Spatially and Time-Resolved Carrier Dynamics in Core-Shell InGaN/GaN Multiple-Quantum Wells on GaN Wire.

Time-resolved cathodoluminescence is a key tool with high temporal and spatial resolution. However, optical spectroscopic information can be also extracted using synchrotron pulses in a hard X-ray nanoprobe, exploiting a phenomenon called X-ray excited optical luminescence. Here, with 20 ps time resolution and 80 nm lateral resolution, we applied this time-resolved X-ray microscopy technique to individual core-shell InGaN/GaN multiple quantum well heterostructures deposited on GaN wires. Our findings suggest that the m-plane related multiple quantum well states govern the carrier dynamics. Likewise, our observations support not only the influence of In incorporation in the recombination rates, but also carrier localization phenomena at the hexagon wire apex. In addition, our experiment calls for further investigations of the spatiotemporal domain on the underlying mechanisms of optoelectronic nanodevices. Its great potential becomes more valuable when time-resolved X-ray excited optical luminescence microscopy is used in operando with other methods, such as X-ray absorption spectroscopy.

A helium mini-cryostat for the nanoprobe beamline ID16B at ESRF: characteristics and performance.

A helium mini-cryostat has been developed for the hard X-ray nanoprobe ID16B of the European Synchrotron to collect X-ray excited optical luminescence and X-ray fluorescence at low temperature (<10 K). The mini-cryostat has been specifically designed to fit within the strong space restrictions and high-demanding mechanical constraints imposed by the beamline to provide vibration-free operation and maximal thermal stability. This paper reports the detailed design, architecture and technical requirements of the mini-cryostat, and presents the first experimental data measured using the cryogenic equipment. The resulting cryo-system features ultimate thermal stability, fast cool-down and ultra-low vibrations. The simultaneous X-ray fluorescence and X-ray excited optical luminescence data acquired from bulk GaN and core/shell InGaN/GaN multi-quantum wells validated the excellent performance of the cryostat with ultimate resolution, stability and sensitivity.

Nanoscale mapping of carrier collection in single nanowire solar cells using X-ray beam induced current.

Here it is demonstrated how nanofocused X-ray beam induced current (XBIC) can be used to quantitatively map the spatially dependent carrier collection probability within nanostructured solar cells. The photocurrent generated by a 50 nm-diameter X-ray beam was measured as a function of position, bias and flux in single p-i-n doped solar-cell nanowires. The signal gathered mostly from the middle segment decays exponentially toward the p- and n-segments, with a characteristic decay length that varies between 50 nm and 750 nm depending on the flux and the applied bias. The amplitude of the XBIC shows saturation at reverse bias, which indicates that most carriers are collected. At forward bias, the relevant condition for solar cells, the carrier collection is only efficient in a small region. Comparison with finite element modeling suggests that this is due to unintentional p-doping in the middle segment. It is expected that nanofocused XBIC could be used to investigate carrier collection in a wide range of nanostructured solar cells.

Nanobeam X-ray Fluorescence Dopant Mapping Reveals Dynamics of in Situ Zn-Doping in Nanowires.

The properties of semiconductors can be controlled using doping, making it essential for electronic and optoelectronic devices. However, with shrinking device sizes it becomes increasingly difficult to quantify doping with sufficient sensitivity and spatial resolution. Here, we demonstrate how X-ray fluorescence mapping with a nanofocused beam, nano-XRF, can quantify Zn doping within in situ doped III-V nanowires, by using large area detectors and high-efficiency focusing optics. The spatial resolution is defined by the focus size to 50 nm. The detection limit of 7 ppm (2.8 × 1017 cm-3), corresponding to about 150 Zn atoms in the probed volume, is bound by a background signal. In solar cell InP nanowires with a p-i-n doping profile, we use nano-XRF to observe an unintentional Zn doping of 5 × 1017 cm-3 in the middle segment. We investigated the dynamics of in situ Zn doping in a dedicated multisegment nanowire, revealing significantly sharper gradients after turning the Zn source off than after turning the source on. Nano-XRF could be used for quantitative mapping of a wide range of dopants in many types of nanostructures.

Spectrally resolved x-ray beam induced current in a single InGaP nanowire.

We demonstrate x-ray absorption fine structure spectroscopy (XAFS) detected by x-ray beam induced current (XBIC) in single n + -i-n + doped nanowire devices. Spatial scans with the 65 nm diameter beam show a peak of the XBIC signal in the middle segment of the nanowire. The XBIC and the x-ray fluorescence signals were detected simultaneously as a function of the excitation energy near the Ga K absorption edge at 10.37 keV. The spectra show similar oscillations around the edge, which shows that the XBIC is limited by the primary absorption. Our results reveal the feasibility of the XBIC detection mode for the XAFS investigation in nanostructured devices.

In operando x-ray imaging of nanoscale devices: Composition, valence, and internal electrical fields.

We introduce a method for directly imaging depletion layers in operando with elemental specificity and chemical speciation at sub-100 nm spatial resolution applicable to today's three-dimensional electronic architectures. These typically contain complex, multicomponent designs consisting of epitaxial heterostructures, buried domains, or nanostructures with different shapes and sizes. Although the variety of devices is immense, they commonly rely on carrier separation in a built-in potential induced by composition or strain gradients. To image these, we scanned a focused synchrotron x-ray nanobeam over a single semiconductor nanowire heterostructure and simultaneously measured the current through the device and the emitted characteristic x-rays as a function of the incoming hard x-ray energy. With these results, it is possible to identify the compositional and molecular structure as well as localize the electrical fields present under typical working conditions. This information allows us to draw an energy band diagram consistent with the elemental distribution and a high-resolution chemical speciation map.

Thin-Wall GaN/InAlN Multiple Quantum Well Tubes.

Thin-wall tubes composed of nitride semiconductors (III-N compounds) based on GaN/InAlN multiple quantum wells (MQWs) are fabricated by metal-organic vapor-phase epitaxy in a simple and full III-N approach. The synthesis of such MQW-tubes is based on the growth of N-polar c-axis vertical GaN wires surrounded by a core-shell MQW heterostructure followed by in situ selective etching using controlled H2/NH3 annealing at 1010 °C to remove the inner GaN wire part. After this process, well-defined MQW-based tubes having nonpolar m-plane orientation exhibit UV light near 330 nm up to room temperature, consistent with the emission of GaN/InAlN MQWs. Partially etched tubes reveal a quantum-dotlike signature originating from nanosized GaN residuals present inside the tubes. The possibility to fabricate in a simple way thin-wall III-N tubes composed of an embedded MQW-based active region offering controllable optical emission properties constitutes an important step forward to develop new nitride devices such as emitters, detectors or sensors based on tubelike nanostructures.

Silane-Induced N-Polarity in Wires Probed by a Synchrotron Nanobeam.

Noncentrosymmetric one-dimensional structures are key driving forces behind advanced nanodevices. Owing to the critical role of silane injection in creating nanosized architectures, it has become a challenge to investigate the induced local lattice polarity in single GaN wires. Thus, if axial and radial structures are well-grown by a silane-mediated approach, an ideal model to study their polar orientations is formed. By combining synchrotron X-ray fluorescence and X-ray excited optical luminescence, we show here experimental evidence of the role of silane to promote the N-polarity, light emission, and elemental incorporation within single wires. In addition, our experiment demonstrates the ability to spatially examine carrier diffusion phenomena without electrical contacts, opening new avenues for further studies with simultaneous optical and elemental sensitivity at the nanoscale.

ID16B: a hard X-ray nanoprobe beamline at the ESRF for nano-analysis.

Within the framework of the ESRF Phase I Upgrade Programme, a new state-of-the-art synchrotron beamline ID16B has been recently developed for hard X-ray nano-analysis. The construction of ID16B was driven by research areas with major scientific and societal impact such as nanotechnology, earth and environmental sciences, and bio-medical research. Based on a canted undulator source, this long beamline provides hard X-ray nanobeams optimized mainly for spectroscopic applications, including the combination of X-ray fluorescence, X-ray diffraction, X-ray excited optical luminescence, X-ray absorption spectroscopy and 2D/3D X-ray imaging techniques. Its end-station re-uses part of the apparatus of the earlier ID22 beamline, while improving and enlarging the spectroscopic capabilities: for example, the experimental arrangement offers improved lateral spatial resolution (∼50 nm), a larger and more flexible capability for in situ experiments, and monochromatic nanobeams tunable over a wider energy range which now includes the hard X-ray regime (5-70 keV). This paper describes the characteristics of this new facility, short-term technical developments and the first scientific results.

Metal organic vapour-phase epitaxy growth of GaN wires on Si (111) for light-emitting diode applications.

GaN wires are grown on a Si (111) substrate by metal organic vapour-phase epitaxy on a thin deposited AlN blanket and through a thin SiNx layer formed spontaneously at the AlN/Si interface. N-doped wires are used as templates for the growth of core-shell InGaN/GaN multiple quantum wells coated by a p-doped shell. Standing single-wire heterostructures are connected using a metallic tip and a Si substrate backside contact, and the electroluminescence at room temperature and forward bias is demonstrated at 420 nm. This result points out the feasibility of lower cost nitride-based wires for light-emitting diode applications.

M-plane core-shell InGaN/GaN multiple-quantum-wells on GaN wires for electroluminescent devices.

Nonpolar InGaN/GaN multiple quantum wells (MQWs) grown on the {11-00} sidewalls of c-axis GaN wires have been grown by organometallic vapor phase epitaxy on c-sapphire substrates. The structural properties of single wires are studied in detail by scanning transmission electron microscopy and in a more original way by secondary ion mass spectroscopy to quantify defects, thickness (1-8 nm) and In-composition in the wells (∼16%). The core-shell MQW light emission characteristics (390-420 nm at 5 K) were investigated by cathodo- and photoluminescence demonstrating the absence of the quantum Stark effect as expected due to the nonpolar orientation. Finally, these radial nonpolar quantum wells were used in room-temperature single-wire electroluminescent devices emitting at 392 nm by exploiting sidewall emission.