我国北方地区对流层中下层臭氧收支

为了揭示我国北方地区对流层中下层臭氧(O₃) 的形成机理以及周边地区的污染输送对我国北方地区对流层中下层O₃收支的影响, 在与外场观测数据比较分析的基础上, 利用全球化学输送模式(MOZART-2) 采用收支分析方法定量分析了影响我国北方地区对流层中下层O₃的各个物理化学过程。结果表明:我国北方地区对流层下层O₃最重要的来源是光化学生成作用, 约占总来源的58.3%(41.5 Tg), 光化学生成反应中HO₂对于O₃生成的贡献最大; 最大的汇是干沉降过程, 约占总汇的43.2%(26.2Tg); 水平净输送作用对我国北方地区对流层中下层O₃收支的影响非常大, 在我国北方地区对流层下层, 41.6%左右的O₃来自水平净输送, 随高度增加, 水平输送影响增大, 我国北方地区对流层中层大约81.5%的O₃来自水平净输送。     

Airborne measurements of turbulent trace gas fluxes and analysis of eddy structure in the convective boundary layer over complex terrain

Using the new high-frequency measurement equipment of the research aircraft DO 128, which is described in detail, turbulent vertical fluxes of ozone and nitric oxide have been calculated from data sampled during the ESCOMPTE program in the south of France. Based on airborne turbulence measurements, radiosonde data and surface energy balance measurements, the convective boundary layer (CBL) is examined under two different aspects. The analysis covers boundary-layer convection with respect to (i) the control of CBL depth by surface heating and synoptic scale influences, and (ii) the structure of convective plumes and their vertical transport of ozone and nitric oxides. The orographic structure of the terrain causes significant differences between planetary boundary layer (PBL) heights, which are found to exceed those of terrain height variations on average. A comparison of boundary-layer flux profiles as well as mean quantities over flat and complex terrain and also under different pollution situations and weather conditions shows relationships between vertical gradients and corresponding turbulent fluxes. Generally, NO_x transports are directed upward independent of the terrain, since primary emission sources are located near the ground. For ozone, negative fluxes are common in the lower CBL in accordance with the deposition of O₃ at the surface.The detailed structure of thermals, which largely carry out vertical transports in the boundary layer, are examined with a conditional sampling technique. Updrafts mostly contain warm, moist and NO_x loaded air, while the ozone transport by thermals alternates with the background ozone gradient. Evidence for handover processes of trace gases to the free atmosphere can be found in the case of existing gradients across the boundary-layer top. An analysis of the size of eddies suggests the possibility of some influence of the heterogeneous terrain in mountainous area on the length scales of eddies.     

西太平洋地区大气边界层内臭氧的季节变化及其影响因子分析

利用臭氧探空资料,分析了西太平洋地区香港(Hong Kong)、那霸(Naha)和札幌(Sapporo)三个站点2000~2010年期间大气边界层内臭氧(O₃)的季节分布和年变化趋势。结果表明,三个站点O₃的季节分布存在明显的差异。其中,那霸和香港大气边界层内O₃季节平均呈双峰值分布,其峰值分别出现在春季和秋季;而札幌站为单峰分布,峰值出现在春季。造成季节分布差异的主要原因包括人为污染源和自然因素如气象条件。另外,三个站点大气边界层内O₃均呈上升趋势。其中札幌、那霸上升最快,分别达0.80 ppb a-1和0.77 ppb a-1。(ppb表示10-9,下同)香港的年际增长较不明显,但秋季增长却非常明显,高达1.21 ppb a-1。结合GOME (Global Ozone Monitoring Experiment) 和SCIAMACHY (Scanning Imaging Absorption Spectro Meter for Atmospheric Chartography)卫星反演的NO₂数据发现,过去10年中国京津唐和东北地区的对流层内NO₂柱总量增加极为迅速。这些O₃前体物通过远距离输送是导致札幌、那霸O₃浓度增加的主要原因之一。珠江三角洲人为污染源的增加及偏北气流的影响,是导致香港地区秋季O₃增加的主要原因。     

Boundary-layer ozone depletion as seen in the Norwegian Arctic in spring

Several years of measurements of ozone, hydrocarbons, sulphate and meteorological parameters from Spitsbergen in the Norwegian Arctic are presented. Most of the measurements were taken on the Zeppelin Mountain at an altitude of 474 m a.s.l. The focus is the episodes of ozone depletion in the lower troposphere in spring, which are studied in a climatological way. Episodes of very low ozone concentrations are a common feature on the Zeppelin Mountain in spring. The low ozone episodes were observed from late March to the beginning of June. When the effect of transport direction was subtracted, the frequenty of the low ozone episodes was found to peak in the beginning of May, possibly reflecting the seasonal cycle in the actual depletion process. Analyses based on trajectory calculations show that most of the episodes occurred when the air masses were transported from W-N. Ozone soundings show that the ozone depletion may extend from the surface and up to 3–4 km altitude. The episodes were associated with a cold boundary layer beneath a thermally stable layer, suppressing mixing with the free troposphere. The concentration of several individual hydrocarbons was much lower during episodes of low ozone than for the average conditions. The change in concentration ratio between the hydrocarbons was in qualitative agreement with oxidation of hydrocarbons by Br and Cl atoms rather than by OH radicals.     

Ozone structure over the equatorial Andes from balloon-borne observations and zonal connection with two tropical sea level sites

In this paper we present first-time measurements of ozone profiles from a high altitude station in Quito, Ecuador (0.19°S, 78.4°W, and 2391 masl) taken from June 2014 to September 2015. We interpret ozone observations in the troposphere, tropopause, and stratosphere through a zonal comparison with data from stations in the Atlantic and Pacific (Natal and San Cristobal from the SHADOZ network). Tropospheric ozone concentrations above the Andes are lower than ozone over San Cristobal and Natal for similar time periods. Ozone variability and pollution layers are also reduced in the troposphere above the Andes. We explain these differences in terms of reduced contributions from the boundary layer and from horizontal transport. In the tropical tropopause layer, ozone is well-mixed up to near the cold point tropopause level. In this regard, our profiles do not show constraints to deep mixing above 14 km, as has been consistently observed at other tropical stations. Total column ozone and stratospheric column ozone are comparable among the three sites. However, the contribution of tropospheric column ozone to total column ozone is significantly lower above the Andes. Our comparisons provide a connection between observations from tropical stations in equatorial South America separated by the wide continental mass. Identified differences in ozone throughout the atmospheric column demonstrate the global benefit of having an ozone sounding station at the equatorial Andes in support of global monitoring networks.     

The transport and redistribution of atmospheric gases in regions of frontal rain

Gases emitted in the planetary boundary layer can be transported very efficiently to the free troposphere through vertical motion along a frontal surface. A mesoscale numerical model was used to simulate the vertical transport of a tracer by clouds during frontogenesis in a moist atmosphere (an evolving Eady wave) in order to illustrate such vertical transport conditions. It is shown that the efficient vertical transport of a tracer occurs only when clouds are present, either when a surface or an in-situ source is considered. Insoluble, partially soluble, and soluble tracers are studied in order to determine the relative importance of vertical transport and scavenging on their redistribution.     

夏季亚洲季风区对流层向平流层输送的源区、路径及其时间尺度的模拟研究

基于NCEP/NCAR分析资料和拉格朗日轨迹输送模式FLEXPART, 通过气块轨迹计算, 对2005年夏季亚洲季风区对流层向平流层输送 (Troposphere to Stratosphere Transport, 简称TST) 的近地层源区、 输送路径及其时间尺度问题进行了一些初步探讨。结果表明: (1) 夏季亚洲季风区TST两个主要的边界层源区, 一个是热带西太平洋地区; 另一个是青藏高原南部、 孟加拉湾以及印度半岛中北部等地区, 上述两个区域与夏季强对流的分布相一致。在对流层顶高度附近 (约16 km高度), 两个近地层源区的垂直输送贡献相当。但进一步分析发现, 穿越对流层顶高度的质量输送只有约10％能够进入20～22 km高度的平流层中, 且主要源于以青藏高原南侧为代表的南亚季风区 (约贡献75%), 这进一步强调了青藏高原及其周边区域在全球TST过程中的重要地位。 (2) 轨迹分析显示, 夏季亚洲季风区对流层进入平流层的 “入口区” 主要在 (25°N～35°N, 90°E～110°E) 区域的青藏高原及其周边区域。TST路径受对流层上层南亚高压闭合环流、 北半球副热带西风急流和赤道东风急流的共同控制。 (3) 亚洲季风区TST两个主要的过程, 一个是和夏季湿对流抬升直接联系的快速输送过程, 它可以使近地层大气在1～2天内输送到平流层中, 贡献了整个TST的10%～30%; 另一个是大气辐射加热所致的大尺度垂直输送, 该输送是一个相对的慢过程, 时间尺度一般为5～30天。此结果意味着, 源于地表的短生命周期的大气污染物可通过光化学反应过程对该区域平流层臭氧及其他大气痕量成分平衡产生重要影响。     

A parameterization of the nocturnal ozone reduction in the residual layer by verticla downward mixing during summer smog situations using sodar data

The reduction of ozone in the nocturnal residual layer by vertical mixing to the surface was investigated for several summer smog episodes on the Swiss plateau in the years 1990 and 1991. Using a limited data set of SODAR measurements and surface ozone concentrations, a parameterization of the ozone depletion in the nocturnal residual layer due to vertical mixing to the ground is proposed. This model is not intended to be physically complete but is rather simple with limited input information required. The nocturnal ozone reduction within the whole planetary boundary layer (nocturnal boundary layer plus residual layer) over the complex terrain of the Swiss plateau for the days investigated is between 20 and 50%.     

Chemical perturbations in the planetary boundary layer and their relevance for chemistry transport modelling

The role of perturbations of reactive trace gas concentration distributions in turbulent flows in the planetary boundary layer (PBL) is discussed. The paper focuses on disturbances with larger spatial scales. Sequential nesting of a chemical transport model is applied to assess the effect of neglecting subgrid chemical perturbations on the formation and loss of ozone, NO _x , peroxyacetyl nitrate (PAN) and HNO₃ calculated with a highly complex chemical mechanism. The results point to characteristic differences regarding the process of mixing of chemically reactive species in the PBL and lower troposphere.     

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。     

Downward transport and modification of tropospheric ozone through moist convection

This study estimated the largely unstudied downward transport and modification of tropospheric ozone associated with tropical moist convection using a coupled meteorology-chemistry model. High-resolution cloud resolving model simulations were conducted for deep moist convection events over West Africa during August 2006 to estimate vertical transport of ozone due to convection. Model simulations realistically reproduced the characteristics of deep convection as revealed by the estimated spatial distribution of temperature, moisture, cloud reflectivity, and vertical profiles of temperature and moisture. Also, results indicated that vertical transport reduced ozone by 50% (50 parts per billion by volume, ppbv) in the upper atmosphere (12–15 km) and enhanced ozone by 39% (10 ppbv) in the lower atmosphere (<2 km). Field observations confirmed model results and indicated that surface ozone levels abruptly increased by 10–30 ppbv in the area impacted by convection due to transport by downdrafts from the upper troposphere. Once in the lower troposphere, the lifetime of ozone decreased due to enhanced dry deposition and chemical sinks. Ozone removal via dry deposition increased by 100% compared to non-convective conditions. The redistribution of tropospheric ozone substantially changed hydroxyl radical formation in the continental tropical boundary layer. Therefore, an important conclusion of this study is that the redistribution of tropospheric ozone, due to deep convection in non-polluted tropical regions, can simultaneously reduce the atmospheric loading of ozone and substantially impact the oxidation capacity of the lower atmosphere via the enhanced formation of hydroxyl radicals.     

Persistent high concentration of ozone during windstorm conditions in southern Korea

Summary Prior to and following the development of a windstorm in the mountainous coastal area of southern Korea, ground level ozone (O₃)-concentrations near Kangnung city, on the lee side of the mountains, show a maximum value at approximately 1300 LST, owing to a photolytic cycle of NO₂–NO–O₃ during the day and a minimum in concentrations at night as a result of the reverse cycle. During the development period of the windstorm, ozone concentrations are generally high all day, and slightly higher during the night. This distribution pattern of ozone is very different from the typical distribution of ozone in the absence of windstorms. High daytime concentrations of ozone during the windstorm are due to both the increase in the amount of ozone from photochemical reactions involving NO_x and the increase in O₃-concentration due to a decrease in the convective boundary layer thickness under the influence of downslope windstorm conditions on the lee-side of the mountains. At night, the windstorm increases in intensity as the westerly winds combine with a katabatic wind blowing downslope toward the surface at the coast. This causes momentum transport of air parcels in the upper levels toward the surface at the coast and the development of internal gravity waves, which generate a hydraulic jump directed upward over the coast and the East sea, thereby reducing to very thin the thickness of the nocturnal surface inversion layer (NSIL). The higher O₃-concentration at night depends mainly upon the shallow NSIL and on some O₃ being transported by the momentum transfer from the upper troposphere toward the ground in windstorm conditions.     

On the dynamics of photochemical smog over the Swiss Middleland — Results of the first POLLUMET field experiment

Summary The Swiss Middleland is a 300×50 km large plain embedded between the Jura, whose highest elevations are between 1000 and 2000m MSL, and the Alps, whose highest peaks are about 400m MSL. Because this plain is the main residence area of Switzerland with a great variety of emission sources, it is also a location with high photosmog concentrations during the summer months.Within the framework of the Swiss POLLUMET (Air Pollution and Meteorology) programme, an initial summer smog field experiment was carried out during July 1990 with the participation of different research groups from Switzerland and Germany. The measurements showed that the ozone concentrations within the atmospheric boundary layer were remarkably variable. The highest concentrations in the upper mixed layer varied between 100 and 130 ppb. The background ozone concentration in the upper atmospheric boundary layer increased from day to day. However, a clear indication of long-range transport could not be found. Remarkable local and regional concentration differences are not only based on the complex structure of the large emission sources (highways, urban plumes). They are also the result of the interaction of convectively driven motion systems like slope and valley winds and mountain-plain circulation.With 14 Figures     

边界层方案对华北低层O3垂直分布模拟的影响

利用WRF-Chem模式,采用3种边界层参数化方案 (YSU, MYJ和ACM2),针对1个晴空、静稳日 (2013年8月26日20:00—27日20:00(北京时)) 进行模拟,着重分析不同边界层参数化方案对夜间残留层形成及日出前后O₃浓度垂直分布形式的模拟效果,并与固城站地面及垂直同步观测资料进行对比。结果表明:3种边界层参数化方案均能够模拟出温度及风速的区域分布形式以及风温垂直结构的变化特征;相比之下,MYJ方案模拟的夜间边界层高度较YSU方案和ACM2方案明显偏高,该对比结果可能是导致近地面污染物浓度模拟差异的重要原因;在夜间稳定层结至日出后稳定状态打破的边界层结构演变过程中,采用YSU方案和ACM2方案模拟的温度和风速垂直扩线形式与观测结果更为接近;同样采用非局地闭合的YSU方案和同时考虑局地和非局地闭合的ACM2方案,对于边界层高度内O₃浓度垂直分布形式的模拟效果具有明显优势。     

中国区域大气本底站近地面臭氧来源贡献及区域代表性

回顾了关于长距离输送对中国区域本底大气臭氧的影响,以及中国区域大气本底站臭氧变化及其区域代表性两方面的研究进展。来自不同污染源区O₃的长距离输送对中国区域O₃影响的研究结果分歧较大,贡献最显著的源区和受体地区也存在争议;同时,鲜有研究考虑到平流层对对流层的O₃贡献,而这部分贡献在前体物排放很少的本底地区非常重要。中国区域各大气本底观测站分别与其周围一定范围内的区域具有相同的对流层O₃柱浓度最大值月份分布,而对与人体健康密切相关的近地面O₃区域特征的分析尚未深入开展;鉴于研究方法的局限性,也尚未深入揭示形成O₃变化区域特征的复杂成因。基于现有研究进展和不足之处,如何利用全球大气化学-环流模式的示踪模拟结果,定量评估来自全球不同地区的O₃对中国本底大气O₃的影响,并进一步评估中国区域6个大气本底站近地面O₃季节变化的区域代表性,是亟待解决的科学问题。     

梅雨锋上边界层中尺度扰动涡旋的个例研究

运用实况自动站、高时空分辨率的雷达和数值模拟资料,对2009年7月24日的梅雨锋暴雨过程进行了分析,结果表明:(1)锋面南侧的暖区弱降水环境内,近地面的风场会有扰动涡旋出现,随着扰动涡旋趋于稳定和向上发展,降水迅速加强,形成短时暴雨,并伴随有大风出现。(2)偏西气流从边界层开始发展并加强为急 流,在向东推进的过程中逐渐抬升,形成了一支从边界层倾斜入对流层低层的急流轴;而偏南气流与偏北风相遇之后,不仅形成风向的辐合和切变,而且在空间上被抬升,形成了一支斜升入流。(3)在近地面风场的切变和 辐合作用下,锋生与辐合同步加强,边界层内的涡度也逐渐增强,由此带动了扰动的发生发展,扰动涡旋在边界层内率先形成,随后,在急流的东传和抬升影响下,扰动涡旋也逐步向东移动、向上发展。(4)近地面风速的加强、风向的辐合切变导致了扰动涡旋的发生和形成,并逐渐发展,这是边界层中尺度扰动涡旋发生发展的动力 因子。     

Observed and modelled “chemical weather” during ESCOMPTE

The new MOdèle de Chimie Atmosphérique à Grande Echelle (MOCAGE) three-dimensional multiscale chemistry and transport model (CTM) has been applied to study heavy pollution episodes observed during the ESCOMPTE experiment. The model considers the troposphere and lower stratosphere, and allows the possibility of zooming from the planetary scale down to the regional scale over limited area subdomains. Like this, it generates its own time-dependent chemical boundary conditions in the vertical and in the horizontal. This paper focuses on the evaluation and quantification of uncertainties related to chemical and transport modelling during two intensive observing periods, IOP2 and IOP4 (June 20–26 and July 10–14, 2001, respectively). Simulations are compared to the database of four-dimensional observations, which includes ground-based sites and aircraft measurements, radiosoundings, and quasi-continuous measurements of ozone by LIDARs. Thereby, the observed and modelled day-to-day variabilities in air composition both at the surface and in the vertical have been assessed. Then, three sensitivity studies are conducted concerning boundary conditions, accuracy of the emission dataset, and representation of chemistry. Firstly, to go further in the analysis of chemical boundary conditions, results from the standard grid nesting set-up and altered configurations, relying on climatologies, are compared. Along with other recent studies, this work advocates the systematic coupling of limited-area models with global CTMs, even for regional air quality studies or forecasts. Next, we evaluate the benefits of using the detailed high-resolution emissions inventory of ESCOMPTE: improvements are noticeable both on ozone reactivity and on the concentrations of various species of the ozone photochemical cycle especially primary ones. Finally, we provide some insights on the comparison of two simulations differing only by the parameterisation of chemistry and using two state-of-the-art chemical schemes for regional photochemical modelling. Regional air quality modelling is found to be highly sensitive to the emission inventory dataset and also to the vertical and horizontal boundary conditions and detailed representation of chemistry. Interestingly enough, they infer the same range of errors compared to total model errors.     

Eddy exchange coefficients in numerical models of the planetary boundary layer

Specification of the eddy exchange coefficients is perhaps one of the most difficult problems in the numerical modeling of the planetary boundary layer. These coefficients have been computed from finite-difference analogs to analytical expressions associated with surface boundary-layer similarity theory, which is based on observations in an equilibrium surface layer. This procedure leads to erroneous results in the region above the surface layer and in a non-equilibrium surface layer. In addition, differencing problems arise in regions of small vertical wind shear. A new turbulence transport model has been obtained through the closure procedures for the transport equations of the Reynolds stress and the turbulent length scale. The new approach could be used to calculate Reynolds stresses and eddy exchange coefficients throughout a non-neutral planetary boundary layer under non-equilibrium conditions.     

Influence of Vertical Eddy Diffusivity Parameterization on Daily and Monthly Mean Concentrations of O3 and NOy

Two parameterization schemes for vertical eddy diffusivity were utilized to investigate their impacts on both the daily and monthly mean concentrations of ozone and NOy, which are the major fractions of the sum of all reactive nitrogen species, i.e., NOy=NO＋NO2＋HNO3＋PAN. Simulations indicate that great changes in the vertical diffusivity usually occur within the planetary boundary layer （PBL）. Daily and monthly mean concentrations of NOy are much more sensitive to changes in the vertical diffusivity than those of ozone and ozone and NOy levels only at or in （relatively） clean sites and areas, where long-range transport plays a crucial role, display roughly equivalent sensitivity. The results strongly suggest that a widely-accepted parameterization scheme be selected and the refinement of the model＇s vertical resolution in the PBL be required, even for regional and long-term studies, and ozone only being examined in an effort to judge the model＇s performance be unreliable, and NOy be included for model evaluations.     

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.