Abstract
In contrast to all other members of the $R{\mathrm{Mn}}_{2}{\mathrm{O}}_{5}$ family with nonzero $4f$ electrons ($R$ = Nd to Lu), ${\mathrm{PrMn}}_{2}{\mathrm{O}}_{5}$ does not show any spin driven ferroelectricity in the magnetically ordered phase. By means of high-field electric polarization measurements up to 45 T, we have found that this exceptional candidate undergoes a spin driven multiferroic phase under magnetic field. X-ray magnetic circular dichroism studies up to 30 T at the Pr ${L}_{2}$ edge show that this ferroelectricity originates from and directly couples to the ferromagnetic component of the ${\mathrm{Pr}}^{3+}$ spins. Experimental observations along with our generalized gradient-approximation $+\phantom{\rule{4pt}{0ex}}U$ calculations reveal that this exotic ferroelectric-ferromagnetic combination stabilizes through the exchange-striction mechanism solely driven by a $3d\ensuremath{-}4f$-type coupling, as opposed to the other $R{\mathrm{Mn}}_{2}{\mathrm{O}}_{5}$ members with $3d\ensuremath{-}3d$ driven ferroelectric-antiferromagnetic-type conventional type-II multiferroicity.
Highlights
The research on functional materials, aiming at the generation of smart devices, witnessed a massive upturn after the advent of materials showing multiple combined properties
By means of high-field electric polarization measurements up to 45 T, we have found that this exceptional candidate undergoes a spin driven multiferroic phase under magnetic field
Experimental observations along with our generalized gradient-approximation + U calculations reveal that this exotic ferroelectric-ferromagnetic combination stabilizes through the exchange-striction mechanism solely driven by a 3d-4 f -type coupling, as opposed to the other RMn2O5 members with 3d-3d driven ferroelectricantiferromagnetic-type conventional type-II multiferroicity
Summary
The research on functional materials, aiming at the generation of smart devices, witnessed a massive upturn after the advent of materials showing multiple combined properties Among such materials, an intriguing family of compounds known as magnetoelectric multiferroics (MEMF) with strongly coupled magnetism and ferroelectricity has attracted special attention [1,2,3]. In type-II multiferroics, spin driven ferroelectricity is caused by magnetic ordering itself, resulting in an intrinsically strong magnetoelectric coupling [3,9,10]. Using the combination of high-field electric polarization, x-ray magnetic circular dichroism (XMCD), and density functional theory (DFT)based calculations, we show that unlike the multiferroicity observed in other RMn2O5 members, the spin driven ferroelectricity in PrMn2O5 originates from and couples to a ferromagnetic component. The as-grown crystals have a thin platelike morphology with the plate surface being perpendicular to the b axis
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