Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system

Abstract

Magnetic order in most materials occurs when magnetic ions with finite moments arrange in a particular pattern below the ordering temperature. Intriguingly, if the crystal electric field (CEF) effect results in a spin-singlet ground state, a magnetic order can still occur due to the exchange interactions between neighboring ions admixing the excited CEF levels. The magnetic excitations in such a state are spin excitons generally dispersionless in reciprocal space. Here we use neutron scattering to study stoichiometric Ni₂Mo₃O₈, where Ni²⁺ ions form a bipartite honeycomb lattice comprised of two triangular lattices, with ions subject to the tetrahedral and octahedral crystalline environment, respectively. We find that in both types of ions, the CEF excitations have nonmagnetic singlet ground states, yet the material has magnetic order. Furthermore, CEF spin excitons from the tetrahedral sites form a dispersive diffusive pattern around the Brillouin zone boundary, likely due to spin entanglement and geometric frustrations.

Some materials can display magnetic order despite having spin-singlet ground state on individual magnetic sites. This arises due to exchange interactions mixing excited crystal electric field states. Here, Gao et al study and example of such a system, Ni₂Mo₃O₈, and find that crystal electric field states in both the paramagnetic and antiferromagnetic states exhibit dispersive excitations.