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Abstract Bridging functionalities in periodic mesoporous organosilicas (PMOs) enable new functionalities for a wide range of applications. Bridge cleavage is frequently observed during anneals required to form porous structures, yet the mechanism of these bridge cleavages has not been completely resolved. Here, these chemical transformations and their kinetic pathways on sub‐millisecond timescales induced by laser heating are revealed. By varying anneal times and temperatures, the transformation dynamics of bridge cleavage and structural transformations and their activation energies are determined. The structural relaxation time for individual reactions and their effective local heating time are determined and compared, and the results directly demonstrate the manipulation of different molecules through kinetic control of the sequence of reactions. By isolating and understanding the earliest stage of structural transformations, this study identifies the kinetic principles for new synthesis and post‐processing routes to control individual molecules and reactions in PMOs and other material systems with multi‐functionalities. 

Here, we report that a source of Si impurities commonly observed on (010) β-Ga2O3 is from exposure of the surface to air. Moreover, we find that a 15 min hydrofluoric acid (HF) (49%) treatment reduces the Si density by approximately 1 order of magnitude on (010) β-Ga2O3 surfaces. This reduction in Si is critical for the elimination of the often observed parasitic conducting channel, which negatively affects transport properties and lateral transistor performance. After the HF treatment, the sample must be immediately put under vacuum, for the Si fully returns within 10 min of additional air exposure. Finally, we demonstrate that performing a 30 min HF (49%) treatment on the substrate before growth has no deleterious effect on the structure or on the epitaxy surface after subsequent Ga2O3 growth. 

Abstract Surface structures on radio-frequency (RF) superconductors are crucially important in determining their interaction with the RF field. Here we investigate the surface compositions, structural profiles, and valence distributions of oxides, carbides, and impurities on niobium (Nb) and niobium–tin (Nb₃Sn)in situunder different processing conditions. We establish the underlying mechanisms of vacuum baking and nitrogen processing in Nb and demonstrate that carbide formation induced during high-temperature baking, regardless of gas environment, determines subsequent oxide formation upon air exposure or low-temperature baking, leading to modifications of the electron population profile. Our findings support the combined contribution of surface oxides and second-phase formation to the outcome of ultra-high vacuum baking (oxygen processing) and nitrogen processing. Also, we observe that vapor-diffused Nb₃Sn contains thick metastable oxides, while electrochemically synthesized Nb₃Sn only has a thin oxide layer. Our findings reveal fundamental mechanisms of baking and processing Nb and Nb₃Sn surface structures for high-performance superconducting RF and quantum applications. 

Abstract Workbench-size particle accelerators, enabled by Nb₃Sn-based superconducting radio-frequency (SRF) cavities, hold the potential of driving scientific discovery by offering a widely accessible and affordable source of high-energy electrons and x-rays. Thin-film Nb₃Sn RF superconductors with high quality factors, high operation temperatures, and high-field potentials are critical for these devices. However, surface roughness, non-stoichiometry, and impurities in Nb₃Sn deposited by conventional Sn-vapor diffusion prevent them from reaching their theoretical capabilities. Here we demonstrate a seed-free electrochemical synthesis that pushes the limit of chemical and physical properties in Nb₃Sn. Utilization of electrochemical Sn pre-deposits reduces the roughness of converted Nb₃Sn by five times compared to typical vapor-diffused Nb₃Sn. Quantitative mappings using chemical and atomic probes confirm improved stoichiometry and minimized impurity concentrations in electrochemically synthesized Nb₃Sn. We have successfully applied this Nb₃Sn to the large-scale 1.3 GHz SRF cavity and demonstrated ultra-low BCS surface resistances at multiple operation temperatures, notably lower than vapor-diffused cavities. Our smooth, homogeneous, high-purity Nb₃Sn provides the route toward high efficiency and high fields for SRF applications under helium-free cryogenic operations. 

Beta-phase gallium oxide ([Formula: see text]-Ga 2 O 3 ) is a promising semiconductor for high frequency, high temperature, and high voltage applications. In addition to the [Formula: see text]-phase, numerous other polymorphs exist and understanding the competition between phases is critical to control practical devices. The phase formation sequence of Ga 2 O 3 , starting from amorphous thin films, was determined using lateral-gradient laser spike annealing at peak temperatures of 500–1400 °C on 400 μs to 10 ms timescales, with transformations characterized by optical microscopy, x-ray diffraction, and transmission electron microscopy (TEM). The resulting phase processing map showed the [Formula: see text]-phase, a defect-spinel structure, first nucleating under all annealing times for temperatures from 650 to 800 °C. The cross-sectional TEM at the onset of the [Formula: see text]-phase formation showed nucleation near the film center with no evidence of heterogeneous nucleation at the interfaces. For temperatures above 850 °C, the thermodynamically stable [Formula: see text]-phase was observed. For anneals of 1–4 ms and temperatures below 1200 °C, small randomly oriented grains were observed. Large grains were observed for anneals below 1 ms and above 1200 °C, with anneals above 4 ms and 1200 °C resulting in textured films. The formation of the [Formula: see text]-phase prior to [Formula: see text]-phase, coupled with the observed grain structure, suggests that the [Formula: see text]-phase is kinetically preferred during thermal annealing of amorphous films, with [Formula: see text]-phase subsequently forming by nucleation at higher temperatures. The low surface energy of the [Formula: see text]-phase implied by these results suggests an explanation for the widely observed [Formula: see text]-phase inclusions in [Formula: see text]-phase Ga 2 O 3 films grown by a variety of synthesis methods.