Effect of Pb Substitution at the Mo site on the Magnetic Properties of the Polar Magnet Fe$_2$Mo$_3$O$_8$

Abstract

The ternary transition-metal oxide Fe$_2$Mo$_3$O$_8$ is a polar magnet characterized by a layered structure of magnetic Fe honeycomb lattices and non-magnetic Mo kagome lattices. Whereas previous studies have primarily focused on the chemical substitution at the Fe sites to modulate the magnetic properties, the Mo sites have remained largely unexplored due to the strong spin-singlet trimerization of Mo$^{4+}$ ions. In this study, we investigated the effect of substituting non-magnetic Pb$^{4+}$ and Zr$^{4+}$ ions into the Mo sites to intentionally disrupt the Mo trimers. Our results reveal that the disruption of the Mo spin-singlet state induces active spins within the Mo layer, resulting in the emergence of a ferromagnetic-like behavior that persists even at room temperature. Quantitative analysis that takes into account the weight fraction of the main phase suggests an effective spin $S = 1/2$ state per active Mo ion upon trimer disruption. These findings demonstrate that controlling non-magnetic cluster states within a polar host via chemical substitution is a promising approach for designing room-temperature magnetoelectric materials.