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Gregor Koblmüller

Publications and source records attributed to Gregor Koblmüller.

At least 19 recordsLinked to original sources

Si- and C-Induced Modifications in Vapor-Solid-Grown InGaAs Nanowires: From Crystal Structure to Carrier Dynamics

Determining the impact of dopants in ternary III-V nanowires (NWs) is crucial for their applications in next-generation optoelectronic and photonic devices; however, the interplay between dopant species, crystal structure, and carrier dynamics in vapor-solid-grown InGaAs NWs remains underexplored. In this study, the influence of silicon (Si) and carbon (C) doping on the structural, morphological, and optical properties of catalyst-free, selective-area grown InGaAs NWs fabricated by molecular beam epitaxy is investigated. Scanning electron microscopy demonstrates that C-doping increases the NW aspect ratio by over 100% compared to undoped NWs, while a concomitant decrease in their planar defect density is observed, indicating enhanced crystal quality with C-doping. Despite their superior crystal quality, the C-doped NWs present a diminished photoluminescence intensity, due to point defects and increased surface recombination velocity. This is further supported by time-resolved photoluminescence spectroscopy, revealing accelerated non-radiative recombination in the C-doped NWs. Lastly, hot-carrier effects in these nanostructures are studied, and their signatures remain observable, albeit with reduced intensity in both Si- and C-doped NWs. This comprehensive study establishes clear correlations between doping parameters and the resulting material characteristics and carrier dynamics, offering valuable insights into the fundamental mechanisms governing the VS-grown InGaAs NWs and their implications in optoelectronic devices.

physics.app-ph

Monolithic axial InGaAs quantum dot emitters in GaAs-based nanowires via Sb-mediated facet engineering

GaAs-based nanowires hosting active quantum heterostructures provide a promising route toward monolithic integration of single-photon sources on silicon, a key requirement for scalable quantum photonics. However, ultrathin axial quantum-emitter formation is often hindered by facet-dependent growth dynamics and rotational twins, which induce lateral overgrowth and compromise interface abruptness. Here, we develop InGaAs-based quantum emitters by tailoring facet evolution via dilute Sb incorporation, which efficiently suppresses twins and promotes confined axial insertion at the growth-front facet. This approach significantly enhances the probability of obtaining abrupt, few-nanometer-thin quantum dots at the nanowire tip. Single-nanowire optical spectroscopy reveals intense, spatially localized emission from the active region with lifetimes as short as (0.51 $\pm$ 0.02) ns, and second-order photon-correlation measurements consistently exhibit pronounced antibunching with $g^{(2)}(0)<0.4$, confirming single-photon emission. These results establish a strong correlation between twin density and axial heterostructure formation, identifying defect control as a key factor in realizing monolithically integrated nanowire single-photon sources.

physics.app-ph

Molecular beam epitaxy of wafer-scale O-band InAs/InGaAs quantum dots on GaAs for quantum photonics

We report a scalable molecular beam epitaxy strategy to achieve a low density of O-band electrically tunable InAs/InGaAs quantum dots (QDs) on GaAs(001) substrates. Our approach is based on a gradient deposition of InAs in the sub-ML regime and subsequent capping with an InGaA strain-reducing layer to redshift the emission wavelength. For different growth conditions, we investigate the optical properties of the dots using photoluminescence mapping and correlate with structural properties determined by scanning transmission electron microscopy. Using a surface roughness modulation technique and synchronizing InAs sub-monolayer deposition cycles with substrate rotation, we control the dot density and position low-density regions (< 1 QD per um^2) on the substrate. Hyperspectral imaging is used to map the spatial and spectral characteristics of many individual dots in the low-density region, confirming that our approach is universally applicable to conventional MBE growth on (001) surfaces. Finally, we tune the QD emission wavelength within the O-band using electric fields and demonstrate single-photon emission with g(2)(0) = 0.020(14).

cond-mat.mtrl-sci

Unraveling Quantum Size-Dependent Optoelectrical Phenomena in Hot Carrier Quantum Well Structures

The enhancement of power conversion efficiency beyond the theoretical limit of single-junction solar cells is a key objective in the advancement of hot carrier solar cells. Recent findings indicate that quantum wells (QWs) can effectively generate hot carriers by confining charged carriers within their potential wells and by optimizing material properties. Here, we investigate the impact of quantum confinement on the thermodynamic properties of photogenerated hot carriers in p-i-n InGaAs/InAlAs heterostructure diodes, utilizing QW thicknesses of 4 nm, 5.5 nm, and 7.5 nm. The optical properties of these nanostructures reveal significant hot carrier effects at various lattice temperatures, with a pronounced effect noted at lower temperatures. The experimental results indicate that the widest QW exhibits stronger hot carrier effects than the thinner QWs. Additionally, the open-circuit voltage of the samples demonstrates a correlation with the degree of quantum confinement, mirroring trends observed in the quasi-Fermi level splitting of hot carriers. However, the magnitudes recorded exceed the bandgap of the quantum structures, suggesting that this behavior may be influenced by the barrier layer. Furthermore, the short-circuit current of the samples reveals a strong dependence on excitation power, but not on the degree of quantum confinement. This indicates that the majority of the photocurrent is generated in the barrier, with negligible contributions from photogenerated carriers within the QWs. This study provides insights into the role of quantum confinement on the opto-electrical properties of non-equilibrium hot carrier populations in QW structures.

physics.app-ph

Telecom quantum dots on GaAs substrates as integration-ready high performance single-photon sources

The development of deterministic single photon sources emitting in the telecommunication bands is a key challenge for quantum communication and photonic quantum computing. Here, we investigate the optical properties and single-photon emission of molecular beam epitaxy grown semiconductor quantum dots emitting in the telecom O- and C- bands. The quantum dots are embedded in a InGaAs matrix with fixed indium content grown on top of a compositionally graded InGaAs buffer. This structure allows for the future implementation of electrically contacted nanocavities to enable high-quality and bright QD emission. In detailed optical characterizations we observe linewidths as low as $ 50 μ$eV, close to the spectrometer resolution limit, low fine structure splittings close to $ 10 μ$eV, and $g^{(2)} (0)$ values as low as $0.08$. These results advance the current performance metrics for MBE-grown quantum dots on GaAs substrates emitting in the telecom bands and showcase the potential of the presented heterostructures for further integration into photonic devices.

cond-mat.mes-hall

Competing mechanisms of dominant radiative and Auger recombination in hot carrier generation in III-V semiconductor nanowires

One-dimensional structures such as nanowires (NWs) show great promise in tailoring the rates of hot carrier thermalization in semiconductors with important implications for the design of efficient hot carrier absorbers. However, fabrication of high-quality, phase-pure crystal structures and control of their intrinsic electronic properties can be challenging, raising concerns about the role of competing radiative and non-radiative recombination mechanisms that govern hot carrier effects. Here, we elucidate the impact of crystal purity and altered electronic properties on the hot carrier properties by comparing two classes of III-V semiconductor NW arrays with similar band-gap energies and geometries, yet different crystal quality: one composed of GaAsSb NWs, free of planar stacking defects, and the other InGaAs NWs with a high density of stacking defects. Photoluminescence spectroscopy demonstrates distinct hot carrier effects in both NW arrays; however, the InGaAs NWs with lower crystal quality exhibit stronger hot carrier effects, as evidenced by increased carrier temperature under identical photoabsorptivity. This difference arises from higher rates of Auger recombination in the InGaAs NWs due to their increased n-type conductivity, as confirmed by excitation power-dependent measurements. Our findings suggest that while enhancing material properties is crucial for improving the performance of hot carrier absorbers, optimizing conditions to increase the rates of Auger recombination will further boost the efficiency of these devices.

physics.app-ph

Interplay of Electron Trapping by Defect Midgap State and Quantum Confinement to Optimize Hot Carrier Effect in a Nanowire Structure

Hot carrier effect, a phenomenon where charge carriers generated by photon absorption remain energetic by not losing much energy, has been one of the leading strategies in increasing solar cell efficiency. Nanostructuring offers an effective approach to enhance hot carrier effect via the spatial confinement, as occurring in a nanowire structure. The recent experimental study by Esmaielpour et al. [ACS Applied Nano Materials 7, 2817 (2024)] reveals a fascinating non-monotonic dependence of the hot carrier effect in nanowire array on the diameter of the nanowire, contrary to what might be expected from quantum confinement alone. We show that this non-monotonic behavior can be explained by a simple model for electron energy loss that involves two principal mechanisms. First, electron-phonon scattering, that increases with nanowire diameter, leading to hot carrier effect that decreases with increasing diameter. Second, electron capture by a defect level within band gap, that is, a midgap state, that decreases with nanowire diameter, leading to hot carrier effect that increases with increasing diameter. The two mechanisms balance at a certain diameter corresponding to optimal hot carrier effect. Our result offers a guideline to optimize hot carrier effect in nanowire solar cells and ultimately their efficiency by adjusting the dimensions and micro-structural properties of nanowires.

cond-mat.mes-hall

Influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics in InGaAs nanowires

Understanding the origin of hot carrier relaxation in nanowires (NWs) with one-dimensional (1D) geometry is significant for designing efficient hot carrier solar cells with such nanostructures. Here, we study the influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics of catalyst-free InGaAs-InAlAs core-shell NWs. Using steady-state and time-resolved photoluminescence (PL) spectroscopy the dependencies of hot carrier effects on the degree of confinement of photo-generated carriers induced by the nanowire diameter are determined at different lattice temperatures. Analysis of excitation-power dependent data and temperature-dependent PL linewidth broadening reveal that at low temperatures, strong Auger recombination and phonon-bottleneck are responsible for hot carrier effects. Our analysis gives also insights into electron-phonon and ionized impurity scattering, showing opposing trends with NW diameter, and it allows to estimate the Fröhlich coupling constant for the InGaAs NWs. Conversely, with increasing lattice temperature, hot carrier relaxation rates increase due to enhanced Shockley-Read Hall and surface recombination. Time-resolved spectroscopy reveals a fourfold increase in the rate of Shockley-Read-Hall recombination from 6 ns at 10 K to 1.5 ns at 150 K. The findings suggest that minimizing defect densities in the bulk and surfaces of these NWs will be key to enhance hot carrier effects towards higher temperatures.

cond-mat.mes-hall

Self-induced ultrafast electron-hole plasma temperature oscillations in nanowire lasers

Nanowire lasers can be monolithically and site-selectively integrated onto silicon photonic circuits. To assess their full potential for ultrafast opto-electronic devices, a detailed understanding of their lasing dynamics is crucial. However, the roles played by their resonator geometry and the microscopic processes that mediate energy exchange between the photonic, electronic, and phononic subsystems are largely unexplored. Here, we study the dynamics of GaAs-AlGaAs core-shell nanowire lasers at cryogenic temperatures using a combined experimental and theoretical approach. Our results indicate that these NW lasers exhibit sustained intensity oscillations with frequencies ranging from 160 GHz to 260 GHz. As the underlying physical mechanism, we identified self-induced electron-hole plasma temperature oscillations resulting from a dynamic competition between photoinduced carrier heating and cooling via phonon scattering. These dynamics are intimately linked to the strong interaction between the lasing mode and the gain material, which arises from the wavelength-scale dimensions of these lasers. We anticipate that our results could lead to new approaches for ultrafast intensity and phase modulation of chip-integrated nanoscale semiconductor lasers.

cond-mat.mes-hall

Hot Carrier Dynamics in InAs-AlAsSb Core-Shell Nanowires

Semiconductor nanowires (NWs) have shown evidence of robust hot carrier effects due to their small dimensions. The relaxation dynamics of hot carriers in these nanostructures, generated by photo-absorption, are of great importance in optoelectronic devices and high efficiency solar cells, such as hot carrier solar cells. Among various III-V semiconductors, indium arsenide (InAs) NWs are promising candidates for their applications in advanced light harvesting devices due to their high photo-absorptivity and high mobility. Here, we investigate the hot carrier dynamics in InAs-AlAsSb core-shell NWs, as well as bare-core InAs NWs, using ultrafast pump-probe spectroscopy with widely tuned pump and probe energies. We have found a lifetime of 2.3 ps for longitudinal optical (LO) phonons and hot electron lifetimes of about 3 ps and 30 ps for carrier-carrier interactions and electron-phonon interactions, respectively. In addition, we have investigated the electronic states in the AlAsSb-shell and found that, despite the large band offset of the core-shell design in the conduction band, excited carriers remain in the shell longer than 100 ps. Our results indicate evidence of plasmon-tailored core-shell NWs for efficient light harvesting devices, which could open potential avenues for improving the efficiency of photovoltaic solar cells.

cond-mat.mtrl-sci

High-dimensional acousto-optoelectric correlation spectroscopy reveals coupled carrier dynamics in polytypic nanowires

The authors combine acousto-optoelectric and multi-channel photon correlation spectroscopy to probe spatio-temporal carrier dynamics induced by a piezoelectric surface acoustic wave (SAW). The technique is implemented by combining phase-locked optical micro-photoluminescence spectroscopy and simultaneous three-channel time resolved detection. From the recorded time correlated single photon counting data the time transients of individual channels and the second and third order correlation functions are obtained with sub-nanosecond resolution. The method is validated by probing the correlations SAW-driven carrier dynamics between three decay channels of a single polytypic semiconductor nanowire on a conventional LiNbO$_\mathrm{3}$ SAW delay line chip. The method can be readily applied to other types of nanosystems and probe SAW-regulated charge state preparation in quantum dots, charge transfer processes in van der Waals heterostructures or other types of hybrid nanoarchitectures.

cond-mat.mes-hall

Dislocation-induced thermal transport anisotropy in single-crystal group-III nitride films

Dislocations, one-dimensional lattice imperfections, are common to technologically important materials such as III-V semiconductors, and adversely affect heat dissipation in e.g., nitride-based high-power electronic devices. For decades, conventional models based on nonlinear elasticity theory have predicted this thermal resistance is only appreciable when heat flux is perpendicular to the dislocations. However, this dislocation-induced anisotropic thermal transport has yet to be seen experimentally. In this study, we measure strong thermal transport anisotropy governed by highly oriented threading dislocation arrays along the cross-plane direction in micron-thick, single-crystal indium nitride (InN) films. We find that the cross-plane thermal conductivity is more than tenfold higher than the in-plane thermal conductivity at 80 K when the dislocation density is on the order of ~3x10^10 cm^-2. This large anisotropy is not predicted by the conventional models. With enhanced understanding of dislocation-phonon interactions, our results open new regimes for tailoring anisotropic thermal transport with line defects, and will facilitate novel methods for directed heat dissipation in thermal management of diverse device applications.

cond-mat.mtrl-sci

Ultrafast photodetection in the quantum wells of single AlGaAs/GaAs-based nanowires

We investigate the ultrafast optoelectronic properties of single Al0.3Ga0.7As/GaAs-core-shell-nanowires. The nanowires contain GaAs-based quantum wells. For a resonant excitation of the quantum wells, we find a picosecond photocurrent which is consistent with an ultrafast lateral expansion of the photogenerated charge carriers. This Dember-effect does not occur for an excitation of the GaAs-based core of the nanowires. Instead, the core exhibits an ultrafast displacement current and a photo-thermoelectric current at the metal Schottky contacts. Our results uncover the optoelectronic dynamics in semiconductor core-shell nanowires comprising quantum wells, and they demonstrate the possibility to use the low-dimensional quantum well states therein for ultrafast photoswitches and photodetectors.

cond-mat.mes-hall

Photocurrents in a Single InAs Nanowire/ Silicon Heterojunction

We investigate the optoelectronic properties of single indium arsenide nanowires, which are grown vertically on p-doped silicon substrates. We apply a scanning photocurrent microscopy to study the optoelectronic properties of the single heterojunctions. The measured photocurrent characteristics are consistent with an excess charge carrier transport through mid-gap trap states, which form at the Si/InAs heterojunctions. Namely, the trap states add an additional transport path across a heterojunction, and the charge of the defects changes the band bending at the junction. The bending gives rise to a photovoltaic effect at a small bias voltage. In addition, we observe a photoconductance effect within the InAs nanowires at large biases.

cond-mat.mes-hall

Directional and dynamic modulation of the optical emission of an individual GaAs nanowire using surface acoustic waves

We report on optical experiments performed on individual GaAs nanowires and the ma- nipulation of their temporal emission characteristics using a surface acoustic wave. We find a pronounced, characteristic suppression of the emission intensity for the surface acoustic wave propagation aligned with the axis of the nanowire. Furthermore, we demonstrate that this quenching is dynamical as it shows a pronounced modulation as the local phase of the surface acoustic wave is tuned. These effects are strongly reduced for a SAW applied in the direction perpendicular to the axis of the nanowire due to their inherent one-dimensional geometry. We resolve a fully dynamic modulation of the nanowire emission up to 678 MHz not limited by the physical properties of the nanowires.

cond-mat.mes-hall

Dynamic Acoustic Control of Individual Optically Active Quantum Dot-like Emission Centers in Heterostructure Nanowires

We probe and control the optical properties of emission centers forming in radial het- erostructure GaAs-Al0.3Ga0.7As nanowires and show that these emitters, located in Al0.3Ga0.7As layers, can exhibit quantum-dot like characteristics. We employ a radio frequency surface acoustic wave to dynamically control their emission energy and occupancy state on a nanosec- ond timescale. In the spectral oscillations we identify unambiguous signatures arising from both the mechanical and electrical component of the surface acoustic wave. In addition, differ- ent emission lines of a single quantum dot exhibit pronounced anti-correlated intensity oscilla- tions during the acoustic cycle. These arise from a dynamically triggered carrier extraction out of the quantum dot to a continuum in the radial heterostructure. Using finite element modeling and Wentzel-Kramers-Brillouin theory we identify quantum tunneling as the underlying mech- anism. These simulation results quantitatively reproduce the observed switching and show that in our systems these quantum dots are spatially separated from the continuum by > 10.5 nm.

cond-mat.mes-hall

Radio frequency occupancy state control of a single nanowire quantum dot

The excitonic occupancy state of a single, nanowire-based, heterostructure quantum dot is dynamically programmed by a surface acoustic wave. The quantum dot is formed by an interface or thickness fluctuation of a GaAs QW embedded in a AlGaAs shell of a GaAs-AlGaAs core-shell nanowire. As we tune the time at which carriers are photogenerated during the acoustic cycle, we find pronounced intensity oscillations of neutral and negatively charged excitons. At high acoustic power levels these oscillations become anticorrelated which enables direct acoustic programming of the dot's charge configuration, emission intensity and emission wavelength. Numerical simulations confirm that the observed modulations arise from acoustically controlled modulations of the electron and electron-hole-pair concentrations at the position of the quantum dot.

cond-mat.mes-hall

Acoustically regulated carrier injection into a single optically active quantum dot

We study the carrier injection into a single InGaAs/GaAs quantum dot regulated by a radio frequency surface acoustic wave. We find that the time of laser excitation during the acoustic cycle programs both the emission intensities and time of formation of neutral $(X^0)$ and negatively charged $(X^-)$ excitons. We identify underlying, characteristic formation pathways of both few-particle states in the time-domain experiments and show that both exciton species can be formed either with the optical pump or at later times by injection of single electrons and holes "surfing" the acoustic wave. All experimental observations are in excellent agreement with calculated electron and hole trajectories in the plane of the two-dimensional wetting layer which is dynamically modulated by the acoustically induced piezoelectric potentials. Taken together, our findings provide insight on both the onset of acousto-electric transport of electrons and holes and their conversion into the optical domain after regulated injection into a single quantum dot emitter.

cond-mat.mes-hall