Absorption properties of urban/suburban aerosols in China

The broadband diffuse radiation method is improved to retrieve the aerosol refractive index imaginary part （AIP） and broadband （400-1000 nm mean） single scattering albedo （SSA）. In this method, four sets of SSA selection criteria are proposed for quality control. The method is used to retrieve AIP, SSA and absorptive optical thickness （AbOT） from routine hourly-exposed pyrheliometer and paranometer measurements over 11 sites （meteorological observatories） in China during 1998-2003. Apart from one suburban site （Ejin Qi）, the other urban sites are all located around big or medium cities. As shown in the retrieval results, annual mean SSA during 1998-2003 changes from 0.941 （Wuhan） to 0.849 （Lanzhou）, and AIP from 0.0054 to 0.0203. The 11-site average annual mean SSA and AIP are 0.898 and 0.0119, respectively. SSA during winter is smaller for most sites. There is an evidently positive correlation between SSA and aerosol optical thickness （AOT） for all sites. There is also a positive correlation between SSA and relative humidity for most sites, but a negative correlation for a few sites, such as Kashi and ǚrǚmqi in Northwest China.     

Climatic change and Chinese population growth dynamics over the last millennium

The climate–population relationship has long been conceived. Although the topic has been repeatedly investigated, most of the related works are Eurocentric or qualitative. Consequently, the relationship between climate and population remains ambiguous. In this study, fine-grained temperature reconstructions and historical population data sets have been employed to statistically test a hypothesized relationship between temperature change and population growth (i.e., cooling associated with below average population growth) in China over the past millennium. The important results were: (1) Long-term temperature change significantly determined the population growth dynamics of China. However, spatial variation existed, whilst population growth in Central China was shown to be responsive to both long- and short-term temperature changes; in marginal areas, population growth was only sensitive to short-term temperature fluctuations. (2) Temporally, the temperature–population relationship was obscured in some periods, which was attributable to the factors of drought and social buffers. In summary, a temperature–population relationship was mediated by geographic factors, the aridity threshold, and social factors. Given the upcoming threat posed by climate change to human societies, this study seeks to improve our knowledge and understanding of the climate–society relationship.     

Scaling of Wall-Normal Turbulence Intensity and Vertical Eddy Structures in the Atmospheric Surface Layer

Adequate high-quality data on three-dimensional velocities in the atmospheric surface layer (height \(\delta \)) were acquired in the field at the Qingtu Lake Observation Array. The measurement range occupies nearly the entire logarithmic layer from approximately \(0.006\delta \)–\(0.2\delta \). The turbulence intensity and eddy structures of the velocity fluctuations in the logarithmic region were primarily analyzed, and their variations in the z (wall-normal) direction were revealed. The primary finding was that the turbulent intensity of wall-normal velocity fluctuations exhibits a sharp upswing in the logarithmic region, which differs from classic scaling law and laboratory results. The upswing of the wall-normal turbulence intensity in the logarithmic region is deemed to be linear based on an ensemble of 20 sets of data. In addition, the wall-normal extent of the correlated structures and wall-normal spectra were compared to low Reynolds number results in the laboratory.     

UV attenuation in the cloudy atmosphere

Ultraviolet (UV) energy absorption plays a very important role in the Earth–atmosphere system. Based on observational data for Beijing, we suggest that some atmospheric constituents utilize or transfer UV energy in chemical and photochemical (C&P) reactions, in addition to those which absorb UV energy directly. These constituents are primarily volatile organic compounds (VOCs) emitted from both vegetative and anthropogenic sources. The total UV energy loss in the cloudy atmosphere for Beijing in 1990 was 78.9 Wm⁻². This attenuation was caused by ozone (48.3 Wm⁻²), other compounds in the atmosphere (26.6 Wm⁻²) and a scattering factor (4.0 Wm⁻²). Our results for a cloudy atmosphere in the Beijing area show that the absorption due to these other compounds occurs largely through the mediation of water vapor. This fraction of energy loss has not been fully accounted for in previous models. Observations and previous models results suggest that 1) a cloudy atmosphere absorbs 25∼30 Wm⁻² more solar shortwave radiation than models predict; and 2) aerosols can significantly decrease the downward mean UV-visible radiation and the absorbed solar radiation at the surface by up to 28 and 23 Wm⁻², respectively. Thus, quantitative study of UV and visible absorption by atmospheric constituents involved in homogeneous and heterogeneous C&P reactions is important for atmospheric models.     

Estimation of Surface-Layer Scaling Parameters in the Unstable Boundary Layer: Implications for Orographic Flow Speed-Up

A method is proposed for estimating the surface-layer depth \((z_s)\) and the friction velocity \((u_*)\) as a function of stability (here quantified by the Obukhov length, L) over the complete range of unstable flow regimes. This method extends that developed previously for stable conditions by Argaín et al. (Boundary-Layer Meteorol 130:15–28, 2009), but uses a qualitatively different approach. The method is specifically used to calculate the fractional speed-up \((\varDelta S)\) in flow over a ridge, although it is suitable for more general boundary-layer applications. The behaviour of \(z_s \left( L\right) \) and \(u_*\left( L\right) \) as a function of L is indirectly assessed via calculation of \(\varDelta S\left( L\right) \) using the linear model of Hunt et al. (Q J R Meteorol Soc 29:16–26, 1988) and its comparison with the field measurements reported in Coppin et al. (Boundary-Layer Meteorol 69:173–199, 1994) and with numerical simulations carried out using a non-linear numerical model, FLEX. The behaviour of \(\varDelta S\) estimated from the linear model is clearly improved when \(u_*\) is calculated using the method proposed here, confirming the importance of accounting for the dependences of \(z_s\left( L \right) \) and \(u_*\left( L \right) \) on L to better represent processes in the unstable boundary layer.     

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.     

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.