Strongly coupled plasmon-exciton hybrid nanostructures are fabricated and their optical properties are studied. The plasmonic and excitonic systems are gold nanoshells and J-aggregates, respectively. Gold nanoshells are tunable plasmonic core-shell nanoparticles which can sustain distinct dipole and quadrupole plasmons with resonant energies dependent on core-size/shell-thickness ratio. J-aggregates are organic semiconducting material with excitons that possess very high oscillator strength making them suitable for coherent interaction with other kinds of excitations. The J-aggregates are formed on the surface of the nanoshells when a water/ethanol (50:50) solution of the dye molecules (2,2'-dimethyl-8-phenyl-5,6,5',6'-dibenzothiacarbocyanine chloride) is added to an aqueous solution of nanoshells. These nanoshell-J-aggregate complexes exhibit coherent coupling between localized plasmons of the nanoshell and excitons of the molecular J-aggregates. Coherent coupling strengths of 120 meV and 100 meV have been measured for dipole and quadrupole plasmon interactions with excitons, respectively. Femtosecond time-resolved transmission spectroscopy studies are carried out in order to understand the possible sources of optical nonlinearities in the nanoshell-J-aggregate hybrid. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The transient behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.

Nous avons étudié la relaxation des polaritons dans une cavité contenant un gaz d'électrons de densité contrôlable. Dans un premier temps, la densité d'électrons a été mesurée. Elle peut être variée entre 0 et 10^11 cm-2. Nous avons ainsi pu étudier un nouveau mécanisme de relaxation : la relaxation par collisions polariton-électron, qui était encore mal connu auparavant. Ce mécanisme permet d'augmenter d'un ordre de grandeur les facteurs d'occupation dans les états de polariton proches de k//=0. La comparaison avec la relaxation par collisions polariton-polariton montre cependant que les deux mécanismes de collisions sont aussi efficaces l'un que l'autre, contrairement à ce qui avait été proposé théoriquement. La différence observée entre théorie et expérience est discutée dans le manuscrit. Enfin, nous avons étudié la photoluminescence résolue en temps des polaritons et montré que les modifications observées sont en grande partie dues aux mécanismes de formation des excitons.

Reproduction de : Thèse de doctorat : Physique Mathématique : Toulon : 2007. / Titre provenant du cadre-titre. Bibliographie p.197-198.

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Orientador: Dario Antonio Donatti / Banca: Fábio Simões de Vicente / Banca: Ivan de Oliveira / Resumo: A incorporação de nanopartículas em matrizes híbridas produz materiais com grande potencial para aplicações em diversas áreas de estudo. Na óptica, sua funcionalidade surge quando elétrons confinados em estruturas tridimensionais nanométricas são excitados. Em princípio, esses materiais exibem nível de energia discreto, apresentando picos estreitos no espectro de absorção. Tal comportamento torna-os atrativos para óptica não-linear e aplicações eletro-ópticas. Neste trabalho, o processo sol-gel foi utilizado para a síntese de nanocompósitos contendo CuCl ou CuBr. Cu2O, HBr e HCl foram utilizados como precursores para os CuBr e CuCl, e a matriz Orgânica/Sílica foi preparada a partir dos alcóxidos 3-glicidoxipropiltrimetoxisilano (GPTS) e Tetraetilortosilicato (TEOS). As amostras foram preparadas na forma de filmes finos depositados sobre lâminas de vidro, utilizando a técnica Dip-Coating. Após a secagem, as amostras foram tratadas num forno convencional e/ou expostas à radiação UV utilizando uma luz negra comercial. A espectroscopia de absorção UV-VIS permitiu identificar estreitas bandas de absorção, bem como sua variação. O espectro de absorção (UV-VIS) registrou à temperatura ambiente picos em 418 e 399 nm para as nanopartículas de CuBr e a 376 e 380 nm para as nanopartículas CuCl, correspondente aos excitons Z1,2 e Z3 respectivamente. Comportamento semelhante foi relatado na literatura / Abstract: The incorporation of nanoparticles in hybrid matrices has produced materials with great potential for applications in many fields of study. In optics, its functionality arises when electrons confined in nanometric three-dimensional structures are excited. At first, these materials exhibit discrete energy level, with sharp peaks in the absorption spectrum. Such behavior makes them attractive to non-linear optical and electro-optical applications. In this work, the sol-gel process was used for the synthesis of nanocomposite containing CuCl or CuBr. These complexes decompose during thermal or ultraviolet treatment, and form copper halide nanoparticles. Cu2O, HCl and HBr were used as precursors for the CuBr and CuCl, and the organic matrix/silica was prepared from alkoxides of 3-glycidoxypropyltrimethoxysilane (GPTS) and tetraethylorthosilicate (TEOS). The samples were made in the form of thin films deposited on glass slides using the dip-coating technique. After drying, they were treated in a conventional oven and/or exposed to UV radiation using a commercial black light. The UV-VIS absorption spectrum allowed to identify narrow absorption bands, such as its variation. The absorption spectrum (UV-Vis) recorded at room temperature showed peaks at 418 and 399 nm CuBr nanoparticles and 376 and 380 to CuCl nanoparticles corresponding to the excitons Z1,2 and Z3 respectively. Similar behavior has been reported in the literature / Mestre

xiv, 114 p. A print copy of this thesis is available through the UO Libraries. Search the library catalog for the location and call number. / Electron spin coherence can arise through a coherent superposition of two spin states in the conduction band of a semiconductor and can persist over remarkably long time and length scales. The robust nature of electron spin coherence makes it an excellent model system for exploring coherent quantum phenomena in semiconductors. This dissertation presents both spectral- and time-domain nonlinear optical studies of electron spin coherence through Λ-type three-level systems in two- and zero-dimensional semiconductor systems. The spectral domain study focuses on the experimental realization of electromagnetically induced transparency (EIT), a phenomenon that exploits destructive interference induced by the spin coherence. Coherent Zeeman Resonance (CZR), a precursor to EIT, is demonstrated in two 2D systems, a GaAs mixed-type quantum well (MTQW) and a modulation doped CdTe quantum well (QW). For these studies, Λ-type three-level systems are formed via dipole coupling of a trion to two electron spin states. The CZR response can be described qualitatively by effective density matrix equations. In addition, effects of manybody Coulomb interactions on CZR are investigated by varying the electron density in the MTQW via optical carrier injection. Time-domain studies based on transient differential transmission (DT) are carried out to explore the excitation, manipulation, and detection of electron spin coherence and to better understand how manybody interactions affect coherent nonlinear optical processes in semiconductors. While electron spin coherence can be formed and detected via resonant excitation of excitons or trions, a surprising observation is that injecting excitons into the 2D electron gas in a modulation doped CdTe QW can significantly alter the oscillatory nonlinear response of the electron spin coherence, while the response remains qualitatively unchanged when trions are injected. These behaviors are attributed to an interplay between manybody effects and carrier heating generated by trion formation from excitons. Finally, donor-bound electrons in GaAs are used as a model of localized electron spins. Spin decoherence of order 10 ns, limited by nuclear hyperfine interactions, is observed. Electron spin rotation induced by a nearly resonant laser pulse is also observed, opening the door for further work on mitigating electron spin decoherence time through optical spin echoes. / Adviser: Hailin Wang

As propriedades ópticas de nanocristais de silício (Si-ncs) têm sido extensivamente estudadas após a primeira demonstração em 1990 de fotoluminescência altamente eficiente em silício poroso. Apesar dos progressos no entendimento da natureza da alta eficiência da luminescência dos Si-ncs e da enorme versatilidade para aplicações optoeletrônicas, este campo ainda é um tema de controvérsia devido à complexidade destes materiais. Além disso, as condições de preparação ainda afetam as propriedades de emissão destes materiais que são de fundamental importância para as aplicações tecnológicas. O presente trabalho teve como objetivo o estudo das propriedades óticas dos Si-ncs e entender os processos fotofisicos envolvidos na recombinação radiativa de éxcitons altamente confinados nesse sistema. Si-ncs embebidos em matriz amorfa de SiO2 foram preparados a partir de filmes de oxido de silício SiyO1-y subestequiométricos (y≥1/3) depositados em substratos de quartzo utilizando um sistema deposição CVD na fase estimulada por plasma (electron cyclotron resonance-plasma enhanced chemical vapor deposition ou ECR-PECVD). Esta técnica oferece boa passivação e estabilidade interfacial Si/SiO2. O tratamento térmico a altas temperaturas (900°C≤Ta≤1100°C) promove a precipitação do silício dentro da matriz, favorecendo um processo de nucleação e crescimento dos Si-ncs. Foram realizados tratamentos térmicos nos filmes sob atmosferas de Argônio (Ar) ou (Ar+5%H2) por duas horas. As distintas atmosferas promoveram a passivação de defeitos superficiais, principalmente de ligações pendentes pelo Hidrogênio. As propriedades associadas diretamente à fabricação, tais como estrutura cristalina, morfologia, tamanho e química da superfície dos Si-ncs foram correlacionadas com os processos de emissão envolvendo éxcitons. A caracterização estrutural foi realizada por Raio-x (XRD), Microscopia de Transmissão de Alta Resolução (HRTEM), Retroespalhamento de Rutherford e Espectroscopia Raman. As medidas óticas foram basicamente Absorção, Excitação Seletiva, Fotoluminescência CW (PL) e Fotoluminescência Resolvida no Tempo. Os resultados da caracterização indicaram que efeitos de confinamento quântico e de estados de superfície dominam o processo de recombinação no Si-nc/SiO2. Em conclusão, os resultados obtidos neste trabalho mostram uma interessante e uma nova correlação entre as condições de fabricação da amostra e os processos de recombinação de éxcitons em Si-nc/SiO2. Todos estes resultados desafiam modelos anteriores propostos para explicar as propriedades ópticas do sistema de Si-nc/SiO2 e prevê ajudar na futura aplicação tecnológica dos mesmos. / The optical properties of silicon nanocrystals (Si-nc) have been extensively studied after the first demonstration in 1990 of highly efficient photoluminescence in porous silicon. Despite progress in understanding the nature of high luminescence efficiency of Si-ncs and versatility for optoelectronic applications, this field is still a subject of controversy due to its complexity. Furthermore, the preparation conditions still affect the emission properties of these materials that are of fundamental importance for technological applications. This work aimed to study the optical properties of Si-ncs and to understand the photophysical processes involved in the radiative recombination of excitons strongly confined in this system. Si-ncs embedded in amorphous SiO2 were prepared from silicon oxide films of substoichiometric SiyO1-y (y≥1/3) deposited on quartz substrates using a CVD deposition system in phase stimulated by plasma (electron cyclotron resonance-plasma enhanced chemical vapor deposition ou ECR-PECVD). This technique provides good passivation and Si/SiO2 interfacial stability. The thermal treatment at high temperatures (900°C≤Ta≤1100°C) promotes the precipitation of silicon within the matrix, favoring a process of nucleation and growth of Si-ncs. The thermal treatments were performed in the films under Argon atmosphere (Ar) or (Ar+5%H2) for two hours. The use of different atmospheres allowed the understand of the passivation process of surface defects, particularly of dangling bonds by Hydrogen. The properties directly related to fabrication such as crystalline structure, morphology, size and surface chemistry of Si-ncs were correlated with emission processes involving excitons. The structural characterization was performed by X-Ray Diffraction (XRD), High resolution transmission electron microscopy (HRTEM), Rutherford Backscattering and Raman spectroscopy. The optical measurements were basically Absorption, Selective excitation, CW photoluminescence (PL) and Time Resolved Photoluminescence. The characterization results indicate that both quantum confinement and surface states effects dominate the recombination process in Si-ncs/SiO2. In conclusion, the results obtained in this work show an interesting and a novel correlation between the sample fabrication conditions and the exciton recombination process in Si-ncs/SiO2. All these results challenges previous models proposed to explain the optical properties of Si-nc systems and are expected to help further technological applications of this system.

Made available in DSpace on 2014-07-29T15:07:06Z (GMT). No. of bitstreams: 1 DissErivelton Oliveira Alves.pdf: 643061 bytes, checksum: 32148288b33769364a665f4bc2c83e1c (MD5) Previous issue date: 2006-08-02 / We investigate the resonant tunneling of electrons and holes in an asymmetric double quantum bit CdTe / CdMnTe in the presence of electric and magnetic fields applied along the growth direction. We show that in this case it is possible to achieve a condition of simultaneous resonant tunneling of electrons and holes with spin set, ie, a resonant tunneling of excitons polarized. Then we calculated the excitonic binding energy as a function of applied fields, showing the strong dependence of the binding energy with the tunneling of carriers. The electronic structure was calculated using the k ~ ~ p multiband Kane model. The eigenstates were obtained by solving numerically the equations ° C ~ the effective mass using the method of inverse power. The effects of lattice strain were treated by the Bir-Pikus model. The energy calculation of excitonic Dial-Up was conducted using the variational method. We consider the perfectly abrupt interfaces of the heterostructures, ie effects of enlargement of the interfaces were neglected. / Investigamos o tunelamento ressonante de elétrons e buracos em um pouco quântico duplo assimétrico de CdTe/CdMnTe na presença de campos elétricos e magnéticos aplicados ao longo da direção de crescimento. Mostramos que neste caso é possível alcançar uma condição de tunelamento ressonante simultâneo de elétrons e buracos com spin definido, isto é , um tunelamento ressonante de éxcitons polarizados. Em seguida calculamos a energia de ligação excitônica em função dos campos aplicados, mostrando a forte dependência da energia de ligação com o tunelamento dos portadores. A estrutura eletrônica foi calculada usando o método ~k ~p no modelo multibandas de Kane. Os autoestados foram obtidos resolvendo-se numericamente a equa¸c ao da massa efetiva usando o método das potência inversa. Os efeitos de tensão da rede cristalina foram tratados pelo modelo de Pikus-Bir. O cálculo de energia de ligaçãoo excitônica foi realizado usando o método variacional. Consideramos as interfaces da heteroestrutura perfeitamente abruptas, isto é, efeitos de alargamento das interfaces foram desprezados.

Orientador: Fernando Iikawa / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Fisica Gleb Wataghin. / Made available in DSpace on 2018-08-12T12:58:46Z (GMT). No. of bitstreams: 1 Gomes_PauloFreitas_D.pdf: 14344200 bytes, checksum: 55a7f7d3b644c0dc43151a411d53757b (MD5) Previous issue date: 2009 / Resumo: No presente trabalho apresentamos um estudo da luminescência de érbio em nanocristais de silício (nc-Si) e nanofios de óxido de zinco (nw-ZnO). Os nanocristais de silício com érbio são obtidos através do tratamento térmico de filmes finos amorfos de sub-óxidos de silício (SiOx) preparados por rf-sputtering, variando a concentração de Oxigênio e érbio durante o crescimento. O érbio é adicionado aos filmes cobrindo parcialmente a superfície do alvo de silício com pequenos cacos de érbio metálico. Medidas de espectroscopia Raman e microscopia eletrônica de alta resolução (HRTEM) fornecem o tamanho e densidade de nanocristais em cada amostra. Medidas de fotoluminescência (PL) dos nanocristais na temperatura ambiente mostram que o tamanho dos nanocristais varia com a concentração de oxigênio e temperatura de tratamento térmico. A dependência da PL dos nanocristais com a temperatura pode ser entendida considerando a competição entre processos radiativos e não-radiativos. Em amostras com érbio a taxa de recombinação não-radiativa é maior que nas amostras sem érbio. O estudo da PL dos nanocristais e dos íons Er3+ mostra que o Er3+ funciona como um centro de recombinação não-radiativa para a energia proveniente da recombinação de portadores nos nanocristais. Neste caso, parte da energia gerada nos nanocristais é transferida para os íons Er3+ ao invés de ser emitida na forma de fótons. Também é possível observar que a intensidade da PL do Er3+ depende da intensidade da PL dos nanocristais e é maior em amostras contendo nanocristais de ~3nm (que emitem em ~1,5eV), indicando que a transferência é ressonante (com a excitação 4I15/2 ---> 4I9/2 do Er3+ que corresponde a uma energia de 1,5eV). Os nanofios de ZnO com érbio são preparados por deposição vapor-liquid-solid (VLS) e por electrospinning. Em amostras preparadas por VLS, o érbio é depositado sobre os nanofios após sua preparação. No electrospinning um composto organometálico de érbio é adicionado ao polímero precursor. É observada luminescência de érbio quando as amostras são excitadas com um comprimento de onda ressonante com algum nível mais energético do Er3+. Nanocristais de E2O3 são observados por HRTEM na superfície dos nanofios preparados por VLS. Medidas de EXAFS revelam que a vizinhança do Er nessas amostras é idêntica à do óxido Er2O3, indicando que não ocorreu dopagem substitucional do ZnO. / Abstract: We present a study of erbium luminescence in silicon nanocrystals (nc-Si) and zinc oxide nanowires (nw-ZnO). Silicon nanocrystals are produced by annealing of amorphous sub-oxide thin films (SiOx) prepared by rf-sputtering varying the oxygen and erbium concentration during growth. Erbium is added by partially covering the silicon target surface with small pieces of metallic erbium. Raman spectroscopy and HRTEM measurements reveal the size and density of nanocrystals in each sample. Photoluminescence (PL) measurements at room temperature show that the nanocrystal size changes with oxygen concentration and annealing temperature. The PL dependence on the temperature can be understood considering a competition between radiative and non-radiative processes. In samples with erbium the non-radiative recombination rate is higher than in samples without erbium. The study of the nanocrystal and Er3+ PL show that Er3+ behaves as non-radiative recombination centers for excited carriers in the nanocrystals. Part of the energy from the nanocrystals is transferred to Er3+ instead of being emitted as light. The Er3+ PL intensity depends on the nanocrystal PL intensity and is higher in samples containing nanocrystals ~3nm (which emit at ~1.5eV), indicating that the energy transfer is resonant (with the 4I15/2 -----> 4I9/2 Er3+excitation at ~1.5eV) ZnO nanowires were prepared by vapor-liquid-solid (VLS) deposition and by electrospinning. In the VLS method erbium is deposited on the nanowires after growth. In the electrospinning method a metallorganic compound is added to the polymer precursor. Erbium PL is observed when the samples are excited by one of the Er3+ higher transitions. Er2O3 nano-crystals are observed by HRTEM on the surface of the nanowires prepared by VLS. EXAFS measurements in these samples show that the Erneighborhood is identical to that of E2O<>3 indicating that there was no substitutional / Doutorado / Física / Doutor em Ciências