José María Álvarez Rodríguez

Universidad Carlos III de Madrid

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Junhua Liu

Universities Space Research Association

Lu Hu

Children's Hospital of Zhejiang University

Zhu Xin

Southwest University

Sarah A. Strode

Morgan State University

Nathalie Rossat

European Southern Observatory

Daniel Brandt

Dalarna University

Michael J. Prather

University of California, Irvine

A. Dobrzycki

European Southern Observatory

Arlene M. Fiore

Lamont-Doherty Earth Observatory

Clare M. Flynn

Uppsala University

Cooperative Institutions

Goddard Space Flight Center

Harvard University Press

Harvard University

European Southern Observatory

Princeton University

National Oceanic and Atmospheric Administration

NSF National Center for Atmospheric Research

University of California, Irvine

Morgan State University

Universities Space Research Association

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Global Atmospheric Chemistry – Which Air Matters

Michael J. Prather Zhu Xin Clare M. Flynn Sarah A. Strode José María Álvarez Rodríguez

Abstract. 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, C2H3NO5, H2O, HOOH, CH3OOH, HCHO, CO, CH4, C2H6, 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 vertically. Six global models have prepared such climatologies (at model resolution) for August with emphasis on the vast central Pacific and Atlantic Ocean basins. We show clear 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 multi-dimensional probability densities of key species weighted by 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. 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 observed climatology is anticipated from the NASA Atmospheric Tomography (ATom) aircraft mission (2015–2020), measuring the key species, executing profiles over the Pacific and Atlantic Ocean basins. This work is a core part of the design of ATom.

Atmospheric chemistry

Tropospheric ozone

Atmospheric models

10.5194/acp-2016-1105

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Stratospheric impact on the Northern Hemisphere winter and spring ozone interannual variability in the troposphere

Junhua Liu José María Álvarez Rodríguez Luke D. Oman A. R. Douglass Mark A. Olsen

Abstract. In this study we use O3 and stratospheric O3 tracer simulations from the high-resolution Goddard Earth Observing System, Version 5 (GEOS-5) Replay run (MERRA-2 GMI at 0.5° model resolution ~ 50 km) and observations from ozonesondes to investigate the interannual variation and vertical extent of the stratospheric ozone impact on tropospheric ozone. Our work focuses on the winter and spring seasons over North America and Europe. The model reproduces the observed interannual variation of tropospheric O3, except for the Pinatubo period from 1991 to 1995 over the region of North America. Ozonesonde data show a negative ozone anomaly in 1992–1994 following the Pinatubo eruption, with recovery thereafter. The simulated anomaly is only half the magnitude of that observed. Our analysis suggests that the simulated Stratosphere-troposphere exchange (STE) flux deduced from the analysis might be too strong over the North American (50° N–70° N) region after the Mt. Pinatubo eruption in the early 1990s, masking the impact of lower stratospheric O3 concentration on tropospheric O3. European ozonesonde measurements show a similar but weaker O3 depletion after the Mt. Pinatubo eruption, which is fully reproduced by the model. Analysis based on a stratospheric O3 tracer (StratO3) identifies differences in strength and vertical extent of stratospheric ozone influence on the tropospheric ozone interannual variation (IAV) between North America and Europe. Over North America, the StratO3 IAV has a significant impact on tropospheric O3 from the upper to lower troposphere and explains about 60 % and 66 % of simulated O3 IAV at 400 hPa, ~ 11 % and 34 % at 700 hPa in winter and spring respectively. Over Europe, the influence is limited to the middle to upper troposphere, and becomes much smaller at 700 hPa. The stronger and deeper stratospheric contributions in the tropospheric O3 IAV over North America shown by the model is likely related to ozonesondes' being closer to the polar vortex in winter with lower geopotential height, lower tropopause height, and stronger coupling to the Arctic Oscillation in the lower troposphere (LT) than over Europe.

Anomaly (physics)

Tropospheric ozone

Ozone Depletion

10.5194/acp-2019-825

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Observations Metadata Database at the European Southern Observatory

A. Dobrzycki Daniel Brandt David Giot J. Lockhart José María Álvarez Rodríguez

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