Determination of the Optimal Shell Thickness for Self-Catalyzed GaAs/AlGaAs Core-Shell Nanowires on Silicon.

We present a set of experimental results showing a combination of various effects, that is, surface recombination velocity, surface charge traps, strain, and structural defects, that govern the carrier dynamics of self-catalyzed GaAs/AlGaAs core-shell nanowires (NWs) grown on a Si(111) substrate by molecular beam epitaxy. Time-resolved photoluminescence of NW ensemble and spatially resolved cathodoluminescence of single NWs reveal that emission intensity, decay time, and carrier diffusion length of the GaAs NW core strongly depend on the AlGaAs shell thickness but in a nonmonotonic fashion. Although 7 nm AlGaAs shell can efficiently suppress the surface recombination velocity of the GaAs NW core, the influence of the surface charge traps and the strain between the core and the shell that redshift the luminescence of the GaAs NW core remain observable in the whole range of the shell thickness. In addition, the band bending effect induced by the surface charge traps can alter the scattering of the excess carriers inside the GaAs NW core at the core/shell interface. If the AlGaAs shell thickness is larger than 50 nm, the luminescence efficiency of the GaAs NW cores deteriorates, ascribed to defect formation inside the AlGaAs shell evidenced by transmission electron microscopy.

Correlation of polarity and crystal structure with optoelectronic and transport properties of GaN/AlN/GaN nanowire sensors.

GaN nanowires (NWs) with an AlN insertion were studied by correlated optoelectronic and aberration-corrected scanning transmission electron microscopy (STEM) characterization on the same single NW. Using aberration-corrected annular bright field and high angle annular dark field STEM, we identify the NW growth axis to be the N-polar [000-1] direction. The electrical transport characteristics of the NWs are explained by the polarization-induced asymmetric potential profile and by the presence of an AlN/GaN shell around the GaN base of the wire. The AlN insertion blocks the electron flow through the GaN core, confining the current to the radial GaN outer shell, close to the NW sidewalls, which increases the sensitivity of the photocurrent to the environment and in particular to the presence of oxygen. The desorption of oxygen adatoms in vacuum leads to a reduction of the nonradiative surface trap density, increasing both dark current and photocurrent.

Visualizing highly localized luminescence in GaN/AlN heterostructures in nanowires.

The optical properties of a stack of GaN/AlN quantum discs (QDiscs) in a GaN nanowire have been studied by spatially resolved cathodoluminescence (CL) at the nanoscale (nanoCL) using a scanning transmission electron microscope (STEM) operating in spectrum imaging mode. For the electron beam excitation in the QDisc region, the luminescence signal is highly localized, with spatial extent as low as 5 nm, due to the high band gap difference between GaN and AlN. This allows the discrimination between the emission of neighbouring QDiscs and evidencing the presence of lateral inclusions, about 3 nm thick and 20 nm long rods (quantum rods, QRods), grown unintentionally on the nanowire sidewalls. These structures, also observed by STEM dark-field imaging, are proved to be optically active in nanoCL, emitting at similar, but usually shorter, wavelengths with respect to most QDiscs.

Room-temperature photodetection dynamics of single GaN nanowires.

We report on the photocurrent behavior of single GaN n-i-n nanowires (NWs) grown by plasma-assisted molecular-beam epitaxy on Si(111). These structures present a photoconductive gain in the range of 10(5)-10(8) and an ultraviolet (350 nm) to visible (450 nm) responsivity ratio larger than 6 orders of magnitude. Polarized light couples with the NW geometry with a maximum photoresponse for polarization along the NW axis. The photocurrent scales sublinearly with optical power, following a I ~ P(ß) law (ß < 1) in the measured range with ß increasing with the measuring frequency. The photocurrent time response remains in the millisecond range, which is in contrast to the persistent (hours) photoconductivity effects observed in two-dimensional photoconductors. The photocurrent is independent of the measuring atmosphere, either in the air or in vacuum. Results are interpreted taking into account the effect of surface states and the total depletion of the NW intrinsic region.

Quantum transport in GaN/AlN double-barrier heterostructure nanowires.

We investigate electronic transport in n-i-n GaN nanowires with and without AlN double barriers. The nanowires are grown by catalyst-free, plasma-assisted molecular beam epitaxy enabling abrupt GaN/AlN interfaces as well as longitudinal n-type doping modulation. At low temperature, transport in n-i-n GaN nanowires is dominated by the Coulomb blockade effect. Carriers are confined in the undoped middle region, forming single or multiple islands with a characteristic length of approximately 100 nm. The incorporation of two AlN tunnel barriers causes confinement to occur within the GaN dot in between. In the case of a 6 nm thick dot and 2 nm thick barriers, we observe characteristic signatures of Coulomb-blockaded transport in single quantum dots with discrete energy states. For thinner dots and barriers, Coulomb-blockade effects do not play a significant role while the onset of resonant tunneling via the confined quantum levels is accompanied by a negative differential resistance surviving up to approximately 150 K.

Ultraviolet photodetector based on GaN/AlN quantum disks in a single nanowire.

We report the demonstration of single-nanowire photodetectors relying on carrier generation in GaN/AlN QDiscs. Two nanowire samples containing QDiscs of different thicknesses are analyzed and compared to a reference binary n-i-n GaN nanowire sample. The responsivity of a single wire QDisc detector is as high as 2 x 10(3) A/W at lambda = 300 nm at room temperature. We show that the insertion of an axial heterostructure drastically reduces the dark current with respect to the binary nanowires and enhances the photosensitivity factor (i.e., the ratio between the photocurrent and the dark current) up to 5 x 10(2) for an incoming light intensity of 5 mW/cm(2). Photocurrent spectroscopy allows identification of the spectral contribution related to carriers generated within large QDiscs, which lies below the GaN band gap due to the quantum confined Stark effect.

Identification of III-N nanowire growth kinetics via a marker technique.

By using a marker technique based on nanowire (NW) heterostructure, we have identified the Ga-limited and N-limited GaN NW growth regimes, which are shifted in comparison to those in two-dimensional GaN layers. The results show that the Ga atoms diffusing along NW sidewalls have a significant contribution to the NW vertical growth. By reducing the substrate temperature, Ga-rich conditions locally activate the lateral growth. In contrast to Ga atoms, the contribution of Al and N adatom diffusion to the NW vertical growth is negligible. Finally, the control of GaN/AlN heterostructures in NWs is demonstrated.

The structural properties of GaN insertions in GaN/AlN nanocolumn heterostructures.

The strain state of 1 and 2.5 nm thick GaN insertions in GaN/AlN nanocolumn heterostructures has been studied by means of a combination of high resolution transmission electron microscopy, Raman spectroscopy and theoretical modeling. It is found that 2.5 nm thick GaN insertions are partially relaxed, which has been attributed to the presence of dislocations in the external AlN capping layer, in close relationship with the morphology of GaN insertions and with the AlN capping mechanism. The observed plastic relaxation in AlN is consistent with the small critical thickness expected for GaN/AlN radial heterostructures.

Interplay between thermodynamics and kinetics in the capping of InAs/GaAs(001) quantum dots.

A microscopic picture for the GaAs overgrowth of self-organized quantum dots is developed. Scanning tunneling microscopy measurements reveal two capping regimes: the first being characterized by a dot shrinking and a backward pyramid-to-dome shape transition. This regime is governed by fast dynamics resulting in island morphologies close to thermodynamic equilibrium. The second regime is marked by a true overgrowth and is controlled by kinetically limited surface diffusion processes. A simple model is developed to describe the observed structural changes which are rationalized in terms of energetic minimization driven by lattice mismatch and alloying.

Hierarchical self-assembly of GaAs/AlGaAs quantum dots.

A novel structure containing self-assembled, unstrained GaAs quantum dots is obtained by combining solid-source molecular beam epitaxy and atomic-layer precise in situ etching. Photo-luminescence (PL) spectroscopy reveals light emission with very narrow inhomogeneous broadening and clearly resolved excited states at high excitation intensity. The dot morphology is determined by scanning probe microscopy and, combined with single band and eight-band k.p theory calculations, is used to interpret PL and single-dot spectra with no adjustable structural parameter.