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Spectroscopie des processus photoélectriques dans les structures et dispositifs III-N / Spectroscopy of photoelectric processes in III-N structures and devicesPiccardo, Marco 23 September 2016 (has links)
Malgré les rapides progrès technologiques dans les nitrures, les propriétés intrinsèques des alliages de nitrures et les processus physiques qui gouvernent la physique de ces dispositifs sont encore mal connus. Au cours de mon travail de thèse, de nouvelles approches expérimentales et théoriques ont été développées pour aborder l’étude des mécanismes microscopiques qui gouvernent les propriétés électroniques des dispositifs à base de nitrures semi-conducteurs. Une nouvelle technique expérimentale permettant de mesurer directement la distribution en énergie des électrons de conduction d’une LED en fonctionnement est explorée. Cette approche permet l’observation directe de populations d’électrons chauds excités dans le dispositif optoélectronique sous injection électrique et émis dans l’ultravide. Une théorie récente de la localisation dans les systèmes désordonnés est appliquée aux matériaux et dispositifs optoélectroniques à base de nitrures. Cette méthode permet pour la première fois la détermination du paysage de localisation induit par le désordre d’alliage sans résoudre l’équation de Schrödinger. Expérimentalement, une signature claire du désordre d’alliage est observée par des mesures de spectroscopie de photocourant dans des puits quantiques d’InGaN sous forme d’une queue d’Urbach pour des excitations d’énergie inférieure à la largeur de la bande interdite. Ceci permet de définir une énergie caractéristique du désordre qui est en excellent accord avec les prédictions fournies par la nouvelle théorie de la localisation. / In spite of the rapid technological progress in nitrides, the intrinsic properties of nitride alloys and the physics of III-N devices are still not well understood. In the course of my thesis work, novel experimental and theoretical approaches to tackle the study of the microscopic mechanisms governing the electronic properties of nitride semiconductors have been developed. A new experimental technique allowing to directly measure the energy distribution of conduction electrons of an operating LED is explored. This approach allows the direct observation of hot electron populations excited in the optoelectronic device under electrical operation and emitted in ultra-high vacuum. A recent theory of localization in disordered systems is applied to nitride materials and optoelectronic devices. This method allows for the first time the determination of the localization landscape induced by alloy disorder without resorting to the Schrödinger equation. Experimentally, a clear signature of alloy disorder is observed by biased photocurrent spectroscopy of InGaN quantum wells in the form of an Urbach tail for below-gap excitation and is found to be in excellent agreement with the predictions given by the novel localization theory.
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Optoperforation of Intact Plant Cells, Spectral Characterization of Alloy Disorder in InAsP Alloy Disorder in InAsP Alloys, and Bimetallic Concentric Surfaces for Metal-Enhanced Fluorescence in Upconverting NanocrystalsMerritt, Travis Robert 24 January 2014 (has links)
The techniques of optoperforation, spectral characterization of alloy disorder, and metal-enhanced fluorescence were applied to previously unconsidered or disregarded systems in order to demonstrate that such applications are both feasible and consequential. These applications were the subject of three disparate works and, as such, are independently discussed.
Despite being ostensibly restricted to mammalian cells, optoperforation was demonstrated in intact plant cells by means of successful femtosecond-laser-mediated infiltration of a membrane impermeable dextran-conjugated dye into cells of vital Arabidopsis seedling stems. By monitoring the rate of dye uptake, and the reaction of both CFP-expressing vacuoles and nanocellulose substrates, the intensity and exposure time of the perforating laser were adjusted to values that both preserved cell vitality and permitted the laser-assisted uptake of the fluorophore. By using these calibrated laser parameters, dye was injected and later observed in targeted cells after 72 hours, all without deleteriously affecting the vital functions of those cells.
In the context of alloy disorder, photoluminescence of excitonic transitions in two InAsxP1-x alloys were studied through temperature and magnetic field strength dependencies, as well as compositionally-dependent time-resolved behavior. The spectral shape, behavior of the linewidths at high magnetic fields, and the divergence of the peak positions from band gap behavior at low temperatures indicated that alloy disorder exists in the x=0.40 composition while showing no considerable presence in the x=0.13 composition. The time-resolved photoluminescence spectrum for both compositions feature a fast and slow decay, with the slow decay lifetime in x=0.40 being longer than that of x=0.13, which may be due to carrier migration between localized exciton states in x=0.40.
In order to achieve broadband metal-enhanced fluorescence in upconverting NaYF4:Yb,Er nanocrystals, two nanocomposite architectures were proposed that retrofit metallic nanoshells to these lanthanide-doped nanocrystals. The typical monometallic construction was rejected in favor of architectures featuring Au-Ag bimetallic concentric surfaces, a decision supported by the considerable overlap of the calculated plasmon modes of the metallic structures with the emission and absorption spectrum of the nanocrystals. Furthermore, precursors of these nanocomposites were synthesized and photoluminescence measurements were carried out, ultimately verifying that these precursors produce the requisite upconversion emissions. / Ph. D.
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