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Abstract In response to global warming, ozone is predicted to increase aloft due to stratospheric cooling but decrease in the tropical lower stratosphere. The ozone reductions have been primarily attributed to a strengthening Brewer‐Dobson circulation, which upwells ozone‐poor air. Yet, this paper finds that strengthening upwelling only explains part of the reduction. The reduction is also driven by tropospheric expansion under global warming, which erodes the ozone layer from below, the low ozone anomalies from which are advected upwards. Strengthening upwelling and tropospheric expansion are correlated under global warming, making it challenging to disentangle their relative contributions. Therefore, chemistry‐climate model output is used to validate an idealized model of ozone photochemistry and transport with a tropopause lower boundary condition. In our idealized decomposition, strengthening upwelling and tropospheric expansion both contribute at leading order to reducing tropical ozone. Tropospheric expansion drives bottom‐heavy reductions in ozone, which decay in magnitude into the mid‐stratosphere.more » « less
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Match, Aaron; Gerber, Edwin P; Fueglistaler, Stephan (, Atmospheric Chemistry and Physics)The ozone layer is often noted to exhibit self-healing, whereby depletion of ozone aloft induces ozone increases below, explained as resulting from enhanced ozone production due to the associated increase in ultraviolet (UV) radiation below. Similarly, ozone enhancement aloft can reduce ozone below (reverse self-healing). This paper considers self-healing and reverse self-healing to manifest a general mechanism we call photochemical adjustment, whereby ozone perturbations lead to a downward cascade of anomalies in UV and ozone. Conventional explanations for self-healing imply that photochemical adjustment is stabilizing, damping perturbations towards the surface. However, photochemical adjustment can be destabilizing if the enhanced UV disproportionately increases the ozone sink, as can occur if the enhanced UV photolyzes ozone to produce atomic oxygen, which speeds up catalytic destruction of ozone. We analyze photochemical adjustment in two linear ozone models (Cariolle v2.9 and LINOZ), finding that (1) photochemical adjustment is destabilizing above 40 km in the tropical stratosphere and (2) self-healing often represents only a small fraction of the total photochemical stabilization. The destabilizing regime above 40 km is reproduced in a much simpler model: the Chapman cycle augmented with destruction of O and O3 by generalized catalytic cycles and transport (the Chapman+2 model). The Chapman+2 model reveals that photochemical destabilization occurs where the ozone sink is more sensitive than the source to perturbations in overhead column ozone, which is found to occur when the window of overlapping absorption by O2 and O3 is optically unsaturated, i.e., when overhead slant column ozone is below approximately 10^18 molec. cm−2.more » « less
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