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; Pengcheng Dai

doi:10.1038/s41467-023-37669-5

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, Pengcheng Dai

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4 Scopus citations

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.

Original language	English
Article number	2051
Journal	Nature Communications
Volume	14
Issue number	1
DOIs	https://doi.org/10.1038/s41467-023-37669-5
State	Published - Dec 2023

Funding

We thank Haoyu Hu and Youzhe Chen for helpful discussions. The INS work at Rice is supported by the U.S. DOE, BES under grant no. DE-SC0012311 (P.D.). The single crystal growth and characterization at Rice are supported by the Robert A. Welch Foundation Grant No. C-1839 (P.D.). S.L. and A.H.N. were supported by the Robert A. Welch Foundation Grant No. C-1818. C.L.H. and E.M. acknowledge support from the Robert A. Welch Foundation Grant No. C-2114. L.B. was supported by the NSF CMMT program under Grant No. DMR-2116515. C.L.H. is also supported by the Ministry of Science and Technology (MOST) in Taiwan under grant No. MOST 109-2112-M-006-026-MY3 and MOST 110-2124-M-006-009. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by ORNL. Experiments at the ISIS Neutron and Muon Source were supported by a beam time allocation RB2090032 and RB2090034 from the Science and Technology Facilities Council. We thank Ross Stewart for performing the INS experiment on the powder samples using LET. We thank Haoyu Hu and Youzhe Chen for helpful discussions. The INS work at Rice is supported by the U.S. DOE, BES under grant no. DE-SC0012311 (P.D.). The single crystal growth and characterization at Rice are supported by the Robert A. Welch Foundation Grant No. C-1839 (P.D.). S.L. and A.H.N. were supported by the Robert A. Welch Foundation Grant No. C-1818. C.L.H. and E.M. acknowledge support from the Robert A. Welch Foundation Grant No. C-2114. L.B. was supported by the NSF CMMT program under Grant No. DMR-2116515. C.L.H. is also supported by the Ministry of Science and Technology (MOST) in Taiwan under grant No. MOST 109-2112-M-006-026-MY3 and MOST 110-2124-M-006-009. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by ORNL. Experiments at the ISIS Neutron and Muon Source were supported by a beam time allocation RB2090032 and RB2090034 from the Science and Technology Facilities Council. We thank Ross Stewart for performing the INS experiment on the powder samples using LET.

Funders	Funder number
ISIS	RB2090034
National Science Foundation	DMR-2116515
U.S. Department of Energy
Welch Foundation	C-1839, C-2114, C-1818
Office of Science
Basic Energy Sciences	DE-SC0012311
Oak Ridge National Laboratory
Science and Technology Facilities Council
Ministry of Science and Technology, Taiwan	109-2112-M-006-026-MY3, 110-2124-M-006-009

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10.1038/s41467-023-37669-5

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Gao, B., Chen, T., Wu, X. C., Flynn, M., Duan, C., Chen, L., Huang, C. L., Liebman, J., Li, S., Ye, F., Stone, M. B., Podlesnyak, A., Abernathy, D. L., Adroja, D. T., Duc Le, M., Huang, Q., Nevidomskyy, A. H., Morosan, E., Balents, L., & Dai, P. (2023). Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system. Nature Communications, 14(1), Article 2051. https://doi.org/10.1038/s41467-023-37669-5

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title = "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.",

author = "Bin Gao and Tong Chen and Wu, {Xiao Chuan} and Michael Flynn and Chunruo Duan and Lebing Chen and Huang, {Chien Lung} and Jesse Liebman and Shuyi Li and Feng Ye and Stone, {Matthew B.} and Andrey Podlesnyak and Abernathy, {Douglas L.} and Adroja, {Devashibhai T.} and {Duc Le}, Manh and Qingzhen Huang and Nevidomskyy, {Andriy H.} and Emilia Morosan and Leon Balents and Pengcheng Dai",

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month = dec,

doi = "10.1038/s41467-023-37669-5",

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Gao, B, Chen, T, Wu, XC, Flynn, M, Duan, C, Chen, L, Huang, CL, Liebman, J, Li, S, Ye, F , Stone, MB , Podlesnyak, A , Abernathy, DL, Adroja, DT, Duc Le, M, Huang, Q, Nevidomskyy, AH, Morosan, E, Balents, L & Dai, P 2023, 'Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system', Nature Communications, vol. 14, no. 1, 2051. https://doi.org/10.1038/s41467-023-37669-5

TY - JOUR

T1 - Diffusive excitonic bands from frustrated triangular sublattice in a singlet-ground-state system

AU - Gao, Bin

AU - Chen, Tong

AU - Wu, Xiao Chuan

AU - Flynn, Michael

AU - Duan, Chunruo

AU - Chen, Lebing

AU - Huang, Chien Lung

AU - Liebman, Jesse

AU - Li, Shuyi

AU - Ye, Feng

AU - Stone, Matthew B.

AU - Podlesnyak, Andrey

AU - Abernathy, Douglas L.

AU - Adroja, Devashibhai T.

AU - Duc Le, Manh

AU - Huang, Qingzhen

AU - Nevidomskyy, Andriy H.

AU - Morosan, Emilia

AU - Balents, Leon

AU - Dai, Pengcheng

PY - 2023/12

Y1 - 2023/12

N2 - 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.

AB - 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.

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VL - 14

JO - Nature Communications

JF - Nature Communications

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M1 - 2051

ER -

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

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