Origin of Polytype Formation in VLS-Grown Ge Nanowires through Defect Generation and Nanowire Kinking

We propose layer-by-layer growth mechanisms to account for planar defect generation leading to kinked polytype nanowires. C_s-corrected scanning transmission electron microscopy enabled identification of stacking sequences of distinct polytype bands found in kinked nanowires, and Raman spectroscopy was used to distinguish polytype nanowires from twinned nanowires containing only the 3C diamond cubic phase. The faceting and atomic-scale defect structures of twinned 3C are compared with those of polytype nanowires to develop a common model linking nucleation pinning to nanowire morphology and phase

Impact of Dopant Compensation on Graded <i>p</i>–<i>n</i> Junctions in Si Nanowires

The modulation between different doping species required to produce a diode in VLS-grown nanowires (NWs) yields a complex doping profile, both axially and radially, and a gradual junction at the interface. We present a detailed analysis of the dopant distribution around the junction. By combining surface potential measurements, performed by KPFM, with finite element simulations, we show that the highly doped (5 × 10¹⁹ cm^–3) shell surrounding the NW can screen the junction’s built in voltage at shell thickness as low as 3 nm. By comparing NWs with high and low doping contrast at the junction, we show that dopant compensation dramatically decreases the electrostatic width of the junction and results in relatively low leakage currents

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

Alloy Fluctuations Act as Quantum Dot-like Emitters in GaAs-AlGaAs Core–Shell Nanowires

GaAs-Al_<i>x</i>Ga_1–<i>x</i>As (AlGaAs) core–shell nanowires show great promise for nanoscale electronic and optoelectronic devices, but the application of these nonplanar heterostructures in devices requires improved understanding and control of nanoscale alloy composition and interfaces. Multiple researchers have observed sharp emission lines of unknown origin below the AlGaAs band edge in photoluminescence (PL) spectra of core–shell nanowires; point defects, alloy composition fluctuations, and self-assembled quantum dots have been put forward as candidate structures. Here we employ laser-assisted atom probe tomography to reveal structural and compositional features that give rise to the sharp PL emission spectra. Nanoscale ellipsoidal Ga-enriched clusters resulting from random composition fluctuations are identified in the AlGaAs shell, and their compositions, size distributions, and interface characteristics are analyzed. Simulations of exciton transition energies in ellipsoidal quantum dots are used to relate the Ga nanocluster distribution with the distribution of sharp PL emission lines. We conclude that the Ga rich clusters can act as discrete emitters provided that the major diameter is ≥4 nm. Smaller clusters are under-represented in the PL spectrum, and spectral lines of larger clusters are broadened, due to quantum tunneling between clusters

He-Ion Microscopy as a High-Resolution Probe for Complex Quantum Heterostructures in Core–Shell Nanowires

Core–shell semiconductor nanowires (NW) with internal quantum heterostructures are amongst the most complex nanostructured materials to be explored for assessing the ultimate capabilities of diverse ultrahigh-resolution imaging techniques. To probe the structure and composition of these materials in their native environment with minimal damage and sample preparation calls for high-resolution electron or ion microscopy methods, which have not yet been tested on such classes of ultrasmall quantum nanostructures. Here, we demonstrate that scanning helium ion microscopy (SHeIM) provides a powerful and straightforward method to map quantum heterostructures embedded in complex III–V semiconductor NWs with unique material contrast at ∼1 nm resolution. By probing the cross sections of GaAs-Al­(Ga)As core–shell NWs with coaxial GaAs quantum wells as well as short-period GaAs/AlAs superlattice (SL) structures in the shell, the Al-rich and Ga-rich layers are accurately discriminated by their image contrast in excellent agreement with correlated, yet destructive, scanning transmission electron microscopy and atom probe tomography analysis. Most interestingly, quantitative He-ion dose-dependent SHeIM analysis of the ternary AlGaAs shell layers and of compositionally nonuniform GaAs/AlAs SLs reveals distinct alloy composition fluctuations in the form of Al-rich clusters with size distributions between ∼1–10 nm. In the GaAs/AlAs SLs the alloy clustering vanishes with increasing SL-period (>5 nm-GaAs/4 nm-AlAs), providing insights into critical size dimensions for atomic intermixing effects in short-period SLs within a NW geometry. The straightforward SHeIM technique therefore provides unique benefits in imaging the tiniest nanoscale features in topography, structure and composition of a multitude of diverse complex semiconductor nanostructures

Quantum Transport and Sub-Band Structure of Modulation-Doped GaAs/AlAs Core–Superlattice Nanowires

Modulation-doped III–V semiconductor nanowire (NW) heterostructures have recently emerged as promising candidates to host high-mobility electron channels for future high-frequency, low-energy transistor technologies. The one-dimensional geometry of NWs also makes them attractive for studying quantum confinement effects. Here, we report correlated investigations into the discrete electronic sub-band structure of confined electrons in the channel of Si δ-doped GaAs−GaAs/AlAs core−superlattice NW heterostructures and the associated signatures in low-temperature transport. On the basis of accurate structural and dopant analysis using scanning transmission electron microscopy and atom probe tomography, we calculated the sub-band structure of electrons confined in the NW core and employ a labeling system inspired by atomic orbital notation. Electron transport measurements on top-gated NW transistors at cryogenic temperatures revealed signatures consistent with the depopulation of the quasi-one-dimensional sub-bands, as well as confinement in zero-dimensional-like states due to an impurity-defined background disorder potential. These findings are instructive toward reaching the ballistic transport regime in GaAs−AlGaAs based NW systems