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Methane, a key fossil fuel, is difficult to transport and difficult to convert to other energy rich chemicals because of the strong CH bond; however, several third-row metal cations readily activate methane to form MCH$_2^+$, a metal carbene, and H$_2$.
In a 2013 spectroscopic investigation using the FELICE intracavity free-electron laser, we have been able to identify product structures of methane activated by four metal cations [1]. The use of FELICE was deemed crucial, as it was suspected that dissociation via IVR-mediated multiple-photon excitation is hampered by a low IVR relaxation rate associated to a low density of states in these four atom species. Although the spectra obtained allowed for convincing product assignments, they also raised questions about unassigned spectral features, such as possible overtones and exceptionally broad band structures.
We recently re-visited this system employing perdeuterated methane CD$_4$ in an attempt to clarify several observations made. We here present the resulting spectra and a consistent spectral analysis.
[1] Lapoutre, V. J. F.; Redlich, B.; van der Meer, A. F. G.; Oomens, J.; Bakker, J. M.; Sweeney, A.; Mookherjee, A.; Armentrout, P. B. Structures of the Dehydrogenation Products of Methane Activation by 5d Transition Metal Cations. J. Phys. Chem. A 117 (20), 4115–4126 (2013).
