High-temperature ferromagnetic metallic phase in LaMnO3/Sr3Al2O6 heterostructure

doi:10.1016/j.jmst.2021.11.071

Abstract

Abstract:

To achieve a flexible single-crystal multifunctional membrane, the freestanding process of a rigid epitaxial transition metal oxide thin film via a buffered water-dissolution sacrificial layer has attracted reasonable attentions. Owing to the difference in chemical potential, specific element affinity, and lattice constant between the target membrane and the sacrificial layer, the freestanding process may cause an indelible change of physics property once the target thin film is sensitive to the above factors. Here, the heterostructures composed of the generally adopted sacrificial layer Sr₃Al₂O₆ (SAO) and LaMnO₃ (LMO) have been systematically investigated. The electrical and magnetic properties of LMO show extreme sensitivity to the thickness of SAO (t_SAO). Then we have also found that LMO/SAO heterostructures can exhibit the coexistence of two ferromagnetic phases, the significantly enhanced Curie temperature ∼342 K, and the large magnetoresistance -23.3% at 300 K, which is similar to the optimal-doped manganite such as La_2/3Sr_1/3MnO₃. X-ray diffraction results show that continuously tunable strain from out-of-plane tension to relaxation and then to compression can be generated by adjusting t_SAO. This strain can stabilize the migrated oxygen from LMO to SAO, which is induced by the large oxygen affinity difference between B-site Mn and Al. It is believed that these unexpected electrical/magnetic phenomena are originated from the combined effects of interfacial element diffusion and strain. Our study provides a strategy for designing new magnetic phases, and a reference for the fundamental understanding of strongly correlated transition metal oxide systems in the freestanding process.

Key words: Sr₃Al₂O₆, LaMnO₃, Oxygen affinity, Oxygen ions migration, Strain effects

Di Wang, Bin He, Jinrui Guo, Qixiang Wang, Chaoqun Shi, Yue Han, Hong Fang, Jie Wang, Nana Zhang, Peng Zhang, Yanan Chen, Changwen Zhang, Weiming Lü, Shishen Yan. High-temperature ferromagnetic metallic phase in LaMnO₃/Sr₃Al₂O₆ heterostructure[J]. J. Mater. Sci. Technol., 2022, 119: 69-74.

Figures/Tables 4

Fig. 1. (a) XRD patterns of the LMO/SAO heterostructures with tSAO = 0, 20 nm grown on STO (001) substrate. Inset: surface morphology of the sample tSAO = 20 nm. (b) High-resolution XRD results around (002) diffraction peaks of the samples with tSAO = 0-20 nm. The LMO peaks of the samples tSAO = 2, 3 nm are fitted by the formula in ref [15]. and the fitting result of the sample tSAO = 2 nm is shown in the inset. (c) tSAO dependence of the c parameter and the out-of-plane strain (εLMO = 100% × (cfilm - cbulk)/cbulk) of LMO.

(a) Temperature dependence of the normalized magnetic moment, M(T)/M(10 K), of LMO/SAO heterostructures with various tSAO. (b) Field dependence of the magnetization of the samples tSAO = 0, 2, 7, and 20 nm at 10 K. Curie temperature Tc and saturation magnetization Msat as a function of tSAO are shown in (c) and (d) respectively. Region Ⅰ (tSAO < 3 nm) and region Ⅱ (tSAO ≥ 3 nm) are filled with yellow and green, respectively.

Fig. 3. (a) Temperature dependence of the resistivity of LMO/SAO heterostructures with various tSAO under 0 T (solid line) and 3 T (dash line) magnetic fields. The insulator-metal transition temperature TIM as a function of tSAO is shown in (b) and the magnetoresistance (MR) as a function of temperature is shown in (c). MR = (ρ3T-ρ0T)/ρ0T × 100%, where ρ0 and ρ3T are the resistivities at 0 T and 3 T, respectively. (d) The change of room temperature (300 K) ρ and room temperature MR against tSAO.

Fig. 4. Schematic diagrams of oxygen ions migration and strain effects in LMO/SAO heterostructures. (a) With the insertion of SAO, oxygen ions migrate from LMO to SAO. (b) Left panel: overhead views of the MnO6 octahedron networks with in-plane compressive (top panel) and tensile (bottom panel) strains. θ and d represent in-plane Mn-O-Mn bond angle and Mn-O bond length, respectively (d2 > d1, θ2 > θ1). Right panel: eg orbital occupancy of Mn3+ at compressive (top panel) and tensile (bottom panel) strains. The in-plane contraction (compressive strain) favors the d3z2-r2 occupancy. The in-plane elongation (tensile strain) with enhanced bond length d2 and bond angle θ2 favors the dx2-y2 occupancy.

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High-temperature ferromagnetic metallic phase in LaMnO₃/Sr₃Al₂O₆ heterostructure

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