REMOTE SENSING OF ATMOSPHERIC TRACE GASES FROM SPACEBORNE UV MEASUREMENTS

Abstract

Satellite measurements of atmospheric trace gases provide continuous long-term information for monitoring the atmospheric chemical environment and air quality at local, regional, and global scales. Trace gas retrievals play a critical role in chemical data assimilation, air quality modeling and forecast, and regulatory decision-making. In this dissertation, I present retrievals of three trace gases species (O3, SO2, and NO2) from measurements of Ultraviolet (UV) radiation made from the imaging spectrometers onboard operational satellites, including the Earth Polychromatic Imaging Camera (EPIC) onboard the Deep Space Climate Observatory (DSCOVR), the Ozone Mapping and Profiler Suite - Nadir Mapper (OMPS-NM) onboard Suomi-NPP (SNPP), and the OMPS-NM onboard NOAA-20 satellite. The retrievals of the trace gas vertical columns are achieved through the Direct Vertical Column Fitting (DVCF) algorithm, which is designed to maximize the absorption signature from the Earth’s atmosphere in the UV spectral range. This dissertation first demonstrates the theoretical basis and mathematical procedures of the DVCF algorithm used for retrieving total vertical columns of ozone (O3) and sulfur dioxide (SO2) from DSCOVR EPIC. We describe algorithm advances, including an improved O3 profile representation that enables profile adjustments from multiple spectral measurements and the spatial optimal estimation (SOE) scheme that reduces O3 artifacts resulted from EPIC’s band-to-band misregistrations. Furthermore, we present detailed error analyses to quantify retrieval uncertainties from various sources, assess EPIC-observed volcanic plumes, and validate O3 and SO2 retrievals with correlative data. The second part of this dissertation presents a suite of efforts to retrieve the tropospheric and stratospheric NO2 vertical columns from the new NOAA-20 OMPS hyperspectral Ultraviolet-Visible (UV-Vis) instrument, covering retrieval algorithm, Stratosphere-Troposphere Separation (STS) scheme, measurement sensitivity assessment, inter-comparison with the Ozone Monitoring Instrument (OMI), evaluation with ground-based Pandora spectrometers, as well as a case study of drastic NO2 changes during COVID-19 pandemic. The third part of my dissertation focuses on validation and algorithm improvements for the tropospheric NO2 retrievals from SNPP OMPS UV measurements. OMPS column NO2 was validated against coincidence measurements from two ground-based MAX-DOAS spectrometers deployed in eastern China. To achieve higher retrieval accuracy, we developed and implemented a series of algorithm improvements, including an explicit aerosol correction scheme to account for changes in measurement sensitivity caused by aerosol scattering and absorption, the replacement of climatological a priori NO2 profile with more accurate NO2 vertical distribution from high-resolution CMAQ model simulations, and the application of model-derived spatial weighting kernel to account for the effect of heterogeneous subpixel distribution. These improvements yield more accurate OMPS NO2 retrievals in better agreement with MAX-DOAS NO2 measurements. The analysis concluded that explicit aerosol correction and a priori profile adjustment are critical for improving satellite NO2 observations in highly polluted regions and spatial downscaling is helpful in resolving NO2 subpixel variations.