Influence of vapor transport equilibration on Raman spectra of Er:LiNbO3 crystals Original Research Article

Raman spectra of as-grown and vapor transport equilibration (VTE) treated Er:LiNbO3 crystals, which have different cut orientations (X-cut and Z-cut), different Er-doping levels (Er:(0.2, 0.4 and 2.0 mol%)LiNbO3) and different VTE durations (80, 120, 150 and 180 h), were recorded at room temperature in the wavenumber range 50–1000 cm−1 by using backward scattering geometry. The spectra were attributed on the basis of their spectral features and the previous experimental work and the most recent theoretical progress in lattice dynamics on pure LiNbO3. In comparison with the pure crystal the most remarkable effect of Er-doping on the Raman spectrum is observed for the E(TO9) mode. It does not appear at 610 cm−1 as the pure crystal, but locates at 633 cm−1. In addition, the doping also results in the lowering of the Raman phonon frequency, the broadening of the Raman linewidth and the changes of the relative Raman intensity of some peaks. The VTE treatment results in the narrowing of the linewidth, the recovery of the lowered phonon frequency and the further changes of relative Raman intensity. The narrowing of Raman linewidth indicates that the VTE processing has brought these crystals closer to stoichiometric composition. The VTE treatment has induced the formation of a precipitate ErNbO4 in the high-doped Er(2.0%):LiNbO3 crystals whether X- or Z-cut. For these precipitated crystals, besides above linewidth and phonon frequency features, they also display more significant Raman intensity changes compared with those not precipitated crystals. In addition, a slight mixing between A1(TO) and E(TO) spectra is also observed for these precipitated crystals. Above doping and VTE effects on Raman spectra were quantitatively or qualitatively correlated with the characteristics of the crystal structure and phonon vibrational system.