Na2IrO3 as a molecular orbital crystal

Abstract

Contrary to previous studies that classify Na2IrO3 as a realization of the Heisenberg-Kitaev model with dominant spin-orbit coupling, we show that this system represents a highly unusual case in which the electronic structure is dominated by the formation of quasi-molecular orbitals (QMOs), with substantial quenching of the orbital moments. The QMOs consist of six atomic orbitals on an Ir hexagon, but each Ir atom belongs to three different QMOs. The concept of such QMOs in solids invokes very different physics compared to the models considered previously. Employing density functional theory calculations and model considerations we find that both the insulating behavior and the experimentally observed zigzag antiferromagnetism in Na2IrO3 naturally follow from the QMO model.

Final version, accepted by PRL

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• Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
• Quantum spin Hall effect in a transition metal oxide Na2IrO3
• The origin of a${}_{1g}$ and e${}_g$' orderings in Na${}_x$CoO${}_2$

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