Direct Observation of Electric-quadrupolar Order in UO2

Abstract

We report direct experimental evidence for long-range antiferro ordering of the electricquadrupole moments on the U ions. Resonant x-ray scattering experiments at the uranium M4 absorption edge show a characteristic dependence in the integrated intensity upon rotation of the crystal around the scattering vector. Although quadrupolar order in uranium dioxide was advocated already in the 1960s no experimental evidence for this phenomenon was provided until now. We conclude with a possible model to explain the phase diagram of the solid solutions of UO2 and NpO2. We suggest that in the region 0.30 < x < 0.75 neither the transverse nor the longitudinal quadrupole ordering can dominate, leading to frustration and only short-range ordering.