The complex interplay of spin, charge, orbital and lattice degrees of freedom provides a plethora of exotic phases and physical phenomena. In recent years, complex spin topologies have emerged as a consequence of the electronic band structure and the interplay between spin and spin-orbit coupling in materials. Here we produce complex topologies of electrical polarization--namely, nanometre-scale vortex-antivortex (that is, clockwise-anticlockwise) arrays that are reminiscent of rotational spin topologies--by making use of the competition between charge, orbital and lattice degrees of freedom in superlattices of alternating lead titanate and strontium titanate layers. Atomic-scale mapping of the polar atomic displacements by scanning transmission electron microscopy reveals the presence of long-range ordered vortex-antivortex arrays that exhibit nearly continuous polarization rotation. Phase-field modelling confirms that the vortex array is the low-energy state for a range of superlattice periods. Within this range, the large gradient energy from the vortex structure is counterbalanced by the corresponding large reduction in overall electrostatic energy (which would otherwise arise from polar discontinuities at the lead titanate/strontium titanate interfaces) and the elastic energy associated with epitaxial constraints and domain formation. These observations have implications for the creation of new states of matter (such as dipolar skyrmions, hedgehog states) and associated phenomena in ferroic materials, such as electrically controllable chirality.
The complete atomic structure of a five-monolayer film of LaAlO3 on SrTiO3 has been determined for the first time by surface x-ray diffraction in conjunction with the coherent Bragg rod analysis phase-retrieval method and further structural refinement. Cationic mixing at the interface results in dilatory distortions and the formation of metallic La(1-x)SrxTiO3. By invoking electrostatic potential minimization, the ratio of Ti{4+}/Ti{3+} across the interface was determined, from which the lattice dilation could be quantitatively explained using ionic radii considerations. The correctness of this model is supported by density functional theory calculations. Thus, the formation of a quasi-two-dimensional electron gas in this system is explained, based on structural considerations.
PILATUS is a silicon hybrid pixel detector system, operating in single-photoncounting mode, that has been developed at the Paul Scherrer Institut for the needs of macromolecular crystallography at the Swiss Light Source (SLS). A calibrated PILATUS module has been characterized with monochromatic synchrotron radiation. The influence of charge sharing on the count rate and the overall energy resolution of the detector were investigated. The dead-time of the system was determined using the attenuated direct synchrotron beam. A single module detector was also tested in surface diffraction experiments at the SLS, whereby its performance regarding fluorescence suppression and saturation tolerance were evaluated, and have shown to greatly improve the sensitivity, reliability and speed of surface diffraction data acquisition.
The structure of a single layer of graphene on Ru(0001) has been studied using surface x-ray diffraction. A surprising superstructure containing 1250 carbon atoms has been determined, whereby 25 x 25 graphene unit cells lie on 23 x 23 unit cells of Ru. Each supercell contains 2 x 2 crystallographically inequivalent subcells caused by corrugation. Strong intensity oscillations in the superstructure rods demonstrate that the Ru substrate is also significantly corrugated down to several monolayers and that the bonding between graphene and Ru is strong and cannot be caused by van der Waals bonds. Charge transfer from the Ru substrate to the graphene expands and weakens the C-C bonds, which helps accommodate the in-plane tensile stress. The elucidation of this superstructure provides important information in the potential application of graphene as a template for nanocluster arrays.
The evolution of the atomic structure of LaAlO 3 grown on SrTiO 3 was investigated using surface x-ray diffraction in conjunction with model-independent, phase-retrieval algorithms between two and five monolayers film thickness. A depolarizing buckling is observed between cation and oxygen positions in response to the electric field of polar LaAlO 3 , which decreases with increasing film thickness. We explain this in terms of competition between elastic strain energy, electrostatic energy, and electronic reconstructions. The findings are qualitatively reproduced by density-functionaltheory calculations. Significant cationic intermixing across the interface extends approximately three monolayers for all film thicknesses. The interfaces of films thinner than four monolayers therefore extend to the surface, which might affect conductivity.
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