Single-Crystal Diffuse Neutron Scattering Study of the Dipole-Octupole Quantum Spin-Ice Candidate Ce2Zr2O7: No Apparent Octupolar Correlations Above T=0.05 K

The insulating magnetic pyrochlore ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ has gained attention as a quantum spin-ice candidate with dipole-octupole character that arises from the crystal-electric-field ground-state doublet for the ${\mathrm{Ce}}^{3+}$ Kramers ion. This dipole-octupole character permits both spin-ice phases based on magnetic dipoles and those based on more-exotic octupoles. This work reports low-temperature neutron diffraction measurements on single-crystal ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ with $Q$ coverage both at low $Q$ , where the magnetic form factor for dipoles is near maximal, and at high $Q$ , covering the region where the magnetic form factor for ${\mathrm{Ce}}^{3+}$ octupoles is near maximal. This study was motivated by recent powder neutron diffraction studies of other Ce-based dipole-octupole pyrochlores, ${\mathrm{Ce}}_2{\mathrm{Sn}}_2{\mathrm{O}}_7$ and ${\mathrm{Ce}}_2{\mathrm{Hf}}_2{\mathrm{O}}_7$ , which each showed temperature-dependent diffuse diffraction at high $Q$ , 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 ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ . 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 ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ , ${\mathrm{Ce}}_2{\mathrm{Sn}}_2{\mathrm{O}}_7$ , and ${\mathrm{Ce}}_2{\mathrm{Hf}}_2{\mathrm{O}}_7$ . 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 ( $T=0.05\mathrm{K}$ ), scattering from octupolar correlations in ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ is not present in the neutron diffraction signal on the level of our observation threshold of around 0.1% of the low- $Q$ dipole scattering. We compare these results to those obtained earlier on powder ${\mathrm{Ce}}_2{\mathrm{Sn}}_2{\mathrm{O}}_7$ and ${\mathrm{Ce}}_2{\mathrm{Hf}}_2{\mathrm{O}}_7$ , and to low-energy inelastic neutron scattering from single-crystal ${\mathrm{Ce}}_2{\mathrm{Zr}}_2{\mathrm{O}}_7$ .