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  • image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Authors: TEULLE, Alexandre;

    The main objective of this thesis is to interpret experimental measurements of the plasmonic properties of goldcolloidal particles.First, we study the optical near-field distribution around nano-platelets thanks to the photomigration technique. Thisindirect photo-chemical mapping uncovers a size effect by shining at 457 nm and 514 nm particles of different sizes, suggesting a quasi-modal response from the surface plasmons supported by these structures. This peculiar response is evidenced in the case of colloidal triangles of 500 nm side length.Then, we show that Two Photon Luminescence (TPL) offers another original way to probe the electromagnetic fielddistribution inside Au particles. We focus the TPL study on gold nano-rods and platelets. TPL maps show a strong confinement of the electromagnetic field inside these objects. Signal localization can be controlled by adjusting incident polarization.Simultaneously, we have developed a new tool based on the Green Dyadic Method (GDM) to reproduce and analyze TPL maps. They confirm specific near-field localization in the metal and provide a new insight into wavelength and particle shape influence. Our model suggests that TPL gives also access to the local density of plasmonic states in the particle and consequently that the coupling between two gold platelets could lead to a new design of a plasmonic modal logic gate. Finally, we have investigated the optical properties of gold nanoparticle chains. These nanoparticles fuse under theelectron beam of the TEM. The fusion shifts plasmons resonances of the chains towards the infrared region. These plasmonic modes have been studied spatially and spectrally using Electron Energy Loss Spectroscopy (EELS). We have developed a theoretical model showing the link between the energy loss of a swift electron and the local density of states. Using the GDM, we have computed EELS maps of these nanoparticle chains.; Cette thèse a pour objectif principal d’interpréter des mesures expérimentales des propriétés plasmoniques denanoparticules d’or cristallines de différentes morphologies.Nous étudions tout d’abord, grâce à un film photosensible, la distribution du champ local autour de nano-prismes d’or.Cette cartographie indirecte révèle un effet de taille en irradiant à 457 nm et 514nm des objets de formes identiques mais de dimensions différentes, suggérant une réponse quasi-modale des plasmons supportés par ces structures. Cette réponse quasimodale est mise en évidence dans le cas de prismes triangulaires de 500 nm de côté.Dans une seconde étape, nous montrons que la luminescence à deux photons (TPL) offre un autre moyen original desonder la distribution du champ électromagnétique à l’intérieur de ces particules. En particulier, nous considérons le cas des nano-bâtonnets et des prismes d’or. Les cartes TPL montrent un fort confinement du champ à l’intérieur de ces objets. La localisation du signal peut être contrôlée en ajustant la polarisation incidente. Parallèlement, nous avons développé un nouvel outil de simulation pour reproduire et interpréter les cartes TPL. Elles confirment la spatialisation spécifique du champ proche et nous renseignent sur l’influence de la longueur d’onde et de la forme des prismes. Notre modèle suggère que la TPL donne aussi accès à la densité locale d’états plasmoniques dans la particule, et que le couplage entre deux nano-prismes peut constituer une nouvelle façon de concevoir des portes logiques modales plasmoniques.Enfin, nous avons étudié les propriétés optiques de chaines de sphères d’or d’une dizaine de nanomètres de diamètre. Les particules constituant ces chaines fusionnent sous l’effet du faisceau du microscope électronique en transmission ce qui conduit à un décalage dans l’infrarouge des modes de résonance plasmon. Nous avons caractérisé spatialement et spectralement ces modes plasmons par spectroscopie de pertes d’énergie (EELS). Grâce à la polyvalence du formalisme des fonctions de Green, et en nous appuyant sur une modélisation théorique montrant le lien entre signal de perte et densité locale d’états, nous avons simulé des cartes EELS de ces objets.

    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ HAL-INSA Toulousearrow_drop_down
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    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ HAL-INSA Toulousearrow_drop_down
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
  • image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Authors: Sun, Dongyue;

    The production of H2 through sunlight-driven water splitting appears to be a promising solution for our future energy supply. Earth-abundant catalysts should be developed to replace platinum as water splitting catalysts. Bio-inspired cobalt diimine-dioxime complexes have emerged as one of the most versatile series of non-noble metal catalysts. In this work, the mechanism for H2 evolution mediated by this series of catalysts has been reinvestigated, and kinetic information have been determined thanks to recent advancements in electrochemical methodology. Their superior hydrogen evolution performance has been shown through comparative catalytic Tafel plots. Secondly, a synthetic route towards the incorporation of fullerene moieties, as electron reservoirs, in the vicinity of the catalytic center, has been developed. The resulting catalyst has shown improved catalytic activity and has been implemented in an operational H2-evoving photocathode based on organic semi-conductors. La production de H2, à partir d'eau et d'énergie solaire, est probablement une solution d'avenir pour le stockage des énergies renouvelables. Pour éviter l’utilisation de platine, des catalyseurs à base de métaux abondants doivent être développés. Les complexes diimine-dioxime de cobalt sont parmi les catalyseurs bio-inspirés les plus performants. Dans ce travail, nous avons dans un premier temps élucidé le mécanisme de production d’hydrogène par ces complexes et extrait les paramètres cinétiques des différentes étapes en utilisant les méthodes et techniques électrochimiques les plus récentes. Une étude comparative via l’établissement d’une « courbe de Tafel catalytique » a mis en évidence l’excellente performance catalytique de ces complexes. Ensuite, une voie de synthèse permettant le couplage de ces complexes avec un motif fullerène réservoir d’électron a été développée, et a permis d’améliorer encore les performances catalytiques. Enfin, ce complexe a été intégré dans une photocathode à base de semi-conducteurs organiques.

    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Hyper Article en Lig...arrow_drop_down
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    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Hyper Article en Lig...arrow_drop_down
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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  • image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Authors: TEULLE, Alexandre;

    The main objective of this thesis is to interpret experimental measurements of the plasmonic properties of goldcolloidal particles.First, we study the optical near-field distribution around nano-platelets thanks to the photomigration technique. Thisindirect photo-chemical mapping uncovers a size effect by shining at 457 nm and 514 nm particles of different sizes, suggesting a quasi-modal response from the surface plasmons supported by these structures. This peculiar response is evidenced in the case of colloidal triangles of 500 nm side length.Then, we show that Two Photon Luminescence (TPL) offers another original way to probe the electromagnetic fielddistribution inside Au particles. We focus the TPL study on gold nano-rods and platelets. TPL maps show a strong confinement of the electromagnetic field inside these objects. Signal localization can be controlled by adjusting incident polarization.Simultaneously, we have developed a new tool based on the Green Dyadic Method (GDM) to reproduce and analyze TPL maps. They confirm specific near-field localization in the metal and provide a new insight into wavelength and particle shape influence. Our model suggests that TPL gives also access to the local density of plasmonic states in the particle and consequently that the coupling between two gold platelets could lead to a new design of a plasmonic modal logic gate. Finally, we have investigated the optical properties of gold nanoparticle chains. These nanoparticles fuse under theelectron beam of the TEM. The fusion shifts plasmons resonances of the chains towards the infrared region. These plasmonic modes have been studied spatially and spectrally using Electron Energy Loss Spectroscopy (EELS). We have developed a theoretical model showing the link between the energy loss of a swift electron and the local density of states. Using the GDM, we have computed EELS maps of these nanoparticle chains.; Cette thèse a pour objectif principal d’interpréter des mesures expérimentales des propriétés plasmoniques denanoparticules d’or cristallines de différentes morphologies.Nous étudions tout d’abord, grâce à un film photosensible, la distribution du champ local autour de nano-prismes d’or.Cette cartographie indirecte révèle un effet de taille en irradiant à 457 nm et 514nm des objets de formes identiques mais de dimensions différentes, suggérant une réponse quasi-modale des plasmons supportés par ces structures. Cette réponse quasimodale est mise en évidence dans le cas de prismes triangulaires de 500 nm de côté.Dans une seconde étape, nous montrons que la luminescence à deux photons (TPL) offre un autre moyen original desonder la distribution du champ électromagnétique à l’intérieur de ces particules. En particulier, nous considérons le cas des nano-bâtonnets et des prismes d’or. Les cartes TPL montrent un fort confinement du champ à l’intérieur de ces objets. La localisation du signal peut être contrôlée en ajustant la polarisation incidente. Parallèlement, nous avons développé un nouvel outil de simulation pour reproduire et interpréter les cartes TPL. Elles confirment la spatialisation spécifique du champ proche et nous renseignent sur l’influence de la longueur d’onde et de la forme des prismes. Notre modèle suggère que la TPL donne aussi accès à la densité locale d’états plasmoniques dans la particule, et que le couplage entre deux nano-prismes peut constituer une nouvelle façon de concevoir des portes logiques modales plasmoniques.Enfin, nous avons étudié les propriétés optiques de chaines de sphères d’or d’une dizaine de nanomètres de diamètre. Les particules constituant ces chaines fusionnent sous l’effet du faisceau du microscope électronique en transmission ce qui conduit à un décalage dans l’infrarouge des modes de résonance plasmon. Nous avons caractérisé spatialement et spectralement ces modes plasmons par spectroscopie de pertes d’énergie (EELS). Grâce à la polyvalence du formalisme des fonctions de Green, et en nous appuyant sur une modélisation théorique montrant le lien entre signal de perte et densité locale d’états, nous avons simulé des cartes EELS de ces objets.

    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ HAL-INSA Toulousearrow_drop_down
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ HAL-INSA Toulousearrow_drop_down
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
  • image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    Authors: Sun, Dongyue;

    The production of H2 through sunlight-driven water splitting appears to be a promising solution for our future energy supply. Earth-abundant catalysts should be developed to replace platinum as water splitting catalysts. Bio-inspired cobalt diimine-dioxime complexes have emerged as one of the most versatile series of non-noble metal catalysts. In this work, the mechanism for H2 evolution mediated by this series of catalysts has been reinvestigated, and kinetic information have been determined thanks to recent advancements in electrochemical methodology. Their superior hydrogen evolution performance has been shown through comparative catalytic Tafel plots. Secondly, a synthetic route towards the incorporation of fullerene moieties, as electron reservoirs, in the vicinity of the catalytic center, has been developed. The resulting catalyst has shown improved catalytic activity and has been implemented in an operational H2-evoving photocathode based on organic semi-conductors. La production de H2, à partir d'eau et d'énergie solaire, est probablement une solution d'avenir pour le stockage des énergies renouvelables. Pour éviter l’utilisation de platine, des catalyseurs à base de métaux abondants doivent être développés. Les complexes diimine-dioxime de cobalt sont parmi les catalyseurs bio-inspirés les plus performants. Dans ce travail, nous avons dans un premier temps élucidé le mécanisme de production d’hydrogène par ces complexes et extrait les paramètres cinétiques des différentes étapes en utilisant les méthodes et techniques électrochimiques les plus récentes. Une étude comparative via l’établissement d’une « courbe de Tafel catalytique » a mis en évidence l’excellente performance catalytique de ces complexes. Ensuite, une voie de synthèse permettant le couplage de ces complexes avec un motif fullerène réservoir d’électron a été développée, et a permis d’améliorer encore les performances catalytiques. Enfin, ce complexe a été intégré dans une photocathode à base de semi-conducteurs organiques.

    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Hyper Article en Lig...arrow_drop_down
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
    image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/
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      image/svg+xml art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos Open Access logo, converted into svg, designed by PLoS. This version with transparent background. http://commons.wikimedia.org/wiki/File:Open_Access_logo_PLoS_white.svg art designer at PLoS, modified by Wikipedia users Nina, Beao, JakobVoss, and AnonMoos http://www.plos.org/ Hyper Article en Lig...arrow_drop_down
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