We present an approach, where point defects and defect complexes are identified using power dependent photoluminescence excitation spectroscopy, impurity data from SIMS and DFT-based calculations accounting for the total charge balance in the crystal. Employing the capabilities of such experimental-computational approach, in this work, the UVC absorption band at 4.7 eV, as well as the 2.7 eV and 3.9 eV luminescence bands in AlN single crystals grown via physical vapor transport (PVT) are studied in detail. Photoluminescence excitation spectroscopy measurements demonstrate the relationship between the defect luminescent bands centered at 3.9 eV and 2.7 eV to the commonly observed absorption band centered at 4.7 eV. Accordingly, the thermodynamic transition energy for the absorption band at 4.7 eV and the luminescence band at 3.9 eV is estimated at 4.2 eV, in agreement with the thermodynamic transition energy for the C N point defect. Finally, the 2.7 eV PL band is the result of a donor-acceptor pair transition between the V N and C N point defects since nitrogen vacancies, is predicted to be present in the crystal in concentrations similar to carbon employing charge balance constrained DFT calculations. Power dependent photoluminescence measurements reveal the presence of the deep donor state with a thermodynamic transition energy of 5.0 eV, which we hypothesize to be nitrogen vacancies in agreement with predictions based on theory. The charge state, concentration and type of impurities in the crystal is calculated considering a fixed amount of impurities and using a density functional theory (DFT) based defect solver, which considers their respective formation energies and the total charge balance in the crystal. The presented results show that nitrogen vacancies are the most likely candidate for the deep donor state involved in the donor acceptor pair transition with peak emission at 2.7 eV for the conditions relevant to PVT growth.

In this work, we employed X-ray photoelectron spectroscopy to determine the band offsets and interface Fermi level at the heterojunction formed by stoichiometric silicon nitride deposited on AlxGa1-xN (of varying Al composition “x”) via low pressure chemical vapor deposition. Silicon nitride is found to form a type II staggered band alignment with AlGaN for all Al compositions (0 ≤ x ≤ 1) and present an electron barrier into AlGaN even at higher Al compositions, where Eg(AlGaN) > Eg(Si3N4). Further, no band bending is observed in AlGaN for x ≤ 0.6 and a reduced band bending (by ∼1 eV in comparison to that at free surface) is observed for x > 0.6. The Fermi level in silicon nitride is found to be at 3 eV with respect to its valence band, which is likely due to silicon (≡Si0/−1) dangling bonds. The presence of band bending for x > 0.6 is seen as a likely consequence of Fermi level alignment at Si3N4/AlGaN hetero-interface and not due to interface states. Photoelectron spectroscopy results are corroborated by current-voltage-temperature and capacitance-voltage measurements. A shift in the interface Fermi level (before band bending at equilibrium) from the conduction band in Si3N4/n-GaN to the valence band in Si3N4/p-GaN is observed, which strongly indicates a reduction in mid-gap interface states. Hence, stoichiometric silicon nitride is found to be a feasible passivation and dielectric insulation material for AlGaN at any composition.

Periodically poled AlN thin films with submicron domain widths were fabricated for nonlinear applications in the UV-VIS region. A procedure utilizing metalorganic chemical vapor deposition growth of AlN in combination with laser interference lithography was developed for making a nanoscale lateral polarity structure (LPS) with domain size down to 600 nm. The Al-polar and N-polar domains were identified by wet etching the periodic LPS in a potassium hydroxide solution and subsequent scanning electron microscopy (SEM) characterization. Fully coalesced and well-defined vertical interfaces between the adjacent domains were established by cross-sectional SEM. AlN LPSs were mechanically polished and surface roughness with a root mean square value of ∼10 nm over a 90 μm × 90 μm area was achieved. 3.8 μm wide and 650 nm thick AlN LPS waveguides were fabricated. The achieved domain sizes, surface roughness, and waveguides are suitable for second harmonic generation in the UVC spectrum.

As an alternative to electrically injected diodes, UV light emission can be obtained via second harmonic generation (SHG). In weakly birefringent materials such as aluminum nitride (AlN), the phase matching of the driving and second harmonic waves can be achieved by the quasi-phase-matching (QPM) technique, where the polarity of the material is periodically changed commensurate with the coherence wavelength. QPM also allows the use of the highest nonlinear susceptibility, and therefore, higher conversion efficiencies are possible. In this work, the QPM SHG of UV light in AlN lateral polar structure-based waveguides is demonstrated. The peak intensity of the frequency doubled laser light was measured at 344 nm and 472 nm wavelengths, in agreement with dispersion-based theoretical predictions. These results confirm the potential of III-nitride-based lateral polar structures for quasi-phase-matched nonlinear optics and for frequency doubling media for UV light generation.