Magnons and Magnetodielectric Effects in CoCr$_2$O$_4$: Raman Scattering Studies

Abstract: Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper reports an inelastic light scattering study of the magnon and phonon spectrum of CoCr$_2$O$_4$ as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature ($T_C \sim 94$ K) of CoCr$_2$O$_4$ we observe a $\omega \sim 16 \,\text{cm}^{-1}$ $\boldsymbol q=0$ magnon having T${1g}$-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T${1g}$-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr$_2$O$_4$. The Raman susceptibility of the T${1g}$-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr$2$O$_4$, suggesting that magnetodielectric behavior in CoCr$_2$O$_4$ primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr$_2$O$_4$ with applied pressure decreases the magnetic field-dependence of the T${1g}$-symmetry magnon Raman susceptibility in CoCr$_2$O$_4$, suggesting that strain can be used to control the magnetodielectric response in CoCr$_2$O$_4$.