Independent ferroelectric contributions and rare-earth-induced polarization reversal in multiferroic TbMn2O5

Three independent contributions to the magnetically induced spontaneous polarization of multiferroic TbMn2O5 are uniquely separated by optical second harmonic generation and an analysis in terms of Landau theory. Two of them are related to the magnetic Mn3+/4+ order and are independent of applied fields of up to 7 T. The third contribution is related to the long-range antiferromagnetic Tb3+ order. It shows a drastic decrease upon the application of a magnetic field and mediates the change of sign of the spontaneous electric polarization in TbMn2O5. The close relationship between the rare-earth long-range order and the non-linear optical properties points to isotropic Tb-Tb exchange and oxygen spin polarization as mechanism for this rare-earth induced ferroelectricity.