平流层臭氧对地表有机氯排放的多耦合响应

采用一个包含平流层化学、辐射、动力相互作用的二维模式,对地表有机氯排放变化影响平流层的具体过程作出评估,从而确定平流层臭氧对于地表有机氯排放的多耦合响应,也检验了“蒙特利尔议定书”的减排效果。结果表明,以议定书框架协议达成的20世纪90年代地表有机氯排放减少按30％计算,通过输送、扩散和一系列化学反应,导致平流层中上层的各活性化学族的浓度发生变化,稳定后平流层40km到48km经向平均的相对变化率,ClOx减少20％,HOx和NOx增加2％左右,O3恢复5％左右。此外,这些成分变化导致平流层中上层辐射加热率增加,平流层变冷趋势减缓0．6K。     

南极臭氧洞与南极涡旋的变化——IAP模式的试验结果

通过对IAP9层全球大气环流模式试验结果的分析,讨论了1987年南极臭氧洞对平流层大气辐射加热率和温、压、风场的影响。结果表明,南半球高纬和极地平流层臭氧含量的耗损,使该地区辐射加热率明显减小,气温明显下降,等压面明显下降,南极涡旋明显加强,说明南极春季涡旋的强弱与该地区臭氧含量及其热状况有密切关系。     

北极臭氧洞

正2020年由于北极地区大气环流异常,春季平流层极涡中温度持续偏低,平流层冰晶云面积也创新高,臭氧的化学损耗更大,低值低于220220 DU,故而首次出现了臭氧洞。在目前大气环境被污染的情况下,南极臭氧洞的变化和北极臭氧洞是否出现等,取决于南北两极春季平流层极涡及其低温状态的变化。2020年春季,首个北极臭氧洞出现与春季平流层极涡的持续低温有关,是由大气环流等自然因素引起的,并无环境指示意义。     

1979～2020年北极和青藏高原臭氧低值区的动力输送特征比较

基于ERA5月平均再分析资料,利用Lorenz环流分解方法从定常和瞬变以及基流和涡旋的角度对比了北极与青藏高原臭氧低值区的动力输送特征。结果表明：动力总输送在两地上平流层作用最强,均使其臭氧浓度降低,且定常输送均强于瞬变输送,纬向与经向输送的作用均大致相反。然而,动力输送在北极地区的作用强度远大于青藏高原地区。北极地区纬向输送使得平流层中上层臭氧浓度降低,平流层下层臭氧浓度升高,经向输送的作用与之相反且强度明显偏弱,二者均主要作用于上平流层。青藏高原地区纬向和经向输送除在上平流层均使得臭氧浓度降低外,二者作用大致相反且强度相当,输送大值区在垂直方向上存在双中心结构,分别位于上平流层与上对流层—下平流层（Upper Troposphere–Lower Stratosphere,简称UTLS）区。两地区纬向和经向输送的差异均主要由定常涡旋输送所造成。青藏高原地区定常与瞬变输送的强度差异没有北极地区大。此外,两地定常和瞬变输送中涡旋对臭氧纬向平均的输送均起到主要作用,体现出涡旋输送在两地臭氧浓度变化的动力输送过程中发挥着至关重要的作用。     

南极臭氧洞计算机模拟

一维时空光化学模式引进垂直运动及离子反应生成的氮氧(NOx)、氢氧(HOx)化合物。模式中采用1978到1983年期间的太阳紫外辐射通量及南极73度的纬向八月份平均温度。 计算结果表明:春季南极出现臭氧洞,主要是第21太阳黑子周峰值期太阳紫外辐射减少造成的。其次,在太阳黑子周峰值期伴随多次大的太阳质子事件,产生大量氮氧、氢氧化合物。在极区太阳质子事件产生的化合物催化破坏平流层臭氧可持续几天至几年。 南极冬春季节强大的下降垂直运动是南极臭氧洞形成发展极其重要的局部动力条件,特别是在极夜期间。太阳升起后,垂直运动的影响不明显。 南极臭氧洞的形成主要是通过光化变化过程,动力过程是其局部的充要条件,人为活动产生的含氯化合物对低层大气臭氧的直接破坏不可忽视。基于上述论点,可以预期进入第22太阳黑子周期,南极及全球大气臭氧的分布状态将会改变,大自然本身自复。     

平流层臭氧变化对对流层气候影响的研究进展

平流层对对流层的作用是准确评估、预测对流层气候变化的一个重要方面。其中平流层成分尤其是臭氧的变化,可以改变平流层乃至对流层的辐射平衡,从而影响平流层、对流层的热动力过程。本文从辐射、动力2个角度介绍了平流层臭氧影响对流层气候变化的若干研究进展。平流层臭氧可以通过长短波辐射的方式对对流层大气造成辐射强迫,利用大气化学气候模式可以定量计算平流层臭氧变化引起的辐射强迫,但是辐射强迫的估算受模式中辐射传输模块本身缺陷的影响存在不确定性。动力方面,平流层臭氧变化产生的辐射效应可以改变温度的垂直和经向梯度,造成波折射指数的变化,进而影响平流层甚至对流层内波的折射与反射,通过上对流层下平流层区域内的波—流相互作用,对对流层气候产生影响。另外,南极臭氧损耗可通过大气环状模影响冬春季中高纬度对流层的天气气候,但是其影响的强度大小以及物理机制仍需进一步的确认。值得注意的是,北极平流层臭氧的变化与北半球中高纬度气候变化之间的关系相比南半球要更加复杂,需要更为深入的研究。     

基于MUAM模拟的20世纪末12月平流层十年际变化

利用中高层大气模式（MUAM）研究20世纪末12月平流层气候态的十年际变化,基于一组敏感性试验评估下边界条件、二氧化碳及臭氧浓度变化对平流层温度变化的分别影响,着重探讨了南北极局部增暖的机制差异。结果表明,相较于20世纪80年代,90年代12月北极中上平流层西风减速,中低层增温,这主要与下边界条件变化导致行星1波的上传显著增强（2波削弱）有关。同一时期,南极平流层低层西风加速温度降低,中上层东风减速温度升高,这主要与南极低平流层显著的臭氧损耗有关;下边界条件变化和中层局地的臭氧增加也有一定的贡献,但低层臭氧损耗所诱导的极涡加速使得波传播环境或条件有利于1～2波上传增强（1波主导）至更高高度可能是最终导致中上层增暖的主要原因。     

未来甲烷排放增加对平流层水汽和全球臭氧的影响

利用一个耦合的大气化学-气候模式(WACCM3)研究了地表甲烷排放增加对平流层水汽和全球臭氧变化的影响.结果表明,如果地表甲烷的排放量在2000年的基础上增加50%(达到政府间气候变化专门委员会A1B排放情景中2050年的值),平流层水汽体积分数将平均增加约0.8×10^-6.南半球平流层甲烷转化为水汽的效率比北半球高.在北半球平流层中,1mol甲烷分子可以转化为约1.63mol的水汽分子,而在南半球1mol甲烷分子大概可以转化为约1.82mol的水汽分子.甲烷排放增加50%将使全球中低纬度地区以及北半球高纬度地区的臭氧柱总量增加1%-3%,使南半球高纬度地区臭氧柱总量增加近8%,而秋季(南半球春季)南极地区臭氧柱总量增加幅度可高达20%,南极臭氧的这种显着增加主要是由于甲烷增加造成的化学反馈所致.在北半球中高纬度地区,甲烷增加引起的臭氧变化主要与甲烷氧化导致的水汽增加有关.研究还表明,未来甲烷排放增加对臭氧的恢复作用其实与溴化物排放的减少一样重要.     

1997年和2011年春季北极臭氧损耗事件的对比分析

采用SLIMCAT化学传输模式以及再分析资料,对比分析了1997和2011年北极地区平流层臭氧异常偏低事件及其成因。结果表明,1997和2011年3月北极地区大气臭氧柱总量（TCO）异常值都达到了约-80 DU,并且在30-200 hPa（中下平流层）区域的大气臭氧柱总量异常约占整层大气臭氧柱总量异常的80%。分析表明发生在这两年的极端臭氧偏低事件均可能是由于上一年冬季的拉尼娜事件导致上传的行星波减少,使得北极极涡加强,平流层温度异常偏低,生成了更多极地云,引起更强的臭氧化学损耗导致的。对比这两年的大气臭氧柱总量变化发现,2011年的柱总量减少得更快。2011年北极地区上对流层下平流层（UTLS）区域臭氧下降要明显强于1997年,其主要原因应该是2010-2011冬季的拉尼娜活动更强,北太平洋海温更高,进一步减弱阿留申低压和平流层波活动。这导致2011年极涡温度异常偏低更强烈,形成了更多的极地平流层云甚至出现了第二类极地平流层云,最终加速该年春季的臭氧化学损耗引起的。     

近30a北极平流层臭氧的季节和年际变化特征

综合利用1978-2011年TOMS（Total Ozone Mapping Spectrometer）和OMI（Ozone Monitoring Instrument）臭氧总量资料,MLS（Microwave Limb Sounder）臭氧廓线资料以及NCEP/NCAR再分析气象场资料,对比研究了近30a南北极臭氧总量的年际变化和季节变化差异,重点分析了2010/2011年冬末春初北极臭氧出现的异常损耗现象,探讨北极春季臭氧低值产生的原因。结果表明：与南极地区一年四季都保持一个臭氧低值中心明显不同,北极臭氧总量的减少则是伴随着整个春夏季（4-8月）,在秋季（10月）达到最低值,冬季（11月-次年2月）北极臭氧快速恢复,这主要是由于南北半球极地地区环流差异和温度差异造成的。南北两极年均O3总量呈下降趋势,两极地区O3总量年际变化最大的季节是春季。近30a,北极在1997和2011年春季（3-4月）分别达到极低值355DU和361DU,但近年来两极臭氧年际变化趋势不明显。2011年春季,北极地区出现的较严重臭氧低值现象从3月中旬至4月中旬持续了近1个月,2010/2011年冬春季平流层低温和臭氧低值对应关系很好。     

Simulation of the influence of ion-produced NOx and HOx radicals on the antarctic ozone depletion with a one-dimensional model

A one-dimensional time-dependent photochemical model is used to simulate the influence of ion-produced NOx, and HOx radicals on the Antarctic ozone depletion in polar night and polar spring at a latitude of 73 degrees south.Vertical transport and nitrogen-oxygen (NOx), hydrogen-oxygen (HOx) production by ionic reactions have been introduced into the model.NOx and HOx produced by precipitating ions are transported into the lower stratosphere by vertical motion and have some effects in the development of the Antarctic ozone depletion.From winter through spring the calculated ozone column decreases to 269.4 DU. However, this value is significantly higher than the total ozone observed at several Antarctic ozone stations.     

近地面臭氧研究进展

近地面臭氧是空气中氮氧化物和挥发性有机物发生光化学反应的产物,其浓度与气象条件密切相关。晴天少云、紫外辐射较强、温度较高、相对湿度较低以及风速较小的天气,均有利于臭氧的生成,其中紫外辐射是产生臭氧最关键的因素。臭氧前体物（氮氧化物和挥发性有机物）的浓度及其比值是影响近地面臭氧浓度的另外三个重要因素。我国大多数城市的O3处于VOC控制区,即NOx浓度的增加会引起O3浓度的降低,而VOCs浓度的增加则会使其浓度升高。因而VOC源解析问题成为近年来O3研究的一个热点问题。同时,由于气溶胶可以直接吸收、散射太阳紫外辐射、短波辐射以及大气长波辐射,因此气溶胶的存在会影响大气中光化学反应的进程,从而影响臭氧的光化学生成,气溶胶对近地面臭氧的影响已成为目前大气环境的前沿课题。     

地面臭氧的变化规律和计算方法的初步研究Ⅰ.紫外波段

通过对广州鼎湖山近地面O3、NOx、太阳辐射、气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳辐射的变化规律,详细讨论了紫外波段、不同天气条件地面O3与NOx,光化学反应、气溶胶、光化辐射等之间复杂的关系.用光能量传输与守恒的观点来考虑大气中与紫外辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明,不同情况下计算值与观测值均吻合较好.     

Evaluation of the use of photochemical indicators to assess ozone—NOx—VOC sensitivity in the Southwestern Iberian Peninsula

Understanding the chemical links between ozone (O₃) and its two main precursors, nitrogen oxides (NOx) and volatile organic compounds (VOC), is important for designing effective photochemical smog reduction strategies. This chemical relationship will determine which precursor (NOx or VOC) emission reduction will be more effective for decreasing the ozone formation. Under certain conditions, ozone levels decrease as a result of a reduction in NOx emissions but do not respond significantly to changes in VOC emissions (NOx-sensitive condition), while under other conditions ozone concentrations decrease in response to reductions in VOCs and may even increase when NOx emissions are reduced (VOC-sensitive conditions). Indicator species can be used to assess the sensitivity of ozone to changes in the emissions of its precursors. These indicators are species or species ratios involved in ozone photochemistry which reflect the primary chemical process through which the ozone was formed. In this work we use the MM5-CAMx model system to explore the behaviour of various indicator species during two meteorological situations featuring different atmospheric conditions in a complex terrain area. The results show that indicators based on nitrogen compounds (i.e,. NOy and NOz) are suitable for defining the transition range from VOC- to NOx-sensitive chemistry, and that despite the uncertainties associated with the use of chemical indicators, the ratios O₃/NOy and O₃/NOz may provide a simple and useful way to summarize the response of ozone to changes in NOx and VOC emissions in Southwestern Spain.     

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.     

地面臭氧的变化规律和计算方法的初步研究Ⅱ.可见光波段

通过对广州鼎湖山近地面O3、NOx、太阳辐射,气象参数等项目的观测和理论分析,研究了地面O3与NOx等微量气体及太阳可见光辐射的变化规律,详细讨论了可见光波段、不同天气条件地面O3与NOx、光化学反应、气溶胶、可见光辐射等之间复杂的关系.提出以光能量传输与守恒的观点来考虑大气中与可见光辐射有关的主要过程,并以此来研究大气光化学过程中所遵循的能量规律,建立了一个简单、实用、省时的统计模式,用于计算地面O3浓度.结果表明:不同情况下,计算值与观测值吻合得均比较一致.     

On the Nonlinear Response of Lower Stratospheric Ozone to NO_x and ClO_x Perturbations for Different CH_4 Sources

The impact of sulfate aerosol, ClO2 and NOx perturbations for two different magnitudes of CH4 sources on lower stratospheric ozone is studied by using a heterogeneous chemical system that consists of 19 species belonging to 5 chemical families (oxygen, hydrogen, nitrogen, chlorine and carbon). The results show that the present modeled photochemical system can present several different solutions, for instance, periodic states and multi-equilibrium states appearing in turn under certain parameter domains, through chlorine chemistry and nitrogen chemistry together with sulfate aerosol as well as the increasing magnitude of CH4 sources. The existence of catastrophic transitions could produce a dramatic reduction in the ozone concentration with the increase of external sources.     

On the nonlinear response of lower stratospheric ozone to NOx and ClOx perturbations for different CH4 sources

The impact of sulfate aerosol, ClOx and NOx perturbations for two different magnitudes of CH4 sources on lower stratospheric ozone is studied by using a heterogeneous chemical system that consists of 19 species belonging to 5 chemical families （oxygen, hydrogen, nitrogen, chlorine and carbon）. The results show that the present modeled photochemical system can present several different solutions, for instance, periodic states and multi-equilibrium states appearing in turn under certain parameter domains, through chlorine chemistry and nitrogen chemistry together with sulfate aerosol as well as the increasing magnitude of CH4 sources. The existence of catastrophic transitions could produce a dramatic reduction in the ozone concentration with the increase of external sources.     

A Possible Photochemical Link Between Stratospheric and Near-Surface Ozone on Swiss Mountain Sites in Late Winter

Record high near-surface ozone concentrations at two elevated sites (Chaumont, 1140 m asl, and Rigi, 1030 m asl) in Switzerland were observed simultaneously with extremely low total ozone during a fair weather period in mid-February 1993. An analysis of ozone, temperature, humidity, and wind profiles suggests that the surface ozone peaks were most possibly generated within the region in a layer between about 1000 and 1500 m asl. Mean diurnal cycles of ozone concentration during the period shows a strong increase from late morning to late afternoon at Chaumont and at the same time a decrease at the high alpine site Jungfraujoch (3580 m asl). The different diurnal ozone cycles can both be explained photochemically by taking into account the large difference in NOx concentrations (about two orders of magnitude) between the sites. Photochemical processes are also indicated by the diurnal cycles of NO2 and NO concentration. As a strong photochemical activity is not expected in mid-February at 47°N, we hypothesize that the extremely low total ozone played a role. Total ozone controls the amount of UV-B radiation reaching the troposphere and thus influences photochemical processes. Using a radiation model, we calculated an increase in ozone photolysis at Chaumont and Jungfraujoch of 73% and 83%, respectively, on the day with the lowest total ozone (243 DU) compared to average February conditions (335 DU). It is suggested that total ozone changes have the potential to stimulate photochemistry sufficiently to produce the observed surface ozone peaks at Chaumont and Rigi of 61 and 64 ppbv, respectively. A fog layer just below Chaumont during these days probably also influenced photochemistry, but on a smaller spatial scale. Our empirical results on the influence of changing UV radiation on tropospheric photochemistry are in close agreement with model studies of other groups. Although this case study represents unique conditions, a distinct anticorrelation between near-surface ozone at Chaumont and total ozone also appears in other years (1992–1997) when selecting fair weather days in mid-February. However, other influences cannot be excluded. The selected days provide evidence of a significant photochemical source of ozone in the mid-latitude lower troposphere in late winter.     

NO<Subscript><Emphasis Type="Italic">x</Emphasis></Subscript> change over China and its influences

A 3-D chemical transport model (OSLO CTM2) is used to investigate the impact of the increase of NOx emission over China. The model is capable to reproduce basically the seasonal variation of surface NOx and ozone over eastern China. NOx emission data and observations reveal that NOx over eastern China increases quite quickly with the economic development of China. Model results indicate that NOx concentration over eastern China increasingly rises with the increase of NOx emission over China, and accelerates to increase in winter. When the NOx emission increases from 1995 to its double, the ratio of NO2/NOx abruptly drops in winter over northern China. Ozone at the surface decreases in winter with the continual enhancement of the NOx level over eastern China, but increases over southern China in summertime. It is noticeable that peak ozone over northern China increases in summer although mean ozone changes little. In summer, ozone increases in the free troposphere dominantly below 500 hPa.Moreover, the increases of total ozone over eastern China are proportional to the increases of NOx emission.In a word, the model results suggest that the relationship between NOx and ozone at the surface would change with NOx increase.