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.     

Implementation of a surface runoff model with Horton and Dunne mechanisms into the regional climate model RegCM_NCC

A surface runoff parameterization scheme that dynamically represents both Horton and Dunne runoff generation mechanisms within a model grid cell together with a consideration of the subgrid-scaie soil heterogeneity, is implemented into the National Climate Center regional climate model （RegCM_NCC）. The effects of the modified surface runoff scheme on RegCMANCC performance are tested with an abnormal heavy rainfall process which occurred in summer 1998. Simulated results show that the model with the original surface runoff scheme （noted as CTL） basically captures the spatial pattern of precipitation, circulation and land surface variables, but generally overestimates rainfall compared to observations. The model with the new surface runoff scheme （noted as NRM） reasonably reproduces the distribution pattern of various variables and effectively diminishes the excessive precipitation in the CTL. The processes involved in the improvement of NRM-simulated rainfall may be as follows： with the new surface runoff scheme, simulated surface runoff is larger, soil moisture and evaporation （latent heat flux） are decreased, the available water into the atmosphere is decreased; correspondingly, the atmosphere is drier and rainfall is decreased through various processes. Therefore, the implementation of the new runoff scheme into the RegCMANCC has a significant effect on results at not only the land surface, but also the overlying atmosphere.     

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.     

Vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai

A comparative study on the vertical distributions of aerosol optical properties during haze and floating dust weather in Shanghai was conducted based on the data obtained from a micro pulse lidar.There was a distinct difference in layer thickness and extinction coefficient under the two types of weather conditions.Aerosols were concentrated below 1 km and the aerosol extinction coefficients ranged from 0.25 to 1.50km^-1 on haze days.In contrast,aerosols with smaller extinction coefficients(0.20 0.35 km^-1) accumulated mainly from the surface to 2 km on floating dust days.The seasonal variations of extinction and aerosol optical depth（AOD） for both haze and floating dust cases were similar greatest in winter,smaller in spring,and smallest in autumn.More than 85%of the aerosols appeared in the atmosphere below 1 km during severe haze and floating dust weather.The diurnal variation of the extinction coefficient of haze exhibited a bimodal shape with two peaks in the morning or at noon,and at nightfall,respectively.The aerosol extinction coefficient gradually increased throughout the day during floating dust weather.Case studies showed that haze aerosols were generated from the surface and then lifted up,but floating dust aerosols were transported vertically from higher altitude to the surface.The AOD during floating dust weather was higher than that during haze.The boundary layer was more stable during haze than during floating dust weather.     

Are Urban-Canopy Velocity Profiles Exponential?

Using analyses of data from extant direct numerical simulations and large-eddy simulations of boundary-layer and channel flows over and within urban-type canopies, sectional drag forces, Reynolds and dispersive shear stresses are examined for a range of roughness densities. Using the spatially-averaged mean velocity profiles these quantities allow deduction of the canopy mixing length and sectional drag coefficient. It is shown that the common assumptions about the behaviour of these quantities, needed to produce an analytical model for the canopy velocity profile, are usually invalid, in contrast to what is found in typical vegetative (e.g. forest) canopies. The consequence is that an exponential shape of the spatially-averaged mean velocity profile within the canopy cannot normally be expected, as indeed the data demonstrate. Nonetheless, recent canopy models that allow prediction of the roughness length appropriate for the inertial layer’s logarithmic profile above the canopy do not seem to depend crucially on their (invalid) assumption of an exponential profile within the canopy.     

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.     

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.     

Statistical estimation of high-resolution surface air temperature from MODIS over the Yangtze River Delta,China

High-resolution surface air temperature data are critical to regional climate modeling in terms of energy balance, urban climate change, and so on. This study demonstrates the feasibility of using Moderate Resolution Imaging Spectroradiometer (MODIS) land surface temperature (LST) to estimate air temperature at a high resolution over the Yangtze River Delta region, China. It is found that daytime LST is highly correlated with maximum air temperature, and the linear regression coefficients vary with the type of land surface. The air temperature at a resolution of 1 km is estimated from the MODIS LST with linear regression models. The estimated air temperature shows a clear spatial structure of urban heat islands. Spatial patterns of LST and air temperature differences are detected, indicating maximum differences over urban and forest regions during summer. Validations are performed with independent data samples, demonstrating that the mean absolute error of the estimated air temperature is approximately 2.5°C, and the uncertainty is about 3.1°C, if using all valid LST data. The error is reduced by 0.4°C (15%) if using best-quality LST with errors of less than 1 K. The estimated high-resolution air temperature data have great potential to be used in validating high-resolution climate models and other regional applications.