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Register a new userCrystal field states of Tb3+ in the pyrochlore spin liquid Tb2Ti2O7 from neutron spectroscopy
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We report time-of-flight neutron scattering measurements of the magnetic spectrum of Tb3+ in Tb2Ti2O7. The data, which extend up to 120 meV and have calibrated intensity, enable us to consolidate and extend previous studies of the single-ion crystal field spectrum. We successfully refine a model for the crystal field potential in Tb2Ti2O7 without relying on data from other rare earth titanate pyrochlores, and we confirm that the ground state is a non-Kramers doublet with predominantly |+/-4> components. We compare the model critically with earlier models.
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High resolution time-of-flight neutron scattering measurements on Tb2Ti2O7 reveal a rich low temperature phase diagram in the presence of a magnetic field applied along [110]. In zero field at T=0.4 K, terbium titanate is a highly correlated cooperative paramagnet with disordered spins residing on a pyrochlore lattice of corner-sharing tetrahedra. Application of a small field condenses much of the magnetic diffuse scattering, characteristic of the disordered spins, into a new Bragg peak characteristic of a polarized paramagnet. At higher fields, a magnetically ordered phase is induced, which supports spin wave excitations indicative of continuous, rather than Ising-like spin degrees of freedom.
We have studied the spin correlations with $bf{k}$= ($frac12$, $frac12$, $frac12$) propagation vector which appear below 0.4, K in tbti spin liquid by combining powder neutron diffraction and specific heat on Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ samples with $x$=0, 0.01, -0.01. The $bf{k}$= ($frac12$, $frac12$, $frac12$) order clearly appears on all neutron patterns by subtracting a pattern at 1.2(1),K. Refining the subtracted patterns at 0.07,K yields two possible spin structures, with spin-ice-like and monopole-like correlations respectively. Mesoscopic correlations involve Tb moments of 1 to 2 mub ordered on a length scale of about 20 AA. In addition, long range order involving a small spin component of 0.1 to 0.2 mub is detected for the $x$= 0 and 0.01 samples showing a peak in the specific heat. Comparison with previous single crystals data suggests that the ($frac12$, $frac12$, $frac12$) order settles in through nanometric spin textures with dominant spin ice character and correlated orientations, analogous to nanomagnetic twins.
In terms of a semi-phenomenological exchange charge model, we have obtained estimates of parameters of the crystal field and parameters of the electron-deformation interaction in terbium titanate Tb2Ti2O7 with a pyrochlore structure. The obtained set of parameters has been refined based on the analysis of spectra of neutron inelastic scattering and Raman light scattering, field dependences of the forced magnetostriction, and temperature dependences of elastic constants.
In a ferromagnet, the spin excitations are the well-studied magnons. In frustrated quantum magnets, long-range magnetic order fails to develop despite a large exchange coupling between the spins. In contrast to the magnons in conventional magnets, their spin excitations are poorly understood. Are they itinerant or localized? Here we show that the thermal Hall conductivity $kappa_{xy}$ provides a powerful probe of spin excitations in the quantum spin ice pyrochlore Tb$_2$Ti$_2$O$_7$. The thermal Hall response is large even though the material is transparent. The Hall response arises from spin excitations with specific characteristics that distinguish them from magnons. At low temperature ($T<$ 1 K), the thermal conductivity imitates that of a dirty metal. Using the Hall angle, we construct a phase diagram showing how the excitations are suppressed by a magnetic field.
We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) mu_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 mu_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.
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