Spatial and Temporal Variability of Ozone Exposure in Forested Areas of the United States and Canada: 1978—1988

Ambient O₃ exposures have reduced growth rates of tree genotypes in some areas of the United States. For characterizing O₃ exposures in forested areas, data from primarily population-oriented sites have been used. It has been speculated that exposures calculated from population-oriented sites provide estimates greater than those that would actually be experienced in the majority of forested areas. Accordingly, we compared 1988 O₃ data from three remote forested sites with data from several population-oriented monitoring sites in and around the mid? and southern Appalachian Mountains. The number of hours ≥0.08 ppm was lower at the remote forested sites than at the nearby population-oriented locations. In addition, we characterized the temporal variability of O₃ exposures in forested regions of the United States and Canada for the period 1978-1988. We found that the years of highest O₃ exposure in the eastern United States during 1978-1988 were 1978, 1980, 1983, and 1988, with 1988 being the worst year in four of seven eastern forest regions. In 1988, the Whiteface Mountain summit site (1483 m) experienced approximately 10 percent more hourly average concentrations ≥0.08 ppm than in the second highest O₃ exposure year (i.e., 1979). Consistently throughout the 11-year period, the highest O₃ exposures at the Whiteface Mountain site occurred during the late evening and early morning hours, with the result that the longterm 7-h (0900-1559h) exposure index could not distinguish those years in which the highest exposures occurred from those in which the lowest occurred. Similar to the Whiteface Mountain site, two high-elevation Shenandoah National Park sites experienced their highest O₃ exposures in 1988. With the exception of 1986, the lower elevation site (Dickey Ridge) consistently experienced more frequent occurrences of hourly average concentrations ≥0.08 ppm than the higher elevation site (Big Meadows).     

An Evaluation of the Kriging Method to Predict 7-h Seasonal Mean Ozone Concentrations for Estimating Crop Losses

Using kriging, a statistical technique, the National Crop Loss Assessment Network (NCLAN) program estimated growing season 5-month (May-September) ambient 7-h mean O₃ concentrations for each of the major crop growing areas of the United States for 1978-1982. The O₃ estimates were used to predict economic benefits anticipated by lowering O₃ levels in the United States. This paper reviews NCLAN’s use of kriging to estimate 7-h seasonal mean O₃ concentrations for crop growing regions. Although the original kriging program used by NCLAN incorrectly calculated the diagonal elements of the kriging equations, this omission did not result in significant errors in the predicted estimates. Most of the data used in estimating the 7-h seasonal values were obtained from urban areas; the use of these data tended to underestimate the 7-h seasonal O₃ concentrations in rural areas. It is recommended that only O₃ data that are representative of agricultural areas and have been collected under accepted quality assurance programs be used In future kriging efforts.     

The Characterization of Ozone Data for Sites Located in Forested Areas of the Eastern United States

Six years (1978-1983) of ozone monitoring data from sites located within six forested areas were examined. Areas that experienced the lowest to the highest ozone exposures were located in (1) northern New England/New York and upper Great Lakes, (2) New York/Pennsylvania/Maryland, (3) southeastern/southern, and (4) New Jersey pinelands. In general, higher ozone concentrations were observed in 1978, 1980 and 1983 as compared to the other three years examined. Ozone concentrations varied considerably within the areas. Recommendations for additional ozone monitoring sites are made. A concentrated effort should be made to examine ozone monitoring data from subsequent years (1984, 1985, and 1986) to explore whether the 6-year period 1978 through 1983 is representative of the annual variability of ozone concentrations over eastern forested areas. To better understand the relationship between ozone exposure and possible forest effects, we recommend that the temporal distributions of elevated ozone concentrations over a growing season be examined. The occurrence of elevated ozone levels during specific growth periods during a season may be an important aspect that biologists may wish to explore.     

Modeling an air pollution episode in northwestern United States: Identifying the effect of nitrogen oxide and volatile organic compound emission changes on air pollutants formation using direct sensitivity analysis

Air quality impacts of volatile organic compound (VOC) and nitrogen oxide (NO_x) emissions from major sources over the northwestern United States are simulated. The comprehensive nested modeling system comprises three models: Community Multiscale Air Quality (CMAQ), Weather Research and Forecasting (WRF), and Sparse Matrix Operator Kernel Emissions (SMOKE). In addition, the decoupled direct method in three dimensions (DDM-3D) is used to determine the sensitivities of pollutant concentrations to changes in precursor emissions during a severe smog episode in July of 2006. The average simulated 8-hr daily maximum O₃ concentration is 48.9 ppb, with 1-hr O₃ maxima up to 106 ppb (40 km southeast of Seattle). The average simulated PM_2.5 (particulate matter with an aerodynamic diameter <2.5 μm) concentration at the measurement sites is 9.06 μg m^?3, which is in good agreement with the observed concentration (8.06 μg m^?3). In urban areas (i.e., Seattle, Vancouver, etc.), the model predicts that, on average, a reduction of NO_x emissions is simulated to lead to an increase in average 8-hr daily maximum O₃ concentrations, and will be most prominent in Seattle (where the greatest sensitivity is??0.2 ppb per % change of mobile sources). On the other hand, decreasing NO_x emissions is simulated to decrease the 8-hr maximum O₃ concentrations in remote and forested areas. Decreased NO_x emissions are simulated to slightly increase PM_2.5 in major urban areas. In urban areas, a decrease in VOC emissions will result in a decrease of 8-hr maximum O₃ concentrations. The impact of decreased VOC emissions from biogenic, mobile, nonroad, and area sources on average 8-hr daily maximum O₃ concentrations is up to 0.05 ppb decrease per % of emission change, each. Decreased emissions of VOCs decrease average PM_2.5 concentrations in the entire modeling domain. In major cities, PM_2.5 concentrations are more sensitive to emissions of VOCs from biogenic sources than other sources of VOCs. These results can be used to interpret the effectiveness of VOC or NO_x controls over pollutant concentrations, especially for localities that may exceed National Ambient Air Quality Standards (NAAQS).

Implications: The effect of NO_x and VOC controls on ozone and PM_2.5 concentrations in the northwestern United States is examined using the decoupled direct method in three dimensions (DDM-3D) in a state-of-the-art three-dimensional chemical transport model (CMAQ). NO_x controls are predicted to increase PM_2.5 and ozone in major urban areas and decrease ozone in more remote and forested areas. VOC reductions are helpful in reducing ozone and PM_2.5 concentrations in urban areas. Biogenic VOC sources have the largest impact on O₃ and PM_2.5 concentrations.     

Ambient Ozone Concentration Patterns among Eastern U.S. Urban Areas Using Factor Analysis

Data on dally maximum ozone concentrations measured at ambient air monitoring stations operated by state and local air pollution control agencies in the Eastern United States were analyzed using principal factor analysis. Four orthogonal factors representing O₃ formation potentials were derived using the statistical package SPSS; these factors accounted for over two-thirds of the variations in 1978 summer O₃ levels at 21 urban-oriented stations. The analysis confirmed that O₃ variations are similar among stations within defined geographical areas; this confirmation supports the widely held theory that ambient O₃ formations are reglonwlde. The analysis suggested that trends analysis for determining general progress in improving O₃ air quality should be based on aggregate statistics from clusters of monitors rather than from a single monitoring station within areas associated with the derived factors.     

DNA damage in Populus tremuloides clones exposed to elevated O3

The effects of elevated concentrations of atmospheric tropospheric ozone (O₃) on DNA damage in five trembling aspen (Populus tremuloides Michx.) clones growing in a free-air enrichment experiment in the presence and absence of elevated concentrations of carbon dioxide (CO₂) were examined. Growing season mean hourly O₃ concentrations were 36.3 and 47.3 ppb for ambient and elevated O₃ plots, respectively. The 4th highest daily maximum 8-h ambient and elevated O₃ concentrations were 79 and 89 ppb, respectively. Elevated CO₂ averaged 524 ppm (+150 ppm) over the growing season. Exposure to O₃ and CO₂ in combination with O₃ increased DNA damage levels above background as measured by the comet assay. Ozone-tolerant clones 271 and 8L showed the highest levels of DNA damage under elevated O₃ compared with ambient air; whereas less tolerant clone 216 and sensitive clones 42E and 259 had comparably lower levels of DNA damage with no significant differences between elevated O₃ and ambient air. Clone 8L was demonstrated to have the highest level of excision DNA repair. In addition, clone 271 had the highest level of oxidative damage as measured by lipid peroxidation. The results suggest that variation in cellular responses to DNA damage between aspen clones may contribute to O₃ tolerance or sensitivity.     

Understanding the Effectiveness of Precursor Reductions in Lowering 8-Hr Ozone Concentrations—Part II. The Eastern United States

Abstract

Analyses of ozone (O₃) measurements in conjunction with photochemical modeling were used to assess the feasibility of attaining the federal 8-hr O₃ standard in the eastern United States. Various combinations of volatile organic compound (VOC) and oxides of nitrogen (NO_x) emission reductions were effective in lowering modeled peak 1-hr O₃ concentrations. VOC emissions reductions alone had only a modest impact on modeled peak 8-hr O₃ concentrations. Anthropogenic NO_x emissions reductions of 46–86% of 1996 base case values were needed to reach the level of the 8-hr standard in some areas. As NO_x emissions are reduced, O₃ production efficiency increases, which accounts for the less than proportional response of calculated 8-hr O₃ levels. Such increases in O₃ production efficiency also were noted in previous modeling work for central California. O₃ production in some urban core areas, such as New York City and Chicago, IL, was found to be VOC-limited. In these areas, moderate NO_x emissions reductions may be accompanied by increases in peak 8-hr O₃ levels. The findings help to explain differences in historical trends in 1- and 8-hr O₃ levels and have serious implications for the feasibility of attaining the 8-hr O₃ standard in several areas of the eastern United States.     

A 13-Week Comparison of Passive and Continuous Ozone Monitors at Forested Sites in North-Central Pennsylvania

ABSTRACT

Ogawa passive O₃ samplers were used in a 13-week study (June 1-September 1, 1999) involving 11 forested and mountaintop sites in north-central Pennsylvania. Four of the sites were collocated with TECO model 49 O₃ analyzers. A significant correlation (p < 0.0001) was found for 24-hr average weekly O₃ concentrations between the two methodologies at the four sites with collocated monitors. As expected, there were positive relationships between increasing elevation of the sites and increasing O₃ concentrations. No O₃ exposure patterns were found on a west-to-east or south-to-north basis; however, the area known for lower O₃ exposures within a smaller subsection of the study area showed consistently lower O₃ exposures. Preliminary results regarding relationships of symptom responses within O₃-sensitive bioindicators are also presented with black cherry (Prunus serotina, Elirli.) and common milkweed (Asclepias syriaca, L.) showing clear evidence of increasing injury with increasing O₃ exposures. Due to the extremely dry conditions encountered in north-central Pennsylvania during the 1999 growing season, O₃-induced symptoms were sporadic and quite delayed until late-season rains during the latter portion of the observation period.     

Ozone Transport

Elevated concentrations of ozone, often above the national ambient air quality standard for photochemical oxidants, have been measured in both urban and rural areas of Connecticut. One such episode took place on June 10, 1974. Ozone levels, after stabilizing at values slightly above the standard (i.e., 80 to 110 ppb; Connecticut generated ozone concentrations), rose sharply late in the afternoon reaching concentrations as high as 310 ppb (almost 4 times the standard) in Hartford. The trajectory of the air mass, which arrived in Hartford at the time of maximum O₃ occurence, had its origin in the metropolitan New York area during the early morning rush hour on the episode day. This illustrates that the advective transport of O₃ and O₃ precursors into Connecticut from New York are probably responsible for a significant portion (approximately two-thirds) of the elevated O₃ concentrations measured throughout Connecticut on days when winds are from the south-southwest direction. The fact that peak O₃ levels occur late in the afternoon, several hours after maximum sunlight intensity, reinforces the conclusion that excessive O₃ concentrations developed as O₃ and ozone precursors were generated in the vicinity of New York City and then drifted inland into Connecticut on the afternoon sea breeze.

It appears to be unrealistic to develop a hydrocarbon control strategy for Connecticut in order to meet the photochemical oxidant ambient air quality standard when O₃ and/or ozone precursors ad-vectively transported into the State cause oxidant levels to exceed the standard. The complete cessation of all anthropogenic hydrocarbon emissions in Connecticut would not necessarily assure that the standard would be attained here. The implication is that a regional (i.e., the eastern part of the United States) hydrocarbon control strategy is needed to reduce adequately ozone formation and transport so as to allow Connecticut to meet the current oxidant standard.     

Soil nitrogen transformations under elevated atmospheric CO₂ and O₃ during the soybean growing season

We investigated the influence of elevated CO₂ and O₃ on soil N cycling within the soybean growing season and across soil environments (i.e., rhizosphere and bulk soil) at the Soybean Free Air Concentration Enrichment (SoyFACE) experiment in Illinois, USA. Elevated O₃ decreased soil mineral N likely through a reduction in plant material input and increased denitrification, which was evidenced by the greater abundance of the denitrifier gene nosZ. Elevated CO₂ did not alter the parameters evaluated and both elevated CO₂ and O₃ showed no interactive effects on nitrifier and denitrifier abundance, nor on total and mineral N concentrations. These results indicate that elevated CO₂ may have limited effects on N transformations in soybean agroecosystems. However, elevated O₃ can lead to a decrease in soil N availability in both bulk and rhizosphere soils, and this likely also affects ecosystem productivity by reducing the mineralization rates of plant-derived residues.     

Co-occurrence patterns of gaseous air pollutant pairs at different minimum concentrations in the United States

The frequency of co-occurrences for SO₂NO₂, SO₂/O₃ and O₃/NO₂ at rural and remote monitoring sites in the United States was characterized for the months of May-September for the years 1978–1982. Minimum hourly concentrations of 0.03 and 0.05 ppm of each gas were used as the criteria for defining a ‘co-occurrence’. The objectives of this study were to:

• 1.(1) identify the types of co-occurrence patterns and their frequency;
• 2.(2) identify whether the frequency of hourly simultaneous co-occurrences increased substantially when the minimum concentration was lowered (e.g. from 0.05 to 0.03 ppm) for each pollutant; and
• 3.(3) determine whether the frequency of co-occurrences showed large year-to-year variation.

For all pollutant pairs and co-occurrence thresholds (i.e. 0.03 and 0.05 ppm), the frequency of daily and hourly co-occurrences was low for most sites. Year-to-year variability was found to be insignificant; most of the monitoring sites experienced co-occurrences of any type less than 12% of the 153 days. Based on our observations, researchers attempting to assess the potential effects of SO₂/NO₂, SO₂/O₃ and O₃/NO₂ in the United States should construct simulated exposure regimes so that

• 1.(1) hourly simultaneous and daily simultaneous-only co-occurrences are fairly rare and
• 2.(2) when co-occurrences are present, complex-sequential and sequential-only co-occurrence patterns predominate.

     

The Impact of Stratospheric Ozone on Tropospheric Air Quality

A background of ozone (O₃), principally of stratospheric origin, is present in the lower free troposphere. Typical mean O₃ levels of 50 ppb, 40 ppb, and 30 ppb are encountered here in spring, summer, and fall, respectively. Maximum hourly O₃ concentrations which are twice these mean values can be expected. Ozone from the free troposphere is routinely brought down to ground level under turbulent atmospheric conditions. Deep and rapid Intrusions of stratospheric air into the lower troposphere are associated with low-pressure troughs and occur regularly. In the mid troposphere, O₃ levels as high as 300 ppb are found within these intrusions. Observational data showing these intrusions, containing high O₃ concentrations, to directly reach ground level are currently lacking. Over the United States, an intrusion was present aloft on 8 9% of the days in 1978. The frequency, however, is somewhat reduced in summer and a northward movement is evident. During 1978, no intrusion occurred south of 30°N between June and August and none south of 40 °N in August.

The hypothesis that low levels of stratospheric O₃ produce disproportionately large amounts of O₃ in the polluted atmosphere cannot be supported from currently known chemistry but should be studied further. The experimental technique involving a ⁷Be/O₃ ratio to estimate the daily stratospheric component of ground level O₃ is unverified and considered to be inadequate for air quality applications. Estimates resulting from such a technique are considered uncertain by a factor of more than three. Specially designed aircraft studies provide the best means to determine quantitatively the impact of stratospheric O₃ on ground level air quality.     

Will photosynthetic capacity of aspen trees acclimate after long-term exposure to elevated CO2 and O3?

Photosynthetic acclimation under elevated carbon dioxide (CO₂) and/or ozone (O₃) has been the topic of discussion in many papers recently. We examined whether or not aspen plants grown under elevated CO₂ and/or O₃ will acclimate after 11 years of exposure at the Aspen Face site in Rhinelander, WI, USA. We studied diurnal patterns of instantaneous photosynthetic measurements as well as A/C_i measurements monthly during the 2004-2008 growing seasons. Our results suggest that the responses of two aspen clones differing in O₃ sensitivity showed no evidence of photosynthetic and stomatal acclimation under either elevated CO₂, O₃ or CO₂ + O₃. Both clones 42E and 271 did not show photosynthetic nor stomatal acclimation under elevated CO₂ and O₃ after a decade of exposure. We found that the degree of increase or decrease in the photosynthesis and stomatal conductance varied significantly from day to day and from one season to another.     

Exposure to moderate concentrations of tropospheric ozone impairs tree stomatal response to carbon dioxide

With rising concentrations of both atmospheric carbon dioxide (CO₂) and tropospheric ozone (O₃), it is important to better understand the interacting effects of these two trace gases on plant physiology affecting land-atmosphere gas exchange. We investigated the effect of growth under elevated CO₂ and O₃, singly and in combination, on the primary short-term stomatal response to CO₂ concentration in paper birch at the Aspen FACE experiment. Leaves from trees grown in elevated CO₂ and/or O₃ exhibited weaker short-term responses of stomatal conductance to both an increase and a decrease in CO₂ concentration from current ambient level. The impairement of the stomatal CO₂ response by O₃ most likely developed progressively over the growing season as assessed by sap flux measurements. Our results suggest that expectations of plant water-savings and reduced stomatal air pollution uptake under rising atmospheric CO₂ may not hold for northern hardwood forests under concurrently rising tropospheric O₃.     

Growth of soybean at future tropospheric ozone concentrations decreases canopy evapotranspiration and soil water depletion

Tropospheric ozone is increasing in many agricultural regions resulting in decreased stomatal conductance and overall biomass of sensitive crop species. These physiological effects of ozone forecast changes in evapotranspiration and thus in the terrestrial hydrological cycle, particularly in intercontinental interiors. Soybean plots were fumigated with ozone to achieve concentrations above ambient levels over five growing seasons in open-air field conditions. Mean season increases in ozone concentrations ([O₃]) varied between growing seasons from 22 to 37% above background concentrations. The objective of this experiment was to examine the effects of future [O₃] on crop ecosystem energy fluxes and water use. Elevated [O₃] caused decreases in canopy evapotranspiration resulting in decreased water use by as much as 15% in high ozone years and decreased soil water removal. In addition, ozone treatment resulted in increased sensible heat flux in all years indicative of day-time increase in canopy temperature of up to 0.7 °C.     

A comparison of North American and Asian exposure–response data for ozone effects on crop yields

Modelling-based studies to assess the extent and magnitude of ozone (O₃) risk to agriculture in Asia suggest that yield losses of 5–20% for important crops may be common in areas experiencing elevated O₃ concentrations. These assessments have relied on European and North American dose–response relationships and hence assumed an equivalent Asian crop response to O₃ for local cultivars, pollutant conditions and climate. To test this assumption we collated comparable dose–response data derived from fumigation, filtration and EDU experiments conducted in Asia on wheat, rice and leguminous crop species. These data are pooled and compared with equivalent North American dose–response relationships. The Asian data show that at ambient O₃ concentrations found at the study sites (which vary between ～35–75 ppb 4–8 h growing season mean), yield losses for wheat, rice and legumes range between 5–48, 3–47 and 10–65%, respectively. The results indicate that Asian grown wheat and rice cultivars are more sensitive to O₃ than the North American dose–response relationships would suggest. For legumes the scatter in the data makes it difficult to reach any equivalent conclusion in relative sensitivities. As such, existing modelling-based risk assessments may have substantially underestimated the scale of the problem in Asia through use of North American derived dose–response relationships.     

Wetfall Deposition and Precipitation Chemistry for a Central Appalachian Forest

Abstract

Although extensive research on acidic deposition has been directed toward spruce-fir forests, less research has been done on the impacts of air pollution on eastern montane hardwood forests. The purpose of this study was to describe precipitation chemistry for several Appalachian hardwood forest sites at or near the Fernow Experimental Forest (FEF) to assess the potential for problems associated with acidic deposition. Emphasis was placed on seasonal patterns of ionic concentrations (H+, Ca++, NH4+; NO3-, and SO4=) and spatial variability of ionic concentrations and deposition among sites. Seasonal patterns of most ions showed highest concentrations during the summer months and deposition of H+ was especially pronounced during this time. Deposition of all ions was generally greater (related to greater precipitation) at three montane forested sample sites compared to a nonforested riverbottom site. Precipitation chemistry at FEF was similar to other sites throughout the eastern United States and contrasted sharply with mid-western and western sites. Eastern sites, including means for FEF sites, were uniformly 3-4 times higher in H+ and SO4= concentration than the mid-western and western sites. Precipitation at FEF was chronically acidic, more so during the growing season, and highest at higher elevations where environmental stresses can be most severe. Furthermore, there were occasional large discrepancies between the low-elevation site and the higher-elevation forested sites for precipitation chemistry and acidic deposition. These results suggest that synoptic-scale (network) data may greatly underestimate the pollutant conditions to which highelevation forest trees are exposed, since network data rarely take elevation into account and typically are based on annual ionic concentration and deposition means that may be considerably lower than those of the growing season.     

Use of Plants for Air Pollution Monitoring

Leaf injury data from acute and chronic exposure studies of Dare soybean were regressed against the logarithms of exposure time and O₃ and SO₂ concentrations to develop a new two-pollutant leaf injury model (which explains 88% of the variance) and to calculate the parameters of best fit for this new model and a previously developed one-pollutant model. Using the calculated parameters, the percentage of leaf surface Injured over a growing season by O₃, SO₂, or both simultaneously was estimated for an ambient air sampling site located 2 miles from a coal burning power plant. For this site, the one- and two-pollutant models predicted that SO₂ effects would be negligible If SO₂ concentrations never exceeded the National Ambient Air Quality Standard (NAAQS) of 0.50 ppm, averaged over 3 h. However, calculations suggest that O₃ may injure up to 24% of Dare soybean leaf surface over a growing season even though the O₃ NAAQS of 0.12 ppm, averaged over 1 h, is never exceeded. Because the 3 h SO₂ standard is exceeded at very few places, the O₃ model is usually sufficient to estimate Dare soybean leaf Injury. Leaf injury is estimated by taking the logarithm of the summation of each daytime hour’s exponentiated O₃ concentration (c) measured at an ambient air sampling site over a growing season. This is expressed as: z = -0.0828 + 0.4876 in (Σco₃ ^2.618), where z is the Gaussian transform of percent leaf injury. The methods developed in this paper, using Dare soybean data as an example, may apply to other plants.     

The use of air quality forecasts to assess impacts of air pollution on crops: Methodology and case study

It has been reported that ambient ozone (O₃), either alone or in concurrence with acid rain precursors, accounts for up to 90% of US crop losses resulting from exposure to all major air pollutants. Crop damage due to O₃ exposure is of particular concern as ambient O₃ concentrations remain high in many major food-producing regions. Assessing O₃ damage to crops is challenging due to the difficulties in determining the reduction in crop yield that results from exposure to surface O₃, for which monitors are limited and mostly deployed in non-rural areas. This work explores the potential benefits of using operational air quality forecast (AQF) data to estimate rural O₃ exposure. Using the results from the first nationwide AQF as a case study, we demonstrate how the O₃ data provided by AQF can be combined with concurrent crop information to assess O₃ damages to soybeans in the United States. We estimate that exposure to ambient O₃ reduces the US soybean production by 10% in 2005.     

Ozone Air Quality over North America: Part I—A Review of Reported Trends

ABSTRACT

Ozone and precursor trends can be used to measure the effectiveness of regulatory programs that have been implemented. In this paper, we review trends in the concentrations of O₃, NO_x, and HCs over North America that have been reported in the literature. Although most existing trend studies are confounded by meteorological variability, both the raw data trends and the trends adjusted for meteorology collectively indicate a general decreasing trend in O concentrations in most areas of the United States during 1985-1996. In Canada, mean daily maximum 1-hr O₃ concentrations at urban sites show mixed trends with a majority of sites showing an increase from 1980 to 1993. Mean daily maximum 1-hr O₃ at most regionally representative Canadian sites appears to decrease from 1985 to 1993 or shows no significant change. There are far fewer data and analyses of NO_x and HC trends. Available studies covering various ranges of years indicate decreases in ambient NO_x and HC concentrations in Los Angeles, CA, decreases in HC concentrations in northeastern U.S. cities, and decreases in NO concentrations in Canadian cities. Two key needs are long-term HC and NO_x measurements, particularly at rural sites, and a systematic comparison of trend detection techniques on a reference data set.