Nuclear spin driven quantum relaxation in LiY₀.998Ho₀.002F₄

Staircase hysteresis loops of the magnetization of a LiY_0.998Ho_0.002F_4 single crystal are observed at subkelvin temperatures and low field sweep rates. This behavior results from quantum dynamics at avoided level crossings of the energy spectrum of single Ho^{3+} ions in the presence of hyperfine interactions. Enhanced quantum relaxation in constant transverse fields allows the study of the relative magnitude of tunnel splittings. At faster sweep rates, non-equilibrated spin-phonon and spin-spin transitions, mediated by weak dipolar interactions, lead to magnetization oscillations and additional steps.