Abstract:
A polymorph of Cu2OSeO3 with the distorted kagome lattice was successfully obtained using the high-pressure synthesis technique (Cu2OSeO3-HP). Selected-area electron diffraction (SAED) and convergent-beam electron diffraction (CBED) measurements have been performed, and the space group was resolved as monoclinic P21/c. The structural analysis using X-ray and neutron powder diffraction suggests that the tetrahedral Cu2+ clusters [similar to those in Cu2OSeO3 ambient-pressure phase (Cu2OSeO3-AP)] exist in Cu2OSeO3-HP but with three symmetry inequivalent sites. No structural change was observed between 1.5 K and the room temperature. The complex magnetic H-T phase diagram was established based on the temperature- and field-dependent magnetization data, indicating two distinct antiferromagnetic phases at low and intermediate temperatures, in addition to the higher-temperature spin-glass-like phase. The low-temperature phase was identified by neutron powder diffraction refinements as a canted noncollinear antiferromagnetic order with a weak ferromagnetic component along the b-axis. A comparison of the local magnetic structure viewed along the distorted kagome lattice for Cu2OSeO3-AP and Cu2OSeO3-HP suggests that the partially released geometrical frustration by structural distortion strongly alters the magnetic order. Size of the refined ordered moment is ~1.00(4) μB in Cu2OSeO3-HP, indicating a large enhancement compared to that of Cu2OSeO3-AP (~0.61 μB). By applying a uniaxial stress, we observed finite enhancement of weak ferromagnetic component in the noncollinear antiferromagnetic phase in Cu2OSeO3-HP, which is the clear evidence of the piezomagnetic effect. Interestingly, the sign of the induced magnetization changes on heating from the low-temperature to the intermediate-temperature phases, indicating a novel piezomagnetic switching effect in this compound.