Global Environmental Multi-scale – Modelling Air Quality And CHemistry Research Articles

An improved representation of aerosol mixing state for air quality–weather interactions

Abstract. We implement a detailed representation of aerosol mixing state in the Global Environmental Multiscale – Modelling Air quality and CHemistry (GEM-MACH) air quality and weather forecast model. Our mixing-state representation includes three categories: one for more hygroscopic aerosol, one for less hygroscopic aerosol with a high black carbon (BC) mass fraction, and one for less hygroscopic aerosol with a low BC mass fraction. The more detailed representation allows us to better resolve two different aspects of aerosol mixing state: differences in hygroscopicity due to aerosol composition and the amount of absorption enhancement of BC due to non-absorbing coatings. Notably, this three-category representation allows us to account for BC thickly coated with primary organic matter, which enhances the absorption of the BC but has a low hygroscopicity. We compare the results of the three-category representation (1L2B, (one hydrophilic, two hydrophobic)) with a simulation that uses two categories, split by hygroscopicity (HYGRO), and a simulation using the original size-resolved internally mixed assumption (SRIM). We perform a case study that is focused on North America during July 2016, when there were intense wildfires over northwestern North America. We find that the more detailed representation of the aerosol hygroscopicity in both 1L2B and HYGRO decreases wet deposition, which increases aerosol concentrations, particularly of less hygroscopic species. The concentration of PM2.5 increases by 23 % on average. We show that these increased aerosol concentrations increase cloud droplet number concentrations and cloud reflectivity in the model, decreasing surface temperatures. Using two categories based on hygroscopicity yields only a modest benefit in resolving the coating thickness on black carbon, however. The 1L2B representation resolves BC with thinner coatings than the HYGRO simulation, resulting in absorption aerosol optical depths that are 3 % less on average, with greater differences over strong anthropogenic source regions. We did not find strong subsequent effects of this decreased absorption on meteorology.

An ensemble-variational inversion system for the estimation of ammonia emissions using CrIS satellite ammonia retrievals

Abstract. An ensemble-variational inversion system is developed for the estimation of ammonia emissions using ammonia retrievals from the Cross-track Infrared Sounder (CrIS) for use in the Global Environmental Multiscale – Modelling Air quality and Chemistry (GEM-MACH) chemical weather model. A novel hybrid method to compare logarithmic retrieval parameters to model profiles is presented. Inversions for the monthly mean ammonia emissions over North America were performed for May to August 2016. Inversions using the hybrid comparison method increased ammonia emissions at most locations within the model domain, with total monthly mean emissions increasing by 11 %–41 %. The use of these revised emissions in GEM-MACH reduced biases with surface ammonia observations by as much as 25 %. The revised ammonia emissions also improved the forecasts of total (fine + coarse) ammonium and nitrate, as well as ammonium wet deposition, with biases decreasing by as much as 13 %, but they did not improve the forecasts of just the fine components of ammonium and nitrate. A comparison of biases resulting from inversions using different comparison methods shows favourable results for the hybrid comparison method.

Assessing the Impact of Corona-Virus-19 on Nitrogen Dioxide Levels over Southern Ontario, Canada

A lockdown was implemented in Canada mid-March 2020 to limit the spread of COVID-19. In the wake of this lockdown, declines in nitrogen dioxide (NO2) were observed from the TROPOspheric Monitoring Instrument (TROPOMI). A method is presented to quantify how much of this decrease is due to the lockdown itself as opposed to variability in meteorology and satellite sampling. The operational air quality forecast model, GEM-MACH (Global Environmental Multi-scale - Modelling Air quality and CHemistry), was used together with TROPOMI to determine expected NO2 columns that represents what TROPOMI would have observed for a non-COVID scenario. Applying this methodology to southern Ontario, decreases in NO2 emissions due to the lockdown were seen, with an average 40% (roughly 10 kt[NO2]/yr) in Toronto and Mississauga and even larger declines in the city center. Natural and satellite sampling variability accounted for as much as 20–30%, which demonstrates the importance of taking meteorology into account. A model run with reduced emissions (from 65 kt[NO2]/yr to 40 kt[NO2]/yr in the Greater Toronto Area) based on emission activity data during the lockdown period was found to be consistent with TROPOMI NO2 columns.

Expansion of a size disaggregation profile library for particulate matter emissions processing from three generic profiles to 36 source-type-specific profiles

ABSTRACT This study describes a significant upgrade to the particulate matter (PM) size disaggregation profile library used for preparing emissions files for the GEM-MACH (Global Environmental Multiscale-Modelling Air-quality and CHemistry) chemical transport model (CTM). This model uses a sectional (bin) approach to represent the PM size distribution, where one configuration employs 12 size bins to disaggregate PM2.5 and PM10 inventory emissions into the first 10 bins ranging from 0.01 to 10.24 μm in diameter. For the size disaggregation step, a small library of three generic PM size disaggregation profiles is currently applied for three broad source categories (area, mobile, and point). However, as might be expected, these generic profiles are not always representative: for example, emissions from two very different area sources ‒ paved road dust and residential wood combustion ‒ are disaggregated using the same generic size distribution profile. In order to improve the current small PM size disaggregation profile library, a comprehensive literature review was conducted: over 100 relevant publications were identified and PM size distribution profiles for 36 different emission source types were selected and compiled. These 36 source-type-specific PM size distribution profiles were then combined based on process type with corresponding PM speciation profiles to create a library of chemically speciated and size-resolved PM disaggregation profiles. This library can now be used by the SMOKE (Sparse Matrix Operator Kernel Emissions) emissions processing system for the 12-bin version of GEM-MACH to perform PM chemical speciation and size allocation in one step. The size-profile data collected and compiled in this study may also be used for emissions processing for other CTMs with a size-resolved representation of PM. Details of the compilation of the 36 PM size disaggregation profiles are discussed, and the differences in processed PM emissions based on the current and updated PM size disaggregation profile libraries are shown. Implications: A new and expanded particulate matter (PM) size disaggregation profile library covering 36 emission source types has been developed based on an extensive literature review. Its use can produce significant changes in the size allocation of bulk PM inventory emissions processed for input to size-resolved PM chemical transport models. Such models are used to predict atmospheric visibility and to simulate the interactions of aerosol particles with atmospheric radiation and with clouds. The use of more accurate, size-resolved primary PM emissions by these models should improve their predictive skill for atmospheric PM processes affecting air quality, meteorology, and climate.

Dimethyl sulfide and its role in aerosol formation and growth in the Arctic summer – a modelling study

Abstract. Atmospheric dimethyl sulfide, DMS(g), is a climatically important sulfur compound and is the main source of biogenic sulfate aerosol in the Arctic atmosphere. DMS(g) production and emission to the atmosphere increase during the summer due to the greater ice-free sea surface and higher biological activity. We implemented DMS(g) in the Environment and Climate Change Canada’s (ECCC) online air quality forecast model, GEM-MACH (Global Environmental Multiscale–Modelling Air quality and CHemistry), and compared model simulations with DMS(g) measurements made in Baffin Bay and the Canadian Arctic Archipelago in July and August 2014. Two seawater DMS(aq) datasets were used as input for the simulations: (1) a DMS(aq) climatology dataset based on seawater concentration measurements (Lana et al., 2011) and (2) a DMS(aq) dataset based on satellite detection (Galí et al., 2018). In general, GEM-MACH simulations under-predict DMS(g) measurements, which is likely due to the negative biases in both DMS(aq) datasets. However, a higher correlation and smaller bias were obtained with the satellite dataset. Agreement with the observations improved when climatological values were replaced by DMS(aq) in situ values that were measured concurrently with atmospheric observations over Baffin Bay and the Lancaster Sound area in July 2014. The addition of DMS(g) to the GEM-MACH model resulted in a significant increase in atmospheric SO2 for some regions of the Canadian Arctic (up to 100 %). Analysis of the size-segregated sulfate aerosol in the model shows that a significant increase in sulfate mass occurs for particles with a diameter smaller than 200 nm due to the formation and growth of biogenic aerosol at high latitudes (>70∘ N). The enhancement in sulfate particles is most significant in the size range from 50 to 100 nm; however, this enhancement is stronger in the 200–1000 nm size range at lower latitudes (<70∘ N). These results emphasize the important role of DMS(g) in the formation and growth of fine and ultrafine sulfate-containing particles in the Arctic during the summertime.

Assessing the impact of shipping emissions on air pollution in the Canadian Arctic and northern regions: current and future modelled scenarios

Abstract. A first regional assessment of the impact of shipping emissions on air pollution in the Canadian Arctic and northern regions was conducted in this study. Model simulations were carried out on a limited-area domain (at 15 km horizontal resolution) centred over the Canadian Arctic, using the Environment and Climate Change Canada's on-line air quality forecast model, GEM-MACH (Global Environmental Multi-scale – Modelling Air quality and CHemistry), to investigate the contribution from the marine shipping emissions over the Canadian Arctic waters (at both present and projected future levels) to ambient concentrations of criteria pollutants (O3, PM2.5, NO2, and SO2), atmospheric deposition of sulfur (S) and nitrogen (N), and atmospheric loading and deposition of black carbon (BC) in the Arctic. Several model upgrades were introduced for this study, including the treatment of sea ice in the dry deposition parameterization, chemical lateral boundary conditions, and the inclusion of North American wildfire emissions. The model is shown to have similar skills in predicting ambient O3 and PM2.5 concentrations in the Canadian Arctic and northern regions, as the current operational air quality forecast models in North America and Europe. In particular, the model is able to simulate the observed O3 and PM components well at the Canadian high Arctic site, Alert. The model assessment shows that, at the current (2010) level, Arctic shipping emissions contribute to less than 1 % of ambient O3 concentration over the eastern Canadian Arctic and between 1 and 5 % of ambient PM2.5 concentration over the shipping channels. Arctic shipping emissions make a much greater contributions to the ambient NO2 and SO2 concentrations, at 10 %–50 % and 20 %–100 %, respectively. At the projected 2030 business-as-usual (BAU) level, the impact of Arctic shipping emissions is predicted to increase to up to 5 % in ambient O3 concentration over a broad region of the Canadian Arctic and to 5 %–20 % in ambient PM2.5 concentration over the shipping channels. In contrast, if emission controls such as the ones implemented in the current North American Emission Control Area (NA ECA) are to be put in place over the Canadian Arctic waters, the impact of shipping to ambient criteria pollutants would be significantly reduced. For example, with NA-ECA-like controls, the shipping contributions to the population-weighted concentrations of SO2 and PM2.5 would be brought down to below the current level. The contribution of Canadian Arctic shipping to the atmospheric deposition of sulfur and nitrogen is small at the current level, < 5 %, but is expected to increase to up to 20 % for sulfur and 50 % for nitrogen under the 2030 BAU scenario. At the current level, Canadian Arctic shipping also makes only small contributions to BC column loading and BC deposition, with < 0.1 % on average and up to 2 % locally over the eastern Canadian Arctic for the former, and between 0.1 % and 0.5 % over the shipping channels for the latter. The impacts are again predicted to increase at the projected 2030 BAU level, particularly over the Baffin Island and Baffin Bay area in response to the projected increase in ship traffic there, e.g., up to 15 % on BC column loading and locally exceeding 30 % on BC deposition. Overall, the study indicates that shipping-induced changes in atmospheric composition and deposition are at regional to local scales (particularly in the Arctic). Climate feedbacks are thus likely to act at these scales, so climate impact assessments will require modelling undertaken at much finer resolutions than those used in the existing radiative forcing and climate impact assessments.

Improving air quality model predictions of organic species using measurement-derived organic gaseous and particle emissions in a petrochemical-dominated region

Abstract. This study assesses the impact of revised volatile organic compound (VOC) and organic aerosol (OA) emissions estimates in the GEM-MACH (Global Environmental Multiscale–Modelling Air Quality and CHemistry) chemical transport model (CTM) on air quality model predictions of organic species for the Athabasca oil sands (OS) region in Northern Alberta, Canada. The first emissions data set that was evaluated (base-case run) makes use of regulatory-reported VOC and particulate matter emissions data for the large oil sands mining facilities. The second emissions data set (sensitivity run) uses total facility emissions and speciation profiles derived from box-flight aircraft observations around specific facilities. Large increases in some VOC and OA emissions in the revised-emissions data set for four large oil sands mining facilities and decreases for others were found to improve the modeled VOC and OA concentration maxima in facility plumes, as shown with the 99th percentile statistic and illustrated by case studies. The results show that the VOC emission speciation profile from each oil sand facility is unique and different from standard petrochemical-refinery emission speciation profiles used for other regions in North America. A significant increase in the correlation coefficient is reported for the long-chain alkane predictions against observations when using the revised emissions based on aircraft observations. For some facilities, larger long-chain alkane emissions resulted in higher secondary organic aerosol (SOA) production, which improved OA predictions in those plumes. Overall, the use of the revised-emissions data resulted in an improvement of the model mean OA bias; however, a decrease in the OA correlation coefficient and a remaining negative bias suggests the need for further improvements to model OA emissions and formation processes. The weight of evidence suggests that the top-down emission estimation technique helps to better constrain the fugitive organic emissions in the oil sands region, which are a challenge to estimate given the size and complexity of the oil sands operations and the number of steps in the process chain from bitumen extraction to refined oil product. This work shows that the top-down emissions estimation technique may help to constrain bottom-up emission inventories in other industrial regions of the world with large sources of VOCs and OA.

Emissions preparation and analysis for multiscale air quality modeling over the Athabasca Oil Sands Region of Alberta, Canada

Abstract. The oil sands (OS) of Alberta, Canada, which are classified as unconventional oil, are the third-largest oil reserves in the world. We describe here a 6-year effort to improve the emissions data used for air quality (AQ) modeling of the roughly 100 km × 100 km oil extraction and processing industrial complex operating in the Athabasca Oil Sands Region (AOSR) of northeastern Alberta. This paper reviews the national, provincial, and sub-provincial emissions inventories that were available during the three phases of the study, supplemented by hourly SO2 and NOx emissions and stack characteristics for larger point sources measured by a continuous emission monitoring system (CEMS), as well as daily reports of SO2 from one AOSR facility for a 1-week period during a 2013 field campaign when the facility experienced upset conditions. Next it describes the creation of several detailed hybrid emissions inventories and the generation of model-ready emissions input files for the Global Environmental Multiscale–Modelling Air quality and CHemistry (GEM-MACH) AQ modeling system that were used during the 2013 field study and for various post-campaign GEM-MACH sensitivity studies, in particular for a high-resolution model domain with 2.5 km grid spacing covering much of western Canada and centered over the AOSR. Lastly, it compares inventory-based bottom-up emissions with aircraft-observation-based top-down emissions estimates. Results show that emissions values obtained from different data sources can differ significantly, such as a possible 10-fold difference in PM2.5 emissions and approximately 40 and 20 % differences for total VOC (volatile organic compound) and SO2 emissions. A novel emissions-processing approach was also employed to allocate emissions spatially within six large AOSR mining facilities in order to address the urban-scale spatial extent of the facilities and the high-resolution 2.5 km model grid. Gridded facility- and process-specific spatial surrogate fields that were generated using spatial information from GIS (geographic information system) shapefiles and satellite images were used to allocate non-smokestack emissions for each facility to multiple grid cells instead of treating these emissions as point sources and allocating them to a single grid cell as is normally done. Facility- and process-specific temporal profiles and VOC speciation profiles were also developed. The pre-2013 vegetation and land-use databases normally used to estimate biogenic emissions and meteorological surface properties were modified to account for the rapid change in land use in the study area due to marked, year-by-year changes in surface mining activities, including the 2013 opening of a new mine. Lastly, mercury emissions data were also processed in addition to the seven criteria-air-contaminant (CAC) species (NOx, VOC, SO2, NH3, CO, PM2.5, and PM10) to support AOSR mercury modeling activities. Six GEM-MACH modeling papers in this special issue used some of these new sets of emissions and land-use input files.

Estimates of exceedances of critical loads for acidifying deposition in Alberta and Saskatchewan

Abstract. Estimates of potential harmful effects on ecosystems in the Canadian provinces of Alberta and Saskatchewan due to acidifying deposition were calculated, using a 1-year simulation of a high-resolution implementation of the Global Environmental Multiscale-Modelling Air-quality and Chemistry (GEM-MACH) model, and estimates of aquatic and terrestrial ecosystem critical loads. The model simulation was evaluated against two different sources of deposition data: total deposition in precipitation and total deposition to snowpack in the vicinity of the Athabasca oil sands. The model captured much of the variability of observed ions in wet deposition in precipitation (observed versus model sulfur, nitrogen and base cation R2 values of 0.90, 0.76 and 0.72, respectively), while being biased high for sulfur deposition, and low for nitrogen and base cations (slopes 2.2, 0.89 and 0.40, respectively). Aircraft-based estimates of fugitive dust emissions, shown to be a factor of 10 higher than reported to national emissions inventories (Zhang et al., 2018), were used to estimate the impact of increased levels of fugitive dust on model results. Model comparisons to open snowpack observations were shown to be biased high, but in reasonable agreement for sulfur deposition when observations were corrected to account for throughfall in needleleaf forests. The model–observation relationships for precipitation deposition data, along with the expected effects of increased (unreported) base cation emissions, were used to provide a simple observation-based correction to model deposition fields. Base cation deposition was estimated using published observations of base cation fractions in surface-collected particles (Wang et al., 2015).Both original and observation-corrected model estimates of sulfur, nitrogen, and base cation deposition were used in conjunction with critical load data created using the NEG-ECP (2001) and CLRTAP (2017) methods for calculating critical loads, using variations on the Simple Mass Balance model for terrestrial ecosystems, and the Steady State Water Chemistry and First-order Acidity Balance models for aquatic ecosystems. Potential ecosystem damage was predicted within each of the regions represented by the ecosystem critical load datasets used here, using a combination of 2011 and 2013 emissions inventories. The spatial extent of the regions in exceedance of critical loads varied between 1 × 104 and 3.3 × 105 km2, for the more conservative observation-corrected estimates of deposition, with the variation dependent on the ecosystem and critical load calculation methodology. The larger estimates (for aquatic ecosystems) represent a substantial fraction of the area of the provinces examined.Base cation deposition was shown to be sufficiently high in the region to have a neutralizing effect on acidifying deposition, and the use of the aircraft and precipitation observation-based corrections to base cation deposition resulted in reasonable agreement with snowpack data collected in the oil sands area. However, critical load exceedances calculated using both observations and observation-corrected deposition suggest that the neutralization effect is limited in spatial extent, decreasing rapidly with distance from emissions sources, due to the rapid deposition of emitted primary dust particles as a function of their size. We strongly recommend the use of observation-based correction of model-simulated deposition in estimating critical load exceedances, in future work.

A chemical transport model study of plume-rise and particle size distribution for the Athabasca oil sands

Abstract. We evaluate four high-resolution model simulations of pollutant emissions, chemical transformation, and downwind transport for the Athabasca oil sands using the Global Environmental Multiscale – Modelling Air-quality and Chemistry (GEM-MACH) model, and compare model results with surface monitoring network and aircraft observations of multiple pollutants, for simulations spanning a time period corresponding to an aircraft measurement campaign in the summer of 2013. We have focussed here on the impact of different representations of the model's aerosol size distribution and plume-rise parameterization on model results. The use of a more finely resolved representation of the aerosol size distribution was found to have a significant impact on model performance, reducing the magnitude of the original surface PM2.5 negative biases 32 %, from −2.62 to −1.72 µg m−3. We compared model predictions of SO2, NO2, and speciated particulate matter concentrations from simulations employing the commonly used Briggs (1984) plume-rise algorithms to redistribute emissions from large stacks, with stack plume observations. As in our companion paper (Gordon et al., 2017), we found that Briggs algorithms based on estimates of atmospheric stability at the stack height resulted in under-predictions of plume rise, with 116 out of 176 test cases falling below the model : observation 1 : 2 line, 59 cases falling within a factor of 2 of the observed plume heights, and an average model plume height of 289 m compared to an average observed plume height of 822 m. We used a high-resolution meteorological model to confirm the presence of significant horizontal heterogeneity in the local meteorological conditions driving plume rise. Using these simulated meteorological conditions at the stack locations, we found that a layered buoyancy approach for estimating plume rise in stable to neutral atmospheres, coupled with the assumption of free rise in convectively unstable atmospheres, resulted in much better model performance relative to observations (124 out of 176 cases falling within a factor of 2 of the observed plume height, with 69 of these cases above and 55 of these cases below the 1 : 1 line and within a factor of 2 of observed values). This is in contrast to our companion paper, wherein this layered approach (driven by meteorological observations not co-located with the stacks) showed a relatively modest impact on predicted plume heights. Persistent issues with over-fumigation of plumes in the model were linked to a more rapid decrease in simulated temperature with increasing height than was observed. This in turn may have led to overestimates of near-surface diffusivity, resulting in excessive fumigation.

OMI satellite observations of decadal changes in ground-level sulfur dioxide over North America

Abstract. Sulfur dioxide (SO2) has a significant impact on the environment and human health. We estimated ground-level sulfur dioxide (SO2) concentrations from the Ozone Monitoring Instrument (OMI) using SO2 profiles from the Global Environmental Multi-scale – Modelling Air quality and CHemistry (GEM-MACH) model over North America for the period of 2005–2015. OMI-derived ground-level SO2 concentrations (r = 0. 61) and trends (r = 0. 74) correlated well with coincident in situ measurements from air quality networks over North America. We found a strong decreasing trend in coincidently sampled ground-level SO2 from OMI (−81 ± 19 %) and in situ measurements (−86 ± 13 %) over the eastern US for the period of 2005–2015, which reflects the implementation of stricter pollution control laws, including flue-gas desulfurization (FGD) devices in power plants. The spatially and temporally contiguous OMI-derived ground-level SO2 concentrations can be used to assess the impact of long-term exposure to SO2 on the health of humans and the environment.

Tropospheric Emission Spectrometer (TES) satellite observations of ammonia, methanol, formic acid, and carbon monoxide over the Canadian oil sands: validation and model evaluation

Abstract. The wealth of air quality information provided by satellite infrared observations of ammonia (NH3), carbon monoxide (CO), formic acid (HCOOH), and methanol (CH3OH) is currently being explored and used for a number of applications, especially at regional or global scales. These applications include air quality monitoring, trend analysis, emissions, and model evaluation. This study provides one of the first direct validations of Tropospheric Emission Spectrometer (TES) satellite-retrieved profiles of NH3, CH3OH, and HCOOH through comparisons with coincident aircraft profiles. The comparisons are performed over the Canadian oil sands region during the intensive field campaign (August–September, 2013) in support of the Joint Canada–Alberta Implementation Plan for Oil Sands Monitoring (JOSM). The satellite/aircraft comparisons over this region during this period produced errors of (i) +0.08 ± 0.25 ppbv for NH3, (ii) +7.5 ± 23 ppbv for CO, (iii) +0.19 ± 0.46 ppbv for HCOOH, and (iv) −1.1 ± 0.39 ppbv for CH3OH. These values mostly agree with previously estimated retrieval errors; however, the relatively large negative bias in CH3OH and the significantly greater positive bias for larger HCOOH and CO values observed during this study warrant further investigation. Satellite and aircraft ammonia observations during the field campaign are also used in an initial effort to perform preliminary evaluations of Environment Canada's Global Environmental Multi-scale – Modelling Air quality and CHemistry (GEM-MACH) air quality modelling system at high resolution (2.5 × 2.5 km2). These initial results indicate a model underprediction of ~ 0.6 ppbv (~ 60 %) for NH3, during the field campaign period. The TES/model CO comparison differences are ~ +20 ppbv (~ +20 %), but given that under these conditions the TES/aircraft comparisons also show a small positive TES CO bias indicates that the overall model underprediction of CO is closer to ~ 10 % at 681 hPa (~ 3 km) during this period.