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Emission information is crucial for air quality modelling and air quality management. In this study, a new approach based on the understanding of the relationship between emissions and measured pollutant concentrations has been proposed to estimate pollutant emissions and source contributions. The retrieval can be made with single point in-situ measurements combined with backward trajectory analyses. The method takes into consideration the effect of meteorology on pollutant transport when evaluating contributions and is independent of energy statistics, therefore can provide frequent updates on emission information. The spatial coverage can be further improved by using measurements from several sites and combining the derived emission fields. The method was applied to yield the source distributions of black carbon (BC) and CO in the North China Plain (NCP) using in-situ measurements from the HaChi (Haze in China) Campaign and to evaluate contributions from specific areas to local concentrations at the measurement site. Results show that this method can yield a reasonable emission field for the NCP and can directly quantify areal source contributions. Major BC and CO emission source regions are Beijing, the western part of Tianjin and Langfang, Hebei, with Tangshan being an additional important CO emission source area. The source contribution assessment suggests that, aside from local emissions in Wuqing, Tianjin and Hebei S, SW (<i>d</i> < 100 km) are the greatest contributors to measured local concentrations, while emissions from Beijing contribute little during summertime.
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Ozone Monitoring Instrument (OMI) tropospheric NO<sub>2</sub> vertical column density data were used in conjunction with in-situ NO<sub>2</sub> concentrations collected by permanently installed monitoring stations to infer 24 h surface-level NO<sub>2</sub> concentrations at 0.1° (~11 km) resolution. The region examined included rural and suburban areas, and the highly industrialised area of Windsor, Ontario, which is situated directly across the US-Canada border from Detroit, MI. Photolytic NO<sub>2</sub> monitors were collocated with standard NO<sub>2</sub> monitors to provide qualitative data regarding NO<sub>z</sub> interference during the campaign. The accuracy of the OMI-inferred concentrations was tested using two-week integrative NO<sub>2</sub> measurements collected with passive monitors at 18 locations, approximating a 15 km grid across the region, for 7 consecutive two-week periods. When compared with these passive results, satellite-inferred concentrations showed an 18% positive bias. The correlation of the passive monitor and OMI-inferred concentrations (<i>R</i>=0.69, <i>n</i>=115) was stronger than that for the passive monitor concentrations and OMI column densities (<i>R</i>=0.52), indicating that using a sparse network of monitoring sites to estimate concentrations improves the direct utility of the OMI observations. OMI-inferred concentrations were then calculated for four years to show an overall declining trend in surface NO<sub>2</sub> concentrations in the region. Additionally, by separating OMI-inferred surface concentrations by wind direction, clear patterns in emissions and affected down-wind regions, in particular around the US-Canada border, were revealed.
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The North China plain is a region with megacities and huge populations. Aerosols over the highly polluted area have a significant impact on the regional and global climate. In order to investigate the physical and chemical characteristics of aerosol particles in elevated layers there, observations were carried out at the summit of Mt. Tai (1534 m a.s.l.) from 19 to 28 April, 2010, when the air masses were advected from the east (phase-I: 19–21 April), from the south (phase-II: 22–25 April), and from the northwest (phase-III: 26–28 April). Individual aerosol particles were identified with transmission electron microscopy (TEM), new particle formation (NPF) and growth events were monitored by a wide-range particle spectrometer, and ion concentrations in PM<sub>2.5</sub> were analyzed. During phase-I and phase-II, haze layers caused by anthropogenic pollution were observed, and a high percentage of particles were sulfur-rich (47–49%). In phase-III, the haze disappeared due to the intrusion of cold air from the northwest, and mineral dust particles from deserts were dominant (43%). NPF followed by particle growth during daytime was more pronounced on hazy than on clear days. Particle growth during daytime resulted in an increase of particle geometric mean diameter from 10–22 nm in the morning to 56–96 nm in the evening. TEM analysis suggests that sulfuric acid and secondary organic compounds should be important factors for particle nucleation and growth. However, the presence of fine anthropogenic particles (e.g., soot, metal, and fly ash) embedded within S-rich particles indicates that they could weaken NPF and enhance particle growth through condensation and coagulation. Abundant mineral particles in phase-III likely suppressed the NPF processes because they supplied sufficient area on which acidic gases or acids condensed.
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Existing theoretical formulations for the size-resolved scavenging coefficient Λ(<i>d</i>) for atmospheric aerosol particles scavenged by rain predict values lower by one to two orders of magnitude than those estimated from field measurements of particle-concentration changes for particles smaller than 3 μm in diameter. Vertical turbulence is not accounted for in the theoretical formulations of Λ(<i>d</i>) but does contribute to the field-derived estimates of Λ(<i>d</i>) due to its influence on the overall concentration changes of aerosol particles in the layers undergoing impaction scavenging. A detailed one-dimensional cloud microphysics model has been used to simulate rain production and below-cloud particle scavenging, and to quantify the contribution of turbulent diffusion to the overall Λ(<i>d</i>) values calculated from particle concentration changes. The relative contribution of vertical diffusion to below-cloud scavenging is found to be largest for submicron particles under weak precipitation conditions. The discrepancies between theoretical and field-derived Λ(<i>d</i>) values can largely be explained by the contribution of vertical diffusion to below-cloud particle scavenging for all particles larger than 0.01 μm in diameter for which field data are available. The results presented here suggest that the current theoretical framework for Λ(<i>d</i>) can provide a reasonable approximation of below-cloud aerosol particle scavenging by rain in size-resolved aerosol transport models if vertical diffusion is also considered by the models.
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In order to use knowledge of past climate change to improve our understanding of the sensitivity of the climate system, detailed knowledge about the time development of radiative forcing (RF) of the earth atmosphere system is crucial. In this study, time series of anthropogenic forcing of climate from pre-industrial times until 2010, for all well established forcing agents, are estimated. This includes presentation of RF histories of well mixed greenhouse gases, tropospheric ozone, direct- and indirect aerosol effects, surface albedo changes, stratospheric ozone and stratospheric water vapour. For long lived greenhouse gases, standard methods are used for calculating RF, based on global mean concentration changes. For short lived climate forcers, detailed chemical transport modelling and radiative transfer modelling using historical emission inventories is performed. For the direct aerosol effect, sulphate, black carbon, organic carbon, nitrate and secondary organic aerosols are considered. For aerosol indirect effects, time series of both the cloud lifetime effect and the cloud albedo effect are presented. Radiative forcing time series due to surface albedo changes are calculated based on prescribed changes in land use and radiative transfer modelling. For the stratospheric components, simple scaling methods are used. Long lived greenhouse gases (LLGHGs) are the most important radiative forcing agent with a RF of 2.83±0.28 W m<sup>−2</sup> in year 2010 relative to 1750. The two main aerosol components contributing to the direct aerosol effect are black carbon and sulphate, but their contributions are of opposite sign. The total direct aerosol effect was −0.48±0.32 W m<sup>−2</sup> in year 2010. Since pre-industrial times the positive RF (LLGHGs and tropospheric O<sub>3</sub>) has been offset mainly by the direct and indirect aerosol effects, especially in the second half of the 20th century, which possibly lead to a decrease in the total anthropogenic RF in the middle of the century. We find a total anthropogenic RF in year 2010 of 1.4 W m<sup>−2</sup>. However, the uncertainties in the negative RF from aerosols are large, especially for the cloud lifetime effect.
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We present a comprehensive characterization of cloud condensation nuclei (CCN) sampled in the Alaskan Arctic during the 2008 Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC) project, a component of the POLARCAT and International Polar Year (IPY) initiatives. Four distinct air mass types were sampled including a cleaner Arctic background and a relatively pristine sea ice boundary layer as well as biomass burning and anthropogenic pollution plumes. Despite differences in chemical composition, inferred aerosol hygroscopicities were fairly invariant and ranged from κ = 0.1–0.3 over the atmospherically-relevant range of water vapor supersaturations studied. Organic aerosols sampled were found to be well-oxygenated, consistent with long-range transport and aerosol aging processes. However, inferred hygroscopicities are less than would be predicted based on previous parameterizations of biogenic oxygenated organic aerosol, suggesting an upper limit on organic aerosol hygroscopicity above which κ is less sensitive to the O:C ratio. Most Arctic aerosols act as CCN above 0.1 % supersaturation, although the data suggest the presence of an externally-mixed, non-CCN-active mode comprising approximately 0–20% of the aerosol number. CCN closure was assessed using measured size distributions, bulk chemical composition, and assumed aerosol mixing states; CCN predictions tended toward overprediction, with the best agreement (±0–20 %) obtained by assuming the aerosol to be externally-mixed with soluble organics. Closure also varied with CCN concentration, and the best agreement was found for CCN concentrations above 100 cm<sup>−3</sup> with a 1.5- to 3-fold overprediction at lower concentrations.
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Evidence for in situ generated atmospheric gravity waves associated with a stratospheric temperature enhancement (STE) are presented. The signatures of two sets of gravity waves are observed by molecular-aerosol lidar in conjunction with the early December 2000 STE event above Sondrestrom, Greenland. The first set of gravity waves shows downward phase progression with a vertical wavelength of ~8 km while the second set shows upward phase progression with a vertical wavelength of ~9 km. With estimates of the background wind fields from synoptic analyses, the various intrinsic gravity wave parameters of these two wave structures are found. The observed wave features compare well to previous numerical modeling predictions.
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To identify the relative contribution of local versus regional sources of particulate matter (PM) in the Greater Athens Area (GAA), simultaneous 24-h mass and chemical composition measurements of size segregated particulate matter (PM<sub>1</sub>, PM<sub>2.5</sub> and PM<sub>10</sub>) were carried out from September 2005 to August 2006 at three locations: one urban (Goudi, Central Athens, "GOU"), one suburban (Lykovrissi, Athens, "LYK") in the GAA and one at a regional background site (Finokalia, Crete, "FKL"). <br><br> The two stations in the GAA exceeded the EU-legislated PM<sub>10</sub> limit values, both in terms of annual average (59.0 and 53.6 μg m<sup>−3</sup> for Lykovrissi and Goudi, respectively) and of 24-h value. High levels of PM<sub>2.5</sub> and PM<sub>1</sub> were also found at both locations (23.5 and 18.6 for Lykovrissi, while 29.4 and 20.2 μg m<sup>−3</sup> for Goudi, respectively). <br><br> Significant correlations were observed between the same PM fractions at both GAA sites indicating important spatial homogeneity within GAA. During the warm season (April to September), the PM<sub>1</sub> ratio between GAA and FKL ranged from 1.1 to 1.3. On the other hand this ratio was significantly higher (1.6–1.7) during the cold season (October to March) highlighting the role of long-range transport and local sources during the warm and cold seasons respectively. Regarding the coarse fraction no seasonal trend was observed for both GAA sites with their ratio (GAA site/FKL) being higher than 2 indicating significant contribution from local sources such as soil and/or road dust. <br><br> Chemical speciation data showed that on a yearly basis, ionic and crustal mass represent up to 67–70% of the gravimetrically determined mass for PM<sub>10</sub> samples in the GAA and 67% for PM<sub>1</sub> samples in LYK. The unidentified mass might be attributed to organic matter (OM) and elemental carbon (EC), in agreement with the results reported by earlier studies in central Athens. At all sites, similar seasonal patterns were observed for nss-SO<sub>4</sub><sup>2−</sup>, a secondary compound, indicating significant contribution from regional sources in agreement with PM<sub>1</sub> observations. <br><br> The contribution of local sources at both GAA sites was also estimated by considering mass and chemical composition measurements at Finokalia as representative of the regional background. Particulate Organic Matter (POM) and EC, seemed to be the main contributor of the local PM mass within the GAA (up to 62% in PM<sub>1</sub>. Dust from local sources contributed also significantly to the local PM<sub>10</sub> mass (up to 33%).
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Intermittent coherent structures can be responsible for a large fraction of the exchange between a forest canopy and the atmosphere. Quantifying their contribution to momentum and heat fluxes is necessary to interpret measurements of trace gases and aerosols within and above forest canopies. The primary objective of the Community Atmosphere-Biosphere Interactions Experiment (CABINEX) field campaign (10 July 2009 to 9 August 2009) was to study the chemistry of volatile organic compounds (VOC) within and above a forest canopy. In this manuscript we provide an analysis of coherent structures and canopy-atmosphere exchange during CABINEX to support in-canopy gradient measurements of VOC. We quantify the number and duration of coherent structure events and their percent contribution to momentum and heat fluxes with two methods: (1) quadrant-hole analysis, and (2) wavelet analysis. Despite differences in the duration and number of events, both methods predict that coherent structures contribute 40–50% to momentum fluxes and 44–65% to heat fluxes during the CABINEX campaign. Contributions associated with coherent structures are slightly greater under stable atmospheric conditions. By comparing heat fluxes within and above the canopy, we determine the degree of coupling between upper canopy and atmosphere, and find that they are coupled the majority of the time. Uncoupled canopy-atmosphere events occur in the early morning (4–8 a.m. local time) approximately 30% of the time. This study confirms that coherent structures contribute significantly to the exchange of heat and momentum between the canopy and atmosphere at the CABINEX site, and indicates the need to include these transport processes when studying the mixing and chemical reactions of trace gases and aerosols between a forest canopy and the atmosphere.
