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Kelly Chance

Publications and source records attributed to Kelly Chance.

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↗

Revisiting the Effectiveness Of HCHO/NO2 Ratios for Inferring Ozone Sensitivity to Its Precursors Using High Resolution Airborne Remote Sensing Observations in A High Ozone Episode During the KORUS-AQ Campaign

The nonlinear chemical processes involved in ozone production (P(O3)) have necessitated using proxy indicators to convey information about the primary dependence of P(O3) on volatile organic compounds (VOCs) or nitrogen oxides (NOx). In particular, the ratio of remotely sensed columns of formaldehyde (HCHO) to nitrogen dioxide (NO2) has been widely used for studying O3 sensitivity. Previous studies found that the errors in retrievals and the incoherent relationship between the column and the near-surface concentrations are a barrier in applying the ratio in a robust way. In addition to these obstacles, we provide calculational-observational evidence, using an ensemble of 0-D photochemical box models constrained by DC-8 aircraft measurements on an ozone event during the Korea-United States Air Quality (KORUS-AQ) campaign over Seoul, to demonstrate the chemical feedback of NO2 on the formation of HCHO is a controlling factor for the transition line between NOx-sensitive and NOx-saturated regimes. A fixed value (~2.7) of the ratio of the chemical loss of NOx (LNOx) to the chemical loss of HO2+RO2 (LROx) perceptibly differentiates the regimes. Following this value, data points with a ratio of HCHO/NO2 less than 1 can be safely classified as NOx-saturated regime, whereas points with ratios between 1 and 4 fall into one or the other regime. We attribute this mainly to the HCHO-NO2 chemical relationship causing the transition line to occur at larger (smaller) HCHO/NO2 ratios in VOC-rich (VOC-poor) environments. We then redefine the transition line to LNOx/LROx~2.7 that accounts for the HCHO-NO2 chemical relationship leading to HCHO = 3.7 × (NO2 – 1.14 × 1016 molec.cm-2). Although the revised formula is locally calibrated (i.e., requires for readjustment for other regions), its mathematical format removes the need for having a wide range of thresholds used in HCHO/NO2 ratios that is a result of the chemical feedback. Therefore, to be able to properly take the chemical feedback into consideration, the use of HCHO = a × (NO2 – b) formula should be preferred to the ratio in future works. We then use the Geostationary Trace gas and Aerosol Sensor Optimization (GeoTASO) airborne instrument to study O3 sensitivity in Seoul. The unprecedented spatial (250 × 250 m2) and temporal (~every 2 h) resolutions of HCHO and NO2 observations form the sensor enhance our understanding of P(O3) in Seoul; rather than providing a crude label for the entire city, more in-depth variabilities in chemical regimes are observed that should be able to inform mitigation strategies correspondingly.

KORUS-AQ; formaldehyde; NOx; VOC; OMI; GeoTASO; oz↗

Explicit Aerosol Correction of OMI Formaldehyde Retrievals

Atmospheric aerosols are significant sources of uncertainty in air mass factor (AMF) calculations for trace gas retrievals using ultraviolet measurements from space. Current trace gas retrievals typically do not consider aerosols explicitly as cloud products partially account for aerosol effects. Here, we propose a new measurement-based approach to correct for aerosols explicitly in the AMF calculation, apply it to Ozone Monitoring Instrument (OMI) formaldehyde (HCHO) retrievals and quantify the aerosol-induced HCHO vertical column density difference for three aerosol types (smoke, dust, and sulfate) during 2006–2007. We use OMI aerosol retrievals for aerosol optical properties and vertical profiles to construct lookup tables of scattering weights as functions of geometry, surface pressure, surface albedo, and aerosol information. The average difference between the National Aeronautics and Space Administration operational OMI HCHO product (not considering aerosols) and the results obtained in this study on a global scale are 27%, 6%, and −0.3% for smoke, dust, and sulfate aerosols, respectively. The region with the largest aerosol effects is East China, where the explicit smoke aerosol correction enhances mean HCHO vertical column densities by 35%, with corrections to individual observations sometimes larger than 100%. The quantified aerosol effects are applicable under clear-sky conditions. This study highlights the need to implement aerosol corrections in the AMF calculation for HCHO retrievals. This is particularly relevant in regions with high levels of pollution where aerosols interfere the most with formaldehyde satellite observations.

Ozone Monitoring Instrument (OMI) formaldehyde (HC↗

Accelerating TEMPO Air Quality Science Through STAQS

Soon after the launch of Tropospheric Emissions: Monitoring of Pollution (TEMPO) mission, NASA is supporting the Synergistic TEMPO Air Quality Science field study (STAQS) in summer 2023. This study’s main objective is to accelerate science with geostationary air quality observations from TEMPO to better understand its use in air pollution research and applications. Science objectives include, but are not limited to, TEMPO L2 product evaluation, the interpretation of the spatiotemporal evolution of TEMPO data during air quality events, assessment of anthropogenic emissions, contributions to chemical transport modeling, and environmental justice applications. These objectives can be accomplished through the integration of satellite data with systematically repeated high-resolution aircraft- and ground-based measurements in multiple urban environments. The primary urban cities considered include Los Angeles, New York City, and Chicago in June-August 2023. Measurements consist of airborne remote sensing observations of air quality constituents of nitrogen dioxide (NO2), formaldehyde (HCHO), ozone, and aerosols using the GeoCape Airborne Simulator and High-Spectral Resolution Lidar 2/Differential Absorption Lidar (HSRL2/DIAL) on the NASA JSC G-V aircraft, greenhouse gas observations from Airborne Visible InfraRed Imaging Spectrometer - Next Generation (AVIRIS-NG) and High Altitude Lidar Observatory (HALO) on the NASA LaRC G-III aircraft, and ground-based remote sensing and in situ observations of ozone, NO2, and HCHO from the Tropospheric Ozone Lidar Network (TOLNet), Pandora spectrometers, and ground-based monitoring networks. Key partnership studies providing in situ airborne observations include the NOAA Atmospheric Emissions and Reactions Observed from Megacities to Marine Areas (AEROMMA) field study on the NASA DC-8 in the same primary target areas as STAQS and Greater New York Oxidant, Tropospheric Halogens, and Aerosol Measurements and Modeling (GOTHAMM) field study on the NSF C-130 near New York City. This presentation will include a current status update of the STAQS mission and an overview of its measurement strategies and science objectives with the goal of promoting continued discussions for building and strengthening collaborations prior to the mission.

Laura Judd↗

The NASA TEMPO Mission: Hourly Daytime Air Pollution Observations for Enhanced Health and Air Quality Applications

The Tropospheric Emissions: Monitoring of Pollution (TEMPO) mission was launched into Geostationary Earth Orbit (GEO) to 91°W longitude on April 7, 2023, and had a successful 3-day First Light period starting July 31 with TEMPO making its first hourly daytime scans across the TEMPO Field of Regard (FoR) covering greater North America on August 2. TEMPO will provide hourly daytime observations of aerosols and trace gases, including criteria pollutants of nitrogen dioxide (NO2), sulfur dioxide (SO2), and ozone (O3), at high spatial resolution (e.g., 2.0 x 4.75 km2) across the FoR. The hyperspectral ultraviolet-to-visible measurements from the TEMPO imaging grating spectrometer will enable an O3 profile product capable of monitoring the daytime diurnal evolution of O3 pollution in the planetary boundary layer and assessing related health impacts. The non-standard or special scan operations of TEMPO at sub-hourly frequency (e.g., 2-10 minutes) over selected slices of the FoR will further enhance air quality monitoring capabilities during disasters (e.g., wildfires, volcanic eruptions, dust storms, industrial accidents) and other episodic events for better understanding emission sources and the evolution of harmful air pollutants. A large diversity of stakeholders and end-users have been engaged in the TEMPO Early Adopters Program, supported by the NASA Applied Sciences Program, which aims to enhance health and air quality applications and maximize the societal benefit of TEMPO data. Key outcomes from the Early Adopters Program include enhanced knowledge and preparation for using TEMPO data, tailoring the data dissemination and visualization tools for TEMPO based on user needs, and broadening the health and air quality applications facet of the mission. This presentation will provide the latest TEMPO mission and Early Adopters Program updates, insight into the health and air quality applications enabled through TEMPO data, and showcase the First Light NO2 imagery and provisional data from the mission.

Remote Sensing↗

Upping the TEMPO on Air Pollution Observations from Space for Enhanced Science Applications

The Tropospheric Emissions: Monitoring of Pollution (TEMPO) mission was launched into Geostationary Earth Orbit (GEO) to 91°W longitude on April 7, 2023, and had a successful First Light period from July 31 – August 2 where the first hourly daytime scans across the TEMPO Field of Regard (FoR) covering greater North America were performed. First light images of nitrogen dioxide (NO2) were released to the public on August 24. In addition to NO2, TEMPO will provide hourly daytime observations of formaldehyde (HCHO), sulfur dioxide (SO2), ozone (O3), bromine (BrO), water vapor (H2O), and aerosols, at high spatial resolution (~2.0 x 4.75 km2) across the FoR. The hyperspectral ultraviolet-to-visible measurements from the TEMPO imaging grating spectrometer will permit an ozone profile retrieval capable of monitoring the diurnal evolution of ozone in the planetary boundary layer. The non-standard or special scan operations of TEMPO at sub-hourly frequency (e.g., 2-10 minutes) over selected slices of the FoR will further enhance monitoring capabilities during air quality disasters (e.g., wildfires, volcanic eruptions, dust storms, industrial accidents), research studies, and field campaign operations. A large diversity of stakeholders and end-users have been engaged in the TEMPO Early Adopters Program, supported by the NASA Applied Sciences Program, which aims to enhance health and air quality applications and maximize the societal benefit of TEMPO data when operational data becomes publicly available in the spring of 2024. Key outcomes from the Early Adopters Program include the pre-launch use of TEMPO proxy data to prepare the community for operational data, tailoring the data dissemination and visualization tools for the mission based on user needs, and enhancing the TEMPO special operations component of the mission through early adopter studies. This presentation will provide the latest TEMPO mission and Early Adopters Program updates, initiatives from the TEMPO special operations, and early demonstrations of science applications enabled through TEMPO data, while also showcasing the First Light imagery.

Air Quality↗

TEMPO Solar Calibration

Explore the source record for details and available documents.

Solar irradiance - ultra violet↗