Internal magnetic field effect on magnetoelectricity in orthorhombic RMnO₃ crystals

We have investigated the role of the 4$f$ moment on the magnetoelectric (ME) effect of orthorhombic $R$MnO$_{3}$ ($R$=rare earth ions). In order to clarify the role of the 4$f$ moment, we prepared three samples: (Eu,Y)MnO$_{3}$ without the 4$f$ moment, TbMnO$_{3}$ with the anisotropic 4$f$ moment, and (Gd,Y)MnO$_{3}$ with the isotropic 4$f$ moment. The ferroelectric behaviors of these samples are different from each other in a zero magnetic field. (Eu,Y)MnO$_{3}$ and (Gd,Y)MnO$_{3}$ show the ferroelectric polarization along the a axis in the ground state, while TbMnO$_{3}$ shows it along the c axis. Such difference may arise from the influence of the anisotropic Tb$^{3+}$ 4$f$ moment. The direction of the ferroelectric polarization of $R$MnO$_{3}$ is determined by the internal magnetic field arising from the 4$f$ moment.