LiCu2O2 is the first multiferroic cuprate to be reported and its ferroelectricity is induced by complex magnetic ordering in ground state, which is still in controversy today. Herein, we have grown nearly untwinned LiCu2O2 single crystals of high quality and systematically investigated their dielectric and ferroelectric behaviours in external magnetic fields. The highly anisotropic response observed in different magnetic fields apparently contradicts the prevalent bc- or ab- plane cycloidal spin model. Our observations give strong evidence supporting a new helimagnetic picture in which the normal of the spin helix plane is along the diagonal of CuO4 squares which form the quasi-1D spin chains by edge-sharing. Further analysis suggests that the spin helix in the ground state is elliptical and in the intermediate state the present c-axis collinear SDW model is applicable with some appropriate modifications. In addition, our studies show that the dielectric and ferroelectric measurements could be used as probes for the characterization of the complex spin structures in multiferroic materials due to the close tie between their magnetic and electric orderings.
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