Spaceborne Observations of Lightning NO2 in the Arctic.

The Arctic region is experiencing notable warming as well as more lightning. Lightning is the dominant source of upper tropospheric nitrogen oxides (NOx), which are precursors for ozone and hydroxyl radicals. In this study, we combine the nitrogen dioxide (NO2) observations from the TROPOspheric Monitoring Instrument (TROPOMI) with Vaisala Global Lightning Dataset 360 to evaluate lightning NO2 (LNO2) production in the Arctic. By analyzing consecutive TROPOMI NO2 observations, we determine the lifetime and production efficiency of LNO2 during the summers of 2019-2021. Our results show that the LNO2 production efficiency over the ocean is ∼6 times higher than over continental regions. Additionally, we find that a higher LNO2 production efficiency is often correlated with lower lightning rates. The summertime lightning NOx emission in the Arctic (north of 70° N) is estimated to be 219 ± 116 Mg of N, which is equal to 5% of anthropogenic NOx emissions. However, for the span of a few hours, the Arctic LNO2 density can even be comparable to anthropogenic NO2 emissions in the region. These new findings suggest that LNO2 can play an important role in the upper-troposphere/lower-stratosphere atmospheric chemical processes in the Arctic, particularly during the summer.

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.

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.

Top-Down NOX Emissions of European Cities Based on the Downwind Plume of Modelled and Space-Borne Tropospheric NO2 Columns.

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April⁻September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R² = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R² = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.

The worldwide COVID-19 lockdown impacts on global secondary inorganic aerosols and radiative budget.

Global lockdown measures to prevent the spread of the coronavirus disease 2019 (COVID-19) led to air pollutant emission reductions. While the COVID-19 lockdown impacts on both trace gas and total particulate pollutants have been widely investigated, secondary aerosol formation from trace gases remains unclear. To that end, we quantify the COVID-19 lockdown impacts on NOx and SO2 emissions and sulfate-nitrate-ammonium aerosols using multiconstituent satellite data assimilation and model simulations. We find that anthropogenic emissions over major polluted regions were reduced by 19 to 25% for NOx and 14 to 20% for SO2 during April 2020. These emission reductions led to 8 to 21% decreases in sulfate and nitrate aerosols over highly polluted areas, corresponding to >34% of the observed aerosol optical depth declines and a global aerosol radiative forcing of +0.14 watts per square meter relative to business-as-usual scenario. These results point to the critical importance of secondary aerosol pollutants in quantifying climate impacts of future mitigation measures.

Global tropospheric ozone responses to reduced NO x emissions linked to the COVID-19 worldwide lockdowns.

Efforts to stem the transmission of coronavirus disease 2019 (COVID-19) led to rapid, global ancillary reductions in air pollutant emissions. Here, we quantify the impact on tropospheric ozone using a multiconstituent chemical data assimilation system. Anthropogenic NO x emissions dropped by at least 15% globally and 18 to 25% regionally in April and May 2020, which decreased free tropospheric ozone by up to 5 parts per billion, consistent with independent satellite observations. The global total tropospheric ozone burden declined by 6TgO3 (∼2%) in May and June 2020, largely due to emission reductions in Asia and the Americas that were amplified by regionally high ozone production efficiencies (up to 4 TgO3/TgN). Our results show that COVID-19 mitigation left a global atmospheric imprint that altered atmospheric oxidative capacity and climate radiative forcing, providing a test of the efficacy of NO x emissions controls for co-benefiting air quality and climate.

Abrupt decline in tropospheric nitrogen dioxide over China after the outbreak of COVID-19.

China's policy interventions to reduce the spread of the coronavirus disease 2019 have environmental and economic impacts. Tropospheric nitrogen dioxide indicates economic activities, as nitrogen dioxide is primarily emitted from fossil fuel consumption. Satellite measurements show a 48% drop in tropospheric nitrogen dioxide vertical column densities from the 20 days averaged before the 2020 Lunar New Year to the 20 days averaged after. This decline is 21 ± 5% larger than that from 2015 to 2019. We relate this reduction to two of the government's actions: the announcement of the first report in each province and the date of a province's lockdown. Both actions are associated with nearly the same magnitude of reductions. Our analysis offers insights into the unintended environmental and economic consequences through reduced economic activities.

Evaluating Sentinel-5P TROPOMI tropospheric NO2 column densities with airborne and Pandora spectrometers near New York City and Long Island Sound.

Airborne and ground-based Pandora spectrometer NO2 column measurements were collected during the 2018 Long Island Sound Tropospheric Ozone Study (LISTOS) in the New York City/Long Island Sound region, which coincided with early observations from the Sentinel-5P TROPOspheric Monitoring Instrument (TROPOMI) instrument. Both airborne- and ground-based measurements are used to evaluate the TROPOMI NO2 Tropospheric Vertical Column (TrVC) product v1.2 in this region, which has high spatial and temporal heterogeneity in NO2. First, airborne and Pandora TrVCs are compared to evaluate the uncertainty of the airborne TrVC and establish the spatial representativeness of the Pandora observations. The 171 coincidences between Pandora and airborne TrVCs are found to be highly correlated (r 2 =0.92 and slope of 1.03), with the largest individual differences being associated with high temporal and/or spatial variability. These reference measurements (Pandora and airborne) are complementary with respect to temporal coverage and spatial representativity. Pandora spectrometers can provide continuous long-term measurements but may lack areal representativity when operated in direct-sun mode. Airborne spectrometers are typically only deployed for short periods of time, but their observations are more spatially representative of the satellite measurements with the added capability of retrieving at subpixel resolutions of 250m×250m over the entire TROPOMI pixels they overfly. Thus, airborne data are more correlated with TROPOMI measurements (r 2 = 0.96) than Pandora measurements are with TROPOMI (r 2 = 0.84). The largest outliers between TROPOMI and the reference measurements appear to stem from too spatially coarse a priori surface reflectivity (0.5°) over bright urban scenes. In this work, this results during cloud-free scenes that, at times, are affected by errors in the TROPOMI cloud pressure retrieval impacting the calculation of tropospheric air mass factors. This factor causes a high bias in TROPOMI TrVCs of 4%-11%. Excluding these cloud-impacted points, TROPOMI has an overall low bias of 19%-33% during the LISTOS timeframe of June-September 2018. Part of this low bias is caused by coarse a priori profile input from the TM5-MP model; replacing these profiles with those from a 12 km North American Model-Community Multiscale Air Quality (NAMCMAQ) analysis results in a 12%-14% increase in the TrVCs. Even with this improvement, the TROPOMI-NAMCMAQ TrVCs have a 7%-19% low bias, indicating needed improvement in a priori assumptions in the air mass factor calculation. Future work should explore additional impacts of a priori inputs to further assess the remaining low biases in TROPOMI using these datasets.