4.8 Article

Mapping hydroxyl variability throughout the global remote troposphere via synthesis of airborne and satellite formaldehyde observations

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.1821661116

Keywords

hydroxyl; formaldehyde; ATom; OMI; troposphere

Funding

  1. NASA ATom Earth Venture Suborbital-2 Program
  2. Atmospheric Composition Campaign Data Analysis and Modeling Grant [NNX14AP48G]
  3. NASA Upper Atmospheric Research Program
  4. NASA Tropospheric Composition Program
  5. NASA Postdoctoral Program at the NASA GSFC
  6. Atmospheric Composition Modeling and Analysis Grant [NNX17AH47G]
  7. Aura Science Team
  8. NSF Atmospheric and Geospace Sciences Postdoctoral Research Fellowship [1524860]
  9. Directorate For Geosciences
  10. Div Atmospheric & Geospace Sciences [1524860] Funding Source: National Science Foundation

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The hydroxyl radical (OH) fuels tropospheric ozone production and governs the lifetime of methane and many other gases. Existing methods to quantify global OH are limited to annual and global-to-hemispheric averages. Finer resolution is essential for isolating model deficiencies and building process-level understanding. In situ observations from the Atmospheric Tomography (ATom) mission demonstrate that remote tropospheric OH is tightly coupled to the production and loss of formaldehyde (HCHO), a major hydrocarbon oxidation product. Synthesis of this relationship with satellite-based HCHO retrievals and model-derived HCHO loss frequencies yields a map of total-column OH abundance throughout the remote troposphere (up to 70% of tropospheric mass) over the first two ATom missions (August 2016 and February 2017). This dataset offers unique insights on near-global oxidizing capacity. OH exhibits significant seasonality within individual hemispheres, but the domain mean concentration is nearly identical for both seasons (1.03 +/- 0.25 x 10(6) cm(-3)), and the biseasonal average North/South Hemisphere ratio is 0.89 +/- 0.06, consistent with a balance of OH sources and sinks across the remote troposphere. Regional phenomena are also highlighted, such as a 10-fold OH depression in the Tropical West Pacific and enhancements in the East Pacific and South Atlantic. This method is complementary to budget-based global OH constraints and can help elucidate the spatial and temporal variability of OH production and methane loss.

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