Ozone Concentrations in Rural Regions of the Yangtze Delta in China

Elevated concentrations of ozone have been observed at six non-urban, surface monitoring sites in the Yangtze Delta of China during a 16-month field experiment carried out in 1999 and 2000 as part of the joint Chinese-American China-MAP Project (the Yangtze Delta of china as an Evolving Metro-Agro-Plex). The average daytime (0900–1600 h) ozone levels for the monitoring period at sites ranged from 35 to 47 ppbv (parts per billion by volume) and the mean ozone levels from 26 to 35 ppbv. Observed data show seasonal variation obviously, with highest mixing ratios of ozone in May. Average daytime ozone levels in May at sites were between 60 and 79 ppbv. High ozone concentrations were most prevalent during the late spring. Frequency counts of hourly mean ozone concentration over 60 ppbv and 40 ppbv appeared peak values of 22–39% and 42–74% in May at sites. Even higher daytime ozone levels were observed during two regional episodes, in which average daytime (0900–1600 h) ozone concentrations during 10 May and 23 May 2000 were 68 to 81 ppbv, during Oct. 18 and Oct. 28, 1999 were 59 to 67 ppbv at sites. Peak value of ozone mixing ratio appearing in late spring, instead of in summer, was attributed to summer monsoon. Backward trajectories showed that ozone episodes associated with meteorological conditions. Also many high ozone levels associated with high CO levels and high CO to NO _x ratios, which suggests a contribution from sources of emission involving incomplete combustion.     

Spectral analysis of the “Koshava” wind

Summary “Koshava” is a gusty wind of changeable intensity, blowing from a south-easterly direction, over Serbia, Romania and Bulgaria. It is caused by the interaction between the synoptic circulation and the orography of the Carpathian and the Balkan mountains. This paper analyzes wind data measured at the Belgrade-Observatory during the longest period of consecutive days of “Koshava” which occurred from 14 January to 13 February 1972. Mean hourly wind speed data has been examined using spectral analysis. The power spectra are calculated using autocorrelation spectral analysis, the multi-taper method and wavelet transform. The maximum of which is about 122 h (5 days) corresponds to the time span of synoptic processes.     

Measurements of surface ozone at semi-arid site Anantapur (14.62°N, 77.65°E, 331 m asl) in India

In the present study, an attempt has been made to examine the governing photochemical processes of surface ozone (O₃) formation in rural site. For this purpose, measurements of surface ozone and selected meteorological parameters have been made at Anantapur (14.62°N, 77.65°E, 331 m asl), a semi-arid zone in India from January 2002 to December 2003. The annual average diurnal variation of O₃ shows maximum concentration 46 ppbv at noon and minimum 25 ppbv in the morning with 1σ standard deviation. The average seasonal variation of ozone mixing ratios are observed to be maximum (about 60 ppbv) during summer and minimum (about 22 ppbv) in the monsoon period. The monthly daytime and nighttime average surface ozone concentration shows a maximum (55 ± 7 ppbv; 37 ± 7.3 ppbv) in March and minimum (28 ± 3.4 ppbv; 22 ± 2.3 ppbv) in August during the study period. The monthly average high (low) O₃ 48.9 ± 7.7 ppbv (26.2 ± 3.5 ppbv) observed at noon in March (August) is due to the possible increase in precursor gas concentration by anthropogenic activity and the influence of meteorological parameters. The rate of increase of surface ozone is high (1.52 ppbv/h) in March and lower (0.40 ppbv/h) in July. The average rate of increase of O₃ from midnight to midday is 1 ppbv/h. Surface temperature is highest (43–44°C) during March and April months leading to higher photochemical production. On the other hand, relative humidity, which is higher during the rainy season, shows negative correlation with temperature and ozone mixing ratio. It can be seen that among the two parameters are measured, correlation of surface ozone with wind speed is better (R ²=0.84) in compare with relative humidity (R ²=0.66).     

A vertical profile of Ozone concentration in the atmosphericboundary layer over central Taiwan

Summary  In the central region of Taiwan, ozone episodes occur most often during autumn. Two field experiments were conducted during the autumns of 1998 and 1999 to analyze the vertical profile of the boundary layer and determine its effects on ozone concentration over the region. The vertical virtual potential temperature and wind profiles were derived from tethersonde data. The NO_x, NMHC and O₃ concentration vertical profiles were monitored up to a height of 500 meters using black-covered Teflon tedler sampling bags. During the experimental periods, nighttime terrestrial long wave radiation could cause the inversion height to reach 500 meters by the following morning. It was shown that these types of synoptic structures suppress the vertical diffusion of NO_x, NMHC and O₃. During the daytime, measurements indicate that pollutants were well mixed in the upper portion of the mixing layer. At night, the ground level ozone concentration was on the decrease but increased with altitude to a height of 500 m. The NO_x decreased with altitude whereas the NMHC showed no significant variations. Received April 13, 2000 Revised July 24, 2000     

Objective synoptic classification combined with high resolution meteorological models for wind mesoscale studies

Summary A methodology developed for automatic classification of Objective Synoptic Processes (OSP) and its application to the study of the mesoscale atmospheric circulatory patterns associated with them is described. The classification was based on the analysis of the evolution of surface pressure and geopotencial height at 500 hPa during three days. An iterative procedure results in an objective grouping of the main configurations describing different large-scale situations. This routine has been applied over an appropriate domain covering the Iberian Peninsula to obtain OSPs in the region for the two month period July–August, using daily synoptic maps for years 1990 to 1999 (a total of 7304 surface and 500 hPa synoptic maps have been used in the analysis). Finally, for a characteristic day for two of the OSPs obtained, a mesoscale meteorological model (TAPM) has been run at high resolution for the region of Catalonia, Northeastern Spain, in order to describe the local atmospheric circulatory patterns associated with a given large-scale situation. Results show that the complex orography modifies the large-scale forcings resulting in wind fields with a very important horizontal variability, significant daily cycle, and specific local features related to orographic elements, which the model was able to incorporate due to the highly-resolved orography used.     

Surface Trace Gases at a Rural Site between the Megacities of Beijing and Tianjin

The North China Plain （NCP） has recently faced serious air quality problems as a result of enhanced gas pollutant emissions due to the process of urbanization and rapid economic growth. To explore regional air pollu- tion in the NCP, measurements of surface ozone （O3）, nitrogen oxides （NOx）, and sulfur dioxide （SO2） were car- ried out from May to November 2013 at a rural site （Xianghe） between the twin megacities of Beijing and Tianjin. The highest hourly ozone average was close to 240 ppbv in May, followed by around 160 ppbv in June and July. High ozone episodes were more notable than in 2005 and were mainly associated with air parcels from the city cluster in the hinterland of the polluted NCP to the southwest of the site. For NOx, an important ozone precur- sor, the concentrations ranged from several ppbv to nearly 180 ppbv in the summer and over 400 ppbv in the fall. The occurrence of high NOx concentrations under calm condi- tions indicated that local emissions were dominant in Xianghe. The double-peak diurnal pattern found in NOx concentrations and NO/NOx ratios was probably shaped by local emissions, photochemical removal, and dilution re- sulting from diurnal variations of surface wind speed and the boundary layer height. A pronounced SO2 daytime peak was noted and attributed to downward mixing from an SO2-rich layer above, while the SO2-polluted air mass transported from possible emission sources, which differed between the non-heating （September and October） and heating （November） periods, was thought to be responsible for night-time high concentrations.     

Relationships between Synoptic Climatology and Atmospheric Pollution at 4 US Cities

Summary  An evaluation of the impacts of weather on pollution, specifically, ozone and total suspended particulates concentration for Summer, is examined in four cities in the U.S.: Birmingham, Cleveland, Philadelphia, and Seattle. These cities were selected because of their different climate regimes and their generally good pollutant and meteorological datasets. This paper uses a synoptic climatological approach, which combines a number of atmospheric factors, to better identify the relationships between atmospheric pollution and climatological conditions. Synoptic events represent holistic units of atmospheric conditions which commonly occur at a given locale, and possess specific weather and pollution characteristics. A number of weather variables, including temperature, are used in the development of a synoptic index, which can be used to identify synoptic events associated with specific pollution episodes. Results from the analysis illustrate that there is a substantial difference in pollution loads under different synoptic patterns, and that the cities do have substantially different relationships. Information from this study could be used to assist in the analysis of the differential impacts of weather and pollution upon human morbidity. Specific information as to the linkages between the synoptic weather patterns, pollution concentrations, and human health could be used in the development of weather/health watch-warning systems to alert the public that a synoptic episode is imminent. Received September 18, 1998     

Volatile organic compounds at a rural site in western Senegal

The objectives of this study were to identify species and levels of volatile organic compounds (VOCs), and determine their oxidation capacity in the rural atmosphere of western Senegal. A field study was conducted to obtain air samples during September 14 and September 15, 2006 for analyses of VOCs. Methanol, acetone, and acetaldehyde were the most abundant detected chemical species and their maximum mixing ratios reached 6 parts per billion on a volume basis (ppbv). Local emission sources such as firewood and charcoal burning strongly influenced VOC concentrations. The VOC concentrations exhibited little temporal variations due to the low reactivity with hydroxyl radicals, with reactivity values ranging from 0.001 to 2.6 s⁻¹. The conditions in this rural site were rather clean. Low ambient NO _x levels limited ozone production. Nitrogen oxide (NO _x ) levels reached values less than 2 ppbv and maximum VOC/NO _x ratios reached 60 ppbvC/ppbv, with an overall average of 2.4 ± 4.5 ppbvC/ppbv. This indicates that the rural western Senegal region is NO _x limited in terms of oxidant formation potential. Therefore, during the study period photochemical ozone production became limited due to low ambient NO _x levels. The estimated ozone formation reactivity for VOCs was low and ranged between −5.5 mol of ozone/mol of benzaldehyde to 0.6 mol/mol of anthropogenic dienes.     

A meteorological analysis of ozone episodes using HYSPLIT model and surface data

Ozone episodes (> 100 ppbv) were observed frequently in Jinan, an urban site located between the highly polluted Yangtze Delta and Beijing–Tianjin region in East China. In this study, the ozone episodes observed in 2004 were analysed using the Hybrid Single-particle Lagrangian Integrated Trajectory (HYSPLIT) model and surface meteorological data, as well as Air Pollution Index (API). The meteorological conditions of episode days and non-episode days were compared and examined, and categorization of 6 groups of backward trajectories was performed. The results show that, most episodes were caused by local photochemical production (e.g., induced by sufficient sunshine duration and high temperature) and pollutant accumulation (e.g., induced by little rainfall and low wind speed), and transport of pollutants from the highly polluted regions could significantly influence the air quality at the site, especially from Yangtze Delta region. In addition, three typical ozone episodes were analysed using HYSPLIT model to infer any long-distance transport and surface meteorological data to infer the local ozone production potential. At last, the functions and inadequacies about the usage of HYSPLIT model combined with surface meteorological data for the analysis of photochemical pollution were discussed.     

Study of ozone distribution over the south-eastern France (ESCOMPTE campaign): discrimination between ozone tendencies due to chemistry and to transport

Ozone tendencies due to chemistry and transport are calculated by a mesoscale model using a fine horizontal resolution (3 km × 3 km), over South-Eastern France. Over that region where the anthropogenic emissions are very strong, ozone pollution is highlighted during two intensive observations periods of the ESCOMPTE campaign, when the sea breeze penetrates far into the Durance and Rhone valleys and the up-slope breezes are developed. From a fine analysis of time series of ozone concentration at different ground stations along these valleys and from numerical results, it is possible to discriminate the tendency due to chemistry from the tendency due to dynamical processes. We can distinguish both processes, either local chemical production/loss or dynamical increase/decrease (transport, deposition) on maps of ozone budget according to the meteorological conditions. In particular, we show that the variations due to transport can be have the same order of magnitude than those due to chemistry, reaching 20 ppbv h⁻¹, whereas those due to chemistry are around 30 ppbv h⁻¹.     

河源市空气质量首要污染物特征及其与气象条件的关系

基于2017-2019年河源市空气质量数据,分析了河源市首要污染物的年际变化特征,同时利用2019年东埔国控站点的首要污染物与气象要素进行了相关性分析,并以典型污染日为案例,分析了气象条件对污染过程的影响。结果表明：2017-2019年细颗粒物（PM_2.5）污染日比重大幅度降低,以臭氧（O₃）为首要污染物的污染日逐年增加,污染形式逐渐从颗粒物污染向臭氧污染发生转变。O₃浓度与温度和湿度分别呈正负相关关系,高浓度O₃主要出现在（20-30℃,25%-55%）阈值之间,在吹西北偏北风时O₃浓度也较高。PM_2.5和PM₁₀与湿度也呈负相关关系,温度与湿度组合在（8-13℃,40%-55%）范围内时两者容易同时出现高值;在夏季PM_2.5和PM₁₀还与温度具有较强的正相关关系,这意味着高温情况下河源有出现颗粒物与O₃复合污染的可能。河源市典型污染日具有风速较小局部扩散不利的特征,低温低湿条件下容易出现PM_2.5污染,且主要受到区域的传输影响;而高温低湿条件下容易发生O₃污染,且较高的前体物浓度容易加剧O₃的本地污染。     

A 10-year study of background surface ozone concentrations on the island of Gozo in the Central Mediterranean

A 10-year study of surface ozone mixing ratios in the Central Mediterranean was conducted based on continuous ozone measurements from 1997 to 2006 by a background regional Global Atmospheric Watch (GAW) station on the island of Gozo. The mean annual maximum mixing ratio is of the order of 66 ppbv in April–May with a broad secondary maximum of 64 ppbv in July–September. No long-term increase or decrease in the background level of surface ozone could be observed over the last 10 years. This is contrary to observations made in the Eastern Mediterranean, where a slow decrease in the background ozone mixing ratio was observed over the past 7 years. Despite the very high average annual ozone mixing ratio exceeding 50 ppbv—in fact, the highest average background ozone mixing ratio ever measured in Europe—, the diurnal O _{3 max}/O _{3 min} index of <1.40 indicates that the island of Gozo is a good site for measuring background surface ozone. However, frequent photosmog events from June to September during the past 10 years with ozone mixing ratios exceeding 90 ppbv indicate that the Central Mediterranean is prone to long-range transport of air pollutants from Europe by northerly winds. This was particularly evident during the so-called “August heatwave” of the year 2003 when the overall ozone mixing ratio was 4.6 ppbv higher than the average of all other 9 months of August since 1997. Air mass back-trajectory analysis of the August 2003 photosmog episodes on Gozo confirmed that ozone pollution originated from the European continent. Regression analysis was used to analyse the 10-year data set in order to model the behaviour of the ozone mixing ratio in terms of the meteorological parameters of wind speed, relative humidity, global radiation, temperature, month of year, wind sector, atmospheric pressure, and time of day (predictors). Most of these predictors were found to significantly affect the ozone mixing ratios. From March to November, the monthly average of the AOT40 threshold value for the protection of crops and vegetation against ozone was constantly exceeded on Gozo during the past 10 years.     

On the vertical structure of composite surface cyclones in the Mediterranean region

Summary The average pressure distribution at mean sea level and the vertical structure of synoptic scale surface cyclones (with central pressure less than 1000 hPa) that occur in the Mediterranean region is studied for a 40 year period (1958–1997) on a seasonal and daily basis. The cyclonic occurrences are studied in three regions of enhanced cyclonic activity: gulf of Genoa, Southern Italy and Cyprus. The cyclones are identified with the aid of an objective method based on grid point values, available every 6 hours. The analysis revealed different characteristics of the cyclones that occur in the three regions, reflecting the different mechanisms that are responsible for their occurrence in each region. For the Genoa region the cyclone pressure minimum is located over the gulf, associated with orographic forcing, while surface dynamics occur further south. Over Southern Italy, the pressure minimum covers a wide area, whilst the surface dynamics are found to act in the same region, becoming more important in winter and spring. The pressure minimum of cyclones over Cyprus is located over the land during winter and spring and is influenced by surface dynamics and orography. Received November 7, 2000 Revised July 14, 2001     

Surface ozone concentration variability in Moscow and Kiev

The comparison is represented of the results of surface ozone concentration measurements in two megalopolises, Moscow and Kiev. A temporal course of ozone concentration and temperature in both cities is close by the shape and is typical of medium-polluted plain stations. In both megalopolises, two maxima are observed within the seasonal ozone concentration variability, in spring and summer, and during the day, a usual ozone concentration maximum (approximately in 2–3 hours after the local noon) and the night one being typical of big cities. An average ozone concentration and an average temperature in corresponding periods are higher in Kiev than in Moscow. Evidently, the summer maximum is associated with photochemical ozone generation processes, and the spring one, with dynamic processes of its transport in the atmosphere. In both megalopolises, the episodes are observed in the warm period under meteorological conditions being unfavorable for the pollutant scattering in the atmosphere when the ozone concentration exceeds the threshold limit value and is dangerous for health. The repeatability of such episodes is the highest one in July-August. In Kiev, such episodes are more frequent than in Moscow. An effective statistical model is constructed for both megalopolises in which the observed ozone concentration is represented in the form of regression function of temperature and relative humidity.     

Modeling of Regional High Ozone Episode Observed at Two Mountain Sites (Mt. Tai and Huang) in East China

A high O₃ episode was observed during 23–25 May 2004 at two high-mountain sites reflecting the regional pattern of air pollutants over East China. This episode lasted about three days with the maximum hourly O₃ mixing ratios reaching 111 and 114 ppbv at Mt. Tai and Huang, respectively. Backward trajectories and meteorological analysis indicated that regional transport, associated with a weak high pressure system over the East China Sea, might play an important role in the formation of this high ozone episode. The nested air quality prediction modeling system (NAQPMS) was applied to investigate the formation and evolution of this high O₃ event. The comparison of model results with observations showed that NAQPMS successfully reproduced the main observed patterns of O₃ and meteorological parameters during the simulated period. The model results with emission over the Yangtze Delta and the East Central China switched on/off clearly showed that ozone and its precursors transported from the Yangtze Delta and the East Central China enhanced the high ozone episode at two sites, with a contribution of 20%–50% during the episode. In addition, based on process analysis with the model, chemical production and regional transport appeared to be the main causes of high ozone episode involving a large amount of high-ozone air masses and precursors transported from the surrounding areas. The horizontal transport is more active during the period of high ozone episode than that during the non-episode at Mt. Tai as well as Mt. Huang.     

A 500 hPa synoptic wildland fire climatology for large Canadian forest fires, 1959–1996

Summary In Canada, the average annual area of burned forest has increased from around 1 million ha in the 1970’s to over 2.5 million ha in the 1990’s. A previous study has identified the link between anomalous mid-tropospheric circulation at 500 hPa over northern North America and wildland fire severity activity in various large regions of Canada over the entire May to August fire season. In this study, a northern North American study region of the hemispheric gridded 5° latitude by 10° longitude 500 hPa dataset is identified and analysed from 1959 to 1996 for a sequence of six monthly periods through the fire season, beginning in April and ending in September. Synoptic types, or modes of upper air behavior, are determined objectively by the eigenvector method employing K-means cluster analysis. Monthly burned areas from the Canadian Large Fire Database (LFDB) for the same period, 1959 to 1996, are analysed in conjunction with the classified monthly 500 hPa synoptic types. Relationships between common monthly patterns of anomalous upper flow and spatial patterns of large fire occurrence are examined at the ecozone level. Average occurrence of a monthly synoptic type associated with very large area burned is approximately 18% of the years from 1959 to 1996. The largest areas burned during the main fire (May to August) season occur in the western Boreal and Taiga ecozones – the Taiga Plains, Taiga Shield, Boreal West Shield and Boreal Plains. Monthly burned areas are also analysed temporally in conjunction with a calculated monthly zonal index (Zi_m) for two separate areas defined to cover western and eastern Canada. In both western and eastern Canada, high area burned is associated with synoptic types with mid-tropospheric ridging in the proximity of the affected region and low Zi_m with weak westerlies and strong meridional flow over western Canada. Received April 3, 2001 Revised July 13, 2001     

Ice Storm ’98 in Southcentral Canada and Northeastern United States: A Climatological Perspective

Summary Dubbed Ice Storm ’98, an extreme weather event characterized by two synoptic systems in succession dropped about 70–100 mm (in terms of water equivalent) of freezing precipitation over southeastern Ontario, southwestern Quebec and northeastern New York during a 6-day period from January 5 to 10 in 1998. Individually, the two synoptic systems were not dramatically more extreme in freezing precipitation than other major freezing rain events (4 since 1961) which occurred in the past over the affected area. Some regions in the target area, however, were impacted more by the second system. Based on an analysis of the 500 hPa vorticity field during the ’98 event, we suggest that the 1997/98 El Ni?o had a role in creating a flow environment conducive to the rapid formation of the second synoptic system. In contrast, other major freezing rain events in the last 30 years involved only one synoptic system per event lasting no more than 3 days, and producing 20–50 mm of precipitation. We have also found that, 3 out of 4 past major freezing rain events since 1958 were associated with the positive phase of the North Atlantic Oscillation (NAO). Consistent with this usual past association between the NAO and a major freezing rain event, Ice Storm ’98 also occurred when the phase of the NAO was positive. Analysis of these 3 past and the ’98 events also indicates an apparent connection between the positive phase of the NAO and the northern Quebec high pressure system, which is an essential synoptic feature of a major freezing rain occurrence over the southcentral region of Canada. As measured by their respective indices, the maximum positive NAO state leads the maximum northern Quebec high by about 2 days (5 days in the ’98 event). There is some suggestive evidence to indicate that the persistence of the northern Quebec high pressure system is connected to the persistence of the positive phase of the NAO. Received January 17, 2000     

Observational study of surface ozone at an urban site in East China

In this study, we present the observational data of near surface ozone and some meteorological parameters during 2004, at an urban site (36°42′ N, 117°08′ E, 34.5 m a.s.l.) of Jinan, China. Hourly ozone concentrations exceeding the standard value of China, 100 ppbv, were observed for 65 h (in 23 days) from April to October, and values exceeding US NAAQS (National Ambient Air Quality Standard) for 1 h ozone, 120 ppbv, were observed for 15 h (in 7 days) from late May to early July. Ozone formation presented the phenomenon of “weekend effect”, especially in summer. Monthly variation of ozone coincided with temperature except for July and August. The low ozone levels in July and August may be due to the short sunshine duration and much rainfall during this period. Among these meteorological parameters, daily averaged ozone shows a significant correlation with temperature (r = 0.66) in the year and with relative humidity (r = − 0.75) in summer. Throughout the year, high ozone concentrations were mainly associated with the wind from 180 to 247.5°, while high ozone concentration seemed to have no obvious correlation with a given wind direction in summer. An anomalous nocturnal high ozone episode during 23–25 May 2004 was investigated. Growth fractions of ozone during the nighttime episode were 62.2% and 71.1% for 23 and 24 May, respectively. Synoptic analysis shows that favorable synoptic condition had presumably elevated the background ozone level in this region. Backward trajectory analysis shows that the increase of ozone concentration and the relatively constant high ozone concentrations during the night of May 23 might originate from the transport of ozone rich air mass above boundary layer. Transport of ozone from Yangtze Delta and East Central China might be a significant process for the high ozone level during night May 24 at Jinan.     

A Comparison of Match Ozonesonde-Derived and 3D Model Ozone Loss Rates in the Arctic Polar Vortex during the Winters of 1994/95 and 1995/96

Ozone loss rates from ozonesonde data reported in the Match experiments of winters 1994/95 and 1995/96 inside the Arctic polar vortex are compared with simulations of the same winters performed using the SLIMCAT 3D chemistry and transport model. For 1994/95 SLIMCAT reproduces the location and timing of the diagnosed ozone destruction, reaching 10 ppbv/sunlit hour in late January as observed. SLIMCAT underestimates the loss rates observed in February and March by 1–3 ppbv/sunlit hour. By the end of March, SLIMCAT ozone exceeds the observations by 25–35%. In January 1995 the ozonesonde-derived loss rates at levels above 525 K are not chemical in origin but due to poor conservation of air parcels. Correcting temperature biases in the model forcing data significantly improved the agreement between the model and observed ozone at the end of winter 1994/95, increasing ozone destruction in SLIMCAT in February and March. The SLIMCAT simulation of winter 1995/96 does not reproduce the maximum ozone loss rates diagnosed by Match of 13 ppbv/sunlit hour. Comparing the data for the two winters reveals that the SLIMCAT photochemistry is least able to reproduce observed losses at low temperatures or when low temperatures coincide with high solar zenith angles (SZA). When cold (T = 192 K), high SZA (90°)matches are excluded from the 1995/96 analysis, agreement between the diagnoses and SLIMCAT is better with ozone loss rates of up to 6 ppbv/sunlit hour. For the rest of the winter SLIMCAT consistently underestimates the Match rates of ozone loss by 1–3 ppbv/sunlit hour. In March 1996 the monthly mean SLIMCAT ozone is 50% greater than observations at 430–540 K. In both winters, ozone destruction rates peaked more rapidly and declined more slowly in the Match observations than in the SLIMCAT simulations. The differences between the observed and modelled cumulative ozone losses demonstrate that the total ozone destruction by the end of the winter is sensitive to errors in the instantaneous ozone loss rates of 1–3 ppbv/sunlit hour.     

Vertical ozone distribution characteristics deduced from ∼ 44,000 re-evaluated Umkehr profiles (1957–2000)

Summary Umkehr observations taken during the 1957–2000 period at 15 stations located between 19 and 52° N have been reanalyzed using a significantly improved algorithm-99, developed by DeLuisi and Petropavlovskikh et al. (2000a,b). The alg-99 utilizes new latitudinal and seasonally dependent first guess ozone and temperature profiles, new vector radiative transfer code, complete aerosol corrections, gravimetric corrections, and others. Before reprocessing, all total ozone values as well as the N-values (radiance) readings were thoroughly re-evaluated. For the first time, shifts in the N-values were detected and provisionally corrected. The re-evaluated Umkehr data set was validated against satellite and ground based measurements. The retrievals with alg-99 show much closer agreement with the lidar and SAGE than with the alg-92. Although the latitudinal coverage is limited, this Umkehr data set contains ∼ 44,000 profiles and represent the longest (∼ 40 years) coherent information on the ozone behavior in the stratosphere of the Northern Hemisphere. The 14-months periods following the El-Chichon and the Mt. Pinatubo eruptions were excluded from the analysis. Then the basic climatological characteristics of the vertical ozone distribution in the 44–52° N and more southern locations are described. Some of these characteristics are not well known or impossible to be determined from satellites or single stations. The absolute and relative variability reach their maximum during winter–spring at altitudes below 24 km; the lower stratospheric layers in the middle latitudes contain ∼ 62% of the total ozone and contribute ∼ 57% to its total variability. The layer-5 (between ∼ 24 and 29 km) although containing 20% of the total ozone shows the least fluctuations, no trend and contributes only ∼ 11% to the total ozone variability. Meridional cross-sections from 19 to 52° N of the vertical ozone distribution and its variability illustrate the changes, and show poleward-decreasing altitude of the ozone maximum. The deduced trends above 33 km confirm a strong ozone decline since the mid-1970s of over 5% per decade without significant seasonal differences. In the mid-latitude stations, the decline in the 15–24 km layer is nearly twice as strong in the winter-spring season but much smaller in the summer and fall. The effect of including 1998 and 1999 years with relatively high total ozone data reduces the overall-declining trend. The trends estimated from alg-99 retrievals are statistically not significantly different from those in WMO 1998a; however, they are stronger by about 1% per decade in the lower stratosphere and thus closer to the estimates by sondes. Comparisons of the integrated ozone loss from the Umkehr measurements with the total ozone changes for the same periods at stations with good records show complete concurrence. The altitude and latitude appearances of the long-term geophysical signals like solar (1–2%) and QBO (2–7%) are investigated. Received April 12, 2001 Revised September 19, 2001