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

Bin Gao, Tong Chen, Xiao-Chuan Wu, Michael Flynn, Chunruo Duan, Lebing Chen, Chien-Lung Huang, Jesse Liebman, Shuyi Li, Feng Ye, Matthew B. Stone, Andrey Podlesnyak, Douglas L. Abernathy, Devashibhai T. Adroja, Manh Duc Le, Qingzhen Huang, Andriy H. Nevidomskyy, Emilia Morosan, Leon Balents and Pengcheng Dai ()
Additional contact information
Bin Gao: Rice University
Tong Chen: Rice University
Xiao-Chuan Wu: University of California
Michael Flynn: University of California
Chunruo Duan: Rice University
Lebing Chen: Rice University
Chien-Lung Huang: Rice University
Jesse Liebman: Rice University
Shuyi Li: Rice University
Feng Ye: Oak Ridge National Laboratory
Matthew B. Stone: Oak Ridge National Laboratory
Andrey Podlesnyak: Oak Ridge National Laboratory
Douglas L. Abernathy: Oak Ridge National Laboratory
Devashibhai T. Adroja: Rutherford Appleton Laboratory
Manh Duc Le: Rutherford Appleton Laboratory
Qingzhen Huang: National Institute of Standards and Technology
Andriy H. Nevidomskyy: Rice University
Emilia Morosan: Rice University
Leon Balents: University of California
Pengcheng Dai: Rice University

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-37669-5

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