Disordered magnetic ground state in a quasi-1-D d4 columnar iridate Sr3LiIrO6

Abstract Spin-orbit coupling (SOC) offers a large variety of novel and extraordinary magnetic and electronic properties in otherwise ‘ordinary pool’ of heavy ion oxides. Here we present a detailed study on an apparently isolated hexagonal 2 H spin-chain d 4 iridate Sr 3 LiIrO 6 (SLIO) with geometric frustration. Our structural studies reveal Li-Ir chemical order with desired stoichiometry in this compound, while x-ray absorption together with x-ray photoemission spectroscopic characterizations establish pure 5+ valence of Ir. We have established a magnetic ground state with finite Ir 5+ magnetic moments in this compound, contrary to the anticipated nonmagnetic J eff = 0 state, through combined dc susceptibility, 7 Li nuclear magnetic resonance (NMR), muon spin relaxation (μSR) and ab-initio electronic structure studies. These investigations together with ac magnetic susceptibility and specific heat measurements reveal that despite having noticeable antiferromagnetic correlation among the Ir 5+ local moments, this system does not magnetically order down to at least 0.05 K, possibly due to geometrical exchange frustration, arising from the comparable nearest- and next-nearest-neighbor interchain Ir-O-O-Ir superexchange interaction strengths with opposite signs. However, the zero-field (ZF) μSR analysis shows emergence of a considerable proportion of spin-freezing on top of a spin-fluctuating dynamic magnetic background down to the lowest measuredtemperature of 1.7 K, possibly due to some inhomogeneity and/or the much stronger intra-column Ir-Ir magnetic exchange interactionstrength relative to the inter-column Ir-Ir ones. The linear temperature dependence of the magnetic specific heat (C m ) in both zero and applied magnetic fields, plus the power-law behavior of the NMR spin-lattice relaxation rate suggest a gapless spinon density of states in this charge gapped disordered magnetic ground state of Sr 3 LiIrO 6 .