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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.

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Electron Tomography of Pencil-Shaped GaN/(In,Ga)N Core-Shell Nanowires

2019, Nicolai, Lars, Gačević, Žarko, Calleja, Enrique, Trampert, Achim

The three-dimensional structure of GaN/(In,Ga)N core-shell nanowires with multi-faceted pencil-shaped apex is analyzed by electron tomography using high-angle annular dark-field mode in a scanning transmission electron microscope. Selective area growth on GaN-on-sapphire templates using a patterned mask is performed by molecular beam epitaxy to obtain ordered arrays of uniform nanowires. Our results of the tomographic reconstruction allow the detailed determination of the complex morphology of the inner (In,Ga)N multi-faceted shell structure and its deviation from the perfect hexagonal symmetry. The tomogram unambiguously identifies a dot-in-a-wire configuration at the nanowire apex including the exact shape and size, as well as the spatial distribution of its chemical composition. © 2019, The Author(s).

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In Situ Transmission Electron Microscopy of Disorder–Order Transition in Epitaxially Stabilized FeGe2

2021, Terker, Markus, Nicolai, Lars, Gaucher, Samuel, Herfort, Jens, Trampert, Achim

Isothermal crystallization of amorphous Ge deposited on a cubic Fe3Si/GaAs(001) substrate is performed by in situ annealing within a transmission electron microscope. It was found that the formation of epitaxially aligned tetragonal FeGe2 is associated with a disorder–order phase transition mainly consisting of a rearrangement of the Fe/vacancy sublattice from a random distribution to alternating filled and empty layers. Additionally, atomically resolved high-angle annular dark-field scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy demonstrated that the vertical lattice spacing of the Ge sublattice reduces across vacancy layers, indicating that strain minimization plays a role in the phase transition process. Crystallization and ordering are both found to proceed layer-by-layer and with square-root-shaped kinetics with a smaller transition rate for the latter.

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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.

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Engineering grain boundaries at the 2D limit for the hydrogen evolution reaction

2020, He, Yongmin, Tang, Pengyi, Hu, Zhili, He, Qiyuan, Zhu, Chao, Wang, Luqing, Zeng, Qingsheng, Golani, Prafful, Gao, Guanhui, Fu, Wei, Huang, Zhiqi, Gao, Caitian, Xia, Juan, Wang, Xingli, Wang, Xuewen, Zhu, Chao, Ramasse, Quentin M., Zhang, Ao, An, Boxing, Zhang, Yongzhe, Martí-Sánchez, Sara, Morante, Joan Ramon, Wang, Liang, Tay, Beng Kang, Yakobson, Boris I., Trampert, Achim, Zhang, Hua, Wu, Minghong, Wang, Qi Jie, Arbiol, Jordi, Liu, Zheng

Atom-thin transition metal dichalcogenides (TMDs) have emerged as fascinating materials and key structures for electrocatalysis. So far, their edges, dopant heteroatoms and defects have been intensively explored as active sites for the hydrogen evolution reaction (HER) to split water. However, grain boundaries (GBs), a key type of defects in TMDs, have been overlooked due to their low density and large structural variations. Here, we demonstrate the synthesis of wafer-size atom-thin TMD films with an ultra-high-density of GBs, up to ~1012 cm−2. We propose a climb and drive 0D/2D interaction to explain the underlying growth mechanism. The electrocatalytic activity of the nanograin film is comprehensively examined by micro-electrochemical measurements, showing an excellent hydrogen-evolution performance (onset potential: −25 mV and Tafel slope: 54 mV dec−1), thus indicating an intrinsically high activation of the TMD GBs.

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Application of electron tomography for comprehensive determination of III-V interface properties

2021, Nicolai, Lars, Biermann, Klaus, Trampert, Achim

We present an electron tomography method for the comprehensive characterization of buried III-V semiconductor interfaces that is based on chemical-sensitive high-angle annular dark-field scanning transmission electron microscopy. For this purpose, an (Al,Ga)As/GaAs multi-layer system grown by molecular beam epitaxy is used as a case study. Isoconcentration surfaces are exploited to obtain topographic height maps of 120 nm × 120 nm area, revealing the interface morphology. By applying the height-height correlation function, we are able to determine important interface properties like root mean square roughness and lateral correlation length of various interfaces of the (Al,Ga)As/GaAs system characterized by different Al concentrations. Height-difference maps based on isosurfaces corresponding to 30% and 70% of the total compositional difference at the interfaces are used to create topographic maps of the interface width and to calculate an average interface width. This methodology proves differences in the properties of direct and inverted interfaces and allows the observation of interfacial anisotropies. © 2021

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Epitaxial synthesis of unintentionally doped p-type SnO (001) via suboxide molecular beam epitaxy

2023, Egbo, Kingsley, Luna, Esperanza, Lähnemann, Jonas, Hoffmann, Georg, Trampert, Achim, Grümbel, Jona, Kluth, Elias, Feneberg, Martin, Goldhahn, Rüdiger, Bierwagen, Oliver

By employing a mixed SnO2 + Sn source, we demonstrate suboxide molecular beam epitaxy (S-MBE) growth of phase-pure single-crystalline metastable SnO (001) thin films on Y-stabilized ZrO2 (001) substrates at a growth rate of ∼1.0 nm/min without the need for additional oxygen. These films grow epitaxially across a wide substrate temperature range from 150 to 450 °C. Hence, we present an alternative pathway to overcome the limitations of high Sn or SnO2 cell temperatures and narrow growth windows encountered in previous MBE growth of metastable SnO. In situ laser reflectometry and line-of-sight quadrupole mass spectrometry were used to investigate the rate of SnO desorption as a function of substrate temperature. While SnO ad-molecule desorption at TS = 450 °C was growth-rate limiting, the SnO films did not desorb at this temperature after growth in vacuum. The SnO (001) thin films are transparent and unintentionally p-type doped, with hole concentrations and mobilities in the range of 0.9-6.0 × 1018 cm-3 and 2.0-5.5 cm2 V-1 s-1, respectively. These p-type SnO films obtained at low substrate temperatures are promising for back-end-of-line (BEOL) compatible applications and for integration with n-type oxides in pn heterojunctions and field-effect transistors.

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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

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Annealing induced atomic rearrangements on (Ga,In) (N,As) probed by hard X-ray photoelectron spectroscopy and X-ray absorption fine structure

2018, Ishikawa, Fumitaro, Higashi, Kotaro, Fuyuno, Satoshi, Morifuji, Masato, Kondow, Masahiko, Trampert, Achim

We study the effects of annealing on (Ga0.64,In0.36) (N0.045,As0.955) using hard X-ray photoelectron spectroscopy and X-ray absorption fine structure measurements. We observed surface oxidation and termination of the N-As bond defects caused by the annealing process. Specifically, we observed a characteristic chemical shift towards lower binding energies in the photoelectron spectra related to In. This phenomenon appears to be caused by the atomic arrangement, which produces increased In-N bond configurations within the matrix, as indicated by the X-ray absorption fine structure measurements. The reduction in the binding energies of group-III In, which occurs concomitantly with the atomic rearrangements of the matrix, causes the differences in the electronic properties of the system before and after annealing.