arXiv subjects

Lutz Geelhaar

Publications and source records attributed to Lutz Geelhaar.

At least 19 recordsLinked to original sources

arXiv2026

Two-step growth of (In,Ga)N pseudo-substrates on GaN templates by plasma-assisted molecular beam epitaxy

(In,Ga)N layers are grown by plasma-assisted molecular beam epitaxy on GaN templates. We introduce a two-step protocol that involves switching the growth conditions from initially N-stable to metal-stable. Reflection high-energy electron diffraction as well as scanning electron and atomic force microscopy reveal that the first step results in a rough intermediate surface with open pits, whereas the final surface is smooth. The narrow linewidth of the photoluminescence band indicates an excellent compositional homogeneity of the upper layer. Its in-plane lattice constant is determined to be $\approx$3.26 \AA from X-ray diffraction measurements. This combination of favorable properties makes these layers attractive as pseudo-substrates for the growth of red-emitting (In,Ga)N light-emitting diodes. In particular, the approach presented here does not require any complex external processing and is, thus, scalable and economical.

cond-mat.mtrl-sci↗

arXiv2026

Simultaneously monitoring Ga adsorption and desorption kinetics on GaN(0001) using four in situ techniques

We present a systematic investigation of Ga adsorption and desorption kinetics on the wurtzite GaN(0001) surface using four in situ techniques operated simultaneously: reflection high-energy electron diffraction, laser reflectometry, line-of-sight quadrupole mass spectrometry, and optical pyrometry. Flux- and temperature-dependent experiments are performed for Ga coverages ranging from the submonolayer to the droplet regime. Despite their distinct transient responses, the signals from all four techniques and their trends with surface coverage are quantitatively reproduced by a unified kinetic model of Ga adsorption, diffusion, and desorption. An Arrhenius analysis of the Ga adlayer desorption yields an activation energy of (2.87 $\pm$ 0.04) eV.

physics.app-ph↗

arXiv2026

Molecular Beam Epitaxy of Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N Nanowires: Towards Group-III Nitride Piezoelectric Nanogenerators with Enhanced Response

We study the molecular beam epitaxy of self-assembled Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N nanowires on conductive TiN layers and demonstrate their application in piezoelectric nanogenerators. Wurtzite Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N nanowires with uniform Sc incorporation are grown across a wide composition range (0<x<0.35). At substrate temperatures below 700 $^\circ{}$C, these nanowires exhibit an inversely tapered morphology, whereas higher temperatures favor the nucleation of additional branches due to a phase separation of Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N into wurtzite AlN and rock-salt ScN. Phase-pure Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N nanowires are integrated into vertical nanogenerators, where the metallic TiN substrate serves as bottom electrode. The fabricated polymer-nanowire composite devices achieve effective piezoelectric charge coefficients of up to 8.5 pC N$^{-1}$ at x=0.32, thus exceeding the piezoelectric response of bulk AlN by nearly a factor of two. Although the charge response remains lower compared to Al$\mathrm{_{1-x}}$Sc$\mathrm{_{x}}$N thin films, the reduced effective dielectric permittivity of the nanowire-polymer composites compensates the reduction in piezoelectric charge coefficient, eventually yielding a higher voltage response and comparable energy harvesting efficiency. Finally, effective medium modeling reveals that the device architecture is the primary factor limiting performance, providing general design principles for highly efficient nanowire-based piezoelectric energy harvesters.

cond-mat.mtrl-sci↗

arXiv2025

Fabrication of (In,Ga)N pseudo-substrates by a three-step growth protocol without ex-situ processing

We fabricate (In,Ga)N pseudo-substrates with a total thickness of ~1 um grown on GaN templates using plasma-assisted molecular beam epitaxy. In a three-step process, we change growth conditions from N-rich to metal-rich in order to sequentially form a roughened GaN layer, relaxed (In,Ga)N nanostructures, and a coalesced, smooth (In,Ga)N layer. Samples are analyzed by scanning electron and atomic force microscopy, X-ray diffraction, as well as photo- and cathodoluminescence spectroscopy. Compared to a reference layer grown directly on GaN, the pseudo-substrate exhibits a higher In content (~0.3), strain relaxation degree (~80%), narrower photoluminescence linewidth, and larger area fraction of bright regions in cathodoluminescence maps, showing the benefits of the three-step growth protocol. This straightforward approach does not necessitate any ex-situ processing and could enable the scalable fabrication of (In,Ga)N pseudo-substrates for high-efficiency red-emitting (In,Ga)N devices.

cond-mat.mtrl-sci↗

arXiv2025

Combining metal dewetting and lateral etching for the scalable top-down fabrication of GaN nanowire arrays with independently tunable diameter and spacing

The top-down fabrication of nanowires based on patterning via metal dewetting is a cost-effective and scalable approach that is particularly suited for applications requiring large arrays of nanowires. Advantageously, the nanowire diameter can be tailored by the initial metal film thickness. However, we show here that metal dewetting inherently leads to a coupling between the nanowire diameter and spacing. To overcome this limitation, we introduce two strategies that are exemplified for GaN nanowires: (i) modification of the surface and interface energies within the dewetting system, and (ii) thinning of the nanowires by lateral etching. In the first strategy, GaN(0001), SiOx, and SiNx substrate surfaces are combined with Au, Pt, and Pt-Au alloy dewetting metals to tune the dewetting behavior. The differences in interface energies affect the relation between nanowire diameter and spacing, albeit within a limited range. The second strategy adds a lateral etching step to the conventional top-down nanowire fabrication process. This step at the same time reduces the nanowire diameter and increases the spacing, thus enabling combinations beyond the constraints of metal dewetting alone. When in addition different initial nanowire diameters are employed, it is possible to independently control diameter and spacing over a substantially extended range. Therefore, the inherent limitation of conventional dewetting-based patterning approaches for the top-down fabrication of nanowires is overcome.

physics.app-ph↗

arXiv2025

Diameter dependence of light absorption in GaAs nanowires evidenced by photoluminescence spectroscopy

Semiconductor nanowires are attractive for photovoltaic applications because light absorption can be enhanced compared to planar layers due to the more complex coupling of light with wavelength-scale matter. However, experimentally it is very challenging to investigate light absorption in single nanowires. Here, we employ photoluminescence spectroscopy as a new method to investigate how the diameter of highly phase-pure GaAs nanowires affects light absorption. The underlying concept is that the absorption of the exciting laser light influences the photogenerated carrier density and in turn spectral features. In particular, we exploit that both the saturation of a specific defect line and the transition from excitonic to electron-hole-plasma recombination occur at well-defined carrier densities. We find that absorption is maximized for a diameter of about 80\,nm. Our approach may be transferred to other material systems and thus enables systematic experimental studies of absorption enhancement in single nanowires.

physics.app-ph↗

arXiv2024

Growth of compositionally uniform $\mathrm{In}_{x}\mathrm{Ga}_{1-x}\mathrm{N}$ layers with low relaxation degree on GaN by molecular beam epitaxy

500-nm-thick $\mathrm{In}_{x}\mathrm{Ga}_{1-x}\mathrm{N}$ layers with $x=$ 0.05-0.14 are grown using plasma-assisted molecular beam epitaxy, and their properties are assessed by a comprehensive analysis involving x-ray diffraction, secondary ion mass spectrometry, and cathodoluminescence as well as photoluminescence spectroscopy. We demonstrate low degrees of strain relaxation (10% for $x=0.12$), low threading dislocation densities ($\mathrm{1\times10^{9}\,cm^{-2}}$ for $x=0.12$), uniform composition both in the growth and lateral direction, and a narrow emission band. The unique sum of excellent materials properties make these layers an attractive basis for the top-down fabrication of ternary nanowires.

cond-mat.mtrl-sci↗

arXiv2024

Uniform large-area surface patterning achieved by metal dewetting for the top-down fabrication of GaN nanowire ensembles

The dewetting of thin Pt films on different surfaces is investigated as a means to provide the patterning for the top-down fabrication of GaN nanowire ensembles. The transformation from a thin film to an ensemble of nanoislands upon annealing proceeds in good agreement with the void growth model. With increasing annealing duration, the size and shape uniformity of the nanoislands improves. This improvement speeds up for higher annealing temperature. After an optimum annealing duration, the size uniformity deteriorates due to the coalescence of neighboring islands. By changing the Pt film thickness, the nanoisland diameter and density can be quantitatively controlled in a way predicted by a simple thermodynamic model. We demonstrate the uniformity of the nanoisland ensembles for an area larger than 1 cm$^2$. GaN nanowires are fabricated by a sequence of dry and wet etching steps, and these nanowires inherit the diameters and density of the Pt nanoisland ensemble used as a mask. Our study achieves advancements in size uniformity and range of obtainable diameters compared to previous works. This simple, economical, and scalable approach to the top-down fabrication of nanowires is useful for applications requiring large and uniform nanowire ensembles with controllable dimensions.

cond-mat.mtrl-sci↗

arXiv2024

ScN/GaN($1\bar{1}00$): a new platform for the epitaxy of twin-free metal-semiconductor heterostructures

We study the molecular beam epitaxy of rock-salt ScN on the wurtzite GaN($1\bar{1}00$) surface. To this end, ScN is grown on free-standing GaN($1\bar{1}00$) substrates and self-assembled GaN nanowires that exhibit ($1\bar{1}00$) sidewalls. On both substrates, ScN crystallizes twin-free thanks to a specific epitaxial relationship, namely ScN(110)[001]$||$GaN($1\bar{1}00$)[0001], providing a congruent, low-symmetry GaN/ScN interface. The 13.1 % uniaxial lattice mismatch occurring in this orientation mostly relaxes within the first few monolayers of growth by forming a coincidence site lattice, where 7 GaN planes coincide with 8 ScN planes, leaving the ScN surface nearly free of extended defects. Overgrowth of the ScN with GaN leads to a kinetic stabilization of the zinc blende phase, that rapidly develops wurtzite inclusions nucleating on {111} nanofacets, commonly observed during zinc blende GaN growth. Our ScN/GaN($1\bar{1}00$) platform opens a new route for the epitaxy of twin-free metal-semiconductor heterostructures made of closely lattice-matched GaN, ScN, HfN and ZrN compounds.

cond-mat.mtrl-sci↗

arXiv2024

Growth kinetics and substrate stability during high-temperature molecular beam epitaxy of AlN nanowires

We study the molecular beam epitaxy of AlN nanowires between 950 and 1215 °C, well above the usual growth temperatures, to identify optimal growth conditions. The nanowires are grown by self-assembly on TiN(111) films sputtered onto Al$_2$O$_3$. Above 1100 °C, the TiN film is seen to undergo grain growth and its surface exhibits {111} facets where AlN nucleation preferentially occurs. Modelling of the nanowire elongation rate measured at different temperatures shows that the Al adatom diffusion length is maximised at 1150 °C, which appears to be the optimum growth temperature. However, analysis of the nanowire luminescence shows a steep increase in the deep-level signal already above 1050 °C, associated with O incorporation from the Al$_2$O$_3$ substrate. Comparison with AlN nanowires grown on Si, MgO and SiC substrates suggests that heavy doping of Si and O by interdiffusion from the TiN/substrate interface increases the nanowire internal quantum efficiency, presumably due to the formation of a SiN$_x$ or AlO$_x$ passivation shell. The outdiffusion of Si and O would also cause the formation of the inversion domains observed in the nanowires. It follows that for optoelectronic and piezoelectric applications, optimal AlN nanowire ensembles should be prepared at 1150 °C on TiN/SiC substrates and will require an ex situ surface passivation.

cond-mat.mtrl-sci↗

arXiv2024

Observation of dielectrically confined excitons in ultrathin GaN nanowires up to room temperature

The realization of semiconductor structures with stable excitons at room temperature is crucial for the development of excitonics and polaritonics. Quantum confinement has commonly been employed for enhancing excitonic effects in semiconductor heterostructures. Dielectric confinement, which is potentially much stronger, has proven to be more difficult to achieve because of the rapid nonradiative surface/interface recombination in hybrid dielectric-semiconductor structures. Here, we demonstrate intense excitonic emission from bare GaN nanowires with diameters down to 6 nm. The large dielectric mismatch between the nanowires and vacuum greatly enhances the Coulomb interaction, with the thinnest nanowires showing the strongest dielectric confinement and the highest radiative efficiency at room temperature. In situ monitoring of the fabrication of these structures allows one to accurately control the degree of dielectric enhancement. These ultrathin nanowires may constitute the basis for the fabrication of advanced low-dimensional structures with an unprecedented degree of confinement.

cond-mat.mes-hall↗

arXiv2024

Molecular Beam Epitaxy of GaN Nanowires on Epitaxial Graphene

We demonstrate an all-epitaxial and scalable growth approach to fabricate single-crystalline GaN nanowires on graphene by plasma-assisted molecular beam epitaxy. As substrate, we explore several types of epitaxial graphene layer structures synthesized on SiC. The different structures differ mainly in their total number of graphene layers. Because graphene is found to be etched under active N exposure, the direct growth of GaN nanowires on graphene is only achieved on multilayer graphene structures. The analysis of the nanowire ensembles prepared on multilayer graphene by Raman spectroscopy and transmission electron microscopy reveals the presence of graphene underneath as well as in between nanowires, as desired for the use of this material as contact layer in nanowire-based devices. The nanowires nucleate preferentially at step edges, are vertical, well aligned, epitaxial, and of comparable structural quality as similar structures fabricated on conventional substrates.

cond-mat.mtrl-sci↗

arXiv2024

Spontaneous nucleation and growth of GaN nanowires: Fundamental role of crystal polarity

We experimentally investigate whether crystal polarity affects the growth of GaN nanowires in plasma-assisted molecular beam epitaxy and whether their formation has to be induced by defects. For this purpose, we prepare smooth and coherently strained AlN layers on 6H-SiC(0001) and SiC(000$\bar{1}$) substrates to ensure a well-defined polarity and an absence of structural and morphological defects. On N-polar AlN, a homogeneous and dense N-polar GaN nanowire array forms, evidencing that GaN nanowires form spontaneously in the absence of defects. On Al-polar AlN, we do not observe the formation of Ga-polar GaN NWs. Instead, sparse N-polar GaN nanowires grow embedded in a Ga-polar GaN layer. These N-polar GaN nanowires are shown to be accidental in that the necessary polarity inversion is induced by the formation of Si$_{x}$N. The present findings thus demonstrate that spontaneously formed GaN nanowires are irrevocably N-polar. Due to the strong impact of the polarity on the properties of GaN-based devices, these results are not only essential to understand the spontaneous formation of GaN nanowires but also of high technological relevance.

cond-mat.mtrl-sci↗

arXiv2024

Self-regulated radius of spontaneously formed GaN nanowires in molecular beam epitaxy

We investigate the axial and radial growth of GaN nanowires upon a variation of the Ga flux during molecular beam epitaxial growth. An increase in the Ga flux promotes radial growth without affecting the axial growth rate. In contrast, a decrease in the Ga flux reduces the axial growth rate without any change in the radius. These results are explained by a kinetic growth model that accounts for both the diffusion of Ga adatoms along the side facets towards the nanowire tip and the finite amount of active N available for the growth. The model explains the formation of a new equilibrium nanowire radius after increasing the Ga flux and provides an explanation for two well known but so far not understood experimental facts: the necessity of effectively N-rich conditions for the spontaneous growth of GaN nanowires and the increase in nanowire radius with increasing III/V flux ratios.

cond-mat.mtrl-sci↗

arXiv2024

Monitoring the formation of nanowires by line-of-sight quadrupole mass spectrometry: a comprehensive description of the temporal evolution of GaN nanowire ensembles

We use line-of-sight quadrupole mass spectrometry to monitor the spontaneous formation of GaN nanowires on Si during molecular beam epitaxy. We find that the temporal evolution of nanowire ensembles is well described by a double logistic function. The analysis of the temporal evolution of nanowire ensembles prepared under a wide variety of growth conditions allows us to construct a growth diagram which can be used to predict the average delay time that precedes nanowire formation.

cond-mat.mtrl-sci↗

arXiv2024

Polarity-induced selective area epitaxy of GaN nanowires

We present a conceptually novel approach to achieve selective area epitaxy of GaN nanowires. The approach is based on the fact that these nanostructures do not form in plasma-assisted molecular beam epitaxy on structurally and chemically uniform cation-polar substrates. By in situ depositing and nitridating Si on a Ga-polar GaN film, we locally reverse the polarity to induce the selective area epitaxy of N-polar GaN nanowires. We show that the nanowire number density can be controlled over several orders of magnitude by varying the amount of pre-deposited Si. Using this growth approach, we demonstrate the synthesis of single-crystalline and uncoalesced nanowires with diameters as small as 20 nm. The achievement of nanowire number densities low enough to prevent the shadowing of the nanowire sidewalls from the impinging fluxes paves the way for the realization of homogeneous core-shell heterostructures without the need of using ex situ pre-patterned substrates.

physics.app-ph↗

arXiv2023

Composition and optical properties of (In,Ga)As nanowires grown by group-III-assisted molecular beam epitaxy

(In,Ga) alloy droplets are used to catalyse the growth of (In,Ga)As nanowires by molecular beam epitaxy on Si(111) substrates. The composition, morphology and optical properties of these nanowires can be tuned by the employed elemental fluxes. To incorporate more than 10% of In, a high In/(In+Ga) flux ratio above 0.7 is required. We report a maximum In content of almost 30% in bulk (In,Ga)As nanowires for an In/(In+Ga) flux ratio of 0.8. However, with increasing In/(In+Ga) fl ux ratio, the nanowire length and diameter are notably reduced. Using photoluminescence and cathodoluminescence spectroscopy on nanowires covered by a passivating (In,Al)As shell, two luminescence bands are observed. A significant segment of the nanowires shows homogeneous emission, with a wavelength corresponding to the In content in this segment, while the consumption of the catalyst droplet leads to a spectrally-shifted emission band at the top of the nanowires. The (In,Ga)As nanowires studied in this work provide a new approach for the integration of infrared emitters on Si platforms.

cond-mat.mtrl-sci↗

arXiv2023

Sequential directional deposition of one-sided (In,Ga)N shells on GaN nanowires by molecular beam epitaxy

Capitalizing on the directed nature of the atomic fluxes in molecular beam epitaxy, we propose and demonstrate the sequential directional deposition of lateral (In,Ga)N shells on GaN nanowires. In this approach, a sub-monolayer thickness of each constituent atomic species, i.e. Ga, In, and N, is deposited subsequently from the same direction by rotating the sample and operating the shutters accordingly. Using multiple iterations of this process, we achieve the growth of homogeneous shells on a single side facet of the nanowires. For higher In content and thus lattice mismatch, we observe a strain-induced bending of the nanowire heterostructures. The incorporation of In and the resulting emission spectra are systematically investigated as a function of both the growth temperature and the In/Ga flux ratio.

cond-mat.mtrl-sci↗