Magnetic field effects in an octupolar quantum spin liquid candidate

Gao, Bin; Chen, Tong; Yan, Han; Duan, Chunruo; Huang, Chien-Lung; Yao, Xu Ping; Ye, Feng; Balz, Christian; Stewart, J. Ross; Nakajima, Kenji; Ohira-Kawamura, Seiko; Xu, Guangyong; Xu, Xianghan; Cheong, Sang-Wook; Morosan, Emilia; Nevidomskyy, Andriy H.; Chen, Gang; Dai, Pengcheng

doi:10.1103/physrevb.106.094425

Title: Magnetic field effects in an octupolar quantum spin liquid candidate

Abstract

Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an octupole QSL, the spin waves carry octupole moments that do not couple, in the leading order, to an external magnetic field or to neutron moments but will contribute to the field dependence of the heat capacity. Here, in this study, we use neutron scattering to show that the application of a large external magnetic field to Ce₂Zr₂O₇, an octupolar QSL candidate, induces an Anderson-Higgs transition by condensing the spinons into a static ferromagnetic ordered state with octupolar spin waves invisible to neutrons but contributing to the heat capacity. Our theoretical calculations also provide a microscopic, qualitative understanding for the presence of octupole scattering at large wave vectors in Ce₂Sn₂O₇ pyrochlore, and its absence in Ce₂Zr₂O₇. Therefore, our resultsmore »« less

Authors:

^[1]; Chen, Tong ^[1];

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

^[1];

^[2];

^[3];

^[4]; Stewart, J. Ross ^[4];

^[5];

^[5]; Xu, Guangyong ^[6]; Xu, Xianghan ^[7]; Cheong, Sang-Wook ^[7]; Morosan, Emilia ^[1]; Nevidomskyy, Andriy H. ^[1];

^[2];

^[1]

Rice Univ., Houston, TX (United States)
Univ. of Hong Kong, Pokfulam (Hong Kong)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
Science and Technology Facilities Council (STFC) (United Kingdom). Rutherford Appleton Lab. (RAL)
Japan Proton Accelerator Research Complex (J-PARC) (Japan)
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
Rutgers Univ., Piscataway, NJ (United States)

Publication Date:: Thu Sep 22 00:00:00 EDT 2022

Research Org.:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Rice Univ., Houston, TX (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); Robert A. Welch Foundation; Research Grants Council (RGC); Gordon and Betty Moore Foundation

OSTI Identifier:: 1890280

Alternate Identifier(s):: OSTI ID: 2281379; OSTI ID: 2281564

Grant/Contract Number:: AC05-00OR22725; SC0012311; SC0019503; FG02-07ER46382; DMR-1917511; C-1839; C-2114; 17306520; GBMF10104

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review. B

Additional Journal Information:: Journal Volume: 106; Journal Issue: 9; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; fractionalization; frustrated magnetism; quantum spin liquid; quasiparticles & collective excitations; pyrochlores; neutron scattering

Citation Formats


                    Gao, Bin, Chen, Tong, Yan, Han, Duan, Chunruo, Huang, Chien-Lung, Yao, Xu Ping, Ye, Feng, Balz, Christian, Stewart, J. Ross, Nakajima, Kenji, Ohira-Kawamura, Seiko, Xu, Guangyong, Xu, Xianghan, Cheong, Sang-Wook, Morosan, Emilia, Nevidomskyy, Andriy H., Chen, Gang, and Dai, Pengcheng. Magnetic field effects in an octupolar quantum spin liquid candidate.  United States: N. p., 2022. 
Web.  doi:10.1103/physrevb.106.094425.

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                    Gao, Bin, Chen, Tong, Yan, Han, Duan, Chunruo, Huang, Chien-Lung, Yao, Xu Ping, Ye, Feng, Balz, Christian, Stewart, J. Ross, Nakajima, Kenji, Ohira-Kawamura, Seiko, Xu, Guangyong, Xu, Xianghan, Cheong, Sang-Wook, Morosan, Emilia, Nevidomskyy, Andriy H., Chen, Gang, & Dai, Pengcheng. Magnetic field effects in an octupolar quantum spin liquid candidate.  United States.  https://doi.org/10.1103/physrevb.106.094425

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                    Gao, Bin, Chen, Tong, Yan, Han, Duan, Chunruo, Huang, Chien-Lung, Yao, Xu Ping, Ye, Feng, Balz, Christian, Stewart, J. Ross, Nakajima, Kenji, Ohira-Kawamura, Seiko, Xu, Guangyong, Xu, Xianghan, Cheong, Sang-Wook, Morosan, Emilia, Nevidomskyy, Andriy H., Chen, Gang, and Dai, Pengcheng. Thu .  
"Magnetic field effects in an octupolar quantum spin liquid candidate".  United States.  https://doi.org/10.1103/physrevb.106.094425.  https://www.osti.gov/servlets/purl/1890280.

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@article{osti_1890280,

  title        = {Magnetic field effects in an octupolar quantum spin liquid candidate},

  author       = {Gao, Bin and Chen, Tong and Yan, Han and Duan, Chunruo and Huang, Chien-Lung and Yao, Xu Ping and Ye, Feng and Balz, Christian and Stewart, J. Ross and Nakajima, Kenji and Ohira-Kawamura, Seiko and Xu, Guangyong and Xu, Xianghan and Cheong, Sang-Wook and Morosan, Emilia and Nevidomskyy, Andriy H. and Chen, Gang and Dai, Pengcheng},

  abstractNote = {Quantum spin liquid (QSL) is a disordered state of quantum-mechanically entangled spins commonly arising from frustrated magnetic dipolar interactions. However, QSL in some pyrochlore magnets can also come from frustrated magnetic octupolar interactions. Although the key signature for both dipolar and octupolar interaction-driven QSL is the presence of a spin excitation continuum (spinons) arising from the spin quantum number fractionalization, an external magnetic field-induced ferromagnetic order will transform the spinons into conventional spin waves in a dipolar QSL. By contrast, in an octupole QSL, the spin waves carry octupole moments that do not couple, in the leading order, to an external magnetic field or to neutron moments but will contribute to the field dependence of the heat capacity. Here, in this study, we use neutron scattering to show that the application of a large external magnetic field to Ce2Zr2O7, an octupolar QSL candidate, induces an Anderson-Higgs transition by condensing the spinons into a static ferromagnetic ordered state with octupolar spin waves invisible to neutrons but contributing to the heat capacity. Our theoretical calculations also provide a microscopic, qualitative understanding for the presence of octupole scattering at large wave vectors in Ce2Sn2O7 pyrochlore, and its absence in Ce2Zr2O7. Therefore, our results identify Ce2Zr2O7 as a strong candidate for an octupolar U(1) QSL, establishing that frustrated magnetic octupolar interactions are responsible for QSL properties in Ce-based pyrochlore magnets.},

  doi          = {10.1103/physrevb.106.094425},

  journal      = {Physical Review. B},

  number       = 9,

  volume       = 106,

  place        = {United States},

  year         = {Thu Sep 22 00:00:00 EDT 2022},

  month        = {Thu Sep 22 00:00:00 EDT 2022}

}

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Title: Magnetic field effects in an octupolar quantum spin liquid candidate

Abstract

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Ground-state phase diagram of dipolar-octupolar pyrochlores journal, September 2020

Sleuthing out exotic quantum spin liquidity in the pyrochlore magnet Ce2Zr2O7 journal, May 2022

Quantum Excitations in Quantum Spin Ice journal, October 2011

LET, a cold neutron multi-disk chopper spectrometer at ISIS journal, May 2011

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4 journal, December 2016

Anisotropic Propagating Excitations and Quadrupolar Effects in Tb 2 Ti 2 O 7 journal, August 2013

Quantum Spin Ices and Topological Phases from Dipolar-Octupolar Doublets on the Pyrochlore Lattice journal, April 2014

Antiferromagnetic spin ice correlations at ( 1 2 , 1 2 , 1 2 ) in the ground state of the pyrochlore magnet Tb 2 Ti 2 O 7 journal, March 2013

Quadrupole order in the frustrated pyrochlore magnet Tb 2 Ti 2 O 7 journal, February 2016

Dirac's “magnetic monopoles” in pyrochlore ice U ( 1 ) spin liquids: Spectrum and classification journal, November 2017

Multiferroicity in spin ice: Towards magnetic crystallography of Tb 2 Ti 2 O 7 in a field journal, June 2015

Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore journal, July 2019

Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet journal, December 2012

Resonating valence bonds: A new kind of insulator? journal, February 1973

Electric dipoles on magnetic monopoles in spin ice journal, January 2012

Generic quantum spin ice journal, September 2012

Spinon Fermi Surface Spin Liquid in a Triangular Lattice Antiferromagnet NaYbSe 2 journal, May 2021

AMATERAS: A Cold-Neutron Disk Chopper Spectrometer journal, January 2011

Candidate Quantum Spin Liquid in the Ce 3 + Pyrochlore Stannate Ce 2 Sn 2 O 7 journal, August 2015

Multipolar interactions in f -electron systems: The paradigm of actinide dioxides journal, June 2009

Magnetic multipoles and correlation shortage in the pyrochlore cerium stannateCe2Sn2O7 journal, April 2020

Frustrated Quantum Rare-Earth Pyrochlores journal, March 2019

Mantid—Data analysis and visualization package for neutron scattering and $μ$ SR experiments
journal, November 2014

Spin Ice, Fractionalization, and Topological Order
journal, March 2012

Dynamically Induced Frustration as a Route to a Quantum Spin Ice State in ${Tb}_{2} {Ti}_{2} O_{7}$ via Virtual Crystal Field Excitations and Quantum Many-Body Effects
journal, April 2007

Implementation of cross correlation for energy discrimination on the time-of-flight spectrometer CORELLI
journal, March 2018

Physical realization of a quantum spin liquid based on a complex frustration mechanism
journal, July 2016

Quantum spin liquids: a review
journal, November 2016

Evidence for a spinon Fermi surface in a triangular-lattice quantum-spin-liquid candidate
journal, December 2016

Experimental Insights into Ground-State Selection of Quantum XY Pyrochlores
journal, March 2018

Quantum Phase Transition in Quantum Spin Liquid Candidate Ce2Zr2O7
dataset, January 2020

Field-Induced Spin-Ice-Like Orders in Spin Liquid ${Tb}_{2} {Ti}_{2} O_{7}$
journal, November 2008

Quantum spin liquid states
journal, April 2017

Seeing the light: Experimental signatures of emergent electromagnetism in a quantum spin ice
journal, August 2012

Dipolar Spin Correlations in Classical Pyrochlore Magnets
journal, October 2004

Spectral periodicity of the spinon continuum in quantum spin ice
journal, August 2017

Quasiparticle Breakdown and Spin Hamiltonian of the Frustrated Quantum Pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$ in a Magnetic Field
journal, August 2017

Field-Induced Order and Spin Waves in the Pyrochlore Antiferromagnet ${Tb}_{2} {Ti}_{2} O_{7}$
journal, May 2006

Pyrochlore U(1) spin liquid of mixed-symmetry enrichments in magnetic fields
journal, March 2020

Spin Correlations in ${Ho}_{2} {Ti}_{2} O_{7}$ : A Dipolar Spin Ice System
journal, July 2001

A quantum liquid of magnetic octupoles on the pyrochlore lattice
journal, March 2020

Power-Law Spin Correlations in the Pyrochlore Antiferromagnet ${Tb}_{2} {Ti}_{2} O_{7}$
journal, July 2012

Quantum Spin Ice Dynamics in the Dipole-Octupole Pyrochlore Magnet ${Ce}_{2} {Zr}_{2} O_{7}$
journal, May 2019

Expanding Lorentz and spectrum corrections to large volumes of reciprocal space for single-crystal time-of-flight neutron diffraction
journal, March 2016

Symmetry enriched U(1) topological orders for dipole-octupole doublets on a pyrochlore lattice
journal, January 2017

Coulombic Quantum Liquids in Spin- $1 / 2$ Pyrochlores
journal, January 2012

Spin liquids in frustrated magnets
journal, March 2010

“Magnetic monopole” condensation of the pyrochlore ice U(1) quantum spin liquid: Application to $\Pr_{2} {Ir}_{2} O_{7}$ and ${Yb}_{2} {Ti}_{2} O_{7}$
journal, November 2016

Quantum spin liquids
journal, January 2020

Magnetic pyrochlore oxides
journal, January 2010

Case for a U(1)π Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce2Zr2O7
journal, April 2022

Pyrochlore photons: The $U (1)$ spin liquid in a $S = \frac{1}{2}$ three-dimensional frustrated magnet
journal, February 2004

Distinguishing dipolar and octupolar quantum spin ices using contrasting magnetostriction signatures
journal, June 2020

Ground-state phase diagram of dipolar-octupolar pyrochlores
journal, September 2020

Sleuthing out exotic quantum spin liquidity in the pyrochlore magnet Ce2Zr2O7
journal, May 2022

Quantum Excitations in Quantum Spin Ice
journal, October 2011

LET, a cold neutron multi-disk chopper spectrometer at ISIS
journal, May 2011

Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
journal, December 2016

Anisotropic Propagating Excitations and Quadrupolar Effects in ${Tb}_{2} {Ti}_{2} O_{7}$
journal, August 2013

Quantum Spin Ices and Topological Phases from Dipolar-Octupolar Doublets on the Pyrochlore Lattice
journal, April 2014

Antiferromagnetic spin ice correlations at ( $\frac{1}{2}$ , $\frac{1}{2}$ , $\frac{1}{2}$ ) in the ground state of the pyrochlore magnet Tb $_{2}$ Ti $_{2}$ O $_{7}$
journal, March 2013

Quadrupole order in the frustrated pyrochlore magnet Tb ₂ Ti ₂ O ₇
journal, February 2016

Dirac's “magnetic monopoles” in pyrochlore ice $U (1)$ spin liquids: Spectrum and classification
journal, November 2017

Multiferroicity in spin ice: Towards magnetic crystallography of ${Tb}_{2} {Ti}_{2} O_{7}$ in a field
journal, June 2015

Experimental signatures of a three-dimensional quantum spin liquid in effective spin-1/2 Ce2Zr2O7 pyrochlore
journal, July 2019

Fractionalized excitations in the spin-liquid state of a kagome-lattice antiferromagnet
journal, December 2012

Resonating valence bonds: A new kind of insulator?
journal, February 1973

Electric dipoles on magnetic monopoles in spin ice
journal, January 2012

Generic quantum spin ice
journal, September 2012

Spinon Fermi Surface Spin Liquid in a Triangular Lattice Antiferromagnet ${NaYbSe}_{2}$
journal, May 2021

AMATERAS: A Cold-Neutron Disk Chopper Spectrometer
journal, January 2011

Candidate Quantum Spin Liquid in the ${Ce}^{3 +}$ Pyrochlore Stannate ${Ce}_{2} {Sn}_{2} O_{7}$
journal, August 2015

Multipolar interactions in $f$ -electron systems: The paradigm of actinide dioxides
journal, June 2009

Magnetic multipoles and correlation shortage in the pyrochlore cerium stannateCe2Sn2O7
journal, April 2020

Frustrated Quantum Rare-Earth Pyrochlores
journal, March 2019