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Enhancement of giant magnetoelectric effect in Ni-doped CaBaCo$_{4}$O$_{7}$

The polar magnet CaBaCo$_{4}$O$_{7}$ is known to exhibit the largest magnetic-field-driven electric polarization change ($ΔP$) associated with an antiferromagnetic (AFM)-ferrimagnetic (FIM) transition in a narrow temperature range between 62 and 69 K. In this work, we investigate the effect of Ni doping on its multiferroic properties, by means of magnetization, electric polarization, dielectric constant, and magnetostriction measurements on single crystals of CaBaCo$_{3.9}$Ni$_{0.1}$O$_{7}$ up to 50 T. In the doped material, two kinds of AFM phases appear below 78 K, accompanying negative $ΔP$. Upon the application of a magnetic field along any crystallographic axis, giant positive $ΔP$ of up to $11 \sim 12$ mC/m$^{2}$ is observed along with an AFM-FIM transition in the whole temperature range below 78 K. The giant magnetoelectric effect inherent in CaBaCo$_{4}$O$_{7}$ can be further enhanced just by a small amount of chemical substitution, in terms of (i) increasing the magnitude of $ΔP$ and (ii) expanding the temperature range in which giant $ΔP$ appears.