Search Results
On the Promotion of Catalytic Reactions by Surface Acoustic Waves
2020, von Boehn, Bernhard, Foerster, Michael, von Boehn, Moritz, Prat, Jordi, Macià, Ferran, Casals, Blai, Khaliq, Muhammad Waqas, Hernández-Mínguez, Alberto, Aballe, Lucia, Imbihl, Ronald
Surface acoustic waves (SAW) allow to manipulate surfaces with potential applications in catalysis, sensor and nanotechnology. SAWs were shown to cause a strong increase in catalytic activity and selectivity in many oxidation and decomposition reactions on metallic and oxidic catalysts. However, the promotion mechanism has not been unambiguously identified. Using stroboscopic X-ray photoelectron spectro-microscopy, we were able to evidence a sub-nanosecond work function change during propagation of 500 MHz SAWs on a 9 nm thick platinum film. We quantify the work function change to 455 μeV. Such a small variation rules out that electronic effects due to elastic deformation (strain) play a major role in the SAW-induced promotion of catalysis. In a second set of experiments, SAW-induced intermixing of a five monolayers thick Rh film on top of polycrystalline platinum was demonstrated to be due to enhanced thermal diffusion caused by an increase of the surface temperature by about 75 K when SAWs were excited. Reversible surface structural changes are suggested to be a major cause for catalytic promotion. © 2020 The Authors. Published by Wiley-VCH GmbH
Impact of Electrical Current on Single GaAs Nanowire Structure
2021, Bahrami, Danial, AlHassan, Ali, Davtyan, Arman, Zhe, Ren, Anjum, Taseer, Herranz, Jesús, Geelhaar, Lutz, Novikov, Dmitri V., Timm, Rainer, Pietsch, Ullrich
The impact of electrical current on the structure of single free-standing Be-doped GaAs nanowires grown on a Si 111 substrate is investigated. Single nanowires have been structurally analyzed by X-ray nanodiffraction using synchrotron radiation before and after the application of an electrical current. The conductivity measurements on single nanowires in their as-grown geometry have been realized via W-probes installed inside a dual-beam focused ion beam/scanning electron microscopy chamber. Comparing reciprocal space maps of the 111 Bragg reflection, extracted perpendicular to the nanowire growth axis before and after the conductivity measurement, the structural impact of the electrical current is evidenced, including deformation of the hexagonal nanowire cross section, tilting, and bending with respect to the substrate normal. For electrical current densities below 30 A mm−2, the induced changes in the reciprocal space maps are negligible. However, for a current density of 347 A mm−2, the diffraction pattern is completely distorted. The mean cross section of the illuminated nanowire volume is reconstructed from the reciprocal space maps before and after the application of electrical current. Interestingly, the elongation of two pairs of opposing side facets accompanied by shrinkage of the third pair of facets is found. The variations in the nanowire diameter, as well as their tilt and bending, are confirmed by scanning electron microscopy. To explain these findings, material melting due to Joule heating during voltage/current application accompanied by anisotropic deformations induced by the W-probe is suggested.
Strategies for Analyzing Noncommon-Atom Heterovalent Interfaces: The Case of CdTe-on-InSb
2019, Luna, Esperanza, Trampert, Achim, Lu, Jing, Aoki, Toshihiro, Zhang, Yong-Hang, McCartney, Martha R., Smith, David J.
Semiconductor heterostructures are intrinsic to a wide range of modern-day electronic devices, such as computers, light-emitting devices, and photodetectors. Knowledge of chemical interfacial profiles in these structures is critical to the task of optimizing the device performance. This work presents an analysis of the composition profile and strain across the noncommon-atom heterovalent CdTe/InSb interface, carried out using a combination of electron microscopy imaging techniques. Because of the close atomic numbers of the constituent elements, techniques such as high-angle annular-dark-field and large-angle bright-field scanning transmission electron microscopy, as well as electron energy-loss spectroscopy, give results from the interface region that are inherently difficult to interpret. By contrast, use of the 002 dark-field imaging technique emphasizes the interface location by comparing differences in structure factors between the two materials. Comparisons of experimental and simulated CdTe-on-InSb profiles reveal that the interface is structurally abrupt to within about 1.5 nm (10–90% criterion), while geometric phase analysis based on aberration-corrected electron microscopy images reveals a minimal level of interfacial strain. The present investigation opens new routes to the systematic investigation of heterovalent interfaces, formed by the combination of other valence-mismatched material systems. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Silane-Mediated Expansion of Domains in Si-Doped κ-Ga2O3 Epitaxy and its Impact on the In-Plane Electronic Conduction
2022, Mazzolini, Piero, Fogarassy, Zsolt, Parisini, Antonella, Mezzadri, Francesco, Diercks, David, Bosi, Matteo, Seravalli, Luca, Sacchi, Anna, Spaggiari, Giulia, Bersani, Danilo, Bierwagen, Oliver, Janzen, Benjamin Moritz, Marggraf, Marcella Naomi, Wagner, Markus R., Cora, Ildiko, Pécz, Béla, Tahraoui, Abbes, Bosio, Alessio, Borelli, Carmine, Leone, Stefano, Fornari, Roberto
Unintentionally doped (001)-oriented orthorhombic κ-Ga2O3 epitaxial films on c-plane sapphire substrates are characterized by the presence of ≈ 10 nm wide columnar rotational domains that can severely inhibit in-plane electronic conduction. Comparing the in- and out-of-plane resistance on well-defined sample geometries, it is experimentally proved that the in-plane resistivity is at least ten times higher than the out-of-plane one. The introduction of silane during metal-organic vapor phase epitaxial growth not only allows for n-type Si extrinsic doping, but also results in the increase of more than one order of magnitude in the domain size (up to ≈ 300 nm) and mobility (highest µ ≈ 10 cm2V−1s−1, with corresponding lowest ρ ≈ 0.2 Ωcm). To qualitatively compare the mean domain dimension in κ-Ga2O3 epitaxial films, non-destructive experimental procedures are provided based on X-ray diffraction and Raman spectroscopy. The results of this study pave the way to significantly improved in-plane conduction in κ-Ga2O3 and its possible breakthrough in new generation electronics. The set of cross-linked experimental techniques and corresponding interpretation here proposed can apply to a wide range of material systems that suffer/benefit from domain-related functional properties.
The Interaction of Extended Defects as the Origin of Step Bunching in Epitaxial III–V Layers on Vicinal Si(001) Substrates
2019, Niehle, Michael, Rodriguez, Jean-Baptiste, Cerutti, Laurent, Tournié, Eric, Trampert, Achim
Several nanometer high steps are observed by (scanning) transmission electron microscopy at the surface and interfaces in heteroepitaxially grown III–Sb layers on vicinal Si(001) substrates. Their relations with antiphase boundaries (APBs) and threading dislocations (TDs) are elaborated. An asymmetric number density of TDs on symmetry-equivalent {111} lattice planes is revealed and explained according to the substrate miscut and the lattice misfit in the heteroepitaxial material system. Finally, a step bunching mechanism is proposed based on the interplay of APBs, TDs, and the vicinal surface of the miscut substrate.
Protection Mechanism against Photocorrosion of GaN Photoanodes Provided by NiO Thin Layers
2020, Kamimura, Jumpei, Budde, Melanie, Bogdanoff, Peter, Tschammer, Carsten, Abdi, Fatwa F., van de Krol, Roel, Bierwagen, Oliver, Riechert, Henning, Geelhaar, Lutz
The photoelectrochemical properties of n-type Ga-polar GaN photoelectrodes covered with NiO layers of different thicknesses in the range 0–20 nm are investigated for aqueous solution. To obtain layers of well-defined thickness and high crystal quality, NiO is grown by plasma-assisted molecular-beam epitaxy. Stability tests reveal that the NiO layers suppress photocorrosion. With increasing NiO thickness, the onset of the photocurrent is shifted to more positive voltages and the photocurrent is reduced, especially for low bias potentials, indicating that hole transfer to the electrolyte interface is hindered by thicker NiO layers. Furthermore, cathodic transient spikes are observed under intermittent illumination, which hints at surface recombination processes. These results are inconsistent with the common explanation of the protection mechanism that the band alignment of GaN/NiO enables efficient hole-injection, thus preventing hole accumulation at the GaN surface that would lead to anodic photocorrosion. Interestingly, the morphology of the etch pits as well as further experiments involving the photodeposition of Ag indicate that photocorrosion of GaN photoanodes is related to reductive processes at threading dislocations. Therefore, it is concluded that the NiO layers block the transfer of photogenerated electrons from GaN to the electrolyte interface, which prevents the cathodic photocorrosion. © 2020 The Authors. Solar RRL published by Wiley-VCH GmbH
Self-Assembly of Well-Separated AlN Nanowires Directly on Sputtered Metallic TiN Films
2020, Azadmand, Mani, Auzelle, Thomas, Lähnemann, Jonas, Gao, Guanhui, Nicolai, Lars, Ramsteiner, Manfred, Trampert, Achim, Sanguinetti, Stefano, Brandt, Oliver, Geelhaar, Lutz
Herein, the self-assembled formation of AlN nanowires (NWs) by molecular beam epitaxy on sputtered TiN films on sapphire is demonstrated. This choice of substrate allows growth at an exceptionally high temperature of 1180 °C. In contrast to previous reports, the NWs are well separated and do not suffer from pronounced coalescence. This achievement is explained by sufficient Al adatom diffusion on the substrate and the NW sidewalls. The high crystalline quality of the NWs is evidenced by the observation of near-band-edge emission in the cathodoluminescence spectrum. The key factor for the low NW coalescence is the TiN film, which spectroscopic ellipsometry and Raman spectroscopy indicate to be stoichiometric. Its metallic nature will be beneficial for optoelectronic devices using these NWs as the basis for (Al,Ga)N/AlN heterostructures emitting in the deep ultraviolet spectral range.
Evolution of Low-Frequency Vibrational Modes in Ultrathin GeSbTe Films
2021, Zallo, Eugenio, Dragoni, Daniele, Zaytseva, Yuliya, Cecchi, Stefano, Borgardt, Nikolai I., Bernasconi, Marco, Calarco, Raffaella
GeSbTe (GST) phase-change alloys feature layered crystalline structures made of lamellae separated by van der Waals (vdW) gaps. This work sheds light on the dependence of interlamellae interactions at the vdW gap on film thickness of GST alloys as probed by vibrational spectroscopy. Molecular beam epitaxy is used for designing GST layers down to a single lamella. By combining density-functional theory and Raman spectroscopy, a direct and simple method is demonstrated to identify the thickness of the GST film. The shift of the vibrational modes is studied as a function of the layer size, and the low-frequency range opens up a new route to probe the number of lamellae for different GST compositions. Comparison between experimental and theoretical Raman spectra highlights the precision growth control obtained by the epitaxial technique.