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• W4368347599 abstract "Understanding the relaxation pathways of photoexcited molecules is essential to gain atomistic-level insight into photochemistry. We performed a time-resolved study of ultrafast molecular symmetry breaking through geometric relaxation (Jahn-Teller distortion) on the methane cation. Attosecond transient absorption spectroscopy with soft x-rays at the carbon K-edge revealed that the distortion occurred within 10 ± 2 femtoseconds after few-femtosecond strong-field ionization of methane. The distortion activated coherent oscillations in the asymmetric scissoring vibrational mode of the symmetry-broken cation, which were detected in the x-ray signal. These oscillations were damped within 58 ± 13 femtoseconds because vibrational coherence was lost with the energy redistributing into lower-frequency vibrational modes. This study completely reconstructs the molecular relaxation dynamics of this prototypical example and opens avenues for exploring complex systems." @default.
• W4368347599 created "2023-05-05" @default.
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• W4368347599 date "2023-05-19" @default.
• W4368347599 modified "2023-09-23" @default.
• W4368347599 title "Femtosecond symmetry breaking and coherent relaxation of methane cations via x-ray spectroscopy" @default.
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• W4368347599 doi "https://doi.org/10.1126/science.adg4421" @default.
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