Infrared and Raman spectra of 4-tert.-butylpyridine (4-bpy) are reported for the first time in the 4000-200 cm(-1) range. Vibrational assignments have been made for fundamental modes on the basis of frequency shifts of the coordinated ligand, and comparison with related molecules. The infrared and Raman spectra of M(4-tbpy)(2)Ni(CN)(4) (where M = Mn, Cd, Fe, Co or Ni; abbreviated to M-Ni-4-tbpy) complexes are reported for the first time. It is shown that the structure of these complexes consists of infinite polymeric layers of [M-Ni(CN)4], analogous to those of Hofmann-type complexes. 4-tbpy molecules bound directly to the metal (M). (C) 1997 Elsevier Science B.V. (C) 1997 Elsevier Science B.V.