强对流天气对O3和CO的垂直输送作用

利用ACTIVE（aerosol and chemical transport in tropical convection）试验资料,取2006年1月20日澳大利亚北部达尔文岛附近发生的一次飑线强对流天气的AE17航次和2006年1月27日无对流天气的AE21航次飞行路径中的探测资料,对澳大利亚达尔文地区夏季风盛行期间发生的有无强对流发生时O₃和CO浓度垂直分布变化进行对比,考察强对流性天气发生对O₃和CO浓度垂直输送作用。深对流云内强烈的垂直上升运动将O₃和CO等化学气体携带输送至对流层上部并在对流层顶堆积,从而在对流层上部产生浓度峰值。当有强对流发生,飞机进入对流云上层时,O₃浓度和CO浓度升高,O₃和CO浓度变率增大,在对流层上部浓度出现峰值;当飞机飞出对流云时,O₃和CO浓度相对较低,在对流云外出现谷值。在无对流发生的条件下O₃和CO浓度相对较小,浓度变率也较小,无峰值产生。分析表明:O₃和CO浓度分布不仅与强对流的垂直输送作用关系密切,且与气象要素垂直和水平分布以及动力输送过程密切相关。     

On the variability and correlation of surface ozone and carbon monoxide observed in Hong Kong using trajectory and regression analyses

This paper investigates, the variability and correlation of surface ozone (Os) and carbon monoxide (CO) observed at Cape D'Aguilar in Hong Kong from 1 January 1994 to 31 December 1995. Statistical analysis shows that the average O3 and CO mixing ratios during the two years are 32±17ppbv and 305±191 ppbv, respectively. The O3/CO ratio ranges from 0.05 to 0.6 ppbv/ppbv with its frequency peaking at 0.15. The raw dataset is divided into six groups using backward trajectory and cluster analyses. For data assigned to the same trajectory type, three groups are further sorted out based on CO and NOX mixing ratios. The correlation coefficients and slopes of O3/CO for the 18 groups are calculated using linear regression analysis. Finally, five kinds of air masses with different chemical features are identified: continental background (CB), marine background (MB), regional polluted continental (RPC), perturbed marine (P*M), and local polluted (LP) air masses. Further studies indicate that O3 and CO in the conti     

The Measurement of Active Chlorine in the Atmosphere by Chemical Amplification

Chemical amplification, CA, a method commonly used for the detection of peroxy radicals, HO₂ and RO₂, was found to be sensitive towards ClOx (Cl+ClO+OClO) as well. ClOx is reduced by NO to Cl atoms which react with carbon monoxide in the presence of O₂. The reaction sequence thus initiated oxidizes CO to CO₂ and NO to NO₂, with a chain length of 300 ± 60. This allows the atmospheric ClOx content to be measured under ambient conditions with a detection limit of better than 1 ppt. In parallel peroxy radicals are indicated with a chain length of 160 ± 15. Chemical amplification is not specific and does not indicate which radical chain it is seeing. Identification relies solely on plausibility. During the ARCtic Tropospheric Ozone Chemistry (ARCTOC) campaign in spring 1995 and 1996 the CA technique was used at Ny-Ålesund. ClOx at mixing ratios of up to 2 ppt were found in the boundary layer under certain conditions. The low concentrations of ClOx indicate that the arctic boundary ozone depletion is mainly driven by bromine.     

云南两次中尺度对流雷暴系统演变和地闪特征

在利用NCEP/NCAR再分析资料诊断分析2010年9月21—23日中尺度对流雷暴系统形成的环流背景基础上,通过云南省闪电定位系统地闪监测资料和FY-2E卫星云图资料的同步叠加, 分析两个中尺度雷暴系统的演变和地闪特征。结果表明:台风凡亚比 (1011) 西行减弱的热带低压为中尺度对流雷暴系统提供有利的暖湿和抬升动力环流背景,促使中尺度弧状对流云带、中尺度雷暴云团和中尺度对流复合体生成和发展。雷暴云团结构和地闪活动空间分布不均匀并随时间变化,且正、负地闪频数与云顶亮温 (TBB) 相关,当TBB降低和等值线密度变大,雷暴云团发展,低TBB中心偏于云团的前部云区,负地闪频数剧增;当TBB达最低值时,雷暴云团成熟,负地闪频数达峰值,正地闪出现;当TBB升高且等值线密度变小时,雷暴云团减弱,低TBB中心靠近云团中心,负地闪频数迅速减小,正地闪频数达到峰值;密集的负地闪出现在雷暴云团前部大的TBB梯度区和TBB不大于-56℃的低值中心附近,正地闪分散在TBB不大于-56℃的低值中心附近,偏于负地闪区域后部发生。     

一次强暴雨过程地闪活动特征与中尺度对流系统和强降水的关系

利用2007年8月8日18时至9日02时发生在陕西关中强暴雨期间的地闪、卫星TBB、雷达回波和地面加密降水资料,通过统计和对比分析的方法,分析了地闪活动特征及其与中尺度对流系统（MCS）和强降水的关系。地闪活动特征分析显示,暴雨过程中负地闪占绝对优势,为总地闪的97.7%。负闪频数和总闪频数的逐时演变趋势完全一致且呈现两峰一谷的趋势,正闪频数的变化呈现三峰两谷的趋势,但是正闪频数最大值与总闪、负闪频数峰值时间一致。负闪活跃期正负闪6 min演变均表现为多峰结构,正闪的波峰提前于负闪的波峰12 min。负闪频数变化和MCS、雷达反射率因子演变对比分析表明,负闪发生区是未来对流云团和对流发展加强区,负闪频数密集区位于对流云团前部TBB等值线密集区,负闪频数的急剧增加意味着未来对流系统的猛烈发展;负闪主要出现在回波强度大于40 dBz的区域,正闪则落到强回波中心两侧30～40 dBz的回波区,中尺度对流系统快速发展加强期,负闪密集区位于回波单体的前沿,中尺度系统发展稳定少动期,负闪大部分集中在各对流单体的强回波中心附近。对比分析地闪与暴雨发生发展的关系可见,地闪的发生和急剧增加对暴雨发生和发展加强有很好指示意义,初闪的发生提前于强降水发生,地闪急剧增加与降水强度猛增密切关联,负地闪发生密集区是未来强降水发生区。     

Regional studies of potential carbon monoxide sources based on space shuttle and aircraft measurements

Carbon monoxide measurements made from the space shuttle show maxima over South America, central Africa, the eastern Mediterranean, and China. The maxima appear to be associated with either concomitant or prior convection in the air masses which carries boundary layer air into the upper troposphere. Previous aircraft measurements of carbon monoxide and ozone over South America are shown to be consistent with this view. In the tropics the three regions of long-term mean rising motion, which form part of the Walker circulation, are associated with elevated carbon monoxide.     

Determination of Dominant Pathways in Chemical Reaction Systems: An Algorithm and Its Application to Stratospheric Chemistry

The analysis of complex chemical reaction systems is frequently complicatedbecause of the coexistence of fast cyclic reaction sequences and slower pathways that yield a net production or destruction of a certain species of interest.An algorithm for the determination of both these types of reaction sequences (in a given reaction system) is presented. Under the assumption that reaction rates are known, it finds the mostimportant pathways by solving a linear optimization problem for each of them.This algorithm may be used as a tool for the interpretation of chemical model runs.For illustration, it is applied to examples in stratospheric chemistry, including the determination of catalytic ozone destruction cycles.     

On the Role of Lightning NOx in the Formation of Tropospheric Ozone Plumes: A Global Model Perspective

A series of ozone transects measured each year from 1987 to 1990 over thewestern Pacific and eastern Indian oceans between mid-November andmid-Decembershows a prominent ozone maximum reaching 50–80 ppbv between 5 and 10 kmin the 20° S–40° S latitude band. This maximum contrasts with ozonemixing ratios lower than20 ppbv measured at the same altitudes in equatorial regions. Analyses witha globalchemical transport model suggest that these elevated ozone values are part ofa large-scale tropospheric ozone plume extending from Africa to the western Pacific acrosstheIndian ocean. These plumes occur several months after the peak in biomassburninginfluence and during a period of high lightning activity in the SouthernHemispheretropical belt. The composition and geographical extent of these plumes aresimilar to theozone layers previously encountered during the biomass burning season in thisregion.Our model results suggest that production of nitrogen oxides from lightningstrokes sustains the NO_x (= NO+NO₂) levels and the ozonephotochemical productionrequired in the upper troposphere to form these persistent elevated ozonelayers emanating from biomass burning regions.     

Segregation and Interpretation of Ozone and Carbon Monoxide Measurements by Air Mass Origin at the TOR Station Mace Head, Ireland from 1987 to 1995

Three independent methods have been used to sort the ozone, carbonmonoxide, and other radiatively important trace gases measured at Mace Head,Ireland, and thereby distinguish clean air masses transported over the NorthAtlantic from the more polluted air masses which have recently travelledfrom the European continent. Over the period April 1987–June 1995 theNorthern Hemisphere surface ozone baseline concentrations exhibited a meanconcentration of 34.8 ppb, with a small positive trend (+0.19 ppbyr^-1), while the corresponding trend in air originating fromthe polluted European areas was negative (–0.39 ppbyr^-1). Carbon monoxide measurements from March 1990 toDecember 1994 showed negative trends for both the unpolluted (–0.17ppb yr^-1) and polluted data (–13.6 ppbyr^-1). Overall the continent of Europe was shown to be a smallnet sink of 2.6 ppb for all occasions when European air was transported tothe North Atlantic.     

A numerical study of tropospheric ozone in the springtime in East Asia

The Models-3 Community Multi-scale Air Quality modeling system (CMAQ)coupled with the Regional Atmospheric Modeling System (RAMS)is applied to East Asia to study the transport and photochemical transformation of tropospheric ozone in March 1998．The calculated mixing ratios of ozone and carbon monoxide are compared with ground 1evel observations at three remote sites in Japan and it is found that the model reproduces the observed features very well．Examination of several high episodes of ozone and carbon monoxide indicates that these elevated levels are found in association with continental outflow,demonstrating the critical role of the rapid transport of carbon monoxide and other ozone precursors from the continental boundary layer．In comparison with available ozonesonde data,it is found that the model-calculated ozone concentrations are generally in good agreement with the measurements,and the stratospheric contribution to surface ozone mixing ratios is quite limited．     

Dynamical and Chemical Features of a Cutoff Low over Northeast China in July 2007: Results from Satellite Measurements and Reanalysis

The European Centre for Medium-Range Weather Forecasts Re-Analysis Interim (ERA-Interim) meteorology and measurements from the Microwave Limb Sounder, High Resolution Dynamics Limb Sounder, and Ozone Monitoring Instrument onboard the Earth Observing System Aura satellite were applied to analyze the dynamical and chemical features of a cutoff low (COL) event over northeast China in early July 2007. The results showed the polar stratospheric origin of an upper-level warm-core cyclone at 100--300 hPa, associated with a funnel-shaped tropopause intruding into the mid-troposphere just above the COL center. The impacts of the stratospheric intrusion on both column ozone and ozone profiles were investigated using satellite measurements. When the intensity of the COL peaked on 10 July 2007, the total column ozone (TCO) increase reached a maximum (40--70 DU). This could be dynamically attributed to both the descent of the tropopause (～75%) and the downward transport of stratospheric ozone across the tropopause (～25%). Analysis of the tropospheric ozone profiles provided evidence for irreversible transport/mixing of ozone-rich stratospheric air across the tropopause near the upper-level front region ahead of the COL center. This ozone intrusion underwent downstream transport by the upper tropospheric winds, leading to further increase in TCO by 12--16 DU over broad regions extending from east China toward the northern Japan Sea via South Korea. Meteorological analysis also showed the precedence of the stratospheric intrusion ahead of the development of cyclones in the middle and lower troposphere.     

The distribution of light nonmethane hydrocarbons over the mid-Atlantic: Results of the Polarstern cruise ANT VII/1

During the cruise ANT VII/1 (September/October 1988) of the German research vessel Polarstern the latitudinal distributions of several nonmethane hydrocarbons were measured over the Atlantic between 45°N and 30°S by in-situ gas chromatography.On the average, the highest mixing ratios of ethane, propane, i- and n-butane, ethene and acetylene were observed in the Northern Hemisphere around 40° N and just north of the intertropical convergence zone, respectively. South of the equator, a bulge in the mixing ratios of ethane and acetylene was observed indicating aged biomass burning emissions. This observation coincided with enhanced tropospheric ozone found in this region at this season. On the average ethane and acetylene mixing ratios were around 500 and 100 ppt, respectively, whereas the levels of the other NMHC were in the range of some ppt up to 100 ppt.compared with the results of the cruise ANT V/5 (March/April, 1987), the ethane mixing ratios in September/October proved to be a factor of 3 lower in the Northern Hemisphere and a factor of 2 higher in the Southern Hemisphere, probably due to seasonal effects. Possible causes are the higher OH radical concentrations in summer, which result in a faster removal of ethane or stronger emission from biomass burning which also peaks in the dry season.The relative pattern of the hydrocarbons just north of the ITCZ was very similar for both measurement series. In this region, the NMHC were advected by long-range transport from the continent, whereas generally the ocean itself acts as a major NMHC source. This is supported by the results of a balance calculation between oceanic emissions and atmospheric removal rates.     

An Algorithm for the Determination of All Significant Pathways in Chemical Reaction Systems

When the output of a complex chemical model is analysed, a typical topic isthe determination of pathways, i.e., reaction sequences, that produce ordestroy a chemical species of interest.A representative example is the investigation of catalytic ozone destruction cycles in the stratosphere.An algorithm for the automatic determination of pathways in any given reactionsystem is presented. Under the assumption that reaction rates are known, it finds all significant pathways, i.e., all pathways with a rate above a prescribed threshold.The algorithm forms pathways step by step, starting from single reactions.The chemical species in the system are consecutively considered as `branching points'.For every branching-point species, each pathway producing it is connected witheach pathway consuming it.Rates proportional to `branching probabilities' are calculated.Pathways with a rate that is smaller than a prescribed threshold arediscarded.If a newly formed pathway contains sub-pathways, e.g., null cycles, it is split into these simpler pathways.In order to demonstrate the performance of the algorithm, it has been applied to the determination of catalytic ozone destruction cycles and methaneoxidation pathways in the stratosphere.     

Numerical Simulation Study on the Impacts of Tropospheric O3 and CO2 Concentration Changes on Winter Wheat. Part II: Simulation Results and Analyses

With the rapid development of industrialization and urbanization, the enrichment of tropospheric ozone and carbon dioxide concentration at striking rates has caused effects on biosphere, especially on crops. It is generally accepted that the increase of CO2 concentration will have obverse effects on plant productivity while ozone is reported as the air pollutant most damaging to agricultural crops and other plants. The Model of Carbon and Nitrogen Biogeochemistry in Agroecosystems (DNDC) was adapted to evaluate simultaneously impacts of climate change on winter wheat. Growth development and yield formation of winter wheat under different O3 and CO2 concentration conditions are simulated with the improved DNDC model whose structure has been described in another paper. Through adjusting the DNDC model applicability, winter wheat growth and development in Gucheng Station were simulated well in 1993 and 1999, which is in favor of modifying the model further. The model was validated against experiment observation, including development stage data, leaf area index, each organ biomass, and total aboveground biomass. Sensitivity tests demonstrated that the simulated results in development stage and biomass were sensitive to temperature change. The main conclusions of the paper are the following: 1) The growth and yield of winter wheat under CO2 concentration of 500 ppmv, 700 ppmv and the current ozone concentration are simulated respectively by the model. The results are well fitted with the observed data of OTCs experiments. The results show that increase of CO2 concentration may improve the growth of winter wheat and elevate the yield. 2) The growth and yield of winter wheat under O3 concentration of 50 ppbv, 100 ppbv, 200 ppbv and the based concentration CO2 are simulated respectively by the model. The simulated curves of stem, leaf, and spike organs growth as well as leaf area index are well accounted with the observed data. The results reveal that ozone has negative e ects on the growth and yield of winter wheat. Ozone accelerates the process of leaf senescence and causes yield loss. Under very high ozone concentration, crops are damaged dramatically and even dead. 3) At last, by the model possible effects of air temperature change and combined effects of O3 and CO2 are estimated respectively. The results show that doubled CO2 concentration may alleviate negative effect of O3 on biomass and yield of winter wheat when ozone concentration is about 70-80 ppbv. The obverse effects of CO2 are less than the adverse effects of O3 when the concentration of ozone is up to 100 ppbv. Future work should determine whether it can be applied to other species by adjusting the values of related parameters, and whether the model can be adapted to predict ozone e ects on crops in farmland environment.     

Evolution of the Total Lightning Activity in a Leading-Line and Trailing Stratiform Mesoscale Convective System over Beijing

Data from the Beijing SAFIR 3000 lightning detection system and Doppler radar provided some insights into the three-dimensional lightning structure and evolution of a leading-line and trailing-stratiform (LLTS) mesoscale convective system (MCS) over Beijing on 31 July 2007. Most of the lightning in the LLTS-MCS was intracloud (IC) lightning, while the mean ratio of positive cloud-to-ground (+CG) lightning to -CG lightning was 1:4, which was higher than the average value from previous studies. The majority of CG lightning occurred in the convective region of the radar echo, particularly at the leading edge of the front. Little IC lightning and little +CG lightning occurred in the stratiform region. The distribution of the CG lightning indicated that the storm had a tilted dipole structure given the wind shear or the tripole charge structure. During the storm’s development, most of the IC lightning occurred at an altitude of ～9.5 km; the lightning rate reached its maximum at 10.5 km, the altitude of IC lightning in the mature stage of the storm. When the thunderstorm began to dissipate, the altitude of the IC lightning decreased gradually. The spatial distribution of lightning was well correlated with the rainfall on the ground, although the peak value of rainfall appeared 75 min later than the peak lightning rate.     

Trace gas measurements during aircraft flights in the tropopause region over Europe and North Africa

During aircraft flights in May 1981 from Munich (40°N) to north of the Spitsbergen Islands (82°N) and to Monrovia, Liberia (6°N), air samples were obtained in the altitude range of 8 to 11 km and during the ascents and descents near the airports. These samples have been analyzed for the trace gas mixing ratios of CH₄, CO and N₂O. The results of these analyses are presented and discussed.The results provide new evidence of tropospheric-stratospheric exchange events in the vicinity of the subpolar and subtropical tropopause foldings and possibly show a case of transport of CO-enriched air in the upper troposphere above the North Atlantic Ocean.     

Convective Redistribution of Ozone and Oxides of Nitrogen in the Troposphere over Europe in Summer and Fall

The fluxes of ozone and NO_x out of the atmospheric boundary layer (ABL) over Europe are calculated in a mesoscale chemical transport model (MCT) and compared with the net chemical production or destruction of ozone and the emissions of precursors within the ABL for two 10 days' periods which had quite different synoptic situations and levels of photochemical activity (1–10 July 1991 (JUL91) and 26 October–4 November 1994 (ON94)). Over the European continent, about 8% of the NO_x emissions were brought from the ABL to the free troposphere as NO_x, while about 15% of the NO_x emissions were brought to the free troposphere as NO_y–NO_x, i.e. as PAN or HNO₃. The convection dominates over the synoptic scale vertical advection as a transport mechanism both for NO_x and NO_y out of the boundary layer in the summertime high pressure situation (JUL91), while in the fall situation (ON94) the convective part was calculated to be the smallest. NO_x was almost completely transformed to NO_y–NO_x or removed within the ABL. Also for NO_y the major part of the atmospheric cycle is confined to the ABL both for JUL91 and ON94. The vertical transport time out of the ABL is of the order of 100h both for the total model domain and over the European continent. The net convective exchange of ozone from the ABL is not a dominant process for the amount of ozone in the ABL averaged over 10 days and the whole domain, but convection reduces the maximum ozone concentration in episodes significantly. The ozone producing efficiency of NO_x is calculated to increase with height to typically 15–20 in the upper half of the troposphere from around 5 in the ABL, but in the middle free troposphere the concentration of NO_x is often too low to cause net chemical formation of ozone there.     

近地层臭氧对我国树木生产力和作物产量的影响:进展与展望

大气污染严重威胁了我国陆地生态系统的固碳能力,但随着减污降碳协同治理的快速推进,减缓大气污染将有利于提升陆地碳汇,并切实推动碳达峰碳中和目标的实现。为了更好地理解大气污染与生态系统固碳的关系,本文以主要空气污染物臭氧（O₃）为例,基于田间控制实验的整合分析、剂量响应关系及机理模型三种评估方法综述了近地层O₃污染对植被碳固定影响的最新进展。尽管不同作物种类以及品种、不同功能型木本植物对O₃的响应有着显著的差异,且各种方法的评估结果也不尽相同,但目前O₃浓度造成我国粮食作物减产、森林生产力降低已是不争的事实。持续升高的O₃浓度将严重威胁我国陆地生态系统的固碳能力。利用我国作物和树木的O₃剂量响应方程进行评估的结果表明,在CO₂减排和O₃污染协同治理下,预计2060年我国树木生物量和作物产量将比当前显著提高,增加陆地生态系统碳汇,助力碳中和目标。最后,对如何提高O₃污染环境下植物固碳能力也进行了展望。     

三维对流云对大气光化学组分的再分布作用及其化学效应

利用一个三维的冰雹云模式与化学组分输送模块耦合，得到云输送引起大气光化学组分的再分布，然后用一个包含详细气相化学反应机制的箱模式研究了云输送引起的气相体积分数的变化及其对大气化学系统产生的影响。结果表明，云输送后O3体积分数大于无云个例，但其后两天内两者的变化趋势相差不大；HNO3、NO2、NO3、PAN等的体积分数均明显高于无云个例，分别增长了87％、70％、62％和49％，其中NO2体积分数的增加主要由于云输送造成，而NO3、HNO3、PAN主要是输送对化学扰动的结果。两天内OH和HO2自由基体积分数比无云个例平均增长了13％和11％。