Impact of Fe-impurity centers on phonon subsystem of wurtzite-type ZnO

The paper addresses the question of the structural and vibrational properties of Fe-doped ZnO in the wurtzite structure with a lattice without an inversion center. The ZnO crystals containing Fe impurities in different charged states are studied by means of density functional theory (DFT) and potential-based methods. A first-principles simulation is performed to determine the local atomic configurations near the considered defects. The DFT results are compared with those obtained using the shell model. Both approaches give a similar pattern of lattice distortion around the Fe-impurity centers occupying cation sites in the isoelectronic charge state Fe^2＋ and single-positive-charge state Fe^3＋. The phonon local symmetrized densities of states projected onto the displacement of ions surrounding the defects are calculated by a well-established recursion method. The frequencies of defect vibrations of various symmetry types induced by Fe impurities are determined. The calculations made it possible to interpret the structure of the phonon sideband accompanying the zero-phonon line in polarized emission spectra attributed to the Fe^3＋ intracenter transitions, as well as to estimate the role of Fe ions in the formation of observed peaks.