L'objet de cette thèse porte sur la conception et la réalisation de deux sources laser non linéaires accordables dans les domaines IR et UV, pour le raccordement de la sensibilité spectrale des détecteurs au moyen du radiomètre cryogénique du laboratoire commun de métrologie (LCM). La source IR est un oscillateur paramétrique optique (OPO) résonant sur les ondes pompe et signal (PRSRO), utilisant un cristal de niobate de lithium à inversion de domaines de polarisation dopé par 5% d'oxyde de magnésium (ppMgCLN). Pompé par un laser Ti:Al2O3 en anneau mono-fréquence et accordable, délivrant 500 mW de puissance utile autour de 795 nm, l'OPO possède un seuil d'oscillation de 110 mW. Une couverture spectrale continue entre 1 µm et 3.5 µm a été obtenue, avec des puissances de l'ordre du mW pour l'onde signal (1 µm à 1.5 µm) et des puissances comprises entre $20$ à $50$ mW pour l'onde complémentaire couvrant un octave de longueur d'onde IR entre 1.7 µm et 3.5 µm. La source UV est obtenue par doublage de fréquence en cavité externe du laser Ti:Al2O3, dans un cristal de triborate de lithium (LiB3O5). Un accord de phase en température à angle d'accord de phase fixé permet l'obtention d'une couverture spectrale comprise entre 390 nm et 405 nm. L'asservissement de la cavité de doublage sur la fréquence du laser Ti:Al2O3 par la méthode de Pound-Drever-Hall, ainsi qu'une adaptation de mode optimale, permet d'obtenir une puissance de 5.64 mW à 400 nm à partir de 480 mW de puissance fondamentale. / The work presented in this PhD dissertation details the strategy adopted to build two non-linear laser sources that are widely in the mid-infrared and blue-UV spectral ranges. These laser sources are needed for the traceability to SI units of coherent light irradiance measurements using a cryogenic radiometer of the using cryogenic radiometer of the Laboratoire commun de métrologie (LCM) .The infrared laser source is an optical parametric oscillator (OPO) resonating on the pump and signal wavelengths (PRSRO) and employing a periodically poled Lithium Niobate non-linear crystal doped with 5% magnesium oxide (ppMgCLN). The PRSRO is pumped by a single-frequency tunable bow-tie ring cavity Titanium-Sapphire laser (Ti:Al2O3) delivering 500 mW output power at 795 nm wavelength, , resulting in a power oscillation threshold of 110 mW. The PRSRO emission could continuously cover the spectral range from 1 µm to 3.5 µm. The level of output power achieved is of the order of 1 mW for the signal wave (1 µm to 1.5 µm) and between 20 mW and 50 mW for idler wave spanning an octave wavelength range (1.7 µm to 3.5 µm).The UV source based on the second harmonic generation on the Titanium-Sapphire tunable laser using an external enhancement cavity containing a critically phase-matched LBO non linear crystal (LiB3O5). Temperature-tuning of the phase-matching condition at a fixed crystal orientation leads to a wide tunability from 390 nm to 405 nm wavelength. The external cavity optical pathlength was actively locked to the laser frequency using a¨Pound-Drever-Hall servo, allowing to extract up to 6 mW power at 400 nm wavelength with a 480 mW pump power. Despite a perfect mode-matching efficiency, the power performance was limited by the poor nonlinear impedance matching of the resonator, due to both the weak nonlinearity of the crystal and the low incoming laser power.

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior / In this work we present the results of L-asparagine H2O crystal growth and the study of their optical properties, linear and nonlinear, of crystal as grown and after being submitted to high doses of X-ray. Crystals were grown in aqueous solution by the method of slow evaporation of the solvent. Measurements optical absorption, Raman, thermal analysis and efficiency of second harmonic generation were carried out. The results demonstrate the good optical quality of the crystals for use in optical devices, comparable to that of KDP (KH2PO4). . / Neste trabalho apresentamos os resultados do crescimento de cristais de L-Asparagina-H2O e do estudo de suas propriedades ópticas, lineares e não lineares, do cristal como é crescido e após ser submetido a altas doses de raios-X. Os cristais foram crescidos em solução aquosa pelo método de evaporação lenta do solvente. Foram realizadas medidas de absorção óptica, Raman, análise térmica e eficiências de geração de segundo harmônico. Os resultados demonstram as boas qualidades ópticas dos cristais para aplicação em dispositivos ópticos, comparáveis ao do KDP (KH2PO4).

Coordenação de Aperfeiçoamento de Pessoal de Nível Superior - CAPES / In this work, we investigated the phenomenon of second harmonic generation in hydrazone compounds. Based on optical absorption measurements, we determined the energy bands corresponding to the first excited state and the energy gap of the compound. Using the X-ray powder diffraction method, we verified the crystalline nature of the samples. The process of second harmonic generation exhibited by these compounds was characterized by the Kurtz and Perry powder method. We noted that these materials have good efficiency at second harmonic generation, being comparable to KDP. The results indicate that these are promising compounds for the development of photonic applications based on second-order nonlinear optical effects. / No presente trabalho, investigamos o fenômeno de geração de segundo harmônico em compostos hidrazônicos. A partir de medidas de absorção ´optica, determinamos as bandas de energia correspondentes aos primeiros estados excitados e a energia do gap dos compostos. Usando a difra¸c˜ao de raio-X m´etodo do p´o, verificamos a natureza cristalina das amostras estudadas. O processo de gera¸c˜ao de segundo harmˆonico exibidos por esses compostos foi caracterizado pelo m´etodo do p´o de Kurtz e Perry. Observamos que esses materiais apresentam boa eficiˆencia de gera¸c˜ao de segundo harmˆonico compar´aveis ao KDP. Os resultados obtidos indicam que esses compostos s˜ao promissores para o desenvolvimento de aplica¸c˜oes fotˆonicas baseado em efeitos ´opticos n˜ao lineares de segunda ordem.

La technique de la génération de second harmonique (SHG) a été employée pour étudier la réponse non linéaire des assemblées de nano particules métalliques aux interfaces liquides. Les nanoparticules ont d’abord été caractérisées en utilisant la génération de second harmonique incohérente, également nommée diffusion hyper Rayleigh. L’étude de particules d’or et d’argent, nanosphères et des nanobâtonnets, ont permis de mettre en évidence l’influence de la couche protectrice de surfactants sur l’hyperpolarisabilité quadratique de ces particules. Ces particules ont ensuite été placées à l’interface air/eau dans une cuve de Langmuir afin d’étudier le rôle des interactions entre les particules sur la réponse optique linéaire et non linéaire. Celle-ci a révélé dans ces films formés à l’interface la présence de couplages forts entre les particules lors de la compression de la surface. Cela conduit à une transition dans le film une fois que la distance entre les particules passe en dessous d’une distance critique. Ces études ont été complétées par des expériences réalisées à l'interface liquide/liquide et sur une électrode de carbone vitreux pour examiner plus en détail le rôle de la rugosité à l’échelle nanométrique dans l’exaltation de la réponse non linéaire SHG / In this work, the nonlinear optical response of assembled metallic nanoparticles at interfaces was studied using Second Harmonic Generation. First, the nanoparticles were characterised using incoherent second harmonic generation, a technique also called Hyper Rayleigh Scattering. Thioalkane-capped silver and gold nanoparticles, both nanospheres and nanorods, were investigated and the role of this capping layer on the quadratic hyperpolarisability of these particles was underlined. The particles were then deposited at the air/liquid interface in a Langmuir trough to investigate the role of the interparticles interactions in large assemblies. Both the linear and the nonlinear optical response of these metallic films formed at the surface of the trough provided evidence of a strong coupling between adjacent particles upon compression leading to a phase transition of the film once the interparticle distance is less than a critical value. These studies were complemented with experiments performed at the liquid/liquid interface and at the glassy carbon/electrolyte interface to examine in greater details the role of roughness at the nanoscale on the enhancement of the SHG response

Le manuscrit présente une étude de la réponse optique non linéaire quadratique et cubique de nano-structures métalliques d'or déposées sur substrat. Le travail s'inscrit plus généralement dans le domaine de la plasmonique non linéaire et vise à mieux comprendre l'interaction entre les nanostructures et la lumière, dans un régime d'intensités incidentes fortes, lorsque la réponse n'est plus linéaire. Les exaltations des champs électromagnétiques locaux dans ces structures par les résonances de plasmon de surface, excitations collectives des électrons de conduction, favorisent en effet considérablement ces processus. Dans le cadre de la réponse quadratique, l'étude a essentiellement porté sur le processus appelé génération de second harmonique (SHG, acronyme pour Second Harmonic Generation) par lequel deux photons incidents à la fréquence fondamentale sont convertis en un photon à la fréquence harmonique double. Ce processus est fortement dépendant de la morphologie des nanostructures métalliques. Pour la réponse cubique, l'étude a porté sur les effets Kerr optiques qui décrivent la variation de l'indice optique des nanostructures avec l'intensité de l'onde incidente. Une attention toute particulière a été donnée aux conditions géométriques d'éclairement effectué avec une grande ouverture numérique. Le champ électromagnétique incident ne doit en effet plus être considéré dans l'approximation paraxiale / The manuscript reports a study about the quadratic and cubic nonlinear optical response from gold metallic nanostructures which are deposited onto substrates. The field of this work is more commonly known as nonlinear plasmonics and it consists in trying to understand the interaction between nanostructures and light, in a regime of high incident intensities when the response is no longer linear. The local electromagnetic field enhancement in these structures due to the surface plasmon resonance, the latters being collectives excitations of the conduction band electrons, increase drastically the cross-section for these processes. In the context of a quadratic response, the study has been focused on the Second Harmonic Generation (SHG) process whereby two incident photons at the fundamental wavelength are converted into one photon at twice the harmonic frequency. This process is highly dependent to the metallic nanostructures morphology. For the cubic response, the study has been focused on the optical Kerr effect which describes the optical index variation of nanostructure with the intensity of the incident wave.Specifics considerations have been taken into account about the geometrical illumination conditions which are performed with a large numerical aperture. The electromagnetic incident field cannot be anymore considered within the paraxial approximation

Ces travaux de thèse portent sur l’étude de différents phénomènes non-linéaires ayantlieu dans le domaine térahertz (THz) au sein de cristaux de structure zinc-blende.En premier lieu, nous avons mis en place au laboratoire deux sources de rayonnementTHz intense, aux caractéristiques temporelles et spectrales bien distinctes. La premièrerepose sur le redressement optique d’une impulsion laser de durée femtoseconde dansun cristal de niobate de lithium, et la seconde est, quant à elle, basée sur la créationd’un plasma par focalisation d’un champ optique compos´e de l’impulsion fondamentalede pompe et de son second harmonique. Ces deux sources permettent de générer desondes THz dont l’amplitude est bien adaptée à la mise en oeuvre d’expériences d’optiquenon-linéaire.Nous avons ensuite caractérisé le comportement non-linéaire de cristaux de structurezinc-blende soumis à des champs THz intenses. Nous nous sommes ainsi intéressés àl’effet Pockels lors de l’interaction d’une impulsion THz intense et d’un champ optiquede faible intensité, dit sonde, au sein du matériau. Ceci nous a conduits à démontrerexpérimentalement et numériquement la possibilité de caractériser la phase spectrale del’impulsion sonde, à l’aide d’une technique équivalente au X-FROG. Nous avons égalementidentifié l’existence d’un processus non-linéaire dit de cascade, consistant en la générationde second harmonique induite par effet Pockels. Enfin, nous avons observé expérimentalementl’apparition d’un effet Kerr THz dans le cristal, nous permettant de déduire unevaleur moyenne de la susceptibilité non-linéaire du troisième ordre de ce matériau, `a l’aidede calculs théoriques et de simulations numériques. / This thesis project aims to study different non-linear processes in zinc-blende crystals,which take place in the terahertz (THz) range.First of all, two different light sources have been built in the laboratory, allowing us togenerate intense THz radiations with different temporal and spectral characteristics. Thefirst source is based on the optical rectification of a femtosecond laser pulse in a lithiumniobate crystal using the tilted pulse front technique, while the second one is based on aplasma, created through the focalization of a two-color femtosecond laser field. These twoTHz sources reach very high amplitudes, which allows us to study non-linear phenomenain the THz range.Among these, we have measured the non-linear behavior of zinc-blende crystals underintense THz radiation. We were particularly interested in the Pockels effect happeningduring the interaction of an intense THz field and a weak optical probe beam. This droveus to the experimental and numerical demonstration of a new method to characterize thespectral phase of the optical probe field. This method is equivalent to the X-FROG technique.We also identified a new non-linear phenomenon, consisting of the cascade of twosecond-order processes, namely the Pockels effect and the Second Harmonic Generation.Finally, we experimentally observed some THz Kerr effect in a gallium phosphide crystal,which allowed us to calculate an average value of its third-order non-linear susceptibility,thanks to theoretical considerations and simulations.

Orientador: Carlos Lenz Cesar / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-08-22T08:41:16Z (GMT). No. of bitstreams: 1 Thomaz_AndreAlexandrede_D.pdf: 9291787 bytes, checksum: 9554ec1cfb5b3952506ff59b61aec5f9 (MD5) Previous issue date: 2013 / Resumo: A comunidade científica concorda que há grandes chances que a próxima revolução tecnológica virá do controle dos processos biológicos. Grandes mudanças são esperadas, desde como produzimos alimentos até como combatemos as doenças. O controle dos processos biológicos nos permitirá produzir carne sintética para alimentação, produzir biocombustíveis retirando CO2 da atmosfera, produzir órgãos inteiros para transplante e combater de forma eficiente doenças como câncer, por exemplo. Está claro para o nosso grupo que para se obter esses resultados é necessário entender a biologia na sua unidade mais básica: a célula. A partir do entendimento e domínio das reações químicas que acontecem dentro da célula, e mais especificamente do controle do DNA, é que vamos conseguir atingir essas previsões e revolucionar a maneira como vivemos hoje. Com esse pensamento em mente, o objetivo dessa tese foi desenvolver uma plataforma fotônica integrada para estudos de processos celulares. Nós acreditamos que as ferramentas fotônicas são as ferramentas que preenchem todos os requisitos para os estudos de processos celulares, pois possibilitam o acompanhamento dos processos em tempo real sem causar dano as células. As técnicas presentes são: fluorescência excitada por 1 ou 2 fotons, geração de segundo ou terceiro harmônico, pinças ópticas, imagem por tempo de vida da fluorescência e "fluorescence correlation spectroscopy" (FCS). Nesta tese demonstramos como montar essa plataforma integrada e mostramos sua versatilidade com resultados em várias áreas da biologia e também para o estudo de quantum dots. / Abstract: The scientific community believes there is a great chance that the next technological revolution is coming from the control of biological processes. Great changes are expected, from the way we produce food up to the way we fight diseases. The control of biological processes will allow us to produce synthetic meat as food, to produce biofuels extracting CO2 directly from the atmosphere, to produce whole synthetic organs for transplant and to fight diseases, like cancer, in more efficient ways. It is clear to our group that in order to obtain these results it is necessary to understand biology from its most basic unity: the cell. Only from understanding and controlling chemical reactions inside a cell, and more specifically from the DNA controlling, it will be possible to achieve these predictions and cause a revolution in the way we live nowadays. Bearing these thoughts in mind, the objective of this thesis was to develop an integrated photonic platform for study of cellular processes. We believe that photonic tools are the only tools that fulfill all the requeriments for studies of cellular processes because they are capable to follow processes in real time without any damage to the cells. The techniques integrated are: 1 or 2 photon excited fluorescence, second or third harmonic generation, optical tweezers, fluorescence lifetime imaging and fluorescence correlation spectroscopy. In this thesis we demonstraded how to assemble this integrated plataform and we showed its versatility with results from different areas of biology and quantum dots. / Doutorado / Física / Doutor em Ciências

[pt] É possível criar uma não-linearidade de segunda ordem em amostras de sílica a partir do processo de polarização. Essas amostras vítreas com o X(2) induzido potencialmente podem ser utilizadas na fabricação de componentes como moduladores ópticos e dobradores de freqüência. O processo de polarização eletrotérmica utiliza alta tensão e alta temperatura e forma uma região de depleção de íons (camada de depleção) onde um campo elétrico intenso é gravado de forma permanente dentro da amostra. Neste trabalho, foram utilizadas diferentes técnicas de caracterização para medir a extensão dessa camada e os resultados foram comparados. As técnicas escolhidas foram: Ataque Químico Interferométrico (com ácido fluorídrico), Maker Fringe, Microscopia Óptica e de Força Atômica e Ataque Interferométrico com Medida de Segundo Harmônico em Tempo Real. Além disso, foram feitos alguns estudos paralelos visando à otimização e a reprodutibilidade do processo de polarização. Foram realizadas dessa forma análises sobre o material dos eletrodos utilizados e sobre a influência da condição inicial da superfície da amostra antes da polarização. / [en] It is possible to create a second order non linearity in silica samples with the poling process. The glass samples with an induced X(2) have a potential application on the fabrication of optical devices such as modulators and frequency converters. In the electrothermal poling process, high voltage and high temperature are applied to the samples forming an ion depleted region (depletion layer), where an intense electric field is permanently recorded. In this work, several characterization techniques have been utilized to measure the width of the depletion layer and compared the obtained results. The chosen techniques were: Interferometric Etching, Maker Fringe, Optical and Atomic Force Microscopy and the Interferometric Etching with Real Time Second Harmonic Measurement. In addition to this, we performed other studies aiming the optimization and reproducibility of the poling process. In this way, we analyzed the material used for the electrodes and the influence of the initial condition of the sample surface before poling.

Orientador: Carlos Lenz César / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Física Gleb Wataghin / Made available in DSpace on 2018-09-01T03:43:43Z (GMT). No. of bitstreams: 1 Pelegati_VitorBianchin_D.pdf: 6822381 bytes, checksum: 86749ce34dc184aeb7ed4b4ee47d70b3 (MD5) Previous issue date: 2016 / Resumo: Técnicas de microscopias ópticas são as principais ferramentas capazes de observar células e tecidos biológicos em tempo real e com mínimo dano. Essa área foi revolucionada recentemente através das microscopias confocais de varredura a laser e as microscopias de óptica não linear, naturalmente confocais. Entre os processos não lineares temos, a fluorescência excitada por dois ou mais fótons, geração de segundo harmônico [Second Harmonic Generation - SHG] e terceiro harmônico [Third Harmonic Generation - THG]. SHG e THG são técnicas de óptica não linear coerentes, não necessitam de marcadores exógenos e permitem reconstrução de imagens em três dimensões com resolução espacial subcelular. As técnicas de fluorescência permitem visualizar estruturas específicas no espaço, mas não permitem discriminar as substâncias químicas nas estruturas celulares, e as técnicas de SHG e THG não possuem especificidade química. Espectroscopia Raman possui especificidade química através das propriedades vibracionais das moléculas e pode ser usada como mecanismo de contraste na aquisição de imagens. Comparada com a espectroscopia/microscopia infravermelho, a microscopia Raman traz a informação das vibrações moleculares do infravermelho para o visível, eliminando os problemas da baixa resolução espacial e opacidade das amostras. Entretanto a baixa sensibilidade dessa técnica implica em tempos de aquisição de imagens muito longos, da ordem de horas, inviabilizando acompanhar a dinâmica de processos celulares em tempo real. Como solução para essa baixa sensibilidade do espalhamento Raman espontâneo, surgiu a microscopia por espalhamento Raman Coerente anti-Stokes [Coherent Anti-Stokes Raman Scattering - CARS]. Comparado com Raman espontâneo, a microscopia CARS representa aumento de 4 a 5 ordens de grandeza na sensitividade da técnica, diminuindo os tempos de aquisição ao ponto de viabilizar a aquisição em taxas de vídeos (mais rápido do que 30 quadros por segundo) e estudos em tempo real. Essa tese é dedicada ao estudo experimental e teórico, assim como de algumas aplicações, das técnicas de óptica não linear, com destaque para processos de óptica não linear coerentes. Apresentamos de forma detalhada três sistemas experimentais para a aquisição de imagens de Raman coerente e um sistema integrado com várias técnicas de óptica não linear. Mostramos as primeiras imagens de CARS realizadas no Brasil. Além do CARS convencional, trabalhamos com outra técnica de CARS de ordem mais alta, o CARS cascata [cascade CARS - CCARS], e, no melhor do nosso conhecimento, apresentamos as primeiras imagens internacionais obtidas com essa metodologia. CCARS aumenta o contraste da técnica CARS, diminuindo o fundo não ressonante, um problema que aflige a comunidade científica dedicada ao uso dessa técnica. Além da diminuição do fundo não ressonante, a emissão do CCARS acontece em um comprimento de onda diferente de qualquer outro efeito não linear coerente, significando um acréscimo de complexidade mínimo para sua detecção quando comparado com o CARS. Por último mostramos algumas aplicações realizadas com o sistema experimental desenvolvido para integrar diversas modalidades ópticas em paralelo, especialmente da geração de harmônicos com a fluorescência excitada por dois fótons e suas variantes, como microscopia de tempo de vida de fluorescência (Fluorescence Lifetime Imaging ¿ FLIM) / Abstract: Optical microscopies techniques are the main tools capable of observing cell and biological tissues in real time and with minimum damage. This area have recently been revolutionized by confocal laser scanning microscopies and non-linear microscopies, naturally confocal. Among the non-linear process we have, the two or more photons excited fluorescence, second harmonic generation [SHG] and third harmonic generation [THG]. SHG and THG are coherent nonlinear techniques, they do not require exogenous markers and allow three dimension imaging reconstruction with subcellular resolution. The fluorescence techniques allow visualizing specific structures in space, but do not allow discriminating the chemical substances in cellular structures, SHG and THG techniques do not have chemical specificity. Raman spectroscopy has chemical specificity through the vibrational properties of the molecules and can be used as a contrast mechanism for imaging acquisition. Compared to infrared spectroscopy/microscopy, Raman microscopy brings information about molecular vibration from infrared to visible, eliminating the low resolution and sample opacity problems. However, this technique low sensibility implies in very long imaging acquisition times, order of hours, making it not viable for following cellular process dynamics in real time. As an answer for the spontaneous Raman scattering low sensibility, the coherent anti-Stokes Raman scattering [CARS] emerged. Compared to spontaneous Raman, CARS microscopy presents an increase of 4 to 5 orders of magnitude in the sensitivity of the technique, lowering the acquisition times to the point of making video acquisition (faster than 30 frames per second) and real time studies possible. This thesis is dedicated to the experimental and theoretical study, as well as some applications, of the non-linear techniques, with emphasis on coherent non-linear optical processes. We present in detailed form three experimental systems for the acquisition of coherent Raman images, and a system with the integration of various non-linear techniques. We show the first CARS images acquired in Brazil. In addition to conventional CARS, we worked with other higher order CARS technique, the cascade CARS [CCARS], and, in the best of our knowledge, we present the first international image acquired with this methodology. CCARS increases the contrast from CARS technique, decreasing the non-resonant background, a problem that afflicts the scientific community dedicated to the use of this technique. Besides the decrease of the non-resonant background, the CCARS emission occurs in a different wavelength from any other non-linear coherent effect, meaning a minimum complexity increase for its detection when compared with CARS. Finally we show some applications performed with the experimental system developed to integrate several optical modalities in parallel, especially the generation of harmonics with two photons excitation fluorescence and their variants such as Fluorescence Lifetime Imaging [FLIM] / Doutorado / Física / Doutor em Ciências / 830406/2010 / CAPES

L'existence de différentes phases, polymorphes, sels, solvates et co-cristaux génère de nombreuses questions concernant la caractérisation des matériaux à l'état solide, en particulier pour l'industrie pharmaceutique. Les problématiques relatives à l'identification des phases et à la surveillance des processus de crist(allisation et de transitions de phase ne peuvent toutefois pas toujours être résolues à l'aide de techniques d'analyse conventionnelles. Dans ce travail, nous développons une approche analytique basée sur le phénomène d'optique non-linéaire de génération de seconde harmonique (GSH). La GSH est une technique sensible et précise pour détecter l'absence de centre d'inversion au sein d'une structure cristalline et pour suivre des modifications subtiles de symétrie. A travers plusieurs exemples, nous montrons comment les mesures de GSH résolues en température (TR-SHG) peuvent être utilisées pour étudier les diagrammes de phases et pour suivre les mécanismes et cinétiques des transitions de phase, y compris pour des transitions de type ordre-désordre. La combinaison de la TR-SHG avec les techniques classiques (XRPD, DSC et microscopie) permet ainsi de démontrer l'utilité et le potentiel de l'optique non-linéaire dans la caractérisation des propriétés physico-chimiques des matériaux. / The existence of different phases, including polymorphs, salts, solvates and co-crystals generates concerns in the characterization of solid-state materials, especially for the pharmaceutical industry. Issues related to the identification of phases and the monitoring of phase transitions and crystallisation processes cannot be always solved using conventionnal techniques. In this work, a complementary analytical approach based on the nonlinear optical phenomena of second harmonic generation (SHG) is developed. SHG is a sensitive and accurate technique to detect the absence of inversion center in the crystalline structure and to capture subtle symmetry changes. Herein, through several examples we show how Temperature-Resolved SHG (TR-SHG) measurements van be used to study phase diagrams and for tracking mechanisms and kinetics of phase transitions including order-disorder phase transitions. The combination of TR-SHG with classical techniques (XRPD, DSC and microscopy) reveals in this study the usefulness and the potentials of nonlinear optics in material characterization.