Dual control of magnetism in LaMnO<sub>3</sub>/BaTiO<sub>3</sub> superlattice by epitaxial strain and ferroelectric polarization

Chen Dong; Yu Ben-Hai

doi:10.7498/aps.69.20200839

Abstract

The controlling of magnetism of perovskite oxides is scientifically interesting and technically important for numerous functionalities in spintronic devices and next-generation magnetic memories. The experimenally prepared superlattices often contain strain, polarization, oxygen vacancy and other factors, which can affect their magnetic properties. The magnetism of superlattice materials, controlled by using both epitaxial strain and ferroelectric polarization, is not only close to the real state of the material, but also can induce rich physical properties. In this work, we demonstrate a strong magnetoelectric coupling that appears in the LaMnO₃/ BaTiO₃ superlattice. First-principles calculations reveal that the reversible transitions among ferromagnetism, ferrimagnetism and anti-ferromagnetism are achieved by precisely controlling the magnitude and spin-direction of the magnetic moments of the Mn ions. A maximal change can be achieved to be 100.1% of the net magnetization by switching the ferroelectric polarization, which is much higher than the previous value 93.9%. The half-metallicity is demonstrated in the MnO₂ layer, and accompanied by the spin polarization of the superlattice varying from 100% to 0. In addition, we realize the coexistence of ferroelectric polarization and metallicity, i.e. “ferroelectric metal”. Neither of the strong covalent Mn—O bond and La—O bond acts as an obstacle that prevents the ferroelectric polarization from penetrating the LMO layer. The Jahn-Teller effect, the tilt and rotation of oxygen octahedron, and the charge transfer of the superlattice are systemically analyzed. The variation of strain and re-orientation of polarization lead the electrons to transfer between the e_g and t_2g orbitals of Mn, which determines the magnetism of our system. Our purpose-designed LMO/BTO superlattice with robust intrinsic magnetoelectric coupling is a particularly interesting model system that can provide guidance for developing the spintronics for future applications.

Keywords:

Authors and contacts

College of Physics and Electronic Engineering, Xinyang Normal University, Xinyang 464000

Corresponding author: Chen Dong, chchendong2010@163.com

Funds: Project supported by the National Natural Science Foundation of China (Grant No. 61475132) and the Key Projects of the Higher Education Institutions of Henan Province (Grant No. 16A140033)

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References

[1]	Fiebig M, Lottermoser T, Meier D, Trassin M 2016 Nat. Rev. Mater. 1 16046 Google Scholar
[2]	Dong S, Liu J M, Cheong S W, Ren Z F 2015 Adv. Phys. 64 519 Google Scholar
[3]	王春雷, 易晓磊, 姚超, 张谦君, 林鹤, 王栋梁, 马衍伟 2015 物理学报 64 117401 Google Scholar Wang C L, Yi X L, Yao C, Zhang Q J, Lin H, Wang D L, Ma Y W 2015 Acta Phys. Sin. 64 117401 Google Scholar
[4]	Yin H, Liu C, Zheng G P, Wang Y, Ren F 2019 Appl. Phys. Lett. 114 192903 Google Scholar
[5]	Dong S, Yamauchi K, Yunoki S, et al. 2009 Phys. Rev. Lett. 103 127201 Google Scholar
[6]	Zhou P X, Dong S, Liu H M, Ma C Y, Yan Z B, Zhong C G, Liu J M 2015 Sci. Rep. 5 13052 Google Scholar
[7]	Feng M H, You S, Cheng N, Du J H 2019 Electrochim. Acta 293 356 Google Scholar
[8]	Sun Z Z, Feng S, Gu C, Cheng N, Liu J 2019 Phys. Chem. Chem. Phys. 21 15206 Google Scholar
[9]	Chen M, Zha R H, Yuan Z Y, et al. 2017 Chem. Eng. J. 313 791 Google Scholar
[10]	倪利红 2012 博士学位论文 (杭州: 浙江大学) Ni L H 2012 Ph. D. Dissertation (Hangzhou: Zhejiang University) (in Chinese)
[11]	Zhou Y J, Rabe K M 2013 Phys. Rev. B 88 094416 Google Scholar
[12]	Zhong C, Lu X, Wan Y, Min Y, Zhao Z, Zhou P, Dong Z, Liu J 2018 J. Magn. Magn. Mater. 466 406 Google Scholar
[13]	Renshaw Wang X, Li C J, et al. 2015 Science 349 716 Google Scholar
[14]	Burton J D, Tsymbal E Y 2009 Phys. Rev. B 80 174406 Google Scholar
[15]	Dong S, Dagotto E 2013 Phys. Rev. B 88 140404R Google Scholar
[16]	Cui B, Song C, Mao H, Wu H, Li F, Peng J, Wang G, Zeng F, Pan F 2015 Adv. Mater. 27 6651 Google Scholar
[17]	Mishina E D, Buryakov A M, Sherstyuk N E, Sigov A S, Rasing T 2016 Ferroelectrics 500 37 Google Scholar
[18]	Weng Y K, Huang X, Yao Y G, Dong S 2015 Phys. Rev. B 92 195114 Google Scholar
[19]	Chen L Y, Chen C L, Jin K X, Wu T 2014 J. Appl. Phys. 116 074102 Google Scholar
[20]	Lysogorskii Y V, Piyanzina I I, Lenotyev A V, et al. 2019 Ferroelectrics 541 74 Google Scholar
[21]	Chen D, Zhang G B, Cheng Z X, Dong S, Wang Y X 2019 IUCrJ 6 189 Google Scholar
[22]	Weng Y K, Lin L F, Dagotto E, Dong S 2016 Phys. Rev. Lett. 117 037601 Google Scholar
[23]	Callori S J, Gabel J, Su D, Sinsheimer J, Fernandez-Serra M V, Dawber M 2012 Phys. Rev. Lett. 109 067601 Google Scholar
[24]	Zhou P X, Liu H M, Yan Z B, Dong S, Liu J M 2014 J. Appl. Phys. 115 17D710 Google Scholar
[25]	Wei L Y, Lian C, Meng S 2017 Phys. Rev. B 95 184102 Google Scholar
[26]	Cheng X R, Shen M R 2007 Solid State Commun. 141 587 Google Scholar
[27]	Zhang H M, Weng Y K, Yao Y X, Dong S 2015 Phys. Rev. B 91 195145 Google Scholar
[28]	赵润, 杨浩 2018 物理学报 67 156101 Google Scholar Zhao R, Yang H 2018 Acta Phys. Sin. 67 156101 Google Scholar
[29]	Sheng J M, Kan X C, Ge H, et al. 2020 Chin. Phys. B 29 057503 Google Scholar
[30]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[31]	Liechtenstein A I, Anisimov V I, Zaanen J 1995 Phys. Rev. B 52 R5467 Google Scholar
[32]	Lee J H, Delaney K T, Bousquet E, Spaldin N A, Rabe K M 2013 Phys. Rev. B 88 174426 Google Scholar
[33]	Broyden C G 1969 AMS Notices 16 670 Google Scholar
[34]	Ciucivara A, Sahu B, Kleinman L 2008 Phys. Rev. B 77 092407 Google Scholar
[35]	Hashimoto T, Ishibashi S, Terakura K 2010 Phys. Rev. B 82 045124 Google Scholar
[36]	Betancourt J, Paudel T R, Tsymbal E Y, Velev J P 2017 Phys. Rev. B 96 045113 Google Scholar
[37]	He J, Borisevich A, Kalinin S V, Pennycook S J, Pantelides S T 2010 Phys. Rev. Lett. 105 227203 Google Scholar
[38]	Sun W, Wang W X, Chen D, Cheng Z X, Wang Y X 2019 Nanoscale 11 9931 Google Scholar
[39]	An M, Weng Y K, Zhang H M, Zhang J J, Zhang Y, Dong S 2017 Phys. Rev. B 96 235112 Google Scholar
[40]	Aruta C, Adamo C, Galdi A, et al. 2009 Phys. Rev. B 80 140405R Google Scholar
[41]	Song G, Zhang W Y 2014 Sci. Rep. 4 4564 Google Scholar
[42]	Liu C, Wang W H, Gong S, Zhang H B, Guo W 2017 Sci. Rep. 7 3856 Google Scholar
[43]	Lee J, Sai N, Cai T, Niu Q, Demkov A A 2010 Phys. Rev. B 81 144425 Google Scholar

Cited By

图 1 LaMnO₃/BaTiO₃超晶格的结构示意图(± P铁电极化的方向如箭头所示)

Figure 1. Schematic structure of the LaMnO₃/BaTiO₃ superlattice. (The arrows denote the directions of ferroelectric polarization).

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图 2 (a)−(n) LaMnO₃/BaTiO₃超晶格的磁序随着外延应变(–3%−3%)和极化方向的变化示意图 (蓝色代表自旋向上的Mn原子, 红色代表自旋向下的Mn原子); (o) 不同应变对应的最稳定结构的能量

Figure 2. (a)−(n) Schematic diagram of the magnetic configuration variation with the epitaxial strain (–3%−3%) and the direction of ferroelectric polarization in the LaMnO₃/BaTiO₃ superlattices (The blue and red balls represent the spin-up and spin-down Mn atoms, respectively); (o) the total energies of the ground-state superlattices under different strains.

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图 3 LaMnO₃/BaTiO₃超晶格的态密度:　(a)–P极化和–3%外延应变时的总态密度和BaTiO₃层的分层态密度; (b) +P极化和–3%外延应变时的总态密度和BaTiO₃层的分层态密度; (c)–P极化和–3%外延应变以及(d) +P极化和–3%外延应变时的LaMnO₃层的分层态密度和Mn原子的e_g/t_2g轨道的态密度

Figure 3. The total density of states (TDOS) and layer-resolved DOS of the BaTiO₃ part of the LaMnO₃/BaTiO₃ superlattice: (a) for the –P case with –3% epitaxial strain; (b) for the +P case with –3% strain. The Mn-e_g/t_2g DOS and the layer-resolved DOS of the LaMnO₃ part (c) for the –P case with –3% epitaxial strain; (d) for the +P case with –3% strain.

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图 4 LaMnO₃/BaTiO₃超晶格的态密度:　(a) –P极化和3%外延应变时的总态密度和BaTiO₃层的分层态密度; (b) +P极化和3%外延应变时的总态密度和BaTiO₃层的分层态密度; (c) –P极化和3%外延应变以及(d) +P极化和3%外延应变时的LaMnO₃层的分层态密度和Mn原子的e_g/t_2g轨道的态密度

Figure 4. The total density of states (TDOS) and layer-resolved DOS of the BaTiO₃ part of the LaMnO₃/BaTiO₃ superlattice: (a) for the –P case with 3% epitaxial strain; (b) for the +P case with 3% strain. The Mn-e_g/t_{2 g} DOS and the layer-resolved DOS of the LaMnO₃ part (c) for the –P case with 3% strain; (d) for the +P case with 3% strain.

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图 5 LaMnO₃/BaTiO₃超晶格在　(a) –P极化和–3%外延应变; (b) –P极化和3%外延应变; (c) +P极化和–3%外延应变和(d) +P极化和3%外延应变条件下的差分电荷密度图(等值面的数值为0.01 e/bohr³)

Figure 5. Charge density difference of the LaMnO₃/BaTiO₃ superlattices for the (a) –P polarization and –3% epitaxial strain; (b) –P polarization and 3% strain; (c) +P polarization and –3% strain; and (d) +P polarization and 3% strain. The isosurface value is set to be 0.01 e/bohr³.

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表 1 计算得到的LaMnO₃/BaTiO₃超晶格的基态性质: m₁和m₂ (μ_B)是Mn原子的平均磁矩, M (μ_B)是超晶格的净磁化强度, 导电性, LaMnO₃层的Jahn-Teller畸变Q₂, Q₃(nm), 氧八面体倾斜角θ和旋转角φ

Table 1. The calculated ground-state properties of the LaMnO₃/BaTiO₃ superlattice at different strains: m₁ and m₂ (μ_B) are the local magnetic moment for the Mn atoms, M (μ_B) is the net magnetization, the conductivity, the Jahn-Teller distortions Q₂, Q₃ (nm), the octahedral tilt angle θ and rotation angle φ (degree) of the LaMnO₃ layers.

应变	极化	磁序	m₁	m₂	M	导电性	θ₁	θ₂	φ₁	φ₂	Q₂	Q₃
—	+	FM	3.56	3.56	14.65	金属	5.7	6.6	4.4	5.3	0.0015	0.0259
—	–	FiM2	3.38	–3.76	6.41	金属	6.5	7.8	5.1	7.1	0.0017	0.0172
—	+	FiM2	3.41	–3.86	6.34	金属	7.2	8.2	4.5	6.9	0.0016	0.0198
—	–	FM	3.59	3.59	14.76	金属	7.5	8.7	5.3	7.8	0.0026	0.0199
—	+	FiM1	3.60	–3.72	6.78	金属	8.8	10.0	3.9	6.9	0.0019	0.0229
—	–	FiM3	3.55	–3.59	7.20	半金属	9.3	10.4	4.1	5.8	–0.0007	0.0347
0	+	A-AFM	3.24	–3.55	—	金属	1.7	1.2	11.7	1.2	0.0010	0.0139
0	–	FM	3.67	3.67	15.28	半金属	7.1	9.1	9.3	0.8	0.0047	0.0042
1%	+	A-AFM	3.66	–3.68	—	金属	9.3	9.9	7.5	6.4	0.0449	0.0272
1%	–	A-AFM	3.46	–3.92	—	半金属	11.5	12.4	4.4	8.0	0.0071	0.0286
2%	+	G-AFM	3.31	–3.95	—	绝缘体	11.9	11.1	6.1	7.0	0.0507	0.0165
2%	–	FiM4	-3.78	3.66	7.24	半金属	12.5	11.1	3.3	8.8	0.0013	0.0114
3%	+	A-AFM	3.71	–3.72	—	绝缘体	12.2	12.2	6.3	7.4	–1.0308	0.0967
3%	–	FM	3.75	3.75	15.17	半金属	13.7	13.3	5.0	8.9	0.0208	0.0324

DownLoad: CSV

表 2 不同外延应变和极化条件下LaMnO₃/BaTiO₃超晶格的Mn-3d轨道(含e_g和t_2g)的电子数

Table 2. Number of electrons for the Mn-3d orbitals (both e_g and t_2g) in the LaMnO₃/BaTiO₃ superlattice at different conditions.

应变	极化	磁序	e_g轨道	t_2g轨道	3d轨道
–3%	–P	FiM2	1.77	3.15	4.92
–3%	+P	FM	1.68	3.26	4.94
0	–P	FM	1.91	3.03	4.94
0	+P	A-AFM	1.75	3.16	4.91
3%	–P	FM	1.80	3.02	4.81
3%	+P	A-AFM	1.60	3.26	4.87

DownLoad: CSV

[1]	Fiebig M, Lottermoser T, Meier D, Trassin M 2016 Nat. Rev. Mater. 1 16046 Google Scholar
[2]	Dong S, Liu J M, Cheong S W, Ren Z F 2015 Adv. Phys. 64 519 Google Scholar
[3]	王春雷, 易晓磊, 姚超, 张谦君, 林鹤, 王栋梁, 马衍伟 2015 物理学报 64 117401 Google Scholar Wang C L, Yi X L, Yao C, Zhang Q J, Lin H, Wang D L, Ma Y W 2015 Acta Phys. Sin. 64 117401 Google Scholar
[4]	Yin H, Liu C, Zheng G P, Wang Y, Ren F 2019 Appl. Phys. Lett. 114 192903 Google Scholar
[5]	Dong S, Yamauchi K, Yunoki S, et al. 2009 Phys. Rev. Lett. 103 127201 Google Scholar
[6]	Zhou P X, Dong S, Liu H M, Ma C Y, Yan Z B, Zhong C G, Liu J M 2015 Sci. Rep. 5 13052 Google Scholar
[7]	Feng M H, You S, Cheng N, Du J H 2019 Electrochim. Acta 293 356 Google Scholar
[8]	Sun Z Z, Feng S, Gu C, Cheng N, Liu J 2019 Phys. Chem. Chem. Phys. 21 15206 Google Scholar
[9]	Chen M, Zha R H, Yuan Z Y, et al. 2017 Chem. Eng. J. 313 791 Google Scholar
[10]	倪利红 2012 博士学位论文 (杭州: 浙江大学) Ni L H 2012 Ph. D. Dissertation (Hangzhou: Zhejiang University) (in Chinese)
[11]	Zhou Y J, Rabe K M 2013 Phys. Rev. B 88 094416 Google Scholar
[12]	Zhong C, Lu X, Wan Y, Min Y, Zhao Z, Zhou P, Dong Z, Liu J 2018 J. Magn. Magn. Mater. 466 406 Google Scholar
[13]	Renshaw Wang X, Li C J, et al. 2015 Science 349 716 Google Scholar
[14]	Burton J D, Tsymbal E Y 2009 Phys. Rev. B 80 174406 Google Scholar
[15]	Dong S, Dagotto E 2013 Phys. Rev. B 88 140404R Google Scholar
[16]	Cui B, Song C, Mao H, Wu H, Li F, Peng J, Wang G, Zeng F, Pan F 2015 Adv. Mater. 27 6651 Google Scholar
[17]	Mishina E D, Buryakov A M, Sherstyuk N E, Sigov A S, Rasing T 2016 Ferroelectrics 500 37 Google Scholar
[18]	Weng Y K, Huang X, Yao Y G, Dong S 2015 Phys. Rev. B 92 195114 Google Scholar
[19]	Chen L Y, Chen C L, Jin K X, Wu T 2014 J. Appl. Phys. 116 074102 Google Scholar
[20]	Lysogorskii Y V, Piyanzina I I, Lenotyev A V, et al. 2019 Ferroelectrics 541 74 Google Scholar
[21]	Chen D, Zhang G B, Cheng Z X, Dong S, Wang Y X 2019 IUCrJ 6 189 Google Scholar
[22]	Weng Y K, Lin L F, Dagotto E, Dong S 2016 Phys. Rev. Lett. 117 037601 Google Scholar
[23]	Callori S J, Gabel J, Su D, Sinsheimer J, Fernandez-Serra M V, Dawber M 2012 Phys. Rev. Lett. 109 067601 Google Scholar
[24]	Zhou P X, Liu H M, Yan Z B, Dong S, Liu J M 2014 J. Appl. Phys. 115 17D710 Google Scholar
[25]	Wei L Y, Lian C, Meng S 2017 Phys. Rev. B 95 184102 Google Scholar
[26]	Cheng X R, Shen M R 2007 Solid State Commun. 141 587 Google Scholar
[27]	Zhang H M, Weng Y K, Yao Y X, Dong S 2015 Phys. Rev. B 91 195145 Google Scholar
[28]	赵润, 杨浩 2018 物理学报 67 156101 Google Scholar Zhao R, Yang H 2018 Acta Phys. Sin. 67 156101 Google Scholar
[29]	Sheng J M, Kan X C, Ge H, et al. 2020 Chin. Phys. B 29 057503 Google Scholar
[30]	Perdew J P, Burke K, Ernzerhof M 1996 Phys. Rev. Lett. 77 3865 Google Scholar
[31]	Liechtenstein A I, Anisimov V I, Zaanen J 1995 Phys. Rev. B 52 R5467 Google Scholar
[32]	Lee J H, Delaney K T, Bousquet E, Spaldin N A, Rabe K M 2013 Phys. Rev. B 88 174426 Google Scholar
[33]	Broyden C G 1969 AMS Notices 16 670 Google Scholar
[34]	Ciucivara A, Sahu B, Kleinman L 2008 Phys. Rev. B 77 092407 Google Scholar
[35]	Hashimoto T, Ishibashi S, Terakura K 2010 Phys. Rev. B 82 045124 Google Scholar
[36]	Betancourt J, Paudel T R, Tsymbal E Y, Velev J P 2017 Phys. Rev. B 96 045113 Google Scholar
[37]	He J, Borisevich A, Kalinin S V, Pennycook S J, Pantelides S T 2010 Phys. Rev. Lett. 105 227203 Google Scholar
[38]	Sun W, Wang W X, Chen D, Cheng Z X, Wang Y X 2019 Nanoscale 11 9931 Google Scholar
[39]	An M, Weng Y K, Zhang H M, Zhang J J, Zhang Y, Dong S 2017 Phys. Rev. B 96 235112 Google Scholar
[40]	Aruta C, Adamo C, Galdi A, et al. 2009 Phys. Rev. B 80 140405R Google Scholar
[41]	Song G, Zhang W Y 2014 Sci. Rep. 4 4564 Google Scholar
[42]	Liu C, Wang W H, Gong S, Zhang H B, Guo W 2017 Sci. Rep. 7 3856 Google Scholar
[43]	Lee J, Sai N, Cai T, Niu Q, Demkov A A 2010 Phys. Rev. B 81 144425 Google Scholar

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Dual control of magnetism in LaMnO₃/BaTiO₃ superlattice by epitaxial strain and ferroelectric polarization

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Dual control of magnetism in LaMnO3/BaTiO3 superlattice by epitaxial strain and ferroelectric polarization

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Dual control of magnetism in LaMnO₃/BaTiO₃ superlattice by epitaxial strain and ferroelectric polarization