Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb2Si2O7

Hester, Gavin; Nair, H. S.; Reeder, T.; Yahne, D. R.; DeLazzer, T. N.; Berges, L.; Ziat, D.; Neilson, J. R.; Aczel, Adam A.; Sala, Gabriele; Quilliam, J. A.; Ross, K. A.

doi:10.1103/PhysRevLett.123.027201

Title: Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: ${Yb}_{2} {Si}_{2} O_{7}$

Abstract

The quantum dimer magnet (QDM) is the canonical example of quantum magnetism. The QDM state consists of entangled nearest-neighbor spin dimers and often exhibits a field-induced triplon Bose-Einstein condensate (BEC) phase. We report on a new QDM in the strongly spin-orbit coupled, distorted honeycomb-lattice material Yb₂Si₂O₇. Our single crystal neutron scattering, specific heat, and ultrasound velocity measurements reveal a gapped singlet ground state at zero field with sharp, dispersive excitations. We find a field-induced magnetically ordered phase reminiscent of a BEC phase, with exceptionally low critical fields of H_c1 ~ 0.4 and H_c2 ~ 1.4 T. Using inelastic neutron scattering in an applied magnetic field we observe a Goldstone mode (gapless to within δE=0.037 meV) that persists throughout the entire field-induced magnetically ordered phase, suggestive of the spontaneous breaking of U(1) symmetry expected for a triplon BEC. However, in contrast to other well-known cases of this phase, the high-field (μ₀H≥1.2 T) part of the phase diagram in Yb₂Si₂O₇ is interrupted by an unusual regime signaled by a change in the field dependence of the ultrasound velocity and magnetization, as well as the disappearance of a sharp anomaly in the specific heat. Finally, these measurements raise the question of how anisotropymore »« less

Authors:

Hester, Gavin ^[1]; Nair, H. S. ^[1]; Reeder, T. ^[1]; Yahne, D. R. ^[1]; DeLazzer, T. N. ^[1]; Berges, L. ^[2]; Ziat, D. ^[2]; Neilson, J. R. ^[1];

^[3];

^[3]; Quilliam, J. A. ^[2]; Ross, K. A. ^[4]

Colorado State Univ., Fort Collins, CO (United States)
Univ. of Sherbrooke, QB (Canada)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Colorado State Univ., Fort Collins, CO (United States); Canadian Inst. for Advanced Research (CIFAR), Toronto, ON (United States)

Publication Date:: Tue Jul 09 00:00:00 EDT 2019

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1607232

Grant/Contract Number:: AC05-00OR22725; DMR-1611217

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review Letters

Additional Journal Information:: Journal Volume: 123; Journal Issue: 2; Journal ID: ISSN 0031-9007

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; antiferromagnetism; critical field; exchange interaction; Goldstone bosons; hard-core bosons; paramagnetism; phase diagrams; triplon

Citation Formats


                    Hester, Gavin, Nair, H. S., Reeder, T., Yahne, D. R., DeLazzer, T. N., Berges, L., Ziat, D., Neilson, J. R., Aczel, Adam A., Sala, Gabriele, Quilliam, J. A., and Ross, K. A. Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb2Si2O7.  United States: N. p., 2019. 
Web.  doi:10.1103/PhysRevLett.123.027201.

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                    Hester, Gavin, Nair, H. S., Reeder, T., Yahne, D. R., DeLazzer, T. N., Berges, L., Ziat, D., Neilson, J. R., Aczel, Adam A., Sala, Gabriele, Quilliam, J. A., & Ross, K. A. Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb2Si2O7.  United States.  https://doi.org/10.1103/PhysRevLett.123.027201

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                    Hester, Gavin, Nair, H. S., Reeder, T., Yahne, D. R., DeLazzer, T. N., Berges, L., Ziat, D., Neilson, J. R., Aczel, Adam A., Sala, Gabriele, Quilliam, J. A., and Ross, K. A. Tue .  
"Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb2Si2O7".  United States.  https://doi.org/10.1103/PhysRevLett.123.027201.  https://www.osti.gov/servlets/purl/1607232.

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@article{osti_1607232,

  title        = {Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb2Si2O7},

  author       = {Hester, Gavin and Nair, H. S. and Reeder, T. and Yahne, D. R. and DeLazzer, T. N. and Berges, L. and Ziat, D. and Neilson, J. R. and Aczel, Adam A. and Sala, Gabriele and Quilliam, J. A. and Ross, K. A.},

  abstractNote = {The quantum dimer magnet (QDM) is the canonical example of quantum magnetism. The QDM state consists of entangled nearest-neighbor spin dimers and often exhibits a field-induced triplon Bose-Einstein condensate (BEC) phase. We report on a new QDM in the strongly spin-orbit coupled, distorted honeycomb-lattice material Yb2Si2O7. Our single crystal neutron scattering, specific heat, and ultrasound velocity measurements reveal a gapped singlet ground state at zero field with sharp, dispersive excitations. We find a field-induced magnetically ordered phase reminiscent of a BEC phase, with exceptionally low critical fields of Hc1 ~ 0.4 and Hc2 ~ 1.4 T. Using inelastic neutron scattering in an applied magnetic field we observe a Goldstone mode (gapless to within δE=0.037 meV) that persists throughout the entire field-induced magnetically ordered phase, suggestive of the spontaneous breaking of U(1) symmetry expected for a triplon BEC. However, in contrast to other well-known cases of this phase, the high-field (μ0H≥1.2 T) part of the phase diagram in Yb2Si2O7 is interrupted by an unusual regime signaled by a change in the field dependence of the ultrasound velocity and magnetization, as well as the disappearance of a sharp anomaly in the specific heat. Finally, these measurements raise the question of how anisotropy in strongly spin-orbit coupled materials modifies the field induced phases of QDMs.},

  doi          = {10.1103/PhysRevLett.123.027201},

  journal      = {Physical Review Letters},

  number       = 2,

  volume       = 123,

  place        = {United States},

  year         = {Tue Jul 09 00:00:00 EDT 2019},

  month        = {Tue Jul 09 00:00:00 EDT 2019}

}

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FIG. 1: a) Crystal structure of Yb₂Si₂O₇ viewed along the c-axis, where Yb atoms are light green and form a distorted honeycomb lattice, Si atoms are blue, and O atoms are red [27]. Intradimer and interdimer bond lengths are shown (3% anisotropy), and J_intra and J_inter exchange tensors are labeled.more »

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Works referencing / citing this record:

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Europium mixed-valence, long-range magnetic order, and dynamic magnetic response in ${EuCu}_{2} {(Si}_{x} {Ge}_{1 - x})_{2}$

Journal Article Nemkovski, Krill S. ; Kozlenko, D. P. ; Alekseev, Pavel A. ; ... - Physical Review B

In mixed-valence or heavy-fermion systems, the hybridization between local f orbitals and conduction band states can cause the suppression of long-range magnetic order, which competes with strong spin uctuations. Ce- and Yb-based systems have been found to exhibit fascinating physical properties (heavy-fermion superconductivity, non-Fermi-liquid states, etc.) when tuned to the vicinity of magnetic quantum critical points by use of various external control parameters (temperature, magnetic eld, chemical composition). Recently, similar effects (mixed-valence, Kondo uctuations, heavy Fermi liquid) have been reported to exist in some Eu-based compounds. Unlike Ce (Yb), Eu has a multiple electron (hole) occupancy of its 4f shell,more »« less
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https://doi.org/10.1103/PhysRevB.94.195101

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Title: Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: Yb 2 Si 2 O 7

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Double-slit photoelectron interference in strong-field ionization of the neon dimer journal, January 2019

Thermodynamics and spin gap of the Heisenberg ladder calculated by the look-ahead Lanczos algorithm journal, November 1994

Crystal Growth of Quantum Magnets in the Rare-Earth Pyrosilicate Family R2Si2O7 (R = Yb, Er) Using the Optical Floating Zone Method journal, April 2019

Frustration and anisotropic exchange in ytterbium magnets with edge-shared octahedra journal, August 2018

Magnetoelastic coupling within a Landau model of phase transitions: Application to the frustrated triangular antiferromagnet CsNiCl 3 journal, July 2011

Magnetic-Field-Induced Condensation of Triplons in Han Purple Pigment B a C u S i 2 O 6 journal, August 2004

Ordered magnetic phases of the frustrated spin-dimer compound Ba 3 Mn 2 O 8 journal, June 2008

Bose-Einstein Condensation of S = 1 Nickel Spin Degrees of Freedom in NiCl 2 − 4 SC ( NH 2 ) 2 journal, February 2006

Lead palladium titanate: A room temperature nanoscale multiferroic thin film journal, February 2020

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data journal, October 2011

Thermodynamic and transport properties of the one-dimensional S=12 antiferromagnet Yb4As3 journal, March 2002

Bose–Einstein condensation in magnetic insulators journal, March 2008

Linear spin wave theory for single-Q incommensurate magnetic structures journal, March 2015

Evidence for Gapped Spin-Wave Excitations in the Frustrated Gd 2 Sn 2 O 7 Pyrochlore Antiferromagnet from Low-Temperature Specific Heat Measurements journal, August 2007

Valence Bonds in Random Quantum Magnets: Theory and Application to YbMgGaO 4 journal, July 2018

Studies of the exactly dimerized bilayer Heisenberg model via strong coupling expansions journal, November 2000

Bose-Einstein condensation in quantum magnets journal, May 2014

The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance journal, August 2011

Field-Induced Magnonic Liquid in the 3D Spin-Dimerized Antiferromagnet Sr 3 Cr 2 O 8 journal, April 2016

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magnetoacoustic properties journal, September 2008

Ultrasonics in the two-dimensional dimer spin system YbAl 3 C 3 journal, December 2012

Zigzag Magnetic Order in the Iridium Oxide Na 2 IrO 3 journal, February 2013

Anyons in an exactly solved model and beyond journal, January 2006

Universal dynamic magnetism in Yb pyrochlores with disparate ground states journal, March 2016

DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data journal, November 2009

Thermal Transport and Strong Mass Renormalization in NiCl 2 − 4 SC ( NH 2 ) 2 journal, January 2011

Orbital-exchange and fractional quantum number excitations in an f-electron metal, Yb 2 Pt 2 Pb journal, June 2016

Bose-Einstein condensation of triplons in Ba 3 Cr 2 O 8 journal, March 2009

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

Spin Gap State of S = 1/2 Heisenberg Antiferromagnet YbAl 3 C 3 journal, December 2007

Field-Induced Bose-Einstein Condensation of Triplons up to 8 K in Sr 3 Cr 2 O 8 journal, November 2009

Quantum Excitations in Quantum Spin Ice journal, October 2011

Polymorphism and crystal data of the rare-earth disilicates of type R.E.2Si2O7 journal, May 1970

The crystal structures of the rare earth pyrosilicates journal, May 1970

Singlet-triplet crossover in the two-dimensional dimer spin system YbAl3C3 journal, June 2013

Quantum Melting of Spin Ice: Emergent Cooperative Quadrupole and Chirality journal, July 2010

Anisotropic Exchange within Decoupled Tetrahedra in the Quantum Breathing Pyrochlore Ba 3 Yb 2 Zn 5 O 11 journal, June 2016

Effect of different resumption strategies to flatten the potential COVID-19 outbreaks amid society reopens: a modeling study in China journal, March 2021

Kitaev materials beyond iridates: Order by quantum disorder and Weyl magnons in rare-earth double perovskites journal, February 2017

Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets journal, May 2014

Quantum spin state in the rare-earth compound YbAl 3 C 3 journal, April 2012

Double-slit photoelectron interference in strong-field ionization of the neon dimer other, January 2019

Spin-Singlet Ground State in the Two-Dimensional Frustrated Triangular Lattice: YbAl 3 C 3 journal, May 2008

Field-induced long-range magnetic order in the spin-singlet ground-state system YbAl 3 C 3 : Neutron diffraction study journal, June 2013

Rare-earth arsenides journal, September 1970

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models journal, January 2009

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3 journal, May 2015

Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for the honeycomb-lattice iridates A 2 IrO 3 journal, July 2015

Double-slit photoelectron interference in strong-field ionization of the neon dimer text, January 2019

Bose-Einstein Condensation in Magnetic Insulators text, January 2007

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magneto-acoustic properties text, January 2008

Quantum Melting of Spin Ice: Emergent Cooperative Quadrupole and Chirality text, January 2009

Singlet-triplet Crossover in the Two-dimensional Dimer Spin System YbAl3C3 text, January 2013

Linear spin wave theory for single-Q incommensurate magnetic structures text, January 2014

Orbital-Exchange and Fractional Quantum Number Excitations in an f-electron Metal Yb$_2$Pt$_2$Pb text, January 2016

Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites text, January 2016

Anyons in an exactly solved model and beyond text, January 2005

Tomonaga–Luttinger liquid behavior and spinon confinement in YbAlO3 journal, February 2019

Synthesis, structure, and electronic properties of the Li 11 RbGd 4 Te 6 O 30 single crystal journal, January 2020

Low-temperature spin dynamics in the TmFeO 3 orthoferrite with a non-Kramers ion journal, January 2020

Title: Novel Strongly Spin-Orbit Coupled Quantum Dimer Magnet: ${Yb}_{2} {Si}_{2} O_{7}$

Double-slit photoelectron interference in strong-field ionization of the neon dimer
journal, January 2019

Thermodynamics and spin gap of the Heisenberg ladder calculated by the look-ahead Lanczos algorithm
journal, November 1994

Crystal Growth of Quantum Magnets in the Rare-Earth Pyrosilicate Family R2Si2O7 (R = Yb, Er) Using the Optical Floating Zone Method
journal, April 2019

Frustration and anisotropic exchange in ytterbium magnets with edge-shared octahedra
journal, August 2018

Magnetoelastic coupling within a Landau model of phase transitions: Application to the frustrated triangular antiferromagnet CsNiCl $_{3}$
journal, July 2011

Magnetic-Field-Induced Condensation of Triplons in Han Purple Pigment ${B a C u S i}_{2} O_{6}$
journal, August 2004

Ordered magnetic phases of the frustrated spin-dimer compound ${Ba}_{3} {Mn}_{2} O_{8}$
journal, June 2008

Bose-Einstein Condensation of $S = 1$ Nickel Spin Degrees of Freedom in ${NiCl}_{2} − 4 SC ({NH}_{2})_{2}$
journal, February 2006

Lead palladium titanate: A room temperature nanoscale multiferroic thin film
journal, February 2020

VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data
journal, October 2011

Thermodynamic and transport properties of the one-dimensional S=12 antiferromagnet Yb4As3
journal, March 2002

Bose–Einstein condensation in magnetic insulators
journal, March 2008

Linear spin wave theory for single-Q incommensurate magnetic structures
journal, March 2015

Evidence for Gapped Spin-Wave Excitations in the Frustrated ${Gd}_{2} {Sn}_{2} O_{7}$ Pyrochlore Antiferromagnet from Low-Temperature Specific Heat Measurements
journal, August 2007

Valence Bonds in Random Quantum Magnets: Theory and Application to ${YbMgGaO}_{4}$
journal, July 2018

Studies of the exactly dimerized bilayer Heisenberg model via strong coupling expansions
journal, November 2000

Bose-Einstein condensation in quantum magnets
journal, May 2014

The new cold neutron chopper spectrometer at the Spallation Neutron Source: Design and performance
journal, August 2011

Field-Induced Magnonic Liquid in the 3D Spin-Dimerized Antiferromagnet ${Sr}_{3} {Cr}_{2} O_{8}$
journal, April 2016

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magnetoacoustic properties
journal, September 2008

Ultrasonics in the two-dimensional dimer spin system YbAl ₃ C ₃
journal, December 2012

Zigzag Magnetic Order in the Iridium Oxide ${Na}_{2} {IrO}_{3}$
journal, February 2013

Anyons in an exactly solved model and beyond
journal, January 2006

Universal dynamic magnetism in Yb pyrochlores with disparate ground states
journal, March 2016

DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009

Thermal Transport and Strong Mass Renormalization in ${NiCl}_{2} − 4 SC ({NH}_{2})_{2}$
journal, January 2011

Orbital-exchange and fractional quantum number excitations in an f-electron metal, Yb ₂ Pt ₂ Pb
journal, June 2016

Bose-Einstein condensation of triplons in ${Ba}_{3} {Cr}_{2} O_{8}$
journal, March 2009

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

Spin Gap State of S = 1/2 Heisenberg Antiferromagnet YbAl ₃ C ₃
journal, December 2007

Field-Induced Bose-Einstein Condensation of Triplons up to 8 K in ${Sr}_{3} {Cr}_{2} O_{8}$
journal, November 2009

Quantum Excitations in Quantum Spin Ice
journal, October 2011

Polymorphism and crystal data of the rare-earth disilicates of type R.E.2Si2O7
journal, May 1970

The crystal structures of the rare earth pyrosilicates
journal, May 1970

Singlet-triplet crossover in the two-dimensional dimer spin system YbAl3C3
journal, June 2013

Quantum Melting of Spin Ice: Emergent Cooperative Quadrupole and Chirality
journal, July 2010

Anisotropic Exchange within Decoupled Tetrahedra in the Quantum Breathing Pyrochlore ${Ba}_{3} {Yb}_{2} {Zn}_{5} O_{11}$
journal, June 2016

Effect of different resumption strategies to flatten the potential COVID-19 outbreaks amid society reopens: a modeling study in China
journal, March 2021

Kitaev materials beyond iridates: Order by quantum disorder and Weyl magnons in rare-earth double perovskites
journal, February 2017

Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets
journal, May 2014

Quantum spin state in the rare-earth compound YbAl $_{3}$ C $_{3}$
journal, April 2012

Double-slit photoelectron interference in strong-field ionization of the neon dimer
other, January 2019

Spin-Singlet Ground State in the Two-Dimensional Frustrated Triangular Lattice: YbAl ₃ C ₃
journal, May 2008

Field-induced long-range magnetic order in the spin-singlet ground-state system YbAl $_{3}$ C $_{3}$ : Neutron diffraction study
journal, June 2013

Rare-earth arsenides
journal, September 1970

Mott Insulators in the Strong Spin-Orbit Coupling Limit: From Heisenberg to a Quantum Compass and Kitaev Models
journal, January 2009

Direct evidence for dominant bond-directional interactions in a honeycomb lattice iridate Na2IrO3
journal, May 2015

Hidden symmetries of the extended Kitaev-Heisenberg model: Implications for the honeycomb-lattice iridates $A_{2} {IrO}_{3}$
journal, July 2015

Double-slit photoelectron interference in strong-field ionization of the neon dimer
text, January 2019

Bose-Einstein Condensation in Magnetic Insulators
text, January 2007

Character of magnetic excitations in a quasi-one-dimensional antiferromagnet near the quantum critical points: Impact on magneto-acoustic properties
text, January 2008

Quantum Melting of Spin Ice: Emergent Cooperative Quadrupole and Chirality
text, January 2009

Singlet-triplet Crossover in the Two-dimensional Dimer Spin System YbAl3C3
text, January 2013

Linear spin wave theory for single-Q incommensurate magnetic structures
text, January 2014

Orbital-Exchange and Fractional Quantum Number Excitations in an f-electron Metal Yb$_2$Pt$_2$Pb
text, January 2016

Kitaev materials beyond iridates: order by quantum disorder and Weyl magnons in rare-earth double perovskites
text, January 2016

Anyons in an exactly solved model and beyond
text, January 2005

Tomonaga–Luttinger liquid behavior and spinon confinement in YbAlO3
journal, February 2019

Synthesis, structure, and electronic properties of the Li ₁₁ RbGd ₄ Te ₆ O ₃₀ single crystal
journal, January 2020

Low-temperature spin dynamics in the ${TmFeO}_{3}$ orthoferrite with a non-Kramers ion
journal, January 2020