ITO is widely regarded as the optimal TCO for serving as front window layer in PSK/c-Si tandem solar cells. It is known to effectively mitigate several stability issues present in perovskite solar cells while demonstrating excellent lateral conductivities and optical transparency across the entire solar spectrum. However, due to the damaging effects of traditional magnetron sputtering methods on the underlying cell precursor and the limited range of annealing temperatures viable for maintaining the stability of Perovskite Solar cells, realizing the full capability of ITO layer is constrained. This investigation focuses on developing and optimizing the front Indium Tin Oxide (ITO) layer properties for high-efficiency monolithic Perovskite/PERC tandem solarcells. The study employs two widely employed industrial techniques, Magnetron Sputtering and Screen Printing for the deposition of ITO thin-films and subsequent metallization of Ag front contacts. The sputtering process parameters, namely the carrier speed, O2 : Ar ratio, and the sputter power were varied to obtain an optimized ITO layer, which exhibited a thickness of 53nm, Rsheet of 107 ohm/□, mobility of 37 cm2/V s, and 90 % average optical transparency between 400−1200nm. A low contact resistivity of 5.4mΩ·cm2 was achieved between the ITO and metal contacts which is the lowest reported value for ITO annealed at low temperature (140 °C). Champion cells, featuring Perovskite on Ohmic substrate and 2T perovskite/PERC tandem cells, exhibited high VOC values of 1.116 V and 1.75 V on 0.97 cm2 cell aperture areas and cell efficiencies of 17.2 % and 23.85 %. Additionally, a large area (158.7 cm2) tandem cell was also fabricated which demonstrated an excellent VOC of 1.75 V . The results of this investigation demonstrates the versatility of ITO layer properties achievable at low-temperatures through Magnetron sputtering and underscores the potential of existing commercialized technologies for the fabrication of high-efficiency tandem solar cells. / ITO anses allmänt vara den optimala TCO för användning som frontfönsterskikt i PSK/c-Si tandemsolceller. Den är känd för att effektivt mildra flera stabilitetsproblem som finns i perovskitsolceller samtidigt som den uppvisar utmärkt lateral konduktivitet och optisk transparens över hela solspektrumet. På grund av de skadliga effekterna av traditionella magnetronförstoftningsmetoder på den underliggande cellprekursorn och det begränsade intervallet av glödgningstemperaturer som är användbara för att upprätthålla stabiliteten hos perovskitsolceller, begränsas dock ITO-skiktens fulla kapacitet. Denna undersökning fokuserar på att utveckla och optimera egenskaperna hos det främre Indium Tin Oxide (ITO)-skiktet för högeffektiva monolitiska Perovskite/PERC tandemsolceller. I studien används två allmänt använda industriella tekniker, magnetronförstoftning och screentryckning, fördeponering av ITO-tunnfilmer och efterföljande metallisering av Ag-frontkontakter. Parametrarna för sputteringsprocessen, nämligen bärarhastigheten, förhållandet O2 : Ar och sputterkraften varierades för att få ett optimerat ITO-lager, som uppvisade en tjocklek på 53nm, Rsheet på 107 ohm/□, rörlighet på 37 cm2/V s och 90 % genomsnittlig optisk transparens mellan 400 − 1200 nm. En låg kontaktresistivitet på 5.4mΩ.cm2 uppnåddes mellan ITO och metallkontakterna, vilket är de lägstarapporterade värdena för ITO glödgat vid låg temperatur (140 °C). Champion-cellerna, med perovskit på ohmskt substrat och 2T perovskit/PERC tandemkonfigurationer, uppvisade höga VOC-värden på 1.116 V och 1.75 V på 0.97 cm2 cellaperturområden och cellverkningsgrader på 17.2 % och 23.85 %. Dessutom tillverkades en tandemcell med stor area (158.7 cm2) som uppvisade en utmärkt VOC på 1.75 V . Resultaten av denna undersökning visar mångsidigheten hos ITO-skiktets egenskaper som kan uppnås vid låga temperaturer genom magnetronförstoftning och understryker potentialen hos befintliga kommersialiserade tekniker för tillverkning av högeffektiva tandemsolceller.

We present an active learning algorithm for identifying viable process conditions in magnetron sputtering experiments. The algorithm trains a classifier to predict which gas pressure and magnetron power combinations yield stable discharge with deposition rates exceeding a minimum threshold. A computation-based oracle that labels experiments using QCM readings facilitates a fully automated learning procedure, laying the groundwork for a self-driving lab where novel materials will be explored for next-generation solar cells. Upon evaluation, the active learning algorithm results in significantly higher sample efficiency than traditional supervised learning across a range of magnetron sputtering experiments. Moreover, a sampling sequence analysis shows that active learning enables an informed search of the process parameter space, generating patterns that approximate Paschen’s law. The work presented in this thesis serves as a first step toward a fully automated materials synthesis process, where the input region of viable synthesis parameters can be identified with minimal experimentation. The solution allows researchers to efficiently narrow the search space of optimal process conditions for targeted materials design.

Ce mémoire présente les efforts effectués pour réduire l'angle de perte de couches de pentoxyde de tantale amorphes telles qu'utilisées pour les miroirs de LIGO. Afin d'améliorer le niveau de relaxation des couches, celles-ci ont été déposées par pulvérisation cathodique magnétron à des températures allant de 50 °C à 480 °C, elles ont subi un recuit thermique rapide, elles ont été implantées par des ions d'oxygène, elles ont été déposées par pulvérisation cathodique magnétron en appliquant une tension de polarisation sur le substrat lors du dépôt allant de 0 V à -450 V et elles ont été déposées par pulvérisation cathodique magnétron pulsée à haute puissance dans le cadre de différentes expériences. L'angle de perte, l'épaisseur, la rugosité, l'indice de réfraction, la composition atomique, la contrainte, l'état de relaxation et le module de Young des couches ont par la suite été trouvés à l'aide de l'ellipsométrie spectralement résolue, la spectrométrie de rétrodiffusion de Rutherford, la détection des reculs élastiques, la spectroscopie Raman, la diffraction de rayons X et la nano-indentation. Il a été trouvé que la température de dépôt améliorait légèrement le degré de relaxation des couches jusqu'à 250 °C, mais qu'elle avait peu d'impact après recuit. Aussi, lors de dépôt à température de la pièce, une forte tension de polarisation réduit l'angle de perte, mais cet effet est encore une fois perdu suite au recuit. Les autres méthodes mentionnées ci-dessus n'ont pas influencé le degré de relaxation des couches selon l'angle de perte, la spectroscopie Raman et la diffraction de rayons X. Cette recherche a été réalisée avec le support financier du CRSNG et du FRQNT (numéro de dossier 206976). / This master's thesis presents the experiments made to reduce the loss angle of tantala coatings similar to those used in LIGO. To improve the relxation level of the coatings they were deposited by magnetron sputtering at temperatures varying from 50 °C to 480 °C. They were also subjected to rapid thermal annealing, and oxygen implantation. In another experiment, the coatings were deposited by magnetron sputtering with substrate biasing varying from 0 V to -450 V at room temperature and at 250 °C. Finally, the coatings of tantala were deposited by high power impulse magnetron sputtering. The loss angle, thickness, roughness, refractive index, atomic composition, stress, the relaxation state and Young's modulus of the coatings were characterized using spectroscopic ellipsometry, Rutherford backscattering, elastic recoil detection, Raman spectroscopy, X-ray diffraction and nanoindentation. It was found that the deposition temperature improved the loss angle until it reached 250 °C. However, annealing the coatings had a superior impact and the influence of the deposition temperature was not visible after annealing. When was applied a high bias to the susbtrate at room temperature, the obtained coating was slightly more relaxed than when a low bias was applied but this effect is, once again, insignificant after annealing. The other methods of deposition mentioned did not improve the loss angle or modify the relaxation state found by Raman spectroscopy and X-ray diffraction of the tantala coatings. This research was made with the financial support of the NSERC and of the FRQNT (file number 206976).

En 2015, le Laser Interferometer Gravitational-Wave Observatory (LIGO) a observé pour la première fois des ondes gravitationnelles générées par la fusion de deux trous noirs. Cette observation résulte de 40 ans d’efforts afin de réduire au minimum les sources de bruit qui affectent l’interféromètre. À ce jour, la sensibilité de LIGO, dans son domaine de fréquence le plus sensible, est limitée par la granularité de la lumière d’une part et, d’autre part, par un phénomène de fluctuations thermiques résultat de la dissipation mécanique dans les couches minces qui constituent ses miroirs, en particulier dans le matériau ayant un haut indice de réfraction : l’oxyde de tantale. Une amélioration de la sensibilité permettrait d’observer davantage d’événement, d’autres phénomènes gravitationnels, ainsi que des détails importants permettant de mieux les comprendre. Ce mémoire présente les résultats de nos recherches afin de diminuer le bruit causé par la dissipation mécanique interne dans les couches à haut indice de réfraction. Pour ce faire, des couches d’oxyde de tantale ont été dopées soit au zirconium ou à la fois au zirconium et au titane, par co-dépôt. Des couches avec différentes quantités de dopant ont été synthétisées par pulvérisation cathodique magnétron sur des substrats de silice semblables à ceux de LIGO. Par la suite, la dissipation mécanique, l’épaisseur, la rugosité, la composition, la densité surfacique, et la microstructure ont été caractérisées par suspension nodale, ellipsométrie résolue spectralement, spectrométrie de rétrodiffusion de Rutherford et la spectroscopie Raman. Il appert que le zirconium permet d’augmenter la température de recuit avant la cristallisation, ce qui permet de diminuer plus amplement la dissipation mécanique interne, mais ne change pas la dissipation à une température de recuit donnée. Il a aussi été déterminé que la concentration de titane permettait de diminuer l’angle de perte, peu importe la concentration de zirconium. Une combinaison des deux dopages et un recuit à haute température permet ainsi de recuire par un facteur d’environ 1.5 la dissipation mécanique interne. La différence de coefficient d’expansion thermique durant les recuits à haute température induit cependant des problèmes de craquement des couches, partiellement résolus par l’application d’une couche de recouvrement en silice. / In 2015, the Laser Interferometer Gravitational-Wave Observatory (LIGO) observed for the first time gravitational waves generated by the merger of two black holes. This observation was the resut of 40 years of efforts to minimize the noise source which affect the the interferometer. To this date, the sensitivity of LIGO, in its most sensitive frequency domain, is limited by the granularity of the light on one hand, on the other, by a phenomenon of thermal fluctuations resulting from the mechanical dissipation in the thin film of the miroir, in particular in the high refractive index material: tantala. An improvement of the sensitivity would allow the measurement of more events, other gravitational phenomena and some details that would result in a better understanding. This master’s thesis presents results of our research to reduce the noise caused by internal mechanical dissipation in high refractive index layers. To do so, tantala layers were doped with either zirconium and titanium by co-deposition. Layers with different amounts of dopant were synthesized by magnetron sputtering on fused silica substrate similar to those of LIGO. Subsequently, mechanical dissipation, thickness, roughness, composition, areal density and microstructure were characterized by gentle nodal suspension, spectrally resolved ellipsometry, Rutherford backscattering spectroscopy, and Raman spectroscopy. It appears that zirconium allows the annealing temperature to be increased before crystallization which further decreases internal mechanical dissipation, but does not change dissipation at a given annealing temperature. It was also determined that the concentration of titanium reduced the loss angle regardless of the zirconium concentration. A combination of the two dopant and high annealing temperatures thus enables the internal mechanical dissipation to be lower by a factor of 1.5.The difference in thermal expansion coefficient during high temperature annealing, however, induces layer cracking problems, partially resolved by the application of a silica cap.

Im Fokus der vorliegenden Arbeit lag die Untersuchung polykristalliner TiO2:Ta-Schichten, hergestellt mittels Gleichstrom-Magnetron-Sputtern durch Verwendung reduzierter keramischer Targets und anschließender thermischer Nachbehandlung im Vakuum der zunächst nichtleitfähigen amorphen Precursorschichten. Es wurden die physikalischen Zusammenhänge, welche die strukturellen, elektrischen und optischen Eigenschaften der kristallinen TiO2:Ta-Schichten beeinflussen analysiert und dabei eine empfindliche Abhängigkeit vom Sauerstofffluss während der Abscheidung festgestellt. Es zeigte sich, dass die Verringerung der kinetischen Energie der Plasmateilchen beim Magnetron-Sputtern durch die Erhöhung des Gesamtdruckes vorteilhaft ist, um das Wachstum des gegenüber Rutil besser leitfähigen Anatas in Verbindung mit dem für niedrige Widerstände notwendigen Sauerstoffdefizit zu realisieren. Bei einem Gesamtdruck von 2 Pa abgeschiedene polykristalline TiO2:Ta-Schichten haben einen spezifischen Widerstand von 1,5·10-3 Ωcm, eine hohe Ladungsträgermobilität (≈8 cm2V-1s-1) und einen geringen Extinktionskoeffizienten von 0,006. Die Abhängigkeit des elektrischen Widerstandes vom Sauerstoffdefizit in der TiO2:Ta-Schicht wurde unter dem Gesichtspunkt der Ladungsträgeraktivierung sowie der Bildung von Ti-Fehlstellen diskutiert, welche vermutlich zur Kompensation und Lokalisierung von freien Elektronen beitragen. Darüber hinaus wurde zur effizienteren Gestaltung der thermischen Nachbehandlung die konventionelle Vakuumtemperung erstmalig erfolgreich durch die Blitzlampentemperung ersetzt. / The work is focused on understanding the physical processes responsible for the modification of the structural, electrical and optical properties of polycrystalline TiO2:Ta films formed by vacuum annealing of initially not conductive amorphous films deposited by direct current magnetron sputtering. It is shown that the oxygen deficiency of amorphous and annealed TiO2:Ta films, respectively, is critical to achieve low resistivity and high optical transmittance of the crystalline films. Increasing the total pressure during magnetron sputter deposition is shown to be beneficial to achieve the desired oxygen deficient anatase growth, which is discussed in terms of energetic particle bombardment. Polycrystalline anatase TiO2:Ta films of low electrical resistivity (1,5·10-3 Ωcm), high free electron mobility (≈8 cm2V-1s-1), and low extinction (0,006) are obtained in this way at a total pressure of 2 Pa. The dependence of the polycrystalline film electrical properties on the oxygen content is discussed in terms of Ta dopant electrical activation as well as transport limiting processes taking into account the formation of Ti-vacancies. In addition, the conventional vacuum annealing has been successfully substituted by the flash lamp annealing in the millisecond range.

The work presented in this thesis deals with experimental and theoretical studies related to alumina thin films. Alumina, Al2O3, is a polymorphic material utilized in a variety of applications, e.g., in the form of thin films. However, controlling thin film growth of this material, in particular at low substrate temperatures, is not straightforward. The aim of this work is to increase the understanding of the basic mechanisms governing alumina growth and to investigate novel ways of synthesizing alumina coatings. The thesis can be divided into two main parts, where the first part deals with fundamental studies of mechanisms affecting alumina growth and the second part with more application-oriented studies of high power impulse magnetron sputter (HiPIMS) deposition of the material. In the first part, it was shown that the thermodynamically stable α phase, which normally is synthesized at substrate temperatures of around 1000 °C, can be grown using reactive sputtering at a substrate temperature of merely 500 °C by controlling the nucleation surface. This was done by predepositing a Cr2O3 nucleation layer. Moreover, it was found that an additional requirement for the formation of the α phase is that the depositions are carried out at low enough total pressure and high enough oxygen partial pressure. Based on these observations, it was concluded that energetic bombardment, plausibly originating from energetic oxygen, is necessary for the formation of α-alumina (in addition to the effect of the chromia nucleation layer). Moreover, the effects of residual water on the growth of crystalline films were investigated by varying the partial pressure of water in the ultra high vacuum (UHV) chamber. Films deposited onto chromia nucleation layers exhibited a columnar structure and consisted of crystalline α-alumina if deposited under UHV conditions. However, as water to a partial pressure of 1*10-5 Torr was introduced, the columnar α-alumina growth was disrupted. Instead, a microstructure consisting of small, equiaxed grains was formed, and the γ-alumina content was found to increase with increasing film thickness. To gain a better understanding of the atomistic processes occurring on the surface, density functional theory based computational studies of adsorption and diffusion of Al, O, AlO, and O2 on different α-alumina (0001) surfaces were also performed. The results give possible reasons for the difficulties in growing the α phase at low temperatures through the identification of several metastable adsorption sites and also show how adsorbed hydrogen might inhibit further growth of α-alumina crystallites. In addition, it was shown that the Al surface diffusion activation energies are unexpectedly low, suggesting that limited surface diffusivity is not the main obstacle for low-temperature α-alumina growth. Instead, it is suggested to be more important to find ways of reducing the amount of impurities, especially hydrogen, in the process and to facilitate α-alumina nucleation when designing new processes for low-temperature deposition of α-alumina. In the second part of the thesis, reactive HiPIMS deposition of alumina was studied. In HiPIMS, a high-density plasma is created by applying very high power to the sputtering magnetron at a low duty cycle. It was found, both from experiments and modeling, that the use of HiPIMS drastically influences the characteristics of the reactive sputtering process, causing reduced target poisoning and thereby reduced or eliminated hysteresis effects and relatively high deposition rates of stoichiometric alumina films. This is not only of importance for alumina growth, but for reactive sputter deposition in general, where hysteresis effects and loss of deposition rate pose a substantial problem. Moreover, it was found that the energetic and ionized deposition flux in the HiPIMS discharge can be used to lower the deposition temperature of α-alumina. Coatings predominantly consisting of the α phase were grown at temperatures as low as 650 °C directly onto cemented carbide substrates without the use of nucleation layers. Such coatings were also deposited onto cutting inserts and were tested in a steel turning application. The coatings were found to increase the crater wear resistance compared to a benchmark TiAlN coating, and the process consequently shows great potential for further development towards industrial applications.

In the present work Mg films prepared by RF magnetron sputtering were studied. Variable energy positron annihilation spectroscopy (VEPAS) was employed for investigation of defects in the Mg films. VEPAS characterization was combined with scanning electron microscopy and X-ray diffraction in order to determine grain size, phase composition and texture. The effect of different deposition rate and deposition temperature, annealing, various substrates and film thickness on the structure and amount of defects present in the Mg films was examined. Defect studies by VEPAS showed that positrons in studied Mg films are trapped at misfit dislocations and at vacancy-like defects in grain boundaries and their density can be reduced by the deposition at elevated temperature. 1

Grâce à ses excellentes propriétés physiques et chimiques (stable thermiquement, bon conducteur électrique et de chaleur, ductile, très dur mécaniquement, bonne inertie chimique), le matériau tantale et son nitrure TaNx sont utilisés comme revêtement de surface des outils, résistance électrique, barrière de diffusion au cuivre, croissance de nanotubes par un procédé chimique catalytique en phase vapeur. C’est ce matériau et son nitrure que nous avons étudiés lors de cette thèse.Aujourd’hui les exigences des industriels nécessitent que la pulvérisation cathodique magnétron (PCM) puisse être appliquée aux pièces de formes complexes. La principale limitation de cette méthode de dépôt est que la plupart des particules pulvérisées sont neutres. Pour contrôler l’énergie et la trajectoire des particules pulvérisées, des nouveaux procédés IPVD (Ionized Physical Vapor Deposition) ont été développés pour ioniser les atomes pulvérisés. Le procédé RF-IPVD (Radio-Frequency Ionized Physical Vapor Deposition) permet, grâce à une boucle placée entre la cible et le substrat et polarisée en RF, de créer un second plasma permettant d’ioniser la vapeur pulvérisée. Un autre procédé a été développé : nommé HIPIMS (High Power Impulse Magnetron Sputtering), ce procédé utilise une alimentation fournissant des impulsions de courte durée et de forte puissance au lieu d’une alimentation DC. Les particules pulvérisées peuvent être ionisées dans le plasma magnétron qui est très dense lors des impulsions. Nous avons réalisé des couches minces de Ta par PCM, RF-IPVD et HIPIMS, et des couches minces de TaNx par PCM et HIPIMS. Les différentes propriétés des décharges et des couches minces sont étudiées et comparées dans ce mémoire. / Thanks to their excellent physical and chimical characteristics such as good stability with temperature, good conductor of heat and electricity, ductility, hardness, chemical inertness and good corrosion resistance, tantalum and its nitride are used in a wide variety of applications such as wear and corrosion-resistant materials, thin film transistors, diffusion barrier for copper and for carbon nanotube grown by CCVD process (catalytically chemical vapor deposition). For some recent industrial demand, it is necessary to deposit on substrates with complex shape. The main disadvantage of the conventional magnetron sputtering (CMS) is that most of the sputtered particles are neutral. To controle the energy and the path of sputtered particles, new magnetron sputtering techniques have been developed for ionizing a significant fraction of sputtered material. A new sputtering process called RF-IPVD consists in ionizing the sputtered vapor by adding second plasma by a RF coil between the target and the substrate. Another method called HIPIMS (High Power Impulsed Magnetron Sputtering), uses high power impulse instead of DC power. During the impulse, the sputtered Ta atoms are ionized in the dense plasma. We have deposited Ta thin films by CMS, RF-IPVD and HIPIMS and TaNx thin films by CMS and HIPIMS. The objective of this thesis is to compare the properties of discharges and thin films deposited by these different techniques.

In dieser Dissertation wurde die Beziehung zwischen den strukturellen, optischen und Ladungstransporteigenschaften von dotierten ZnO- und Zn1-xMgxO-Schichten eingehend untersucht. Das Ziel war es, die oben genannten Zusammenhänge weiter aufzuklären, wodurch sich anschließend Ansätze für eine zielgerichtete Verbesserung der Schichteigenschaften ableiten lassen. Zunächst konzentriert sich die Arbeit auf das Wachstum der ZnO-Schichten, um wichtige strukturelle Parameter, wie zum Beispiel Korngrößen und Defektdichten, mittels Röntgendiffraktometrie und Transmissionselektronenmikroskopie zu bestimmen. Diese strukturellen Parameter wurden dann als Modellparameter für die theoretische Modellierung des Transports der freien Ladungsträger verwendet. Temperaturabhängige Hall-, Leitfähigkeits- und Seebeck-Koeffizient-Messungen zeigten, dass der elektrische Transport hauptsächlich durch die Streuung der Ladungsträger an ionisierten Störstellen und Korngrenzen limitiert wird. Im Rahmen dieser Arbeit wurde die theoretische Beschreibung der Streuung an Korngrenzen auf entartet dotierte Halbleiter erweitert. Diese Ergebnisse wurden dann genutzt, um ein qualitatives Modell zu formulieren, welches den Zusammenhang zwischen dem Magnetron-Sputter-Abscheidungsprozess und den strukturellen und elektrischen Eigenschaften der Schichten herstellt. Gemäß diesem Modell sind die Schichteigenschaften bei niedrigen Abscheidungstemperaturen hauptsächlich durch die Bildung akzeptoratiger Sauerstoffzwischengitterdefekte bestimmt, die einen Teil der extrinsischen Dotanden kompensieren. Diese Defekte werden durch ein Bombardement der wachsenden Schicht mit hochenergetischen negativen Sauerstoffionen verursacht. Bei höheren Abscheidungstemperaturen dominiert die Bildung von sekundären Phasen oder Defektkomplexen, in denen der Dotant elektrisch inaktiv ist. / In this thesis, the relation between the structural, optical, and charge carrier transport properties of magnetron sputtered doped ZnO and Zn1-xMgxO films has been investigated in detail. The objective was to clarify the above mentioned relations, which allows to derive solutions for a deliberate improvement of the layer properties. The work first focusses on the growth of the ZnO layers to determine important structural properties like grain sizes and defect densities via X-ray diffraction and transmission electron microscopy investigations. These structural properties were then used as model parameters for the theoretical modelling of the charge carrier transport. The temperature dependent Hall, conductivity and Seebeck coefficient measurements show that the transport is mainly limited by grain boundary scattering and ionized impurity scattering. The theoretical description of the grain boundary scattering has been extended in this work to also include degenerate semiconductors. Based on the results on the structural and electronic properties, in a next step a qualitative model was developed which explains the correlation between the magnetron sputtering deposition process and the structural and electronic properties of the films. According to this model, the properties of the films are mainly influenced by the formation of electrically active acceptor-like oxygen interstitial defects at low deposition temperatures, which lead to a partial compensation of the extrinsic donors. These defects are caused by a bombardment of the growing film by high-energetic negative oxygen ions. At higher deposition temperatures, the formation of secondary phases or defect complexes, in which the dopant is electrically inactive, prevails.

Ce travail porte sur la synthèse de couches minces de nanoparticules de silicium (np-Si) encapsulées dans une matrice diélectrique en vue d’une application en tant que couche active pour les cellules solaires de 3ème génération. La technique utilisée pour la synthèse des np-Si est la pyrolyse laser. Cette technique nous a permis d’obtenir des np-Si cristallines d’environ 5 nm de diamètre avec une distribution en taille étroite. Par ailleurs, l’utilisation de gaz précurseurs spécifiques (PH₃, B₂H₆) dans le mélange réactionnel a rendu possible le dopage (type n ou p) des np-Si. Le dopage effectif des np-Si a pu être mis en évidence par des mesures de résonance paramagnétique électronique (RPE). Des films de np-Si seules ont pu être déposés in-situ via la création d’un jet supersonique de gaz contenant les particules de silicium. Les caractérisations optoélectroniques de ces couches ont montré un effet de confinement quantique fort au sein de films, garantissant ainsi un élargissement important du gap du silicium de 1.12 eV (pour le silicium massif) à environ 2 eV (pour les np-Si) ; prérequis indispensable pour réaliser une cellule tandem tout silicium. Des mesures de résistivité sur ces films ont permis de confirmer l’activité des dopants au sein des np-Si. Pour les np-Si dopées au phosphore une diminution de la résistivité de plus de 5 ordres de grandeurs par rapport au np-Si intrinsèques a été observée. Le couplage entre la pyrolyse laser et la pulvérisation magnétron via notre dispositif original de synthèse s’est révélé parfaitement adapté à l’élaboration de couches minces nanocomposites np-Si/SiO₂. Un comportement de type diode a pu être mis en évidence sur une jonction constituée par la superposition d’une couche nanocomposites (type n) sur un substrat de silicium massif (type p). Au-delà de la simple application au photovoltaïque, le procédé couplé, largement éprouvé et optimisé au cours de ce travail de thèse, pourrait permettre la réalisation d’une multitude de couches nanocomposites différentes, puisque la nature chimique des particules et de la matrice peuvent être choisies indépendamment. / This work focuses on the synthesis of thin films composed of silicon nanoparticles (np- Si) embedded in a dielectric matrix for application as an active layer for the third generation solar cells. The technique used for the synthesis of np-Si is the laser pyrolysis. This technique allowed us to obtain 5 nm cristalline np -Si with a narrow size distribution. Furthermore, the use of specific precursor gases (PH₃, B₂H₆) in the reaction mixture enables doping (n or p -type) of np -Si. Effective np -Si doping has been demonstrated by measurements of electron paramagnetic resonance (EPR). Films made of np-Si only, have been deposited in situ by creating a supersonic jet of gas containing the silicon particles. Optoelectronic characterization of these layers showed a strong quantum confinement effect in films, thus ensuring a significant widening of the gap of 1.12 eV silicon (for bulk silicon) to about 2 eV (np -Si); which is an essential prerequisite to achieve a silicon tandem cell. Resistivity measurements on these films have confirmed the dopants activity in the np -Si. For np -Si doped with phosphorus, a significant decrease of the resistivity of more than five orders of magnitude compared to the intrinsic np -Si was observed. Coupling between laser pyrolysis and magnetron sputtering through our original synthesis device proved to be perfectly suited for the elaboration of nanocomposite thin films np-Si/SiO₂. A diode-type behavior has been highlighted on a junction formed by the superposition of a nanocomposite layer (n-type) on a bulk silicon substrate (p-type ). Beyond the simple application to photovoltaics , the coupled process, widely used and optimized during this work could allow the production of a multitude of different nanostructured layers , since the chemical nature of the particles and the matrix can be chosen independently.