Characteristics of carbonyl compounds in ambient air of Shanghai,China

The levels of carbonyl compounds in Shanghai ambient air were measured in five periods from January 2007 to October 2007 (covering winter, high-air-pollution days, spring, summer and autumn). A total of 114 samples were collected and eighteen carbonyls were identified. Formaldehyde, acetaldehyde and acetone were the most abundant carbonyls and their mean concentrations of 19.40 ± 12.00, 15.92 ± 12.07 and 11.86 ± 7.04 μg m⁻³ respectively, in the daytime for five sampling periods. Formaldehyde and acetaldehyde showed similar diurnal profiles with peak mixing ratios in the morning and early afternoon during the daytime. Their mean concentrations were highest in summer and lowest in winter. Acetone showed reversed seasonal variation. The high molecular weight (HMW, ≥C5) carbonyls also showed obvious diurnal variations with higher concentrations in the daytime in summer and autumn, while they were all not detected in winter. Formaldehyde and acetaldehyde played an important role in removing OH radicals in the atmosphere, but the contribution of acetone was below 1%. The carbonyls levels in high-air-pollution days were reported. More carbonyl species with higher concentrations were found in high-air-pollution days than in spring. These carbonyls were transported with other pollutants from north and northwest in March 27 to April 2, 2007 and then mixed with local sources. Comparing with Beijing and Guangzhou, the concentrations of formaldehyde and acetaldehyde in Shanghai were the highest, which indicated that the air pollution in Shanghai was even worse than expected.     

Adaptation of Pressure Based CFD Solvers for Mesoscale Atmospheric Problems

General purpose Computational Fluid Dynamics (CFD) solvers are frequently used in small-scale urban pollution dispersion simulations without a large extent of ver- tical flow. Vertical flow, however, plays an important role in the formation of local breezes, such as urban heat island induced breezes that have great significance in the ventilation of large cities. The effects of atmospheric stratification, anelasticity and Coriolis force must be taken into account in such simulations. We introduce a general method for adapting pressure based CFD solvers to atmospheric flow simulations in order to take advantage of their high flexibility in geometrical modelling and meshing. Compressibility and thermal stratification effects are taken into account by utilizing a novel system of transformations of the field variables and by adding consequential source terms to the model equations of incompressible flow. Phenomena involving mesoscale to microscale coupled effects can be analyzed without model nesting, applying only local grid refinement of an arbitrary level. Elements of the method are validated against an analytical solution, results of a reference calculation, and a laboratory scale urban heat island circulation experiment. The new approach can be applied with benefits to several areas of application. Inclusion of the moisture transport phenomena and the surface energy balance are important further steps towards the practical application of the method.     

Vertical and Horizontal Transport of Energy and Matter by Coherent Motions in a Tall Spruce Canopy

In the framework of the EGER (ExchanGE processes in mountainous Regions) project, the contribution of coherent structures to vertical and horizontal transports in a tall spruce canopy is investigated. The combination of measurements done in both the vertical and horizontal directions allows us to investigate coherent structures, their temporal scales, their role in flux transport, vertical coupling between the sub-canopy, canopy and air above the canopy, and horizontal coupling in the sub-canopy layer. The temporal scales of coherent structures detected with the horizontally distributed systems in the sub-canopy layer are larger than the temporal scales of coherent structures detected with the vertically distributed systems. The flux contribution of coherent structures to the momentum and sensible heat transport is found to be dominant in the canopy layer. Carbon dioxide and latent heat transport by coherent structures increase with height and reach a maximum at the canopy height. The flux contribution of the ejection decreases with increasing height and becomes dominant above the canopy level. The flux fraction transported during the sweep increases with height and becomes the dominant exchange process at the upper canopy level. The determined exchange regimes indicate consistent decoupling between the sub-canopy, canopy and air above the canopy during evening, nighttime and morning hours, whereas the coupled states and coupled by sweep states between layers are observed mostly during the daytime. Furthermore, the horizontal transport of sensible heat by coherent structures is investigated, and the heterogeneity of the contribution of coherent events to the flux transport is demonstrated. A scheme to determine the horizontal coupling by coherent structures in the sub-canopy layer is proposed, and it is shown that the sub-canopy layer is horizontally coupled mainly in the wind direction. The vertical coupling in most cases is observed together with streamwise horizontal coupling, whereas the cross-stream direction is decoupled.     

对流和层状云系电活动,对流及降水特性的相关分析

通过对６次不同云系电特性、回波、对流及降水特性的综合分析，探讨了它们之间的相关性。结果表明：除不稳定能量外，－１０℃层和０℃层高度以及他们之间的高度差、０℃层与云顶的高度差也是表征雷暴动力和电特性的重要参量；雷暴云起电过程对冰相作用有较强的依赖性；雷暴中的电活动与对流活动成正相关，闪电多发生在３０ｄＢｚ强回波高度大于－１０℃层高度时段内，强烈的电活动与强降雨有很好的对应关系，而与一般性降雨对应关系较差；在雷暴消散期，闪电可能会影响雷暴的特性     

Climatic regime shift and decadal anomalous events in China

Climatic time series from historical documents and instrumental records from China showed temporal and regional patterns in the last two to three centuries, including two multidecadal oscillations at quasi-20-year and quasi-70-year timescales revealed by signal analysis from wavelet transform. Climatic anomalous events on the decadal timescale were identified based on the two oscillations when their positive (or negative) phases coincide with each other to amplify amplitude. The coldest event occurred in the decade of 1965–1975 in eastern China, while the periods of 1920–1930, 1940–1950, and 1988–2000 appeared to be warmer in most parts of China. For the precipitation series in northern China, the dry anomalous event was found in the late 1920s, while the wet anomalous event occurred in the 1950s. A severe drought in 1927–1929 in northern China coincided with the anomalous warm and dry decade, caused large-scale famine in nine provinces over northern China. Climatic anomalous events with a warm-dry or cold-wet association in the physical climate system would potentially cause severe negative impacts on natural ecosystem in the key vulnerable region over northern China. The spatial pattern of summer rainfall anomalies in the eastern China monsoon region showed an opposite variations in phase between the Yellow River Valley (North China) and the mid-low Yangtze River Valley as well as accompanied the shift of the northernmost monsoon boundary. Climatic regime shifts for different time points in the last 200 years were identified. In North China, transitions from dry to wet periods occurred around 1800, 1875, and 1940 while the transitions from wet to dry periods appeared around 1840, 1910, and the late 1970s. The reversal transition in these time points can also be found in the lower Yangtze River. Climatic regime shifts in China were linked to the interaction of mid- and low latitude atmospheric circulations (the westerly flow and the monsoon flow) when they cross the Tibetan Plateau in East Asia.     

呼和浩特市降水化学特征分析

对2006年呼和浩特市降水离子监测资料进行分析,结果表明:降水呈碱性,季节分布明显,夏季降水集中且pH值为全年最低,冬季降水量少,pH值较高;SO42-离子为主要致酸离子,阳离子中Ca2+,Mg2+离子的浓度很高;降水中主要成分之间相关性显著,Ca2+的中和作用较强;降水气团的后向轨迹分析表明蒙古国的沙漠地区是呼和浩特冬春季碱性降水的主要来源,夏季较低的pH值降水则部分源于我国的华中、华北地区的酸性污染物中长距离输送。     

不同垂直分辨率对台风数值模拟影响的敏感性试验

利用新一代数值预报模式ARW(Advance Research WRF),模拟试验了在不同垂直分辨率条件下模式对"罗莎"台风的预报性能。试验结果表明,数值模式的垂直分辨率变化对台风路径预报效果的影响不大,但对台风强度和结构的预报效果有明显影响。但是,对于一定的水平分辨率而言,有一个与之匹配的垂直分辨率,垂直分辨率低于或者高于这个相匹配的阈值,模式的预报性能都会下降。     

Atmospheric chemistry of hydrogen fluoride

Although a large volume of monitoring and computer simulation data exist for global coverage of HF, study of HF in the troposphere is still limited to industry whose primary interest is the safety and risk assessment of HF release because it is a toxic gas. There is very limited information on atmospheric chemistry, emission sources, and the behavior of HF in the environment. We provide a comprehensive review on the atmospheric chemistry of HF, modeling the reactions and transport of HF in the atmosphere, the removal processes in the vertical layer immediately adjacent to the surface (up to approximately 500 m) and recommend research needed to improve our understanding of atmospheric chemistry of HF in the troposphere. The atmospheric chemistry, emissions, and surface boundary layer transport of hydrogen fluoride (HF) are summarized. Although HF is known to be chemically reactive and highly soluble, both factors affect transport and removal in the atmosphere, the chemistry can be ignored when the HF concentration is at a sufficiently low level (e.g., 10 ppmv). At a low concentration, the capability for HF to react in the atmosphere is diminished and therefore the species can be mathematically treated as inert during the transport. At a sufficiently high concentration of HF (e.g., kg/s release rate and thousands of ppm), however, HF can go through a series of rigorous chemical reactions including polymerization, depolymerization, and reaction with water to form molecular complex. As such, the HF species cannot be considered as inert because the reactions could intimately influence the plume’s thermodynamic properties affecting the changes in plume temperature and density. The atmospheric residence time of HF was found to be less than four (4) days, and deposition (i.e., atmosphere to surface transport) is the dominant mechanism that controls the removal of HF and its oligomers from the atmosphere. The literature data on HF dry deposition velocity was relatively high compared to many commonly found atmospheric species such as ozone, sulfur dioxide, nitrogen oxides, etc. The global average of wet deposition velocity of HF was found to be zero based on one literature source. Uptake of HF by rain drops is limited by the acidity of the rain drops, and atmospheric particulate matter contributes negligibly to HF uptake. Finally, given that the reactivity of HF at a high release rate and elevated mole concentration cannot be ignored, it is important to incorporate the reaction chemistry in the near-field dispersion close to the proximity of the release source, and to incorporate the deposition mechanism in the far-field dispersion away from the release source. In other words, a hybrid computational scheme may be needed to address transport and atmospheric chemistry of HF in a range of applications. The model uncertainty will be limited by the precision of boundary layer parameterization and ability to accurately model the atmospheric turbulence.     

Multi-Source Emission Determination Using an Inverse-Dispersion Technique

Inverse-dispersion calculations can be used to infer atmospheric emission rates through a combination of downwind gas concentrations and dispersion model predictions. With multiple concentration sensors downwind of a compound source (whose component positions are known) it is possible to calculate the component emissions. With this in mind, a field experiment was conducted to examine the feasibility of such multi-source inferences, using four synthetic area sources and eight concentration sensors arranged in different configurations. Multi-source problems tend to be mathematically ill-conditioned, as expressed by the condition number κ. In our most successful configuration (average κ = 4.2) the total emissions from all sources were deduced to within 10% on average, while component emissions were deduced to within 50%. In our least successful configuration (average κ = 91) the total emissions were calculated to within only 50%, and component calculations were highly inaccurate. Our study indicates that the most accurate multi-source inferences will occur if each sensor is influenced by only a single source. A “progressive” layout is the next best: one sensor is positioned to “see” only one source, the next sensor is placed to see the first source and another, a third sensor is placed to see the previous two plus a third, and so on. When it is not possible to isolate any sources κ is large and the accuracy of a multi-source inference is doubtful.     

How effective is the new generation of GPM satellite precipitation in characterizing the rainfall variability over Malaysia?

We investigated the potential of the new generation of satellite precipitation product from the Global Precipitation Mission (GPM) to characterize the rainfall in Malaysia. Most satellite precipitation products have limited ability to precisely characterize the high dynamic rainfall variation that occurred at both time and scale in this humid tropical region due to the coarse grid size to meet the physical condition of the smaller land size, sub-continent and islands. Prior to the status quo, an improved satellite precipitation was required to accurately measure the rainfall and its distribution. Subsequently, the newly released of GPM precipitation product at half-hourly and 0.1° resolution served an opportunity to anticipate the aforementioned conflict. Nevertheless, related evidence was not found and therefore, this study made an initiative to fill the gap. A total of 843 rain gauges over east (Borneo) and west Malaysia (Peninsular) were used to evaluate the rainfall the GPM rainfall data. The assessment covered all critical rainy seasons which associated with Asian Monsoon including northeast (Nov. - Feb.), southwest (May - Aug.) and their subsequent inter-monsoon period (Mar. - Apr. & Sep. - Oct.). The ability of GPM to provide quantitative rainfall estimates and qualitative spatial rainfall patterns were analysed. Our results showed that the GPM had good capacity to depict the spatial rainfall patterns in less heterogeneous rainfall patterns (Spearman’s correlation, 0.591 to 0.891) compared to the clustered one (r = 0.368 to 0.721). Rainfall intensity and spatial heterogeneity that is largely driven by seasonal monsoon has significant influence on GPM ability to resolve local rainfall patterns. In quantitative rainfall estimation, large errors can be primarily associated with the rainfall intensity increment. 77% of the error variation can be explained through rainfall intensity particularly the high intensity (> 35 mm d^-1). A strong relationship between GPM rainfall and error was found from heavy (~35 mm d^-1) to violent rain (160 mm d^-1). The output of this study provides reference regarding the performance of GPM data for respective hydrology studies in this region.