Direct growth of crystalline SiGe nanowires on superconducting NbTiN thin films.

Novel heterostructures created by coupling one-dimensional semiconductor nanowires with a superconducting thin film show great potential toward next-generation quantum computing. Here, by growing high-crystalline SiGe nanowires on a NbTiN thin film, the resulting heterostructure exhibits Ohmic characteristics as well as a shift of the superconducting transition temperature (Tc). The structure was characterized at atomic resolution showing a sharp SiGe/NbTiN interface without atomic interdiffusion. Lattice spacing, as calculated from large-area x-ray diffraction experiments, suggests a potential preferredd-spacing matching between (200) NbTiN and (110) SiGe grains. The observed out-of-plane compressive strain within the NbTiN films coupled with SiGe nanowires explains the downward shift of the superconductivity behavior. The presented results post scientific insights toward functional heterostructures by coupling multi-dimensional materials, which could enable tunable superconductivity that benefits the quantum science applications.

Combining Laue diffraction with Bragg coherent diffraction imaging at 34-ID-C.

Measurement modalities in Bragg coherent diffraction imaging (BCDI) rely on finding a signal from a single nanoscale crystal object which satisfies the Bragg condition among a large number of arbitrarily oriented nanocrystals. However, even when the signal from a single Bragg reflection with (hkl) Miller indices is found, the crystallographic axes on the retrieved three-dimensional (3D) image of the crystal remain unknown, and thus localizing in reciprocal space other Bragg reflections becomes time-consuming or requires good knowledge of the orientation of the crystal. Here, the commissioning of a movable double-bounce Si (111) monochromator at the 34-ID-C endstation of the Advanced Photon Source is reported, which aims at delivering multi-reflection BCDI as a standard tool in a single beamline instrument. The new instrument enables, through rapid switching from monochromatic to broadband (pink) beam, the use of Laue diffraction to determine crystal orientation. With a proper orientation matrix determined for the lattice, one can measure coherent diffraction patterns near multiple Bragg peaks, thus providing sufficient information to image the full strain tensor in 3D. The design, concept of operation, the developed procedures for indexing Laue patterns, and automated measuring of Bragg coherent diffraction data from multiple reflections of the same nanocrystal are discussed.

Stress-induced surface instabilities and defects in thin films sputter deposited on compliant substrates.

Existing analyses predict that thin metal films deposited on compliant substrates are subject to a variety of surface instabilities, such as wrinkles, folds, creases, etc., that become more prominent with increased compressive residual stress. Under compressive stress, cracks have been assumed to form only when the interfacial strength is weak, allowing the film to detach from the substrate. In this work, we demonstrate that cracks also form on surfaces under compressive mismatch strain when the interface is strong. In particular, we consider metal alloy films sputter deposited under bias on elastomers with different thicknesses, curing temperatures or surface treatments. The deposition parameters created residual compressive strains and strong adhesion in the bilayers. Samples without surface treatment formed wrinkles and through-thickness cracks at 0.25-0.4% mismatch strains. Only through-thickness cracks were observed in UV treated samples. The crack spacing was found to decrease by a factor of 4 when the surface was UV treated and by a factor of 3 as the elastomer thickness decreased from 30 to 6 µm. Cracks penetrated through the elastomer, 15-30 times deeper than the film thickness, and formed in all samples with a brittle coating. A numerical model was developed to explain the formation of through-thickness cracks and wrinkles under applied compressive mismatch strains. The model suggests that cracks can initiate from the peak of wrinkles when the critical fracture strength of the coating is exceeded. For the UV treated samples, through-thickness cracks are possibly impacted by the formation of an embrittled near surface PDMS layer.

Smallest metallic nanorods using physical vapor deposition.

Physical vapor deposition provides a controllable means of growing two-dimensional metallic thin films and one-dimensional metallic nanorods. While theories exist for the growth of metallic thin films, their counterpart for the growth of metallic nanorods is absent. Because of this absence, the lower limit of the nanorod diameter is theoretically unknown; consequently the experimental pursuit of the smallest nanorods has no clear target. This Letter reports a closed-form theory that defines the diameter of the smallest metallic nanorods using physical vapor deposition. Further, the authors verify the theory using lattice kinetic Monte Carlo simulations and validate the theory using published experimental data. Finally, the authors carry out a series of theory-guided experiments to grow well-separated metallic nanorods of ∼10 nm in diameter, which are the smallest ever reported using physical vapor deposition.

A controlled nucleation and growth of Si nanowires by using a TiN diffusion barrier layer for lithium-ion batteries.

Uniform size of Si nanowires (NWs) is highly desirable to enhance the performance of Si NW-based lithium-ion batteries. To achieve a narrow size distribution of Si NWs, the formation of bulk-like Si structures such as islands and chunks needs to be inhibited during nucleation and growth of Si NWs. We developed a simple approach to control the nucleation of Si NWs via interfacial energy tuning between metal catalysts and substrates by introducing a conductive diffusion barrier. Owing to the high interfacial energy between Au and TiN, agglomeration of Au nanoparticle catalysts was restrained on a TiN layer which induced the formation of small Au nanoparticle catalysts on TiN-coated substrates. The resulting Au catalysts led to the nucleation and growth of Si NWs on the TiN layer with higher number density and direct integration of the Si NWs onto current collectors without the formation of bulk-like Si structures. The lithium-ion battery anodes based on Si NWs grown on TiN-coated current collectors showed improved specific gravimetric capacities (>30%) for various charging rates and enhanced capacity retention up to 500 cycles of charging-discharging.

Three-dimensional X-ray diffraction imaging of dislocations in polycrystalline metals under tensile loading.

The nucleation and propagation of dislocations is an ubiquitous process that accompanies the plastic deformation of materials. Consequently, following the first visualization of dislocations over 50 years ago with the advent of the first transmission electron microscopes, significant effort has been invested in tailoring material response through defect engineering and control. To accomplish this more effectively, the ability to identify and characterize defect structure and strain following external stimulus is vital. Here, using X-ray Bragg coherent diffraction imaging, we describe the first direct 3D X-ray imaging of the strain field surrounding a line defect within a grain of free-standing nanocrystalline material following tensile loading. By integrating the observed 3D structure into an atomistic model, we show that the measured strain field corresponds to a screw dislocation.

Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive.

In this work we explore how an electrolyte additive (fluorinated ethylene carbonate - FEC) mediates the thickness and composition of the solid electrolyte interphase formed over a silicon anode in situ as a function of state-of-charge and cycle. We show the FEC condenses on the surface at open circuit voltage then is reduced to C-O containing polymeric species around 0.9 V (vs. Li/Li+). The resulting film is about 50 Å thick. Upon lithiation the SEI thickens to 70 Å and becomes more organic-like. With delithiation the SEI thins by 13 Å and becomes more inorganic in nature, consistent with the formation of LiF. This thickening/thinning is reversible with cycling and shows the SEI is a dynamic structure. We compare the SEI chemistry and thickness to 280 Å thick SEI layers produced without FEC and provide a mechanism for SEI formation using FEC additives.

Self-organization of helium precipitates into elongated channels within metal nanolayers.

Material degradation due to precipitation of implanted helium (He) is a key concern in nuclear energy. Decades of research have mapped out the fate of He precipitates in metals, from nucleation and growth of equiaxed bubbles and voids to formation and bursting of surface blisters. By contrast, we show that He precipitates confined within nanoscale metal layers depart from their classical growth trajectories: They self-organize into elongated channels. These channels form via templated nucleation of He precipitates along layer surfaces followed by their growth and spontaneous coalescence into stable precipitate lines. The total line length and connectivity increases with the amount of implanted He, indicating that these channels ultimately interconnect into percolating "vascular" networks. Vascularized metal composites promise a transformative solution to He-induced damage by enabling in operando outgassing of He and other impurities while maintaining material integrity.

Strong, Ductile, and Thermally Stable bcc-Mg Nanolaminates.

Magnesium has attracted attention worldwide because it is the lightest structural metal. However, a high strength-to-weight ratio remains its only attribute, since an intrinsic lack of strength, ductility and low melting temperature severely restricts practical applications of Mg. Through interface strains, the crystal structure of Mg can be transformed and stabilized from a simple hexagonal (hexagonal close packed hcp) to body center cubic (bcc) crystal structure at ambient pressures. We demonstrate that when introduced into a nanocomposite bcc Mg is far more ductile, 50% stronger, and retains its strength after extended exposure to 200 C, which is 0.5 times its homologous temperature. These findings reveal an alternative solution to obtaining lightweight metals critically needed for future energy efficiency and fuel savings.