Abrupt GaP/GaAs Interfaces in Self-Catalyzed Nanowires

We achieve the self-catalyzed growth of pure GaP nanowires and GaAs_1–<i>x</i>P_<i>x</i>/GaAs_1–<i>y</i>P_<i>y</i> nanowire heterostructures by solid-source molecular beam epitaxy. Consecutive segments of nearly pure GaAs and GaP are fabricated by commuting the group V fluxes. We test different flux switching procedures and measure the corresponding interfacial composition profiles with atomic resolution using high-angle annular dark field scanning transmission electron microscopy. Interface abruptness is drastically improved by switching off all the molecular beam fluxes for a short time at the group V commutation. Finally, we demonstrate that the morphology of the growth front can be either flat or truncated, depending on the growth conditions. The method presented here allows for the facile synthesis of high quality GaP/GaAs axial heterostructures directly on Si (111) wafers

Sharpening the Interfaces of Axial Heterostructures in Self-Catalyzed AlGaAs Nanowires: Experiment and Theory

The growth of III–III–V axial heterostructures in nanowires via the vapor–liquid–solid method is deemed to be unfavorable because of the high solubility of group III elements in the catalyst droplet. In this work, we study the formation by molecular beam epitaxy of self-catalyzed GaAs nanowires with Al_<i>x</i>Ga_1–<i>x</i>As insertions. The composition profiles are extracted and analyzed with monolayer resolution using high-angle annular dark-field scanning transmission electron microscopy. We test successfully several growth procedures to sharpen the heterointerfaces. For a given nanowire geometry, prefilling the droplet with Al atoms is shown to be the most efficient way to reduce the width of the GaAs/Al_<i>x</i>Ga_1–<i>x</i>As interface. Using the thermodynamic data available in the literature, we develop numerical and analytical models of the composition profiles, showing very good agreement with experiments. These models suggest that atomically sharp interfaces are attainable for catalyst droplets of small volumes

Measuring and Modeling the Growth Dynamics of Self-Catalyzed GaP Nanowire Arrays

The bottom-up fabrication of regular nanowire (NW) arrays on a masked substrate is technologically relevant, but the growth dynamic is rather complex due to the superposition of severe shadowing effects that vary with array pitch, NW diameter, NW height, and growth duration. By inserting GaAsP marker layers at a regular time interval during the growth of a self-catalyzed GaP NW array, we are able to retrieve precisely the time evolution of the diameter and height of a single NW. We then propose a simple numerical scheme which fully computes shadowing effects at play in infinite arrays of NWs. By confronting the simulated and experimental results, we infer that re-emission of Ga from the mask is necessary to sustain the NW growth while Ga migration on the mask must be negligible. When compared to random cosine or random uniform re-emission from the mask, the simple case of specular reflection on the mask gives the most accurate account of the Ga balance during the growth

Growth of Vertical GaAs Nanowires on an Amorphous Substrate via a Fiber-Textured Si Platform

We demonstrate the vertical self-catalyzed molecular beam epitaxy (MBE) growth of GaAs nanowires on an amorphous SiO₂ substrate by using a smooth [111] fiber-textured silicon thin film with very large grains, fabricated by aluminum-induced crystallization. This generic platform paves the way to the use of inexpensive substrates for the fabrication of dense ensembles of vertically standing nanowires (NWs) with promising perspectives for the integration of NWs in devices

Photon Cascade from a Single Crystal Phase Nanowire Quantum Dot

We report the first comprehensive experimental and theoretical study of the optical properties of single crystal phase quantum dots in InP nanowires. Crystal phase quantum dots are defined by a transition in the crystallographic lattice between zinc blende and wurtzite segments and therefore offer unprecedented potential to be controlled with atomic layer accuracy without random alloying. We show for the first time that crystal phase quantum dots are a source of pure single-photons and cascaded photon-pairs from type II transitions with excellent optical properties in terms of intensity and line width. We notice that the emission spectra consist often of two peaks close in energy, which we explain with a comprehensive theory showing that the symmetry of the system plays a crucial role for the hole levels forming hybridized orbitals. Our results state that crystal phase quantum dots have promising quantum optical properties for single photon application and quantum optics

Determination of n‑Type Doping Level in Single GaAs Nanowires by Cathodoluminescence

We present an effective method of determining the doping level in n-type III–V semiconductors at the nanoscale. Low-temperature and room-temperature cathodoluminescence (CL) measurements are carried out on single Si-doped GaAs nanowires. The spectral shift to higher energy (Burstein–Moss shift) and the broadening of luminescence spectra are signatures of increased electron densities. They are compared to the CL spectra of calibrated Si-doped GaAs layers, whose doping levels are determined by Hall measurements. We apply the generalized Planck’s law to fit the whole spectra, taking into account the electron occupation in the conduction band, the bandgap narrowing, and band tails. The electron Fermi levels are used to determine the free electron concentrations, and we infer nanowire doping of 6 × 10¹⁷ to 1 × 10¹⁸ cm^–3. These results show that cathodoluminescence provides a robust way to probe carrier concentrations in semiconductors with the possibility of mapping spatial inhomogeneities at the nanoscale

Morphology Tailoring and Growth Mechanism of Indium-Rich InGaN/GaN Axial Nanowire Heterostructures by Plasma-Assisted Molecular Beam Epitaxy

We investigate the growth mechanism of axially heterostructured InGaN/GaN nanowires (NWs) as a function of the flux conditions. The InGaN heterostructure morphology critically depends on the In/Ga flux ratio affecting the local V/III ratio at the NW growth front. Locally N-rich conditions are associated with tapered island-like morphologies, while metal-rich conditions, leading to the formation of a stable Indium adsorbed layer at the NW growth front, promote the growth of heterostructures with a disk-like shape. Based on experimental results and theoretical predictions, we demonstrate that this indium ad-layer acts as a surfactant inducing a modification of the InGaN heterostructure growth mode. The impact of flux conditions and strain relaxation on the Indium incorporation are also addressed. The resulting insertions present abrupt interfaces and a homogeneous In distribution for In contents up to 40%