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Through long-range transport of dust, the North-African desert supplies essential minerals to the Amazon rain forest. Since North African dust reaches South America mostly during the Northern Hemisphere winter, the dust sources active during winter are the main contributors to the forest. Given that the Bodélé depression area in southwestern Chad is the main winter dust source, a close link is expected between the Bodélé emission patterns and volumes and the mineral supply flux to the Amazon. <br><br> Until now, the particular link between the Bodélé and the Amazon forest was based on sparse satellite measurements and modeling studies. In this study, we combine a detailed analysis of space-borne and ground data with reanalysis model data and surface measurements taken in the central Amazon during the Amazonian Aerosol Characterization Experiment (AMAZE-08) in order to explore the validity and the nature of the proposed link between the Bodélé depression and the Amazon forest. <br><br> This case study follows the dust events of 11–16 and 18–27 February 2008, from the emission in the Bodélé over West Africa (most likely with contribution from other dust sources in the region) the crossing of the Atlantic Ocean, to the observed effects above the Amazon canopy about 10 days after the emission. The dust was lifted by surface winds stronger than 14 m s<sup>−1</sup>, usually starting early in the morning. The lofted dust, mixed with biomass burning aerosols over Nigeria, was transported over the Atlantic Ocean, and arrived over the South American continent. The top of the aerosol layer reached above 3 km, and the bottom merged with the boundary layer. The arrival of the dusty air parcel over the Amazon forest increased the average concentration of aerosol crustal elements by an order of magnitude.
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Column-averaged volume mixing ratios of carbon dioxide (<i>X</i><sub>CO<sub>2</sub></sub>) during the period from January 2007 to May 2008 over Tsukuba, Japan, were derived using CO<sub>2</sub> concentrations measured by Continuous CO<sub>2</sub> Measuring Equipment (CME). The CMEs were installed on Japan Airlines Corporation (JAL) commercial airliners, which frequently fly to and from Narita Airport. It was assumed that CO<sub>2</sub> profiles over Tsukuba and Narita are the same. CO<sub>2</sub> profile data for 493 flights on clear-sky days were analyzed in order to calculate <i>X</i><sub>CO<sub>2</sub></sub> with one of two ancillary datasets: "Tsukuba observational" data (rawinsonde and meteorological tower), or "global" forecast/reanalysis and climatological data (NCEP and CIRA-86). The amplitude of the seasonal variation of <i>X</i><sub>CO<sub>2</sub></sub> using the ancillary data measured in Tsukuba (<i>X</i><sub>CO<sub>2</sub></sub> (Tsukuba observational)) was determined by a least squares fit using a harmonic function to roughly evaluate the seasonal variation over Tsukuba. The highest and lowest values of the obtained fitted curve in 2007 for <i>X</i><sub>CO<sub>2</sub></sub> (Tsukuba observational) were 386.4 ± 1.0 and 381.7 ± 1.0 ppm in May and September, respectively, where the errors represent 1 standard deviation of the fit residuals. The dependence of <i>X</i><sub>CO<sub>2</sub></sub> on the type of ancillary dataset was evaluated. The average difference between <i>X</i><sub>CO<sub>2</sub></sub> from global climatological data, <i>X</i><sub>CO<sub>2</sub></sub> (global), and <i>X</i><sub>CO<sub>2</sub></sub> (Tsukuba observational), i.e., the bias of <i>X</i><sub>CO<sub>2</sub></sub> (global) based on <i>X</i><sub>CO<sub>2</sub></sub> (Tsukuba observational), was found to be −0.621 ppm with a standard deviation of 0.682 ppm. The uncertainty of <i>X</i><sub>CO<sub>2</sub></sub> (global) based on <i>X</i><sub>CO<sub>2</sub></sub> (Tsukuba observational) was estimated to be 0.922 ppm. This small uncertainty relative to the GOSAT precision suggests that calculating <i>X</i><sub>CO<sub>2</sub></sub> using data from airliners and global climatological data can be applied to the validation of GOSAT products for <i>X</i><sub>CO<sub>2</sub></sub> over airports worldwide.
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Sander et al. (2006) proposed that CaCO<sub>3</sub> precipitation can be an important factor in triggering tropospheric ozone depletion events. Recently, Morin et al. (2008b) presented calculations with the FREZCHEM model and concluded that their results and interpretation cast doubt on the validity of this hypothesis. In this joint publication, we have re-analyzed the implications of the FREZCHEM results and show how they can be reconciled with the proposal of Sander et al. (2006). The chemical predictions of both approaches are consistent. Although an interpretation solely based on the alkalinity change in the brine does not support the conclusion of Sander et al. (2006), we show that the bromide/alkalinity ratio (which increases during the cooling of the brine) can be used as an indicator of the potential for triggering bromine explosions.
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Airborne measurements from two consecutive days, analysed with the aid of an aerosol-adiabatic cloud parcel model, are used to study the effect of carbonaceous aerosol particles on the reflectivity of sunlight by water clouds. The measurements, including aerosol chemistry, aerosol microphysics, cloud microphysics, cloud gust velocities and cloud light extinction, were made below, in and above stratocumulus over the northwest Atlantic Ocean. On the first day, the history of the below-cloud fine particle aerosol was marine and the fine particle sulphate and organic carbon mass concentrations measured at cloud base were 2.4 μg m<sup>−3</sup> and 0.9 μg m<sup>−3</sup> respectively. On the second day, the below-cloud aerosol was continentally influenced and the fine particle sulphate and organic carbon mass concentrations were 2.3 μg m<sup>−3</sup> and 2.6 μg m<sup>−3</sup> respectively. Over the range 0.06–0.8 μm diameter, the shapes of the below-cloud size distributions were similar on both days and the number concentrations were approximately a factor of two higher on the second day. The cloud droplet number concentrations (CDNC) on the second day were approximately three times higher than the CDNC measured on the first day. Using the parcel model to separate the influence of the differences in gust velocities, we estimate from the vertically integrated cloud light scattering measurements a 6% increase in the cloud albedo principally due to the increase in the carbonaceous components on the second day. Assuming no additional absorption by this aerosol, a 6% albedo increase translates to a local daytime radiative cooling of ∼12 W m<sup>−2</sup>. This result provides observational evidence that the role of anthropogenic carbonaceous components in the cloud albedo effect can be much larger than that of anthropogenic sulphate, as some global simulations have indicated.
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Hypothetical reductions in future emissions of ozone-depleting substances (ODSs) and N<sub>2</sub>O are evaluated in terms of effects on equivalent effective stratospheric chlorine (EESC), globally-averaged total column ozone, and radiative forcing through 2100. Due to the established success of the Montreal Protocol, these actions can have only a fraction of the impact on ozone depletion that regulations already in force have had. If all anthropogenic ODS and N<sub>2</sub>O emissions were halted beginning in 2011, ozone is calculated to be higher by about 1–2% during the period 2030–2100 compared to a case of no additional restrictions. Direct radiative forcing by 2100 would be about 0.23 W/m<sup>2</sup> lower from the elimination of anthropogenic N<sub>2</sub>O emissions and about 0.005 W/m<sup>2</sup> lower from the destruction of the chlorofluorocarbon (CFC) bank. Due to the potential impact of N<sub>2</sub>O on future ozone levels, we provide an approach to incorporate it into the EESC formulation, which is used extensively in ozone depletion analyses. The ability of EESC to describe total ozone changes arising from additional ODS and N<sub>2</sub>O controls is also quantified.
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Absorbing aerosols (AAs) such as black carbon (BC) or dust absorb incoming solar radiation, perturb the temperature structure of the atmosphere, and influence cloud cover. Previous studies have described conditions under which AAs either increase or decrease cloud cover. The effect depends on several factors, including the altitude of the AA relative to the cloud and the cloud type. We attempt to categorize the effects into several likely regimes. Cloud cover is decreased if the AAs are embedded in the cloud layer. AAs below cloud may enhance convection and cloud cover. AAs above cloud top stabilize the underlying layer and tend to enhance stratocumulus clouds but may reduce cumulus clouds. AAs can also promote cloud cover in convergent regions as they enhance deep convection and low level convergence as it draws in moisture from ocean to land regions. Most global model studies indicate a regional variation in the cloud response but generally increased cloud cover over oceans and some land regions, with net increased low-level and/or reduced upper level cloud cover. The result is a net negative semi-direct effect feedback from the cloud response to AAs. In some of these climate model studies, the cooling effect of BC due to cloud changes is strong enough to essentially cancel the warming direct effects.
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In May 2008, the measurement campaign IMPACT for observation of atmospheric aerosol and cloud properties was conducted in Cabauw, The Netherlands. With a nudged version of the coupled aerosol-climate model ECHAM5-HAM we simulate the size distribution and chemical composition of the aerosol and the associated aerosol optical thickness (AOT) for the campaign period. Synoptic scale meteorology is represented realistically through nudging of the vorticity, the divergence, the temperature and the surface pressure. Simulated concentrations of aerosol sulfate and organics at the surface are generally within a factor of two from observed values. The monthly averaged AOT from the model is 0.33, about 20% larger than observed. For selected periods of the month with relatively dry and moist conditions discrepancies are approximately −30% and +15%, respectively. Discrepancies during the dry period are partly caused by inaccurate representation of boundary layer (BL) dynamics by the model affecting the simulated AOT. The model simulates too strong exchange between the BL and the free troposphere, resulting in weaker concentration gradients at the BL top than observed for aerosol and humidity, while upward mixing from the surface layers into the BL appears to be underestimated. The results indicate that beside aerosol sulfate and organics also aerosol ammonium and nitrate significantly contribute to aerosol water uptake. The simulated day-to-day variability of AOT follows synoptic scale advection of humidity rather than particle concentration. Even for relatively dry conditions AOT appears to be strongly influenced by the diurnal cycle of RH in the lower boundary layer, further enhanced by uptake and release of nitric acid and ammonia by aerosol water.
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In addition to microphysical changes in clouds, changes in nucleation processes of ice cloud due to aerosols would result in substantial changes in cloud top temperature as mildly supercooled clouds are glaciated through heterogenous nucleation processes. Measurements from multiple sensors on multiple observing platforms over the Atlantic Ocean show that the cloud effective temperature increases with mineral dust loading with a slope of +3.06 °C per unit aerosol optical depth. The macrophysical changes in ice cloud top distributions as a consequence of mineral dust-cloud interaction exert a strong cooling effect (up to 16 Wm<sup>−2</sup>) of thermal infrared radiation on cloud systems. Induced changes of ice particle size by mineral dusts influence cloud emissivity and play a minor role in modulating the outgoing longwave radiation for optically thin ice clouds. Such a strong cooling forcing of thermal infrared radiation would have significant impacts on cloud systems and subsequently on climate.
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Semivolatile organic and inorganic aerosol species partition between the gas and aerosol particle phases to maintain thermodynamic equilibrium. Liquid-liquid phase separation into an organic-rich and an aqueous electrolyte phase can occur in the aerosol as a result of the salting-out effect. Such liquid-liquid equilibria (LLE) affect the gas/particle partitioning of the different semivolatile compounds and might significantly alter both particle mass and composition as compared to a one-phase particle. We present a new liquid-liquid equilibrium and gas/particle partitioning model, using as a basis the group-contribution model AIOMFAC (Zuend et al., 2008). This model allows the reliable computation of the liquid-liquid coexistence curve (binodal), corresponding tie-lines, the limit of stability/metastability (spinodal), and further thermodynamic properties of multicomponent systems. Calculations for ternary and multicomponent alcohol/polyol-water-salt mixtures suggest that LLE are a prevalent feature of organic-inorganic aerosol systems. A six-component polyol-water-ammonium sulphate system is used to simulate effects of relative humidity (RH) and the presence of liquid-liquid phase separation on the gas/particle partitioning. RH, salt concentration, and hydrophilicity (water-solubility) are identified as key features in defining the region of a miscibility gap and govern the extent to which compound partitioning is affected by changes in RH. The model predicts that liquid-liquid phase separation can lead to either an increase or decrease in total particulate mass, depending on the overall composition of a system and the particle water content, which is related to the hydrophilicity of the different organic and inorganic compounds. Neglecting non-ideality and liquid-liquid phase separations by assuming an ideal mixture leads to an overestimation of the total particulate mass by up to 30% for the composition and RH range considered in the six-component system simulation. For simplified partitioning parametrizations, we suggest a modified definition of the effective saturation concentration, <i>C</i><sub>j</sub><sup>*</sup>, by including water and other inorganics in the absorbing phase. Such a <i>C</i><sub>j</sub><sup>*</sup> definition reduces the RH-dependency of the gas/particle partitioning of semivolatile organics in organic-inorganic aerosols by an order of magnitude as compared to the currently accepted definition, which considers the organic species only.
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The "Blue Sky Project" was proposed in 1998 to investigate by how much emissions should be reduced to increase blue sky frequency in Beijing, which hosted the Summer Olympics in 2008. This paper focuses on the temporal variation of visibility and its dependence on meteorological conditions and suspended particles at Beijing using the hourly observed visibility data at Beijing Capital International Airport (BCIA) from 1999 to 2007. It has been found that about 47.8% (24.2%) of the hours in Beijing are "bad" ("good") hours with visibility below 10 km (equal or higher than 20 km) between 1999 and 2007. Due to the high Relative Humidity (RH), summer is the season with the lowest mean visibility in a year. Although PM<sub>10</sub> index was reported in a decreasing trend (Chan and Yao, 2008), the increase of RH has resulted in a decreasing trend of visibility over BCIA in the summer from 1999 to 2007. To ensure blue sky ("good" visibility) for Olympics 2008, daily mean PM<sub>10</sub> index should have been reduced from 81 to 44. This requires that not only vehicle emissions, but also other emissions should be limited. Observations verify that blue-sky-hour rate increased significantly after mean PM<sub>10</sub> index was reduced to 53 during Olympics 2008, however, the visibility of 2009 returned to the mean level from 1999 to 2007 during the period 8−24 August. RH (aerosol) contribute 24% (76%) of the improvement of visibility during August 2008.
