关于大气臭氧问题的主要研究进展

大气臭氧是非常重要的温室气体,其在全球的分布具有不均匀性,受到人类活动的显著影响,近几十年来由于对流层臭氧增加造成正的辐射强迫会增加大气温室效应,而平流臭氧减少会使其吸收的紫外线辐射减少,为负的辐射强迫,使得平流层大气降温。因此关于大气臭氧浓度变化及其对气候的影响是非常复杂的,一直是科学界研究的热点和难点问题。自从20世纪50年代末到70年代就发现臭氧浓度有减少的趋势。1985年英国南极考察队在南纬60°地区观测发现存在大气臭氧层空洞;自此开始,大气臭氧问题引起了世界各国的极大关注,并给予很多研究。目前,平流层和对流层臭氧浓度的观测仍然是研究的重点。鉴于对流层臭氧浓度持续升高和平流层臭氧浓度的不断下降,以及他们在对流层和平流层大气温度中所起的不同作用,本文将主要针对近五年来大气臭氧相关的研究进展进行简要的综述,包括对流层和平流层臭氧浓度及其观测研究,和人类活动的影响等方面进行分述。最后给出目前研究工作的不足和未来工作展望。     

对流层臭氧的控制因子

讨论了控制对流层臭氧水平的两个因子,得出了这样的结论:气流流动和光化学反应是对流层臭氧的重要来源,但两者在指定的位置和时间的相对重要性没有弄清楚,另列出了对流层臭氧研究中存在的困难.     

大气对流层顶的臭氧时空分布变化

 利用1958~2001年的臭氧垂直分布和NCEP资料,计算出全球对流层顶的气候场,并对其空间分布、季节、年际和年代际演变进行了分析.结果表明:①对流层顶臭氧质量比呈纬向分布的特征明显,南北半球中纬度和南极为高值区,赤道和北极为低值区,且与对流层顶高度和温度场有对应关系;②从400~70 hPa的温度和臭氧质量比垂直经向剖面中,显现出对流层顶的上层和下层由于具有不同的物理和化学过程导致垂直分布存在差异;③对流层顶臭氧质量比纬向距平场的年代际变率具有不同位相的时空演变尺度,南半球的时空差异比北半球大,南极最不稳定,低纬和赤道地区幅度变化较小,但时间尺度较大;④极地各季节对流层顶的臭氧分布和高度场特征相似,低纬则与温度场分布较一致;⑤对流层顶断裂带中臭氧质量比最大值出现在春季,秋季为最小值,其对应的纬度存在明显的季节空间经向波动,夏季达到最高纬度,冬季到达最低纬度;⑥对流层顶臭氧质量比纬向距平的季节变率表现出准半年变化趋势,且两半球变化趋势相反.     

Seasonal variation of global stratosphere-troposphere mass exchange

By Wei formula in pressure coordinate, the stratosphere-troposphere mass exchange (STME) is diagnosed globally for 44 years from 1958 to 2001 using the European Center for Medium-Range Weather Forecasts (ECMWF) reanalysis datasets. Regions of mass flux into the stratosphere are found over Indonesia, bay of Bangladesh and the mid-west coast of South Africa. Compensating mass outflow from the stratosphere appears mainly over mid-latitudes near large-scale troughs. Upward and downward transport of mass at the middle and high latitudes accompany with each other. Mass flux into troposphere is stronger in autumn and winter than in spring and summer. Strong downward mass flux into the troposphere occurs in eastern Asia the whole year with nearly stable sites. Although the area of eastern Asia accounts for only 5.6% of that of the northern hemisphere (NH), its net mass exchange reaches 15.83% of that of the NH, which means that research on STME of eastern Asia is greatly important to that of the NH and even the global areas. Air across the tropopause enters more from stratosphere to troposphere than that from troposphere to stratosphere, which is possibly related with systematic bias of the assimilated datasets and with persistent rise of the tropopause height. Contributions of the mass exchange and the mass flux exchange in the NH and southern hemisphere (SH) on their latitudes increase from equator to pole, with larger contributions in the NH. Mass exchange and mass flux exchange per areas at high latitudes are larger than that at low latitudes, which means greater mass exchange efficiency at high latitudes.     

Seasonal variation of global stratosphere-troposphere mass exchange

By Wei formula in pressure coordinate, the stratosphere-troposphere mass exchange (STME) is diagnosed globally for 44 years from 1958 to 2001 using the European Center for Medium-Range Weather Forecasts (ECMWF) reanalysis datasets. Regions of mass flux into the stratosphere are found over Indonesia, bay of Bangladesh and the mid-west coast of South Africa. Compensating mass outflow from the stratosphere appears mainly over mid-latitudes near large-scale troughs. Upward and downward transport of mass at the middle and high latitudes accompany with each other. Mass flux into troposphere is stronger in autumn and winter than in spring and summer. Strong downward mass flux into the troposphere occurs in eastern Asia the whole year with nearly stable sites. Although the area of eastern Asia accounts for only 5.6% of that of the northern hemisphere (NH), its net mass exchange reaches 15.83% of that of the NH, which means that research on STME of eastern Asia is greatly important to that of the NH and even the global areas. Air across the tropopause enters more from stratosphere to troposphere than that from troposphere to stratosphere, which is possibly related with systematic bias of the assimilated datasets and with persistent rise of the tropopause height. Contributions of the mass exchange and the mass flux exchange in the NH and southern hemisphere (SH) on their latitudes increase from equator to pole, with larger contributions in the NH. Mass exchange and mass flux exchange per areas at high latitudes are larger than that at low latitudes, which means greater mass exchange efficiency at high latitudes.     

利用探空资料对对流层-平流层热力结构的分析

利用16个探空站近6年的高分辨率探空资料,采用经验正交函数和数值积分等方法,分析了对流层、对流层顶和平流层下层的温度层结特征,主要得出以下结论:①对流层顶温度年变幅最小,对流层上层和平流层下层(包括对流层顶)与对流层中低层具有相反的温度变化趋势.②不同地区对流层顶高度表现为随纬度升高而降低的规律,平均每升高1°对流层顶高度下降44 m,同纬度高原地区对流层顶高度高于平原地区.③各站对流层平均温度总体表现为单峰型结构,与地面温度的季节变化特征相同,只是年较差小于地面.④对流层顶高度与对流层平均温度具有显著的正相关关系,对流层增温时对流层顶高度升高,对流层顶高度主要取决于对流层热力状况.     

Mass exchange between stratosphere and trotosphere over the Tibetan Plateau and its surroundings

Using NCEP dataset we calculate the exchange of mass across the thermal tropopause by the Wei's method from 1978 to 1997 over the Tibetan Plateau and its surroundings. We also calculate the annual variation of aerosol and ozone of 100 hPa level with the monthly SAGE dataset from July 1988 to December 1993. Results indicate that ( i ) the mass from troposphere to stratosphere is magistral station in summer over the Tibetan Plateau and its surroundings. The air transport reaches the summit in midsummer with two large value centers, which lie in the north of Bengal Bay and southeastern Tibetan Plateau, respectively. A large value center, which lies over the Tibetan Plateau, is smaller than that aforementioned. In winter, the mass transport is from stratosphere to troposphere, and reaches the minimum in January. ( ii ) As far as the 19-year mean cross-tropopause mass exchange from June to September is concerned, the net mass transport is 14.84x1018 kg from troposphere to stratosphere. So the area from the Tibetan Plateau to the Bengal Bay is a channel through which the mass of lower atmosphere layer gets into upper troposphere and lower stratosphere. (iii) The cross-tropopause mass may take the lower level aerosol to the tropopause. Then, the concentration of aerosol near the tropopause becomes larger, which may cause the content of ozone to reduce.     

对流层顶大气臭氧的季节变化研究

 采用季节划分和季节突变的概念、理论及方法,对44a(1958~2001年)的大气臭氧资料及对流层顶气压场资料进行了计算,并分析了对流层顶大气臭氧的季节变化.结果发现对流层顶大气臭氧的季节变化在全球大部分区域中的突变性都比较明显,表明对流层顶大气臭氧的季节变化受到上对流层和下平流层中多种因素的影响.通过分析还发现,利用曾庆存所定义的参数R_W(t)及有关的一些概念和方法确能很好地反映对流层顶大气臭氧的季节变化.     

对流层垂直臭氧分布变化量对生物质燃烧响应的模拟研究

 采用区域气候模式与大气化学模式相连接的模式系统,模拟研究了对流层垂直臭氧分布变化量对东南亚生物质燃烧排放源强变化的响应程度.结果表明,源区对流层臭氧垂直积分浓度对燃烧源强变化十分敏感,下游区次之.特别是在对流层的中低层影响最显著,但对源区臭氧的贡献比下游区要大得多.在对流层中高层,源区和下游区受影响程度相当.对流层低层源区臭氧增加的时间超前下游区,超前的时间随高度的增加而减小,而在对流层中层出现滞后现象,到对流层高层臭氧最大值出现的时间相同.     

穿越东亚不同定义对流层顶质量和臭氧通量的分析

选取动力学和热力学定义的对流层顶作为平流层和对流层之间的分界,并利用等熵坐标下的Wei公式对东亚地区穿越对流层顶的质量和臭氧通量进行了分析,结果发现对流层顶的选择对于研究平流层与对流层交换方面的作用至关重要.东亚地区质量和臭氧通量交换在整体上具有明显的年代际变化特征,1958～2001年近44a的通量交换距平变化可以分为3个比较稳定的时段:即1958～1971,1972～1985和1986～2001年.在这3个时段中,通量交换距平分布表现为"负正负"的变化趋势,说明在东亚地区质量和臭氧净通量交换情况为先增强后减弱.东亚地区平流层和对流层之间质量和臭氧交换正距平区在东北平原和华北平原附近经历了一个逐渐增强的变化过程,表明这些区域在东亚地区平流层和对流层之间的质量和臭氧通量交换中扮演着越来越重要的角色.     

Ozone vertical variations during a typhoon derived from the OMI observations and reanalysis data

Typhoon is considered to play a key role in the dynamical exchange processes taking place between the troposphere and stratosphere. In this paper, the impact of typhoon on the ozone distribution in the upper troposphere and middle stratosphere is investigated using ozone profiles measured by Aura’s Ozone Monitoring Instrument and meteorological fields from reanalysis data. During the passage of Typhoon Hai-Tang in 2005 over the western North Pacific, low values of ozone column above 200 hPa and ozone mixing ratio between the upper troposphere and the middle stratosphere (from 200 to 50 hPa) are observed right above the typhoon’s track, a result due to the strong upward propagation of air associated with overshooting convection in typhoon. A comparative analysis of different stages of Hai-Tang suggests that in the region where typhoon has higher intensity the troposphere-to-stratosphere transport is enhanced. These results indicated that the typhoon has a significant impact on the ozone variation in the upper troposphere and the middle stratosphere.     

南亚地区生物体燃烧对昆明地区对流层中下层臭氧浓度的影响

2001-03-21在昆明用电化学臭氧探空仪探测到了对流层低层异常的高浓度臭氧分布。这个个例中昆明对流层低层异常的高浓度臭氧分布特征不同于2001-03-08的昆明个例。使用NCEP分析资料、中尺度数值模式MM5模拟的大气环流数据、卫星观测的东南亚地区的生物体燃烧状况、气溶胶指数等资料,分析了这段时间的天气形势、大气环流、空气块后向轨迹以及生物体燃烧产生的烟尘轨迹,结果发现高浓度的臭氧空气来源于有生物体燃烧的南亚地区。这与以往研究中东南亚地区生物体燃烧导致华南地区对流层低层臭氧浓度异常增高有所不同。     

南亚地区生物体燃烧对昆明地区对流层中下层臭氧浓度的影响

2001-03-21在昆明用电化学臭氧探空仪探测到了对流层低层异常的高浓度臭氧分布。这个个例中昆明对流层低层异常的高浓度臭氧分布特征不同于2001-03-08的昆明个例。使用NCEP分析资料、中尺度数值模式MM5模拟的大气环流数据、卫星观测的东南亚地区的生物体燃烧状况、气溶胶指数等资料,分析了这段时间的天气形势、大气环流、空气块后向轨迹以及生物体燃烧产生的烟尘轨迹,结果发现高浓度的臭氧空气来源于有生物体燃烧的南亚地区。这与以往研究中东南亚地区生物体燃烧导致华南地区对流层低层臭氧浓度异常增高有所不同。     

南亚季风环流与臭氧时空分布变化关系的特征分析

利用2005年1月至2017年12月搭载在美国环境监测Aura卫星上的臭氧监测仪（Ozone Monitoring Instrument, OMI）数据和NCEP气象资料,在夏季风环流指数定义方法的基础上,重新定义了南亚区域冬季风环流指数,并分别计算了南亚夏季风和冬季风环流指数. 结合冬夏两季环流的强弱变化采用相关分析、合成分析和奇异值分解（Singular Value Decomposition, SVD）等方法,探讨了环流异常形势下臭氧的时空变化特征. 结果表明:①南亚夏季纬向环流与经向环流的强度变化存在一致性,冬季经向环流与纬向环流的强度变化差异较大. ②南亚臭氧柱总量的季节变化明显,且近13年来臭氧柱总量整体呈上升趋势. ③夏季（冬季）风环流指数与对流层中低（中高）层和平流层中低层臭氧的相关性显著,但夏季平流层和对流层的相关趋势相反. ④夏季风环流增强对应青藏高原?伊朗高原上空及南侧区域的上升运动增强,对臭氧的输送作用是造成对流层臭氧分布呈现差异的原因. ⑤冬季风环流强弱期的垂直上升和下沉运动中心的移动,以及南北向、东西向气流交汇区的差异是造成臭氧分布不同的原因.     

平流层极地臭氧损耗影响对流层气候的研究进展

大气平流层臭氧的严重损耗将导致到达地面的太阳紫外辐射增加已经是公共社会普遍关切的问题。最近几年,平流层臭氧损耗能否对对流层大气环流和气候产生重要影响也引起了广泛的重视,并且已成为大气科学的一个热点问题。观测研究表明近二三十年来在两极臭氧严重损耗的季节,地表气温有明显的变暖趋势,也就是欧亚大陆1—3月份和南极半岛12—5月份的地面温度呈现显著增温。这些增温趋势很可能是平流层两极的严重臭氧损耗造成的。当然,这些增温并非是由臭氧损耗的辐射效应直接造成的,而是通过波－流相互作用以及平流层－对流层相互作用等动力学过程实现的。大量的数值模拟工作也对此问题进行了研究,一些模拟结果与观测结果基本一致,另一些则发现平流层臭氧损耗的强迫作用较弱,也有模拟工作认为其他外界强迫如温室气体增加和热带海面温度升高也非常重要。作者综述了这一研究领域在近几年的最新研究进展,总结有关的观测分析和数值模拟结果,阐述平流层极地臭氧损耗可能影响地面温度的物理机制,以及澄清各种争论要点。     

中国西南上空大气臭氧垂直分布的结构特征

 用球载电化学臭氧探空仪于2001年春季在中国西南昆明上空测得臭氧垂直分布的精细结构,结果表明臭氧垂直廓线具有多层次特征.在21～30km高度之间是臭氧分压多峰值的极大值层,极大值平均为15.13mPa,臭氧混合比极大值平均高度在30.2km.对流层顶附近臭氧分压存在极小值,且有南风分量的极大风层对应.对流层上层和平流层低层出现臭氧峰值时,其峰值层附近具有显著的冷平流特征.在5km以下观测到了不稳定的对流层臭氧高浓度峰值层.     

东亚和西太平洋地区Hadley环流对对流层臭氧分布的影响

 采用了后向轨迹方法,利用臭氧混合比ρ₃和风场资料,来探讨东亚和西太平洋地区上空Hadley 环流对对流层臭氧分布的影响,文中对所研究关键点上7月份对流层高、中、低三层的轨迹进行分向统计后,计算方向概率与ρ₃的相关系数,得出了东亚和西太平洋地区Hadley 环流水平平流作用对臭氧分布的影响.结果表明:①青藏高原地区上空对流层低层Hadley 环流水平平流作用将会使臭氧混合比减少,而对应的高层南半球Hadley环流下沉支,其总体效果则是使臭氧增加;②在西太平洋地区上空对流层低层,北半球Hadley环流上升支其作用是使臭氧混合比减少,对应的高层南半球Hadley环流下沉支,其影响较弱;③另外,东亚季风的水平平流作用似乎和臭氧的分布也有联系,这还有待于进一步研究.     

Global distribution of peroxyacetyl nitrate

Nitrogen oxides (NOx) have a central role in the chemistry of the atmosphere, especially in key processes relating to ozone, hydroxyl-radical (OH) and acid formation. High reactivity of NOx (lifetime of 0.5-2 days) precludes hemispheric-scale transport and it has been proposed that non-methane hydrocarbons present in the troposphere can transform NOx into its organic forms principally as peroxyacetyl nitrate (PAN). PAN is highly stable in the colder regions of the middle and upper troposphere and can provide a mechanism for NOx storage and transport. Once transported, PAN and its homologues can easily release free NOx in warmer atmospheric conditions. PAN is probably ubiquitous and its concentrations could exceed those of NOx in clean tropospheric conditions. Here we present the first view of the global distribution of PAN based on extensive shipboard and aircraft measurements. PAN is more abundant in the Northern than in the Southern Hemisphere and in the continental than in the marine troposphere. In contrast to its behaviour in polluted atmospheres, PAN mixing ratios in winter greatly exceed those in summer. These measurements provide a basis for assessing the significance of PAN as a reservoir of NOx and for extending and validating reactive nitrogen chemistry theory in the troposphere.     

基于OMI数据分析青藏高原周边对流层低层臭氧的分布特征

提出一种利用地形海拔落差以及臭氧总量差来估算对流层低层大气臭氧浓度的方法.根据搭载于美国宇航局Aura卫星上的臭氧监测仪(OMI)提供的臭氧总量日观测数据,利用该方法计算出青藏高原与其周边地区四川盆地及印度北部的地形海拔落差及臭氧总量差,进一步分析了该地区低层大气臭氧的分布特征.结果表明:青藏高原周边地区对流层低层大气臭氧分布呈明显的季节变化,且低层大气臭氧分布有南北差异,南部臭氧含量高于北部.     

Detection of bromine monoxide in a volcanic plume

The emission of volcanic gases usually precedes eruptive activity, providing both a warning signal and an indication of the nature of the lava soon to be erupted. Additionally, volcanic emissions are a significant source of gases and particles to the atmosphere, influencing tropospheric and stratospheric trace-gas budgets. Despite some halogen species having been measured in volcanic plumes (mainly HCl and HF), little is known about bromine compounds and, in particular, gas-phase reactive bromine species. Such species are especially important in the stratosphere, as reactive bromine-despite being two orders of magnitude less abundant than chlorine-accounts for about one-third of halogen-catalysed ozone depletion. In the troposphere, bromine-catalysed complete ozone destruction has been observed to occur regularly during spring in the polar boundary layers as well as in the troposphere above the Dead Sea basin. Here we report observations of BrO and SO2 abundances in the plume of the Soufrière Hills volcano (Montserrat) in May 2002 by ground-based multi-axis differential optical absorption spectroscopy. Our estimate of BrO emission leads us to conclude that local ozone depletion and small ozone 'holes' may occur in the vicinity of active volcanoes, and that the amount of bromine emitted from volcanoes might be sufficiently large to play a role not only in the stratosphere, but also in tropospheric chemistry.