Esta tesis describe el diseño, la fabricación y la caracterización óptica de sistemas plasmónicos resonantes capaces de confinar y aumentar campos de luz en la escala manométrica. En primer lugar, se utilizaron modelos numéricos 3D para diseñar diferentes geometras de nanoestructuras plasmónicas acopladas, a través del cálculo de la respuesta óptica de su campo lejano y cercano. Sobre la base de estas simulaciones se fabricaron las nanoestructuras por litografía de haz electrónico. Se puso especial énfasis en el aumento de la resolución y la optimización de la reproducibilidad de parámetros críticos como la forma de las partículas y el gap entre ellas. Por último, se empleó espectroscopía de campo lejano combinada con espectroscopía de luminiscencia inducida por dos fotones (TPL) para sondar la respuesta óptica local de las geometrías optimizadas. Hemos centrado nuestra atención en diferentes tipos de estructuras metálicas: dímeros, antenas con gap, conjuntos finitos de partículas en cadenas y en forma de estrella. Los dímeros tienen una fuerte amplificación del campo en su gap nanométrico por el acoplamiento en campo cercano de sus resonancias plasmonicas dipolares. Análogamente, antenas con gap, formadas por dos barras de oro adyacentes que soportan resonancias multipolares, pueden acoplar de manera eficiente la luz y concentrarla en volúmenes pequeños. Se ha demostrado que cadenas finitas de partículas son buenos candidatos para guiar la luz a través de secciones transversales por debajo de la longitud de onda y aquí demostramos que también se pueden utilizar como nanolentes capaces de concentrar la luz en su extremo. La distribución del campo cercano en conjuntos de partículas de oro en forma de estrella presenta una fuerte dependencia con la polarización del campo incidente que puede ser explotada para dirigirse dinámicamente a nano-objetos. La espectroscopía de campo lejano de conjuntos de dímeros y de cadenas finitas de partculas se comparó con la espectroscopía de TPL. Nuestro principal resultado es mostrar que la TPL es preferentemente sensible a los campos locales, permitiendo evaluar características espectrosc ópicas que no podrían resolverse de otro modo. A fin de superar las limitaciones de las medidas de conjuntos, en una segunda etapa se dedicó un considerable esfuerzo a construir y optimizar un montaje óptico para medir la señal de TPL de estructuras únicas. El uso de la micro-espectroscopía de TPL permitió obtener mapas espectrales de los modos de antenas aisladas con resolución espacial. Como se predijo mediante cálculos, hemos sido capaces de visualizar directamente, en la resonancia, la señal de TPL amplificada dentro del gap. Nuestros resultados muestran cómo las medidas de TPL pueden compararse directamente con la distribución de la cuarta potencia del campo local calculado. Mediante el análisis de la evolución de la señal de TPL en función de la longitud de onda incidente en el gap y en las extremidades de la antena tenemos más conocimiento sobre el mecanismo físico detrás de la resonancia de la antena. Finalmente, la microscopía de TPL se utilizó para sondar el campo cercano para diferentes orientaciones de la polarización lineal incidente sobre los conjuntos de partículas en forma de estrella. Se demuestra que, a diferencia del espectro de dispersión, la distribución de TPL en la estructura depende drásticamente del estado de polarización incidente. Nuestro estudio aporta una contribución significativa al campo de la óptica de plasmones, proponiendo nuevas geometrías para confinar de manera eficiente los campos ópticos a la escala nanometrica, aportando un profundo conocimiento sobre el uso de micro-espectroscopa de TPL como sonda óptica local. Nuestros resultados tendrán importancia en aplicaciones tales como espectroscopía mejorada, biosensores y la interacción luz-materia, donde se necesita evaluar el campo experimentado por una pequeña cantidad de materia cercana a la nanoestructura. / This thesis describes the design, fabrication and the optical characterization of plasmon-resonant systems able to confine and enhance light fields down to the sub-wavelength scale. Extensive 3D numerical modeling was first used to design different geometries of coupled plasmonic nanostructures through the calculation of their far-field and near-field optical response. On the basis of simulations, the nanostructures were fabricated by e-beam lithography and thin film deposition. Special efforts were devoted to increasing the resolution and optimizing the reproducibility of critical parameters such as particle shape and interparticle gaps. Finally, far-field spectroscopy combined with two-photon induced luminescence (TPL) spectroscopy was used to probe the local optical response of the optimized architectures. We focused our attention on different families of structures: metal dimers, bar antennas, finite chains of nanoparticles and star-like particle arrangements. Particle dimers feature strong field enhancements in their sub-wavelength gap due to near-field coupling of their dipolar localized plasmon resonances. Based on the same physics, gap antennas, formed by two adjacent gold bars supporting multipolar resonances can efficiently couple to propagating light and concentrate it into tiny volumes. While finite particle chains were previously shown by other authors to be good candidates to guide light through subwavelength cross-sections, we show here that they can also be used as efficient nanolenses able to concentrate light at their extremity. Finally, the near-field distribution in star-like arrangements of gold nanoparticles exhibits a strong dependence with the incident field polarization which can be exploited for dynamical optical addressing of nano-objects. We have compared the far field spectroscopy of large ensembles of dimers and finite chains to TPL spectroscopy. Our main result is to show that TPL is preferentially sensitive to local fields and that it enables the assessment of spectroscopic features which cannot be resolved otherwise. In order to overcome the limitations of measurements on large ensembles a considerable effort was dedicated to mounting and optimizing an optical set-up enabling TPL measurement of single structures. Using the developed TPL micro-spectroscopy, spatially resolved spectral mode mapping on single resonant gap-antennas was achieved. As predicted by calculations, we were able to directly visualize at resonance the strongly enhanced TPL signal within the gap. Our results show how TPL scans can be directly compared with the convoluted distribution of the fourth power of the calculated local mode field. By monitoring the evolution with the incident wavelength of the TPL signal within the gap and at the antenna extremities we got further insight in the physical mechanism behind the buildup of the antenna’s resonance. Finally, TPL microscopy was used to probe the local fields under different orientations of the incident linear polarization near star-like arrangement of gold disks. It is shown that, unlike the scattering spectrum, the TPL distribution over the structure is found to depend drastically on the incident polarization state. Our study brings a significant contribution to the field of Plasmon optics by proposing novel geometries able to efficiently confine optical fields down to the nanometric scale, but also by providing deep insight into the use of TPL microspectroscopy to probe their local optical response. Our findings are foreseen to be important in applications such as enhanced spectroscopy, bio-sensing and enhanced light-matter interaction, where one needs to assess the actual field experienced by small amounts of matter.

No description available.

In this thesis, we have reported the MBE growth, design, and fabrication of the InGaAs quantum dots (QDs) laser/semiconductor optical amplifier, broadband QDs structure, coupled double cavity structure for terahertz emission on GaAs substrate. The emission wavelengths of the strain-induced S-K growth mode QDs structures are adjusted through the composition of QDs and strain-compensated capping layer. Also, the technique of growing high quality InGaAs QDs with solid source molecular beam epitaxy has been established and characterized by double crystal X-ray diffraction, transmission electron microscopy, photoluminescence, electroluminescence measurements. For 1.3£gm QDs laser samples, ridge waveguide lasers of the Fabry-Perot (FP) type are fabricated by wet-etching process. From the QDs laser L-I curve, the e2-hh2 transition at £f =1160nm have larger optical gain than e1-hh1 transition at £f =1220nm. The FP laser with 0.6£gm cavity length shows a lasing peak of 1160nm at threshold. As the cavity length increase to 2£gm, the lasing peak red shift to 1220nm (closed to ground state emission wavelength). This energy band gap transition phenomenon is obvious especially in the QDs laser with quantum well (QW) structure. When the injection current increase, two lasing peaks at £f= 1160 and 1175nm are observed sequentially. This unique lasing behavior is shown to be consistent with carriers localized in noninteracting dots. For the application of 1.3£gm light source, we optimum the growth condition for different needs in optical coherent tomography (OCT) light source, tandem solar cell, terahertz emission light source, etc. For the super luminescence diode (SLED) in OCT, we design multi-stacked asymmetric QDs structure (AMQD), QDs in the well structure (DWell), Dwell with p-doping in well structure to investigate the carrier recombination condition and bandwidth. Comparing with 5 structures in this study, the Dwell with p-doping in well structure has a maximum EL bandwidth exceed 198nm. The large bandwidth is attributed to the QW which increases the carrier capture rate and the p-doping which provide the efficient holes in valance band. This structure provides an excellent SLED light source solution to replace the existing program. For the tandem solar cell, we use the multi-stack QDs to compose broadband absorption in 1eV range. In order to avoid the degradation in the open circuit voltage, we use InGaAs QW to reduce the QDs strain. We observed the doping effect on the built in field through the photo-reflectance measurements. For the better photocurrent collection, we use p-doping in the QW to increase the built-in field intensity to obtain higher efficiency. For the terahertz emission, the QDs embedded in coupled double-cavity structures with an AlAs/GaAs intermediate distributed Bragg reflector (DBR) are grown on GaAs substrates. Two emission peaks at 1180, 1206 nm from the QDs corresponding to the coupled double-cavity resonant modes are observed in the high reflection band. The frequency differences for the two resonant coupled modes are of 5.5 terahertz, and have been successfully controlled by changing the pair numbers for the intermediate DBR. In addition, we have grown the InGa(Al)As nanostructures on InP substrate. The lattice constant difference between InGaAs and InP is relatively smaller compare with GaAs substrate, and it will be more challenge in epitaxial growth. After we investigate the strain, surface morphologies, optical properties for the nanostructures, we find the group III elements play an important role in the morphologies. Wire formation is attributed by the enhanced adatom diffusion length in the stepped surface front along [0-11] direction for the presence of Ga both in the nanostructure and buffer layer. Finally, we established QDs, Qwires database for the valuable new possibilities for designing new and original structures.

In this article, a multiple-responsive polymer micelles system was constructed by using ionic bond to link the hydrophobic tetraphenylthiophene (TP) fluorophores, which possess the property of aggregation-induced emission enhancement (AIEE), with the hydrophilic poly(N-isopropyl acrylamide) (PNIPAM). The susceptibility of the ionic ammonium-sulfonate (Am-Sul) bonds towards metal ions, acid and base triggered the AIEE-operative fluorescence (FL) response. To exercise the idea, PNIPAM with sulfonate terminal was primarily prepared to react with TP-derivatives functionalized with ammonium groups to generate polymer complex of TP-PNIPAM. When in water, the polymer complex TP-PNIPAM formed micelles with the aggregated TP core interconnecting the hydrophilic PNIPAM shell by the ionic Am-Sul bonds. With the operative AIEE effect, the aggregated TP core of the micelles fluoresced but upon the additions of metal ions, acid and base, the ionic bonds dissociated to result in the collapse of the micelles and the FL quenching. A novel fluorogenic sensor capable to respond to multi-stimuli was therefore constructed. Amphiphilic micelle systems with the hydrophilic poly(N-isopropyl amide) (PNIPAM) shell and the hydrophobic tetraphenylthiophene (TP), which has the novel aggregation-induced emission enhancement (AIEE) feature, core inter-connected by ionic bonds were prepared in this study to explore the AIEE-operative emission response towards critical micelle concentration (CMC) and lower critical solution temperature (LCST). To exercise the idea, TP functionalized ammonium cations and PNIPAM with terminal sulfonate group were individually prepared and mixed together to yield three amphiphilic TP-PNIPAM complexes with different hydrophobic TP to the hydrophilic PNIPAM (x/y) ratios. When in aqueous solution, TP-PNIPAMs form micelles with the aggregated TP core, which emits strongly due to the operative AIEE effect, encompassed by the PNIPAM shell. The resultant CMC and LCST of the TP-PNIPAM micelles can be varied by changing the hydrophobic to the hydrophilic x/y ratio and can be monitored by the AIEE-dominant fluorescence responses towards concentration and temperature variables.

We have designed and synthesized a bistable pseudo-rotaxane carrying a fluorescent boradiazaindacene (BODIPY) unit. The intensity of the emission signal is dependent on the position of the cucurbituril (CB7) unit over the axle component. Thus, pH modulated switching of the CB7 wheel is accompanied by significant changes in the emission spectrum. Additionally, a thiosulfate-sulfite-iodate oscillating reaction which generates large amplitude pH oscillations can be carried out in the same solution. In such a solution, in response to changing pH, the position of the wheel component seems to change without outside intervention.

Time Resolved OSL (TR-OSL) is a technique to record the luminescence decay curve data after a brief stimulation pulse and can possibly be used for the separation of luminescence signals from quartz and feldspars. In this study luminescence emission from quartz and feldspar samples was investigated. TR-OSL signals of these samples were studied for the variations with preheating and annealing temperature, stimulation pulse width and total stimulation time, optical bleaching, radiation dose and measurement temperature. TR-OSL decay lifetime of quartz samples was found as ~40 &micro / s. Na-feldspar and K-feldspar luminescence signals were deconvoluted using a linear sum of three exponential decays with lifetimes about 45 &micro / s, 8 &micro / s and 1 &micro / s and about 35 &micro / s, 7 &micro / s and 0.6 &micro / s, respectively. Since feldspars signals have a component with lifetime similar to that of quartz (~40 &micro / s), luminescence signal separation with TR-OSL seems to be not straightforward.

The aim of this current work is to analyze the behavior of OSL (Optically Stimulated Luminescence) signals of irradiated spices with respect to time, temperature, origin and the type. Throughout the experiments, 3 different type spices from four different origins were stored at 4&deg / C and 25&deg / C for six months after irradiation. During experiments, unirradiated red pepper, thyme and cumin samples were analyzed by using OSL technique in order to determine the background OSL signal values of samples. Samples were irradiated 10 kGy by Cobalt 60 gamma source in TAEK (Turkey Atomic Energy Association). After irradiation process, OSL signal values of different samples were analyzed according to the given parameters. In order to determine the effect of temperature on OSL signal loss, temperature (4&deg / C- 25&deg / C) was set as storage temperature. The analyses were made monthly. According to the statistical analyses (ANOVA- General Linear Model), origin and type of samples were detected as significant parameters of design experiment. Time and temperature effect on OSL signal loss changed with respect to origin and type of samples. After six months storage period, OSL signal was lost for most of the origin and sample type. At the end of sixth month, an ESR analysis was performed to detect the accuracy of the OSL technique. With respect to the results of these experiments, it was seen that, due to optical fading, most of the samples was observed as unirradiated by OSL technique, however ESR analyze the samples as irradiated at the end of sixth month. Irradiation had a detrimental effect on the microbiological load of the samples and resulted 6 log reduction on the microbial population. After irradiation, no colony formation was observed in total bacteria and yeast- mold count. During six month period, no injury recovery was observed.

Luminescence is the emission of light resulting from radiative transition of an atom from an excited state to a ground state. This radiative transition yields emission of photons and the luminescence is the general name which is used to classify &ldquo / cold emission&rdquo / other than the blackbody radiation. Spectroscopy involves the measurement of intensity of emitted, absorbed or scattered electromagnetic radiation as a function of wavelength. Thus, it is a valuable tool in the study of understanding the luminescence production mechanisms. Measurement of emission spectra gives information about the energy levels of transition and structure, geometry and composition of the sample. In this study, a versatile luminescence emission spectrometer was designed and developed with the main aim of measuring Photoluminescence (PL), Thermoluminescence (TL) and Optically Stimulated Luminescence (OSL) emission spectra of materials relevant for dosimetry. The spectrometer was constructed around a Littrow type monochromator by developing the necessary hardware, firmware and software. Wavelength calibration, measurement of spectral response and determination of resolution of the spectrometer were done using calibration lamps and a calibrated spectroradiometer. Finally the performance of the constructed spectrometer was tested by measuring the emission spectra of materials such as BeO, Al2O3 and CaF2 wherever possible the measured spectra were compared with the ones reported in the literature.

Afin d'accéder à des agents de contraste efficaces, il est essentiel d'optimiser simultanément les paramètres moléculaires influençant la relaxivité : nombre de molécules d'eau en première sphère de coordination, échange de l'eau, dynamique de rotation du complexe, relaxation électronique, distance Gd(III)-proton. Le but de ce travail est double. D'une part, il s'agit de concevoir et étudier des complexes possédant un nombre élevé de molécules d'eau coordinées et de comprendre l'influence de la sphère de coordination du métal sur la stabilité des complexes et la relaxation électronique. D'autre part, nous avons utilisé les ligands comme chromophores pour la mise au point de sondes luminescentes pour l'imagerie biomédicale.<br />Nous présentons la structure, la stabilité et la relaxivité de complexes de Gd(III) de deux séries de ligands tripodes dérivés du picolinate basés, soit sur le cycle 1,4,7-triazacyclononane, soit sur un pivot amine tertiaire. Ces complexes possèdent une relaxivité élevée dans l'eau et dans le sérum et peuvent former des interactions non-covalentes avec l'albumine sérique. L'interprétation de la relaxivité des protons de l'eau au moyen de nouvelles méthodes relaxométriques basées sur l'utilisation de solutés sondes nous a permis de montrer que la présence de groupement picolinate et du cycle 1,4,7-triazacyclononane pouvait conduire à des complexes de Gd(III) possédant des propriétés de relaxation électronique favorables.<br />Du fait de la présence de chromophores picolinate, les complexes d'Eu(III) et Tb(III) avec ces ligands donnent lieu à une luminescence intense dans le visible. D'autres complexes dérivés de l'unité 8 hydroxyquinoléine possèdent une luminescence élevée dans l'infrarouge et ont également été étudiés.

L'objectif de ce travail était de dater des coulées volcaniques de la Chaîne des Puys (Massif Central, France) situées chronologiquement dans la période de l'événement paléomagnétique de Laschamp (30-50 ka). Les méthodes utilisées étaient la thermoluminescence et la luminescence stimulée optiquement appliquées à des grains de quartz et à des galets quartzeux extraits de sédiments cuits par ces coulées. Ces minéraux émettent des signaux de luminescence dont le comportement est souvent irrégulier. Leur paléodose a donc été déterminée par différentes méthodes pour choisir celles qui seraient les plus appropriées à l'obtention de résultats fiables. Ces intercomparaisons ont mis en évidence une dispersion des résultats supérieure à ce qui pouvait être attendu au regard des incertitudes habituellement associées à chacune d'entre elles. Dans la plupart des cas, ces observations ont conduit à proposer un intervalle assez large dans lequel est compris l'âge probable de l'échantillon.