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Characteristics and formation mechanism of continuous hazes in China: a case study during the autumn of 2014 in the North China Plain

Four extreme haze episodes occurred in October 2014 in the North China Plain (NCP). To clarify the formation mechanism of hazes in autumn, strengthened observations were conducted in Beijing from 5 October to 2 November. The meteorological parameters, satellite data, chemical compositions and optical properties of aerosols were obtained. The hazes originated from the NCP, developing in the southwest and northeast directions, with the highest concentration of PM2.5 of 469 μg m−3 in Beijing. The NCP was dominated by a weak high pressure system during the haze episode, which resulted in low surface wind speed and relatively stagnant weather. Moreover, the wind slowed down around Beijing city. The secondary aerosols NO3− was always higher than that of SO42−, which indicated the motor vehicles played a more important part in the hazes in October 2014, even though the oxidation rate from SO2 to SO42− was faster than that of NOx to NO3−. Sudden increases of the concentrations of organic matter, Cl− and BC (black carbon) before each haze episode implied that regional transport of pollutants by biomass burning was important for haze formation during autumn. A satellite map of fire points and the backward trajectories of the air masses also indicated this pollution source. The distinct decrease in the PBL (planetary boundary layer) height during four haze episodes restrained the vertical dispersion of the air pollutants. Water vapor also played a vital role in the formation of hazes by accelerating the chemical transformation of secondary pollutants, leading to hygroscopic growth of aerosols and altering the thermal balance of the atmosphere.
Airborne observations and simulations of three-dimensional radiative interactions between Arctic boundary layer clouds and ice floes

Based on airborne spectral imaging observations, three-dimensional (3-D) radiative effects between Arctic boundary layer clouds and highly variable Arctic surfaces were identified and quantified. A method is presented to discriminate between sea ice and open water under cloudy conditions based on airborne nadir reflectivity γλ measurements in the visible spectral range. In cloudy cases the transition of γλ from open water to sea ice is not instantaneous but horizontally smoothed. In general, clouds reduce γλ above bright surfaces in the vicinity of open water, while γλ above open sea is enhanced. With the help of observations and 3-D radiative transfer simulations, this effect was quantified to range between 0 and 2200 m distance to the sea ice edge (for a dark-ocean albedo of αwater = 0.042 and a sea-ice albedo of αice = 0.91 at 645 nm wavelength). The affected distance Δ L was found to depend on both cloud and sea ice properties. For a low-level cloud at 0–200 m altitude, as observed during the Arctic field campaign VERtical Distribution of Ice in Arctic clouds (VERDI) in 2012, an increase in the cloud optical thickness τ from 1 to 10 leads to a decrease in Δ L from 600 to 250 m. An increase in the cloud base altitude or cloud geometrical thickness results in an increase in Δ L; for τ = 1/10 Δ L = 2200 m/1250 m in case of a cloud at 500–1000 m altitude. To quantify the effect for different shapes and sizes of ice floes, radiative transfer simulations were performed with various albedo fields (infinitely long straight ice edge, circular ice floes, squares, realistic ice floe field). The simulations show that Δ L increases with increasing radius of the ice floe and reaches maximum values for ice floes with radii larger than 6 km (500–1000 m cloud altitude), which matches the results found for an infinitely long, straight ice edge. Furthermore, the influence of these 3-D radiative effects on the retrieved cloud optical properties was investigated. The enhanced brightness of a dark pixel next to an ice edge results in uncertainties of up to 90 and 30 % in retrievals of τ and effective radius reff, respectively. With the help of Δ L, an estimate of the distance to the ice edge is given, where the retrieval uncertainties due to 3-D radiative effects are negligible.
Water soluble aerosols and gases at a UK background site – Part 1: Controls of PM2.5 and PM10 aerosol composition

There is limited availability of long-term, high temporal resolution, chemically speciated aerosol measurements which can provide further insight into the health and environmental impacts of particulate matter. The Monitor for AeRosols and Gases (MARGA, Applikon B.V., NL) allows for the characterisation of the inorganic components of PM10 and PM2.5 (NH4+, NO3-, SO42-, Cl-, Na+, K+, Ca2+, Mg2+) and inorganic reactive gases (NH3, SO2, HCl, HONO and HNO3) at hourly resolution. The following study presents 6.5 years (June 2006 to December 2012) of quasi-continuous observations of PM2.5 and PM10 using the MARGA at the UK EMEP supersite, Auchencorth Moss, SE Scotland. Auchencorth Moss was found to be representative of a remote European site with average total water soluble inorganic mass of PM2.5 of 3.82 μg m−3. Anthropogenically derived secondary inorganic aerosols (sum of NH4+, NO3- and nss-SO42−) were the dominating species (63 %) of PM2.5. In terms of equivalent concentrations, NH4+ provided the single largest contribution to PM2.5 fraction in all seasons. Sea salt was the main component (73 %) of the PMcoarse fraction (PM10-PM2.5), though NO3- was also found to make a relatively large contribution to the measured mass (17 %) providing evidence of considerable processing of sea salt in the coarse mode. There was on occasions evidence of aerosol from combustion events being transported to the site in 2012 as high K+ concentrations (deviating from the known ratio in sea salt) coincided with increases in black carbon at the site. Pollution events in PM10 (defined as concentrations > 12 μg m−3) were on average dominated by NH4+ and NO3-, where smaller loadings at the site tended to be dominated by sea salt. As with other western European sites, the charge balance of the inorganic components resolved were biased towards cations, suggesting the aerosol was basic or more likely that organic acids contributed to the charge balance. This study demonstrates the UK background atmospheric composition is primarily driven by meteorology with sea salt dominating air masses from the Atlantic Ocean and the Arctic, whereas secondary inorganic aerosols tended to dominate air masses from continental Europe.
Formation and aging of secondary organic aerosol from toluene: changes in chemical composition, volatility, and hygroscopicity

Secondary organic aerosol (SOA) is transformed after its initial formation, but this chemical aging of SOA is poorly understood. Experiments were conducted in the Carnegie Mellon environmental chamber to form secondary organic aerosol (SOA) from the photo-oxidation of toluene and other small aromatic volatile organic compounds (VOCs) in the presence of NOx under different oxidizing conditions. The effects of the oxidizing condition on organic aerosol (OA) composition, mass yield, volatility, and hygroscopicity were explored. Higher exposure to the hydroxyl radical resulted in different OA composition, average carbon oxidation state (OSc), and mass yield. The OA oxidation state generally increased during photo-oxidation, and the final OA OSc ranged from −0.29 to 0.16 in the performed experiments. The volatility of OA formed in these different experiments varied by as much as a factor of 30, demonstrating that the OA formed under different oxidizing conditions can have a significantly different saturation concentration. There was no clear correlation between hygroscopicity and oxidation state for this relatively hygroscopic SOA.
Climate responses to anthropogenic emissions of short-lived climate pollutants

Policies to control air quality focus on mitigating emissions of aerosols and their precursors, and other short-lived climate pollutants (SLCPs). On a local scale, these policies will have beneficial impacts on health and crop yields, by reducing particulate matter (PM) and surface ozone concentrations; however, the climate impacts of reducing emissions of SLCPs are less straightforward to predict. In this paper we consider a set of idealized, extreme mitigation strategies, in which the total anthropogenic emissions of individual SLCP emissions species are removed. This provides an upper bound on the potential climate impacts of such air quality strategies. We focus on evaluating the climate responses to changes in anthropogenic emissions of aerosol precursor species: black carbon (BC), organic carbon (OC) and sulphur dioxide (SO2). We perform climate integrations with four fully coupled atmosphere–ocean global climate models (AOGCMs), and examine the effects on global and regional climate of removing the total land-based anthropogenic emissions of each of the three aerosol precursor species. We find that the SO2 emissions reductions lead to the strongest response, with all models showing an increase in surface temperature focussed in the Northern Hemisphere mid and (especially) high latitudes, and showing a corresponding increase in global mean precipitation. Changes in precipitation patterns are driven mostly by a northward shift in the ITCZ (Intertropical Convergence Zone), consistent with the hemispherically asymmetric warming pattern driven by the emissions changes. The BC and OC emissions reductions give a much weaker response, and there is some disagreement between models in the sign of the climate responses to these perturbations. These differences between models are due largely to natural variability in sea-ice extent, circulation patterns and cloud changes. This large natural variability component to the signal when the ocean circulation and sea-ice are free-running means that the BC and OC mitigation measures do not necessarily lead to a discernible climate response.
Particulate matter, air quality and climate: lessons learned and future needs

The literature on atmospheric particulate matter (PM), or atmospheric aerosol, has increased enormously over the last 2 decades and amounts now to some 1500–2000 papers per year in the refereed literature. This is in part due to the enormous advances in measurement technologies, which have allowed for an increasingly accurate understanding of the chemical composition and of the physical properties of atmospheric particles and of their processes in the atmosphere. The growing scientific interest in atmospheric aerosol particles is due to their high importance for environmental policy. In fact, particulate matter constitutes one of the most challenging problems both for air quality and for climate change policies. In this context, this paper reviews the most recent results within the atmospheric aerosol sciences and the policy needs, which have driven much of the increase in monitoring and mechanistic research over the last 2 decades. The synthesis reveals many new processes and developments in the science underpinning climate–aerosol interactions and effects of PM on human health and the environment. However, while airborne particulate matter is responsible for globally important influences on premature human mortality, we still do not know the relative importance of the different chemical components of PM for these effects. Likewise, the magnitude of the overall effects of PM on climate remains highly uncertain. Despite the uncertainty there are many things that could be done to mitigate local and global problems of atmospheric PM. Recent analyses have shown that reducing black carbon (BC) emissions, using known control measures, would reduce global warming and delay the time when anthropogenic effects on global temperature would exceed 2 °C. Likewise, cost-effective control measures on ammonia, an important agricultural precursor gas for secondary inorganic aerosols (SIA), would reduce regional eutrophication and PM concentrations in large areas of Europe, China and the USA. Thus, there is much that could be done to reduce the effects of atmospheric PM on the climate and the health of the environment and the human population. A prioritized list of actions to mitigate the full range of effects of PM is currently undeliverable due to shortcomings in the knowledge of aerosol science; among the shortcomings, the roles of PM in global climate and the relative roles of different PM precursor sources and their response to climate and land use change over the remaining decades of this century are prominent. In any case, the evidence from this paper strongly advocates for an integrated approach to air quality and climate policies.
Black carbon emissions from Russian diesel sources: case study of Murmansk

Black carbon (BC) is a potent pollutant because of its effects on climate change, ecosystems and human health. Black carbon has a particularly pronounced impact as a climate forcer in the Arctic because of its effect on snow albedo and cloud formation. We have estimated BC emissions from diesel sources in the Murmansk Region and Murmansk City, the largest city in the world above the Arctic Circle. In this study we developed a detailed inventory of diesel sources including on-road vehicles, off-road transport (mining, locomotives, construction and agriculture), ships and diesel generators. For on-road transport, we conducted several surveys to understand the vehicle fleet and driving patterns, and, for all sources, we also relied on publicly available local data sets and analysis. We calculated that BC emissions in the Murmansk Region were 0.40 Gg in 2012. The mining industry is the largest source of BC emissions in the region, emitting 69 % of all BC emissions because of its large diesel consumption and absence of emissions controls. On-road vehicles are the second largest source, emitting about 13 % of emissions. Old heavy duty trucks are the major source of emissions. Emission controls on new vehicles limit total emissions from on-road transportation. Vehicle traffic and fleet surveys show that many of the older cars on the registry are lightly or never used. We also estimated that total BC emissions from diesel sources in Russia were 50.8 Gg in 2010, and on-road transport contributed 49 % of diesel BC emissions. Agricultural machinery is also a significant source Russia-wide, in part because of the lack of controls on off-road vehicles.
A tropospheric chemistry reanalysis for the years 2005–2012 based on an assimilation of OMI, MLS, TES, and MOPITT satellite data

We present the results from an 8-year tropospheric chemistry reanalysis for the period 2005–2012 obtained by assimilating multiple data sets from the OMI, MLS, TES, and MOPITT satellite instruments. The reanalysis calculation was conducted using a global chemical transport model and an ensemble Kalman filter technique that simultaneously optimises the chemical concentrations of various species and emissions of several precursors. The optimisation of both the concentration and the emission fields is an efficient method to correct the entire tropospheric profile and its year-to-year variations, and to adjust various tracers chemically linked to the species assimilated. Comparisons against independent aircraft, satellite, and ozonesonde observations demonstrate the quality of the analysed O3, NO2, and CO concentrations on regional and global scales and for both seasonal and year-to-year variations from the lower troposphere to the lower stratosphere. The data assimilation statistics imply persistent reduction of model error and improved representation of emission variability, but they also show that discontinuities in the availability of the measurements lead to a degradation of the reanalysis. The decrease in the number of assimilated measurements increased the ozonesonde-minus-analysis difference after 2010 and caused spurious variations in the estimated emissions. The Northern/Southern Hemisphere OH ratio was modified considerably due to the multiple-species assimilation and became closer to an observational estimate, which played an important role in propagating observational information among various chemical fields and affected the emission estimates. The consistent concentration and emission products provide unique information on year-to-year variations in the atmospheric environment.
Observations of relative humidity effects on aerosol light scattering in the Yangtze River Delta of China

Scattering of solar radiation by aerosol particles is highly dependent on relative humidity (RH) as hygroscopic particles take up water with increasing RH. To achieve a better understanding of the effect of aerosol hygroscopic growth on light scattering properties and radiative forcing, the aerosol scattering coefficients at RH in the range of 40 to ~ 90 % were measured using a humidified nephelometer system in the Yangtze River Delta of China in March 2013. In addition, the aerosol size distribution and chemical composition were measured. During the observation period, the mean and standard deviation (SD) of enhancement factors at RH = 85 % for the scattering coefficient (f(85 %)), backscattering coefficient (fb(85 %)), and hemispheric backscatter fraction (fβ(85 %)) were 1.58 ± 0.12, 1.25 ± 0.07, and 0.79 ± 0.04, respectively, i.e., aerosol scattering coefficient and backscattering coefficient increased by 58 and 25 % as the RH increased from 40 to 85 %. Concurrently, the aerosol hemispheric backscatter fraction decreased by 21 %. The relative amount of organic matter (OM) or inorganics in PM1 was found to be a main factor determining the magnitude of f(RH). The highest values of f(RH) corresponded to the aerosols with a small fraction of OM, and vice versa. The relative amount of NO3− in fine particles was strongly correlated with f(85 %), which suggests that NO3− played a vital role in aerosol hygroscopic growth during this study. The mass fraction of nitrate also had a close relationship to the curvature of the humidograms; higher mass fractions of nitrate were associated with humidograms that had the least curvature. Aerosol hygroscopic growth caused a 47 % increase in the calculated aerosol direct radiative forcing at 85 % RH, compared to the forcing at 40 % RH.
On the ability of a global atmospheric inversion to constrain variations of CO2 fluxes over Amazonia

The exchanges of carbon, water and energy between the atmosphere and the Amazon basin have global implications for the current and future climate. Here, the global atmospheric inversion system of the Monitoring of Atmospheric Composition and Climate (MACC) service is used to study the seasonal and interannual variations of biogenic CO2 fluxes in Amazonia during the period 2002–2010. The system assimilated surface measurements of atmospheric CO2 mole fractions made at more than 100 sites over the globe into an atmospheric transport model. The present study adds measurements from four surface stations located in tropical South America, a region poorly covered by CO2 observations. The estimates of net ecosystem exchange (NEE) optimized by the inversion are compared to an independent estimate of NEE upscaled from eddy-covariance flux measurements in Amazonia. They are also qualitatively evaluated against reports on the seasonal and interannual variations of the land sink in South America from the scientific literature. We attempt at assessing the impact on NEE of the strong droughts in 2005 and 2010 (due to severe and longer-than-usual dry seasons) and the extreme rainfall conditions registered in 2009. The spatial variations of the seasonal and interannual variability of optimized NEE are also investigated. While the inversion supports the assumption of strong spatial heterogeneity of these variations, the results reveal critical limitations of the coarse-resolution transport model, the surface observation network in South America during the recent years and the present knowledge of modelling uncertainties in South America that prevent our inversion from capturing the seasonal patterns of fluxes across Amazonia. However, some patterns from the inversion seem consistent with the anomaly of moisture conditions in 2009.