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Photoinduced quantum dynamics in molecules have hierarchical temporalstructures with different energy scales that are associated with electron andnuclear motions. Femtosecond-to-attosecond transient absorption spectroscopy(TAS) using high-harmonic generation (HHG) with a photon energy below 300 eVhas been a powerful tool to observe such electron and nuclear dynamics in atable-top manner. However, comprehensive measurements of the electronic,vibrational, and rotational molecular dynamics have not yet been achieved.Here, we demonstrate HHG-based TAS at the nitrogen K-edge (400 eV) for thefirst time, and observe all the electronic, vibrational, and rotational degreesof freedom in a nitric oxide molecule at attosecond to sub-picosecond timescales. This method of employing core-to-valence transitions offers anall-optical approach to reveal complete molecular dynamics in photochemicalreactions with element and electronic state specificity.

Real-time observation of electronic, vibrational, and rotational dynamics in nitric oxide with attosecond soft X-ray pulses at 400 eV