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Understanding the relaxation pathways of photoexcited molecules is essentialto gain atomistic level insight into photochemistry. Herein, we perform atime-resolved study of ultrafast molecular symmetry breaking via geometricrelaxation (Jahn-Teller distortion) on the methane cation. Attosecond transientabsorption spectroscopy with soft X-rays at the carbon K-edge reveals that thedistortion occurs within $10\pm 2$ femtoseconds after few-femtosecondstrong-field ionization of methane. The distortion activates coherentoscillations in the scissoring vibrational mode of the symmetry broken cation,which are detected in the X-ray signal. These oscillations are damped within$58\pm13$ femtoseconds, as vibrational coherence is lost with the energyredistributing into lower-frequency vibrational modes. This study completelyreconstructs the molecular relaxation dynamics of this prototypical example andopens new avenues for exploring complex systems.

Femtosecond Symmetry Breaking and Coherent Relaxation of Methane Cations at the Carbon K-Edge