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Long-term record of aerosol optical properties and chemical composition from a high-altitude site (Manora Peak) in Central Himalaya

A long-term study, conducted from February 2005 to July 2008, involving chemical composition and optical properties of ambient aerosols from a high-altitude site (Manora Peak: 29.4° N, 79.5° E, ~1950 m a.s.l.) in the central Himalaya is reported here. The total suspended particulate (TSP) mass concentration varied from 13 to 272 μg m−3 over a span of 42 months. Aerosol optical depth (AOD) and TSP increase significantly during the summer (April–June) due to increase in the concentration of mineral dust associated with the long-range transport from desert regions (from the middle-East and Thar Desert in western India). The seasonal variability in the carbonaceous species (EC, OC) is also significantly pronounced, with lower concentrations during the summer and monsoon (July–August) and relatively high during the post-monsoon (September–November) and winter (December–March). On average, total carbonaceous aerosols (TCA) and water-soluble inorganic species (WSIS) contribute nearly 25 and 10% of the TSP mass, respectively. The WSOC/OC ratios range from 0.36 to 0.83 (average: 0.55 ± 0.15), compared to lower ratios in the Indo-Gangetic Plain (range: 0.35–0.40), and provide evidence for the enhanced contribution from secondary organic aerosols. The mass fraction of absorbing EC ranged from less than a percent (during the summer) to as high as 7.6% (during the winter) and absorption coefficient (babs, at 678 nm) varied between 0.9 to 33.9 Mm−1 (1 Mm−1=10−6 m−1). A significant linear relationship between babs and EC (μgC m−3) yields a slope of 12.2 (± 2.3) m2 g−1, which is used as a measure of the mass absorption efficiency (σabs) of EC.
Mid-latitude ozone monitoring with the GOMOS-ENVISAT experiment version 5: the noise issue

The GOMOS ozone profiles have been analysed to evaluate the GOMOS ability to capture the long-term ozone evolution at mid-latitudes during the expected recovery phase of the ozone layer. Version 5 of the operational GOMOS ozone data has been compared with data from two of the longest ground-based instruments based on different techniques and already involved with many other previous space instrument validations. Comparisons between ground-based and GOMOS data confirm the occurrence of spurious retrievals mainly occurring since 2006. Using a selected set of data it is shown that some bad retrievals are induced by the increasing dark charge of the detectors combined with an inadequate method for its correction. This effect does not only induce a continuous bias, but is rather exhibiting a bimodal distribution including the correct profiles and the bad retrievals. For long-term analyses it is recommended filtering the data according to background light conditions and star temperature (spectrum shape). The new method of the dark charge estimate proposed to be implemented in the version 6 of the ESA algorithm seems to significantly reduce the occurrence of such effects and should allow to monitor stratospheric ozone using GOMOS data with greater confidence.
Decadal regional air quality simulations over Europe in present climate: near surface ozone sensitivity to external meteorological forcing

Regional climate-air quality decadal simulations over Europe were carried out with the RegCM3/CAMx modeling system for the time slice 1991–2000, in order to study the impact of different meteorological forcing on surface ozone. The RegCM3 regional climate model was firstly constrained by the ERA40 reanalysis dataset which is considered as an experiment with perfect meteorological boundary conditions and then it was constrained by the global circulation model ECHAM5. A number of meteorological parameters were examined including the 500 mb geopotential height, solar radiation, temperature, cloud liquid water path, planetary boundary layer height and surface wind. The different RegCM meteorological forcing resulted in changes of near surface ozone over Europe ranging between ± 4 ppb for winter and summer. The area showing the greatest sensitivity in O3 during winter is central and southern Europe while in summer central north continental Europe. The different meteorological forcing impacts on the atmospheric circulation, which in turn affects cloudiness and solar radiation, temperature, wind patterns and the meteorology depended biogenic emissions. For comparison reasons, the impact of chemical boundary conditions on surface ozone was additionally examined with a series of sensitivity studies, indicating that surface ozone changes are comparable to those caused by the different meteorological forcing. These findings suggest that, when it comes to regional climate-air quality simulations, the selection of external meteorological forcing can be as important as the selection of adequate chemical lateral boundary conditions.
Ground-based remote sensing of an elevated forest fire aerosol layer at Whistler, BC: implications for interpretation of mountaintop chemistry

On 30 August 2009, intense forest fires in interior British Columbia (BC) coupled with winds from the east and northeast resulted in transport of a broad forest fire plume across southwestern BC. The physico-chemical and optical characteristics of the plume as observed from Saturna Island (AERONET), CORALNet-UBC and the Whistler Mountain air chemistry facility were consistent with forest fire plumes that have been observed elsewhere in continental North America. However, the importance of three-dimensional transport in relation to the interpretation of mountaintop chemistry observations is highlighted on the basis of deployment of both a CL31 ceilometer and a single particle mass spectrometer (SPMS) in a mountainous setting. The SPMS is used to identify the biomass plume based on levoglucosan and potassium markers. Data from the SPMS are also used to show that the biomass plume was correlated with nitrate, but not correlated with sulphate or sodium. This study not only provides baseline measurements of biomass burning plume physico-chemical characteristics in western Canada, but also highlights the importance of lidar remote sensing methods in the interpretation of mountaintop chemistry measurements.
Trend and characteristics of atmospheric emissions of Hg, As, and Se from coal combustion in China, 1980–2007

Emissions of hazardous trace elements in China are of great concern because of their negative impacts on local air quality as well as on regional environmental health and ecosystem risks. In this paper, the atmospheric emissions of mercury (Hg), arsenic (As), and selenium (Se) from coal combustion in China for the period 1980–2007 are estimated on the basis of coal consumption data and emission factors, which are specified by different categories of combustion facilities, coal types, and the equipped air pollution control devices configuration (Dust collectors, FGD, etc.). Specifically, multi-year emission inventories of Hg, As, and Se from 30 provinces and 4 economic sectors (thermal power, industry, residential use, and others) are evaluated and analyzed in detail. Furthermore, the gridded distribution of provincial-based Hg, As, and Se emissions in 2005 at a resolution of 1° × 1° is also plotted. It shows that the calculated national total atmospheric emissions of Hg, As, and Se from coal combustion have rapidly increased from 73.59 t, 635.57 t, and 639.69 t in 1980 to 305.95 t, 2205.50 t, and 2352.97 t in 2007, at an annually averaged growth rate of 5.4%, 4.7%, and 4.9%, respectively. The industrial sector is the largest source for Hg, As, and Se, accounting for about 50.8%, 61.2%, and 56.2% of the national totals, respectively. The share of power plants is 43.3% for mercury, 24.9% for arsenic, and 33.4% for selenium, respectively. Also, it shows remarkably different regional contribution characteristics of these 3 types of trace elements, the top 5 provinces with the heaviest mercury emissions in 2007 are Shandong (34.40 t), Henan (33.63 t), Shanxi (21.14 t), Guizhou (19.48 t), and Hebei (19.35 t); the top 5 provinces with the heaviest arsenic emissions in 2007 are Shandong (219.24 t), Hunan (213.20 t), Jilin (141.21 t), Hebei (138.54 t), and Inner Mongolia (127.49 t); while the top 5 provinces with the heaviest selenium emissions in 2007 are Shandong (289.11 t), Henan (241.45 t), Jiangsu (175.44 t), Anhui (168.89 t), and Hubei (163.96 t). Between 2000 and 2007, provinces always rank at the top five largest Hg, As, and Se emission sources are: Shandong, Hebei, Shanxi, Henan, and Jiangsu, most of which are located in the east and are traditional industry-based or economically energy intensive areas in China. Notably, Hg, As, and Se emissions from coal combustion in China begin to grow at a more moderate pace since 2005. Emissions from coal-fired power plants sector began to decrease though the coal use had been increasing steadily, which can be mainly attributed to the increasing use of wet flue gas desulfurization (WFGD) in power plants, thus the further research and control orientations of importance for these hazardous trace elements should be the industrial sector.
Source identification and budget analysis on elevated levels of formaldehyde within the ship plumes: a ship-plume photochemical/dynamic model analysis

Elevated levels of formaldehyde (HCHO) along the ship corridors have been observed by satellite sensors, such as ESA/ERS-2 GOME (Global Ozone Monitoring Experiment), and were also simulated by global 3-D chemistry-transport models. In this study, three likely sources of the elevated HCHO levels in the ship plumes as well as their contributions to the elevated HCHO levels (budget) were investigated using a newly-developed ship-plume photochemical/dynamic model: (1) primary HCHO emission from ships; (2) secondary HCHO production via the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) emitted from ships; and (3) atmospheric oxidation of CH4 within the ship plumes. For this ship-plume modelling study, the ITCT 2K2 (Intercontinental Transport and Chemical Transformation 2002) ship-plume experiment, which was carried out about 100 km off the coast of California on 8 May 2002 (11:00 local standard time), was chosen as a base study case because it is the best defined in terms of (1) meteorological data, (2) in-plume chemical composition, and (3) background chemical composition. From multiple ship-plume model simulations for the ITCT 2K2 ship-plume experiment case, CH4 oxidation by elevated levels of in-plume OH radicals was found to be the main factor responsible for the elevated levels of HCHO in the ITCT 2K2 ship-plume. More than ~88% of the HCHO for the ITCT 2K2 ship-plume is produced by this atmospheric chemical process, except in the areas close to the ship stacks where the main source of the elevated HCHO levels would be primary HCHO from the ships (due to the deactivation of CH4 oxidation from the depletion of in-plume OH radicals). Because of active CH4 oxidation by OH radicals, the instantaneous chemical lifetime of CH4 (τCH4) decreased to ~0.45 yr inside the ship plume, which is in contrast to τCH4 of ~1.1 yr in the background (up to ~41% decrease) for the ITCT 2K2 ship-plume case. A variety of likely ship-plume situations at three different latitudinal locations within the global ship corridors was also studied to determine the enhancements in the HCHO levels in the marine boundary layer (MBL) influenced by ship emissions. It was found that the ship-plume HCHO levels could be 19.9–424.9 pptv higher than the background HCHO levels depending on the latitudinal locations of the ship plumes (i.e., intensity of solar radiation and temperature), MBL stability and NOx emission rates. On the other hand, NMVOC emissions from ships were not found to be a primary source of photochemical HCHO production inside ship plumes due to their rapid and individual dilution. However, the diluted NMVOCs would contribute to the HCHO productions in the background air.
Glyoxal vertical columns from GOME-2 backscattered light measurements and comparisons with a global model

Glyoxal vertical column densities have been retrieved from nadir backscattered radiances measured from 2007 to 2009 by the spaceborne GOME-2/METOP-A sensor. The retrieval algorithm is based on the DOAS technique and optimized settings have been used to determine glyoxal slant columns. The liquid water absorption is accounted for using a two-step DOAS approach, leading to a drastic improvement of the fit quality over remote clear water oceans. Air mass factors are calculated by means of look-up tables of weighting functions pre-calculated with the LIDORT v3.3 radiative transfer model and using a priori glyoxal vertical distributions provided by the IMAGESv2 chemical transport model. The total error estimate comprises random and systematic errors associated to the DOAS fit, the air mass factor calculation and the cloud correction. The highest glyoxal vertical column densities are mainly observed in continental tropical regions, while the mid-latitude columns strongly depend on the season with maximum values during warm months. An anthropogenic signature is also observed in highly populated regions of Asia. Comparisons with glyoxal columns simulated with IMAGESv2 in different regions of the world generally point to a missing glyoxal source, most probably of biogenic origin.
Global and regional trends in aerosol optical depth based on remote sensing products and pollutant emission estimates between 2000 and 2009

This study evaluates global and regional aerosol optical depth (AOD) trends in view of aerosol (precursor) emission changes between 2000 and 2009. We use AOD products from MODIS, MISR and AERONET, and emission estimates from the EMEP, REAS and IPCC inventories. First we compare trends in global Level 3 AOD products of MODIS, MISR and AERONET (Level 2). We find generally negative trends over Europe and North America, whereas over South and East Asia they are mostly positive. The negative trends over parts of Europe and North-East America appear to be significant. Second, we analyze MODIS Level 2 AODs for three selected regions with good data coverage (Central Mediterranean, North-East America and East Asia) and compare with Level 3 products. This corroborates that the 2000–2009 AOD trend over the Central Mediterranean is negative and corresponds well with the MODIS Level 3 analysis. Also for North-East America the trend is generally negative and in agreement with MODIS Level 3 products. For East Asia the trends derived from Level 2 products are mostly positive and correspond with the MODIS Level 3 results. Over Europe, the trends in aerosol single scattering albedo, as derived from MISR data, appear to be positive (declining solar radiation absorption), whereas this is not the case over the USA, though these data are not yet validated. Third we compare trends in AOD with emission changes of SO2, NOx, NH3 and black carbon. We associate the downward trends in AOD over Europe and North America with decreasing emissions of SO2, NOx, and other criteria pollutants, and consequently declining aerosol concentrations. Over East Asia the MODIS Level 2 trends are generally positive, consistent with increasing pollutant emissions by fossil energy use and growing industrial and urban activities. It appears that SO2 emission changes dominate the AOD trends, although especially in Asia NOx emissions may become increasingly important. Our results suggest that solar brightening due to decreasing SO2 emissions and resulting downward AOD trends over Europe may have weakened in the 2000s compared to the 1990s.
Emission location dependent ozone depletion potentials for very short-lived halogenated species

We present trajectory-based estimates of Ozone Depletion Potentials (ODPs) for very short-lived halogenated source gases as a function of surface emission location. The ODPs are determined by the fraction of source gas and its degradation products which reach the stratosphere, depending primarily on tropospheric transport and chemistry, and the effect of the resulting reactive halogen in the stratosphere, which is determined by stratospheric transport and chemistry, in particular by stratospheric residence time. Reflecting the different timescales and physico-chemical processes in the troposphere and stratosphere, the estimates are based on calculation of separate ensembles of trajectories for the troposphere and stratosphere. A methodology is described by which information from the two ensembles can be combined to give the ODPs. The ODP estimates for a species with a fixed 20 d lifetime, representing a compound like n-propyl bromide, are presented as an example. The estimated ODPs show strong geographical and seasonal variation, particularly within the tropics. The values of the ODPs are sensitive to the inclusion of a convective parametrization in the trajectory calculations, but the relative spatial and seasonal variation is not. The results imply that ODPs are largest for emissions from south and south-east Asia during Northern Hemisphere summer and from the western Pacific during Northern Hemisphere winter. Large ODPs are also estimated for emissions throughout the tropics with non-negligible values also extending into northern mid-latitudes, particularly in the summer. These first estimates, whilst made under some simplifying assumptions, show larger ODPs for certain emission regions, particularly south Asia in NH summer, than have typically been reported by previous studies which used emissions distributed evenly over land surfaces.
Global atmospheric model for mercury including oxidation by bromine atoms

Global models of atmospheric mercury generally assume that gas-phase OH and ozone are the main oxidants converting Hg0 to HgII and thus driving mercury deposition to ecosystems. However, thermodynamic considerations argue against the importance of these reactions. We demonstrate here the viability of atomic bromine (Br) as an alternative Hg0 oxidant. We conduct a global 3-D simulation with the GEOS-Chem model assuming gas-phase Br to be the sole Hg0 oxidant (Hg + Br model) and compare to the previous version of the model with OH and ozone as the sole oxidants (Hg + OH/O3 model). We specify global 3-D Br concentration fields based on our best understanding of tropospheric and stratospheric Br chemistry. In both the Hg + Br and Hg + OH/O3 models, we add an aqueous photochemical reduction of HgII in cloud to impose a tropospheric lifetime for mercury of 6.5 months against deposition, as needed to reconcile observed total gaseous mercury (TGM) concentrations with current estimates of anthropogenic emissions. This added reduction would not be necessary in the Hg + Br model if we adjusted the Br oxidation kinetics downward within their range of uncertainty. We find that the Hg + Br and Hg + OH/O3 models are equally capable of reproducing the spatial distribution of TGM and its seasonal cycle at northern mid-latitudes. The Hg + Br model shows a steeper decline of TGM concentrations from the tropics to southern mid-latitudes. Only the Hg + Br model can reproduce the springtime depletion and summer rebound of TGM observed at polar sites; the snowpack component of GEOS-Chem suggests that 40% of HgII deposited to snow in the Arctic is transferred to the ocean and land reservoirs, amounting to a net deposition flux to the Arctic of 60 Mg a−1. Summertime events of depleted Hg0 at Antarctic sites due to subsidence are much better simulated by the Hg + Br model. Model comparisons to observed wet deposition fluxes of mercury in the US and Europe show general consistency. However the Hg + Br model does not capture the summer maximum over the southeast US because of low subtropical Br concentrations while the Hg + OH/O3 model does. Vertical profiles measured from aircraft show a decline of Hg0 above the tropopause that can be captured by both the Hg + Br and Hg + OH/O3 models, except in Arctic spring where the observed decline is much steeper than simulated by either model; we speculate that oxidation by Cl species might be responsible. The Hg + Br and Hg + OH/O3 models yield similar global budgets for the cycling of mercury between the atmosphere and surface reservoirs, but the Hg + Br model results in a much larger fraction of mercury deposited to the Southern Hemisphere oceans.