Nonlinear imaging of nanostructures using beams with binary phase modulation.

We demonstrate nonlinear microscopy of oriented nanowires using excitation beams with binary phase modulation. A simple and intuitive optical scheme comprising a spatial light modulator gives us the possibility to control the phase across an incident Hermite-Gaussian beam of order (1,0) (HG10 mode). This technique allows us to gradually vary the spatial distribution of the longitudinal electric fields in the focal volume, as demonstrated by second-harmonic generation from vertically-aligned GaAs nanowires. These results open new opportunities for the full control of polarization in the focal volume to enhance light interaction with nanostructured materials.

Lithography-free shell-substrate isolation for core-shell GaAs nanowires.

A facile and scalable lithography-free technique(5) for the rapid construction of GaAs core-shell nanowires incorporating shell isolation from the substrate is reported. The process is based on interrupting NW growth and applying a thin spin-on-glass (SOG) layer to the base of the NWs and resuming core-shell NW growth. NW growth occurred in an atmospheric pressure metalorganic vapour phase epitaxy (MOVPE) system with gold nanoparticles used as catalysts for the vapour-liquid-solid growth. It is shown that NW axial core growth and radial shell growth can be resumed after interruption and even exposure to air. The SOG residues and native oxide layer that forms on the NW surface are shown to prevent or perturb resumption of epitaxial NW growth if not removed. Both HF etching and in situ annealing of the air-exposed NWs in the MOVPE were shown to remove the SOG residues and native oxide layer. While both procedures are shown capable of removing the native oxide and enabling resumption of epitaxial NW growth, in situ annealing produced the best results and allowed construction of pristine core-shell NWs. No growth occurred on SOG and it was observed that axial NW growth was more rapid when a SOG layer covered the substrate. The fabricated p-core/n-shell NWs exhibited diode behaviour upon electrical testing. The isolation of the NW shells from the substrate was confirmed by scanning electron microscopy and electrical measurements. The crystal quality of the regrown core-shell NWs was verified with a high resolution transmission electron microscope. The reported technique potentially provides a pathway using MOVPE for scalable and high-throughput production of shell-substrate isolated core-shell NWs on an industrial scale.

A technique for large-area position-controlled growth of GaAs nanowire arrays.

We demonstrate a technique for fabricating position-controlled, large-area arrays of vertical semiconductor nanowires (NWs) with adjustable periods and NW diameters. In our approach, a Au-covered GaAs substrate is first coated with a thin film of photoresponsive azopolymer, which is exposed twice to a laser interference pattern forming a 2D surface relief grating. After dry etching, an array of polymer islands is formed, which is used as a mask to fabricate a matrix of gold particles. The Au particles are then used as seeds in vapour-liquid-solid growth to create arrays of vertical GaAs NWs using metalorganic vapour phase epitaxy. The presented technique enables producing NWs of uniform size distribution with high throughput and potentially on large wafer sizes without relying on expensive lithography techniques. The feasibility of the technique is demonstrated by arrays of vertical NWs with periods of 255-1000 nm and diameters of 50-80 nm on a 2 × 2 cm area. The grown NWs exhibit high long range order and good crystalline quality. Although only GaAs NWs were grown in this study, in principle, the presented technique is suitable for any material available for Au seeded NW growth.

Wafer-scale self-organized InP nanopillars with controlled orientation for photovoltaic devices.

A unique wafer-scale self-organization process for generation of InP nanopillars is demonstrated, which is based on maskless ion-beam etching (IBE) of InP developed to obtain the nanopillars, where the height, shape, and orientation of the nanopillars can be varied by controlling the processing parameters. The fabricated InP nanopillars exhibit broadband suppression of the reflectance, 'black InP,' a property useful for solar cells. The realization of a conformal p-n junction for carrier collection, in the fabricated solar cells, is achieved by a metalorganic vapor phase epitaxy (MOVPE) overgrowth step on the fabricated pillars. The conformal overgrowth retains the broadband anti-reflection property of the InP nanopillars, indicating the feasibility of this technology for solar cells. Surface passivation of the formed InP nanopillars using sulfur-oleylamine solution resulted in improved solar-cell characteristics. An open-circuit voltage of 0.71 V and an increase of 0.13 V compared to the unpassivated device were achieved.

Fabrication of dual-type nanowire arrays on a single substrate.

A novel method for fabricating dual-type nanowire (NW) arrays is presented. Two growth steps, selective-area epitaxy (SAE) in the first step and vapor-liquid-solid (VLS) in the second step, are used to grow two types of NWs on the same GaAs substrate. Different precursors can be used for the growth steps, resulting in sophisticated compositional control, as demonstrated for side-by-side grown GaAs and InP NWs. It was found that parasitic growth occurs on the NWs already present on the substrate during the second growth step and that the SAE NWs shadow the growth of the VLS NWs. Optical reflectance measurements revealed the dual-type array having improved light trapping properties compared to single-type arrays. Dual-type NW arrays could be practical for thermoelectric generation, photovoltaics and sensing where composition control of side-by-side NWs and complex configurations are beneficial.

Second-harmonic generation imaging of semiconductor nanowires with focused vector beams.

We use second-harmonic generation (SHG) with focused vector beams to investigate individual vertically aligned GaAs nanowires. Our results provide direct evidence that SHG from oriented nanowires is mainly driven by the longitudinal field along the nanowire growth axis. Consequently, focused radial polarization provides a superior tool to characterize such nanowires compared to linear polarization, also allowing this possibility in the native growth environment. We model our experiments by describing the SHG process for zinc-blende structure and dipolar bulk nonlinearity.

Aluminum-Induced photoluminescence red shifts in core-shell GaAs/Al(x)Ga(1-x)As nanowires.

We report a new phenomenon related to Al-induced carrier confinement at the interface in core-shell GaAs/Al(x)Ga(1-x)As nanowires grown using metal-organic vapor phase epitaxy with Au as catalyst. All Al(x)Ga(1-x)As shells strongly passivated the GaAs nanowires, but surprisingly the peak photoluminescence (PL) position and the intensity from the core were found to be a strong function of Al composition in the shell at low temperatures. Large and systematic red shifts of up to ~66 nm and broadening in the PL emission from the GaAs core were observed when the Al composition in the shell exceeded 3%. On the contrary, the phenomenon was observed to be considerably weaker at the room temperature. Cross-sectional transmission electron microscopy reveals Al segregation in the shell along six Al-rich radial bands displaying a 3-fold symmetry. Time-resolved PL measurements suggest the presence of indirect electron-hole transitions at the interface at higher Al composition. We discuss all possibilities including a simple shell-core-shell model using simulations where the density of interface traps increases with the Al content, thus creating a strong local electron confinement. The carrier confinement at the interface is most likely related to Al inhomogeneity and/or Al-induced traps. Our results suggest that a low Al composition in the shell is desirable in order to achieve ideal passivation in GaAs nanowires.

High quality GaAs nanowires grown on glass substrates.

We report for the first time the growth of GaAs nanowires directly on low-cost glass substrates using atmospheric pressure metal organic vapor phase epitaxy via a vapor-liquid-solid mechanism with gold as catalyst. Substrates used in this work were of float glass type typically seen in household window glasses. Growth of GaAs nanowires on glass were investigated for growth temperatures between 410 and 580 °C. Perfectly cylindrical nontapered nanowires with a growth rate of ~33 nm/s were observed at growth temperatures of 450 and 470 °C, whereas highly tapered pillar-like wires were observed at 580 °C. Nanowires grew horizontally on the glass surface at 410 °C with a tendency to grow in vertically from the substrate as the growth temperature was increased. X-ray diffraction and transmission electron microscopy revealed that the nanowires have a perfect zinc blende structure with no planar structural defects or stacking faults. Strong photoluminescence emission was observed both at low temperature and room temperature indicating a high optical quality of GaAs nanowires. Growth comparison on impurity free fused silica substrate suggests unintentional doping of the nanowires from the glass substrate.