Ground State of BaFe2S3 from Lattice and Spin Dynamics

Abstract

We investigate the interplay between lattice symmetry, phonons, and magnetism in the quasi-one-dimensional ladder compound BaFe$_2$S$_3$ by combining polarized synchrotron infrared spectroscopy, hybrid-functional density functional theory calculations, and inelastic neutron scattering. Lattice-dynamics analysis reveals that the crystal symmetry is lower than previously proposed and is consistent with a $P1$ space group at low temperature. Several infrared-active phonon modes exhibit pronounced anomalies at both the structural transition temperature $T_S \approx 125$--$130$~K and the Néel temperature $T_N \approx 95$~K. First-principles calculations show that the modes affected at $T_S$ predominantly involve displacements that modulate magnetic exchange pathways. Neutron scattering demonstrates that below $T_N$ the magnetic order is three-dimensional, long-ranged, and static. Between $T_N$ and $T_S$, the system displays three-dimensional short-range dynamic magnetic correlations, which disappear above $T_S$. The structural transition thus coincides with the onset of magnetic fluctuations rather than with static magnetic order. Our results indicate that short-range, dynamical magnetic correlations are sufficient to drive a static structural instability, providing a magnetically driven mechanism reminiscent of the iron-pnictide 122 family, yet realized here in a quasi-one-dimensional Mott system. These findings highlight the central role of magnetoelastic coupling in iron-based superconductors beyond the itinerant regime.