Continuous Spin Excitations in the Three-Dimensional Frustrated Magnet K2Ni2⁢(SO4)3

Yao, Weiliang; Huang, Qing; Xie, Tao; Podlesnyak, Andrey; Brassington, Alexander; Xing, Chengkun; Mudiyanselage, Ranuri S. Dissanayaka; Wang, Haozhe; Xie, Weiwei; Zhang, Shengzhi; Lee, Minseong; Zapf, Vivien S.; Bai, Xiaojian; Tennant, D. Alan; Liu, Jian; Zhou, Haidong

doi:10.1103/PhysRevLett.131.146701

Continuous Spin Excitations in the Three-Dimensional Frustrated Magnet K₂Ni₂⁢(SO₄)₃

Journal Article · Tue Oct 03 00:00:00 EDT 2023 · Physical Review Letters

DOI:https://doi.org/10.1103/PhysRevLett.131.146701· OSTI ID:2572560

Yao, Weiliang ^[1]; Huang, Qing ^[2]; Xie, Tao ^[3]; ^[3]; Brassington, Alexander ^[2]; Xing, Chengkun ^[2]; ^[4]; Wang, Haozhe ^[5]; Xie, Weiwei ^[6]; ^[7]; ^[7]; ^[7]; Bai, Xiaojian ^[8]; Tennant, D. Alan ^[2]; Liu, Jian ^[2]; ^[2]

University of Tennessee, Knoxville, TN (United States); Rice University, Houston, TX (United States)
University of Tennessee, Knoxville, TN (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Rutgers University, Piscataway, NJ (United States)
Michigan State University, East Lansing, MI (United States)
Rutgers University, Piscataway, NJ (United States); Michigan State University, East Lansing, MI (United States)
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Louisiana State University, Baton Rouge, LA (United States)

Continuous spin excitations are widely recognized as one of the hallmarks of novel spin states in quantum magnets, such as quantum spin liquids (QSLs). Here, we report the observation of such kind of excitations in K₂Ni₂(SO₄)₃, which consists of two sets of intersected spin-1 (Ni²⁺) trillium lattices. Our inelastic neutron scattering measurement on single crystals clearly shows a dominant excitation continuum, which exhibits a distinct temperature-dependent behavior from that of spin waves and is rooted in strong quantum spin fluctuations. Further using the self-consistent-Gaussian-approximation method, we determine that the fourth- and fifth nearest-neighbor exchange interactions are dominant. These two bonds together form a unique three-dimensional network of corner-sharing tetrahedra, which we name as a “hypertrillium” lattice. In conclusion, our results provide direct evidence for the existence of QSL features in K₂Ni₂(SO₄)₃ and highlight the potential for the hypertrillium lattice to host frustrated quantum magnetism.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: 89233218CNA000001; AC05-00OR22725; SC0020254; SC0022311

OSTI ID:: 2572560

Alternate ID(s):: OSTI ID: 2007710

Report Number(s):: LA-UR--23-31901; 1079-7114; 10.1103/PhysRevLett.131.146701

Journal Information:: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 14 Vol. 131; ISSN 1079-7114; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

References (68)

Über Doppelsulfate vom Langbeinit‐Typ, AB (SO₄)₃ Gattow, G.; Zemann, J. Zeitschrift für anorganische und allgemeine Chemie, Vol. 293, Issue 5-6 https://doi.org/10.1002/zaac.19582930502	journal	February 1958
Phase transitions in langbeinites I: Crystal chemistry and structures of K-double sulfates of the langbeinite type M 2 + + K2(SO4)3, M + +=Mg, Ni, Co, Zn, Ca Speer, D.; Salje, E. Physics and Chemistry of Minerals, Vol. 13, Issue 1 https://doi.org/10.1007/BF00307309	journal	January 1986
Zur Theorie des Ferromagnetismus Bloch, F. Zeitschrift f�r Physik, Vol. 61, Issue 3-4 https://doi.org/10.1007/BF01339661	journal	March 1930
Recent advances in magnetic structure determination by neutron powder diffraction Rodríguez-Carvajal, Juan Physica B: Condensed Matter, Vol. 192, Issue 1-2 https://doi.org/10.1016/0921-4526(93)90108-I	journal	October 1993
Horace : Software for the analysis of data from single crystal spectroscopy experiments at time-of-flight neutron instruments Ewings, R. A.; Buts, A.; Le, M. D. Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 834 https://doi.org/10.1016/j.nima.2016.07.036	journal	October 2016
Neutron Scattering with a Triple-Axis Spectrometer Shirane, Gen; Shapiro, Stephen M.; Tranquada, John M. https://doi.org/10.1017/CBO9780511534881	book	January 2009
Understanding Doping of Quantum Materials Zunger, Alex; Malyi, Oleksandr I. Chemical Reviews, Vol. 121, Issue 5 https://doi.org/10.1021/acs.chemrev.0c00608	journal	January 2021
Spin liquids in frustrated magnets Balents, Leon Nature, Vol. 464, Issue 7286 https://doi.org/10.1038/nature08917	journal	March 2010
Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet Han, Tian-Heng; Helton, Joel S.; Chu, Shaoyan Nature, Vol. 492, Issue 7429 https://doi.org/10.1038/nature11659	journal	December 2012
Evidence for a spinon Fermi surface in a triangular-lattice quantum-spin-liquid candidate Shen, Yao; Li, Yao-Dong; Wo, Hongliang Nature, Vol. 540, Issue 7634 https://doi.org/10.1038/nature20614	journal	December 2016
Quantum criticality and universal scaling of a quantum antiferromagnet Lake, Bella; Tennant, D. Alan; Frost, Chris D. Nature Materials, Vol. 4, Issue 4 https://doi.org/10.1038/nmat1327	journal	March 2005
Proximate Kitaev quantum spin liquid behaviour in a honeycomb magnet Banerjee, A.; Bridges, C. A.; Yan, J. -Q. Nature Materials, Vol. 15, Issue 7 https://doi.org/10.1038/nmat4604	journal	April 2016
Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4 Paddison, Joseph A. M.; Daum, Marcus; Dun, Zhiling Nature Physics, Vol. 13, Issue 2 https://doi.org/10.1038/nphys3971	journal	December 2016
Majorana fermions in the Kitaev quantum spin system α-RuCl3 Do, Seung-Hwan; Park, Sang-Youn; Yoshitake, Junki Nature Physics, Vol. 13, Issue 11 https://doi.org/10.1038/nphys4264	journal	September 2017
Order-by-disorder and spiral spin-liquid in frustrated diamond-lattice antiferromagnets Bergman, Doron; Alicea, Jason; Gull, Emanuel Nature Physics, Vol. 3, Issue 7 https://doi.org/10.1038/nphys622	journal	May 2007
Magnon bound states versus anyonic Majorana excitations in the Kitaev honeycomb magnet α-RuCl3 Wulferding, Dirk; Choi, Youngsu; Do, Seung-Hwan Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15370-1	journal	March 2020
Excitations in the field-induced quantum spin liquid state of α-RuCl3 Banerjee, Arnab; Lampen-Kelley, Paula; Knolle, Johannes npj Quantum Materials, Vol. 3, Issue 1 https://doi.org/10.1038/s41535-018-0079-2	journal	February 2018
Experimental identification of quantum spin liquids Wen, Jinsheng; Yu, Shun-Li; Li, Shiyan npj Quantum Materials, Vol. 4, Issue 1 https://doi.org/10.1038/s41535-019-0151-6	journal	April 2019
Weak-coupling to strong-coupling quantum criticality crossover in a Kitaev quantum spin liquid α-RuCl3 Han, Jae-Ho; Do, Seung-Hwan; Choi, Kwang-Yong npj Quantum Materials, Vol. 8, Issue 1 https://doi.org/10.1038/s41535-023-00563-w	journal	June 2023
Continuum of quantum fluctuations in a three-dimensional S = 1 Heisenberg magnet Plumb, K. W.; Changlani, Hitesh J.; Scheie, A. Nature Physics, Vol. 15, Issue 1 https://doi.org/10.1038/s41567-018-0317-3	journal	October 2018
Two-dimensional spin liquid behaviour in the triangular-honeycomb antiferromagnet TbInO3 Clark, Lucy; Sala, Gabriele; Maharaj, Dalini D. Nature Physics, Vol. 15, Issue 3 https://doi.org/10.1038/s41567-018-0407-2	journal	January 2019
Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore Gao, Bin; Chen, Tong; Tam, David W. Nature Physics, Vol. 15, Issue 10 https://doi.org/10.1038/s41567-019-0577-6	journal	July 2019
Order as an effect of disorder Villain, J.; Bidaux, R.; Carton, J. -P. Journal de Physique, Vol. 41, Issue 11 https://doi.org/10.1051/jphys:0198000410110126300	journal	January 1980
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
Kinetically inhibited order in a diamond-lattice antiferromagnet MacDougall, G. J.; Gout, D.; Zarestky, J. L. Proceedings of the National Academy of Sciences, Vol. 108, Issue 38 https://doi.org/10.1073/pnas.1107861108	journal	September 2011
Quantum spin liquids: a review Savary, Lucile; Balents, Leon Reports on Progress in Physics, Vol. 80, Issue 1 https://doi.org/10.1088/0034-4885/80/1/016502	journal	November 2016
Linear spin wave theory for single-Q incommensurate magnetic structures Toth, S.; Lake, B. Journal of Physics: Condensed Matter, Vol. 27, Issue 16 https://doi.org/10.1088/0953-8984/27/16/166002	journal	March 2015
Raman spectroscopic diagnostic of quantum spin liquids Wulferding, Dirk; Choi, Youngsu; Lee, Wonjun Journal of Physics: Condensed Matter, Vol. 32, Issue 4 https://doi.org/10.1088/1361-648X/ab45c4	journal	October 2019
Recent progress on magnetic-field studies on quantum-spin-liquid candidates Ma, Zhen; Ran, Kejing; Wang, Jinghui Chinese Physics B, Vol. 27, Issue 10 https://doi.org/10.1088/1674-1056/27/10/106101	journal	October 2018
Finite field regime for a quantum spin liquid in α − RuCl 3 Balz, Christian; Lampen-Kelley, Paula; Banerjee, Arnab Physical Review B, Vol. 100, Issue 6 https://doi.org/10.1103/PhysRevB.100.060405	journal	August 2019
Low-energy magnons in the chiral ferrimagnet Cu 2 OSeO 3 : A coarse-grained approach Luo, Yi; Marcus, G. G.; Trump, B. A. Physical Review B, Vol. 101, Issue 14 https://doi.org/10.1103/PhysRevB.101.144411	journal	April 2020
Magnetic field effects in an octupolar quantum spin liquid candidate Gao, Bin; Chen, Tong; Yan, Han Physical Review B, Vol. 106, Issue 9 https://doi.org/10.1103/PhysRevB.106.094425	journal	September 2022
Frustrated magnetic interactions in FeSe Gu, Yiqing; Wang, Qisi; Wo, Hongliang Physical Review B, Vol. 106, Issue 6 https://doi.org/10.1103/PhysRevB.106.L060504	journal	August 2022
Temperature dependence of the magnetic excitations in iron Lynn, J. W. Physical Review B, Vol. 11, Issue 7 https://doi.org/10.1103/PhysRevB.11.2624	journal	April 1975
Temperature dependence of the dynamic susceptibility of nickel Lynn, J. W.; Mook, H. A. Physical Review B, Vol. 23, Issue 1 https://doi.org/10.1103/PhysRevB.23.198	journal	January 1981
Mean-field approach to magnetic ordering in highly frustrated pyrochlores Reimers, J. N.; Berlinsky, A. J.; Shi, A. -C. Physical Review B, Vol. 43, Issue 1 https://doi.org/10.1103/PhysRevB.43.865	journal	January 1991
Spin dynamics in the quasi-one-dimensional S = 1 2 antiferromagnet BaCu 2 Si 2 O 7 Zheludev, A.; Kenzelmann, M.; Raymond, S. Physical Review B, Vol. 65, Issue 1 https://doi.org/10.1103/PhysRevB.65.014402	journal	November 2001
Geometric frustration inherent to the trillium lattice, a sublattice of the B20 structure Hopkinson, John M.; Kee, Hae-Young Physical Review B, Vol. 74, Issue 22 https://doi.org/10.1103/PhysRevB.74.224441	journal	December 2006
Microscopic model for spiral ordering along (110) on the MnSi lattice Hopkinson, John M.; Kee, Hae-Young Physical Review B, Vol. 75, Issue 6 https://doi.org/10.1103/PhysRevB.75.064430	journal	February 2007
Fate of partial order on trillium and distorted windmill lattices Isakov, Sergei V.; Hopkinson, John M.; Kee, Hae-Young Physical Review B, Vol. 78, Issue 1 https://doi.org/10.1103/PhysRevB.78.014404	journal	July 2008
Absent pinch points and emergent clusters: Further neighbor interactions in the pyrochlore Heisenberg antiferromagnet Conlon, P. H.; Chalker, J. T. Physical Review B, Vol. 81, Issue 22 https://doi.org/10.1103/PhysRevB.81.224413	journal	June 2010
Highly frustrated magnetism in SrHo 2 O 4 : Coexistence of two types of short-range order Young, O.; Wildes, A. R.; Manuel, P. Physical Review B, Vol. 88, Issue 2 https://doi.org/10.1103/PhysRevB.88.024411	journal	July 2013
NaCaN i 2 F 7 : A frustrated high-temperature pyrochlore antiferromagnet with S = 1 N i 2 + Krizan, J. W.; Cava, R. J. Physical Review B, Vol. 92, Issue 1 https://doi.org/10.1103/PhysRevB.92.014406	journal	July 2015
Low-temperature crystal and magnetic structure of α − RuCl 3 Cao, H. B.; Banerjee, A.; Yan, J. -Q. Physical Review B, Vol. 93, Issue 13 https://doi.org/10.1103/PhysRevB.93.134423	journal	April 2016
Phase diagram of α − RuCl 3 in an in-plane magnetic field Sears, J. A.; Zhao, Y.; Xu, Z. Physical Review B, Vol. 95, Issue 18 https://doi.org/10.1103/PhysRevB.95.180411	journal	May 2017
Order by Quantum Disorder in Er 2 Ti 2 O 7 Savary, Lucile; Ross, Kate A.; Gaulin, Bruce D. Physical Review Letters, Vol. 109, Issue 16 https://doi.org/10.1103/PhysRevLett.109.167201	journal	October 2012
Scattering Continuum and Possible Fractionalized Excitations in α − RuCl 3 Sandilands, Luke J.; Tian, Yao; Plumb, Kemp W. Physical Review Letters, Vol. 114, Issue 14 https://doi.org/10.1103/PhysRevLett.114.147201	journal	April 2015
Evidence for a Field-Induced Quantum Spin Liquid in α - RuCl 3 Baek, S. -H.; Do, S. -H.; Choi, K. -Y. Physical Review Letters, Vol. 119, Issue 3 https://doi.org/10.1103/PhysRevLett.119.037201	journal	July 2017
Antiferromagnetic Resonance and Terahertz Continuum in α − RuCl 3 Little, A.; Wu, Liang; Lampen-Kelley, P. Physical Review Letters, Vol. 119, Issue 22 https://doi.org/10.1103/PhysRevLett.119.227201	journal	November 2017
Spin-Glass Ground State in a Triangular-Lattice Compound YbZnGaO 4 Ma, Zhen; Wang, Jinghui; Dong, Zhao-Yang Physical Review Letters, Vol. 120, Issue 8 https://doi.org/10.1103/PhysRevLett.120.087201	journal	February 2018
Multi- q Mesoscale Magnetism in CeAuSb 2 Marcus, Guy G.; Kim, Dae-Jeong; Tutmaher, Jacob A. Physical Review Letters, Vol. 120, Issue 9 https://doi.org/10.1103/PhysRevLett.120.097201	journal	February 2018
Magnetic Excitations of the Classical Spin Liquid MgCr 2 O 4 Bai, X.; Paddison, J. A. M.; Kapit, E. Physical Review Letters, Vol. 122, Issue 9 https://doi.org/10.1103/PhysRevLett.122.097201	journal	March 2019
Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet Ce 2 Zr 2 O 7 Gaudet, J.; Smith, E. M.; Dudemaine, J. Physical Review Letters, Vol. 122, Issue 18 https://doi.org/10.1103/PhysRevLett.122.187201	journal	May 2019
Scattering Signatures of Bond-Dependent Magnetic Interactions Paddison, Joseph A. M. Physical Review Letters, Vol. 125, Issue 24 https://doi.org/10.1103/PhysRevLett.125.247202	journal	December 2020
Magnetic Field Induced Quantum Spin Liquid in the Two Coupled Trillium Lattices of K2Ni2(SO4)3 Živković, Ivica; Favre, Virgile; Salazar Mejia, Catalina Physical Review Letters, Vol. 127, Issue 15 https://doi.org/10.1103/PhysRevLett.127.157204	journal	October 2021
Geometric Frustration on the Trillium Lattice in a Magnetic Metal-Organic Framework Bulled, Johnathan M.; Paddison, Joseph A. M.; Wildes, Andrew Physical Review Letters, Vol. 128, Issue 17 https://doi.org/10.1103/PhysRevLett.128.177201	journal	April 2022
Spiral Spin Liquid on a Honeycomb Lattice Gao, Shang; McGuire, Michael A.; Liu, Yaohua Physical Review Letters, Vol. 128, Issue 22 https://doi.org/10.1103/PhysRevLett.128.227201	journal	June 2022
Order from disorder in a kagomé antiferromagnet Chubukov, Andrey Physical Review Letters, Vol. 69, Issue 5 https://doi.org/10.1103/PhysRevLett.69.832	journal	August 1992
Case for a U(1)π Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce2Zr2O7 Smith, E. M.; Benton, O.; Yahne, D. R. Physical Review X, Vol. 12, Issue 2 https://doi.org/10.1103/PhysRevX.12.021015	journal	April 2022
Magnetic pyrochlore oxides Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E. Reviews of Modern Physics, Vol. 82, Issue 1 https://doi.org/10.1103/RevModPhys.82.53	journal	January 2010
VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data Momma, Koichi; Izumi, Fujio Journal of Applied Crystallography, Vol. 44, Issue 6 https://doi.org/10.1107/S0021889811038970	journal	October 2011
Mesoscopic Phase Coherence in a Quantum Spin Fluid Xu, G.; Broholm, C.; Soh, Y. -A. Science, Vol. 317, Issue 5841 https://doi.org/10.1126/science.1143831	journal	August 2007
Orbital-exchange and fractional quantum number excitations in an f-electron metal, Yb ₂ Pt ₂ Pb Wu, L. S.; Gannon, W. J.; Zaliznyak, I. A. Science, Vol. 352, Issue 6290 https://doi.org/10.1126/science.aaf0981	journal	June 2016
Neutron scattering in the proximate quantum spin liquid α-RuCl ₃ Banerjee, Arnab; Yan, Jiaqiang; Knolle, Johannes Science, Vol. 356, Issue 6342 https://doi.org/10.1126/science.aah6015	journal	June 2017
A Field Guide to Spin Liquids Knolle, J.; Moessner, R. Annual Review of Condensed Matter Physics, Vol. 10, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031218-013401	journal	March 2019
Pressure-Tuned Interactions in Frustrated Magnets: Pathway to Quantum Spin Liquids? Biesner, Tobias; Uykur, Ece Crystals, Vol. 10, Issue 1 https://doi.org/10.3390/cryst10010004	journal	December 2019
Crystallography of some double sulfates and chromates McMurdie, H. F.; Morris, M. C.; deGroot, J. Journal of Research of the National Bureau of Standards Section A: Physics and Chemistry, Vol. 75A, Issue 5 https://doi.org/10.6028/jres.075A.034	journal	September 1971
Ground State Selection and Spin-Liquid Behaviour in the Classical Heisenberg Model on the Breathing Pyrochlore Lattice Benton, Owen; Shannon, Nic Journal of the Physical Society of Japan, Vol. 84, Issue 10 https://doi.org/10.7566/JPSJ.84.104710	journal	October 2015

Similar Records

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO₄

Journal Article · Sun Dec 04 19:00:00 EST 2016 · Nature Physics · OSTI ID:1361300

Spin liquid state in the disordered triangular lattice Sc₂Ga₂CuO₇ revealed by NMR

Journal Article · Sun Apr 17 20:00:00 EDT 2016 · Physical Review B · OSTI ID:1259550

Related Subjects

75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
Antiferromagnets
Condensed Matter
Materials and Applied Physics
Frustrated magnetism
Inelastic neutron scattering
Spin liquid

Continuous Spin Excitations in the Three-Dimensional Frustrated Magnet K2Ni2⁢(SO4)3

Citation Formats

References (68)

Similar Records

Related Subjects

Continuous Spin Excitations in the Three-Dimensional Frustrated Magnet K₂Ni₂⁢(SO₄)₃