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Register a new userPropagation control of octahedral tilt in SrRuO3 via artificial heterostructuring
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Bonding geometry engineering of metal-oxygen octahedra is a facile way of tailoring various functional properties of transition metal oxides. Several approaches, including epitaxial strain, thickness, and stoichiometry control, have been proposed to efficiently tune the rotation and tilting of the octahedra, but these approaches are inevitably accompanied by unnecessary structural modifications such as changes in thin-film lattice parameters. In this study, we propose a method to selectively engineer the octahedral bonding geometries, while maintaining other parameters that might implicitly influence the functional properties. A concept of octahedral tilt propagation engineering has been developed using atomically designed SrRuO3/SrTiO3 superlattices. In particular, the propagation of RuO6 octahedral tilting within the SrRuO3 layers having identical thicknesses was systematically controlled by varying the thickness of adjacent SrTiO3 layers. This led to a substantial modification in the electromagnetic properties of the SrRuO3 layer, significantly enhancing the magnetic moment of Ru. Our approach provides a method to selectively manipulate the bonding geometry of strongly correlated oxides, thereby enabling a better understanding and greater controllability of their functional properties.
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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.
Polarized neutron reflectometry measurements are presented exploring the evolution of ferrimagnetism in GdTiO$_3$ films as they are confined between SrTiO$_3$ layers of variable thicknesses. As GdTiO$_3$ films approach the thin layer limit and are confined within a substantially thicker SrTiO$_3$ matrix, the TiO$_6$ octahedral tilts endemic to GdTiO$_3$ coherently relax toward the undistorted, cubic phase of SrTiO$_3$. Our measurements reveal that the ferrimagnetic state within the GdTiO$_3$ layers survives as the TiO$_6$ octahedral tilts in the GdTiO$_3$ layers are suppressed. Furthermore, our data suggest that a magnetic dead layer develops within the GdTiO$_3$ layer at each GdTiO$_3$/ SrTiO$_3$ interface. The ferrimagnetic moment inherent to the core GdTiO$_3$ layers is negligibly (in models with dead layers) or only weakly (in models without dead layers) impacted as the octahedral tilt angles are suppressed by more than 50$%$ and the $t_{2g}$ bandwidth is dramatically renormalized.
In this work, the BiFeO3 (BFO)/SrRuO3 (SRO) heterostructure was fabricated and the anomalous Hall effect (AHE) was investigated the in BFO/SRO. It is found the nonmonotonic anomalous Hall resistivity behavior in BFO/SRO is originated from the inhomogeneous SRO layer instead of the topological Hall effect. It is surprised that the AHE in BFO/SRO structure can be manipulated by ferroelectric polarization of BFO. Moreover, an inhomogeneous phenomenological model has been applied on those structure. Furthermore, the modification of band structure in SRO under ferroelectric polarization was discussed by first principle calculation. The ferroelectric-manipulated AHE suggests a new pathway to realize nonvolatile, reversible and low energy-consuming voltage-controlled spintronic devices.
Distortions of the oxygen octahedra influence the fundamental electronic structure of perovskite oxides, such as their bandwidth and exchange interactions. Utilizing a fully ab-initio methodology based on density functional theory plus dynamical mean field theory (DFT+DMFT), we study the crystal and magnetic structure of SrMoO$_3$. Comparing our results with DFT+$U$ performed on the same footing, we find that DFT+$U$ overestimates the propensity for magnetic ordering, as well as the octahedral rotations, leading to a different ground state structure. This demonstrates that structural distortions can be highly sensitive to electronic correlation effects, and to the considered magnetic state, even in a moderately correlated metal such as SrMoO$_3$. Moreover, by comparing different downfolding schemes, we demonstrate the robustness of the DFT+DMFT method for obtaining structural properties, highlighting its versatility for applications to a broad range of materials.
The Hall effect in SrRuO$_3$ thin-films near the thickness limit for ferromagnetism shows an extra peak in addition to the ordinary and anomalous Hall effects. This extra peak has been attributed to a topological Hall effect due to two-dimensional skyrmions in the film around the coercive field; however, the sign of the anomalous Hall effect in SrRuO$_3$ can change as a function of saturation magnetization. Here we report Hall peaks in SrRuO$_3$ in which volumetric magnetometry measurements and magnetic force microscopy indicate that the peaks result from the superposition of two anomalous Hall channels with opposite sign. These channels likely form due to thickness variations in SrRuO$_3$, creating two spatially separated magnetic regions with different saturation magnetizations and coercive fields. The results are central to the development of strongly correlated materials for spintronics.
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