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

TL;DR

This paper investigates how spin-orbital entanglement in Ni$^{2+}$ ions within a diamond lattice Mott insulator leads to emergent quantum criticality, contrasting magnetic order with spin-orbital singlet states, and explores responses to external fields.

Contribution

It provides a theoretical framework for understanding the interplay of spin, orbital physics, and quantum criticality in $d^8$ Mott insulators on a diamond lattice, highlighting the role of spin-orbit coupling.

Findings

Spin-orbital entanglement can induce a quantum critical point.

Magnetic field response is linked to the spin-orbital structure.

Competition between superexchange and spin-orbit coupling drives phase transitions.

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.