Model of a GaAs Quantum Dot in a Direct Band Gap AlGaAs Wurtzite Nanowire.

We present a study with a numerical model based on k→·p→, including electromechanical fields, to evaluate the electromechanical and optoelectronic properties of single GaAs quantum dots embedded in direct band gap AlGaAs nanowires. The geometry and the dimensions of the quantum dots, in particular the thickness, are obtained from experimental data measured by our group. We also present a comparison between the experimental and numerically calculated spectra to support the validity of our model.

Photoluminescence Redistribution of InGaN Nanowires Induced by Plasmonic Silver Nanoparticles.

Hybrid nanostructures based on InGaN nanowires with decorated plasmonic silver nanoparticles are investigated in the present study. It is shown that plasmonic nanoparticles induce the redistribution of room temperature photoluminescence between short-wavelength and long-wavelength peaks of InGaN nanowires. It is defined that short-wavelength maxima decreased by 20%, whereas the long-wavelength maxima increased by 19%. We attribute this phenomenon to the energy transfer and enhancement between the coalesced part of the NWs with 10-13% In content and the tips above with an In content of about 20-23%. A proposed Fröhlich resonance model for silver NPs surrounded by a medium with refractive index of 2.45 and spread 0.1 explains the enhancement effect, whereas the decreasing of the short-wavelength peak is associated with the diffusion of charge carriers between the coalesced part of the NWs and the tips above.

Self-assembled photonic structure: a Ga optical antenna on GaP nanowires.

Semiconductor nanowires are the perfect platform for nanophotonic applications owing to their resonant, waveguiding optical properties and technological capabilities providing control over their crystalline and chemical compositions. The vapor-liquid-solid growth mechanism allows the formation of hybrid metal-dielectric nanostructures promoting sub-wavelength light manipulation. In this work, we explore both experimentally and numerically the plasmonic effects promoted by a gallium (Ga) nanoparticle optical antenna decorating the facet of gallium phosphide (GaP) nanowires. Raman, photoluminescence and near-field mapping techniques are used to study the effects. We demonstrate several phenomena including field enhancement, antenna effect and increase in internal reflection. We show that the observed effects have to be considered when nanowires with a plasmonic particle are used in nanophotonic circuits and discuss the ways for utilization of these effects for efficient coupling of light into nanowire waveguide and field tailoring. The results open up promising pathways for the development of both passive and active nanophotonic elements, light harvesting and sensorics.

Direct Band Gap AlGaAs Wurtzite Nanowires.

Wurtzite AlGaAs is a technologically promising yet unexplored material. Here we study it both experimentally and numerically. We develop a complete numerical model based on an 8-band k→·p→ method, including electromechanical fields, and calculate the optoelectronic properties of wurtzite AlGaAs nanowires with different Al content. We then compare them with our experimental data. Our results strongly suggest that wurtzite AlGaAs is a direct band gap material. Moreover, we have also numerically obtained the band gap of wurtzite AlAs and the valence band offset between AlAs and GaAs in the wurtzite symmetry.

Selective Area Epitaxy of GaN Nanowires on Si Substrates Using Microsphere Lithography: Experiment and Theory.

GaN nanowires were grown using selective area plasma-assisted molecular beam epitaxy on SiOx/Si(111) substrates patterned with microsphere lithography. For the first time, the temperature-Ga/N2 flux ratio map was established for selective area epitaxy of GaN nanowires. It is shown that the growth selectivity for GaN nanowires without any parasitic growth on a silica mask can be obtained in a relatively narrow range of substrate temperatures and Ga/N2 flux ratios. A model was developed that explains the selective growth range, which appeared to be highly sensitive to the growth temperature and Ga flux, as well as to the radius and pitch of the patterned pinholes. High crystal quality in the GaN nanowires was confirmed through low-temperature photoluminescence measurements.

Anisotropic Radiation in Heterostructured "Emitter in a Cavity" Nanowire.

Tailorable synthesis of axially heterostructured epitaxial nanowires (NWs) with a proper choice of materials allows for the fabrication of novel photonic devices, such as a nanoemitter in the resonant cavity. An example of the structure is a GaP nanowire with ternary GaPAs insertions in the form of nano-sized discs studied in this work. With the use of the micro-photoluminescence technique and numerical calculations, we experimentally and theoretically study photoluminescence emission in individual heterostructured NWs. Due to the high refractive index and near-zero absorption through the emission band, the photoluminescence signal tends to couple into the nanowire cavity acting as a Fabry-Perot resonator, while weak radiation propagating perpendicular to the nanowire axis is registered in the vicinity of each nano-sized disc. Thus, within the heterostructured nanowire, both amplitude and spectrally anisotropic photoluminescent signals can be achieved. Numerical modeling of the nanowire with insertions emitting in infrared demonstrates a decay in the emission directivity and simultaneous rise of the emitters coupling with an increase in the wavelength. The emergence of modulated and non-modulated radiation is discussed, and possible nanophotonic applications are considered.

Purcell Effect and Beaming of Emission in Hybrid AlGaAs Nanowires with GaAs Quantum Dots.

Control of directionality of emissions is an important task for the realization of novel nanophotonic devices based on nanowires. Most of the existing approaches providing high directionality of the light emitted from nanowires are based on the utilization of the tapered shape of nanowires, serving as nanoantenna coupling with the light waveguided in nanowire and the directional output beam. Here we report the beaming of the emitted light with wavelength near 800 nm by naturally formed core-shell AlGaAs NW with multiply GaAs quantum dots (QDs) diameter 30 nm and height 10 nm, while the diameter of NW 130 nm, what does not support efficient emission into waveguided modes, including the mode HE11. Experimental measurements show that intensity of emission for directions in the vicinity of the axis of NW is about two orders of magnitude higher than for perpendicular directions. The developed theoretical approach allowed us to calculate the probability of spontaneous emission for various directions and into waveguided modes and showed that highly directional radiation can be provided by the intrinsic emission properties of cylindrical NW. Our results suggest that for the small diameter of NW, directional emissions are associated with an TM0 leaky mode (when electric field oriented in axial direction) and therefore manifests in an existence of axial electric dipole transitions in quantum dots.

Red GaPAs/GaP Nanowire-Based Flexible Light-Emitting Diodes.

We demonstrate flexible red light-emitting diodes based on axial GaPAs/GaP heterostructured nanowires embedded in polydimethylsiloxane membranes with transparent electrodes involving single-walled carbon nanotubes. The GaPAs/GaP axial nanowire arrays were grown by molecular beam epitaxy, encapsulated into a polydimethylsiloxane film, and then released from the growth substrate. The fabricated free-standing membrane of light-emitting diodes with contacts of single-walled carbon nanotube films has the main electroluminescence line at 670 nm. Membrane-based light-emitting diodes (LEDs) were compared with GaPAs/GaP NW array LED devices processed directly on Si growth substrate revealing similar electroluminescence properties. Demonstrated membrane-based red LEDs are opening an avenue for flexible full color inorganic devices.

Tailoring Morphology and Vertical Yield of Self-Catalyzed GaP Nanowires on Template-Free Si Substrates.

Tailorable synthesis of III-V semiconductor heterostructures in nanowires (NWs) enables new approaches with respect to designing photonic and electronic devices at the nanoscale. We present a comprehensive study of highly controllable self-catalyzed growth of gallium phosphide (GaP) NWs on template-free silicon (111) substrates by molecular beam epitaxy. We report the approach to form the silicon oxide layer, which reproducibly provides a high yield of vertical GaP NWs and control over the NW surface density without a pre-patterned growth mask. Above that, we present the strategy for controlling both GaP NW length and diameter independently in single- or two-staged self-catalyzed growth. The proposed approach can be extended to other III-V NWs.

Effect of crystal structure on the Young's modulus of GaP nanowires.

Young's modulus of tapered mixed composition (zinc-blende with a high density of twins and wurtzite with a high density of stacking faults) gallium phosphide (GaP) nanowires (NWs) was investigated by atomic force microscopy. Experimental measurements were performed by obtaining bending profiles of as-grown inclined GaP NWs deformed by applying a constant force to a series of NW surface locations at various distances from the NW/substrate interface. Numerical modeling of experimental data on bending profiles was done by applying Euler-Bernoulli beam theory. Measurements of the nano-local stiffness at different distances from the NW/substrate interface revealed NWs with a non-ideal mechanical fixation at the NW/substrate interface. Analysis of the NWs with ideally fixed base resulted in experimentally measured Young's modulus of 155 ± 20 GPa for ZB NWs, and 157 ± 20 GPa for WZ NWs, respectively, which are in consistence with a theoretically predicted bulk value of 167 GPa. Thus, impacts of the crystal structure (WZ/ZB) and crystal defects on Young's modulus of GaP NWs were found to be negligible.

Multi-colour light emission from InGaN nanowires monolithically grown on Si substrate by MBE.

InGaN nanostructures are among the most promising candidates for visible solid-state lighting and renewable energy sources. To date, there is still a lack of information about the influence of the growth conditions on the physical properties of these nanostructures. Here, we extend the study of InGaN nanowires growth directly on Si substrates by plasma-assisted molecular beam epitaxy. The results of the study showed that under appropriate growth conditions a change in the growth temperature of just 10 °C leads to a significant change in the structural and optical properties of the nanowires. InGaN nanowires with the areas containing 4%-10% of In with increasing tendency towards the top are formed at the growth temperature of 665 °C, while at the growth temperatures range of 655 °C-660 °C the spontaneously core-shell NWs are typically presented. In the latter case, the In contents in the core and the shell are about an order of magnitude different (e.g. 35% and 4% for 655 °C, respectively). The photoluminescence study of the NWs demonstrates a shift in the spectra from blue to orange in accordance with an increase of In content. Based on these results, a novel approach to the monolithic growth of InxGa1-xN NWs with multi-colour light emission on Si substrates by setting a temperature gradient over the substrate surface is proposed.

Influence of TOPO and TOPO-CdSe/ZnS Quantum Dots on Luminescence Photodynamics of InP/InAsP/InPHeterostructure Nanowires.

The passivation influence by ligands coverage with trioctylphosphine oxide (TOPO) and TOPO including colloidal CdSe/ZnS quantum dots (QDs) on optical properties of the semiconductor heterostructure, namely an array of InP nanowires (NWs) with InAsP nanoinsertion grown by Au-assisted molecular beam epitaxy on Si (111) substrates, was investigated. A significant dependence of the photoluminescence (PL) dynamics of the InAsP insertions on the ligand type was shown, which was associated with the changes in the excitation translation channels in the heterostructure. This change was caused by a different interaction of the ligand shells with the surface of InP NWs, which led to the formation of different interfacial low-energy states at the NW-ligand boundary, such as surface-localized antibonding orbitals and hybridized states that were energetically close to the radiating state and participate in the transfer of excitation. It was shown that the quenching of excited states associated with the capture of excitation to interfacial low-energy traps was compensated by the increasing role of the "reverse transfer" mechanism. As a result, the effectiveness of TOPO-CdSe/ZnS QDs as a novel surface passivation coating was demonstrated.

Structural and Optical Properties of Self-Catalyzed Axially Heterostructured GaPN/GaP Nanowires Embedded into a Flexible Silicone Membrane.

Controlled growth of heterostructured nanowires and mechanisms of their formation have been actively studied during the last decades due to perspectives of their implementation. Here, we report on the self-catalyzed growth of axially heterostructured GaPN/GaP nanowires on Si(111) by plasma-assisted molecular beam epitaxy. Nanowire composition and structural properties were examined by means of Raman microspectroscopy and transmission electron microscopy. To study the optical properties of the synthesized nanoheterostructures, the nanowire array was embedded into the silicone rubber membrane and further released from the growth substrate. The reported approach allows us to study the nanowire optical properties avoiding the response from the parasitically grown island layer. Photoluminescence and Raman studies reveal different nitrogen content in nanowires and parasitic island layer. The effect is discussed in terms of the difference in vapor solid and vapor liquid solid growth mechanisms. Photoluminescence studies at low temperature (5K) demonstrate the transition to the quasi-direct gap in the nanowires typical for diluted nitrides with low N-content. The bright room temperature photoluminescent response demonstrates the potential application of nanowire/polymer matrix in flexible optoelectronic devices.

Low-Temperature In-Induced Holes Formation in Native-SiOx/Si(111) Substrates for Self-Catalyzed MBE Growth of GaAs Nanowires.

The reduction of substrate temperature is important in view of the integration of III-V materials with a Si platform. Here, we show the way to significantly decrease substrate temperature by introducing a procedure to create nanoscale holes in the native-SiOx layer on Si(111) substrate via In-induced drilling. Using the fabricated template, we successfully grew self-catalyzed GaAs nanowires by molecular-beam epitaxy. Energy-dispersive X-ray analysis reveals no indium atoms inside the nanowires. This unambiguously manifests that the procedure proposed can be used for the growth of ultra-pure GaAs nanowires.

Effect of the Uniaxial Compression on the GaAs Nanowire Solar Cell.

Research regarding ways to increase solar cell efficiency is in high demand. Mechanical deformation of a nanowire (NW) solar cell can improve its efficiency. Here, the effect of uniaxial compression on GaAs nanowire solar cells was studied via conductive atomic force microscopy (C-AFM) supported by numerical simulation. C-AFM I-V curves were measured for wurtzite p-GaAs NW grown on p-Si substrate. Numerical simulations were performed considering piezoresistance and piezoelectric effects. Solar cell efficiency reduction of 50% under a -0.5% strain was observed. The analysis demonstrated the presence of an additional fixed electrical charge at the NW/substrate interface, which was induced due to mismatch between the crystal lattices, thereby affecting the efficiency. Additionally, numerical simulations regarding the p-n GaAs NW solar cell under uniaxial compression were performed, showing that solar efficiency could be controlled by mechanical deformation and configuration of the wurtzite and zinc blende p-n segments in the NW. The relative solar efficiency was shown to be increased by 6.3% under -0.75% uniaxial compression. These findings demonstrate a way to increase efficiency of GaAs NW-based solar cells via uniaxial mechanical compression.

Control of Conductivity of InxGa1-xAs Nanowires by Applied Tension and Surface States.

The electronic properties of semiconductor AIIIBV nanowires (NWs) due to their high surface/volume ratio can be effectively controlled by NW strain and surface electronic states. We study the effect of applied tension on the conductivity of wurtzite InxGa1-xAs (x ∼ 0.8) NWs. Experimentally, conductive atomic force microscopy is used to measure the I-V curves of vertically standing NWs covered by native oxide. To apply tension, the microscope probe touching the NW side is shifted laterally to produce a tensile strain in the NW. The NW strain significantly increases the forward current in the measured I-V curves. When the strain reaches 4%, the I-V curve becomes almost linear, and the forward current increases by 3 orders of magnitude. In the latter case, the tensile strain is supposed to shift the conduction band minima below the Fermi level, whose position, in turn, is fixed by surface states. Consequently, the surface conductivity channel appears. The observed effects confirm that the excess surface arsenic is responsible for the Fermi level pinning at oxidized surfaces of III-As NWs.

Nanowire Quantum Dots Tuned to Atomic Resonances.

Quantum dots tuned to atomic resonances represent an emerging field of hybrid quantum systems where the advantages of quantum dots and natural atoms can be combined. Embedding quantum dots in nanowires boosts these systems with a set of powerful possibilities, such as precise positioning of the emitters, excellent photon extraction efficiency and direct electrical contacting of quantum dots. Notably, nanowire structures can be grown on silicon substrates, allowing for a straightforward integration with silicon-based photonic devices. In this work we show controlled growth of nanowire-quantum-dot structures on silicon, frequency tuned to atomic transitions. We grow GaAs quantum dots in AlGaAs nanowires with a nearly pure crystal structure and excellent optical properties. We precisely control the dimensions of quantum dots and their position inside nanowires and demonstrate that the emission wavelength can be engineered over the range of at least 30 nm around 765 nm. By applying an external magnetic field, we are able to fine-tune the emission frequency of our nanowire quantum dots to the D2 transition of 87Rb. We use the Rb transitions to precisely measure the actual spectral line width of the photons emitted from a nanowire quantum dot to be 9.4 ± 0.7 µeV, under nonresonant excitation. Our work brings highly desirable functionalities to quantum technologies, enabling, for instance, a realization of a quantum network, based on an arbitrary number of nanowire single-photon sources, all operating at the same frequency of an atomic transition.

Unified mechanism of the surface Fermi level pinning in III-As nanowires.

Fermi level pinning at the oxidized (110) surfaces of III-As nanowires (GaAs, InAs, InGaAs, AlGaAs) is studied. Using scanning gradient Kelvin probe microscopy, we show that the Fermi level at oxidized cleavage surfaces of ternary Al x Ga1-x As (0 ≤ x ≤ 0.45) and Ga x In1-x As (0 ≤ x ≤ 1) alloys is pinned at the same position of 4.8 ± 0.1 eV with regard to the vacuum level. The finding implies a unified mechanism of the Fermi level pinning for such surfaces. Further investigation, performed by Raman scattering and photoluminescence spectroscopy, shows that photooxidation of the Al x Ga1-x As and Ga x In1-x As nanowires leads to the accumulation of an excess of arsenic on their crystal surfaces which is accompanied by a strong decrease of the band-edge photoluminescence intensity. We conclude that the surface excess arsenic in crystalline or amorphous forms is responsible for the Fermi level pinning at oxidized (110) surfaces of III-As nanowires.

Anapoles in Free-Standing III-V Nanodisks Enhancing Second-Harmonic Generation.

Nonradiating electromagnetic configurations in nanostructures open new horizons for applications due to two essential features: a lack of energy losses and invisibility to the propagating electromagnetic field. Such radiationless configurations form a basis for new types of nanophotonic devices, in which a strong electromagnetic field confinement can be achieved together with lossless interactions between nearby components. In our work, we present a new design of free-standing disk nanoantennas with nonradiating current distributions for the optical near-infrared range. We show a novel approach to creating nanoantennas by slicing III-V nanowires into standing disks using focused ion-beam milling. We experimentally demonstrate the suppression of the far-field radiation and the associated strong enhancement of the second-harmonic generation from the disk nanoantennas. With a theoretical analysis of the electromagnetic field distribution using multipole expansions in both spherical and Cartesian coordinates, we confirm that the demonstrated nonradiating configurations are anapoles. We expect that the presented procedure of designing and producing disk nanoantennas from nanowires becomes one of the standard approaches to fabricating controlled chains of standing nanodisks with different designs and configurations. These chains can be essential building blocks for new types of lasers and sensors with low power consumption.

Dopant-stimulated growth of GaN nanotube-like nanostructures on Si(111) by molecular beam epitaxy.

In this paper we study growth of quasi-one-dimensional GaN nanowires (NWs) and nanotube (NT)-like nanostructures on Si(111) substrates covered with a thin AlN layer grown by means of plasma-assisted molecular beam epitaxy. In the first part of our study we investigate the influence of the growth parameters on the geometrical properties of the GaN NW arrays. First, we find that the annealing procedure carried out prior to deposition of the AlN buffer affects the elongation rate and the surface density of the wires. It has been experimentally demonstrated that the NW elongation rate and the surface density drastically depend on the substrate growth temperature, where 800 °C corresponds to the maximum elongation rate of the NWs. In the second part of the study, we introduce a new dopant-stimulated method for GaN nanotube-like nanostructure synthesis using a high-intensity Si flux. Transmission electron microscopy was used to investigate the morphological features of the GaN nanostructures. The synthesized structures have a hexagonal cross-section and possess high crystal quality. We propose a theoretical model of the novel nanostructure formation which includes the role of the dopant Si. Some of the Si-doped samples were studied with the photoluminescence (PL) technique. The analysis of the PL spectra shows that the highest value of donor concentration in the nanostructures exceeds 5∙1019 cm-3.