Utilizando cristais de KCl:SH- dopados com centros F2+ na ausência de centros F e F2, permitiu-nos estudar o Dicroísmo Circular Magnético (DCM) em absorção das transições 1s ?g(493?m) e 1s ?g - 2py?w (509 ?m) como função do campo magnético de 0 < H < 48 KG e temperatura entre 1.5 < T < 77K. A transição 1s ?g, 2p? (1.4 ?m) em absorção não apresentou DCM dentro do limite de detecção de nosso equipamento (1.2 X 10-4); o mesmo aconteceu com a transição (2p?w- 1s ?g) em emissão (1.2 X 10-4). Irradiando com luz polarizada na banda ?, os centros F2+ se .reorienta ao longo da direção [110] em até 1.5 K, apresentando uma forte birrefringência. Medidas em absorção com centros F2+ alinhados em várias geometrias, permitiu estudar a contribuição ao DCM de cada orientação do defeito. Apresentamos um modelo teórico em bom acordo com os resultados experimentais. Utilizando uma técnica de Detecção óptica de EPR, determinamos o fator de Landé para o estado fundamental (g =1.965 ± 0.007) e o tempo de relaxação spin-rede do estado fundamental a H = 3.2 KG, que é típico do processo direto T1-1 = 4.3 X 10-2cotgh(g?H/2kT). / Using KCl:SH- doped with F2+ centers without F and F2, we studied the Magnetic Circular Dichroism (MCD), in absorption of yhe transition 1s ?g(493?m) and 1s ?g - 2py?w (509 ?m) as a function of the magnetic field 0 < H < 48 KG and temperature 1.5 < T < 77K. The transition 1s ?g, 2p? (1.4 ?m) does not present any MCD within the limit of detection of our equipament (1.2 X 10-4); No dichroism has been observed in emission in the 2p?w- 1s ?g transition (1.2 X 10-4). F2+ centers reorient along the [110] direction down to 1.5 K by polarized light excitation in the ? bands and present a strong birefringence. Measurements in absorption with aligned F2+ in various geometry allows as to determine the contribution of each orientation to the DCM. A theorical model is presented in good agrement with the experimental results. The optical detection of the EPR in X-band give the Landé factor af the graund state is g =1.965 ± 0.007) and the spin-lattice relaxation measured at H = 3.2 KG is typical of a direct process T1-1 = 4.3 X 10-2cotgh(g?H/2kT).

Les fibres dopées erbium couvrent de nombreuses applications, particulièrement dans le domaine des télécommunications terrestres et sous marines, avec les amplificateurs optiques. Aujourd’hui, il existe un réel intérêt pour l’industrie spatiale d’utiliser ces fibres dans les satellites. Cependant, pour utiliser leur potentiel, une qualification en milieu radiatif doit être effectuée, c'est justement l'objet principal de ce travail de thèse. Grâce au partenariat industriel avec Draka-Prysmian, nous avons accès à une grande diversité de fibres en termes de compositions chimiques : ceci nous permet d’étudier leur sensibilité aux radiations, et de comprendre le rôle essentiel des dopants et des codopants dans cette sensibilité. Une étude de celle-ci en temps réel, associée à une caractérisation pré et post-irradiation des fibres optiques, rend possible l'identification fine des défauts induits sous irradiation, et la compréhension de leur mécanisme de formation, en fonction de la composition de ces fibres. Cette étude permet ainsi de proposer un modèle physique de leur dégradation, et aussi de leur guérison, complété par un modèle d'amplificateur. Il permet de prédire, en fonction de la composition des fibres, le comportement quantitatif des amplificateurs optiques associés, en termes de gain et et de bande passante, versus un dépôt de dose typique d'une mission spatiale ; il répond ainsi aux attentes des principaux acteurs du domaine. En outre, le bénéfice de ce travail ouvre des portes dans le domaine de la dosimétrie par fibre optique active, dans différents environnements radiatifs autres que le domaine spatial, tels que le milieu médical ou l'environnement nucléaire. / Erbium-doped optical fibers open up many applications, especially in the field of terrestrial and underwater telecommunications, with optical amplifiers. Nowadays, there is a real interest for the space industry to use these fibers in satellites. However, in order to use their full potential, qualification in radiative environments is to be carried out, this is the main focus of this PhD work. Thanks to the partnership with Draka-Prysmian group, we have a full access to a large diversity of specialty fibers, in terms of chemical compositions : this allows us to study their sensitivity to radiations, and to determine the important role of dopants and co-dopants in this sensitivity. A real-time study of it, associated with a qualification of pristine and irradiated optical samples, enables the detection of radiation-induced defects, and the understanding of their creation process, as a function of the fiber structure. This study provides a physical model describing the degradation and the recovery of these fibers, enhanced with an amplifier modeling. It allows the prediction of the quantitative behavior of specialty fiber-based amplifiers, in terms of gain and bandwidth, versus the chemical composition of the fibers used, for a typical space mission dose ; thus this modeling meets the needs of the spatial market key actors. Furthermore, the benefit of this work opens up another avenues for some larger opportunities, in various radiative environments, such as the medical field or the areas of nuclear facilities.

When doing computations on the negatively (positively) charged NV-center in diamond, the common procedure is to add (subtract) an electron from the system. However, when using periodic boundary conditions, this addition/subtraction of an electron from the supercell would result in a divergent electrostatic energy. So an artificial background jellium charge of opposite charge that compensate the electronic charge to make the supercell neutral is needed. This introduces further problems that needs corrections. And this method is especially problematic for slab supercells, as the compensating background charge leads to a dipole, which diverges as the vacuum between the slab images increases. An alternative, recently proposed way of charging the NV-center is to introduce electron donors/acceptors in the form of nitrogen/boron atoms (at substitutional sites in the diamond lattice). In this way, we keep the supercell/slab neutral, and avoid correction schemes. In this work we verify that the addition of a substitutional nitrogen atom indeed has the same effect on the NV-center as the more traditional method of adding an extra electron to the system. Further, we investigate the effects of 1. Adding two substitutional nitrogen atoms to the system (3 nitrogen atoms in total, neutral supercell), 2. Adding a substitutional nitrogen atom and an electron to the system (2 nitrogen atom in total, negatively charged supercell), 3. Adding two electrons to the system (1 nitrogen atom, doubly negatively charged supercell). Additionally, we investigate the addition of acceptor dopants (boron) in order to analyze the effect on the electronic structure of the NV-center and diamond.

Neste trabalho foram analisados 49 diamantes coloridos da coleção Luiz Paixão incorporados 1954 ao acervo do Museu de Geociências do IGc-USP. Os diamantes foram pesados, medidos, fotografados e alguns foram escolhidos para análise espectroscópica no UV-VIS com a finalidade de auxiliar no estudo de centros de cor e distinção sobre a origem da cor nos diamantes quanto esta ser natural ou artificialmente induzida. Pelo resultado da interpretação dos espectros obtidos, uma parte desta coleção de diamantes coloridos sofreu tratamentos de cor por irradiação, demonstrando que no Brasil na época da formação desta coleção já era possivel de encontrar diamantes tratados o que é um fato interessnte considerando os poucos reatores nucleares existentes na época. / This work presents results of an analysis of 49 colored diamonds from the Luiz Paixão Collection, donated 1954 to the Geological Museum of Geoscience Institute of University of São Paulo. They have been measured, photographed and some have been selected for detailed spectroscopic analysis by UV/VIS spectroscopy. By this method it is possible to detect if the color of the diamond is natural or produced by treatment. The presence of specific absorption peaks and their intensity in the spectrograms revealed that all blue and green diamonds indeed showed signs of treatment and their color is not natural. This is a very interesting fact and shows that already in times before the donation treated diamonds were apparently easily available in Brasil. Considering the paucity of nuclear reactors in the United States or in Europe in those times this result is very surprising.

O objetivo deste trabalho é o desenvolvimento de um laser de centro de cor para aplicações em espectroscopia. O laser opera em regime CW e a cavidade óptica utilizada é do tipo X, com dois espelhos esféricos intracavidade astigmáticamente compensados. O meio ativo utilizado foi um cristal de KCl:Li+ com centros FA (II), e como fonte de bombeamento foi empregado um laser de Ar+ em 514nm. O limiar de potência de bombeamento foi de 120 mW, a eficiência energética foi de 2,8% e o intervalo de sintonia obtido vai de 2,56 a 2,82 &#956m numa potência de bombeamento de 700mW. O laser opera também com a cavidade na configuração anel. Para testar o LCC foram feitas aplicações empregando a técnica de espectroscopia intercavidade em cristais de KCl: Li+: NO-2: NO-3 e KBr:OH-. / The present work shows the development of a color Center laser for spectroscopy application. It is a CW laser which uses an X-type cavity with two astigmatically compensated intracavity spherical mirrors. The laser can be converted to a ring laser. The used active medium was a KCl:Li+ single crystal with a FA (II) centers and the pumping source was an Ar+ laser (&#955= 514nm, 700mW). Pump power at threshold was measured to be 120mW. The tuning range was 2.56&#60 &#955 &#60 2.82 &#956m and the slope efficiency was 2,8%. To test the color center laser we measured intracavity spectra of KCl: Li+: NO-2: NO-3 and KBr:OH- single crystals.

Neste trabalho foram analisados 49 diamantes coloridos da coleção Luiz Paixão incorporados 1954 ao acervo do Museu de Geociências do IGc-USP. Os diamantes foram pesados, medidos, fotografados e alguns foram escolhidos para análise espectroscópica no UV-VIS com a finalidade de auxiliar no estudo de centros de cor e distinção sobre a origem da cor nos diamantes quanto esta ser natural ou artificialmente induzida. Pelo resultado da interpretação dos espectros obtidos, uma parte desta coleção de diamantes coloridos sofreu tratamentos de cor por irradiação, demonstrando que no Brasil na época da formação desta coleção já era possivel de encontrar diamantes tratados o que é um fato interessnte considerando os poucos reatores nucleares existentes na época. / This work presents results of an analysis of 49 colored diamonds from the Luiz Paixão Collection, donated 1954 to the Geological Museum of Geoscience Institute of University of São Paulo. They have been measured, photographed and some have been selected for detailed spectroscopic analysis by UV/VIS spectroscopy. By this method it is possible to detect if the color of the diamond is natural or produced by treatment. The presence of specific absorption peaks and their intensity in the spectrograms revealed that all blue and green diamonds indeed showed signs of treatment and their color is not natural. This is a very interesting fact and shows that already in times before the donation treated diamonds were apparently easily available in Brasil. Considering the paucity of nuclear reactors in the United States or in Europe in those times this result is very surprising.

O objetivo deste trabalho é o desenvolvimento de um laser de centro de cor para aplicações em espectroscopia. O laser opera em regime CW e a cavidade óptica utilizada é do tipo X, com dois espelhos esféricos intracavidade astigmáticamente compensados. O meio ativo utilizado foi um cristal de KCl:Li+ com centros FA (II), e como fonte de bombeamento foi empregado um laser de Ar+ em 514nm. O limiar de potência de bombeamento foi de 120 mW, a eficiência energética foi de 2,8% e o intervalo de sintonia obtido vai de 2,56 a 2,82 &#956m numa potência de bombeamento de 700mW. O laser opera também com a cavidade na configuração anel. Para testar o LCC foram feitas aplicações empregando a técnica de espectroscopia intercavidade em cristais de KCl: Li+: NO-2: NO-3 e KBr:OH-. / The present work shows the development of a color Center laser for spectroscopy application. It is a CW laser which uses an X-type cavity with two astigmatically compensated intracavity spherical mirrors. The laser can be converted to a ring laser. The used active medium was a KCl:Li+ single crystal with a FA (II) centers and the pumping source was an Ar+ laser (&#955= 514nm, 700mW). Pump power at threshold was measured to be 120mW. The tuning range was 2.56&#60 &#955 &#60 2.82 &#956m and the slope efficiency was 2,8%. To test the color center laser we measured intracavity spectra of KCl: Li+: NO-2: NO-3 and KBr:OH- single crystals.

We report on the systematic characterization of the optical properties of diamond color centers based on Pb impurities. An ensemble photoluminescence analysis of their spectral emission was performed at different excitation wavelengths in the 405–520 nm range and at different temperatures in the 4–300 K range. The series of observed spectral features consist of different emission lines associated with Pb-related defects. Finally, a room-temperature investigation of single-photon emitters under 490.5 nm laser excitation is reported, revealing different spectral signatures with respect to those already reported under 514 nm excitation. This work represents a substantial progress with respect to previous studies on Pb-related color centers, both in the attribution of an articulated series of spectral features and in the understanding of the formation process of this type of defect, thus clarifying the potential of this system for high-impact applications in quantum technologies.

The advent of ultrafast lasers has enabled micromachining schemes that cannot be achieved by other current techniques. Laser direct writing has emerged as one of the possible routes for fabrication of optical waveguides in transparent materials. In this thesis, the advantages and limitations of this technique are explored. Two extended-cavity ultrafast lasers were built and characterized as the laser sources for this study, with improved performance over existing systems. Waveguides are fabricated in oxide glass, chalcogenide glass, and polymers, these being the three major classes of materials for the telecommunication industry. Standard waveguide metrology is performed on the fabricated waveguides, including refractive index profiling and mode analysis. Furthermore, a finite-difference beam propagation method for wave propagation in 3D-waveguides is proposed. The photo-structural modifications underlying the changes in the material optical properties after exposure are investigated. The highly nonlinear processes of the light/matter interaction during the writing process are described using a free electron model. UV/visible absorption spectroscopy, photoluminescence spectroscopy and Raman spectroscopy are used to assess the changes occurring at the atomic level. Finally, the impact of laser direct writing on nonlinear waveguide applications is discussed.

Im Rahmen der vorliegenden Dissertation wurden neuartige integrierte Einzelphotonenquellen (EPQ) und ihre Anwendung für die Quanteninformationsverarbeitung entwickelt und untersucht. Die Erzeugung von Einzelphotonen basiert auf einzelnen Defektzentren in nanometergroßen Diamantkristallen mit einzigartigen optischen Eigenschaften: Stabilität bei Zimmertemperatur ohne optisches Blinken. Diamantkristalle mit Größen bis unter 20nm wurden mit neuartigen „pick-and-place“ Techniken (z.B. mit einem Atomkraftmikroskop) in komplexe photonische Strukturen integriert. Zwei unterschiedliche Ansätze für die Realisierung der neuartigen EPQ wurden verfolgt. Beim ersten werden fluoreszierende Diamantkristalle in nano- und mikrometergroße Faser-basierte oder resonante Strukturen in einem „bottom-up“ Ansatz integriert, dadurch werden zusätzliche optische Komponenten überflüssig und das Gesamtsystem ultra-stabil und wartungsfrei. Der zweite Ansatz beruht auf einem Festkörperimmersionsmikroskop (FIM). Seine Festkörperimmersionslinse wirkt wie eine dielektrische Antenne für die Emission der Defektzentren. Es ermöglicht die höchsten bisher erreichten Photonenzählraten von Stickstoff-Fehlstellen von bis zu 2.4Mcts/s und Einsammeleffizienzen von bis zu 4.2%. Durch Anwendung des FIM bei cryogenen Temperaturen wurden neuartige Anwendungen und fundamentale Untersuchungen möglich, weil Photonenraten signifikant erhöht wurden. Die Bestimmung der spektralen Diffusionszeit eines einzelnen Defektzentrums (2.2µs) gab neue Erkenntnisse über die Ursachen von spektraler Diffusion. Spektrale Diffusion ist eine limitierende Eigenschaft für die Realisierung von Quanteninformationsanwendungen. Das Tisch-basierte FIM wurde außerdem als kompakte mobile EPQ mit Ausmaßen von nur 7x19x23cm^3 realisiert. Es wurde für ein Quantenkryptographie-Experiment implementiert, zum ersten Mal mit Siliziumdefektzentren. Des Weiteren wurde ein neues Konzept für die Erzeugung von infraroten EPQ entwickelt und realisiert. / The presented thesis covers the development and investigation of novel integrated single photon (SP) sources and their application for quantum information schemes. SP generation was based on single defect centers in diamond nanocrystals. Such defect centers offer unique optical properties as they are room temperature stable, non-blinking, and do not photo-bleach over time. The fluorescent nanocrystals are mechanically stable, their size down to 20nm enabled the development of novel nano-manipulation pick-and-place techniques, e.g., with an atomic force microscope, for integration into photonic structures. Two different approaches were pursued to realize novel SP sources. First, fluorescent diamond nanocrystals were integrated into nano- and micrometer scaled fiber devices and resonators, making them ultra-stable and maintenance free. Secondly, a solid immersion microscope (SIM) was developed. Its solid immersion lens acts as a dielectric antenna for the emission of defect centers, enabling the highest photon rates of up to 2.4Mcts/s and collection efficiencies of up to 4.2% from nitrogen vacancy defect centers achieved to date. Implementation of the SIM at cryogenic temperatures enabled novel applications and fundamental investigations due to increased photon rates. The determination of the spectral diffusion time of a single nitrogen vacancy defect center (2.2µs) gave new insights about the mechanisms causing spectral diffusion. Spectral diffusion is a limiting property for quantum information applications. The table-top SIM was integrated into a compact mobile SP system with dimension of only 7x19x23cm^3 while still maintaining record-high stable SP rates. This makes it interesting for various SP applications. First, a quantum key distribution scheme based on the BB84 protocol was implemented, for the first time also with silicon vacancy defect centers. Secondly, a conceptually novel scheme for the generation of infrared SPs was introduced and realized.