The atomic structure of ultrathin oxide films and interfaces studied by surface X-ray diffraction

X-ray diffraction (XRD) studies of the atomic structure of ultrathin oxide films and interfaces are presented, which are conducted within the framework of the Sonderforschungsbereich 762 (functionality of oxide interfaces). Knowledge of the atomic structure is at the heart of the study of functional oxides. XRD allows the investigation of complex systems frequently encountered in oxide systems (large unit cells, complex relaxation patterns, and structural and chemical disorder). Results are combined with first-principles calculations and complementary techniques providing a thorough understanding of the oxides' functionality. The structure analysis of the approximant (AP) to the 2D oxidic quasicrystal (QC) based on BaTiO3 (BTO) is discussed, the first oxide-type QC discovered. This AP is related to the Kepler tiling described 400 years ago. The LaFeO3/SrTiO3 interface is examined, which is a prototype for the formation of a 2D electron gas (2DEG). Subtle interfacial chemical roughness in combination with oxygen off-stoichiometry strongly influences the critical LaFeO3 thickness for the 2DEG formation. Finally, the analysis of the multiferroic BTO/ME(001) (ME = Fe, Pd, Pt) interface reveals that a submonolayer of impurities is the origin for the inversion of the BTO film/vacuum termination from BaO on Fe(001) to TiO2 on Pt(001)

X-ray structure analysis of the InSb ( )-(3 × 3) reconstruction

The (3 × 3) reconstruction of the InSb( ) surface has been analysed using grazing incidence X-ray diffraction. The reconstruction is characterized by hexamers above a complete InSb double-layer centred around an Sb atom. No vacancies are found in the structure as predicted theoretically. The results agree with scanning tunnelling microscopy measurements

Jahn-Teller stabilization of a "polar" metal oxide surface: Fe3O4(001)

Using ab initio thermodynamics we compile a phase diagram for the surface of Fe3O4(001) as a function of temperature and oxygen pressures. A hitherto ignored polar termination with octahedral iron and oxygen forming a wave-like structure along the [110]-direction is identified as the lowest energy configuration over a broad range of oxygen gas-phase conditions. This novel geometry is confirmed in a x-ray diffraction analysis. The stabilization of the Fe3O4(001)-surface goes together with dramatic changes in the electronic and magnetic properties, e.g., a halfmetal-to-metal transition.Comment: 4 pages, 4 figure

Giant spin Hall effect and spin-orbit torques in 5d transition metal-aluminum alloys from extrinsic scattering

The generation of spin currents from charge currents via the spin Hall effect (SHE) is of fundamental and technological interest. Here, some of the largest SHEs yet observed via extrinsic scattering are found in a large class of binary compounds formed from a 5d element and aluminum, with a giant spin Hall angle (SHA) of ≈1 in the compound Os22Al78. A critical composition of the 5d element is found at which there is a structural phase boundary between poorly and highly textured crystalline material, where the SHA exhibits its largest value. Furthermore, a systematic increase is found in the spin Hall conductivity (SHC) and SHA at this critical composition as the atomic number of the 5d element is systematically increased. This clearly shows that the SHE and SHC are derived from extrinsic scattering mechanisms related to the potential mismatch between the 5d element and Al. These studies show the importance of extrinsic mechanisms derived from potential mismatch as a route to obtaining large spin Hall angles with high technological impact. Indeed, it is demonstrated that a state-of-the-art racetrack device has a several-fold increased current-induced domain wall efficiency using these materials as compared to prior-art materials

2D honeycomb transformation into dodecagonal quasicrystals driven by electrostatic forces

Dodecagonal oxide quasicrystals are well established as examples of long-range aperiodic order in two dimensions. However, despite investigations by scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), low-energy electron microscopy (LEEM), photoemission spectroscopy as well as density functional theory (DFT), their structure is still controversial. Furthermore, the principles that guide the formation of quasicrystals (QCs) in oxides are elusive since the principles that are known to drive metallic QCs are expected to fail for oxides. Here we demonstrate the solution of the oxide QC structure by synchrotron-radiation based surface x-ray diffraction (SXRD) refinement of its largest-known approximant. The oxide QC formation is forced by large alkaline earth metal atoms and the reduction of their mutual electrostatic repulsion. It drives the n = 6 structure of the 2D Ti2O3 honeycomb arrangement via Stone–Wales transformations into an ordered structure with empty n = 4, singly occupied n = 7 and doubly occupied n = 10 rings, as supported by DFT

Crystal-field mediated electronic transitions of EuS up to 35 GPa

An advanced experimental and theoretical model to explain the correlation between the electronic and local structure of Eu2+ in two different environments within a same compound, EuS, is presented. EuX monochalcogenides (X: O, S, Se, Te) exhibit anomalies in all their properties around 14 GPa with a semiconductor to metal transition. Although it is known that these changes are related to the 4f75d0 → 4f65d1 electronic transition, no consistent model of the pressure-induced modifications of the electronic structure currently exists. We show, by optical and x-ray absorption spectroscopy, and by ab initio calculations up to 35 GPa, that the pressure evolution of the crystal field plays a major role in triggering the observed electronic transitions from semiconductor to the half-metal and finally to the metallic state

Long-range supercurrents through a chiral non-collinear antiferromagnet in lateral Josephson junctions

The proximity-coupling of a chiral non-collinear antiferromagnet (AFM)1,2,3,4,5 with a singlet superconductor allows spin-unpolarized singlet Cooper pairs to be converted into spin-polarized triplet pairs6,7,8, thereby enabling non-dissipative, long-range spin correlations9,10,11,12,13,14. The mechanism of this conversion derives from fictitious magnetic fields that are created by a non-zero Berry phase15 in AFMs with non-collinear atomic-scale spin arrangements1,2,3,4,5. Here we report long-ranged lateral Josephson supercurrents through an epitaxial thin film of the triangular chiral AFM Mn3Ge (refs. 3,4,5). The Josephson supercurrents in this chiral AFM decay by approximately one to two orders of magnitude slower than would be expected for singlet pair correlations9,10,11,12,13,14 and their response to an external magnetic field reflects a clear spatial quantum interference. Given the long-range supercurrents present in both single- and mixed-phase Mn3Ge, but absent in a collinear AFM IrMn16, our results pave a way for the topological generation of spin-polarized triplet pairs6,7,8 via Berry phase engineering15 of the chiral AFMs

Structure and magnetism of EuS on Bi₂Se₃(0001)

The rocksalt-type ferromagnetic (FM) insulator EuS (bulk TC = 17 K) grown on Bi2Se3 with well-matched (111) plane of the film and (0001) plane of the substrate is studied. The system may feature magnetic proximity effect breaking the time-reversal symmetry and opening a bandgap in the metallic topologically protected surface state of Bi2Se3. The experimental X-ray diffraction studies are combined with ab initio calculations to resolve contradictory results concerning the enhancement of the TC up to 300 K and the degree of induced magnetization in the system. It is concluded that previous studies relied on idealized and unconfirmed structure models. Herein, it is shown by surface X-ray diffraction (SXRD) with ab initio calculations that a two double layer-thick EuS film grows with a sharp interface and without chemical intermixing in a single domain state in an FCC-type stacking on the Bi2Se3(0001) surface in which the topmost layer is metallic, thereby lifting polarity. A large pz-orbital-derived top-layer sulfur magnetic moment of 0.6 μB is found, whereas for europium, μEu = 6.9 μB throughout the film is found. No magnetization within the first Bi2Se3 quintuple layer is found. The calculation of the exchange parameters Jij indicates a complex FM and antiferromagnetic ordering between europium and sulfur with a maximum Néel temperature of 226 K