A review on current status and mechanisms of room-temperature magnetoelectric coupling in multiferroics for device applications

Single-phase multiferroic materials that allow the coexistence of ferroelectric and magnetic ordering above room temperature are highly desirable, motivating an ongoing search for mechanisms for unconventional ferroelectricity in magnetic oxides. Here, we report an antisite defect mechanism for room temperature ferroelectricity in epitaxial thin films of yttrium orthoferrite, YFeO3, a perovskite-structured canted antiferromagnet. A combination of piezoresponse force microscopy, atomically resolved elemental mapping with aberration corrected scanning transmission electron microscopy and density functional theory calculations reveals that the presence of YFe antisite defects facilitates a non-centrosymmetric distortion promoting ferroelectricity. This mechanism is predicted to work analogously for other rare earth orthoferrites, with a dependence of the polarization on the radius of the rare earth cation. Our work uncovers the distinctive role of antisite defects in providing a mechanism for ferroelectricity in a range of magnetic orthoferrites and further augments the functionality of this family of complex oxides for multiferroic applications.

/pdf/an-antisite-defect-mechanism-for-room-temperature-455r4scs2h.pdf

An antisite defect mechanism for room temperature ferroelectricity in orthoferrites.

Here, we report the possible origin of natural and magnetic field induced polar order near room temperature (RT) in $\mathrm{Pr}{\mathrm{Fe}}_{1/2}{\mathrm{Cr}}_{1/2}{\mathrm{O}}_{3}$. The temperature-dependent Raman spectroscopy (RS) and synchrotron x-ray diffraction experiments disregard any change in the structure at low temperatures, which is not compatible with the emergence of natural ferroelectricity in this sample. Further, inelastic neutron scattering, neutron Compton scattering, neutron resonance transmission analysis and magnetic field-dependent RS experiments, suggest an increase in the delocalization of ${\mathrm{Pr}}^{3+}$ ions in $\mathrm{Pr}{\mathrm{Fe}}_{1/2}{\mathrm{Cr}}_{1/2}{\mathrm{O}}_{3}$ with respect to the parent compound $\mathrm{PrFe}{\mathrm{O}}_{3}$. The evaluation of the present results reveals that more delocalized ${\mathrm{Pr}}^{3+}$ ions and strong spin-phonon coupling in $\mathrm{Pr}{\mathrm{Fe}}_{1/2}{\mathrm{Cr}}_{1/2}{\mathrm{O}}_{3}$ seem to be a driving force for the observed natural and magnetic field induced switchable polar order in $\mathrm{Pr}{\mathrm{Fe}}_{1/2}{\mathrm{Cr}}_{1/2}{\mathrm{O}}_{3}$. The present results provide a significant contribution in understanding the ferroelectric polarization and progress in the search for RT magnetodielectric materials.

Origin of natural and magnetic field induced polar order in orthorhombic Pr Fe 1 /2 Cr 1 /2 O 3

Morphology, structure and magnetic behavior of orthorhombic and hexagonal HoFeO3 synthesized via solution combustion approach

The magnetic behavior of a rare-earth orthoferrite ErFeO3 single crystal can be controlled by low magnetic fields from a few to hundreds of Oe. Here we investigated a high-quality ErFeO3 single crystal in the temperature range of 5-120 K, with two types of spin switching in the field-cooled-cooling (FCC) and field-cooled-warming (FCW) processes below the temperature of the spin reorientation (SR) transition from Γ4 to Γ2 at 98-88 K. The magnitude of the applied magnetic fields can regulate two types of spin switching along the a-axis of the ErFeO3 single crystal but does not affect the type and temperature range of the SR transition. An interesting "multi-step" type-II spin switching is observed in FCW under low magnetic fields (H < 18 Oe) just below the SR transition temperature, which is associated with the interaction and the change of magnetic configurations from rare-earth and iron magnetic sublattices. When the magnetic field is lower than 15 Oe, the type-II spin switching in the FCW process gradually changes to a continuous magnetic transition along the a-axis of the ErFeO3 single crystal. As the magnetic field is reduced to less than 17 Oe, the type-I spin switching in the FCW process also transforms into a continuous magnetic transition. Understanding the magnetic reversal effects will help us explore the potential applications of these magnetic materials for future information devices.

Low field control of spin switching and continuous magnetic transition in an ErFeO3 single crystal

The current scenario in multiferroics demands a breakthrough discovery of promising materials after ${\mathrm{BiFeO}}_{3}$. Recently, the controversial discovery of room temperature ferroelectricity (FE) in ${\mathrm{SmFeO}}_{3}$ [Lee et al., Phys. Rev. Lett. 107, 117201 (2011); Kuo et al., Phys. Rev. Lett. 113, 217203 (2014)] inspires the investigation of ${\mathrm{HoFeO}}_{3}$. Here we report a natural ferroelectric order around 210 K (${T}_{\text{FE}}$) along the $c$ axis with a reasonably large polarization of $\ensuremath{\sim}0.29\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{C}/{\mathrm{cm}}^{2}$ for a 10 kV/cm poling field. The strong magnetoelectric coupling of $\ensuremath{\sim}22$% is observed at 210 K at 30 kOe, below which it decreases with a further increase in magnetic field. The synchrotron and neutron diffraction results confirm that a shift of O atoms along the $c$ axis, on the polar $P{b}^{\ensuremath{'}}{n}^{\ensuremath{'}}{2}_{1}$ magnetic space, causes the FE in ${\mathrm{HoFeO}}_{3}$. The potential results of reasonably high ferroelectric polarization associated with a strong magnetoelectric coupling at higher temperature are fascinating and create a renewed attention for searching promising candidates with a natural ferroelectric order and higher ${T}_{\text{FE}}$ in the rest of the $R{\mathrm{FeO}}_{3}$ series.

/pdf/natural-ferroelectric-order-near-ambient-temperature-in-the-3cx3o80e9a.pdf

Natural ferroelectric order near ambient temperature in the orthoferrite HoFeO 3

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Natural ferroelectric order near ambient temperature in the orthoferrite HoFeO 3