High-quality metal halide perovskite single crystals have low defect densities and excellent photophysical properties, yet thin films are the most sought after material geometry for optoelectronic devices. Perovskite single-crystal thin films (SCTFs) would be highly desirable for high-performance devices, but their growth remains challenging, particularly for inorganic metal halide perovskites. Herein, we report the facile vapor-phase epitaxial growth of cesium lead bromide perovskite (CsPbBr) continuous SCTFs with controllable micrometer thickness, as well as nanoplate arrays, on traditional oxide perovskite SrTiO(100) substrates. Heteroepitaxial single-crystal growth is enabled by the serendipitous incommensurate lattice match between these two perovskites, and overcoming the limitation of island-forming Volmer-Weber crystal growth is critical for growing large-area continuous thin films. Time-resolved photoluminescence, transient reflection spectroscopy, and electrical transport measurements show that the CsPbBr epitaxial thin film has a slow charge carrier recombination rate, low surface recombination velocity (10 cm s), and low defect density of 10 cm, which are comparable to those of CsPbBr single crystals. This work suggests a general approach using oxide perovskites as substrates for heteroepitaxial growth of halide perovskites. The high-quality halide perovskite SCTFs epitaxially integrated with multifunctional oxide perovskites could open up opportunities for a variety of high-performance optoelectronics devices.
Skyrmions hold promise for next-generation magnetic storage as their nanoscale dimensions may enable high information storage density and their low threshold for current-driven motion may enable ultra-low energy consumption. Skyrmion-hosting nanowires not only serve as a natural platform for magnetic racetrack memory devices but also stabilize skyrmions. Here we use the topological Hall effect (THE) to study phase stability and current-driven dynamics of skyrmions in MnSi nanowires. THE is observed in an extended magnetic field-temperature window (15–30 K), suggesting stabilization of skyrmions in nanowires compared with the bulk. Furthermore, we show in nanowires that under the high current density of 108–109 A m−2, the THE decreases with increasing current densities, which demonstrates the current-driven motion of skyrmions generating the emergent electric field in the extended skyrmion phase region. These results open up the exploration of skyrmions in nanowires for fundamental physics and magnetic storage technologies.
Magnetic skyrmions are topologically stable whirlpool-like spin textures that offer great promise as information carriers for future spintronic devices. To enable such applications, particular attention has been focused on the properties of skyrmions in highly confined geometries such as one-dimensional nanowires. Hitherto, it is still experimentally unclear what happens when the width of the nanowire is comparable to that of a single skyrmion. Here, we achieve this by measuring the magnetoresistance in ultra-narrow MnSi nanowires. We observe quantized jumps in magnetoresistance versus magnetic field curves. By tracking the size dependence of the jump number, we infer that skyrmions are assembled into cluster states with a tunable number of skyrmions, in agreement with the Monte Carlo simulations. Our results enable an electric reading of the number of skyrmions in the cluster states, thus laying a solid foundation to realize skyrmion-based memory devices.
The synthesis and characterization of a new layered compound with the composition (PbSe)1·16TiSe2 in thin-film form is reported in this study. The structure of the new compound was characterized by specular and in-plane synchrotron x-ray diffraction studies, which indicate that the compound can be described as a layered intergrowth of PbSe and TiSe2 in which the individual constituents are precisely layered yet rotationally (turbostratically) disordered with an average in-plane domain size in the order of 10 nm. In contrast to crystalline (PbSe)1·16(TiSe2)2 prepared by solid-state reaction at high temperature, the electrical resistivity in the range 20–300 K is nearly temperature independent. The Seebeck coefficient at room temperature was measured to be S = −66(1) μV/K at the carrier concentration of n = 2·1(5) × 1021 cm−3, indicating behavior characteristic of a heavily doped semiconductor. The electrical transport properties for the (PbSe)1·16TiSe2 compound are compared and contrasted to those of other misfi t-layered and turbostratically disordered (MX)1+δ(TX2)n compounds.
Using dynamic cantilever magnetometry we measure an enhanced skyrmion lattice phase extending from around 29 K down to at least 0.4 K in single MnSi nanowires (NWs). Although recent experiments on two-dimensional thin films show that reduced dimensionality stabilizes the skyrmion phase, our results are surprising given that the NW dimensions are much larger than the skyrmion lattice constant. Furthermore, the stability of the phase depends on the orientation of the NWs with respect to the applied magnetic field, suggesting that an effective magnetic anisotropy, likely due to the large surface-to-volume ratio of these nanostructures, is responsible for the stabilization. The compatibility of our technique with nanometer-scale samples paves the way for future studies on the effect of confinement and surfaces on magnetic skyrmions.
Cobalt phosphosulfide (CoPS) has recently emerged as a promising earth-abundant electrocatalyst for the hydrogen evolution reaction (HER). Nonetheless, the influence of crystallographic surface on the HER activity of CoPS and other nonmetallic electrocatalysts remains an important open question in the design of high-performance catalysts. Herein, the HER activities of the (100) and (111) facets of CoPS single crystals were studied using complementary experimental and computational approaches. Natural (111) and polished (100) facets of CoPS single crystals were selectively exposed to reveal that the HER behaviors on these two facets are quite different, with current density–potential curves crossing near 0.35 V vs RHE. Computational analysis can explain this phenomenon in terms of strongly differing H atom adsorption free energies and H–H recombination barriers on the facets, in conjunction with a simple kinetic model. At low potential (0–0.35 V), H adsorption (Volmer step) is rate limiting due to the endergonic adsorption on the (111) facet vs exergonic adsorption on the (100) facet, yielding a faster HER rate for the latter. However, at high potential (>0.35 V), H2 recombination/desorption becomes limiting and thus the (111) facet, with lower associated barriers, shows better HER activity. Explicit consideration of both steps and their interplay allows for a comprehensive description of the overpotential-dependence of the HER activity. This integrated study yields additional insight into the factors which govern the facet-dependence of catalytic activity on nonmetallic electrocatalysts and can further improve the design of advanced nanostructured HER catalysts.
Magnetic skyrmions are topologically stable vortex-like spin structures that are promising for next generation information storage applications. Materials that host magnetic skyrmions, such as MnSi and FeGe with the noncentrosymmetric cubic B20 crystal structure, have been shown to stabilize skyrmions upon nanostructuring. Here, we report a chemical vapor deposition method to selectively grow nanowires (NWs) of cubic FeGe out of three possible FeGe polymorphs for the first time using finely ground particles of cubic FeGe as seeds. X-ray diffraction and transmission electron microscopy (TEM) confirm that these micron-length NWs with ∼100 nm to 1 μm diameters have the cubic B20 crystal structure. Although FeGe NWs are also formed, the two types of NWs can be readily differentiated by their faceting. Lorentz TEM imaging of the cubic FeGe NWs reveals a skyrmion lattice phase under small applied magnetic fields (∼0.1 T) at 233 K, a skyrmion chain state at lower temperatures (95 K) and under high magnetic fields (∼0.4 T), and a larger skyrmion stability window than bulk FeGe. This synthetic approach to cubic FeGe NWs that support stabilized skyrmions opens a route toward the exploration of new skyrmion physics and devices based on similar nanostructures.
Silicon is an extremely important technological material, but its current industrial production by the carbothermic reduction of SiO2 is energy intensive and generates CO2 emissions. Herein, we developed a more sustainable method to produce silicon nanowires (Si NWs) in bulk quantities through the direct electrochemical reduction of CaSiO3, an abundant and inexpensive Si source soluble in molten salts, at a low temperature of 650 °C by using low‐melting‐point ternary molten salts CaCl2–MgCl2–NaCl, which still retains high CaSiO3 solubility, and a supporting electrolyte of CaO, which facilitates the transport of O2− anions, drastically improves the reaction kinetics, and enables the electrolysis at low temperatures. The Si nanowire product can be used as high‐capacity Li‐ion battery anode materials with excellent cycling performance. This environmentally friendly strategy for the practical production of Si at lower temperatures can be applied to other molten salt systems and is also promising for waste glass and coal ash recycling.
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