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Global atmospheric chemistry – which air matters

Prather, M., X. Zhu, C. M. Flynn, S. Strode, J. Rodriguez, S. Steenrod, J. Liu, J. Lamarque, A. M. Fiore, L. W. Horowitz, J. Mao, L. Murray, D. Shindell, and S. C. Wofsy (2017), Global atmospheric chemistry – which air matters, Atmos. Chem. Phys., 17, 9081-9102, doi:10.5194/acp-17-9081-2017.

An approach for analysis and modeling of global atmospheric chemistry is developed for application to measurements that provide a tropospheric climatology of those heterogeneously distributed, reactive species that control the loss of methane and the production and loss of ozone. We identify key species (e.g., O3 , NOx , HNO3 , HNO4 , C2 H3 NO5 , H2 O, HOOH, CH3 OOH, HCHO, CO, CH4 , C2 H6 , acetaldehyde, acetone) and presume that they can be measured simultaneously in air parcels on the scale of a few km horizontally and a few tenths of a km vertically. As a first step, six global models have prepared such climatologies sampled at the modeled resolution for August with emphasis on the vast central Pacific Ocean basin. Objectives of this paper are to identify and characterize differences in model-generated reactivities as well as species covariances that could readily be discriminated with an unbiased climatology. A primary tool is comparison of multidimensional probability densities of key species weighted by the mass of such parcels or frequency of occurrence as well as by the reactivity of the parcels with respect to methane and ozone. The reactivity-weighted probabilities tell us which parcels matter in this case, and this method shows skill in differentiating among the models’ chemistry. Testing 100 km scale models with 2 km measurements using these tools also addresses a core question about model resolution and whether fine-scale atmospheric structures matter to the overall ozone and methane budget. A new method enabling these six global chemistry–climate models to ingest an externally sourced climatology and then compute air parcel reactivity is demonstrated. Such an objective climatology containing these key species is anticipated from the NASA Atmospheric Tomography (ATom) aircraft mission (2015–2020), executing profiles over the Pacific and Atlantic Ocean basins. This modeling study addresses a core part of the design of ATom.

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Tropospheric Composition Program (TCP)