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Personne :
Boudreau, Denis

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Boudreau

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Denis

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Université Laval. Département de chimie

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ncf10368871

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Résultats de recherche

Voici les éléments 1 - 7 sur 7
  • PublicationAccès libre
    A metal-enhanced Hg2+-responsive fluorescent nanoprobe: from morphological design to application to natural waters
    (American Chemical Society, 2022-06-22) Picard-Lafond, Audrey; Boudreau, Denis; Larivière, Dominic
    Metal-enhanced fluorescence (MEF) is a powerful tool in the design of sensitive chemical sensors by improving brightness and photostability to target-responsive fluorophores. Compounding these advantages with the modest hardware requirements of fluorescent sensing compared to that of centralized elemental analysis instruments, expanding the use of MEF to the detection of low-level inorganic pollutants is a compelling aspiration. Among the latter, monitoring mercury in the environment, where some of its species disseminate through the food chain and, in time, to humans, has elicited a broad research effort towards the development of Hg2+-responsive fluorescent sensors. Herein, a Hg2+-sensitive MEF-enabled probe was conceived by grafting a Hg2+-responsive fluorescein derivative to concentric Ag@SiO2 NPs, where the metallic core enhances fluorescent emission of molecular probes embedded in a surrounding silica shell. Time-resolved fluorescence measurements showed that the fluorophore’s excited state lifetime decreases from 3.9 ns in a solid, coreless silica sphere, to 0.4 ns in the core-shell nanoprobe, granting the dye a better resistance to photobleaching. The Ag-core system showed a sizable improvement in limit of detection at 2 nM (0.4 ppb) compared to 50 nM (10 ppb) in the silica-only colloids and its effectiveness for natural water analysis was demonstrated. Overall, the reported nanoarchitecture hints at the potential of MEF for heavy metal detection by fluorescence detection.
  • PublicationAccès libre
    Enhancing galvanic replacement in plasmonic hollow nanoparticles : understanding the role of the speciation of metal ion precursors
    (Wiley, 2020-04-22) Boudreau, Denis; Richard-Daniel, Josée
    Hollow nanostructures offer great potential for plasmonic applications due to their strong and highly tunable localized surface plasmon resonance. The relationship between the plasmonic properties and geometry of hollow nanoparticles, such as core-shell size ratio, concentricity of the cavity and porosity of the wall, is well documented. Nanoscale galvanic replacement provides a simple, versatile and powerful route for the preparation of such hollow structures. Here we demonstrate how the efficiency of reductant-assisted galvanic replacement processes can be enhanced by controlling the degree of hydration and hydrolysis of the metal ion precursor using pH and pL as key control parameters (by analogy to pH, the letter p in the expression pL is used to indicate the decimal cologarithm associated with the concentration of the ligand L). Adjusting precursor speciation prior to the sacrificial template’s hollowing process offers a new strategy to tune the morphology and optical properties of plasmonic hollow nanostructures.
  • PublicationAccès libre
    Acting as a molecular tailor : dye structural modifications for improved sensitivity towards lysophosphatidic acids sensing
    (American Chemiscal Society, 2022-12-28) Fontaine, Nicolas; Harter, Lara; Marette, André; Boudreau, Denis
    Lysophosphatidic acids (LPA) are key biomarkers for several physiological processes, the monitoring of which can provide insights into the host’s health. Common lab-based techniques for their detection are cumbersome, expensive and necessitate specialized personnel to operate. LPA-sensitive fluorescent probes have been described, albeit for non-aqueous conditions, which impedes their use in biological matrices. In this paper, we explore in detail the influence of structure on the extent of aggregation-induced fluorescence quenching using specially synthesized styrylpyridinium dyes bearing structural adaptations to bestow them enhanced affinity towards LPA in aqueous media. Spectroscopic investigations supported by time-resolved fluorimetry revealed the contribution of excimer formation to the fluorescence quenching mechanism displayed by the fluorescent probes. Experimental observations of the influence of structure on detection sensitivity were supported by DFT calculations.
  • PublicationAccès libre
    Pushing the limits of surface-enhanced raman spectroscopy (SERS) with deep learning : identification of multiple species with closely related molecular structures
    (Society for Applied Spectroscopy, 2022-01-26) Boudreau, Denis; Fillion, Daniel; Fontaine, Nicolas; Fortin, Hubert; Lebrun, Alexis; Barbier, Olivier
    Raman spectroscopy is a non-destructive and label-free molecular identification technique capable of producing highly specific spectra with various bands correlated to molecular structure. Moreover, the enhanced detection sensitivity offered by Surface-Enhanced Raman spectroscopy (SERS) allows analyzing mixtures of related chemical species in a relatively short measurement time. Combining SERS with deep learning algorithms allows in some cases to increase detection and classification capabilities even further. The present study evaluates the potential of applying deep learning algorithms to SERS spectroscopy to differentiate and classify different species of bile acids, a large family of molecules with low Raman cross sections and molecular structures that often differ by a single hydroxyl group. Moreover, the study of these molecules is of interest for the medical community since they have distinct pathological roles and are currently viewed as potential markers of gut microbiome imbalances. A Convolutional Neural Network (CNN) model was developed and used to classify SERS spectra from five bile acid species. The model succeeded in identifying the five analytes despite very similar molecular structures and was found to be reliable even at low analyte concentrations.
  • PublicationAccès libre
    A glycan-based plasmonic sensor for prostate cancer diagnosis
    (Royal Society of Chemistry, 2021-10-01) Lamarre, Mathieu; Bansept, Marc-Antoine; Boudreau, Denis; Tremblay, Thomas; Fradet, Vincent; Giguère, Denis; Robitaille, Karine
    Prostate cancer affects thousands of men who undergo clinical screening tests every year. The main biomarker used for the diagnosis of prostate cancer, prostate specific antigen (PSA), presents limitations that justify investigating new biomarkers to improve reliability. Antibodies against the tumor-associated carbohydrate antigen (Tn), or TACA, develop early in carcinogenesis, making them an interesting alternative as a target for prostate cancer diagnostics. In this work, the Tn antigen was synthesized and immobilized on a surface plasmon resonance sensor coated with a polydopamine/polyethylene oxide mixed layer used both as an anchoring surface for Tn capture moieties and to minimize surface fouling. The sensor could be regenerated and reused at least 60 times without any significant loss in sensitivity. Anti-Tn antibodies were detected in the 0-10 nM concentration range with detection limits of 0.1 and 0.3 nM in spiked buffer solutions and diluted human blood serum samples, respectively. Finally, as a proof-of-concept, this carbohydrate-based sensor was used to successfully discriminate blood serum samples from prostate cancer-free and prostate cancer patients.
  • PublicationAccès libre
    Nucleation points : the forgotten parameter in the synthesis of hydrogel-coated gold nanoparticles
    (Basel, 2021-01-26) Sepulveda, Adolfo; Picard-Lafond, Audrey; Boudreau, Denis; Marette, André
    The implementation of gold-hydrogel core-shell nanomaterials in novel light-driven technologies requires the development of well-controlled and scalable synthesis protocols with precisely tunable properties. Herein, new insights are presented concerning the importance of using the concentration of gold cores as a control parameter in the seeded precipitation polymerization process to modulate—regardless of core size—relevant fabrication parameters such as encapsulation yield, particle size and shrinkage capacity. Controlling the number of nucleation points results in the facile tuning of the encapsulation process, with yields reaching 99% of gold cores even when using different core sizes at a given particle concentration. This demonstration is extended to the encapsulation of bimodal gold core mixtures with equally precise control on the encapsulation yield, suggesting that this principle could be extended to encapsulating cores composed of other materials. These findings could have a significant impact on the development of stimuli-responsive smart materials.
  • PublicationAccès libre
    Thinking outside the shell : novel sensors designed from plasmon-enhanced fluorescent concentric nanoparticles
    (Cambridge Royal Society of Chemistry, 2020-08-20) Asselin, Jérémie; Picard-Lafond, Audrey; Boudreau, Denis; Fontaine, Nicolas
    The alteration of photophysical properties of fluorophores in the vicinity of a metallic nanostructure, a phenomenon termed plasmon- or metal-enhanced fluorescence (MEF), has been investigated extensively and used in a variety of proof-of-concept demonstrations over the years. A particularly active area of development in this regard has been the design of nanostructures where fluorophore and metallic core are held in a stable geometry that imparts improved luminosity and photostability to a plethora of organic fluorophores. This minireview presents an overview of MEF-based concentric core–shell sensors developed in the past few years. These architectures expand the range of applications of nanoparticles (NPs) beyond the uses possible with fluorescent molecules. Design aspects that are being described include the influence of the nanocomposite structure on MEF, notably the dependence of fluorescence intensity and lifetime on the distance to the plasmonic core. The chemical composition of nanocomposites as a design feature is also discussed, taking as an example the use of non-noble plasmonic metals such as indium as core materials to enhance multiple fluorophores throughout the UV-Vis range and tune the sensitivity of halide-sensing fluorophores operating on the principle of collisional quenching. Finally, the paper describes how various solid substrates can be functionalized with MEF-based nanosensors to bestow them with intense and photostable pH-sensitive properties for use in fields such as medical therapy and diagnostics, dentistry, biochemistry and microfluidics.