Disorder-induced proximate quantum spin ice phase in Pr$_2$Sn$_2$O$_7$
Yi Luo, Joseph A. M. Paddison, Brenden R. Ortiz, Miles Knudtson, Stephen D. Wilson, Jue Liu, Benjamin A. Frandsen, Si Athena Chen, Matthias Frontzek, Andrey Podlesnyak, Adam A. Aczel
公開日: 2025/8/26
Abstract
We report a comprehensive bulk characterization and neutron scattering investigation of single-crystalline Pr$_2$Sn$_2$O$_7$, a magnetic pyrochlore synthesized via a flux-growth method. Unpolarized neutron diffuse scattering reveals the emergence of spin-ice correlations below $T \sim 1$ 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 $T_f \approx 0.15$ 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 $T_f$. Meanwhile, an incipient (100)-type magnetic order begins to nucleate, and a gapped excitation centered at $\hbar\omega = 0.23$ meV persists. We further identify two distinct dynamical timescales above $T_f$, a slow component $\tau_{\mathrm{slow}} \sim 10^{-5}$ s and a fast component $\tau_{\mathrm{fast}} \sim 10^{-10}$ s, in quantitative agreement with theoretical predictions for QSI systems. Taken together, these results indicate that Pr$_2$Sn$_2$O$_7$ enters a disorder-induced spin-frozen phase below $T_f$, lying in close proximity to a $U(1)$ quantum spin liquid.