Investigation of tropospheric bro using space-based total column bro measurements

• Main Author: Choi, Sungyeon
• Other Authors: Curry, Judith A., Joiner, Joanna, Huey, Greg, Nenes, Athanasios, Weber, Rodney, School of Earth and Atmospheric Sciences, College of Sciences, Earth and Atmospheric Sciences
• Format: Doctoral or Postdoctoral Thesis
• Language: unknown
• Published: Georgia Institute of Technology 2012
• Subjects: Chemistry; DOAS; Remote sensing; Arctic; Bromine; Troposphere; BrO; Tropospheric chemistry; Tropospheric aerosols; Bromine compounds; Halogens; albedo
• Online Access: http://hdl.handle.net/1853/43682

We derive tropospheric column BrO during the ARCTAS and ARCPAC field campaigns in spring 2008 using retrievals of total column BrO from the satellite UV nadir sensors OMI and GOME-2 using a radiative transfer model and stratospheric column BrO from a photochemical simulation. We conduct a comprehensive comparison of satellite-derived tropospheric BrO column to aircraft in-situ observations of BrO and related species. The aircraft profiles reveal that tropospheric BrO, when present during April 2008, was distributed over a broad range of altitudes rather than being confined to the planetary boundary layer (PBL). Perturbations to the total column resulting from tropospheric BrO are the same magnitude as perturbations due to longitudinal variations in the stratospheric component, so proper accounting of the stratospheric signal is essential for accurate determination of satellite-derived tropospheric BrO. We find reasonably good agreement between satellite-derived tropospheric BrO and columns found using aircraft in-situ BrO profiles, particularly when satellite radiances were obtained over bright surfaces (albedo >0.7), for solar zenith angle <80 degree and clear sky conditions. The rapid activation of BrO due to surface processes (the bromine explosion) is apparent in both the OMI and GOME-2 based tropospheric columns. The wide orbital swath of OMI allows examination of the evolution of tropospheric BrO on about hourly time intervals near the pole. Low surface pressure, strong wind, and high PBL height are associated with an observed BrO activation event, supporting the notion of bromine activation by high winds over snow. We also provide monthly climatological maps of free tropospheric BrO volume mixing ratio (VMR) derived using the so-called cloud slicing technique. In this approach, the derived slope of the total column BrO versus cloud pressure is proportional to free tropospheric BrO VMR. Estimated BrO VMR shows a minimum in the tropics and greater values at higher latitudes in both hemispheres. High ...