Atmospheric Chemistry and Physics Discussions, vol. 8 (2008) pp. 16381-16407
We have developed a new technique for estimating ozone mixing ratio inside deep convective clouds. The technique uses the concept of an optical centroid cloud pressure that is indicative of the photon path inside clouds. Radiative transfer calculations based on realistic cloud vertical structure as provided by CloudSat radar data show that because deep convective clouds are optically thin near the top, photons can penetrate significantly inside the cloud. This photon penetration coupled with in-cloud scattering produces optical centroid pressures that are hundreds of hPa inside the cloud. We use the measured column ozone and the optical centroid cloud pressure derived using the effects of rotational-Raman scattering to estimate O3 mixing ratio in the upper regions of deep convective clouds. The data are obtained from the Ozone Monitoring Instrument (OMI) aboard NASA's Aura satellite. Our results show that low O3 concentrations in these clouds are a common occurrence throughout much of the tropical Pacific. Ozonesonde measurements in the tropics following convective activity also show very low concentrations of O3 in the upper troposphere. These low amounts are attributed to vertical injection of ozone poor oceanic boundary layer air during convection into the upper troposphere followed by convective outflow. Over South America and Africa, O3 mixing ratio inside deep convective clouds often exceeds 50 ppbv which is comparable to mean background (cloud-free) concentrations. These areas contain higher amounts of ozone precursors due to biomass burning and lightning. Assuming that O3 is well mixed (i.e. constant mixing ratio with height) up to the tropopause, we can estimate the stratospheric column O3 over clouds. Stratospheric column ozone derived in this manner agrees well with that retrieved independently with the Aura Microwave Limb Sounder (MLS) instrument and thus provides a consistency check of our method.
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