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We report for the first time phonon properties of [(C3H7)4N][M(N(CN)2)3] with MMn, Co, Ni (TPrAM), and theoretical Density Functional Theory (DFT) data for isolated TPrA+ cation obtained using harmonic and anharmonic approximation. Manganese compound undergoes one structural temperature‐induced phase transition, whereas others exhibit multiple structural phase transitions in a broad temperature ranges...