SR study of the dipole-octupole quantum spin ice candidate Ce2Zr2O7

The Ce3+ pseudospin-1/2 degrees of freedom in Ce2Zr2O7 possess both dipolar and octupolar character which enables the possibility of novel quantum spin liquid ground states in this material. Here we report muon spin relaxation and rotation (mu SR ) measurements on single-crystal samples of Ce2Zr2O7 in zero magnetic field and in magnetic fields directed along the [1, 1 over bar , 0] and [1, 1, 1] crystallographic directions, and for magnetic fields directed both longitudinal and transverse to the direction of muon polarization. Our zero-field results show no signs of magnetic ordering or spin freezing, consistent with earlier zero-field mu SR measurements on a powder sample of Ce2Zr2O7, and also with the expectations for a quantum spin ice. However, we measure a more gentle relaxation rate for Ce2Zr2O7 in zero field at low temperatures than was previously reported. This difference in relaxation rate is likely due to the low oxidation and, correspondingly, the high stoichiometry of our singlecrystal samples. Longitudinal field measurements confirm that the magnetic dipole moments in Ce2Zr2O7 remain dynamic at T = 0.1 K on the microsecond timescale. For both [1, 1 over bar , 0] and [1, 1, 1] magnetic fields, our mu SR Knight shift measurements show a field-induced leveling off of the magnetic susceptibility at low temperature which is qualitatively consistent with corresponding calculations using the numerical-linked-cluster method in combination with recent estimates for the nearest-neighbor exchange parameters of Ce2Zr2O7.