The ground state of the quantum spin ice candidate magnet Yb2Ti2O7 is known to be sensitive to weak disorder at the ∼ 1 % level which occurs in single crystals grown from the melt. Powders produced by solid state synthesis tend to be stoichiometric and display large and sharp heat capacity anomalies at relatively high temperatures, TC ∼ 0.26 K. We have carried out neutron elastic and inelastic measurements on well characterized and equilibrated stoichiometric powder samples of Yb2Ti2O7 which show resolution-limited Bragg peaks to appear at low temperatures, but whose onset correlates with temperatures much higher than TC . The corresponding magnetic structure is best described as an ice-like splayed ferromagnet. The spin dynamics in Yb2Ti2O7 are shown to be gapless on an energy scale < 0.09 meV at all temperatures, and organized into a continuum of scattering with vestiges of highly overdamped ferromagnetic spin waves present. These excitations differ greatly from conventional spin waves predicted for Yb2Ti2O7's mean field ordered state, but appear robust to weak disorder as they are largely consistent with those displayed by nonstoichiometric crushed single crystals and single crystals, as well as by powder samples of Yb2Ti2O7's sister quantum magnet Yb2Sn2O7.

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 Yb2Ti2O7. 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, ≈ 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 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 CEF transitions out of the GS, and the GS 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 CEF lifetime as is induced in stoichiometric Yb2Ti2O7 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 Yb2+xTi2−xO7+y, in addition to producing a small fraction of Yb-ions in defective environments with grossly different CEF eigenvalues and eigenvectors.

Neutron scattering measurements on the pyrochlore magnet Ce2Zr2O7 reveal an unusual crystal field splitting of its lowest J = 5/2 multiplet, such that its ground state doublet is composed of mJ = ± 3/2, giving these doublets a dipole -octupole (DO) character with local Ising anisotropy. Its magnetic susceptibility shows weak antiferromagnetic correlations with θCW = -0.4(2) K, leading to a naive expectation of an All-In, All-Out ordered state at low temperatures. Instead our low energy inelastic neutron scattering measurements show a dynamic quantum spin ice state, with suppressed scattering near |Q| = 0, and no long range order at low temperatures. This is consistent with recent theory predicting symmetry enriched U(1) quantum spin liquids for such DO doublets decorating the pyrochlore lattice. Finally, we show that disorder, especially oxidation of powder samples, is important in Ce2Zr2O7 and could play an important role in the low temperature behaviour of this material.The rare-earth pyrochlore oxides R 2 B 2 O 7 , where R 3+ and B 4+ consist generally of rare earth and transitionmetal ions respectively, display a wealth of both exotic and conventional magnetic ground states. Their R 3+ ions decorate a network of corner-sharing tetrahedra, one of the archetypes for geometrical frustration in three dimensions. Due to strong crystal electric field (CEF) effects, the nature of the magnetic interactions in such materials are strongly influenced by their single-ion physics [1][2][3]. A naive theoretical description of the magnetic interactions in rare-earth pyrochlores is generally performed by introducing an ad hoc effective single-ion term in addition to Heisenberg exchange interactions. For example, Heisenberg antiferromagnetism with an effective Ising anisotropy leads to non-frustrated All-In, All-Out (AIAO) magnetic order, as seen in several heavy rare earth iridate pyrochlores [4,5] and illustrated in the insert to Fig.1(a). Heisenberg ferromagnetism and an effective Ising anisotropy give rise to a classical spin ice ground state [6], as seen in (Ho,Dy) 2 Ti 2 O 7 [7, 8] and illustrated as the 2I2O local structure in the inset to Fig.1(a). However, to capture all the physics that can arise at low temperatures, the magnetic interactions should be projected into pseudo-spin operators acting solely on the low energy CEF states [3,[9][10][11][12][13]. This procedure has been applied for example in the Yb 3+ [11,14,15] and Er 3+ [12, 16-18] XY pyrochlores where CEF effects give rise to effective S = 1/2 quantum degrees of freedom that interact via anisotropic exchange interactions.More recently, it has been realized that the precise composition of the ground state crystal field doublets in rare-earth pyrochlores is crucial in determining the form of the microscopic Hamiltonian, and in itself, diversifies the possibility of quantum magnetic states [3,19]. This has been appreciated for some time in the case of non-Kramers doublets, based on magnetic ions with an even number of electrons such as the 4f 2 configuratio...