Simulation of Tropospheric Ozone with MOZART-2： An Evaluation Study over East Asia

Climate changes induced by human activities have attracted a great amount of attention. With this, a coupling system of an atmospheric chemistry model and a climate model is greatly needed in China for better understanding the interaction between atmospheric chemical components and the climate. As the first step to realize this coupling goal, the three-dimensional global atmospheric chemistry transport model MOZART-2 (the global Model of Ozone and Related Chemical Tracers, version 2) coupled with CAM2 (the Community Atmosphere Model, version 2) is set up and the model results are compared against observations obtained in East Asia in order to evaluate the model performance. Comparison of simulated ozone mixing ratios with ground level observations at Minamitorishima and Ryori and with ozonesonde data at Naha and Tateno in Japan shows that the observed ozone concentrations can be reproduced reasonably well at Minamitorishima but they tend to be slightly overestimated in winter and autumn while underestimated a little in summer at Ryori. The model also captures the general features of surface CO seasonal variations quite well, while it underestimates CO levels at both Minamitorishima and Ryori. The underestimation is primarily associated with the emission inventory adopted in this study. Compared with the ozonesonde data, the simulated vertical gradient and magnitude of ozone can be reasonably well simulated with a little overestimation in winter, especially in the upper troposphere. The model also generally captures the seasonal, latitudinal and altitudinal variations in ozone concentration. Analysis indicates that the underestimation of tropopause height in February contributes to the overestimation of winter ozone in the upper and middle troposphere at Tateno.     

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．     

A Three-Dimensional Simulation of HO x Concentrations Over East Asia During TRACE-P

The Models-3 Community Multi-scale Air Quality modeling system (CMAQ) coupled with the Regional Atmospheric Modeling System (RAMS) is used to simulate three-dimensional concentration distributions of hydroxyl (OH) and hydroperoxyl (HO₂) radicals over the western Pacific Ocean during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) field campaign. Modeled values of OH and HO₂ and their closely related chemical species and photolysis rates are compared with observational data collected onboard the DC-8 aircraft. Comparison shows that the model reasonably reproduced these observed values over a broad range of conditions with an overall tendency to overestimate the measured OH and HO₂ by a factor of 1.56 and 1.24, respectively. A case study of OH, HO₂ and their closely related chemical species and photolysis rates along the DC-8 flights 11 and 12 conducted on 17–18 March 2001 shows that the model reproduces the temporal and spatial variations reasonable well, and produces more reliable OH and HO₂ concentrations in the polluted environment than in the clean marine boundary layer.     

Correlation between black carbon aerosols, carbon monoxide and tropospheric ozone over a tropical urban site

Black carbon aerosols plays an important role in the earth's radiative balance and little is known of their concentrations, distributions, source strength, and especially the aerosol chemistry of the developing world. The present study addresses the impact of back carbon aerosols on different atmospheric species like CO and tropospheric ozone over an urban environment, namely Hyderabad, India. Ozone concentration varies from 14 to 63 ppbv over the study area. Diurnal variations of ozone suggest that ozone concentration starts increasing gradually after sunrise, attaining a maximum value by evening time and decreasing gradually thereafter. Black carbon (BC) aerosol mass concentrations varies from 1471 to 11,175 ng m⁻³. The diurnal variations of BC suggest that the concentrations are increased by a factor of 2 during morning (06:00–09:00 h) and evening hours (18:00 to 22:00 h) compared to afternoon hours. Positive correlation has been observed between BC and CO (r²=0.74) with an average slope of 6.4×10⁻³ g BC/g CO. The slope between black carbon aerosol mass concentration and tropospheric ozone suggests that every 1 μg m⁻³ increase in black carbon aerosol mass concentration causes a 3.5 μg m⁻³ reduction in tropospheric ozone. The results have been discussed in detail in the paper.     

区域气候模式REMO对东亚季风季节变化的模拟研究

将欧洲区域气候模式REMO首次应用于东亚区域,利用该模式对1980年和1990年东亚季风季节变化进行了模拟研究,并将模拟结果与NCEP再分析资料进行比较,以检验该模式对东亚季风的模拟能力.研究表明,区域气候模式REMO能够较好地模拟出东亚地区高、低空的大气环流特征,模拟的高度场、流场和温度场与NCEP再分析资料场都比较一致.模拟结果显示了东亚季风的月变化和季节转换特征.模拟的降水场与GPCC降水资料的对比结果表明,REMO能较为成功地模拟出东亚地区降水的空间分布,并能较好地反映降水的季节变化及主要降水趋势,夏季降水模拟偏大,整个区域平均的降水量偏差约为18%左右.     

The simulation of aerosol transport over East Asia region

This study was carried out to understand the contribution of PM10 from China emission to Seoul Metropolitan Area (SMA) during high concentration period in January, 2007. The hourly PM10 concentration in Seoul Metropolitan Area had reached up to over 150 μg/m³ on 17th and 23rd of January in 2007. The aerosol transports from China along the Northwestern wind becomes the background concentrations in Korea and the assessment of the amount of contribution from China is very important in managing the air quality improvement plan in SMA.The U.S. EPA's Models-3/CMAQ (Community Multiscale Air Quality) was used to simulate PM10 concentration. The CMAQ performance was evaluated by comparing with the measurements in SMA for the episode period. The predictions were relatively in a good agreement with the measurements.The results show that the PM10 transport from China to Korea is significant and its contribution reaches up to 80% in the episode period. In order to assess more extensively the aerosol transport in East Asia region, the study to run the model in full year with speciated PM component measurements in super site is underway.     

东亚太平洋地区近地面臭氧的季节和年际变化特征及其与东亚季风的关系

利用东亚清洁背景站近地面臭氧观测资料,结合风场和降水资料,分析东亚各地区臭氧的多年季节变化特征,并探讨东亚太平洋地区臭氧的季节和年际变化与季风的关系以及影响近地层臭氧的主要因子。结果表明：东亚大部分地区与北半球背景站观测一致,近地层臭氧季节变化表现为春季最高、夏季最低的特征;但在东亚中纬度33～43°N,臭氧表现为夏季最高,而在东亚20°N以南地区臭氧则表现为冬末、春初最高。东亚太平洋沿岸近地面臭氧的季节变化主要受东亚冬、夏季风环流的季节变化控制。该地区不同纬度上春季峰值出现时间的差异与亚洲大陆春季不同时期污染物输送路径的差异有关。对东亚太平洋沿岸对流层顶附近位势涡度、高空急流和垂直环流季节变化的分析表明,冬春季可能是平流层向对流层输送的最强期,对近地面臭氧贡献最大。初夏至秋季（5-11月）,平流层向对流层输送较弱,对近地面臭氧贡献较小。东亚太平洋地区夏季风爆发的时间和强度以及季风环流型的年际差异是导致该地区春、夏季臭氧年际变化的主要原因;而季风降水和云带位置以及平流层一对流层交换是造成臭氧年际变化的其他原因。     

未来东亚地区硫化物沉降及输送的预测

采用东亚未来二氧化硫排放量的预测资料,利用东亚硫化物输送模式拟了未来１５年东亚各地区的硫化物沉降量、相互输送量的变化趋势力其对土壤的影响。结果表明,未来１５年东亚各地区的硫化物沉降量将日益增多,一些地区硫化物沉降量大大超出了土壤对酸沉降的承受能力,对周边地区硫化物的输送量也将进一步加大,形势相当严峻。     

Responses of the tropospheric ozone and odd hydrogen radicals to column ozone change

The response of tropospheric ozone to a change in solar UV penetration due to perturbation on column ozone depends critically on the tropospheric NO _x (NO+NO₂) concentration. At high NO _x or a polluted area where there is net ozone production, a decrease in column ozone will increase the solar UV penetration to the troposphere and thus increase the tropospheric ozone concentration. However, the opposite will occur, for example, at a remote oceanic area where NO _x is so low that there is net ozone destruction. This finding may have important implication on the interpretation of the long term trend of tropospheric ozone. A change in column ozone will also induce change in tropospheric OH, HO₂, and H₂O₂ concentrations which are major oxidants in the troposphere. Thus, the oxidation capacity and, in turn, the abundances of many reduced gases will be perturbed. Our model calculations show that the change in OH, HO₂, and H₂O₂ concentrations are essentially independent of the NO _x concentration.     

The photochemistry of synoptic-scale ozone synthesis: Implications for the global tropospheric ozone budget

The oxidation of nonmethane hydrocarbons represents a source of tropospheric ozone that is primarily confined to the boundary layers of several highly industrialized regions. (Each region has an area greater than one million km²). Using a photochemical model, the global tropospheric ozone budget is reexamined by including the in-situ production from these localized regimes. The results from these calculations suggest that the net source due to this photochemistry, which takes place on the synoptic scale, is approximately as large as the amount calculated for global scale photochemical processes which consider only the oxidation of methane and carbon monoxide. Such a finding may have a considerable impact on our understanding of the tropospheric ozone budget. The model results for ozone show reasonable agreement with the climatological summer distribution of ozone and the oxides of nitrogen at the surface and with the vertical distribution of ozone and nonmethane hydrocarbons obtained during a 1980 field program.     

Budget Calculations for Ozone and Its Precursors: Seasonal and Episodic Features Based on Model Simulations

Results from two air quality models (LOTOS, EURAD) have been used toanalyse the contribution of the different terms in the continuity equationto the budget of ozone, NO_x and PAN. Both models cover largeparts of Europe and describe the processes relevant for troposphericchemistry and dynamics. One of the models is designed to simulate episodesin the order of 1–2 weeks (EURAD), the other is focussing on theseasonal scale (LOTOS). Based on EURAD simulations it is found that theatmospheric boundary layer (ABL) in Central Europe during a summer-smogepisode in 1990 acts as a source of ozone, which is partly exported from theproduction region in Central Europe. About 40% of the ozone producedchemically in the ABL is lost from Central Europe due to net transport(large-scale and turbulent), 40% are deposited within the domain. Vertical mass exchange of ozone is dominated by the prevailing subsidenceand averaged vertical mass fluxes are directed downward. Averaged massfluxes of PAN, which has no stratospheric source, are upward in the upperpart of the ABL. The results from LOTOS are discussed for the same episodeand for a two month period (July/August 1990). The budget calculation showlarger chemical production for the LOTOS model compared to EURAD. Therelative importance of deposition and net transport, however, is in the sameorder. Differences between the two-month calculation and the one weekepisode are only important for Western Europe where the chemical production is enhanced by 30% during the summer-smog episode. The dependence ofthe results on initial and boundary values is discussed for ozone on thebasis of a simple sensitivity study with EURAD where ozone in the FT is setto 10 ppb initially. This leads to a reversal in the direction of averagedozone mass fluxes in the upper part of the ABL.     

Impact of Long-range Desert Dust Transport on Hydrometeor Formation over Coastal East Asia

Model simulations and hydrological reanalysis data for 2007 are applied to investigate the impact of long-range desert dust transport on hydrometeor formation over coastal East Asia.Results are analyzed from Hong Kong and Shanghai,which are two representative coastal cities of East Asia.Long-range desert dust transport impacts mainly spring and summer clouds and precipitation over coastal East Asia.In spring,clouds and precipitation come mainly from large-scale condensation and are impacted mainly by dust from the Gobi,Sahara,and Thar deserts.These desert dusts can participate in the precipitation within and below the clouds.At lower latitudes,the dust particles act mainly as water nuclei.At higher latitudes,they act as both water nuclei and ice nuclei.The effect of Gobi,Sahara,and Thar dust on large-scale clouds and precipitation becomes stronger at higher latitudes.In summer,clouds and precipitation over coastal East Asia come mainly from convection and are impacted mainly by dust from the Taklamakan,Arabian,and Karakum-Kavir deserts.Most Taklamakan dust particles can participate in precipitation within convective clouds as ice nuclei,while Arabian and Karakum-Kavir dust particles participate only as water nuclei in precipitation below the clouds.The effect of Taklamakan dust on convective clouds and precipitation becomes stronger at lower latitudes.Of all the desert dusts,that from the Gobi and Taklamakan deserts has the relatively largest impact.Gobi dust impacts climate change in coastal East Asia by affecting spring water clouds at higher latitudes.     

我国和东亚地区硫化物跨边界输送态势研究

本文利用污染物三维欧拉长距离输送实用模式,较详细地模拟了我国和东亚地区硫化物跨地区、跨边界输送态势,分析了东亚地区硫化物输送通量随高度、季节变化的分布特点,讨论了不同地区边界上硫化物的跨边界输送通量及流的收支平衡,并给出了我国和周边国家和地区之间硫化物的相互输送量。结果表明,我国向外输送的硫化物占周边国家和地区总硫沉降的比例并不大,各地区硫沉降的主要来源是自身排放;硫化物长距离输送中硫酸根的输送占重要地位,各地区硫酸根沉降中的外来比例较大。我们初步总结出一个东亚地区硫化物输送的概念模式：在低层,夏季主要自西南向东北输送,冬季长江以北自北向南输送,长江以南由西南向北输送,并在长江中下游地区形成一个较强的硫化物辐合带,在高层,无论冬夏均由西向东输送,并随高空带变化,中层为二者的过渡,春秋季的情形界于冬夏之间,偏向冬季。     

区域气候模式在东亚地区的应用研究——垂直分辨率与侧边界对夏季季风降水影响研究

将美国国家大气研究中心（NCAR）的区域气候模式（RegCM2-1996）设置在东亚-西太平洋区域（简称东亚区域气候模式RegCM2/EA）。利用该模式研究东亚区域气候模式的几个重要问题，即：垂直分辨率的影响，侧边界条件（如嵌套技术、缓冲区宽度、不同资料）的重要性等。数值试验结果表明：细垂直分辨率模拟的降水分布优于粗分辨率模式，但容易引起“数值点暴雨”；RegCM2/EA与不同来源的大尺度侧边界嵌套，模拟的降水会有明显的不同；当用RegCM2/EA模拟较大区域时，应该取较宽的缓冲区；在各种嵌套方案中，指数松弛嵌套方法最好。这些结果为进一步探讨东亚区域气候模式的特点以及发展与改造区域气候模式提供一定的依据。研究结果还需要用更多的数值试验来验证。     

Seasonal Variation of the East Asian Subtropical Westerly Jet and Its Association with the Heating Field over East Asia

The structure and seasonal variation of the East Asian Subtropical Westerly Jet （EAWJ） and associations with heating fields over East Asia are examined by using NCEP/NCAR reanalysis data. Obvious differences exist in the westerly jet intensity and location in different regions and seasons due to the ocean-land distribution and seasonal thermal contrast, as well as the dynamic and thermodynamic impacts of the Tibetan Plateau. In winter, the EAWJ center is situated over the western Pacific Ocean and the intensity is reduced gradually from east to west over the East Asian region. In summer, the EAWJ center is located over the north of the Tibetan Plateau and the jet intensity is reduced evidently compared with that in winter. The EAWJ seasonal evolution is characterized by the obvious longitudinal inconsistency of the northward migration and in-phase southward retreat of the EAWJ axis. A good correspondence between the seasonal variations of EAWJ and the meridional differences of air temperature （MDT） in the mid-upper troposphere demonstrates that the MDT is the basic reason for the seasonal variation of EAWJ. Correlation analyses indicate that the Kuroshio Current region to the south of Japan and the Tibetan Plateau are the key areas for the variations of the EAWJ intensities in winter and in summer, respectively. The strong sensible and latent heating in the Kuroshio Current region is closely related to the intensification of EAWJ in winter. In summer, strong sensible heating in the Tibetan Plateau corresponds to the EAWJ strengthening and southward shift, while the weak sensible heating in the Tibetan Plateau is consistent with the EAWJ weakening and northward migration.     

Changing trends in tropospheric methane and carbon monoxide: A sensitivity analysis of the OH-radical

A sensitivity analysis is performed in order to study recently observed changes in atmospheric methane and carbon monoxide trends. For the analysis we have adapted a one-dimensional transport/chemistry model in order to comply with changes in vertical transport, stratosphere-troposphere flux of ozone, the water vapour cycle and the short-wave radiative transfer. In addition we have formulated an improved relationship which expresses the steady state OH concentration in terms of longer lived compounds which has a fair agreement with the one-dimensional model results. An analysis of the observed changes and trends in methane and carbon monoxide shows that both emissions and changes in global OH concentrations can be main causes for the observed changes. Average methane emissions have slowed down, particularly in the NH, in the last five years, though perhaps not very significantly. Carbon monoxide emissions are decreasing faster in the last couple of years than in the period 1983–1990. The study suggests that climate fluctuations (tropospheric water vapour, temperature and convective activity) and the stratospheric ozone depletion (tropospheric UV radiation) have a significant influence on tropospheric composition and thus on trends in methane and carbon monoxide concentrations.The IMAU is partner in the Netherlands Centre for Climate Research (CCR).     

A Modeling Study of Seasonal Variation of Atmospheric Aerosols over East Asia

In this study, a regional air quality model system (RAQMS) was applied to investigate the spatial distributions and seasonal variations of atmospheric aerosols in 2006 over East Asia. Model validations demonstrated that RAQMS was able to reproduce the evolution processes of aerosol components reasonably well. Ground-level PM₁₀ (particles with aerodynamic diameter ≤10 μm) concentrations were highest in spring and lowest in summer and were characterized by three maximum centers: the Taklimakan Desert (～1000 μg m^-3), the Gobi Desert (～400 μg m^-3), and the Huabei Plain (～300 μm^-3) of China. Vertically, high PM₁₀ concentrations ranging from 100 μg m^-3 to 250 μg m^-3 occurred from the surface to an altitude of 6000 m at 30^o--45^oN in spring. In winter, the vertical gradient was so large that most aerosols were restricted in the boundary layer. Both sulfate and ammonium reached their highest concentrations in autumn, while nitrate reached its maximum level in winter. Black carbon and organic carbon aerosol concentrations reached maximums in winter. Soil dust were strongest in spring, whereas sea salt exerted the strongest influence on the coastal regions of eastern China in summer. The estimated burden of anthropogenic aerosols was largest in winter (1621 Gg) and smallest in summer (1040 Gg). The sulfate burden accounted for ～42% of the total anthropogenic aerosol burden. The dust burden was about twice the anthropogenic aerosol burden, implying the potentially important impacts of the natural aerosols on air quality and climate over East Asia.     

Numerical Investigation of the Influence of Mineral Dust on the Tropospheric Chemistry of East Asia

An investigation of the influence of mineral dust ontrace gas cycles in the troposphere is carried out inthis study. A 3D regional scale atmospheric chemistrymodel (STEM-III) which includes aerosol processes isused for the numerical simulations for May 1987.Heterogeneous interactions between gaseous species(SO₂, N₂O₅, HNO₃, HO₂andH₂O₂) and the dust particles are considered.Emissions of dust behind convective cold fronts aremodeled. The transport and distribution of mineraldust predicted from the model is compared withsatellite measurements (aerosol index from TOMS). Themodel is shown to capture the synoptic variability inthe observed aerosol index. Calculations show twomajor dust events in May 1987, during which thedust levels close to the source reach more than500 g/m³. The transport of dust is mostlyrestricted towards the north, with the net continentaloutflow of 6 Tg for the entire month. Results showthat the presence of mineral aerosol can greatlyimpact sulfate and nitrate distributions. Averagedover the month of May, the presence of dust isestimated to increase particulate sulfate and nitratelevels in east Asia by 40%. Furthermore, the sulfateand nitrate on the dust particles are predicted to beassociated with the coarse mode (3–5 m particlediameter), consistent with observations over Japan.The influence of mineral dust on the photochemicaloxidant cycle is also investigated. For the entiremonth, a5–10% decrease in boundary layer ozone ispredicted by the model closer to regions of higherdust levels. The ratio of nitric acid to NO_x overmarine regions is reduced by a factor between 1 and 2in the boundary layer to more than 2 in the freetroposphere as a result of aerosol processes.     

东亚地区春季二氧化硫的输送与转化过程研究I.模式及其验证

结合新近评估的东亚地区污染源资料,作者利用一个耦合的区域化学输送模式系统以探讨东亚地区春季期间气象过程、气相与液相化学过程、非均相化学过程、气溶胶过程和干湿沉降过程对二氧化硫输送及转化过程的影响,并研究二氧化硫和硫酸盐气溶胶的空间分布及变化特征.模拟的二氧化硫和硫酸盐气溶胶的浓度值与2001年春季飞机和地面获取的观测值进行了比较.比较结果显示,模拟值与观测值具有很好的一致性,模式系统很好地反映了二氧化硫和硫酸盐气溶胶的分布特征和变化规律,再现了许多观测到的重要特征,为进一步分析模拟结果奠定了基础.     

Simulated seasonal variations in nitrogen wet deposition over East Asia

近20年来我国的酸雨和酸沉降分布发生了较大变化,其中一个重要变化是硝酸根离子明显增加,这主要是氮氧化物排放增加所导致的。为了评估氮氧化物排放对酸雨和酸沉降的影响,本文利用区域大气化学模式RAMS-CMAQ模拟分析了东亚地区氮氧化物排放、输送和化学转化过程以及降水时空变化对氮氧化物和氮沉降量时空分布的影响,并借助于中国气象台站和东亚酸沉降监测网的观测数据评估了模式结果的合理性。模拟结果显示,东亚地区氮湿沉降的季节变化十分显著,氮湿沉降通量在1~18 kg N ha~(-1) yr~(-1)之间;春夏两季湿沉降占全年的71%,其中夏季占42.7%。