Growth and Characterisation of GaAs/AlGaAs Core-shell Nanowires for Optoelectronic Device Applications
Creators: name: Jiang, Nian
Publisher: name: The Australian National University
Year: 2015
Subjects: Metal Organic Chemical Vapour Deposition
Nanowires
semiconductor
electron microscopy
microtomy
spectroscopy
GaAs

description: III-V semiconductor nanowires have been investigated as key components for future electronic and optoelectronic devices and systems due to their direct band gap and high electron mobility. Amongst the III-V semiconductors, the planar GaAs material system has been extensively studied and used in industries. Accordingly, GaAs nanowires are the prime candidates for nano-scale devices. However, the electronic performance of GaAs nanowires has yet to match that of state-of-the-art planar GaAs devices. The present deficiency of GaAs nanowires is typically attributed to the large surface-to- volume ratio and the tendency for non-radiative recombination centres to form at the surface. The favoured solution of this problem is by coating GaAs nanowires with AlGaAs shells, which replaces the GaAs surface with GaAs/AlGaAs interface. This thesis presents a systematic study of GaAs/AlGaAs core-shell nanowires grown by metal organic chemical vapour deposition (MOCVD), including understanding the growth, and characterisation of their structural and optical properties. The structures of the nanowires were mainly studied by scanning electron microscopy and transmis- sion electron microscopy (TEM). A procedure of microtomy was developed to prepare the cross-sectional samples for the TEM studies. The optical properties were charac- terised by photoluminescence (PL) spectroscopy. Carrier lifetimes were measured by time-resolved PL. The growth of AlGaAs shell was optimised to obtain the best optical properties, e.g. the strongest PL emission and the longest minority carrier lifetimes. The sidewalls of the vapour-liquid-solid (VLS) grown GaAs nanowires were investi- gated. It was found that a Reuleaux triangle with 3 {112}A curved surfaces is the actual shape of the nanowire at the growth interface. This Reuleaux triangle changes into well defined {112} facets as a result of the simultaneous radial growth. A theoretical model was developed to explain the orientations of nanowire sidewall facets. The sidewalls of GaAs nanowires were found to transform to {110} facets at high temperature as a result of surface atom migration. The rate of the facet transformation was found to be controlled by temperature and the difference in the surface energies, which leads to different faceting behaviour along the length of the nanowire. While the sidewalls of the top segment were fully transformed into {110} facets, the sidewalls of the bottom of the nanowires were a mixture of {110} and {112} facets. This facet-change along the length of the nanowire directly affected the subsequent growth of AlGaAs shell. This was relevant to the non-uniform PL emission and the minority carrier lifetimes (tmc) along the GaAs/AlGaAs core-shell nanowires. The strongest PL emission and longest tmc was observed where the GaAs core had six {110} facets. PL intensity and tmc decreased towards the bottom of the nanowire where the sidewall facets of the GaAs core consisted of both {110} and {112} facets. The effect of AlGaAs shell growth parameters (including V/III ratio, temperature and time) on the optical properties of GaAs/AlGaAs core-shell nanowires was investigated on nanowires catalysed by Au particles with a diameter of 50 nm. The V/III ratio and shell growth temperature were found to profoundly affect the optical properties. A high V/III ratio and/or a high growth temperature dramatically increased tmc. Further increasing the V/III ratio and/or growth temperature resulted in drop of tmc. Interme- diate V/III ratio and shell growth temperature were chosen as a compromise to achieve long tPL. The AlGaAs shell growth time also showed a significant effect on tmc. tmc increased with shell growth time to a maximum, followed by a further drop with longer shell growth time. With the optimised AlGaAs shell growth, an average carrier life- time of (1.02 ± 0.4) ns was achieved from single GaAs/AlGaAs core-shell nanowires at room temperature. This is comparable to self-assisted nanowires grown by molec- ular beam epitaxy and also proved that Au catalyst is not detrimental to the optical properties in VLS-grown GaAs nanowires. The long lifetimes are mainly attributed to the improvement of the GaAs/AlGaAs interface quality that is comparable with planar heterostructures. The effect of AlGaAs shell growth time and shell thickness on tPL were investigated. It was found that both the shell thickness and shell growth time affected tmc. A certain shell thickness is required to prevent the carriers generated in GaAs core from tunnelling through the AlGaAs shell and recombining at the free surface of GaAs cap layer. Beyond this thickness, the shell growth time, which is related to the diffusion at the heterointer- face, becomes the primary parameter controlling the carrier lifetimes. Lifetimes as long as 1.9 ns were achieved by reducing the effect of diffusion. This work presents an in-depth understanding of the geometry of GaAs nanowires, demonstrates GaAs/AlGaAs core-shell nanowires with optical quality comparable with planar heterostructures and reveals intriguing structural/optical behaviour of the nano- wires. These findings will greatly assist the fabrication of efficient nanowire devices and show a strong future for nano-optoelectronic devices based on nanowires.