Search Results
Dressed j eff-1/2 objects in mixed-valence lacunar spinel molybdates
The lacunar-spinel chalcogenides exhibit magnetic centers in the form of transition-metal tetrahedra. On the basis of density-functional computations, the electronic ground state of an Mo413+ tetrahedron has been postulated as single-configuration a12 e4 t25, where a1, e, and t2 are symmetry-adapted linear combinations of single-site Mo t2g atomic orbitals. Here we unveil the many-body tetramer wave-function: we show that sizable correlations yield a weight of only 62% for the a12 e4 t25 configuration. While spin–orbit coupling within the peculiar valence orbital manifold is still effective, the expectation value of the spin–orbit operator and the g factors deviate from figures describing nominal t5jeff = 1/2 moments. As such, our data documents the dressing of a spin–orbit jeff = 1/2 object with intra-tetramer excitations. Our results on the internal degrees of freedom of these magnetic moments provide a solid theoretical starting point in addressing the intriguing phase transitions observed at low temperatures in these materials.
Localized crystallization in shear bands of a metallic glass
Stress-induced viscous flow is the characteristic of atomic movements during plastic deformation of metallic glasses in the absence of substantial temperature increase, which suggests that stress state plays an important role in mechanically induced crystallization in a metallic glass. However, it is poorly understood. Here, we report on the stress-induced localized crystallization in individual shear bands of Zr60Al15Ni25 metallic glass subjected to cold rolling. We find that crystallization in individual shear bands preferentially occurs in the regions neighboring the amorphous matrix, where the materials are subjected to compressive stresses demonstrated by our finite element simulations. Our results provide direct evidence that the mechanically induced crystallization kinetics is closely related with the stress state. The crystallization kinetics under compressive and tensile stresses are interpreted within the frameworks of potential energy landscape and classical nucleation theory, which reduces the role of stress state in mechanically induced crystallization in a metallic glass.
Imaging Shock Waves in Diamond with Both High Temporal and Spatial Resolution at an XFEL
The advent of hard x-ray free-electron lasers (XFELs) has opened up a variety of scientific opportunities in areas as diverse as atomic physics, plasma physics, nonlinear optics in the x-ray range and protein crystallography. In this article, we access a new field of science by measuring quantitatively the local bulk properties and dynamics of matter under extreme conditions, in this case by using the short XFEL pulse to image an elastic compression wave in diamond. The elastic wave was initiated by an intense optical laser pulse and was imaged at different delay times after the optical pump pulse using magnified x-ray phase-contrast imaging. The temporal evolution of the shock wave can be monitored, yielding detailed information on shock dynamics, such as the shock velocity, the shock front width and the local compression of the material. The method provides a quantitative perspective on the state of matter in extreme conditions.
Ultrasmall SnO₂ nanocrystals: hot-bubbling synthesis, encapsulation in carbon layers and applications in high capacity Li-ion storage
Ultrasmall SnO2 nanocrystals as anode materials for lithium-ion batteries (LIBs) have been synthesized by bubbling an oxidizing gas into hot surfactant solutions containing Sn-oleate complexes. Annealing of the particles in N2 carbonifies the densely packed surface capping ligands resulting in carbon encapsulated SnO2 nanoparticles (SnO2/C). Carbon encapsulation can effectively buffer the volume changes during the lithiation/delithiation process. The assembled SnO2/C thus deliver extraordinarily high reversible capacity of 908 mA·h·g−1 at 0.5 C as well as excellent cycling performance in the LIBs. This method demonstrates the great potential of SnO2/C nanoparticles for the design of high power LIBs.
On Curie temperature of B20-MnSi films
B20-type MnSi is the prototype magnetic skyrmion material. Thin films of MnSi show a higher Curie temperature than their bulk counterpart. However, it is not yet clear what mechanism leads to the increase of the Curie temperature. In this work, we grow MnSi films on Si(100) and Si(111) substrates with a broad variation in their structures. By controlling the Mn thickness and annealing parameters, the pure MnSi phase of polycrystalline and textured nature as well as the mixed phase of MnSi and MnSi1.7 are obtained. Surprisingly, all these MnSi films show an increased Curie temperature of up to around 43 K. The Curie temperature is likely independent of the structural parameters within our accessibility including the film thickness above a threshold, strain, cell volume and the mixture with MnSi1.7. However, a pronounced phonon softening is observed for all samples, which can tentatively be attributed to slight Mn excess from stoichiometry, leading to the increased Curie temperature.
Author Correction: Surface acoustic wave nebulization improves compound selectivity of low-temperature plasma ionization for mass spectrometry
Correction to: Scientific Reports https://doi.org/10.1038/s41598-021-82423-w, published online 03 February 2021
Transition from a uni- to a bimodal interfacial charge distribution in LaAlO 3 / SrTiO 3 upon cooling
We present a combined resonant soft X-ray reflectivity and electric transport study of LaAlO 3/SrTiO 3 field effect devices. The depth profiles with atomic layer resolution that are obtained from the resonant reflectivity reveal a pronounced temperature dependence of the two-dimensional electron liquid at the LaAlO 3/SrTiO 3 interface. At room temperature the corresponding electrons are located close to the interface, extending down to 4 unit cells into the SrTiO 3 substrate. Upon cooling, however, these interface electrons assume a bimodal depth distribution: They spread out deeper into the SrTiO 3 and split into two distinct parts, namely one close to the interface with a thickness of about 4 unit cells and another centered around 9 unit cells from the interface. The results are consistent with theoretical predictions based on oxygen vacancies at the surface of the LaAlO 3 film and support the notion of a complex interplay between structural and electronic degrees of freedom. © 2020, The Author(s).
Surface acoustic wave nebulization improves compound selectivity of low-temperature plasma ionization for mass spectrometry
Mass spectrometry coupled to low-temperature plasma ionization (LTPI) allows for immediate and easy analysis of compounds from the surface of a sample at ambient conditions. The efficiency of this process, however, strongly depends on the successful desorption of the analyte from the surface to the gas phase. Whilst conventional sample heating can improve analyte desorption, heating is not desirable with respect to the stability of thermally labile analytes. In this study using aromatic amines as model compounds, we demonstrate that (1) surface acoustic wave nebulization (SAWN) can significantly improve compound desorption for LTPI without heating the sample. Furthermore, (2) SAWN-assisted LTPI shows a response enhancement up to a factor of 8 for polar compounds such as aminophenols and phenylenediamines suggesting a paradigm shift in the ionization mechanism. Additional assets of the new technique demonstrated here are (3) a reduced analyte selectivity (the interquartile range of the response decreased by a factor of 7)—a significant benefit in non-targeted analysis of complex samples—and (4) the possibility for automated online monitoring using an autosampler. Finally, (5) the small size of the microfluidic SAWN-chip enables the implementation of the method into miniaturized, mobile LTPI probes.
Nano-imaging confirms improved apatite precipitation for high phosphate/silicate ratio bioactive glasses
Bioactive glasses convert to a biomimetic apatite when in contact with physiological solutions; however, the number and type of phases precipitating depends on glass composition and reactivity. This process is typically followed by X-ray diffraction and infrared spectroscopy. Here, we visualise surface mineralisation in a series of sodium-free bioactive glasses, using transmission electron microscopy (TEM) with energy-dispersive X-ray spectroscopy (EDXS) and X-ray nano-computed tomography (nano-CT). In the glasses, the phosphate content was increased while adding stoichiometric amounts of calcium to maintain phosphate in an orthophosphate environment in the glass. Calcium fluoride was added to keep the melting temperature low. TEM brought to light the presence of phosphate clustering and nearly crystalline calcium fluoride environments in the glasses. A combination of analytical methods, including solid-state NMR, shows how with increasing phosphate content in the glass, precipitation of calcium fluoride during immersion is superseded by fluorapatite precipitation. Nano-CT gives insight into bioactive glass particle morphology after immersion, while TEM illustrates how compositional changes in the glass affect microstructure at a sub-micron to nanometre-level.
Critical current modulation induced by an electric field in superconducting tungsten-carbon nanowires
The critical current of a superconducting nanostructure can be suppressed by applying an electric field in its vicinity. This phenomenon is investigated throughout the fabrication and electrical characterization of superconducting tungsten-carbon (W-C) nanostructures grown by Ga+ focused ion beam induced deposition (FIBID). In a 45 nm-wide, 2.7 μm-long W-C nanowire, an increasing side-gate voltage is found to progressively reduce the critical current of the device, down to a full suppression of the superconducting state below its critical temperature. This modulation is accounted for by the squeezing of the superconducting current by the electric field within a theoretical model based on the Ginzburg–Landau theory, in agreement with experimental data. Compared to electron beam lithography or sputtering, the single-step FIBID approach provides with enhanced patterning flexibility and yields nanodevices with figures of merit comparable to those retrieved in other superconducting materials, including Ti, Nb, and Al. Exhibiting a higher critical temperature than most of other superconductors, in which this phenomenon has been observed, as well as a reduced critical value of the gate voltage required to fully suppress superconductivity, W-C deposits are strong candidates for the fabrication of nanodevices based on the electric field-induced superconductivity modulation.