In situ observation of the percolation threshold in multiphase magma analogues.

Magmas vesiculate during ascent, producing complex interconnected pore networks, which can act as outgassing pathways and then deflate or compact to volcanic plugs. Similarly, in-conduit fragmentation events during dome-forming eruptions create open systems transiently, before welding causes pore sealing. The percolation threshold is the first-order transition between closed- and open-system degassing dynamics. Here, we use time-resolved, synchrotron-source X-ray tomography to image synthetic magmas that go through cycles of opening and closing, to constrain the percolation threshold Φ C at a range of melt crystallinity, viscosity and overpressure pertinent to shallow magma ascent. During vesiculation, we observed different percolative regimes for the same initial bulk crystallinity depending on melt viscosity and gas overpressure. At high viscosity (> 106 Pa s) and high overpressure (~ 1-4 MPa), we found that a brittle-viscous regime dominates in which brittle rupture allows system-spanning coalescence at a low percolation threshold (Φ C ~0.17) via the formation of fracture-like bubble chains. Percolation was followed by outgassing and bubble collapse causing densification and isolation of the bubble network, resulting in a hysteresis in the evolution of connectivity with porosity. At low melt viscosity and overpressure, we observed a viscous regime with much higher percolation threshold (Φ C > 0.37) due to spherical bubble growth and lower degree of crystal connection. Finally, our results also show that sintering of crystal-free and crystal-bearing magma analogues is characterised by low percolation thresholds (Φ C = 0.04 - 0.10). We conclude that the presence of crystals lowers the percolation threshold during vesiculation and may promote outgassing in shallow, crystal-rich magma at initial stages of Vulcanian and Strombolian eruptions.

Author Correction: Laser-wakefield accelerators for high-resolution X-ray imaging of complex microstructures.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

Laser-wakefield accelerators for high-resolution X-ray imaging of complex microstructures.

Laser-wakefield accelerators (LWFAs) are high acceleration-gradient plasma-based particle accelerators capable of producing ultra-relativistic electron beams. Within the strong focusing fields of the wakefield, accelerated electrons undergo betatron oscillations, emitting a bright pulse of X-rays with a micrometer-scale source size that may be used for imaging applications. Non-destructive X-ray phase contrast imaging and tomography of heterogeneous materials can provide insight into their processing, structure, and performance. To demonstrate the imaging capability of X-rays from an LWFA we have examined an irregular eutectic in the aluminum-silicon (Al-Si) system. The lamellar spacing of the Al-Si eutectic microstructure is on the order of a few micrometers, thus requiring high spatial resolution. We present comparisons between the sharpness and spatial resolution in phase contrast images of this eutectic alloy obtained via X-ray phase contrast imaging at the Swiss Light Source (SLS) synchrotron and X-ray projection microscopy via an LWFA source. An upper bound on the resolving power of 2.7 ± 0.3 µm of the LWFA source in this experiment was measured. These results indicate that betatron X-rays from laser wakefield acceleration can provide an alternative to conventional synchrotron sources for high resolution imaging of eutectics and, more broadly, complex microstructures.

Observation of polar vortices in oxide superlattices.

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.

Spatial control of functional properties via octahedral modulations in complex oxide superlattices.

Control of atomic structure, namely the topology of the corner-connected metal-oxygen octahedra, has emerged as an important route to tune the functional properties at oxide interfaces. Here we investigate isovalent manganite superlattices (SLs), [(La(0.7)Sr(0.3)MnO(3))n/(Eu(0.7)Sr(0.3)MnO(3))n] × m, as a route to spatial control over electronic bandwidth and ferromagnetism through the creation of octahedral superstructures. Electron energy loss spectroscopy confirms a uniform Mn valence state throughout the SLs. In contrast, the presence of modulations of the MnO(6) octahedral rotations along the growth direction commensurate with the SL period is revealed by scanning transmission electron microscopy and X-ray diffraction. We show that the Curie temperatures of the constituent materials can be systematically engineered via the octahedral superstructures leading to a modulated magnetization in samples where the SL period is larger than the interfacial octahedral coupling length scale, whereas a single magnetic transition is observed in the short-period SLs.

Effect of interfacial octahedral behavior in ultrathin manganite films.

We investigate structural coupling of the MnO6 octahedra across a film/substrate interface and the resultant changes of the physical properties of ultrathin La2/3Sr1/3MnO3 (LSMO) films. In order to isolate the effect of interfacial MnO6 octahedral behavior from that of epitaxial strain, LSMO films are grown on substrates with different symmetry and similar lattice parameters. Ultrathin LSMO films show an increased magnetization and electrical conductivity on cubic (LaAlO3)0.3(Sr2AlTaO6)0.7 (LSAT) compared to those grown on orthorhombic NdGaO3 (NGO) substrates, an effect that subsides as the thickness of the films is increased. This study demonstrates that interfacial structural coupling can play a critical role in the functional properties of oxide heterostructures.

Evolution of the interfacial structure of LaAlO3 on SrTiO3.

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. Based on these structures, the threshold for formation of a two-dimensional electron system at a film thickness of 4 monolayers is quantitatively explained. The findings are also qualitatively reproduced by density-functional-theory calculations.

Synchrotron radiation hardness studies of PILATUS II.

A synchrotron beam has been used to investigate the radiation tolerance of a PILATUS II module. It has been demonstrated that radiation-induced threshold shifts become significant above 30 Mrad. Individual adjustment of pixel thresholds after irradiation enabled retention of standard behaviour in excess of 40 Mrad. This implies that a module can be continuously irradiated for in excess of 40 days at an individual pixel count rate of 10(6) counts s(-1).

Performance of single-photon-counting PILATUS detector modules.

PILATUS is a silicon hybrid pixel detector system, operating in single-photon-counting 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.

Graphene on Ru(0001): a 25 x 25 supercell.

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.

Structural basis for the conducting interface between LaAlO3 and SrTiO3.

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.

Surface of strontium titanate.

We report the first complete determination, using surface x-ray diffraction, of the surface structure of TiO2-terminated SrTiO3(001), both at room temperature in vacuum, and also hot, under typical conditions used for thin film growth. The cold structure consists of a mixture of a (1x1) relaxation and (2x1) and (2x2) reconstructions. The latter disappear over several minutes upon heating. The structures are best modeled by a TiO2-rich surface similar to that proposed by Erdman et al. [Nature (London) 419, 55 (2002).10.1038/nature01010]. Both reconstructions have been shown by density functional theory to be energetically favorable. The calculated (1x1) surface energy is higher, indicating that it may be a disordered mixture of the reconstructions. Atomic displacements are significant down to three unit cells, which may have important implications on possible surface ferroelectric phenomena in SrTiO3.

Energetic surface smoothing of complex metal-oxide thin films.

A novel energetic smoothing mechanism in the growth of complex metal-oxide thin films is reported from in situ kinetic studies of pulsed laser deposition of on , using x-ray reflectivity. Below 50% monolayer coverage, prompt insertion of energetic impinging species into small-diameter islands causes them to break up to form daughter islands. This smoothing mechanism therefore inhibits the formation of large-diameter 2D islands and the seeding of 3D growth. Above 50% coverage, islands begin to coalesce and their breakup is thereby suppressed. The energy of the incident flux is instead rechanneled into enhanced surface diffusion, which leads to an increase in the effective surface temperature of DeltaT approximately 500 K. These results have important implications on optimal conditions for nanoscale device fabrication using these materials.

Improved data acquisition in grazing-incidence X-ray scattering experiments using a pixel detector.

The use of an area detector in grazing-incidence X-ray experiments lends many advantages in terms of both speed and reliability. Here a discussion is given of the procedures established using the PILATUS pixel detector developed at the Swiss Light Source for optimizing data acquisition and analysis of surface diffraction data at the Materials Science beamline, especially with regard to reflectivity measurements, crystal truncation and fractional order rods, and grazing-incidence diffraction experiments.