High-Performance Multiwavelength GaNAs Single Nanowire Lasers.

In this study, we report a significant enhancement in the performance of GaNAs-based single nanowire lasers through optimization of growth conditions, leading to a lower lasing threshold and higher operation temperatures. Our analysis reveals that these improvements in the laser performance can be attributed to a decrease in the density of localized states within the material. Furthermore, we demonstrate that owing to their excellent nonlinear optical properties, these nanowires support self-frequency conversion of the stimulated emission through second harmonic generation (SHG) and sum-frequency generation (SFG), providing coherent light emission in the cyan-green range. Mode-specific differences in the self-conversion efficiency are revealed and explained by differences in the light extraction efficiency of the converted light caused by the electric field distribution of the fundamental modes. Our work, therefore, facilitates the design and development of multiwavelength coherent light generation and higher-temperature operation of GaNAs nanowire lasers, which will be useful in the fields of optical communications, sensing, and nanophotonics.

Wafer-scale integration of GaAs/AlGaAs core-shell nanowires on silicon by the single process of self-catalyzed molecular beam epitaxy.

GaAs/AlGaAs core-shell nanowires, typically having 250 nm diameter and 6 µm length, were grown on 2-inch Si wafers by the single process of molecular beam epitaxy using constituent Ga-induced self-catalysed vapor-liquid-solid growth. The growth was carried out without specific pre-treatment such as film deposition, patterning, and etching. The outermost Al-rich AlGaAs shells form a native oxide surface protection layer, which provides efficient passivation with elongated carrier lifetime. The 2-inch Si substrate sample exhibits a dark-colored feature due to the light absorption of the nanowires where the reflectance in the visible wavelengths is less than 2%. Homogeneous and optically luminescent and adsorptive GaAs-related core-shell nanowires were prepared over the wafer, showing the prospect for large-volume III-V heterostructure devices available with this approach as complementary device technologies for integration with silicon.

Designing Semiconductor Nanowires for Efficient Photon Upconversion via Heterostructure Engineering.

Energy upconversion via optical processes in semiconductor nanowires (NWs) is attractive for a variety of applications in nano-optoelectronics and nanophotonics. One of the main challenges is to achieve a high upconversion efficiency and, thus, a wide dynamic range of device performance, allowing efficient upconversion even under low excitation power. Here, we demonstrate that the efficiency of energy upconversion via two-photon absorption (TPA) can be drastically enhanced in core/shell NW heterostructures designed to provide a real intermediate TPA step via the band states of the narrow-bandgap region with a long carrier lifetime, fulfilling all the necessary requirements for high-efficiency two-step TPA. We show that, in radial GaAs(P)/GaNAs(P) core/shell NW heterostructures, the upconversion efficiency increases by 500 times as compared with that of the constituent materials, even under an excitation power as low as 100 mW/cm2 that is comparable to the 1 sun illumination. The upconversion efficiency can be further improved by 8 times through engineering the electric-field distribution of the excitation light inside the NWs so that light absorption is maximized within the desired region of the heterostructure. This work demonstrates the effectiveness of our approach in providing efficient photon upconversion by exploring core/shell NW heterostructures, yielding an upconversion efficiency being among the highest reported in semiconductor nanostructures. Furthermore, our work provides design guidelines for enhancing efficiency of energy upconversion in NW heterostructures.

Self-assembled nanodisks in coaxial GaAs/GaAsBi/GaAs core-multishell nanowires.

III-V semiconductor nanowires (NWs), such as those based on GaAs, are attractive for advanced optoelectronic and nanophotonic applications. The addition of Bi into GaAs offers a new avenue to enhance the near-infrared device performance and to add new functionalities, by utilizing the remarkable valence band structure and the giant bowing in the bandgap energy. Here, we report that alloying with Bi also induces the formation of optically-active self-assembled nanodisks caused by Bi segregation. They are located in the vicinity to the 112 corners of the GaAsBi shell and are restricted to twin planes. Furthermore, the Bi composition in the disks is found to correlate with their lateral thickness. The higher Bi composition in the disks with respect to the surrounding matrix provides a strong confinement for excitons along the NW axis, giving rise to narrow emission lines (<450 µeV) with the predominant emission polarization orthogonal to the NW axis. Our findings, therefore, open a new possibility to fabricate self-assembled quantum structures by combining advantages of dilute bismide alloys and lattice engineering in nanowires.

Effects of thermal annealing on localization and strain in core/multishell GaAs/GaNAs/GaAs nanowires.

Core/shell nanowire (NW) heterostructures based on III-V semiconductors and related alloys are attractive for optoelectronic and photonic applications owing to the ability to modify their electronic structure via bandgap and strain engineering. Post-growth thermal annealing of such NWs is often involved during device fabrication and can also be used to improve their optical and transport properties. However, effects of such annealing on alloy disorder and strain in core/shell NWs are not fully understood. In this work we investigate these effects in novel core/shell/shell GaAs/GaNAs/GaAs NWs grown by molecular beam epitaxy on (111) Si substrates. By employing polarization-resolved photoluminescence measurements, we show that annealing (i) improves overall alloy uniformity due to suppressed long-range fluctuations in the N composition; (ii) reduces local strain within N clusters acting as quantum dot emitters; and (iii) leads to partial relaxation of the global strain caused by the lattice mismatch between GaNAs and GaAs. Our results, therefore, underline applicability of such treatment for improving optical quality of NWs from highly-mismatched alloys. They also call for caution when using ex-situ annealing in strain-engineered NW heterostructures.

Controlling Bi-Provoked Nanostructure Formation in GaAs/GaAsBi Core-Shell Nanowires.

We control the formation of Bi-induced nanostructures on the growth of GaAs/GaAsBi core-shell nanowires (NWs). Bi serves as not only a constituent but also a surfactant and nanowire growth catalyst. Thus, we paved a way to achieve unexplored III-V nanostructures employing the characteristic supersaturation of catalyst droplets, structural modifications induced by strain, and incorporation into the host GaAs matrix correlated with crystalline defects and orientations. When Ga is deficient during growth, Bi accumulates on the vertex of core GaAs NWs and serves as a nanowire growth catalyst for the branched structures to azimuthal <112>. We find a strong correlation between Bi accumulation and stacking faults. Furthermore, Bi is preferentially incorporated on the GaAs (112)B surface, leading to spatially selective Bi incorporation into a confined area that has a Bi concentration of over 7%. The obtained GaAs/GaAsBi/GaAs heterostructure with an interface defined by the crystalline twin defects in a zinc-blende structure can be potentially applied to a quantum confined structure. Our finding provides a rational design concept for the creation of GaAsBi based nanostructures and the control of Bi incorporation beyond the fundamental limit.

Near-Infrared Lasing at 1 µm from a Dilute-Nitride-Based Multishell Nanowire.

A coherent photon source emitting at near-infrared (NIR) wavelengths is at the heart of a wide variety of applications ranging from telecommunications and optical gas sensing to biological imaging and metrology. NIR-emitting semiconductor nanowires (NWs), acting both as a miniaturized optical resonator and as a photonic gain medium, are among the best-suited nanomaterials to achieve such goals. In this study, we demonstrate the NIR lasing at 1 µm from GaAs/GaNAs/GaAs core/shell/cap dilute nitride nanowires with only 2.5% nitrogen. The achieved lasing is characterized by an S-shape pump-power dependence and narrowing of the emission line width. Through examining the lasing performance from a set of different single NWs, a threshold gain, gth, of 4100-4800 cm-1, was derived with a spontaneous emission coupling factor, ß, up to 0.8, which demonstrates the great potential of such nanophotonic material. The lasing mode was found to arise from the fundamental HE11a mode of the Fabry-Perot cavity from a single NW, exhibiting optical polarization along the NW axis. Based on temperature dependence of the lasing emission, a high characteristic temperature, T0, of 160 (±10) K is estimated. Our results, therefore, demonstrate a promising alternative route to achieve room-temperature NIR NW lasers thanks to the excellent alloy tunability and superior optical performance of such dilute nitride materials.

Annealing induced atomic rearrangements on (Ga,In) (N,As) probed by hard X-ray photoelectron spectroscopy and X-ray absorption fine structure.

We study the effects of annealing on (Ga0.64,In0.36) (N0.045,As0.955) using hard X-ray photoelectron spectroscopy and X-ray absorption fine structure measurements. We observed surface oxidation and termination of the N-As bond defects caused by the annealing process. Specifically, we observed a characteristic chemical shift towards lower binding energies in the photoelectron spectra related to In. This phenomenon appears to be caused by the atomic arrangement, which produces increased In-N bond configurations within the matrix, as indicated by the X-ray absorption fine structure measurements. The reduction in the binding energies of group-III In, which occurs concomitantly with the atomic rearrangements of the matrix, causes the differences in the electronic properties of the system before and after annealing.

GaAsBi/GaAs multi-quantum well LED grown by molecular beam epitaxy using a two-substrate-temperature technique.

We report a GaAs0.96Bi0.04/GaAs multiple quantum well (MQW) light emitting diode (LED) grown by molecular beam epitaxy using a two-substrate-temperature (TST) technique. In particular, the QWs and the barriers in the intrinsic region were grown at the different temperatures of [Formula: see text] = 350 °C and [Formula: see text] respectively. Investigations of the microstructure using transmission electron microscopy (TEM) reveal homogeneous MQWs free of extended defects. Furthermore, the local determination of the Bi distribution profile across the MQWs region using TEM techniques confirm the uniform Bi distribution, while revealing a slightly chemically graded GaAs-on-GaAsBi interface due to Bi surface segregation. Despite this small broadening, we found that Bi segregation is significantly reduced (up to 18% reduction) compared to previous reports on Bi segregation in GaAsBi/GaAs MQWs. Hence, the TST procedure proves as a very efficient method to reduce Bi segregation and thus increase the quality of the layers and interfaces. These improvements positively reflect in the optical properties. Room temperature photoluminescence and electroluminescence (EL) at 1.23 µm emission wavelength are successfully demonstrated using TST MQWs containing less Bi content than in previous reports. Finally, LED fabricated using the present TST technique show current-voltage (I-V) curves with a forward voltage of 3.3 V at an injection current of 130 mA under 1.0 kA cm-2 current excitation. These results not only demonstrate that TST technique provides optical device quality GaAsBi/GaAs MQWs but highlight the relevance of TST-based growth techniques on the fabrication of future heterostructure devices based on dilute bismides.

Dilute Nitride Nanowire Lasers Based on a GaAs/GaNAs Core/Shell Structure.

Nanowire (NW) lasers operating in the near-infrared spectral range are of significant technological importance for applications in telecommunications, sensing, and medical diagnostics. So far, lasing within this spectral range has been achieved using GaAs/AlGaAs, GaAs/GaAsP, and InGaAs/GaAs core/shell NWs. Another promising III-V material, not yet explored in its lasing capacity, is the dilute nitride GaNAs. In this work, we demonstrate, for the first time, optically pumped lasing from the GaNAs shell of a single GaAs/GaNAs core/shell NW. The characteristic "S"-shaped pump power dependence of the lasing intensity, with the concomitant line width narrowing, is observed, which yields a threshold gain, gth, of 3300 cm-1 and a spontaneous emission coupling factor, ß, of 0.045. The dominant lasing peak is identified to arise from the HE21b cavity mode, as determined from its pronounced emission polarization along the NW axis combined with theoretical calculations of lasing threshold for guided modes inside the nanowire. Even without intentional passivation of the NW surface, the lasing emission can be sustained up to 150 K. This is facilitated by the improved surface quality due to nitrogen incorporation, which partly suppresses the surface-related nonradiative recombination centers via nitridation. Our work therefore represents the first step toward development of room-temperature infrared NW lasers based on dilute nitrides with extended tunability in the lasing wavelength.

Metamorphic GaAs/GaAsBi Heterostructured Nanowires.

GaAs/GaAsBi coaxial multishell nanowires were grown by molecular beam epitaxy. Introducing Bi results in a characteristic nanowire surface morphology with strong roughening. Elemental mappings clearly show the formation of the GaAsBi shell with inhomogeneous Bi distributions within the layer surrounded by the outermost GaAs, having a strong structural disorder at the wire surface. The nanowire exhibits a predominantly ZB structure from the bottom to the middle part. The polytipic WZ structure creates denser twin defects in the upper part than in the bottom and middle parts of the nanowire. We observe room temperature cathodoluminescence from the GaAsBi nanowires with a broad spectral line shape between 1.1 and 1.5 eV, accompanied by multiple peaks. A distinct energy peak at 1.24 eV agrees well with the energy of the reduced GaAsBi alloy band gap by the introduction of 2% Bi. The existence of localized states energetically and spatially dispersed throughout the NW are indicated from the low temperature cathodoluminescence spectra and images, resulting in the observed luminescence spectra characterized by large line widths at low temperatures as well as by the appearance of multiple peaks at high temperatures and for high excitation powers.

Suppression of non-radiative surface recombination by N incorporation in GaAs/GaNAs core/shell nanowires.

III-V semiconductor nanowires (NWs) such as GaAs NWs form an interesting artificial materials system promising for applications in advanced optoelectronic and photonic devices, thanks to the advantages offered by the 1D architecture and the possibility to combine it with the main-stream silicon technology. Alloying of GaAs with nitrogen can further enhance performance and extend device functionality via band-structure and lattice engineering. However, due to a large surface-to-volume ratio, III-V NWs suffer from severe non-radiative carrier recombination at/near NWs surfaces that significantly degrades optical quality. Here we show that increasing nitrogen composition in novel GaAs/GaNAs core/shell NWs can strongly suppress the detrimental surface recombination. This conclusion is based on our experimental finding that lifetimes of photo-generated free excitons and free carriers increase with increasing N composition, as revealed from our time-resolved photoluminescence (PL) studies. This is accompanied by a sizable enhancement in the PL intensity of the GaAs/GaNAs core/shell NWs at room temperature. The observed N-induced suppression of the surface recombination is concluded to be a result of an N-induced modification of the surface states that are responsible for the nonradiative recombination. Our results, therefore, demonstrate the great potential of incorporating GaNAs in III-V NWs to achieve efficient nano-scale light emitters.

Selective synthesis of compound semiconductor/oxide composite nanowires.

Semiconductor/oxide composite nanowires (NWs) were synthesized by molecular beam epitaxial growth and subsequent wet oxidation. Nonselective and selective oxidation conditions applied to the GaAs/AlGaAs core-shell NWs grown on silicon substrates produced GaOx/AlGaOx and GaAs/AlGaOx NWs, respectively. The oxidized amorphous AlGaOx shell produced cathodoluminescence over a wide spectral range encompassing ultraviolet and visible wavelengths, possibly sourced from molecular species related to oxygen. The wire core was buried in the oxides when the diameter of the oxide shell increased, forming a planar structure. These composites are expected to pave the way to future electrical and optical functions for NWs.

Growth of dilute nitride GaAsN/GaAs heterostructure nanowires on Si substrates.

The concept of band engineering dilute nitride semiconductors into nanowires is introduced. Using plasma-assisted molecular beam epitaxy, dilute nitride GaAsN/GaAs heterostructure nanowires are grown on silicon (111) substrates. Growth of the nanowires under high As overpressure results in a regular wire diameter of 350 nm with a length exceeding 3 µm. The GaAsN/GaAs nanowires show characteristics including favorable vertical alignment, hexagonal cross-sectional structure with {110} facets, regions of wurtzite and zinc-blende phases, and a core-shell-type heterostructure. The nanowires are composed of GaAsN shells containing up to 0.3% nitrogen surrounding GaAs cores. Panchromatic cathodoluminescence images show intensity modulation along the length of the nanowires that is possibly related to the interfaces of wurtzite/zinc-blende regions. Photoluminescence with peak wavelengths between 870 and 920 nm is clearly observed at room temperature. The spectral red shift depends on the amount of introduced nitrogen. These results reveal a method for precise lattice and band engineering of nanowires composed of dilute nitride semiconductors.

Epitaxial lift-off for sample preparation of x-ray absorption fine structure.

We propose a simple sample preparation technique of x-ray absorption fine structure (XAFS) for its application to the individual layer of practical compound semiconductor devices. An epitaxial lift-off process enables the investigation of pure uppermost thin epitaxial layer without containing information of the bottom-side layers as well as substrate. The plain procedure offers smooth thin film with desired thickness preserving its crystallographic structure, suitable for the measurement. We carry out XAFS measurements for 2.0 and 0.2 microm thick GaAs epitaxial layer at transmission and fluorescence mode, respectively. Clear extended-XAFS oscillation is obtained, and the radial distribution function of which deduces accurate first nearest-neighbor Ga-As bond length to be 2.46 A for both the samples. That shows the feasibility of the proposed technique for the analysis of the precise atomic configurations of thin film semiconductors.