Evolution of Magnetism in the Na_(3-d)Na_(1-x)Mg_xIr₂O₆ Series of Honeycomb Iridates

The structural and magnetic properties of a new series of iridium-based honeycomb lattices with the formula Na3-delta(Na1-xMgx)Ir2O6 (x = 0 to 1) are reported. As x and delta are increased, the honeycomb lattice contracts and the strength of the antiferromagnetic interactions decreases systematically due to a reduction in Ir-O-Ir bond angles. Samples with imperfect stoichiometry exhibit disordered magnetic freezing at temperatures Tf between 3.4 K and 5 K. This glassy magnetism likely arises due to the presence of non-magnetic Ir3+, which are distributed randomly throughout the lattice, with a possible additional contribution from stacking faults. Together, these results demonstrate that chemical defects and non-stoichiometry have a significant effect on the magnetism of compounds in the A2IrO3 materials family.