On the mean daily and seasonal variations of the vertical ozone profiles in the lower troposphere

During the 15 year period that the Zugspitze cable car has operated between the valley (1 km a.s.l.) and Zugspitze peak (3 km a.s.l.) at the northern border of the Bavarian Alps, it has been used for investigating the profiles of meteorological and atmospheric electrical parameters, and Aitken nuclei. This cable railway is rather steep and is suspended mostly far away from the ground. From 1980 to 1982 nearly 2000 ozone profiles were additionalyrecorded. The data collected offer a profound basis in order to study the time variations of the lower tropospheric ozone profile depending on the hour of the day during all the seasons. In this paper the following are reported: the shape and time behaviour of ozone profiles in different seasons depending on the vertical mixing intensity, stratospheric intrusions and the penetration depth of the stratospheric O₃.     

Trends in ground level ozone concentrations in the European Union

Following the Council Directive 92/72/EEC on air pollution by ozone the Member States of the European Union have to inform the European Commission on ozone concentrations and exceedances of threshold values within their territory. Using the available information covering the period of 5 years (1994–1998), the data has been analysed for a possible trend in statistical parameters (50- and 98-percentiles) and number and severity of exceedances. Time series are relatively short but the data suggest that there might be a small increasing trend in the 50 percentile values. The ozone peak values, expressed as 98-percentile values or as number of exceedance days tend to decrease. However, these conclusions must be interpreted carefully as on the short time scales considered here meteorological variations and inter-annual changes may play an important role. The decrease in peak values is most likely caused by the decrease in European ozone precursor emissions since 1990; insufficient data is available to explain the increasing 50-percentile values. Possible explanations are an increase in tropospheric ozone background values caused by a world-wide increase in CH₄, CO and NO_x emissions or a reduced ozone titration by reduced NO_x emissions on the local scale. The data submitted under the ozone directive is insufficient to provide firm conclusions on this point.     

合肥科学岛低对流层二氧化碳时空分布特征

依据合肥市科学岛2013~2016年的CO₂体积比浓度廓线,分别从夜间、季节和年度分析了亚热带季风气候的CO₂分布特点和合肥科学岛的CO₂源汇特征.（1）大气CO₂体积比浓度随高度增加而减小,390m的CO₂浓度约为15m浓度的95%,夜间随时间推移浓度增加幅度约5%,天亮时CO₂浓度有减小的趋势;（2）测量点高度大于100m时,季节特征较明显,CO₂体积比浓度夏季最低,冬季最高,浓度相差约10×10^-6;（3）测量点高度大于100m时,2013~2016年CO₂体积比浓度的年分布随高度变化的梯度相关系数大于0.9,体积比浓度年增长约2.1648×10^-6.通过三个时间尺度的CO₂体积比浓度廓线分析得出,CO₂浓度特征是动植物活动和大气运动等共同作用的结果;CO₂长期循环过程中,存在近地面CO₂向高空的传输效应.     

Studying high ozone concentrations by using the Danish Eulerian model

The long-range transport of air pollutants (LRTAP) over Europe is studied by a mathematical model based on a system of partial differential equations (PDEs). The number of PDEs is equal to the number of species studied and the model contains 35 species at present. Among the species are NO, NO₂, NO₃⁻, HNO₃, NH₃, NH₄⁺, O₃, PAN, SO₂, SO₄²⁻ and may hydrocarbons. Most of the 70 chemical reactions involved in the model are nonlinear (including here many photochemical reactions).The model requires large sets of input data. Emissions of SO₂, NO_x, NH₃ and both natural and anthropogenic volatile organic compounds (VOC) are needed in the model. The meteorological data consist of fields of wind velocities, precipitation, surface temperatures, temperatures of the boundary layer, relative humidities and cloud cover, which are read in the beginning of every 6-h interval. Both daytime and nighttime mixing heights are used in the model.Many of the species in the model vary on a diurnal basis. An investigation of the main mechanisms that determine the diurnal variation of the ozone concentrations is performed. One of the important conditions that is necessary if one wants to represent correctly the diurnal variations of the concentrations is to have access to meteorological data that vary diurnally. This is especially true for the temperature and the mixing height.The use of modern numerical algorithms (which are combined with vectorization of the most time-consuming numerical procedures) allows one to perform long-term runs with the model on several high-speed computers. Results obtained in runs with meteorological data for July 1985 and August–October 1989 are discussed. The computed concentrations and depositions are compared with measurements taken at stations located in different European countries. The agreement between calculated concentrations and measurements is reasonably good.Results obtained with several scenarios, in which the NO_x emission and/or the anthropogenic VOC emissions are varied, are presented. Several main conclusions are drawn by studying the results obtained during the comparisons. Some plans for future development of the models are discussed.     

2016年中国城市臭氧浓度的时空变化规律

随着城市化进程的加快和机动车保有量的急剧增加,导致我国很多地区臭氧（O₃）前体物（挥发性有机物和氮氧化物）排放量显著增加,臭氧污染现象日益突出.臭氧污染对人体健康、植被生长、生态环境等具有重要影响,已成为学术界研究的热点.为揭示全国尺度近地面臭氧的时空变化规律,本文基于2016年中国364个城市的监测数据分析了中国城市O₃浓度的时空变化特征,并采用Global Moran''s I和Getis-Ord G_i^*指数,揭示了2016年中国城市O₃污染的空间集聚和冷热点区域的时空特征.结果表明,在全国尺度上,2016年中国城市年均O₃浓度为100.2 μg·m^-3,北方城市和南方城市O₃浓度分别具有显著的倒"V"和"M"型月变化规律,且呈现夏季高、春秋季居中、冬季最低的特征;中国城市O₃浓度具有显著的空间分异规律,中部和东部是O₃污染的高发区,西部地区和黑龙江省的O₃污染处于较低水平;中国城市O₃浓度具有显著的集聚性特征,且呈现1-5月由南向北而6-12月由北向南扩展的年周期循环特征,热点地区主要集中在华北、华中和华东地区.     

全球大气降水年均氚浓度恢复模型(1960-2014年)

运用环境同位素氚（³H）建立模型来定量研究地下水运动规律已被广泛应用于水文地质和环境监测领域,大气降水氚浓度是这类模型中必须的输入值.目前已建立的全球大气降水氚浓度模型（MGMTP）为这一领域的研究提供了一种恢复全球范围内年平均氚浓度的新方法,但该氚浓度模型后期恢复数据出现异常负值及面临适用年限等问题.因此,本文选用国际原子能机构和世界气象组织提供的1960—2014年全球氚浓度值实测资料,基于因子分析法拓展了MGMTP模型的适用年份,并对不同的数据预处理及分析方法进行了对比,同时对MGMTP模型提及的"异常负值"问题进行了进一步明确与改进.最后把模型应用于南北半球的典型站点,将恢复得到的数据与实测数据进行对比,发现拓展后的MGMTP模型结果能较好地拟合实测数据.研究表明,该模型具有简单易用、时间序列长、全球性适用等优点,尤其对缺少大气降水氚浓度实测数据的地区具有重要参考价值.     

Sensitivity of future ozone concentrations in the northeast USA to regional climate change

An air quality modeling system was used to simulate the effects on ozone concentration in the northeast USA from climate changes projected through the end of the twenty-first century by the National Center for Atmospheric Research’s (NCAR’s) parallel climate model, a fully coupled general circulation model, under a higher and a lower scenario of future global changes in concentrations of radiatively active constituents. The air quality calculations were done with both a global chemistry-transport model and a regional air quality model focused on the northeast USA. The air quality simulations assumed no changes in regional anthropogenic emissions of the chemical species primarily involved in the chemical reactions of ozone creation and destruction, but only accounted for changes in the climate. Together, these idealized global and regional model simulations provide insights into the contribution of possible future climate changes on ozone. Over the coming century, summer climate is projected to be warmer and less cloudy for the northeast USA. These changes are considerably larger under the higher scenario as compared with the lower. Higher temperatures also increase biogenic emissions. Both mean daily and 8-h maximum ozone increase from the combination of three factors that tend to favor higher concentrations: (1) higher temperatures change the rates of reactions and photolysis rates important to the ozone chemistry; (2) lower cloudiness (higher solar radiation) increases the photolysis reaction rates; and (3) higher biogenic emissions increase the concentration of reactive species. Regional model simulations with two cumulus parameterizations produce ozone concentration changes that differ by approximately 10%, indicating that there is considerable uncertainty in the magnitude of changes due to uncertainties in how physical processes should be parameterized in the models. However, the overall effect of the climate changes simulated by these models – in the absence of reductions in regional anthropogenic emissions – would be to increase ozone concentrations.     

Calculation of long term averaged ground level ozone concentrations

Seasonal averaged ground level concentrations for O₃ have been calculated for The Netherlands by means of a two-layer Lagrangian long-range transport (LRT) model. The model includes emissions, nonlinear atmospheric chemistry, dry deposition, exchange between boundary layer (BL) and free troposphere (FT) and fumigation between a mixed layer and an aged smog layer. Concentrations of primary and secondary pollutants in the FT are obtained from a two-dimensional global model developed by Isaksen.In the reference calculation the modelled concentrations of Ox (sum of O₃ and NO₂) and O₃ are in fair agreement with measurements. The NO_x (sum of NO and NO₂) and NO₂ concentrations are under-estimated by the model but there is a good temporal correlation between calculated and measured concentrations. Validation of other components involved in the chemical scheme is hardly possible due to the paucity of measured data. It can only be stated that the results presented in this paper are not in disagreement with measured or modelled data presented in the literature.In a number of sensitivity runs the influence of European anthropogenic emissions of NO_x and volatile organic compounds (VOC) has been investigated. The calculations indicate that the influence of European emissions on the growing season, daytime averaged (May–September, 10–17 h) O₃ concentrations in The Netherlands is small. For European reductions in the order of tens of per cents a VOC emission reduction is more effective than a NO_x emission reduction in lowering the O₃ concentrations. For strong reductions (about 70%) VOC and NO_x are equally effective. The effects of the modelled underprediction of NO_x concentrations on the production of O₃ on a European scale are probably small. On a local scale the effects are more pronounced due to the NO/O₃ titration (photostationary equilibrium). Therefore, an empirical correction is applied on the modelled O₃ concentrations. After this correction, it is shown that daytime O₃ levels during the growing season increase when European NO_x emissions are reduced (2.0–7.7.% increase at 50% NO_x emission reduction). A reduction in VOC emission leads to decreasing O₃ levels (9% reduction for 40% VOC emission reduction, 16% reduction for 70% VOC emission reduction). For a combined reduction of both VOC and NO_x slightly decreasing ground level O₃ concentrations are expected.     

Aerosol effects on ozone concentrations in Beijing: A model sensitivity study

Most previous O₃ simulations were based only on gaseous phase photochemistry. However, some aerosol-related processes, namely, heterogeneous reactions occurring on the aerosol surface and photolysis rate alternated by aerosol radiative influence, may affect O₃ photochemistry under high aerosol loads. A three-dimensional air quality model, Models-3/Community Multi-scale Air Quality-Model of Aerosol Dynamics, Reaction, Ionization, and Dissolution, was employed to simulate the effects of the above-mentioned processes on O₃ formation under typical high O₃ episodes in Beijing during summer. Five heterogeneous reactions, i.e., NO₂, NO₃, N₂O₅, HO₂, and O₃, were individually investigated to elucidate their effects on O₃ formation. The results showed that the heterogeneous reactions significantly affected O₃ formation in the urban plume. NO₂ heterogeneous reaction increased O₃ to 90 ppb, while HO₂ heterogeneous reaction decreased O₃ to 33 ppb. In addition, O₃ heterogeneous loss decreased O₃ to 31 ppb. The effects of NO₂, NO₃, and N₂O₅ heterogeneous reactions showed opposite O₃ concentration changes between the urban and extra-urban areas because of the response of the reactions to the two types of O₃ formation regimes. When the aerosol radiative influence was included, the photolysis rate decreased and O₃ decreased significantly to 73 ppb O₃. The two aerosol-related processes should be considered in the study of O₃ formation because high aerosol concentration is a ubiquitous phenomenon that affects the urban- and regional air quality in China.     

A characterization of the spatiotemporal variability of non-urban ozone concentrations over the eastern United States

The spatial and temporal variability of the daily 1-h maximum O₃ concentrations over non-urban areas of the eastern United States of America was examined for the period 1985–1990 using principal component analysis. Utilization of Kaiser's Varimax orthogonal rotation led to the delineation of six contiguous subregions or “influence regimes” which together accounted for 64.02% of the total variance. Each subregion displayed statistically unique O₃ characteristics and corresponded well with the path and frequency of anticyclones. When compared to the entire domain, the mid-Atlantic and south subregions observe higher mean daily 1-h maximum concentrations. Concentrations are near the domain average for the northeast and southwest subregions and are lowest in the Great Lakes and Florida subregions. The percentage of observations exceeding 120 ppb were greates in the mid-Atlantic and southwest subregions, near the domain average in the northeast and south subregions, and lowest in the Great Lakes and Florida subregions.Examination of the time series of the principal component scores associated with the subregions indicated that Great Lakes and mid-Atlantic subregions tend to observe a stronger seasonal cycle, with maximum concentrations occurring during the last week in June and first week in July, respectively. The strength of this seasonality is weakened for the northeast and south subregions and its timing delayed, until the end of July and the first of August, respectively. The southwest subregion experiences a greatly diminished seasonality, with maximum concentrations delayed until the middle of August. The seasonality found in the Florida subregion is unique in both its strength and timing, as the highest concentrations consistently occur during the months of April and May. The time series were then deseasonalized and autocorrelations and spectral density estimates calculated, revealing that persistence is much more prevalent in the Florida (autocorrelation significant to a lag of 4 days), south (3 days) and southwest (3 days) subregions. Conversely, autocorrelations are only significant to a lag of one day in the northeast and two days for the Great Lakes and mid-Atlantic subregions.     

南京地区近地面臭氧浓度与气象条件关系研究

通过分析2013—2015年南京地区相关气象要素对近地面臭氧浓度的影响,建立了用于不同季节高浓度臭氧污染事件的预报预警模型,并归纳总结了南京地区高浓度臭氧出现的天气形势.结果表明,近地面臭氧浓度的变化与气象要素密切相关,气温、能见度、日照小时、总(净)辐射辐照度等要素与O_3浓度呈显著正相关,与相对湿度、总(低)云量呈负相关.高浓度臭氧污染是多因子综合作用的结果,典型气象条件表现为:太阳辐射强,低云量少,相对湿度适宜,地面小风速及特定的风向.通过定义高浓度臭氧潜势指数HOPI和风向指数WDI,并综合考虑14:00地面气温、相对湿度及8:00各标准层的相关气象要素,建立了逐季节多指标叠套的高浓度臭氧预报方程.采用2016年资料对其进行检验,发现预报值与观测值的相关系数分别达0.72(冬季)、0.76(春季)和0.73(夏季),说明方程具有较好的拟合效果和可预报性.通过普查历史天气图,归纳了伴随南京地区高浓度臭氧事件出现的8种主要天气形势,即高压类(高压中心G0、高压后部G1)、低压类(低压底部D0、低压前部D1、低压倒槽D2)、均压类(高压相关的均压JG、低压相关的均压JD、其它均压J).其中,以高压后部地面形势出现概率最大,低压前部均压场出现时对应臭氧平均浓度最高.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

北京地区对流层低层臭氧及硫酸盐气溶胶的时空分布

基于OMI/Aura卫星资料,分析了北京地区2007~2016年近10a对流层O₃浓度（0~3km）、硫酸盐气溶胶光学厚度（0~2km）、SO₂（边界层以内）柱浓度时空演变特征.结果表明,近10a来北京地区O₃浓度总体呈现上升趋势,最低值在2007年,浓度为33.65 μg/m³;硫酸盐气溶胶污染总体变化呈现先下降后增长的趋势,2007年硫酸盐气溶胶污染最为严重,2011年污染最轻,对应的AOD值为0.252,但在2014年以后,硫酸盐气溶胶污染又出现增长趋势;SO₂浓度在2007~2016年总体呈现下降的变化趋势,且下降趋势明显,最高值为2007年,最低值出现在2016年,最低值比最高值降低了60.42%,但在2011年污染出现反弹.北京O₃季节变化明显,夏季高、春秋次之、冬季低;硫酸盐气溶胶污染季节特征与O₃相同;SO₂污染主要集中在冬季,采暖期污染程度高于非采暖期.     

Regionalization based on spatial and seasonal variation in ground-level ozone concentrations across China

Owing to the vast territory of China and strong regional characteristic of ozone pollution,it's desirable for policy makers to have a targeted and prioritized regulation and ozone pollution control strategy in China based on scientific evidences. It's important to assess its current pollution status as well as spatial and temporal variation patterns across China.Recent advances of national monitoring networks provide an opportunity to insight the actions of ozone pollution. Here, we present rotated empirical orthogonal function(REOF)analysis that was used on studying the spatiotemporal characteristics of daily ozone concentrations. Based on results of REOF analysis in pollution seasons for 3 years' observations, twelve regions with clear patterns were identified in China. The patterns of temporal variation of ozone in each region were separated well and different from each other, reflecting local meteorological, photochemical or pollution features. A rising trend in annual averaged Eight-hour Average Ozone Concentrations(O_3-8 hr) from 2014 to 2016 was observed for all regions, except for the Tibetan Plateau. The mean values of annual and 90 percentile concentrations for all 338 cities were 82.6 ± 14.6 and 133.9 ± 25.8 μg/m~3,respectively, in 2015. The regionalization results of ozone were found to be influenced greatly by terrain features, indicating significant terrain and landform effects on ozone spatial correlations. Among 12 regions, North China Plain, Huanghuai Plain, Central Yangtze River Plain, Pearl River Delta and Sichuan Basin were realized as priority regions for mitigation strategies, due to their higher ozone concentrations and dense population.     

Relationships between synoptic-scale atmospheric circulation and ozone concentrations in Metropolitan Pittsburgh,Pennsylvania

A synoptic climatology demonstrates the relationships between the atmospheric circulation and surface ozone (O₃) concentrations. To deduce these associations, a subjective synoptic classification scheme is applied to 10 years' O₃ data from the Pittsburgh metropolitan area. The results focus on four aspects of the atmospheric circulation-O₃ relationship: average, extreme-event, between season and year-to year conditions. On average, each of the nine circulation types is related to a characteristic O₃ concentration level and cumulative O₃ dose. Extreme high-O₃ events are associated with either the western side of a slowly migrating anticyclone or a stagnating extended high-pressure ridge; low-O₃ events are experienced under cool and cloudy cyclonic conditions. Between-season variations in the average and extreme circulation-O₃ relationshipsare observed: the high-pressure features that produce the high st O₃ levels in summer are related to low levels in winter, while circulation patterns that contribute very little to summertime O₃ build-up are associated with the highest levels of wintertime O₃. The latter situation could be caused by tropopause folding and the introduction of stratospheric ozone in winter months. While zonal (meridional) circulation regimes tend to produce lower (higher) mean annual O₃ levels, such year-to-year changes in synoptic-type frequencies do not appear to be strongly related to interannual variations in O₃, and other non-climatic factors appear to be of greater importance.     

Model calculating annual mean atmospheric dispersion factor for coastal site of nuclear power plant

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Evaluation and comparison of statistical forecast models for daily maximum ozone concentrations

Three statistical models that estimate daily maximum ozone (O₃) concentrations in the lower Fraser Valley of British Columbia (BC) are specified using measured concentrations from two monitoring stations during the time period 1978–1985. The three models are (1) a univariate deterministic/stochastic model, (2) a univariate autoregressive integrated moving average (ARIMA) model, and (3) a bivariate temperature and persistence based regression model.The three models as well as a persistence forecast are tested by comparison with O₃ concentrations observed during 1986; it is concluded that the bivariate model is superior to both unvariate models and persistence. The ARIMA model has nearly the same predictive capability as persistance while the mixed deterministic/stochastic model performs the worst. This suggests that the traditional time series technique of decomposing a series into a trend, a cycle and a stochastic component may not be appropriate for O₃ air quality forecasting.