ALBERT

Description: Using the monthly precipitation series of 32 meteorological stations in the Yellow River basin from 1951 to 2003, the precipitation cycles were discussed using the Maximum Entropy Method (MEM), the spatial distribution of the precipitation cycles were analysed, and the possible driving factors of the cycles investigated. The results show that the precipitation in the Yellow River has decadal (60a), inter-decadal (25a and 14a) and inter-annual cycles (9a and 3a). The main oscillations over the whole basin are 3a and 9a. There are clearer inter-decadal variations in the riverhead area with much greater water resources, and north of the region of LanHe main stream. The decadal signals are detected in the inner area with less precipitation and Wei River basin. These differences are possibly related to some physical processes, such as the mutual action of sea and atmosphere, and solar activities.

Description: The seasonal variations in background aerosol optical depth (AOD) and aerosol type are investigated over various ecosystems in China based upon three years' worth of meteorological data and data collected by the Chinese Sun Hazemeter Network. In most parts of China, AODs are at a maximum in spring or summer and at a minimum in autumn or winter. Minimum values (0.10~0.20) of annual mean AOD at 500 nm are found in the Qinghai-Tibetan Plateau, which is located in the remote northeast corner of China, the northern forest ecosystems and Hainan Island. Annual mean AOD ranges from 0.25 to 0.30 over desert and oasis areas as well as the desertification grasslands in northern China; the annual mean AOD over the Loess Plateau is moderately high at 0.36. Regions where the highest density of agricultural and industrial activities are located and where anthropogenic sulphate aerosol and soil aerosol emissions are consistently high throughout the whole year (e.g. the central-eastern, southern and eastern coastal regions of China) experience annual mean AODs ranging from 0.50~0.80. Remarkable seasonal changes in the main types of aerosol over northern China (characterized by the Angstrom exponent, α) are seen. Due to biomass and fossil fuel burning from extensive agricultural practices in northern rural areas, concentrations of smoke and soot aerosols rise dramatically during autumn and winter (high α), while the main types of aerosol during spring and summer are dust and soil aerosols (low α). Over southeast Asia, biomass burning during the spring leads to increases in smoke and soot emissions. Over the Tibetan Plateau and Hainan Island where the atmosphere is pristine, the main types of aerosol are dust and sea salt, respectively.

Description: Atmospheric aerosols can contain thousands of organic compounds which impact aerosol surface tension, affecting aerosol properties such as heterogeneous reactivity, ice nucleation, and cloud droplet formation. We present new experimental data for the surface tension of complex, reactive organic–inorganic aqueous mixtures mimicking tropospheric aerosols. Each solution contained 2–6 organic compounds, including methylglyoxal, glyoxal, formaldehyde, acetaldehyde, oxalic acid, succinic acid, leucine, alanine, glycine, and serine, with and without ammonium sulfate. We test two semi-empirical surface tension models and find that most reactive, complex, aqueous organic mixtures which do not contain salt are well described by a weighted Szyszkowski–Langmuir (S-L) model which was first presented by Henning et al. (2005). Two approaches for modeling the effects of salt were tested: (1) the Tuckermann approach (an extension of the Henning model with an additional explicit salt term), and (2) a new implicit method proposed here which employs experimental surface tension data obtained for each organic species in the presence of salt used with the Henning model. We recommend the use of method (2) for surface tension modeling of aerosol systems because the Henning model (using data obtained from organic–inorganic systems) and Tuckermann approach provide similar modeling results and goodness-of-fit (χ2) values, yet the Henning model is a simpler and more physical approach to modeling the effects of salt, requiring less empirically determined parameters.

Description: The reactive uptake of carbonyl-containing volatile organic compounds (cVOCs) by aqueous atmospheric aerosols is a likely source of particulate organic material. The aqueous-phase secondary organic products of some cVOCs are surface-active. Therefore, cVOC uptake can lead to organic film formation at the gas-aerosol interface and changes in aerosol surface tension. We examined the chemical reactions of two abundant cVOCs, formaldehyde and acetaldehyde, in water and aqueous ammonium sulfate (AS) solutions mimicking tropospheric aerosols. Secondary organic products were identified using Aerosol Chemical Ionization Mass Spectrometry (Aerosol-CIMS), and changes in surface tension were monitored using pendant drop tensiometry. Hemiacetal oligomers and aldol condensation products were identified using Aerosol-CIMS. Acetaldehyde depresses surface tension to 65(±2) dyn cm−1 in pure water (a 10% surface tension reduction from that of pure water) and 62(±1) dyn cm−1 in AS solutions (a 20.6% reduction from that of a 3.1 M AS solution). Surface tension depression by formaldehyde in pure water is negligible; in AS solutions, a 9% reduction in surface tension is observed. Mixtures of these species were also studied in combination with methylglyoxal in order to evaluate the influence of cross-reactions on surface tension depression and product formation in these systems. We find that surface tension depression in the solutions containing mixed cVOCs exceeds that predicted by an additive model based on the single-species isotherms.

Description: The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia, was investigated between 11 July and 26 August 2011 using measurements of PM2.5 mass and PM2.5 chemical composition (black carbon, organic matter, anions, cations and 33 elements). This was part of the BORTAS-B (quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which investigated the atmospheric chemistry and transport of seasonal boreal wildfire emissions over eastern Canada in 2011. The US EPA Positive Matrix Factorization (PMF) receptor model was used to determine the average mass (percentage) source contribution over the 45 days, which was estimated to be as follows: long-range transport (LRT) pollution: 1.75 μg m−3 (47%); LRT pollution marine mixture: 1.0 μg m−3 (27.9%); vehicles: 0.49 μg m−3 (13.2%); fugitive dust: 0.23 μg m−3 (6.3%); ship emissions: 0.13 μg m−3 (3.4%); and refinery: 0.081 μg m−3 (2.2%). The PMF model describes 87% of the observed variability in total PM2.5 mass (bias = 0.17 and RSME = 1.5 μg m−3). The factor identifications are based on chemical markers, and they are supported by air mass back trajectory analysis and local wind direction. Biomass burning plumes, found by other surface and aircraft measurements, were not significant enough to be identified in this analysis. This paper presents the results of the PMF receptor modelling, providing valuable insight into the local and upwind sources impacting surface PM2.5 in Halifax and a vital comparative data set for the other collocated ground-based observations of atmospheric composition made during BORTAS-B.

Description: A three-dimensional variational data assimilation (3-DVAR) algorithm for aerosols in a WRF/Chem model is presented. The WRF/Chem model uses the MOSAIC (Model for Simulating Aerosol Interactions and Chemistry) scheme, which explicitly treats eight major species (elemental/black carbon, organic carbon, nitrate, sulfate, chloride, ammonium, sodium and the sum of other inorganic, inert mineral and metal species) and represents size distributions using a sectional method with four size bins. The 3-DVAR scheme is formulated to take advantage of the MOSAIC scheme in providing comprehensive analyses of species concentrations and size distributions. To treat the large number of state variables associated with the MOSAIC scheme, this 3-DVAR algorithm first determines the analysis increments of the total mass concentrations of the eight species, defined as the sum of the mass concentrations across all size bins, and then distributes the analysis increments over four size bins according to the background error variances. The number concentrations for each size bin are adjusted based on the ratios between the mass and number concentrations of the background state. Additional flexibility is incorporated to further lump the eight mass concentrations, and five lumped species are used in the application presented. The system is evaluated using the analysis and prediction of PM2.5 in the Los Angeles basin during the CalNex 2010 field experiment, with assimilation of surface PM2.5 and speciated concentration observations. The results demonstrate that the data assimilation significantly reduces the errors in comparison with a simulation without data assimilation and improved forecasts of the concentrations of PM2.5 as well as individual species for up to 24 h. Some implementation difficulties and limitations of the system are discussed.

Description: China disposes of bulk Municipal Solid Waste (MSW) by landfilling, resulting in a large quantity of mercury that enters landfills through waste. A detailed study on atmospheric mercury emissions from MSW landfills in China is necessary to understand mercury behavior from this source. Between 2003 and 2006, mercury airborne emissions through different pathways, as well as mercury speciation in Landfill Gas (LFG) were measured at 5 MSW landfills in Guiyang and Wuhan, China. The results showed that mercury content in the substrate increased the magnitude of mercury emissions, with the highest emission rate measured at the working face and in uncovered waste areas, and the lowest measured near soil covers and vegetated areas. Meteorological parameters, especially solar radiation, influenced the diurnal pattern of mercury surface-air emissions. Total Gaseous Mercury (TGM) in LFG varied from 2.0 to 1406.0 ng m−3, Monomethyl Mercury (MMHg) and Dimethyl Mercury (DMHg) in LFG averaged at 1.93 and 9.21 ng m−3, and accounted for 0.51% and 1.79% of the TGM in the LFG, respectively. Total mercury emitted from the five landfills ranged from 17 to 3300 g yr−1, with the highest from the working face, then soil covering, and finally the vent pipes.

Description: Field measurements of atmospheric peroxides were obtained during the summer on two consecutive years over urban Beijing, which highlighted the impacts of aerosols on the chemistry of peroxide compounds and hydroperoxyl radicals (HO2). The major peroxides were determined to be hydrogen peroxide (H2O2), methyl hydroperoxide (MHP), and peroxyacetic acid (PAA). A negative correlation was found between H2O2 and PAA in rainwater, providing evidence for a conversion between H2O2 and PAA in the aqueous phase. A standard gas phase chemistry model based on the NCAR Master Mechanism provided a good reproduction of the observed H2O2 profile on non-haze days but greatly overpredicted the H2O2 level on haze days. We attribute this overprediction to the reactive uptake of HO2 by the aerosols, since there was greatly enhanced aerosol loading and aerosol liquid water content on haze days. The discrepancy between the observed and modeled H2O2 can be diminished by adding to the model a newly proposed transition metal ion catalytic mechanism of HO2 in aqueous aerosols. This confirms the importance of the aerosol uptake of HO2 and the subsequent aqueous phase reactions in the reduction of H2O2. The closure of HO2 and H2O2 between the gas and aerosol phases suggests that the aerosols do not have a net reactive uptake of H2O2, because the conversion of HO2 to H2O2 on aerosols compensates for the H2O2 loss. Laboratory studies for the aerosol uptake of H2O2 in the presence of HO2 are urgently required to better understand the aerosol uptake of H2O2 in the real atmosphere.

Description: Asian aerosols are among the most complex yet widely studied components of the atmosphere not only due to their seasonal variability but also their effects on climate change. Four Aerosol Robotic Network (AERONET) sites have been selected to represent aerosol properties dominated by pollution (Taihu), mixed complex particle types (Xianghe), desert-urban (SACOL), and biomass (Mukdahan) in East Asia during the 2001–2010 period. The volume size distribution, aerosol optical depth (τ and τabs), Ångström exponent (α and αabs), and the single scattering co-albedo (ωoabs) parameters over the four selected sites have been used to (a) illustrate seasonal changes in aerosol size and composition and (b) discern the absorptive characteristics of black carbon (BC), organic carbon (OC), mineral dust particles, and mixtures. A strongly absorbing mineral dust influence is seen at the Xianghe, Taihu, and SACOL sites during the spring months (MAM), as given by coarse mode dominance, mean α440–870 〈 1, and mean αabs440–870 〉 1.5. There is a shift towards weakly absorbing pollution (sulfate) and biomass (OC) aerosol dominance in the summer (JJA) and autumn (SON) months, as given by a strong fine mode influence, α440–870 〉 1, and αabs440–870 〈 1.5. A winter season (DJF) shift toward strongly fine mode, absorbing particles (BC and OC) is observed at Xianghe and Taihu (αabs440–870 〉 1 and αabs440–870 〉 1.5). At Mukdahan, a strong fine mode influence is evident year round, with weakly and strongly absorbing biomass particles dominant in the autumn and winter months, respectively, while particles exhibit variable absorption during the spring season. A classification method using α440–870 and ωoabs440 is developed in order to infer the seasonal physico-chemical properties of the aerosol types, such as fine and coarse mode, weak and strong absorption, at the four selected Asian sites.