Phonon Spectra in the Parent Superconducting Iron-tuned Telluride Fe$_{1+x}$Te from Inelastic Neutron Scattering and Ab Initio Calculations

TL;DR

This study combines inelastic neutron scattering and ab initio calculations to investigate phonon spectra in Fe$_{1+x}$Te, revealing spin-phonon coupling, anharmonic effects, and the importance of spin polarization in modeling lattice dynamics.

Contribution

It provides new insights into the temperature-dependent phonon behavior and the role of spin and van der Waals interactions in theoretical descriptions of Fe$_{1+x}$Te.

Findings

Temperature-dependent change in phonon spectra indicates spin-phonon coupling.

Phonon hardening with temperature suggests strong anharmonicity.

Including spin polarization improves theoretical phonon spectra accuracy.

Abstract

We report inelastic neutron scattering measurements of phonon spectra in the parent superconductor iron-tuned chalcogenide Fe$_{1+x}$Te, for two different x contents (x $\leq$ 0.11), using neutron time-of-flight technique. Thermal neutron spectroscopy allowed to collect the low-temperature Stokes spectra over an extended Q-range, at 2, 40 and 120K - hence covering both the magnetic monoclinic and the paramagnetic tetragonal phases. Whereas cold-neutrons allowed to measure high-resolution anti-Stokes spectra at 140, 220 and 300K, thus covering the tetragonal phase. Our results evidence a spin-phonon coupling behaviour 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.