Controlled in-plane rotation of the magnetic easy axis in manganite heterostructures by tailoring the interface oxygen network could allow the development of correlated oxide-based magnetic tunnelling junctions with non-collinear magnetization, with possible practical applications as miniaturized high-switching-speed magnetic random access memory (MRAM) devices. Here, we demonstrate how to manipulate magnetic and electronic anisotropic properties in manganite heterostructures by engineering the oxygen network on the unit-cell level. The strong oxygen octahedral coupling is found to transfer the octahedral rotation, present in the NdGaO3 (NGO) substrate, to the La2/3Sr1/3MnO3 (LSMO) film in the interface region. This causes an unexpected realignment of the magnetic easy axis along the short axis of the LSMO unit cell as well as the presence of a giant anisotropic transport in these ultrathin LSMO films. As a result we possess control of the lateral magnetic and electronic anisotropies by atomic-scale design of the oxygen octahedral rotation.

Document VersionEarly version, also known as pre-print Link back to DTU Orbit Citation (APA):Chen, Y., Trier, F., Wijnands, T., Green, R. J., Gauquelin, N., Egoavil, R., ... Pryds, N. (2015). Extreme mobility enhancement of two-dimensional electron gases at oxide interfaces via charge transfer induced modulation doping. Nature Materials, 14(8) Supplementary Information, Fig. S1). For all samples, with the d-LAO film thickness up to 20 nm, atomic force microscopy (AFM) images show regular surface terraces with a step height of 0.4 nm (Fig. 1b), similar to that of the original STO substrate and indicating uniform film growth. Representative samples were investigated further by scanning transmission electron microscopy (STEM). Our subsequent spectroscopic measurements reveal dramatic electronic reconstruction in the LSMO-buffered samples. Firstly, different from the unbuffered d-LAO/STO sample where the 2DEG is coupled strongly to a large content of oxygen vacancies extending more than 3 nm deep into STO 24 , all buffered samples show a rather low content of Ti 3+ far below the detection limit of our in situ X-ray photoelectron

We present a theory describing the local electronic properties of the perovskite rare-earth nickelates-materials which have negative charge transfer energies, strong O 2p - Ni 3d covalence, and breathing-mode lattice distortions at the origin of highly studied metal-insulator and antiferromagnetic ordering transitions. Utilizing a full-orbital, full-correlation double-cluster approach, we find strong charge fluctuations, in agreement with a bond disproportionation interpretation. The double-cluster formulation permits the inclusion of necessary orbital degeneracies and Coulomb interactions to calculate resonant x-ray spectral responses, with which we find excellent agreement with well-established experimental results. This previously absent, crucial link between theory and experiment provides validation of the recently proposed bond disproportionation theory, and provides an analysis methodology for spectroscopic studies of engineered phases of nickelates and other high-valence transition-metal compounds