Abstract

The mechanisms of molecular vibrational energy relaxation at surfaces have received a great deal of theoretical attention, but surface vibrational relaxation measurements have been largely confined to high surface area materials,¹ which are difficult to characterize. Recently,² vibrational relaxation dynamics has been probed in monolayer Langmuir-Blodgett molecular films at bulk metal surfaces using picosecond infrared-visible sum frequency generation (SFG). In the present paper, the picosecond transient SFG technique is extended to molecular adsorbates at clean, well-characterized single crystal surfaces in an ultrahigh vacuum environment.

© 1990 Optical Society of America