Role of Hydrogen in the spin-orbital-entangled quantum liquid candidate H${}_3$LiIr${}_2$O${}_6$

Abstract

Motivated by recent reports of H${}_3$LiIr${}_2$O${}_6$ as a spin-orbital-entangled quantum liquid, we investigate via a combination of density functional theory and non-perturbative exact diagonalization the microscopic nature of its magnetic interactions. We find that while the interlayer O-H-O bond geometry strongly affects the local magnetic couplings, these bonds are likely to remain symmetrical due to large zero-point fluctuations of the H positions. In this case, the estimated magnetic model lies close to the classical tricritical point between ferromagnetic, zigzag and incommensurate spiral orders, what may contribute to the lack of magnetic ordering. However, we also find that substitution of H by D (deuterium) as well as disorder-induced inhomogeneities destabilize the O-H/D-O bonds modifying strongly the local magnetic couplings. These results suggest that the magnetic response in H${}_3$LiIr${}_2$O${}_6$ is likely sensitive to both the stoichiometry and microstructure of the samples and emphasize the importance of a careful treatment of hydrogen for similar systems.

accepted in Phys. Rev. Lett

References in corpus (20)

• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Models and Materials for Generalized Kitaev Magnetism
• Hyper-honeycomb iridate $\beta$-Li2IrO3 as a platform for Kitaev magnetism
• Crystal field splitting and correlation effect on the electronic structure of A2IrO3
• Valence Bonds in Random Quantum Magnets: Theory and Application to YbMgGaO4
• Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for honeycomb lattice iridates A2IrO3
• Non-coplanar and counter-rotating incommensurate magnetic order stabilized by Kitaev interactions in $\gamma$-Li2IrO3
• Unconventional magnetic order on the hyperhoneycomb Kitaev lattice in $\beta$-Li2IrO3: full solution via magnetic resonant x-ray diffraction
• Scaling and data collapse from local moments in frustrated disordered quantum spin systems
• Disorder in a quantum spin liquid: flux binding and local moment formation
• Pressure-induced dimerization and valence bond crystal formation in the Kitaev-Heisenberg magnet alpha-RuCl3
• Competition between spin-orbit coupling, magnetism, and dimerization in the honeycomb iridates: $\alpha$-Li${}_2$IrO${}_3$ under pressure
• Importance of Spin-Orbit Coupling in Organic BEDT-TTF and BEDT-TSF Salts
• Strong effect of hydrogen order on magnetic Kitaev interactions in H${}_3$LiIr${}_2$O${}_6$
• Detuning the Honeycomb of $\alpha$-RuCl${}_3$: Pressure-Dependent Optical Studies Reveal Broken Symmetry
• Magnetic structure and excitation spectrum of the hyperhoneycomb Kitaev magnet $\beta$-Li${}_2$IrO${}_3$
• Magnetic field-induced evolution of intertwined orders in the Kitaev magnet $\beta$-Li${}_2$IrO${}_3$
• Theory of a quantum spin liquid in hydrogen-intercalated honeycomb iridate, H3LiIr2O6
• Analysis of the optical conductivity for A2IrO3 (A = Na, Li) from first principles
• Electronic excitations in $\gamma$-Li${}_2$IrO${}_3$

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