Cette thèse s’intéresse à une technique de caractérisation particulièrement bien adaptée à l’étude de couches diélectriques ultra-minces sur semiconducteurs. La génération de seconde harmonique (SHG) est une méthode très prometteuse, basée sur l’optique non-linéaire. Un laser est focalisé sur l'échantillon à caractériser et le signal à deux fois la fréquence fondamentale est mesuré. Pour les matériaux centrosymétriques comme c-Si, SiO2 et Al2O3, le signal SHG est dû aux défauts et au champ électrique Edc d’interface (induit par les charges préexistantes Qox et/ou piégées au niveau des pièges d’interface Dit). La SHG donne ainsi accès à la qualité des interfaces entre diélectriques/semiconducteurs. Néanmoins, le signal SHG dépend aussi des phénomènes de propagation optique dans les structures multicouches. Pour cette raison, nous avons développé un programme de simulation qui prend en compte les phénomènes optiques et les champs électriques statiques aux interfaces. Nous avons utilisé la SHG pour analyser la qualité de passivation de structures Al2O3/Si préparées avec des procédés différents et nous avons montré une corrélation entre SHG et mesure de durée de vie des porteurs de charges. Les valeurs de Qox et Dit ont été extraites par des mesures de capacité-tension et elles ont permis de calculer le champ Edc. La simulation optique, avec les valeurs extraites de Edc a permis de reproduire les données expérimentales de SHG dans ces structures. La SHG a été utilisée également pour la caractérisation des substrats Silicium-sur-Isolant (SOI). Pour les structures SOI épaisses, la simulation et les résultats expérimentaux ont montré que la réponse SHG est dominée par les interférences optiques (faible impact de Edc). Pour les structures SOI ultraminces, les interfaces sont couplées électriquement et des valeurs de Edc sont nécessaires pour reproduire les données expérimentales par simulation. Cela implique que pour les SOI ultraminces, la SHG pourrait donner accès aux champs électriques au niveau des interfaces d’une manière non-destructive. / This PhD work was developed in the context of research for novel characterization methods for ultra-thin dielectric films on semiconductors and their interfacial quality. Second harmonic generation (SHG) is a very promising non-invasive technique based on nonlinear optics. A laser emitting at the fundamental frequency is incident upon the sample which responds through its 2nd order polarization, generating a signal at twice the fundamental frequency. For centrosymmetric materials such as c-Si, amorphous SiO2 or Al2O3, the SHG signal is mainly due to the defects and to the static electric field Edc present at the interface (due to pre-existing charges Qox and/or photo-injected charge trapping/detrapping at interface traps Dit). Thus, SHG measurement gives access to the quality of dielectric/semiconductor interfaces. Nevertheless, the SHG signal is also dependent on multilayer optical propagation phenomena. For this reason, we have developed a simulation program which accounts for the optical phenomena and the static electric fields at the interfaces. We have used SHG to monitor the passivation quality of Al2O3/Si structures prepared with different processes and showed a correlation between SHG and minority carrier lifetime measurements. Qox and Dit were extracted from capacitance-voltage measurements and helped calculating the Edc values. The optical simulation, fed with known Edc values reproduced the experimental SHG data in these structures. The SHG was also used for Silicon-on-Insulator (SOI) substrates characterization. In thick SOI structures, both simulations and experimental results show that the SHG response is mainly given by optical interferences (Edc has no impact). In ultrathin SOI, the interfaces are electrically coupled and Edc is needed as input in the simulation in order to reproduce the experimental SHG data. This implies that in ultrathin SOI, SHG can access the interface electric fields in a non-destructive way.

VO2-based films are thermochromic and exhibit high or low infrared transmittance when the temperature is below or above a critical temperature. The thermochromic switching is passive and reversible, and therefore VO2 based films are promising for energy-efficient window appli­cations. However the practicaluse of VO2 for energy-efficient windows has long been hampered by low luminous transmittance and low solar energy transmittance modulation. The main goal of this dissertation work is to address these issues. The first half of the work proposes the concept of nanothermochromics for simultaneous improvement of luminous transmittance and modulation of solar energy throughput. nanoth­ermochromics considers VO2 nanoparticle composite layers, whose optical properties were modeled by effective medium theories. Calculations on VO2 spheroids have shown that VO2 nanoparticles, especially nanospheres, can offer dramatically improved luminous transmittance and solar transmittance modulation that are not possible for films. Calculations done on coreshell nanoparticles showed comparable improvements and offer an opportunity to reduce the material costs. It was also found that the composite of In2O3:Sn (ITO) and VO2 can yield moderately high luminous transmittance, solar transmittance modulation and low-emittance properties. In the second half of the dissertation work, Mg-doped VO2 films were sputter deposited. Their band gaps and Mg-content were investigated by means of optical absorption measurement and Rutherford backscattering spectrometry, respectively. The band gaps of VO2 were found to increase by ∼3.9±0.5 eV per unit of atom ratio Mg/(Mg+V) for 0<Mg/(Mg+V)<0.21. Computations based on effective medium theory were done to estimate the performance of Mg­-doped VO2 films and nanoparticle composite layers. The results suggest that moderately doped VO2 films with 0<Mg/(Mg+V)<0.06 perform better than un-doped films and that the perfor­mance can be further enhanced with one layer of antireflection coating. The best results were achieved by un-doped VO2 nanospheres, closely followed by the VO2 nanospheres with low Mg-content. Furthermore, the an experimental study on sputter deposited VO2 nanorods has identified the geometry of the oxygen gas inlet, the type of substrate, the substrate temperature and the layer thickness as important factors that influence the growth morphology. Taken as a whole, nanothermochromics offered by VO2 nanoparticles was shown to be the best solution for VO2 based thermochromic energy-efficient window coatings.

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<p>In this thesis we report on the metal-mediated-thermally induced changes of the structural and optical properties of hydrogenated amorphous silicon deposited by hot-wire CVD, where aluminium and nickel were used to induce crystallization. The metal-coated amorphous silicon was subjected to a thermal annealing regime of between 150 and 520&deg / C. The structural measurements, obtained by Raman spectroscopy, show partial crystallization occurring at 350 &deg / C. At the higher annealing temperatures of 450&deg / C and 520&deg / C complete crystallization occurs. Reflection and transmission measurements in the UV-visible range were then used to extract the optical properties. By adopting the effective medium approximation a single optical model could be constructed that could successfully model material that was in different structural phases, irrespective of metal contamination. Changes in the absorption of the material in various stages of transition were confirmed with a directly measured absorption technique, and the modelled absorption closely followed the same trends This study forms part of the larger overall solar cell research project, of which the primary aim is to eventually develop a silicon solar panel that optimises the characteristics for best performance.</p>

<p>Hydrogenated amorphous silicon (a-Si:H) is second only to crystalline silicon in volume manufacturing of solar cells due to its attractive characteristics for solar panel manufacturing. These are lower manufacturing costs, and the fact that it can be deposited on any surface, and in any shape even on flexible substrates. The metal induced crystallization of hydrogenated amorphous silicon has been the subject of intense scrutiny in recent years. By combining the technology of hydrogenated amorphous silicon thin films with the superior characteristics of c-Si material, it is hoped that more efficient solar cells can be produced. In this thesis we report on the metal-mediated-thermally induced changes of the structural and optical properties of hydrogenated amorphous silicon deposited by hot-wire CVD, where aluminium and nickel were used to induce crystallization. The metal-coated amorphous silicon was subjected to a thermal annealing regime of between 150 and 520&deg / C. The structural measurements, obtained by Raman spectroscopy, show partial crystallization occurring at 350 &deg / C. At the higher annealing temperatures of 450&deg / C and 520&deg / C complete crystallization occurs. Reflection and transmission measurements in the UV-visible range were then used to extract the optical properties. By adopting the effective medium approximation a single optical model could be constructed that couldsuccessfully model material that was in different structural phases, irrespective of metal contamination. Changes in the absorption of the material in various stages of transition were confirmed with a directly measured absorption technique, and the modelled absorption closely followed the same trends This study forms part of the larger overall solar cell research project, of which the primary aim is to eventually develop a silicon solar panel that optimises the characteristics for best performance.</p>

Optical properties of copper oxide nanoparticles in a silica matrix thin film have been investigated. Films were prepared on Si substrates from a sol-gel by spin coating. Four samples with different thicknesses, from 14,5-109 nm, were fabricated. Optical properties were measured with Variable Angle Spectroscopic Ellipsometry. The aim of the project was to gain further understanding of these films that are interesting in applications for solar absorbers as solar selective coatings. Ellipsometricangles Ψ and Δ were measured in the wavelength range from 250-1700 nm. A dispersion model was developed and fitted to experimental data with acceptable results.

<p>Hydrogenated amorphous silicon (a-Si:H) is second only to crystalline silicon in volume manufacturing of solar cells due to its attractive characteristics for solar panel manufacturing. These are lower manufacturing costs, and the fact that it can be deposited on any surface, and in any shape even on flexible substrates. The metal induced crystallization of hydrogenated amorphous silicon has been the subject of intense scrutiny in recent years. By combining the technology of hydrogenated amorphous silicon thin films with the superior characteristics of c-Si material, it is hoped that more efficient solar cells can be produced. In this thesis we report on the metal-mediated-thermally induced changes of the structural and optical properties of hydrogenated amorphous silicon deposited by hot-wire CVD, where aluminium and nickel were used to induce crystallization. The metal-coated amorphous silicon was subjected to a thermal annealing regime of between 150 and 520&deg / C. The structural measurements, obtained by Raman spectroscopy, show partial crystallization occurring at 350 &deg / C. At the higher annealing temperatures of 450&deg / C and 520&deg / C complete crystallization occurs. Reflection and transmission measurements in the UV-visible range were then used to extract the optical properties. By adopting the effective medium approximation a single optical model could be constructed that couldsuccessfully model material that was in different structural phases, irrespective of metal contamination. Changes in the absorption of the material in various stages of transition were confirmed with a directly measured absorption technique, and the modelled absorption closely followed the same trends This study forms part of the larger overall solar cell research project, of which the primary aim is to eventually develop a silicon solar panel that optimises the characteristics for best performance.</p>

<p>In this thesis we report on the metal-mediated-thermally induced changes of the structural and optical properties of hydrogenated amorphous silicon deposited by hot-wire CVD, where aluminium and nickel were used to induce crystallization. The metal-coated amorphous silicon was subjected to a thermal annealing regime of between 150 and 520&deg / C. The structural measurements, obtained by Raman spectroscopy, show partial crystallization occurring at 350 &deg / C. At the higher annealing temperatures of 450&deg / C and 520&deg / C complete crystallization occurs. Reflection and transmission measurements in the UV-visible range were then used to extract the optical properties. By adopting the effective medium approximation a single optical model could be constructed that could successfully model material that was in different structural phases, irrespective of metal contamination. Changes in the absorption of the material in various stages of transition were confirmed with a directly measured absorption technique, and the modelled absorption closely followed the same trends This study forms part of the larger overall solar cell research project, of which the primary aim is to eventually develop a silicon solar panel that optimises the characteristics for best performance.</p>

Philosophiae Doctor - PhD / In this thesis we report on the metal-mediated-thermally induced changes of the structural and optical properties of hydrogenated amorphous silicon deposited by hot-wire CVD, where aluminium and nickel were used to induce crystallization. The metal-coated amorphous silicon was subjected to a thermal annealing regime of between 150 and 520°C. The structural measurements, obtained by Raman spectroscopy, show partial crystallization occurring at 350 °C. At the higher annealing temperatures of 450°C and 520°C complete crystallization occurs. Reflection and transmission measurements in the UV-visible range were then used to extract the optical properties. By adopting the effective medium approximation a single optical model could be constructed that could successfully model material that was in different structural phases, irrespective of metal contamination. Changes in the absorption of the material in various stages of transition were confirmed with a directly measured absorption technique, and the modelled absorption closely followed the same trends This study forms part of the larger overall solar cell research project, of which the primary aim is to eventually develop a silicon solar panel that optimises the characteristics for best performance. / South Africa

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