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Register a new userInterface control of ferroelectricity in a SrRuO3/BaTiO3/SrRuO3 capacitor and its critical thickness
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The atomic-scale synthesis of artificial oxide heterostructures offers new opportunities to create novel states that do not occur in nature. The main challenge related to synthesizing these structures is obtaining atomically sharp interfaces with designed termination sequences. Here, we demonstrate that the oxygen pressure (PO2) during growth plays an important role in controlling the interfacial terminations of SrRuO3/BaTiO3/SrRuO3 (SRO/BTO/SRO) ferroelectric capacitors. The SRO/BTO/SRO heterostructures were grown by the pulsed laser deposition (PLD) method. The top SRO/BTO interface grown at high PO2 (around 150 mTorr) usually exhibited a mixture of RuO2-BaO and SrO-TiO2 terminations. By reducing PO2, we obtained atomically sharp SRO/BTO top interfaces with uniform SrO-TiO2 termination. Using capacitor devices with symmetric and uniform interfacial termination, we were able to demonstrate for the first time that the ferroelectric (FE) critical thickness can reach the theoretical limit of 3.5 unit cells (u.c.).
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Atomically engineered oxide multilayers and superlattices display unique properties responsive to the electronic and atomic structures of the interfaces. We have followed the growth of ferroelectric BaTiO3 on SrRuO3 electrode with in situ atomic scale analysis of the surface structure at each stage. An oxygen-induced surface reconstruction of SrRuO3 leads to formation of SrO rows spaced at twice the bulk periodicity. This reconstruction modifies the structure of the first BaTiO3 layers grown subsequently, including intermixing observed with cross-section spectroscopy. These observations reveal that this common oxide interface is much more interesting than previously reported, and provide a paradigm for oxygen engineering of oxide structure at an interface.
Structural studies on ultrathin SrRuO3/BaTiO3/SrRuO3 capacitors, with BaTiO3 thicknesses of between 5 nm and 30 nm, show well-defined interfaces between ferroelectric BaTiO3 and electrode SrRuO3 layers. In these capacitors, we cannot observe any extrinsic electrical effects due to either the formation of an insulating interfacial passive layer or passive-layer-induced charge injection. Such high quality interfaces result in very good fatigue endurance, even for the 5 nm thick BaTiO3 capacitor.
The electronic properties of SrRuO3/LaAlO3 (SRO/LAO) superlattices with different interlayer thicknesses of SRO layers were studied. As the thickness of SRO layers is reduced, the superlattices exhibit a metal-insulator transition implying transformation into a more localized state from its original bulk metallic state. The strain effect on the metal-insulator transition was also examined. The origin of the metal-insulator transition in ultrathin SRO film is discussed. All the superlattices, even those with SRO layers as thin as 2 unit cells, are ferromagnetic at low temperatures. Moreover, we demonstrate field effect devices based on such multilayer superlattice structures.
The recent observation of Weyl fermions in the itinerant 4d ferromagnetic perovskite SrRuO3 points to this material being a good platform for exploring novel physics related to a pair of Weyl nodes in epitaxial heterostructures. In this letter, we report the thickness-dependent magnetotransport properties of ultra-high-quality epitaxial SrRuO3 films grown under optimized conditions on SrTiO3 substrates. Signatures of Weyl fermion transport, i.e., unsaturated linear positive magnetoresistance accompanied by a quantum oscillation having a {pi} Berry phase, were observed in films with thicknesses as small as 10 nm. Residual resistivity increased with decreasing film thickness, indicating disorder near the interface between SrRuO3 and the SrTiO3 substrate. Since this disorder affects the magnetic and electrical properties of the films, the Curie temperature decreases and the coercive field increases with decreasing thickness. Thickness-dependent magnetotransport measurements revealed that the threshold residual resistivity ratio (RRR) to observe Weyl fermion transport is 21. These results provide guidelines for realizing quantum transport of Weyl fermions in SrRuO3 near heterointerfaces.
Manipulation of octahedral distortion at atomic length scale is an effective means to tune the physical ground states of functional oxides. Previous work demonstrates that epitaxial strain and film thickness are variable parameters to modify the octahedral rotation and tilt. However, selective control of bonding geometry by structural propagation from adjacent layers is rarely studied. Here we propose a new route to tune the ferromagnetic response in SrRuO3 (SRO) ultrathin layers by oxygen coordination of adjacent SrCuO2 (SCO) layers. The infinite-layered CuO2 in SCO exhibits a structural transformation from planar-type to chain-type as reducing film thickness. These two orientations dramatically modify the polyhedral connectivity at the interface, thus altering the octahedral distortion of SRO. The local structural variation changes the spin state of Ru and hybridization strength between Ru 4d and O 2p orbitals, leading to a significant change in the magnetoresistance and anomalous Hall resistivity of SRO layers. These findings could launch further investigations into adaptive control of magnetoelectric properties in quantum oxide heterostructures using oxygen coordination.
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