A study of ground-level ozone pollution, ozone precursors and subtropical meteorological conditions in central Taiwan

Hourly concentrations of ozone (O(3)), 55 volatile organic compounds (VOCs, ozone precursors) and nitrogen oxides (NOx) were measured at an upwind urban site, a downwind suburban site, and a rural site in central Taiwan, from January 2003 to December 2006. VOC and NOx mean concentrations showed a gradient from high to low across the urban (56 ppb and 34 ppb), suburban (38 ppb and 27 ppb) and rural sites (25 ppb and 21 ppb) but a reverse gradient in ozone across these sites (24, 27, and 29 ppb, respectively). Although there was about twice the difference in VOC concentrations between the urban and rural sites, nearly 65% ozone formation potential was contributed to by the same 9 VOCs. Seasonal patterns showed peak ozone levels in autumn and minima in summer at the urban site, but minima in winter at the downwind suburban and rural sites. Ozone precursor levels, on the other hand, were lowest in summer and highest in winter. The diurnal pattern showed that ozone levels peaked one hour later at the rural site than at the urban site. The ethylbenzene to m,p-xylene ratio, an indicator of the age of the air mass, increased from 0.4 at the urban site to 0.6 at the suburban site and 0.8 at the rural site during daily peak ozone times. This finding suggests the transport of ozone and precursors from upwind to downwind producing elevated ozone levels in the suburban and rural areas. Ozone episodes occurred mostly in days with a mean midday UV index of 6.5 (1 UV index=100 J m(-2)) and wind speed at 1.3 m s(-1) at all three sites.     

Forest Vegetation Monitoring and Foliar Chemistry of Red Spruce and Red Maple at Acadia National Park in Maine

The USDA Forest Service Forest Health Monitoring (FHM) program indicators, including forest mensuration, crown condition classification, and damage and mortality indicators were used in the Cadillac Brook and Hadlock Brook watershed forests at Acadia National Park (ANP) along coastal Maine. Cadillac Brook watershed burned in a wildfire in 1947. Hadlock Brook watershed, undisturbed for several centuries, serves as the reference site. These two small watersheds have been gauged and monitored at ANP since 1998 as part of the Park Research and Intensive Monitoring of Ecosystems Network (PRIMENet). Forest vegetation at Hadlock Brook was dominated by late successional species such as Acer saccharum, Fagus grandifolia, Betula alleghaniensis, Acer rubrum and Picea rubens. Forest vegetation at Cadillac Brook, on the other hand, was younger and more diverse and included those species found in Hadlock as well as early successional species such as Betula papyrifera and Populus grandidentata. Differences in forest species composition and stand structure were attributed to the severe wildfire that affected the Cadillac Brook watershed. Overall, the forests at these ANP watersheds were healthy with a low percentage (相似文献   

Reduced sulfur compounds in ambient air surrounding an industrial region in Korea

The atmospheric concentrations of several reduced sulfur compounds (RSCs) including H(2)S, CH(3)SH, DMS, CS(2), and DMDS were measured concurrently from a series of field campaigns covering multiple locations in the surroundings of a large industrial region (August 2004 to September 2005). These field studies have been designed and undertaken to inspect the concentrations of RSCs in ambient air. The RSC concentrations were found to occur in a highly variable range. H(2)S (1.06 +/- 2.07 ppb) was found to be the most abundant RSC followed by CS(2) (0.84 +/- 0.54 ppb), DMDS (0.36 +/- 1.21 ppb), DMS (0.24 +/- 0.83 ppb), and CH(3)SH (0.11 +/- 0.23 ppb). The RSC levels measured at the study area were comparable to those observed previously from other polluted environmental settings. When these RSC data were examined further in terms of spatial (industrial vs. non-industrial sites) and seasonal (summer vs. winter seasons) grouping schemes, differences in their concentration levels were statistically insignificant in most cases. In contrast, there were fairly strong variations in temporal patterns over a diurnal cycle. If these RSC concentration data were converted to diagnose the malodor strengths, their effects were in most cases insignificant with minor contribution towards odor nuisances.     

Monitoring ammonia in urban, inner alpine and pre-alpine ambient air

Passive samplers were used to monitor ammonia concentrations at rural inner alpine and pre-alpine, as well as urban, sites in Austria and Bavaria. Elevated concentrations were measured both at farms (up to 36 microg NH3 m(-3)) and at urban locations (up to 28 microg NH3 m(-3)). At urban locations a linear relationship between the traffic density and the NH3 concentration was found, but there was no marked seasonal trend. The highest ammonia concentrations were measured in a traffic tunnel (up to 78 microg NH3 m(-3)). The presence of livestock breeding or small scale alpine pastures resulted in elevated concentrations at the rural sites (8.1-12 and 2.5-4.6 microg NH3 m(-3), respectively), compared to the surrounding areas (3.1 and 0.9 microg NH3 m(-3)). Agriculture related sources are usually limited either spatially or seasonally. As the emissions were moderate in our case, a rapid removal and dilution of ammonia was possible and therefore the NH3 burden was only local. Sources related to traffic are more evenly distributed both geographically and seasonally. The WHO guideline, annual average concentration of 8 microg m(-3) for the protection of vegetation, was only exceeded at farms, at the urban station with the heaviest traffic and in the Tauerntunnel.     

Trend, seasonal and multivariate modelling study of wet precipitation data from the Austrian Monitoring Network (1990-1997)

The aim of the present study was to analyse the data structure of a large data set from rainwater samples collected during a long-term interval (1990-1997) by the Austrian Precipitation Monitoring Network. Eleven sampling sites from the network were chosen as data sources (chemical concentrations of major ions only) covering various location characteristics (height above sea level, rural and urban sampling positions, Alpine rim and Alpine valley disposition, etc.). The analytical results were treated by the application of already classical environmetric approaches, such as linear regression analysis, time-series analysis and principal components analysis (PCA). For most of the sampling sites, a distinct trend of acidity decrease of the wet precipitation was observed. An overall decrease in sulfate concentration for the whole period and all sites of 3.9% year(-1) (2.0 muequiv. L(-1) year(-1)) was found. The free acidity decrease for most of the sites was between 3.5 and 10.9% year(-1). No significant linear trends were found for nitrate. Base cations either decreased (mean percentage decrease for calcium was 5.4% year(-1) and for magnesium 4.4% year(-1)) or did not show any significant change (sodium, potassium). The overall decrease in ammonium concentration was 2.3% year(-1). Further, some typical "rural" (summer minima and winter maxima) and "urban" (winter minima and spring maxima) seasonal behaviour for the majority of the sites in consideration could be defined, indicating the influence of local emission sources. Several latent factors, named "anthropogenic", "crustal" and "mixed salt", were revealed by the multivariate modelling procedure (PCA) possessing a similar structure for most of the sites. The unavoidable exceptions observed were indications of the influence of sporadic local events (construction and agricultural activities, secondary emission sources, etc.), and an effort was made to explain these exceptions.     

Characteristics of surface ozone at an urban site of Xi'an in Northwest China

Surface ozone concentrations in Xi'an, China were monitored from March 23, 2008 to January 12, 2009 using the Model ML/EC9810 ozone analyzer. The daily average O(3) ranged from <1 ppb to 64.2 ppbv with an annual average of 16.0 ppbv. The seasonal average of O(3) in summer (32.5 ppbv) was more than 10 times higher than that in winter (3.0 ppbv). A significant positive correlation was found between ozone concentration and ambient temperature, indicating that the intensity of solar radiation was one of the several major factors controlling surface ozone production. Using the NOAA HYSPLIT 4 trajectory model, the three longest O(3) pollution episodes were found to be associated with the high biogenic volatile organic carbon (BVOC) emissions from the vegetation of Qinling Mountains. No significant weekday and weekend difference in O(3) levels was detected due to the non-significant change in NO(x) emissions. O(3) depletion by NO emission directly emitted from vehicles, low oxygenated VOC concentrations, and low-level solar radiation caused by high aerosol loading all contributed to the low levels of O(3) found in Xi'an compared to other cities and rural areas.     

A field evaluation of a piezo-optical dosimeter for environmental monitoring of nitrogen dioxide

Measurements of 8-hour time-weighted average NO(2) concentrations are reported at 7 different locations in the region of Dunkirk over 5 consecutive days using PiezOptic monitoring badges previously calibrated for the range 0-70 ppb together with data from chemiluminescent analysers in 5 sites (4 fixed and one mobile). The latter facilities also provided data on ozone and NO concentrations and meteorological conditions. Daily averages from the two pairs of badges in different types of sampling cover in each site have been compared with data from the chemiluminescent analysers, and found largely to agree within error margins of +/-30%. Although NO(2) and ozone concentrations were low, rendering detailed discussion impossible, the general features followed expected patterns.     

2008-2016年臭氧监测试点城市的臭氧污染特征

选取臭氧试点城市北京、沈阳、上海和重庆,通过对2008-2016年臭氧监测数据进行分析研究,可以看出4个试点城市中北京的臭氧污染最严重。4个城市的臭氧污染特征均为高浓度臭氧所占比例较大,高值比较高,低浓度臭氧所占比例较小。北京、沈阳和上海的年平均臭氧浓度总体呈上升趋势。北京、上海、重庆、沈阳4个城市9年的超标天数比例分别为15.9%、7.7%、3.9%、6.5%。上海的臭氧浓度在秋季非常高。2012年的臭氧变化趋势比较异常,可能是由于2012年发生的不寻常气候条件导致。4个城市的臭氧浓度变化和气象条件的变化显著相关。     

PM10 Particulates in Relation to Other Atmospheric Pollutants

Concentrations of PM10 particulates have been compared to the concentrations of oxides of nitrogen and sulphur dioxide at the fourteen Automatic Urban Monitoring Network (AUN) sites operating during 1993, 1994 and 1995 using fully ratified data.Factors which are considered include diurnal variations in concentrations of the various substances, ratios between concentrations of PM10 and the other substances and differences between relationships in summer and winter and between weekdays and weekends. In addition temporal patterns of concentrations are considered. Variations between different cities is demonstrated. Differences in the seasonal size distribution are identified. It is shown that there is a good degree of consistency in concentrations of PM10 across urban areas at background locations and that there is evidence for long range transport of PM10.     

A New All Season Passive Sampling System for Monitoring Ozone in Air

A new all season passive sampling system for monitoring O₃ in the atmosphere has been developed in the laboratory and validated in the field. The unique features for this system include a newly designed passive sampler and a rain shelter, which allow the passive sampler to be installed in the field facing downwards. An equation associated with meteorological parameters is used to calculate the passive sampling rates. This system has been extensively tested in the lab (temperature from –18 to 20°C, relative humidity from 13 to 81%, and wind speed from 0.5 to 150 cm/s) and validated in the field in climates of all seasons. The accuracy of the ozone concentrations in the atmosphere obtained with the use of the new passive sampling system was higher than 85% compared to those obtained with continuous ozone analyzers. The new ozone passive sampling system can be used to measure ambient O₃ concentrations ranging from 3 ppb to 1000 ppb based on one-day exposure and 0.1 ppb to 140 ppb for a monthly exposure period. It is also reasonable to conclude that the new passive sampling system can be used for eight-hour exposure study because of the low field blanks and high sampling rates.     

Vertical ozone distributions observed using tethered ozonesondes in a coastal industrial city, Kaohsiung, in southern Taiwan

This work presents the vertical distributions of ozone and meteorological parameters observed with tethered ozonesondes and meteorological radiosondes in the lower atmosphere during an ozone episode on March 25–27, 2003, in Kaohsiung City in southern Taiwan. Kaohsiung is a coastal industrial city with inland mountain ranges to the east. Extremely complicated ozone structures were identified that spanned day and night during the experimental period. During afternoons, the lower atmosphere was divided into two stratified air layers with substantially different ozone concentrations. On the episode day (March 26), average ozone concentration in the near-ground layer was 85 ppb and the aloft layer was 140 ppb. A very high ozone peak of 199 ppb measured aloft likely resulted from an elevated large point source. Several no-ozone air layers, distributed throughout 400–750 m, were observed to transport onshore during the nigh. As well, elevated ozone layers peaking at 60–90 ppb and 90–160 ppb were detected below and above the no-ozone air layers, respectively. These complicated ozone structures were likely formed through titration of plumes from large point sources and the circulations of sea breezes or combined sea-breeze/mountain flows in the study area.     

Vertical ozone characteristics in urban boundary layer in Beijing

Vertical ozone and meteorological parameters were measured by tethered balloon in the boundary layer in the summer of 2009 in Beijing, China. A total of 77 tethersonde soundings were taken during the 27-day campaign. The surface ozone concentrations measured by ozonesondes and TEI 49C showed good agreement, albeit with temporal difference between the two instruments. Two case studies of nocturnal secondary ozone maxima are discussed in detail. The development of the low-level jet played a critical role leading to the observed ozone peak concentrations in nocturnal boundary layer (NBL). The maximum of surface ozone was 161.7 ppbv during the campaign, which could be attributed to abundant precursors storage near surface layer at nighttime. Vertical distribution of ozone was also measured utilizing conventional continuous analyzers on 325-m meteorological observation tower. The results showed the NBL height was between 47 and 280 m, which were consistent with the balloon data. Southerly air flow could bring ozone-rich air to Beijing, and the ozone concentrations exceeded the China’s hourly ozone standard (approximately 100 ppb) above 600 m for more than 12 h.     

A Simulation Study to Assess the Sensitivity of a Forest Health Monitoring Network to Outbreaks of Defoliating Insects

The sensitivity of the United States Forest Health Monitoring network to outbreaks of defoliating insects was examined by means of a simulation study. A model constructed specifically for the study was used to generate a wide variety of defoliation patterns in forested landscapes. Forest configuration was that of Minnesota, USA, as expressed by the GAP land cover classification. Combinations of model parameters were based on a Latin Hypercube sample. The relationship between the average number of plots defoliated and outbreak characteristics was then examined via multiple regression. Both theoretical and model results pointed to a strong, linear relationship between the average number of plots defoliated and outbreak size. Model results provided additional insight, suggesting a significant relationship between the average number of plots defoliated and other outbreak characteristics after outbreak size was taken into account.     

Errors in ozone risk assessment using standard conditions for converting ozone concentrations obtained by passive samplers in mountain regions

Passive samplers are often employed to measure ozone concentrations in remote areas such as mountain forests. The potential ozone risk for vegetation is then assessed by calculating the AOT40 exposure index (accumulated hourly ozone concentration exceedances above 40 ppb, i.e. AOT40 = Σ([O(3)] - 40)Δt for any hourly ozone concentration [O(3)] > 40 ppb). AOT40 is customary calculated on the basis of ozone concentrations expressed as a volumetric mixing ratio, while lab sheets normally report ozone concentrations from passive samplers in mass units per cubic metre. Concentrations are usually converted from mass units to ppb using a standard conversion factor taking SATP (Standard Ambient Temperature and Pressure) conditions into account. These conditions, however, can vary considerably with elevation. As a consequence, the blanket application of a standard conversion factor may lead to substantial errors in reporting and mapping ozone concentrations and therefore in assessing potential ozone risk in mountain regions. In this paper we carry out a sensitivity analysis of the effects of uncertainties in estimations of air temperature (T) and atmospheric pressure (P) on the concentration conversion factor, and present two examples from two monitoring and mapping exercises carried out in the Italian Alps. We derived P and T at each site from adiabatic lapse rates for temperature and pressure and analysed the magnitude of error in concentration estimations. Results show that the concentration conversion is much more sensitive to uncertainties in P gradient estimation than to air temperature errors. The concentration conversion factor (cf) deviates 5% from the standard transformation at an elevation of 500 m asl. As a consequence, the standard estimated AOT40 at this elevation is about 13% less than the actual value. AOT40 was found to be underestimated by an average between 25% and 34% at typical elevations of mountain forest stands in the Italian Alps when a correct conversion factor for transforming ozone concentrations from μg m(-3) to ppb is not applied.     

Insights into ozone deposition patterns from decade-long ozone flux measurements over a mixed temperate forest

Long-term fluxes of ozone (O(3)) were measured over a mixed temperate forest using the aerodynamic gradient method. The long-term average O(3) flux (F) was -366 ng m(-2) s(-1) for the period 2000-2010, corresponding to an average O(3) concentration of 48 μg m(-3) and a deposition velocity v(d) of 9 mm s(-1). Average nocturnal ozone deposition amounted to -190 ng m(-2) s(-1), which was about one third of the daytime flux. Also during the winter period substantial O(3) deposition was measured. In addition, total O(3) fluxes were found to differ significantly among canopy wetness categories. During the day, highest deposition fluxes were generally measured for a dry canopy, whereas a rain-wetted canopy constituted the best sink at night. Flux partitioning calculations revealed that the stomatal flux (F(s)) contributed 20% to the total F but the F(s)/F fraction was subject to seasonal and diurnal changes. The annual concentration-based index AOT40 (accumulated dose over a threshold of 40 ppb) and the Phytotoxic Ozone Dose (POD(1) or accumulated stomatal flux above a threshold of 1 nmol m(-2) s(-1)) were related in a curvilinear way. The O(3) deposition was found to be largely controlled by non-stomatal sinks, whose strength was enhanced by high friction velocities (u(*)), optimizing the mechanical mixing of O(3) into the canopy and the trunk space. The long-term geometrical mean of the non-stomatal resistance (R(ns)) was 136 s m(-1) but lower R(ns) values were encountered during the winter half-year due to higher u(*). The R(ns) was also subject to a marked diurnal variability, with low R(ns) in the morning hours, when turbulence took off. We speculate that non-stomatal deposition was largely driven by scavenging of ozone by biogenic volatile organic compounds (BVOCs) and especially NO emitted from the crown or the forest floor.     

Evaluation of biological stability and corrosion potential in drinking water distribution systems: a case study

The appearance of assimilable organic carbon (AOC), microbial regrowth, disinfection by-products (DBPs), and pipe corrosion in drinking water distribution systems are among those major safe drinking water issues in many countries. The water distribution system of Cheng-Ching Lake Water Treatment Plant (CCLWTP) was selected in this study to evaluate the: (1) fate and transport of AOC, DBPs [e.g., trihalomethanes (THMs), haloacetic acids (HAAs)], and other organic carbon indicators in the selected distribution system, (2) correlations between AOC (or DBPs) and major water quality parameters [e.g. dissolved oxygen (DO), free residual chlorine, and bacteria, and (3) causes and significance of corrosion problems of the water pipes in this system. In this study, seasonal water samples were collected from 13 representative locations in the distribution system for analyses of AOC, DBPs, and other water quality indicators. Results indicate that residual free chlorine concentrations in the distribution system met the drinking water standards (0.2 to 1 mg l(-1)) established by Taiwan Environmental Protection Administration (TEPA). Results show that AOC measurements correlated positively with total organic carbon (TOC) and UV-254 (an organic indicator) values in this system. Moreover, AOC concentrations at some locations were higher than the 50 microg acetate-C l(-1) standard established by Taiwan Water Company. This indicates that the microbial regrowth might be a potential water quality problem in this system. Higher DO measurements (>5.7 mg l(-1)) might cause the aerobic biodegradation of THMs and HAAs in the system, and thus, low THMs (<0.035 mg l(-1)) and HAAs (<0.019 mg l(-1)) concentrations were observed at all sampling locations. Results from the observed negative Langelier Saturation Index (LSI) values, higher Ryznar Stability Index (RSI) values, and high Fe3+ concentrations at some pipe-end locations indicate that highly oxidative and corrosive conditions occurred. This reveals that pipe replacement should be considered at these locations. These findings would be helpful in managing the water distribution system for maintaining a safe drinking water quality.     

Baseline ambient gaseous ammonia concentrations in the Four Corners area and eastern Oklahoma, USA

Ambient ammonia monitoring using Ogawa passive samplers was conducted in the Four Corners area and eastern Oklahoma, USA during 2007. The resulting data will be useful in the multipollutant management of ozone, nitrogen oxides, and visibility (atmospheric regional haze) in the Four Corners area, an area with growing oil/gas production and increasing coal-based power plant construction. The passive monitoring data also add new ambient ammonia concentration information for the U.S. and will be useful to scientists involved in present and future visibility modeling exercises. Three week integrated passive ammonia samples were taken at five sites in the Four Corners area and two sites in eastern Oklahoma from December, 2006 through December, 2007 (January, 2008 for two sites). Results show significantly higher regional background ammonia concentrations in eastern Oklahoma (1.8 parts per billion (ppb) arithmetic mean) compared to the Four Corners area (0.2 ppb arithmetic mean). Annual mean ammonia concentrations for all Four Corners area sites for the 2007 study ranged from 0.2 ppb to 1.5 ppb. Peak ambient ammonia concentrations occurred in the spring and summer in both areas. The passive samplers deployed at the Stilwell, Oklahoma site compared favorably with other passive samplers and a continuous ammonia monitoring instrument.     

Variation of Surface Ozone in the Ambient Air of Auckland, New Zealand

A study has been performed on the characteristics and behavior of surface ozone concentrations at four monitoring sites in Auckland, New Zealand (37 degrees S, 174.8 degrees E) for a four-year period (October 1997-October 2001). One monitoring site (rural) was located upwind of the Auckland urban complex, a second downwind (rural-coastal), and a third within the urban area, while the fourth was an elevated urban-city site located 250 m up the Sky Tower in the central city. In contrast to the high elevation site, the diurnal behaviour of ozone at the three low elevation sites followed a typical solar radiation cycle with high ozone during the day and low nocturnal values. The effect of NO(x) titration was distinct at the urban sites. There was also a seasonal variability in the measured ozone levels with high concentrations in spring and a significant summer minimum. The observed surface ozone concentrations in Auckland were significantly lower than other cities of the world, although a potential for high oxidant formation existed. Observed ozone episodes appear to have been either generated locally or the precursors transported via the prevailing southwest wind. A unique feature of Auckland's air quality is the dilution of polluted city air due to the mixing of east-coast air into the clean west-coast circulation leading to the overall lower average concentrations in summer. A second feature is the potential interaction between sea salt particles and ozone that may provide an additional ozone loss mechanism.     

Near-surface ozone levels and trends at rural stations in France over the 1995–2003 period

There is a considerable interest in quantifying near-surface ozone concentrations and associated trends, as they serve to define the impacts on ozone of the anthropogenic precursors reductions and to evaluate the effects of emission control strategies. A statistical test has been used to the ozone air concentrations measured in the French rural monitoring network stations, called MERA, in order to bring out spatio-temporal trends in air quality in France over the 1995-2003 period. The non-parametric Mann-Kendall test has been developed for detecting and estimating monotonic trends in the time series and applied in our study at annual values: mean, 98th percentile and median based on hourly averaged ozone concentrations and applied to daily maxima. In France, when averaged overall 9 stations between 1995 and 2003, a slight increasing trend of the O(3) levels (+0.6 +/- 1.3% year( - 1)) is observed, which is strongly influenced by the concentrations of the high altitude stations. In stations below 1000 m a mean rate of -0.48% year( - 1) from annual average concentrations, of -0.45% year( - 1) for medians and of +0.56% year( - 1) for P.98 over the 1995-2003 period were obtained. In stations above 1,000 m a mean rate of +1.75% year( - 1) from annual averages values, of +4.05% year( - 1) for medians and of +2.55% year( - 1) for P.98 were calculated over the 1997-2003 period. This situation is comparable to the one observed in other countries. In Europe and in France a reduction of precursor emissions is observed whereas a slight increasing trend of the O(3) levels is observed over the 1995-2003 period. One reason is the non-linearity of chemical ozone production with respect to precursor emissions. Possible explanations are an increase in near-surface ozone values caused by a reduced ozone titration by reduced NO( x ), the meteorological parameters change, an increase in bio-geogenic compound concentrations, the intercontinental transport from North America and Asia and the influence of stratospheric-tropospheric exchanges. These possible explanations must be interpreted carefully as on the short time scales considered.     

Ambient ozone injury to forest plants in Northeast and North Central USA: 16?years of biomonitoring

The US Forest Service administers a long-term, nationwide ozone biomonitoring program in partnership with other state and federal agencies to address national concerns about ozone impacts on forest health. Biomonitoring surveys begun in 1994 in the East and 1998 in the West provide important regional information on ozone air quality and a field-based record of ozone injury unavailable from any other data source. Surveys in the Northeast and North Central subregions cover 450 field sites in 24 states where ozone-sensitive plants are evaluated for ozone-induced foliar injury every year. Sites are typically large, undisturbed openings (>3 acres in size) close to forested areas where >3 bioindicator species are available for evaluation. Over the 16-year sampling period, injury indices have fluctuated annually in response to seasonal ozone concentrations and site moisture conditions. Sites with and without injury occur at all ozone exposures but when ambient concentrations are relatively low, the percentage of uninjured sites is much greater than the percentage of injured sites; and regardless of ozone exposure, when drought conditions prevail, the percentage of uninjured sites is much greater than the percentage of injured sites. Results indicate a declining trend in foliar injury especially after 2002 when peak ozone concentrations declined across the entire region.