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Disorder-induced proximate quantum spin ice phase in Pr2Sn2O7

We report a comprehensive bulk characterization and neutron scattering investigation of single-crystalline Pr2Sn2O7, a magnetic pyrochlore synthesized via a flux-growth method. Unpolarized neutron diffuse scattering reveals the emergence of spin-ice correlations below T ∼ 1 K, evidenced by the development of anisotropic pinch-point features that are consistent with quantum-spin-ice (QSI) behavior. A.C. susceptibility measurements indicate a progressive slowing of spin dynamics in this regime, culminating in complete spin freezing below Tf ≈ 0.15 K. Inelastic neutron scattering at T = 0.5 K reveals a broad spectrum of quasi-elastic magnetic excitations, with intensity in the low-energy range [0, 0.2] meV significantly suppressed below Tf. Meanwhile, an incipient (100)-type magnetic order begins to nucleate, and a gapped excitation centered at ℏω = 0.23 meV persists. We further identify two distinct dynamical timescales above Tf , a slow component τ_slow ∼ 10^−5 s and a fast component τ_fast ∼ 10^−10 s, in quantitative agreement with theoretical predictions for QSI systems. Taken together, these results indicate that Pr2Sn2O7 enters a disorder-induced spin-frozen phase below Tf , lying in close proximity to a U(1) quantum spin liquid

Luo, Yi [ORNL] (ORCID:000900048710428X)↗

Materials Data on Pr2Sn2O7 by Materials Project

Pr2Sn2O7 crystallizes in the cubic Fd-3m space group. The structure is three-dimensional. Pr3+ is bonded in a distorted body-centered cubic geometry to eight O2- atoms. There are two shorter (2.33 Å) and six longer (2.62 Å) Pr–O bond lengths. Sn4+ is bonded to six equivalent O2- atoms to form corner-sharing SnO6 octahedra. The corner-sharing octahedral tilt angles are 50°. All Sn–O bond lengths are 2.10 Å. There are two inequivalent O2- sites. In the first O2- site, O2- is bonded to four equivalent Pr3+ atoms to form OPr4 tetrahedra that share corners with sixteen OPr4 tetrahedra and edges with six equivalent OPr2Sn2 tetrahedra. In the second O2- site, O2- is bonded to two equivalent Pr3+ and two equivalent Sn4+ atoms to form a mixture of distorted corner and edge-sharing OPr2Sn2 tetrahedra.

36 MATERIALS SCIENCE↗