Abstract
Firefly bioluminescence has attracted great attention for many years. Some details of the mechanism underlying firefly bioluminescence remain elusive. In this study the formation and decomposition reactions of firefly dioxetanone (DO) have been investigated in the gas phase and in a solvent model with an appropriate dielectric constant. Firefly DO is identified as a key intermediate. The formation of DO involves a stepwise reaction mechanism: first the formation of the four-membered ring on the singlet potential surface but not on the triplet and then the departure of the PO 4 CH 3 2 - group. For the decomposition of DO, two possible reaction paths are proposed, one of which is reported for the first time.
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