Role of disorder in the electronic and magnetic properties of Ag${}_3$LiIr${}_2$O${}_6$

Abstract

The nature of magnetism in the intercalated honeycomb iridate Ag${}_3$LiIr${}_2$O${}_6$ has been a subject of recent intensive debate, where the absence or presence of antiferromagnetic order has been reported to be related to possible structural disorder effects and, an enhanced Ir-O hybridization and itinerancy with respect to the parent Li${}_2$IrO${}_3$ has been suggested as the origin of distinct x-ray spectroscopy features. In the present work we investigate the microscopic nature of the electronic and magnetic properties of Ag${}_3$LiIr${}_2$O${}_6$ via a combination of density functional theory combined with exact diagonalization of ab initio-derived models for various experimental and theoretical structures. We evaluate two possible scenarios, the itinerant quasimolecular framework (QMO) on the one hand, and the localized relativistic $j_{\mathrm{eff}}=1/2$ and $j_{\mathrm{eff}}=3/2$ picture on the other hand, and find that the latter description is still viable for this system. We further calculate resonant inelastic x-ray scattering spectra and show that agreement with experimental observations can be obtained if the presence of Ag vacancies leading to changes in Ir filling and structural disorder is assumed. Finally, we show that the experimentally observed antiferromagnetic spiral magnetic order is reproduced by our ab-initio derived magnetic models.

published in PRB; added Ref. [37]

References in corpus (16)

• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• $\alpha$-RuCl3: a Spin-Orbit Assisted Mott Insulator on a Honeycomb Lattice
• Models and Materials for Generalized Kitaev Magnetism
• On the Origin of Zigzag Magnetic Order in Iridium Oxide Na2IrO3
• Kitaev magnetism in honeycomb RuCl3 with intermediate spin-orbit coupling
• Crystal field splitting and correlation effect on the electronic structure of A2IrO3
• Thermodynamic Evidence of Proximity to a Kitaev Spin-Liquid in Ag${}_3$LiIr${}_2$O${}_6$
• Vacancy-induced low-energy density of states in the Kitaev spin liquid
• Resonant inelastic x-ray incarnation of Young's double-slit experiment
• EDRIXS: An open source toolkit for simulating spectra of resonant inelastic x-ray scattering
• Modified Curie-Weiss Law for $j_{\mathrm{eff}}$ Magnets
• Effect of structural disorder on the Kitaev magnet Ag${}_3$LiIr${}_2$O${}_6$
• Analysis of the optical conductivity for A2IrO3 (A = Na, Li) from first principles
• Nearly itinerant electronic groundstate in the intercalated honeycomb iridate Ag${}_3$LiIr${}_2$O${}_6$
• NMR Investigation on Honeycomb Iridate Ag${}_3$LiIr${}_2$O${}_6$
• Electronic excitations in $\gamma$-Li${}_2$IrO${}_3$

Cited by in corpus (1)

• On the electronic ground state of two non-magnetic pentavalent honeycomb iridates