Strong interplay between ferroelectric and magnetic orders in novel complex oxides

Multiferroics, where ferroelectric and magnetic orders are concurrently present, reveal new physical properties due to the strong interplay between the dual order parameters. The emergence of the unprecedented cross-coupling effects in such materials has offered a new vein of essential understanding of correlated spin and lattice degrees of freedom and the related macroscopic phenomena, and has invigorated the application in future generations of novel devices. Recently, the enhanced coupling has been discovered in the new class of materials called spin-driven ferroelectrics in which ferroelectric order originates from the exchange striction of special types of magnetic orders with broken inversion symmetry. However, the driven ferroelectric polarization appears to be minuscule, compared with that of the typical ferroelectrics. Thus, one of the demanding challenges of the multiferroics research is finding systems or ways to escalate the magnitude of polarization. Herein, we present discoveries of new multiferroics which exhibit giant ferroelectricity due to the new exchange striction mechanism through rare-earth and transition-metal ions and their strong tunability of polarization by applying magnetic fields. (1) New multiferroic of single-crystalline orthorhombic HoMnO3 was, for the first time, grown by the flux method. The crystals with incommensurate E-type magnetic structure exhibit much large ferroelectric polarization with the direction along the c-axis, completely different from the theoretical predictions. From the analysis, the polarization can be described by the new emerging mechanism of Ho-Mn exchange striction. (3) Tunable giant ferroelecric polarization in the multiferroic GdMn2O5 has been demonstrated. The ferroelectric polarization in this compound is found to be the largest and be varied repeatedly with the largest change by applying external magnetic fields among the spin-driven ferroelectrics known to date. In addition, contrary to the known origin for ferroelectricity in REMn2O5 (RE=rare earth ions), the Mn-Mn exchange striction mechanism, the complete magnetic structure constructed by the x-ray resonant scattering experiment clarify that the giant ferroelectricity in GdMn2O5 results mainly from the Gd-Mn symmetric exchange striction.Ph. D.Includes bibliographical referencesIncludes vitaby Nara Le