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

Run Zhao, Chao Yang, Hongguang Wang (), Kai Jiang (), Hua Wu, Shipeng Shen, Le Wang, Young Sun, Kuijuan Jin, Ju Gao, Li Chen, Haiyan Wang, Judith L. MacManus-Driscoll, Peter A. Aken, Jiawang Hong (), Weiwei Li () and Hao Yang ()
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Run Zhao: Nanjing University of Aeronautics and Astronautics
Chao Yang: Beijing Institute of Technology
Hongguang Wang: Max Planck Institute for Solid State Research, Heisenbergstr. 1
Kai Jiang: East China Normal University
Hua Wu: Donghua University
Shipeng Shen: Chinese Academy of Science
Le Wang: Chinese Academy of Science
Young Sun: Chongqing University
Kuijuan Jin: Chinese Academy of Science
Ju Gao: Suzhou University of Science and Technology
Li Chen: Purdue University
Haiyan Wang: Purdue University
Judith L. MacManus-Driscoll: University of Cambridge
Peter A. Aken: Max Planck Institute for Solid State Research, Heisenbergstr. 1
Jiawang Hong: Beijing Institute of Technology
Weiwei Li: Nanjing University of Aeronautics and Astronautics
Hao Yang: Nanjing University of Aeronautics and Astronautics

Nature Communications, 2022, vol. 13, issue 1, 1-9

Abstract: Abstract 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.

Date: 2022
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DOI: 10.1038/s41467-022-30074-4

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