Vibrational energy relaxation of excited free OH stretching mode at the surface of ice: An ab initio molecular dynamics simulation study

The vibrational energy relaxation dynamics of the excited free OH bond on the ice surface are investigated using ab initio molecular dynamics (AIMD) simulations. The present AIMD study reproduces experimental results obtained via pump-probe sum-frequency generation spectroscopy. Simulations were conducted at 100 and 200 K for ice surfaces and compared with previous results at 300 K for water surfaces. The relaxation mechanisms were analyzed by selectively constraining specific vibrational modes,