Deep Ultraviolet Light Emitters Research Articles

Temperature-Dependent Optical Behaviors and Demonstration of Carrier Localization in Polar and Semipolar AlGaN Multiple Quantum Wells

Semipolar AlGaN multiple quantum wells (MQWs) have unique advantages in deep ultraviolet light emitters due to the weak Quantum-Confined Stark Effect. However, their applications are hampered by the poor crystalline quality of semipolar AlGaN thin films. Different treatments were developed to improve the crystal quality of semipolar AlGaN, including a multistep in situ thermal annealing technique proposed by our group. In this work, temperature-dependent and time-resolved photoluminescence characterizations were performed to reveal the carrier localization in the MQW region. The degree of carrier localization in semipolar AlGaN MQWs grown on top of the in situ-annealed AlN is similar to that of conventional ex situ face-to-face annealing, both of which are significantly stronger than that of the c-plane counterpart. Moreover, MQWs on in situ-annealed AlN show drastically reduced dislocation densities, demonstrating its great potential for the future development of high-efficiency optoelectronic devices.

Improved crystallinity and surface morphology of a-plane AlN grown on high temperature annealed AlN/sapphire template by pulsed-flow mode metal-organic vapor phase epitaxy

Preparing high quality non-polar aluminum nitride (AlN) templates is the key to improving the performance of non-polar deep-ultraviolet light-emitting diodes. In this study, we investigated the effect of buffer layer on the crystallinity and surface morphology of a-plane AlN films regrown by pulsed-flow mode (PM) metal-organic vapor phase epitaxy (MOVPE). Three buffer layers were compared including low-temperature AlN buffer layer grown by MOVPE (MO-buffer), sputtered AlN buffer layer (SP-buffer), and high-temperature annealed sputtered AlN buffer layer (HTA-buffer). It is found that the (11-20) plane x-ray rocking curve-full width at half maximum (XRC-FWHM) values of a-plane AlN films are significantly reduced after the regrowth process. Thanks to the high crystalline quality of HTA-buffer, AlN regrown on HTA-buffer exhibits the smallest (11-20) plane XRC-FWHM values of 1260/1440 arcsec along the [0001]/[1-100] direction. The mosaic tilt and basal plane stacking fault density are estimated to be 0.41° and 1.76 106 cm−1, respectively. The surface shows a uniform stripe-like pattern with the lowest root mean square value of 0.82 nm. Furthermore, the a-plane AlN epilayer regrown on HTA-buffer displays a weak in-plane stress anisotropy and high optical transmittance in the ultraviolet-visible region. Our work suggests that combining the PM regrowth with HTA-AlN buffer layer is a promising route to prepare high-quality a-plane AlN templates for efficient non-polar deep-ultraviolet light emitters.

Improving Charge Carrier Transport Properties in AlGaN Deep Ultraviolet Light Emitters Using Al-Content Engineered Superlattice Electron Blocking Layer

In this study, we investigate a unique Al-content engineered superlattice electron blocking layer (AESL-EBL) for improving the charge carrier transport properties of AlGaN quantum well (QW) deep ultraviolet (DUV) light-emitting diode (LED) structures. LED structures without EBL, with conventional bulk EBL (BEBL), and superlattice EBL (SL-EBL) are used for comparison. It is found that the LED structure with the AESL-EBL can exhibit superior electron blocking and hole injection, leading to reduced efficiency droop and improved light output power, compared to LED structures without EBL and with BEBL. Notably, the LED structure with AESL-EBL also outperforms the LED structure with SL-EBL, benefitting from the Al-content engineered SL. In the end, such an ASEL-EBL is applied to a DUV laser diode structure, and by optimizing the device structure low Mg-induced internal loss of around 1 cm−1 can be obtained.

Enhanced semiconductor nanowires improve safety of deep ultraviolet light emitters

Tunnel junctions and polarization doping may overcome challenges with short wavelength LEDs.

Recombination dynamics of indirect excitons in hexagonal BN epilayers containing polytypic segments grown by chemical vapor deposition using carbon-free precursors

Hexagonal (h) BN is a semiconductor that crystallizes in layers of a two-dimensional honeycomb structure. Since hBN exhibits high quantum efficiency (QE) near-band edge emission at around 5.8 eV in spite of the indirect bandgap, hBN has a potential for the use in deep-ultraviolet light emitters. For elucidating the emission dynamics of indirect excitons (iXs) in hBN, spatially and temporally resolved luminescence measurements were carried out on hBN epilayers grown using carbon-free precursors. In addition to major μm-side flat-topped (0001) hBN columnar grains, sub-μm-scale polytypic segments were identified, which were likely formed by certain growth instabilities. The hBN domains exhibited predominant emissions of phonon-assisted fundamental iXs at 5.7–5.9 eV and a less-pronounced 4.0-eV emission band. The photoluminescence lifetime (τPL) for the iX emissions was 54 ps, which most likely represents the midgap recombination lifetime (τMGR) for an iX reservoir. Because τPL did not change while the cathodoluminescence (CL) intensity increased with temperature above 100 K, both the immobile character of iXs and strong exciton–phonon interaction seem significant for procreating the high QE. The CL intensity and τPL of the 5.5 eV band monotonically decreased with temperature, indicating that τPL represents τMGR, most probably a nonradiative lifetime, around the real states. Equally significant emissions at 6.035 eV at 12 K and 6.0–6.1 eV at 300 K were observed from the polytypic segments, most probably graphitic bernal BN, which also exhibited negligible thermal quenching property.

Regulation of surface kinetics: rapid growth of n-AlGaN with high conductivity for deep-ultraviolet light emitters

Surface kinetics in Al-rich AlGaN growth are regulated to realize a growth window allowing a higher rate as well as a lower temperature. Hence a rate of 2.3 μm h−1 at 1050 °C is achieved for n-Al0.55Ga0.45N with the typical step-terrace morphology.

Electronic degeneracy conduction in highly Si-doped Al0.6Ga0.4N layers based on the carrier compensation effect

Electronic degeneracy to express metallic conduction in Al-rich AlGaN for the electron injection layer enhances the efficiencies of deep ultraviolet light emitters. This study systematically demonstrates the Si doping range and conditions to realize degenerate n-type Al0.6Ga0.4N layers based on the electron compensation effect. The temperature-independent electron concentrations resulting from the degenerate band appear in high Si doping conditions to overcome the electron compensation due to carbon on nitrogen sites (CN). However, excessive Si doping of over 4.0 × 1019 cm−3 leads to the collapse of the electronic degeneracy and a switch to the temperature-dependent electron transport via the impurity bands, where the luminescence bands originating from III vacancy-Si complexes (VIII-nSi) are dominant. The key parameter is the effective donor concentration, Nd − Na, based on the reduction in electron concentrations via acceptor-like deep levels such as CN and VIII-nSi. The Hall-effect analyses for n-type Al0.6Ga0.4N layers with various Si concentrations yielded an Nd − Na value of (9.5 ± 2.9) × 1018 cm−3 to vanish the ionization energy of Si donors, which is approximately six times higher than that in GaN. The results suggest not only the optimal doping range to obtain an Al-rich AlGaN layer with metallic conduction but also the necessity of the growth condition to minimize electron compensation.

Molecular Beam Epitaxy of III-Nitride Nanowires: Emerging Applications From Deep-Ultraviolet Light Emitters and Micro-LEDs to Artificial Photosynthesis

Low-dimensional nanowires have received increased interest as building blocks for electronic and photonic devices. In this article, we review the recent progress made on III -nitridenanowire photonic devices by molecular beam epitaxy (MBE), with a focus on micro-LED s, deep-ultraviolet (UV)-light emitters, and solar fuel and artificial photosynthesis devices. The challenges and prospects of III -nitride nanowires for these applications are also discussed.

Optical and interface characteristics of Al0.56Ga0.44N/Al0.62Ga0.38N multiquantum wells with ∼280 nm emission grown by plasma-assisted molecular beam epitaxy

We have investigated the nature of Al0.56Ga0.44N/Al0.62Ga0.38N multiquantum wells grown by plasma-assisted molecular beam epitaxy for application in deep-ultraviolet light emitters. Excitation and temperature-dependent and time-resolved photoluminescence measurements and transmission and reflectance spectroscopy have been complemented by high-angle annular dark field scanning transmission electron microscopy. The 3 nm quantum wells are characterized by interface roughness having a height of 0.3–1 nm and the maximum value is in excellent agreement with values obtained from calculations done to analyze the measured photoluminescence lineshape. The radiative lifetime increases with temperature, suggesting the role of electron-hole scattering to cool photoexcited carriers to the ground state of the quantum wells.

Heavy Mg-doping of (Al,Ga)N films for potential applications in deep ultraviolet light-emitting structures

Doping of high aluminum-containing (Al,Ga)N thin films has remained a challenging problem that has hindered progress in the development of deep ultraviolet light-emitters. This paper reports on the synthesis and use of heavily doped (Al,Ga)N films in deep ultraviolet (∼274 nm) light-emitting structures; these structures were synthesized by molecular beam epitaxy under liquid-metal growth conditions that facilitate the incorporation of extremely high density of Mg dopant impurities (up to 5 × 1019 cm−3) into aluminum-rich (Al,Ga)N thin films. Prototypical light-emitting diode structures incorporating Al0.7Ga0.3N films doped with Mg impurities that ionize to give free hole carrier concentrations of up to 6 × 1017 cm−3 exhibit external quantum efficiencies of up 0.56%; this is an improvement from previous devices made from molecular beam epitaxy-grown materials. This improvement is believed to be due to the high hole carrier concentration enabled by the relatively low activation energy of 220 meV compared to the expected values of 408–507 meV for Al0.7Ga0.3N films.

85% internal quantum efficiency of 280-nm AlGaN multiple quantum wells by defect engineering

In this study, high internal-quantum-efficiency (IQE) AlGaN multiple quantum wells (MQWs) were successfully demonstrated on low-defect-density AlN templates with nano-patterned sapphire substrates. These templates consisted of AlN structures with 0∼30 periods superlattices (SLs) by alternating high (100) and low (25) V/III ratios under a low growth temperature (1130 °C). Compared to conventional high crystal-quality AlN epilayers achieved at temperatures ≥1300 °C, lower thermal budget can reduce the production cost and wafer warpage. Via optimization of the SL period, the AlN crystallinity was systematically improved. Strong dependence of SL period number on the X-ray full-width-at-half-maximum (FWHM) of the AlN epilayer was observed. The AlN template with 20-period SLs exhibited the lowest FWHM values for (0002) and (10ī2), namely 331 and 652 arcsec, respectively, as well as an ultra-low etching pit density of 1 × 105 cm−2. The relative IQE of 280 nm AlGaN MQWs exhibited a dramatically increase from 22.8% to 85% when the inserted SL increased from 0 to 20 periods. It has hardly ever been reported for the AlGaN MQW sample. The results indicate that the engineered AlN templates have high potential applications in deep ultraviolet light emitters.

Enhanced ultraviolet emission and its irreversible temperature antiquenching behavior of twofold coordinated silicon centers in silica glass

It has been well documented that an oxygen divacancy center, or a twofold-coordinated Si center, in silica glass yields a singlet-to-singlet photoluminescence (PL) emission at 4.4 eV with a decay time of ∼4 ns. Although the 4.4-eV PL band is interesting in terms of a deep-ultraviolet light emitter, the emission efficiency has been too low to be considered for a practical application. In this work, we show that a highly luminescent silica glass, with an internal quantum yield of 68% for the 4.4-eV PL band at room temperature, can be prepared when micrometer-sized silica powders are heat treated at ∼1900 °C under inert gas atmosphere by using a high-frequency induction heating unit equipped with a graphite crucible. We also show that the intensity of the 4.4-eV emission in the thus prepared silica glass exhibits an irreversible temperature antiquenching behavior in the temperature region below ∼320 K during heating-cooling cycles. The anomalous temperature dependencies of the 4.4-eV emission can be interpreted in terms of thermally activated trapping-detrapping processes of photoexcited electrons associated with deep trap states.

Dilute-As AlNAs Alloy for Deep-Ultraviolet Emitter.

The band structures of dilute-As AlNAs alloys with As composition ranging from 0% up to 12.5% are studied by using First-Principle Density Functional Theory (DFT) calculation. The energy band gap shows remarkable reduction from 6.19 eV to 3.87 eV with small amount of As content in the AlNAs alloy, which covers the deep ultraviolet (UV) spectral regime. A giant bowing parameter of 30.5 eV ± 0.5 eV for AlNAs alloy is obtained. In addition, our analysis shows that the crossover between crystal field split-off (CH) band and heavy hole (HH) bands occurs in the dilute-As AlNAs alloy with As-content of ~1.5%. This result implies the possibility of dominant transverse electric (TE)-polarized emission by using AlNAs alloy with dilute amount of As-content. Our findings indicate the potential of dilute-As AlNAs alloy as the new active region material for TE-polarized III-Nitride-based deep UV light emitters.

Direct band gap carbon superlattices with efficient optical transition

We report pure carbon-based superlattices that exhibit direct band gaps and excellent optical absorption and emission properties at the threshold energy. The structures are nearly identical to that of cubic diamond except that defective layers characterized by five- and seven-membered rings are intercalated in the diamond lattice. The direct band gaps lie in the range of 5.6~5.9 eV, corresponding to wavelengths of 210~221 nm. The dipole matrix elements of direct optical transition are comparable to that of GaN, suggesting that the superlattices are promising materials as an efficient deep ultraviolet light emitter. Molecular dynamics simulations show that the superlattices are thermally stable even at a high temperature of 2000 K. We provide a possible route to the synthesis of superlattices through wafer bonding of diamond (100) surfaces.

Color-Saturated ZnO Deep-Ultraviolet Light Emitters with AlN Server Layer

Color-Saturated ZnO Deep-Ultraviolet Light Emitters with AlN Server Layer

High Mg-content wurtzite MgZnO alloys and their application in deep-ultraviolet light-emitters pumped by accelerated electrons

High Mg-content single-phase wurtzite MgZnO alloys with a bandgap of 4.35 eV have been obtained on sapphire substrate by introducing a composition-gradient MgxZn1−xO buffer layer. By employing the accelerated electrons obtained in a solid-state structure as an excitation source, an emission at around 285 nm, which is originated from the near-band-edge emission of the Mg0.51Zn0.49O active layer, has been observed. The results reported in this paper may provide a promising route to high performance deep-ultraviolet light-emitting devices by bypassing the challenging doping issues of wide bandgap semiconductors.

Enhanced vertical and lateral hole transport in high aluminum-containing AlGaN for deep ultraviolet light emitters

Improved p-type conductivity is demonstrated in AlGaN:Mg superlattice (SL) cladding layers with average Al composition ∼60%. The vertical conductivity ranges from 6.6 × 10−5 S/cm at a DC current of 1 mA to ∼0.1 S/cm at 550 mA and approaches the lateral conductivity that was obtained from Hall-effect measurements. The effective acceptor activation energy (EA) in the SL was determined to be 17 meV, nearly 10× smaller than EA in homogeneous p-GaN. The devices sustain current densities of 11 kA/cm2 under DC and up to 21 kA/cm2 under pulsed operation.

Crystallinity improvement of hexagonal boron nitride films by molybdenum catalysts during microwave plasma chemical vapor deposition and post-annealing

Hexagonal boron nitride (hBN) is a promising deep ultraviolet light emitter. Here we report the catalytic growth of hBN films by microwave plasma chemical vapor deposition (MPCVD). The hBN films were first grown on Mo/Si substrate from a gas mixture of N2, BF3, and H2 and then annealed in nitrogen for 3h at 900°C. The Mo catalysts exhibit obvious catalyzing effects in improving the crystallinity of the hBN films during the growth and annealing processes. Well-crystallized hBN films with small Raman peak width of 9.3cm−1 and sharp photoluminescence emission peak at 293nm were obtained.

Deep Ultraviolet Light-Emitting Hexagonal Boron Nitride Synthesized at Atmospheric Pressure

Materials emitting light in the deep ultraviolet region around 200 nanometers are essential in a wide-range of applications, such as information storage technology, environmental protection, and medical treatment. Hexagonal boron nitride (hBN), which was recently found to be a promising deep ultraviolet light emitter, has traditionally been synthesized under high pressure and at high temperature. We successfully synthesized high-purity hBN crystals at atmospheric pressure by using a nickel-molybdenum solvent. The obtained hBN crystals emitted intense 215-nanometer luminescence at room temperature. This study demonstrates an easier way to grow high-quality hBN crystals, through their liquid-phase deposition on a substrate at atmospheric pressure.

Synthesis of high-purity boron nitride single crystals under high pressure by using Ba–BN solvent

High-purity cubic boron nitride (cBN) and hexagonal boron nitride (hBN) single crystals were synthesised at 4.5 GPa and 1500 °C using barium boron nitride as a solvent. Secondary ion mass spectrometry was used to analyse impurities in the crystals. Fine cBN and hBN crystals, whose oxygen and carbon concentrations were less than 10 18 atoms/cm 3, were obtained, and their band-edge optical properties were measured by cathodoluminescence spectroscopy. High-purity hBN single crystals exhibited intense ultraviolet emission, demonstrating their promise for use as deep ultraviolet-light emitters.