Giant Magnetocrystalline Anisotropy in Honeycomb Iridate NiIrO3 with Large Coercive Field Exceeding 17 T

Abstract

The realization of unconventional quantum phases in frustrated and spin-orbit coupled materials remains at the forefront of quantum materials research. Here we report the synthesis and discovery of NiIrO3, the first honeycomb iridate with coupled 3d-5d magnetic sublattices, through a soft topotactic reaction. Structural analysis reveals an ilmenite-type stacking of edge-sharing NiO6 and IrO6 octahedral honeycomb sublattices in a Kitaev geometry. Comprehensive magnetic and electrical transport measurements unveil its long-range ferrimagnetic order below 213 K, which is in sharp contrast to the predominantly antiferromagnetic order in the known honeycomb iridates. Notably, the titled compound displays an exceptionally large magnetocrystalline anisotropy energy of 32.2 meV/f.u. and a giant coercivity with coercive field exceeding 17.3 T below 4.2 K, both ranking among the highest observed in iridates to date. Combined experimental and theoretical investigations indicate that the exceptional anisotropy and coercivity originate from the synergistic effect between strong lattice frustration in the coupled 3d-5d honeycomb lattice network and the robust spin-orbit coupling of the Ir4+ (Jeff = 1/2) state. This work positions NiIrO3 as a promising platform to investigate low-dimensional and frustrated quantum spin systems, and highlights its potential for spintronic applications through the targeted engineering of 3d-5d interactions.