Sb-saturated high-temperature growth of extended, self-catalyzed GaAsSb nanowires on silicon with high quality
P. Schmiedeke, M. Dblinger, M. A. Meinhold-Heerlein, C. Doganlar, J. J. Finley, G. Koblmüller
Nanotechnology 35 (5), 55601 (2024).
Ternary GaAsSb nanowires (NW) are key materials for integrated high-speed photonic applications on silicon (Si), where homogeneous, high aspect-ratio dimensions and high-quality properties for controlled absorption, mode confinement and waveguiding are much desired. Here, we demonstrate a unique high-temperature (high-T >650 degrees C) molecular beam epitaxial (MBE) approach to realize self-catalyzed GaAsSb NWs site-selectively on Si with high aspect-ratio and non-tapered morphologies under antimony (Sb)-saturated conditions. While hitherto reported low-moderate temperature growth processes result in early growth termination and inhomogeneous morphologies, the non-tapered nature of NWs under high-T growth is independent of the supply rates of relevant growth species. Analysis of dedicated Ga-flux and growth time series, allows us to pinpoint the microscopic mechanisms responsible for the elimination of tapering, namely concurrent vapor-solid, step-flow growth along NW side-facets enabled by enhanced Ga diffusion under the high-T growth. Performing growth in an Sb-saturated regime, leads to high Sb-content in VLS-GaAsSb NW close to 30% that is independent of Ga-flux. This independence enables multi-step growth via sequentially increased Ga-flux to realize uniform and very long (>7 mu m) GaAsSb NWs. The excellent properties of these NWs are confirmed by a completely phase-pure, twin-free zincblende (ZB) crystal structure, a homogeneous Sb-content along the VLS-GaAsSb NW growth axis, along with remarkably narrow, single-peak low-temperature photoluminescence linewidth (<15 meV) at wavelengths of similar to 1100-1200 nm.
Axial Growth Characteristics of Optically Active InGaAs Nanowire Heterostructures for Integrated Nanophotonic Devices
H. W. Jeong, A. Ajay, M. Döblinger, S. Sturm, M. G. Ruiz, R. Zell, N. Mukhundhan, D. Stelzner, J. Lähnemann, K. Müller-Caspary, J. J. Finley, G. Koblmüller
Acs Applied Nano Materials 7 (3), 3032-3041 (2024).
III-V semiconductor nanowire (NW) heterostructures with axial InGaAs active regions hold large potential for diverse on-chip device applications, including site-selectively integrated quantum light sources, NW lasers with high material gain, as well as resonant tunneling diodes and avalanche photodiodes. Despite various promising efforts toward high-quality single or multiple axial InGaAs heterostacks using noncatalytic growth mechanisms, the important roles of facet-dependent shape evolution, crystal defects, and the applicability to more universal growth schemes have remained elusive. Here, we report the growth of optically active InGaAs axial NW heterostructures via completely catalyst-free, selective-area molecular beam epitaxy directly on silicon (Si) using GaAs-(Sb) NW arrays as tunable, high-uniformity growth templates and highlight fundamental relationships between structural, morphological, and optical properties of the InGaAs region. Structural, compositional, and 3D-tomographic characterizations affirm the desired directional growth along the NW axis with no radial growth observed. Clearly distinct luminescence from the InGaAs active region is demonstrated, where tunable array-geometry parameters and In content up to 20% are further investigated. Based on the underlying twin-induced growth mode, we further describe the facet-dependent shape and interface evolution of the InGaAs segment and its direct correlation with emission energy.
Self-Induced Ultrafast Electron-Hole-Plasma Temperature Oscillations in Nanowire Lasers
A. Thurn, J. Bissinger, S. Meinecke, P. Schmiedeke, S. S. Oh, W. W. Chow, K. Lüdge, G. Koblmüller, J. J. Finley
Physical Review Applied 20 (3), 34045 (2023).
Nanowire lasers can be monolithically and site-selectively integrated onto silicon photonic circuits. To assess their full potential for ultrafast optoelectronic 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 have 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 optimised approaches for ultrafast intensity and phase modulation of chip-integrated semiconductor lasers at the nanoscale.
Structural properties of graded In x Ga 1-x As metamorphic buffer layers for quantum dots emitting in the telecom bands
B. Scaparra, A. Ajay, P. S. Avdienko, Y. Y. Xue, H. Riedl, P. Kohl, B. Jonas, B. Costa, E. Sirotti, P. Schmiedeke, V. Villafañe, I. D. Sharp, E. Zallo, G. Koblmüller, J. J. Finley, K. Müller
Materials for Quantum Technology 3 (3), 35004 (2023).
In recent years, there has been a significant increase in interest in tuning the emission wavelength of InAs quantum dots (QDs) to wavelengths compatible with the already existing silica fiber networks. In this work, we develop and explore compositionally graded In x Ga 1-x As metamorphic buffer layers (MBLs), with lattice constant carefully tailored to tune the emission wavelengths of InAs QDs towards the telecom O-band. The designed heterostructure is grown by molecular beam epitaxy (MBE), where a single layer of InAs QDs is grown on top of the MBL and is capped with a layer having a fixed indium (In) content. We investigate the structural properties of the grown MBLs by reciprocal space mapping, as well as transmission electron microscopy, and verify the dependence of the absorption edge of the MBL on the In-content by photothermal deflection spectroscopy measurements. This allows us to identify a growth temperature range for which the MBLs achieve a near-equilibrium strain relaxation for In-content up to similar to 30 % . Furthermore, we explore the emission wavelength tunability of QDs grown on top of a residual strained layer with a low density of dislocations. Specifically, we demonstrate a characteristic red-shift of the QD photoluminescence towards the telecom O-band (1300 nm) at low temperature. This study provides insights into the relaxation profiles and dislocation propagation in compositionally graded MBLs grown via MBE thus paving the way for realizing MBE-grown heterostructures containing InAs QDs for advanced nanophotonic devices emitting in the telecom bands.
Sb-Mediated Tuning of Growth- and Exciton Dynamics in Entirely Catalyst-Free GaAsSb Nanowires
H. W. Jeong, A. Ajay, H. T. Yu, M. Döblinger, N. Mukhundhan, J. J. Finley, G. Koblmüller
Small 19 (16), 12 (2023).
Vapor-liquid-solid (VLS) growth is the mainstream method in realizing advanced semiconductor nanowires (NWs), as widely applied to many III-V compounds. It is exclusively explored also for antimony (Sb) compounds, such as the relevant GaAsSb-based NW materials, although morphological inhomogeneities, phase segregation, and limitations in the supersaturation due to Sb strongly inhibit their growth dynamics. Fundamental advances are now reported here via entirely catalyst-free GaAsSb NWs, where particularly the Sb-mediated effects on the NW growth dynamics and physical properties are investigated in this novel growth regime. Remarkably, depending on GaAsSb composition and nature of the growth surface, both surfactant and anti-surfactant action is found, as seen by transitions between growth acceleration and deceleration characteristics. For threshold Sb-contents up to 3-4%, adatom diffusion lengths are increased approximate to sevenfold compared to Sb-free GaAs NWs, evidencing the significant surfactant effect. Furthermore, microstructural analysis reveals unique Sb-mediated transitions in compositional structure, as well as substantial reduction in twin defect density, approximate to tenfold over only small compositional range (1.5-6% Sb), exhibiting much larger dynamics as found in VLS-type GaAsSb NWs. The effect of such extended twin-free domains is corroborated by approximate to threefold increases in exciton lifetime (approximate to 4.5 ns) due to enlarged electron-hole pair separation in these phase-pure NWs.
Enhanced growth and properties of non-catalytic GaAs nanowires via Sb surfactant effects
A. Ajay, H. Jeong, T. Schreitmueller, M. Doeblinger, D. Ruhstorfer, N. Mukhundhan, P. Koolen, J. J. Finley, G. Koblmüller
Applied Physics Letters 121 (7), 72107 (2022).
We report the effects of antimony (Sb) surfactant on the growth and correlated structural and optical properties of non-catalytic GaAs nanowires (NW) grown by selective area epitaxy on silicon. Strong enhancements in the axial growth with very high aspect ratio up to 50 are observed by the addition of small traces of Sb (1%-2%), contrasting the commonly reported growth limiting behavior of Sb in GaAs(Sb) NWs. The Sb surfactant effect modifies the growth facet structure from a pyramidal-shaped growth front terminated by {1-1-0} planes to a flat (111)B growth plane, that is even further improved by the presence of Si co-dopants. Additional benefits are seen by the substantial change in microstructure, from a heavily defected layer stacking in Sb-free GaAs NWs to a twinned phase-pure zinc blende structure in Sb-mediated GaAs(Sb) NWs. We directly confirm the impact of the altered microstructure on the optical emission and carrier recombination dynamics via observation of long, few-ns carrier lifetimes in the GaAs(Sb) NWs using steady-state and time-resolved photoluminescence spectroscopy. (C) 2022 Author(s).
Purcell enhanced coupling of nanowire quantum emitters to silicon photonic waveguides
N. Mukhundhan, A. Ajay, J. Bissinger, J. J. Finley, G. Koblmüller
Optics Express 29 (26), 43068-43081 (2021).
We design a quantum dot (QD) embedded in a vertical-cavity photonic nanowire (NW), deterministically integrated on a silicon-on-insulator (SOI) waveguide (WG), as a novel quantum light source in a quantum photonic integrated circuit (QPIC). Using a broadband QD emitter, we perform finite-difference time domain simulations to systematically tune key geometrical parameters and to explore the coupling mechanisms of the emission to the NW and WG modes. We find distinct Fabry-Perot resonances in the Purcell enhanced emission that govern the outcoupled power into the fundamental TE mode of the SOI-WG. With an optimized geometry that places the QD emitter in a finite NW in close proximity to the WG, we obtain peak outcoupling efficiencies for polarized emission as high as eighty percent. (C) 2021 Optical Society of America under the terms of the OSA Open Access Publishing Agreement.
Charge-neutral nonlocal response in superconductor-InAs nanowire hybrid devices
A. O. Denisov, A. V. Bubis, S. U. Piatrusha, N. A. Titova, A. G. Nasibulin, J. Becker, J. Treu, D. Ruhstorfer, G. Koblmüller, E. S. Tikhonov, V. S. Khrapai
Semiconductor Science and Technology 36 (9), 09lt04 (2021).
Nonlocal quasiparticle transport in normal-superconductor-normal (NSN) hybrid structures probes sub-gap states in the proximity region and is especially attractive in the context of Majorana research. Conductance measurement provides only partial information about nonlocal response composed from both electron-like and hole-like quasiparticle excitations. In this work, we show how a nonlocal shot noise measurement delivers a missing puzzle piece in NSN InAs nanowire-based devices. We demonstrate that in a trivial superconducting phase quasiparticle response is practically charge-neutral, dominated by the heat transport component with a thermal conductance being on the order of conductance quantum. This is qualitatively explained by numerous Andreev reflections of a diffusing quasiparticle, that makes its charge completely uncertain. Consistently, strong fluctuations and sign reversal are observed in the sub-gap nonlocal conductance, including occasional Andreev rectification signals. Our results prove conductance and noise as complementary measurements to characterize quasiparticle transport in superconducting proximity devices.
Ultrathin catalyst-free InAs nanowires on silicon with distinct 1D sub-band transport properties
F. del Giudice, J. Becker, C. de Rose, M. Doblinger, D. Ruhstorfer, L. Suomenniemi, J. Treu, H. Riedl, J. J. Finley, G. Koblmüller
Nanoscale 12 (42), 21857-21868 (2020).
Ultrathin InAs nanowires (NW) with a one-dimensional (1D) sub-band structure are promising materials for advanced quantum-electronic devices, where dimensions in the sub-30 nm diameter limit together with post-CMOS integration scenarios on Si are much desired. Here, we demonstrate two site-selective synthesis methods that achieve epitaxial, high aspect ratio InAs NWs on Si with ultrathin diameters below 20 nm. The first approach exploits direct vapor-solid growth to tune the NW diameter by interwire spacing, mask opening size and growth time. The second scheme explores a unique reverse-reaction growth by which the sidewalls of InAs NWs are thermally decomposed under controlled arsenic flux and annealing time. Interesting kinetically limited dependencies between interwire spacing and thinning dynamics are found, yielding diameters as low as 12 nm for sparse NW arrays. We clearly verify the 1D sub-band structure in ultrathin NWs by pronounced conductance steps in low-temperature transport measurements using back-gated NW-field effect transistors. Correlated simulations reveal single- and double degenerate conductance steps, which highlight the rotational hexagonal symmetry and reproduce the experimental traces in the diffusive 1D transport limit. Modelling under the realistic back-gate configuration further evidences regimes that lead to asymmetric carrier distribution and breakdown of the degeneracy depending on the gate bias.
Quantum-confinement enhanced thermoelectric properties in modulation-doped GaAs-AlGaAs core-shell nanowires
S. Fust, A. Faustmann, D. J. Carrad, J. Bissinger, B. Loitsch, M. Döblinger, J. Becker, G. Abstreiter, J. J. Finley, G. Koblmueller
Advanced Materials 32, 1905458 (2019).
Nanowires (NWs) hold great potential in advanced thermoelectrics due to their reduced dimensions and low-dimensional electronic character. However, unfavorable links between electrical and thermal conductivity in state-of-the-art unpassivated NWs have, so far, prevented the full exploitation of their distinct advantages. A promising model system for a surface-passivated one-dimensional (1D)-quantum confined NW thermoelectric is developed that enables simultaneously the observation of enhanced thermopower via quantum oscillations in the thermoelectric transport and a strong reduction in thermal conductivity induced by the core–shell heterostructure. High-mobility modulation-doped GaAs/AlGaAs core–shell NWs with thin (sub-40 nm) GaAs NW core channel are employed, where the electrical and thermoelectric transport is characterized on the same exact 1D-channel. 1D-sub-band transport at low temperature is verified by a discrete stepwise increase in the conductance, which coincided with strong oscillations in the corresponding Seebeck voltage that decay with increasing sub-band number. Peak Seebeck coefficients as high as ≈65–85 µV K−1 are observed for the lowest sub-bands, resulting in equivalent thermopower of S2σ ≈ 60 µW m−1 K−2 and S2G ≈ 0.06 pW K−2 within a single sub-band. Remarkably, these core–shell NW heterostructures also exhibit thermal conductivities as low as ≈3 W m−1 K−1, about one order of magnitude lower than state-of-the-art unpassivated GaAs NWs.
Breakdown of corner states and carrier localization by monolayer fluctuations in a radial nanowire quantum wells
M. M. Sonner, A. Sitek, L. Janker, D. Rudolph, D. Ruhstorfer, M. Döblinger, A. Manolescu, G. Abstreiter, J. J. Finley, A. Wixforth, G. Koblmueller, H. J. Krenner
Nano Lett. 19 (5), 3336-3343 (2019).
We report a comprehensive study of the impact of the structural properties in radial GaAs-Al0.3Ga0.7As nanowire-quantum well heterostructures on the optical recombination dynamics and electrical transport properties, emphasizing particularly the role of the commonly observed variations of the quantum well thickness at different facets. Typical thickness fluctuations of the radial quantum well observed by transmission electron microscopy lead to pronounced localization. Our optical data exhibit clear spectral shifts and a multipeak structure of the emission for such asymmetric ring structures resulting from spatially separated, yet interconnected quantum well systems. Charge carrier dynamics induced by a surface acoustic wave are resolved and prove efficient carrier exchange on native, subnanosecond time scales within the heterostructure. Experimental findings are corroborated by theoretical modeling, which unambiguously show that electrons and holes localize on facets where the quantum well is the thickest and that even minute deviations of the perfect hexagonal shape strongly perturb the commonly assumed 6-fold symmetric ground state.