Effect of nonmagnetic dilution in honeycomb lattice iridates Na$_2$IrO$_3$ and Li$_2$IrO$_3$

Abstract

We have synthesized single crystals of Na$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and polycrystals of Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ and studied the effect of magnetic depletion on the magnetic properties by measurements of the magnetic susceptibility, specific heat and magnetocaloric effect at temperatures down to 0.1~K. In both systems, the non-magnetic substitution rapidly changes the magnetically ordered ground state into a spin glass, indicating strong frustration. While for the Li system the Weiss temperature $\Theta_{\rm W}$ remains unchanged up to $x=0.55$, a strong decrease $|\Theta_{\rm W}|$ is found for the Na system. This suggests that only for the former system magnetic exchange beyond nearest neighbors is dominating. This is also corroborated by the observation of a smeared quantum phase transition in Li$_2$(Ir$_{1-x}$Ti$_x$)O$_3$ near $x=0.5$, i.e. much beyond the site percolation threshold of the honeycomb lattice.