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

Photoinduced quantum dynamics in molecules have hierarchical temporal structures with entangled electronic and nuclear motions. Femtosecond-to-attosecond transient absorption spectroscopy (TAS) using high-harmonic generation (HHG) in the extreme ultraviolet region with a photon energy below 100 eV has been a powerful method for observing such dynamics. However, complete measurements of the electronic, vibrational, and rotational molecular dynamics have not yet been achieved. Recent progress of attosecond HHG in the soft X-ray (SX) region around the water window (284-543 eV) has opened a new possibility of TAS with element specificity by using well-defined core electronic states. Here, we show that TAS in the SX region, around 400 eV, can probe multi-time-scale dynamics of the electronic, vibrational, and rotational degrees of freedom in a nitric oxide molecule at attosecond to sub-picosecond time scales, which provides a complete view of the phototriggered dynamics. This method of employing a photon-in/photon-out measurement using broadband attosecond SX pulses offers a unified approach to understand complete molecular dynamics with element specificity.