The complete Raman spectrum of crystalline octacarbonyldicobalt(0), Co
2(CO)8, has been successfully obtained for the first time by using a F
ourier transform instrument together with a spinning sample cell to av
oid decomposition of Co2(CO)8 upon exposure to the near-IR laser radia
tion used to excite the spectrum. Previously, only limited regions of
the Raman spectrum could be obtained with visible laser excitation bec
ause of extensive sample burning. The new FT-Raman results, combined w
ith the related IR data from the literature, provide a better descript
ion of the vibrational properties of this important binary metal carbo
nyl complex.