Effective rectification of terahertz electromagnetic fields in a ferrimagnetic iron garnet

It is found that single-cycle THz electromagnetic fields efficiently excite a GHz spin resonance mode in ferrimagnetic ${\mathrm{Tm}}₃{\mathrm{Fe}}₅{\mathrm{O}}₁₂$, despite the near absence of GHz spectral components in the exciting THz pulse. By analyzing how the efficiency of excitation depends on the orientation and strength of the THz electric field, we show that it can be explained in terms of the nonlinear THz inverse Cotton-Mouton effect. Here, the THz electric field gets effectively rectified and acts on the ferrimagnetic spins as a unipolar effective magnetic field pulse. This interpretation is confirmed by a theoretical model based on the phenomenological analysis of the effective magnetic field, combined with the equations of motion derived from the effective Lagrangian for a ferrimagnet. Moreover, by using the outcome of two-dimensional THz spectroscopy, we conjecture a quantum-mechanical interpretation of the observed effect in terms of impulsive stimulated Raman scattering of THz photons by the crystal-field split $f\text{\ensuremath{-}}f$ electronic transitions of ${\mathrm{Tm}}³⁺$.