Enhancement of Single-Photon Purity and Coherence of III-Nitride Quantum Dot with Polarization-Controlled Quasi-Resonant Excitation.

III-Nitride semiconductor-based quantum dots (QDs) play an essential role in solid-state quantum light sources because of their potential for room-temperature operation. However, undesired background emission from the surroundings deteriorates single-photon purity. Moreover, spectral diffusion causes inhomogeneous broadening and limits the applications of QDs in quantum photonic technologies. To overcome these obstacles, it is demonstrated that directly pumping carriers to the excited state of the QD reduces the number of carriers generated in the vicinities. The polarization-controlled quasi-resonant excitation is applied to InGaN QDs embedded in GaN nanowire. To analyze the different excitation mechanisms, polarization-resolved absorptions are investigated under the above-barrier bandgap, below-barrier bandgap, and quasi-resonant excitation conditions. By employing polarization-controlled quasi-resonant excitation, the linewidth is reduced from 353 to 272 µeV, and the second-order correlation value is improved from 0.470 to 0.231. Therefore, a greater single-photon purity can be obtained at higher temperatures due to decreased linewidth and background emission.

Modeling of the electron beam induced current signal in nanowires with an axial p-n junction.

A tridimensional mathematical model to calculate the electron beam induced current (EBIC) of an axial p-n nanowire junction is proposed. The effect of the electron beam and junction parameters on the distribution of charge carriers and on the collected EBIC current is reported. We demonstrate that the diffusion of charge carriers within the wire is strongly influenced by the electrical state of its lateral surface which is characterized by a parameter called surface recombination velocity (vr). When the surface recombination is weak (i.e. lowvrvalue), the diffusion of charge carriers occurs in one dimension (1D) along the wire axis, and, in this case, the use of bulk EBIC models to extract the diffusion length (L) of charge carriers is justified. However, when the surface effects are strong (i.e. highvrvalues), the diffusion happens in three dimensions (3D). In this case, the EBIC profiles depend onvrvalue and two distinct cases can be defined. If theLis larger than the nanowire radius (ra), the EBIC profiles show a strong dependency with this parameter. This gives evidence that the recombination of generated carriers on the surface throughvris the dominant process. In this situation, a decrease of two orders of magnitude in the EBIC profiles computed with a high and a lowvrvalue is observed in neutral regions of the junction. For the case ofLsmaller thanrathe dependency of the EBIC profiles on thevris weak, and the prevalent recombination mechanism is the bulk recombination process.

Investigation of the effect of the doping order in GaN nanowire p-n junctions grown by molecular-beam epitaxy.

We analyse the electrical and optical properties of single GaN nanowire p-n junctions grown by plasma-assisted molecular-beam epitaxy using magnesium and silicon as doping sources. Different junction architectures having either a n-base or a p-base structure are compared using optical and electrical analyses. Electron-beam induced current (EBIC) microscopy of the nanowires shows that in the case of a n-base p-n junction the parasitic radial growth enhanced by the magnesium (Mg) doping leads to a mixed axial-radial behaviour with strong wire-to-wire fluctuations of the junction position and shape. By reverting the doping order p-base p-n junctions with a purely axial well-defined structure and a low wire-to-wire dispersion are achieved. The good optical quality of the top n nanowire segment grown on a p-doped stem is preserved. A hole concentration in the p-doped segment exceeding 1018 cm-3 was extracted from EBIC mapping and photoluminescence analyses. This high concentration is reached without degrading the nanowire morphology.

Corrigendum: Optical properties of GaN nanowires grown on chemical vapor deposited-graphene (2019 Nanotechnology 30 214005).

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Improvement of carrier collection in Si/a-Si:H nanowire solar cells by using hybrid ITO/silver nanowires contacts.

Optoelectronic devices based on high aspect ratio nanowires bring new challenges for transparent electrodes, which can be well addressed by using hybrid structures. Here we demonstrate that a composite contact to radial junction nanowire solar cells made of a thin indium-tin oxide (ITO) layer and silver nanowires greatly improves the collection of charge carriers as compared to a single thick ITO layer by reducing the series resistance losses while improving the transparency. The optimization is performed on p-i-n solar cells comprising of dense non-vertical nanowires with a p-doped c-Si core and an ultra-thin a-Si:H absorption layer grown by plasma-enhanced chemical vapor deposition on glass substrates. The optimal hybrid contact developed in this work is demonstrated to increase the solar cell conversion efficiency from 4.3% to 6.6%.

Nanoscale electrical analyses of axial-junction GaAsP nanowires for solar cell applications.

Axial p-n and p-i-n junctions in GaAs0.7P0.3 nanowires are demonstrated and analyzed using electron beam induced current microscopy. Organized self-catalyzed nanowire arrays are grown by molecular beam epitaxy on nanopatterned Si substrates. The nanowires are doped using Be and Si impurities to obtain p- and n-type conductivity, respectively. A method to determine the doping type by analyzing the induced current in the vicinity of a Schottky contact is proposed. It is demonstrated that for the applied growth conditions using Ga as a catalyst, Si doping induces an n-type conductivity contrary to the GaAs self-catalyzed nanowire case, where Si was reported to yield a p-type doping. Active axial nanowire p-n junctions having a homogeneous composition along the axis are synthesized and the carrier concentration and minority carrier diffusion lengths are measured. To the best of our knowledge, this is the first report of axial p-n junctions in self-catalyzed GaAsP nanowires.

Image-based autofocusing system for nonlinear optical microscopy with broad spectral tuning.

We present an image-based autofocusing system applied in nonlinear microscopy and spectroscopy with a wide range of excitation wavelengths. The core of the developed autofocusing system consists of an adapted two-step procedure maximizing an image score with six different image scorings algorithms implemented to cover different types of focusing scenarios in automated regime for broad wavelength region. The developed approach is combined with an automated multi-axis alignment procedure. We demonstrate the key abilities of the autofocusing procedure on different types of structures: single nanoparticles, nanowires and complex 3D nanostructures. Based on these experiments, we determine the optimal autofocusing algorithms for different types of structures and applications.

Investigation of GaN nanowires containing AlN/GaN multiple quantum discs by EBIC and CL techniques.

In this work, nanoscale electrical and optical properties of n-GaN nanowires (NWs) containing GaN/AlN multiple quantum discs (MQDs) grown by molecular beam epitaxy are investigated by means of single wire I(V) measurements, electron beam induced current microscopy (EBIC) and cathodoluminescence (CL) analysis. A strong impact of non-intentional AlN and GaN shells on the electrical resistance of individual NWs is put in evidence. The EBIC mappings reveal the presence of two regions with internal electric fields oriented in opposite directions: one in the MQDs region and the other in the adjacent bottom GaN segment. These fields are found to co-exist under zero bias, while under an external bias either one or the other dominates the current collection. In this way EBIC maps allow us to locate the current generation within the wire under different bias conditions and to give the first direct evidence of carrier collection from AlN/GaN MQDs. The NWs have been further investigated by photoluminescence and CL analyses at low temperature. CL mappings show that the near band edge emission of GaN from the bottom part of the NW is blue-shifted due to the presence of the radial shell. In addition, it is observed that CL intensity drops in the central part of the NWs. Comparing the CL and EBIC maps, this decrease of the luminescence intensity is attributed to an efficient charge splitting effect due to the electric fields in the MQDs region and in the GaN base.

Determination of n-Type Doping Level in Single GaAs Nanowires by Cathodoluminescence.

We present an effective method of determining the doping level in n-type III-V semiconductors at the nanoscale. Low-temperature and room-temperature cathodoluminescence (CL) measurements are carried out on single Si-doped GaAs nanowires. The spectral shift to higher energy (Burstein-Moss shift) and the broadening of luminescence spectra are signatures of increased electron densities. They are compared to the CL spectra of calibrated Si-doped GaAs layers, whose doping levels are determined by Hall measurements. We apply the generalized Planck's law to fit the whole spectra, taking into account the electron occupation in the conduction band, the bandgap narrowing, and band tails. The electron Fermi levels are used to determine the free electron concentrations, and we infer nanowire doping of 6 × 1017 to 1 × 1018 cm-3. These results show that cathodoluminescence provides a robust way to probe carrier concentrations in semiconductors with the possibility of mapping spatial inhomogeneities at the nanoscale.

Epitaxy of GaN Nanowires on Graphene.

Epitaxial growth of GaN nanowires on graphene is demonstrated using molecular beam epitaxy without any catalyst or intermediate layer. Growth is highly selective with respect to silica on which the graphene flakes, grown by chemical vapor deposition, are transferred. The nanowires grow vertically along their c-axis and we observe a unique epitaxial relationship with the ⟨21̅1̅0⟩ directions of the wurtzite GaN lattice parallel to the directions of the carbon zigzag chains. Remarkably, the nanowire density and height decrease with increasing number of graphene layers underneath. We attribute this effect to strain and we propose a model for the nanowire density variation. The GaN nanowires are defect-free and they present good optical properties. This demonstrates that graphene layers transferred on amorphous carrier substrates is a promising alternative to bulk crystalline substrates for the epitaxial growth of high quality GaN nanostructures.

Flexible Light-Emitting Diodes Based on Vertical Nitride Nanowires.

We demonstrate large area fully flexible blue LEDs based on core/shell InGaN/GaN nanowires grown by MOCVD. The fabrication relies on polymer encapsulation, nanowire lift-off and contacting using silver nanowire transparent electrodes. The LEDs exhibit rectifying behavior with a light-up voltage around 3 V. The devices show no electroluminescence degradation neither under multiple bending down to 3 mm curvature radius nor in time for more than one month storage in ambient conditions without any protecting encapsulation. Fully transparent flexible LEDs with high optical transmittance are also fabricated. Finally, a two-color flexible LED emitting in the green and blue spectral ranges is demonstrated combining two layers of InGaN/GaN nanowires with different In contents.

Color control of nanowire InGaN/GaN light emitting diodes by post-growth treatment.

Core/shell InGaN/GaN nanowire light emitting diodes (LEDs) based on vertically standing single nanowires and nanowire arrays were fabricated and extensively characterized. The emission of single wire LEDs with the same conformal contact geometry as the array device exhibits the same broadening as the array LED electroluminescence, which proves an excellent wire-to-wire homogeneity. The electroluminescence spectra present two peaks corresponding to the m-plane InGaN quantum well (blue emission) and to an In-rich region at the m-plane-semipolar plane junction (green emission), in agreement with structural characterizations. Modification of the contact layout and a post-growth plasma treatment enable strongly suppressing the unwanted green electroluminescence while increasing the intensity in the blue spectral range for the same injected electrical power. Electron beam induced current mapping proves the inhibition of the electrical activity of the top part of the nanowire after plasma treatment. Inductively coupled plasma etching of the In-rich region permits one to completely remove the green emission for all injection currents, but loss of intensity in the blue spectral range is observed. Selectively contacting the m-plane and plasma treatment of the top part of the nanowire appear as a viable solution for controlling the color of core/shell nanowire LEDs with an inhomogeneous indium composition.

Correlation of microphotoluminescence spectroscopy, scanning transmission electron microscopy, and atom probe tomography on a single nano-object containing an InGaN/GaN multiquantum well system.

A single nanoscale object containing a set of InGaN/GaN nonpolar multiple-quantum wells has been analyzed by microphotoluminescence spectroscopy (µPL), high-resolution scanning transmission electron microscopy (HR-STEM) and atom probe tomography (APT). The correlated measurements constitute a rich and coherent set of data supporting the interpretation that the observed µPL narrow emission lines, polarized perpendicularly to the crystal c-axis and with energies in the interval 2.9-3.3 eV, are related to exciton states localized in potential minima induced by the irregular 3D In distribution within the quantum well (QW) planes. This novel method opens up interesting perspectives, as it will be possible to apply it on a wide class of quantum confining emitters and nano-objects.

First demonstration of plasmonic GaN quantum cascade detectors with enhanced efficiency at normal incidence.

We have designed, fabricated and measured the first plasmon-assisted normal incidence GaN/AlN quantum cascade detector (QCD) making use of the surface plasmon resonance of a two-dimensional nanohole Au array integrated on top of the detector absorption region. The spectral response of the detector at room temperature is peaked at the plasmon resonance of 1.82 µm. We show that the presence of the nanohole array induces an absolute enhancement of the responsivity by a factor of ~30 over that of the bare device at normal incidence and by a factor of 3 with respect to illumination by the 45° polished side facet. We show that this significant improvement arises from two phenomena, namely, the polarization rotation of the impinging light from tangential to normal induced by the plasmonic structure and from the enhancement of the absorption cross-section per quantum well due to the near-field optical intensity of the plasmonic wave.

Assessing individual radial junction solar cells over millions on VLS-grown silicon nanowires.

Silicon nanowires (SiNWs) grown on low-cost substrates provide an ideal framework for the monolithic fabrication of radial junction photovoltaics. However, the quality of junction formation over a random matrix of SiNWs, fabricated via a vapor-liquid-solid (VLS) mechanism, has never been assessed in a realistic context. To address this, we probe the current response of individual radial junction solar cells under electron-beam and optical-beam excitations. Excellent current generation from the radial junction units, compared to their planar counterparts, has been recorded, indicating a high junction quality and effective doping in the ultra-thin SiNWs with diameters thinner than 20 nm. Interestingly, we found that the formation of radial junctions by plasma deposition can be quite robust against geometrical disorder and even the crossings of neighboring cell units. These results provide a strong support to the feasibility of building high-quality radial junction solar cells over high-throughput VLS-grown SiNWs on low-cost substrates.

Enriching the Deep-Red Emission in (Mg, Ba)3M2GeO8: Mn4+ (M = Al, Ga) Compositions for Light-Emitting Diodes.

Red emission from Mn4+-containing oxides inspired the development of high color rendering and cost-effective white-light-emitting diodes (WLEDs). Aiming at this fact, a series of new crystallographic site modified (Mg, Ba)3M2GeO8: Mn4+ (M = Al, Ga) compositions were developed with strong deep-red emission in the reaction to UV and blue lights. The Mg3Al2GeO8 host is composed of three phases: orthorhombic-Mg3Ga2GeO8, orthorhombic-Mg2GeO4, and cubic-MgAl2O4. However, Mg3Ga2GeO8 secured an orthorhombic crystal structure. Interestingly, Mg3Al2GeO8: Mn4+ showed a 13-fold more intense emission than Mg3Ga2GeO8: Mn4+ since Mn4+ occupancy was preferable to [AlO6] sites compared to [GaO6]. The coexisting phases of MgAl2O4 and Mg2GeO4 in Mg3Al2GeO8: Mn4+ contributed to Mn4+ luminescence by providing additional [AlO6] and [MgO6] octahedrons for Mn4+ occupancy. Further, these sites reduced the natural reduction probability of Mn4+ to Mn2+ in [AlO4] tetrahedrons, which was confirmed using cathodoluminescence analysis for the first time. A cationic substitution strategy was employed on Mg3M2GeO8: Mn4+ to improve the luminescence, and Mg3-xBaxM2GeO8: Mn4+ (M = Al, Ga) phosphors were synthesized. Partial substitution of larger Ba2+ ions in Mg2+ sites caused structural distortions and generated a new Ba impurity phase, which improved the photoluminescence. Compositionally tuned Mg2.73Ba0.27Al1.993GeO8: 0.005Mn4+ exhibited a 35-fold higher emission than that of Mg3Ga1.993GeO8: 0.005Mn4+. Additionally, this could retain 70% of its ambient emission intensity at 453 K. A warm WLED with a correlated color temperature (CCT) of 3730 K and a CRI of 89 was fabricated by combining the optimized red component with Y3Al5O12: Ce3+ and 410 nm blue LED. By tuning the ratio of blue (BaMgAl10O17: Eu2+), green (Ce0.63Tb0.37MgAl11O19), and red (Mg2.73Ba0.27Al2GeO8: 0.005Mn4+) phosphors, another WLED was developed using a 280 nm UV-LED chip. This showed natural white emission with a CRI of 79 and a CCT of 5306 K. Meanwhile, three red LEDs were also fabricated using the Mg2.73Ba0.27Al1.993GeO8: 0.005Mn4+ phosphor with commercial sources. These could be potential pc-LEDs for plant growth 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.

Nanometer scale spectral imaging of quantum emitters in nanowires and its correlation to their atomically resolved structure.

We report the spectral imaging in the UV to visible range with nanometer scale resolution of closely packed GaN/AlN quantum disks in individual nanowires using an improved custom-made cathodoluminescence system. We demonstrate the possibility to measure full spectral features of individual quantum emitters as small as 1 nm and separated from each other by only a few nanometers and the ability to correlate their optical properties to their size, measured with atomic resolution. The direct correlation between the quantum disk size and emission wavelength provides evidence of the quantum confined Stark effect leading to an emission below the bulk GaN band gap for disks thicker than 2.6 nm. With the help of simulations, we show that the internal electric field in the studied quantum disks is smaller than what is expected in the quantum well case. We show evidence of a clear dispersion of the emission wavelengths of different quantum disks of identical size but different positions along the wire. This dispersion is systematically correlated to a change of the diameter of the AlN shell coating the wire and is thus attributed to the related strain variations along the wire. The present work opens the way both to fundamental studies of quantum confinement in closely packed quantum emitters and to characterizations of optoelectronic devices presenting carrier localization on the nanometer scale.

Electromechanical conversion efficiency of GaN NWs: critical influence of the NW stiffness, the Schottky nano-contact and the surface charge effects.

The piezoelectric nanowires (NWs) are considered as promising nanomaterials to develop high-efficient piezoelectric generators. Establishing the relationship between their characteristics and their piezoelectric conversion properties is now essential to further improve the devices. However, due to their nanoscale dimensions, the NWs are characterized by new properties that are challenging to investigate. Here, we use an advanced nano-characterization tool derived from AFM to quantify the piezo-conversion properties of NWs axially compressed with a well-controlled applied force. This unique technique allows to establish the direct relation between the output signal generation and the NW stiffness and to quantify the electromechanical coupling coefficient of GaN NWs, which can reach up to 43.4%. We highlight that this coefficient is affected by the formation of the Schottky nano-contact harvesting the piezo-generated energy, and is extremely sensitive to the surface charge effects, strongly pronounced in sub-100 nm wide GaN NWs. These results constitute a new building block in the improvement of NW-based nanogenerator devices.

The elevated colour rendering of white-LEDs by microwave-synthesized red-emitting (Li, Mg)3RbGe8O18:Mn4+ nanophosphors.

The bright red emissive nature of low-cost Mn4+ ions can replace the commercially available Eu2+-doped nitrides/oxynitrides for application in white light-emitting diodes (W-LED). Herein, the Mn4+-doped Li3RbGe8O18 (LRGO) phosphor was synthesized via the solid-state reaction (SSR), microwave-assisted diffusion (MWD), and microwave-assisted sol-gel (MWS) techniques. The MWS-derived crystalline nanoparticles having sizes less than 200 nm exhibited higher red emission intensity at around 668 nm as compared to that of the micron-sized particles obtained with other approaches, owing to the improved compositional homogeneity provided by the MWS technique. The effect of microwaves was studied to gain the optimized morphology with enhanced red emission brightness. Obtained samples showed narrow red emission maxima at 668 nm under UV (300 nm) and blue (455 nm) excitations owing to 2Eg → 4A2g: Mn4+ transitions with the possibility of degeneracy. The existence of doubly degenerate forms and the splitting of 2E2g and 4A2g levels were further confirmed via low-temperature photoluminescence (PL) analysis. The emission intensity was also enhanced by the Mg2+ co-doping of MWS-derived LRGO:Mn4+ nanophosphors. Comparative photoluminescence analysis indicated that the optimized MWS route and the Mg2+ co-doping enhanced the red emission intensity by 182% as compared to the solid-state-derived LRGO:Mn4+. The optimized Mg2+ co-doped nanophosphor showed ∼99% red colour purity under UV and blue excitations. Finally, several W-LEDs were fabricated by combining the mixture of yellow-emitting YAG:Ce3+ phosphor and the optimized red-emitting LRGO:Mn4+,Mg2+ nanophosphor on a 460 nm blue-LED chip. The chromaticity of W-LEDs was tuned from bluish-white with the correlated color temperature of 6952 K, to pure white with the CCT of 5025 K. The color rendering index was also improved from 71 to 92, which could be suitable for indoor lighting applications.