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

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

doi:10.1038/s41467-023-37669-5

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

Journal Article · 11 April 2023 · Nature Communications

DOI: https://doi.org/10.1038/s41467-023-37669-5 · OSTI ID:1971021

^[1];

^[2];

^[3]; Duan, Chunruo ^[1];

^[1]; Huang, Chien-Lung ^[4];

^[1]; Li, Shuyi ^[1];

^[5];

^[6];

^[6]; Huang, Qingzhen ^[7];

^[1]; Morosan, Emilia ^[1]; Balents, Leon ^[8];

^[1]

Rice Univ., Houston, TX (United States)
Univ. of California, Santa Barbara, CA (United States)
Univ. of California, Davis, CA (United States); Boston Univ., MA (United States)
Rice Univ., Houston, TX (United States); National Cheng Kung University (Taiwan)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Rutherford Appleton Laboratory (United Kingdom)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Univ. of California, Santa Barbara, CA (United States); Canadian Institute for Advanced Research (Canada)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Robert A. Welch Foundation; National Science Foundation (NSF); Taiwan Ministry of Science and Technology (MOST)

Grant/Contract Number:: AC05-00OR22725; SC0012311

OSTI ID:: 1971021

Alternate ID(s):: OSTI ID: 1971053

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 14; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

References (31)

Metamagnetic transitions and magnetoelectricity in the spin-1 honeycomb antiferromagnet Ni 2 Mo 3 O 8 Tang, Y. S.; Zhang, J. H.; Lin, L. Physical Review B, Vol. 103, Issue 1 https://doi.org/10.1103/PhysRevB.103.014112	journal	January 2021
Paramagnetic excitations in singlet ground statePrNi2Si2 Blanco, J. A.; Nicklow, R. M.; Schmitt, D. Physical Review B, Vol. 56, Issue 18 https://doi.org/10.1103/PhysRevB.56.11666	journal	November 1997
Disentangling orbital and spin exchange interactions for Co 2 + on a rocksalt lattice Sarte, P. M.; Cowley, R. A.; Rodriguez, E. E. Physical Review B, Vol. 98, Issue 2 https://doi.org/10.1103/PhysRevB.98.024415	journal	July 2018
Noncollinear antiferromagnetic order and effect of spin-orbit coupling in spin-1 honeycomb lattice Li, Shuyi; Le, Manh Duc; Loganathan, Vaideesh Physical Review Materials, Vol. 6, Issue 1 https://doi.org/10.1103/PhysRevMaterials.6.014405	journal	January 2022
Design and operation of the wide angular-range chopper spectrometer ARCS at the Spallation Neutron Source Abernathy, D. L.; Stone, M. B.; Loguillo, M. J. Review of Scientific Instruments, Vol. 83, Issue 1 https://doi.org/10.1063/1.3680104	journal	January 2012
Large easy-axis anisotropy in the one-dimensional magnet BaMo ( PO 4 ) 2 Abdeldaim, Aly H.; Badrtdinov, Danis I.; Gibbs, Alexandra S. Physical Review B, Vol. 100, Issue 21 https://doi.org/10.1103/PhysRevB.100.214427	journal	December 2019
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
Implementation of cross correlation for energy discrimination on the time-of-flight spectrometer CORELLI Ye, Feng; Liu, Yaohua; Whitfield, Ross Journal of Applied Crystallography, Vol. 51, Issue 2 https://doi.org/10.1107/S160057671800403X	journal	March 2018
The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance Ehlers, G.; Podlesnyak, A. A.; Niedziela, J. L. Review of Scientific Instruments, Vol. 82, Issue 8 https://doi.org/10.1063/1.3626935	journal	August 2011
Principles of Neutron Scattering from Condensed Matter Boothroyd, Andrew T. Oxford University Press https://doi.org/10.1093/oso/9780198862314.001.0001	book	July 2020
Dirac Magnons in a Honeycomb Lattice Quantum XY Magnet CoTiO 3 Yuan, Bo; Khait, Ilia; Shu, Guo-Jiun Physical Review X, Vol. 10, Issue 1 https://doi.org/10.1103/PhysRevX.10.011062	journal	March 2020
Induced-Moment Ferromagnetism in Pr 3 Tl Andres, K.; Bucher, E.; Darack, S. Physical Review B, Vol. 6, Issue 7 https://doi.org/10.1103/PhysRevB.6.2716	journal	October 1972
Temperature dependence of magnetic excitations in singlet-ground-state systems. II. Excited-state spin waves near the Curie temperature in Pr 3 Tl Buyers, W. J. L.; Holden, T. M.; Perreault, A. Physical Review B, Vol. 11, Issue 1 https://doi.org/10.1103/PhysRevB.11.266	journal	January 1975
High-Temperature Terahertz Optical Diode Effect without Magnetic Order in Polar FeZnMo 3 O 8 Yu, Shukai; Gao, Bin; Kim, Jae Wook Physical Review Letters, Vol. 120, Issue 3 https://doi.org/10.1103/PhysRevLett.120.037601	journal	January 2018
Spin-orbit exciton in a honeycomb lattice magnet CoTiO3 : Revealing a link between magnetism in d - and f -electron systems Yuan, Bo; Stone, M. B.; Shu, Guo-Jiun Physical Review B, Vol. 102, Issue 13 https://doi.org/10.1103/PhysRevB.102.134404	journal	October 2020
Spin-orbit excitons in CoO Sarte, P. M.; Songvilay, M.; Pachoud, E. Physical Review B, Vol. 100, Issue 7 https://doi.org/10.1103/PhysRevB.100.075143	journal	August 2019
Spin liquids in frustrated magnets Balents, Leon Nature, Vol. 464, Issue 7286 https://doi.org/10.1038/nature08917	journal	March 2010
Possible Anomalies at a Semimetal-Semiconductor Transistion Halperin, B. I.; Rice, T. M. Reviews of Modern Physics, Vol. 40, Issue 4 https://doi.org/10.1103/RevModPhys.40.755	journal	October 1968
Frustrated spin one on a diamond lattice in NiRh 2 O 4 Chamorro, J. R.; Ge, L.; Flynn, J. Physical Review Materials, Vol. 2, Issue 3 https://doi.org/10.1103/PhysRevMaterials.2.034404	journal	March 2018
Confirming the trilinear form of the optical magnetoelectric effect in the polar honeycomb antiferromagnet Co2Mo3O8 Reschke, S.; Farkas, D. G.; Strinić, A. npj Quantum Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41535-021-00417-3	journal	January 2022
Quantum spin liquids Broholm, C.; Cava, R. J.; Kivelson, S. A. Science, Vol. 367, Issue 6475 https://doi.org/10.1126/science.aay0668	journal	January 2020
Magnetic Excitations and Magnetic Ordering in Praseodymium Houmann, J. G.; Chapellier, M.; Mackintosh, A. R. Physical Review Letters, Vol. 34, Issue 10 https://doi.org/10.1103/PhysRevLett.34.587	journal	March 1975
Collinear magnetic structure and multiferroicity in the polar magnet Co 2 Mo 3 O 8 Tang, Y. S.; Wang, S. M.; Lin, L. Physical Review B, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevB.100.134112	journal	October 2019
N i 2 M o 3 O 8 : Complex antiferromagnetic order on a honeycomb lattice Morey, Jennifer R.; Scheie, Allen; Sheckelton, John P. Physical Review Materials, Vol. 3, Issue 1 https://doi.org/10.1103/PhysRevMaterials.3.014410	journal	January 2019
Quantum spin liquid states Zhou, Yi; Kanoda, Kazushi; Ng, Tai-Kai Reviews of Modern Physics, Vol. 89, Issue 2 https://doi.org/10.1103/RevModPhys.89.025003	journal	April 2017
Spin-glass order induced by dynamic frustration Goremychkin, E. A.; Osborn, R.; Rainford, B. D. Nature Physics, Vol. 4, Issue 10 https://doi.org/10.1038/nphys1028	journal	July 2008
Giant thermal Hall effect in multiferroics Ideue, T.; Kurumaji, T.; Ishiwata, S. Nature Materials, Vol. 16, Issue 8 https://doi.org/10.1038/nmat4905	journal	May 2017
Quantum Spin Liquids in Frustrated Spin-1 Diamond Antiferromagnets Buessen, Finn Lasse; Hering, Max; Reuther, Johannes Physical Review Letters, Vol. 120, Issue 5 https://doi.org/10.1103/PhysRevLett.120.057201	journal	January 2018
Frustrated Ising chains on the triangular lattice in Sr 3 NiIrO 6 Toth, S.; Wu, W.; Adroja, D. T. Physical Review B, Vol. 93, Issue 17 https://doi.org/10.1103/PhysRevB.93.174422	journal	May 2016
Order-by-disorder from bond-dependent exchange and intensity signature of nodal quasiparticles in a honeycomb cobaltate Elliot, M.; McClarty, P. A.; Prabhakaran, D. Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-23851-0	journal	June 2021
Magnetic Excitons in Singlet—Ground-State Ferromagnets Birgeneau, R. J.; Als-Nielsen, J.; Bucher, E. Physical Review Letters, Vol. 27, Issue 22 https://doi.org/10.1103/PhysRevLett.27.1530	journal	November 1971

Similar Records

Electronic structure of the frustrated diamond lattice magnet NiRh2O4

Journal Article · 2022 · Physical Review. B · OSTI ID:1889167

Zager, B.; Chamorro, J. R.; Ge, L.; +8 more

Singlet-ground-state paramagnetic centers in CuO[sub 2] layers as seen from [sup 169]Tm NMR in TmBa[sub 2]Cu[sub 3]O[sub 6+[ital x]] superconductors

Journal Article · 1995 · Physical Review, B: Condensed Matter; (United States) · OSTI ID:6701493

Bakharev, O N; Witteveen, J; Brom, H B; +3 more

Orbital Degeneracy Removed by Charge Order in Triangular Antiferromagnet AgNiO{sub 2}

Journal Article · 2007 · Physical Review Letters · OSTI ID:21024272

Wawrzynska, E; Coldea, R; Wheeler, E M; +6 more

Related Subjects

36 MATERIALS SCIENCE
magnetic properties and materials
quantum fluids and solids

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

Citation Formats

References (31)

Similar Records

Related Subjects