The anharmonicity and lifetime of the CH stretching vibration of the H
-terminated diamond H/C(111)-(1 x 1) surface are investigated. It is f
ound that the nu1 --> 2 transition is 110 cm-1 lower than the nu0 -->
1 fundamental. Theoretical calculations show good agreement with the e
xperimental observations and predict the existence of a strongly bound
two-phonon bound state. A vibrational lifetime of 19 ps and a similar
ground-state recovery time are measured.