Structural, magnetic, and spin dynamical properties of the polar antiferromagnets Ni3−xCoxTeO6(x=1,2)

We present results of a multimethod investigation of the polar antiferromagnets $\mathrm{N}{\mathrm{i}}_{2}\mathrm{CoTe}{\mathrm{O}}_{6}$ and $\mathrm{NiC}{\mathrm{o}}_{2}\mathrm{Te}{\mathrm{O}}_{6}$, inspired by the colossal magnetoelectric effect present in $\mathrm{N}{\mathrm{i}}_{3}\mathrm{Te}{\mathrm{O}}_{6}$. Both compounds crystalize in the same polar space group $R3$ as $\mathrm{N}{\mathrm{i}}_{3}\mathrm{Te}{\mathrm{O}}_{6}$, preserving the crystal symmetry at least from room temperature down to 2 K. $\mathrm{N}{\mathrm{i}}_{2}\mathrm{CoTe}{\mathrm{O}}_{6}$ and $\mathrm{NiC}{\mathrm{o}}_{2}\mathrm{Te}{\mathrm{O}}_{6}$ undergo antiferromagnetic phase transitions at ${T}_{\mathrm{N}}=55$ and 52 K, and spin-flop transitions at an external magnetic field of approximately 8 and 4 T, respectively. Both compounds present an incommensurate antiferromagnetic helical structure with spins lying in the $ab$ plane, in contrast to the collinear one along the $c$ axis in $\mathrm{N}{\mathrm{i}}_{3}\mathrm{Te}{\mathrm{O}}_{6}$. Moreover, dielectric anomalies are observed at their antiferromagnetic phase transitions, suggesting a magnetoelectric behavior. Spin and lattice dynamics studies by a combination of infrared, Raman, and terahertz spectroscopies were performed. Below ${T}_{\mathrm{N}}$, in both $\mathrm{N}{\mathrm{i}}_{2}\mathrm{CoTe}{\mathrm{O}}_{6}$ and $\mathrm{NiC}{\mathrm{o}}_{2}\mathrm{Te}{\mathrm{O}}_{6}$, low-frequency spin excitations extremely sensitive to external magnetic field were observed. At least one of these magnons was simultaneously seen in Raman and THz spectra of both compounds, therefore we propose to assign them to electromagnons.