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Ambient concentrations of trace elements with 2 h time resolution were measured in PM10–2.5, PM2.5–1.0 and PM1.0–0.3 size ranges at kerbside, urban background and rural sites in London during winter 2012. Samples were collected using rotating drum impactors (RDIs) and subsequently analysed with synchrotron radiation-induced X-ray fluorescence spectrometry (SR-XRF). Quantification of kerb and urban increments (defined as kerb-to-urban and urban-to-rural concentration ratios, respectively), and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure. Traffic-related elements yielded the highest kerb increments, with values in the range of 10.4 to 16.6 for SW winds (3.3–6.9 for NE) observed for elements influenced by brake wear (e.g. Cu, Sb, Ba) and 5.7 to 8.2 for SW (2.6–3.0 for NE) for other traffic-related processes (e.g. Cr, Fe, Zn). Kerb increments for these elements were highest in the PM10–2.5 mass fraction, roughly twice that of the PM1.0–0.3 fraction. These elements also showed the highest urban increments (~ 3.0), although no difference was observed between brake wear and other traffic-related elements. All elements influenced by traffic exhibited higher concentrations during morning and evening rush hours, and on weekdays compared to weekends, with the strongest trends observed at the kerbside site, and additionally enhanced by winds coming directly from the road, consistent with street canyon effects. Elements related to mineral dust (e.g. Al, Si, Ca, Sr) showed significant influences from traffic-induced resuspension, as evidenced by moderate kerb (3.4–5.4 for SW, 1.7–2.3 for NE) and urban (~ 2) increments and increased concentrations during peak traffic flow. Elements related to regional transport showed no significant enhancement at kerb or urban sites, with the exception of PM10–2.5 sea salt (factor of up to 2), which may be influenced by traffic-induced resuspension of sea and/or road salt. Heavy-duty vehicles appeared to have a larger effect than passenger vehicles on the concentrations of all elements influenced by resuspension (including sea salt) and wearing processes. Trace element concentrations in London were influenced by both local and regional sources, with coarse and intermediate fractions dominated by traffic-induced resuspension and wearing processes and fine particles influenced by regional transport.

Solid fuel emissions, including those from biomass burning, are increasing in urban areas across the European Union due to rising energy costs and government incentives to use renewable energy sources for heating. In order to help protect human health as well as to improve air quality and pollution abatement strategies, the sources of combustion aerosols, their contributions, and the processes they undergo need to be better understood. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was therefore deployed at an urban background site between January and February 2012 to investigate solid fuel organic aerosols (SFOA) in London. The variability of SFOA was examined and the factors governing the split between the two SFOA factors derived from Positive Matrix Factorisation (PMF) were assessed. The concentrations of both factors were found to increase during the night and during cold periods, consistent with domestic space heating activities. The split between the two factors is likely governed predominantly by differences in burn conditions where SFOA1 best represents more efficient burns and SFOA2 best represents less efficient burns. The differences in efficiency may be due to burner types or burn phase, for example. Different fuel types and levels of atmospheric processing also likely contribute to the two factors. As the mass spectral profile of SFOA is highly variable, the findings from this study may have implications for improving future source apportionment and factorisation analyses. During the winter, SFOA was found to contribute 38% to the total non-refractory submicron organic aerosol (OA) mass, with similar contributions from both SFOA factors (20% from SFOA1 and 18% from SFOA2). A similar contribution of SFOA was derived for the same period from a compact time-of-flight AMS (cToF-AMS), which measured for a full calendar year at the same site. The seasonality of SFOA was investigated using the year-long data set where concentrations were greatest in the autumn and winter. During the summer, SFOA contributed 11% to the organic fraction, where emissions resulted from different anthropogenic activities such as barbecues and domestic garden wood burning. The significant contribution of SFOA to total organic mass throughout the year suggests that the negative effects on health and air quality, as well as climate, are not just confined to winter as exposure to these aerosols and the associated black carbon can also occur during the summer, which may have significant implications for air-quality policies and mitigation strategies.

We present high-resolution atmospheric chemistry transport model (ACTM) simulations of secondary organic aerosol (SOA) formation over the UK for 2012. Our simulations include additional diesel-related intermediate volatility organic compound (IVOC) emissions derived directly from comprehensive field measurements at an urban background site in London during the 2012 Clean Air for London (ClearfLo) campaign. Our IVOC emissions are added proportionally to VOC emissions, as opposed to proportionally to primary organic aerosol (POA) as has been done by previous ACTM studies seeking to simulate the effects of these missing emissions. Modelled concentrations are evaluated against hourly and daily measurements of organic aerosol (OA) components derived from aerosol mass spectrometer (AMS) measurements also made during the ClearfLo campaign at three sites in the London area. Good hourly performance in comparison to the measurements was shown, giving confidence in the SOA prediction skill of the ACTM system used. According to the model simulations, diesel-related IVOCs can explain on average ~30% of the annual SOA in and around London. Furthermore, the 90-th percentile of modelled daily SOA concentrations for the whole year is 3.8 μg m−3 (more than 40% of which is produced from the missing diesel precursors), constituting a notable addition to total particulate matter. More measurements of these precursors (currently not included in official emissions inventories) is recommended. During the period of concurrent measurements, SOA concentrations at the Detling rural background location east of London were greater than at the central London location. The model shows that this was caused by an intense pollution plume with a strong gradient of imported SOA passing over the rural location. This demonstrates the value of modelling for supporting the interpretation of measurements taken at different sites or for short durations.

Solid fuel emissions, including those from biomass burning, are increasing in urban areas across the European Union due to rising energy costs and government incentives to use renewable energy sources for heating. In order to help protect human health as well as to improve air quality and pollution abatement strategies, the sources of combustion aerosols, their contributions, and the processes they undergo need to be better understood. A high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was therefore deployed at an urban background site between January and February 2012 to investigate solid fuel organic aerosols (SFOA) in London. The variability of SFOA was examined and the factors governing the split between the two SFOA factors derived from Positive Matrix Factorisation (PMF) were assessed. The concentrations of both factors were found to increase during the night and during cold periods, consistent with domestic space heating activities. The split between the two factors is likely governed predominantly by differences in burn conditions where SFOA1 best represents more efficient burns and SFOA2 best represents less efficient burns. The differences in efficiency may be due to burner types or burn phase, for example. Different fuel types and levels of atmospheric processing also likely contribute to the two factors. As the mass spectral profile of SFOA is highly variable, the findings from this study may have implications for improving future source apportionment and factorisation analyses. During the winter, SFOA was found to contribute 38% to the total non-refractory submicron organic aerosol (OA) mass, with similar contributions from both SFOA factors (20% from SFOA1 and 18% from SFOA2). A similar contribution of SFOA was derived for the same period from a compact time-of-flight AMS (cToF-AMS), which measured for a full calendar year at the same site. The seasonality of SFOA was investigated using the year-long data set where concentrations were greatest in the autumn and winter. During the summer, SFOA contributed 11% to the organic fraction, where emissions resulted from different anthropogenic activities such as barbecues and domestic garden wood burning. The significant contribution of SFOA to total organic mass throughout the year suggests that the negative effects on health and air quality, as well as climate, are not just confined to winter as exposure to these aerosols and the associated black carbon can also occur during the summer, which may have significant implications for air-quality policies and mitigation strategies.

Ambient concentrations of trace elements with 2 h time resolution were measured in PM10–2.5, PM2.5–1.0 and PM1.0–0.3 size ranges at kerbside, urban background and rural sites in London during winter 2012. Samples were collected using rotating drum impactors (RDIs) and subsequently analysed with synchrotron radiation-induced X-ray fluorescence spectrometry (SR-XRF). Quantification of kerb and urban increments (defined as kerb-to-urban and urban-to-rural concentration ratios, respectively), and assessment of diurnal and weekly variability provided insight into sources governing urban air quality and the effects of urban micro-environments on human exposure. Traffic-related elements yielded the highest kerb increments, with values in the range of 10.4 to 16.6 for SW winds (3.3–6.9 for NE) observed for elements influenced by brake wear (e.g. Cu, Sb, Ba) and 5.7 to 8.2 for SW (2.6–3.0 for NE) for other traffic-related processes (e.g. Cr, Fe, Zn). Kerb increments for these elements were highest in the PM10–2.5 mass fraction, roughly twice that of the PM1.0–0.3 fraction. These elements also showed the highest urban increments (~ 3.0), although no difference was observed between brake wear and other traffic-related elements. All elements influenced by traffic exhibited higher concentrations during morning and evening rush hours, and on weekdays compared to weekends, with the strongest trends observed at the kerbside site, and additionally enhanced by winds coming directly from the road, consistent with street canyon effects. Elements related to mineral dust (e.g. Al, Si, Ca, Sr) showed significant influences from traffic-induced resuspension, as evidenced by moderate kerb (3.4–5.4 for SW, 1.7–2.3 for NE) and urban (~ 2) increments and increased concentrations during peak traffic flow. Elements related to regional transport showed no significant enhancement at kerb or urban sites, with the exception of PM10–2.5 sea salt (factor of up to 2), which may be influenced by traffic-induced resuspension of sea and/or road salt. Heavy-duty vehicles appeared to have a larger effect than passenger vehicles on the concentrations of all elements influenced by resuspension (including sea salt) and wearing processes. Trace element concentrations in London were influenced by both local and regional sources, with coarse and intermediate fractions dominated by traffic-induced resuspension and wearing processes and fine particles influenced by regional transport.

Substantial amounts of secondary organic aerosol (SOA) can be formed from isoprene epoxydiols (IEPOX), which are oxidation products of isoprene mainly under low-NO conditions. Total IEPOX-SOA, which may include SOA formed from other parallel isoprene oxidation pathways, was quantified by applying positive matrix factorization (PMF) to aerosol mass spectrometer (AMS) measurements. The IEPOX-SOA fractions of organic aerosol (OA) in multiple field studies across several continents are summarized here and show consistent patterns with the concentration of gas-phase IEPOX simulated by the GEOS-Chem chemical transport model. During the Southern Oxidant and Aerosol Study (SOAS), 78 % of PMF-resolved IEPOX-SOA is accounted by the measured IEPOX-SOA molecular tracers (2-methyltetrols, C5-Triols, and IEPOX-derived organosulfate and its dimers), making it the highest level of molecular identification of an ambient SOA component to our knowledge. An enhanced signal at C5H6O+ (m/z 82) is found in PMF-resolved IEPOX-SOA spectra. To investigate the suitability of this ion as a tracer for IEPOX-SOA, we examine fC5H6O(fC5H6O= C5H6O+/OA) across multiple field, chamber, and source data sets. A background of ~ 1.7 ± 0.1 ‰ (‰ = parts per thousand) is observed in studies strongly influenced by urban, biomass-burning, and other anthropogenic primary organic aerosol (POA). Higher background values of 3.1 ± 0.6 ‰ are found in studies strongly influenced by monoterpene emissions. The average laboratory monoterpene SOA value (5.5 ± 2.0 ‰) is 4 times lower than the average for IEPOX-SOA (22 ± 7 ‰), which leaves some room to separate both contributions to OA. Locations strongly influenced by isoprene emissions under low-NO levels had higher fC5H6O (~ 6.5 ± 2.2 ‰ on average) than other sites, consistent with the expected IEPOX-SOA formation in those studies. fC5H6O in IEPOX-SOA is always elevated (12–40 ‰) but varies substantially between locations, which is shown to reflect large variations in its detailed molecular composition. The low fC5H6O (< 3 ‰) reported in non-IEPOX-derived isoprene-SOA from chamber studies indicates that this tracer ion is specifically enhanced from IEPOX-SOA, and is not a tracer for all SOA from isoprene. We introduce a graphical diagnostic to study the presence and aging of IEPOX-SOA as a triangle plot of fCO2 vs. fC5H6O. Finally, we develop a simplified method to estimate ambient IEPOX-SOA mass concentrations, which is shown to perform well compared to the full PMF method. The uncertainty of the tracer method is up to a factor of ~ 2, if the fC5H6O of the local IEPOX-SOA is not available. When only unit mass-resolution data are available, as with the aerosol chemical speciation monitor (ACSM), all methods may perform less well because of increased interferences from other ions at m/z 82. This study clarifies the strengths and limitations of the different AMS methods for detection of IEPOX-SOA and will enable improved characterization of this OA component.

Assessment of the impacts of brown carbon (BrC) requires accurate determination of its physical properties, but a model must be invoked to derive these from instrument data. Ambient measurements were made in London at a site influenced by traffic and solid fuel (principally wood) burning, apportioned by single particle soot photometer data and optical properties measured using multiwavelength photoacoustic spectroscopy. Two models were applied: a commonly used Mie model treating the particles as single-coated spheres and a Rayleigh-Debye-Gans approximation treating them as aggregates of smaller-coated monomers. The derived solid fuel BrC parameters at 405nm were found to be highly sensitive to the model treatment, with a mass absorption cross section ranging from 0.47 to 1.81m(2)/g and imaginary refractive index from 0.013 to 0.062. This demonstrates that a detailed knowledge of particle morphology must be obtained and invoked to accurately parameterize BrC properties based on aerosol phase measurements.

We evaluate predictions from the Community Multiscale Air Quality (CMAQ version 4.7.1) model against a suite of airborne and ground-based meteorological measurements, gas- and aerosol-phase inorganic measurements, and black carbon (BC) measurements over Southern California during the CalNex field campaign in May/June 2010. Ground-based measurements are from the CalNex Pasadena ground site, and airborne measurements took place onboard the Center for Interdisciplinary Remotely-Piloted Aircraft Studies (CIRPAS) Navy Twin Otter and the NOAA WP-3D aircraft. BC predictions are in general agreement with observations at the Pasadena ground site and onboard the WP-3D, but are consistently overpredicted when compared to Twin Otter measurements. Adjustments to predicted inorganic mass concentrations, based on predicted aerosol size distributions and the AMS transmission efficiency, are shown to be significant. Owing to recent shipping emission reductions, the dominant source of sulfate in the L.A. Basin may now be long-range transport. Sensitivity studies suggest that severely underestimated ammonia emissions, and not the exclusion of crustal species (Ca2 +, K+, and Mg2 +), are the single largest contributor to measurement/model disagreement in the eastern part of the L.A. Basin. Despite overstated NOx emissions, total nitrate concentrations are underpredicted, which suggests a missing source of HNO 3 and/or overprediction of deposition rates. Adding gas-phase NH 3 measurements and size-resolved measurements, up to 10 μm, of nitrate and various cations (e.g. Na+, Ca2 +, K +) to routine monitoring stations in the L.A. Basin would greatly facilitate interpreting day-to-day fluctuations in fine and coarse inorganic aerosol. Key pointsWe measured inorganic gas- and aerosol-phase species during CalNexWe compare ground-based and airborne measurements to CMAQ predictionsMeasure/model agreement varies depending on the species and location © 2012. American Geophysical Union. All Rights Reserved.

Objective To report a cost-effective and scientifically based algorithm for the clinical assessment and treatment of patients with transient ischemic attack (TIA) or minor ischemic stroke. Design We comprehensively reviewed the literature on the epidemiologic features, assessment approaches, and treatment recommendations for ischemic cerebrovascular disease and developed an algorithm by using the available clinical and research data to support all decision-making steps. Material and Methods For patients with TIA or minor ischemic stroke, the appropriate setting for investigation (inpatient or outpatient), suggested diagnostic tests, use of anticoagulants and antiplatelet agents, and indications for surgical treatment are reviewed. Results Although stroke is a common cause of death and lost productivity in the United States, the clinical assessment of patients with TIA or minor ischemic stroke has lacked consistency. The simplified algorithm clarifies patients who may be candidates for hospitalization and possible anticoagulation therapy. Initial diagnostic studies should include computed tomography of the head without use of a contrast agent, which quickly distinguishes nonhemorrhagic from hemorrhagic cerebrovascular disease. Evolving noninvasive studies of the cerebral vasculature are providing increasingly sensitive means of detecting stenoses, yet cerebral angiography remains the "gold standard." Treatment options depend on the pathophysiologic findings on diagnostic evaluation. Conclusion The assessment of patients with ischemic cerebrovascular disease is complex. The simplified algorithmic approach reported herein necessitates entry of appropriate patients into the algorithm. Because of clinical heterogeneity, an algorithm may apply to a wide spectrum of patients but will not cover every situation; hence, evaluation must be guided by a patient's unique history and findings on examination and by the physician's clinical experience.