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Raman spectroscopy is employed to probe directly the soft rotation and tilting modes, which are two primary order parameters predicted in the hybrid improper ferroelectric material Ca$_3$Mn$_2$O$_7$. We observe a giant softening of the 107-cm$^{-1}$ octahedron tilting mode by 26~cm$^{-1}$, on heating through the structural transition from a ferroelectric to paraelectric orthorhombic phase. This is contrasted by a small softening of the 150-cm$^{-1}$ rotational mode by 6~cm$^{-1}$. In the intermediate phase, the competing soft modes with different symmetries coexist, bringing about many-faceted anomalies in spin excitations and lattice vibrations. Our work demonstrates that the soft rotation and tilt patterns, relying on a phase-transition path, are a key factor in determining ferroelectric, magnetic, and lattice properties of Ca$_3$Mn$_2$O$_7$.
Standing on successful first principles predictions for new functional ferroelectric materials, a number of new ferroelectrics have been experimentally discovered. Utilizing trilinear coupling of two types of octahedron rotations, hybrid improper fer
The charged domain walls in ferroelectric materials exhibit intriguing physical properties. We examine herein the charged-domain-wall structures in Ca$_{3-x}$Sr$_x$Ti$_2$O$_7$ using transmission electron microscopy. When viewed along the [001] axis,
Magnetic structure of the multiferroic Ca$_{2}$CoSi$_{2}$O$_{7}$ was determined by neutron diffraction techniques. Combination of the polycrystalline and single-crystal samples experiments revealed a collinear antiferromagnetic structure with the eas
We study magnetic and multiferroic behavior in Ca$_3$Co$_{2-x}$Mn$_{x}$O$_6$ ($x sim$0.97) by high-field measurements of magnetization ($M$), magnetostriction ($L$($H$)/$L$), electric polarization ($P$), and magnetocaloric effect. This study also giv
Ferroic materials are well known to exhibit heterogeneity in the form of domain walls. Understanding the properties of these boundaries is crucial for controlling functionality with external stimuli and for realizing their potential for ultra-low pow