The formation of the micro- and nanodomain structures during polarization reversal has been studied in single crystal lithium niobate with inhomogeneously modified conductivity. It is well known that the vacuum annealing and plasma-source ion irradiation of the lithium niobate crystals leads to sufficient increase of the bulk conductivity due to out-diffusion of the oxygen from the sample surface. Creation of layers with modified conductivity leads to inhomogeneous distribution of applied electric field in bulk of ferroelectric crystals. Polarization reversal in such a crystals permits to localize charged domain walls in the bulk. Methods of creation of charged domain walls can be used for the construction of the waveguide structures, optical modulators and resonators. The main conclusions of the work: 1) It was shown that plasma-source ion irradiation and vacuum annealing leads to inhomogeneous change of absorption and increase of the conductivity, which can be attributed to the out-diffusion of oxygen and lithium segregation in the surface layer of crystal. 2) Inhomogeneous distribution of electric field in the bulk of modified crystals leads to significant decrease of switched layer thickness. 3) Effect of formation and growth of non-through domains with charged domain walls has been revealed. 4) Analysis of switching current by modified Kolmogorov-Avraami formula permit to determine mobility of domain wall and threshold filed of polarization reversal. / Целью работы являлось экспериментальное исследование формирования микро- и нанодоменных структур в монокристаллах ниобата лития с неоднородно модифицированной проводимостью. Известно, что обработка воздействием низкоэнергетичного ионно-плазменного облучения и восстановительного отжига приводит к резкому увеличению проводимости кристаллов за счёт аут-диффузии кислорода с поверхности. Создание слоёв с измененной проводимостью приводит к неоднородному распределению электрического поля в объёме сегнетоэлектрических кристаллов, что позволяет создавать внутри-объёмные заряженные доменные структуры при переключении поляризации. Методы создания заряженных доменных структур используются для создания элементов интегральных оптических устройств: волноводных структур, оптических модуляторов и резонаторов. Основные выводы работы: 1) Показано, что ионно-плазменное облучение и восстановительный отжиг кристаллов приводят к неоднородному изменению поглощения и увеличению проводимости, что может быть отнесено за счёт аут-диффузии кислорода и сегрегации лития в поверхностном слое. 2) Установлено, что неоднородное распределение электрического поля в объёме модифицированных кристаллов приводит к значительному понижению порогового поля переключения поляризации, за счёт уменьшения толщины переключаемого слоя. 3) Впервые обнаружен и изучен эффект формирования и роста несквозных доменов с заряженными доменными стенками. 4) Анализ тока переключения модифицированной формулой Колмогорова-Аврами позволил определить подвижность доменной стенки и пороговое поле начала переключения.

[pt] Corpos relativamente pequenos do sistema solar não possuem atmosfera (ou muito rarefeita, chamada exosfera) e nem campo magnético: encontram-se praticamente desprotegidos da influência do ambiente espacial no qual estão inseridos. Tais corpos (como a maioria dos asteroides, luas e cometas distantes do Sol), estão sujeitos aos efeitos do chamado intemperismo espacial. Com o objetivo de simular e estudar este fenômeno em laboratório, três amostras de meteoritos do tipo condrito ordinário foram irradiadas por feixes de H(positivo) com energia de 1,0 MeV. Uma das amostras foi, também, irradiada por feixe de N(positivo) de 2,0 MeV. Os efeitos da irradiação foram monitorados por espectroscopias Raman e UV-VIS-NIR. Os resultados Raman mostram variações sistemáticas do número de onda, da intensidade e da largura das bandas vibracionais estudadas, evidências de modificações estruturais. As seções de choque de destruição das ligações Si-O presentes nas estruturas cristalinas foram determinadas. A espectroscopia UV-VIS-NIR por refletância de esfera integrada foi usada para monitorar as modificações nas características espectrais. Os espectros obtidos mostram escurecimento e avermelhamento progressivos das amostras irradiadas; a amplitude destas modificações depende do conteúdo inicial de ferro na estrutura. É proposto que o avermelhamento observado com o aumento da fluência (ou dose) da irradiação deve-se ao aumento do coeficiente de absorção na faixa azul que, por sua vez, decorre da diminuição do gap óptico do material. Estes resultados são relevantes para a modelagem da evolução físico-química de asteroides expostos ao vento solar. / [en] Relatively small bodies in the solar system have no atmosphere (or very thin, called the exosphere) and no magnetic field: they are virtually unprotected from the influence of the space environment in which they are inserted. Such bodies (like most asteroids, moons, and comets far from the sun), are subject to the effects of so-called space weathering. To simulate and study this phenomenon in the laboratory, three samples of ordinary chondrite meteorites were irradiated by H(positive) beams with 1.0 MeV energy. One of the samples was also irradiated by a 2.0 MeV N(positive) beam. The effects of irradiation were monitored by Raman and UV-VIS-NIR spectroscopies. The Raman results show systematic variations in the wavenumber, intensity, and width of the studied vibrational bands, evidence of structural modifications. The shock sections of the destruction of Si-O bonds present in the crystalline structures were determined. Integrated sphere reflectance UV-VIS-NIR spectroscopy was used to monitor changes in spectral characteristics. The obtained spectra show progressive darkening and reddening of the irradiated samples; The extent of these modifications depends on the initial iron content in the structure. It is proposed that the redness observed with the increase of irradiation creep (or dose) is due to the increase in the absorption coefficient in the blue band, which, in turn, results from the decrease of the optical gap of the material. These results are relevant for modeling the physicochemical evolution of asteroids exposed to the solar Wind.

Résumé Dans la présente thèse, nous avons étudié la déformation anisotrope par bombardement ionique de nanoparticules d'or intégrées dans une matrice de silice amorphe ou d'arséniure d’aluminium cristallin. On s’est intéressé à la compréhension du mécanisme responsable de cette déformation pour lever toute ambigüité quant à l’explication de ce phénomène et pour avoir une interprétation consistante et unique. Un procédé hybride combinant la pulvérisation et le dépôt chimique en phase vapeur assisté par plasma a été utilisé pour la fabrication de couches nanocomposites Au/SiO2 sur des substrats de silice fondue. Des structures à couches simples et multiples ont été obtenues. Le chauffage pendant ou après le dépôt active l’agglomération des atomes d’Au et par conséquent favorise la croissance des nanoparticules. Les nanocomposites Au/AlAs ont été obtenus par implantation ionique de couches d’AlAs suivie de recuit thermique rapide. Les échantillons des deux nanocomposites refroidis avec de l’azote liquide ont été irradiés avec des faisceaux de Cu, de Si, d’Au ou d’In d’énergie allant de 2 à 40 MeV, aux fluences s'étendant de 1×1013 à 4×1015 ions/cm2, en utilisant le Tandem ou le Tandetron. Les propriétés structurales et morphologiques du nanocomposite Au/SiO2 sont extraites en utilisant des techniques optiques car la fréquence et la largeur de la résonance plasmon de surface dépendent de la forme et de la taille des nanoparticules, de leur concentration et de la distance qui les séparent ainsi que des propriétés diélectriques du matériau dans lequel les particules sont intégrées. La cristallinité de l’arséniure d’aluminium est étudiée par deux techniques: spectroscopie Raman et spectrométrie de rétrodiffusion Rutherford en mode canalisation (RBS/canalisation). La quantité d’Au dans les couches nanocomposites est déduite des résultats RBS. La distribution de taille et l’étude de la transformation de forme des nanoparticules métalliques dans les deux nanocomposites sont déterminées par microscopie électronique en transmission. Les résultats obtenus dans le cadre de ce travail ont fait l’objet de trois articles de revue. La première publication montre la possibilité de manipuler la position spectrale et la largeur de la bande d’absorption des nanoparticules d’or dans les nanocomposites Au/SiO2 en modifiant leur structure (forme, taille et distance entre particules). Les nanoparticules d’Au obtenues sont presque sphériques. La bande d’absorption plasmon de surface (PS) correspondante aux particules distantes est située à 520 nm. Lorsque la distance entre les particules est réduite, l’interaction dipolaire augmente ce qui élargit la bande de PS et la déplace vers le rouge (602 nm). Après irradiation ionique, les nanoparticules sphériques se transforment en ellipsoïdes alignés suivant la direction du faisceau. La bande d’absorption se divise en deux bandes : transversale et longitudinale. La bande correspondante au petit axe (transversale) est décalée vers le bleu et celle correspondante au grand axe (longitudinale) est décalée vers le rouge indiquant l’élongation des particules d’Au dans la direction du faisceau. Le deuxième article est consacré au rôle crucial de la déformation plastique de la matrice et à l’importance de la mobilité des atomes métalliques dans la déformation anisotrope des nanoparticules d’Au dans les nanocomposites Au/SiO2. Nos mesures montrent qu'une valeur seuil de 2 keV/nm (dans le pouvoir d'arrêt électronique) est nécessaire pour la déformation des nanoparticules d'or. Cette valeur est proche de celle requise pour la déformation de la silice. La mobilité des atomes d’Au lors du passage d’ions est confirmée par le calcul de la température dans les traces ioniques. Le troisième papier traite la tentative de formation et de déformation des nanoparticules d’Au dans une matrice d’arséniure d’aluminium cristallin connue pour sa haute résistance à l’amorphisation et à la déformation sous bombardement ionique. Le résultat principal de ce dernier article confirme le rôle essentiel de la matrice. Il s'avère que la déformation anisotrope du matériau environnant est indispensable pour la déformation des nanoparticules d’or. Les résultats expérimentaux mentionnés ci-haut et les calculs de températures dans les traces ioniques nous ont permis de proposer le scénario de déformation anisotrope des nanoparticules d’Au dans le nanocomposite Au/SiO2 suivant: - Chaque ion traversant la silice fait fondre brièvement un cylindre étroit autour de sa trajectoire formant ainsi une trace latente. Ceci a été confirmé par la valeur seuil du pouvoir d’arrêt électronique. - L’effet cumulatif des impacts de plusieurs ions conduit à la croissance anisotrope de la silice qui se contracte dans la direction du faisceau et s’allonge dans la direction perpendiculaire. Le modèle de chevauchement des traces ioniques (overlap en anglais) a été utilisé pour valider ce phénomène. - La déformation de la silice génère des contraintes qui agissent sur les nanoparticules dans les plans perpendiculaires à la trajectoire de l’ion. Afin d’accommoder ces contraintes les nanoparticules d’Au se déforment dans la direction du faisceau. - La déformation de l’or se produit lorsqu’il est traversé par un ion induisant la fusion d’un cylindre autour de sa trajectoire. La mobilité des atomes d’or a été confirmée par le calcul de la température équivalente à l’énergie déposée dans le matériau par les ions incidents. Le scénario ci-haut est compatible avec nos données expérimentales obtenues dans le cas du nanocomposite Au/SiO2. Il est appuyé par le fait que les nanoparticules d’Au ne se déforment pas lorsqu’elles sont intégrées dans l’AlAs résistant à la déformation. / Abstract In the present thesis, we study the anisotropic deformation of gold nanoparticles embedded in amorphous silica or crystalline aluminum arsenide, under ion bombardment. We try to comprehend the mechanism responsible for this deformation and to remove any ambiguity related to the explanation of this phenomenon. A hybrid process combining sputtering and plasma enhanced chemical vapour deposition was used to fabricate Au/SiO2 layers on fused silica substrates. Structures with single and multilayer were obtained. Heating during or after deposition activates the Au atom agglomeration and favours the growth of the nanoparticles. Also, a Au/AlAs nanocomposite was obtained by ion implantation of AlAs films, followed by rapid thermal annealing. The samples of the two nanocomposites, cooled with liquid nitrogen, were irradiated with 2 to 40 MeV Cu, Si, Au or In ion beams, at fluences ranging from 1×1013 to 4×1015 ions/cm2, using a Tandem or Tandetron accelerator. The structural and morphological properties of the Au/SiO2 nanocomposite were extracted by optical means; the frequency and the width of surface plasmon resonance band depend on the nanoparticle shape and size, their concentration, the inter-particle distance and the dielectric properties of material in which the particles are embedded. The aluminum arsenide crystallinity was studied by two techniques: Raman spectroscopy and Rutherford backscattering spectrometry in channelling configuration (RBS/ channelling). The Au concentration in the nanocomposite layers was deducted from RBS results. The size distribution and metallic nanoparticles shape transformation in both nanocomposites were observed by electronic transmission microscopy. The results obtained within the framework of this work are the subject of three journal papers. The first publication shows the possibility of manipulating the width and spectral position of the gold nanoparticle absorption band in Au/SiO2 nanocomposites by modifying their structure (form, size and inter-particle distance). The obtained Au nanoparticles are nearly spherical. The surface plasmon (PS) absorption band corresponding to the distant particles is located at 520 nm. After ion irradiation, the spherical nanoparticles transform into ellipsoids aligned along the ion beam. The absorption band splits into two bands: transversal and longitudinal. The band corresponding to the ellipsoids small axis (transversal) is blue-shifted and that corresponding to the long axis (longitudinal) is red-shifted indicating the elongation of particles in the beam direction. The second paper is consecrated to the crucial role of the plastic deformation of the matrix and to the importance of the metal atomic mobility in the anisotropic nanoparticles deformation in Au/SiO2 nanocomposites. Our measurements show that a threshold value of 2 keV/nm (electronic stopping power) is necessary for the deformation of Au nanoparticles. This value is close to that required for silica deformation. Mobility of the Au atoms at the time of the ion passage is confirmed by temperature calculation within the ionic track. The third paper treats the attempt of formation and deformation of Au nanoparticles in crystalline aluminum arsenide matrix known by its high resistance to amorphisation and deformation under ionic bombardment. The principal result of the last article confirms the essential role of the matrix. It proves that the anisotropic deformation of surrounding material is indispensable for gold nanoparticles deformation. The experimental results mentioned above and temperature calculations within ionic tracks allowed us to propose the following anisotropic deformation scenario of Au nanoparticles embedded in Au/SiO2 nanocomposite: - Each ion crossing the silica melts (very briefly) a narrow cylinder around its trajectory forming thus a latent track. This is consistent with the observed threshold value in the electronic stopping power. - The cumulative effect of many separate ion impacts leads to the anisotropic growth of the silica matrix which contracts in the direction of the beam and elongates in the perpendicular direction. The overlap model of the ionic tracks was used to validate this phenomenon. - The deformation of silica generates strains which act on the nanoparticles in the plane perpendicular to the ion trajectory. In order to accommodate these strains, the Au nanoparticles deform in the beam direction. - The deformation of nanoparticles occurs each time an ion traverses the gold particle and melts a cylinder around its trajectory. The mobility of the gold atoms was confirmed by a calculation of the equivalent temperature from the deposited energy in the material by incident ions. The scenario above is compatible with our experimental data obtained in the case of the Au/SiO2 nanocomposite. It is further supported by the fact that the Au nanoparticules do not deform when they are integrated in AlAs which is resistant to the deformation.

<p>In high-temperature superconductors a large region of the magnetic phase diagram is occupied by a vortex phase that displays a number of exciting phenomena. At low temperatures, vortices form a truly superconducting solid phase which at high temperatures turns into a dissipative vortex liquid. The character of the transition between these two phases depends on the amount and type of disorder present in the system. For weak point disorder the vortex solid-to-liquid transition is a first-order melting. In the presence of strong point disorder the solid is thought to be a vortex-glass and the transition into the liquid is instead of second order. When the disorder is correlated, like twin boundaries or artificially introduced columnar defects, the transition is also second order, but has essentially different properties. In this work, the transition between the solid and liquid phases of the vortex state has been studied by resistive transport measurements in mainly YBa2Cu3O7-[delta](YBCO) single crystals with different types of disorder.</p><p>The vortex-glass transition has been investigated in an extended model for the vortex-liquid resistivity close to the transition that takes into account both the temperature and magnetic field dependence of the transition line. The resistivity of samples with different properties was measured with various contact configurations at several magnetic fields and analyzed within this model. For each sample, attempts were made to scale the transition curves to one curve according to a suitable scaling variable predicted by the model. Good scaling was found in a number of different situations. The influence of increasing anisotropy and angular dependence of the magnetic field in the model were also considered.</p><p>The vortex solid-to-liquid transition was also studied in heavy-ion irradiated YBCO single crystals. The ions create columnar defects in the sample that act as correlated disorder. A magnetic field was applied at a tilt angle with respect to the direction of the columns. At the transition the resistance disappears as a power law with different exponents in the three orthogonal directions considered. This provides evidence for a new type of critical behavior with fully anisotropic critical scaling properties not previously found in any physical system.</p><p>The effect on the vortex solid-to-liquid transition of high magnetic fields applied parallel to the superconducting layers of underdoped YBCO single crystals was also studied. Some novel features were observed: a sharp kink appearing close to Tc at high magnetic fields and a triple dip in the angular dependence of the resistivity close to B||ab in some regions of the phase diagram.</p> / <p>I högtemperatursupraledare består en stor del av det magnetiska fasdiagrammet av en vortexfas som uppvisar ett flertal spännande fenomen. Vid låga temperaturer bildar vortexarna en fast vortexfas utan elektriskt motstånd. Vid högre temperatur övergår denna fas till en dissipativ vortexvätska. Egenskaperna hos denna fasövergång beror på oordningen i form av defekter. Vid svag punktoordning är fasomvandlingen mellan det fasta och flytande vortextillståndet en första ordningens smältövergång. Vid stark punktoordning anses den fasta fasen vara ett vortexglas och övergången till vortexvätskan är istället av andra ordningen. När oordningen är korrelerad, som för tvillinggränser eller artificiellt skapade kolumndefekter, är övergången också av andra ordningen men med väsentligt annorlunda egenskaper. I detta arbete har övergången mellan det fasta och det flytande vortextillståndet studerats med resistiva transportmätningar i framförallt enkristaller av YBa2Cu3O7-[delta] (YBCO) med olika typer av oordning.</p><p>Vortexglasövergången har undersökts i en utvidgad modell för resistansen i vortexvätskan nära fasövergången där hänsyn tas till såväl temperatur- som fältberoendet. Resistansen hos prover med olika egenskaper mättes i varierande magnetfält och i flera kontaktkonfigurationer och analyserades inom denna modell. Övergångskurvorna skalades till en kurva med en skalningsvariabel som givits av modellen. God skalning uppnåddes i flera olika fall. Effekten av ökande anisotropi och vinkelberoendet i modellen undersöktes också.</p><p>Vortexövergången mellan det fasta och det flytande vortextillståndet undersöktes även i enkristaller av YBCO bestrålade med tunga joner. Jonerna skapade kolumndefekter som fungerar som korrelerad oordning. Vinkeln mellan pålagt magnetfält och dessa kolumndefekter varierades. Vid fasövergången avtar resistansen som en potenslag med olika exponenter i de tre undersökta ortogonala riktningarna. Detta ger experimentell belägg för en ny typ av kritiskt beteende med fullständigt anisotropa kritiska skalningsegenskaper.</p><p>Egenskaparna hos på vortexövergången mellan fast och flytande fas vid höga magnetfält parallella med de supraledande lagren hos underdopade YBCO enkristaller undersöktes också. Några nya effekter observerades: en skarp knyck uppstod nära Tc vid höga magnetfält och en tredubbel dipp i den vinkelberoende resistiviteten nära B||ab i några regioner av fasdiagrammet.</p>

Résumé Dans la présente thèse, nous avons étudié la déformation anisotrope par bombardement ionique de nanoparticules d'or intégrées dans une matrice de silice amorphe ou d'arséniure d’aluminium cristallin. On s’est intéressé à la compréhension du mécanisme responsable de cette déformation pour lever toute ambigüité quant à l’explication de ce phénomène et pour avoir une interprétation consistante et unique. Un procédé hybride combinant la pulvérisation et le dépôt chimique en phase vapeur assisté par plasma a été utilisé pour la fabrication de couches nanocomposites Au/SiO2 sur des substrats de silice fondue. Des structures à couches simples et multiples ont été obtenues. Le chauffage pendant ou après le dépôt active l’agglomération des atomes d’Au et par conséquent favorise la croissance des nanoparticules. Les nanocomposites Au/AlAs ont été obtenus par implantation ionique de couches d’AlAs suivie de recuit thermique rapide. Les échantillons des deux nanocomposites refroidis avec de l’azote liquide ont été irradiés avec des faisceaux de Cu, de Si, d’Au ou d’In d’énergie allant de 2 à 40 MeV, aux fluences s'étendant de 1×1013 à 4×1015 ions/cm2, en utilisant le Tandem ou le Tandetron. Les propriétés structurales et morphologiques du nanocomposite Au/SiO2 sont extraites en utilisant des techniques optiques car la fréquence et la largeur de la résonance plasmon de surface dépendent de la forme et de la taille des nanoparticules, de leur concentration et de la distance qui les séparent ainsi que des propriétés diélectriques du matériau dans lequel les particules sont intégrées. La cristallinité de l’arséniure d’aluminium est étudiée par deux techniques: spectroscopie Raman et spectrométrie de rétrodiffusion Rutherford en mode canalisation (RBS/canalisation). La quantité d’Au dans les couches nanocomposites est déduite des résultats RBS. La distribution de taille et l’étude de la transformation de forme des nanoparticules métalliques dans les deux nanocomposites sont déterminées par microscopie électronique en transmission. Les résultats obtenus dans le cadre de ce travail ont fait l’objet de trois articles de revue. La première publication montre la possibilité de manipuler la position spectrale et la largeur de la bande d’absorption des nanoparticules d’or dans les nanocomposites Au/SiO2 en modifiant leur structure (forme, taille et distance entre particules). Les nanoparticules d’Au obtenues sont presque sphériques. La bande d’absorption plasmon de surface (PS) correspondante aux particules distantes est située à 520 nm. Lorsque la distance entre les particules est réduite, l’interaction dipolaire augmente ce qui élargit la bande de PS et la déplace vers le rouge (602 nm). Après irradiation ionique, les nanoparticules sphériques se transforment en ellipsoïdes alignés suivant la direction du faisceau. La bande d’absorption se divise en deux bandes : transversale et longitudinale. La bande correspondante au petit axe (transversale) est décalée vers le bleu et celle correspondante au grand axe (longitudinale) est décalée vers le rouge indiquant l’élongation des particules d’Au dans la direction du faisceau. Le deuxième article est consacré au rôle crucial de la déformation plastique de la matrice et à l’importance de la mobilité des atomes métalliques dans la déformation anisotrope des nanoparticules d’Au dans les nanocomposites Au/SiO2. Nos mesures montrent qu'une valeur seuil de 2 keV/nm (dans le pouvoir d'arrêt électronique) est nécessaire pour la déformation des nanoparticules d'or. Cette valeur est proche de celle requise pour la déformation de la silice. La mobilité des atomes d’Au lors du passage d’ions est confirmée par le calcul de la température dans les traces ioniques. Le troisième papier traite la tentative de formation et de déformation des nanoparticules d’Au dans une matrice d’arséniure d’aluminium cristallin connue pour sa haute résistance à l’amorphisation et à la déformation sous bombardement ionique. Le résultat principal de ce dernier article confirme le rôle essentiel de la matrice. Il s'avère que la déformation anisotrope du matériau environnant est indispensable pour la déformation des nanoparticules d’or. Les résultats expérimentaux mentionnés ci-haut et les calculs de températures dans les traces ioniques nous ont permis de proposer le scénario de déformation anisotrope des nanoparticules d’Au dans le nanocomposite Au/SiO2 suivant: - Chaque ion traversant la silice fait fondre brièvement un cylindre étroit autour de sa trajectoire formant ainsi une trace latente. Ceci a été confirmé par la valeur seuil du pouvoir d’arrêt électronique. - L’effet cumulatif des impacts de plusieurs ions conduit à la croissance anisotrope de la silice qui se contracte dans la direction du faisceau et s’allonge dans la direction perpendiculaire. Le modèle de chevauchement des traces ioniques (overlap en anglais) a été utilisé pour valider ce phénomène. - La déformation de la silice génère des contraintes qui agissent sur les nanoparticules dans les plans perpendiculaires à la trajectoire de l’ion. Afin d’accommoder ces contraintes les nanoparticules d’Au se déforment dans la direction du faisceau. - La déformation de l’or se produit lorsqu’il est traversé par un ion induisant la fusion d’un cylindre autour de sa trajectoire. La mobilité des atomes d’or a été confirmée par le calcul de la température équivalente à l’énergie déposée dans le matériau par les ions incidents. Le scénario ci-haut est compatible avec nos données expérimentales obtenues dans le cas du nanocomposite Au/SiO2. Il est appuyé par le fait que les nanoparticules d’Au ne se déforment pas lorsqu’elles sont intégrées dans l’AlAs résistant à la déformation. / Abstract In the present thesis, we study the anisotropic deformation of gold nanoparticles embedded in amorphous silica or crystalline aluminum arsenide, under ion bombardment. We try to comprehend the mechanism responsible for this deformation and to remove any ambiguity related to the explanation of this phenomenon. A hybrid process combining sputtering and plasma enhanced chemical vapour deposition was used to fabricate Au/SiO2 layers on fused silica substrates. Structures with single and multilayer were obtained. Heating during or after deposition activates the Au atom agglomeration and favours the growth of the nanoparticles. Also, a Au/AlAs nanocomposite was obtained by ion implantation of AlAs films, followed by rapid thermal annealing. The samples of the two nanocomposites, cooled with liquid nitrogen, were irradiated with 2 to 40 MeV Cu, Si, Au or In ion beams, at fluences ranging from 1×1013 to 4×1015 ions/cm2, using a Tandem or Tandetron accelerator. The structural and morphological properties of the Au/SiO2 nanocomposite were extracted by optical means; the frequency and the width of surface plasmon resonance band depend on the nanoparticle shape and size, their concentration, the inter-particle distance and the dielectric properties of material in which the particles are embedded. The aluminum arsenide crystallinity was studied by two techniques: Raman spectroscopy and Rutherford backscattering spectrometry in channelling configuration (RBS/ channelling). The Au concentration in the nanocomposite layers was deducted from RBS results. The size distribution and metallic nanoparticles shape transformation in both nanocomposites were observed by electronic transmission microscopy. The results obtained within the framework of this work are the subject of three journal papers. The first publication shows the possibility of manipulating the width and spectral position of the gold nanoparticle absorption band in Au/SiO2 nanocomposites by modifying their structure (form, size and inter-particle distance). The obtained Au nanoparticles are nearly spherical. The surface plasmon (PS) absorption band corresponding to the distant particles is located at 520 nm. After ion irradiation, the spherical nanoparticles transform into ellipsoids aligned along the ion beam. The absorption band splits into two bands: transversal and longitudinal. The band corresponding to the ellipsoids small axis (transversal) is blue-shifted and that corresponding to the long axis (longitudinal) is red-shifted indicating the elongation of particles in the beam direction. The second paper is consecrated to the crucial role of the plastic deformation of the matrix and to the importance of the metal atomic mobility in the anisotropic nanoparticles deformation in Au/SiO2 nanocomposites. Our measurements show that a threshold value of 2 keV/nm (electronic stopping power) is necessary for the deformation of Au nanoparticles. This value is close to that required for silica deformation. Mobility of the Au atoms at the time of the ion passage is confirmed by temperature calculation within the ionic track. The third paper treats the attempt of formation and deformation of Au nanoparticles in crystalline aluminum arsenide matrix known by its high resistance to amorphisation and deformation under ionic bombardment. The principal result of the last article confirms the essential role of the matrix. It proves that the anisotropic deformation of surrounding material is indispensable for gold nanoparticles deformation. The experimental results mentioned above and temperature calculations within ionic tracks allowed us to propose the following anisotropic deformation scenario of Au nanoparticles embedded in Au/SiO2 nanocomposite: - Each ion crossing the silica melts (very briefly) a narrow cylinder around its trajectory forming thus a latent track. This is consistent with the observed threshold value in the electronic stopping power. - The cumulative effect of many separate ion impacts leads to the anisotropic growth of the silica matrix which contracts in the direction of the beam and elongates in the perpendicular direction. The overlap model of the ionic tracks was used to validate this phenomenon. - The deformation of silica generates strains which act on the nanoparticles in the plane perpendicular to the ion trajectory. In order to accommodate these strains, the Au nanoparticles deform in the beam direction. - The deformation of nanoparticles occurs each time an ion traverses the gold particle and melts a cylinder around its trajectory. The mobility of the gold atoms was confirmed by a calculation of the equivalent temperature from the deposited energy in the material by incident ions. The scenario above is compatible with our experimental data obtained in the case of the Au/SiO2 nanocomposite. It is further supported by the fact that the Au nanoparticules do not deform when they are integrated in AlAs which is resistant to the deformation.

In high-temperature superconductors a large region of the magnetic phase diagram is occupied by a vortex phase that displays a number of exciting phenomena. At low temperatures, vortices form a truly superconducting solid phase which at high temperatures turns into a dissipative vortex liquid. The character of the transition between these two phases depends on the amount and type of disorder present in the system. For weak point disorder the vortex solid-to-liquid transition is a first-order melting. In the presence of strong point disorder the solid is thought to be a vortex-glass and the transition into the liquid is instead of second order. When the disorder is correlated, like twin boundaries or artificially introduced columnar defects, the transition is also second order, but has essentially different properties. In this work, the transition between the solid and liquid phases of the vortex state has been studied by resistive transport measurements in mainly YBa2Cu3O7-[delta](YBCO) single crystals with different types of disorder. The vortex-glass transition has been investigated in an extended model for the vortex-liquid resistivity close to the transition that takes into account both the temperature and magnetic field dependence of the transition line. The resistivity of samples with different properties was measured with various contact configurations at several magnetic fields and analyzed within this model. For each sample, attempts were made to scale the transition curves to one curve according to a suitable scaling variable predicted by the model. Good scaling was found in a number of different situations. The influence of increasing anisotropy and angular dependence of the magnetic field in the model were also considered. The vortex solid-to-liquid transition was also studied in heavy-ion irradiated YBCO single crystals. The ions create columnar defects in the sample that act as correlated disorder. A magnetic field was applied at a tilt angle with respect to the direction of the columns. At the transition the resistance disappears as a power law with different exponents in the three orthogonal directions considered. This provides evidence for a new type of critical behavior with fully anisotropic critical scaling properties not previously found in any physical system. The effect on the vortex solid-to-liquid transition of high magnetic fields applied parallel to the superconducting layers of underdoped YBCO single crystals was also studied. Some novel features were observed: a sharp kink appearing close to Tc at high magnetic fields and a triple dip in the angular dependence of the resistivity close to B||ab in some regions of the phase diagram. / I högtemperatursupraledare består en stor del av det magnetiska fasdiagrammet av en vortexfas som uppvisar ett flertal spännande fenomen. Vid låga temperaturer bildar vortexarna en fast vortexfas utan elektriskt motstånd. Vid högre temperatur övergår denna fas till en dissipativ vortexvätska. Egenskaperna hos denna fasövergång beror på oordningen i form av defekter. Vid svag punktoordning är fasomvandlingen mellan det fasta och flytande vortextillståndet en första ordningens smältövergång. Vid stark punktoordning anses den fasta fasen vara ett vortexglas och övergången till vortexvätskan är istället av andra ordningen. När oordningen är korrelerad, som för tvillinggränser eller artificiellt skapade kolumndefekter, är övergången också av andra ordningen men med väsentligt annorlunda egenskaper. I detta arbete har övergången mellan det fasta och det flytande vortextillståndet studerats med resistiva transportmätningar i framförallt enkristaller av YBa2Cu3O7-[delta] (YBCO) med olika typer av oordning. Vortexglasövergången har undersökts i en utvidgad modell för resistansen i vortexvätskan nära fasövergången där hänsyn tas till såväl temperatur- som fältberoendet. Resistansen hos prover med olika egenskaper mättes i varierande magnetfält och i flera kontaktkonfigurationer och analyserades inom denna modell. Övergångskurvorna skalades till en kurva med en skalningsvariabel som givits av modellen. God skalning uppnåddes i flera olika fall. Effekten av ökande anisotropi och vinkelberoendet i modellen undersöktes också. Vortexövergången mellan det fasta och det flytande vortextillståndet undersöktes även i enkristaller av YBCO bestrålade med tunga joner. Jonerna skapade kolumndefekter som fungerar som korrelerad oordning. Vinkeln mellan pålagt magnetfält och dessa kolumndefekter varierades. Vid fasövergången avtar resistansen som en potenslag med olika exponenter i de tre undersökta ortogonala riktningarna. Detta ger experimentell belägg för en ny typ av kritiskt beteende med fullständigt anisotropa kritiska skalningsegenskaper. Egenskaparna hos på vortexövergången mellan fast och flytande fas vid höga magnetfält parallella med de supraledande lagren hos underdopade YBCO enkristaller undersöktes också. Några nya effekter observerades: en skarp knyck uppstod nära Tc vid höga magnetfält och en tredubbel dipp i den vinkelberoende resistiviteten nära B||ab i några regioner av fasdiagrammet. / QC 20110125

Les carcinomes épidermoïdes de la tête et du cou sont souvent de mauvais pronostic, en raison de leur résistance aux traitements suivie de récidives loco-régionales, voire de métastases. Ce travail s'est focalisé sur le rôle des cellules souches cancéreuses (CSC) dans la radiorésistance d'un modèle cellulaire de cancer du larynx, SQ20B, ainsi que sur leur ciblage thérapeutique en association avec la radiothérapie photonique ou par ions carbone. Une sous-population a été isolée à partir de la lignée SQ20B par tris cellulaires successifs selon 3 critères spécifiques des CSC de tumeurs ORL : exclusion du Hoechst 33342, expression de CD44 et activité élevée de l'aldéhyde déshydrogénase (ALDH). Les cellules SQ20B/SP/CD44 high/ALDHhigh présentent bien les caractéristiques de CSC (tumorisphères, tumorigénèse, radiorésistance). La résistance des CSC aux 2 types d'irradiation, par rapport aux cellules « non souche » SQ20B/SP/CD44low/ALDHlow, implique une diminution de la mort par apoptose, une augmentation des capacités prolifératives ainsi qu'une surexpression de la voie de l'autorenouvellement Bmi1. L'effet radiosensibilisant de 3 molécules ciblant les CSC a été démontré : la mort apoptotique induite par l'UCN-01 en inhibant l'arrêt en phase G2/M ; les capacités prolifératives ciblées par l'acide trans-rétinoïque (ATRA) induisant la différenciation ; et la voie de l'autorenouvellement Bmi-1 inhibée par l'artésunate. Seule ou associées (UCN-01 + ATRA), elles agissent en synergie avec une irradiation par photons ou ions carbone. Des études pré-clinique, puis clinique, devraient confirmer l'intérêt du ciblage des CSC dans le contrôle de l'échappement de ces cancers radiorésistants / Head and neck squamous cell carcinomas (HNSCC) have a poor prognosis, due to their resistance to standard treatments. In most cases, locoregional recurrence or metastases occur. This study has focused on the role of cancer stem cells (CSC) in the radioresistance of the SQ20B HNSCC cell line and their therapeutic targeting in association with photon or carbon ions irradiation. A subpopulation of SQ20B-CSC has been isolated by cell sorting based on 3 specific characteristics of HNSCC-CSC : Hoechst 33342 exclusion, CD44 expression and high aldehyde dehydrogenase activity (ALDH). SQ20B/SP/CD44high/ALDHhigh cells show the CSC characteristics (in vitro and in vivo tumorigenesis, high radioresistance). The response of CSC to both types of irradiation was compared to the non-“stem cells” SQ20B/SP/CD44low sub-population. The observed radioresistance involves a decrease in apoptotic cell death, an increase in proliferative capacities and an overexpression of the Bmi1 self-renewing signaling pathway. The radiosensitizing effects of 3 molecules targeting the CSC has been demonstrated : an induction of apoptotic cell death by the inhibition of the G2/M phase arrest after a treatment with UCN01 ; an inhibition of proliferative capacities using the all-trans-retinoic acid (ATRA) which induce their differentiation ; and an inhibition of Bmi1 by artesunate. These treatments, alone or in combination (UCN01+ATRA) have a synergistic effect with photon or carbon ion irradiation to overcome CSC radioresistance. Preclinical and clinical studies should confirm the benefit of targeting CSC and improve the control of tumor escape in patients with radioresistant HNSCC cancers

V této práci je představeno zařízení pro ozařování MeV ionty při tandemovém urychlovači na univerzitě v Uppsale. Jsou podány základy teorie interakce iontů s pevnou látkou a modifikace materiálu pomocí iontů s vysokou energií. Zařízení tandemového urychlovače je popsáno počínaje generací iontů a konče dopadem iontů na vzorek v hlavní komoře zařízení pro iontové ozařování. Následně jsou detailně charakterizovány modifikace systému pro přesun vzorků a popsán princip jeho funkce. Pilotní aplikace upraveného systému v oblasti materiálových modifikací je prezentována na příkladu ozařování Ge kvantových teček. Homogenita rozložení iontů na vzorku při ozařování je testována pomocí simulace elektrostatického deflektoru.

FeCrAl alloys are being investigated as candidate materials for replacing zirconium based alloys as nuclear reactor fuel cladding because of their superior high temperature oxidation resistance in steam environments. Unirradiated FeCrAl as well as Fe²⁺ ion irradiated FeCrAl to a peak dose of 20DPA were mechanically tested and compared against each other. Nanohardness tests were performed on both the unirradiated and irradiated conditions and it was found that the irradiated alloy was about 1GPa harder than its unirradiated counterpart. TEM <i>in situ</i> tensile tests were performed using the Bruker push to pull device alongside a PI95 Picoindenter on single crystals with grain orientations 001, 011 and 111. The unirradiated 001 grains tended to fail without yielding in a brittle manner while the irradiated 001 grain yielded and reached an ultimate tensile strength before failure. The unirradiated 011 grains behaved in a mixed manner, where one failed without yielding and one slipped many times before failing. The irradiated 011 grain yielded and failed quickly thereafter. The unirradiated 111 grain yielded, slipped and twinned before failing and both irradiated 111 grains slipped. Two general trends were observed. One, each unirradiated single grain was stronger than its irradiated counterpart. This trend is indicative of the ion irradiated microstructure facilitating bulklike mechanical behavior in the irradiated samples whereas the unirradiated samples exhibited mechanical size effects due to either the total lack of preexisting defects or the ability for existing defects to escape easily to the surface of the sample resulting in a pristine, defect free sample. Two, regardless of irradiation condition, the 001 grain orientation was brittle, the 011 grain orientation deformed in a mixed brittle/ductile manner and the 111 grain orientation was ductile through all tests. These results are indicative of the geometry of the BCC crystal structure and the slip system involving these orientations.

Self-organization is a hot topic as it has the potential to create surface patterns on the nanoscale avoiding cost-intensive top-down approaches. Although chemists have promising results in this area, ion irradiation can create self-organized surface patterns in a more controlled manner. Different regimes of pattern formation under ion irradiation were described so far by 2D models. Here, two new regimes have been studied experimentally, which require modeling in 3D: subsurface point defect kinetics as well as ion impact-induced melt pool formation. This thesis deals with self-organized pattern formation on Ge and Si surfaces under normal incidence irradiation with heavy monatomic and polyatomic ions of energies up to several tens of keV. Irradiation has been performed using liquid metal ion sources in a focused ion beam facility with mass-separation as well as by conventional broad beam ion implantation. Irradiated samples have been analyzed mainly by scanning electron microscopy. Related to the specific irradiation conditions, investigation and discussion of pattern formation has been divided into two parts: (i) formation of Ge morphologies due to point defect kinetics and (ii) formation of Ge and Si morphologies due to melt pool dynamics. Point defect kinetics dominates pattern formation on Ge under irradiation with monatomic ions at room temperature. Irradiation of Ge with Bi and Ge ions at fluences up to 10^17 cm^(-2) has been performed. Comprehensive studies show for the first time that morphologies change from flat surfaces over hole to nanoporous, sponge-like patterns with increasing ion energy. This study is consistent with former irradiations of Ge with a few ion energies. Based on my studies, a consistent, qualitative 3D model of morphology evolution has been developed, which attributes the ion energy dependency of the surface morphology to the depth dependency of point defect creation and relaxation. This model has been proven by atomistic computer experiments, which reproduce the patterns found in real irradiation experiments. At extremely high energy densities deposited by very heavy ions another mechanism dominates pattern formation. The formation of Ge and Si dot patterns by very heavy, monatomic and polyatomic Bi ion irradiation has been studied in detail for the first time. So far, this formation of pronounced dot pattern cannot be explained by any model. Comprehensive, experimental studies have shown that pattern formation on Ge is related to extremely high energy densities deposited by each polyatomic ion locally. The simultaneous impact of several atoms leads to local energy densities sufficient to cause local melting. Heating of Ge substrates under ion irradiation increases the achievable energy density in the collision cascade substantially. This prediction has been confirmed experimentally: it has been found that the threshold for nanomelting can be lowered by substrate heating, which allows pattern formation also under heavy, monatomic ion irradiation. Extensive studies of monatomic Bi irradiation of heated Ge have shown that morphologies change from sponge-like over highly regular dot patterns to smooth surfaces with increasing substrate temperature. The change from sponge-like to dot pattern is correlated to the melting of the ion collision cascade volume, with energy densities sufficient for melt pool formation at the surface. The model of pattern formation on Ge due to extremely high deposited energy densities is not specific to a single element. Therefore, Si has been studied too. Dot patterns have been found for polyatomic Bi ion irradiation of hot Si, which creates sufficiently high energy densities to allow ion impact-induced melt pool formation. This proves that pattern formation by melt pool formation is a novel, general pattern formation mechanism. Using molecular dynamics simulations of project partners, the correlation between dot patterning and ion impact-induced melt pool formation has been proven. The driving force for dot pattern formation due to high deposited energy densities has been identified and approximated in a first continuum description.