Plasmonic CO₂ methanation using γ-Al₂O₃-supported Ru nanorods was carried out under continuous-flow conditions without conventional heating, using mildly concentrated sunlight as the sole and sustainable energy source (AM 1.5, irradiance 5.5–14.4 kW·m⁻² = 5.5–14.4 suns). Under 12.5 suns, a CO₂ conversion exceeding 97% was achieved with complete selectivity towards CH₄ and a stable production rate (261.9 mmol·g^{−1 Ru·h−1}) for at least 12 h. The CH₄ production rate showed an exponential increase with increasing light intensity, suggesting that the process was mainly promoted by photothermal heating. This was confirmed by the apparent activation energy of 64.3 kJ·mol⁻¹, which is very similar to the activation energy obtained for reference experiments in dark (67.3 kJ·mol⁻¹). The flow rate influence was studied under 14.4 suns, achieving a CH₄ production plateau of 264 µmol min⁻¹ (792 mmol·g^{−1 Ru·h−1}) with a constant catalyst bed temperature of approximately 204^◦C.

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Sunlight-powered reduction of CO₂ to fuels and chemicals is a promising strategy to close the carbon loop and facilitate the energy transition. In this research, we demonstrate that Au nanoparticles supported on TiO₂ are an efficient plasmonic catalyst for the sunlight-powered reverse water-gas shift (rWGS) reaction. A maximum CO production rate of 429 mmol ⋅ g_Au⁻¹ ⋅ h⁻¹ with a selectivity of 98 % and an apparent quantum efficiency of 4.7 % were achieved using mildly concentrated sunlight (1.44 W ⋅ cm⁻² equals 14.4 sun). The CO production rate showed an exponential increase with increasing light intensity, suggesting that the process is mainly promoted by a photothermal effect. Thermal reference experiments with the same catalysts promoted CH₄ formation, dropping the CO selectivity to 70 %. Thus, mildly concentrated sunlight can efficiently and selectively enhance the promotion of the rWGS reaction without using external heating.

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The growth of Sn-rich group-IV semiconductors at the nanoscale can enrich the understanding of the fundamental properties of metastable GeSn alloys. Here, we demonstrate the effect of the growth conditions on the morphology and composition of Ge/GeSn core/shell nanowires by correlating the experimental observations with a theoretical interpretation based on a multiscale approach. We show that the cross-sectional morphology of Ge/GeSn core/shell nanowires changes from hexagonal to dodecagonal upon increasing the supply of the Sn precursor. This transformation strongly influences the Sn distribution as a higher Sn content is measured under the {112} growth front. Ab initio DFT calculations provide an atomic-scale explanation by showing that Sn incorporation is favored at the {112} surfaces, where the Ge bonds are tensile-strained. A phase-field continuum model was developed to reproduce the morphological transformation and the Sn distribution within the wire, shedding light on the complex growth mechanism and unveiling the relation between segregation and faceting. The tunability of the photoluminescence emission with the change in composition and morphology of the GeSn shell highlights the potential of the core/shell nanowire system for optoelectronic devices operating at mid-infrared wavelengths.

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We show a hard superconducting gap in a Ge-Si nanowire Josephson transistor up to in-plane magnetic fields of 250 mT, an important step toward creating and detecting Majorana zero modes in this system. A hard gap requires a highly homogeneous tunneling heterointerface between the superconducting contacts and the semiconducting nanowire. This is realized by annealing devices at 180 °C during which aluminum interdiffuses and replaces the germanium in a section of the nanowire. Next to Al, we find a superconductor with lower critical temperature (TC = 0.9 K) and a higher critical field (BC = 0.9-1.2 T). We can therefore selectively switch either superconductor to the normal state by tuning the temperature and the magnetic field and observe that the additional superconductor induces a proximity supercurrent in the semiconducting part of the nanowire even when the Al is in the normal state. In another device where the diffusion of Al rendered the nanowire completely metallic, a superconductor with a much higher critical temperature (TC = 2.9 K) and critical field (BC = 3.4 T) is found. The small size of these diffusion-induced superconductors inside nanowires may be of special interest for applications requiring high magnetic fields in arbitrary direction.

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High aspect-ratio InSb nanowires (NWs) of high chemical purity are sought for implementing advanced quantum devices. The growth of InSb NWs is challenging, generally requiring a stem of a foreign material for nucleation. Such a stem tends to limit the length of InSb NWs and its material becomes incorporated in the InSb segment. Here, we report on the growth of chemically pure InSb NWs tens of microns long. Using a selective-area mask in combination with gold as a catalyst allows complete omission of the stem, thus demonstrating that InSb NWs can grow directly from the substrate. The introduction of the selective-area mask gives rise to novel growth kinetics, demonstrating high growth rates and complete suppression of layer deposition on the mask for Sb-rich conditions. The crystal quality and chemical purity of these NWs is reflected in the significant enhancement of low-temperature electron mobility, yielding an average of 4.4 × 10⁴ cm²/(V s), compared to previously studied InSb NWs grown on stems.

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We demonstrate the merits of an unexplored precursor, tetrasilane (Si₄H₁₀), as compared to disilane (Si₂H₆) for the growth of defect-free, epitaxial hexagonal silicon (Si). We investigate the growth kinetics of hexagonal Si shells epitaxially around defect-free wurtzite gallium phosphide (GaP) nanowires. Two temperature regimes are identified, representing two different surface reaction mechanisms for both types of precursors. Growth in the low temperature regime (415 °C-600 °C) is rate limited by interaction between the Si surface and the adsorbates, and in the high temperature regime (600 °C-735 °C) by chemisorption. The activation energy of the Si shell growth is 2.4 ±0.2 eV for Si₂H₆ and 1.5 ±0.1 eV for Si₄H₁₀ in the low temperature regime. We observe inverse tapering of the Si shells and explain this phenomenon by a basic diffusion model where the substrate acts as a particle sink. Most importantly, we show that, by using Si₄H₁₀ as a precursor instead of Si₂H₆, non-tapered Si shells can be grown with at least 50 times higher growth rate below 460 °C. The lower growth temperature may help to reduce the incorporation of impurities resulting from the growth of GaP.

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We report on the selective-area chemical beam epitaxial growth of InAs in-plane, one-dimensional (1D) channels using patterned SiO2-coated InP(001), InP(111)B, and InP(011) substrates to establish a scalable platform for topological superconductor networks. Top-view scanning electron micrographs show excellent surface selectivity and dependence of major facet planes on the substrate orientations and ridge directions, and the ratios of the surface energies of the major facet planes were estimated. Detailed structural properties and defects in the InAs nanowires (NWs) were characterized by transmission electron microscopic analysis of cross-sections perpendicular to the NW ridge direction and along the NW ridge direction. Electrical transport properties of the InAs NWs were investigated using Hall bars, a field effect mobility device, a quantum dot, and an Aharonov-Bohm loop device, which reflect the strong spin-orbit interaction and phase-coherent transport characteristic present in the selectively grown InAs systems. This study demonstrates that selective-area chemical beam epitaxy is a scalable approach to realize semiconductor 1D channel networks with the excellent surface selectivity and this material system is suitable for quantum transport studies.

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Semiconductor nanowires are ideal for realizing various low-dimensional quantum devices. In particular, topological phases of matter hosting non-Abelian quasiparticles (such as anyons) can emerge when a semiconductor nanowire with strong spin-orbit coupling is brought into contact with a superconductor. To exploit the potential of non-Abelian anyons - which are key elements of topological quantum computing - fully, they need to be exchanged in a well-controlled braiding operation. Essential hardware for braiding is a network of crystalline nanowires coupled to superconducting islands. Here we demonstrate a technique for generic bottom-up synthesis of complex quantum devices with a special focus on nanowire networks with a predefined number of superconducting islands. Structural analysis confirms the high crystalline quality of the nanowire junctions, as well as an epitaxial superconductor-semiconductor interface. Quantum transport measurements of nanowire 'hashtags' reveal Aharonov-Bohm and weak-antilocalization effects, indicating a phase-coherent system with strong spin-orbit coupling. In addition, a proximity-induced hard superconducting gap (with vanishing sub-gap conductance) is demonstrated in these hybrid superconductor-semiconductor nanowires, highlighting the successful materials development necessary for a first braiding experiment. Our approach opens up new avenues for the realization of epitaxial three-dimensional quantum architectures which have the potential to become key components of various quantum devices.

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We have critically evaluated the deposition parameter space of very high frequency plasma-enhanced chemical vapour deposition discharges near the amorphous to crystalline transition for intrinsic a-Si:H passivation layers on Si (1 1 1) wafers. Using a low silane concentration in the SiH₄-H₂ feedstock gas mixture that created amorphous material just before the transition, we have obtained samples with excellent surface passivation. Also, an a-Si:H matrix was grown with embedded local epitaxial growth of crystalline cones on a Si (1 1 1) substrate, as was revealed with a combined scanning electron and high-resolution transmission electron microscopy study. This local epitaxial growth was introduced by a decrease of the silane concentration in the feedstock gas or an increase in discharge power at low silane concentration. Together with the samples on Si (1 1 1) substrates, layers were co-deposited on Si (1 0 0) substrates. This resulted in void-rich, mono-crystalline epitaxial layers on Si (1 0 0). The epitaxial growth on Si (1 0 0) was compared to the local epitaxial growth on Si (1 1 1). The sparse surface coverage of cones seeded on the Si (1 1 1) substrate is most probably enabled by a combination of nucleation at steps and kinks in the (1 1 1) surface and intense ion bombardment at low silane concentration. The effective carrier lifetime of this sample is low and does not increase upon post-deposition annealing. Thus, sparse local epitaxial growth on Si (1 1 1) is enough to obstruct crystalline silicon surface passivation by amorphous silicon.

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Semiconductor nanowires are nanoscale structures holding promise in many fields such as optoelectronics, quantum computing, and thermoelectrics. Nanowires are usually grown vertically on (111)-oriented substrates, while (100) is the standard in semiconductor technology. The ability to grow and to control impurity doping of 〈100〉 nanowires is crucial for integration. Here, we discuss doping of single-crystalline 〈100〉 nanowires, and the structural and optoelectronic properties of p-n junctions based on 〈100〉 InP nanowires. We describe a novel approach to achieve low resistance electrical contacts to nanowires via a gradual interface based on p-doped InAsP. As a first demonstration in optoelectronic devices, we realize a single nanowire light emitting diode in a 〈100〉-oriented InP nanowire p-n junction. To obtain high vertical yield, which is necessary for future applications, we investigate the effect of the introduction of dopants on the nanowire growth.

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Nanowire based solar cells have attracted great attention due to their potential for high efficiency and low device cost. Photovoltaic devices based on InP nanowires now have characteristics comparable to InP bulk solar cells. A detailed and direct correlation of the influence of growth conditions on performance is necessary to improve efficiency further. We explored the effects of the growth temperature, and of the addition of HCl during growth, on the efficiency of nanowire array based solar cell devices. By increasing HCl, the saturation dark current was reduced, and thereby the nanowire solar cell efficiency was enhanced from less than 1% to 7.6% under AM 1.5 illumination at 1 sun. At the same time, we observed that the solar cell efficiency decreased by increasing the tri-methyl-indium content, strongly suggesting that these effects are carbon related.

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A method to control the hydrophobicity and dielectric constant of mesoporous silica films for ultralow-k-applications is described. Several surfactants have been used as sacrificial materials in (organo)silicate matrixes, prepared from tetraethoxysilane and methyltrimethoxysilane. To elucidate the relation between the composition of the films and their structure, the synthesis, chemical composition, mechanical properties, pore structure, crystallinity, and dielectric constant of the films were investigated. The high extent to which organic groups can be incorporated in these thin films opens the possibility to obtain a fully hydrophobic surface. Further, a combination of tetraethoxysilane and methyltrimethoxysilane leads to dense matrixes. The film properties were optimized for low-A- applications by varying the processing conditions. Films containing 50-60% methyltrimethoxysilane in tetraethoxysilane and cetyl trimethylammonium bromide as a surfactant appear most attractive as a low-A- material. These films are hydrophobic, have a dense matrix, and exhibit the smallest pore sizes (∼3 nm), which may facilitate integration issues.@en