Studies of Multiferroic System LiCu2O2 I Sample Characterization and Relationship between Magnetic Properties and Multiferroic Nature

Single-crystal samples of LiCu2O2 with spin 1/2 Cu2+ chains of edge-sharing CuO4 square planes (ribbon chains), have been characterized by X-ray diffraction, thermogravimetric analysis, and magnetic measurements. Neither the atomic deficiency nor the mixing of Cu and Li atoms has been found, indicating that lattice defects conceived as a possible origin of the reported multiferroic behavior can be excluded. Anomalies found in the data of specific heat and neutron magnetic Bragg reflections show clear evidence that the system exhibits successive magnetic transitions at TN1=24.5 K and TN2=22.8 K. Based on the magnetic structures in the intermediate (TN2<T<TN1) and low temperature (T<TN2) phases, determined by the combined studies of neutron scattering and 7Li-NMR measurements, we can consistently understand the fact that the multiferroic properties are observed only below TN2 by considering existing theories.