Maskless Preparation of Spatially-Resolved Plasmonic Nanoparticles on Polydimethylsiloxane via In Situ Fluoride-Assisted Synthesis

Here, a fluoride-assisted route for the controlled in-situ synthesis of metal nanoparticles (NPs) (i.e., AgNPs, AuNPs) on polydimethylsiloxane (PDMS) is reported. The size and coverage of the NPs on the PDMS surface are modulated with time and over space during the synthetic process, leveraging the improved yield (10×) and faster kinetics (100×) of NP formation in the presence of F⁻ ions, compared to fluoride-free approaches. This enables the maskless preparation of both linear and step gradients and patterns of NPs in 1D and 2D on the PDMS surface. As an application in flexible plasmonics/photonics, continuous and step-wise spatial modulations of the plasmonic features of PDMS slabs with 1D and 2D AgNP gradients on the surface are demonstrated. An excellent spatially resolved tuning of key optical parameters, namely, optical density from zero to 5 and extinction ratio up to 100 dB, is achieved with AgNP gradients prepared in AgF solution for 12 minutes; the performance are comparable to those of commercial dielectric/interference filters. When used as a rejection filter in optical fluorescence microscopy, the AgNP-PDMS slabs are able to reject the excitation laser at 405 nm and retain the green fluorescence of microbeads (100 µm) used as test cases.     

Novel Bi-Doped Amorphous SnOx Nanoshells for Efficient Electrochemical CO2 Reduction into Formate at Low Overpotentials

Engineering novel Sn-based bimetallic materials could provide intriguing catalytic properties to boost the electrochemical CO₂ reduction. Herein, the first synthesis of homogeneous Sn_1−xBi_x alloy nanoparticles (x up to 0.20) with native Bi-doped amorphous SnO_x shells for efficient CO₂ reduction is reported. The Bi-SnO_x nanoshells boost the production of formate with high Faradaic efficiencies (>90%) over a wide potential window (−0.67 to −0.92 V vs RHE) with low overpotentials, outperforming current tin oxide catalysts. The state-of-the-art Bi-SnO_x nanoshells derived from Sn_0.80Bi_0.20 alloy nanoparticles exhibit a great partial current density of 74.6 mA cm⁻² and high Faradaic efficiency of 95.8%. The detailed electrocatalytic analyses and corresponding density functional theory calculations simultaneously reveal that the incorporation of Bi atoms into Sn species facilitates formate production by suppressing the formation of H₂ and CO.     

Crack initiation and propagation in braided SiC/SiC composite tubes: Effect of braiding angle

Crack initiation and propagation in three braided SiC/SiC composite tubes with different braiding angles are investigated by in situ tensile tests with synchrotron micro-computed tomography. Crack networks are precisely detected after an image subtraction procedure based on Digital Volume Correlation. FFT based simulations are performed on the full-resolution 3D images to assess elastic stress/strain fields. Quantitative measurements of the crack geometries are performed using a novel method based on grey levels. The results show that braiding angle has no obvious effect on the location of crack onsets (initiation always occurs at tow interfaces), whereas it significantly affects the paths of crack propagation. This work provides an explicit demonstration of the crack propagation scenarios with respect to the mesoscopic fibre architectures.     

In situ characterization of LiY(WO4)2 nanotubes for electrochemical energy storage

Here, LiY(WO₄)₂ nanotubes are prepared via a feasible electrospinning technique. This new anode material shows excellent electrochemical properties. The capacity loss of LiY(WO₄)₂ nanotubes is as low as 6.9% after 156 cycles, while bulk LiY(WO₄)₂ presents the capacity loss higher than 55.0%. Even after 600 long-life cycles, the capacity loss of the nanotubes is only 9%. It can be seen that the hollow structure with a rough surface and a porous morphology contributes to the improvement of electrochemical performance. Furthermore, online X-ray diffraction (XRD) method is firstly applied to understand the lithium ions insertion/extraction mechanism of LiY(WO₄)₂ nanotubes. It can be concluded that it is an asymmetrical two-phase reaction. A phase transformation from LiY(WO₄)₂ to Li₃Y(WO₄)₂ can be obviously seen from the in situ XRD during discharge process. While Li₂Y(WO₄)₂ appears as an intermediate phase with a reverse charge reaction. In addition, in situ XRD also demonstrates that LiY(WO₄)₂ nanotubes have surprised electrochemical reversibility. All the above results indicate that LiY(WO₄)₂ nanotubes can be expected to be anode candidate for rechargeable lithium ion batteries (LIBs).     

In-situ TEM observation of structural changes in nano-crystalline CoCrCuFeNi multicomponent high-entropy alloy (HEA) under fast electron irradiation by high voltage electron microscopy (HVEM)

The structural changes induced in a CoCrCuFeNi multicomponent nano-crystalline high-entropy alloy (HEA) under fast electron irradiation were investigated by in-situ transmission electron microscopy (TEM) using a high voltage electron microscope (HVEM). A fine-grained face centered cubic (fcc) single phase was obtained in the sputtered specimens. The fcc solid solution showed high phase stability against irradiation over a wide temperature range from 298 to 773 K, and remained as the main constituent phase even when the samples were irradiated up to 40 displacement per atom (dpa). Moreover, the irradiation did not seem to induce grain coarsening. This is the first report on the irradiation damage in 5-component HEA under MeV electron irradiation.     

A miniature triaxial apparatus for investigating the micromechanics of granular soils with in situ X-ray micro-tomography scanning

The development of a miniature triaxial apparatus is presented. In conjunction with an X-ray micro-tomography (termed as X-ray μCT hereafter) facility and advanced image processing techniques, this apparatus can be used for in situ investigation of the micro-scale mechanical behavior of granular soils under shear. The apparatus allows for triaxial testing of a miniature dry sample with a size of \mathrm{8}\hspace{0.17em}\mathrm{mm}\times \mathrm{16}\hspace{0.17em}\mathrm{mm} (diameter \times height). In situ triaxial testing of a 0.4–0.8 mm Leighton Buzzard sand (LBS) under a constant confining pressure of 500 kPa is presented. The evolutions of local porosities (i.e., the porosities of regions associated with individual particles), particle kinematics (i.e., particle translation and particle rotation) of the sample during the shear are quantitatively studied using image processing and analysis techniques. Meanwhile, a novel method is presented to quantify the volumetric strain distribution of the sample based on the results of local porosities and particle tracking. It is found that the sample, with nearly homogenous initial local porosities, starts to exhibit obvious inhomogeneity of local porosities and localization of particle kinematics and volumetric strain around the peak of deviatoric stress. In the post-peak shear stage, large local porosities and volumetric dilation mainly occur in a localized band. The developed triaxial apparatus, in its combined use of X-ray μCT imaging techniques, is a powerful tool to investigate the micro-scale mechanical behavior of granular soils.     

Coupling in situ experiments and modeling – Opportunities for data fusion,machine learning,and discovery of emergent behavior

This paper reviews recent studies, that not only includes both experiments and modeling components, but celebrates a close coupling between these techniques, in order to provide insights into the plasticity and failure of polycrystalline metals. Examples are provided of studies across multiple-scales, including, but not limited to, density functional theory combined with atom probe tomography, molecular dynamics combined with in situ transmission electron miscopy, discrete dislocation dynamics combined with nanopillars experiments, crystal plasticity combined with digital image correlation, and crystal plasticity combined with in situ high energy X-ray diffraction. The close synergy between in situ experiments and modeling provides new opportunities for model calibration, verification, and validation, by providing direct means of comparison, thus removing aspects of epistemic uncertainty in the approach. Further, data fusion between in situ experimental and model-based data, along with data driven approaches, provides a paradigm shift for determining the emergent behavior of deformation and failure, which is the foundation that underpins the mechanical behavior of polycrystalline materials.     

Evolution of properties of parts during MIM and sintering of recycled oxide particles

Metal injection moulding (MIM) is an established process for high volume production of complex shaped metallic parts using commercially available feedstocks. The characteristics of parts after moulding, debinding, and sintering cannot be simply predictable from raw materials because the properties get altered with the process parameters and the corresponding levels of porosity during processing steps. In this study, physical properties, microstructure, and mechanical properties of the MIM parts have been characterised to understand the evolution of strength during various steps in MIM processing. Feedstocks with different binder loading show a considerable difference in physical as well as mechanical characteristics. During sintering of parts which have solid loading of grinding sludge, simultaneous in situ reduction and densification takes place, whereas only densification occurs in carbonyl iron parts. It is, therefore, possible to make complex shaped parts of different levels of porosity from downgraded shop floor metallic waste.     

In situ TEM observations of fracture in nanolaminated metallic thin films

Fracture of single crystal nanolaminated thin films has been investigated through in situ straining of cross-sectional samples of Cu/Ni nanolaminates grown on Cu (001) single crystal substrates. The earlest stages of deformation exhibits a confined layer slip mechanism. With continued straining, unstable fracture occurs creating a mixed-mode crack that propagates across the nanolaminate, roughly perpendicular to the interfaces. Eventually, stable crack growth with intense plastic deformation ahead of the crack tip occurs over many bilayers in the direction of crack growth. Simultaneously, plasticity was seen to spread only 1 or 2 bilayer distances normal to the crack, creating an extremely localized plastic zone. Transmission electron microscopic (TEM) examination after the test did not reveal the presence of dislocations in the crack wake, except where severe crack deflection was observed. By comparison, the plastic zone size in the substrate was greater by several of orders of magnitude.