Continuum of quantum fluctuations in a three-dimensional S=1 Heisenberg magnet
Abstract
Conventional crystalline magnets are characterized by symmetry breaking and normal modes of excitation called magnons, with quantized angular momentum $$\hbar$$. Neutron scattering correspondingly features extra magnetic Bragg diffraction at low temperatures and dispersive inelastic scattering associated with single magnon creation and annihilation. Exceptions are anticipated in so-called quantum spin liquids, as exemplified by the one-dimensional spin-1/2 chain, which has no magnetic order and where magnons accordingly fractionalize into spinons with angular momentum $$\hbar$$/2. This is spectacularly revealed by a continuum of inelastic neutron scattering associated with two-spinon processes. Here, we report evidence for these key features of a quantum spin liquid in the three-dimensional antiferromagnet NaCaNi2F7. We show that despite the complication of random Na1+–Ca2+ charge disorder, NaCaNi2F7 is an almost ideal realization of the spin-1 antiferromagnetic Heisenberg model on a pyrochlore lattice. Magnetic Bragg diffraction is absent and 90% of the neutron spectral weight forms a continuum of magnetic scattering with low-energy pinch points, indicating NaCaNi2F7 is in a Coulomb-like phase. Our results demonstrate that disorder can act to freeze only the lowest-energy magnetic degrees of freedom; at higher energies, a magnetic excitation continuum characteristic of fractionalized excitations persists.
- Authors:
-
[1];
- Johns Hopkins Univ., Baltimore, MD (United States)
- Princeton Univ., NJ (United States). Dept. of Chemistry
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research; Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering
- National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Johns Hopkins Univ., Baltimore, MD (United States); National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Center for Neutron Research; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1559715
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Physics
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 1; Journal ID: ISSN 1745-2473
- Publisher:
- Nature Publishing Group (NPG)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Plumb, K. W., Changlani, Hitesh J., Scheie, A., Zhang, Shu, Krizan, J. W., Rodriguez-Rivera, J. A., Qiu, Yiming, Winn, B., Cava, R. J., and Broholm, C. L. Continuum of quantum fluctuations in a three-dimensional S=1 Heisenberg magnet. United States: N. p., 2018.
Web. doi:10.1038/s41567-018-0317-3.
Plumb, K. W., Changlani, Hitesh J., Scheie, A., Zhang, Shu, Krizan, J. W., Rodriguez-Rivera, J. A., Qiu, Yiming, Winn, B., Cava, R. J., & Broholm, C. L. Continuum of quantum fluctuations in a three-dimensional S=1 Heisenberg magnet. United States. https://doi.org/10.1038/s41567-018-0317-3
Plumb, K. W., Changlani, Hitesh J., Scheie, A., Zhang, Shu, Krizan, J. W., Rodriguez-Rivera, J. A., Qiu, Yiming, Winn, B., Cava, R. J., and Broholm, C. L. Mon .
"Continuum of quantum fluctuations in a three-dimensional S=1 Heisenberg magnet". United States. https://doi.org/10.1038/s41567-018-0317-3. https://www.osti.gov/servlets/purl/1559715.
@article{osti_1559715,
title = {Continuum of quantum fluctuations in a three-dimensional S=1 Heisenberg magnet},
author = {Plumb, K. W. and Changlani, Hitesh J. and Scheie, A. and Zhang, Shu and Krizan, J. W. and Rodriguez-Rivera, J. A. and Qiu, Yiming and Winn, B. and Cava, R. J. and Broholm, C. L.},
abstractNote = {Conventional crystalline magnets are characterized by symmetry breaking and normal modes of excitation called magnons, with quantized angular momentum $\hbar$. Neutron scattering correspondingly features extra magnetic Bragg diffraction at low temperatures and dispersive inelastic scattering associated with single magnon creation and annihilation. Exceptions are anticipated in so-called quantum spin liquids, as exemplified by the one-dimensional spin-1/2 chain, which has no magnetic order and where magnons accordingly fractionalize into spinons with angular momentum $\hbar$/2. This is spectacularly revealed by a continuum of inelastic neutron scattering associated with two-spinon processes. Here, we report evidence for these key features of a quantum spin liquid in the three-dimensional antiferromagnet NaCaNi2F7. We show that despite the complication of random Na1+–Ca2+ charge disorder, NaCaNi2F7 is an almost ideal realization of the spin-1 antiferromagnetic Heisenberg model on a pyrochlore lattice. Magnetic Bragg diffraction is absent and 90% of the neutron spectral weight forms a continuum of magnetic scattering with low-energy pinch points, indicating NaCaNi2F7 is in a Coulomb-like phase. Our results demonstrate that disorder can act to freeze only the lowest-energy magnetic degrees of freedom; at higher energies, a magnetic excitation continuum characteristic of fractionalized excitations persists.},
doi = {10.1038/s41567-018-0317-3},
journal = {Nature Physics},
number = 1,
volume = 15,
place = {United States},
year = {Mon Oct 29 00:00:00 EDT 2018},
month = {Mon Oct 29 00:00:00 EDT 2018}
}
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Works referenced in this record:
Insulating spin glasses
journal, March 1979
- Villain, Jacques
- Zeitschrift f�r Physik B Condensed Matter and Quanta, Vol. 33, Issue 1
Molecular Spin Resonance in the Geometrically Frustrated Magnet by Inelastic Neutron Scattering
journal, October 2008
- Tomiyasu, K.; Suzuki, H.; Toki, M.
- Physical Review Letters, Vol. 101, Issue 17
Valence-Bond Crystal and Anisotropic Excitation Spectrum on 3-Dimensionally Frustrated Pyrochlore
journal, December 1998
- Isoda, Makoto; Mori, Shigeyoshi
- Journal of the Physical Society of Japan, Vol. 67, Issue 12
Order by Distortion and String Modes in Pyrochlore Antiferromagnets
journal, January 2002
- Tchernyshyov, Oleg; Moessner, R.; Sondhi, S. L.
- Physical Review Letters, Vol. 88, Issue 6
Mantid—Data analysis and visualization package for neutron scattering and SR experiments
journal, November 2014
- Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
- Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764
Spin Disorder on a Triangular Lattice
journal, September 2005
- Nakatsuji, S.
- Science, Vol. 309, Issue 5741
Frustrated order by disorder: The pyrochlore anti-ferromagnet with bond disorder
journal, December 2001
- Bellier-Castella, L.; Gingras, M. Jp; Holdsworth, P. Cw
- Canadian Journal of Physics, Vol. 79, Issue 11-12
Halperin-Saslow modes as the origin of the low-temperature anomaly in
journal, April 2009
- Podolsky, Daniel; Kim, Yong Baek
- Physical Review B, Vol. 79, Issue 14
Order-by-disorder and spiral spin-liquid in frustrated diamond-lattice antiferromagnets
journal, May 2007
- Bergman, Doron; Alicea, Jason; Gull, Emanuel
- Nature Physics, Vol. 3, Issue 7
Spin-Ice State of the Quantum Heisenberg Antiferromagnet on the Pyrochlore Lattice
journal, April 2016
- Huang, Yuan; Chen, Kun; Deng, Youjin
- Physical Review Letters, Vol. 116, Issue 17
Statics and Dynamics of Incommensurate Spin Order in a Geometrically Frustrated Antiferromagnet
journal, December 2005
- Chung, J. -H.; Matsuda, M.; Lee, S. -H.
- Physical Review Letters, Vol. 95, Issue 24
Magnetic Coulomb Phase in the Spin Ice Ho2Ti2O7
journal, September 2009
- Fennell, T.; Deen, P. P.; Wildes, A. R.
- Science, Vol. 326, Issue 5951
: A frustrated high-temperature pyrochlore antiferromagnet with
journal, July 2015
- Krizan, J. W.; Cava, R. J.
- Physical Review B, Vol. 92, Issue 1
Spin Freezing in Geometrically Frustrated Antiferromagnets with Weak Disorder
journal, April 2007
- Saunders, T. E.; Chalker, J. T.
- Physical Review Letters, Vol. 98, Issue 15
Sum rules for the frequency spectrum of linear magnetic chains
journal, July 1974
- Hohenberg, P. C.; Brinkman, W. F.
- Physical Review B, Vol. 10, Issue 1
Topological Spin Glass in Diluted Spin Ice
journal, June 2015
- Sen, Arnab; Moessner, R.
- Physical Review Letters, Vol. 114, Issue 24
Low-temperature properties of classical geometrically frustrated antiferromagnets
journal, November 1998
- Moessner, R.; Chalker, J. T.
- Physical Review B, Vol. 58, Issue 18
Pyrochlore Antiferromagnet: A Three-Dimensional Quantum Spin Liquid
journal, March 1998
- Canals, B.; Lacroix, C.
- Physical Review Letters, Vol. 80, Issue 13
MACS—a new high intensity cold neutron spectrometer at NIST
journal, January 2008
- Rodriguez, J. A.; Adler, D. M.; Brand, P. C.
- Measurement Science and Technology, Vol. 19, Issue 3
Emergent excitations in a geometrically frustrated magnet
journal, August 2002
- Lee, S. -H.; Broholm, C.; Ratcliff, W.
- Nature, Vol. 418, Issue 6900
Liquidlike correlations in single-crystalline Y Mo O : An unconventional spin glass
journal, February 2014
- Silverstein, H. J.; Fritsch, K.; Flicker, F.
- Physical Review B, Vol. 89, Issue 5
Polarized neutron scattering on HYSPEC: the HYbrid SPECtrometer at SNS
journal, June 2017
- Zaliznyak, Igor A.; Savici, Andrei T.; Ovidiu Garlea, V.
- Journal of Physics: Conference Series, Vol. 862
Colloquium : Spontaneous magnon decays
journal, January 2013
- Zhitomirsky, M. E.; Chernyshev, A. L.
- Reviews of Modern Physics, Vol. 85, Issue 1
Hydrodynamic theory of spin waves in spin glasses and other systems with noncollinear spin orientations
journal, September 1977
- Halperin, B. I.; Saslow, W. M.
- Physical Review B, Vol. 16, Issue 5
Dipolar Spin Correlations in Classical Pyrochlore Magnets
journal, October 2004
- Isakov, S. V.; Gregor, K.; Moessner, R.
- Physical Review Letters, Vol. 93, Issue 16
Absent pinch points and emergent clusters: Further neighbor interactions in the pyrochlore Heisenberg antiferromagnet
journal, June 2010
- Conlon, P. H.; Chalker, J. T.
- Physical Review B, Vol. 81, Issue 22
Glassy Statics and Dynamics in the Chemically Ordered Pyrochlore Antiferromagnet
journal, July 1999
- Gardner, J. S.; Gaulin, B. D.; Lee, S. -H.
- Physical Review Letters, Vol. 83, Issue 1
Ordering in the pyrochlore antiferromagnet due to Dzyaloshinsky-Moriya interactions
journal, March 2005
- Elhajal, Maged; Canals, Benjamin; Sunyer, Raimon
- Physical Review B, Vol. 71, Issue 9
Direct Measurement of the Spin Hamiltonian and Observation of Condensation of Magnons in the 2D Frustrated Quantum Magnet
journal, March 2002
- Coldea, R.; Tennant, D. A.; Habicht, K.
- Physical Review Letters, Vol. 88, Issue 13
Static and dynamic -like short-range order in a frustrated magnet with exchange disorder
journal, January 2016
- Ross, K. A.; Krizan, J. W.; Rodriguez-Rivera, J. A.
- Physical Review B, Vol. 93, Issue 1
Properties of a Classical Spin Liquid: The Heisenberg Pyrochlore Antiferromagnet
journal, March 1998
- Moessner, R.; Chalker, J. T.
- Physical Review Letters, Vol. 80, Issue 13
: A single-crystal high-temperature pyrochlore antiferromagnet
journal, June 2014
- Krizan, J. W.; Cava, R. J.
- Physical Review B, Vol. 89, Issue 21
Less than 50% sublattice polarization in an insulating kagomé antiferromagnet at
journal, October 1997
- Lee, S. -H.; Broholm, C.; Collins, M. F.
- Physical Review B, Vol. 56, Issue 13
Power-law spin correlations in pyrochlore antiferromagnets
journal, January 2005
- Henley, C. L.
- Physical Review B, Vol. 71, Issue 1
Dissociation of spin objects in geometrically frustrated
journal, July 2004
- Kamazawa, K.; Park, S.; Lee, S. -H.
- Physical Review B, Vol. 70, Issue 2
NaSrMn 2 F 7 , NaCaFe 2 F 7 , and NaSrFe 2 F 7 : novel single crystal pyrochlore antiferromagnets
journal, November 2016
- Sanders, M. B.; Krizan, J. W.; Plumb, K. W.
- Journal of Physics: Condensed Matter, Vol. 29, Issue 4
Ordering by quantum fluctuations in a strongly frustrated Heisenberg antiferromagnet
journal, April 1991
- Harris, A. B.; Berlinsky, A. J.; Bruder, C.
- Journal of Applied Physics, Vol. 69, Issue 8
The “Coulomb Phase” in Frustrated Systems
journal, August 2010
- Henley, Christopher L.
- Annual Review of Condensed Matter Physics, Vol. 1, Issue 1
Spin Dynamics in Pyrochlore Heisenberg Antiferromagnets
journal, June 2009
- Conlon, P. H.; Chalker, J. T.
- Physical Review Letters, Vol. 102, Issue 23
Frustrated order by disorder: The pyrochlore anti-ferromagnet with bond disorder
journal, January 2001
- Bellier-Castella, L.; Gingras, M. J. P.; Holdsworth, P. C. W.
- Canadian Journal of Physics, Vol. 79, Issue 11-12
Polarized neutron scattering on HYSPEC: the HYbrid SPECtrometer at SNS
text, January 2016
- Zaliznyak, Igor A.; Savici, Andrei T.; Garlea, V. Ovidiu
- arXiv
Order by distortion and string modes in pyrochlore antiferromagnet
text, January 2001
- Tchernyshyov, O.; Moessner, R.; Sondhi, S. L.
- arXiv
Ordering in the pyrochlore antiferromagnet due to Dzyaloshinsky-Moriya interactions
text, January 2005
- Elhajal, M.; Canals, B.; Borrell, R. Sunyer i.
- arXiv
Order by disorder and spiral spin liquid in frustrated diamond lattice antiferromagnets
text, January 2006
- Bergman, Doron; Alicea, Jason; Gull, Emanuel
- arXiv
Exchange Monte Carlo Method and Application to Spin Glass Simulations
text, January 1995
- Hukushima, Koji; Nemoto, Koji
- arXiv
Properties of a classical spin liquid: the Heisenberg pyrochlore antiferromagnet
text, January 1997
- Moessner, R.; Chalker, J. T.
- arXiv
Low-temperature properties of classical, geometrically frustrated antiferromagnets
text, January 1998
- Moessner, R.; Chalker, J. T.
- arXiv
Pyrochlore Antiferromagnet: A Three-Dimensional Quantum Spin Liquid
text, January 1998
- Canals, Benjamin; Lacroix, Claudine
- arXiv
Mean-field approach to magnetic ordering in highly frustrated pyrochlores
journal, January 1991
- Reimers, J. N.; Berlinsky, A. J.; Shi, A. -C.
- Physical Review B, Vol. 43, Issue 1
Quantum spin liquid: The Heisenberg antiferromagnet on the three-dimensional pyrochlore lattice
journal, January 2000
- Canals, Benjamin; Lacroix, Claudine
- Physical Review B, Vol. 61, Issue 2
Quantum dimer models and effective Hamiltonians on the pyrochlore lattice
journal, March 2006
- Moessner, R.; Sondhi, S. L.; Goerbig, M. O.
- Physical Review B, Vol. 73, Issue 9
Partial order from disorder in a classical pyrochlore antiferromagnet
journal, October 2008
- Chern, Gia-Wei; Moessner, R.; Tchernyshyov, O.
- Physical Review B, Vol. 78, Issue 14
Entropy Balance and Evidence for Local Spin Singlets in a Kagomé-Like Magnet
journal, March 2000
- Ramirez, A. P.; Hessen, B.; Winklemann, M.
- Physical Review Letters, Vol. 84, Issue 13
Exchange Monte Carlo Method and Application to Spin Glass Simulations
journal, June 1996
- Hukushima, Koji; Nemoto, Koji
- Journal of the Physical Society of Japan, Vol. 65, Issue 6
A single crystal high-temperature pyrochlore antiferromagnet
text, January 2014
- Krizan, J. W.; Cava, R. J.
- arXiv
Mantid - Data Analysis and Visualization Package for Neutron Scattering and $μSR$ Experiments
text, January 2014
- Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
- arXiv
Spin Freezing in Geometrically Frustrated Antiferromagnets with Weak Disorder
text, January 2006
- Saunders, T. E.; Chalker, J. T.
- arXiv
Properties of a classical spin liquid: the Heisenberg pyrochlore antiferromagnet
text, January 1997
- Moessner, R.; Chalker, J. T.
- arXiv
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- Ghosh, Pratyay; Iqbal, Yasir; Müller, Tobias
- npj Quantum Materials, Vol. 4, Issue 1
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journal, October 2018
- Fennell, T.; Harris, M. J.; Calder, S.
- Nature Physics, Vol. 15, Issue 1
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journal, July 2019
- Gao, Bin; Chen, Tong; Tam, David W.
- Nature Physics, Vol. 15, Issue 10
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journal, March 2020
- Sibille, Romain; Gauthier, Nicolas; Lhotel, Elsa
- Nature Physics
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journal, July 2019
- Müller, Patrick; Lohmann, Andre; Richter, Johannes
- Physical Review B, Vol. 100, Issue 2
Goldstone modes in the emergent gauge fields of a frustrated magnet
journal, January 2020
- Garratt, S. J.; Chalker, J. T.
- Physical Review B, Vol. 101, Issue 2
Dynamical Structure Factor of the Three-Dimensional Quantum Spin Liquid Candidate
journal, April 2019
- Zhang, Shu; Changlani, Hitesh J.; Plumb, Kemp W.
- Physical Review Letters, Vol. 122, Issue 16
Breathing chromium spinels: a showcase for a variety of pyrochlore Heisenberg Hamiltonians
text, January 2019
- Ghosh, Pratyay; Iqbal, Yasir; Müller, Tobias
- Freie Universität Berlin
Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore
text, January 2019
- Gao, Bin; Chen, Tong; Tam, David W.
- arXiv
A quantum liquid of magnetic octupoles on the pyrochlore lattice
text, January 2019
- Sibille, Romain; Gauthier, Nicolas; Lhotel, Elsa
- arXiv