Magnetoelectric and structural properties of Y2CoMnO6: The role of antisite defects

We have carried out an investigation on the magnetoelectric properties of the presumed multiferroic Y2CoMnO6 with different degrees of Co/Mn atomic ordering. The magnetic ground state was studied by neutron diffraction, showing a collinear ferromagnetic (FM) ordering of Co and Mn moments with a small antiferromagnetic canting. No superstructure peaks from an E-type magnetic structure were detected in our measurements. Magnetic measurements reveal FM transitions with pinned magnetic domains. The degree of Co/Mn ordering affects the Curie temperature only a little, but has strong effects on the magnetic hysteresis loops, and the FM moment signal at high field increases with increasing such order. The loops display steps at critical fields whose number and extent depends on each specimen. The most ordered sample exhibits the greatest steps ascribed to the alignment of magnetic domains separated by antiphase boundaries. All samples are insulators exhibiting low dielectric loss and dielectric constants at low temperature. On warming, they show a step increase in the real dielectric permittivity accompanied by peaks in the dielectric loss typical of thermally activated hopping processes. At room temperature, the huge values of the dielectric constant reveal the presence of Maxwell-Wagner depletion layers. Pyroelectric measurements reveal a high polarization at low temperature for these compounds that increases with increasing the Co/Mn ordering. There is no correlation between the magnetic transition and the onset of pyroelectric current. No significant changes are observed in the pyroelectric effect measured under an external magnetic field, so magnetoelectric coupling is negligible. This paper identifies the pyroelectric current as thermally stimulated depolarization current ascribed to the reorientation of defect dipoles with activation energy of about 0.05 eV. Therefore, no ferroelectric transition occurs in these compounds, discarding the existence of intrinsic magnetoelectric multiferroicity.
For financial support we thank the Spanish Ministerio de Economía y Competitividad (MINECO) (Projects No. MAT2012-38213-C02-01 and -02 and No. MAT2015-68760-C1-1 and -2-P, cofunded by the European Regional Development Fund [ERDF] from the European Union) and Diputación General de Aragón (DGA, project E-69). J.A. Rodríguez-Velamazan acknowledges CSIC for the JAEdoc contract.