Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3

Abstract Albeit having great potential toward unprecedented type of applications such as magnetoelectric (ME) sensors and memories, practically useful single‐phase multiferroics that show large coupling between ferromagnetism and ferroelectricity at ambient temperatures are still lacking. Here, the...

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Main Authors: Ji‐Hun Park, Jae‐Hyeon Cho, Nyun Jong Lee, Hyun‐Jae Lee, Ju‐Hyeon Lee, Geon‐Ju Lee, Frederick P. Marlton, Motohiro Suzuki, Manuel Hinterstein, Yoon Seok Oh, Ji‐Won Choi, Geon‐Tae Hwang, Jun Hee Lee, Sanghoon Kim, Kee Hoon Kim, Wook Jo
Format: Article
Language:English
Published: Wiley-VCH 2025-02-01
Series:Advanced Electronic Materials
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Online Access:https://doi.org/10.1002/aelm.202400370
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author Ji‐Hun Park
Jae‐Hyeon Cho
Nyun Jong Lee
Hyun‐Jae Lee
Ju‐Hyeon Lee
Geon‐Ju Lee
Frederick P. Marlton
Motohiro Suzuki
Manuel Hinterstein
Yoon Seok Oh
Ji‐Won Choi
Geon‐Tae Hwang
Jun Hee Lee
Sanghoon Kim
Kee Hoon Kim
Wook Jo
author_facet Ji‐Hun Park
Jae‐Hyeon Cho
Nyun Jong Lee
Hyun‐Jae Lee
Ju‐Hyeon Lee
Geon‐Ju Lee
Frederick P. Marlton
Motohiro Suzuki
Manuel Hinterstein
Yoon Seok Oh
Ji‐Won Choi
Geon‐Tae Hwang
Jun Hee Lee
Sanghoon Kim
Kee Hoon Kim
Wook Jo
author_sort Ji‐Hun Park
collection DOAJ
description Abstract Albeit having great potential toward unprecedented type of applications such as magnetoelectric (ME) sensors and memories, practically useful single‐phase multiferroics that show large coupling between ferromagnetism and ferroelectricity at ambient temperatures are still lacking. Here, the discovery of a new type of perovskite ferroelectrics (Pb,M)(Fe1/2Nb1/2)O3 (M = Fe, Co, Ni) is reported with a magnetically‐active metal ion introduced into a cuboctahedrally‐coordinated Pb position, which exhibits enhanced ME coupling owing to the development of simultaneous soft‐ferromagnetism and lone‐pair ferroelectricity persistent above room temperature. These Pb‐site engineered (Pb,M)(Fe1/2Nb1/2)O3 perovskites exhibit a ME coupling coefficient of ≈40–60 ps m−1, a saturated electric polarization of 14–17 µC cm−2 and a saturation magnetization of 0.15–0.3 µB f.u−1. X‐ray absorption spectroscopy combined with first‐principles calculations demonstrates that the induced ferromagnetism originates from the ferromagnetic superexchange interaction coming from ≈90° bonding between the magnetic ions at the Pb site. The present discovery of the enhanced ME coupling in the Pb‐site engineered perovskite ferroelectrics may provide unforeseen opportunities for applying conventional displacive ferroelectricity in the field of spintronics where ferromagnetism is essentially required.
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spelling doaj-art-ffcd2071545641fd8febd33a5e8ff1952025-08-20T03:47:49ZengWiley-VCHAdvanced Electronic Materials2199-160X2025-02-01112n/an/a10.1002/aelm.202400370Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3Ji‐Hun Park0Jae‐Hyeon Cho1Nyun Jong Lee2Hyun‐Jae Lee3Ju‐Hyeon Lee4Geon‐Ju Lee5Frederick P. Marlton6Motohiro Suzuki7Manuel Hinterstein8Yoon Seok Oh9Ji‐Won Choi10Geon‐Tae Hwang11Jun Hee Lee12Sanghoon Kim13Kee Hoon Kim14Wook Jo15Department of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaDepartment of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaDepartment of Physics University of Ulsan Ulsan 44610 Republic of KoreaDepartment of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaDepartment of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaDepartment of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaCentre for Clean Energy Technology School of Mathematical and Physical Sciences Faculty of Science University of Technology Sydney Sydney New South Wales 2007 AustraliaJapan Synchrotron Radiation Research Institute Sayo Hyogo 679–5198 JapanInstitute for Applied Materials Karlsruhe Institute of Technology (KIT) Haid‐und‐Neu Strasse 7 76131 Karlsruhe GermanyDepartment of Physics Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaElectronic Materials Center Korea Institute of Science and Technology (KIST) Seoul 02792 Republic of KoreaDepartment of Materials Science and Engineering Pukyong National University Busan 42601 Republic of KoreaDepartment of Energy and Chemical Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaDepartment of Physics University of Ulsan Ulsan 44610 Republic of KoreaDepartment of Physics and Astronomy CeNSCMR & Institute of Applied Physics Seoul National University Seoul 151–747 Republic of KoreaDepartment of Materials Science and Engineering Ulsan National Institute of Science and Technology (UNIST) Ulsan 44919 Republic of KoreaAbstract Albeit having great potential toward unprecedented type of applications such as magnetoelectric (ME) sensors and memories, practically useful single‐phase multiferroics that show large coupling between ferromagnetism and ferroelectricity at ambient temperatures are still lacking. Here, the discovery of a new type of perovskite ferroelectrics (Pb,M)(Fe1/2Nb1/2)O3 (M = Fe, Co, Ni) is reported with a magnetically‐active metal ion introduced into a cuboctahedrally‐coordinated Pb position, which exhibits enhanced ME coupling owing to the development of simultaneous soft‐ferromagnetism and lone‐pair ferroelectricity persistent above room temperature. These Pb‐site engineered (Pb,M)(Fe1/2Nb1/2)O3 perovskites exhibit a ME coupling coefficient of ≈40–60 ps m−1, a saturated electric polarization of 14–17 µC cm−2 and a saturation magnetization of 0.15–0.3 µB f.u−1. X‐ray absorption spectroscopy combined with first‐principles calculations demonstrates that the induced ferromagnetism originates from the ferromagnetic superexchange interaction coming from ≈90° bonding between the magnetic ions at the Pb site. The present discovery of the enhanced ME coupling in the Pb‐site engineered perovskite ferroelectrics may provide unforeseen opportunities for applying conventional displacive ferroelectricity in the field of spintronics where ferromagnetism is essentially required.https://doi.org/10.1002/aelm.202400370ferroelectricity/ferroelectric oxidesferromagnetism/ferromagnetic oxidesmagnetoelectric couplingmultiferroicssuperexchange interaction
spellingShingle Ji‐Hun Park
Jae‐Hyeon Cho
Nyun Jong Lee
Hyun‐Jae Lee
Ju‐Hyeon Lee
Geon‐Ju Lee
Frederick P. Marlton
Motohiro Suzuki
Manuel Hinterstein
Yoon Seok Oh
Ji‐Won Choi
Geon‐Tae Hwang
Jun Hee Lee
Sanghoon Kim
Kee Hoon Kim
Wook Jo
Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
Advanced Electronic Materials
ferroelectricity/ferroelectric oxides
ferromagnetism/ferromagnetic oxides
magnetoelectric coupling
multiferroics
superexchange interaction
title Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
title_full Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
title_fullStr Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
title_full_unstemmed Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
title_short Enhanced Coupling Between Soft Ferromagnetism and Displacive Ferroelectricity in the Pb‐Site Modified PbFe1/2Nb1/2O3
title_sort enhanced coupling between soft ferromagnetism and displacive ferroelectricity in the pb site modified pbfe1 2nb1 2o3
topic ferroelectricity/ferroelectric oxides
ferromagnetism/ferromagnetic oxides
magnetoelectric coupling
multiferroics
superexchange interaction
url https://doi.org/10.1002/aelm.202400370
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