Photon correlations in the collective emission of hybrid gold-(CdSe/CdS/CdZnS) nanocrystal supraparticles.

We investigate the photon statistics of the light emitted by single self-assembled hybrid gold-CdSe/CdS/CdZnS colloidal nanocrystal supraparticles through the detailed analysis of the intensity autocorrelation function(). We first reveal that, despite the large number of nanocrystals involved in the supraparticle emission, antibunching can be observed. We then present a model based on non-coherent Förster energy transfer and Auger recombination that well captures photon antibunching.

High-directivity far-field radiation of quantum dot-based single-photon emitter coupled to polymeric circular waveguide resonant grating.

Solid-state single-photon emitters (SPEs) commonly encounter the limitation of quasi-omnidirectional radiation patterns, which poses challenges in utilizing their emission with conventional optical instruments. In this study, we demonstrate the tailoring of the far-field radiation patterns of SPEs based on colloidal quantum dots (QDs), both theoretically and experimentally, by employing a polymer-based dielectric antenna. We introduce a simple and cost-effective technique, namely low one-photon absorption direct laser writing, to achieve precise coupling of a QD into an all-polymer circular waveguide resonance grating.

On-Chip 3D Printing of Polymer Waveguide-Coupled Single-Photon Emitter Based on Colloidal Quantum Dots.

In the field of quantum technology, there has been a growing interest in fully integrated systems that employ single photons due to their potential for high performance and scalability. Here, a simple method is demonstrated for creating on-chip 3D printed polymer waveguide-coupled single-photon emitters based on colloidal quantum dots (QDs). By using a simple low-one photon absorption technique, we were able to create a 3D polymeric crossed-arc waveguide structure with a bright QD on top.

Fluorescence decay enhancement and FRET inhibition in self-assembled hybrid gold CdSe/CdS/CdZnS colloidal nanocrystal supraparticles.

We report on the synthesis of hybrid light emitting particles with a diameter ranging between 100 and 500 nm, consisting in a compact semiconductor CdSe/CdS/CdZnS nanocrystal aggregate encapsulated by a controlled nanometric size silica and gold layers. We first characterize the Purcell decay rate enhancement corresponding to the addition of the gold nanoshell as a function of the particle size and find a good agreement with the predictions of numerical simulations. Then, we show that the contribution corresponding to Förster resonance energy transfer is inhibited.

Correction: Gold plasmonic enhanced luminescence of silica encapsulated semiconductor hetero-nanoplatelets.

[This corrects the article DOI: 10.1039/D1NA00273B.].

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.

Position-controlled quantum emitters with reproducible emission wavelength in hexagonal boron nitride.

Single photon emitters (SPEs) in low-dimensional layered materials have recently gained a large interest owing to the auspicious perspectives of integration and extreme miniaturization offered by this class of materials. However, accurate control of both the spatial location and the emission wavelength of the quantum emitters is essentially lacking to date, thus hindering further technological steps towards scalable quantum photonic devices. Here, we evidence SPEs in high purity synthetic hexagonal boron nitride (hBN) that can be activated by an electron beam at chosen locations.

Gold plasmonic enhanced luminescence of silica encapsulated semiconductor hetero-nanoplatelets.

Optical properties of nanocrystals have the potential to drive the next generation of optoelectronic devices. However, a number of technological limitations remain to be overcome. Nanocrystals' emission is strongly impacted by the chemical environment and high excitation power.

Controllable movement of single-photon source in multifunctional magneto-photonic structures.

Quantum dot (QD) coupling in nanophotonics has been widely studied for various potential applications in quantum technologies. Micro-machining has also attracted substantial research interest due to its capacity to use miniature robotic tools to make precise controlled movements. In this work, we combine fluorescent QDs and magnetic nanoparticles (NPs) to realize multifunctional microrobotic structures and demonstrate the manipulation of a coupled single-photon source (SPS) in 3D space via an external magnetic field.

Photostability and long-term preservation of a colloidal semiconductor-based single photon emitter in polymeric photonic structures.

Colloidal semiconductor quantum dots (QDs) are promising candidates for various applications in electronics and quantum optics. However, they are sensitive and vulnerable to the chemical environment due to their highly dynamic surface with a large portion of exposed atoms. Hence, oxidation and detrimental defects on the nanocrystal (NC) interface dramatically deteriorate their optical as well as electrical properties.

CdSe/CdS Dot-in-Rods Nanocrystals Fast Blinking Dynamics.

Analyzing the autocorrelation function of the fluorescence intensity, we demonstrate that these nanoemitters are characterized by a short value of the mean duration of bright periods (ten to a few hundreds of microseconds). The comparison of the results obtained for samples with different geometries shows that not only the shell thickness is crucial but also the shape of the dot-in-rods. Increasing the shell aspect ratio results in shorter bright periods suggesting that surface traps impact the stability of the fluorescence intensity.

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.

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.

Spatially uniform enhancement of single quantum dot emission using plasmonic grating decoupler.

We demonstrate a spatially uniform enhancement of individual quantum dot (QD) fluorescence emission using plasmonic grating decouplers on thin gold or silver films. Individual QDs are deposited within the grating in a controlled way to investigate the position dependency on both the radiation pattern and emission enhancement. We also describe the optimization of the grating decoupler.

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.

FDTD simulations of localization and enhancements on fractal plasmonics nanostructures.

A parallelized 3D FDTD (Finite-Difference Time-Domain) solver has been used to study the near-field electromagnetic intensity upon plasmonics nanostructures. The studied structures are obtained from AFM (Atomic Force Microscopy) topography measured on real disordered gold layers deposited by thermal evaporation under ultra-high vacuum. The simulation results obtained with these 3D metallic nanostructures are in good agreement with previous experimental results: the localization of the electromagnetic intensity in subwavelength areas ("hot spots") is demonstrated; the spectral and polarization dependences of the position of these "hot spots" are also satisfactory; the enhancement factors obtained are realistic compared to the experimental ones.

Controlled modification of single colloidal CdSe/ZnS nanocrystal fluorescence through interactions with a gold surface.

Single colloidal CdSe/ZnS nanocrystals are deposited at various distances from a gold film in order to improve their performance as single photon sources. Photon antibunching is demonstrated and the experimental curves are accurately fitted by theoretical equations. Emission lifetime and intensity are measured and found in excellent agreement with theoretical values.

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%.

Non-blinking semiconductor colloidal quantum dots for biology, optoelectronics and quantum optics.

Twinkle, twinkle: The blinking of semiconductor colloidal nanocrystals is the main inconvenience of these bright nanoemitters. There are various approaches for obtaining non-blinking nanocrystals, one of which is to grow a thick coat of CdS on the CdSe core (see picture). Applications of this method in the fields of optoelectronic devices, biologic labelling and quantum information processing are discussed.

Towards non-blinking colloidal quantum dots.

At a single-molecule level, fluorophore emission intensity fluctuates between bright and dark states. These fluctuations, known as blinking, limit the use of fluorophores in single-molecule experiments. The dark-state duration shows a universal heavy-tailed power-law distribution characterized by the occurrence of long non-emissive periods.

Emission characterization of a single CdSe-ZnS nanocrystal with high temporal and spectral resolution by photon-correlation Fourier spectroscopy.

We report a spectroscopic study of single colloidal CdSe/ZnS nanocrystals at low temperature. We use photon-correlation Fourier spectroscopy, a technique based on measuring the correlations of the intensities detected at the outputs of a Michelson interferometer. Spectral diffusion over a few microeV is evidenced, on a typical time scale of 200 micros.

Spatial distribution of the intensity noise of a vertical-cavity surface-emitting semiconductor laser.

We studied anticorrelated quantum fluctuations between the TEM(00) and the TEM(01) transverse modes of a vertical-cavity surface-emitting semiconductor laser by measuring the transverse spatial distribution of the laser beam intensity noise. Our experimental results are found to be in good agreement with the predictions of a phenomenological model that accounts for quantum correlations between transverse modes in a light beam.

Bunching and antibunching in the fluorescence of semiconductor nanocrystals.

The fluorescence of single-colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. Over a short time scale, the autocorrelation function shows complete antibunching, indicating single-photon emission and atomiclike behavior. Over longer time scales (up to tens of seconds), we measure a bunching effect that is due to fluorescence intermittency and that cannot be described by fluctuations between two states with constant rates.

Photon-correlation Fourier spectroscopy.

We describe a method to probe the spectral fluctuations of a transition over broad ranges of frequencies and timescales with the high spectral resolution of Fourier spectroscopy, and a temporal resolution as high as the excited state lifetime, even in the limit of very low photocounting rates. The method derives from a simple relation between the fluorescence spectral dynamics of a single radi-ating dipole and its fluorescence intensity correlations at the outputs of a continuously scanning Michelson interferometer. These findings define an approach to investigate the fast fluorescence spectral dynamics of single molecules and other faint light sources beyond the time-resolution capabilities of standard spectroscopy experiments.