RESUMO
Giant shell CdSe/CdS quantum dots are bright and flexible emitters, with near-unity quantum yield and suppressed blinking, but their single photon purity is reduced by efficient multiexcitonic emission. We report the observation, at the single dot level, of a large blueshift of the photoluminescence biexciton spectrum (24 ± 5 nm over a sample of 32 dots) for pure-phase wurtzite quantum dots. By spectral filtering, we demonstrate a 2.3 times reduction of the biexciton quantum yield relative to the exciton emission, while preserving as much as 60% of the exciton single photon emission, thus improving the purity from g2(0) = 0.07 ± 0.01 to g2(0) = 0.03 ± 0.01. At a larger pump fluency, spectral purification is even more effective with up to a 6.6 times reduction in g2(0), which is due to the suppression of higher order excitons and shell states experiencing even larger blueshifts. Our results indicate the potential for the synthesis of engineered giant shell quantum dots, with further increased biexciton blueshifts, for quantum optical applications requiring both high purity and brightness.
RESUMO
Electron transfer to an individual quantum dot promotes the formation of charged excitons with enhanced recombination pathways and reduced lifetimes. Excitons with only one or two extra charges have been observed and exploited for very efficient lasing or single-quantum dot light-emitting diodes. Here, by room-temperature time-resolved experiments on individual giant-shell CdSe/CdS quantum dots, we show the electrochemical formation of highly charged excitons containing more than 12 electrons and 1 hole. We report the control over intensity blinking, along with a deterministic manipulation of quantum dot photodynamics, with an observed 210-fold increase in the decay rate, accompanied by 12-fold decrease in the emission intensity, while preserving single-photon emission characteristics. These results pave the way for deterministic control over the charge state, and room-temperature decay rate engineering for colloidal quantum dot-based classical and quantum communication technologies.
RESUMO
Quantum emitters radiate light omni-directionally, making it hard to collect and use the generated photons. Here, we propose a three-dimensional metal-dielectric parabolic antenna surrounding an individual quantum dot as a source of collimated single photons, which can then be easily extracted and manipulated. Our fabrication method relies on a single optically induced polymerization step once the selected emitter has been localized by confocal microscopy. Compared to conventional nanoantennas, our geometry does not require near-field coupling, and it is, therefore, very robust against misalignment issues and minimally affected by absorption in the metal. The parabolic antenna provides one of the largest reported experimental directivities ( D = 106) and the lowest beam divergences (Θ1/2 = 13.5°) and a broadband operation over all of the visible and near-infrared range together with extraction efficiency of more than 96%, offering a practical advantage for quantum technological applications.
