Accurate determination of the anisotropy factors and the phase differences of Raman polarizabilities in some uniaxial crystals: the case of lithium niobate

The present study highlights self-consistently helpful improvements dedicated to overcoming the difficulty resulting from the fitting procedure of integrated Raman intensities recorded according to the rotation crystal method described earlier. To this end, the anisotropy factors of Raman polarizabilities and the corresponding relative phases are determined within the framework of the exact mathematical derivation of the phase factors. These are the relevant parameters of the Raman efficiency relations which are numerically difficult to obtain from the fitting of the integrated areas. The present theoretical approach is then applied to the modes of the A(1) and Ey symmetry species of the lithium niobate (LN) crystal point group. All the expressions of the Raman absolute intensities of the A(1) and Ey irreducible representations initially imply three parameters to be determined from the fitting computations. However, from the derived analytical expressions of the phase differences, the number of parameters involved in the fitting procedure is reduced from 3 to 2, thus improving the statistics of the numerical treatment.