Dipolar spin ice regime proximate to an all-in-all-out N\'{e}el ground state in the dipolar-octupolar pyrochlore Ce2_2Sn2_2O7_7

The dipolar-octupolar (DO) pyrochlores, R$_2$M$_2$O$_7$ (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. We present neutron diffraction measurements on newly synthesized hydrothermally-grown Ce$_2$Sn$_2$O$_7$ powders that show a broad signal at low scattering vectors, reminiscent of a dipolar spin ice. This is strikingly different from previous neutron diffraction on powder samples grown from solid-state synthesis, which found diffuse scattering at high scattering vectors associated with magnetic octupoles. This raises the question about subtle crystalline structural differences and in particular the potential role of disorder that is present in the different samples. We quantify any differences through complementary neutron structure refinement and atomic PDF measurements but detect no oxidation or other crystallographic disorder in the hydrothermally-grown samples. To interpret the new diffuse scattering, we characterize the exchange interaction parameters in the near-neighbor XYZ model Hamiltonian associated with DO pyrochlores by fitting quantum numerical linked cluster expansions (NLCE) to heat capacity and magnetic susceptibility measurements, and classical Monte Carlo calculations to the diffuse neutron diffraction of the newly synthesized Ce$_2$Sn$_2$O$_7$ samples. This places Ce$_2$Sn$_2$O$_7$'s ground state within the ordered dipolar all-in-all-out (AIAO) N\'{e}el phase with quantum Monte-Carlo calculations showing a transition to long-range order at temperatures below those accessed experimentally. We conclude that new hydrothermally-grown Ce$_2$Sn$_2$O$_7$ samples host a finite-temperature proximate dipolar spin ice phase, above the expected transition to AIAO N\'{e}el order.Comment: 11 pages, 11 figure

Quantum Spin Ice Response to a Magnetic Field in the Dipole-Octupole Pyrochlore Ce2_2Zr2_2O7_7

We report new heat capacity measurements on single crystal Ce$_2$Zr$_2$O$_7$ down to $\sim$ 0.1 K in a magnetic field along the $[1,\bar{1}, 0]$ direction. These new 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 humps by the $[1,\bar{1}, 0]$ field at $\sim$ 2 T. 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 ($\alpha$-chains) is polarized by the field while the other ($\beta$-chains) remains free. Our theoretical modelling suggests that the $\beta$-chains are close to a critical state, with nearly-gapless excitations. We also report new elastic and inelastic neutron scattering measurements on single crystal Ce$_2$Zr$_2$O$_7$ in $[1, \bar{1}, 0]$ and $[0, 0, 1]$ magnetic fields at temperatures down to 0.03 K. The elastic scattering behaves consistently with the formation of independent chains for a $[1, \bar{1}, 0]$ field, while the $[0, 0, 1]$ field produces a single field-induced magnetic Bragg peak at $(0, 2, 0)$ and equivalent wavevectors, indicating a polarized spin ice for fields above $\sim$ 3 T. For both $[1, \bar{1}, 0]$ and $[0, 0, 1]$ 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 modelling 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 Ce$_2$Zr$_2$O$_7$ and the smallness of the parameter $\theta$ which controls the mixing between dipolar and octupolar degrees of freedom. These results support previous estimates of the microscopic exchange parameters.Comment: 20 pages, 10 figure

Reply to "Comment on: 'Case for a U(1)π_\pi Quantum Spin Liquid Ground State in the Dipole-Octupole Pyrochlore Ce2Zr2O7\mathrm{Ce}_2\mathrm{Zr}_2\mathrm{O}_7' "

In his comment [arXiv:2209.03235], S. W. Lovesey argues that our analysis of neutron scattering experiments performed on Ce$_2$Zr$_2$O$_7$ is invalid. Lovesey argues that we have not properly accounted for the higher-order multipolar contributions to the magnetic scattering and that our use of pseudospin-$1/2$ operators to describe the scattering is inappropriate. In this reply, we show that the multipolar corrections discussed by Lovesey only become significant at scattering wavevectors exceeding those accessed in our experiments. This in no way contradicts or undermines our work, which never claimed a direct observation of scattering from higher-order multipoles. We further show that Lovesey's objections to our use of pseudospins are unfounded, and that the pseudospin operators are able to describe all magnetic scattering processes at the energy scale of our experiments, far below the crystal field gap. Finally, we comment on certain assumptions in Lovesey's calculations of the scattering amplitude which are inconsistent with experiment.Comment: 6 pages, 1 figur

Measurement of the Spectral Shape of the beta-decay of 137Xe to the Ground State of 137Cs in EXO-200 and Comparison with Theory

We report on a comparison between the theoretically predicted and experimentally measured spectra of the first-forbidden non-unique $\beta$-decay transition ^{137}\textrm{Xe}(7/2^-)\to\,^{137}\textrm{Cs}(7/2^+). The experimental data were acquired by the EXO-200 experiment during a deployment of an AmBe neutron source. The ultra-low background environment of EXO-200, together with dedicated source deployment and analysis procedures, allowed for collection of a pure sample of the decays, with an estimated signal-to-background ratio of more than 99-to-1 in the energy range from 1075 to 4175 keV. In addition to providing a rare and accurate measurement of the first-forbidden non-unique $\beta$-decay shape, this work constitutes a novel test of the calculated electron spectral shapes in the context of the reactor antineutrino anomaly and spectral bump.Comment: Version as accepted by PR