Manipulating multiple order parameters via oxygen vacancies: The case of
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:
-
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- Nanjing Univ. of Aeronautics and Astronautics (China). College of Science; Univ. of Cambridge (United Kingdom). Dept. of Materials Science and Metallurgy
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science and Technology Division
- Chinese Academy of Sciences (CAS), Beijing (China). Beijing National Lab. for Condensed Matter Physics. Inst. of Physics
- Univ. of Electronic Science and Technology of China, Chengdu (China). State Key Lab. of Electronic Thin Films and Integrated Devices
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Chinese Academy of Sciences (CAS), Hefei (China). High Magnetic Field Lab.
- Texas A & M Univ., College Station, TX (United States). Materials Science and Engineering Program. Dept. of Electrical and Computer Engineering
- Nanjing Univ. of Aeronautics and Astronautics (China). College of Science
- Soochow Univ., Suzhou (China). College of Physics, Optoelectronics and Energy
- National Inst. of Scientific Research-Energy, Materials and Telecommunications (INRS-EMT), Varennes, QC (Canada)
- Soochow Univ., Suzhou (China). Center for Soft Condensed Matter Physics and Interdisciplinary Research
- 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 University, 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); National Science Foundation (NSF); National Basic Research Program of China; National Natural Science Foundation of China (NSFC); 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:
- Journal Article: 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. https://doi.org/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. 2017.
"Manipulating multiple order parameters via oxygen vacancies: The case of Eu0.5Ba0.5TiO3-δ". United States. https://doi.org/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},
url = {https://www.osti.gov/biblio/1457304},
journal = {Physical Review B},
issn = {2469-9950},
number = 11,
volume = 96,
place = {United States},
year = {Wed Sep 06 00:00:00 EDT 2017},
month = {Wed Sep 06 00:00:00 EDT 2017}
}
Web of Science
Works referenced in this record:
Dielectric, magnetic and structural properties of novel multiferroic Eu 0.5 Ba 0.5 TiO 3 ceramics
journal, December 2010
- Goian, V.; Kamba, S.; Nuzhnyy, D.
- Journal of Physics: Condensed Matter, Vol. 23, Issue 2
Functional Ion Defects in Transition Metal Oxides
journal, August 2013
- Kalinin, S. V.; Spaldin, N. A.
- Science, Vol. 341, Issue 6148
Room-temperature magnetoresistance in an oxide material with an ordered double-perovskite structure
journal, October 1998
- Kobayashi, K. -I.; Kimura, T.; Sawada, H.
- Nature, Vol. 395, Issue 6703
Oxygen-Vacancy-Induced Polar Behavior in (LaFeO 3 ) 2 /(SrFeO 3 ) Superlattices
journal, April 2014
- Mishra, Rohan; Kim, Young-Min; Salafranca, Juan
- Nano Letters, Vol. 14, Issue 5
Persistent optically induced magnetism in oxygen-deficient strontium titanate
journal, March 2014
- Rice, W. D.; Ambwani, P.; Bombeck, M.
- Nature Materials, Vol. 13, Issue 5
Oxygen-Vacancy-Induced Antiferromagnetism to Ferromagnetism Transformation in Eu0.5Ba0.5TiO3−δ Multiferroic Thin Films
journal, September 2013
- Li, Weiwei; Zhao, Run; Wang, Le
- Scientific Reports, Vol. 3, Issue 1
Simple ways of determining perovskite structures
journal, November 1975
- Glazer, A. M.
- Acta Crystallographica Section A, Vol. 31, Issue 6
Why Are There so Few Magnetic Ferroelectrics?
journal, July 2000
- Hill, Nicola A.
- The Journal of Physical Chemistry B, Vol. 104, Issue 29
Coupling between magnetism and dielectric properties in quantum paraelectric
journal, July 2001
- Katsufuji, T.; Takagi, H.
- Physical Review B, Vol. 64, Issue 5
Magnetic and superconducting phases at the LaAlO /SrTiO interface: The role of interfacial Ti 3 electrons
journal, January 2012
- Pavlenko, N.; Kopp, T.; Tsymbal, E. Y.
- Physical Review B, Vol. 85, Issue 2
Room-temperature ferroelectricity in SrTiO 3 nanodots array formed by an ac -bias field
journal, September 2013
- Yeog Son, Jong; Lee, Jung-Hoon; Myung Jang, Hyun
- Applied Physics Letters, Vol. 103, Issue 10
A multiferroic material to search for the permanent electric dipole moment of the electron
journal, July 2010
- Rushchanskii, K. Z.; Kamba, S.; Goian, V.
- Nature Materials, Vol. 9, Issue 8
The classification of tilted octahedra in perovskites
journal, November 1972
- Glazer, A. M.
- Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 28, Issue 11
Origin of ferroelectricity in perovskite oxides
journal, July 1992
- Cohen, Ronald E.
- Nature, Vol. 358, Issue 6382
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface
journal, January 2004
- Ohtomo, A.; Hwang, H. Y.
- Nature, Vol. 427, Issue 6973
Multiferroics: Past, present, and future
journal, October 2010
- Spaldin, Nicola A.; Cheong, Sang-Wook; Ramesh, Ramamoorthy
- Physics Today, Vol. 63, Issue 10
Antiferromagnetic superexchange via states of titanium in EuTiO as seen from hybrid Hartree-Fock density functional calculations
journal, June 2011
- Akamatsu, Hirofumi; Kumagai, Yu; Oba, Fumiyasu
- Physical Review B, Vol. 83, Issue 21
Multiferroics progress and prospects in thin films
journal, January 2007
- Ramesh, R.; Spaldin, Nicola A.
- Nature Materials, Vol. 6, Issue 1, p. 21-29
Ferroelectromagnets
journal, July 1982
- Smolenskiĭ, G. A.; Chupis, I. E.
- Soviet Physics Uspekhi, Vol. 25, Issue 7
Electronic structure of the spin- quantum magnet TiOCl
journal, September 2005
- Hoinkis, M.; Sing, M.; Schäfer, J.
- Physical Review B, Vol. 72, Issue 12
Influence of strain and oxygen vacancies on the magnetoelectric properties of multiferroic bismuth ferrite
journal, June 2005
- Ederer, Claude; Spaldin, Nicola A.
- Physical Review B, Vol. 71, Issue 22
Role of Ti Antisitelike Defects in
journal, October 2009
- Choi, Minseok; Oba, Fumiyasu; Tanaka, Isao
- Physical Review Letters, Vol. 103, Issue 18
Study of strain fields at a-Si/c-Si interface
journal, April 2004
- Yu, Zhiheng; Muller, David A.; Silcox, John
- Journal of Applied Physics, Vol. 95, Issue 7
Direct imaging of the coexistence of ferromagnetism and superconductivity at the LaAlO3/SrTiO3 interface
journal, September 2011
- Bert, Julie A.; Kalisky, Beena; Bell, Christopher
- Nature Physics, Vol. 7, Issue 10, p. 767-771
Atomically Resolved Mapping of Polarization and Electric Fields Across Ferroelectric/Oxide Interfaces by Z-contrast Imaging
journal, April 2011
- Chang, Hye Jung; Kalinin, Sergei V.; Morozovska, Anna N.
- Advanced Materials, Vol. 23, Issue 21
Epitaxial BiFeO3 Multiferroic Thin Film Heterostructures
journal, March 2003
- Wang, J.; Neaton, J. B.; Zheng, H.
- Science, Vol. 299, Issue 5613, p. 1719-1722
Multiferroic and magnetoelectric materials
journal, August 2006
- Eerenstein, W.; Mathur, N. D.; Scott, J. F.
- Nature, Vol. 442, Issue 7104
Anti-ferrodistortive-Like Oxygen-Octahedron Rotation Induced by the Oxygen Vacancy in Cubic SrTiO 3
journal, October 2012
- Choi, Minseok; Oba, Fumiyasu; Kumagai, Yu
- Advanced Materials, Vol. 25, Issue 1
Multiferroic Vacancies at Ferroelectric Surfaces
journal, September 2015
- Shimada, Takahiro; Wang, Jie; Araki, Yasumitsu
- Physical Review Letters, Vol. 115, Issue 10
Coupling between the magnetism and dielectric properties in
journal, January 2004
- Wu, Hua; Jiang, Qing; Shen, Wen Zhong
- Physical Review B, Vol. 69, Issue 1
Works referencing / citing this record:
Interface Engineered Room‐Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films
journal, November 2019
- Li, Weiwei; Zhu, Bonan; He, Qian
- Advanced Science, Vol. 7, Issue 1
Origin of Improved Photoelectrochemical Water Splitting in Mixed Perovskite Oxides
journal, September 2018
- Li, Weiwei; Jiang, Kai; Li, Zhongguo
- Advanced Energy Materials, Vol. 8, Issue 31
A DFT investigation of the role of oxygen vacancies on the structural, electronic and magnetic properties of ATiO 3 (A = Mn, Fe, Ni) multiferroic materials
journal, January 2018
- Ribeiro, R. A. P.; Longo, E.; Andrés, J.
- Physical Chemistry Chemical Physics, Vol. 20, Issue 45
Oxygen-vacancy-mediated dielectric property in perovskite Eu 0.5 Ba 0.5 TiO 3-δ epitaxial thin films
journal, April 2018
- Li, Weiwei; Gu, Junxing; He, Qian
- Applied Physics Letters, Vol. 112, Issue 18
Oxygen-vacancy-mediated dielectric property in perovskite Eu0.5Ba0.5TiO3-δ epitaxial thin films
text, January 2018
- Li, Weiwei; Gu, J.; He, Q.
- Apollo - University of Cambridge Repository
Origin of Improved Photoelectrochemical Water Splitting in Mixed Perovskite Oxides
text, January 2018
- Li, Weiwei; Jiang, K.; Li, Z.
- Apollo - University of Cambridge Repository
Interface Engineered Room-Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films.
text, January 2020
- Li, Weiwei; Zhu, Bonan; He, Qian
- Apollo - University of Cambridge Repository
Interface Engineered Room-Temperature Ferromagnetic Insulating State in Ultrathin Manganite Films.
text, January 2019
- Li, Weiwei; Zhu, Bonan; He, Qian
- Apollo - University of Cambridge Repository