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Black carbon (BC) particles accumulated in the Arctic troposphere and deposited on snow have been calculated to have significant effects on radiative forcing of the Arctic regional climate. Applying cluster analysis technique on 10-day backward trajectories, seven distinct transport pathways (or clusters) affecting Alert (82.5° N, 62.5° W), Nunavut in Canada are identified in this work. Transport frequency associated with each pathway is obtained as the fraction of trajectories in that cluster. Based on atmospheric transport frequency and BC surface flux from surrounding regions (i.e. North America, Europe, and former USSR), a linear regression model is constructed to investigate the inter-annual variations of BC observed at Alert in January and April, representative of winter and spring respectively, between 1990 and 2005. Strong correlations are found between BC concentrations predicted with the regression model and measurements at Alert for both seasons (<i>R</i><sup>2</sup> equals 0.77 and 0.81 for winter and spring, respectively). Results imply that atmospheric transport and BC emission are the major contributors to the inter-annual variations in BC concentrations observed at Alert in the cold seasons for the 16-year period. Other factors, such as deposition, could also contribute to the variability in BC concentrations but were not considered in this analysis. Based on the regression model the relative contributions of regional BC emissions affecting Alert are attributed to the Eurasian sector, composed of the European Union and the former USSR, and the North American sector. Considering both seasons, the model suggests that former USSR is the major contributor to the near-surface BC levels at the Canadian high Arctic site with an average contribution of about 67% during the 16-year period, followed by European Union (18%) and North America (15%). In winter, the atmospheric transport of BC aerosols from Eurasia is found to be even more predominant with a multi-year average of 94%. The model estimates smaller contribution from the Eurasian sector in spring (70%) than that in winter. It is also found that the inter-annual variation in Eurasian contributions depends mainly on the reduction of emissions, while the changes in both emission and atmospheric transport contributed to the inter-annual variation of North American contributions.
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Submicron particles collected at Whistler, British Columbia, at 1020 m a.s.l. during May and June 2008 on Teflon filters were analyzed by Fourier transform infrared (FTIR) and X-ray fluorescence (XRF) techniques for organic functional groups (OFG) and elemental composition. Organic mass (OM) concentrations ranged from less than 0.5 to 3.1 μg m<sup>−3</sup>, with a project mean and standard deviation of 1.3±1.0 μg m<sup>−3</sup> and 0.21±0.16 μg m<sup>−3</sup> for OM and sulfate, respectively. On average, organic hydroxyl, alkane, and carboxylic acid groups represented 34%, 33%, and 23% of OM, respectively. Ketone, amine and organosulfate groups constituted 6%, 5%, and <1% of the average organic aerosol composition, respectively. Measurements of volatile organic compounds (VOC), including isoprene and monoterpenes from biogenic VOC (BVOC) emissions and their oxidation products (methyl-vinylketone / methacrolein, MVK/MACR), were made using co-located proton transfer reaction mass spectrometry (PTR-MS). We present chemically-specific evidence of OFG associated with BVOC emissions. Positive matrix factorization (PMF) analysis attributed 65% of the campaign OM to biogenic sources, based on the correlations of one factor to monoterpenes and MVK/MACR. The remaining fraction was attributed to anthropogenic sources based on a correlation to sulfate. The functional group composition of the biogenic factor (consisting of 32% alkane, 25% carboxylic acid, 21% organic hydroxyl, 16% ketone, and 6% amine groups) was similar to that of secondary organic aerosol (SOA) reported from the oxidation of BVOCs in laboratory chamber studies, providing evidence that the magnitude and chemical composition of biogenic SOA simulated in the laboratory is similar to that found in actual atmospheric conditions. The biogenic factor OM is also correlated to dust elements, indicating that dust may act as a non-acidic SOA sink. This role is supported by the organic functional group composition and morphology of single particles, which were analyzed by scanning transmission X-ray microscopy near edge X-ray absorption fine structure (STXM-NEXAFS).
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Considering the Mediterranean as a region of high evaporation and low precipitation, evaluations of sinks and sources of moisture and precipitation in the Mediterranean basin have been carried out within the frame of the CIRCE (Climate Change and Impact Research: the Mediterranean Environment) project. Besides these evaluations, residence time and stagnation/ventilation analyses have been carried out to investigate transport to and from the Mediterranean basin and in the basin itself. A Lagrangian moisture diagnosis method calculating budgets of evaporation minus precipitation was applied to a 5.5 year (October 1999–April 2005) trajectory data set and evaluated for eight representative Mediterranean Regions Of Interest (ROI). The Mediterranean basin has been identified as a major source of moisture and precipitation to the surrounding land area and to the basin itself. Main regions of stagnation, i.e. the Po basin, have been defined on a seasonal basis through residence time analysis. Evaluation of the transport to and from the basin shows that the Mediterranean is a crossroad of airstreams where air enters mainly from the northwest and continues in two separate streams, one going southwest over North Africa into the trade wind zone and the other one to the northeast through Central Asia.
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Elemental carbon (EC) in size-segregated aerosol samples were determined at five urban, one suburban, and one rural locations in the Pearl River Delta region in South China during 2006–2008 period. The size modal characteristics of EC were different at the urban and suburban/rural locations. The urban EC had a dominant condensation mode with a mass median aerodynamic diameter (MMAD) in the 0.36–0.43 μm range and a slightly less abundant mode in the droplet mode size (MMAD: 0.8–1.1 μm), while the suburban/rural EC had a prominent mode in the droplet mode size (MMAD: 0.7–1.1 μm) and a minor condensation mode (MMAD: 0.22–0.33 μm). Calculations using Mie theory and the measured size distributions of EC, organic carbon, and major inorganic ions indicate that EC-containing particles contributed 76±20% of the observed light extinction at the urban sites. Among the EC-containing particles, EC mass alone contributed 21±11% of the observed light extinction while non-EC materials on the EC particles (i.e., organic matter, ammonium sulfate, and water) contributed 55±15%. At the suburban/rural locations, EC-containing particles contributed 37–48% of the measured light extinction, with EC mass contributing 4–10% and non-EC coating materials contributing the remaining light extinction. Our results suggest that EC-containing particles were important to the overall light extinction in the urban atmospheres due to their more abundant presence from vehicular emissions. The EC-containing particles in the suburban/rural locations had a reduced but still significant contribution to light extinction budget.
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In this study, we report measurements of CFC-12 (CCl<sub>2</sub>F<sub>2</sub>) in firn air and in air extracted from shallow ice cores from three Antarctic sites. The firn air data are consistent with the known atmospheric history of CFC-12. In contrast, some of the ice core samples collected near the firn-ice transition exhibit anomalously high CFC-12 levels. Together, the ice core and firn air data provide evidence for the presence of modern air entrapped in the shallow ice core samples that likely contained open pores at the time of collection. We propose that this is due to closure of the open pores after drilling, entrapping modern air and resulting in elevated CFC-12 mixing ratios. Our results reveal that open porosity can exist below the maximum depth at which firn air samples can be collected, particularly at sites with lower accumulation rates. CFC-12 measurements demonstrate that post-drilling closure of open pores can lead to a change in the composition of bubble air in shallow ice cores through purely physical processes. The results have implications for investigations involving trace gas composition of bubbles in shallow ice cores collected near the firn-ice transition.
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This paper introduces a method for recovering global fields of near-surface net available energy (the sum of the sensible and latent heat flux or the difference between the net radiation and surface heat accumulation) using satellite visible and infra-red products derived from the AIRS (Atmospheric Infrared Sounder) and MODIS (MOderate Resolution Imaging Spectroradiometer) platforms. The method focuses on first specifying net surface radiation by considering its various shortwave and longwave components. This was then used in a surface energy balance equation in conjunction with satellite day-night surface temperature difference to derive 12 h discrete time estimates of surface system heat capacity and heat accumulation, leading directly to a retrieval for surface net available energy. Both net radiation and net available energy estimates were evaluated against ground truth data taken from 30 terrestrial tower sites affiliated to the FLUXNET network covering 7 different biome classes. This revealed a relatively good agreement between the satellite and tower data, with a pooled root mean square deviation of 98 and 72 W m<sup>−2</sup> for net radiation and net available energy, respectively, with little bias particularly for the net available energy.
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This paper introduces a new method for recovering global fields of latent heat flux. The method focuses on specifying Bowen ratio fields through exploiting air temperature and vapour pressure measurements obtained from infra-red soundings of the AIRS (Atmospheric Infrared Sounder) sensor onboard the NASA-Aqua platform. Through combining these Bowen ratio retrievals with satellite surface net available energy data we have specified estimates of global surface latent heat flux at the 1° by 1° scale. These estimates were evaluated against data from 30 terrestrial tower flux sites covering a broad spectrum of biomes. Taking monthly average 13:30 local time (LT) data for 2003, this revealed a relatively good agreement between the satellite and tower measurements of latent heat flux, with a pooled root mean square deviation of 79 W m<sup>−2</sup>, and no significant bias. The results show particular promise for this approach under warm, moist conditions, but weaknesses under arid or semi-arid conditions subject to high radiative loads.
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A spatial-temporal analysis has been conducted using satellite observed distributions of rain frequency, NO<sub>2</sub> concentration and aerosol, with focus on the spring season. As revealed by measurements from 1998–2009 over Shanghai, China, the suppression of rain is mainly attributed to the reduction of rain occurrence rather than changes in rain intensity. The overall features emerge from the region-by-region analyses that there is an inverse relationship between the rain frequency and the pollution and associated aerosols at continental scale in spring. The enhancement of pollution-produced CCN in addition to mineral dust from long-term transport suppresses the rain frequency, as favored by topography, wind, and other meteorological conditions.
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As part of the Fire Lab at Missoula Experiments (FLAME) in 2006–2007, we examined hygroscopic properties of particles emitted from open combustion of 33 select biomass fuels. Measurements of humidification growth factors for subsaturated water relative humidity (RH) conditions were made with a hygroscopic tandem differential mobility analyzer (HTDMA) for dry particle sizes of 50, 100 and 250 nm. Results were then fit to a single-parameter model to obtain the hygroscopicity parameter, κ. Particles in freshly emitted biomass smoke exhibited a wide range of hygroscopicity (individual modes with 0<κ<1.0), spanning a range from the hygroscopicity of fresh diesel soot emissions to that of pure inorganic salts commonly found in the ambient aerosol. Smoke aerosols dominated by carbonaceous species typically had a unimodal growth factor with corresponding mean κ=0.1 (range of 0<κ<0.4). Those with a substantial inorganic mass fraction typically separated into less- and more-hygroscopic modes at high RH, the latter with mean κ=0.4 (range of 0.1<κ<1). The bimodal κ distributions were indicative of smoke chemical heterogeneity at a single particle size, whereas heterogeneity as a function of size was indicated by typically decreasing κ values with increasing dry particle diameters. Hygroscopicity varied strongly with biomass fuel type and, to a lesser extent, with combustion conditions. Among the most hygroscopic smokes were those from palmetto, rice straw, and sawgrass, while smoke particles from coniferous species such as spruces, firs, pines, and duffs were among the least hygroscopic. Overall, hygroscopicity decreased with increasing ratios of total carbon to inorganic ions as measured in PM<sub>2.5</sub> filter samples. Despite aerosol heterogeneity, reconstructions of κ using PM<sub>2.5</sub> bulk chemical composition data fell along a 1:1 line with measured ensemble κ values.
