Abstract
Methanol is a benchmark for understanding tropospheric oxidation, but is underpredicted by up to 100% in atmospheric models. Recent work has suggested this discrepancy can be reconciled by the rapid reaction of hydroxyl and methylperoxy radicals with a methanol branching fraction of 30%. However, for fractions below 15%, methanol underprediction is exacerbated. Theoretical investigations of this reaction are challenging because of intersystem crossing (ISC) between singlet and triplet surfaces – ~45% of reaction products are obtained via intersystem crossing of a pre-product complex – which demands experimental determinations of product branching. Here we report the direct measurements of methanol from this reaction. A branching fraction below 15% is established, consequently highlighting a large gap in the understanding of global methanol sources. These results support the recent high-level theoretical work and substantially reduce its uncertainties.
Original language | English |
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Article number | 4343 |
Number of pages | 9 |
Journal | Nature Communications |
Volume | 9 |
DOIs | |
Publication status | Published - 19 Oct 2018 |
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Professor Dudley E Shallcross
- School of Chemistry - Professor of Atmospheric Chemistry
- Cabot Institute for the Environment
- Atmospheric Chemistry
Person: Academic , Member