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Register a new userSpatially-resolved luminescence and crystal structure of single core-shell nanowires measured in the as-grown geometry
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Added by
Jonas L\\\"ahnemann
Publication date
2020
fields
Physics
and research's language is
English
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We report on the direct correlation between the structural and optical properties of single, as-grown core-multi-shell GaAs/In$_{0.15}$Ga$_{0.85}$As/GaAs/AlAs/GaAs nanowires. Fabricated by molecular beam epitaxy on a pre-patterned Si(111) substrate, on a row of well separated nucleation sites, it was possible to access individual nanowires in the as-grown geometry. The polytype distribution along the growth axis of the nanowires was revealed by synchrotron-based nanoprobe X-ray diffraction techniques monitoring the axial 111 Bragg reflection. For the same nanowires, the spatially-resolved emission properties were obtained by cathodoluminescence hyperspectral linescans in a scanning electron microscope. Correlating both measurements, we reveal a blueshift of the shell quantum well emission energy combined with an increased emission intensity for segments exhibiting a mixed structure of alternating wurtzite and zincblende stacking compared with the pure crystal polytypes. The presence of this mixed structure was independently confirmed by cross-sectional transmission electron microscopy.
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While the properties of wurtzite GaAs have been extensively studied during the past decade, little is known about the influence of the crystal polytype on ternary (In,Ga)As quantum well structures. We address this question with a unique combination of correlated, spatially-resolved measurement techniques on core-shell nanowires that contain extended segments of both the zincblende and wurtzite polytypes. Cathodoluminescence hyperspectral imaging reveals a blueshift of the quantum well emission energy by $75pm15$ meV in the wurtzite polytype segment. Nanoprobe x-ray diffraction and atom probe tomography enable $mathbf{k}cdotmathbf{p}$ calculations for the specific sample geometry to reveal two comparable contributions to this shift. First, there is a 30% drop in In mole fraction going from the zincblende to the wurtzite segment. Second, the quantum well is under compressive strain, which has a much stronger impact on the hole ground state in the wurtzite than in the zincblende segment. Our results highlight the role of the crystal structure in tuning the emission of (In,Ga)As quantum wells and pave the way to exploit the possibilities of three-dimensional bandgap engineering in core-shell nanowire heterostructures. At the same time, we have demonstrated an advanced characterization toolkit for the investigation of semiconductor nanostructures.
Quantum wells in InAs/GaSb heterostructures can be tuned to a topological regime associated with the quantum spin Hall effect, which arises due to an inverted band gap and hybridized electron and hole states. Here, we investigate electron-hole hybridization and the fate of the quantum spin Hall effect in a quasi one-dimensional geometry, realized in a core-shell-shell nanowire with an insulator core and InAs and GaSb shells. We calculate the band structure for an infinitely long nanowire using $mathbf{k cdot p}$ theory within the Kane model and the envelope function approximation, then map the result onto a BHZ model which is used to investigate finite-length wires. Clearly, quantum spin Hall edge states cannot appear in the core-shell-shell nanowires which lack one-dimensional edges, but in the inverted band-gap regime we find that the finite-length wires instead host localized states at the wire ends. These end states are not topologically protected, they are four-fold degenerate and split into two Kramers pairs in the presence of potential disorder along the axial direction. However, there is some remnant of the topological protection of the quantum spin Hall edge states in the sense that the end states are fully robust to (time-reversal preserving) angular disorder, as long as the bulk band gap is not closed.
We have used scanning tunneling microscopy and spectroscopy to resolve the spatial variation of the density of states of twisted graphene layers on top of a highly oriented pyrolytic graphite substrate. Owing to the twist a moire pattern develops with a periodicity that is substantially larger than the periodicity of a single layer graphene. The twisted graphene layer has electronic properties that are distinctly different from that of a single layer graphene due to the nonzero interlayer coupling. For small twist angles (about 1-3.5 degree) the integrated differential conductivity spectrum exhibits two well-defined Van Hove singularities. Spatial maps of the differential conductivity that are recorded at energies near the Fermi level exhibit a honeycomb structure that is comprised of two inequivalent hexagonal sub-lattices. For energies |E-E_F|>0.3 eV the hexagonal structure in the differential conductivity maps vanishes. We have performed tight-binding calculations of the twisted graphene system using the propagation method, in which a third graphene layer is added to mimic the substrate. This third layer lowers the symmetry and explains the development of the two hexagonal sub-lattices in the moire pattern. Our experimental results are in excellent agreement with the tight-binding calculations.
Several of the key issues of planar (Al,Ga)N-based deep-ultraviolet light emitting diodes could potentially be overcome by utilizing nanowire heterostructures, exhibiting high structural perfection and improved light extraction. Here, we study the spontaneous emission of GaN/(Al,Ga)N nanowire ensembles grown on Si(111) by plasma-assisted molecular beam epitaxy. The nanowires contain single GaN quantum disks embedded in long (Al,Ga)N nanowire segments essential for efficient light extraction. These quantum disks are found to exhibit intense emission at unexpectedly high energies, namely, significantly above the GaN bandgap, and almost independent of the disk thickness. An in-depth investigation of the actual structure and composition of the nanowires reveals a spontaneously formed Al gradient both along and across the nanowire, resulting in a complex core/shell structure with an Al deficient core and an Al rich shell with continuously varying Al content along the entire length of the (Al,Ga)N segment. This compositional change along the nanowire growth axis induces a polarization doping of the shell that results in a degenerate electron gas in the disk, thus screening the built-in electric fields. The high carrier density not only results in the unexpectedly high transition energies, but also in radiative lifetimes depending only weakly on temperature, leading to a comparatively high internal quantum efficiency of the GaN quantum disks up to room temperature.
The strain configuration induced by the lattice mismatch in a core-shell nanowire is calculated analytically, taking into account the crystal anisotropy and the difference in stiffness constants of the two materials. The method is applied to nanowires with the wurtzite structure or the zinc-blende structure with the hexagonal / trigonal axis along the nanowire, and the results are compared to available numerical calculations and experimental data. It is also applied to multishell nanowires, and to core-shell nanowires grown along the $<001>$ axis of cubic semiconductors.
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