MSi4P4 compounds (M = Fe, Ru, Os) were studied at 300 K by Raman and IR spe
ctroscopy. The low symmetry and the absence of a center of inversion were c
onfirmed. The low-wavenumber modes are downshifted after substitution of Ru
and Os for Fe, These modes were assigned to relative motions of octahedra
and tetrahedra (SiP4 or PSi4) units. The upshift of high-energy modes was r
elated to electronic transfer between the metal and the Si-P host lattice a
nd to steric effects due to the atomic size increase from Fe to Os. Copyrig
ht (C) 1999 John Wiley & Sons, Ltd.