Liquidlike correlations in single-crystalline Y2Mo2O7: An unconventional spin glass

The spin-glass behavior of Y2Mo2O7 has remained a puzzle for nearly three decades. Free of bulk disorder within the resolution of powder diffraction methods, it is thought that this material is a rare realization of a spin glass resulting from weak disorder such as bond disorder or local lattice distortions. Here we report on the single-crystal growth of Y2Mo2O7. Using neutron scattering, we present isotropic magnetic diffuse scattering occurring below the spin-glass transition. Our attempts to model the diffuse scattering using a computationally exhaustive search of a class of simple spin Hamiltonians show no agreement with the experimentally observed energy-integrated (diffuse) neutron scattering. This suggests that spin degrees of freedom are insufficient to describe this system. Indeed, a T2 temperature dependence in the heat capacity and density functional theory calculations hint at the presence of a significant frozen degeneracy in both the spin and orbital degrees of freedom resulting from spin-orbital coupling (Kugel-Khomskii type) and random fluctuations in the Mo environment at the local level.