Frustrated $J_1-J_2$ Diamond Lattice Antiferromagnet Co$_2$Ti$_3$O$_8$ with a Vacancy-ordered Spinel Structure Synthesized via a Topochemical Reaction

Abstract: Metastable Co$_2$Ti$_3$O$_8$ was synthesized through a topochemical reaction using Li$_2$CoTi$_3$O$_8$ as the precursor, resulting in a vacancy-ordered spinel structure. Crystal structure analysis confirmed that Co ions selectively occupy the A-site, giving rise to a frustrated diamond lattice. Magnetic susceptibility and heat capacity measurements revealed antiferromagnetic order at 4.4 K, which is markedly suppressed compared to the negative Weiss temperature of ${\sim}-27$ K, indicating a high degree of frustration effects. Pulsed high-field magnetization measurements revealed a four-step successive magnetic phase transition, demonstrating that Co$_2$Ti$_3$O$_8$ is a promising candidate for a frustrated $J_1-J_2$ diamond lattice. Additionally, the $J_2/J_1$ ration estimated from the molecular field approximation suggests the possibility of a spiral ordered ground state. These observations highlight the potential of frustrated magnetism in ordered spinel structures to expand the material search space for quantum magnetism, including magnetic skyrmions.