Size-Limited Room Temperature Single-Photon Emission from Sidewall-Treated Fractional Dimension InGaN Quantum Dots: Determined by Density-of-States-Corrected Ultrafast Carrier Dynamics and Improved Signal-to-Noise Ratio

Original Abstract

Room-temperature single-photon emission (SPE) resulting from a biexciton-exciton cascaded decay is demonstrated for the first time from chemically and photoelectrochemically etched site-controlled In0.14Ga0.86N quantum dots (QDs) embedded in vertical GaN nanowires. Diameter-dependent biexciton-exciton dynamics are analysed to determine the eligibility of QD as a single-photon emitter. The signal-to-noise ratio degrades with increasing QD diameter. Background noise photons pose a bottleneck to achieving SPE. This is also explained from a carrier dynamics perspective. Surface recombination contributes to inhomogeneous broadening at QD diameters larger than 35 nm. Below 35 nm, density-of-states-corrected Auger gradually becomes the principal biexciton-decay route with further reduction in QD diameter, thereby quenching the possibility of thermal broadening and setting a threshold for SPE. Below 9 nm, the Auger recombination rate becomes manyfold of other decay rates, causing multi-photon suppression via single Auger decay to form an exciton. Surface recombination probability of this exciton is minimized while biexciton state filling probability is maximized by reducing sidewall surface states through wet-treatment. These improve biexciton state preparation and enhance the single-photon purity of the exciton towards the exciton Bohr radius (3 nm) regime. Far away from this regime, higher-order autocorrelations to characterize quantum emission involving multi-photon events are discussed. This study establishes a generalized physical framework for predetermining SPE probability as a function of QD surface and geometry down to the exciton Bohr radius regime, with practical implementations. This work shows the pathway to design and develop next-generation semiconductor QDs for high-purity room-temperature SPE.