Decreases in stratospheric NOxassociated with enhanced aerosol have been observed after large volcanic eruptions, for example, after the eruption of Mount Pinatubo in 1991. While the 1991 Mount Pinatubo eruption was the last large explosive eruption, recent studies have shed light on the impacts of moderate‐sized eruptions since the year 2000 on the global stratospheric aerosol budget. We use an ensemble of simulations from a coupled climate‐chemistry model to quantify and analyze changes in NO and NO2(NOx), N2O5, HNO3, ClO, and ClONO2during periods of increased stratospheric volcanic aerosol concentrations since 2000. By using an ensemble approach, we are able to distinguish forced responses from internal variability. We also compare the model ensemble results to satellite measurements of these changes in atmospheric composition, including measurements from the Optical Spectrograph and Infrared Imaging Spectrometer on the Odin satellite and the Aura Microwave Limb Sounder. We find decreases in stratospheric NOxconcentrations up to 20 hPa, consistent with increases in stratospheric HNO3concentrations. The HNO3perturbations also extend higher, up to 5 hPa, associated with periods of increased volcanic aerosol concentrations in both model simulations and observations, though correlations with volcanic aerosol are considerably higher in the model simulations. The model simulates increases in ClO at altitudes and magnitudes similar to the NOxreductions, but this response is below the detectable limit in the available observations (100 pptv). We also demonstrate the value of accounting for transport‐related anomalies of atmospheric trace gases by regression onto N2O anomalies.
The inorganic chlorine (Cly) and odd nitrogen (NOy) chemical families influence stratospheric O3. In January 2020 Australian wildfires injected record‐breaking amounts of smoke into the southern stratosphere. Within 1–2 months ground‐based and satellite observations showed Clyand NOywere repartitioned. By May, lower stratospheric HCl columns declined by ∼30% and ClONO2columns increased by 40%–50%. The Clyperturbations began and ended near the equinoxes, increased poleward, and peaked at the winter solstice. NO2decreased from February to April, consistent with sulfate aerosol reactions, but returned to typical values by June ‐ months before the Clyrecovery. Transport tracers show that dynamics not chemistry explains most of the observed O3decrease after April, with no significant transport earlier. Simulations assuming wildfire smoke behaves identically to sulfate aerosols couldn't reproduce observed Clychanges, suggesting they have different composition and chemistry. This undermines our ability to predict ozone in a changing climate.
more » « less- PAR ID:
- 10370611
- Publisher / Repository:
- DOI PREFIX: 10.1029
- Date Published:
- Journal Name:
- Geophysical Research Letters
- Volume:
- 49
- Issue:
- 14
- ISSN:
- 0094-8276
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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