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Cloud condensation nuclei as a modulator of ice processes in Arctic mixed-phase clouds

We propose that cloud condensation nuclei (CCN) concentrations are important for modulating ice formation of Arctic mixed-phase clouds, through modification of the droplet size distribution. Aircraft observations from the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) study in northern Alaska in April 2008 allow for identification and characterization of both aerosol and trace gas pollutants, which are then compared with cloud microphysical properties. Consistent with previous studies, we find that the concentration of precipitating ice particles (>400 μm) is correlated with the concentration of large droplets (>30 μm). We are further able to link the observed microphysical conditions to aerosol pollution, originating mainly from long range transport of biomass burning emissions. The case studies demonstrate that polluted mixed-phase clouds have narrower droplet size distributions and contain 1–2 orders of magnitude fewer precipitating ice particles than clean clouds at the same temperature. This suggests an aerosol indirect effect leading to greater cloud lifetime, greater cloud emissivity, and reduced precipitation. This result is opposite to the glaciation indirect effect, whereby polluted clouds are expected to precipitate more readily due to an increase in the concentration of particles acting as ice nuclei.
The effects of a solar eclipse on photo-oxidants in different areas of China

This study investigates the effects of the total solar eclipse of 22 July 2009 on surface ozone and other photo-oxidants over China. A box model was used to study the sensitivity of ozone to the limb darkening effect during an eclipse event, and to show that the impact on ozone is small (less than 0.5 %). In addition, the regional model WRF-Chem was applied to study the effects of the eclipse on meteorological and chemical parameters, focusing on different regions in China. Chemical and meteorological observations were used to validate the model and to show that it can capture the effects of the total solar eclipse well. Model calculations show distinct differences in the spatial distributions of meteorological and chemical parameters with and without the eclipse. The maximum impacts of the eclipse occur over the area of totality, where there is a decrease in surface temperature of 1.5 °C and decrease in wind speed of 1 m s−1. The maximum impacts on atmospheric pollutants occur over parts of north and east China where emissions are greater, with an increase of 5 ppbv in NO2 and 25 ppbv in CO and a decrease of 10 ppbv in O3 and 4 ppbv in NO. This study also demonstrates the effects of the solar eclipse on surface photo-oxidants in different parts of China. Although the sun was obscured to a smaller extent in polluted areas than in clean areas, the impacts of the eclipse in polluted areas are greater and last longer than they do in clean areas. In contrast, the change in radical concentrations (OH, HO2 and NO3) in clean areas is much larger than in polluted areas mainly because of the limited source of radicals in these areas. The change in radical concentrations during the eclipse reveals that nighttime chemistry dominates in both clean and polluted areas. As solar eclipses provide a natural opportunity to test more thoroughly our understanding of atmospheric chemistry, especially that governed by photolysis, a comprehensive experimental campaign during a future solar eclipse is highly desirable.
Acetone variability in the upper troposphere: analysis of CARIBIC observations and LMDz-INCA chemistry-climate model simulations

This paper investigates the acetone variability in the upper troposphere (UT) as sampled during the CARIBIC airborne experiment and simulated by the LMDz-INCA global chemistry climate model. The aim is to (1) describe spatial distribution and temporal variability of acetone; (2) propose benchmarks deduced from the observed data set; and (3) investigate the representativeness of the observational data set. According to the model results, South Asia (including part of the Indian Ocean, all of India, China, and the Indochinese peninsula) and Europe (including Mediterranean Sea) are net source regions of acetone, where nearly 25 % of North Hemispheric (NH) primary emissions and nearly 40 % of the NH chemical production of acetone take place. The impact of these net source regions on continental upper tropospheric acetone is studied by analysing CARIBIC observations of 2006 and 2007 when most flight routes stretched between Frankfurt (Germany) and Manila (Philippines), and by focussing over 3 sub-regions where acetone variability is strong: Europe-Mediterranean, Central South China and South China Sea. Important spatial variability was observed over different scales: (1) east-west positive gradient of annually averaged acetone vmr in UT over the Eurasian continent, namely a factor two increase from east to west; (2) ocean/continent contrast with 50 % enhancement over the continents; (3) the acetone volume mixing ration (vmr) may vary in summer by more than 1000 pptv within only 5 latitude-longitude degrees; (4) the standard deviation for measurements acquired during a short flight sequence over a sub-region may reach 40 %. Temporal variability is also important: (1) the acetone volume mixing ratio (vmr) in the UT varies with the season, increasing from winter to summer by a factor 2 to 4; (2) a difference as large as 200 pptv may be observed between successive inbound and outbound flights over the same sub-region due to different flight specifications (trajectory in relation to the plume, time of day). A satisfactory agreement for the abundance of acetone is found between model results and observations, with e.g. only 30 % overestimation of the annual average over Central-South China and the South China Sea (between 450 and 600 pptv), and an underestimation by less than 20 % over Europe-Mediterranean (around 800 pptv). Consequently, annual budget terms could be computed with LMDz-INCA, yielding a global atmospheric burden of 7.2 Tg acetone, a 127 Tg yr−1 global source/sink strength, and a 21-day mean residence time. Moreover the study shows that LMDz-INCA can reproduce the impact of summer convection over China when boundary layer compounds are lifted to cruise altitude of 10–11 km and higher. The consequent enhancement of acetone vmr during summer is reproduced by LMDz-INCA, to reach agreement on an observed maximum of 970 ± 400 pptv (average during each flight sequence over the defined zone ± standard deviation). The summer enhancement of acetone is characterized by a high spatial and temporal heterogeneity, showing the necessity to increase the airborne measurement frequency over Central-South China and the South China Sea in August and September, when the annual maximum is expected (daily average model values reaching potentially 3000 pptv). In contrast, the annual cycle in the UT over Europe-Mediterranean is not reproduced by LMDz-INCA, in particular the observed summer enhancement of acetone to 1400 ± 400 pptv after long-range transport of free tropospheric air masses over North Atlantic Ocean is not reproduced. In view of the agreement on the acetone annual cycle at surface level, this disagreement in UT over Europe indicates misrepresentation of simulated transport of primary acetone or biased spatial distribution of acetone chemical sinks and secondary sources. The sink and source budget in long-range transported free tropospheric air masses may be studied by analysing atmospheric chemical composition observed by CARIBIC in summer flights between North America and Europe.
European source and sink areas of CO2 retrieved from Lagrangian transport model interpretation of combined O2 and CO2 measurements at the high alpine research station Jungfraujoch

The University of Bern monitors carbon dioxide (CO2) and oxygen (O2) at the High Altitude Research Station Jungfraujoch since the year 2000 by means of flasks sampling and since 2005 using a continuous in situ measurement system. This study investigates the transport of CO2 and O2 towards Jungfraujoch using backward Lagrangian Particle Dispersion Model (LPDM) simulations and utilizes CO2 and O2 signatures to classify air masses. By investigating the simulated transport patterns associated with distinct CO2 concentrations it is possible to decipher different source and sink areas over Europe. The highest CO2 concentrations, for example, were observed in winter during pollution episodes when air was transported from Northeastern Europe towards the Alps, or during south Foehn events with rapid uplift of polluted air from Northern Italy, as demonstrated in two case studies. To study the importance of air-sea exchange for variations in O2 concentrations at Jungfraujoch the correlation between CO2 and APO (Atmospheric Potential Oxygen) deviations from a seasonally varying background was analyzed. Anomalously high APO concentrations were clearly associated with air masses originating from the Atlantic Ocean, whereas low APO concentrations were found in air masses advected either from the east from the Eurasian continent in summer, or from the Eastern Mediterranean in winter. Those air masses with low APO in summer were also strongly depleted in CO2 suggesting a combination of CO2 uptake by vegetation and O2 uptake by dry summer soils. Other subsets of points in the APO-CO2 scatter plot investigated with respect to air mass origin included CO2 and APO background values and points with regular APO but anomalous CO2 concentrations. Background values were associated with free tropospheric air masses with little contact with the boundary layer during the last few days, while high or low CO2 concentrations reflect the various levels of influence of anthropogenic emissions and the biosphere. The pronounced cycles of CO2 and O2 exchanges with the biosphere and the ocean cause clusters of points and lead to a seasonal pattern.
Elucidating determinants of aerosol composition through particle-type-based receptor modeling

An aerosol time-of-flight mass spectrometer (ATOFMS) was deployed at a semi-rural site in southern Ontario to characterize the size and chemical composition of individual particles. Particle-type-based receptor modelling of these data was used to investigate the determinants of aerosol chemical composition in this region. Individual particles were classified into particle-types and positive matrix factorization (PMF) was applied to their temporal trends to separate and cross-apportion particle-types to factors. The extent of chemical processing for each factor was assessed by evaluating the internal and external mixing state of the characteristic particle-types. The nine factors identified helped to elucidate the coupled interactions of these determinants. Nitrate-laden dust was found to be the dominant type of locally emitted particles measured by ATOFMS. Several factors associated with aerosol transported to the site from intermediate local-to-regional distances were identified: the Organic factor was associated with a combustion source to the north-west; the ECOC Day factor was characterized by nearby local-to-regional carbonaceous emissions transported from the south-west during the daytime; and the Fireworks factor consisted of pyrotechnic particles from the Detroit region following holiday fireworks displays. Regional aerosol from farther emissions sources was reflected through three factors: two Biomass Burning factors and a highly chemically processed Long Range Transport factor. The Biomass Burning factors were separated by PMF due to differences in chemical processing which were in part elucidated by the passage of two thunderstorm gust fronts with different air mass histories. The remaining two factors, ECOC Night and Nitrate Background, represented the night-time partitioning of nitrate to pre-existing particles of different origins. The distinct meteorological conditions observed during this month-long study in the summer of 2007 provided a unique range of temporal variability, enabling the elucidation of the determinants of aerosol chemical composition, including source emissions, chemical processing, and transport, at the Canada-US border. This paper presents the first study to elucidate the coupled influences of these determinants on temporal variability in aerosol chemical composition using single particle-type-based receptor modelling.
Detection from space of a reduction in anthropogenic emissions of nitrogen oxides during the Chinese economic downturn

Rapid economic and industrial development in China and relatively weak emission controls have resulted in significant increases in emissions of nitrogen oxides (NOx) in recent years, with the exception of late 2008 to mid 2009 when the economic downturn led to emission reductions detectable from space. Here vertical column densities (VCDs) of tropospheric NO2 retrieved from satellite observations by SCIAMACHY, GOME-2 and OMI (both by KNMI and by NASA) are used to evaluate changes in emissions of NOx from October 2004 to February 2010 identifying impacts of the economic downturn. Data over polluted regions of Northern East China suggest an increase of 27–33 % in 12-month mean VCD of NO2 prior to the downturn, consistent with an increase of 49 % in thermal power generation (TPG) reflecting the economic growth. More detailed analysis is used to quantify changes in emissions of NOx in January over the period 2005–2010 when the effect of the downturn was most evident. The GEOS-Chem model is employed to evaluate the effect of changes in chemistry and meteorology on VCD of NO2. This analysis indicates that emissions decreased by 20 % from January 2008 to January 2009, close to the reduction of 18 % in TPG that occurred over the same interval. A combination of three independent approaches indicates that the economic downturn was responsible for a reduction in emissions by 9–11 % in January 2009 with an additional decrease of 10 % attributed to the slow-down in industrial activity associated with the coincident celebration of the Chinese New Year; errors in the estimate are most likely less than 3.4 %.
Variability of aerosol optical properties in the Western Mediterranean Basin

Aerosol light scattering, absorption and particulate matter (PM) concentrations were measured at Montseny, a regional background site in the Western Mediterranean Basin (WMB) which is part of the European Supersite for Atmospheric Aerosol Research (EUSAAR). Off line analyses of 24 h PM filters collected with Hi-Vol instruments were performed for the determination of the main chemical components of PM. Mean scattering and hemispheric backscattering coefficients (@ 635 nm) were 26.6±23.2 Mm−1 and 4.3±2.7 Mm−1, respectively and the mean aerosol absorption coefficient (@ 637 nm) was 2.8±2.2 Mm−1. Mean values of Single Scattering Albedo (SSA) and Ångström exponent (å) (calculated from 450 nm to 635 nm) at MSY were 0.90±0.05 and 1.3±0.5 respectively. A clear relationship was observed between the PM1/PM10 and PM2.5/PM10 ratios as a function of the calculated Ångström exponents. Mass scattering cross sections (MSC) for fine mass and sulfate at 635 nm were 2.8±0.5 m2 g−1 and 11.8±2.2 m2 g−1, respectively, while the mean aerosol absorption cross section (MAC) was 10.4±2.0 m2 g−1. The variability in aerosol optical properties in the WMB were largely explained by the origin and ageing of air masses over the measurement site. The MAC values appear dependent of particles aging: similar to the expected absorption cross-section for fresh emissions under Atlantic Advection episodes and higher under aerosol pollution episodes. The analysis of the Ångström exponent as a function of the origin the air masses revealed that polluted winter anticyclonic conditions and summer recirculation scenarios typical of the WMB led to an increase of fine particles in the atmosphere (å = 1.5±0.1) while the aerosol optical properties under Atlantic Advection episodes and Saharan dust outbreaks were clearly dominated by coarser particles (å = 1.0±0.4). The sea breeze played an important role in transporting pollutants from the developed WMB coastlines towards inland rural areas, changing the optical properties of aerosols. Aerosol scattering and backscattering coefficients increased by around 40 % in the afternoon when the sea breeze was fully developed while the absorption coefficient increased by more than 100 % as a consequence of the increase in the equivalent black carbon concentration (EBC) observed at MSY under sea breeze circulation.
Gaseous pollutants in Beijing urban area during the heating period 2007–2008: variability, sources, meteorological, and chemical impacts

Gaseous pollutants, NOy/NOx, SO2, CO, and O3, were measured at an urban site in Beijing from 17 November 2007 to 15 March 2008. The average concentrations (with ± 1σ) of NO, NO2, NOx, NOy, CO, SO2, and O3 were 29.0 ± 2.7 ppb, 33.7 ± 1.4 ppb, 62.7 ± 4.0 ppb, 72.8 ± 4.5 ppb, 1.99 ± 0.13 ppm, 31.9 ± 2.0 ppb, and 11.9 ± 0.8 ppb, respectively, with hourly maxima of 200.7 ppb, 113.5 ppb, 303.9 ppb, 323.2 ppb, 15.06 ppm, 147.3 ppb, and 69.7 ppb, respectively. The concentrations of the pollutants show "saw-toothed" patterns, which are attributable mainly to changes in wind direction and speed. The frequency distributions of the hourly mean concentrations of NOy, SO2, CO, and O3 can all be decomposed in the two Lorentz curves, with their peak concentrations representing background levels under different conditions. During the observation period, the average ratio NOx/NOy was 0.86 ± 0.10, suggesting that the gaseous pollutants in Beijing in winter are mainly from local emissions. Data of O3, NOz, and NOx/NOy indicate that photochemistry can take place in Beijing even in the cold winter period. Based on the measurements of O3, NOx, and NOy, ozone production efficiency (OPE) is estimated to be in the range of 0–8.9 (ppb ppb−1) with the mean(± 1σ) and median values being 1.1(± 1.6) and 0.5 (ppb ppb−1), respectively, for the winter 2007–2008 in Beijing. This low OPE would cause a photochemical O3 source of 5 ppb day−1, which is small but significant for surface O3 in winter in Beijing. Downward transport of O3-rich air from the free troposphere is the more important factor for the enhancement of the O3 level in the surface layer, while high NO level for the destruction of O3. The concentrations of SO2, CO, and NOx are strongly correlated among each other, indicating that they are emitted by some common sources. Multiple linear regression analysis is applied to the concentrations of NOy, SO2, and CO and empirical equations are obtained for the NOy concentration. Based the equations, the relative contributions from mobile and point sources to NOy is estimated to be 66 ± 30 % and 40 ± 16 %, respectively, suggesting that even in the heating period, mobile sources in Beijing contribute more to NOy than point sources.
Characteristics, seasonality and sources of carbonaceous and ionic components in the tropical aerosols from Indian region

To better characterize the tropical aerosols in Indian region, PM10 samples collected from Chennai, India (13.04° N; 80.17° E) were analyzed for carbonaceous and water-soluble ionic components. Concentration ranges of elemental carbon (EC) and organic carbon (OC) were 2.4–14 μg m−3 (ave. 6.5 μg m−3) and 3.2–15.6 μg m−3 (ave. 9.1 μg m−3) in winter samples whereas they were 1.1–2.5 μg m−3 (ave. 1.6 μg m−3) and 4.1–17.6 μg m−3 (ave. 9.7 μg m−3) in summer samples, respectively. Concentration of secondary organic carbon (SOC) retrieved from EC-tracer method was 4.6±2.8 μg m−3 in winter and 4.3±2.8 μg m−3 in summer. OC accounted for 38.5±14 % (n = 49) of combined concentrations of carbonaceous and ionic components in PM10. We also found that OC concentrations are generally higher than those of SO42− (8.8±2.5 μg m−3 and 4.1±2.7 μg m−3 in winter and summer, respectively), which was the most abundant ionic species (57 %) followed by NH4+ (15 %) >NO3−>Cl−>K+>Na+> Ca2+>MSA−>Mg2+. The mass fractions of EC, organic matter (OM) and ionic species varied seasonally, following the air mass trajectories and corresponding source strength. Based on mass concentration ratios of selected components and relations of EC and OC to marker species, we found that biofuel/biomass burning is a major source of atmospheric aerosols in South and Southeast Asia. The high concentrations of SOC and WSOC/OC ratios (ave. 0.45; n = 49) as well as good correlations between SOC and WSOC suggest that the secondary production of organic aerosols during long-range atmospheric transport is also significant in this region. This study provides the baseline data of carbonaceous aerosols for southern part of the Indian subcontinent.
Analysis of the formation of fog and haze in North China Plain (NCP)

North China Plain (NCP) is one of the most populated and polluted regions in China. During the recent years, haze and fog occur frequently and cause severely low visibility in this region. In order to better understand the impact of aerosol particles on the formation of haze and fog, a long-term record of haze and fog occurrences in the past 56 yr (from 1954–2009) over NCP is analyzed. The results show that there are rapid changes in the occurrences of haze and fog over NCP. The occurrences of haze and fog were low during 1970–1980, and reached a maximum during 1981–1998. After 1999, the occurrences of haze and fog slightly decreased. There was a nonlinear relationship between the occurrences of haze and fog. When the occurrence of haze was lower than 40 days yr−1, the occurrence of fog was strongly proportional to the occurrence of haze. However, when the occurrence of haze was high (larger than 75 days yr−1), the occurrence of fog was not sensitive to the occurrence of haze. In order to better understand the relationship between the occurrences of haze and fog as well as the effect of aerosol particles on the formation of haze and fog, an in-situ field experiment was conducted during a period with a mixed occurrence of haze and fog. The analysis of the experiment suggests that there were considerably high aerosol concentrations during the measurement period with an averaged aerosol number concentration of 24 000 cm−3. The measurement also shows that a large amount of aerosol particles can act as condensation nuclei to enhance the formation of fog droplets. As a result, a large amount of fog droplets (>1000 cm−3) with small size (5–6 μm) were observed during the fog period, resulting in extremely low visibility (less than 100 m).