Terahertz Crystal-Field Transitions and Quasi Ferromagnetic Magnon Excitations in a Noncollinear Magnet for Hybrid Spin-Wave Computation

The complexity of interactions between the crystal-field and unusual noncollinear spin arrangement in nontrivial magnets demands novel tools to unravel the mystery underneath. In this work, we study such interaction dynamics of crystal-field excitations (CFE) and low-energy magnetic excitations in orthochromite TmCrO₃ with controls of temperature and magnetic field using high-resolution magneto-terahertz (THz) time-domain spectroscopy. The THz energy spectrum spanning 0.5-10 meV possesses a low-frequency spin-excitation (magnon) mode and a multitude of CFE modes at 10 K, all of which uniquely embody a range of phenomena. For the magnon mode, a temperature dependence of peak frequency is induced by magnetic interactions between Tm and Cr subsystems. While a change from blue to red shift of peak frequency of this mode marks the magnetization reversal transition, the spin-reorientation temperature and change of magnetic anisotropy are depicted by different features of field and temperature dependent peak frequency dynamics. The modes corresponding to CFE are robust and laden with a multitude of submodes, which are attributes of nontrivial interactions across different transitions. These modes are suppressed only upon substitution of Tb³⁺ at the Tm³⁺ site, which suggests a dominant role of single-ion anisotropy in controlling entire THz excitation spectra. Overall, this remarkable range of phenomena seen through the unique lens of all-optical THz tools provides deeper insights into the origin of magnetic phases in systems with complex interactions between rare-earth and transition metal ions and provides a multitude of novel combinations of closely spaced modes for emerging hybrid spin-wave computation.