Optical sum-frequency generation (SFG) is used to characterize CO stre
tching vibrations on Pt(111) and Pt(110) surfaces, Different adsorptio
n sites (terminal bridge and step sites) are identified in the SFG spe
ctra of CO on Pt(111), in good quantitative agreement with previous in
frared relation-absorption experiments on this system. For CO on Pt(11
0) we only observe CO molecules on terminal sites. The measured CO str
etching vibration frequencies on Pt(110), both for low and high covera
ges, are at variance with the results of previous infrared studies. Ou
r SFG results for CO on Pt(110) art confirmed by independent EELS meas
urements which, in addition, also reveal the frustrated rotational mod
e and the metal-CO vibration, The measured frequency of 2065 cm(-1) fo
r low CO coverage on Pt(110)-(1x2) is consistent with a previously pro
posed empirical relation between the frequency of an isolated adsorbed
CO molecule and the coordination number of the binding Pt surface ato
m.