12B.1 An expanded definition of the odd oxygen family for tropospheric ozone budgets: Implications for ozone lifetime, stratospheric influence, and source tagging (Invited Presentation)

Thursday, 16 January 2020: 8:30 AM
207 (Boston Convention and Exhibition Center)
Kelvin Bates, Harvard University, Cambridge, MA; and D. J. Jacob

Models of tropospheric ozone commonly define an ”odd oxygen” family (Ox), comprising ozone and species with which it rapidly cycles, in order to compute tropospheric ozone budgets and lifetimes. A major Ox loss is the O(1D) + H2O → 2OH reaction, but this may not be an actual loss because the resulting hydrogen oxide (HOx) radicals regenerate ozone in the presence of nitrogen oxides. We recently introduced an expanded odd oxygen family, Oy ≡ Ox + Oz, to include both the traditional Ox and an additional subfamily, Oz, consisting of HOx and its reservoirs. Here, we demonstrate the application of this expanded odd oxygen family in the computation of ozone budgets and in both source perturbation and ozone tagging simulations using GEOS-Chem, a global chemical transport model. We show that the Oy framework reveals a longer tropospheric mean lifetime of ozone (73 davs vs. 24 days) and greater stratospheric contribution (26% vs. 9%) than derived from the standard Ox budget. In perturbation experiments, changes in nitrogen oxide (NOx) emissions lead to changes in the efficiency of cycling between the Oy subfamilies, altering the balance between Ox and Oz, which in turn helps to explain the non-linearities inherent to the ozone budget. In tagging simulations, ozone can be tracked both by its primary sources and by the number of cycles it undergoes between Ox and Oz, revealing the spatial and temporal variability in tropospheric ozone lifetime, primary source influence, and cycling efficiency. Tracking the Oy budget may provide better understanding of the discrepancies between global models in their computations of ozone sources and sinks.
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