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Title: Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb 2 Ti 2 O 7

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 » small fraction of Yb ions in defective environments with grossly different crystalline electric field eigenvalues and eigenvectors.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4];  [4];  [5]
  1. McMaster Univ., Hamilton, ON (Canada)
  2. Colorado State Univ., Fort Collins, CO (United States)
  3. Brockhouse Institute for Materials Research, Hamilton, ON (Canada)
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  5. 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}
}

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Works referencing / citing this record:

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


Nearest-neighbour resonating valence bonds in YbMgGaO4
journal, June 2017


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


Role of defects in determining the magnetic ground state of ytterbium titanate
journal, February 2019


A novel type of splayed ferromagnetic order observed in Yb 2 Ti 2 O 7
journal, August 2016


Crystal fields and magnetic structure of the Ising antiferromagnet Er 3 Ga 5 O 12
journal, November 2019


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


Role of defects in determining the magnetic ground state of ytterbium titanate.
text, January 2019


A novel type of splayed ferromagnetic order observed in Yb2Ti2O7
text, January 2016


Nearest-neighbor resonating valence bonds in YbMgGaO4
text, January 2017