Correlated optical and electrical analyses of inhomogeneous core/shell InGaN/GaN nanowire light emitting diodes.

The performance of core-shell InGaN/GaN nanowire (NW) light emitting diodes (LEDs) can be limited by wire-to-wire electrical inhomogeneities. Here we investigate an array of core-shell InGaN/GaN NWs which are morphologically identical, but present electrical dissimilarities in order to understand how the nanoscale phenomena observed in individual NWs affect the working performance of the whole array. The LED shows a low number of NWs (∼20%) producing electroluminescence under operating conditions. This is related to a presence of a potential barrier at the interface between the NW core and the radially grown n-doped layer, which differently affects the electrical properties of the NWs although they are morphologically identical. The impact of the potential barrier on the performance of the NW array is investigated by correlating multi-scanning techniques, namely electron beam induced current microscopy, electroluminescence mapping and cathodoluminescence analysis. It is found that the main cause of inhomogeneity in the array is related to a non-optimized charge injection into the active region, which can be overcome by changing the contact architecture so that the electrons become injected directly in the n-doped underlayer. The LED with so-called 'front-n-contacting' is developed leading to an increase of the yield of emitting NWs from 20% to 65%.

Optical properties of GaN nanowires grown on chemical vapor deposited-graphene.

Optical properties of GaN nanowires (NWs) grown on chemical vapor deposited-graphene transferred on an amorphous support are reported. The growth temperature was optimized to achieve a high NW density with a perfect selectivity with respect to a SiO2 surface. The growth temperature window was found to be rather narrow (815°C ± 5°C). Steady-state and time-resolved photoluminescence from GaN NWs grown on graphene was compared with the results for GaN NWs grown on conventional substrates within the same molecular beam epitaxy reactor showing a comparable optical quality for different substrates. Growth at temperatures above 820 °C led to a strong NW density reduction accompanied with a diameter narrowing. This morphology change leads to a spectral blueshift of the donor-bound exciton emission line due to either surface stress or dielectric confinement. Graphene multi-layered micro-domains were explored as a way to arrange GaN NWs in a hollow hexagonal pattern. The NWs grown on these domains show a luminescence spectral linewidth as low as 0.28 meV (close to the set-up resolution limit).

Piezo-generator integrating a vertical array of GaN nanowires.

We demonstrate the first piezo-generator integrating a vertical array of GaN nanowires (NWs). We perform a systematic multi-scale analysis, going from single wire properties to macroscopic device fabrication and characterization, which allows us to establish for GaN NWs the relationship between the material properties and the piezo-generation, and to propose an efficient piezo-generator design. The piezo-conversion of individual MBE-grown p-doped GaN NWs in a dense array is assessed by atomic force microscopy (AFM) equipped with a Resiscope module yielding an average output voltage of 228 ± 120 mV and a maximum value of 350 mV generated per NW. In the case of p-doped GaN NWs, the piezo-generation is achieved when a positive piezo-potential is created inside the nanostructures, i.e. when the NWs are submitted to compressive deformation. The understanding of the piezo-generation mechanism in our GaN NWs, gained from AFM analyses, is applied to design a piezo-generator operated under compressive strain. The device consists of NW arrays of several square millimeters in size embedded into spin-on glass with a Schottky contact for rectification and collection of piezo-generated carriers. The generator delivers a maximum power density of ∼12.7 mW cm(-3). This value sets the new state of the art for piezo-generators based on GaN NWs and more generally on nitride NWs, and offers promising prospects for the use of GaN NWs as high-efficiency ultra-compact energy harvesters.

Self-induced growth of vertical GaN nanowires on silica.

We study the self-induced growth of GaN nanowires on silica. Although the amorphous structure of this substrate offers no possibility of an epitaxial relationship, the nanowires are remarkably aligned with the substrate normal whereas, as expected, their in-plane orientation is random. Their structural and optical characteristics are compared to those of GaN nanowires grown on standard crystalline Si (111) substrates. The polarity inversion domains are much less frequent, if not totally absent, in the nanowires grown on silica, which we find to be N-polar. This work demonstrates that high-quality vertical GaN nanowires can be elaborated without resorting to bulk crystalline substrates.

Dual antiferromagnetic coupling at La0.67Sr0.33MnO3/SrRuO3 interfaces.

We have studied the magnetic hysteresis cycle of La0.67Sr0.33MnO3/SrRuO3 antiferromagnetically coupled bilayers, by magnetometry and polarized neutron reflectometry. A positive exchange bias as well as an unusual asymmetry are observed on the magnetic reversal process of the La0.67Sr0.33MnO3 layer. Through an extended Stoner-Wohlfarth model comprising the magnetic anisotropy of both layers, we give experimental evidence that this asymmetry originates from two different but well-defined antiferromagnetic coupling strengths at the interface between the two magnetic oxides. The possible origin of this dual coupling is discussed in view of our experimental results.

Nanometer-scale, quantitative composition mappings of InGaN layers from a combination of scanning transmission electron microscopy and energy dispersive x-ray spectroscopy.

Using elastic scattering theory we show that a small set of energy dispersive x-ray spectroscopy (EDX) measurements is sufficient to experimentally evaluate the scattering function of electrons in high-angle annular dark field scanning transmission microscopy (HAADF-STEM). We then demonstrate how to use this function to transform qualitative HAADF-STEM images of InGaN layers into precise, quantitative chemical maps of the indium composition. The maps obtained in this way combine the resolution of HAADF-STEM and the chemical precision of EDX. We illustrate the potential of such chemical maps by using them to investigate nanometer-scale fluctuations in the indium composition and their impact on the growth of epitaxial InGaN layers.

Photovoltaic properties of GaAsP core-shell nanowires on Si(001) substrate.

We report on the growth and electro-optical studies of photovoltaic properties of GaAsP nanowires. Low density GaAsP nanowires were grown by Au assisted MOVPE on Si(001) substrates using a two step procedure to form a radial p-n junction. The STEM analyses show that the nanowires have cubic structure with the alloy composition GaAs0.88P0.12 in the nanowire core and GaAs0.76P0.24 in the shell. The nanowire ensembles were processed in the form of sub-millimeter size mesas. The photovoltaic properties were characterized by optical beam induced current (OBIC) and electronic beam induced current (EBIC) maps. Both OBIC and EBIC maps show that the photovoltage is generated by the nanowires; however, a strong signal variation from wire to wire is observed. Only one out of six connected nanowires produce a measurable signal. These strong fluctuations can be tentatively explained by the variation of the resistance of the nanowire-to-substrate connection, which is highly sensitive to the quality of the Si-GaAsP interface. This study demonstrates the importance of the spatially resolved charge collection microscopy techniques for the diagnosis of failures in nanowire photovoltaic devices.

Morphology of self-catalyzed GaN nanowires and chronology of their formation by molecular beam epitaxy.

GaN nanowires are synthesized by plasma-assisted molecular beam epitaxy on Si(111) substrates. The strong impact of the cell orientation relative to the substrate on the nanowire morphology is shown. To study the kinetics of growth, thin AlN markers are introduced periodically during NW growth. These markers are observed in single nanowires by transmission electron microscopy, giving access to the chronology of the nanowire formation and to the time evolution of the nanowire morphology. A long delay precedes the beginning of nanowire formation. Then, their elongation proceeds at a constant rate. Later, shells develop on the side-wall facets by ascending growth of layer bunches which first agglomerate at the nanowire foot.

Optical spectroscopy of two-dimensional layered (C(6)H(5)C(2)H(4)-NH(3))(2)-PbI(4) perovskite.

We report on optical spectroscopy (photoluminescence and photoluminescence excitation) on two-dimensional self-organized layers of (C(6)H(5)C(2)H(4)-NH(3))(2)-PbI(4) perovskite. Temperature and excitation power dependance of the optical spectra gives a new insight into the excitonic and the phononic properties of this hybrid organic/inorganic semiconductor. In particular, exciton-phonon interaction is found to be more than one order of magnitude higher than in GaAs QWs. As a result, photoluminescence emission lines have to be interpreted in the framework of a polaron model.

Bloch oscillations of THz acoustic phonons in coupled nanocavity structures.

Nanophononic Bloch oscillations and Wannier-Stark ladders have been recently predicted to exist in specifically tailored structures formed by coupled nanocavities. Using pump-probe coherent phonon generation techniques we demonstrate that Bloch oscillations of terahertz acoustic phonons can be directly generated and probed in these complex nanostructures. In addition, by Fourier transforming the time traces we had access to the proper eigenmodes in the frequency domain, thus evidencing the related Wannier-Stark ladder. The observed Bloch oscillation dynamics are compared with simulations based on a model description of the coherent phonon generation and photoelastic detection processes.

Al5+αSi5+δN12, a new Nitride compound.

The family of III-Nitride semiconductors has been under intensive research for almost 30 years and has revolutionized lighting applications at the dawn of the 21st century. However, besides the developments and applications achieved, nitride alloys continue to fuel the quest for novel materials and applications. We report on the synthesis of a new nitride-based compound by using annealing of AlN heteroepitaxial layers under a Si-atmosphere at temperatures between 1350 °C and 1550 °C. The structure and stoichiometry of this compound are investigated by high resolution transmission electron microscopy (TEM) techniques and energy dispersive X-Ray (EDX) spectroscopy. Results are supported by density functional theory (DFT) calculations. The identified structure is a derivative of the parent wurtzite AlN crystal where the anion sublattice is fully occupied by N atoms and the cation sublattice is the stacking of 2 different planes along <0001>: The first one exhibits a ×3 periodicity along <11-20> with 1/3 of the sites being vacant. The rest of the sites in the cation sublattice are occupied by an equal number of Si and Al atoms. Assuming a semiconducting alloy, a range of stoichiometries is proposed, Al5+αSi5+δN12 with α being between -2/3 and 1/4 and δ between 0 and 3/4.

An aqueous one-pot route to gold/quantum rod heterostructured nanoparticles functionalized with DNA.

We report an original approach exploiting the photoelectrochemical properties of quantum rods and the versatility of Au(I) organometallic chemistry to control DNA surface grafting. This one-pot aqueous approach provides Janus biofunctionalized nanoparticles, the assembly of which should results in the emergence of synergistic properties.

Core-shell InGaN/GaN nanowire light emitting diodes analyzed by electron beam induced current microscopy and cathodoluminescence mapping.

We report on the electron beam induced current (EBIC) microscopy and cathodoluminescence (CL) characterization correlated with compositional analysis of light emitting diodes based on core/shell InGaN/GaN nanowire arrays. The EBIC mapping of cleaved fully operational devices allows to probe the electrical properties of the active region with a nanoscale resolution. In particular, the electrical activity of the p-n junction on the m-planes and on the semi-polar planes of individual nanowires is assessed in top view and cross-sectional geometries. The EBIC maps combined with CL characterization demonstrate the impact of the compositional gradients along the wire axis on the electrical and optical signals: the reduction of the EBIC signal toward the nanowire top is accompanied by an increase of the CL intensity. This effect is interpreted as a consequence of the In and Al gradients in the quantum well and in the electron blocking layer, which influence the carrier extraction efficiency. The interface between the nanowire core and the radially grown layer is shown to produce in some cases a transitory EBIC signal. This observation is explained by the presence of charged traps at this interface, which can be saturated by electron irradiation.

Facet and in-plane crystallographic orientations of GaN nanowires grown on Si(111).

We have determined the in-plane orientation of GaN nanowires relative to the Si (111) substrate on which they were grown. We used x-ray diffraction pole figure measurements to evidence two types of crystallographic orientation, all the nanowires having [Formula: see text] lateral facets. The proportion of these two orientations was determined and shown to be influenced by the pre-deposition of Al(Ga)N intermediate layers. In the main orientation, the GaN basal [Formula: see text] directions are aligned with the [Formula: see text] directions. This orientation corresponds to an in-plane coincidence of GaN and Si lattices.

Zinc blende GaAsSb nanowires grown by molecular beam epitaxy.

We report the growth of GaAsSb nanowires (NWs) on GaAs(111)B substrates by Au-assisted molecular beam epitaxy. The structural characteristics of the GaAsSb NWs have been investigated in detail. Their Sb mole fraction was found to be about 25%. Their crystal structure was found to be pure zinc blende (ZB), in contrast to the wurtzite structure observed in GaAs NWs grown under similar conditions. The ZB GaAsSb NWs exhibit rotational twins around their [111]B growth axis, with twin-free segments as long as 500 nm. The total volumes of GaAsSb segments with twinned and un-twinned orientations, respectively, were found to be equal by x-ray diffraction analysis of NW ensembles.

Determination of the local concentrations of Mn interstitials and antisite defects in GaMnAs.

We present a method for the determination of the local concentrations of interstitial and substitutional Mn atoms and As antisite defects in GaMnAs. The method relies on the sensitivity of the structure factors of weak reflections to the concentrations and locations of these minority constituents. High spatial resolution is obtained by combining structure factor measurement and x-ray analysis in a transmission electron microscope. We demonstrate the prevalence of interstitials with As nearest neighbors in as-grown layers.