Emergent multiferroism with magnetodielectric coupling in EuTiO₃ created by a negative pressure control of strong spin-phonon coupling

Journal Article · Mon May 02 00:00:00 EDT 2022 · Nature Communications

DOI:https://doi.org/10.1038/s41467-022-30074-4· OSTI ID:2470871

Zhao, Run ^[1]; Yang, Chao ^[2]; Wang, Hongguang ^[3]; Jiang, Kai ^[4]; Wu, Hua ^[5]; Shen, Shipeng ^[6]; Wang, Le ^[7]; Sun, Young ^[8]; Jin, Kuijuan ^[6]; Gao, Ju ^[9]; Chen, Li ^[10]; Wang, Haiyan ^[10]; MacManus-Driscoll, Judith L. ^[11]; van Aken, Peter A. ^[3]; Hong, Jiawang ^[12]; Li, Weiwei ^[13]; Yang, Hao ^[14]

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1. Nanjing University of Aeronautics and Astronautics (China); Suzhou University of Science and Technology (China)
2. Beijing Institute of Technology (China); Jishou University, Hunan (China)
3. Max Planck Institute for Solid State Research, Stuttgart (Germany)
4. East China Normal University, Shanghai (China)
5. Donghua University, Shanghai (China)
6. Chinese Academy of Sciences (CAS), Beijing (China)
7. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States); Chinese Academy of Sciences (CAS), Beijing (China)
8. Chongqing University (China)
9. Suzhou University of Science and Technology (China)
10. Purdue University, West Lafayette, IN (United States)
11. University of Cambridge (United Kingdom)
12. Beijing Institute of Technology (China)
13. Nanjing University of Aeronautics and Astronautics (China); University of Cambridge (United Kingdom)
14. Nanjing University of Aeronautics and Astronautics (China)

Negative pressure has emerged as a powerful tool to tailor the physical properties of functional materials. However, a negative pressure control of spin-phonon coupling for engineering magnetism and multiferroicity has not been explored to date. Here, using uniform three-dimensional strain-induced negative pressure in nanocomposite films of (EuTiO₃)_0.5:(MgO)_0.5, we demonstrate an emergent multiferroicity with magnetodielectric coupling in EuTiO₃, matching exactly with density functional theory calculations. Density functional theory calculations are further used to explore the underlying physics of antiferromagnetic-paraelectric to ferromagnetic-ferroelectric phase transitions, the spin-phonon coupling, and its correlation with negative pressures. The observation of magnetodielectric coupling in the EuTiO₃ reveals that an enhanced spin-phonon coupling originates from a negative pressure induced by uniform three-dimensional strain. Our work provides a route to creating multiferroicity and magnetoelectric coupling in single-phase oxides using a negative pressure approach.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: USDOE; National Key Basic Research Program of China; National Nature Science Foundation of China; Natural Science Fund Project of Hunan Province; Scientific Research Fund of Hunan Provincial Education Department; Beijing Natural Science Foundation; European Union’s Horizon 2020 research and innovation programme
• Grant/Contract Number: AC02-05CH11231
• OSTI ID: 2470871
• Journal Information: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 13; ISSN 2041-1723
• Publisher: Nature Publishing Group
• Country of Publication: United States
• Language: English

Related Subjects

36 MATERIALS SCIENCE
Ferroelectrics and multiferroics
Magnetic properties and materials
Science & Technology - Other Topics