Neutron spectroscopic study of crystalline electric field excitations in stoichiometric and lightly stuffed Yb2Ti2O7

Gaudet, J.; Maharaj, D. D.; Sala, G.; Kermarrec, E.; Ross, K. A.; Dabkowska, H. A.; Kolesnikov, A. I.; Granroth, G. E.; Gaulin, B. D.

doi:10.1103/PhysRevB.92.134420

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

DOI:https://doi.org/10.1103/PhysRevB.92.134420· OSTI ID:1224753

Gaudet, J. ^[1]; Maharaj, D. D. ^[1]; Sala, G. ^[1]; Kermarrec, E. ^[1]; Ross, K. A. ^[2]; Dabkowska, H. A. ^[3]; Kolesnikov, A. I. ^[4]; Granroth, G. E. ^[4]; Gaulin, B. D. ^[5]

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)

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 Yb_2+xTi_2–xO_7+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 m_J = ±1/2, as expected. However, stuffing at low temperatures in Yb_2+xTi_2–xO_7+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 Yb_2+xTi_2–xO_7+y, in addition to producing a small fraction of Yb ions in defective environments with grossly different crystalline electric field eigenvalues and eigenvectors.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1224753

Alternate ID(s):: OSTI ID: 1224372

Journal Information:: Physical Review. B, Condensed Matter and Materials Physics, Journal Name: Physical Review. B, Condensed Matter and Materials Physics Journal Issue: 13 Vol. 92; ISSN 1098-0121; ISSN PRBMDO

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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