Selectivity Map for Molecular Beam Epitaxy of Advanced III-V Quantum Nanowire Networks.

Selective-area growth is a promising technique for enabling of the fabrication of the scalable III-V nanowire networks required to test proposals for Majorana-based quantum computing devices. However, the contours of the growth parameter window resulting in selective growth remain undefined. Herein, we present a set of experimental techniques that unambiguously establish the parameter space window resulting in selective III-V nanowire networks growth by molecular beam epitaxy. Selectivity maps are constructed for both GaAs and InAs compounds based on in situ characterization of growth kinetics on GaAs(001) substrates, where the difference in group III adatom desorption rates between the III-V surface and the amorphous mask area is identified as the primary mechanism governing selectivity. The broad applicability of this method is demonstrated by the successful realization of high-quality InAs and GaAs nanowire networks on GaAs, InP, and InAs substrates of both (001) and (111)B orientations as well as homoepitaxial InSb nanowire networks. Finally, phase coherence in Aharonov-Bohm ring experiments validates the potential of these crystals for nanoelectronics and quantum transport applications. This work should enable faster and better nanoscale crystal engineering over a range of compound semiconductors for improved device performance.

Three-dimensional magneto-photoluminescence as a probe of the electronic properties of crystal-phase quantum disks in GaAs nanowires.

Crystal-phase engineering has emerged as a novel method of bandgap engineering, made feasible by the high surface-to-volume ratio of nanowires. There remains intense debate about the exact characteristics of the band structure of the novel crystal phases, such as wurtzite GaAs, obtained by this approach. We attack this problem via a low-temperature angle-dependent magneto-photoluminescence study of wurtzite/zinc-blende quantum disks in single GaAs nanowires. The exciton diamagnetic coefficient is proportional to the electron-hole correlation length, enabling a determination of the spatial extent of the exciton wave function in the plane and along the confinement axis of the crystal-phase quantum disks. Depending on the disk nature, the diamagnetic coefficient measured in Faraday geometry ranges between 25 and 75 µeV/T(2). For a given disk, the diamagnetic coefficient remains constant upon rotation of the magnetic field. Along with our envelope function calculation accounting for excitonic effects, we demonstrate that the electron effective mass in wurtzite GaAs quantum disks is heavy, mostly isotropic and results from mixing of the two lower-energy conduction bands with Γ7 and Γ8 symmetries. Finally, we discuss the implications of the results of the angle dependent magneto-luminescence for the likely symmetry of the exciton states. This work provides important insight in the band structure of wurtzite GaAs for future nanowire-based polytypic bandgap engineering.

Pressure tuning of the optical properties of GaAs nanowires.

The tuning of the optical and electronic properties of semiconductor nanowires can be achieved by crystal phase engineering. Zinc-blende and diamond semiconductors exhibit pressure-induced structural transitions as well as a strong pressure dependence of the band gaps. When reduced to nanoscale dimensions, new phenomena may appear. We demonstrate the tuning of the optical properties of GaAs nanowires and the induction of a phase transition by applying an external pressure. The dependence of the E(0) gap on the applied pressure was measured, and a direct-to-indirect transition was found. Resonant Raman scattering was obtained by pressure tuning of the E(0) and the E(0) + Δ(SO) gaps with respect to the excitation energy. The resonances of the longitudinal optical modes LO and 2LO indicate the presence of electron-phonon Fröhlich interactions. These measurements show for the first time a variation of ionicity in GaAs when in nanowire form. Furthermore, the dependence of the lattice constant on applied pressure was estimated. Finally, we found a clear indication of a structural transition above 16 GPa.

Suppression of three dimensional twinning for a 100% yield of vertical GaAs nanowires on silicon.

Multiple seed formation by three-dimensional twinning at the initial stages of growth explains the manifold of orientations found when self-catalyzed GaAs nanowires grow on silicon. This mechanism can be tuned as a function of the growth conditions by changing the relative size between the GaAs seed and the Ga droplet. We demonstrate how growing under high V/III ratio results in a 100% yield of vertical nanowires on silicon(111). These results open up the avenue towards the efficient integration of III-V nanowire arrays on the silicon platform.

Mobility and carrier density in p-type GaAs nanowires measured by transmission Raman spectroscopy.

The unambiguous measurement of carrier concentration and mobility in semiconductor nanowires remains a challenging task. This is a consequence of their one-dimensional nature and the incompatibility with Hall or van der Pauw measurements. We propose a method that allows the direct determination of mobility and carrier concentration in nanowires in a contact-less manner. We demonstrate how forward Raman scattering enables the measurement of phonon-plasmon interactions. By applying this method to p-type GaAs nanowires, we were able to directly obtain values of the carrier concentration between 3.0 × 10(17) and 7.4 × 10(18) cm(-3) and a mobility of 31 cm(2) (V s)(-1) at room temperature. This study opens the path towards the study of plasmon-phonon interactions in semiconductor nanowires.

Untangling the electronic band structure of wurtzite GaAs nanowires by resonant Raman spectroscopy.

In semiconductor nanowires, the coexistence of wurtzite and zinc-blende phases enables the engineering of the electronic structure within a single material. This presupposes an exact knowledge of the band structure in the wurtzite phase. We demonstrate that resonant Raman scattering is a important tool to probe the electronic structure of novel materials. Exemplarily, we use this technique to elucidate the band structure of wurtzite GaAs at the Γ point. Within the experimental uncertainty we find that the free excitons at the edge of the wurtzite and the zinc-blende band gap exhibit equal energies. For the first time we show that the conduction band minimum in wurtzite GaAs is of Γ(7) symmetry, meaning a small effective mass. We further find evidence for a light-hole-heavy-hole splitting of 103 meV at 10 K.

Three-dimensional multiple-order twinning of self-catalyzed GaAs nanowires on Si substrates.

In this paper we introduce a new paradigm for nanowire growth that explains the unwanted appearance of parasitic nonvertical nanowires. With a crystal structure polarization analysis of the initial stages of GaAs nanowire growth on Si substrates, we demonstrate that secondary seeds form due to a three-dimensional twinning phenomenon. We derive the geometrical rules that underlie the multiple growth directions observed experimentally. These rules help optimizing nanowire array devices such as solar or water splitting cells or of more complex hierarchical branched nanowire devices.

In(Ga)As quantum dot formation on group-III assisted catalyst-free InGaAs nanowires.

Growth of GaAs and In(x)Ga(1-x)As nanowires by the group-III assisted molecular beam epitaxy growth method on (001)GaAs/SiO(2) substrates is studied in dependence on growth temperature, with the objective of maximizing the indium incorporation. Nanowire growth was achieved for growth temperatures as low as 550 °C. The incorporation of indium was studied by low temperature micro-photoluminescence spectroscopy, Raman spectroscopy and electron energy loss spectroscopy. The results show that the incorporation of indium achieved by lowering the growth temperature does not have the effect of increasing the indium concentration in the bulk of the nanowire, which is limited to 3-5%. For growth temperatures below 575 °C, indium rich regions form at the surface of the nanowires as a consequence of the radial growth. This results in the formation of quantum dots, which exhibit spectrally narrow luminescence.

InAs quantum dot arrays decorating the facets of GaAs nanowires.

InAs quantum dot arrays are obtained on GaAs nanowire facets by molecular beam epitaxy. The GaAs nanowires are first grown by the gallium-assisted catalyst-free method. Decoration of the nanowire facets with InAs quantum dots is achieved only when the facets are capped with an ultrathin AlAs layer, as demonstrated by atomic force, high-resolution electron microscopy, and energy-dispersive X-ray spectroscopy line scans. The excitation of single and double excitons in the quantum dots are demonstrated by low-temperature photoluminescence spectroscopy realized on the single nanowires. This new type of heterostructures opens a new avenue to the fabrication of highly efficient single-photon sources, novel quantum optics experiments, as well as the realization of intermediate-band nanowire solar cells for third-generation photovoltaics.

P-doping mechanisms in catalyst-free gallium arsenide nanowires.

Doped catalyst-free GaAs nanowires have been grown by molecular beam epitaxy with the gallium-assisted method. The spatial dependence of the dopant concentration and resistivity have been measured by Raman spectroscopy and four point electrical measurements. Along with theoretical considerations, the doping mechanisms have been revealed. Two competing mechanisms have been revealed: dopant incorporation from the side facets and from the gallium droplet. In the latter incorporation path, doping compensation seems to play an important role in the effective dopant concentration. Hole concentrations of at least 2.4 x 10(18) cm(-3) have been achieved, which to our knowledge is the largest p doping range obtained up to date. This work opens the avenue for the use of doped GaAs nanowires in advanced applications and in mesoscopic physics experiments.

Controlled synthesis of InAs wires, dot and twin-dot array configurations by cleaved edge overgrowth.

We present experimental results on the controlled synthesis of InAs ordered nanostructures with three different grades of complexity: nanowires, quantum dot arrays, and double quantum dot arrays. A model for the diffusion of In adatoms on (110) surfaces explains the observed ordering and establishes general criteria for the optimized fabrication of the three different InAs nanostructure configurations, as a function of the growth conditions. These results are important for the use of ordered InAs nanostructures in future optoelectronic applications.