Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed
Abstract
Time-of-flight neutron spectroscopy has been used to determine the crystalline electric field Hamiltonian, eigenvalues and eigenvectors appropriate to the J=7/2 Yb3+ ion in the candidate quantum spin ice pyrochlore magnet Yb2Ti2O7. The precise ground state of this exotic, geometrically frustrated magnet is known to be sensitive to weak disorder associated with the growth of single crystals from the melt. Such materials display weak “stuffing,” wherein a small proportion, approximately 2%, of the nonmagnetic Ti4+ sites are occupied by excess Yb3+. We have carried out neutron spectroscopic measurements on a stoichiometric powder sample of Yb2Ti2O7, as well as a crushed single crystal with weak stuffing and an approximate composition of Yb2+xTi2–xO7+y with x = 0.046. All samples display three crystalline electric field transitions out of the ground state, and the ground state doublet itself is identified as primarily composed of mJ = ±1/2, as expected. However, stuffing at low temperatures in Yb2+xTi2–xO7+y induces a similar finite crystalline electric field lifetime as is induced in stoichiometric Yb2Ti2O7 by elevated temperature. In conclusion, an extended strain field exists about each local “stuffed” site, which produces a distribution of random crystalline electric field environments in the lightly stuffed Yb2+xTi2–xO7+y, in addition to producing amore »
- Authors:
-
- McMaster Univ., Hamilton, ON (Canada)
- Colorado State Univ., Fort Collins, CO (United States)
- Brockhouse Institute for Materials Research, Hamilton, ON (Canada)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- McMaster Univ., Hamilton, ON (Canada); Brockhouse Institute for Materials Research, Hamilton, ON (Canada); Canadian Institute for Materials Research, Toronto, ON (Canada)
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1224753
- Alternate Identifier(s):
- OSTI ID: 1224372
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Journal Article: Accepted Manuscript
- Journal Name:
- Physical Review. B, Condensed Matter and Materials Physics
- Additional Journal Information:
- Journal Volume: 92; Journal Issue: 13; Journal ID: ISSN 1098-0121
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Gaudet, J., Maharaj, D. D., Sala, G., Kermarrec, E., Ross, K. A., Dabkowska, H. A., Kolesnikov, A. I., Granroth, G. E., and Gaulin, B. D. Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7. United States: N. p., 2015.
Web. doi:10.1103/PhysRevB.92.134420.
Gaudet, J., Maharaj, D. D., Sala, G., Kermarrec, E., Ross, K. A., Dabkowska, H. A., Kolesnikov, A. I., Granroth, G. E., & Gaulin, B. D. Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7. United States. https://doi.org/10.1103/PhysRevB.92.134420
Gaudet, J., Maharaj, D. D., Sala, G., Kermarrec, E., Ross, K. A., Dabkowska, H. A., Kolesnikov, A. I., Granroth, G. E., and Gaulin, B. D. 2015.
"Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7". United States. https://doi.org/10.1103/PhysRevB.92.134420. https://www.osti.gov/servlets/purl/1224753.
@article{osti_1224753,
title = {Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7},
author = {Gaudet, J. and Maharaj, D. D. and Sala, G. and Kermarrec, E. and Ross, K. A. and Dabkowska, H. A. and Kolesnikov, A. I. and Granroth, G. E. and Gaulin, B. D.},
abstractNote = {Time-of-flight neutron spectroscopy has been used to determine the crystalline electric field Hamiltonian, eigenvalues and eigenvectors appropriate to the J=7/2 Yb3+ ion in the candidate quantum spin ice pyrochlore magnet Yb2Ti2O7. The precise ground state of this exotic, geometrically frustrated magnet is known to be sensitive to weak disorder associated with the growth of single crystals from the melt. Such materials display weak “stuffing,” wherein a small proportion, approximately 2%, of the nonmagnetic Ti4+ sites are occupied by excess Yb3+. We have carried out neutron spectroscopic measurements on a stoichiometric powder sample of Yb2Ti2O7, as well as a crushed single crystal with weak stuffing and an approximate composition of Yb2+xTi2–xO7+y with x = 0.046. All samples display three crystalline electric field transitions out of the ground state, and the ground state doublet itself is identified as primarily composed of mJ = ±1/2, as expected. However, stuffing at low temperatures in Yb2+xTi2–xO7+y induces a similar finite crystalline electric field lifetime as is induced in stoichiometric Yb2Ti2O7 by elevated temperature. In conclusion, an extended strain field exists about each local “stuffed” site, which produces a distribution of random crystalline electric field environments in the lightly stuffed Yb2+xTi2–xO7+y, in addition to producing a small fraction of Yb ions in defective environments with grossly different crystalline electric field eigenvalues and eigenvectors.},
doi = {10.1103/PhysRevB.92.134420},
url = {https://www.osti.gov/biblio/1224753},
journal = {Physical Review. B, Condensed Matter and Materials Physics},
issn = {1098-0121},
number = 13,
volume = 92,
place = {United States},
year = {Tue Oct 27 00:00:00 EDT 2015},
month = {Tue Oct 27 00:00:00 EDT 2015}
}
Web of Science
Works referenced in this record:
Oxide pyrochlores — A review
journal, January 1983
- Subramanian, M. A.; Aravamudan, G.; Subba Rao, G. V.
- Progress in Solid State Chemistry, Vol. 15, Issue 2
Magnetic pyrochlore oxides
journal, January 2010
- Gardner, Jason S.; Gingras, Michel J. P.; Greedan, John E.
- Reviews of Modern Physics, Vol. 82, Issue 1
Spin Ice State in Frustrated Magnetic Pyrochlore Materials
journal, November 2001
- Bramwell, S. T.
- Science, Vol. 294, Issue 5546
Magnetic monopoles in spin ice
journal, January 2008
- Castelnovo, C.; Moessner, R.; Sondhi, S. L.
- Nature, Vol. 451, Issue 7174
Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets
journal, April 2000
- den Hertog, Byron C.; Gingras, Michel J. P.
- Physical Review Letters, Vol. 84, Issue 15
Crystal-field interaction in the pyrochlore magnet Ho2Ti2O7
journal, May 2000
- Rosenkranz, S.; Ramirez, A. P.; Hayashi, A.
- Journal of Applied Physics, Vol. 87, Issue 9
Geometrical Frustration in the Ferromagnetic Pyrochlore
journal, September 1997
- Harris, M. J.; Bramwell, S. T.; McMorrow, D. F.
- Physical Review Letters, Vol. 79, Issue 13
The Structure and Entropy of Ice and of Other Crystals with Some Randomness of Atomic Arrangement
journal, December 1935
- Pauling, Linus
- Journal of the American Chemical Society, Vol. 57, Issue 12
Ferromagnetic Transition of Pyrochlore Compound Yb 2 Ti 2 O 7
journal, November 2003
- Yasui, Yukio; Soda, Minoru; Iikubo, Satoshi
- Journal of the Physical Society of Japan, Vol. 72, Issue 11
Higgs transition from a magnetic Coulomb liquid to a ferromagnet in Yb2Ti2O7
journal, January 2012
- Chang, Lieh-Jeng; Onoda, Shigeki; Su, Yixi
- Nature Communications, Vol. 3, Issue 1
First-Order Transition in the Spin Dynamics of Geometrically Frustrated
journal, February 2002
- Hodges, J. A.; Bonville, P.; Forget, A.
- Physical Review Letters, Vol. 88, Issue 7
Two-Dimensional Kagome Correlations and Field Induced Order in the Ferromagnetic Pyrochlore
journal, November 2009
- Ross, K. A.; Ruff, J. P. C.; Adams, C. P.
- Physical Review Letters, Vol. 103, Issue 22
Dimensional evolution of spin correlations in the magnetic pyrochlore Yb Ti O
journal, November 2011
- Ross, K. A.; Yaraskavitch, L. R.; Laver, M.
- Physical Review B, Vol. 84, Issue 17
Pyrochlore photons: The spin liquid in a three-dimensional frustrated magnet
journal, February 2004
- Hermele, Michael; Fisher, Matthew P. A.; Balents, Leon
- Physical Review B, Vol. 69, Issue 6
Quantum spin ice: a search for gapless quantum spin liquids in pyrochlore magnets
journal, May 2014
- Gingras, M. J. P.; McClarty, P. A.
- Reports on Progress in Physics, Vol. 77, Issue 5
Bulk magnetization of the heavy rare earth titanate pyrochlores - a series of model frustrated magnets
journal, December 1999
- Bramwell, S. T.; Field, M. N.; Harris, M. J.
- Journal of Physics: Condensed Matter, Vol. 12, Issue 4
Coulombic Quantum Liquids in Spin- Pyrochlores
journal, January 2012
- Savary, Lucile; Balents, Leon
- Physical Review Letters, Vol. 108, Issue 3
Spin liquid regimes at nonzero temperature in quantum spin ice
journal, May 2013
- Savary, Lucile; Balents, Leon
- Physical Review B, Vol. 87, Issue 20
Quantum Excitations in Quantum Spin Ice
journal, October 2011
- Ross, Kate A.; Savary, Lucile; Gaulin, Bruce D.
- Physical Review X, Vol. 1, Issue 2
Lightly stuffed pyrochlore structure of single-crystalline Yb Ti O grown by the optical floating zone technique
journal, November 2012
- Ross, K. A.; Proffen, Th.; Dabkowska, H. A.
- Physical Review B, Vol. 86, Issue 17
Stuffed rare earth pyrochlore solid solutions
journal, October 2006
- Lau, G. C.; Muegge, B. D.; McQueen, T. M.
- Journal of Solid State Chemistry, Vol. 179, Issue 10
Long- and short-range order in stuffed titanate pyrochlores
journal, January 2008
- Lau, G. C.; McQueen, T. M.; Huang, Q.
- Journal of Solid State Chemistry, Vol. 181, Issue 1
Quantum spin fluctuations in the spin-liquid state of Tb 2 Ti 2 O 7
journal, December 2011
- Takatsu, Hiroshi; Kadowaki, Hiroaki; Sato, Taku J.
- Journal of Physics: Condensed Matter, Vol. 24, Issue 5
Exotic transition in the three-dimensional spin-liquid candidate Tb Ti O
journal, November 2011
- Yaouanc, A.; Dalmas de Réotier, P.; Chapuis, Y.
- Physical Review B, Vol. 84, Issue 18
Studies of ( and Yb); new results
journal, March 2006
- Dalmas de Réotier, P.; Glazkov, V.; Marin, C.
- Physica B: Condensed Matter, Vol. 374-375
Heat-capacity measurements on rare-earth double oxides R2M2O7
journal, September 1969
- Blöte, H. W. J.; Wielinga, R. F.; Huiskamp, W. J.
- Physica, Vol. 43, Issue 4
Single-crystal versus polycrystalline samples of magnetically frustrated Yb Ti O : Specific heat results
journal, November 2011
- Yaouanc, A.; Dalmas de Réotier, P.; Marin, C.
- Physical Review B, Vol. 84, Issue 17
Fractional Spin Textures in the Frustrated Magnet
journal, March 2011
- Sen, Arnab; Damle, Kedar; Moessner, Roderich
- Physical Review Letters, Vol. 106, Issue 12
Magnetothermal study of the hybrid frustrated magnet
journal, October 2009
- Ke, X.; West, D. V.; Cava, R. J.
- Physical Review B, Vol. 80, Issue 14
Quenched crystal-field disorder and magnetic liquid ground states in
journal, June 2015
- Gaulin, B. D.; Kermarrec, E.; Dahlberg, M. L.
- Physical Review B, Vol. 91, Issue 24
Vacancy defects and monopole dynamics in oxygen-deficient pyrochlores
journal, April 2014
- Sala, G.; Gutmann, M. J.; Prabhakaran, D.
- Nature Materials, Vol. 13, Issue 5
Matrix Elements and Operator Equivalents Connected with the Magnetic Properties of Rare Earth Ions
journal, March 1952
- Stevens, K. W. H.
- Proceedings of the Physical Society. Section A, Vol. 65, Issue 3
SEQUOIA: A Newly Operating Chopper Spectrometer at the SNS
journal, November 2010
- Granroth, G. E.; Kolesnikov, A. I.; Sherline, T. E.
- Journal of Physics: Conference Series, Vol. 251
Crystal electric field in the R 2 Ti 2 O 7 pyrochlore compounds
journal, May 2012
- Bertin, A.; Chapuis, Y.; Dalmas de Réotier, P.
- Journal of Physics: Condensed Matter, Vol. 24, Issue 25
Anisotropic exchange in frustrated pyrochlore Yb 2 Ti 2 O 7
journal, November 2009
- Cao, H. B.; Gukasov, A.; Mirebeau, I.
- Journal of Physics: Condensed Matter, Vol. 21, Issue 49
The crystal field and exchange interactions in Yb 2 Ti 2 O 7
journal, September 2001
- Hodges, J. A.; Bonville, P.; Forget, A.
- Journal of Physics: Condensed Matter, Vol. 13, Issue 41
Optical spectroscopy of and and crystal-field parameters in rare-earth titanate pyrochlores
journal, August 2004
- Malkin, B. Z.; Zakirov, A. R.; Popova, M. N.
- Physical Review B, Vol. 70, Issue 7
Treating crystal field parameters in lower than cubic symmetries
journal, January 1984
- Walter, U.
- Journal of Physics and Chemistry of Solids, Vol. 45, Issue 4
Theoretical Investigation of Some Magnetic and Spectroscopic Properties of Rare-Earth Ions
journal, September 1962
- Freeman, A. J.; Watson, R. E.
- Physical Review, Vol. 127, Issue 6
Ising Pyrochlore Magnets: Low-Temperature Properties, “Ice Rules,” and Beyond
journal, August 1999
- Siddharthan, R.; Shastry, B. S.; Ramirez, A. P.
- Physical Review Letters, Vol. 83, Issue 9
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
DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data
journal, November 2009
- Azuah, Richard Tumanjong; Kneller, Larry R.; Qiu, Yiming
- Journal of Research of the National Institute of Standards and Technology, Vol. 114, Issue 6
Magnetic Monopoles in Spin Ice
journal, January 2008
- Castelnovo, C.; Moessner, R.; Sondhi, S. L.
- Topologica, Vol. 1, Issue 1
Quantum spin fluctuations in the spin liquid state of Tb2Ti2O7
text, January 2011
- Takatsu, Hiroshi; Kadowaki, Hiroaki; Sato, Taku J.
- arXiv
Spin Liquid Regimes at Nonzero Temperature in Quantum Spin Ice
text, January 2013
- Savary, Lucile; Balents, Leon
- arXiv
Dipolar Interactions and Origin of Spin Ice in Ising Pyrochlore Magnets
text, January 2000
- Hertog, Byron C. den; Gingras, Michel J. P.
- arXiv
Ising pyrochlore magnets: Low temperature properties, ice rules and beyond
text, January 1999
- Siddharthan, R.; Shastry, B. S.; Ramirez, A. P.
- arXiv
Works referencing / citing this record:
Ground state selection under pressure in the quantum pyrochlore magnet Yb2Ti2O7
journal, March 2017
- Kermarrec, E.; Gaudet, J.; Fritsch, K.
- Nature Communications, Vol. 8, Issue 1
Nearest-neighbour resonating valence bonds in YbMgGaO4
journal, June 2017
- Li, Yuesheng; Adroja, Devashibhai; Voneshen, David
- Nature Communications, Vol. 8, Issue 1
Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
journal, December 2016
- Paddison, Joseph A. M.; Daum, Marcus; Dun, Zhiling
- Nature Physics, Vol. 13, Issue 2
Role of defects in determining the magnetic ground state of ytterbium titanate
journal, February 2019
- Bowman, D. F.; Cemal, E.; Lehner, T.
- Nature Communications, Vol. 10, Issue 1
A novel type of splayed ferromagnetic order observed in Yb 2 Ti 2 O 7
journal, August 2016
- Yaouanc, A.; Dalmas de Réotier, P.; Keller, L.
- Journal of Physics: Condensed Matter, Vol. 28, Issue 42
Crystal fields and magnetic structure of the Ising antiferromagnet
journal, November 2019
- Cai, Y.; Wilson, M. N.; Beare, J.
- Physical Review B, Vol. 100, Issue 18
Magnetic excitations in the ground state of
journal, December 2017
- Peçanha-Antonio, Viviane; Feng, Erxi; Su, Yixi
- Physical Review B, Vol. 96, Issue 21
Role of defects in determining the magnetic ground state of ytterbium titanate.
text, January 2019
- Bowman, Df; Cemal, E.; Lehner, T.
- Apollo - University of Cambridge Repository
A novel type of splayed ferromagnetic order observed in Yb2Ti2O7
text, January 2016
- Yaouanc, A.; de Reotier, P. Dalmas; Keller, L.
- arXiv
Continuous excitations of the triangular-lattice quantum spin liquid YbMgGaO4
text, January 2016
- Paddison, J. A. M.; Daum, M.; Dun, Z. L.
- arXiv
Nearest-neighbor resonating valence bonds in YbMgGaO4
text, January 2017
- Li, Yuesheng; Adroja, Devashibhai; Voneshen, David
- arXiv
Effect of Chemical Pressure on the Crystal Electric Field States of Erbium Pyrochlore Magnets
text, January 2017
- Gaudet, J.; Hallas, A. M.; Kolesnikov, A. I.
- arXiv