The Raman spectra of (CH3),NMnC13 (TMMC) and (CH3),NCdCI3 OMCC) single crystals have been studied at different pressures between 0 and 6 kbar and at temperatures ranging from 80 to 300 K. The P , T phase diagrams of TMMC and TMCC have been determined, and a generalized phase diagram for these systems is proposed. This diagram includes four different structural modificiations whose structures are discussed on the basis of the present Raman results and of previously published structural data. Phase 1 is hexagonal (P6,/m, Z = 2 space group) and exhibits orientational disorder of the (CH3)4Nf groups; phases 11,111 and IV are monoclinic and apparently ordered. Phase 111 (P2,/rn, Z = 2) exhibits a re-entrant character. The Raman spectra of phase I1 are consistent with the P2,/a, 2 = 4 space group induced by anti-phase translations of the octahedra chains, but do not reveal any feature that could be related to an incommensurability. It is concluded that the structure of phase IV is very complex (for instance P2,/rn, Z = 8 or P2,/a, Z = 12). The orderdisorder processes and their possible coupling with other lattice dynamic properties are considered, to explain the 10 I1 and l o 111 transitions; additional structural information is needed in order to choose between the different models examined.