Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7

Sala, Gabriele; Maharaj, Dalini D.; Stone, Matthew B.; Dabkowska, H. A.; Gaulin, Bruce D.

doi:10.1103/PhysRevB.97.224409

Title: Crystal field excitations from ${Yb}^{3 +}$ ions at defective sites in highly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$

Abstract

The pyrochlore magnet Yb₂Ti₂O₇ has been proposed as a quantum spin ice candidate, a spin liquid state expected to display emergent quantum electrodynamics with gauge photons among its elementary excitations. However, Yb₂Ti₂O₇'s ground state is known to be very sensitive to its precise stoichiometry. Powder samples, produced by solid-state synthesis at relatively low temperatures, tend to be stoichiometric, while single crystals grown from the melt tend to display weak “stuffing” wherein ~2% of the Yb³⁺, normally at the A site of the A₂B₂O₇ pyrochlore structure, reside as well at the B site. In these samples Yb³⁺ ions should exist in defective environments at low levels and be subjected to crystalline electric fields very different from those at the stoichiometric A sites. Neutron scattering measurements of Yb³⁺ in four compositions of Yb_2+xTi_2-xO_7-y show the spectroscopic signatures for these defective Yb³⁺ ions and explicitly demonstrate that the spin anisotropy of the Yb³⁺ moment changes from XY-like for stoichiometric Yb³⁺ to Ising-like for “stuffed” B site Yb³⁺ or for A site Yb³⁺ in the presence of oxygen vacancies.

Authors:

Sala, Gabriele ^[1]; Maharaj, Dalini D. ^[2];

^[3]; Dabkowska, H. A. ^[4]; Gaulin, Bruce D. ^[5]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division; McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
McMaster Univ., Hamilton, ON (Canada). Brockhouse Inst. for Materials Research
McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy and Brockhouse Inst. for Materials Research; Canadian Inst. for Advanced Research (CIFAR), Toronto (Canada)

Publication Date:: Mon Jun 11 00:00:00 EDT 2018

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

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); Natural Sciences and Engineering Research Council of Canada (NSERC)

OSTI Identifier:: 1474482

Alternate Identifier(s):: OSTI ID: 1441113

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Physical Review B

Additional Journal Information:: Journal Volume: 97; Journal Issue: 22; Journal ID: ISSN 2469-9950

Publisher:: American Physical Society (APS)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; crystal defects; electric field effects; frustrated magnetism; magnetism; pyrochlore; rare-earth alloys; spin ice; time of flight neutron spectroscopy

Citation Formats


                    Sala, Gabriele, Maharaj, Dalini D., Stone, Matthew B., Dabkowska, H. A., and Gaulin, Bruce D. Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7.  United States: N. p., 2018. 
Web.  doi:10.1103/PhysRevB.97.224409.

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                    Sala, Gabriele, Maharaj, Dalini D., Stone, Matthew B., Dabkowska, H. A., & Gaulin, Bruce D. Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7.  United States.  https://doi.org/10.1103/PhysRevB.97.224409

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                    Sala, Gabriele, Maharaj, Dalini D., Stone, Matthew B., Dabkowska, H. A., and Gaulin, Bruce D. Mon .  
"Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7".  United States.  https://doi.org/10.1103/PhysRevB.97.224409.  https://www.osti.gov/servlets/purl/1474482.

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@article{osti_1474482,

  title        = {Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7},

  author       = {Sala, Gabriele and Maharaj, Dalini D. and Stone, Matthew B. and Dabkowska, H. A. and Gaulin, Bruce D.},

  abstractNote = {The pyrochlore magnet Yb2Ti2O7 has been proposed as a quantum spin ice candidate, a spin liquid state expected to display emergent quantum electrodynamics with gauge photons among its elementary excitations. However, Yb2Ti2O7's ground state is known to be very sensitive to its precise stoichiometry. Powder samples, produced by solid-state synthesis at relatively low temperatures, tend to be stoichiometric, while single crystals grown from the melt tend to display weak “stuffing” wherein ~2% of the Yb3+, normally at the A site of the A2B2O7 pyrochlore structure, reside as well at the B site. In these samples Yb3+ ions should exist in defective environments at low levels and be subjected to crystalline electric fields very different from those at the stoichiometric A sites. Neutron scattering measurements of Yb3+ in four compositions of Yb2+xTi2-xO7-y show the spectroscopic signatures for these defective Yb3+ ions and explicitly demonstrate that the spin anisotropy of the Yb3+ moment changes from XY-like for stoichiometric Yb3+ to Ising-like for “stuffed” B site Yb3+ or for A site Yb3+ in the presence of oxygen vacancies.},

  doi          = {10.1103/PhysRevB.97.224409},

  journal      = {Physical Review B},

  number       = 22,

  volume       = 97,

  place        = {United States},

  year         = {Mon Jun 11 00:00:00 EDT 2018},

  month        = {Mon Jun 11 00:00:00 EDT 2018}

}

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Title: Crystal field excitations from Yb 3 + ions at defective sites in highly stuffed Yb 2 Ti 2 O 7

Abstract

Citation Formats

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions journal, March 1952

Spin dynamics in geometrically frustrated compounds journal, February 2003

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

From Spin Glass to Quantum Spin Liquid Ground States in Molybdate Pyrochlores journal, September 2014

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS journal, November 2010

Reentrant Phase Diagram of Yb 2 Ti 2 O 7 in a ⟨ 111 ⟩ Magnetic Field journal, September 2017

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

Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7 journal, March 2017

Recent advances in magnetic structure determination by neutron powder diffraction journal, October 1993

First-order magnetic transition in Yb 2 Ti 2 O 7 journal, June 2014

Observation of magnetic fragmentation in spin ice journal, April 2016

Gapless quantum excitations from an icelike splayed ferromagnetic ground state in stoichiometric Yb 2 Ti 2 O 7 journal, February 2016

Low-energy electrodynamics of novel spin excitations in the quantum spin ice Yb2Ti2O7 journal, September 2014

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

Quasiparticle Breakdown and Spin Hamiltonian of the Frustrated Quantum Pyrochlore Yb 2 Ti 2 O 7 in a Magnetic Field journal, August 2017

Treating crystal field parameters in lower than cubic symmetries journal, January 1984

Dimensional evolution of spin correlations in the magnetic pyrochlore Yb 2 Ti 2 O 7 journal, November 2011

Acoustic signatures of the phases and phase transitions in Yb 2 Ti 2 O 7 journal, April 2016

Rods of Neutron Scattering Intensity in Yb 2 Ti 2 O 7 : Compelling Evidence for Significant Anisotropic Exchange in a Magnetic Pyrochlore Oxide journal, May 2011

Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores journal, April 2014

Vindication of Yb 2 Ti 2 O 7 as a Model Exchange Quantum Spin Ice journal, August 2012

Thermodynamic properties of Yb 2 Ti 2 O 7 pyrochlore as a function of temperature and magnetic field: Validation of a quantum spin ice exchange Hamiltonian journal, May 2013

Ferromagnetic ordered phase of quantum spin ice system Yb 2 Ti 2 O 7 under [001] magnetic field journal, May 2016

Unconventional magnetic ground state in Yb 2 Ti 2 O 7 journal, October 2013

Effect of chemical pressure on the crystal electric field states of erbium pyrochlore magnets journal, January 2018

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

Studies of ( and Yb); new results journal, March 2006

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

Magnetic pyrochlore oxides journal, January 2010

Dilute stuffing in the pyrochlore iridate Eu 2 Ir 2 O 7 journal, June 2018

First-Order Transition in the Spin Dynamics of Geometrically Frustrated Yb 2 Ti 2 O 7 journal, February 2002

Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets journal, April 2000

A measure of monopole inertia in the quantum spin ice Yb2Ti2O7 journal, December 2015

Quantum Excitations in Quantum Spin Ice journal, October 2011

Ferromagnetic Transition of Pyrochlore Compound Yb 2 Ti 2 O 7 journal, November 2003

Magnetic excitations in the ground state of Yb 2 Ti 2 O 7 journal, December 2017

Zero-point entropy in ‘spin ice’ journal, May 1999

Spin liquid regimes at nonzero temperature in quantum spin ice journal, May 2013

Effects of stuffing on the atomic and electronic structure of the pyrochlore Yb 2 Ti 2 O 7 journal, June 2018

Atomic structure study of the pyrochlore Y b 2 T i 2 O 7 and its relationship with low-temperature magnetic order journal, March 2017

Heat-capacity measurements on rare-earth double oxides R2M2O7 journal, September 1969

Impact of stoichiometry of Yb 2 Ti 2 O 7 on its physical properties journal, March 2017

Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7 journal, May 2000

First-principles calculation and experimental investigation of lattice dynamics in the rare-earth pyrochlores R 2 Ti 2 O 7 ( R = Tb , Dy , Ho ) journal, June 2016

Lightly stuffed pyrochlore structure of single-crystalline Yb 2 Ti 2 O 7 grown by the optical floating zone technique journal, November 2012

Two-Dimensional Kagome Correlations and Field Induced Order in the Ferromagnetic X Y Pyrochlore Yb 2 Ti 2 O 7 journal, November 2009

Introduction to Frustrated Magnetism book, January 2011

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

Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7 journal, January 2012

Geometrical Frustration in the Ferromagnetic Pyrochlore Ho 2 Ti 2 O 7 journal, September 1997

Quantum fluctuations in spin-ice-like Pr2Zr2O7 journal, June 2013

Spin Ice State in Frustrated Magnetic Pyrochlore Materials journal, November 2001

Crystal electric field in the R 2 Ti 2 O 7 pyrochlore compounds journal, May 2012

Transitions and Spin Dynamics at Very Low Temperature in the Pyrochlores Yb 2 Ti 2 O 7 and Gd 2 Sn 2 O 7 journal, January 2004

Spin-spin correlations in Yb_{2}Ti_{2}O_{7} : A polarized neutron scattering study journal, November 2004

Local susceptibility of the Yb 2 Ti 2 O 7 rare earth pyrochlore computed from a Hamiltonian with anisotropic exchange journal, April 2011

Magnetic monopoles in spin ice journal, January 2008

Single-crystal versus polycrystalline samples of magnetically frustrated Yb 2 Ti 2 O 7 : Specific heat results journal, November 2011

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb 2 Ti 2 O 7 journal, October 2015

Title: Crystal field excitations from ${Yb}^{3 +}$ ions at defective sites in highly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions
journal, March 1952

Spin dynamics in geometrically frustrated compounds
journal, February 2003

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

From Spin Glass to Quantum Spin Liquid Ground States in Molybdate Pyrochlores
journal, September 2014

SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010

Reentrant Phase Diagram of ${Yb}_{2} {Ti}_{2} O_{7}$ in a $⟨ 111 ⟩$ Magnetic Field
journal, September 2017

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

Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7
journal, March 2017

Recent advances in magnetic structure determination by neutron powder diffraction
journal, October 1993

First-order magnetic transition in ${Yb}_{2} {Ti}_{2} O_{7}$
journal, June 2014

Observation of magnetic fragmentation in spin ice
journal, April 2016

Gapless quantum excitations from an icelike splayed ferromagnetic ground state in stoichiometric ${Yb}_{2} {Ti}_{2} O_{7}$
journal, February 2016

Low-energy electrodynamics of novel spin excitations in the quantum spin ice Yb2Ti2O7
journal, September 2014

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

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

Treating crystal field parameters in lower than cubic symmetries
journal, January 1984

Dimensional evolution of spin correlations in the magnetic pyrochlore Yb $_{2}$ Ti $_{2}$ O $_{7}$
journal, November 2011

Acoustic signatures of the phases and phase transitions in ${Yb}_{2} {Ti}_{2} O_{7}$
journal, April 2016

Rods of Neutron Scattering Intensity in ${Yb}_{2} {Ti}_{2} O_{7}$ : Compelling Evidence for Significant Anisotropic Exchange in a Magnetic Pyrochlore Oxide
journal, May 2011

Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores
journal, April 2014

Vindication of ${Yb}_{2} {Ti}_{2} O_{7}$ as a Model Exchange Quantum Spin Ice
journal, August 2012

Thermodynamic properties of Yb $_{2}$ Ti $_{2}$ O $_{7}$ pyrochlore as a function of temperature and magnetic field: Validation of a quantum spin ice exchange Hamiltonian
journal, May 2013

Ferromagnetic ordered phase of quantum spin ice system Yb ₂ Ti ₂ O ₇ under [001] magnetic field
journal, May 2016

Unconventional magnetic ground state in Yb $_{2}$ Ti $_{2}$ O $_{7}$
journal, October 2013

Effect of chemical pressure on the crystal electric field states of erbium pyrochlore magnets
journal, January 2018

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

Studies of ( and Yb); new results
journal, March 2006

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

Magnetic pyrochlore oxides
journal, January 2010

Dilute stuffing in the pyrochlore iridate ${Eu}_{2} {Ir}_{2} O_{7}$
journal, June 2018

First-Order Transition in the Spin Dynamics of Geometrically Frustrated ${Yb}_{2} {Ti}_{2} O_{7}$
journal, February 2002

Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets
journal, April 2000

A measure of monopole inertia in the quantum spin ice Yb2Ti2O7
journal, December 2015

Quantum Excitations in Quantum Spin Ice
journal, October 2011

Ferromagnetic Transition of Pyrochlore Compound Yb ₂ Ti ₂ O ₇
journal, November 2003

Magnetic excitations in the ground state of ${Yb}_{2} {Ti}_{2} O_{7}$
journal, December 2017

Zero-point entropy in ‘spin ice’
journal, May 1999

Spin liquid regimes at nonzero temperature in quantum spin ice
journal, May 2013

Effects of stuffing on the atomic and electronic structure of the pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$
journal, June 2018

Atomic structure study of the pyrochlore $Y b_{2} T i_{2} O_{7}$ and its relationship with low-temperature magnetic order
journal, March 2017

Heat-capacity measurements on rare-earth double oxides R2M2O7
journal, September 1969

Impact of stoichiometry of ${Yb}_{2} {Ti}_{2} O_{7}$ on its physical properties
journal, March 2017

Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7
journal, May 2000

First-principles calculation and experimental investigation of lattice dynamics in the rare-earth pyrochlores $R_{2} {Ti}_{2} O_{7}$ $(R = Tb, Dy, Ho)$
journal, June 2016

Lightly stuffed pyrochlore structure of single-crystalline Yb $_{2}$ Ti $_{2}$ O $_{7}$ grown by the optical floating zone technique
journal, November 2012

Two-Dimensional Kagome Correlations and Field Induced Order in the Ferromagnetic $X Y$ Pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$
journal, November 2009

Introduction to Frustrated Magnetism
book, January 2011

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

Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7
journal, January 2012

Geometrical Frustration in the Ferromagnetic Pyrochlore ${Ho}_{2} {Ti}_{2} O_{7}$
journal, September 1997

Quantum fluctuations in spin-ice-like Pr2Zr2O7
journal, June 2013

Spin Ice State in Frustrated Magnetic Pyrochlore Materials
journal, November 2001

Crystal electric field in the R ₂ Ti ₂ O ₇ pyrochlore compounds
journal, May 2012

Transitions and Spin Dynamics at Very Low Temperature in the Pyrochlores Yb ₂ Ti ₂ O ₇ and Gd ₂ Sn ₂ O ₇
journal, January 2004

Spin-spin correlations in Yb_{2}Ti_{2}O_{7} : A polarized neutron scattering study
journal, November 2004

Local susceptibility of the Yb ₂ Ti ₂ O ₇ rare earth pyrochlore computed from a Hamiltonian with anisotropic exchange
journal, April 2011

Magnetic monopoles in spin ice
journal, January 2008

Single-crystal versus polycrystalline samples of magnetically frustrated Yb $_{2}$ Ti $_{2}$ O $_{7}$ : Specific heat results
journal, November 2011

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$
journal, October 2015