Mono- and Biexponential Luminescence Decays of Individual Single-Walled Carbon Nanotubes

We have studied the exciton recombination dynamics of individual (6,4) and (6,5) single-walled carbon nanotubes embedded in aqueous gels or deposited on glass surfaces. CoMoCat nanotubes systematically display short monoexponential photoluminescence (PL) decays presumably due to defects introduced during their synthesis. In contrast HiPco nanotubes can either display mono- or biexponential PL decays depending on the environmental conditions. Transition from bi- to monoexponential decays can be reproduced by a simple three level model taking into account defect-dependent nonradiative decay mechanisms

Quantum yield optimized fluorophores for site-specific labeling and super-resolution imaging

Single molecule applications, saturated pattern excitation microscopy, or stimulated emission depletion (STED) microscopy demand for bright and highly stable fluorescent dyes1,2. Despite of intensive research the choice of fluorphores is still very limited. Typically a stable fluorescent dyes is covalently attached to the target. This methodology brings forward a number of limitations, in particular, in case of protein labeling. First of all the fluorescent probes need to be attached selectively and site-specifically to prevent unspecific background. This often requires single cysteine mutations for covalent protein modification. Employing quantum dots allows overcoming problems of photo-bleaching3-6. However, the downsides are their large size, rendering the probe inaccessible to spatially confined architectures, issues in biocompatibility due to proper particle coating, and cellular toxicity6-8. Here we propose a new method to overcome the above outlined problems

Luminescence Decay and the Absorption Cross-Section of Individual Single-Walled Carbon Nanotubes

The absorption cross section of highly luminescent individual single-walled carbon nanotubes is determined using time-resolved and cw luminescence spectroscopy. A mean value of 1x10-17 cm2 per carbon atom is obtained for (6,5) tubes excited at their second optical transition, and corroborated by single tube photothermal absorption measurements. Biexponential luminescence decays are systematically observed, with short and long lifetimes around 45 and 250 ps. This behavior is attributed to the band edge exciton fine structure with a dark level lying a few meV below a bright one

Multiple Routes for Glutamate Receptor Trafficking: Surface Diffusion and Membrane Traffic Cooperate to Bring Receptors to Synapses

Trafficking of glutamate receptors into and out of synapses is critically involved in the plasticity of excitatory synaptic transmission. Endocytosis and exocytosis of receptors have initially been thought to account alone for this trafficking. However, membrane proteins also traffic through surface lateral diffusion in the plasma membrane. We describe developments in electrophysiological and optical approaches that have allowed for the real time measurement of glutamate receptor surface trafficking in live neurons. These include (i) specific imaging of surface receptors using a pH sensitive fluorescent protein, (ii) design of a photoactivable drug to inactivate locally surface receptors and monitor electrophysiologically their recovery, and (iii)application of single molecule fluorescence microscopy to directly track the movement of individual surface receptors with nanometer resolution inside and outside synapses. Altogether, these approaches have demonstrated that glutamate receptors diffuse at high rates in the neuronal membrane and suggest a key role for surface diffusion in the regulation of receptor numbers at synapses

Observation of intrinsic size effects in the optical response of individual gold nanoparticles

The Photothermal Heterodyne Imaging method is used to study for the first time the absorption spectra of individual gold nanoparticles with diameters down to 5 nm. Intrinsic size effects wich result in a broadening of the Surface Plasmon resonance are unambiguously observed. Dispersions in the peak energies and homogeneous widths of the single particle resonances are revealed. The experimental results are analysed within the frame of Mie theory

Absorption spectroscopy of individual single-walled carbon nanotubes

Current methods for producing single-walled carbon nanotubes (SWNTs) lead to heterogeneous samples containing mixtures of metallic and semiconducting species with a variety of lengths and defects. Optical detection at the single nanotube level should thus offer the possibility to examine these heterogeneities provided that both SWNT species are equally well detected. Here, we used photothermal heterodyne detection to record absorption images and spectra of individual SWNTs. Because this photothermal method relies only on light absorption, it readily detects metallic nanotubes as well as the emissive semiconducting species. The first and second optical transitions in individual semicontucting nanotubes have been probed. Comparison between the emission and absorption spectra of the lowest-lying optical transition reveal mainly small Stokes shifts. Side bands in the near-infrared absorption spectra are observed and assigned to exciton-phonon bound states. No such sidebands are detected around the lowest transition of metallic nanotubes

Revealing the Exciton Fine Structure in Lead Halide Perovskite Nanocrystals

Lead-halide perovskite nanocrystals (NCs) are attractive nano-building blocks for photovoltaics and optoelectronic devices as well as quantum light sources. Such developments require a better knowledge of the fundamental electronic and optical properties of the band-edge exciton, whose fine structure has long been debated. In this review, we give an overview of recent magneto-optical spectroscopic studies revealing the entire excitonic fine structure and relaxation mechanisms in these materials, using a single-NC approach to get rid of their inhomogeneities in morphology and crystal structure. We highlight the prominent role of the electron-hole exchange interaction in the order and splitting of the bright triplet and dark singlet exciton sublevels and discuss the effects of size, shape anisotropy and dielectric screening on the fine structure. The spectral and temporal manifestations of thermal mixing between bright and dark excitons allows extracting the specific nature and strength of the exciton–phonon coupling, which provides an explanation for their remarkably bright photoluminescence at low temperature although the ground exciton state is optically inactive. We also decipher the spectroscopic characteristics of other charge complexes whose recombination contributes to photoluminescence. With the rich knowledge gained from these experiments, we provide some perspectives on perovskite NCs as quantum light sources

Photothermal heterodyne imaging of individual nonfluorescent nanoclusters and nanocrystals

We introduce a new, highly sensitive, and simple heterodyne optical method for imaging individual nonfluorescent nanoclusters and nanocrystals. A 2 order of magnitude improvement of the signal is achieved compared to previous methods. This allows for the unprecedented detection of individual small absorptive objects such as metallic clusters (of 67 atoms) or nonluminescent semiconductor nanocrystals. The measured signals are in agreement with a calculation based on the scattering field theory from a photothermal-induced modulated index of refraction profile around the nanoparticle