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Abstract: Traditional Eulerian air quality models are unable to accurately simulate sub-grid scale processes, such as the near-source transport and chemistry of point source plumes, because they assume instantaneous mixing of the emitted pollutants within the grid cell containing the release, and neglect the turbulent segregation effects that limit the near-source mixing of emitted pollutants with the background atmosphere (e.g., Kramm and Meixner, 2000). Observations by Dlugi et al. (2010) show that the segregation of chemically reactive species can slow effective second-order reaction rates by as much as 15%, due to inhomogeneous mixing of the reactants. This limitation of traditional grid models applies to both “off-line” models, in which externally derived meteorology is used to drive the chemistry model, and newer “on-line” models, such as the Weather Research and Forecasting model with Chemistry (WRF/Chem), that simulate the emissions, transport, mixing, and chemical transformation of trace gases and aerosols simultaneously with the meteorology. While a number of approaches have been used in the past to address this limitation, the approach that has been most effectively used in operational models is the plume-in-grid (PinG) approach, in which a reactive plume model is embedded within the grid model to resolve sub-grid scale plumes. This paper describes the implementation of such a PinG treatment in WRF/Chem, based on a similar extension to the U.S. EPA Community Multi-scale Air Quality (CMAQ) model. The treatment, referred to as Advanced Plume Treatment, has been tested in CMAQ over more than a decade and has been used successfully in both episodic and long-term applications for assessing point source contributions to ozone and particulate matter. This paper presents the application of the PinG version of WRF/Chem for a three-day episode in July 2001, including a model performance evaluation and comparison of model results with and without PinG treatment. The results from the model application show that overall model performance is only slightly affected when the PinG treatment is used, although there are some generally small improvements, with the PinG treatment showing a 5% lower bias in predicting ozone concentrations, and 3% lower bias in sulfate predictions. However, the predicted spatial patterns of ozone and PM2.5 concentrations from the two simulations show both large decreases of up to 40 ppb ozone and 14 μg m−3 PM2.5, and increases of up to 80 ppb ozone and 33 μg m−3 PM2.5 as a result of using the PinG treatment. These differences are attributed to both direct effects of the PinG treatment (i.e., differences in dispersion, transport and chemistry of point source emissions) and indirect effects (i.e., impacts of air quality changes on meteorology). [Copyright &y& Elsevier]

Abstract: Ecosystems and the atmosphere: This review describes the state of understanding the processes involved in the exchange of trace gases and aerosols between the earth''s surface and the atmosphere. The gases covered include NO, NO2, HONO, HNO3, NH3, SO2, DMS, Biogenic VOC, O3, CH4, N2O and particles in the size range 1 nm–10 μm including organic and inorganic chemical species. The main focus of the review is on the exchange between terrestrial ecosystems, both managed and natural and the atmosphere, although some new developments in ocean–atmosphere exchange are included. The material presented is biased towards the last decade, but includes earlier work, where more recent developments are limited or absent. New methodologies and instrumentation have enabled, if not driven technical advances in measurement. These developments have advanced the process understanding and upscaling of fluxes, especially for particles, VOC and NH3. Examples of these applications include mass spectrometric methods, such as Aerosol Mass Spectrometry (AMS) adapted for field measurement of atmosphere–surface fluxes using micrometeorological methods for chemically resolved aerosols. Also briefly described are some advances in theory and techniques in micrometeorology. For some of the compounds there have been paradigm shifts in approach and application of both techniques and assessment. These include flux measurements over marine surfaces and urban areas using micrometeorological methods and the up-scaling of flux measurements using aircraft and satellite remote sensing. The application of a flux-based approach in assessment of O3 effects on vegetation at regional scales is an important policy linked development secured through improved quantification of fluxes. The coupling of monitoring, modelling and intensive flux measurement at a continental scale within the NitroEurope network represents a quantum development in the application of research teams to address the underpinning science of reactive nitrogen in the cycling between ecosystems and the atmosphere in Europe. Some important developments of the science have been applied to assist in addressing policy questions, which have been the main driver of the research agenda, while other developments in understanding have not been applied to their wider field especially in chemistry-transport models through deficiencies in obtaining appropriate data to enable application or inertia within the modelling community. The paper identifies applications, gaps and research questions that have remained intractable at least since 2000 within the specialized sections of the paper, and where possible these have been focussed on research questions for the coming decade. [Copyright &y& Elsevier]

This paper presents airborne measurements of multiple atmospheric trace constituents including greenhouse gases (such as CO 2 , CH 4 , O 3 ) and biomass burning tracers (such as CO, CH 3 CN) downwind of an exceptionally large wildfire. In summer 2013, the Rim wildfire, ignited just west of the Yosemite National Park, California, and burned over 250,000 acres of the forest during the 2-month period (17 August to 24 October) before it was extinguished. The Rim wildfire plume was intercepted by flights carried out by the NASA Ames Alpha Jet Atmospheric eXperiment (AJAX) on 29 August and the NASA DC-8, as part of SEAC 4 RS (Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys), on 26 and 27 August during its intense, primary burning period. AJAX revisited the wildfire on 10 September when the conditions were increasingly smoldering, with slower growth. The more extensive payload of the DC-8 helped to bridge key measurements that were not available as part of AJAX (e. g. CO). Data analyses are presented in terms of emission ratios (ER), emission factors (EF) and combustion efficiency and are compared with previous wildfire studies. ERs were 8.0 ppb CH 4 (ppm CO 2 ) −1 on 26 August, 6.5 ppb CH 4 (ppm CO 2 ) −1 on 29 August and 18.3 ppb CH 4 (ppm CO 2 ) −1 on 10 September 2013. The increase in CH 4 ER from 6.5 to 8.0 ppb CH 4 (ppm CO 2 ) −1 during the primary burning period to 18.3 ppb CH 4 (ppm CO 2 ) −1 during the fire's slower growth period likely indicates enhanced CH 4 emissions from increased smoldering combustion relative to flaming combustion. Given the magnitude of the Rim wildfire, the impacts it had on regional air quality and the limited sampling of wildfire emissions in the western United States to date, this study provides a valuable dataset to support forestry and regional air quality management, including observations of ERs of a wide number of species from the Rim wildfire. [ABSTRACT FROM AUTHOR]

Abstract: This paper complements the information previously published (Atmospheric Environment 45, 641–649) on gaseous and particulate emissions from wildfires in Portugal for summer 2009, in an attempt at obtaining more extensive, complete and representative databases on emission factors and detailed chemical characterisation of smoke particles. Here, emission factors for carbon oxides (CO2 and CO), total hydrocarbons (THC), fine (PM2.5) and coarse (PM2.5–10) particles obtained for fires occurring in Portugal in summer 2010 are presented. The carbonaceous content (OC and EC), water-soluble ions, elements and organic composition of smoke particles were, respectively, analysed by a thermal-optical transmission technique, ion chromatography, instrumental neutron activation analysis (INAA) and gas chromatography-mass spectrometry (GC–MS). The particle mass concentrations were in the ranges 0.69–25 mg m−3 for PM2.5 and 0.048–3.1 mg m−3 for PM2.5–10. PM2.5 particles represented 91 ± 5.7% of the PM10 mass. The OC/EC ratios in fine and coarse particles ranged from 2.5 to 205 and from 1.7 to 328, respectively. The water-soluble ions represented, on average, 3.9% and 2.8% of PM2.5 and PM2.5–10 mass, respectively. In general, the dominant ions in the water extracts were Na+, , Cl− and for the PM2.5 fraction, and K+, Mg2+, Ca2+ and for the PM2.5–10 fraction. The K+/EC and K+/OC ratios obtained in this study were, on average, 0.22 ± 0.23 and 0.011 ± 0.014 for PM2.5 and 0.83 ± 1.0 and 0.024 ± 0.023 for PM2.5–10 particles, respectively. The K+/levoglucosan ratio was, on average, 2.0 for PM2.5 and 3.1 for PM2.5−10 particles. Levoglucosan was detected at mass fractions of 1.6–8.7 mg g−1 OC in PM2.5 and 2.7–56 mg g−1 OC in PM2.5–10. The dominant elements detected in the smoke samples were Na, Br, Cr, Fe, K, Rb and Zn. The most representative organic constituents in the smoke samples were acids, alcohols, terpenoid-type compounds, sugars and phenols, in both size fractions. [Copyright &y& Elsevier]

Abstract: Over twenty modeling groups are participating in the Air Quality Model Evaluation International Initiative (AQMEII) in which a variety of mesoscale photochemical and aerosol air quality modeling systems are being applied to continental-scale domains in North America and Europe for 2006 full-year simulations for model inter-comparisons and evaluations. To better understand the reasons for differences in model results among these participating groups, each group was asked to use the same source of emissions and boundary concentration data for their simulations. This paper describes the development and application of the boundary concentration data for this AQMEII modeling exercise. The European project known as GEMS (Global and regional Earth-system Monitoring using Satellite and in-situ data) has produced global-scale re-analyses of air quality for several years, including 2006 (http://gems.ecmwf.int). The GEMS trace gas and aerosol data were made available at 3-hourly intervals on a regular latitude/longitude grid of approximately 1.9° resolution within 2 “cut-outs” from the global model domain. One cut-out was centered over North America and the other over Europe, covering sufficient spatial domain for each modeling group to extract the necessary time- and space-varying (horizontal and vertical) concentrations for their mesoscale model boundaries. Examples of the impact of these boundary concentrations on the AQMEII continental simulations are presented to quantify the sensitivity of the simulations to boundary concentrations. In addition, some participating groups were not able to use the GEMS data and instead relied upon other sources for their boundary concentration specifications. These are noted, and the contrasting impacts of other data sources for boundary data are presented. How one specifies four-dimensional boundary concentrations for mesoscale air quality simulations can have a profound impact on the model results, and hence, this aspect of data preparation must be performed with considerable care. [Copyright &y& Elsevier]

Abstract: Quantifying trace gas emissions and the influence of surface exchange processes on the atmosphere is a necessary step towards the control of global greenhouse gas emissions and reliability of air quality models. This paper proposes a procedure based on the mass balance method and implemented on highly resolved aircraft data. It allows one to estimate surface exchanges on areas of several km2 and heterogeneous features exploiting the characteristics of convective boundary layer during steady state conditions that permit the estimation of emission/absorption terms as functions of advective fluxes only. A nonparametric approach is adopted and the fluxes on the surface of a virtual box surrounding the area of interest are reconstructed on the basis of scalar densities and wind vectors using Shepard functions. Two different techniques are also proposed to face lack of data on the top surface of the box. The method has been applied to experimental data coming from measurement campaigns on two different sites. It provides realistic estimates of the CO2 emission/absorption in the considered areas that are in good agreement with CO2 fluxes evaluated by Airborne Eddy Covariance and confirm the suitability of the proposed approach for the assessment of turbulent exchange of trace gases by composite landscapes. Uncertainties on the estimated emissions due to both propagation of the experimental error and interpolation have been quantified by bootstrap analysis as 6%. [Copyright &y& Elsevier]

Abstract: Contemporary human activities such as tropical deforestation, land clearing for agriculture, pest control and grassland management lead to biomass burning, which in turn leads to land-cover changes. However, biomass burning emissions are not correctly measured and the methods to assess these emissions form a part of current research area. The traditional methods for estimating aerosols and trace gases released into the atmosphere generally use emission factors associated with fuel loading and moisture characteristics and other parameters that are hard to estimate in near real-time applications. In this paper, fire radiative power (FRP) products were extracted from Moderate Resolution Imaging Spectroradiometer (MODIS) and from the Geostationary Operational Environmental Satellites (GOES) fire products and new South America generic biomes FRE-based smoke aerosol emission coefficients were derived and applied in 2002 South America fire season. The inventory estimated by MODIS and GOES FRP measurements were included in Coupled Aerosol-Tracer Transport model coupled to the Brazilian developments on the Regional Atmospheric Modeling System (CATT-BRAMS) and evaluated with ground truth collected in Large Scale Biosphere–Atmosphere Smoke, Aerosols, Clouds, rainfall, and Climate (SMOCC) and Radiation, Cloud, and Climate Interactions (RaCCI). Although the linear regression showed that GOES FRP overestimates MODIS FRP observations, the use of a common external parameter such as MODIS aerosol optical depth product could minimize the difference between sensors. The relationship between the PM2.5μm (Particulate Matter with diameter less than 2.5 μm) and CO (Carbon Monoxide) model shows a good agreement with SMOCC/RaCCI data in the general pattern of temporal evolution. The results showed high correlations, with values between 0.80 and 0.95 (significant at 0.5 level by student t test), for the CATT-BRAMS simulations with PM2.5μm and CO. [Copyright &y& Elsevier]