The interplay of crystal-field transitions and exchange spin dynamics in a ferrimagnet

Abstract

Rare-earth iron garnets offer an ideal platform for exploring the interplay of low-energy excitations and the complex temperature-dependent magnetization dynamics. In these systems, exchange coupling between rare-earth and iron sublattices generates high-frequency collective spin excitations. In addition, the robust spin-orbit coupling of localized 4$f$ electrons triggers the crystal-electric-field (CEF) transitions at THz frequencies. Despite extensive research into the garnet spin dynamics, the interplay between CEF excitations and exchange modes has remained largely unmapped. Using temperature-dependent THz time-domain spectroscopy, we demonstrate a hybridization between the Yb-ion CEF excitation and the Yb-Fe exchange mode in Gd$_{3/2}$Yb$_{1/2}$BiFe$_{5}$O$_{12}$. This coupling is characterized by a significant redistribution of spectral and temporal weights as the material approaches its magnetization compensation temperature. Notably, the Yb-Fe exchange mode exhibits an anomalous redshift upon cooling -- a reversal of the conventional blue shift typically driven by increased exchange coupling. We trace this phenomenon to a modification of Yb-Fe exchange anisotropy, driven by the interplay of the Fe exchange field and Yb CEF excitations. These findings highlight the critical role of CEF-mediated exchange coupling in shaping low-energy spin dynamics, positioning rare-earth garnets as a cornerstone for future THz spintronic technologies.