Strong Terahertz Emission and Its Origin from Catalyst-Free InAs Nanowire Arrays

The unique features of nanowires (NW), such as the high aspect ratio and extensive surface area, are expected to play a key role in the development of very efficient semiconductor surface emitters in the terahertz (THz) spectral range. Here, we report on optically excited THz emission from catalyst-free grown arrays of intrinsically n-type InAs NWs using THz time-domain spectroscopy. Depending on the aspect ratio, the THz emission efficiency of the n-type InAs NWs is found to be up to ∼3 times stronger than that of bulk p-type InAs, known as currently the most efficient semiconductor-based THz surface emitter. Characteristic differences from bulk p-type InAs are particularly revealed from excitation wavelength-dependent measurements, showing monotonously increasing THz pulse amplitude in the NW arrays with increasing photon energy. Further polarization-dependent and two-color pump–probe experiments elucidate the physical mechanism of the THz emission: In contrast to bulk p-type InAs, where the anisotropic photoconductivity in the surface electric field is the dominant cause for THz pulse generation, the origin of the intrinsic THz emission in the NWs is based on the photo-Dember effect. The strong THz emission from high aspect ratio NW arrays further suggests an improved out-coupling of the radiation, while further enhancements in efficiency using core–shell NW geometries are discussed

Connecting Composition-Driven Faceting with Facet-Driven Composition Modulation in GaAs–AlGaAs Core–Shell Nanowires

Ternary III–V alloys of tunable bandgap are a foundation for engineering advanced optoelectronic devices based on quantum-confined structures including quantum wells, nanowires, and dots. In this context, core–shell nanowires provide useful geometric degrees of freedom in heterostructure design, but alloy segregation is frequently observed in epitaxial shells even in the absence of interface strain. High-resolution scanning transmission electron microscopy and laser-assisted atom probe tomography were used to investigate the driving forces of segregation in nonplanar GaAs–AlGaAs core–shell nanowires. Growth-temperature-dependent studies of Al-rich regions growing on radial {112} nanofacets suggest that facet-dependent bonding preferences drive the enrichment, rather than kinetically limited diffusion. Observations of the distinct interface faceting when pure AlAs is grown on GaAs confirm the preferential bonding of Al on {112} facets over {110} facets, explaining the decomposition behavior. Furthermore, three-dimensional composition profiles generated by atom probe tomography reveal the presence of Al-rich nanorings perpendicular to the growth direction; correlated electron microscopy shows that short zincblende insertions in a nanowire segment with predominantly wurtzite structure are enriched in Al, demonstrating that crystal phase engineering can be used to modulate composition. The findings suggest strategies to limit alloy decomposition and promote new geometries of quantum confined structures

Hot Electron Dynamics in InAs–AlAsSb Core–Shell Nanowires

Semiconductor nanowires (NWs) have shown evidence of robust hot-carrier effects due to their small dimensions, making them attractive for advanced photoenergy conversion concepts. Especially, indium arsenide (InAs) NWs are promising candidates for harvesting hot carriers due to their high absorption coefficient, high carrier mobility, and large effective electron-to-hole mass difference. Here, we investigate the cooling and recombination dynamics of photoexcited hot carriers in pure and passivated InAs NWs by using ultrafast near-infrared pump–probe spectroscopy. We observe reduced Auger recombination in pure InAs NWs compared to that in passivated ones and associate this with charge-carrier separation by surface band bending. Similarly, faster carrier cooling by electron–hole scattering is observed in passivated InAs–AlAsSb NWs at high carrier densities in excess of 1018 cm–3, where hot electron lifetimes in this regime increase substantially with the pump fluence due to Auger heating. These results emphasize the importance of type-II alignment for charge-carrier separation in hot-carrier devices to suppress carrier-mediated cooling channels. In addition, a separate charge-carrier population lasting up to several nanoseconds is observed for photoexcitation of the NW shell. Despite the high conduction band offset, carrier migration is not observed in the range of 40 ps to 2 ns. This observation may open avenues for core–shell NW multijunction solar cells

3D Bragg Coherent Diffraction Imaging of Extended Nanowires: Defect Formation in Highly Strained InGaAs Quantum Wells

InGaAs quantum wells embedded in GaAs nanowires can serve as compact near-infrared emitters for direct integration onto Si complementary metal oxide semiconductor technology. While the core–shell geometry in principle allows for a greater tuning of composition and emission, especially farther into the infrared, the practical limits of elastic strain accommodation in quantum wells on multifaceted nanowires have not been established. One barrier to progress is the difficulty of directly comparing the emission characteristics and the precise microstructure of a single nanowire. Here we report an approach to correlating quantum well morphology, strain, defects, and emission to understand the limits of elastic strain accommodation in nanowire quantum wells specific to their geometry. We realize full 3D Bragg coherent diffraction imaging (BCDI) of intact quantum wells on vertically oriented epitaxial nanowires, which enables direct correlation with single-nanowire photoluminescence. By growing In0.2Ga0.8As quantum wells of distinct thicknesses on different facets of the same nanowire, we identified the critical thickness at which defects are nucleated. A correlation with a traditional transmission electron microscopy analysis confirms that BCDI can image the extended structure of defects. Finite element simulations of electron and hole states explain the emission characteristics arising from strained and partially relaxed regions. This approach, imaging the 3D strain and microstructure of intact nanowire core–shell structures with application-relevant dimensions, can aid the development of predictive models that enable the design of new compact infrared emitters

Metawissen - domainabhaengig oder domainunabhaengig?

SIGLETIB: RO 684 (15) / FIZ - Fachinformationszzentrum Karlsruhe / TIB - Technische InformationsbibliothekDEGerman

Crystal Phase Quantum Dots in the Ultrathin Core of GaAs–AlGaAs Core–Shell Nanowires

Semiconductor quantum dots embedded in nanowires (NW-QDs) can be used as efficient sources of nonclassical light with ultrahigh brightness and indistinguishability, needed for photonic quantum information technologies. Although most NW-QDs studied so far focus on heterostructure-type QDs that provide an effective electronic confinement potential using chemically distinct regions with dissimilar electronic structure, homostructure NWs can localize excitons at crystal phase defects in leading to NW-QDs. Here, we optically investigate QD emitters embedded in GaAs–AlGaAs core–shell NWs, where the excitons are confined in an ultrathin-diameter NW core and localized along the axis of the NW core at wurtzite (WZ)/zincblende (ZB) crystal phase defects. Photoluminescence (PL)-excitation measurements performed on the QD-emission reveal sharp resonances arising from excited electronic states of the axial confinement potential. The QD-like nature of the emissive centers are suggested by the observation of a narrow PL line width, as low as ∼300 μeV, and confirmed by the observation of clear photon antibunching in autocorrelation measurements. Most interestingly, time-resolved PL measurements reveal a very short radiative lifetime <1 ns, indicative of a transition from a type-II to type-I band alignment of the WZ/ZB crystal interface in GaAs due to the strong quantum confinement in the ultrathin NW core

Correlated Chemical and Electrically Active Dopant Analysis in Catalyst-Free Si-Doped InAs Nanowires

Direct correlations between dopant incorporation, distribution, and their electrical activity in semiconductor nanowires (NW) are difficult to access and require a combination of advanced nanometrology methods. Here, we present a comprehensive investigation of the chemical and electrically active dopant concentrations in n-type Si-doped InAs NW grown by catalyst-free molecular beam epitaxy using various complementary techniques. N-type carrier concentrations are determined by Seebeck effect measurements and four-terminal NW field-effect transistor characterization and compared with the Si dopant distribution analyzed by local electrode atom probe tomography. With increased dopant supply, a distinct saturation of the free carrier concentration is observed in the mid-10¹⁸ cm^–3 range. This behavior coincides with the incorporated Si dopant concentrations in the bulk part of the NW, suggesting the absence of compensation effects. Importantly, excess Si dopants with very high concentrations (>10²⁰ cm^–3) segregate at the NW sidewall surfaces, which confirms recent first-principles calculations and results in modifications of the surface electronic properties that are sensitively probed by field-effect measurements. These findings are expected to be relevant also for doping studies of other noncatalytic III–V NW systems

Axial Growth Characteristics of Optically Active InGaAs Nanowire Heterostructures for Integrated Nanophotonic Devices

III–V semiconductor nanowire (NW) heterostructures with axial InGaAs active regions hold large potential for diverse on-chip device applications, including site-selectively integrated quantum light sources, NW lasers with high material gain, as well as resonant tunneling diodes and avalanche photodiodes. Despite various promising efforts toward high-quality single or multiple axial InGaAs heterostacks using noncatalytic growth mechanisms, the important roles of facet-dependent shape evolution, crystal defects, and the applicability to more universal growth schemes have remained elusive. Here, we report the growth of optically active InGaAs axial NW heterostructures via completely catalyst-free, selective-area molecular beam epitaxy directly on silicon (Si) using GaAs(Sb) NW arrays as tunable, high-uniformity growth templates and highlight fundamental relationships between structural, morphological, and optical properties of the InGaAs region. Structural, compositional, and 3D-tomographic characterizations affirm the desired directional growth along the NW axis with no radial growth observed. Clearly distinct luminescence from the InGaAs active region is demonstrated, where tunable array–geometry parameters and In content up to 20% are further investigated. Based on the underlying twin-induced growth mode, we further describe the facet-dependent shape and interface evolution of the InGaAs segment and its direct correlation with emission energy

Lattice-Matched InGaAs–InAlAs Core–Shell Nanowires with Improved Luminescence and Photoresponse Properties

Core–shell nanowires (NW) have become very prominent systems for band engineered NW heterostructures that effectively suppress detrimental surface states and improve performance of related devices. This concept is particularly attractive for material systems with high intrinsic surface state densities, such as the low-bandgap In-containing group-III arsenides, however selection of inappropriate, lattice-mismatched shell materials have frequently caused undesired strain accumulation, defect formation, and modifications of the electronic band structure. Here, we demonstrate the realization of closely lattice-matched radial InGaAs–InAlAs core–shell NWs tunable over large compositional ranges [<i>x</i>(Ga)∼<i>y</i>(Al) = 0.2–0.65] via completely catalyst-free selective-area molecular beam epitaxy. On the basis of high-resolution X-ray reciprocal space maps the strain in the NW core is found to be insignificant (ε < 0.1%), which is further reflected by the absence of strain-induced spectral shifts in luminescence spectra and nearly unmodified band structure. Remarkably, the lattice-matched InAlAs shell strongly enhances the optical efficiency by up to 2 orders of magnitude, where the efficiency enhancement scales directly with increasing band offset as both Ga- and Al-contents increase. Ultimately, we fabricated vertical InGaAs−InAlAs NW/Si photovoltaic cells and show that the enhanced internal quantum efficiency is directly translated to an energy conversion efficiency that is ∼3–4 times larger as compared to an unpassivated cell. These results highlight the promising performance of lattice-matched III–V core–shell NW heterostructures with significant impact on future development of related nanophotonic and electronic devices