Davide Priante

The recombination mechanisms leading to amplified spontaneous emission at the true-green wavelength in CH3NH3PbBr3 perovskites

We investigated the mechanisms of radiative recombination in a CH3NH3PbBr3 hybrid perovskite material using low-temperature, power-dependent (77 K), and temperature-dependent photoluminescence (PL) measurements. Two bound-excitonic radiative transitions related to grain size inhomogeneity were identified. Both transitions led to PL spectra broadening as a result of concurrent blue and red shifts of these excitonic peaks. The red-shifted bound-excitonic peak dominated at high PL excitation led to a true-green wavelength of 553 nm for CH3NH3PbBr3 powders that are encapsulated in polydimethylsiloxane. Amplified spontaneous emission was eventually achieved for an excitation threshold energy of approximately 350 μJ/cm2. Our results provide a platform for potential extension towards a true-green light-emitting device for solid-state lighting and display applications.

Droop-free Al x Ga 1-x N/Al y Ga 1-y N quantum-disks-in-nanowires ultraviolet LED emitting at 337 nm on metal/silicon substrates

Currently the AlGaN-based ultraviolet (UV) solid-state lighting research suffers from numerous challenges. In particular, low internal quantum efficiency, low extraction efficiency, inefficient doping, large polarization fields, and high dislocation density epitaxy constitute bottlenecks in realizing high power devices. Despite the clear advantage of quantum-confinement nanostructure, it has not been widely utilized in AlGaN-based nanowires. Here we utilize the self-assembled nanowires (NWs) with embedding quantum-disks (Qdisks) to mitigate these issues, and achieve UV emission of 337 nm at 32 A/cm2 (80 mA in 0.5 × 0.5 mm2 device), a turn-on voltage of ~5.5 V and droop-free behavior up to 120 A/cm2 of injection current. The device was grown on a titanium-coated n-type silicon substrate, to improve current injection and heat dissipation. A narrow linewidth of 11.7 nm in the electroluminescence spectrum and a strong wavefunctions overlap factor of 42% confirm strong quantum confinement within uniformly formed AlGaN/AlGaN Qdisks, verified using transmission electron microscopy (TEM). The nitride-based UV nanowires light-emitting diodes (NWs-LEDs) grown on low cost and scalable metal/silicon template substrate, offers a scalable, environment friendly and low cost solution for numerous applications, such as solid-state lighting, spectroscopy, medical science and security.

Enhanced Etching, Surface Damage Recovery, and Submicron Patterning of Hybrid Perovskites using a Chemically Gas-Assisted Focused-Ion Beam for Subwavelength Grating Photonic Applications

The high optical gain and absorption of organic-inorganic hybrid perovskites have attracted attention for photonic device applications. However, owing to the sensitivity of organic moieties to solvents and temperature, device processing is challenging, particularly for patterning. Here, we report the direct patterning of perovskites using chemically gas-assisted focused-ion beam (GAFIB) etching with XeF2 and I2 precursors. We demonstrate etching enhancement in addition to controllability and marginal surface damage compared to focused-ion beam (FIB) etching without precursors. Utilizing the GAFIB etching, we fabricated a uniform and periodic submicron perovskite subwavelength grating (SWG) absorber with broadband absorption and nanoscale precision. Our results demonstrate the use of FIB as a submicron patterning tool and a means of providing surface treatment (after FIB patterning to minimize optical loss) for perovskite photonic nanostructures. The SWG absorber can be patterned on perovskite solar cells to enhance the device efficiency through increasing light trapping and absorption.

Focused-ion beam patterning of organolead trihalide perovskite for subwavelength grating nanophotonic applications

The coherent amplified spontaneous emission and high photoluminescence quantum efficiency of organolead trihalide perovskite have led to research interest in this material for use in photonic devices. In this paper, the authors present a focused-ion beam patterning strategy for methylammonium lead tribromide (MAPbBr3) perovskite crystal for subwavelength grating nanophotonic applications. The essential parameters for milling, such as the number of scan passes, dwell time, ion dose, ion current, ion incident angle, and gas-assisted etching, were experimentally evaluated to determine the sputtering yield of the perovskite. Based on our patterning conditions, the authors observed that the sputtering yield ranged from 0.0302 to 0.0719 μm3/pC for the MAPbBr3 perovskite crystal. Using XeF2 for the focused-ion beam gas-assisted etching, the authors determined that the etching rate was reduced to between 0.40 and 0.97, depending on the ion dose, compared with milling with ions only. Using the optimized patterning...

Real-Space Visualization of Energy Loss and Carrier Diffusion in a Semiconductor Nanowire Array Using 4D Electron Microscopy

A breakthrough in the development of 4D scanning ultrafast electron microscopy is described for real-time and space imaging of secondary electron energy loss and carrier diffusion on the surface of an array of nanowires as a model system, providing access to a territory that is beyond the reach of either static electron imaging or any time-resolved laser spectroscopy.

Highly uniform ultraviolet-A quantum-confined AlGaN nanowire LEDs on metal/silicon with a TaN interlayer

In this paper, we describe ultraviolet-A (UV-A) light-emitting diodes (LEDs) emitting at 325 nm based on a highly uniform structure of quantum-confined AlGaN quantum-disk nanowires (NWs). By incorporating a 20 nm TaN interlayer between a Ti pre-orienting layer and the silicon substrate, we eliminated the potential barrier for carrier injection and phonon transport, and inhibited the formation of interfacial silicide that led to device failure. Compared to previous reports on metal substrate, we achieved a 16 × reduction in root-mean-square (RMS) roughness, from 24 nm to 1.6 nm, for the samples with the Ti/TaN metal-bilayer, owing to the effective diffusion barrier characteristic of TaN. This was confirmed using energy dispersive X-ray spectroscopy (EDXS) and electron energy loss spectroscopy (EELS). We achieved a considerable increase in the injection current density (up to 90 A/cm2) compared to our previous studies, and an optical power of 1.9 μW for the 0.5 × 0.5 mm2 NWs-LED. This work provides a feasible pathway for both a reliable and stable UV-A device operation at elevated current injection, and eventually towards low-cost production of UV devices, leveraging on the scalability of silicon substrates.

Role of quantum-confined stark effect on bias dependent photoluminescence of N-polar GaN/InGaN multi-quantum disk amber light emitting diodes

We study the impact of quantum-confined stark effect (QCSE) on bias dependent micro-photoluminescence emission of the quantum disk (Q-disk) based nanowires light emitting diodes (NWs-LED) exhibiting the amber colored emission. The NWs are found to be nitrogen polar (N-polar) verified using KOH wet chemical etching and valence band spectrum analysis of high-resolution X-ray photoelectron spectroscopy. The crystal structure and quality of the NWs were investigated by high-angle annular dark field - scanning transmission electron microscopy. The LEDs were fabricated to acquire the bias dependent micro-photoluminescence spectra. We observe a redshift and a blueshift of the μPL peak in the forward and reverse bias conditions, respectively, with reference to zero bias, which is in contrast to the metal-polar InGaN well-based LEDs in the literature. Such opposite shifts of μPL peak emission observed for N-polar NWs-LEDs, in our study, are due to the change in the direction of the internal piezoelectric field. The quenching of PL intensity, under the reverse bias conditions, is ascribed to the reduction of electron-hole overlap. Furthermore, the blueshift of μPL emission with increasing excitation power reveals the suppression of QCSE resulting from the photo-generated carriers. Thereby, our study confirms the presence of QCSE for NWs-LEDs from both bias and power dependent μPL measurements. Thus, this study serves to understand the QCSE in N-polar InGaN Q-disk NWs-LEDs and other related wide-bandgap nitride nanowires, in general.We study the impact of quantum-confined stark effect (QCSE) on bias dependent micro-photoluminescence emission of the quantum disk (Q-disk) based nanowires light emitting diodes (NWs-LED) exhibiting the amber colored emission. The NWs are found to be nitrogen polar (N-polar) verified using KOH wet chemical etching and valence band spectrum analysis of high-resolution X-ray photoelectron spectroscopy. The crystal structure and quality of the NWs were investigated by high-angle annular dark field - scanning transmission electron microscopy. The LEDs were fabricated to acquire the bias dependent micro-photoluminescence spectra. We observe a redshift and a blueshift of the μPL peak in the forward and reverse bias conditions, respectively, with reference to zero bias, which is in contrast to the metal-polar InGaN well-based LEDs in the literature. Such opposite shifts of μPL peak emission observed for N-polar NWs-LEDs, in our study, are due to the change in the direction of the internal piezoelectric field. Th...

Enhancing the Light-Extraction Efficiency of an AlGaN Nanowire Ultraviolet Light-Emitting Diode by Using Nitride/Air Distributed Bragg Reflector Nanogratings

The performance and efficiency of AlGaN ultraviolet light-emitting diodes have been limited by the extremely low light-extraction efficiency (LEE) due to the intrinsic material properties of AlGaN. Here, to enhance the LEE of the device, we demonstrate an AlGaN nanowire light-emitting diode (NW-LED) integrated with nitride/air distributed Bragg reflector (DBR) nanogratings. Compared to a control device (only mesa), the AlGaN NW-LED with the nitride/air DBR nanogratings exhibits enhancement in the light output power and external quantum efficiency (EQE) by a factor of ∼1.67. The higher light output power and EQE are attributed mainly to the multiple reflectances laterally for the transverse magnetic (TM)-polarized light and scattering introduced by the nanogratings. To further understand the LEE enhancement, the electrical field distribution, extraction ratio, and polar pattern of the AlGaN NW-LED with and without the nitride/air DBR nanogratings were analyzed using the finite-difference time-domain method. It was observed that the TM-field emission was confined and scattered upward, whereas the polar pattern was intensified for the AlGaN NW-LED with the nanogratings. Our approach to enhance the LEE via the nitride/air DBR nanogratings can provide a promising route for increasing the efficiency of AlGaN-based LEDs, also, to functioning as facet mirror for AlGaN-based laser diodes.

Quantified Hole Concentration in AlGaN Nanowires for High-Performance Ultraviolet Emitters

p-Type doping in wide bandgap and new classes of ultra-wide bandgap materials has long been a scientific and engineering problem. The challenges arise from the large activation energy of dopants and high densities of dislocations in materials. We report here, a significantly enhanced p-type conduction using high-quality AlGaN nanowires. For the first time, the hole concentration in Mg-doped AlGaN nanowires is quantified. The incorporation of Mg into AlGaN was verified by correlation with photoluminescence and Raman measurements. The open-circuit potential measurements further confirmed the p-type conductivity, while Mott-Schottky experiments measured a hole concentration of 1.3 × 1019 cm-3. These results from photoelectrochemical measurements allow us to design prototype ultraviolet (UV) light-emitting diodes (LEDs) incorporating the AlGaN quantum-disks-in-nanowire and an optimized p-type AlGaN contact layer for UV-transparency. The ∼335 nm LEDs exhibited a low turn-on voltage of 5 V with a series resistance of 32 Ω, due to the efficient p-type doping of the AlGaN nanowires. The bias-dependent Raman measurements further revealed the negligible self-heating of devices. This study provides an attractive solution to evaluate the electrical properties of AlGaN, which is applicable to other wide bandgap nanostructures. Our results are expected to open doors to new applications for wide and ultra-wide bandgap materials.

Unleashing the potential of molecular beam epitaxy grown AlGaN-based ultraviolet-spectrum nanowires devices

Abstract. There have been recent research advances in AlGaN-based self-assembled nanowires (NWs) as building blocks for ultraviolet (UV) optoelectronics grown by plasma-assisted molecular beam epitaxy. We review the basic growth kinetics on various foundry-compatible-metal/silicon-based substrates and the epistructure design for UV devices. We highlight the use of diffusion-barrier-metal thin film on silicon substrate as a solution to enhance device performance. NWs offer the opportunity to mitigate the detrimental quantum-confined Stark effect (QCSE), which lowers the recombination rate thereby reducing the device efficiency. On the other hand, the polarization-induced doping from the graded composition along NWs can be advantageous for eluding the inefficient doping in AlGaN-based UV devices. Sidewall surface states and the associate passivation treatment, as well as the use of ultrafast electron-microscopy characterization, are crucial investigations in shedding light on device performance under the influence of surface dangling bonds. For investigating the electrical performance of individual NWs and NWs light-emitting diode as a single entity, recent reports based on conductive atomic force microscopy measurements provide fast-prototyping in-process pass-fail evaluation and a means of improving growth for high-performance devices. Stress tests of NWs devices, crucial for reliable operation, are also discussed. Beyond applications in LEDs, an AlGaN-based NWs solar-blind photodetector demonstrated leveraging on the dislocation-free active region, reduced QCSE, enhanced light absorption, and tunable-composition features. The review opens pathways and offers insights for practical realization of AlGaN-based axial NWs devices on scalable and low-cost silicon substrates.