Localization of plasmon modes in a 2D photonic nanostructure with a controlled disorder.

In this paper, we focus on the optical properties of disordered hole arrays etched in a gold thin film. The disorder is induced and controlled using hole displacements following a Gaussian distribution and starting from a periodic array. The nanostructures present a transition from ordered arrays to short-range ordered arrays and random arrays by increasing the disorder amount. The associated optical properties are characterized in far and near fields by complementary approaches (absorption spectroscopy, classical scanning near field optical microscopy (SNOM) and Finite Difference Time Domain (FDTD) simulations). By increasing the disorder, a broadened absorption up to 30% in the far-field is achieved. Experiments in agreement with FDTD simulations point out the energy localization induced by the disorder and the dependence on the amount of disorder and on the excitation wavelength. By using a controlled disorder, we also show that the effect of these two parameters is also closely linked.

Measuring the orientation of a single CdSe/CdS nanocrystal at the end of a near-field tip for the realization of a versatile active SNOM probe.

The orientation of a CdSe/CdS nanocrystal attached at the end of a scanning near field optical microscope (SNOM) tip is analyzed by its coupling with a flat gold layer. The Purcell factors for a set of distances to the gold surface are measured after a NC is caught by a SNOM tip. These measurements are compared with the modeling of the emission of a 2D dipole on a gold layer taking into account the layer of polymer serving as a glue for the NC. The 2D dipole is perpendicular to the c-axis of the NC, which is the growth axis. The behavior of the Purcell factor as a function of the distance to the gold layer depends on the angle made by this axis and the surface. The adjustment of the experimental results and the modelization gives the orientation of the NC at the end of the SNOM tip. Different orientations of the c-axis are determined.

Unraveling the time cross correlations of an emitter switching between two states with the same fluorescence intensity.

The autocorrelation function of the fluorescence intensity of a nanoemitter is measured with the standard Hanbury-Brown and Twiss setup. Time-tagging of the photodetection events during all the experiment has opened new possibilities in terms of post-selection techniques that enable to go beyond the blinking and antibunching characterization. Here, we first present a new method developed to investigate in detail the antibunching of a fluorophore switching between two emitting states. Even if they exhibit the same fluorescence intensity, their respective amount of antibunching can be measured using the gap between their respective decay rates. The method is then applied to a nanoemitter consisting in a colloidal quantum dot coupled to a plasmonic resonator. The relative quantum efficiency of the charged and neutral biexcitons are determined.

Thermal activation of non-radiative Auger recombination in charged colloidal nanocrystals.

Applications of semiconductor nanocrystals such as biomarkers and light-emitting optoelectronic devices require that their fluorescence quantum yield be close to 100%. However, such quantum yields have not been obtained yet, in part, because non-radiative Auger recombination in charged nanocrystals could not be suppressed completely. Here, we synthesize colloidal core/thick-shell CdSe/CdS nanocrystals with 100% quantum yield and completely quenched Auger processes at low temperatures, although the nanocrystals are negatively photocharged. Single particle and ensemble spectroscopy in the temperature range 30-300 K shows that the non-radiative Auger recombination is thermally activated around 200 K. Experimental results are well described by a model suggesting a temperature-dependent delocalization of one of the trion electrons from the CdSe core and enhanced Auger recombination at the abrupt CdS outer surface. These results point to a route for the design of core/shell structures with 100% quantum yield at room temperature.

Bright and grey states in CdSe-CdS nanocrystals exhibiting strongly reduced blinking.

When compared to standard colloidal nanocrystals, individual CdSe-CdS core-shell nanocrystals with thick shells exhibit strongly reduced blinking. Analyzing the photon statistics and lifetime of the on state, we first demonstrate that bright periods correspond to single photon emission with a fluorescence quantum efficiency of the monoexcitonic state greater than 95%. We also show that low intensity emitting periods are not dark but correspond to a grey state, with a fluorescence quantum efficiency of 19%. From these measurements, we deduce the radiative lifetime (45 ns) and the Auger lifetime (10.5 ns) of the grey state.