Single Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin Ice Candidate Ce${}_2$Zr${}_2$O${}_7$: No Apparent Octupolar Correlations Above $T=0.05$ K

Abstract

The insulating magnetic pyrochlore Ce${}_2$Zr${}_2$O${}_7$ has gained attention as a quantum spin ice candidate with dipole-octupole character arising from the crystal electric field ground state doublet for the Ce${}^{3+}$ ion. This permits both spin ice phases based on magnetic dipoles and those based on more-exotic octupoles. We report low-temperature neutron diffraction measurements on single crystal Ce${}_2$Zr${}_2$O${}_7$ with $Q$-coverage both at low $Q$ where the magnetic form factor for dipoles is near maximal and at high $Q$ where the magnetic form factor for Ce${}^{3+}$ octupoles is near maximal. This study was motivated by recent powder neutron diffraction studies of other Ce-based dipole-octupole pyrochlores, Ce${}_2$Sn${}_2$O${}_7$ and Ce${}_2$Hf${}_2$O${}_7$, which each showed temperature-dependent diffuse diffraction at high $Q$ that was interpreted as arising from octupolar correlations. Our measurements use an optimized single crystal diffuse scattering instrument that allows us to screen against strong Bragg scattering from Ce${}_2$Zr${}_2$O${}_7$. The temperature-difference neutron diffraction reveals a low-$Q$ peak consistent with dipolar spin ice correlations reported in previous work, and an alternation between positive and negative net intensity at higher $Q$. These features are consistent with our numerical-linked-cluster calculations using pseudospin interaction parameters previously reported for Ce${}_2$Zr${}_2$O${}_7$, Ce${}_2$Sn${}_2$O${}_7$, and Ce${}_2$Hf${}_2$O${}_7$. Importantly, neither the measured data nor any of the NLC calculations show evidence for increased scattering at high $Q$ resulting from octupolar correlations. We conclude that at the lowest attainable temperature for our measurements ($T=0.05$ K), scattering from octupolar correlations in Ce${}_2$Zr${}_2$O${}_7$ is not present in the neutron diffraction signal on the level of our observation threshold of ~ 0.1 % of the low-$Q$ dipole scattering.

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• Thermodynamics of the Heisenberg antiferromagnet on the maple-leaf lattice
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