Neutron Spectroscopic Study of Crystalline Electric Field Excitations in Stochiometric and Lightly Stuffed Yb2Ti2O7

Abstract

Time-of-flight neutron spectroscopy has been used to determine the crystalline electric field (CEF) Hamiltonian, eigenvalues and eigenvectors appropriate to the $J$ = 7/2 Yb${}^{3+}$ ion in the candidate quantum spin ice pyrochlore magnet $\mathrm{Y}{\mathrm{b}}_2\mathrm{T}{\mathrm{i}}_2{\mathrm{O}}_7$. The precise ground state (GS) 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, $\approx$ 2\%, of the non-magnetic Ti${}^{4+}$ sites are occupied by excess Yb${}^{3+}$. We have carried out neutron spectroscopic measurements on a stoichiometric powder sample of Yb${}_2$Ti${}_2$O${}_7$, as well as a crushed single crystal with weak stuffing and an approximate composition of Yb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$ with $x$ = 0.046. All samples display three CEF transitions out of the GS, and the GS doublet itself is identified as primarily composed of m${}_J$ = $\pm$1/2, as expected. However,"stuffing" at low temperatures in Yb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$ induces a similar finite CEF lifetime as is induced in stoichiometric Yb${}_2$Ti${}_2$O${}_7$ by elevated temperature. We conclude that an extended strain field exists about each local "stuffed" site, which produces a distribution of random CEF environments in the lightly stuffed Yb${}_{2+x}$Ti${}_{2-x}$O${}_{7+y}$, in addition to producing a small fraction of Yb-ions in defective environments with grossly different CEF eigenvalues and eigenvectors.

11 pages, 9 figures, 4 tables

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