scholarly journals Identifying the sources driving observed PM<sub>2.5</sub> temporal variability over Halifax, Nova Scotia, during BORTAS-B

2013 ◽  
Vol 13 (14) ◽  
pp. 7199-7213 ◽  
Author(s):  
M. D. Gibson ◽  
J. R. Pierce ◽  
D. Waugh ◽  
J. S. Kuchta ◽  
L. Chisholm ◽  
...  

Abstract. The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia, was investigated between 11 July and 26 August 2011 using measurements of PM2.5 mass and PM2.5 chemical composition (black carbon, organic matter, anions, cations and 33 elements). This was part of the BORTAS-B (quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which investigated the atmospheric chemistry and transport of seasonal boreal wildfire emissions over eastern Canada in 2011. The US EPA Positive Matrix Factorization (PMF) receptor model was used to determine the average mass (percentage) source contribution over the 45 days, which was estimated to be as follows: long-range transport (LRT) pollution: 1.75 μg m−3 (47%); LRT pollution marine mixture: 1.0 μg m−3 (27.9%); vehicles: 0.49 μg m−3 (13.2%); fugitive dust: 0.23 μg m−3 (6.3%); ship emissions: 0.13 μg m−3 (3.4%); and refinery: 0.081 μg m−3 (2.2%). The PMF model describes 87% of the observed variability in total PM2.5 mass (bias = 0.17 and RSME = 1.5 μg m−3). The factor identifications are based on chemical markers, and they are supported by air mass back trajectory analysis and local wind direction. Biomass burning plumes, found by other surface and aircraft measurements, were not significant enough to be identified in this analysis. This paper presents the results of the PMF receptor modelling, providing valuable insight into the local and upwind sources impacting surface PM2.5 in Halifax and a vital comparative data set for the other collocated ground-based observations of atmospheric composition made during BORTAS-B.

2013 ◽  
Vol 13 (2) ◽  
pp. 4491-4533 ◽  
Author(s):  
M. D. Gibson ◽  
J. R. Pierce ◽  
D. Waugh ◽  
J. S. Kuchta ◽  
L. Chisholm ◽  
...  

Abstract. The source attribution of observed variability of total PM2.5 concentrations over Halifax, Nova Scotia was investigated between 11 July–26 August 2011 using measurements of PM2.5 mass and PM2.5 chemical composition (black carbon, organic matter, anions, cations and 33 elements). This was part of the BORTAS-B (quantifying the impact of BOReal forest fires on Tropospheric oxidants using aircraft and satellites) experiment, which investigated the atmospheric chemistry and transport of seasonal boreal wild fire emissions over eastern Canada in 2011. The US EPA Positive Matrix Factorization (PMF) receptor model was used to determine the average mass (percentage) source contribution over the 45 days, which was estimated to be: Long-Range Transport (LRT) Pollution 1.75 μg m−3 (47%), LRT Pollution Marine Mixture 1.0 μg m−3 (27.9%), Vehicles 0.49 μg m−3 (13.2%), Fugitive Dust 0.23 μg m−3 (6.3%), Ship Emissions 0.13 μg m−3 (3.4%) and Refinery 0.081 μg m−3 (2.2%). The PMF model describes 87% of the observed variability in total PM2.5 mass (bias = 0.17 and RSME = 1.5 μg m−3). The factor identifications are based on chemical markers, and they are supported by air mass back trajectory analysis and local wind direction. Biomass burning plumes, found by other surface and aircraft measurements, were not significant enough to be identified in this analysis. This paper presents the results of the PMF receptor modelling, providing valuable insight into the local and upwind sources impacting surface PM2.5 in Halifax during the BORTAS-B mission.


2013 ◽  
Vol 13 (2) ◽  
pp. 4127-4181 ◽  
Author(s):  
P. I. Palmer ◽  
M. Parrington ◽  
J. D. Lee ◽  
A. C. Lewis ◽  
A. R. Rickard ◽  
...  

Abstract. We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of airmasses that contain the emission products from seasonal boreal wildfires and how these airmasses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada. The planned July 2010 deployment of the ARA was postponed by 12 months because of activities related to the dispersal of material emitted by the Eyjafjallajökull volcano. However, most other planned model and measurement activities, including ground-based measurements at the Dalhousie University Ground Station (DGS), enhanced ozonesonde launches, and measurements at the Pico Atmospheric Observatory in the Azores, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 included the same measurements, but included the ARA, special satellite observations and a more comprehensive measurement suite at the DGS. The high-frequency aircraft data provided a comprehensive snapshot of the pyrogenic plumes from wildfires. The coordinated ground-based and sonde data provided detailed but spatially-limited information that put the aircraft data into context of the longer burning season. We coordinated aircraft vertical profiles and overpasses of the NASA Tropospheric Emission Spectrometer and the Canadian Atmospheric Chemistry Experiment. These space-borne data, while less precise than other data, helped to relate the two-week measurement campaign to larger geographical and longer temporal scales. We interpret these data using a range of chemistry models: from a near-explicit gas-phase chemical mechanism, which tests out understanding of the underlying chemical mechanism, to regional and global 3-D models of atmospheric transport and lumped chemistry, which helps to assess the performance of the simplified chemical mechanism and effectively act as intermediaries between different measurement types. We also present an overview of some of the new science that has originated from this project from the mission planning and execution to the analysis of the ground-based, aircraft, and space-borne data.


2013 ◽  
Vol 13 (13) ◽  
pp. 6239-6261 ◽  
Author(s):  
P. I. Palmer ◽  
M. Parrington ◽  
J. D. Lee ◽  
A. C. Lewis ◽  
A. R. Rickard ◽  
...  

Abstract. We describe the design and execution of the BORTAS (Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) experiment, which has the overarching objective of understanding the chemical aging of air masses that contain the emission products from seasonal boreal wildfires and how these air masses subsequently impact downwind atmospheric composition. The central focus of the experiment was a two-week deployment of the UK BAe-146-301 Atmospheric Research Aircraft (ARA) over eastern Canada, based out of Halifax, Nova Scotia. Atmospheric ground-based and sonde measurements over Canada and the Azores associated with the planned July 2010 deployment of the ARA, which was postponed by 12 months due to UK-based flights related to the dispersal of material emitted by the Eyjafjallajökull volcano, went ahead and constituted phase A of the experiment. Phase B of BORTAS in July 2011 involved the same atmospheric measurements, but included the ARA, special satellite observations and a more comprehensive ground-based measurement suite. The high-frequency aircraft data provided a comprehensive chemical snapshot of pyrogenic plumes from wildfires, corresponding to photochemical (and physical) ages ranging from < 1 day to ~


2012 ◽  
Vol 12 (12) ◽  
pp. 31629-31661 ◽  
Author(s):  
K. A. Tereszchuk ◽  
G. González Abad ◽  
C. Clerbaux ◽  
J. Hadji-Lazaro ◽  
D. Hurtmans ◽  
...  

Abstract. To further our understanding of the effects of biomass burning emissions on atmospheric composition, the Quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites (BORTAS) campaign was conducted on 12 July to 3 August 2011 during the Boreal forest fire season in Canada. The simultaneous aerial, ground and satellite measurement campaign sought to record instances of Boreal biomass burning to measure the tropospheric volume mixing ratios (VMRs) of short- and long-lived trace molecular species from biomass burning emissions. The goal was to investigate the connection between the composition and the distribution of these pyrogenic outflows and their resulting perturbation to atmospheric chemistry, with particular focus on oxidant species to determine the overall impact on the oxidizing capacity of the free troposphere. Measurements of pyrogenic trace species in Boreal biomass burning plumes were made by the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) onboard the Canadian Space Agency (CSA) SCISAT-1 satellite during the BORTAS campaign. Even though most biomass burning smoke is typically confined to the boundary layer, emissions are often injected directly into the upper troposphere via fire-related convective processes, thus allowing space-borne instruments to measure these pyrogenic outflows. An extensive set of 15 molecules, CH3OH, CH4, C2H2, C2H6, C3H6O, CO, HCN, HCOOH, HNO3, H2CO, NO, NO2, OCS, O3 and PAN have been analyzed. Included in this analysis is the calculation of age-dependent sets of enhancement ratios for each of the species.


2019 ◽  
Vol 12 (3) ◽  
pp. 1209-1225 ◽  
Author(s):  
Christoph A. Keller ◽  
Mat J. Evans

Abstract. Atmospheric chemistry models are a central tool to study the impact of chemical constituents on the environment, vegetation and human health. These models are numerically intense, and previous attempts to reduce the numerical cost of chemistry solvers have not delivered transformative change. We show here the potential of a machine learning (in this case random forest regression) replacement for the gas-phase chemistry in atmospheric chemistry transport models. Our training data consist of 1 month (July 2013) of output of chemical conditions together with the model physical state, produced from the GEOS-Chem chemistry model v10. From this data set we train random forest regression models to predict the concentration of each transported species after the integrator, based on the physical and chemical conditions before the integrator. The choice of prediction type has a strong impact on the skill of the regression model. We find best results from predicting the change in concentration for long-lived species and the absolute concentration for short-lived species. We also find improvements from a simple implementation of chemical families (NOx = NO + NO2). We then implement the trained random forest predictors back into GEOS-Chem to replace the numerical integrator. The machine-learning-driven GEOS-Chem model compares well to the standard simulation. For ozone (O3), errors from using the random forests (compared to the reference simulation) grow slowly and after 5 days the normalized mean bias (NMB), root mean square error (RMSE) and R2 are 4.2 %, 35 % and 0.9, respectively; after 30 days the errors increase to 13 %, 67 % and 0.75, respectively. The biases become largest in remote areas such as the tropical Pacific where errors in the chemistry can accumulate with little balancing influence from emissions or deposition. Over polluted regions the model error is less than 10 % and has significant fidelity in following the time series of the full model. Modelled NOx shows similar features, with the most significant errors occurring in remote locations far from recent emissions. For other species such as inorganic bromine species and short-lived nitrogen species, errors become large, with NMB, RMSE and R2 reaching >2100 % >400 % and <0.1, respectively. This proof-of-concept implementation takes 1.8 times more time than the direct integration of the differential equations, but optimization and software engineering should allow substantial increases in speed. We discuss potential improvements in the implementation, some of its advantages from both a software and hardware perspective, its limitations, and its applicability to operational air quality activities.


2015 ◽  
Vol 42 (12) ◽  
pp. 1071-1089
Author(s):  
Alan Chan ◽  
Bruce G. Fawcett ◽  
Shu-Kam Lee

Purpose – Church giving and attendance are two important indicators of church health and performance. In the literature, they are usually understood to be simultaneously determined. The purpose of this paper is to estimate if there a sustainable church congregation size using Wintrobe’s (1998) dictatorship model. The authors want to examine the impact of youth and adult ministry as well. Design/methodology/approach – Using the data collected from among Canadian Baptist churches in Eastern Canada, this study investigates the factors affecting the level of the two indicators by the panel-instrumental variable technique. Applying Wintrobe’s (1998) political economy model on dictatorship, the equilibrium level of worship attendance and giving is predicted. Findings – Through various simulation exercises, the actual church congregation sizes is approximately 50 percent of the predicted value, implying inefficiency and misallocation of church resources. The paper concludes with insights on effective ways church leaders can allocate scarce resources to promote growth within churches. Originality/value – The authors are the only researchers getting the permission from the Atlantic Canada Baptist Convention to use their mega data set on church giving and congregation sizes as per the authors’ knowledge. The authors are also applying a theoretical model on dictatorship to religious/not for profits organizations.


2014 ◽  
Vol 7 (4) ◽  
pp. 5447-5464 ◽  
Author(s):  
S. Tilmes ◽  
M. J. Mills ◽  
U. Niemeier ◽  
H. Schmidt ◽  
A. Robock ◽  
...  

Abstract. A new Geoengineering Model Intercomparison Project (GeoMIP) experiment "G4 specified stratospheric aerosols" (short name: G4SSA) is proposed to investigate the impact of stratospheric aerosol geoengineering on atmospheric composition, climate, and the environment. In contrast to the earlier G4 GeoMIP experiment, which requires an emission of sulphur dioxide (SO2) into the model, a prescribed aerosol forcing file is provided to the community, to be consistently applied to future model experiments between 2020 and 2100. This stratospheric aerosol distribution, with a total burden of about 2 Tg S has been derived using the ECHAM5-HAM microphysical model, based on a continuous annual tropical emission of 8 Tg SO2 year−1. A ramp-up of geoengineering in 2020 and a ramp-down in 2070 over a period of two years are included in the distribution, while a background aerosol burden should be used for the last 3 decades of the experiment. The performance of this experiment using climate and chemistry models in a multi-model comparison framework will allow us to better understand the significance of the impact of geoengineering and the abrupt termination after 50 years on climate and composition of the atmosphere in a changing environment. The zonal and monthly mean stratospheric aerosol input dataset is available at https://www2.acd.ucar.edu/gcm/geomip-g4-specified-stratospheric-aerosol-data-set.


2005 ◽  
Vol 13 ◽  
pp. 891-893
Author(s):  
Thierry Fouchet

AbstractIn this brief summary, I present recent progress on our knowledge of the Giant Planets and Titan atmospheric composition, as well as the impact of this progress on our understanding of Solar System formation, and atmospheric chemistry.


2020 ◽  
Author(s):  
Rachael Rhodes ◽  
Xin Yang ◽  
Eric Wolff

&lt;p&gt;It is important to understand the magnitude and rate of past sea ice changes, as well as their timing relative to abrupt shifts in other components of Earth&amp;#8217;s climate system. Furthermore, records of past sea ice over the last few centuries are urgently needed to assess the scale of natural (internal) variability over decadal timescales. By continuously recording past atmospheric composition, polar ice cores have the potential to document changing sea ice conditions if atmospheric chemistry is altered. &amp;#160;Sea salt aerosol, specifically sodium (Na), and bromine enrichment (Br&lt;sub&gt;enr&lt;/sub&gt;, Br/Na enriched relative to seawater ratio) are two ice core sea ice proxies suggested following this premise.&lt;/p&gt;&lt;p&gt;Here we aim to move beyond a conceptual understanding of the controls on Na and Br&lt;sub&gt;enr&lt;/sub&gt; in ice cores by using process-based modelling to test hypotheses. We present results of experiments using a 3D global chemical transport model (p-TOMCAT) that represents marine aerosol emission, transport and deposition. Critically, the complex atmospheric chemistry of bromine is also included. Three fundamental issues will be examined: 1) the partitioning of Br between gas and aerosol phases, 2) sea salt aerosol production from first-year versus multi-year sea ice, and 3) the impact of increased acidity in the atmosphere due to human activity in the Arctic.&lt;/p&gt;


2016 ◽  
Vol 16 (4) ◽  
pp. 1937-1953 ◽  
Author(s):  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  

Abstract. Continuous hourly measurements of gas-phase ammonia (NH3(g)) were taken from 13 July to 7 August 2014 on a research cruise throughout Baffin Bay and the eastern Canadian Arctic Archipelago. Concentrations ranged from 30 to 650 ng m−3 (40–870 pptv) with the highest values recorded in Lancaster Sound (74°13′ N, 84°00′ W). Simultaneous measurements of total ammonium ([NHx]), pH and temperature in the ocean and in melt ponds were used to compute the compensation point (χ), which is the ambient NH3(g) concentration at which surface–air fluxes change direction. Ambient NH3(g) was usually several orders of magnitude larger than both χocean and χMP (< 0.4–10 ng m3) indicating these surface pools are net sinks of NH3. Flux calculations estimate average net downward fluxes of 1.4 and 1.1 ng m−2 s−1 for the open ocean and melt ponds, respectively. Sufficient NH3(g) was present to neutralize non-sea-salt sulfate (nss-SO42−) in the boundary layer during most of the study. This finding was corroborated with a historical data set of PM2.5 composition from Alert, Nunavut (82°30′ N, 62°20′ W) wherein the median ratio of NH4+/nss-SO42− equivalents was greater than 0.75 in June, July and August. The GEOS-Chem chemical transport model was employed to examine the impact of NH3(g) emissions from seabird guano on boundary-layer composition and nss-SO42− neutralization. A GEOS-Chem simulation without seabird emissions underestimated boundary layer NH3(g) by several orders of magnitude and yielded highly acidic aerosol. A simulation that included seabird NH3 emissions was in better agreement with observations for both NH3(g) concentrations and nss-SO42− neutralization. This is strong evidence that seabird colonies are significant sources of NH3 in the summertime Arctic, and are ubiquitous enough to impact atmospheric composition across the entire Baffin Bay region. Large wildfires in the Northwest Territories were likely an important source of NH3, but their influence was probably limited to the Central Canadian Arctic. Implications of seabird-derived N-deposition to terrestrial and aquatic ecosystems are also discussed.


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