Evaluation of Uncertainties in the Anthropogenic SO2 Emissions in the USA from the OMI Point Source Catalog.

Satellite remote sensing is a promising method of monitoring emissions that may be missing in inventories, but the accuracy of these estimates is often not clear. We demonstrate here a comprehensive evaluation of errors in anthropogenic sulfur dioxide (SO2) emission estimates from NASA's OMI point source catalog for the contiguous US by comparing emissions from the catalog with high-quality emission inventory data over different dimensions including size of individual sources, aggregate vs individual source errors, and potential bias in individual source estimates over time. For sources that are included in the catalog, we find that errors in aggregate (sum of error for all included sources) are relatively low. Errors for individual sources in any given year can be substantial, however, with over- or underestimates in terms of total error ranging from -80 to 110 kt (roughly 10-90th percentile). We find that these errors are not necessarily random over time and that there can be consistently positive or negative biases for individual sources. We did not find any overall statistical relationship between the degree of isolation of a source and bias, either at a 40 or 70 km scales. For a sub-set of sources where inventory emissions over a radius of 70 km around an OMI detection are larger than twice the emissions within 40 km, the OMI value is consistently overestimated. We find, as expected, that emission sources not included in the catalog are the largest aggregate source of difference between the satellite estimates and inventories, especially in more recent years where source emission magnitudes have been decreasing and note that trends in satellite detections do not necessarily track trends in total emissions. We find that the OMI-based SO2 emissions are accurate in aggregate, when summed over a number of sources, but must be interpreted more cautiously at the individual source level. Similar analyses would be valuable for other satellite emission estimates; however, in many cases, the appropriate high-quality reference data may need to be generated.

Aircraft and satellite observations reveal historical gap between top-down and bottom-up CO2 emissions from Canadian oil sands.

Measurement-based estimates of greenhouse gas (GHG) emissions from complex industrial operations are challenging to obtain, but serve as an important, independent check on inventory-reported emissions. Such top-down estimates, while important for oil and gas (O&G) emissions globally, are particularly relevant for Canadian oil sands (OS) operations, which represent the largest O&G contributor to national GHG emissions. We present a multifaceted top-down approach for estimating CO2 emissions that combines aircraft-measured CO2/NOx emission ratios (ERs) with inventory and satellite-derived NOx emissions from Ozone Monitoring Instrument (OMI) and TROPOspheric Ozone Monitoring Instrument (TROPOMI) and apply it to the Athabasca Oil Sands Region (AOSR) in Alberta, Canada. Historical CO2 emissions were reconstructed for the surface mining region, and average top-down estimates were found to be >65% higher than facility-reported, bottom-up estimates from 2005 to 2020. Higher top-down vs. bottom-up emissions estimates were also consistently obtained for individual surface mining and in situ extraction facilities, which represent a growing category of energy-intensive OS operations. Although the magnitudes of the measured discrepancies vary between facilities, they combine such that the observed reporting gap for total AOSR emissions is ≥(31 ± 8) Mt for each of the last 3 years (2018-2020). This potential underestimation is large and broadly highlights the importance of continued review and refinement of bottom-up estimation methodologies and inventories. The ER method herein offers a powerful approach for upscaling measured facility-level or regional fossil fuel CO2 emissions by taking advantage of satellite remote sensing observations.

Airborne Emission Rate Measurements Validate Remote Sensing Observations and Emission Inventories of Western U.S. Wildfires.

Carbonaceous emissions from wildfires are a dynamic mixture of gases and particles that have important impacts on air quality and climate. Emissions that feed atmospheric models are estimated using burned area and fire radiative power (FRP) methods that rely on satellite products. These approaches show wide variability and have large uncertainties, and their accuracy is challenging to evaluate due to limited aircraft and ground measurements. Here, we present a novel method to estimate fire plume-integrated total carbon and speciated emission rates using a unique combination of lidar remote sensing aerosol extinction profiles and in situ measured carbon constituents. We show strong agreement between these aircraft-derived emission rates of total carbon and a detailed burned area-based inventory that distributes carbon emissions in time using Geostationary Operational Environmental Satellite FRP observations (Fuel2Fire inventory, slope = 1.33 ± 0.04, r2 = 0.93, and RMSE = 0.27). Other more commonly used inventories strongly correlate with aircraft-derived emissions but have wide-ranging over- and under-predictions. A strong correlation is found between carbon monoxide emissions estimated in situ with those derived from the TROPOspheric Monitoring Instrument (TROPOMI) for five wildfires with coincident sampling windows (slope = 0.99 ± 0.18; bias = 28.5%). Smoke emission coefficients (g MJ-1) enable direct estimations of primary gas and aerosol emissions from satellite FRP observations, and we derive these values for many compounds emitted by temperate forest fuels, including several previously unreported species.

Global fine-scale changes in ambient NO2 during COVID-19 lockdowns.

Nitrogen dioxide (NO2) is an important contributor to air pollution and can adversely affect human health1-9. A decrease in NO2 concentrations has been reported as a result of lockdown measures to reduce the spread of COVID-1910-20. Questions remain, however, regarding the relationship of satellite-derived atmospheric column NO2 data with health-relevant ambient ground-level concentrations, and the representativeness of limited ground-based monitoring data for global assessment. Here we derive spatially resolved, global ground-level NO2 concentrations from NO2 column densities observed by the TROPOMI satellite instrument at sufficiently fine resolution (approximately one kilometre) to allow assessment of individual cities during COVID-19 lockdowns in 2020 compared to 2019. We apply these estimates to quantify NO2 changes in more than 200 cities, including 65 cities without available ground monitoring, largely in lower-income regions. Mean country-level population-weighted NO2 concentrations are 29% ± 3% lower in countries with strict lockdown conditions than in those without. Relative to long-term trends, NO2 decreases during COVID-19 lockdowns exceed recent Ozone Monitoring Instrument (OMI)-derived year-to-year decreases from emission controls, comparable to 15 ± 4 years of reductions globally. Our case studies indicate that the sensitivity of NO2 to lockdowns varies by country and emissions sector, demonstrating the critical need for spatially resolved observational information provided by these satellite-derived surface concentration estimates.

Disentangling the Impact of the COVID-19 Lockdowns on Urban NO2 From Natural Variability.

TROPOMI satellite data show substantial drops in nitrogen dioxide (NO2) during COVID-19 physical distancing. To attribute NO2 changes to NO x emissions changes over short timescales, one must account for meteorology. We find that meteorological patterns were especially favorable for low NO2 in much of the United States in spring 2020, complicating comparisons with spring 2019. Meteorological variations between years can cause column NO2 differences of ~15% over monthly timescales. After accounting for solar angle and meteorological considerations, we calculate that NO2 drops ranged between 9.2% and 43.4% among 20 cities in North America, with a median of 21.6%. Of the studied cities, largest NO2 drops (>30%) were in San Jose, Los Angeles, and Toronto, and smallest drops (<12%) were in Miami, Minneapolis, and Dallas. These normalized NO2 changes can be used to highlight locations with greater activity changes and better understand the sources contributing to adverse air quality in each city.

Enhanced Capabilities of TROPOMI NO2: Estimating NOX from North American Cities and Power Plants.

The TROPOspheric Monitoring Instrument (TROPOMI) is used to derive top-down NOX emissions for two large power plants and three megacities in North America. We first re-process the vertical column NO2 with an improved air mass factor to correct for a known systematic low bias in the operational retrieval near urban centers. For the two power plants, top-down NOX emissions agree to within 10% of the emissions reported by the power plants. We then derive top-down NOX emissions rates for New York City, Chicago, and Toronto, and compare them to projected bottom-up emissions inventories. In this analysis of 2018 NOX emissions, we find a +22% overestimate for New York City, a -21% underestimate in Toronto, and good agreement in Chicago in the projected bottom-up inventories when compared to the top-down emissions. Top-down NOX emissions also capture intraseasonal variability, such as the weekday versus weekend effect (emissions are +45% larger on weekdays versus weekends in Chicago). Finally, we demonstrate the enhanced capabilities of TROPOMI, which allow us to derive a NOX emissions rate for Chicago using a single overpass on July 7, 2018. The large signal-to-noise ratio of TROPOMI is well-suited for estimating NOX emissions from relatively small sources and for sub-seasonal timeframes.

Exploiting OMI NO2 satellite observations to infer fossil-fuel CO2 emissions from U.S. megacities.

Fossil-fuel CO2 emissions and their trends in eight U.S. megacities during 2006-2017 are inferred by combining satellite-derived NOX emissions with bottom-up city-specific NOX-to-CO2 emission ratios. A statistical model is fit to a collection NO2 plumes observed from the Ozone Monitoring Instrument (OMI), and is used to calculate top-down NOX emissions. Decreases in OMI-derived NOX emissions are observed across the eight cities from 2006 to 2017 (-17% in Miami to -58% in Los Angeles), and are generally consistent with long-term trends of bottom-up inventories (-25% in Miami to -49% in Los Angeles), but there are some interannual discrepancies. City-specific NOX-to-CO2 emission ratios, used to calculate inferred CO2, are estimated through annual bottom-up inventories of NOX and CO2 emissions disaggregated to 1 × 1 km2 resolution. Over the study period, NOX-to-CO2 emission ratios have decreased by ~40% nationwide (-24% to -51% for our studied cities), which is attributed to a faster reduction in NOX when compared to CO2 due to policy regulations and fuel type shifts. Combining top-down NOX emissions and bottom-up NOX-to-CO2 emission ratios, annual fossil-fuel CO2 emissions are derived. Inferred OMI-based top-down CO2 emissions trends vary between +7% in Dallas to -31% in Phoenix. For 2017, we report annual fossil-fuel CO2 emissions to be: Los Angeles 113 ±â€¯49 Tg/yr; New York City 144 ±â€¯62 Tg/yr; and Chicago 55 ±â€¯24 Tg/yr. A study in the Los Angeles area, using independent methods, reported a 2013-2016 average CO2 emissions rate of 104 Tg/yr and 120 Tg/yr, which suggests that the CO2 emissions from our method are in good agreement with other studies' top-down estimates. We anticipate future remote sensing instruments - with better spatial and temporal resolution - will better constrain the NOX-to-CO2 ratio and reduce the uncertainty in our method.

High resolution mapping of nitrogen dioxide with TROPOMI: First results and validation over the Canadian oil sands.

TROPOMI, on-board the Sentinel-5 Precursor satellite is a nadir-viewing spectrometer measuring reflected sunlight in the ultraviolet, visible, near-infrared, and shortwave infrared spectral range. From these spectra several important air quality and climate-related atmospheric constituents are retrieved at an unprecedented high spatial resolution, including nitrogen dioxide (NO2). We present the first retrievals of TROPOMI NO2 over the Canadian Oil Sands, contrasting them with observations from the OMI satellite instrument, and demonstrate its ability to resolve individual plumes and highlight its potential for deriving emissions from individual mining facilities. Further, the first TROPOMI NO2 validation is presented, consisting of aircraft and surface in-situ NO2 observations, as well as ground-based remote-sensing measurements between March and May 2018. Our comparisons show that the TROPOMI NO2 vertical column densities are highly correlated with the aircraft and surface in-situ NO2 observations, and the ground-based remote-sensing measurements with a low bias (15-30 %) over the Canadian Oil Sands. PLAIN LANGUAGE SUMMARY: Nitrogen dioxide (NO2) is a pollutant that is linked to respiratory health issues and has negative environmental impacts such as soil and water acidification. Near the surface the most significant sources of NO2 are fossil fuel combustion and biomass burning. With a recently launched satellite instrument (TROPOspheric Monitoring Instrument; TROPOMI) NO2 can be measured with an unprecedented combination of accuracy, spatial coverage, and resolution. This work presents the first TROPOMI NO2 measurements near the Canadian Oil Sands and shows that these measurements have an outstanding ability to detect NO2 on a very high horizontal resolution that is unprecedented for satellite NO2 observations. Further, these satellite measurements are in excellent agreement with aircraft and ground-based measurements.

Assessing snow extent data sets over North America to inform and improve trace gas retrievals from solar backscatter.

Accurate representation of surface reflectivity is essential to tropospheric trace gas retrievals from solar backscatter observations. Surface snow cover presents a significant challenge due to its variability and thus snow-covered scenes are often omitted from retrieval data sets; however, the high reflectance of snow is potentially advantageous for trace gas retrievals. We first examine the implications of surface snow on retrievals from the upcoming TEMPO geostationary instrument for North America. We use a radiative transfer model to examine how an increase in surface reflectivity due to snow cover changes the sensitivity of satellite retrievals to NO2 in the lower troposphere. We find that a substantial fraction (>50%) of the TEMPO field of regard can be snow covered in January, and that the average sensitivity to the tropospheric NO2 column substantially increases (doubles) when the surface is snow covered. We then evaluate seven existing satellite-derived or reanalysis snow extent products against ground station observations over North America to assess their capability of informing surface conditions for TEMPO retrievals. The Interactive Multisensor Snow and Ice Mapping System (IMS) had the best agreement with ground observations (accuracy of 93%, precision of 87%, recall of 83%). Multiangle Implementation of Atmospheric Correction (MAIAC) retrievals of MODIS-observed radiances had high precision (90% for Aqua and Terra), but underestimated the presence of snow (recall of 74% for Aqua, 75% for Terra). MAIAC generally outperforms the standard MODIS products (precision of 51%, recall of 43% for Aqua; precision of 69%, recall of 45% for Terra). The Near-real-time Ice and Snow Extent (NISE) product had good precision (83%) but missed a significant number of snow-covered pixels (recall of 45%). The Canadian Meteorological Centre (CMC) Daily Snow Depth Analysis Data set had strong performance metrics (accuracy of 91%, precision of 79%, recall of 82%). We use the F score, which balances precision and recall, to determine overall product performance (F = 85%, 82(82)%, 81%, 58%, 46(54)% for IMS, MAIAC Aqua(Terra), CMC, NISE, MODIS Aqua(Terra) respectively) for providing snow cover information for TEMPO retrievals from solar backscatter observations. We find that using IMS to identify snow cover and enable inclusion of snow-covered scenes in clear-sky conditions across North America in January can increase both the number of observations by a factor of 2.1 and the average sensitivity to the tropospheric NO2 column by a factor of 2.7.

A Decade of Change in NO2 and SO2 over the Canadian Oil Sands As Seen from Space.

A decade (2005-2014) of observations from the Ozone Monitoring Instrument (OMI) were used to examine trends in nitrogen dioxide (NO2) and sulfur dioxide (SO2) over a large region of western Canada and the northern United States, with a focus on the Canadian oil sands. In the oil sands, primarily over an area of intensive surface mining, NO2 tropospheric vertical column densities (VCDs) are seen to be increasing by as much as 10%/year, with the location of the largest trends in a newly developing NO2 "lobe" well removed from surface monitoring stations. SO2 VCDs in the oil sands have remained approximately constant. The only other significant increase in the region was seen in NO2 over Bakken gas fields in North Dakota which showed increases of up to 5%/yr. By contrast, other locations in the region show substantial declines in both pollutants, providing strong evidence to the efficacy of environmental pollution control measures implemented by both nations. The OMI-derived trends were found to be consistent with those from the Canadian surface monitoring network, although in the case of SO2, it was necessary to apply a correction in order to remove the residual signal from volcanic eruptions present in the OMI data.