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Sungyeon Choi

Publications and source records attributed to Sungyeon Choi.

High-Resolution Mapping of Nitrogen Oxide Emissions in Large US Cities From TROPOMI Retrievals of Tropospheric Nitrogen Dioxide Columns

Satellite-derived spatiotemporal patterns of nitrogen oxide (NO x ) emissions can improve accuracy of emission inventories to better support air quality and climate research and policy studies. In this study, we develop a new method by coupling the chemical transport Model-Independent SATellite-derived Emission estimation Algorithm for Mixed-sources (MISATEAM) with a divergence method to map high-resolution NO x emissions across US cities using TROPOspheric Monitoring Instrument (TROPOMI) tropospheric nitrogen dioxide (NO 2 ) retrievals. The accuracy of the coupled method is validated through application to synthetic NO 2 observations from the NASA-Unified Weather Research and Forecasting (NU-WRF) model, with a horizontal spatial resolution of 4 km × 4 km for 33 large and mid-size US cities. Validation reveals excellent agreement between inferred and NU-WRF-provided emission magnitudes (R= 0.99, normalized mean bias, NMB = −0.01) and a consistent spatial pattern when comparing emissions for individual grid cells (R=0.88 ± 0.06). We then develop a TROPOMI-based database reporting annual emissions for 39 US cities at a horizontal spatial resolution of 0.05° × 0.05° from 2018 to 2021. This database demonstrates a strong correlation (R= 0.90) with the National Emission Inventory (NEI) but reveals some bias (NMB = −0.24). There are noticeable differences in the spatial patterns of emissions in some cities. Our analysis suggests that uncertainties in TROPOMI-based emissions and potential misallocation of emissions and/or missing sources in bottom-up emission inventories both contribute to these differences.

NOx emissions↗

Revised estimates of NO 2 reductions during the COVID-19 lockdowns using updated TROPOMI NO 2 retrievals and model simulations

The TROPOspheric Monitoring Instrument (TROPOMI) observed unprecedented declines in NO 2 vertical column densities (VCD) over the world's most densely populated cities during the 2020 COVID-19 lockdowns. These favorable changes in NO 2 air quality were correlated with sharp reductions in traffic volume and economic activity during the lockdowns. In this comprehensive global study, we provide revised estimates of the declines in anthropogenic emissions for 36 megacities using a novel methodology for disentangling the anthropogenic emissions from the meteorological transport and natural variability. We further quantify the uncertainty associated with changes in the a priori profile shape information during the lockdowns due to reduced emissions. Satellite NO 2 retrieval techniques calculate an air mass factor that requires a priori NO 2 profile shape information representative of the local atmosphere. This information, which is typically obtained from a chemical transport model (CTM), was not available for the early studies. This study also accounts for the satellite sampling errors resulting from the selective sampling of non-cloudy scenes during the study period. For our analysis, we used CTM simulations that were generated with and without COVID-impacted emissions. We perform retrievals of tropospheric NO 2 columns with the NASA NO 2 algorithm, and then use observed and simulated data to disentangle the meteorological transport from the contribution due anthropogenic emissions. We found that the meteorological transport was most significant source of variability ranging between −35% and 22% of the change total tropospheric VCD. We also find that not accounting for changes in the a priori NO 2 profile shape information during the lockdowns resulted in systematic retrieval errors that were up to 12% of the estimated decline, and the elimination of cloud contaminated scenes resulted in sampling errors that in general ranged between varied ±15%.

NO2↗

Characterization of Errors in Satellite-Based HCHO/NO 2 Tropospheric Column Ratios With Respect to Chemistry, Column-to-PBL Translation, Spatial Representation, and Retrieval Uncertainties

The availability of formaldehyde (HCHO) (a proxy for volatile organic compound reactivity) and nitrogen dioxide (NO 2 ) (a proxy for nitrogen oxides) tropospheric columns from ultraviolet–visible (UV–Vis) satellites has motivated many to use their ratios to gain some insights into the near-surface ozone sensitivity. Strong emphasis has been placed on the challenges that come with transforming what is being observed in the tropospheric column to what is actually in the planetary boundary layer (PBL) and near the surface; however, little attention has been paid to other sources of error such as chemistry, spatial representation, and retrieval uncertainties. Here we leverage a wide spectrum of tools and data to quantify those errors carefully. Concerning the chemistry error, a well-characterized box model constrained by more than 500 h of aircraft data from NASA's air quality campaigns is used to simulate the ratio of the chemical loss of HO 2 + RO 2 (LRO x ) to the chemical loss of NO x (LNO x ). Subsequently, we challenge the predictive power of HCHO/NO 2 ratios (FNRs), which are commonly applied in current research, in detecting the underlying ozone regimes by comparing them to LRO x /LNO x . FNRs show a strongly linear (R 2 =0.94) relationship with LRO x /LNO x , but only on the logarithmic scale. Following the baseline (i.e., ln(LRO x /LNO x ) = −1.0 ± 0.2) with the model and mechanism (CB06, r2) used for segregating NO x -sensitive from VOC-sensitive regimes, we observe a broad range of FNR thresholds ranging from 1 to 4. The transitioning ratios strictly follow a Gaussian distribution with a mean and standard deviation of 1.8 and 0.4, respectively. This implies that the FNR has an inherent 20 % standard error (1σ) resulting from not accurately describing the RO x –HO x cycle. We calculate high ozone production rates (PO 3 ) dominated by large HCHO × NO 2 concentration levels, a new proxy for the abundance of ozone precursors. The relationship between PO 3 and HCHO × NO 2 becomes more pronounced when moving towards NO x -sensitive regions due to nonlinear chemistry; our results indicate that there is fruitful information in the HCHO × NO 2 metric that has not been utilized in ozone studies. The vast amount of vertical information on HCHO and NO 2 concentrations from the air quality campaigns enables us to parameterize the vertical shapes of FNRs using a second-order rational function permitting an analytical solution for an altitude adjustment factor to partition the tropospheric columns into the PBL region. We propose a mathematical solution to the spatial representation error based on modeling isotropic semivariograms. Based on summertime-averaged data, the Ozone Monitoring Instrument (OMI) loses 12 % of its spatial information at its native resolution with respect to a high-resolution sensor like the TROPOspheric Monitoring Instrument (TROPOMI) (> 5.5 × 3.5 km 2 ). A pixel with a grid size of 216 km 2 fails at capturing ∼ 65 % of the spatial information in FNRs at a 50 km length scale comparable to the size of a large urban center (e.g., Los Angeles). We ultimately leverage a large suite of in situ and ground-based remote sensing measurements to draw the error distributions of daily TROPOMI and OMI tropospheric NO 2 and HCHO columns. At a 68 % confidence interval (1σ), errors pertaining to daily TROPOMI observations, either HCHO or tropospheric NO 2 columns, should be above 1.2–1.5 × 10 16 molec. cm −2 to attain a 20 %–30 % standard error in the ratio. This level of error is almost non-achievable with the OMI given its large error in HCHO. The satellite column retrieval error is the largest contributor to the total error (40 %–90 %) in the FNRs. Due to a stronger signal in cities, the total relative error (< 50 %) tends to be mild, whereas areas with low vegetation and anthropogenic sources (e.g., the Rocky Mountains) are markedly uncertain (> 100 %). Our study suggests that continuing development in the retrieval algorithm and sensor design and calibration is essential to be able to advance the application of FNRs beyond a qualitative metric.

Amir H. Souri↗

Evaluation of the Stratospheric and Tropospheric Bromine Burden over Fairbanks, Alaska Based on Column Retrievals of Bromine Monoxide

In spring 2011, columns of bromine monoxide (BrO) were retrieved over Fairbanks, Alaska using a ground-based multifunction differential optical absorption spectroscopy (MFDOAS) instrument. MFDOAS vertical column BrO is consistently lower than retrievals from the satellite-based Ozone Monitoring Instrument (OMI), with a relative bias of 20 ± 14%. Numerous tropical-based studies suggest that 5 ± 2 ppt of bromine from very short-lived substances (VSLS) reaches the stratosphere. We evaluate upper limits on the contribution of VSLS to stratospheric bromine by treating the column retrievals of BrO as purely stratospheric and modeling the ratio of BrO to total inorganic bromine. The OMI and MFDOAS retrievals respectively present 8 and 5 ppt upper limits on the stratospheric injection of VSLS, and kinetic uncertainties in the daytime partitioning of bromine species decrease both values by ~1.6 ppt. The OMI-based estimate is in agreement with the 5 ppt tropical-based value for stratospheric injection of VSLS if the tropospheric column of BrO is 1.5 × 10(exp 13) molecules/cu. cm over Fairbanks, which is within the range of uncertainty of a second ground-based instrument that monitored tropospheric BrO during the campaign. Because our ground-based instruments detected no BrO near the surface, this value for tropospheric BrO would originate from the free troposphere and is in agreement with previous retrievals of background tropospheric BrO. Our calculations of tropospheric BrO over Fairbanks are most sensitive to uncertainties in the stratospheric loading of VSLS, followed by the difference between the OMI and MFDOAS retrievals of BrO.

Pamela A. Wales↗

Assessment of NO2 Observations During DISCOVER-AQ and KORUS-AQ Field Campaigns

NASA’s Deriving Information on Surface Conditions from Column and Vertically Resolved Observations Relevant to Air Quality (DISCOVER-AQ, conducted in 2011–2014) campaign in the United States and the joint NASA and National Institute of Environmental Research (NIER) Korea–United States Air Quality Study (KORUS-AQ, conducted in 2016) in South Korea were two field study programs that provided comprehensive, integrated data sets of airborne and surface observations of atmospheric constituents, including nitrogen dioxide (NO2), with the goal of improving the interpretation of spaceborne remote sensing data. Various types of NO2 measurements were made, including in situ concentrations and column amounts of NO2 using ground- and aircraft-based instruments, while NO2 column amounts were being derived from the Ozone Monitoring Instrument (OMI) on the Aura satellite. This study takes advantage of these unique datasets by first evaluating in situ data taken from two different instruments on the same aircraft platform, comparing coincidently sampled profile-integrated columns from aircraft spirals with remotely sensed column observations from ground-based Pandora spectrometers, intercomparing column observations from the ground (Pandora), aircraft (in situ vertical spirals), and space (OMI), and evaluating NO2 simulations from coarse Global Modeling Initiative (GMI) and high-resolution regional models. We then use these data to interpret observed discrepancies due to differences in sampling and deficiencies in the data reduction process. Finally, we assess satellite retrieval sensitivity to observed and modeled a priori NO2 profiles. Contemporaneous measurements from two aircraft instruments that likely sample similar air masses generally agree very well but are also found to differ in integrated columns by up to 31.9 %. These show even larger differences with Pandora, reaching up to 53.9 %, potentially due to a combination of strong gradients in NO2 fields that could be missed by aircraft spirals and errors in the Pandora retrievals. OMI NO2 values are about a actor of 2 lower in these highly polluted environments due in part to inaccurate retrieval assumptions (e.g., a priori pro-files) but mostly to OMI’s large footprint (>312 km2).

Nitrogen dioxide↗

Decoupling the Effects of Anthropogenic Emission Reductions from the Meteorology and Natural Emissions in TROPOMI NO 2 Retrievals During the 2020 COVID-19 Lockdowns

Satellite measurements during the COVID-19 lockdowns that began in 2020 revealed unprecedented reductions in NO 2 tropospheric vertical column densities (VCD). These reductions have largely been attributed to reduced anthropogenic emissions associated with abrupt decreases in road traffic and other power consuming business activities. Although decreased emissions tended to be the main contributor to the observed NO 2 VCD reduction, meteorological variability also played a role. Whereas the observed VCD changes were predominantly negative in places where public health policies were strictly enforced, meteorology had both positive and negative effects over short time intervals. Here, we present results from a global study of the NO 2 reductions aimed at disentangling the meteorological and natural emission variability from the anthropogenic emissions over the world’s most populated megacities. For this study, NASA’s TROPOMI NO 2 algorithm was used in conjunction with the Global Modeling Initiative (GMI) chemical transport model to separate the contributions due emissions and meteorology. A priori NO 2 profiles were generated from two GMI simulations performed for 2020 at a resolution of 0.25° longitude x 0.25° latitude. The first simulation used updated, COVID-impacted NOX emissions based on Forster et al. (2020), while the second simulation used the 2019 emissions with the 2020 meteorology, referred to here as 2020BAU. The 2020BAU data set allowed for the decoupling of the emission component from the meteorology. When compared to the same period in 2019, NO 2 column amounts during the lockdowns were reduced in 35 out of 36 cities. While reduced emissions contributed most to the observed total change in NO 2 during the lockdowns, the effects of meteorology were significant, ranging between 40% (Chennai) and 15% (Beijing). In China, an increase in NO 2 levels due to meteorology were observed in five out of the seven cities considered in the study. Use of different a-priori NO 2 profiles from the two simulations in our TROPOMI retrievals allowed for a determination of retrieval errors that ranged from -1.7% to -11.0%. We used the quality assurance flag > 0.75 to select the highest quality scenes in the study period. Using the GMI, we estimated the sampling biases to be in the range -11% to 10% of the total change for the cities in our study.

Brad Fisher↗

Verification of TROPOMI NO2 Product Using OMI NO2 algorithm

We evaluated S5P TROPOspheric Monitoring Instrument (TROPOMI) operational nitrogen dioxide (NO2) product by comparing with the NO2 retrievals from Ozone Monitoring Instrument (OMI) onboard NASA’s Aura satellite. We compared spatially matched NO2 vertical column density (VCD) data from OMI and TROPOMI to identify any discrepancies between the two operational products. We also applied OMI Air-Mass Factor (AMF) algorithm to TROPOMI Slant Column Density (SCD) data (v02.03.01) aiming to create long-term merged NO2 Earth Science Data Record (https://disc.gsfc.nasa.gov/datasets/TROPOMI_MINDS_NO2_1.1/summary ). The algorithm (version 4.0) uses new Geometry-dependent Lambertian Equivalent surface Reflectivity (GLER) product available for each TROPOMI pixel. GLER is pre-calculated using the vector linearized discrete ordinate radiative transfer (VLIDORT) model, which uses as input high-resolution bidirectional reflectance distribution function (BRDF) information from NASA's Aqua Moderate Resolution Imaging Spectroradiometer (MODIS) over land and the wind-dependent Cox–Munk wave-facet slope distribution over water, the latter with a contribution from the water-leaving radiance based on MODIS gap-filled in-water chlorophyll-a data. The GLER data, combined with consistently retrieved cloud parameters, provide improved information for the calculation of the scattering weight profiles. Additional AMF improvements result from using high resolution (0.25o latitude x 0.25o longitude) a priori NO2 profile shapes and other auxiliary information from the Global Modeling Initiative (GMI) Replay simulation sampled using S5P orbital simulator. Our TROPOMI_MINDS_NO2 algorithm employs the stratosphere-troposphere separation scheme, de-striping, and surface snow/ice treatment consistently with the latest OMI NO2 re-processing (version 4). We evaluate the TROPOMI_MINDS_NO2 product by comparing with the S5P operational NO2 product as well as with independent NO2 observations from ground-based Pandora and aircraft observations. Our results indicate that the new TROPOMI_MINDS_NO2 retrievals are generally higher than the S5P operational NO2 product over polluted regions and show improved agreement with independent validation data.

TROPOMI↗

Comparing Satellite Measurements of Volcanic SO2 Mass from OMI, OMPS and TROPOMI

Sulfur dioxide (SO2) is a major air pollutant that contributes to acid rain and aerosol formation (e.g., sulfates), adversely affects the environment and human health, and explosive volcanic SO2 emissions can impact climate. The majority of SO2 emissions are related to anthropogenic processes (e.g., fossil fuel burning, metal ore smelting operations), although natural processes such as volcanic eruptions and degassing also play an important role as anthropogenic SO2 emissions continue to decline. Generally, the most interest in volcanoes occurs during major eruptions. We will focus on comparing volcanic SO2 outgassing that occurs on an almost daily basis from lesser known volcanoes using satellite data. At NASA’s Global Sulfur Dioxide Monitoring Home page (https://so2.gsfc.nasa.gov/), we have been posting daily SO2 maps from 40 volcanic and industrial regions around the world using measurements from three satellite instruments; the Ozone Monitoring Instrument (OMI) onboard NASA’s Earth Observing System Aura satellite, the Ozone Monitoring and Profiler Suite (OMPS) onboard the NASA-NOAA Suomi National Polar-orbiting Partnership (NPP) satellite, and the TROPOspheric Monitoring Instrument (TROPOMI) onboard the ESA/Copernicus Sentinel-5 Precursor satellite. These instruments in low Earth sun-synchronous polar orbits with 1:30-2:00 pm equator crossing local time provide daily SO2 maps at different spatial resolutions: 13 x 24 km2, 50 x 50 km2 and 5.5 x 3.5 km2 for OMI, OMPS and TROPOMI respectively. Data from OMI are available since October 2004 (partial coverage since 2008), from OMPS since 2012 and from TROPOMI since 2018. We will present comparative SO2 mass time-series (see Hunga-Tonga plot) and statistical analyses of recent eruptions that have data from all the instruments.

SO2↗

Has NO(2) in Metropolitan Areas Returned to Pre-COVID-19 Levels as Measured by OMI Satellite Data?

Nitrogen oxides (NOx = NO + NO2) are primarily emitted through the combustion of fossil fuels, such as automobiles and power plants. NOx can contribute to chemical reactions that produce ozone and fine particulate matter (PM2.5) pollution. Using tropospheric vertical column density (TVCD) NO2 data from satellite hyperspectral instruments, such as the Ozone Monitoring Instrument (OMI) on board NASA’s EOS Aura satellite, one can monitor changes in NO2 pollution during “black-swan” events, such as mobility restrictions during COVID-19 lockdowns. Our OMI team has created the Global Nitrogen Dioxide Monitoring Home Page (https://so2.gsfc.nasa.gov/no2/no2_index.html ) where we display NO2 TVCD time series, animated maps, and COVID-specific NO2 anomalies comparing to a pre-COVID five-year average for 317 cities and regions around the world. During the pandemic as a result of the widespread lockdowns, many areas saw low NO2 anomalies superimposed on the natural weather related NO2 changes, such as seasonal NO2 cycle. Has NO2 levels returned to pre-Covid-19 levels in large metropolitan areas? We analyze NO2 time series from March through September for the years 2020-2023 using as a reference the average NO2 from 2015-2019 for those months. We will present data from selected cities that represent all countries.

Keith D Evans↗