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We have investigated the origin of the magnetic dipole correlations $\langle \sigma_{\boldsymbol{Q}}^z \sigma_{\boldsymbol{-Q}}^z \rangle$ characterized by the modulation wave vector $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ observed in the frustrated pyrochlore magnet Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$. This magnetic short-range order cannot be accounted for by adding further-neighbor exchange interactions to the nearest-neighbor pseudospin-$\tfrac{1}{2}$ Hamiltonian for quantum pyrochlore magnets. Using classical Monte Carlo simulation and quantum simulation based on thermally pure quantum (TPQ) states we have shown that the spin correlations with $\boldsymbol{k} \sim (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$ are induced at low temperatures by a three-spin interaction of a form $\sigma_{\boldsymbol{r}}^{\pm} \sigma_{\boldsymbol{r}^{\prime}}^z \sigma_{\boldsymbol{r}^{\prime \prime}}^z $, which is a correction to the Hamiltonian due to the low crystal-field excitation. Simulations using TPQ states have shown that the spin correlations coexist with electric quadrupole correlations $\langle \sigma_{\boldsymbol{Q}}^{\alpha} \sigma_{\boldsymbol{-Q}}^{\beta} \rangle$ ($\alpha, \beta = x, y$) with $\boldsymbol{k} \sim \boldsymbol{0}$. These results suggest that the putative quantum spin liquid state of Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ is located close to phase boundaries of the spin-ice, quadrupole-ordered, and magnetic-ordered states in the classical approximation, and that the three-spin interaction brings about a quantum disordered ground state with both spin and quadrupole correlations., Comment: 28 pages, 25 figures

Spin correlations of the frustrated pyrochlore oxide Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ have been investigated by using inelastic neutron scattering on single crystalline samples ($x=-0.007, 0.000,$ and $0.003$), which have the putative quantum-spin-liquid (QSL) or electric-quadrupolar ground states. Spin correlations, which are notably observed in nominally elastic scattering, show short-ranged correlations around $L$ points [$q = (\tfrac{1}{2},\tfrac{1}{2},\tfrac{1}{2})$], tiny antiferromagnetic Bragg scattering at $L$ and $\Gamma$ points, and pinch-point type structures around $\Gamma$ points. The short-ranged spin correlations were analyzed using a random phase approximation (RPA) assuming the paramagnetic state and two-spin interactions among Ising spins. These analyses have shown that the RPA scattering intensity well reproduces the experimental data using temperature and $x$ dependent coupling constants of up to 10-th neighbor site pairs. This suggests that no symmetry breaking occurs in the QSL sample, and that a quantum treatment beyond the semi-classical RPA approach is required. Implications of the experimental data and the RPA analyses are discussed., Comment: 13 pages, 11 figures

We have studied long range orders of electric quadrupole moments described by an effective pseudospin-$\frac{1}{2}$ Hamiltonian representing pyrochlore magnets with non-Kramers ions under [111] magnetic field, in relevance to Tb$_{2}$Ti$_{2}$O$_{7}$. Order parameters and phase transitions of this frustrated system are investigated using classical Monte-Carlo simulations. In zero field, the model undergoes a first-order phase transition from a paramagnetic state to an ordered state with an antiparallel arrangement of pseudospins. This pseudospin order is characterized by the wavevector $\boldsymbol{k}=0$ and is selected by an energetic or an order-by-disorder mechanism from degenerate $\boldsymbol{k}=(h,h,h)$ mean-field orders. Under [111] magnetic field this three-dimensional quadrupole order is transformed to a quasi two-dimensional quadrupole order on each kagom\'{e} lattice separated by field-induced ferromagnetic triangular lattices. We discuss implication of the simulation results with respect to experimental data of Tb$_{2}$Ti$_{2}$O$_{7}$., Comment: 11 pages, 10 figures; Fig. 1 and Eqs. (A1), (A2), (A3) are corrected (v3)

The ground states of the frustrated pyrochlore oxide Tb$_{2+x}$Ti$_{2-x}$O$_{7+y}$ have been studied by inelastic neutron scattering experiments. Three single-crystal samples are investigated; one shows no phase transition ($x=-0.007