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Dipolar spin ice regime proximate to an all-in-all-out N\'{e}el ground state in the dipolar-octupolar pyrochlore Ce₂Sn₂O₇

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arxiv 2211.15140 v2 pith:3XP5OMN7 submitted 2022-11-28 cond-mat.str-el

Dipolar spin ice regime proximate to an all-in-all-out N\'{e}el ground state in the dipolar-octupolar pyrochlore Ce₂Sn₂O₇

classification cond-mat.str-el
keywords dipolarspingrownquantumdiffractionhydrothermallyneutronphase
verification ladder T0 review T1 audit T2 compute T3 formal T4 reserved
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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. New single crystals and powders of Ce$_2$Sn$_2$O$_7$, synthesized by hydrothermal techniques, present an opportunity for a new characterization of the exchange parameters in Ce$_2$Sn$_2$O$_7$ 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 Ce$_2$Sn$_2$O$_7$ samples, we place 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. Indeed, our new neutron diffraction measurements on the hydrothermally grown Ce$_2$Sn$_2$O$_7$ powders show a broad signal at low scattering wave vectors, reminiscent of a \textit{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 {\it octupoles} and suggested an octupolar quantum spin ice state. 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.

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