Phonon dynamics with collective spin excitations and orbital ordering in quasi-two-dimensional La1.4Sr1.6Mn2 O7

Abstract

This paper discusses the coupling between spin-wave-mediated magnetic interactions and lattice degrees of freedom in bilayer La1.4Sr1.6Mn2O7 (BL-LSMO-0.3). The thermal evolution of the Raman shift, as obtained from micro-Raman spectroscopic measurements over a wide temperature range, reveals the evolution of phonon dynamics while the system undergoes a balance between double and superexchange spin-spin interactions through spin-wave modulation in different magnetic phases. The evolution of relative magnetoelastic coupling strengths for nearest-neighbor ferromagnetic and next-nearest-neighbor antiferromagnetic superexchange interactions in the high-temperature canted antiferromagnetic phases are estimated. We have also demonstrated the existence of orbital ordering and its correlation with spin-phonon dynamics in the canted antiferromagnetic phases of BL-LSMO-0.3 from the detailed analysis of the high-wave-number orbiton-related phonon modes. Our study further reveals the absence of charge ordering in the compound. The complex coupling of lattice distortion, orbital ordering, the nearest- and next-nearest-neighbor spin-spin interactions in determining the canted spin states of the system is discussed. © 2025 American Physical Society.