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A small airplane made 597 aerosol optical property (light absorption and light scattering) vertical profile measurements over a rural Oklahoma site between March 2000 and December 2007. The aerosol profiles obtained during these 8 yr of measurements suggest significant seasonal differences in aerosol loading (scattering and absorption). The highest amounts of scattering and absorbing aerosol are observed during the summer and the lowest loading occurs during the winter. The relative contribution of aerosol absorption is highest in the winter (i.e., single scattering albedo is lowest in winter), particularly aloft. Aerosol absorption generally decreased with altitude below ~1.5 km and then was relatively constant or decreased more gradually above that. Aerosol scattering decreased sharply with altitude below ~1.5 km but, unlike absorption, also decreased at higher altitudes, albeit less sharply. Scattering Ångström exponents suggest that the aerosol was dominated by sub-micron aerosol during the summer at all altitudes, but that larger particles were present, especially in the spring and winter above 1 km. The seasonal variability observed for aerosol loading is consistent with AERONET aerosol optical depth (AOD) although the AOD values calculated from in situ adjusted to ambient conditions and matching wavelengths are up to a factor of two lower than AERONET AOD values depending on season. The column averaged single scattering albedo derived from in situ airplane measurements are similar in value to the AERONET single scattering albedo inversion product but the seasonal patterns are different – possibly a consequence of the strict constraints on obtaining single scattering albedo from AERONET data. A comparison of extinction Ångström exponent and asymmetry parameter from the airplane and AERONET platforms suggests similar seasonal variability with smaller particles observed in the summer and fall and larger particles observed in spring and winter. The observed seasonal cycle of aerosol loading corresponds with changes in air mass back trajectories: the aerosol scattering was higher when transport was from polluted areas (e.g., the Gulf Coast) and lower when the air came from cleaner regions and/or the upper atmosphere.
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SOA formation from benzene, toluene, <i>m</i>-xylene, and their corresponding phenolic compounds were investigated using the UCR/CE-CERT Environmental Chamber to evaluate the importance of phenolic compounds as intermediate species in aromatic SOA formation. SOA formation yield measurements coupled to gas-phase yield measurements indicate that approximately 20% of the SOA of benzene, toluene, and <i>m</i>-xylene could be ascribed to the phenolic route under low NO<sub>x</sub> conditions. The SOA densities tend to be initially as high as approximately 1.8 g cm<sup>−3</sup> and eventually reach the range of 1.3–1.4 g cm<sup>−3</sup>. The final SOA density was found to be independent of elemental ratio (O/C) indicating that applying constant density (e.g., 1.4 g cm<sup>−3</sup>) to SOA formed from different aromatic compounds tested in this study is a reasonable approximation. Results from a novel on-line PILS-TOFMS (Particle-into-Liquid Sampler coupled with Agilent Time-of-Flight Mass Spectrometer) are reported. Major signals observed by the on-line/off-line Agilent TOFMS indicated that products had the same number of carbon atoms as their parent aromatics, suggesting importance of ring-retaining products or ring-opening products following ring-cleavage.
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Since 1999 Cairo and the Nile delta region have suffered from air pollution episodes called the "black cloud" during the fall season. These have been attributed to either burning of agriculture waste or long-range transport of desert dust. Here we present a detailed analysis of the optical and microphysical aerosol properties, based on satellite data. Monthly mean values of Moderate Resolution Imaging Spectroradiometer (MODIS) aerosol optical depth (AOD) at 550 nm were examined for the 10 yr period from 2000–2009. Significant monthly variability is observed in the AOD with maxima in April or May (~0.5) and October (~0.45), and a minimum in December and January (~0.2). Monthly mean values of UV Aerosol Index (UVAI) retrieved by the Ozone Monitoring Instrument (OMI) for 4 yr (2005–2008) exhibit the same AOD pattern. The carbonaceous aerosols during the black cloud periods are confined to the planetary boundary layer (PBL), while dust aerosols exist over a wider range of altitudes, as shown by Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) aerosol profiles. The monthly climatology of Multi-angle Imaging SpectroRadiometer (MISR) data show that the aerosols during the black cloud periods are spherical with a higher percentage of small and medium size particles, whereas the spring aerosols are mostly large non-spherical particles. All of the results show that the air quality in Cairo and the Nile delta region is subject to a complex mixture of air pollution types, especially in the fall season, when biomass burning contributes to a background of urban pollution and desert dust.
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This paper describes the background, instrumentation, goals, and the regional influences on the HUMPPA-COPEC intensive field measurement campaign, conducted at the Boreal forest research station SMEAR II (Station for Measuring Ecosystem-Atmosphere Relation) in Hyytiälä, Finland from 12 July–12 August 2010. The prevailing meteorological conditions during the campaign are examined and contrasted with those of the past six years. Back trajectory analyses show that meteorological conditions at the site in 2010 were characterized by a higher proportion of southerly flow than in the other years studied. As a result the summer of 2010 was anomalously warm and high in ozone making the campaign relevant for the analysis of possible future climates. A comprehensive land use analysis, provided on both 5 and 50 km scales, shows that the main vegetation types surrounding the site on both the regional and local scales are: coniferous forest (Scots pine and/or Norway spruce); mixed forest (Birch and conifers); and woodland scrub (e.g. Willows, Aspen); indicating that the campaign results can be taken as representative of the Boreal forest ecosystem. In addition to the influence of biogenic emissions, the measurement site was occasionally impacted by sources other than vegetation. Specific tracers have been used here to identify the time periods when such sources have impacted the site namely: biomass burning (acetonitrile and CO), urban anthropogenic pollution (pentane and SO<sub>2</sub>) and the nearby Korkeakoski sawmill (enantiomeric ratio of chiral monoterpenes). None of these sources dominated the study period, allowing the Boreal forest summertime emissions to be assessed and contrasted with various other source signatures.
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During the 1998, 2000, 2001, 2008, and 2009 summer intensives of the Program for Research on Oxidants: PHotochemistry, Emissions and Transport (PROPHET), ambient measurement of nitrogen oxides (NO + NO<sub>2</sub> = NO<sub>x</sub>) were conducted. NO and NO<sub>x</sub> mole fractions displayed a diurnal pattern with NO<sub>x</sub> frequently highest in early morning. This pattern has often been observed in other rural areas. In this paper, we discuss the potential sources and contributing factors of the frequently observed morning pulse of NO<sub>x</sub>. Of the possible potential contributing factors to the observed morning pulse of NO and NO<sub>x</sub>, we find that surface-layer transport and slow upward mixing from soil emissions, related to the thermodynamic stability in the nocturnal boundary layer (NBL) before its morning breakup are the largest contributors. The morning NO<sub>x</sub> peak can significantly impact boundary layer chemistry, e.g. through production of HONO on surfaces, and by increasing the importance of NO<sub>3</sub> chemistry in the morning boundary layer.
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Dust optical properties over North Africa and the Arabian Peninsula are extracted from the quality assured multi-year datasets obtained at 14 sites of the Aerosol Robotic Network (AERONET). We select the data with (a) large aerosol optical depth (AOD ≥ 0.4 at 440 nm) and (b) small Ångström exponent (Å<sub>ext</sub> ≤ 0.2) for retaining high accuracy and reducing interference of non-dust aerosols. The result indicates that the major fraction of high aerosol optical depth days are dominated by dust over these sites even though it varies depending on location and time. We have found that the annual mean and standard deviation of single scattering albedo, asymmetry parameter, real refractive index, and imaginary refractive index for Saharan and Arabian desert dust is 0.944 ± 0.005, 0.752 ± 0.014, 1.498 ± 0.032, and 0.0024 ± 0.0034 at 550 nm wavelength, respectively. Dust aerosol selected by this method is less absorbing than the previously reported values over these sites. The weaker absorption of dust from this study is consistent with the studies using remote sensing techniques from satellite. These results can help to constrain uncertainties in estimating global dust shortwave radiative forcing.
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The trends and spreads of tropospheric and stratospheric temperature are discussed in terms of three groups of datasets in 1979–2008. These datasets include (a) three satellite observations of Microwave Sounding Units (MSU) measurements, (b) five radiosonde observations and (c) five reanalysis products. The equivalent tropospheric and stratospheric temperature from radiosonde and reanalyses are calculated based on the vertical weighting function of the MSU channel 2 (CH2) and channel 4 (CH4) measurements, respectively. The results show that both cooling in the stratosphere and warming in troposphere significantly depends on the datasets and latitudes.
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Using a Large-Eddy Simulation model, we have systematically studied the inability of boundary layer turbulence to efficiently mix reactive species. This creates regions where the species are accumulated in a correlated or anti-correlated way, thereby modifying the mean reactivity. We quantify this modification by the intensity of segregation, <i>I</i><sub>S</sub>, and analyse the driving mechanisms: heterogeneity of the surface moisture and heat fluxes, various background wind patterns and non-uniform isoprene emissions. The heterogeneous surface conditions are characterized by cool and wet forested patches with high isoprene emissions, alternated with warm and dry patches that represents pasture with relatively low isoprene emissions. For typical conditions in the Amazon rain forest, applying homogeneous surface forcings and in the absence of free tropospheric NO<sub>x</sub>, the isoprene-OH reaction rate is altered by less than 10%. This is substantially smaller than the previously assumed <i>I</i><sub>S</sub> of 50% in recent large-scale model analyses of tropical rain forest chemistry. Spatial heterogeneous surface emissions enhance the segregation of species, leading to alterations of the chemical reaction rates up to 20%. The intensities of segregation are enhanced when the background wind direction is parallel to the borders between the patches and reduced in the case of a perpendicular wind direction. The effects of segregation on trace gas concentrations vary per species. For the highly reactive OH, the differences in concentration averaged over the boundary layer are less than 2% compared to homogeneous surface conditions, while the isoprene concentration is increased by as much as 12% due to the reduced chemical reaction rates. These processes take place at the sub-grid scale of chemistry transport models and therefore need to be parameterized.
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Ångström coefficients are commonly used to parameterize the slow wavelength dependence of aerosol scattering, absorption, and extinction coefficients and single scattering albedo. Here we introduce simple analytical relationships between these coefficients that establish a framework for intercomparison between theory and experimental results from different instruments and platforms and allow for closure studies and improved physical understanding.
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An innovative approach using mobile lidar measurements was implemented to test the performances of chemistry-transport models in simulating mass concentrations (PM<sub>10</sub>) predicted by chemistry-transport models. A ground-based mobile lidar (GBML) was deployed around Paris onboard a van during the MEGAPOLI (Megacities: Emissions, urban, regional and Global Atmospheric POLlution and climate effects, and Integrated tools for assessment and mitigation) summer experiment in July 2009. The measurements performed with this Rayleigh-Mie lidar are converted into PM<sub>10</sub> profiles using optical-to-mass relationships previously established from in situ measurements performed around Paris for urban and peri-urban aerosols. The method is described here and applied to the 10 measurements days (MD). MD of 1, 15, 16 and 26 July 2009, corresponding to different levels of pollution and atmospheric conditions, are analyzed here in more details. Lidar-derived PM<sub>10</sub> are compared with results of simulations from POLYPHEMUS and CHIMERE chemistry-transport models (CTM) and with ground-based observations from the AIRPARIF network. GBML-derived and AIRPARIF in situ measurements have been found to be in good agreement with a mean Root Mean Square Error RMSE (and a Mean Absolute Percentage Error MAPE) of 7.2 μg m<sup>−3</sup> (26.0%) and 8.8 μg m<sup>−3</sup> (25.2%) with relationships assuming peri-urban and urban-type particles, respectively. The comparisons between CTMs and lidar at ~200 m height have shown that CTMs tend to underestimate wet PM<sub>10</sub> concentrations as revealed by the mean wet PM<sub>10</sub> observed during the 10 MD of 22.4, 20.0 and 17.5 μg m<sup>−3</sup> for lidar with peri-urban relationship, and POLYPHEMUS and CHIMERE models, respectively. This leads to a RMSE (and a MAPE) of 6.4 μg m<sup>−3</sup> (29.6%) and 6.4 μg m<sup>−3</sup> (27.6%) when considering POLYPHEMUS and CHIMERE CTMs, respectively. Wet integrated PM<sub>10</sub> computed (between the ground and 1 km above the ground level) from lidar, POLYPHEMUS and CHIMERE results have been compared and have shown similar results with a RMSE (and MAPE) of 6.3 mg m<sup>−2</sup> (30.1%) and 5.2 mg m<sup>−2</sup> (22.3%) with POLYPHEMUS and CHIMERE when comparing with lidar-derived PM<sub>10</sub> with periurban relationship. The values are of the same order of magnitude than other comparisons realized in previous studies. The discrepancies observed between models and measured PM<sub>10</sub> can be explained by difficulties to accurately model the background conditions, the positions and strengths of the plume, the vertical turbulent diffusion (as well as the limited vertical model resolutions) and chemical processes as the formation of secondary aerosols. The major advantage of using vertically resolved lidar observations in addition to surface concentrations is to overcome the problem of limited spatial representativity of surface measurements. Even for the case of a well-mixed boundary layer, vertical mixing is not complete, especially in the surface layer and near source regions. Also a bad estimation of the mixing layer height would introduce errors in simulated surface concentrations, which can be detected using lidar measurements. In addition, horizontal spatial representativity is larger for altitude integrated measurements than for surface measurements, because horizontal inhomogeneities occurring near surface sources are dampened.
