Exploring Multiferroic Behavior in CaZnFeOsO$_6$: A Novel Layered 3$d$-5$d$ Double Perovskite Compound

Abstract: We present a novel multiferroic double perovskite compound, CaZnFeOsO$_6$ (CZFOO), exhibiting combined ferroelectric and ferrimagnetic properties. Through ab initio density functional theory calculations, we predict CZFOO as a unique example of an A-site and B-site ordered double perovskite structure, AA'BB'O$_6$. In this compound, Fe$^{3+}$ and Os$^{5+}$ ions generate substantial magnetization, while Ca$^{2+}$ and Zn$^{2+}$ ions create a layerwise polar environment, resulting in a synergistic combination for multiferroicity. We determine the magnitude of the spontaneous polarization, $\vert P_s \vert$, to be 16.8 $\mu$ C/cm$^2$, and the magnetic moment is approximately 2 $\mu_B$ per formula unit. The remarkable ferroelectric and ferrimagnetic behaviors exhibited by CZFOO make it a promising candidate for various device applications. Despite the significant magnetization and polarization observed, surpassing those of other double perovskites, we find a weak spin-orbit coupling, leading to the absence of any significant magnetoelectric effect in CZFOO. Our findings shed light on the potential of CZFOO as a multiferroic material and provide insights into the intricate interplay between ferroelectricity and ferrimagnetism in double perovskite compounds.