arXiv subjects

Lutz Geelhaar

Publications and source records attributed to Lutz Geelhaar.

At least 37 records · Page 2Linked to original sources

arXiv2023

Growth mechanisms in molecular beam epitaxy for GaN-(In,Ga)N core-shell nanowires emitting in the green spectral range

Using molecular beam epitaxy, we demonstrate the growth of (In,Ga)N shells emitting in the green spectral range around very thin (35 nm diameter) GaN core nanowires. These GaN nanowires are obtained by self-assembled growth on TiN. We present a qualitative shell growth model accounting for both the three-dimensional nature of the nanostructures as well as the directionality of the atomic fluxes. This model allows us, on the one hand, to optimise the conditions for high and homogeneous In incorporation and, on the other hand, to explain the influence of changes in the growth conditions on the sample morphology and In content. Specifically, the impact of the V/III and In/Ga flux ratios, the rotation speed and the rotation direction are investigated. Notably, with In acting as surfactant, the ternary (In,Ga)N shells are much more homogeneous in thickness along the NW length than their binary GaN counterparts.

cond-mat.mtrl-sci↗

arXiv2023

Density control of GaN nanowires at the wafer scale using self-assembled SiN$_x$ patches on sputtered TiN(111)

The self-assembly of heteroepitaxial GaN nanowires using either molecular beam epitaxy (MBE) or metal-organic vapor phase epitaxy (MOVPE) mostly results in wafer-scale ensembles with ultrahigh ($>10$ $μ$m$^{-2}$) or ultralow ($<1$ $μ$m$^{-2}$) densities, respectively. A simple means to tune the density of well-developed nanowire ensembles between these two extremes is generally lacking. Here, we examine the self-assembly of SiN$_x$ patches on TiN(111) substrates which are eventually acting as seeds for the growth of GaN nanowires. We first found that if prepared by reactive sputtering, the TiN surface is characterized by \{100\} facets for which the GaN incubation time is extremely long. Fast GaN nucleation is only obtained after deposition of a sub-monolayer of SiN$_x$ atoms prior to the GaN growth. By varying the amount of pre-deposited SiN$_x$, the GaN nanowire density could be tuned by three orders of magnitude with excellent uniformity over the entire wafer, bridging the density regimes conventionally attainable by direct self-assembly with MBE or MOVPE. The analysis of the nanowire morphology agrees with a nucleation of the GaN nanowires on nanometric SiN$_x$ patches. The photoluminescence analysis of single freestanding GaN nanowires reveals a band edge luminescence dominated by excitonic transitions that are broad and blue shifted compared to bulk GaN, an effect that is related to the small nanowire diameter and to the presence of a thick native oxide. The approach developed here can be principally used for tuning the density of most III-V semiconductors nucleus grown on inert surfaces like 2D materials.

cond-mat.mtrl-sci↗

arXiv2023

Lattice parameters of Sc$_{\boldsymbol{\mathsf{x}}}$Al$_{\boldsymbol{\mathsf{1-x}}}$N layers grown on GaN(0001) by plasma-assisted molecular beam epitaxy

An accurate knowledge of the lattice parameters of the new nitride Sc$_\textit{x}$Al$_\textit{1-x}$N is essential for understanding the elastic and piezoelectric properties of this compound as well as for the ability to engineer its strain state in heterostructures. Using high-resolution x-ray diffractometry, we determine the lattice parameters of 100-nm-thick undoped Sc$_\textit{x}$Al$_\textit{1-x}$N layers grown on GaN(0001) templates by plasma-assisted molecular beam epitaxy. The Sc content $\textit{x}$ of the layers is measured independently by both x-ray photoelectron spectroscopy and energy-dispersive x-ray spectroscopy and ranges from 0 to 0.25. The in-plane lattice parameter of the layers linearly increases with increasing $\textit{x}$, while their out-of-plane lattice parameter remains constant. Layers with $\textit{x}$ $\approx$ 0.09 are found to be lattice matched to GaN, resulting in a smooth surface and a structural perfection equivalent to that of the GaN underlayer. In addition, a two-dimensional electron gas is induced at the Sc$_\textit{x}$Al$_\textit{1-x}$N/GaN heterointerface, with the highest sheet electron density and mobility observed for lattice-matched conditions.

cond-mat.mtrl-sci↗

arXiv2023

Bismuth surfactant-enhanced III-As epitaxy on GaAs(111)A

Quantum dot (QD) growth on high ($c_{3v}$) symmetry GaAs{111} surfaces holds promise for efficient entangled photon sources. Unfortunately, homoepitaxy on GaAs{111} surfaces suffers from surface roughness/defects and InAs deposition does not natively support Stranski-Krastanov (SK) QD growth. Surfactants have been identified as effective tools to alter the epitaxial growth process of III-V materials, however, their use remains unexplored on GaAs{111}. Here, we investigate Bi as a surfactant in III-As molecular beam epitaxy (MBE) on GaAs(111)A substrates, demonstrating that Bi can eliminate surface defects/hillocks in GaAs and (Al,Ga)As layers, yielding atomically-smooth hillock-free surfaces with RMS roughness values as low as 0.13 nm. Increasing Bi fluxes are found to result in smoother surfaces and Bi is observed to increase adatom diffusion. The Bi surfactant is also shown to trigger a morphological transition in InAs/GaAs(111)A films, directing the 2D InAs layer to rearrange into 3D nanostructures, which are promising candidates for high-symmetry quantum dots. The desorption activation energy ($U_{Des}$) of Bi on GaAs(111)A was measured by reflection high energy electron diffraction (RHEED), yielding $U_{Des}$ = 1.7 $\pm$ 0.4 eV. These results illustrate the potential of Bi surfactants on GaAs(111)A and will help pave the way for GaAs(111)A as a platform for technological applications including quantum photonics.

cond-mat.mtrl-sci↗

arXiv2022

Carrier Recombination in Highly Uniform and Phase-Pure GaAs/(Al,Ga)As Core/Shell Nanowire Arrays on Si(111): Mott Transition and Internal Quantum Efficiency

GaAs-based nanowires are among the most promising candidates for realizing a monolithical integration of III-V optoelectronics on the Si platform. To realize their full potential for applications as light absorbers and emitters, it is crucial to understand their interaction with light governing the absorption and extraction efficiency, as well as the carrier recombination dynamics determining the radiative efficiency. Here, we study the spontaneous emission of zincblende GaAs/(Al,Ga)As core/shell nanowire arrays by $μ$-photoluminescence spectroscopy. These ordered arrays are synthesized on patterned Si(111) substrates using molecular beam epitaxy, and exhibit an exceptionally low degree of polytypism for interwire separations exceeding a critical value. We record emission spectra over more than five orders of excitation density for both steady-state and pulsed excitation to identify the nature of the recombination channels. An abrupt Mott transition from excitonic to electron-hole-plasma recombination is observed, and the corresponding Mott density is derived. Combining these experiments with simulations and additional direct measurements of the external quantum efficiency using a perfect diffuse reflector as reference, we are able to extract the internal quantum efficiency as a function of carrier density and temperature as well as the extraction efficiency of the nanowire array. The results vividly document the high potential of GaAs/(Al,Ga)As core/shell nanowires for efficient light emitters integrated on the Si platform. Furthermore, the methodology established in this work can be applied to nanowires of any other materials system of interest for optoelectronic applications.

cond-mat.mtrl-sci↗

arXiv2022

A route for the top-down fabrication of ordered ultrathin GaN nanowires

Ultrathin GaN nanowires (NWs) are attractive to maximize surface effects and as building block in high-frequency transistors. Here, we introduce a facile route for the top-down fabrication of ordered arrays of GaN NWs with aspect ratios exceeding $10$ and diameters below $20\,$nm. Highly uniform thin GaN NWs are first obtained by using electron beam lithography to pattern a Ni/SiN$_x$ hard mask, followed by dry etching and wet etching in hot KOH. The SiN$_x$ is found to work as an etch stop during wet etching in hot KOH. Arrays with NW diameters down to $(33 \pm5)\,$nm can be achieved with a yield exceeding $99.9\,\%$. Further reduction of the NW diameter down to $5\,$nm is obtained by applying digital etching which consists in plasma oxidation followed by wet etching in hot KOH. The NW radial etching depth is tuned by varying the RF power during plasma oxidation. NW breaking or bundling is observed for diameters below $\approx 20\,$nm, an effect that is associated to capillary forces acting on the NWs during sample drying in air. This effect can be principally mitigated using critical point dryers. Interestingly, this mechanical instability of the NWs is found to occur at much smaller aspect ratios than what is predicted for models dealing with macroscopic elastic rods. Explicit calculations of buckling states show an improved agreement when considering an inclined water surface, as can be expected if water assembles into droplets. The proposed fabrication route can be principally applied to any GaN/SiN$_{x}$ nanostructures and allows regrowth after removal of the SiN$_{x}$ mask.

cond-mat.mtrl-sci↗

arXiv2022

Exploiting of flux shadowing effect on In$_{x}$Ga$_{1-x}$As asymmetric shell growth for strain and bending engineering in GaAs - In$_{x}$Ga$_{1-x}$As core - shell NW arrays

Here we report on non-uniform shell growth of In(x)Ga(1-x)As onto GaAs nanowire (NW) core by molecular beam epitaxy (MBE). The growth was realized on pre-patterned silicon substrates with pitch size (p) ranging from 0.1 um to 10 um. Considering the preferable bending direction with respect to the MBE cells as well as the layout of the substrate pattern, we are able to modify the strain distribution along the NW growth axis and the subsequent bending profile. For NW arrays with high number density, the obtained bending profile of the NWs is composed of straight (barely-strained) and bent (strained) segments with different lengths which depend on the pitch size. A precise control of the bent and straight NW segment length provides a recipe to design NW based devices with length selective strain distribution.

physics.ins-det↗

arXiv2021

Drastic effect of sequential deposition resulting from flux directionality on the luminescence efficiency of nanowire shells

Core-shell nanowire heterostructures form the basis for many innovative devices. When compound nanowire shells are grown by directional deposition techniques, the azimuthal position of the sources for the different constituents in the growth reactor, substrate rotation, and nanowire self-shadowing inevitably lead to sequential deposition. Here, we uncover for In$_{0.15}$Ga$_{0.85}$As/GaAs shell quantum wells grown by molecular beam epitaxy a drastic impact of this sequentiality on the luminescence efficiency. The photoluminescence intensity of shell quantum wells grown with a flux sequence corresponding to migration enhanced epitaxy, i. e. when As and the group-III metals essentially do not impinge at the same time, is more than two orders of magnitude higher than for shell quantum wells prepared with substantially overlapping fluxes. Transmission electron microscopy does not reveal any extended defects explaining this difference. Our analysis of photoluminescence transients shows that co-deposition has two detrimental microscopic effects. First, a higher density of electrically active point defects leads to internal electric fields reducing the electron-hole wave function overlap. Second, more point defects form that act as nonradiative recombination centers. Our study demonstrates that the source arrangement of the growth reactor, which is of mere technical relevance for planar structures, can have drastic consequences for the materials properties of nanowire shells. We expect that this finding holds also for other alloy nanowire shells.

cond-mat.mtrl-sci↗

arXiv2021

In-situ X-ray analysis of misfit strain and curvature of bent polytypic GaAs-In(x)Ga(1-x)As core-shell nanowires

Misfit strain in core-shell nanowires can be elastically released by nanowire bending in case of asymmetric shell growth around the nanowire core. In this work, we investigate the bending of GaAs nanowires during the asymmetric overgrowth by an In(x)Ga(1-x)As shell caused by avoiding substrate rotation. We observe that the nanowire bending direction depends on the nature of the substrate's oxide layer, demonstrated by Si substrates covered by native and thermal oxide layers. Further, we follow the bending evolution by time-resolved in-situ X-ray diffraction measurements during the deposition of the asymmetric shell. The XRD measurements give insight into the temporal development of the strain as well as the bending evolution in the core-shell nanowire.

physics.ins-det↗

arXiv2020

Beam damage of single semiconductor nanowires during X-ray nano beam diffraction experiments

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, we compare 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 3rd generation source PETRA III. Using an incident X-ray beam energy of 9 keV and photon flux of 10$^{10}$s$^{-1}$, the axial lattice parameter and tilt of individual GaAs/In$_{0.2}$Ga$_{0.8}$As/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 are 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 to 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.

cond-mat.mtrl-sci↗

arXiv2020

Spatially-resolved luminescence and crystal structure of single core-shell nanowires measured in the as-grown geometry

We report on the direct correlation between the structural and optical properties of single, as-grown core-multi-shell GaAs/In$_{0.15}$Ga$_{0.85}$As/GaAs/AlAs/GaAs nanowires. Fabricated by molecular beam epitaxy on a pre-patterned Si(111) substrate, on a row of well separated nucleation sites, it was possible to access individual nanowires in the as-grown geometry. The polytype distribution along the growth axis of the nanowires was revealed by synchrotron-based nanoprobe X-ray diffraction techniques monitoring the axial 111 Bragg reflection. For the same nanowires, the spatially-resolved emission properties were obtained by cathodoluminescence hyperspectral linescans in a scanning electron microscope. Correlating both measurements, we reveal a blueshift of the shell quantum well emission energy combined with an increased emission intensity for segments exhibiting a mixed structure of alternating wurtzite and zincblende stacking compared with the pure crystal polytypes. The presence of this mixed structure was independently confirmed by cross-sectional transmission electron microscopy.

cond-mat.mes-hall↗

arXiv2019

Coaxial GaAs/(In,Ga)As dot-in-a-well nanowire heterostructures for electrically driven infrared light generation on Si in the telecommunication O band

Core-shell GaAs-based nanowires monolithically integrated on Si constitute a promising class of nanostructures that could enable light emitters for fast inter- and intrachip optical connections. We introduce and fabricate a novel coaxial GaAs/(In,Ga)As dot-in-a-well nanowire heterostructure to reach spontaneous emission in the Si transparent region, which is crucial for applications in Si photonics. Specifically, we achieve room temperature emission at 1.27 $μ$m in the telecommunication O band. The presence of quantum dots in the heterostructure is evidenced by a structural analysis based on scanning transmission electron microscopy. The spontaneous emission of these nanowire structures is investigated by cathodoluminescence and photoluminescence spectroscopy. Thermal redistribution of charge carriers to larger quantum dots explains the long wavelength emission achieved at room temperature. Finally, in order to demonstrate the feasibility of the presented nanowire heterostructures as electrically driven light emitters monolithically integrated on Si, a light emitting diode is fabricated exhibiting room-temperature electroluminescence at 1.26 $μ$m.

cond-mat.mtrl-sci↗

arXiv2019

Influence of the source arrangement on shell growth around GaN nanowires in molecular beam epitaxy

In a combined experimental and theoretical study, we investigate the influence of the material source arrangement in a molecular beam epitaxy (MBE) system on the growth of nanowire (NW) core-shell structures. In particular, we study the shell growth of GaN around GaN template NWs under the boundary condition that Ga and N do not impinge on a given sidewall facet at the same time. Our experiments with different V/III ratios and substrate temperatures show that obtaining shells with homogeneous thickness along the whole NW length is not straightforward. Analyzing in detail the shell morphology with and without substrate rotation, we find that the different azimuthal angles of the sources have a major impact on the Ga adatom kinetics and the final shell morphology. On the basis of these experimental results, we develop a diffusion model which takes into account different NW facets and the substrate. The model allows to describe well the experimental shell profiles and predicts that homogeneous shell growth can be achieved if the Ga and N source are arranged next to each other or for very high rotation speeds. Moreover, the modeling reveals that the growth on a given side facet can be categorized within one rotation in four different phases: the Ga wetting phase, the metal-rich growth phase, the N-rich growth phase, and the dissociation phase. The striking difference to growth processes on planar samples is that, in our case, diffusion takes place between different regions, i.e. the sidewall vs. the top facet and substrate, out of which on one N impinges not continuously, resulting in complex gradients in chemical potential that are modulated in time by substrate rotation. The comprehensiveness of our model provides a deep understanding of diffusion processes and the resulting adatom concentration, and could be applied to other 3D structures and material systems

physics.app-ph↗

arXiv2019

Self-assembly of well-separated AlN nanowires directly on sputtered metallic TiN films

We demonstrate the self-assembled formation of AlN nanowires by molecular beam epitaxy on sputtered TiN films on sapphire. This choice of substrate allows growth at an exceptionally high temperature of 1180 °C. In contrast to previous reports, the nanowires are well separated and do not suffer from pronounced coalescence. This achievement is explained by sufficient Al adatom diffusion on the substrate and the nanowire sidewalls. The high crystalline quality of the nanowires is evidenced by the observation of near band edge emission in the cathodoluminescence spectrum. The key factor for the low nanowire coalescence is the TiN film, which spectroscopic ellipsometry and Raman spectroscopy indicate to be stoichiometric. Its metallic nature will be beneficial for optoelectronic devices employing these nanowires as the basis for (Al,Ga)N/AlN heterostructures emitting in the deep ultraviolet spectral range.

cond-mat.mtrl-sci↗

arXiv2019

Electroluminescence and current-voltage measurements of single (In,Ga)N/GaN nanowire light-emitting diodes in the nanowire ensemble

We present the combined analysis of the electroluminescence (EL) as well as the 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 the 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 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.

physics.app-ph↗

arXiv2019

Correlated nanoscale analysis of the emission from wurtzite versus zincblende (In,Ga)As/GaAs nanowire core-shell quantum wells

While the properties of wurtzite GaAs have been extensively studied during the past decade, little is known about the influence of the crystal polytype on ternary (In,Ga)As quantum well structures. We address this question with a unique combination of correlated, spatially-resolved measurement techniques on core-shell nanowires that contain extended segments of both the zincblende and wurtzite polytypes. Cathodoluminescence hyperspectral imaging reveals a blueshift of the quantum well emission energy by $75\pm15$ meV in the wurtzite polytype segment. Nanoprobe x-ray diffraction and atom probe tomography enable $\mathbf{k}\cdot\mathbf{p}$ calculations for the specific sample geometry to reveal two comparable contributions to this shift. First, there is a 30% drop in In mole fraction going from the zincblende to the wurtzite segment. Second, the quantum well is under compressive strain, which has a much stronger impact on the hole ground state in the wurtzite than in the zincblende segment. Our results highlight the role of the crystal structure in tuning the emission of (In,Ga)As quantum wells and pave the way to exploit the possibilities of three-dimensional bandgap engineering in core-shell nanowire heterostructures. At the same time, we have demonstrated an advanced characterization toolkit for the investigation of semiconductor nanostructures.

cond-mat.mes-hall↗

arXiv2019

Analysis of incubation time preceding the Ga-assisted nucleation and growth of GaAs nanowires on Si(111)

The incubation time preceding nucleation and growth of surface nanostructures is interesting from a fundamental viewpoint but also of practical relevance as it determines statistical properties of nanostructure ensembles such as size homogeneity. Using in situ reflection high-energy electron diffraction, we accurately deduce the incubation times for Ga-assisted GaAs nanowires grown on unpatterned Si(111) substrates by molecular beam epitaxy under different conditions. We develop a nucleation model that explains and fits very well the data. We find that, for a given temperature and Ga flux, the incubation time always increases with decreasing As flux and becomes infinite at a certain minimum flux, which is larger for higher temperature. For given As and Ga fluxes, the incubation time always increases with temperature and rapidly tends to infinity above 640 °C under typical conditions. The strong temperature dependence of the incubation time is reflected in a similar variation of the nanowire number density with temperature. Our analysis provides understanding and guidance for choosing appropriate growth conditions that avoid unnecessary material consumption, long nucleation delays, and highly inhomogeneous ensembles of nanowires. On a more general ground, the existence of a minimum flux and maximum temperature for growing surface nanostructures should be a general phenomenon pertaining for a wide range of material-substrate combinations.

cond-mat.mtrl-sci↗

arXiv2019

Bismuth-surfactant-induced growth and structure of InAs/GaAs(110) quantum dots

We explore the Bi-surfactant-directed self-assembly and structure of InAs quantum dots grown on GaAs(110) by molecular beam epitaxy. The addition of a Bi flux during InAs deposition changes the InAs growth mode from two-dimensional (2D) Frank-van der Merwe to Stranski-Krastanov, resulting in the formation of three-dimensional (3D) InAs islands on the surface. Furthermore, exposing static InAs 2D layers to Bi induces a rearrangement of the strained layer into 3D islands. We explore the effect of varying the InAs thickness and Bi flux for these two growth approaches, observing a critical thickness for 3D island formation in both cases. Characterization of (110) InAs quantum dots with high-resolution transmission electron microscopy reveals that larger islands grown by the Stranski-Krastanov mode are plastically relaxed, while small islands grown by the on-demand approach are coherent. Strain relaxation along the [1-10] direction is achieved by 90 degree pure-edge dislocations with dislocation lines running along [001]. In contrast, strain relief along [001] is by 60 degree misfit dislocations. This behaviour is consistent with observations of planar (In,Ga)As/GaAs(110) layers. These results illustrate how surfactant Bi can provoke and control quantum dot formation where it normally does not occur.

cond-mat.mtrl-sci↗