Emergent quantum criticality from spin-orbital entanglement in $d^8$ Mott insulators: the case of a diamond lattice antiferromagnet

Abstract

Motivated by the recent activities on the Ni-based diamond lattice antiferromagnet NiRh${}_2$O${}_4$, we theoretically explore on a general ground the unique spin and orbital physics for the Ni${}^{2+}$ ions with a $3d^8$ electron configuration in the tetrahedral crystal field environment and on a diamond lattice Mott insulator. The superexchange interaction between the local moments usually favors magnetic orders. Due to the particular electron configuration of the Ni${}^{2+}$ ion with a partially filled upper $t_{2g}$ level and a fully filled lower $e_g$ level, the atomic spin-orbit coupling becomes active at the linear order and would favor a spin-orbital-entangled singlet with quenched local moments in the single-ion limit. Thus, the spin-orbital entanglement competes with the superexchange and could drive the system to a quantum critical point that separates the spin-orbital singlet and the magnetic order. We further explore the effects of magnetic field and uniaxial pressure. The non-trivial response to the magnetic field is intimately tied to the underlying spin-orbital structure of the local moments. We discuss the future experiments such as doping and pressure, and point out the correspondence between different electron configurations.

arXiv comment6+3 pages, 3+2 figures, 1 table

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• Quantum Spin Supersolid as a precursory Dirac Spin Liquid in a Triangular Lattice Antiferromagnet
• The Curious Case of NiRh${}_2$O${}_4$: A Spin-Orbit Entangled Diamond Lattice Paramagnet
• Electronic structure of the frustrated diamond lattice magnet NiRh${}_2$O${}_4$
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• Magnetic ordering in the $J_{\mathrm{eff}}$ = 0 Nickelate NiRh${}_2$O${}_4$ prepared via a solid-state metathesis