Composition and optical properties of (In, Ga)As nanowires grown by group-III-assisted molecular beam epitaxy.

(In, Ga) alloy droplets are used to catalyse the growth of (In, Ga)As nanowires by molecular beam epitaxy on Si(111) substrates. The composition, morphology and optical properties of these nanowires can be tuned by the employed elemental fluxes. To incorporate more than 10% of In, a high In/(In+Ga) flux ratio above 0.7 is required. We report a maximum In content of almost 30% in bulk (In, Ga)As nanowires for an In/(In+Ga) flux ratio of 0.8. However, with increasing In/(In+Ga) flux ratio, the nanowire length and diameter are notably reduced. Using photoluminescence and cathodoluminescence spectroscopy on nanowires covered by a passivating (In, Al)As shell, two luminescence bands are observed. A significant segment of the nanowires shows homogeneous emission, with a wavelength corresponding to the In content in this segment, while the consumption of the catalyst droplet leads to a spectrally-shifted emission band at the top of the nanowires. The (In,Ga)As nanowires studied in this work provide a new approach for the integration of infrared emitters on Si platforms.

Growth kinetics and substrate stability during high-temperature molecular beam epitaxy of AlN nanowires.

We study the molecular beam epitaxy of AlN nanowires between 950 °C and 1215 °C, well above the usual growth temperatures, to identify optimal growth conditions. The nanowires are grown by self-assembly on TiN(111) films sputtered onto Al2O3. Above 1100 °C, the TiN film is seen to undergo grain growth and its surface exhibits {111} facets where AlN nucleation preferentially occurs. Modeling of the nanowire elongation rate measured at different temperatures shows that the Al adatom diffusion length maximizes at 1150 °C, which appears to be the optimum growth temperature. However, analysis of the nanowire luminescence shows a steep increase in the deep-level signal already above 1050 °C, associated with O incorporation from the Al2O3substrate. Comparison with AlN nanowires grown on Si, MgO and SiC substrates suggests that heavy doping of Si and O by interdiffusion from the TiN/substrate interface increases the nanowire internal quantum efficiency, presumably due to the formation of a SiNxor AlOxpassivation shell. The outdiffusion of Si and O would also cause the formation of the inversion domains observed in the nanowires. It follows that for optoelectronic and piezoelectric applications, optimal AlN nanowire ensembles should be prepared at 1150 °C on TiN/SiC substrates and will require anex situsurface passivation.

Coalescence, crystallographic orientation and luminescence of ZnO nanowires grown on Si(001) by chemical vapour transport.

We analyse the morphological, structural and luminescence properties of self-assembled ZnO nanowires grown by chemical vapour transport on Si(001). The examination of nanowire ensembles by scanning electron microscopy reveals that a non-negligible fraction of nanowires merge together forming coalesced aggregates during growth. We show that the coalescence degree can be unambiguously quantified by a statistical analysis of the cross-sectional shape of the nanowires. The examination of the structural properties by x-ray diffraction evidences that the nanowires crystallize in the wurtzite phase, elongate along the c-axis, and are randomly oriented in plane. The luminescence of the ZnO nanowires, investigated by photoluminescence and cathodoluminescence spectroscopy, is characterized by two bands, the near-band-edge emission and the characteristic defect-related green luminescence of ZnO. The cross-correlation of scanning electron micrographs and monochromatic cathodoluminescence intensity maps reveals that: (i) coalescence joints act as a source of non-radiative recombination, and (ii) the luminescence of ZnO nanowires is inhomogeneously distributed at the single nanowire level. Specifically, the near-band-edge emission arises from the nanowire cores, while the defect-related green luminescence originates from the volume close to the nanowire sidewalls. Two-dimensional simulations of the optical guided modes supported by ZnO nanowires allow us to exclude waveguiding effects as the underlying reason for the luminescence inhomogeneities. We thus attribute this observation to the formation of a core-shell structure in which the shell is characterized by a high concentration of green-emitting radiative point defects as compared to the core.

Spatially-resolved luminescence and crystal structure of single core-shell nanowires measured in the as-grown geometry.

We report on the direct correlation between the structural and optical properties of single, as-grown core-multi-shell GaAs/In0.15Ga0.85As/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.

Assessment of AlGaN/AlN superlattices on GaN nanowires as active region of electron-pumped ultraviolet sources.

In this paper, we describe the design and characterization of 400 nm long (88 periods) Al x Ga1-x N/AlN (0 ≤ x ≤ 0.1) quantum dot superlattices deposited on self-assembled GaN nanowires for application in electron-pumped ultraviolet sources. The optical performance of GaN/AlN superlattices on nanowires is compared with the emission of planar GaN/AlN superlattices with the same periodicity and thickness grown on bulk GaN substrates along the N-polar and metal-polar crystallographic axes. The nanowire samples are less sensitive to nonradiative recombination than planar layers, attaining internal quantum efficiencies (IQE) in excess of 60% at room temperature even under low injection conditions. The IQE remains stable for higher excitation power densities, up to 50 kW cm-2. We demonstrate that the nanowire superlattice is long enough to collect the electron-hole pairs generated by an electron beam with an acceleration voltage V A = 5 kV. At such V A, the light emitted from the nanowire ensemble does not show any sign of quenching under constant electron beam excitation (tested for an excitation power density around 8 kW cm-2 over the scale of minutes). Varying the dot/barrier thickness ratio and the Al content in the dots, the nanowire peak emission can be tuned in the range from 340 to 258 nm.

Absence of Quantum-Confined Stark Effect in GaN Quantum Disks Embedded in (Al,Ga)N Nanowires Grown by Molecular Beam Epitaxy.

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 light 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.

Crystal Phase Quantum Well Emission with Digital Control.

One of the major challenges in the growth of quantum well and quantum dot heterostructures is the realization of atomically sharp interfaces. Nanowires provide a new opportunity to engineer the band structure as they facilitate the controlled switching of the crystal structure between the zinc-blende (ZB) and wurtzite (WZ) phases. Such a crystal phase switching results in the formation of crystal phase quantum wells (CPQWs) and quantum dots (CPQDs). For GaP CPQWs, the inherent electric fields due to the discontinuity of the spontaneous polarization at the WZ/ZB junctions lead to the confinement of both types of charge carriers at the opposite interfaces of the WZ/ZB/WZ structure. This confinement leads to a novel type of transition across a ZB flat plate barrier. Here, we show digital tuning of the visible emission of WZ/ZB/WZ CPQWs in a GaP nanowire by changing the thickness of the ZB barrier. The energy spacing between the sharp emission lines is uniform and is defined by the addition of single ZB monolayers. The controlled growth of identical quantum wells with atomically flat interfaces at predefined positions featuring digitally tunable discrete emission energies may provide a new route to further advance entangled photons in solid state quantum systems.

Effect of doping on the far-infrared intersubband transitions in nonpolar m-plane GaN/AlGaN heterostructures.

This paper assesses the effects of Si doping on the properties of nonpolar m-plane GaN/AlGaN quantum wells (QWs) designed for intersubband (ISB) absorption in the far-infrared spectral range. For doping levels up to 3 × 10(12) cm(-2), structural analysis reveals uniform QWs with abrupt interfaces and no epitaxially induced defects. Cathodoluminescence spectroscopy confirms the homogeneity of the multiple QWs along the growth direction. Increasing the doping density in the QWs from 1 × 10(11) cm(-2) to 3 × 10(12) cm(-2) induces a broadening of the photoluminescence as well as a reduction of the exciton localization energy in the alloy. Also, enhancement of the ISB absorption is observed, along with a blue shift and widening of the absorption peak. The magnitude of the ISB absorption saturates for doping levels around 1 × 10(12) cm(-2), and the blue shift and broadening increase less than theoretically predicted for the samples with higher doping levels. This is explained by the presence of free carriers in the excited electron level due to the increase of the Fermi level energy.

Nonpolar m-plane GaN/AlGaN heterostructures with intersubband transitions in the 5-10 THz band.

This paper assesses intersubband (ISB) transitions in the 1-10 THz frequency range in nonpolar m-plane GaN/AlGaN multi-quantum-wells deposited on free-standing semi-insulating GaN substrates. The quantum wells (QWs) were designed to contain two confined electronic levels, decoupled from the neighboring wells. Structural analysis reveals flat and regular QWs in the two perpendicular in-plane directions, with high-angle annular dark-field scanning transmission electron microscopy images showing inhomogeneities of the Al composition in the barriers along the growth axis. We do not observe extended structural defects (stacking faults or dislocations) introduced by the epitaxial process. Low-temperature ISB absorption from 1.5 to 9 THz (6.3-37.4 meV) is demonstrated, covering most of the 7-10 THz band forbidden to GaAs-based technologies.

Current path in light emitting diodes based on nanowire ensembles.

Light emitting diodes (LEDs) have been fabricated using ensembles of free-standing (In, Ga)N/GaN nanowires (NWs) grown on Si substrates in the self-induced growth mode by molecular beam epitaxy. Electron-beam-induced current analysis, cathodoluminescence as well as biased µ-photoluminescence spectroscopy, transmission electron microscopy, and electrical measurements indicate that the electroluminescence of such LEDs is governed by the differences in the individual current densities of the single-NW LEDs operated in parallel, i.e. by the inhomogeneity of the current path in the ensemble LED. In addition, the optoelectronic characterization leads to the conclusion that these NWs exhibit N-polarity and that the (In, Ga)N quantum well states in the NWs are subject to a non-vanishing quantum confined Stark effect.

Correlation between In content and emission wavelength of In(x)Ga(1-x)N/GaN nanowire heterostructures.

GaN nanowire ensembles with axial In(x)Ga(1-x)N multi-quantum-wells (MQWs) were grown by molecular beam epitaxy. In a series of samples we varied the In content in the MQWs from almost zero to around 20%. Within the nanowire ensemble, the MQWs fluctuate strongly in composition and size. Statistical information about the composition was obtained from x-ray diffraction and Raman spectroscopy. Photoluminescence at room temperature was obtained in the range of 2.2 to 2.5 eV, depending on In content. Contrary to planar MQWs, the intensity increases with increasing In content. We compare the observed emission energies with transition energies obtained from a one-dimensional model, and conclude that several mechanisms for carrier localization affect the luminescence of these three-dimensional structures.

Continuous-flux MOVPE growth of position-controlled N-face GaN nanorods and embedded InGaN quantum wells.

We demonstrate the fabrication of N-face GaN nanorods by metal organic vapour phase epitaxy (MOVPE), using continuous-flux conditions. This is in contrast to other approaches reported so far, which have been based on growth modes far off the conventional growth regimes. For position control of nanorods an SiO(2) masking layer with a dense hole pattern on a c-plane sapphire substrate was used. Nanorods with InGaN/GaN heterostructures have been grown catalyst-free. High growth rates up to 25 microm h(-1) were observed and a well-adjusted carrier gas mixture between hydrogen and nitrogen enabled homogeneous nanorod diameters down to 220 nm with aspect ratios of approximately 8:1. The structural quality and defect progression within nanorods were determined by transmission electron microscopy (TEM). Different emission energies for InGaN quantum wells (QWs) could be assigned to different side facets by room temperature cathodoluminescence (CL) measurements.