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Oliver Brandt

Publications and source records attributed to Oliver Brandt.

At least 73 records · Page 4Linked to original sources

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↗

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↗

Elastic vs. plastic strain relaxation in coalesced GaN nanowires: an x-ray diffraction study

The coalescence in dense arrays of spontaneously formed GaN nanowires proceeds by bundling: adjacent nanowires bend and merge at their top, thus reducing their surface energy at the expense of the elastic energy of bending. We give a theoretical description of the energetics of this bundling process. The bending energy is shown to be substantially reduced by the creation of dislocations at the coalescence joints. A comparison of experimental and calculated x-ray diffraction profiles from ensembles of bundled nanowires demonstrates that a large part of the bending energy is indeed relaxed by plastic deformation. The residual bending manifests itself by extended tails of the diffraction profiles.

cond-mat.mtrl-sci↗

Influence of strain relaxation in axial (In,Ga)N/GaN nanowire heterostructures on their electronic properties

We present a systematic study of the influence of elastic strain relaxation on the built-in electrostatic potentials and the electronic properties of axial (In,Ga)N/GaN nanowire heterostructures. We employ and evaluate analytical and numerical approaches to compute strain and polarization potentials. These two ingredients then enter an eight-band k.p model to compute electron and hole ground states and energies. Our analysis reveals that for a sufficiently large ratio between the thickness of the (In,Ga)N disk and the diameter of the nanowire, the elastic relaxation leads to a significant reduction of the built-in electrostatic potential in comparison to a planar system of similar layer thickness and In content. However, a complete elimination of the built-in potential cannot be achieved in axial nanowire heterostructures. Nevertheless, the reduction of the built-in electrostatic potential leads to a significant modification of the electron and hole energies. Our findings indicate that the range of accessible ground state transition energies in an axial (In,Ga)N/GaN nanowire heterostructure is limited due to the reduced influence of polarization potentials for thicker disks. Additionally, we find that strain and polarization potentials induce complex confinement features of electrons and holes, which depend on the In content, shape, and dimensions of the heterostructure.

cond-mat.mes-hall↗

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↗

Individual electron and hole localization in submonolayer InN quantum sheets embedded in GaN

We investigate sub-monolayer InN quantum sheets embedded in GaN(0001) by temperature-dependent photoluminescence spectroscopy under both continuous-wave and pulsed excitation. Both the peak energy and the linewidth of the emission band associated with the quantum sheets exhibit an anomalous dependence on temperature indicative of carrier localization. Photoluminescence transients reveal a power law decay at low temperatures reflecting that the recombining electrons and holes occupy spatially separate, individual potential minima reminiscent of conventional (In,Ga)N(0001) quantum wells exhibiting the characteristic disorder of a random alloy. At elevated temperatures, carrier delocalization sets in and is accompanied by a thermally activated quenching of the emission. We ascribe the strong nonradiative recombination to extended states in the GaN barriers and confirm our assumption by a simple rate-equation model.

cond-mat.mes-hall↗

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↗

Counterintuitive strain distribution in axial (In,Ga)N/GaN nanowires

We study the three-dimensional deformation field induced by an axial (In,Ga)N segment in a GaN nanowire. Using the finite element method within the framework of linear elasticity theory, we study the dependence of the strain field on the ratio of segment length and nanowire radius. Contrary to intuition, the out-of-plane-component of the elastic strain tensor is found to assume large negative values for a length-to-radius ratio close to one. We show that this unexpected effect is a direct consequence of the deformation of the nanowire at the free sidewalls and the associated large shear strain components. Simulated reciprocal space maps of a single (In,Ga)N/GaN nanowire demonstrate that nanofocus x-ray diffraction is a suitable technique to assess this peculiar strain state experimentally.

cond-mat.mtrl-sci↗

Comparison of the luminous efficiency of Ga- and N-polar In$_{x}$Ga$_{1-x}$N/In$_{y}$Ga$_{1-y}$N quantum wells grown by plasma-assisted molecular beam epitaxy

We investigate the luminescence of Ga- and N-polar In$_{x}$Ga$_{1-x}$N/In$_{y}$Ga$_{1-y}$N quantum wells (QWs) grown by plasma-assisted molecular beam epitaxy on freestanding GaN as well as 6H-SiC substrates. In striking contrast to their Ga-polar counterparts, the N-polar QWs prepared on freestanding GaN do not exhibit any detectable photoluminescence. Theoretical simulations of the band profiles combined with resonant excitation of the QWs allow us to rule out carrier escape and subsequent surface recombination as the reason for the absence of luminescence. To explore the hypothesis of a high concentration of nonradiative defects at the interfaces between wells and barriers, we analyze Ga- and N-polar QWs prepared on 6H-SiC as a function of the well width. Intense luminescence is observed for both Ga- and N polar samples. As expected, the luminescence of the Ga-polar QWs quenches and red-shifts with increasing well width due to the quantum confined Stark effect. In contrast, both the intensity and the energy of the luminescence from the N-polar samples are essentially independent of well width. Transmission electron microscopy reveals that the N-polar QWs exhibit abrupt interfaces and homogeneous composition, excluding emission from In-rich clusters as the reason for this anomalous behavior. The microscopic origin of the luminescence in the N-polar QWs is elucidated using spatially resolved cathodoluminescence spectroscopy. Regardless of well width, the luminescence is found to not originate from the N-polar QWs, but from the semipolar facets of v-pit defects. These results cast serious doubts on the potential of N-polar QWs grown by plasma-assisted molecular beam epitaxy for the development of long-wavelength light emitting diodes. What remains to be seen is whether unconventional growth conditions may enable a significant reduction in the concentration of nonradiative defects.

cond-mat.mtrl-sci↗

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↗

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↗

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↗

Investigating the origin of the nonradiative decay of bound excitons in GaN nanowires

We investigate the origin of the fast recombination dynamics of bound and free excitons in GaN nanowire ensembles by temperature-dependent photoluminescence spectroscopy using both continuous-wave and pulsed excitation. The exciton recombination in the present GaN nanowires is dominated by a nonradiative channel between 10 and 300 K. Furthermore, bound and free excitons in GaN NWs are strongly coupled even at low temperatures resulting in a common lifetime of these states. By solving the rate equations for a coupled two-level system, we show that one cannot, in practice, distinguish whether the nonradiative decay occurs directly via the bound or indirectly via the free state. The nanowire surface and coalescence-induced dislocations appear to be the most obvious candidates for nonradiative defects, and we thus compare the exciton decay times measured for a variety of GaN nanowire ensembles with different surface-to-volume ratio and coalescence degrees. The data are found to exhibit no correlation with either of these parameters, i. e., the dominating nonradiative channel in the GaN nanowires under investigation is neither related to the nanowire surface, nor to coalescence-induced defects for the present samples. Hence, we conclude that nonradiative point defects are the origin of the fast recombination dynamics of excitons in GaN nanowires.

cond-mat.mtrl-sci↗

Luminescence associated with stacking faults in GaN

Basal-plane stacking faults are an important class of optically active structural defects in wurtzite semiconductors. The local deviation from the 2H stacking of the wurtzite matrix to a 3C zinc-blende stacking induces a bound state in the gap of the host crystal, resulting in the localization of excitons. Due to the two-dimensional nature of these planar defects, stacking faults act as quantum wells, giving rise to radiative transitions of excitons with characteristic energies. Luminescence spectroscopy is thus capable of detecting even a single stacking fault in an otherwise perfect wurtzite crystal. This review draws a comprehensive picture of the luminescence properties related to stacking faults in GaN. The emission energies associated with different types of stacking faults as well as factors that can shift these energies are discussed. In this context, the importance of the quantum-confined Stark effect in these zinc-blende/wurtzite heterostructures, which results from the spontaneous polarization of wurtzite GaN, is underlined. This discussion is extended to zinc-blende segments in a wurtzite matrix. Furthermore, other factors affecting the emission energy and linewidth of stacking fault-related peaks as well as results obtained at room temperature are addressed. The considerations presented in this article should be transferable also to other wurtzite semiconductors.

cond-mat.mtrl-sci↗

Sub-meV linewidth in GaN nanowire ensembles: absence of surface excitons due to the field-ionization of donors

We observe unusually narrow donor-bound exciton transitions (0.4 meV) in the photoluminescence spectra of GaN nanowire ensembles grown on Si(111) substrates at very high (> 850 degrees Celsius) temperatures. The spectra of these samples reveal a prominent transition of excitons bound to neutral Si impurities which is not observed for samples grown under standard conditions. Motivated by these experimental results, we investigate theoretically the impact of surface-induced internal electric fields on the binding energy of donors by a combined Monte Carlo and envelope function approach. We obtain the ranges of doping and diameter for which the potential is well described using the Poisson equation, where one assumes a spatially homogeneous distribution of dopants. Our calculations also show that surface donors in nanowires with a diameter smaller than 100 nm are ionized when the surface electric field is larger than about 10 kV/cm, corresponding to a doping level higher than 2 x 10^16 cm^-3. This result explains the experimental observation: since the (D+,X) complex is not stable in GaN, surface-donor-bound excitons do not contribute to the photoluminescence spectra of GaN nanowires above a certain doping level, and the linewidth reflects the actual structural perfection of the nanowire ensemble.

cond-mat.mes-hall↗

Localization and defects in axial (In,Ga)N/GaN nanowire heterostructures investigated by spatially-resolved luminescence spectroscopy

(In,Ga)N insertions embedded in self-assembled GaN nanowires are of current interest for applications in solid state light emitters. Such structures exhibit a notoriously broad emission band. We use cathodoluminescence spectral imaging in a scanning electron microscope and micro-photoluminescence spectroscopy on single nanowires to learn more about the mechanisms underlying this emission. We observe a shift of the emission energy along the stack of six insertions within single nanowires that may be explained by compositional pulling. Our results also corroborate reports that the localization of carriers at potential fluctuations within the insertions plays a crucial role for the luminescence of these nanowire based emitters. Furthermore, we resolve contributions from both structural and point defects in our measurements.

cond-mat.mtrl-sci↗

Statistical analysis of the shape of one-dimensional nanostructures: determining the coalescence degree of spontaneously formed GaN nanowires

Single GaN nanowires formed spontaneously on a given substrate represent nanoscopic single crystals free of any extended defects. However, due to the high area density of thus formed GaN nanowire ensembles, individual nanowires coalesce with others in their immediate vicinity. This coalescence process may introduce strain and structural defects, foiling the idea of defect-free material due to the nanowire geometry. To investigate the consequences of this process, a quantitative measure of the coalescence of nanowire ensembles is required. We derive objective criteria to determine the coalescence degree of GaN nanowire ensembles. These criteria are based on the area-perimeter relationship of the cross-sectional shapes observed, and in particular on their circularity. Employing these criteria, we distinguish single nanowires from coalesced aggregates in an ensemble, determine the diameter distribution of both, and finally analyze the coalescence degree of nanowire ensembles with increasing fill factor.

cond-mat.mes-hall↗

Coupling of exciton states as the origin of their biexponential decay dynamics in GaN nanowires

Using time-resolved photoluminescence spectroscopy, we explore the transient behavior of bound and free excitons in GaN nanowire ensembles. We investigate samples with distinct diameter distributions and show that the pronounced biexponential decay of the donor-bound exciton observed in each case is not caused by the nanowire surface. At long times, the individual exciton transitions decay with a common lifetime, which suggests a strong coupling between the corresponding exciton states. A system of non-linear rate-equations taking into account this coupling directly reproduces the experimentally observed biexponential decay.

cond-mat.mtrl-sci↗