Atmosphere, Volume 6, Issue 3 (March 2015) – 9 articles , Pages 209-409

A large number of studies on trace metals and metalloids (TMs) accumulations in peatlands have been reported in Europe and North America. Comparatively little information is available on peat chronological records of atmospheric TMs flux in China. Therefore, the objective of our study was to determine the concentrations and accumulation rates (ARs) of TMs in Motianling peatland from Great Hinggan Mountain, northeast China, and to assess these in relation to establish a historical profile of atmospheric metal emissions from anthropogenic sources. To meet these aims we analyzed 14 TMs (As, Ba, Cd, Co, Cr, Cu, Mo, Ni, Pb, Sr, Sb, Tl, and Zn) and Pb isotopes (²⁰⁶Pb, ²⁰⁷Pb, ²⁰⁸Pb) using ICP-AES and ICP-MS, respectively, in three peat sections dated by ²¹⁰Pb and ¹³⁷Cs techniques (approximately spanning the last 200 years). There is a general agreement in the elemental concentration profiles which suggests that all investigated elements were conserved in the Motianling bog. Three principal components were discriminated by principal component analysis (PCA) based on Eigen-values >1 and explaining 85% of the total variance of element concentrations: the first component representing Ba, Co, Cr, Mo, Ni, Sr and Tl reflected the lithogenic source; the second component covering As, Cu and Sb, and Cd is associated with an anthropogenic source from ore mining and processing; the third component (Pb isotope, Pb and Zn) is affected by anthropogenic Pb pollution from industrial manufacturing and fossil-fuel combustion. The pre-industrial background of typical pollution elements was estimated as the average concentrations of TMs in peat samples prior to 1830 AD and with a ²⁰⁷Pb/²⁰⁶Pb ratio close to 1.9. ARs and enrichment factors (EFs) of TMs suggested enhanced metal concentrations near the surface of the peatland (in peat layers dated from the 1980s) linked to an increasing trend since the 2000s. This pollution pattern is also fingerprinted by the Pb isotopic composition, even after the ban of leaded gasoline use in China. Emissions from coal and leaded gasoline combustions in northern China are regarded as one of the major sources of anthropogenic Pb input in this region; meanwhile, the long-distance transportation of Pb-bearing aerosols from Mongolia should be also taken into consideration. The reconstructed history of TMs’ pollution over the past ca. 200 years is in agreement with the industrial development in China and clearly illustrates the influence of human activities on local rural environments. This study shows the utility of taking multi-cores to show the heterogeneity in peat accumulation and applying PCA, EF and Pb isotope methods in multi-proxies analyses for establishing a high resolution geochemical metal record from peatland. Full article

Secondary organic carbon (SOC) formation and its effects on human health require better understanding in Chinese megacities characterized by a severe particulate pollution and robust economic reform. This study investigated organic carbon (OC) and elemental carbon (EC) in PM_2.5 and PM_0.25 collected 8–20 March 2012. Samples were collected inside and outside a classroom in a middle school at Xi’an. On average, OC and EC accounted for 20%–30% of the particulate matter (PM) mass concentration. By applying the EC-tracer method, SOC’s contribution to OC in both PM size fractions was demonstrated. The observed changes in SOC:OC ratios can be attributed to variations in the primary production processes, the photochemical reactions, the intensity of free radicals, and the meteorological conditions. Total carbon (TC) source apportionment by formula derivation showed that coal combustion, motor vehicle exhaust, and secondary formation were the major sources of carbonaceous aerosol. Coal combustion appeared to be the largest contributor to TC (50%), followed by motor vehicle exhaust (25%) and SOC (18%) in both size fractions. Full article

Based on the operational regional ensemble prediction system (REPS) in China Meteorological Administration (CMA), this paper carried out comparison of two initial condition perturbation methods: an ensemble transform Kalman filter (ETKF) and a dynamical downscaling of global ensemble perturbations. One month consecutive tests are implemented to evaluate the performance of both methods in the operational REPS environment. The perturbation characteristics are analyzed and ensemble forecast verifications are conducted; furthermore, a TC case is investigated. The main conclusions are as follows: the ETKF perturbations contain more power at small scales while the ones derived from downscaling contain more power at large scales, and the relative difference of the two types of perturbations on scales become smaller with forecast lead time. The growth of downscaling perturbations is more remarkable, and the downscaling perturbations have larger magnitude than ETKF perturbations at all forecast lead times. However, the ETKF perturbation variance can represent the forecast error variance better than downscaling. Ensemble forecast verification shows slightly higher skill of downscaling ensemble over ETKF ensemble. A TC case study indicates that the overall performance of the two systems are quite similar despite the slightly smaller error of DOWN ensemble than ETKF ensemble at long range forecast lead times. Full article

Market strategies have greatly incentivized the use of diesel engines for land transportation. These engines are responsible for a large fraction of black carbon (BC) emissions in the extra-tropical Northern Hemisphere, with significant effects on both air quality and global climate. In addition to direct radiative forcing, planetary-scale transport of BC to the Arctic region may significantly impact the surface albedo of this region through wet and dry deposition on ice and snow. A sensitivity study is made with the University of L’Aquila climate-chemistry-aerosol model by eliminating on-road diesel emissions of BC (which represent approximately 50% of BC emissions from land transportation). According to the model and using emission scenarios for the year 2000, this would imply an average change in tropopause direct radiative forcing (RF) of −0.054 W∙m⁻² (globally) and −0.074 W∙m⁻² over the Arctic region, with a peak of −0.22 W∙m⁻² during Arctic springtime months. These RF values increase to −0.064, −0.16 and −0.50 W∙m⁻², respectively, when also taking into account the BC snow-albedo forcing. The calculated BC optical thickness decrease (at λ = 0.55 µm) is 0.48 × 10⁻³ (globally) and 0.74 × 10⁻³ over the Arctic (i.e., 10.5% and 16.5%, respectively), with a peak of 1.3 × 10⁻³ during the Arctic springtime. Full article

In this paper we suggest Penning ionization as an important route of formation for ionic species in upper planetary atmospheres. Our goal is to provide relevant tools to researchers working on kinetic models of atmospheric interest, in order to include Penning ionizations in their calculations as fast processes promoting reactions that cannot be neglected. Ions are extremely important for the transmission of radio and satellite signals, and they govern the chemistry of planetary ionospheres. Molecular ions have also been detected in comet tails. In this paper recent experimental results concerning production of simple ionic species of atmospheric interest are presented and discussed. Such results concern the formation of free ions in collisional ionization of H₂O, H₂S, and NH₃ induced by highly excited species (Penning ionization) as metastable noble gas atoms. The effect of Penning ionization still has not been considered in the modeling of terrestrial and extraterrestrial objects so far, even, though metastable helium is formed by radiative recombination of He⁺ ions with electrons. Because helium is the second most abundant element of the universe, Penning ionization of atomic or molecular species by He^*(2³S₁) is plausibly an active route of ionization in relatively dense environments exposed to cosmic rays. Full article

Studies show a divergence in correlation between aerosol and cloud proxies, which has been thought of in the past as the results of varying physical mechanisms. Though modeling studies have supported this idea, from an observational standpoint it is difficult to attribute with confidence the correlations to specific physical mechanisms. We explore a methodology to assess the correlation between cloud water path and aerosol optical depth using Moderate-resolution Imaging Spectroradiometer (MODIS) Aqua retrieved aerosol and cloud properties for absorbing and non-absorbing aerosol types over land and over the Atlantic Ocean for various meteorological conditions. The data covers a three-month period, June through August, during which different aerosol types are predominant in specific regions. Our approach eliminates outliers; sorts the data into aerosol bins; and the mean Aerosol Optical Depth (AOD) value for each bin and the corresponding mean Cloud Water Path (CWP) value are determined. The mean CWP is plotted against the mean AOD. The response curve for all aerosol types shows a peak CWP value corresponding to an aerosol loading value AOD_peak. The peak is used to divide the total range of aerosol loading into two sub ranges. For AOD value below AOD_peak, mean CWP and mean AOD are positively correlated. The correlation between mean CWP and mean AOD is negative for aerosol loading above AOD_peak. Irrespective of aerosol type, atmospheric water vapor content and lower tropospheric static stability, the peak observed for each aerosol type seems to describe a universal feature that calls for further investigation. It has been observed for a variety of geographical locations and different seasons. Full article

An approach based on the Penman-Monteith equation was used to estimate the actual evapotranspiration from local meteorological data over non-homogeneous land cover in a Mediterranean site in the south-east of Italy, with two six month data sets from two different years of measurements (2006 and 2009). The “critical resistance” formulation was used in different forms to model the surface resistance, together with some modifications to take into account the soil moisture content. One, two, or three model parameters were estimated, one of them related to the atmospheric resistance and the others to the surface resistance, and the calibration was made by either linear regression or nonlinear minimization of a proper cost function, depending on the applicability. Two kinds of cost functions were tested, the first depending on both the latent heat flux and the difference between screen air temperature and surface radiometric temperature, and the second depending on the temperature difference only. In all cases the calculated fluxes give better results with respect to both a flux-gradient approach and a complementarity based method, that require comparable data inputs. However the calibration by the temperature differences only, that requires no turbulent flux measurements, considerably increases the statistical uncertainty of the calibration parameters. The inclusion of the soil moisture did not significantly improve the model results in the considered site. Full article

Due to the highly heterogeneous and dynamic nature of urban areas in Chinese cities, air pollution exhibits well-defined spatial variations. Rapid urbanization in China has heightened the importance of understanding and characterizing atmospheric particulate matter (PM) concentrations and their spatiotemporal variations. To investigate the small-scale spatial variations in PM in Xiamen, total suspended particulate (TSP), PM₁₀, PM₅ and PM_2.5 measurements were collected between August and September in 2012. Their average mass concentrations were 102.50 μg∙m⁻³, 82.79 μg∙m⁻³, 55.67 μg∙m⁻³ and 43.70 μg∙m⁻³, respectively. Organic carbon (OC) and elemental carbon (EC) in PM_2.5 were measured using thermal optical transmission. Based on the PM concentrations for all size categories, the following order for the different functional areas studied was identified: hospital > park > commercial area > residential area > industrial area. OC contributed approximately 5%–23% to the PM_2.5 mass, whereas EC accounted for 0.8%–6.95%. Secondary organic carbon constituted most of the carbonaceous particles found in the park, commercial, industrial and residential areas, with the exception of hospitals. The high PM and EC concentrations in hospitals were primarily caused by vehicle emissions. Thus, the results suggest that long-term plans should be to limit the number of vehicles entering hospital campuses, construct large-capacity underground parking structures, and choose hospital locations far from major roads. Full article

Measurements at the Grand Bay National Estuarine Research Reserve support a range of research activities aimed at improving the understanding of the atmospheric fate and transport of mercury. Routine monitoring was enhanced by two intensive measurement periods conducted at the site in summer 2010 and spring 2011. Detailed meteorological data are required to properly represent the weather conditions, to determine the transport and dispersion of plumes and to understand the wet and dry deposition of mercury. To describe the mesoscale features that might influence future plume calculations for mercury episodes during the Grand Bay Intensive campaigns, fine-resolution meteorological simulations using the Weather Research and Forecasting (WRF) model were conducted with various initialization and nudging configurations. The WRF simulations with nudging generated reasonable results in comparison with conventional observations in the region and measurements obtained at the Grand Bay site, including surface and sounding data. The grid nudging, together with observational nudging, had a positive effect on wind prediction. However, the nudging of mass fields (temperature and moisture) led to overestimates of precipitation, which may introduce significant inaccuracies if the data were to be used for subsequent atmospheric mercury modeling. The regional flow prediction was also influenced by the reanalysis data used to initialize the WRF simulations. Even with observational nudging, the summer case simulation results in the fine resolution domain inherited features of the reanalysis data, resulting in different regional wind patterns. By contrast, the spring intensive period showed less influence from the reanalysis data. Full article