Advanced Scanning Probe Nanolithography Using GaN Nanowires.

A fundamental understanding and advancement of nanopatterning and nanometrology are essential in the future development of nanotechnology, atomic scale manipulation, and quantum technology industries. Scanning probe-based patterning/imaging techniques have been attractive for many research groups to conduct their research in nanoscale device fabrication and nanotechnology mainly due to its cost-effective process; however, the current tip materials in these techniques suffer from poor durability, limited resolution, and relatively high fabrication costs. Here, we report on employing GaN nanowires as a robust semiconductor material in scanning probe lithography (SPL) and microscopy (SPM) with a relatively low-cost fabrication process and the capability to provide sub-10 nm lithography and atomic scale (<1 nm) patterning resolution in field-emission scanning probe lithography (FE-SPL) and scanning tunneling microscopy (STM), respectively. We demonstrate that GaN NWs are great candidates for advanced SPL and imaging that can provide atomic resolution imaging and sub-10 nm nanopatterning on different materials in both vacuum and ambient operations.

Thermal and efficiency droop in InGaN/GaN light-emitting diodes: decoupling multiphysics effects using temperature-dependent RF measurements.

Multiphysics processes such as recombination dynamics in the active region, carrier injection and transport, and internal heating may contribute to thermal and efficiency droop in InGaN/GaN light-emitting diodes (LEDs). However, an unambiguous methodology and characterization technique to decouple these processes under electrical injection and determine their individual roles in droop phenomena is lacking. In this work, we investigate thermal and efficiency droop in electrically injected single-quantum-well InGaN/GaN LEDs by decoupling the inherent radiative efficiency, injection efficiency, carrier transport, and thermal effects using a comprehensive rate equation approach and a temperature-dependent pulsed-RF measurement technique. Determination of the inherent recombination rates in the quantum well confirms efficiency droop at high current densities is caused by a combination of strong non-radiative recombination (with temperature dependence consistent with indirect Auger) and saturation of the radiative rate. The overall reduction of efficiency at elevated temperatures (thermal droop) results from carriers shifting from the radiative process to the non-radiative processes. The rate equation approach and temperature-dependent pulsed-RF measurement technique unambiguously gives access to the true recombination dynamics in the QW and is a useful methodology to study efficiency issues in III-nitride LEDs.

Polarization-pinned emission of a continuous-wave optically pumped nonpolar GaN-based VCSEL using nanoporous distributed Bragg reflectors.

A nonpolar GaN-based vertical-cavity surface-emitting laser (VCSEL) using nanoporous bottom epitaxial distributed Bragg reflector (DBR) is demonstrated at room temperature (RT) under continuous-wave (CW) optical pumping. The porous layers enable the epitaxial growth of lattice-matched high-reflectance DBRs without sacrificing the conductive properties needed for high-performance VCSELs. The 2-λ cavity VCSEL reported here employs a hybrid design with top dielectric DBR and bottom nanoporous DBR. Single longitudinal mode lasing is observed at 462 nm with a threshold power density of ~5 kW/cm2 and a FWHM of ~0.12 nm. The emission polarization was pinned in the a-direction at all measured locations.

Spectrally-resolved internal quantum efficiency and carrier dynamics of semipolar [Formula: see text] core-shell triangular nanostripe GaN/InGaN LEDs.

We investigate the spectrally resolved internal quantum efficiency (IQE) and carrier dynamics in semipolar [Formula: see text] core-shell triangular nanostripe light-emitting diodes (TLEDs) using temperature-dependent photoluminescence (TDPL) and time-resolved photoluminescence (TRPL) at various excitation energy densities. Using electroluminescence, photoluminescence, and cathodoluminescence measurements, we verify the origins of the broad emission spectra from the nanostructures and confirm that localized regions of high-indium-content InGaN exist along the apex of the nanostructures. Spectrally resolved IQE measurements are then performed, with the spectra integrated from 400-450 nm and 450-500 nm to obtain the IQE of the QWs mainly near the sidewalls and apex of the TLEDs, respectively. TDPL and TRPL are used to decouple the radiative and non-radiative carrier lifetimes for different regions of the emission spectra. We observe that the IQE is higher for the spectral region between 450 nm and 500 nm compared to the IQE between 400 and 450 nm. This result is in contrast to the typical observation that the IQE of planar GaN-based LEDs is lower for longer wavelengths (i.e., higher indium contents). We also observe a longer non-radiative recombination lifetime for the longer wavelength portion of the spectrum. Several explanations are proposed for the improved IQE and longer non-radiative lifetime observed near the apex of the nanostructures. The results show that nanostructures may be leveraged to design more efficient green LEDs, potentially addressing a long-standing challenge in GaN-based materials.

Insufficiency of the Young's modulus for illustrating the mechanical behavior of GaN nanowires.

We use a non-classical modified couple stress theory including the acceleration gradients (MCST-AG), to precisely demonstrate the size dependency of the mechanical properties of gallium nitride (GaN) nanowires (NWs). The fundamental elastic constants, Young's modulus and length scales of the GaN NWs were estimated both experimentally, using a novel experimental technique applied to atomic force microscopy, and theoretically, using atomic simulations. The Young's modulus, static and the dynamic length scales, calculated with the MCST-AG, were found to be 323 GPa, 13 and 14.5 nm, respectively, for GaN NWs from a few nanometers radii to bulk radii. Analyzing the experimental data using the classical continuum theory shows an improvement in the experimental results by introducing smaller error. Using the length scales determined in MCST-AG, we explain the inconsistency of the Young's moduli reported in recent literature, and we prove the insufficiency of the Young's modulus for predicting the mechanical behavior of GaN NWs.

Scalable Top-Down Approach Tailored by Interferometric Lithography to Achieve Large-Area Single-Mode GaN Nanowire Laser Arrays on Sapphire Substrate.

GaN nanowires are promising for optical and optoelectronic applications because of their waveguiding properties and large optical band gap. However, developing a precise, scalable, and cost-effective fabrication method with a high degree of controllability to obtain high-aspect-ratio nanowires with high optical properties and minimum crystal defects remains a challenge. Here, we present a scalable two-step top-down approach using interferometric lithography, for which parameters can be controlled precisely to achieve highly ordered arrays of nanowires with excellent quality and desired aspect ratios. The wet-etch mechanism is investigated, and the etch rates of m-planes {11̅00} (sidewalls) were measured to be 2.5 to 70 nm/h depending on the Si doping concentration. Using this method, uniform nanowire arrays were achieved over a large area (>105 µm2) with an spect ratio as large as 50, a radius as small as 17 nm, and atomic-scale sidewall roughness (<1 nm). FDTD modeling demonstrated HE11 is the dominant transverse mode in the nanowires with a radius of sub-100 nm, and single-mode lasing from vertical cavity nanowire arrays with different doping concentrations on a sapphire substrate was interestingly observed in photoluminescence measurements. High Q-factors of ∼1139-2443 were obtained in nanowire array lasers with a radius and length of 65 nm and 2 µm, respectively, corresponding to a line width of 0.32-0.15 nm (minimum threshold of 3.31 MW/cm2). Our results show that fabrication of high-quality GaN nanowire arrays with adaptable aspect ratio and large-area uniformity is feasible through a top-down approach using interferometric lithography and is promising for fabrication of III-nitride-based nanophotonic devices (radial/axial) on the original substrate.

Carrier Dynamics and Electro-Optical Characterization of High-Performance GaN/InGaN Core-Shell Nanowire Light-Emitting Diodes.

In this work, we demonstrate high-performance electrically injected GaN/InGaN core-shell nanowire-based LEDs grown using selective-area epitaxy and characterize their electro-optical properties. To assess the quality of the quantum wells, we measure the internal quantum efficiency (IQE) using conventional low temperature/room temperature integrated photoluminescence. The quantum wells show a peak IQE of 62%, which is among the highest reported values for nanostructure-based LEDs. Time-resolved photoluminescence (TRPL) is also used to study the carrier dynamics and response times of the LEDs. TRPL measurements yield carrier lifetimes in the range of 1-2 ns at high excitation powers. To examine the electrical performance of the LEDs, current density-voltage (J-V) and light-current density-voltage (L-J-V) characteristics are measured. We also estimate the peak external quantum efficiency (EQE) to be 8.3% from a single side of the chip with no packaging. The LEDs have a turn-on voltage of 2.9 V and low series resistance. Based on FDTD simulations, the LEDs exhibit a relatively directional far-field emission pattern in the range of [Formula: see text]15°. This work demonstrates that it is feasible for electrically injected nanowire-based LEDs to achieve the performance levels needed for a variety of optical device applications.

Explanation of low efficiency droop in semipolar (202¯1¯) InGaN/GaN LEDs through evaluation of carrier recombination coefficients.

We report the carrier dynamics and recombination coefficients in single-quantum-well semipolar (202¯1¯) InGaN/GaN light-emitting diodes emitting at 440 nm with 93% peak internal quantum efficiency. The differential carrier lifetime is analyzed for various injection current densities from 5 A/cm2 to 10 kA/cm2, and the corresponding carrier densities are obtained. The coupling of internal quantum efficiency and differential carrier lifetime vs injected carrier density (n) enables the separation of the radiative and nonradiative recombination lifetimes and the extraction of the Shockley-Read-Hall (SRH) nonradiative (A), radiative (B), and Auger (C) recombination coefficients and their n-dependency considering the saturation of the SRH recombination rate and phase-space filling. The results indicate a three to four-fold higher A and a nearly two-fold higher B0 for this semipolar orientation compared to that of c-plane reported using a similar approach [A. David and M. J. Grundmann, Appl. Phys. Lett. 96, 103504 (2010)]. In addition, the carrier density in semipolar (202¯1¯) is found to be lower than the carrier density in c-plane for a given current density, which is important for suppressing efficiency droop. The semipolar LED also shows a two-fold lower C0 compared to c-plane, which is consistent with the lower relative efficiency droop for the semipolar LED (57% vs. 69%). The lower carrier density, higher B0 coefficient, and lower C0 (Auger) coefficient are directly responsible for the high efficiency and low efficiency droop reported in semipolar (202¯1¯) LEDs.

GaN nanowire tips for nanoscale atomic force microscopy.

Imaging of high-aspect-ratio nanostructures with sharp edges and straight walls in nanoscale metrology by atomic force microscopy (AFM) has been challenging due to the mechanical properties and conical geometry of the majority of available commercial tips. Here we report on the fabrication of GaN probes for nanoscale metrology of high-aspect-ratio structures to enhance the resolution of AFM imaging and improve the durability of AFM tips. GaN nanowires were fabricated using bottom-up and top-down techniques and bonded to Si cantilevers to scan vertical trenches on Si substrates. Over several scans, the GaN probes demonstrated excellent durability while scanning uneven structures and showed resolution enhancements in topography images, independent of scan direction, compared to commercial Si tips.

Nonpolar InGaN/GaN Core-Shell Single Nanowire Lasers.

We report lasing from nonpolar p-i-n InGaN/GaN multi-quantum well core-shell single-nanowire lasers by optical pumping at room temperature. The nanowire lasers were fabricated using a hybrid approach consisting of a top-down two-step etch process followed by a bottom-up regrowth process, enabling precise geometrical control and high material gain and optical confinement. The modal gain spectra and the gain curves of the core-shell nanowire lasers were measured using micro-photoluminescence and analyzed using the Hakki-Paoli method. Significantly lower lasing thresholds due to high optical gain were measured compared to previously reported semipolar InGaN/GaN core-shell nanowires, despite significantly shorter cavity lengths and reduced active region volume. Mode simulations show that due to the core-shell architecture, annular-shaped modes have higher optical confinement than solid transverse modes. The results show the viability of this p-i-n nonpolar core-shell nanowire architecture, previously investigated for next-generation light-emitting diodes, as low-threshold, coherent UV-visible nanoscale light emitters, and open a route toward monolithic, integrable, electrically injected single-nanowire lasers operating at room temperature.

Internal quantum efficiency and carrier dynamics in semipolar (2021) InGaN/GaN light-emitting diodes.

The internal quantum efficiencies (IQE) and carrier lifetimes of semipolar (202¯1¯) InGaN/GaN LEDs with different active regions are measured using temperature-dependent, carrier-density-dependent, and time-resolved photoluminescence. Three active regions are investigated: one 12-nm-thick single quantum well (SQW), two 6-nm-thick QWs, and three 4-nm-thick QWs. The IQE is highest for the 12-nm-thick SQW and decreases as the well width decreases. The radiative lifetimes are similar for all structures, while the nonradiative lifetimes decrease as the well width decreases. The superior IQE and longer nonradiative lifetime of the SQW structure suggests using thick SQW active regions for high brightness semipolar (202¯1¯) LEDs.

Tailoring the morphology and luminescence of GaN/InGaN core-shell nanowires using bottom-up selective-area epitaxy.

Controlled bottom-up selective-area epitaxy (SAE) is used to tailor the morphology and photoluminescence properties of GaN/InGaN core-shell nanowire arrays. The nanowires are grown on c-plane sapphire substrates using pulsed-mode metal organic chemical vapor deposition. By varying the dielectric mask configuration and growth conditions, we achieve GaN nanowire cores with diameters ranging from 80 to 700 nm that exhibit various degrees of polar, semipolar, and nonpolar faceting. A single InGaN quantum well (QW) and GaN barrier shell is also grown on the GaN nanowire cores and micro-photoluminescence is obtained and analyzed for a variety of nanowire dimensions, array pitch spacings, and aperture diameters. By increasing the nanowire pitch spacing on the same growth wafer, the emission wavelength redshifts from 440 to 520 nm, while increasing the aperture diameter results in a ∼35 nm blueshift. The thickness of one QW/barrier period as a function of pitch and aperture diameter is inferred using scanning electron microscopy, with larger pitches showing significantly thicker QWs. Significant increases in indium composition were predicted for larger pitches and smaller aperture diameters. The results are interpreted in terms of local growth conditions and adatom capture radius around the nanowires. This work provides significant insight into the effects of mask configuration and growth conditions on the nanowire properties and is applicable to the engineering of monolithic multi-color nanowire LEDs on a single chip.

Optical properties of plasmonic light-emitting diodes based on flip-chip III-nitride core-shell nanowires.

In this work, we utilize the finite difference time domain (FDTD) method to investigate the Purcell factor, light extraction efficiency (EXE), and cavity quality parameter (Q), and to predict the modulation response of Ag-clad flip-chip GaN/InGaN core-shell nanowire light-emitting diodes (LEDs) with the potential for electrical injection. We consider the need for a pn-junction, the effects of the substrate, and the limitations of nanoscale fabrication techniques in the evaluation. The investigated core-shell nanowire consists of an n-GaN core, surrounded by nonpolar m-plane quantum wells, p-GaN, and silver cladding layers. The core-shell nanowire geometry exhibits a Purcell factor of 57, resulting in a predicted limit of 30 GHz for the 3dB modulation bandwidth.

Optical polarization characteristics of semipolar (3031) and (3031) InGaN/GaN light-emitting diodes.

Linear polarized electroluminescence was investigated for semipolar (3031) and (3031) InGaN light-emitting diodes (LEDs) with various indium compositions. A high degree of optical polarization was observed for devices on both planes, ranging from 0.37 at 438 nm to 0.79 at 519 nm. The extracted valence band energy separation was consistent with the optical polarization ratios. The effect of anisotropic strain on the valance band structure was studied using k?p method for the above two planes. The theoretical calculations are consistent with the experimental results.