深对流云输送对于对流层O3、NOx在分析的作用

利用一个冰雹云模式与云化学输送模块耦合而成的三维对流云化学／输送模式, 研究对流云对重要的大气污染物臭氧 （Ｏ３）、氮氧化物 （ＮＯｘ, 包括ＮＯ 和ＮＯ２） 的输送作用。模式较好地体现了一个单体积云的发展过程及其特征。云化学／输送模式的结果表明, 云内强烈的垂直输送能在３０ ｍ ｉｎ 左右, 把低层低体积分数的Ｏ３和高体积分数的ＮＯ２快速、有效地输送到对流层的上部, 造成化学物种的再分布。而在云顶附近, 由于对流穿透了对流层的顶部,造成了上层高体积分数Ｏ３的向下侵入,说明云的对流活动除了能把边界层内的污染物向上输送, 其夹卷作用还可以造成平流层和对流层化学物质的交换。     

对流云中冰相过程的三维数值模拟 Ⅱ：繁生过程作用

在可压缩三维冷云数值模式里对冰晶繁生过程进行了参数化,显式考虑了过冷滴冻结破裂和Hallett-Mossop两个繁生机制,并对冰晶浓度进行了订正。对暖底孤立积云的模拟实例表明繁生作用对对流系统宏观特征没有显著改变,地面总降水略有增加,最大雨强增大且时间提前。繁生过程的主要作用是改变了云的微物理结构特征,使云中冰化时间提早,冰化程度大大加强,引起云上部增暖并抬高云顶。在所考虑的两个繁生机制中,冻结破裂繁生机制是引起微物理结构发生变化的主要过程。还对各冰相微物理过程的相对作用进行了分析。     

利用卫星资料分析对流层臭氧柱总量分布特征及其可能的原因

利用卫星资料计算得到的对流层臭氧柱总量数据分析了近20年来全球对流层臭氧柱总量的全球分布特征,并对我国对流层臭氧的季节变化做了研究。利用对流层污染测量仪（MOPITT）的CO和全球臭氧监测仪（GOME）和大气制图扫描成像吸收光谱仪（SCIAMACHY）的NO2数据分析了关于对流层臭氧的分布特征及其原因。得出中高纬度地区对流层臭氧浓度存在规律的年内变化,对流层臭氧高浓度值的分布及变化与人类活动有密切关切。     

对流云中冰相过程的三维数值模拟——Ⅱ:繁生过程作用

在可压缩三维冷云数值模式里对冰晶繁生过程进行了参数化,显式考虑了过冷滴冻结破裂和Hallett-Mossop两个繁生机制,并对冰晶浓度进行了订正。对暖底孤立积云的模拟实例表明繁生作用对对流系统宏观特征没有显著改变,地面总降水略有增加,最大雨强增大且时间提前。繁生过程的主要作用是改变了云的微物理结构特征,使云中冰化时间提早,冰化程度大大加强,引起云上部增暖并抬高云顶。在所考虑的两个繁生机制中,冻结破裂繁生机制是引起微物理结构发生变化的主要过程。还对各冰相微物理过程的相对作用进行了分析。     

一次深对流过程对不同溶解度大气化学气体成分垂直再分布作用的模拟

结合MEIC大气污染物排放源清单,利用耦合了大气化学模式的中尺度气象数值模式WRF-Chem,对2016年5月6日广东地区一次深对流天气过程及其大气化学气体成分变化进行模拟,着重研究深对流系统对大气化学气体成分再分布的影响。结果表明:数值模拟较真实地再现了这次深对流天气过程中大气污染物的时空分布特征。通过计算,评估了这次对流降水对不同溶解度的大气污染气体的湿清除效率,发现湿清除过程对低溶解度大气污染气体CO、NO_2和O_3的湿清除效率几乎可以忽略不计,而对SO_2、H_2O_2和HNO_3的湿清除效率则分别达到50.8%、98.6%和38.2%。随着溶解度的增大,清除效率并不一定增大,这是因为大气物理和化学过程共同影响着气体污染物的清除效率。     

中国地区对流层臭氧变化和分布的数值研究

利用三维中尺度非静力模式ＭＭ５和化学模式,对１９９４年８月１６～１８日,１９９５年１月７～９日冬夏两个不同时期中国大陆大气对流层臭氧及其前体物质的分布进行了数值模拟。同时深入地分析了青藏高原地区夏季对流层臭氧的分布。模拟结果地面臭氧和ＮＯｘ的分布与观测结果基本一致,人类活动和光化过程是决定地面臭氧和ＮＯｘ的主要因子。对流层臭氧浓度的分布与气流的辐合辐散存在较好的对应关系,辐合区臭氧浓度较高,辐散区臭氧浓度较低。夏季,青藏高原中低空存在很强的辐合气流,使周边臭氧向高原辐合;而高原高空,受南亚高压控制存在很强的反气旋环流,臭氧由高原向周边辐散。冬季,受西风气流控制,臭氧分布表征大尺度特征。西风急流区臭氧浓度偏低,而急流两侧臭氧浓度偏高。     

北半球春季大气臭氧年际变化特征及其对大气温度和环流场的影响

北半球春季中高纬地区大气臭氧总量具有明显的年际变化，正（负）异常时，与其相应对的流层平均温度、位势高度场均为负（正）异常，平流层异常情况相反，北大西洋地区大气臭氧年际异常与其他地区正好相反，这是区别大气臭氧与其他温室气体影响的重要标志。     

平流层臭氧季节变化的动力和光化学作用之比较

1992年到2005年的HALOE资料显示, 在臭氧光化损耗中, ClOx 和NOx 的贡献大小和作用位置有所差异。SOCRATES3模式模拟表明, 两半球夏季高纬极区的臭氧减少, 主要是NOx的化学贡献; 北极春季和南极冬季副极地臭氧的变化, 主要是动力输送引起。南、北极春季臭氧减少的化学机制也有所不同, 南极春季的臭氧耗损包括极区内ClOx 的异相化学作用和副极区NOx的化学作用; 北极春季的臭氧耗损主要以NOx 和ClOx 的气相化学作用为主, 其中NOx 的作用更大。动力和光化学在臭氧变化中的贡献表明, 整个中低平流层及低纬平流层高层的动力输送贡献可达到45%, 而高纬平流层中上层, 化学作用贡献在65%以上。     

青藏高原周边对流层顶的时空分布、热力成因及动力效应分析

利用多套、多种再分析资料的逐日气候平均场,通过对比分析,揭示了青藏高原周边区域对流层顶分布及其季节演变的独特特征,并分析了其热力成因以及气候学效应。结果表明,与同纬度的落矶山和太平洋地区相比,青藏高原及伊朗高原区域对流层顶高度的冬夏变化幅度更大。冬季副热带对流层顶断裂带（热带对流层顶与极地对流层顶之间高度剧烈变化的过渡带）位于青藏与伊朗两个高原上空,春季开始两个高原上空对流层顶抬升迅速,夏季最高可超过热带对流层顶的高度（超过100 hPa）,成为同纬度甚至全球对流层顶最高点。青藏与伊朗两个高原上空对流层顶的剧烈抬高,对应两个高原上空大气气柱比同纬度明显偏暖,同时伴随着青藏与伊朗两个高原上空位势涡度值的明显降低。因此,在青藏与伊朗两个高原区域,由春至夏等熵面强烈下凹,同时等位涡面剧烈抬升;夏季时等位涡面及对流层顶断裂带在青藏高原北部成近乎上下垂直分布,与南北倾斜分布的等位温面接近正交分布。这种特征与夏季同纬度其他地区相对平缓的对流层顶断裂带、等位涡面以及等熵面的经向分布形成强烈对比。进一步研究发现,青藏与伊朗两个高原上空由春至夏迅速发展的强大热源是引起上述对流层顶变化特征的主要原因。不同的是,青藏高原上空主要由发展强烈的对流凝结潜热所主导,而伊朗高原上空则主要由绝热下沉加热引起;此外,由春季至夏季,随着青藏高原地区对流层顶与等熵面剧烈相交分布的形成,南亚高压也逐步控制青藏高原上空,在南亚高压东缘盛行的偏北气流作用下,中高纬度平流层的高位涡空气得以在青藏高原东缘及东亚地区沿剧烈倾斜的等熵面被输送到较低纬度的对流层。与降水的季节演变对比可知,平流层高位涡输送的出现、加强和减弱与夏季降水的发展、加强与减弱成同步对应关系。从而证实了青藏高原影响夏季东亚地区形成独特气候格局的事实,说明在这种影响过程中,平流层-对流层动力相互作用过程不可忽视。      

对流云对大气气溶胶和相对湿度变化响应的数值模拟

利用二维面对称分档云模式研究了气溶胶颗粒物浓度和尺度谱分布对混合相对流云微物理过程和降水的影响, 并重点讨论了气溶胶效应随环境相对湿度的变化。结果表明, 在初始热力和动力条件相同的情况下, 相对清洁的海洋性云在发展和成熟阶段能更有效地产生雨滴、 冰晶和霰粒, 形成更强的雷达反射率。随着气溶胶浓度增加, 比如在本文模拟的污染大陆性云中, 气溶胶粒子数浓度的增加限制云滴增长, 不利于降水粒子的形成。模拟结果也发现, 环境相对湿度对气溶胶效应有显著影响, 即当地面相对湿度从50%增大到70%时, 所模拟的云从浅对流泡发展为深对流云; 气溶胶对云微物理特性和降水的影响在干空气中较小, 但在湿空气中表现非常显著, 这与前人结果一致。随着相对湿度的增加, 冰相粒子出现的时间提前, 增长加快, 云砧范围扩大, 但相对来说, 降水起始时间对相对湿度的变化比气溶胶更敏感。     

Formulation and Evaluation of IMS, an Interactive Three-Dimensional Tropospheric Chemical Transport Model 2. Model Chemistry and Comparison of Modelled CH4, CO, and O3 with Surface Measurements

In part two of this series of papers on the IMS model, we present the chemistry reaction mechanism usedand compare modelled CH₄, CO, and O₃ witha dataset of annual surface measurements. The modelled monthly and 24-hour mean tropospheric OH concentrationsrange between 5–22 × 10⁵ moleculescm^–3, indicating an annualaveraged OH concentration of about 10 × 10⁵ moleculescm^–3. This valueis close to the estimated 9.7 ± 0.6 × 10⁵ moleculescm^–3 calculated fromthe reaction of CH₃CCl₃ with OH radicals.Comparison with CH₄ generally shows good agreementbetween model and measurements, except for the site at Barrow where modelledwetland emission in the summer could be a factor 3 too high.For CO, the pronounced seasonality shown in the measurements is generally reproduced by the model; however, the modelled concentrations are lower thanthe measurements. This discrepancy may due to lower the CO emission,especially from biomass burning,used in the model compared with other studies.For O₃, good agreement between the model and measurements is seenat locations which are away from industrial regions. The maximum discrepancies between modelled results and measurementsat tropical and remote marine sites is about 5–10 ppbv,while the discrepancies canexceed 30 ppbv in the industrial regions.Comparisons in rural areas at European and American continental sites arehighly influenced by the local photochemicalproduction, which is difficult to model with a coarse global CTM.The very large variations of O₃ at these locations vary from about15–25 ppbv in Januaryto 55–65 ppbv in July–August. The observed annual O₃amplitude isabout 40 ppbv compared with about 20 ppbv in the model. An overall comparison of modelled O₃ with measurements shows thatthe O₃seasonal surface cycle is generally governed bythe relative importance of two key mechanisms that drivea springtime ozone maximum and asummertime ozone maximum.     

Formulation and Evaluation of IMS, an Interactive Three-Dimensional Tropospheric Chemical Transport Model 3. Comparison of Modelled C2–C5 Hydrocarbons with Surface Measurements

In part 3 of this series of papers on a new 3-D global troposphericchemical transport model, using an Integrated Modelling System (IMS), anevaluation of the model performance in simulating global distributions andseasonal variations for volatile organic compounds (VOCs) in the atmosphere,is presented. Comparisons of model OH concentrations with previous modelstudies show consistent modelled OH levels from the subtropics tomidlatitudes, while more discrepancies occur over the tropical lowlatitudes, with IMS predicting the highest levels of OH. The close agreementbetween modelled OH concentrations over midlatitudes, where high surfaceNO_xand VOC concentrations are also found, is indicative of the strongphotochemical coupling between NO_x, VOCs and O₃ overthese latitudes. IMSOH concentrations in the Northern Hemisphere (NH) midlatitudes during summerare generally lower than available measurements, implying that models ingeneral are underestimating OH levels at this location and time of year.Substantial differences between model OH concentrations over low latitudesclearly highlight areas of uncertainty between models. IMS OH concentrationsare the highest in general of the models compared, one possible reason isthat biogenic emissions of species such as isoprene and monoterpenes arehighest in IMS, leading to higher O₃ levels and hence higher OH.Generally, the IMS VOC concentrations show a similar seasonality to themeasurements at most locations. In general though, IMS tends to underestimatethe NH wintertime VOC maximum and overestimate the NH summertime VOCminimum. Such an overestimate in summer could be due to IMSunderestimating OH levels, or an overestimation of VOC emissions or possiblya problem with model transport, all of these possibilities are explored.Except for n-pentane, the model underprediction of a VOC maximum during theNH winter month strongly suggests a missing emission mechanism in the modelor an underestimate of an existing one. It is very likely that there is alack of time varying emission sources in the model to account for theseasonal change in emission behaviour such as increasing energy usage (e.g.,electricity and gas), road transportation, engine performance, and otheranthropogenic factors which show strong seasonal characteristics. Theanomalous overprediction of wintertime n-pentane compared with its closesummertime prediction with the measurements suggest that emissions in thiscase may be too high.     

微物理过程分档处理的三维对流云模式研究

在三维完全弹性冰雹云参数化模式动力框架和二维面对称分档模式(微物理过程分档处理)的基础上,建立粒子全分档的三维对流云分档模式.利用建立的分档模式对2000年6月29日美国堪萨斯州的一次超级单体风暴进行了模拟,并将模拟结果与三维冰雹云参数化模式的模拟结果作了对比.结果表明:分档模式可以较好地模拟出强对流云中两支上升气流,模拟得到的最大上升气流速度大于参数化模式;分档模式模拟得到的雷达回波强度、顶高和回波宽度更接近实测.     

The Radiative-Dynamical Effects of High Cloud on Global Ozone Distribution

Previous studies (e.g., Dessler et al., 1996; Haigh, 1984) have discussed the effect of cloud on modelled ozone distribution through changes in the radiative heating in the lower stratosphere. Here the relationship is investigated using an interactive chemical-radiative- transport 2D model. It is shown that, while similar cooling in the lower stratosphere due to high cloud is found, the effect on ozone is not as previously expected. The inclusion of high cloud is found to bring about a warming of the troposphere, resulting in a net heating in the lower stratosphere. This strengthens the circulation, leading to a decrease in total tropical ozone. Importantly, the effect of the cloud-induced temperature changes on heating rates does not combine linearly with the direct radiative effect of cloud changes. The possibility of a link between the high cloud increases and total ozone decreases observed in some regions during strong El Niño episodes is investigated. The possible impact on ozone of a global trend in high cloud cover is also discussed.     

当前对流层臭氧数值模式研究中的若干问题

对当前对流层臭氧(O3)数值模式研究中存在的若干问题以及需要重点研究的方向进行了评述,内容包括O3前体物的生态源及其模拟、对流层化学机制、大气化学研究中的气象模式以及大气化学模式与气象模式的相容性等.     

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。     

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.     

一次对流云团过程结构特征的观测和模拟研究

为了解2015年8月22日发生在北京东部的一次对流云团的生消演变过程及微物理特征,使用耦合了CAMS云微物理方案的WRF中尺度云分辨模式对此次过程进行数值模拟。由于研究的对流云团尺度较小,对时空分辨率要求较高,把LAPS(Local Analysis and Prediction System)局地分析和预报系统同化多源观测资料后输出的高分辨率的中尺度分析场作为模式的初始场。将模拟结果与FY-2F卫星、北京SA波段多普勒天气雷达、地面雨量站等观测资料进行对比分析。同时,研究了对流云团中的微物理含量分布,深入分析此次过程的降水机制。结果表明:模式能够较好地模拟出对流云团在生成、发展、成熟和消散的四个不同阶段的演变规律,整个对流云系的发展持续4 h左右,对北京有直接影响的对流单体的生命时长在1 h左右;模拟的自然云云带分布和演变规律、小尺度云团的尺度、位置、形状和垂直结构都与观测资料有较好的一致性;模式也能模拟出降水落区和量级及强中心的位置。此次对流云过程主要为冷暖混合云系结构,云中过冷水丰沛,降水机制以冷云降水为主,暖区供水云对降水的发展有促进作用,霰融化为雨滴是主要的成雨过程。