Since several decades, the dynamics and vitrification kinetics of supercooled liquids are the subject of active research in science and engineering. Profiting from modern detector technology and highly brilliant fourth-generation synchrotron radiation, we apply temperature scanning X-ray photon correlation spectroscopy (XPCS) to probe the dynamics of a Pt-based metallic glass former in the glass, glass transition region, and supercooled liquid, covering up to six orders of magnitude in timescales. Our data demonstrates that the structural α-relaxation process is still observable in the glass, although it is partially masked by a faster source of decorrelation observed at atomic scale. We present an approach that interprets these findings as the superposition of heterogeneous liquid-like and stress-driven ballistic-like atomic motions. This work not only extends the dynamical range probed by standard isothermal XPCS but also adds a different view on the α-relaxation across the glass transition and provides insights into the anomalous, compressed temporal decay of the density-density correlation functions observed in metallic glasses and many out-of-equilibrium soft materials.
A two-dimensional numerical model for self-propagating reactions in Al/Ni multilayer foils was developed. It was used to study thermal properties, convective heat loss, and the effect of initial temperature on the self-propagating reaction in Al/Ni multilayer foils. For model adjustments by experimental results, these Al/Ni multilayer foils were fabricated by the magnetron sputtering technique with a 1:1 atomic ratio. Heat of reaction of the fabricated foils was determined employing Differential Scanning Calorimetry (DSC). Self-propagating reaction was initiated by an electrical spark on the surface of the foils. The movement of the reaction front was recorded with a high-speed camera. Activation energy is fitted with these velocity data from the high-speed camera to adjust the numerical model. Calculated reaction front temperature of the self-propagating reaction was compared with the temperature obtained by time-resolved pyrometer measurements. X-ray diffraction results confirmed that all reactants reacted and formed a B2 NiAl phase. Finally, it is predicted that (1) increasing thermal conductivity of the final product increases the reaction front velocity; (2) effect of heat convection losses on reaction characteristics is insignificant, e.g., the foils can maintain their characteristics in water; and (3) with increasing initial temperature of the foils, the reaction front velocity and the reaction temperature increased.
Reactive multilayer systems represent an innovative approach for potential usage in chip joining applications. As there are several factors governing the energy release rate and the stored chemical energy, the impact of the morphology and the microstructure on the reaction behavior is of great interest. In the current work, 3D reactive microstructures with nanoscale Al/Ni multilayers were produced by alternating deposition of pure Ni and Al films onto nanostructured Si substrates by magnetron sputtering. In order to elucidate the influence of this 3D morphology on the phase transformation process, the microstructure and the morphology of this system were characterized and compared with a flat reactive multilayer system on a flat Si wafer. The characterization of both systems was carried out before and after a rapid thermal annealing treatment by using scanning and transmission electron microscopy of the cross sections, selected area diffraction analysis, and differential scanning calorimetry. The bent shape of multilayers caused by the complex topography of silicon needles of the nanostructured substrate was found to favor the atomic diffusion at the early stage of phase transformation and the formation of two intermetallic phases Al0.42Ni0.58 and AlNi3, unlike the flat multilayers that formed a single phase AlNi after reaction.
Surface structuring methods are crucial in semiconductor manufacturing, as they enable the creation of intricate structures on the semiconductor surface, influencing the material's electrical, mechanical, and chemical properties. Herein, one such structuring method known as reactive ion etching to create black Si structures on silicon substrates is employed. After thermal oxidation, their influence on the reaction of Al/Ni nanoscale multilayers is studied. It reveals distinct reactive behaviors without corresponding differences in energy release during differential scanning calorimetry measurements. Higher oxidized black Si structure densities result in elevated temperatures and faster reaction propagation, showing fewer defects and reduced layer connections in cross‐sectional analyses. The properties of the reactive multilayers (RML) on high structure density show the same performance as a reaction on flat thermal SiO2, causing delamination when exceeding 23 structures per μm2. Conversely, lower structure density ensures attachment of RML to the substrate due to an increased number of defects, acting as predetermined breaking points for the AlNi alloy. By establishing the adhesion between the reacted multilayer and the substrate, surface structuring could lead to a potential increase in bond strength when using RML for bonding.
Free‐standing Ni/Al multilayer films with a planar morphology, a bilayer thickness of 20 nm, and an average composition of Ni50Al50 (at%) deposited by direct current magnetron sputtering are investigated by nanocalorimetry and conventional calorimetry. Both the novel fast differential scanning calorimeter (FDSC) Flash DSC 2+ from Mettler–Toledo (MT) and conventional calorimeter MT DSC 3 are used to cover a range of heating rates from 0.1 to 104 K s−1. A quantitative kinetic study of the interdiffusion and phase reaction sequence is performed via a Kissinger analysis covering five orders of magnitude of heating rates. Using the calorimetric data, the derived apparent activation energies suggest monotonic reaction kinetics over the entire range of heating rates applied. To correct the thermal lag at the highest heating rates with the FDSC for nonadhered free‐standing films, a new methodology for its correction is used. Overall, this work extends the application of commercial FDSC to nonadhered films.