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 ${Yb}_{2} {Ti}_{2} O_{7}$

Journal Article · Mon Jun 11 00:00:00 EDT 2018 · Physical Review B

DOI:https://doi.org/10.1103/PhysRevB.97.224409· OSTI ID:1474482

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)

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.

View Accepted Manuscript (DOE)

View Accepted Manuscript (Publisher)

Cite

Export

Save

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

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

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1474482

Alternate ID(s):: OSTI ID: 1441113

Journal Information:: Physical Review B, Vol. 97, Issue 22; ISSN 2469-9950

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 6 works

Citation information provided by
Web of Science

References (59)

Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions Stevens, K. W. H. Proceedings of the Physical Society. Section A, Vol. 65, Issue 3 https://doi.org/10.1088/0370-1298/65/3/308	journal	March 1952
Spin dynamics in geometrically frustrated compounds Yaouanc, A.; de Réotier, P. Dalmas; Bonville, P. Physica B: Condensed Matter, Vol. 326, Issue 1-4 https://doi.org/10.1016/S0921-4526(02)01664-2	journal	February 2003
Mantid—Data analysis and visualization package for neutron scattering and $μ$ SR experiments 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 https://doi.org/10.1016/j.nima.2014.07.029	journal	November 2014
From Spin Glass to Quantum Spin Liquid Ground States in Molybdate Pyrochlores Clark, L.; Nilsen, G. J.; Kermarrec, E. Physical Review Letters, Vol. 113, Issue 11 https://doi.org/10.1103/PhysRevLett.113.117201	journal	September 2014
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E. Journal of Physics: Conference Series, Vol. 251 https://doi.org/10.1088/1742-6596/251/1/012058	journal	November 2010
Reentrant Phase Diagram of ${Yb}_{2} {Ti}_{2} O_{7}$ in a $⟨ 111 ⟩$ Magnetic Field Scheie, A.; Kindervater, J.; Säubert, S. Physical Review Letters, Vol. 119, Issue 12 https://doi.org/10.1103/PhysRevLett.119.127201	journal	September 2017
Experimental Insights into Ground-State Selection of Quantum XY Pyrochlores Hallas, Alannah M.; Gaudet, Jonathan; Gaulin, Bruce D. Annual Review of Condensed Matter Physics, Vol. 9, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031016-025218	journal	March 2018
Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7 Kermarrec, E.; Gaudet, J.; Fritsch, K. Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms14810	journal	March 2017
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
First-order magnetic transition in ${Yb}_{2} {Ti}_{2} O_{7}$ Lhotel, E.; Giblin, S. R.; Lees, M. R. Physical Review B, Vol. 89, Issue 22 https://doi.org/10.1103/PhysRevB.89.224419	journal	June 2014
Observation of magnetic fragmentation in spin ice Petit, S.; Lhotel, E.; Canals, B. Nature Physics, Vol. 12, Issue 8 https://doi.org/10.1038/nphys3710	journal	April 2016
Gapless quantum excitations from an icelike splayed ferromagnetic ground state in stoichiometric ${Yb}_{2} {Ti}_{2} O_{7}$ Gaudet, J.; Ross, K. A.; Kermarrec, E. Physical Review B, Vol. 93, Issue 6 https://doi.org/10.1103/PhysRevB.93.064406	journal	February 2016
Low-energy electrodynamics of novel spin excitations in the quantum spin ice Yb2Ti2O7 Pan, LiDong; Kim, Se Kwon; Ghosh, A. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5970	journal	September 2014
Seeing the light: Experimental signatures of emergent electromagnetism in a quantum spin ice Benton, Owen; Sikora, Olga; Shannon, Nic Physical Review B, Vol. 86, Issue 7 https://doi.org/10.1103/PhysRevB.86.075154	journal	August 2012
Quasiparticle Breakdown and Spin Hamiltonian of the Frustrated Quantum Pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$ in a Magnetic Field Thompson, J. D.; McClarty, P. A.; Prabhakaran, D. Physical Review Letters, Vol. 119, Issue 5 https://doi.org/10.1103/PhysRevLett.119.057203	journal	August 2017
Treating crystal field parameters in lower than cubic symmetries Walter, U. Journal of Physics and Chemistry of Solids, Vol. 45, Issue 4 https://doi.org/10.1016/0022-3697(84)90147-1	journal	January 1984
Dimensional evolution of spin correlations in the magnetic pyrochlore Yb $_{2}$ Ti $_{2}$ O $_{7}$ Ross, K. A.; Yaraskavitch, L. R.; Laver, M. Physical Review B, Vol. 84, Issue 17 https://doi.org/10.1103/PhysRevB.84.174442	journal	November 2011
Acoustic signatures of the phases and phase transitions in ${Yb}_{2} {Ti}_{2} O_{7}$ Bhattacharjee, Subhro; Erfanifam, S.; Green, E. L. Physical Review B, Vol. 93, Issue 14 https://doi.org/10.1103/PhysRevB.93.144412	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 Thompson, Jordan D.; McClarty, Paul A.; Rønnow, Henrik M. Physical Review Letters, Vol. 106, Issue 18 https://doi.org/10.1103/PhysRevLett.106.187202	journal	May 2011
Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores Sala, G.; Gutmann, M. J.; Prabhakaran, D. Nature Materials, Vol. 13, Issue 5 https://doi.org/10.1038/nmat3924	journal	April 2014
Vindication of ${Yb}_{2} {Ti}_{2} O_{7}$ as a Model Exchange Quantum Spin Ice Applegate, R.; Hayre, N. R.; Singh, R. R. P. Physical Review Letters, Vol. 109, Issue 9 https://doi.org/10.1103/PhysRevLett.109.097205	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 Hayre, N. R.; Ross, K. A.; Applegate, R. Physical Review B, Vol. 87, Issue 18 https://doi.org/10.1103/PhysRevB.87.184423	journal	May 2013
Ferromagnetic ordered phase of quantum spin ice system Yb ₂ Ti ₂ O ₇ under [001] magnetic field Hamachi, Noriaki; Yasui, Yukio; Araki, Koji AIP Advances, Vol. 6, Issue 5 https://doi.org/10.1063/1.4944337	journal	May 2016
Unconventional magnetic ground state in Yb $_{2}$ Ti $_{2}$ O $_{7}$ D’Ortenzio, R. M.; Dabkowska, H. A.; Dunsiger, S. R. Physical Review B, Vol. 88, Issue 13 https://doi.org/10.1103/PhysRevB.88.134428	journal	October 2013
Effect of chemical pressure on the crystal electric field states of erbium pyrochlore magnets Gaudet, J.; Hallas, A. M.; Kolesnikov, A. I. Physical Review B, Vol. 97, Issue 2 https://doi.org/10.1103/PhysRevB.97.024415	journal	January 2018
Coulombic Quantum Liquids in Spin- $1 / 2$ Pyrochlores Savary, Lucile; Balents, Leon Physical Review Letters, Vol. 108, Issue 3 https://doi.org/10.1103/PhysRevLett.108.037202	journal	January 2012
Studies of ( and Yb); new results Dalmas de Réotier, P.; Glazkov, V.; Marin, C. Physica B: Condensed Matter, Vol. 374-375 https://doi.org/10.1016/j.physb.2005.11.037	journal	March 2006
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6 https://doi.org/10.6028/jres.114.025	journal	November 2009
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
Dilute stuffing in the pyrochlore iridate ${Eu}_{2} {Ir}_{2} O_{7}$ Telang, Prachi; Mishra, Kshiti; Sood, A. K. Physical Review B, Vol. 97, Issue 23 https://doi.org/10.1103/PhysRevB.97.235118	journal	June 2018
First-Order Transition in the Spin Dynamics of Geometrically Frustrated ${Yb}_{2} {Ti}_{2} O_{7}$ Hodges, J. A.; Bonville, P.; Forget, A. Physical Review Letters, Vol. 88, Issue 7 https://doi.org/10.1103/PhysRevLett.88.077204	journal	February 2002
Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets den Hertog, Byron C.; Gingras, Michel J. P. Physical Review Letters, Vol. 84, Issue 15 https://doi.org/10.1103/PhysRevLett.84.3430	journal	April 2000
A measure of monopole inertia in the quantum spin ice Yb2Ti2O7 Pan, LiDong; Laurita, N. J.; Ross, Kate A. Nature Physics, Vol. 12, Issue 4 https://doi.org/10.1038/nphys3608	journal	December 2015
Quantum Excitations in Quantum Spin Ice Ross, Kate A.; Savary, Lucile; Gaulin, Bruce D. Physical Review X, Vol. 1, Issue 2 https://doi.org/10.1103/PhysRevX.1.021002	journal	October 2011
Ferromagnetic Transition of Pyrochlore Compound Yb ₂ Ti ₂ O ₇ Yasui, Yukio; Soda, Minoru; Iikubo, Satoshi Journal of the Physical Society of Japan, Vol. 72, Issue 11 https://doi.org/10.1143/JPSJ.72.3014	journal	November 2003
Magnetic excitations in the ground state of ${Yb}_{2} {Ti}_{2} O_{7}$ Peçanha-Antonio, Viviane; Feng, Erxi; Su, Yixi Physical Review B, Vol. 96, Issue 21 https://doi.org/10.1103/PhysRevB.96.214415	journal	December 2017
Zero-point entropy in ‘spin ice’ Ramirez, A. P.; Hayashi, A.; Cava, R. J. Nature, Vol. 399, Issue 6734 https://doi.org/10.1038/20619	journal	May 1999
Spin liquid regimes at nonzero temperature in quantum spin ice Savary, Lucile; Balents, Leon Physical Review B, Vol. 87, Issue 20 https://doi.org/10.1103/PhysRevB.87.205130	journal	May 2013
Effects of stuffing on the atomic and electronic structure of the pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$ Ghosh, Soham S.; Manousakis, Efstratios Physical Review B, Vol. 97, Issue 24 https://doi.org/10.1103/PhysRevB.97.245117	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 Mostaed, Ali; Balakrishnan, Geetha; Lees, Martin Richard Physical Review B, Vol. 95, Issue 9 https://doi.org/10.1103/PhysRevB.95.094431	journal	March 2017
Heat-capacity measurements on rare-earth double oxides R2M2O7 Blöte, H. W. J.; Wielinga, R. F.; Huiskamp, W. J. Physica, Vol. 43, Issue 4 https://doi.org/10.1016/0031-8914(69)90187-6	journal	September 1969
Impact of stoichiometry of ${Yb}_{2} {Ti}_{2} O_{7}$ on its physical properties Arpino, K. E.; Trump, B. A.; Scheie, A. O. Physical Review B, Vol. 95, Issue 9 https://doi.org/10.1103/PhysRevB.95.094407	journal	March 2017
Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7 Rosenkranz, S.; Ramirez, A. P.; Hayashi, A. Journal of Applied Physics, Vol. 87, Issue 9 https://doi.org/10.1063/1.372565	journal	May 2000
First-principles calculation and experimental investigation of lattice dynamics in the rare-earth pyrochlores $R_{2} {Ti}_{2} O_{7}$ $(R = Tb, Dy, Ho)$ Ruminy, M.; Valdez, M. Núñez; Wehinger, B. Physical Review B, Vol. 93, Issue 21 https://doi.org/10.1103/PhysRevB.93.214308	journal	June 2016
Lightly stuffed pyrochlore structure of single-crystalline Yb $_{2}$ Ti $_{2}$ O $_{7}$ grown by the optical floating zone technique Ross, K. A.; Proffen, Th.; Dabkowska, H. A. Physical Review B, Vol. 86, Issue 17 https://doi.org/10.1103/PhysRevB.86.174424	journal	November 2012
Two-Dimensional Kagome Correlations and Field Induced Order in the Ferromagnetic $X Y$ Pyrochlore ${Yb}_{2} {Ti}_{2} O_{7}$ Ross, K. A.; Ruff, J. P. C.; Adams, C. P. Physical Review Letters, Vol. 103, Issue 22 https://doi.org/10.1103/PhysRevLett.103.227202	journal	November 2009
Introduction to Frustrated Magnetism Lacroix, Claudine; Mendels, Philippe; Mila, Frédéric Springer Series in Solid-State Sciences https://doi.org/10.1007/978-3-642-10589-0	book	January 2011
Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets Gingras, M. J. P.; McClarty, P. A. Reports on Progress in Physics, Vol. 77, Issue 5 https://doi.org/10.1088/0034-4885/77/5/056501	journal	May 2014
Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7 Chang, Lieh-Jeng; Onoda, Shigeki; Su, Yixi Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1989	journal	January 2012
Geometrical Frustration in the Ferromagnetic Pyrochlore ${Ho}_{2} {Ti}_{2} O_{7}$ Harris, M. J.; Bramwell, S. T.; McMorrow, D. F. Physical Review Letters, Vol. 79, Issue 13 https://doi.org/10.1103/PhysRevLett.79.2554	journal	September 1997
Quantum fluctuations in spin-ice-like Pr2Zr2O7 Kimura, K.; Nakatsuji, S.; Wen, J-J. Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms2914	journal	June 2013
Spin Ice State in Frustrated Magnetic Pyrochlore Materials Bramwell, S. T. Science, Vol. 294, Issue 5546 https://doi.org/10.1126/science.1064761	journal	November 2001
Crystal electric field in the R ₂ Ti ₂ O ₇ pyrochlore compounds Bertin, A.; Chapuis, Y.; Dalmas de Réotier, P. Journal of Physics: Condensed Matter, Vol. 24, Issue 25 https://doi.org/10.1088/0953-8984/24/25/256003	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 Bonville, P.; Hodges, J. A.; Bertin, E. Hyperfine Interactions, Vol. 156/157, Issue 1-4 https://doi.org/10.1023/B:HYPE.0000043235.21257.13	journal	January 2004
Spin-spin correlations in Yb_{2}Ti_{2}O_{7} : A polarized neutron scattering study Gardner, J. S.; Ehlers, G.; Rosov, N. Physical Review B, Vol. 70, Issue 18 https://doi.org/10.1103/PhysRevB.70.180404	journal	November 2004
Local susceptibility of the Yb ₂ Ti ₂ O ₇ rare earth pyrochlore computed from a Hamiltonian with anisotropic exchange Thompson, J. D.; McClarty, P. A.; Gingras, M. J. P. Journal of Physics: Condensed Matter, Vol. 23, Issue 16 https://doi.org/10.1088/0953-8984/23/16/164219	journal	April 2011
Magnetic monopoles in spin ice Castelnovo, C.; Moessner, R.; Sondhi, S. L. Nature, Vol. 451, Issue 7174 https://doi.org/10.1038/nature06433	journal	January 2008
Single-crystal versus polycrystalline samples of magnetically frustrated Yb $_{2}$ Ti $_{2}$ O $_{7}$ : Specific heat results Yaouanc, A.; Dalmas de Réotier, P.; Marin, C. Physical Review B, Vol. 84, Issue 17 https://doi.org/10.1103/PhysRevB.84.172408	journal	November 2011
Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed ${Yb}_{2} {Ti}_{2} O_{7}$ Gaudet, J.; Maharaj, D. D.; Sala, G. Physical Review B, Vol. 92, Issue 13 https://doi.org/10.1103/PhysRevB.92.134420	journal	October 2015

Similar Records

Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed

{Yb}_{2} {Ti}_{2} O_{7}

Journal Article · Tue Oct 27 00:00:00 EDT 2015 · Physical Review. B, Condensed Matter and Materials Physics · OSTI ID:1474482

Gaudet, J.; Maharaj, D. D.; Sala, G.; +6 more

XY antiferromagnetic ground state in the effective

S = \frac{1}{2}

pyrochlore

{Yb}_{2} {Ge}_{2} O_{7}

Journal Article · Tue Mar 01 00:00:00 EST 2016 · Physical Review B · OSTI ID:1474482

Hallas, Alannah M.; Gaudet, J.; Wilson, Murray N.; +10 more

Gapless quantum excitations from an icelike splayed ferromagnetic ground state in stoichiometric

{Yb}_{2} {Ti}_{2} O_{7}

Journal Article · Wed Feb 03 00:00:00 EST 2016 · Physical Review B · OSTI ID:1474482

Gaudet, J.; Ross, K. A.; Kermarrec, E.; +4 more

Related Subjects

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

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

Citation Formats

References (59)

Similar Records

Related Subjects

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