The nonlinear optical (NLO) properties were investigated in various extended　π-conjugated chromophores: cyanine and alkyne carbocations; porphyrin dimers; and squaraine compounds that possess electronic, double resonance, and vibronic based NLO properties. In summary: (i) It was demonstrated that the alkyne carbocations have very similar optical properties to traditional cyanine dyes. Our theoretical results establish that the alkyne carbocations, in spite of their significant degree of bond-length alternation, behave in the same way as cyanine dyes. (ii) The nature of the -bridge in porphyrin dimers tunes the electronic coupling strength, which in turn determines the splitting of the energy levels and the (non)linear optical properties. (iii) We have shown that the origin of the lowest TPA-active states in squaraines is dependent on the nature of substituent donor moiety, changing from predominantly electronic to vibronic in character. For all squaraines containing indolinylidenemethyl donors, a vibronic origin for the TPA peak, and the energy and lineshape of the experimentally observed lowest TPA peak in these compounds were confirmed.

The objective of this thesis was to develop novel technologies for measuring the physical characteristics of high-speed pulse trains, for use in performance monitoring applications. This thesis describes the development of three separate techniques that perform measurements in either the time domain, frequency domain or the phase space of the optical signal. The first section investigates phase-sensitive pulse measurement techniques. A high- resolution SHG-FROG apparatus was custom-designed to measure 40GHz RZ pulse trains, from which an operational characterisation of a Mach-Zehnder modulator (MZM) was realised. A numerical model of a nonlinear pulse compressor was developed to compress 40GHz RZ pulses from 8.5ps down to 3.4ps. These pulses were time-division multiplexed to 80GHz, and phase-retrievals of the 80GHz pulse trains were measured. A comparison between the techniques of SHG-FROG and linear spectrogram has been undertaken for 10GHz pulse sources, exposing SHG-FROG's weaknesses at this particular repetition rate. The second section investigates a simple, time-averaged, nonlinear detection technique. Two-photon absorption in a GaAs/InGaAs quantum-well laser diode was used to measure the duty cycle (and by extension, the pulse duration) of a range of pulse sources. This technique was further developed to measure the extinction ratio of NRZ pulse trains. Additionally, the pulse duration of a mode-locked laser source was measured using the nonlinear absorption in a 1-m length of As2Se3 Chalcogenide glass fiber. This demonstrates that the nonlinear properties of this glass may well find application in future instrumentation. The third section investigates the development of an ultra-high resolution swept heterodyne spectrometer. This spectrometer was used to spectrally-distinguish repetitive 8-bit NRZ patterns at 2.5Gbit/s. It was also used to measure the chirp parameter of an X-cut LiNbO3 MZM, revealing a chirp parameter of απ/2 < 0.1 across a modulation band- width of 250-2500MHz. Additionally, the distinctive CW spectrum of a DFB laser diode was measured. Analysis of the measured CW spectrum yielded a linewidth enhancement factor of α≃ 1.8 and also the relative intensity noise of the DFB laser diode.

The objective of this thesis was to develop novel technologies for measuring the physical characteristics of high-speed pulse trains, for use in performance monitoring applications. This thesis describes the development of three separate techniques that perform measurements in either the time domain, frequency domain or the phase space of the optical signal. The first section investigates phase-sensitive pulse measurement techniques. A high- resolution SHG-FROG apparatus was custom-designed to measure 40GHz RZ pulse trains, from which an operational characterisation of a Mach-Zehnder modulator (MZM) was realised. A numerical model of a nonlinear pulse compressor was developed to compress 40GHz RZ pulses from 8.5ps down to 3.4ps. These pulses were time-division multiplexed to 80GHz, and phase-retrievals of the 80GHz pulse trains were measured. A comparison between the techniques of SHG-FROG and linear spectrogram has been undertaken for 10GHz pulse sources, exposing SHG-FROG's weaknesses at this particular repetition rate. The second section investigates a simple, time-averaged, nonlinear detection technique. Two-photon absorption in a GaAs/InGaAs quantum-well laser diode was used to measure the duty cycle (and by extension, the pulse duration) of a range of pulse sources. This technique was further developed to measure the extinction ratio of NRZ pulse trains. Additionally, the pulse duration of a mode-locked laser source was measured using the nonlinear absorption in a 1-m length of As2Se3 Chalcogenide glass fiber. This demonstrates that the nonlinear properties of this glass may well find application in future instrumentation. The third section investigates the development of an ultra-high resolution swept heterodyne spectrometer. This spectrometer was used to spectrally-distinguish repetitive 8-bit NRZ patterns at 2.5Gbit/s. It was also used to measure the chirp parameter of an X-cut LiNbO3 MZM, revealing a chirp parameter of απ/2 < 0.1 across a modulation band- width of 250-2500MHz. Additionally, the distinctive CW spectrum of a DFB laser diode was measured. Analysis of the measured CW spectrum yielded a linewidth enhancement factor of α≃ 1.8 and also the relative intensity noise of the DFB laser diode.

The objective of this thesis was to develop novel technologies for measuring the physical characteristics of high-speed pulse trains, for use in performance monitoring applications. This thesis describes the development of three separate techniques that perform measurements in either the time domain, frequency domain or the phase space of the optical signal. The first section investigates phase-sensitive pulse measurement techniques. A high- resolution SHG-FROG apparatus was custom-designed to measure 40GHz RZ pulse trains, from which an operational characterisation of a Mach-Zehnder modulator (MZM) was realised. A numerical model of a nonlinear pulse compressor was developed to compress 40GHz RZ pulses from 8.5ps down to 3.4ps. These pulses were time-division multiplexed to 80GHz, and phase-retrievals of the 80GHz pulse trains were measured. A comparison between the techniques of SHG-FROG and linear spectrogram has been undertaken for 10GHz pulse sources, exposing SHG-FROG's weaknesses at this particular repetition rate. The second section investigates a simple, time-averaged, nonlinear detection technique. Two-photon absorption in a GaAs/InGaAs quantum-well laser diode was used to measure the duty cycle (and by extension, the pulse duration) of a range of pulse sources. This technique was further developed to measure the extinction ratio of NRZ pulse trains. Additionally, the pulse duration of a mode-locked laser source was measured using the nonlinear absorption in a 1-m length of As2Se3 Chalcogenide glass fiber. This demonstrates that the nonlinear properties of this glass may well find application in future instrumentation. The third section investigates the development of an ultra-high resolution swept heterodyne spectrometer. This spectrometer was used to spectrally-distinguish repetitive 8-bit NRZ patterns at 2.5Gbit/s. It was also used to measure the chirp parameter of an X-cut LiNbO3 MZM, revealing a chirp parameter of απ/2 < 0.1 across a modulation band- width of 250-2500MHz. Additionally, the distinctive CW spectrum of a DFB laser diode was measured. Analysis of the measured CW spectrum yielded a linewidth enhancement factor of α≃ 1.8 and also the relative intensity noise of the DFB laser diode.

The objective of this thesis was to develop novel technologies for measuring the physical characteristics of high-speed pulse trains, for use in performance monitoring applications. This thesis describes the development of three separate techniques that perform measurements in either the time domain, frequency domain or the phase space of the optical signal. The first section investigates phase-sensitive pulse measurement techniques. A high- resolution SHG-FROG apparatus was custom-designed to measure 40GHz RZ pulse trains, from which an operational characterisation of a Mach-Zehnder modulator (MZM) was realised. A numerical model of a nonlinear pulse compressor was developed to compress 40GHz RZ pulses from 8.5ps down to 3.4ps. These pulses were time-division multiplexed to 80GHz, and phase-retrievals of the 80GHz pulse trains were measured. A comparison between the techniques of SHG-FROG and linear spectrogram has been undertaken for 10GHz pulse sources, exposing SHG-FROG's weaknesses at this particular repetition rate. The second section investigates a simple, time-averaged, nonlinear detection technique. Two-photon absorption in a GaAs/InGaAs quantum-well laser diode was used to measure the duty cycle (and by extension, the pulse duration) of a range of pulse sources. This technique was further developed to measure the extinction ratio of NRZ pulse trains. Additionally, the pulse duration of a mode-locked laser source was measured using the nonlinear absorption in a 1-m length of As2Se3 Chalcogenide glass fiber. This demonstrates that the nonlinear properties of this glass may well find application in future instrumentation. The third section investigates the development of an ultra-high resolution swept heterodyne spectrometer. This spectrometer was used to spectrally-distinguish repetitive 8-bit NRZ patterns at 2.5Gbit/s. It was also used to measure the chirp parameter of an X-cut LiNbO3 MZM, revealing a chirp parameter of απ/2 < 0.1 across a modulation band- width of 250-2500MHz. Additionally, the distinctive CW spectrum of a DFB laser diode was measured. Analysis of the measured CW spectrum yielded a linewidth enhancement factor of α≃ 1.8 and also the relative intensity noise of the DFB laser diode.

The objective of this thesis was to develop novel technologies for measuring the physical characteristics of high-speed pulse trains, for use in performance monitoring applications. This thesis describes the development of three separate techniques that perform measurements in either the time domain, frequency domain or the phase space of the optical signal. The first section investigates phase-sensitive pulse measurement techniques. A high- resolution SHG-FROG apparatus was custom-designed to measure 40GHz RZ pulse trains, from which an operational characterisation of a Mach-Zehnder modulator (MZM) was realised. A numerical model of a nonlinear pulse compressor was developed to compress 40GHz RZ pulses from 8.5ps down to 3.4ps. These pulses were time-division multiplexed to 80GHz, and phase-retrievals of the 80GHz pulse trains were measured. A comparison between the techniques of SHG-FROG and linear spectrogram has been undertaken for 10GHz pulse sources, exposing SHG-FROG's weaknesses at this particular repetition rate. The second section investigates a simple, time-averaged, nonlinear detection technique. Two-photon absorption in a GaAs/InGaAs quantum-well laser diode was used to measure the duty cycle (and by extension, the pulse duration) of a range of pulse sources. This technique was further developed to measure the extinction ratio of NRZ pulse trains. Additionally, the pulse duration of a mode-locked laser source was measured using the nonlinear absorption in a 1-m length of As2Se3 Chalcogenide glass fiber. This demonstrates that the nonlinear properties of this glass may well find application in future instrumentation. The third section investigates the development of an ultra-high resolution swept heterodyne spectrometer. This spectrometer was used to spectrally-distinguish repetitive 8-bit NRZ patterns at 2.5Gbit/s. It was also used to measure the chirp parameter of an X-cut LiNbO3 MZM, revealing a chirp parameter of απ/2 < 0.1 across a modulation band- width of 250-2500MHz. Additionally, the distinctive CW spectrum of a DFB laser diode was measured. Analysis of the measured CW spectrum yielded a linewidth enhancement factor of α≃ 1.8 and also the relative intensity noise of the DFB laser diode.

Neste trabalho estudamos o processo de absorção de dois fótons em compostos azoaromáticos, abordando tanto aspectos fundamentais quanto aplicados. Moléculas azo-aromáticos têm recebido especial atenção nos últimos anos devido as suas potencias aplicações em dispositivos para armazenamento óptico de informação, modulação da luz e geração de relevos em superfície, processes estes associados ao mecanismo de foto isomerização. Os trabalhos apresentados nessa tese tiveram como principal foco explorar o fenômeno de absorção de dois fótons, utilizando a propriedade de foto-isomerização das moléculas azo-aromáticas. Nosso objetivo foi estudar as vantagens que podem ser obtidas pela utilização de pulsos intensos de luz, que interagem de maneira não linear com a matéria, para desenvolver aplicações utilizando compostos azo-aromáticos. Inicialmente, estudamos o processo de absorção de dois fótons em uma nova família de compostos azo-aromáticos, denominados Salen Dyes. Investigamos a influencia da presença de íons metálicos no processo de absorção de dois fótons dessas moléculas. Nossos resultados mostraram que, devido a ausência de conjugação entre as estruturas azo-aromáticas conectadas pelo metal, este tem pouca influência no processo não linear estudado. Pelo uso de um modelo de soma de estado para a seção de choque de absorção de dois fótons, fomos capazes de determinar os momentos de dipolo de transição destas moléculas. Em seguida, implementamos uma técnica para estudar o processo de armazenamento óptico, induzido através da orientação molecular dos compostos azo-aromáticos, via absorção de dois fótons. Observamos que de fato é possível se observar birrefringência induzida por dois fótons nestas moléculas, a qual esta confinada ao volume focal, conforme demonstrado pela obtenção de armazenamento tri-dimensional. Finalmente, exploramos o processo de controle coerente via formatação de pulsos ultra-curtos para manipular o processo de birrefringência induzida por dois fótons em compostos azo-aromáticos. Foi demonstrado que apenas a através da manipulação da fase do pulso ultra-curto, é possível modular a birrefringência induzida em filmes de compostos azo-aromáticos. / Here we investigated fundamental and applied aspects of the two-photon absorption process in azoaromatic compounds. Azoaromatic molecules have been studied in the last few years due to their applications in optical storage devices, light modulators and surface relief gratings, processes related to the photo-isomerization mechanism. The main focus of the results presented in this thesis was to explore the two-photon absorption process, taking advantage of the intrinsic photo-isomerization of the azo-aromatic chromophores. Our main goal was to study the advantages of utilizing intense pulses, which promote nonlinear excitation, to develop application with azo-aromatic compounds. Initially, we studied the two-photon absorption process in a new class of azo-aromatic compounds, named Salen Dyes. We investigated the influence of metal ions, presented in the Salen Dyes structure, on the two-photon absorption spectrum. Our results revealed that the metals have practically no influence in the nonlinear optical properties due to the lack of conjugation between the azo-moieties in the Salen Dyes. Through a theoretical model based on a sum-over-states calculation, we were able to determine the transition dipole moment of these molecules. Subsquently, we implememnted a technique to study the two-photon induced birefringence, resulting from the molecular re-orientation, in azo-aromatic compounds. We observed that the two-photon induced birefringence is confined to the focal volume, s demonstrated in a three dimensional optical storage experiment. Finally, we used coherent control processes to manipulate the two-photon induced birefringence in azo-compounds. It was demonstrated that it is possible to modulate the optically induced birefringence by manipulating the phase of the ultra-short pulses, via pulse shaping techniques.

Neste trabalho estudamos a forma de linha na absorção de dois fotons nas transições 4f7 de defeitos cristalinos superpostas com bandas de absorção multifonons. Escrevemos o perfil de linha sob a forma de Fano. O íon em estudo é Eu++ como defeito em um cristal de CaF2. Apresentamos o desenvolvimento da instrumentação necessária para realização do experimento, e obtemos resultados de ótima qualidade. / In this work we study the absorption of two photons in the electronic transition within the 4f 7configuration wich is superposed to the vibronic structure of 4f 7 - 4f65d transition. We describe the line shape with the Fano\'s formalism. The study was carried out on Eu+2 doped CaF2. The experimental apparatus was build and the results obtained are in good agreement with the theoretical predictions.

Neste trabalho apresentamos resultados de birrefringência opticamente induzida via absorção de um e dois fótons em filmes casting de poli (metil metacrilato) (PMMA), contendo uma nova série de compostos azoaromáticos chamados de corantes Salen, os quais podem ser usados em aplicações de memória óptica. Para a birrefringência opticamente induzida por um fóton, foi necessário um tempo de escrita maior para os compostos com metal na estrutura em comparação com o composto Salen que não contém metal, provavelmente devido a agregações do grupo azoaromático na estrutura do polímero diminuindo a mobilidade molecular. Além disso, como uma novidade em memórias ópticas deste tipo, birrefringência opticamente induzida por dois fótons pôde ser realizada nos filmes de Salen, o que pode permitir sua aplicação em memória óptica tridimensional. / In this work we present the one- and two-photon optically induced birefringence in cast films of amorphous poly(methyl methacrylate) (PMMA), containing a new series of organometallic azoaromatic compounds, referred to as Salen dyes, which may be used in optical storage applications. For the one-photon optically induced birefringence, longer writing times were required for the organometallic compounds in comparison with the nonmetal one, probably due to the higher degree of aggregation in the azoaromatic moieties that precludes molecular orientation. Furthermore, as a novelty concerning optical storage, two-photon optically induced birefringence could be achieved in the Salen dyes guest-host films, which allows their application in three-dimensional optical memories.

Submitted by Mario BC (mario@bc.ufrpe.br) on 2016-12-07T12:55:23Z No. of bitstreams: 1 Geimson Ayrcton dos Santos.pdf: 2542495 bytes, checksum: c8980a31079b32fd9ab6810390ce0a4d (MD5) / Made available in DSpace on 2016-12-07T12:55:23Z (GMT). No. of bitstreams: 1 Geimson Ayrcton dos Santos.pdf: 2542495 bytes, checksum: c8980a31079b32fd9ab6810390ce0a4d (MD5) Previous issue date: 2016-08-30 / Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPES / In this work we study a resonant fluorescence signal generated by two-photon absorption in rubidium vapor, when the atomic system interacts with a continuous wave laser from a diode laser beam and one ultrashort pulse train from a femtosecond Ti:sapphire laser, in the ladder transition 5S1/2 -> 5P3/2 -> 5D5/2. The atoms contained in a closed and heated cells interact with the pair of laser beams in a co-propagating con guration. The laser beams have wavelengths of about 780 nm and linear and parallel polarization. We analyze the fluorescence signal detected forward, in the same direction of the incidence laser beams, as well as in the direction perpendicular to lasers ( fluorescence at 90º). We analyze the fluorescence signal at 421 nm generated by the spontaneous decay of the excited state 6P3/2 to the ground state 5S1/2 of rubidium, as a function of the many parameters of the system, such as: the signal polarization with respect to the polarization of the laser beams, the frequency and the intensity of the diode laser, and the atomic density of the sample. We observed saturation e ects on the fluorescence detected signal varying the intensity of the laser diode and the atomic density. E ects of an optical pumping from the diode laser beam on the fluorescence signal were observed and explained with a simple theoretical model. / Neste trabalho estudamos um sinal de fluorescência ressonante por dois fótons em vapor de rubídio ao interagir com um feixe de laser de diodo e com um laser de Ti:sa ra de femtossegundos na transição em cascata 5S1/2 -> 5P3/2 -> 5D5/2. Os átomos contidos em uma célula fechada e aquecida interagem com os feixes de lasers na configuração copropagante, tendo comprimentos de onda em torno de 780 nm e polarizações lineares e paralelas entre si. Analisamos o sinal de fluorescência detectado para frente, na direção de incidência dos lasers, bem como na direção perpendicular aos lasers (fluorescência a 90º ). Analisamos o sinal de fluorescência no comprimento de onda 421 nm devido ao decaimento espontâneo do estado excitado 6P3/2 para o estado fundamental 5S1/2, em função de vários parâmetros do sistema, como a polarização do sinal em relação a polarização dos lasers, em função da frequência de varredura do laser de diodo e em função da densidade atômica da amostra. Observamos efeitos de saturação no sinal de fluorescência variando-se a intensidade do laser de diodo e a densidade atômica. Efeitos de bombeio óptico do laser de diodo no sinal de fluorescência detectado também foram observados e explicados com um modelo teórico simples.