INFRARED and Raman spectroscopy have proved to be useful tools in research of the solid state, for instance as in studies of polymers (ELLIOTT, 1959), ice crystals (OcKMAN, 1958), or semi-conductors (FAN, 1956; HARRICK, 1960). The previous research experience of the authors of this article has been mainly in the field of organometallics, one which is believed to be potentially useful to the solid state chemist. Semiconductor-like crystals have already been produced from metal organic compounds such as the metal salts of tetracyanoquinodimethane (KEPLER, BIERSTEDT and MERRIFIELD, 1960), and further interchange between the field of solid state and organometallic chemistry is likely to become important. To the extent that infrared and Raman spectroscopy will be used to obtain fundamental understanding of solid state devices of this cross-breeding, knowledge of the spectroscopy of organometallics itself is a proper beginning. Inclusion of this article in the present series is hoped to bring solid state chemists into closer contact with the development of organometallics through a discussion of spectroscopic advances made in that field.