Giant Tunability of Rashba Splitting at Cation-Exchanged Polar Oxide Interfaces by Selective Orbital Hybridization.

The 2D electron gas (2DEG) at oxide interfaces exhibits extraordinary properties, such as 2D superconductivity and ferromagnetism, coupled to strongly correlated electrons in narrow d-bands. In particular, 2DEGs in KTaO3 (KTO) with 5d t2g orbitals exhibit larger atomic spin-orbit coupling and crystal-facet-dependent superconductivity absent for 3d 2DEGs in SrTiO3 (STO). Herein, by tracing the interfacial chemistry, weak anti-localization magneto-transport behavior, and electronic structures of (001), (110), and (111) KTO 2DEGs, unambiguously cation exchange across KTO interfaces is discovered. Therefore, the origin of the 2DEGs at KTO-based interfaces is dramatically different from the electronic reconstruction observed at STO interfaces. More importantly, as the interface polarization grows with the higher order planes in the KTO case, the Rashba spin splitting becomes maximal for the superconducting (111) interfaces approximately twice that of the (001) interface. The larger Rashba spin splitting couples strongly to the asymmetric chiral texture of the orbital angular moment, and results mainly from the enhanced inter-orbital hopping of the t2g bands and more localized wave functions. This finding has profound implications for the search for topological superconductors, as well as the realization of efficient spin-charge interconversion for low-power spin-orbitronics based on (110) and (111) KTO interfaces.

Long-Range Magnetic Order in Oxide Quantum Wells Hosting Two-Dimensional Electron Gases.

To incorporate spintronics functionalities into two-dimensional devices, it is strongly desired to get two-dimensional electron gases (2DEGs) with high spin polarization. Unfortunately, the magnetic characteristics of the typical 2DEG at the LaAlO3/SrTiO3 interface are very weak due to the nonmagnetic character of SrTiO3 and LaAlO3. While most of the previous works focused on perovskite oxides, here, we extended the exploration for magnetic 2DEG beyond the scope of perovskite combinations, composing 2DEG with SrTiO3 and NaCl-structured EuO that owns a large saturation magnetization and a fairly high Curie temperature. We obtained the 2DEGs that show long-range magnetic order and thus unusual behaviors marked by isotropic butterfly shaped magnetoresistance and remarkable anomalous Hall effect. We found evidence for the presence of more conductive domain walls than elsewhere in the oxide layer where the 2DEG resides. More than that, a relation between interfacial magnetism and carrier density is established. On this basis, the intermediate magnetic states between short-range and long-range ordered states can be achieved. The present work provides guidance for the design of high-performance magnetic 2DEGs.

Unusual Electric and Optical Tuning of KTaO3-Based Two-Dimensional Electron Gases with 5d Orbitals.

Controlling electronic processes in low-dimension electron systems is centrally important for both fundamental and applied researches. While most of the previous works focused on SrTiO3-based two-dimensional electron gases (2DEGs), here we report on a comprehensive investigation in this regard for amorphous-LaAlO3/KTaO3 2DEGs with the Fermi energy ranging from ∼13 meV to ∼488 meV. The most important observation is the dramatic variation of the Rashba spin-orbit coupling (SOC) as Fermi energy sweeps through 313 meV: The SOC effective field first jumps and then drops, leading to a cusp of ∼2.6 T. Above 313 meV, an additional species of mobile electrons emerges, with a 50-fold enhanced Hall mobility. A relationship between spin relaxation distance and the degree of band filling has been established in a wide range. It indicates that the maximal spin precession length is ∼70.1 nm and the maximal Rashba spin splitting energy is ∼30 meV. Both values are much larger than the previously reported ones. As evidenced by density functional theory calculation, these unusual phenomena are closely related to the distinct band structure of the 2DEGs composed of 5d electrons. The present work further deepens our understanding of perovskite conducting interfaces, particularly those composed of 5d transition-metal oxides.

Magnetic Anisotropy Controlled by Distinct Interfacial Lattice Distortions at the La1- xSr xCoO3/La2/3Sr1/3MnO3 Interfaces.

Interface engineering is an important approach leading to multifunctional artificial materials. Although most of the previous works focused on the effects of the rotation/tilting of interfacial oxygen octahedron on perovskite multilayers, here, we report on a new kind of lattice distortion characterized by an off-center shift of the Mn ions within the MnO6 oxygen octahedra at the interfaces of La1- xSr xCoO3/La2/3Sr1/3MnO3/La1- xSr xCoO3/LaAlO3 trilayers ( x = 0-1/3), which drives the initially perpendicularly aligned magnetic axis of the La2/3Sr1/3MnO3 (LSMO) film toward the in-plane direction, though the film is in a strongly compressive state. It is further found that the magnetic anisotropy considerably depends on the content of Sr in La1- xSr xCoO3, enhancing as x decreases. The maximal anisotropy constant at 10 K is +2.5 × 106 erg/cm3 for the trilayers with x = 0, whereas it is -1.5 × 105 erg/cm3 for a bare LSMO film on LaAlO3. On the basis of the analysis of X-ray absorption spectroscopy and the results of density functional theory calculations, we found that the off-center displacement of the Mn ions has caused a strong orbital reconstruction at interfaces, resulting in the anomalous spin orientation against magnetoelastic coupling.