arXiv subjects

Timur Flissikowski

Publications and source records attributed to Timur Flissikowski.

15 recordsLinked to original sources

arXiv2024

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

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

cond-mat.mes-hall↗

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 $\mu$-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↗

arXiv2021

Interface recombination in Ga- and N-polar GaN/(Al,Ga)N quantum wells grown by molecular beam epitaxy

We explore and systematically compare the morphological, structural and optical properties of GaN/(Al,Ga)N multiple quantum wells (MQWs) grown by plasma-assisted molecular beam epitaxy (PA-MBE) on freestanding GaN$(0001)$ and GaN$(000\bar{1})$ substrates. Samples of different polarity are found to be comparable in terms of their morphological and structural perfection and exhibit essentially identical quantum well widths and Al content. Regardless of the crystal orientation, the exciton decay in the MQWs at 10 K is dominantly radiative and the photoluminescence (PL) energy follows the quantum confined Stark effect (QCSE) for different quantum well widths. A prominent free-to-bound transition involving interface shallow donors is, however, visible for the N-polar MQWs. At room-temperature, in contrast, the exciton decay in all samples is dominated by nonradiative recombination taking place at point defects, presumably Ca or V N located at the bottom QW interface. Remarkably, the N-polar MQWs exhibit a higher PL intensity and longer decay times than the Ga-polar MQWs at room-temperature. This improved internal quantum efficiency is attributed to the beneficial orientation of the internal electric field that effectively reduces the capture rate of minority carriers by interface trap states.

cond-mat.mtrl-sci↗

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

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↗

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

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↗

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

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↗

arXiv2014

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↗

arXiv2014

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↗

arXiv2013

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↗

arXiv2011

Coexistence of quantum-confined Stark effect and localized states in an (In,Ga)N/GaN nanowire heterostructure

We analyze the emission of single GaN nanowires with (In,Ga)N insertions using both micro-photoluminescence and cathodoluminescence spectroscopy. The emission spectra are dominated by a green luminescence band that is strongly blueshifted with increasing excitation density. In conjunction with finite-element simulations of the structure to obtain the piezoelectric polarization, these results demonstrate that our (In,Ga)N/GaN nanowire heterostructures are subject to the quantum-confined Stark effect. Additional sharp peaks in the spectra, which do not shift with excitation density, are attributed to emission from localized states created by compositional fluctuations in the ternary (In,Ga)N alloy.

cond-mat.mtrl-sci↗