Experimental demonstration of hybrid improper ferroelectricity and presence of abundant charged walls in (Ca,Sr)${}_3$Ti${}_2$O${}_7$ crystals

Abstract

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 ferroelectricity has been theoretically predicted in ordered perovskites and the Ruddlesden-Popper compounds (Ca${}_3$Ti${}_2$O${}_7$, Ca${}_3$Mn${}_2$O${}_7$, and (Ca/Sr/Ba)${}_3$(Sn/Zr/Ge)${}_2$O${}_7$). However, the ferroelectricity of these compounds has never been experimentally confirmed and even their polar nature has been under debate. Here we provide the first experimental demonstration of room-temperature switchable polarization in the bulk crystals of Ca${}_3$Ti${}_2$O${}_7$ as well as Sr-doped Ca${}_3$Ti${}_2$O${}_7$. In addition, (Ca,Sr)${}_3$Ti${}_2$O${}_7$ is found to exhibit an intriguing ferroelectric domain structure resulting from orthorhombic twins and (switchable) planar polarization. The planar domain structure accompanies abundant charged domain walls with conducting head-to-head and insulating tail-to-tail configurations, which exhibit two-order-of-magnitude conduction difference. These discoveries provide new research opportunities not only on new stable ferroelectrics of Ruddlesden-Popper compounds, but also on meandering conducting domain walls formed by planar polarization.

References in corpus (3)

• Conduction at domain walls in insulating Pb(Zr${}_{0.2}$Ti${}_{0.8}$)O${}_3$ thin films
• Coercive fields in ultrathin BaTiO3 capacitors
• Coexistence of Weak Ferromagnetism and Ferroelectricity in the High Pressure LiNbO3-type Phase of FeTiO3

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• Improper ferroelectricity in stuffed aluminate sodalites for pyroelectric energy harvesting
• Ferroelectricity of Dion-Jacobson layered perovskites CsNdNb${}_2$O${}_7$ and RbNdNb${}_2$O${}_7$
• Multiferroic properties of oxygen functionalized magnetic i-MXene
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• Electric field driven octahedral rotation in perovskite
• Negative piezoelectricity in quasi-two/one-dimensional ferroelectrics
• Direct Visualization of Irreducible Ferrielectricity in Crystals
• Symmetry analysis of magnetoelectric effects in perovskite-based multiferroics
• Perspective on 2D perovskite ferroelectrics and multiferroics
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• Probing $C{a}_{3}T{i}_2{O}_7$ crystal structure at the atomic level: Insights from ${}^{111m}Cd{/}^{111}Cd$ PAC spectroscopy and ab-initio studies
• Switchable Polarization in an A-site Deficient Perovskite through Vacancy and Cation Engineering
• Triggered ferroelectricity in HfO${}_2$ from hybrid phonons and higher-order dynamical charges
• Stabilization of layered perovskite structures via strontium substitution in Ca${}_3$Ti${}_2$O${}_7$ revealed via elemental mapping
• Recipes for improper ferroelectricity in hybrid perovskites
• Revival of Layered Ferroelectrics in Thin Films
• Current Flow Mapping in Conducting Ferroelectric Domain Walls using Scanning NV-Magnetometry
• Breaking symmetry to create a parallel-plate varactor dielectric with unparalleled microwave performance
• Influence of a Realistic Multiorbital Band Structure on Conducting Domain Walls in Perovskite Ferroelectrics
• Charged domain boundaries stabilized by translational symmetry breaking in the hybrid improper ferroelectric Ca${}_{3-x}$Sr${}_x$Ti${}_2$O${}_7$
• Intervention Strategies for Polarization Switching in Hybrid Improper Ferroelectrics