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
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| Main Authors: | , , , , , , , , , , |
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| Format: | Preprint |
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2024
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| _version_ | 1866912354057322496 |
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| author | Smith, E. M. Schäfer, R. Dudemaine, J. Placke, B. Yuan, B. Morgan, Z. Ye, F. Moessner, R. Benton, O. Bianchi, A. D. Gaulin, B. D. |
| author_facet | Smith, E. M. Schäfer, R. Dudemaine, J. Placke, B. Yuan, B. Morgan, Z. Ye, F. Moessner, R. Benton, O. Bianchi, A. D. Gaulin, B. D. |
| contents | 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. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2407_07640 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | 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 Smith, E. M. Schäfer, R. Dudemaine, J. Placke, B. Yuan, B. Morgan, Z. Ye, F. Moessner, R. Benton, O. Bianchi, A. D. Gaulin, B. D. Strongly Correlated Electrons 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. |
| title | 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 |
| topic | Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2407.07640 |