Group-III-nitride semiconductors have shown enormous potential as light sources for full-colour displays, optical storage and solid-state lighting. Remarkably, InGaN blue- and green-light-emitting diodes (LEDs) emit brilliant light although the threading dislocation density generated due to lattice mismatch is six orders of magnitude higher than that in conventional LEDs. Here we explain why In-containing (Al,In,Ga)N bulk films exhibit a defect-insensitive emission probability. From the extremely short positron diffusion lengths (<4 nm) and short radiative lifetimes of excitonic emissions, we conclude that localizing valence states associated with atomic condensates of In-N preferentially capture holes, which have a positive charge similar to positrons. The holes form localized excitons to emit the light, although some of the excitons recombine at non-radiative centres. The enterprising use of atomically inhomogeneous crystals is proposed for future innovation in light emitters even when using defective crystals.
Influences of point defects on the nonradiative processes in ZnO were studied using steady-state and time-resolved photoluminescence (PL) spectroscopy making a connection with the results of positron annihilation measurement. Free excitonic PL intensity naturally increased with the increase in the nonradiative PL lifetime (τnr). Density or size of Zn vacancies (VZn) decreased and τnr increased with increasing growth temperature in heteroepitaxial films grown on a ScAlMgO4 substrate. Use of homoepitaxial substrate further decreased the VZn density. However, τnr was the shortest for the homoepitaxial film; i.e., no clear dependence was found between τnr and density / size of VZn or positron scattering centers. The results indicated that nonradiative recombination processes are not solely governed by single point defects, but by certain defect species introduced by the presence of VZn such as vacancy complexes.
Room-temperature nonradiative lifetime (τnr) of the near-band-edge excitonic photoluminescence (PL) peak in {0001} polar, (112¯0), (11¯00), and (001) nonpolar GaN was shown to increase with the decrease in density or size of Ga vacancies (VGa) and with the decrease in gross density of point defects including complexes, leading to the increase in the PL intensity. As the edge threading dislocation density decreased, density or size of VGa tended to decrease and τnr tended to increase. However, there existed remarkable exceptions. The results indicate that nonradiative recombination process is governed not by single point defects, but by certain defects introduced with the incorporation of VGa, such as VGa-defect complexes.
Defects in GaN grown using metalorganic chemical vapor deposition were studied through the use of monoenergetic positron beams. For Mg-doped GaN, no large change in the diffusion length of positrons was observed before and after activation of Mg. This was attributed to the scattering of positrons by potentials caused by electric dipoles of Mg–hydrogen pairs. For Si-doped GaN, the line-shape parameter S increased as carrier density increased, suggesting an introduction of Ga vacancy due to the Fermi level effect. Based on these results, we discuss the effects of the growth polar direction of GaN on optical properties in this article. Although the optical properties of a GaN film grown toward the Ga face direction exhibited excitonic features, a film grown toward the N face (−c) direction exhibited broadened photoluminescence and transmittance spectra, and a Stokes shift of about 20 meV was observed. This difference was attributed to extended band-tail states introduced by high concentrations of donors and acceptor-type defects in −c GaN.
The internal quantum efficiency (ηint) of the near-band-edge (NBE) excitonic photoluminescence (PL) in ZnO epilayers was significantly improved by eliminating point defects, as well as by the use of ZnO high-temperature-annealed self-buffer layer (HITAB) on a ScAlMgO4 substrate as epitaxial templates. Negatively charged Zn vacancy (VZn) concentration was greatly reduced by high-temperature growth, and slower postgrowth cooling (annealing) under minimum oxygen pressure further reduced the gross concentration of positively and negatively charged and neutral point defects, according to the suppression of nonequilibrium defect quenching. The nonradiative PL lifetime (τnr) at room temperature was increased by decreasing the gross concentration of point defects, as well as by decreasing the concentration of VZn. Accordingly, certain point defect complexes incorporated with VZn (VZn-X complexes) are assigned to the dominant nonradiative recombination centers. As a result of the elimination of point defects, a record long τnr (3.8ns) at 300K was demonstrated. Because the radiative lifetime (τr) is in principle constant in bulk and epitaxial ZnO, the increase in τnr gave rise to the increase in ηint. Rich structures originating from exciton-polaritons and excited states of excitons were eventually observed in the low-temperature PL spectrum of the improved ZnO epilayer on HITAB, of which ηint of the NBE emission was 6.3% at 300K.
Large electron capture-cross-section of the major nonradiative recombination centers in Mg-doped GaN epilayers grown on a GaN substrateThe nonradiative lifetime (s NR ) of the near-band-edge emission in various quality GaN samples is compared with the results of positron annihilation measurement, in order to identify the origin and to determine the capture-cross-section of the major intrinsic nonradiative recombination centers (NRCs). The room-temperature s NR of various n-type GaN samples increased with decreasing the concentration of divacancies composed of a Ga vacancy (V Ga ) and a N vacancy (V N ), namely, V Ga V N . The s NR value also increased with increasing the diffusion length of positrons, which is almost proportional to the inverse third root of the gross concentration of all point defects. The results indicate that major intrinsic NRC in n-type GaN is V Ga V N . From the relationship between its concentration and s NR , its hole capture-cross-section is estimated to be about 7 Â 10 À14 cm 2 . Different from the case of 4H-SiC, the major NRCs in p-type and n-type GaN are different: the major NRCs in Mg-doped p-type GaN epilayers are assigned to multiple vacancies containing a V Ga and two (or three) V N s, namely, V Ga (V N ) n (n ¼ 2 or 3). The ion-implanted Mgdoped GaN films are found to contain larger size vacancy complexes such as (V Ga ) 3 (V N ) 3 . In analogy with GaN, major NRCs in Al 0.6 Ga 0.4 N alloys are assigned to vacancy complexes containing an Al vacancy or a V Ga . Published by AIP Publishing. https://doi.
Luminescence dynamics for the near-band-edge (NBE) emission peak at around 250 nm of c-plane Si-doped Al0.6Ga0.4N films grown on AlN templates by low-pressure metalorganic vapor phase epitaxy were studied using deep ultraviolet time-resolved photoluminescence and time-resolved cathodoluminescence spectroscopies. For the films with the Si-doping concentration, [Si], lower than 1.9 × 1017 cm–3, the doping lessened the concentration of cation vacancies, [VIII], through the surfactant effect or the aid of the reactant doping in a form of H3SiNH2. However, the room-temperature nonradiative lifetime, and, consequently, the equivalent value of internal quantum efficiency in the weak excitation regime steeply decreased when [Si] exceeded 1018 cm−3. Simultaneously, the intensity ratio of the deep-state emission band to the NBE emission abruptly increased. Because the increase in [Si] essentially gives rise to the increase in [VIII] (for [Si]>1.9×1017 cm−3) and the overcompensation of Si is eventually observed for the film with [Si] = 4.0 × 1018 cm−3, the formation of acceptor-type native-defect complexes containing Si such as VIII-SiIII is suggested.
Vacancy‐type defects in Mg‐implanted GaN are probed using monoenergetic positron beams. Mg+ ions are implanted to provide a 500‐nm‐deep box profile with Mg concentrations, [Mg], of 1 × 1017–1 × 1019 cm−3 at room temperature. In the as‐implanted samples, the major defect species is a complex of a Ga vacancy (VGa) and a nitrogen vacancy (VN). After annealing above 1000 °C, the major defect species is changed to vacancy clusters due to vacancy agglomeration. This agglomeration is suppressed, and the agglomeration onset temperature is decreased with a decreasing [Mg]. For samples with [Mg] ≥ 1 × 1018 cm−3, the trapping rate of positrons by vacancy‐type defects decrease after annealing above 1100–1200 °C. This decreases is attributed to the change in the defect charge states from neutral to positive due to a downward shift of the Fermi level. The carrier trapping/detrapping properties of the vacancy‐type defects and their time dependences are also revealed.
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