Interfacial Vibrational Dynamics of Ice I(h) and Liquid Water

[Image: see text] Insights into energy flow dynamics at ice surfaces are essential for understanding chemical dynamics relevant to atmospheric and geographical sciences. Here, employing ultrafast surface-specific spectroscopy, we report the interfacial vibrational dynamics of ice I(h). A comparison to liquid water surfaces reveals accelerated vibrational energy relaxation and dissipation at the ice surface for hydrogen-bonded OH groups. In contrast, free-OH groups sticking into the vapor phase exhibit substantially slower vibrational dynamics on ice. The acceleration and deceleration of vibrational dynamics of these different OH groups at the ice surface are attributed to enhanced intermolecular coupling and reduced rotational mobility, respectively. Our results highlight the unique properties of free-OH groups on ice, putatively linked to the high catalytic activities of ice surfaces.