Abstract

La0.7Sr0.3MnO3, a half-metallic ferromagnet with full spin polarization, is generally used as a standard spin injector in heterostructures. However, the magnetism of La0.7Sr0.3MnO3 is strongly modified near interfaces, which was addressed as “dead-layer” phenomenon whose origin is still controversial. Here, both magnetic and structural properties of La0.7Sr0.3MnO3/SrTiO3 heterostructures were investigated, with emphasis on the quantitative analysis of oxygen octahedral rotation (OOR) across interfaces using annular-bright-field imaging. OOR was found to be significantly altered near interface for both La0.7Sr0.3MnO3 and SrTiO3, as linked to the magnetism deterioration. Especially in La0.7Sr0.3MnO3/SrTiO3 superlattices, the almost complete suppression of OOR in 4 unit-cell-thick La0.7Sr0.3MnO3 results in a canted ferromagnetism. Detailed comparisons between strain and OOR relaxation and especially the observation of an unexpected La0.7Sr0.3MnO3 lattice c expansion near interfaces, prove the relevance of OOR for the magnetic properties. These results indicate the capability of tuning the magnetism by engineering OOR at the atomic scale.

Highlights

  • Proposed[22,23]; interfacial orbital reconstruction might occur destroying the double-exchange interaction close to the interface[24,25,26]; there might be interfacial charge transfer[18,27,28,29]

  • An oxygen octahedral rotation (OOR) mismatch of ~10° across the LSMO/STO hetero-interface leads to a significant alteration of the rotation angles in both STO and LSMO layers, such that the suppression of OOR in LSMO can be intuitively linked to the deterioration of magnetism

  • Two representative samples were selected: (1) a triple layer sandwich-like sample consisted of two LSMO layers with thicknesses of 10 and 20 u.c. spaced by a 3 u.c. thick STO interlayer; (2) a LSMO/STO superlattice consisting of 15 bilayers of 4 u.c. thick LSMO and 6 u.c. thick STO

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Summary

Introduction

Proposed[22,23]; interfacial orbital reconstruction might occur destroying the double-exchange interaction close to the interface[24,25,26]; there might be interfacial charge transfer[18,27,28,29]. In LSMO/STO based heterostructures, both LSMO and STO have ABO3 type perovskite structure, but due to different tolerance factors, STO is cubic at room temperature with a transition to a tetragonal phase below 105 K, whereas LSMO is rhombohedral in bulk[31], but orthorhombic/tetragonal in thin films[32,33] This demonstrates that the perovskite structure is versatile in accommodating chemical strain, as well as external structural strain. The almost complete suppression of OOR in 4 u.c. thick LSMO within a LSMO/STO superlattice results in a strongly canted magnetism, which discloses the previously reported magnetic-dead-layer phenomenon These findings suggest an efficient interfacial engineering mechanism of magnetic and electronic properties through OOR coupling at the atomic scale

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Conclusion

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