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A steady-state analysis of the temperature responses of water vapor and aerosol lifetimes

The dominant removal mechanism of soluble aerosol is wet deposition. The atmospheric lifetime of aerosol, relevant for aerosol radiative forcing, is therefore coupled to the atmospheric cycling time of water vapor. This study investigates the coupling between water vapor and aerosol lifetimes in a well-mixed atmosphere. Based on a steady-state study by Pruppacher and Jaenicke (1995) we describe the coupling in terms of the processing efficiency of air by clouds and the efficiencies of water vapor condensation, of aerosol activation, and of the transfer from cloud water to precipitation. We extend this to expressions for the temperature responses of the water vapor and aerosol lifetimes. Previous climate model results (Held and Soden, 2006) suggest a water vapor lifetime temperature response of +5.3 ± 2.0% K−1. This can be used as a first guess for the aerosol lifetime temperature response, but temperature sensitivities of the aerosol lifetime simulated in recent aerosol–climate model studies extend beyond this range and include negative values. This indicates that other influences probably have a larger impact on the computed aerosol lifetime than its temperature response, more specifically changes in the spatial distributions of aerosol (precursor) emissions and precipitation patterns, and changes in the activation efficiency of aerosol. These are not quantitatively evaluated in this study but we present suggestions for model experiments that may help to understand and quantify the different factors that determine the aerosol atmospheric lifetime.
Overview of the Mount Tai Experiment (MTX2006) in central East China in June 2006: studies of significant regional air pollution

We conducted an intensive field campaign at the summit of Mt. Tai (36.26° N, 117.11° E, 1534 m above sea level), Shandong Province, located at the center of central East China, during the period 28 May to 30 June 2006, to study seasonal maxima of regional air pollution with respect to ozone (O3) and aerosols. The specific objectives, campaign design, and major findings are summarized. High concentrations of O3 and its precursors, and aerosols, were detected and studied in the context of annual variations. Most importantly, we identified that emissions from regional-scale open crop residue burning after the harvesting of winter wheat, together with photochemical aging, strongly increased the concentrations of O3, aerosols, and primary pollutants in this month of year. Studies of in situ photochemical activity, regional source attribution of O3, O3–aerosol interactions, validation of satellite observations of tropospheric NO2, behaviors of volatile organic compounds and organic/inorganic aerosol species, loss rates of black carbon (BC), and instrument inter-comparisons are also summarized. The observed BC levels must have a strong impact on the regional climate.
High abundances of water-soluble dicarboxylic acids, ketocarboxylic acids and α-dicarbonyls in the mountaintop aerosols over the North China Plain during wheat burning season

Aerosol (TSP) samples were collected at the summit of Mount Tai (elevation: 1534 m a.s.l., 36.25° N, 117.10° E) located in the North China Plain using a high-volume air sampler and pre-combusted quartz filters. Sampling was conducted on day/night or 3 h basis in the period from 29 May to 28 June 2006 during the field burning of wheat straw residue and the post-burning season. The filter samples were analyzed for low-molecular-weight dicarboxylic acids, ketoacids and α-dicarbonyls using capillary gas chromatography (GC) and GC-MS employing water extraction and butyl ester derivatization. Molecular distributions of dicarboxylic acids (C2-C11, 220–6070 ng m−3) were characterized by a predominance of oxalic (C2) acid (105–3920 ng m−3) followed by succinic (C4) or malonic (C3) acid. Unsaturated aliphatic diacids, including maleic (M), isomaleic (iM) and fumaric (F) acids, were also detected together with aromatic diacids (phthalic, isophthalic and terephthalic acids). ω-oxocarboxylic acids (C2-C9, 24–610 ng m−3) were detected as the second most abundant compound class with the predominance of glyoxylic acid (11–360 ng m−3), followed by α-ketoacid (pyruvic acid, 3–140 ng m−3) and α-dicarbonyls (glyoxal, 1–230 ng m−3 and methylglyoxal, 2–120 ng m−3). We found that these levels (>6000 ng m−3 for diacids) are several times higher than those reported in Chinese megacities at ground levels. The concentrations of diacids increased from late May to early June, showing a maximum on 7 June, and then significantly decreased during the period 8–11 June, when the wind direction shifted from southerly to northerly. Similar temporal trends were found for ketocarboxylic acids and α-dicarbonyls as well as total carbon (TC) and water-soluble organic carbon (WSOC). The temporal variations of water-soluble organics were interpreted by the direct emission from the field burning of agricultural wastes (wheat straw) in the North China Plain and the subsequent photochemical oxidation of volatile and semi-volatile organic precursors emitted from field burning as well as dark ozonolysis of volatile organic compounds and other organics, accretion reactions and oxidation of nonvolatile organics such as unsaturated fatty acids. This study demonstrates that the field burning of agricultural wastes in early summer strongly influenced the air quality of the free troposphere over the North China Plain.
Self-limited uptake of α-pinene oxide to acidic aerosol: the effects of liquid–liquid phase separation and implications for the formation of secondary organic aerosol and organosulfates from epoxides

The reactive uptake of α-pinene oxide (αPO) to acidic sulfate aerosol was studied under humid conditions in order to gain insight into the effects of liquid–liquid phase separation on aerosol heterogeneous chemistry and to elucidate further the formation of secondary organic aerosol and organosulfates from epoxides. A continuous flow environmental chamber was used to monitor changes in diameter of monodisperse, deliquesced, acidic sulfate particles exposed to αPO at 25% and 50% RH (relative humidity). In order to induce phase separation and probe potential limits to particle growth from acidic uptake, αPO was introduced over a wide range of concentrations, from 200 ppb to 5 ppm. Uptake was observed to be highly dependent on initial aerosol pH. Significant uptake of αPO to aerosol was observed with initial pH < 0. When exposed to 200 ppb αPO, aerosol with pH = -0.5 showed 23% growth, and 6% volume growth was observed at pH = 0. Aerosol with pH = 1 showed no growth. The extreme acidity required for efficient αPO uptake suggests that this chemistry is typically not a major route to formation of aerosol mass or organosulfates in the atmosphere. Effective partition coefficients (Kp, eff) were in the range of (0.1–2) x 10-4 m3μg-1 and were correlated to initial particle acidity and particle organic content; particles with higher organic content had lower partition coefficients. Effective uptake coefficients (γeff) ranged from 0.1 to 1.1 x 10-4 and are much lower than recently reported for uptake to bulk solutions. In experiments in which αPO was added to bulk H2SO4 solutions, phase separation was observed for mass loadings similar to those observed with particles, and product distributions were dependent on acid concentration. Liquid–liquid phase separation in bulk experiments, along with our observations of decreased uptake to particles with the largest growth factors, suggests an organic coating forms upon uptake to particles, limiting reactive uptake.
Quantitative evaluation of emission controls on primary and secondary organic aerosol sources during Beijing 2008 Olympics

To assess the primary and secondary sources of fine organic aerosols after the aggressive implementation of air pollution controls during the 2008 Beijing Olympic Games, 12 h PM2.5 values were measured at an urban site at Peking University (PKU) and an upwind rural site at Yufa during the CAREBEIJING-2008 (Campaigns of Air quality REsearch in BEIJING and surrounding region) summer field campaign. The average PM2.5 concentrations were 72.5 ± 43.6 μg m−3 and 64.3 ± 36.2 μg m−3 (average ± standard deviation, below as the same) at PKU and Yufa, respectively, showing the lowest concentrations in recent years. Combining the results from a CMB (chemical mass balance) model and secondary organic aerosol (SOA) tracer-yield model, five primary and four secondary fine organic aerosol sources were compared with the results from previous studies in Beijing. The relative contribution of mobile sources to PM2.5 concentrations was increased in 2008, with diesel engines contributing 16.2 ± 5.9% and 14.5 ± 4.1% and gasoline vehicles contributing 10.3 ± 8.7% and 7.9 ± 6.2% to organic carbon (OC) at PKU and Yufa, respectively. Due to the implementation of emission controls, the absolute OC concentrations from primary sources were reduced during the Olympics, and the contributions from secondary formation of OC represented a larger relative source of fine organic aerosols. Compared with the non-controlled period prior to the Olympics, primary vehicle contributions were reduced by 30% at the urban site and 24% at the rural site. The reductions in coal combustion contributions were 57% at PKU and 7% at Yufa. Our results demonstrate that the emission control measures implemented in 2008 significantly alleviated the primary organic particle pollution in and around Beijing. However, additional studies are needed to provide a more comprehensive assessment of the emission control effectiveness on SOA formation.
Evaluation of spatio-temporal variability of Hamburg Aerosol Climatology against aerosol datasets from MODIS and CALIOP

The new global aerosol climatology named HAC (Hamburg Aerosol Climatology) is compared against MODIS (Collection 5, 2000–2007) and CALIOP (Level 2-version 3, 2006–2011) retrievals. The comparison of aerosol optical depth (AOD) from HAC against MODIS shows larger HAC AOD values over regions with higher aerosol loads and smaller HAC AOD values than MODIS for regions with lower loads. The HAC data are found to be more reliable over land and for low AOD values. The largest differences between HAC and MODIS occur from March to August for the Northern Hemisphere and from September to February for the Southern Hemisphere. In addition, both the spectral variability and vertical distribution of the HAC AOD are examined at selected AERONET (1998–2007) sites, representative of main aerosol types (pollutants, sea salt, biomass and dust). Based on comparisons against spectral AOD values from AERONET, the mean absolute percentage error in HAC AOD data is 25% at ultraviolet wavelengths (400 nm), 6–12% at visible and 18% at near-infrared (1000 nm). For the same AERONET sites, the HAC AOD vertical distribution is compared against CALIOP space lidar data. On a daily average basis, HAD AOD is less by 9% in the lowest 3 km than CALIOP values, especially for sites with biomass burning smoke, desert dust and sea salt spray. Above the boundary layer, the HAC AOD vertical distribution is reliable.
Recommendations for reporting "black carbon" measurements

Although black carbon (BC) is one of the key atmospheric particulate components driving climate change and air quality, there is no agreement on the terminology that considers all aspects of specific properties, definitions, measurement methods, and related uncertainties. As a result, there is much ambiguity in the scientific literature of measurements and numerical models that refer to BC with different names and based on different properties of the particles, with no clear definition of the terms. The authors present here a recommended terminology to clarify the terms used for BC in atmospheric research, with the goal of establishing unambiguous links between terms, targeted material properties and associated measurement techniques.
Pauci ex tanto numero: reduce redundancy in multi-model ensembles

We explicitly address the fundamental issue of member diversity in multi-model ensembles. To date, no attempts in this direction have been documented within the air quality (AQ) community despite the extensive use of ensembles in this field. Common biases and redundancy are the two issues directly deriving from lack of independence, undermining the significance of a multi-model ensemble, and are the subject of this study. Shared, dependant biases among models do not cancel out but will instead determine a biased ensemble. Redundancy derives from having too large a portion of common variance among the members of the ensemble, producing overconfidence in the predictions and underestimation of the uncertainty. The two issues of common biases and redundancy are analysed in detail using the AQMEII ensemble of AQ model results for four air pollutants in two European regions. We show that models share large portions of bias and variance, extending well beyond those induced by common inputs. We make use of several techniques to further show that subsets of models can explain the same amount of variance as the full ensemble with the advantage of being poorly correlated. Selecting the members for generating skilful, non-redundant ensembles from such subsets proved, however, non-trivial. We propose and discuss various methods of member selection and rate the ensemble performance they produce. In most cases, the full ensemble is outscored by the reduced ones. We conclude that, although independence of outputs may not always guarantee enhancement of scores (but this depends upon the skill being investigated), we discourage selecting the members of the ensemble simply on the basis of scores; that is, independence and skills need to be considered disjointly.
The influence of cruise ship emissions on air pollution in Svalbard – a harbinger of a more polluted Arctic?

In this study we have analyzed whether tourist cruise ships have an influence on measured sulfur dioxide (SO2), ozone (O3), Aitken mode particle and equivalent black carbon (EBC) concentrations at Ny Ålesund and Zeppelin Mountain on Svalbard in the Norwegian Arctic during summer. We separated the measurement data set into periods when ships were present and periods when ships were not present in the Kongsfjord area, according to a long-term record of the number of passengers visiting Ny Ålesund. We show that when ships with more than 50 passengers cruise in the Kongsfjord, measured daytime mean concentrations of 60 nm particles and EBC in summer show enhancements of 72 and 45%, respectively, relative to values when ships are not present. Even larger enhancements of 81 and 72% were found for stagnant conditions. In contrast, O3 concentrations were 5% lower on average and 7% lower under stagnant conditions, due to titration of O3 with the emitted nitric oxide (NO). The differences between the two data subsets are largest for the highest measured percentiles, while relatively small differences were found for the median concentrations, indicating that ship plumes are sampled relatively infrequently even when ships are present although they carry high pollutant concentrations. We estimate that the ships increased the total summer mean concentrations of SO2, 60 nm particles and EBC by 15, 18 and 11%, respectively. Our findings have two important implications. Firstly, even at such a remote Arctic observatory as Zeppelin, the measurements can be influenced by tourist ship emissions. Careful data screening is recommended before summertime Zeppelin data is used for data analysis or for comparison with global chemistry transport models. However, Zeppelin remains as one of the most valuable Arctic observatories, as most other Arctic observatories face even larger local pollution problems. Secondly, given landing statistics of tourist ships on Svalbard, it is suspected that large parts of the Svalbard archipelago are affected by cruise ship emissions. Thus, our results may be taken as a warning signal of future pan-Arctic conditions if Arctic shipping becomes more frequent and emission regulations are not strict enough.
Characterization of minerals in air dust particles in the state of Tamilnadu, India through ftir spectroscopy

The abstract of this paper explains the presence of minerals in air which causes great concern regarding public health issues. The spectroscopic investigation of air dust particles of several samples in various locations in the state of Tamilnadu, India is reported. Qualitative analyses were carried out to determine the major and minor constituent minerals present in the samples based on the FTIR absorption peaks. This study also identified the minerals like quartz, asbestos, kaolinite, calcite, hematite, montmorillonite, nacrite and several other trace minerals in the air dust particles. The presents of quartz is mainly found in all the samples invariably. Hence the percentage of quartz and its crystalline nature were determined with the help of extinction co-efficient and crystallinity index respectively.