This thesis deals with the growth of GaAs nanowires (NWs) by molecular beam epitaxy (MBE) using vapor-liquid-solid method on various substrates including GaAs(111)B, Si(111) and graphene. The growth of the NWs on GaAs substrates was carried out by Au-catalyzed technique, whereas the growths on Si and graphene substrates were carried out using self-catalyzed technique that has been the main focus of this thesis. The long-term goal of this work was to produce p-n radial junction GaAs NWs for solar cell applications.Necessary conditions were established for obtaining vertical self-catalyzed GaAs NWs on Si(111), which is reproducible from run-to-run. One of the major issues in these NWs grown by both Au-and self-catalyzed techniques is their crystal structure. The Au-catalyzed GaAs NWs usually adopt a wurtzite (WZ) crystal phase, whereas the self-catalyzed NWs a zinc blende (ZB) phase. However, in both the cases the NWs contain stacking faults, rotational twins or/and a mixed crystal phase. The ZB and WZ phases show different optical properties, and one phase might be favored over other for certain applications. Therefore the crystal phase was controlled within single NWs by tuning the V/III ratio and introducing GaAsSb inserts. The change of the crystal phases was correlated with the change in the contact angle of the Ga droplet.Since the discovery of graphene, an ultra-thin two-dimensional material, the research on graphene has become an active field in recent years due to its remarkable properties including excellent electrical and thermal conductivities, mechanical strength and flexibility, and optical transparency. By growing the semiconductor NWs on graphene, a completely new hybrid system can be envisioned where the unique properties of both NWs and graphene can be utilized. Therefore we established a method for the growth of semiconductor NWs on graphene by demonstrating epitaxial growth of vertical GaAs and InAs NWs on different graphitic substrates.Core-shell heterostructure, doping, optical properties, and position controlled growth of self-catalyzed GaAs NWs were investigated. Growth of GaAs/GaAsSb coreshell NWs where the Sb content was tuned from about 10% -70% was studied. The effect of growth temperature and the Sb flux on the morphology of GaAsSb shell was investigated. In addition, by utilizing the core-shell geometry where the shell copies the crystal phase of the core, WZ phase of GaAsSb was demonstrated. Successful p-type doping of GaAs core using Be as dopant, and n-type doping of GaAs shell using Si and Te as dopants were achieved. To investigate the optical properties, GaAs/AlGaAs coreshell NWs were grown with different V/III ratios during the core growth. The NWs grown with high V/III ratio, despite containing a higher density of twinned ZB and WZ GaAs with SFs, were found to have superior optical quality as compared to the NWs grown with low V/III ratio that contain pure ZB GaAs. The observed V/III ratio dependent optical quality was correlated to the intrinsic defects such as As vac...

The optical properties of the wurtzite (WZ) GaAs crystal phase found in nanowires (NWs) are a highly controversial topic. Here, we study high-quality pure WZ GaAs/AlGaAs core-shell NWs grown by Au-assisted molecular beam epitaxy (MBE) with microphotoluminescence spectroscopy (μ-PL) and (scanning) transmission electron microscopy on the very same single wire. We determine the room temperature (294 K) WZ GaAs bandgap to be 1.444 eV, which is ∼20 meV larger than in zinc blende (ZB) GaAs, and show that the free exciton emission at 15 K is at 1.516 eV. On the basis of time- and temperature-resolved μ-PL results, we propose a Γ(8) conduction band symmetry in WZ GaAs. We suggest a method for quantifying the optical quality of NWs, taking into consideration the difference between the room and low temperature integrated PL intensity, and demonstrate that Au-assisted GaAs/AlGaAs core-shell NWs can have high PL brightness up to room temperature.

Semiconductor nanowire lasers can produce guided coherent light emission with miniaturized geometry, bringing about new possibilities for a variety of applications including nanophotonic circuits, optical sensing, and on-chip and chip-to-chip optical communications. Here, we report on the realization of single-mode and room-temperature lasing from 890 to 990 nm, utilizing a novel design of single nanowires with GaAsSb-based multiple axial superlattices as a gain medium under optical pumping. The control of lasing wavelength via compositional tuning with excellent room-temperature lasing performance is shown to result from the unique nanowire structure with efficient gain material, which delivers a low lasing threshold of ∼6 kW/cm (75 μJ/cm per pulse), a lasing quality factor as high as 1250, and a high characteristic temperature of ∼129 K. These results present a major advancement for the design and synthesis of nanowire laser structures, which can pave the way toward future nanoscale integrated optoelectronic systems with superior performance.

We report on a crystal phase-dependent photoluminescence (PL) polarization effect in individual wurtzite GaAs nanowires with a zinc blende GaAsSb insert grown by Au-assisted molecular beam epitaxy. The PL emission from the zinc blende GaAsSb insert is strongly polarized along the nanowire axis while the emission from the wurtzite GaAs nanowire is perpendicularly polarized. The results indicate that the crystal phases, through optical selection rules, are playing an important role in the alignment of the PL polarization in nanowires besides the linear polarization induced by the dielectric mismatch. The strong excitation power dependence and long recombination lifetimes ( approximately 4 ns) from the wurtzite GaAs and zinc blende GaAsSb-related PL emission strongly indicate the existence of type II band alignments in the nanowire due to the presence of nanometer thin zinc blende segments and stacking faults in the wurtzite GaAs barrier.

The many outstanding properties of graphene have impressed and intrigued scientists for the last few decades. Its transparency to light of all wavelengths combined with a low sheet resistance makes it a promising electrode material for novel optoelectronics. So far, no one has utilized graphene as both the substrate and transparent electrode of a functional optoelectronic device. Here, we demonstrate the use of double-layer graphene as a growth substrate and transparent conductive electrode for an ultraviolet light-emitting diode in a flip-chip configuration, where GaN/AlGaN nanocolumns are grown as the light emitting structure using plasma-assisted molecular beam epitaxy. Although the sheet resistance is increased after nanocolumn growth compared with pristine double-layer graphene, our experiments show that the double-layer graphene functions adequately as an electrode. The GaN/AlGaN nanocolumns are found to exhibit a high crystal quality with no observable defects or stacking faults. Room temperature electroluminescence measurements show a GaN related near bandgap emission peak at 365 nm and no defect-related yellow emission.

In this work we have investigated the variation of Sb concentration among and within zinc blende (ZB) GaAsSb inserts in wurtzite (WZ) GaAs bare-core and WZ GaAs/AlGaAs core-shell nanowires (NWs) grown by Au-assisted molecular beam epitaxy. The Sb concentration variation was related to the optical properties as determined by photoluminescence (PL). The NW structure and the Sb concentration were studied by transmission electron microscopy (TEM), energy dispersive x-ray spectroscopy (EDX) and quantitative high angle annular dark field scanning TEM (HAADF STEM). A clear trend relating the maximum Sb concentration with the insert length was observed: the longer the insert, the higher the Sb concentration. In addition, there are graded Sb concentration gradients both along and across the GaAsSb inserts. The influence of the Sb concentration variation on the PL emission from the GaAsSb inserts was investigated with correlated micro-PL and TEM-EDX on the same single NWs. Based on the PL results and the observed Sb concentration profiles, we propose a qualitative energy band diagram for a typical ZB GaAsSb insert in a WZ GaAs NW for the heterostructured NWs studied here. Type I transitions within the central region of the ZB GaAsSb inserts were found to dominate the insert-related PL emission. Weak type II transitions within the inserts due to the graded Sb concentration were observed as well. Using an existing empirical model, the Sb concentrations were additionally determined from the ground state PL energies (type I transition). For the average Sb concentration, the concentrations based on PL were in agreement with EDX and quantitative HAADF STEM results.

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The performance of GaAs nanowire (NW) devices depends critically on the presence of crystallographic defects in the NWs such as twinning planes and stacking faults, and considerable effort has been devoted to understanding and preventing the occurrence of these. For self-catalysed GaAs NWs grown by molecular beam epitaxy (MBE) in particular, there are in addition other types of defects that may be just as important for NW-based optoelectronic devices. These are the point defects such as the As vacancy and the Ga antisite occurring due to the inherently Ga-rich conditions of the self-catalysed growth. Here we demonstrate experimentally the effects of these point defects on the optical properties of GaAs/AlGaAs core-shell NWs grown by self-catalysed MBE. The present results enable insight into the role of the point defects both on their own and in conjunction with crystallographic planar defects.