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    Beam damage of single semiconductor nanowires during X-ray nanobeam diffraction experiments
    (Chester : IUCr, 2020) Al Hassan, Ali; Lähnemann, Jonas; Davtyan, Arman; Al-Humaidi, Mahmoud; Herranz, Jesús; Bahrami, Danial; Anjum, Taseer; Bertram, Florian; Dey, Arka Bikash; Geelhaar, Lutz; Pietsch, Ullrich
    Nanoprobe X-ray diffraction (nXRD) using focused synchrotron radiation is a powerful technique to study the structural properties of individual semiconductor nanowires. However, when performing the experiment under ambient conditions, the required high X-ray dose and prolonged exposure times can lead to radiation damage. To unveil the origin of radiation damage, a comparison is made of nXRD experiments carried out on individual semiconductor nanowires in their as-grown geometry both under ambient conditions and under He atmosphere at the microfocus station of the P08 beamline at the third-generation source PETRA III. Using an incident X-ray beam energy of 9 keV and photon flux of 1010 s-1, the axial lattice parameter and tilt of individual GaAs/In0.2Ga0.8As/GaAs core-shell nanowires were monitored by continuously recording reciprocal-space maps of the 111 Bragg reflection at a fixed spatial position over several hours. In addition, the emission properties of the (In,Ga)As quantum well, the atomic composition of the exposed nanowires and the nanowire morphology were studied by cathodoluminescence spectroscopy, energy-dispersive X-ray spectroscopy and scanning electron microscopy, respectively, both prior to and after nXRD exposure. Nanowires exposed under ambient conditions show severe optical and morphological damage, which was reduced for nanowires exposed under He atmosphere. The observed damage can be largely attributed to an oxidation process from X-ray-induced ozone reactions in air. Due to the lower heat-transfer coefficient compared with GaAs, this oxide shell limits the heat transfer through the nanowire side facets, which is considered as the main channel of heat dissipation for nanowires in the as-grown geometry.
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    Self-Assembly of Well-Separated AlN Nanowires Directly on Sputtered Metallic TiN Films
    (Weinheim : Wiley-VCH, 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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    Epitaxial synthesis of unintentionally doped p-type SnO (001) via suboxide molecular beam epitaxy
    (Melville, NY : AIP, 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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    Dislocation and indium droplet related emission inhomogeneities in InGaN LEDs
    (Bristol : IOP Publ., 2021) van Deurzen, Len; Gómez Ruiz, Mikel; Lee, Kevin; Turski, Henryk; Bharadwaj, Shyam; Page, Ryan; Protasenko, Vladimir; Xing, Huili (Grace); Lähnemann, Jonas; Jena, Debdeep
    This report classifies emission inhomogeneities that manifest in InGaN quantum well blue light-emitting diodes grown by plasma-assisted molecular beam epitaxy on free-standing GaN substrates. By a combination of spatially resolved electroluminescence and cathodoluminescence measurements, atomic force microscopy, scanning electron microscopy and hot wet potassium hydroxide etching, the identified inhomogeneities are found to fall in four categories. Labeled here as type I through IV, they are distinguishable by their size, density, energy, intensity, radiative and electronic characteristics and chemical etch pits which correlates them with dislocations. Type I exhibits a blueshift of about 120 meV for the InGaN quantum well emission attributed to a perturbation of the active region, which is related to indium droplets that form on the surface in the metal-rich InGaN growth condition. Specifically, we attribute the blueshift to a decreased growth rate of and indium incorporation in the InGaN quantum wells underneath the droplet which is postulated to be the result of reduced incorporated N species due to increased N2 formation. The location of droplets are correlated with mixed type dislocations for type I defects. Types II through IV are due to screw dislocations, edge dislocations, and dislocation bunching, respectively, and form dark spots due to leakage current and nonradiative recombination.
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    Top-down fabrication of ordered arrays of GaN nanowires by selective area sublimation
    (Cambridge : Royal Society of Chemistry, 2019) Fernández-Garrido, Sergio; Auzelle, Thomas; Lähnemann, Jonas; Wimmer, Kilian; Tahraoui, Abbes; Brandt, Oliver
    We demonstrate the top-down fabrication of ordered arrays of GaN nanowires by selective area sublimation of pre-patterned GaN(0001) layers grown by hydride vapor phase epitaxy on Al2O3. Arrays with nanowire diameters and spacings ranging from 50 to 90 nm and 0.1 to 0.7 µm, respectively, are simultaneously produced under identical conditions. The sublimation process, carried out under high vacuum conditions, is analyzed in situ by reflection high-energy electron diffraction and line-of-sight quadrupole mass spectrometry. During the sublimation process, the GaN(0001) surface vanishes, giving way to the formation of semi-polar {1103} facets which decompose congruently following an Arrhenius temperature dependence with an activation energy of (3.54 ± 0.07) eV and an exponential prefactor of 1.58 × 1031 atoms per cm2 per s. The analysis of the samples by lowerature cathodoluminescence spectroscopy reveals that, in contrast to dry etching, the sublimation process does not introduce nonradiative recombination centers at the nanowire sidewalls. This technique is suitable for the top-down fabrication of a variety of ordered nanostructures, and could possibly be extended to other material systems with similar crystallographic properties such as ZnO. © 2019 The Royal Society of Chemistry.
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    Electroluminescence and current-voltage measurements of single-(In,Ga)N/GaN-nanowire light-emitting diodes in a nanowire ensemble
    (Frankfurt, M. : Beilstein-Institut zur Förderung der Chemischen Wissenschaften, 2019) van Treeck, David; Ledig, Johannes; Scholz, Gregor; Lähnemann, Jonas; Musolino, Mattia; Tahraoui, Abbes; Brandt, Oliver; Waag, Andreas; Riechert, Henning; Geelhaar, Lutz
    We present the combined analysis of electroluminescence (EL) and current-voltage (I-V) behavior of single, freestanding (In,Ga)N/GaN nanowire (NW) light-emitting diodes (LEDs) in an unprocessed, self-assembled ensemble grown by molecular beam epitaxy. The data were acquired in a scanning electron microscope equipped with a micromanipulator and a luminescence detection system. Single NW spectra consist of emission lines originating from different quantum wells, and the width of the spectra increases with decreasing peak emission energy. The corresponding I-V characteristics are described well by a modified Shockley equation. The key advantage of this measurement approach is the possibility to correlate the EL intensity of a single-NW LED with the actual current density in this NW. This way, the external quantum efficiency (EQE) can be investigated as a function of the current in a single-NW LED. The comparison of the EQE characteristic of single NWs and the ensemble device allows for a quite accurate determination of the actual number of emitting NWs in the working ensemble LED and the respective current densities in its individual NWs. This information is decisive for a meaningful and comprehensive characterization of a NW ensemble device, rendering the measurement approach employed here a very powerful analysis tool. © 2019 van Treeck et al.
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    Luminescence of group-III-V nanowires containing heterostructures – the role of polytypism, polarization fields and carrier localization
    (Berlin : Humboldt-Universität zu Berlin, 2013) Lähnemann, Jonas
    In dieser Dissertation wird die spektrale und örtliche Verteilung der Lumineszenz von Heterostrukturen in selbstorganisierten Nanodrähten (ND) mit Hilfe von Kathodolumineszenz-Spektroskopie (KL) im Rasterelektronenmikroskop untersucht. Diese Methode wird ergänzt durch Messungen der kontinuierlichen und zeitaufgelösten Mikro-Photolumineszenz. Drei verschiedene Strukturen werden behandelt: (i) GaAs-ND bestehend aus Segmenten der Wurtzit (WZ) bzw. Zinkblende (ZB) Kristallstrukturen, (ii) auf GaN-ND überwachsene GaN-Mikrokristalle und (iii) (In,Ga)N Einschlüsse in GaN-ND. Die gemischte Kristallstruktur der GaAs-ND führt zu komplexen Emissionsspektren. Dabei wird entweder ausschließlich Lumineszenz bei Energien unterhalb der ZB Bandlücke, oder aber zusätzlich bei höheren Energien, gemessen. Diese Differenz wird durch unterschiedliche Dicken der ZB und WZ Segmente erklärt. Messungen bei Raumtemperatur zeigen, dass die Bandlücke von WZ-GaAs mindestens 55 meV größer als die von ZB-GaAs ist. Die Lumineszenz-Spektren der GaN-Mikrokristalle enthalten verschiedene Emissionslinien, die auf Stapelfehler (SF) zurückzuführen sind. SF sind ZB Quantentöpfe verschiedener Dicke in einem WZ-Kristall und es wird gezeigt, dass ihre Emissionsenergie durch die spontane Polarisation bestimmt wird. Aus einer detaillierten statistischen Analyse der Emissionsenergien der verschiedenen SF-Typen werden Emissionsenergien von 3.42, 3.35 und 3.29 eV für die intrinsischen (I1 und I2) sowie für extrinsische SF ermittelt. Aus den entsprechenden Energiedifferenzen wird -0.022C/m² als experimenteller Wert für die spontane Polarisation von GaN bestimmt. Die Bedeutung sowohl der piezoelektrischen Polarisation als auch die der Lokalisierung von Ladungsträgern wird für (In,Ga)N-Einschlüsse in GaN-ND gezeigt. Hierbei spielt nicht nur die Lokalisierung von Exzitonen, sondern auch die individueller Elektronen und Löcher an unterschiedlichen Potentialminima eine Rolle.