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.