arXiv subjects

Jonas Lähnemann

Publications and source records attributed to Jonas Lähnemann.

At least 37 records · Page 2Linked to original sources

arXiv2021

Correlated and in-situ electrical transmission electron microscopy studies and related membrane fabrication

Understanding the interplay between the structure, composition and opto-electronic properties of semiconductor nano-objects requires combining transmission electron microscopy (TEM) based techniques with electrical and optical measurements on the very same specimen. Recent developments in TEM technologies allow not only the identification and in-situ electrical characterization of a particular object, but also the direct visualization of its modification in-situ by techniques such as Joule heating. Over the past years, we have carried out a number of studies in these fields that are reviewed in this contribution. In particular, we discuss here i) correlated studies where the same unique object is characterized electro-optically and by TEM, ii) in-situ Joule heating studies where a solid-state metal-semiconductor reaction is monitored in the TEM, and iii) in-situ biasing studies to better understand the electrical properties of contacted single nanowires. In addition, we provide detailed fabrication steps for the silicon nitride membranes crucial to these correlated and in-situ measurements.

physics.app-ph↗

arXiv2021

Carrier diffusion in GaN -- a cathodoluminescence study. I: Temperature-dependent generation volume

The determination of the carrier diffusion length of semiconductors such as GaN and GaAs by cathodoluminescence imaging requires accurate knowledge about the spatial distribution of generated carriers. To obtain the lateral distribution of generated carriers for sample temperatures between 10 and 300 K, we utilize cathodoluminescence intensity profiles measured across single quantum wells embedded in thick GaN and GaAs layers. Thin (Al,Ga)N and (Al,Ga)As barriers, respectively, prevent carriers diffusing in the GaN and GaAs layers to reach the well, which would broaden the profiles. The experimental cathodoluminescence profiles are found to be systematically wider than the energy loss distributions calculated by means of the Monte Carlo program CASINO, with the width monotonically increasing with decreasing temperature. This effect is observed for both GaN and GaAs and becomes more pronounced for higher acceleration voltages. We discuss this phenomenon in terms of both, the electron-phonon interaction controlling the energy relaxation of hot carriers, and the shape of the initial carrier distribution. Finally, we present a phenomenological approach to simulate the carrier generation volume that can be used for the investigation of the temperature dependence of carrier diffusion.

cond-mat.mtrl-sci↗

arXiv2021

Carrier diffusion in GaN -- a cathodoluminescence study. II: Ambipolar vs. exciton diffusion

We determine the diffusion length of excess carriers in GaN by spatially resolved cathodoluminescence spectroscopy utilizing a single quantum well as carrier collector or carrier sink. Monochromatic intensity profiles across the quantum well are recorded for temperatures between 10 and 300 K. A classical diffusion model accounts for the profiles acquired between 120 and 300 K, while for temperatures lower than 120 K, a quantum capture process has to be taken into account in addition. Combining the diffusion length extracted from these profiles and the effective carrier lifetime measured by time-resolved photoluminescence experiments, we deduce the carrier diffusivity as a function of temperature. The experimental values are found to be close to theoretical ones for the ambipolar diffusivity of free carriers limited only by intrinsic phonon scattering. This agreement is shown to be fortuitous. The high diffusivity at low temperatures instead originates from an increasing participation of excitons in the diffusion process.

cond-mat.mtrl-sci↗

arXiv2021

Carrier diffusion in GaN -- a cathodoluminescence study. III: Nature of nonradiative recombination at threading dislocations

We investigate the impact of threading dislocations with an edge component (a or a+c-type) on carrier recombination and diffusion in GaN(0001) layers close to the surface as well as in the bulk. To this end, we utilize cathodoluminescence imaging of the top surface of a GaN(0001) layer with a deeply buried (In,Ga)N quantum well. Varying the acceleration voltage of the primary electrons and comparing the signal from the layer and the quantum well enables us to probe carrier recombination at depths ranging from the close vicinity of the surface to the position of the quantum well. Our experiments are accompanied by fully three-dimensional Monte Carlo simulations of carrier drift, diffusion, and recombination in the presence of the surface, the quantum well, and the dislocation, taking into account the dislocation strain field and the resulting piezoelectric field at the dislocation outcrop. Near the surface, this field establishes an exciton dead zone around the dislocation, the extent of which is not related to the carrier diffusion length. However, reliable values of the carrier diffusion length can be extracted from the dipole-like energy shift observed in hyperspectral cathodoluminescence maps recorded around the dislocation outcrop at low acceleration voltages. For high acceleration voltages, allowing us to probe a depth where carrier recombination is unaffected by surface effects, we observe a much stronger contrast than expected from the piezoelectric field alone. This finding provides unambiguous experimental evidence for the strong nonradiative activity of edge threading dislocations in bulk GaN and hence also in buried heterostructures.

cond-mat.mtrl-sci↗

arXiv2021

Bandgap widening and behavior of Raman-active phonon modes of cubic single-crystalline (In,Ga)$_2$O$_3$ alloy films

The influence of Ga incorporation into cubic In$_2$O$_3$ on the electronic and vibrational properties is discussed for (In$_{1-x}$,Ga$_x$)$_2$O$_3$ alloy films grown by molecular beam epitaxy. Using spectroscopic ellipsometry, a linear dependence of the absorption onset on the Ga content $x$ is found with a blueshift of up to 150 meV for $x = 0.1$. Consistently, the fundamental band gap exhibits a blueshift as determined by hard X-ray photoelectron spectroscopy. The dependence of the absorption onset and the effective electron mass on the electron concentration is derived from the infrared dielectric functions for a Sn doped alloy film. The influence of alloying on phonon modes is analyzed on the basis of Raman spectroscopic measurements. The frequencies of several phonon modes are identified as sensitive measures for the spectroscopic determination of the Ga content.

cond-mat.mtrl-sci↗

arXiv2021

Dislocation and Indium Droplet Related Emission Inhomogeneities in InGaN LEDs

This report classifies emission inhomogeneities that manifest in InGaN quantum well blue light-emitting diodes grown by plasma-assisted molecular beam epitaxy on free-standing GaN substrates. By a combination of spatially resolved electroluminescence and cathodoluminescence measurements, atomic force microscopy, scanning electron microscopy and hot wet KOH etching, the identified inhomogeneities are found to fall in four categories. Labeled here as type I through IV, they are distinguishable by their size, density, energy, intensity, radiative and electronic characteristics and chemical etch pits which correlates them with dislocations. Type I exhibits a blueshift of about 120 meV for the InGaN quantum well emission attributed to a perturbation of the active region, which is related to indium droplets that form on the surface in the metal-rich InGaN growth condition. Specifically, we attribute the blueshift to a decreased growth rate of and indium incorporation in the InGaN quantum wells underneath the droplet which is postulated to be the result of reduced incorporated N species due to increased N$_{2}$ formation. The location of droplets are correlated with mixed type dislocations for type I defects. Types II through IV are due to screw dislocations, edge dislocations, and dislocation bunching, respectively, and form dark spots due to leakage current and nonradiative recombination.

cond-mat.mtrl-sci↗

arXiv2021

Molecular beam epitaxy of single-crystalline bixbyite (In$_{1-x}$Ga$_x$)$_2$O$_3$ films ($x \leq 0.18$): Structural properties and consequences of compositional inhomogeneity

In this work, we show the heteroepitaxial growth of single-crystalline bixbyite (In$_{1-x}$Ga$_x$)$_2$O$_3$ films on (111)-oriented yttria-stabilized zirconia substrates using plasma-assisted molecular beam epitaxy under various growth conditions. A pure In$_2$O$_3$ buffer layer between the substrate and (In$_{1-x}$Ga$_x$)$_2$O$_3$ alloy is shown to result in smoother film surfaces and significantly improved crystallinity. Symmetric out-of-plane 2$θ- ω$ x-ray diffraction scans show a single (111) crystal orientation and transmission electron microscopy confirms the single-crystallinity up to $x = 0.18$ and only slight film quality deterioration with increasing Ga content. Partially relaxed layers are demonstrated via reciprocal space mapping with lattice parameters fitting well to Vegard's law. However, the Ga cations are not evenly distributed within the films containing nominally $x > 0.11$: inclusions with high Ga density up to $x = 0.50$ are observed within a "matrix" with $x \approx 0.08$. The cubic bixbyite phase is preserved, in both the "matrix" and the inclusions. Moreover, for $x \geq 0.11$, both the Raman phonon lines as well as the optical absorption onset remain nearly constant. Hard x-ray photoelectron spectroscopy measurements also indicate a widening of the band gap and exhibit similar saturation of the Ga 2p core level position for high Ga contents. This saturation behavior of the spectroscopic properties further supports the limited Ga incorporation into the "matrix" of the film.

cond-mat.mtrl-sci↗

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↗

arXiv2020

Plasma-assisted molecular beam epitaxy of NiO on GaN(00.1)

The growth of NiO on GaN(00.1) substrates by plasma-assisted molecular beam epitaxy under oxygen rich conditions was investigated at growth temperatures between 100 $^{\circ}$C and 850 $^{\circ}$C. Epitaxial growth of NiO(111) with two rotational domains, with epitaxial relation $\normalsize{}\mathrm{\mathrm{\mathrm{NiO}(1\bar{\mathrm{1}}0)}\:||\:\mathrm{\mathrm{GaN}(11.0)}}$ and $\mathrm{\mathrm{\mathrm{NiO}\mathrm{(10\bar{\mathrm{1}})}\:||\:\mathrm{GaN(11.0)}}}$, was observed by X-ray diffraction (XRD) and confirmed by in-situ reflection high-energy electron diffraction as well as transmission electron microscopy (TEM) and electron backscatter diffraction. With respect to the high lattice mismatch of 8.1 % and a measured low residual tensile layer strain, growth by lattice matching epitaxy or domain matching epitaxy is discussed. The morphology measured by atomic force microscopy showed a grainy surface, probably arising from the growth by the columnar rotational domains visible in TEM micrographs. The domain sizes measured by AFM and TEM increase with the growth temperature, indicating an increasing surface diffusion length. Growth at 850 $^{\circ}$C, however, involved local decomposition of the GaN substrate that lead to an interfacial $\mathrmβ$-Ga$\mathrm{_{2}}$O$\mathrm{_{3}}$($\bar{\mathrm{2}}$01) layer and a high NiO surface roughness. Raman mesurements of the quasi-forbidden one-phonon peak indicate increasing layer quality (decreasing defect density) with increasing growth temperature. The results above suggest optimum growth temperatures around 700 $^{\circ}$C for high layer and interface quality.

physics.app-ph↗

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

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

Determination of the carrier diffusion length in GaN from cathodoluminescence maps around threading dislocations: fallacies and opportunities

We investigate, both theoretically and experimentally, the drift, diffusion, and recombination of excitons in the strain field of an edge threading dislocation intersecting the GaN{0001} surface. We calculate and measure hyperspectral cathodoluminescence maps around the dislocation outcrop for temperatures between 10 to 200 K. Contrary to common belief, the cathodoluminescence intensity contrast is only weakly affected by exciton diffusion, but is caused primarily by exciton dissociation in the piezoelectric field at the dislocation outcrop. Hence, the extension of the dark spots around dislocations in the luminescence maps cannot be used to determine the exciton diffusion length. However, the cathodoluminescence energy contrast, reflecting the local bandgap variation in the dislocation strain field, does sensitively depend on the exciton diffusion length and hence enables its experimental determination.

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

Top-down fabrication of ordered arrays of GaN nanowires by selective area sublimation

We demonstrate the top-down fabrication of ordered arrays of GaN nanowires by selective area sublimation of pre-patterned GaN(0001) layers grown by hydride vapor phase epitaxy on Al$_{2}$O$_{3}$. Arrays with nanowire diameters and spacings ranging from 50 to 90 nm and 0.1 to 0.7 $μ$m, respectively, are simultaneously produced under identical conditions. The sublimation process, carried out under high vacuum conditions, is analyzed \emph{in situ} by reflection high-energy electron diffraction and line-of-sight quadrupole mass spectromety. During the sublimation process, the GaN(0001) surface vanishes, giving way to the formation of semi-polar $\lbrace1\bar{1}03\rbrace$ facets which decompose congruently following an Arrhenius temperature dependence with an activation energy of ($3.54 \pm 0.07$) eV and an exponential prefactor of $1.58\times10^{31}$ atoms cm$^{-2}$ s$^{-1}$. The analysis of the samples by low-temperature cathodoluminescence spectroscopy reveals that, in contrast to dry etching, the sublimation process does not introduce nonradiative recombination centers at the nanowire sidewalls. This technique is suitable for the top-down fabrication of a variety of ordered nanostructures, and could possibly be extended to other material systems with similar crystallographic properties such as ZnO.

physics.app-ph↗

arXiv2019

Effect of the nanowire diameter on the linearity of the response of GaN-based heterostructured nanowire photodetectors

Nanowire photodetectors are investigated because of their compatibility with flexible electronics, or for the implementation of on-chip optical interconnects. Such devices are characterized by ultrahigh photocurrent gain, but their photoresponse scales sublinearly with the optical power. Here, we present a study of single-nanowire photodetectors displaying a linear response to ultraviolet illumination. Their structure consists of a GaN nanowire incorporating an AlN/GaN/AlN heterostructure, which generates an internal electric field. The activity of the heterostructure is confirmed by the rectifying behavior of the current-voltage characteristics in the dark, as well as by the asymmetry of the photoresponse in magnitude and linearity. Under reverse bias (negative bias on the GaN cap segment), the detectors behave linearly with the impinging optical power when the nanowire diameter is below a certain threshold ($\approx$ 80 nm), which corresponds to the total depletion of the nanowire stem due to the Fermi level pinning at the sidewalls. In the case of nanowires that are only partially depleted, their nonlinearity is explained by a nonlinear variation of the diameter of their central conducting channel under illumination.

cond-mat.mes-hall↗

arXiv2019

Effect of Ge-doping on the short-wave, mid- and far-infrared intersubband transitions in GaN/AlGaN heterostructures

This paper assesses the effects of Ge-doping on the structural and optical (band-to-band and intersubband (ISB)) properties of GaN/AlGaN multi-quantum wells (QWs) designed to display ISB absorption in the short-wave, mid- and far-infrared ranges (SWIR, MIR, and FIR, respectively). The standard c-plane crystallographic orientation is considered for wells absorbing in the SWIR and MIR spectral regions, whereas the FIR structures are grown along the nonpolar m-axis. In all cases, we compare the characteristics of Ge-doped and Si-doped samples with the same design and various doping levels. The use of Ge appears to improve the mosaicity of the highly lattice-mismatched GaN/AlN heterostructures. However, when reducing the lattice mismatch, the mosaicity is rather determined by the substrate and does not show any dependence on the dopant nature or concentration. From the optical point of view, by increasing the dopant density, we observe a blueshift of the photoluminescence in polar samples due to the screening of the internal electric field by free carriers. In the ISB absorption, on the other hand, there is a systematic improvement of the linewidth when using Ge as a dopant for high doping levels, whatever the spectral region under consideration (i.e. different QW size, barrier composition and crystallographic orientation).

physics.app-ph↗