Removal of chlorofluorocarbons by increased mass exchange between the stratosphere and troposphere in a changing climate

Chlorofluorocarbons (CFCs), along with bromine compounds, have been unequivocally identified as being responsible for most of the anthropogenic destruction of stratospheric ozone. With curbs on emissions of these substances, the recovery of the ozone layer will depend on their removal from the atmosphere. As CFCs have no significant tropospheric removal process, but are rapidly photolysed above the lower stratosphere, the timescale for their removal is set mainly by the rate at which air is transported from the troposphere into the stratosphere. Using a global climate model we predict that, in response to the projected changes in greenhouse-gas concentrations during the first half of the twenty-first century, this rate of mass exchange will increase by 3% per decade. This increase is due to more vigorous extra-tropical planetary waves emanating from the troposphere. We estimate that this increase in mass exchange will accelerate the removal of CFCs to an extent that recovery to levels currently predicted for 2050 and 2080 will occur 5 and 10 years earlier, respectively.     

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。     

Detection of stratospheric ozone intrusions by windprofiler radars

Stratospheric ozone attenuates harmful ultraviolet radiation and protects the Earth's biosphere. Ozone is also of fundamental importance for the chemistry of the lowermost part of the atmosphere, the troposphere. At ground level, ozone is an important by-product of anthropogenic pollution, damaging forests and crops, and negatively affecting human health. Ozone is critical to the chemical and thermal balance of the troposphere because, via the formation of hydroxyl radicals, it controls the capacity of tropospheric air to oxidize and remove other pollutants. Moreover, ozone is an important greenhouse gas, particularly in the upper troposphere. Although photochemistry in the lower troposphere is the major source of tropospheric ozone, the stratosphere-troposphere transport of ozone is important to the overall climatology, budget and long-term trends of tropospheric ozone. Stratospheric intrusion events, however, are still poorly understood. Here we introduce the use of modern windprofiler radars to assist in such transport investigations. By hourly monitoring the radar-derived tropopause height in combination with a series of frequent ozonesonde balloon launches, we find numerous intrusions of ozone from the stratosphere into the troposphere in southeastern Canada. On some occasions, ozone is dispersed at altitudes of two to four kilometres, but on other occasions it reaches the ground, where it can dominate the ozone density variability. We observe rapid changes in radar tropopause height immediately preceding these intrusion events. Such changes therefore serve as a valuable diagnostic for the occurrence of ozone intrusion events. Our studies emphasize the impact that stratospheric ozone can have on tropospheric ozone, and show that windprofiler data can be used to infer the possibility of ozone intrusions, as well as better represent tropopause motions in association with stratosphere-troposphere transport.     

亚印太交汇区低纬上空不同层次大气臭氧的时空变化分析

 利用ECMWF 195709~200208共45a的多层臭氧质量混合比月平均资料,详细分析了亚印太交汇区(AIPO)低纬地带上空平流层、对流层各层次上臭氧浓度的分布特征.结果表明:①区域上空对流层、平流层及臭氧总量大尺度特征均显著,纬度带分布特征明显;②对流层和平流层臭氧各个季节变化趋势相反,平流层臭氧和臭氧总量各个季节变化趋势一致;同一层次夏季臭氧浓度变化趋势与其他3个季节变化趋势相反;③区域上空20~3hPa是臭氧浓度的高值区,50~30hPa臭氧平均变化幅度最大;④对流层臭氧距平变化在整个高度上较为一致,正、负距平随季节绕赤道做南、北半球摆动,且存在季节性突变;⑤赤道上空有明显从平流层上层随季节逐渐往较低层传播的臭氧正负距平现象.     

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.     

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。     

CMIP5模拟的平流层21世纪温度变化趋势

21世纪平流层气候变化主要由两个因素所决定,一个是臭氧层恢复造成的变暖,另一个是温室气体增加造成的变冷。针对在这两种相反的辐射效应作用下,平流层气温如何变化这一重要问题, 使用CMIP5未来情景模拟试验的结果, 对2006-2100年间的平流层温度的变化趋势进行分析。结果表明, 臭氧恢复的增温效应在平流层低层起主导作用, 而温室气体增加的冷却效应在平流层高层起主导作用, 因此, 平流层低层(70 hPa 以下)呈变暖趋势, 而平流层中高层呈变冷趋势。通过对包含完整平流层的气候模式(高顶模式)和只包含部分平流层的气候模式(低顶模式)预估的温度趋势的差异进行分析, 发现高顶模式预估的变暖趋势大于低顶模式的结果, 这意味着模式是否包含完整平流层有可能对预估的平流层和对流层未来气候变化有重要影响。     

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.     

Low European methyl chloroform emissions inferred from long-term atmospheric measurements

Methyl chloroform (CH3CCl3, 1,1,1,-trichloroethane) was used widely as a solvent before it was recognized to be an ozone-depleting substance and its phase-out was introduced under the Montreal Protocol. Subsequently, its atmospheric concentration has declined steadily and recent European methyl chloroform consumption and emissions were estimated to be less than 0.1 gigagrams per year. However, data from a short-term tropospheric measurement campaign (EXPORT) indicated that European methyl chloroform emissions could have been over 20 gigagrams in 2000 (ref. 6), almost doubling previously estimated global emissions. Such enhanced emissions would significantly affect results from the CH3CC13 method of deriving global abundances of hydroxyl radicals (OH) (refs 7-12)-the dominant reactive atmospheric chemical for removing trace gases related to air pollution, ozone depletion and the greenhouse effect. Here we use long-term, high-frequency data from Mace Head, Ireland and Jungfraujoch, Switzerland, to infer European methyl chloroform emissions. We find that European emission estimates declined from about 60 gigagrams per year in the mid-1990s to 0.3-1.4 and 1.9-3.4 gigagrams per year in 2000-03, based on Mace Head and Jungfraujoch data, respectively. Our European methyl chloroform emission estimates are therefore higher than calculated from consumption data, but are considerably lower than those derived from the EXPORT campaign in 2000 (ref. 6).     

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.     

Extensive halogen-mediated ozone destruction over the tropical Atlantic Ocean

Increasing tropospheric ozone levels over the past 150 years have led to a significant climate perturbation; the prediction of future trends in tropospheric ozone will require a full understanding of both its precursor emissions and its destruction processes. A large proportion of tropospheric ozone loss occurs in the tropical marine boundary layer and is thought to be driven primarily by high ozone photolysis rates in the presence of high concentrations of water vapour. A further reduction in the tropospheric ozone burden through bromine and iodine emitted from open-ocean marine sources has been postulated by numerical models, but thus far has not been verified by observations. Here we report eight months of spectroscopic measurements at the Cape Verde Observatory indicative of the ubiquitous daytime presence of bromine monoxide and iodine monoxide in the tropical marine boundary layer. A year-round data set of co-located in situ surface trace gas measurements made in conjunction with low-level aircraft observations shows that the mean daily observed ozone loss is approximately 50 per cent greater than that simulated by a global chemistry model using a classical photochemistry scheme that excludes halogen chemistry. We perform box model calculations that indicate that the observed halogen concentrations induce the extra ozone loss required for the models to match observations. Our results show that halogen chemistry has a significant and extensive influence on photochemical ozone loss in the tropical Atlantic Ocean boundary layer. The omission of halogen sources and their chemistry in atmospheric models may lead to significant errors in calculations of global ozone budgets, tropospheric oxidizing capacity and methane oxidation rates, both historically and in the future.     

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.     

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.     

Recent Northern Hemisphere tropical expansion primarily driven by black carbon and tropospheric ozone

Observational analyses have shown the width of the tropical belt increasing in recent decades as the world has warmed. This expansion is important because it is associated with shifts in large-scale atmospheric circulation and major climate zones. Although recent studies have attributed tropical expansion in the Southern Hemisphere to ozone depletion, the drivers of Northern Hemisphere expansion are not well known and the expansion has not so far been reproduced by climate models. Here we use a climate model with detailed aerosol physics to show that increases in heterogeneous warming agents--including black carbon aerosols and tropospheric ozone--are noticeably better than greenhouse gases at driving expansion, and can account for the observed summertime maximum in tropical expansion. Mechanistically, atmospheric heating from black carbon and tropospheric ozone has occurred at the mid-latitudes, generating a poleward shift of the tropospheric jet, thereby relocating the main division between tropical and temperate air masses. Although we still underestimate tropical expansion, the true aerosol forcing is poorly known and could also be underestimated. Thus, although the insensitivity of models needs further investigation, black carbon and tropospheric ozone, both of which are strongly influenced by human activities, are the most likely causes of observed Northern Hemisphere tropical expansion.     

Detection of human influence on sea-level pressure

Greenhouse gases and tropospheric sulphate aerosols--the main human influences on climate--have been shown to have had a detectable effect on surface air temperature, the temperature of the free troposphere and stratosphere and ocean temperature. Nevertheless, the question remains as to whether human influence is detectable in any variable other than temperature. Here we detect an influence of anthropogenic greenhouse gases and sulphate aerosols in observations of winter sea-level pressure (December to February), using combined simulations from four climate models. We find increases in sea-level pressure over the subtropical North Atlantic Ocean, southern Europe and North Africa, and decreases in the polar regions and the North Pacific Ocean, in response to human influence. Our analysis also indicates that the climate models substantially underestimate the magnitude of the sea-level pressure response. This discrepancy suggests that the upward trend in the North Atlantic Oscillation index (corresponding to strengthened westerlies in the North Atlantic region), as simulated in a number of global warming scenarios, may be too small, leading to an underestimation of the impacts of anthropogenic climate change on European climate.     

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.     

Enhancements in biologically effective ultraviolet radiation following volcanic eruptions.

Aerosols injected into the stratosphere by large volcanic eruptions may induce ozone destruction through processes including heterogeneous chemical reactions. The effect of ozone reductions on surface ultraviolet irradiation is not obvious, however, because aerosols also increase the reflection of sunlight. Here we use a radiative transfer model to estimate the changes in biologically effective ultraviolet radiation (UV-BE) at the Earth's surface produced by the El Chichón (1982) and Mount Pinatubo (1991) eruptions. We find that in both cases surface UV-BE intensity can increase because the effect of ozone depletion outweighs the increased scattering.     

大气臭氧垂直分布的非均匀结构

 对昆明地区2001年春季探测的臭氧分压廓线数据的非均匀结构进行了分析.采用结构函数和双曲分布函数建立自相似的标度律,进而描述臭氧垂直空间中的非均匀结构(如,间歇性、粗糙度、标度指数、功率谱指数、分数维等).计算结果表明:①臭氧分压垂直空间分布序列的分数维在1～2之间;功率谱指数为1～3.②在不同高度层上,对流层顶附近的分数维最大D=1.365;而对流层中的则最小D=1.205.③平流层臭氧分压的垂直间歇性强且粗糙;对流层顶附近的垂直间歇性弱又光滑,并存在着很强的奇异性.     

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.     

Surface ozone monitoring and background characteristics at Zhongshan Station over Antarctica

Seasonal variation in surface ozone and the relationship between the background ozone concentration and wind were evaluated at Zhongshan Station,Antarctica using 2008 data.The wind frequency from the station area was only 2%,while the prevailing wind frequency was much larger (79.2%).This indicates that the surface ozone observations were not affected by the human activities at the station,and therefore could be counted as background concentrations of surface ozone along Antarctic coast.The concentration of surface ozone shows a distinct annual variation with the yearly mean of 25.0 nmol mol-1 and the maximum in winter,the minimum in summer.The surface ozone concentration had a strong negative correlation with ultraviolet radiation,and the mean values during polar night were one to two times higher than those in summer.These results imply that photochemical destruction of ozone dominates over Antarctica.The ozone depletion events at Zhongshan Station were obviously related to lower temperatures and higher BrO concentrations.Backward trajectory analysis reveals that the ozone depletion events are predominately caused by the high BrO concentrations.