Phonon spectra in the parent superconducting iron-tuned telluride Fe1+xTe from inelastic neutron scattering and ab initio calculations

We report inelastic neutron scattering measurements of phonon spectra in the parent superconductor iron-tuned chalcogenide $\mathrm{F}{\mathrm{e}}_{1+x}\mathrm{Te}$ for two different $x$ contents $(x\ensuremath{\le}0.11)$ using neutron time-of-flight technique. Thermal neutron spectroscopy allowed the collection of the low-temperature Stokes spectra over an extended $Q$ range at 2, 40, and 120 K, hence covering both the magnetic monoclinic and the paramagnetic tetragonal phases, whereas cold neutrons allowed the measurement of high-resolution anti-Stokes spectra at 140, 220, and 300 K, thus covering the tetragonal phase. Our results evidence a spin-phonon coupling behavior towards the observed noticeable temperature-dependent change of the Stokes spectra across the transition temperatures. On the other hand, the anti-Stokes spectra reveal a pronounced hardening of the low-energy, acoustic region of the phonon spectrum upon heating, indicating a strong anharmonicity and a subtle dependence of phonons on structural evolution within the tetragonal phase. Experimental results are accompanied by ab initio calculations of phonon spectra of the tetragonal stoichiometric phase for a comparison with the high-resolution anti-Stokes spectra. Calculations included different density functional methods. Spin polarization and van der Waals interaction were either considered or neglected, individually or concomitantly, in order to study their respective effect on lattice dynamics description. Our results suggest that including van der Waals interaction has only a slight effect on phonon dynamics; however, phonon spectra are better described when spin polarization is included in a cooperative way with van der Waals interactions.