TY - JOUR KW - Transmission electron microscopy KW - Scanning electron microscopy KW - Iron compounds KW - Polarization KW - Bismuth compounds KW - Ferroelectricity KW - Ferroelectric polarization KW - Bismuth ferrite KW - High resolution transmission electron microscopy KW - Scanning transmission electron microscopy KW - Doping (additives) KW - Semiconductor doping KW - Differential phase contrast KW - Differential phase contrast imaging KW - Functional properties KW - Periodic distortions KW - Polarization gradients AU - M Campanini AU - R Erni AU - C.-H Yang AU - Ramamoorthy Ramesh AU - M.D Rossell AB - The ultimate challenge for the development of new multiferroics with enhanced properties lies in achieving nanoscale control of the coupling between different ordering parameters. In oxide-based multiferroics, substitutional cation dopants offer the unparalleled possibility to modify both the electric and magnetic properties at a local scale. Herein it is demonstrated the formation of a dopant-controlled polar pattern in BiFeO3 leading to the spontaneous instauration of periodic polarization waves. In particular, nonpolar Ca-doped rich regions act as spacers between consecutive dopant-depleted regions displaying coupled ferroelectric states. This alternation of layers with different ferroelectric state creates a novel vertical polar structure exhibiting giant polarization gradients as large as 70 μC cm-2 across 30 Å thick domains. The drastic change in the polar state of the film is visualized using high-resolution differential phase-contrast imaging able to map changes in ferroelectric polarization at atomic scale. Furthermore, a periodic distortion in the Fe - O - Fe bonding angle suggests a local variation in the magnetic ordering. The findings provide a new insight into the role of doping and reveal hitherto unexplored means to tailor the functional properties of multiferroics by doping engineering. © 2018 American Chemical Society. BT - Nano Letters DO - 10.1021/acs.nanolett.7b03817 LA - eng M1 - 2 N1 - cited By 15 N2 - The ultimate challenge for the development of new multiferroics with enhanced properties lies in achieving nanoscale control of the coupling between different ordering parameters. In oxide-based multiferroics, substitutional cation dopants offer the unparalleled possibility to modify both the electric and magnetic properties at a local scale. Herein it is demonstrated the formation of a dopant-controlled polar pattern in BiFeO3 leading to the spontaneous instauration of periodic polarization waves. In particular, nonpolar Ca-doped rich regions act as spacers between consecutive dopant-depleted regions displaying coupled ferroelectric states. This alternation of layers with different ferroelectric state creates a novel vertical polar structure exhibiting giant polarization gradients as large as 70 μC cm-2 across 30 Å thick domains. The drastic change in the polar state of the film is visualized using high-resolution differential phase-contrast imaging able to map changes in ferroelectric polarization at atomic scale. Furthermore, a periodic distortion in the Fe - O - Fe bonding angle suggests a local variation in the magnetic ordering. The findings provide a new insight into the role of doping and reveal hitherto unexplored means to tailor the functional properties of multiferroics by doping engineering. © 2018 American Chemical Society. PB - American Chemical Society PY - 2018 SP - 717 EP - 724 T2 - Nano Letters TI - Periodic Giant Polarization Gradients in Doped BiFeO3 Thin Films VL - 18 SN - 15306984 ER -