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

The pyrochlore magnet Yb 2Ti 2O 7 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, Yb 2Ti 2O 7'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 Yb 3+, normally at the A site of the A 2B 2O 7 pyrochlore structure, reside as well at the B site. In these samples Yb 3+ 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 Yb 3+ in four compositions of Yb 2+xTi 2-xO 7-y show the spectroscopic signatures for these defective Yb 3+ ions and explicitly demonstrate that the spin anisotropy of the Yb 3+ moment changes from XY-like for stoichiometric Yb 3+ to Ising-like for “stuffed” B site Yb 3+ or for A site Yb 3+ in the presence of oxygen vacancies.
Authors:
 [1] ;  [2] ; ORCiD logo [3] ;  [4] ;  [5]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division; McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
  2. McMaster Univ., Hamilton, ON (Canada). Dept. of Physics and Astronomy
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  4. McMaster Univ., Hamilton, ON (Canada). Brockhouse Inst. for Materials Research
  5. 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:
Grant/Contract Number:
AC05-00OR22725
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)
Research Org:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Natural Sciences and Engineering Research Council of Canada (NSERC)
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
OSTI Identifier:
1474482
Alternate Identifier(s):
OSTI ID: 1441113

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., Web. doi:10.1103/PhysRevB.97.224409.
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. doi:10.1103/PhysRevB.97.224409.
Sala, Gabriele, Maharaj, Dalini D., Stone, Matthew B., Dabkowska, H. A., and Gaulin, Bruce D.. 2018. "Crystal field excitations from Yb3+ ions at defective sites in highly stuffed Yb2Ti2O7". United States. doi:10.1103/PhysRevB.97.224409.
@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 = {2018},
month = {6}
}