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Title: Manipulating multiple order parameters via oxygen vacancies: The case of E u 0.5 B a 0.5 Ti O 3 - δ

Abstract

Controlling functionalities, such as magnetism or ferroelectricity, by means of oxygen vacancies ($${V}_{\mathrm{O}}$$) is a key issue for the future development of transition-metal oxides. Progress in this field is currently addressed through $${V}_{\mathrm{O}}$$ variations and their impact on mainly one order parameter. In this paper, we reveal a mechanism for tuning both magnetism and ferroelectricity simultaneously by using $${V}_{\mathrm{O}}$$. Combining experimental and density-functional theory studies of $$\mathrm{E}{\mathrm{u}}_{0.5}\mathrm{B}{\mathrm{a}}_{0.5}\mathrm{Ti}{\mathrm{O}}_{3{-}{\delta}}$$, we demonstrate that oxygen vacancies create $$\mathrm{T}{\mathrm{i}}^{3+}3{d}^{1}$$ defect states, mediating the ferromagnetic coupling between the localized Eu $$4{f}^{7}$$ spins, and increase an off-center displacement of Ti ions, enhancing the ferroelectric Curie temperature. Finally, the dual function of Ti sites also promises a magnetoelectric coupling in the $$\mathrm{E}{\mathrm{u}}_{0.5}\mathrm{B}{\mathrm{a}}_{0.5}\mathrm{Ti}{\mathrm{O}}_{3{-}{\delta}}$$.

Authors:
 [1];  [2];  [3];  [4];  [5];  [6];  [5];  [7];  [8];  [9];  [3];  [3];  [3];  [6];  [7];  [5];  [10];  [11];  [11];  [12] more »;  [12];  [3];  [3];  [6];  [5];  [9];  [10];  [8];  [2];  [8] « less
  1. Nanjing Univ. of Aeronautics and Astronautics (China). College of Science; Univ. of Cambridge (United Kingdom). Dept. of Materials Science and Metallurgy
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
  3. Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics
  4. Univ. of Electronic Science and Technology of China, Chengdu (China). State Key Lab. of Electronic Thin Films and Integrated Devices
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  6. Chinese Academy of Sciences (CAS), Hefei (China). High Magnetic Field Lab.
  7. Texas A & M Univ., College Station, TX (United States). Materials Science and Engineering Program. Dept. of Electrical and Computer Engineering
  8. Nanjing Univ. of Aeronautics and Astronautics (China). College of Science
  9. Soochow Univ., Suzhou (China). College of Physics, Optoelectronics and Energy
  10. National Inst. of Scientific Research-Energy, Materials and Telecommunications (INRS-EMT), Varennes, QC (Canada)
  11. Soochow Univ., Suzhou (China). Center for Soft Condensed Matter Physics and Interdisciplinary Research
  12. Chinese Academy of Sciences (CAS), Ningbo (China). Key Lab. of Magnetic Materials and Devices. Ningbo Inst. of Materials Technology and Engineering
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Texas A & M Univ., College Station, TX (United States); Nanjing Univ. of Aeronautics and Astronautics (China); Soochow Univ., Suzhou (China); Chinese Academy of Sciences (CAS), Beijing (China); National Inst. of Scientific Research-Energy, Materials and Telecommunications (INRS-EMT), Varennes, QC (Canada)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF); National Basic Research Program of China; National Natural Science Foundation of China (NNSFC); Program for Postgraduates Research Innovation in University of Jiangsu Province (China); Natural Sciences and Engineering Research Council of Canada (NSERC); Fonds de recherche du Québec - Nature et technologies (FRQNT) (Canada)
OSTI Identifier:
1457304
Alternate Identifier(s):
OSTI ID: 1378818
Report Number(s):
LA-UR-15-29487
Journal ID: ISSN 2469-9950; TRN: US1901351
Grant/Contract Number:  
AC52-06NA25396; DMR-1643911; DMR-1565822; 2014CB921001; 11274237; U1632122; 11004145; 51202153; U1332209; U1435208; 11134012; 11174355; 11474349; 11227405; CXZZ13_0798
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review B
Additional Journal Information:
Journal Volume: 96; Journal Issue: 11; Journal ID: ISSN 2469-9950
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ferroelectricity; magnetoelectric effect; vacancies; multiferroics; oxides; thin films; transition metals; magnetization measurements; optical second-harmonic generation

Citation Formats

Li, Weiwei, He, Qian, Wang, Le, Zeng, Huizhong, Bowlan, John, Ling, Langsheng, Yarotski, Dmitry A., Zhang, Wenrui, Zhao, Run, Dai, Jiahong, Gu, Junxing, Shen, Shipeng, Guo, Haizhong, Pi, Li, Wang, Haiyan, Wang, Yongqiang, Velasco-Davalos, Ivan A., Wu, Yangjiang, Hu, Zhijun, Chen, Bin, Li, Run-Wei, Sun, Young, Jin, Kuijuan, Zhang, Yuheng, Chen, Hou-Tong, Ju, Sheng, Ruediger, Andreas, Shi, Daning, Borisevich, Albina Y., and Yang, Hao. Manipulating multiple order parameters via oxygen vacancies: The case of Eu0.5Ba0.5TiO3-δ. United States: N. p., 2017. Web. doi:10.1103/PhysRevB.96.115105.
Li, Weiwei, He, Qian, Wang, Le, Zeng, Huizhong, Bowlan, John, Ling, Langsheng, Yarotski, Dmitry A., Zhang, Wenrui, Zhao, Run, Dai, Jiahong, Gu, Junxing, Shen, Shipeng, Guo, Haizhong, Pi, Li, Wang, Haiyan, Wang, Yongqiang, Velasco-Davalos, Ivan A., Wu, Yangjiang, Hu, Zhijun, Chen, Bin, Li, Run-Wei, Sun, Young, Jin, Kuijuan, Zhang, Yuheng, Chen, Hou-Tong, Ju, Sheng, Ruediger, Andreas, Shi, Daning, Borisevich, Albina Y., & Yang, Hao. Manipulating multiple order parameters via oxygen vacancies: The case of Eu0.5Ba0.5TiO3-δ. United States. doi:10.1103/PhysRevB.96.115105.
Li, Weiwei, He, Qian, Wang, Le, Zeng, Huizhong, Bowlan, John, Ling, Langsheng, Yarotski, Dmitry A., Zhang, Wenrui, Zhao, Run, Dai, Jiahong, Gu, Junxing, Shen, Shipeng, Guo, Haizhong, Pi, Li, Wang, Haiyan, Wang, Yongqiang, Velasco-Davalos, Ivan A., Wu, Yangjiang, Hu, Zhijun, Chen, Bin, Li, Run-Wei, Sun, Young, Jin, Kuijuan, Zhang, Yuheng, Chen, Hou-Tong, Ju, Sheng, Ruediger, Andreas, Shi, Daning, Borisevich, Albina Y., and Yang, Hao. Wed . "Manipulating multiple order parameters via oxygen vacancies: The case of Eu0.5Ba0.5TiO3-δ". United States. doi:10.1103/PhysRevB.96.115105. https://www.osti.gov/servlets/purl/1457304.
@article{osti_1457304,
title = {Manipulating multiple order parameters via oxygen vacancies: The case of Eu0.5Ba0.5TiO3-δ},
author = {Li, Weiwei and He, Qian and Wang, Le and Zeng, Huizhong and Bowlan, John and Ling, Langsheng and Yarotski, Dmitry A. and Zhang, Wenrui and Zhao, Run and Dai, Jiahong and Gu, Junxing and Shen, Shipeng and Guo, Haizhong and Pi, Li and Wang, Haiyan and Wang, Yongqiang and Velasco-Davalos, Ivan A. and Wu, Yangjiang and Hu, Zhijun and Chen, Bin and Li, Run-Wei and Sun, Young and Jin, Kuijuan and Zhang, Yuheng and Chen, Hou-Tong and Ju, Sheng and Ruediger, Andreas and Shi, Daning and Borisevich, Albina Y. and Yang, Hao},
abstractNote = {Controlling functionalities, such as magnetism or ferroelectricity, by means of oxygen vacancies (${V}_{\mathrm{O}}$) is a key issue for the future development of transition-metal oxides. Progress in this field is currently addressed through ${V}_{\mathrm{O}}$ variations and their impact on mainly one order parameter. In this paper, we reveal a mechanism for tuning both magnetism and ferroelectricity simultaneously by using ${V}_{\mathrm{O}}$. Combining experimental and density-functional theory studies of $\mathrm{E}{\mathrm{u}}_{0.5}\mathrm{B}{\mathrm{a}}_{0.5}\mathrm{Ti}{\mathrm{O}}_{3{-}{\delta}}$, we demonstrate that oxygen vacancies create $\mathrm{T}{\mathrm{i}}^{3+}3{d}^{1}$ defect states, mediating the ferromagnetic coupling between the localized Eu $4{f}^{7}$ spins, and increase an off-center displacement of Ti ions, enhancing the ferroelectric Curie temperature. Finally, the dual function of Ti sites also promises a magnetoelectric coupling in the $\mathrm{E}{\mathrm{u}}_{0.5}\mathrm{B}{\mathrm{a}}_{0.5}\mathrm{Ti}{\mathrm{O}}_{3{-}{\delta}}$.},
doi = {10.1103/PhysRevB.96.115105},
journal = {Physical Review B},
number = 11,
volume = 96,
place = {United States},
year = {2017},
month = {9}
}

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