the 1981-1985 period, elevated Quarter 1 haze values (bext>0.2 km-1) are observed between the Great Lakes and the Ohio River Valley. Another region of cold-season haze is observed over the Gulf states between Texas and Florida. Elevated winter-time haze is also evident along the mid-Atlantic coast from North Carolina to New Jersey. The summer time (June, July, August) bext trends for the fifteen year period 198095 are presented in Figure 2. The trends were computed for the 75th and 90th percentile using data from all stations east of the Mississippi River (eastern U.S.), north of Virginia and east of Ohio (northeastern U.S.) and south of Tennessee and east of Mississippi (southeastern U.S.). As shown, over the eastern U.S. there was a 17% decrease in the 90th percentile bext over the fifteen year period, and a 9% decrease of the 75th percentile. Larger decreases in bext were observed in the southeastern U.S., where the 90th and 75th percentiles decreased by 20% and 12 % respectively. Both trends are significant at the 95th percentile using student's t-distribution. The decreases over the Northeast for the 90th and 75th percentiles where 16% and 8% respectively. As a result of the decline over the eastern U.S., by 1991-95, the extinction coefficient was below 0.2 km-1 throughout most including the summer season (Figure 1). The haze pattern and trends over the visually pristine inter-mountain western U.S. can not be evaluated due to the poor distance resolution of the visual range database. Very few monitoring sites report visibility above 30-50 km (0.038<bext<0.063). 3 Elevated haze (bext>0.1 km-1) can be observed throughout the Pacific coast of the U.S. The worst haze can be found in California, throughout the San Joaquin and the Los Angeles basin. The haze is worst during the cold season (Quarters 4 and 1) when bext exceeds 0.2 km-1). During the period 1981-1995, the level of haze has significantly (10%) declined throughout the Pacific coast, including the San Joaquin and Los Angeles basins. Since sulfate constitutes 40-70% (NAPAP 1990??) of the light scattering aerosol over the eastern US, the trend of bext is compared to the sulfur emission trends in Figure 3. The emission data prior to 1985 were taken from Knudson (1985) and Husar (1986) while the values after 1985 were from the NEI (19??). An unusual feature of the sulfur emissions data is the sharp drop in 1995. The comparison in Figure 3. indicates that both the eastern U.S. average bext and sulfur emissions have declined about 10% during the 15year period. Declines are also evident for the Northeastern and the Southeastern U.S. However, the relationship varies significantly from year to year. 4. Discussion Since the late 1980s, visibility trend maps, similar to the ones presented here, were used in the National Air Quality and Emissions Trends report issued by EPA. The Trend Report is the official yearly report card on the nations air quality. This haze trend update indicates that during the 1990-1995 period, the haziness has declined significantly (~10%) throughout the country. The frequency of eastern U.S. haze episodes (90th percentile of bext) has declined even faster. Since the visibility-derived haziness is a surrogate for PM2.5 concentration, this report implies that there was also a significant (~10%) decline in the national PM2.5 levels as well. The causes of the haze and PM2.5 decline were not investigated here in detail. However, it is noted that the haze decline coincided with comparable reductions in the sulfur emissions in the eastern US. In order to establish fully the causality of the observed reductions, additional work needs to be focused on the trends of specific aerosol chemical species, possible changes in the oxidation capacity of the atmosphere and trends of relevant meteorological variables. This suggests that the haze trend data provides a way to monitor the effectiveness of the emission reductions from the 1990 Clean Air Act Amendment. Previous work (Husar and Wilson, 1993) has also linked the regional and seasonal shifts in eastern U.S. haziness to haze precursor emission pattern. 4 It is regrettable that this may be the last U.S. haze trend update based on the surface visibility observations. After 1995, increasing number of visibility data are collected by automatic light scattering sensors that are not fully compatible with the 50year long human observations. [Secondly, the U.S. EPA has discontinued support for this type of visibility trend analyses] References Elridge, R. G., 1986. Climatic visibilities of the United States. J. Appl. Meteorol. 5, 227-282. Ferman, M.A., Wolff, G.T., and Kelly, N.A., 1981. The nature and sources of haze in the Shenandoah Valley/Blue Ridge Mountains area, J. Air Poll. Contr. Assoc. 31, 1074. Griffing G.W., 1980. Relationships between the prevailing visibility, nephelometer scattering coefficient, and sunphotometer turbidity coefficient. Atmos. Environ. 14, 577-584. Holzworth, G.C., 1972. Mixing heights, wind speeds, and potential for urban air pollution throughout the contiguous United States, Environmental Protection Agency, Office of Air Programs, RTP, NC, January. Husar, R.B., Gillani, N.V., Husar, J.D., Paley, C.C., and Turcu, P.N., 1976. Long-range transport of pollutants observed through visibility contour maps, weather maps and trajectory analysis. Preprint volume: Third Symposium on Turbulence, Diffusion and Air Pollution, American Meteorological Society, Reno, NV pp. 344-347. Husar, R.B., Poll, D.E., Holloway, J.M., Wilson, W.E. and Ellestad, T.G., 1979. Trends of eastern U.S. haziness since 1948. Preprint Volume: Fourth Symposium on Turbulence, Diffusion and Air Pollution, American Meteorological Society, Boston, MA pp. 249-256. Husar, R.B., Holloway, J.M., Poll, D.E. and Wilson, W.E., 1981. Spatial and temporal pattern of eastern U.S. haziness: a summary. Atmos. Environ. 15, 1919-1928. Husar, R.B., 1986. Emissions of sulfur dioxide and nitrogen oxides and trends for eastern north America. In Acid Deposition: Long-Term Trends. National Academy Press , Washington, D.C. 1986; pp 48-92. Husar R.B. and Patterson D.E., 1986. Haze Climate of the United States. U.S. Environmental Protection Agency, EPA-600/3-86-071, Research Triangle Park, NC. Husar R.B. and Wilson W.E., 1993. Haze and Sulfur Emission Trends in the Eastern United States, Environ Sci. Technol., 27, 12-16. Husar R.B., Elkins, J.B. and Wilson, W.E., 1994. U.S. Visibility Trends, 1960-1992, Regional and National. Presented at 87th Annual A&WMA Meeting, 19-24 June, Cincinnati, Ohio. Knudson, D.A., 1985. Estimated monthly emissions of sulfur dioxide and oxides of nitrogen for the 48 contiguous states, 1975-1984. U.S. Department of Energy, ANL/EES-TM-318, Vol 1. Koschmieder H., 1926. Theorie der horizontalen Sichtweite, Beit. Phys. Atmos., 12, 33-55. Leaderer, B.P. and Stolwijk, J.A., 1979. Optical properties of urban aerosol and their relation to chemical composition. Presented at the New York Academy of Science Symposium on Aerosols: Anthropogenic and Natural Sources and Transport, Jan. 9-12. Miller, M.E., Canfield, N.L., Ritter, T.A. and Weaver, C.R., 1972. Visibility changes in Ohio, Kentucky, and Tennessee from 1962 to 1969. Monthly Weather Review 100, 67-71. Munn, R.E., 1973. Secular increases in summer haziness in the Atlantic provinces, Atmosphere, 11, 156161. NAPAP, 1990. Acid Deposition: State of Science and Technology. Visibility: Existing and Historical Conditions-Causes and Effects. Report 24, National Acid Precipitation Assessment Program, Washington D.C.; Robinson, E. and Valente, R.J., 1982. Atmospheric turbidity over the United States, 1948-1978. Research Publication GMR-3474, Env #92, General Motors Corp. 5 Schichtel, B.A., Husar, R.B. Wilson, W.E., Poirot, R. and Malm, W.C., 1991. Reconciliation of visibility and aerosol composition data over the U.S, 84th Annual A&WMA meeting, June16-21, Vancouver. Sloane, C.S., 1982. Visibility Trends II: Methods of Analysis, Atmos. Environ. 16, 41. Sloane, C.S., 1982. Visibility Trends II: Mideastern United States, Atmos. Environ. 16, 2309. Sloane, C.S., 1982. Summertime visibility declines: meteorological influences. Atmos. Environ. 17, 763774. Sloane, C.S., 1984. Meteorologically adjusted air quality trends: visibility, Atmos. Environ. 18, 12171229. Trijonis, J., 1982. Existing and natural background levels of visibility and fine particles in the rural East. Atmos. Environ. 16, 2431. Waggoner, A.P. and Weiss, R.E., 1986. Impact of the chemical and physical properties of fine and coarse particles on visibility. In Aerosols Lee S. D., Schneider T., Grant L.D., and Verkerk P.J. (Eds.). Lewis Publishers, Chelsea, MI. Weiss, R.E., Waggonner, A.P., Charlson, R.J. and Ahlquist, N.C., 1977. Sulfate aerosol: its geographical extent in the midwestern and southern United States. Science 197, 997-998. Wolff, G.T., Kelly, N.A. and Ferman, M.A., 1982. Source regions of summertime ozone and haze episodes in the eastern United States. Water Air Pollution. 6 7 Figure 1. United States trend maps for the 75th percentile RH corrected extinction coefficient, b ext for winter (Q1), spring (Q2), summer (Q3), and fall (Q4). b ext [km-1] is derived from visual range, VR, data by bext =1.9/VR. Data during natural obstructions to vision (rain, snow, fog) were eliminated. 8 9 Eastern US 0.32 0.3 0.3 16% / 15 Yrs 90% Conf. 0.28 0.26 0.26 0.2 bext (1/km) bext (1/km) 0.22 0.24 0.22 0.2 9% / 15 Yrs 85% Conf. 0.24 0.22 0.2 8% / 15 Yrs 65% Conf. 0.18 0.18 0.18 0.16 0.16 0.16 0.14 0.14 80 83 86 89 92 12% / 15 Yrs 95% Conf. 0.14 80 95 20% / 15 Yrs 95% Conf. 0.28 0.26 0.24 Southeastern US 0.32 0.3 17% / 15 Yrs 95% Conf. 0.28 bext (1/km) Northeastern US 0.32 83 86 89 92 95 80 83 86 Year Year 89 92 95 Year 90th Percentile - Top Trends 75th Percentile - Bottom Trends Figure 2. Trends of the summertime 90th and 75th percentile light extinction for the eastern, Northeastern and Southeastern US from 1980-95. The confidence level for each trend is based on the two sided Student's t-distribution. Eastern US Southeastern US Northeastern US 0.2 0.2 0.2 10.5 75th %-ile bext Sulfur Emissions 0.14 7.5 6.5 5.5 80 83 86 89 Year 92 95 0.16 75th %-ile bext 3.3 0.12 2.8 0.1 2.3 0.14 0.18 2.3 Sulfur Emissions 0.16 0.14 1.8 0.12 0.12 0.1 80 83 86 89 Year 92 95 bext (1/km) 8.5 3.8 bext (1/km) 0.16 0.18 Yearly Sulfur Emissions (Million Tons Sulfur) Sulfur Emissions 75th %-ile bext Yearly Sulfur Emissions (Million Tons Sulfur) 9.5 bext (1/km) Yearly Sulfur Emissions (Million Tons Sulfur) 4.3 0.18 1.3 0.1 80 83 86 89 92 95 Year Figure 3. Comparison of the annual sulfur emission trends and summertime 75th percentile light extinction coefficient for the eastern US, Northeastern US and Southeastern US. During 1980-95, the eastern US haze and sulfur emission have declined at a comparable rate of 10%. 10