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Communication: Photodissociation of CH3
CHO at 308 nm: Observation of H-roaming, CH3
-roaming, and transition state pathways together along the ground state surface
4.K. L. K. Lee, M. S. Quinn, A. T. Maccarone, K. Nauta, P. L. Houston, S. A. Reid, M. J. T. Jordan, and S. H. Kable, Chem. Sci. 5, 4633 (2014), and references therein.
5.B. R. Heazlewood, M. J. T. Jordan, S. H. Kable, T. M. Selby, D. L. Osborn, B. C. Shepler, B. J. Braams, and J. M. Bowman, Proc. Natl. Acad. Sci. U. S. A. 105, 12719 (2008).
7.L. Rubio-Lago, G. A. Amaral, A. Arregui, J. G. Izquierdo, F. Wang, D. Zaouris, T. N. Kitsopoulos, and L. Banares, Phys. Chem. Chem. Phys. 9, 6123 (2007).
15.G. de Wit, B. R. Heazlewood, M. S. Quinn, A. T. Maccarone, K. Nauta, S. A. Reid, M. J. T. Jordan, and S. H. Kable, Faraday Discuss. 157, 227 (2012).
20.B. R. Heazlewood, A. T. Maccarone, D. U. Andrews, D. L. Osborn, L. B. Harding, S. J. Klippenstein, M. J. T. Jordan, and S. H. Kable, Nat. Chem. 3, 443 (2001).
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Following photodissociation of acetaldehyde (CH3CHO) at 308 nm, the CO(v = 1–4) fragment is acquired using time-resolved Fourier-transform infrared emission spectroscopy. The CO(v = 1) rotational distribution shows a bimodal feature; the low- and high-J components result from H-roaming around CH3CO core and CH3-roaming around CHO radical, respectively, in consistency with a recent assignment by Kable and co-workers (Lee et al., Chem. Sci. 5, 4633 (2014)). The H-roaming pathway disappears at the CO(v ≥ 2) states, because of insufficient available energy following bond-breaking of H + CH3CO. By analyzing the CH4
emission spectrum, we obtained a bimodal vibrational distribution; the low-energy component is ascribed to the transition state (TS) pathway, consistent with prediction by quasiclassical trajectory calculations, while the high-energy component results from H- and CH3-roamings. A branching fraction of H-roaming/CH3-roaming/TS contribution is evaluated to be (8% ± 3%)/(68% ± 10%)/(25% ± 5%), in which the TS pathway was observed for the first time. The three pathways proceed concomitantly along the electronic ground state surface.
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