arXiv subjects

Pedro M. R. Paulo

Publications and source records attributed to Pedro M. R. Paulo.

2 recordsLinked to original sources

arXiv2026

Photoluminescence Dynamics of CdSe QD/polymer Langmuir-Blodgett Thin Films: Morphology Effects

Thin films of colloidal semiconductor CdSe quantum-dots (QDs) and a styrene/maleic anhydride copolymer were prepared by the Langmuir-Blodgett technique and their photoluminescence was characterized by confocal fluorescence lifetime microscopy. In the films, the photoluminescence dynamics are strongly affected by excitation energy migration between close-packed quantum-dots and energy trapping by surface-defective QDs or small clusters of aggregated QDs. Polymer/QD films with more aggregated QD regions exhibit lower PL intensities and faster decays, which we attribute primarily to the increased ability of excitations to find trap sites among more close-packed QD regions. This was confirmed by comparing films from bilayer or co-spreading deposition, and varying the QD-to-polymer composition or the surface pressure at deposition. The more regular films, such as those obtained by bilayer deposition at high-pressure, display more surface emission intensity and decays with less accentuated curvature. Decay analysis was performed with a model that accounts for excitation energy migration and trapping in the films. In the framework of the model, the photoluminescence dynamics are related to film morphology through the density of energy traps. A lower amount of QD clustering in the films reflects on a lower density of energy traps and, thus, on more emissive QD films, as inferred here for bilayer films relatively to co-spreading films.

cond-mat.mtrl-sci↗

arXiv2012

Optical detection of single non-absorbing molecules using the surface plasmon of a gold nanorod

Current optical detection schemes for single molecules require light absorption, either to produce fluorescence or direct absorption signals. This severely limits the range of molecules that can be detected, because most molecules are purely refractive. Metal nanoparticles or dielectric resonators detect non-absorbing molecules by a resonance shift in response to a local perturbation of the refractive index, but neither has reached single-protein sensitivity. The most sensitive plasmon sensors to date detect single molecules only when the plasmon shift is amplified by a highly polarizable label or by a localized precipitation reaction on the particle's surface. Without amplification, the sensitivity only allows for the statistical detection of single molecules. Here we demonstrate plasmonic detection of single molecules in realtime, without the need for labeling or amplification. We monitor the plasmon resonance of a single gold nanorod with a sensitive photothermal assay and achieve a ~ 700-fold increase in sensitivity compared to state-of-the-art plasmon sensors. We find that the sensitivity of the sensor is intrinsically limited due to spectral diffusion of the SPR. We believe this is the first optical technique that detects single molecules purely by their refractive index, without any need for photon absorption by the molecule. The small size, bio-compatibility and straightforward surface chemistry of gold nanorods may open the way to the selective and local detection of purely refractive proteins in live cells.

physics.chem-ph↗