Competing between oxygen tilts and polar shifts in BiFeO 3 thin films

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1 Journées Electromagnons Institut Néel Competing between oxygen tilts and polar shifts in BiFeO 3 thin films B. Dkhil Laboratoire Structures, Propriétés et Modélisation des Solides, CNRS-UMR 8580, Ecole Centrale Paris, France brahim.dkhil@ecp.fr

2 What does people have usually in mind about multiferroicity? [Wang, Liu, Ren, Adv. Phys. (2009)]

3 What about elasticity (in perovskite)? Polar shift Oxygen octahedra tilts/rotations a b Or FE like BaTiO 3 non-fe like SrTiO 3 ω Both perovskite instabilities coexist in FE BiFeO 3 at RT

4 Bulk BiFeO 3 : what we can believe FERROELECTRICITY/ELASTICITY T C ~ 1100K, R3c Polarization along [111] P~90C/m² Strong oxygen tilting (a - a - a - ) ~ 13 ANTIFERROMAGNETISM T N ~ 640K G-type + non-commensurable cycloide (~64nm) Magnetism is perpendicular to FE polarization G-type Ordering M Fe1 [111] G-type Ordering + Spin- Orbit Interactions [111] M Fe1 M Fe2 M M Fe2 Canting??? : weak ferromagnetism

5 Goals Oxygen octahedra tilts (usually neglected) play a key role Tilts fight against the polarization : strong competition Tilts strongly affect the phase transition : especially unexpected behavior of the temperature of the ferroelectric transition!!!! New approach to design multiferroic with improved magnetoelectric properties

6 Menu Strain-engineering in BFO films Phase transitions in BFO films Conclusion

7 Strain engineering or why going towards thin films Pertsev s phase diagram [Pertsev et al., PRL98] Strain-polarization coupling : Case of BaTiO 3 LGD approach Misfit : - 2% [Shirokov, Yuzyuk, Dkhil, Lemanov, PRB07] [Pertsev, Dkhil, APL08]

8 Case of 70nm-thick BFO onto SrTiO 3 (STO) SrTiO 3 (STO) Misfit strain of 1.4% Electric field (MV/m) P Z (µc/cm²) Current (µa) Voltage (V) But only a weak, if any, increasing of the polarization -400 Analogy with MPB-like behavior i.e. Rotation of the polarization [Jang et al., PRL08]

9 So let us try to force a giant polarization : BiFeO 3 thin film onto LaAlO 3 (LAO) LAO LaAlO 3 (LAO) Misfit strain of 4.8% Still monoclinic!!!!! Béa, Dupé, Fusil, Mattana, Jacquet, Warot-Fonrose, Wilhelm, Rogalev, Petit, Cros, Anane, Petroff, Bouzehouane, Geneste, Dkhil, Lisenkov, Ponomareva, Bellaiche, Bibes, Barthelemy, PRL09

10 Why is it still monoclinic? LAO [Hatch, Ederer, Spaldin, PRB10] Cm Cc STO Dupé, Canero-Infante, Geneste, Janolin, Bibes, Barthélémy, Lisenkov, Bellaiche, Ravy, Dkhil, PRB10

11 Evidence of Cc to Cm phase transition under misfit-strain

12 Oxygen tilts fight against the polarization in BFO

13 Menu Strain-engineering in BFO films Phase transitions in BFO films Conclusion

14 Consequences on phase transitions in BFO films

15 Effect on the FE transition evidenced using XRD

16 Effect on the FE transition evidenced using XRD (T) = (c FE film (T)-c PE film (T))/c FE film (300K) c PE film (T)=a PE bulk (T) [1+2 film /( film -1) (a subst (T)/a PE bulk (T)-1)] (T)=A+B*(T C -T) 1/ c BFO Do not forget that T C bulk ~ 1100K!!!! c (Å) c STO T (K) The ferroelectric T C temperature decreases under compressive stresses!!!

17 Effect on the FE transition evidenced using XRD 200nm T c, bulk =1100K~830 C T c, film =1030K~760 C dirty -like BFO film H. Toupet, F. Le Marrec, C. Lichtensteiger, B. Dkhil, M.G. Karkut, PRB10

18 T C decreasing evidenced by PFM ms= -2.3% ms= -0.8%

19 What about T N the AFM phase transition BFO//STO BFO//GSO

20 Phase diagram in BFO films : experimental and theoretical comparison Calculations based on I. A. Kornev, S. Lisenkov, R. Haumont, B. Dkhil, L. Bellaiche, PRL07 ( bulk BFO) Typical phase diagram for perovskite-like ferroelectrics without oxygen tilts Higher magnetoelectric effect is expected

21 Phase transitions in BFO films or how oxygen tilts and polar shifts compete Infante, Lisenkov, Dupé, Bibes, Fusil, Jacquet, Geneste, Petit, Courtial, Juraszek, Bellaiche, Barthélémy, Dkhil, PRL10

22 Menu Strain-engineering in BFO films Phase transitions in BFO films Conclusion

23 Conclusion = Goals Oxygen octahedra tilts (usually neglected) play a key role Tilts fight against the polarization Tilts strongly affect the phase transition New approach to design high magnetoelectric coupling

24 The people who really worked B. Dupé, I.C. Infante, P. Gemeiner, G. Geneste, P.-E. Janolin, I. Kornev : ECP, France I.C. Infante, S. Fusil, E. Jacquet, M. Bibes, A. Barthélémy : UMR CNRS- Thalès, France S. Lisenkov, I. Ponamoreva, L. Bellaiche : Univ. Arkansas, USA H. Toupet, F. Le Marrec : Univ. of Jules Verne, France

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