arXiv subjects

Lutz Geelhaar

Publications and source records attributed to Lutz Geelhaar.

At least 55 records · Page 3Linked to original sources

arXiv2019

Axial GaAs/Ga(As,Bi) Nanowire Heterostructures

Bi-containing III-V semiconductors constitute an exciting class of metastable compounds with wide-ranging potential optoelectronic and electronic applications. However, the growth of III-V-Bi alloys requires group-III-rich growth conditions, which pose severe challenges for planar growth. In this work, we exploit the naturally-Ga-rich environment present inside the metallic droplet of a self-catalyzed GaAs nanowire to synthesize metastable GaAs/GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ axial nanowire heterostructures with high Bi contents. The axial GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ segments are realized with molecular beam epitaxy by first enriching only the vapor-liquid-solid (VLS) Ga droplets with Bi, followed by exposing the resulting Ga-Bi droplets to As$_2$ at temperatures ranging from 270 to 380$\,^{\circ}$C to precipitate GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ only under the nanowire droplets. Microstructural and elemental characterization reveals the presence of single crystal zincblende GaAs$_{1-\text{x}}$Bi$_{\text{x}}$ axial nanowire segments with Bi contents up to (10$\pm$2)$\%$. This work illustrates how the unique local growth environment present during the VLS nanowire growth can be exploited to synthesize heterostructures with metastable compounds.

cond-mat.mtrl-sci↗

arXiv2018

Optimization of ohmic contacts to n-type GaAs nanowires

III-V nanowires are comprehensively studied because of their suitability for optoelectronic quantum technology applications. However, their small dimensions and the spatial separation of carriers from the wire surface render electrical contacting difficult. Systematically studying ohmic contact formation by diffusion to $n$-doped GaAs nanowires, we provide a set of optimal annealing parameters for Pd/Ge/Au ohmic contacts. We reproducibly achieve low specific contact resistances of $\sim2\times10^{-7}\,Ω\text{cm}^2$ at room temperature becoming an order of magnitude higher at $T\simeq4.2\,$K. We provide a phenomenological model to describe contact resistances as a function of diffusion parameters. Implementing a transfer-matrix method, we numerically study the influence of the Schottky barrier on the contact resistance. Our results indicate that contact resistances can be predicted using various barrier shapes but further insights into structural properties would require a full microscopic understanding of the complex diffusion processes.

cond-mat.mes-hall↗

arXiv2018

Self-Assembled formation of long, thin, and uncoalesced GaN nanowires on crystalline TiN films

We investigate in detail the self-assembled nucleation and growth of GaN nanowires by molecular beam epitaxy on crystalline TiN films. We demonstrate that this type of substrate allows the growth of long and thin GaN nanowires that do not suffer from coalescence, which is in contrast to the growth on Si and other substrates. Only beyond a certain nanowire length that depends on the nanowire number density and exceeds here 1.5 μm, coalescence takes place by bundling, i.e. the same process as on Si. By analyzing the nearest neighbor distance distribution, we identify diffusion-induced repulsion of neighboring nanowires as the main mechanism limiting the nanowire number density during nucleation on TiN. Since on Si the final number density is determined by shadowing of the impinging molecular beams by existing nanowires, it is the difference in adatom surface diffusion that enables on TiN the formation of nanowire ensembles with reduced number density. These nanowire ensembles combine properties that make them a promising basis for the growth of core-shell heterostructures.

cond-mat.mtrl-sci↗

arXiv2017

Quenching of the luminescence intensity of GaN nanowires under electron beam exposure: Impact of C adsorption on the exciton lifetime

Electron irradiation of GaN nanowires in a scanning electron microscope strongly reduces their luminous efficiency as shown by cathodoluminescence imaging and spectroscopy. We demonstrate that this luminescence quenching originates from a combination of charge trapping at already existing surface states and the formation of new surface states induced by the adsorption of C on the nanowire sidewalls. The interplay of these effects leads to a complex temporal evolution of the quenching, which strongly depends on the incident electron dose per area. Time-resolved photoluminescence measurements on electron-irradiated samples reveal that the carbonaceous adlayer affects both the nonradiative and the radiative recombination dynamics.

cond-mat.mes-hall↗

arXiv2017

Diameter evolution of selective area grown Ga-assisted GaAs nanowires

We present a novel two-step approach for the selective area growth (SAG) of GaAs nanowires (NWs) by molecular beam epitaxy which has enabled a detailed exploration of the NW diameter evolution. In the first step, the growth parameters are optimized for the nucleation of vertically-oriented NWs. In the second step, the growth parameters are chosen to optimize the NW shape, allowing NWs with a thin diameter (45 nm) and an untapered morphology to be realized. This result is in contrast to the commonly observed thick, inversely tapered shape of SAG NWs. We quantify the flux dependence of radial vapour-solid (VS) growth and build a model that takes into account diffusion on the NW sidewalls to explain the observed VS growth rates. Combining this model for the radial VS growth with an existing model for the droplet dynamics at the NW top, we achieve full understanding of the diameter of NWs over their entire length and the evolution of the diameter and tapering during growth. We conclude that only the combination of droplet dynamics and VS growth results in an untapered morphology. This result enables NW shape engineering and has important implications for doping of NWs.

cond-mat.mes-hall↗

arXiv2017

Surface preparation and patterning by nano imprint lithography for the selective area growth of GaAs nanowires on Si(111)

The selective area growth of Ga-assisted GaAs nanowires (NWs) with a high vertical yield on Si(111) substrates is still challenging. Here, we explore different surface preparations and their impact on NW growth by molecular beam epitaxy. We show that boiling the substrate in ultrapure water leads to a significant improvement in the vertical yield of NWs (realizing 80%) grown on substrates patterned by electron-beam lithography (EBL). Tentatively, we attribute this improvement to a reduction in atomic roughness of the substrate in the mask opening. On this basis, we transfer our growth results to substrates processed by a technique that enables the efficient patterning of large arrays, nano imprint lithography (NIL). In order to obtain hole sizes below 50 nm, we combine the conventional NIL process with an indirect pattern transfer (NIL-IPT) technique. Thereby, we achieve smaller hole sizes than previously reported for conventional NIL and growth results that are comparable to those achieved on EBL patterned substrates.

cond-mat.mtrl-sci↗

arXiv2017

Radial Stark effect in (In,Ga)N nanowires

We study the luminescence of unintentionally doped and Si-doped In$_x$Ga$_{1-x}$N nanowires with a low In content (x<0.2) grown by molecular beam epitaxy on Si substrates. The emission band observed at 300 K from the unintentionally doped samples is centered at much lower energies (800 meV) than expected from the In content measured by x-ray diffractometry and energy dispersive x-ray spectroscopy. This discrepancy arises from the pinning of the Fermi level at the sidewalls of the nanowires, which gives rise to strong radial built-in electric fields. The combination of the built-in electric fields with the compositional fluctuations inherent to (In,Ga)N alloys induces a competition between spatially direct and indirect recombination channels. At elevated temperatures, electrons at the core of the nanowire recombine with holes close to the surface, and the emission from unintentionally doped nanowires exhibits a Stark shift of several hundreds of meV. The competition between spatially direct and indirect transitions is analyzed as a function of temperature for samples with various Si concentrations. We propose that the radial Stark effect is responsible for the broadband absorption of (In,Ga)N nanowires across the entire visible range, which makes these nanostructures a promising platform for solar energy applications.

cond-mat.mtrl-sci↗

arXiv2017

Modelling the electronic properties of GaAs polytype nanostructures: impact of strain on the conduction band character

We study the electronic properties of GaAs nanowires composed of both the zincblende and wurtzite modifications using a ten-band k.p model. In the wurtzite phase, two energetically close conduction bands are of importance for the confinement and the energy levels of the electron ground state. These bands form two intersecting potential landscapes for electrons in zincblende/wurtzite nanostructures. The energy difference between the two bands depends sensitively on strain, such that even small strains can reverse the energy ordering of the two bands. This reversal may already be induced by the non-negligible lattice mismatch between the two crystal phases in polytype GaAs nanostructures, a fact that was ignored in previous studies of these structures. We present a systematic study of the influence of intrinsic and extrinsic strain on the electron ground state for both purely zincblende and wurtzite nanowires as well as for polytype superlattices. The coexistence of the two conduction bands and their opposite strain dependence results in complex electronic and optical properties of GaAs polytype nanostructures. In particular, both the energy and the polarization of the lowest intersubband transition depends on the relative fraction of the two crystal phases in the nanowire.

cond-mat.mes-hall↗

arXiv2017

Fine structure of excitons in InAs quantum dots on GaAs(110) planar layers and nanowire facets

We investigate the optical properties of InAs quantum dots grown by molecular beam epitaxy on GaAs(110) using Bi as a surfactant. The quantum dots are synthesized on planar GaAs(110) substrates as well as on the {110} sidewall facets of GaAs nanowires. At 10 K, neutral excitons confined in these quantum dots give rise to photoluminescence lines between 1.1 and 1.4 eV. Magneto-photoluminescence spectroscopy reveals that for small quantum dots emitting between 1.3 and 1.4 eV, the electron-hole coherence length in and perpendicular to the (110) plane is on the order of 5 and 2 nm, respectively. The quantum dot photoluminescence is linearly polarized, and both binding and antibinding biexcitons are observed, two findings that we associate with the strain in the (110) plane This strain leads to piezoelectric fields and to a strong mixing between heavy and light hole states, and offers the possibility to tune the degree of linear polarization of the exciton photoluminescence as well as the sign of the binding energy of biexcitons.

cond-mat.mes-hall↗

arXiv2017

Self-assembly of InAs nanostructures on the sidewalls of GaAs nanowires directed by a Bi surfactant

Surface energies play a dominant role in the self-assembly of three dimensional (3D) nanostructures. In this letter, we show that using surfactants to modify surface energies can provide a means to externally control nanostructure self-assembly, enabling the synthesis of novel hierarchical nanostructures. We explore Bi as a surfactant in the growth of InAs on the {1-10} sidewall facets of GaAs nanowires. The presence of surface Bi induces the formation of InAs 3D islands by a process resembling the Stranski-Krastanov mechanism, which does not occur in the absence of Bi on these surfaces. The InAs 3D islands nucleate at the corners of the {1-10} facets above a critical shell thickness and then elongate along <110> directions in the plane of the nanowire sidewalls. Exploiting this growth mechanism, we realize a series of novel hierarchical nanostructures, ranging from InAs quantum dots on single {1-10} nanowire facets to zig-zag shaped nanorings completely encircling nanowire cores. Photoluminescence spectroscopy and cathodoluminescence spectral line scans reveal that small surfactant-induced InAs 3D islands behave as optically active quantum dots. This work illustrates how surfactants can provide an unprecedented level of external control over nanostructure self-assembly.

cond-mat.mes-hall↗

arXiv2017

Quantum dot self-assembly driven by a surfactant-induced morphological instability

In strained heteroepitaxy, two-dimensional (2D) layers can exhibit a critical thickness at which three-dimensional (3D) islands self-assemble, relieving misfit strain at the cost of an increased surface area. Here we show that such a morphological phase transition can be induced on-demand using surfactants. We explore Bi as a surfactant in the growth of InAs on GaAs(110), and find that the presence of surface Bi induces Stranski-Krastanov growth of 3D islands, while growth without Bi always favors 2D layer formation. Exposing a static two monolayer thick InAs layer to Bi rapidly transforms the layer into 3D islands. Density functional theory calculations reveal that Bi reduces the energetic cost of 3D island formation by modifying surface energies. These 3D nanostructures behave as optically active quantum dots. This work illustrates how surfactants can enable quantum dot self-assembly where it otherwise would not occur.

cond-mat.mtrl-sci↗

arXiv2016

Nature of excitons bound to inversion domain boundaries: Origin of the 3.45-eV luminescence lines in spontaneously formed GaN nanowires on Si(111)

We investigate the 3.45-eV luminescence band of spontaneously formed GaN nanowires on Si(111) by photoluminescence and cathodoluminescence spectroscopy. This band is found to be particularly prominent for samples synthesized at comparatively low temperatures. At the same time, these samples exhibit a peculiar morphology, namely, isolated long nanowires are interspersed within a dense matrix of short ones. Cathodoluminescence intensity maps reveal the 3.45-eV band to originate primarily from the long nanowires. Transmission electron microscopy shows that these long nanowires are either Ga polar and are joined by an inversion domain boundary with their short N-polar neighbors, or exhibit a Ga-polar core surrounded by a N-polar shell with a tubular inversion domain boundary at the core/shell interface. For samples grown at high temperatures, which exhibit a uniform nanowire morphology, the 3.45-eV band is also found to originate from particular nanowires in the ensemble and thus presumably from inversion domain boundaries stemming from the coexistence of N- and Ga-polar nanowires. For several of the investigated samples, the 3.45-eV band splits into a doublet. We demonstrate that the higher-energy component of this doublet arises from the recombination of two-dimensional excitons free to move in the plane of the inversion domain boundary. In contrast, the lower-energy component of the doublet originates from excitons localized in the plane of the inversion domain boundary. We propose that this in-plane localization is due to shallow donors in the vicinity of the inversion domain boundaries.

cond-mat.mes-hall↗

arXiv2016

Exciton dynamics in GaAs/(Al,Ga)As core-shell nanowires with shell quantum dots

We study the dynamics of excitons in GaAs/(Al,Ga)As core-shell nanowires by continuous-wave and time-resolved photoluminescence and photoluminescence excitation spectroscopy. Strong Al segregation in the shell of the nanowires leads to the formation of Ga-rich inclusions acting as quantum dots. At 10 K, intense light emission associated with these shell quantum dots is observed. The average radiative lifetime of excitons confined in the shell quantum dots is 1.7 ns. We show that excitons may tunnel toward adjacent shell quantum dots and nonradiative point defects. We investigate the changes in the dynamics of charge carriers in the shell with increasing temperature, with particular emphasis on the transfer of carriers from the shell to the core of the nanowires. We finally discuss the implications of carrier localization in the (Al,Ga)As shell for fundamental studies and optoelectronic applications based on core-shell III-As nanowires.

cond-mat.mes-hall↗

arXiv2016

Molecular beam epitaxy of single crystalline GaN nanowires on a flexible Ti foil

We demonstrate the self-assembled growth of vertically aligned GaN nanowire ensembles on a flexible Ti foil by plasma-assisted molecular beam epitaxy. The analysis of single nanowires by transmission electron microscopy reveals that they are single crystalline. Low-temperature photoluminescence spectroscopy demonstrates that, in comparison to standard GaN nanowires grown on Si, the nanowires prepared on the Ti foil exhibit a equivalent crystalline perfection, a higher density of basal-plane stacking faults, but a reduced density of inversion domain boundaries. The room-temperature photoluminescence spectrum of the nanowire ensemble is not influenced or degraded by the bending of the substrate. The present results pave the way for the fabrication of flexible optoelectronic devices based on GaN nanowires on metal foils.

cond-mat.mtrl-sci↗

arXiv2015

Improved control over spontaneously formed GaN nanowires in molecular beam epitaxy using a two-step growth process

We investigate the influence of modified growth conditions during the spontaneous formation of GaN nanowires on Si(111) in plasma-assisted molecular beam epitaxy. We find that a two-step growth approach, where the substrate temperature is increased during the nucleation stage, is an efficient method to gain control over the area coverage, average diameter, and coalescence degree of GaN nanowire ensembles. Furthermore, we also demonstrate that the growth conditions employed during the incubation time that precedes nanowire nucleation do not influence the properties of the final nanowire ensemble. Therefore, when growing GaN nanowires at elevated temperatures or with low Ga/N ratios, the total growth time can be reduced significantly by using more favorable growth conditions for nanowire nucleation during the incubation time.

cond-mat.mtrl-sci↗

arXiv2015

Computing Equilibrium Shapes of Wurtzite Crystals: The Example of GaN

Crystal morphologies are important for the design and functionality of devices based on low-dimensional nanomaterials. The equilibrium crystal shape (ECS) is a key quantity in this context. It is determined by surface energies, which are hard to access experimentally but can generally be well predicted by first-principles methods. Unfortunately, this is not necessarily so for polar and semipolar surfaces of wurtzite crystals. By extending the concept of Wulff construction, we demonstrate that the ECSs can nevertheless be obtained for this class of materials. For the example of GaN, we identify different crystal shapes depending on the chemical potential, shedding light on experimentally observed GaN nanostructures.

cond-mat.mtrl-sci↗

arXiv2014

Compatibility of the selective area growth of GaN nanowires on AlN-buffered Si substrates with the operation of light emitting diodes

AlN layers with thicknesses between 2 and 14 nm were grown on Si(111) substrates by molecular beam epitaxy. The effect of the AlN layer thickness on the morphology and nucleation time of spontaneously formed GaN nanowires (NWs) was investigated by scanning electron microscopy and line-of-sight quadrupole mass spectrometry, respectively. We observed that the alignment of the NWs grown on these layers improves with increasing layer thickness while their nucleation time decreases. Our results show that 4 nm is the smallest thickness of the AlN layer that allows the growth of well-aligned NWs with short nucleation time. Such an AlN buffer layer was successfully employed, together with a patterned SiOx mask, for the selective-area growth (SAG) of vertical GaN NWs. In addition, we fabricated light-emitting diodes (LEDs) from NW ensembles that were grown by means of self-organization phenomena on bare and on AlN-buffered Si substrates. A careful characterization of the optoelectronic properties of the two devices showed that the performance of NW-LEDs on bare and AlN-buffered Si is similar. Electrical conduction across the AlN buffer is facilitated by a high number of grain boundaries that were revealed by transmission electron microscopy. These results demonstrate that grainy AlN buffer layers on Si are compatible both with the SAG of GaN NWs and LED operation. Therefore, this study is a first step towards the fabrication of LEDs on Si substrates based on homogeneous NW ensembles.

cond-mat.mtrl-sci↗

arXiv2014

Understanding peculiarities in the optoelectronic characteristics of light emitting diodes based on (In,Ga)N/GaN nanowires

We investigate the effect of the p-type top contact on the optoelectronic characteristics of light emitting diodes (LEDs) based on (In,Ga)N/GaN nanowire (NW) ensembles grown by molecular beam epitaxy on Si substrates. We compare devices fabricated with either Ni/Au or indium tin oxide (ITO) top contact. The NW-LEDs with ITO exhibit a number density of NWs emitting electroluminescence about ten times higher, significantly lower turn-on voltage and series resistance, and a relative external quantum efficiency more than one order of magnitude higher than the sample with Ni/Au. These results show that limitations in the performance of such devices reported so far can be overcome by improving the p-type top-contact.

cond-mat.mtrl-sci↗