Short-term variations in the oxidizing power of the atmosphere

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Abstract
The hydroxyl radical is the predominant atmospheric oxidant, responsible for removing a wide range of trace gases, including greenhouse gases, from the atmosphere. Determination of trends and variability in hydroxyl radical concentrations is critical to understanding whether the 'cleansing' properties of the atmosphere are changing. The variability in hydroxyl radical concentrations on annual to monthly timescales, however, is difficult to quantify. Here we show records of carbon monoxide containing radiocarbon (14CO), which is oxidized by hydroxyl radicals, from clean-air sites at Baring Head, New Zealand, and Scott Base, Antarctica, spanning 13 years. Using a model study, we correct for known variations in production of 14CO (refs 6, 7), allowing us to exploit this species as a diagnostic for short term changes in hydroxyl radical concentrations. We find no significant long-term trend in hydroxyl radical concentrations but provide evidence for recurring short-term variations of around ten per cent persisting for a few months. We also find decreases in hydroxyl radical concentrations of up to 20 per cent, apparently triggered by the eruption of Mt Pinatubo in 1991 and by the occurrence of extensive fires in Indonesia in 1997.