Strain-induced effects in colloidal quantum dots: lifetime measurements and blinking statistics

Abstract A series of samples of CdSe/Cd x Zn 1−x S core/shell quantum dots have been synthesized in order to measure the influence of lattice-mismatch-induced strain on the photoluminescence (PL) and blinking behaviour. The PL spectra show a significant variation of the fluorescence wavelength even though the colloidal quantum dots (cQDs) are similar in size. The PL excitation spectra show a gradual splitting of the first exciton level as the proportion of Zn is increased in the shell and as the shell grows. On the other hand, blinking studies clearly demonstrate a significant dependence on the amount of Zn present in the shell. Distributions of on and off times go from the usual power-law distributions to power-law distributions with exponential cut-offs. These cut-offs become increasingly pronounced as the proportion of Zn increases. We interpret these results in the framework of diffusion-controlled electron transfer. Exciton relaxation lifetime measurements strongly suggest that lattice mismatch is responsible for a greater number of defects in core/shell cQDs. Therefore, strain and lattice mismatch are shown to be parameters of significant importance for the electronic structure of nanocrystals, influencing the photoluminescence, exciton relaxation lifetime and blinking behaviour

Toward Automatic Label-Free Whispering Gallery Modes Biodetection with a Quantum Dot-Coated Microsphere Population

We explore a new calibration-free approach to biodetection based on whispering gallery modes (WGMs) without a reference measure and relative shifts. Thus, the requirement to keep track of the sensor position is removed, and a freely moving population of fluorophore-doped polystyrene microspheres can now fulfill this role of sensing resonator. Breaking free from fixed surface-based biosensing promotes adhesion between the microsphere sensors and the analytes since both can now be thoroughly mixed. The 70-nm-wide spectrum of green fluorescent microbeads allows us to monitor over 20 WGMs simultaneously without needing evanescent light coupling into the microspheres, hence enabling remote sensing. Since the exact radius of each microsphere is unknown a priori, it requires algorithmic analyses to obtain a reliable result for the refractive index of a solution. We first test our approach with different solutions of alcohol in water obtaining 3 × 10−4 precision on the refractive index at lower concentrations. Then, the solutions of bacterial spores in water yield clear evidence of biodetection in the statistical analysis of WGMs from 50 microspheres. To extend the fluorescence spectral range of our WGM sensors, we present preliminary results on coating microspheres with CdSe/ZnS quantum dots