Benedikt Placke

Abstract:

The dipolar-octupolar (DO) pyrochlores, R2M2O7 (R=Ce,Sm,Nd), are key players in the search for realizable novel quantum spin liquid (QSL) states as a large parameter space within the DO pyrochlore phase diagram is theorized to host QSL states of both dipolar and octupolar nature. New single crystals and powders of Ce2Sn2O7, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce2Sn2O7 using the near-neighbor XYZ model Hamiltonian associated with DO pyrochlores. Utilizing quantum numerical linked cluster expansion fits to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the new hydrothermally grown Ce2Sn2O7 samples, we place Ce2Sn2O7's ground state within the ordered dipolar all-in-all-out (AIAO) Néel phase, with quantum Monte Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce2Sn2O7 powders show a broad signal at low scattering wave vectors, reminiscent of a dipolar spin ice, in striking contrast from previous powder neutron diffraction on samples grown from solid-state synthesis, which found diffuse scattering at high scattering wave vectors associated with magnetic octupoles and suggested an octupolar quantum spin ice state. We conclude that new hydrothermally grown Ce2Sn2O7 samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO Néel order.

Abstract:

We propose a simple family of valence-bond crystals as potential ground states of the S=1/2 and S=1 Heisenberg antiferromagnet on the pyrochlore lattice. Exponentially numerous in the linear size of the system, these can be visualized as hard-hexagon coverings, with each hexagon representing a resonating valence-bond ring. This ensemble spontaneously breaks rotation, inversion, and translation symmetries. A simple, yet accurate, variational wave function allows a precise determination of the energy, confirmed by the density matrix renormalization group and numerical linked cluster expansion, and extended by an analysis of excited states. The identification of the origin of the stability indicates applicability to a broad class of frustrated lattices, which we demonstrate for the checkerboard and ruby lattices. Our work suggests a perspective on such quantum magnets, in which unfrustrated motifs are effectively uncoupled by the frustration of their interactions.

Abstract:

The pyrochlore magnet Ce2Zr2O7 has attracted much attention as a quantum spin ice candidate whose novelty derives in part from the dipolar-octupolar nature of the Ce3+ pseudospin-1/2 degrees of freedom it possesses. We report heat capacity measurements on single crystal samples of Ce2Zr2O7 down to T∼0.1K in a magnetic field along the [1,1¯,0] direction. These measurements show that the broad hump in the zero-field heat capacity moves higher in temperature with increasing field strength and is split into two separate humps by the [1,1¯,0] magnetic field at ∼2T. These separate features are due to the decomposition of the pyrochlore lattice into effectively decoupled chains for fields in this direction: One set of chains (α chains) is polarized by the field while the other (β chains) remains free. This situation is similar to that observed in the classical spin ices Ho2Ti2O7 and Dy2Ti2O7, but with the twist that here the strong transverse exchange interactions produce substantial quantum effects. Our theoretical modeling suggests that the β chains are close to a critical state, with nearly-gapless excitations. We also report elastic and inelastic neutron scattering measurements on single crystal Ce2Zr2O7 in [1,1¯,0] and [0,0,1] magnetic fields at temperatures down to T=0.03K. The elastic scattering behaves consistently with the formation of independent chains for a [1,1¯,0] field, while the [0,0,1] field produces a single field-induced elastic magnetic Bragg peak at (0,2,0) and equivalent wavevectors, indicating a polarized spin ice state for fields above ∼3T. For both [1,1¯,0] and [0,0,1] magnetic fields, our inelastic neutron scattering results show an approximately-dispersionless continuum of scattering that increases in both energy and intensity with increasing field strength. By modeling the complete set of experimental data using numerical linked cluster and semiclassical molecular dynamics calculations, we demonstrate the dominantly multipolar nature of the exchange interactions in Ce2Zr2O7 and the smallness of the parameter θ, which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters and place strong constraints on the theoretical description of this prominent spin ice candidate.

Abstract:

We analyze the thermodynamic properties of the random-bond Ising model (RBIM) on closed hyperbolic surfaces using Monte Carlo and high-temperature series expansion techniques. We also analyze the dual-RBIM, that is, the model that in the absence of disorder is related to the RBIM via the Kramers-Wannier duality. Even on self-dual lattices this model is different from the RBIM, unlike in the Euclidean case. We explain this anomaly by a careful rederivation of the Kramers-Wannier duality. For the (dual-)RBIM, we compute the paramagnet-to-ferromagnet phase transition as a function of both temperature T and the fraction of antiferromagnetic bonds p. We find that as temperature is decreased in the RBIM, the paramagnet gives way to either a ferromagnet or a spin-glass phase via a second-order transition compatible with mean-field behavior. In contrast, the dual-RBIM undergoes a strongly first-order transition from the paramagnet to the ferromagnet both in the absence of disorder and along the Nishimori line. We study both transitions for a variety of hyperbolic tessellations and comment on the role of coordination number and curvature. The extent of the ferromagnetic phase in the dual-RBIM corresponds to the correctable phase of hyperbolic surface codes under independent bit- and phase-flip noise.