Quantum dots (QDs) based on III-nitride semiconductors are promising for single photon emission at non-cryogenic temperatures due to their large exciton binding energies. Here, we demonstrate GaN QD single photon emitters operating at 300 K with g (2) (0) = 0.17±0.08 under continuous wave excitation. At this temperature, single photon emission rates up to 6 × 10 6 s −1 are reached while g (2) (0) ≤ 0.5 is maintained. Our results are achieved for GaN QDs embedded in a planar AlN layer grown on silicon, representing a promising pathway for future interlinkage with optical waveguides and cavities. These samples allow exploring the limiting factors to key performance metrics for single photon sources, such as brightness and single photon purity. While high brightness is assured by large exciton binding energies, the single photon purity is mainly affected by the spectral overlap with the biexcitonic emission. Thus, the performance of a GaN QD as a single photon emitter depends on the balance between the emission linewidth and the biexciton binding energy. We identify small GaN QDs with an emission energy in excess of 4.2 eV as promising candidates for future room temperature applications, since the biexciton binding energy becomes comparable to the average emission linewidth of around 55 meV.Quantum dots (QDs) based on III-V semiconductors have attracted a lot of attention for their use as nonclassical light sources, with the single photon source being the simplest and most elemental representative. Such a source of single photons should be as bright as possible, while retaining a high single photon purity [1, 2]. However, key metrics for such QD-based single photon sources are usually achieved at cryogenic temperatures with the seminal In(Ga)As/(Al)GaAs system [3][4][5]. Identifying a material platform that can enable sufficiently performant single photon sources up to room temperature remains a challenging quest. In this respect, the main contenders are point defects in wide-bandgap semiconductors (2D materials [6] and bulk semiconductors [7, 8]), nitrogen and silicon vacancies in diamond [9], as well as semiconductor QDs [10][11][12]. It would be advantageous to employ a material system with high integrability into a suitable photonic environment that offers epitaxial control. In this regard, III-nitrides offer a unique possibility as bipolar doping can be achieved, foreign and homoepitaxial substrates are available, and growth and processing techniques are well established, leading to their widespread implementation at an industrial scale for solid state lighting.III-nitrides have shown promising advances in terms of single photon emission (SPE) by employing GaN/AlN [13,14], GaN/AlGaN [15,16] and InGaN/GaN QDs [17][18][19][20][21]. Furthermore, SPE at temperatures as high as 350 K [22] and two-photon emission up to 50 K [23] have been demonstrated. The progress towards room temperature operation is directly linked to the exciton-phonon coupling. With rising temperature the phonon bath becomes * sebastian.tamariz...
c-plane GaN/AlN quantum dots (QDs) are promising zero-dimensional quantum nanostructures that exhibit single photon emission properties up to room temperature and even above. In this context, it is of prime interest to gain a deeper insight into the recombination dynamics of photogenerated electron-hole pairs captured by such dots. Hence, in this work, we study the time-resolved photoluminescence (PL) properties in the low injection regime and at cryogenic temperatures of c-plane GaN/AlN QD ensembles emitting above the bulk GaN bandgap in order to properly understand the nature of the recombination channels behind the observed non-exponential decay time profiles. Such decays reveal the existence of a relaxation channel competing with the radiative recombination one. It is thus observed that for the former process the dynamics is independent of the dot height, which is attributed to a reversible nonradiative transfer that could be mediated by a spin-flip process to a dark-level state. The radiative recombination process is recognizable thanks to the characteristic dependence of its lifetime with the emission energy, which is well accounted for by the built-in electric field inherent to quantum nanostructures grown along the c-axis and the variations in the lateral confinement at play in such QDs. Those conclusions are drawn from the analysis of the time-evolution of the PL spectra by means of a simple analytical model that enables to exclude any screening of the built-in electric field. III. RESULTS
Full control over the density and emission properties of GaN quantum dots (QDs) should be feasible, provided that the growth proceeds in the Stranski-Krastanov (SK) growth mode. In this work, we derive the phase diagram for GaN QD formation on AlN by NH3-molecular beam epitaxy and analyze the corresponding optical signature by micro-photoluminescence (μ-PL). Interestingly, the growth window for SK-GaN QDs is very narrow due to the relatively small lattice mismatch of the GaN/AlN system (2.5%), constituting a fundamental challenge for QD growth control. By relying on bulk AlN single crystal substrates, we demonstrate QD density control over three orders of magnitude, from 108 to 1011 cm−2 by changing the growth rate. In contrast, the QD density is pinned to 2 × 1010 cm−2 when growing on AlN/sapphire templates, which exhibit dislocation densities on the order of 1010 cm−2. Thanks to QD densities as low as 108 cm−2 on bulk AlN, we can probe the emission of spatially isolated single GaN QDs by μ-PL on unprocessed samples.
III-nitride quantum dots (QDs) are a promising system actively studied for their ability to maintain single photon emission up to room temperature. Here, we report on the evolution of the emission properties of self-assembled GaN/AlN QDs for temperatures ranging from 5 to 300 K. We carefully track the photoluminescence of a single QD and measure an optimum single photon purity of g(2)(0) = 0.05 ± 0.02 at 5 K and 0.17 ± 0.08 at 300 K. We complement this study with temperature dependent time-resolved photoluminescence measurements (TRPL) performed on a QD ensemble to further investigate the exciton recombination dynamics of such polar zero-dimensional nanostructures. By comparing our results to past reports, we emphasize the complexity of recombination processes in this system. Instead of the more conventional mono-exponential decay typical of exciton recombination, TRPL transients display a bi-exponential feature with short- and long-lived components that persist in the low excitation regime. From the temperature insensitivity of the long-lived excitonic component, we first discard the interplay of dark-to-bright state refilling in the exciton recombination process. Besides, this temperature-invariance also highlights the absence of nonradiative exciton recombinations, a likely direct consequence of the strong carrier confinement observed in GaN/AlN QDs up to 300 K. Overall, our results support the viability of these dots as a potential single-photon source for quantum applications at room temperature.
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