For He-3-CO and He-4-CO van der Waals bimers, fully resolved infrared
spectra in the 4.7 mu m region near the fundamental band origin of the
CO monomer have been measured for the first time. Only a small fracti
on of the observed lines could be assigned using conventional empirica
l spectroscopic techniques, and little additional insight was gained f
rom synthetic spectra generated from a published ab initio potential f
or this system. However, a complete set of unique assignments was made
on the basis of comparisons with synthetic spectra generated from a v
ariety of trial potential energy surfaces, and least-squares fits to t
he observed transition frequencies were used to determine a new anisot
ropic potential energy surface for this system. This new surface is mu
ch deeper and has a much stronger well depth anisotropy than the best
previous one, and its predictions of very low temperature microwave li
ne broadening cross sections raise serious questions regarding the met
hodology for calculating that property.