Decoupling in the Vertical Shape of HCHO During a Sea Breeze Event: the Effect on Trace Gas Satellite Retrievals and Column-to-surface Translation

The effect of sea breeze circulation on stratification of the vertical formaldehyde (HCHO) concentration vertical profiles is explored using a regional atmospheric chemical transport model (CTM) for three synoptically stagnant days focused on the east coast of the U.S in June 2018. During this event, a significant thermal contrast between the Atlantic Ocean and the terrestrial regions (12-17 degrees C), observed by moderate resolution imaging spectroradiometer (MODIS) and well-captured by the WRF-CMAQ model (15-18 degrees C), is conducive to monsoon-like flow, perpendicular to the shorelines, carrying clean marine air masses over the land within a few hundreds of meters above the surface. In contrast, the westerly continental polluted air masses prevail in higher altitudes. These two conflicting flows result in atypical vertical shapes of HCHO concentrations increasing with altitude. This decoupling pattern is so pronounced that we observe total column HCHO negatively correlate with surface concentrations. Comparisons of an accredited global model, GEOS-CF, to surface wind measurements and MODIS skin temperature indicate its poor representation of the sea breeze timing and strength, resulting in GEOS-CF HCHO vertical shapes being drastically different from the WRF-CMAQ. Based on radiative transfer calculations, the differences in the vertical distribution of HCHO between the WRF-CMAQ and that of GEOS-CF in the first 3 km are sufficient to induce a 20-30% error in air mass factors (thus total vertical HCHO column abundances). Through an experiment involving converting HCHO total columns to surface mixing ratios, we demonstrate that GEOS-CF allocates noticeably more HCHO molecules (40-150%) to the surface layer due to the misrepresentation of the vertical shape of HCHO during the sea breeze event. It is known that a significant fraction of the human population lives in coastal areas prone to detrimental effects caused by air pollution, and elevated pollutant concentrations usually occur in synoptically stagnant atmospheric conditions when local circulation patterns come into play; accordingly, our experiments emphasize the importance of the effect a priori profiles can have on satellite-derived applications under such conditions. To ensure that the quantitative representation of satellite-based trace gas retrievals on a daily basis is trustworthy and useable for air quality applications, atmospheric models providing a priori profiles for satellite retrievals should be welltuned to reproduce complex local circulation such as sea-land breezes.