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Register a new userAtomic-resolution TEM Studies of Pillar-Matrix Structures in Epitaxially Grown Ultrathin ZrO2-La2/3Sr1/3MnO3 Films
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Authors
Dan Zhou
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We studied ZrO2-La2/3Sr1/3MnO3 pillar matrix thin films which were found to show anomalous magnetic and electron transport properties controlled by the amount of ZrO2. With the application of an aberration corrected transmission electron microscope, structure and chemical information of the system, especially of the pillar matrix interface were revealed at atomic resolution. Minor amounts of Zr were found to occupy Mn positions within the matrix and its solubility within the matrix was found to be less than 6 mol%. Moreover, the Zr concentration reached minimum concentration at the pillar matrix interface accompanied by oxygen deficiency. La and Mn diffusion into the pillar was observed along with a change of the Mn valence state. La and Mn positions inside ZrO2 pillars were also revealed at atomic resolution. These results provide detailed information for future studies of macroscopic properties of these materials.
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We analyze X-ray diffraction data used to extract cell parameters of ultrathin films on closely matching substrates. We focus on epitaxial La2/3Sr1/3MnO3 films grown on (001) SrTiO3 single crystalline substrates. It will be shown that, due to extremely high structural similarity of film and substrate, data analysis must explicitly consider the distinct phase of the diffracted waves by substrate and films to extract reliable unit cell parameters. The implications of this finding for the understanding of strain effects in ultrathin films and interfaces will be underlined
The electronic structure and equilibrium geometry of La2/3Sr1/3MnO3 are studied theoretically by means of density functional calculations. The doping is treated by introducing holes and a compensating jellium background. The results for the local density approximation (LDA) agree with previous LDA calculations, with an equilibrium volume 5.3% too small and with both majority and minority spin states present at the Fermi level for the relaxed system. The generalised gradient approximation (GGA) offers a qualitatively improved description of the system, with a more realistic volume, and a half-metallic behaviour for the relaxed structure, which enables studies needing theoretical relaxation.The ideal MnO2-terminated (001) surface is then described with explicit doping.
Epitaxial ferroelectric HfO2 films are the most suitable to investigate intrinsic properties of the material and for prototyping emerging devices. Ferroelectric Hf0.5Zr0.5O2(111) films have been epitaxially stabilized on La2/3Sr1/3MnO3(001) electrodes. This epitaxy, considering the symmetry dissimilarity and the huge lattice mismatch, is not compatible with conventional mechanisms of epitaxy. To gain insight into the epitaxy mechanism, scanning transmission electron microscopy characterization of the interface was performed, revealing arrays of dislocations with short periodicities. These observed periodicities agree with the expected for domain matching epitaxy, indicating that this unconventional mechanism could be the prevailing factor in the stabilization of ferroelectric Hf0.5Zr0.5O2 with (111) orientation in the epitaxial Hf0.5Zr0.5O2(111)/La2/3Sr1/3MnO3(001) heterostructure.
Understanding and manipulating properties emerging at a surface or an interface require a thorough knowledge of structure-property relationships. We report a study of a prototype oxide system, La2/3Sr1/3MnO3 grown on SrTiO3(001), by combining in-situ angle-resolved x-ray photoelectron spectroscopy, ex-situ x-ray diffraction, and scanning transmission electron microscopy/spectroscopy with electric transport measurements. We find that La2/3Sr1/3MnO3 films thicker than 20 unit cells (u.c.) exhibit a universal behavior with no more than one u.c. intermixing at the interface but at least 3 u.c. of Sr segregation near the surface which is (La/Sr)O terminated. The conductivity vs film thickness shows the existence of nonmetallic layers with thickness ~ 6.5 +/- 0.9 u.c., which is independent of film thickness but mainly relates to the deviation of Sr concentration near the surface region. Below 20 u.c., the surface of the films appears mixed (La/Sr)O with MnO2 termination. Decreasing film thickness to less than 10 u.c. leads to the enhanced deviation of chemical composition in the films and eventually drives the film insulating. Our observation offers a natural explanation for the thickness-driven metal-nonmetal transition in thin films based on the variation of film stoichiometry.
A Mn valence instability on La2/3Ca1/3MnO3 thin films, grown on LaAlO3 (001)substrates is observed by x-ray absorption spectroscopy at the Mn L-edge and O K-edge. As-grown samples, in situ annealed at 800 C in oxygen, exhibit a Curie temperature well below that of the bulk material. Upon air exposure a reduction of the saturation magnetization, MS, of the films is detected. Simultaneously a Mn2+ spectral signature develops, in addition to the expected Mn3+ and Mn4+ contributions, which increases with time. The similarity of the spectral results obtained by total electron yield and fluorescence yield spectroscopy indicates that the location of the Mn valence anomalies is not confined to a narrow surface region of the film, but can extend throughout the whole thickness of the sample. High temperature annealing at 1000 C in air, immediately after growth, improves the magnetic and transport properties of such films towards the bulk values and the Mn2+ signature in the spectra does not appear. The Mn valence is then stable even to prolonged air exposure. We propose a mechanism for the Mn2+ ions formation and discuss the importance of these observations with respect to previous findings and production of thin films devices.
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