Ba[(Zn_(1-x)Mg_x)_(1/3)Ta(2/3)]O_3(BZMT,x=0,0.2,0.4,0.6,0.8,and 1.0)solid solution ceramics were synthesized by a conventional solid-state sintering technique.Vibration spectra(Raman spectroscopy and Fourier trans form far-infrared reflection spectroscopy)and X-ray diffraction(XRD)were employed to evaluate the correla tion between microstructures and phonon modes of these solid solutions.Spectroscopic and structural data show sensitivity to structural evolution of samples with Mg^(2+)concentration,and a 1:2 ordered phase appears when x≥0.2.The unit cell parameters decrease with increasing Mg^(2+)content.The ordering degree reaches a relative maximum value in the range of Mg^(2+)content,0.4≤x<0.6.The phonon modes were assigned,and the correlation of phonon vibrations in the microstructure were analyzed.The position and width of the phonon modes were determined and correlated to the ionic radii for the different atoms substituted in the B'-site.