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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
21

Diode-Pumped High-Energy Laser Amplifiers for Ultrashort Laser Pulses The PENELOPE Laser System

Löser, Markus 16 November 2017 (has links)
The ultrashort chirped pulse amplification (CPA) laser technology opens the path to high intensities of 10^21 W/cm² and above in the laser focus. Such intensities allow laser-matter interaction in the relativistic intensity regime. Direct diode-pumped ultrashort solid-state lasers combine high-energy, high-power and efficient amplification together, which are the main advantages compared to flashlamp-pumped high-energy laser systems based on titanium-doped sapphire. Development within recent years in the field of laser diodes makes them more and more attractive in terms of total costs, compactness and lifetime. This work is dedicated to the Petawatt, ENergy-Efficient Laser for Optical Plasma Experiments (PENELOPE) project, a fully and directly diode-pumped laser system under development at the Helmholtz–Zentrum Dresden – Rossendorf (HZDR), aiming at 150 fs long pulses with energies of up to 150 J at repetition rates of up to 1 Hz. The focus of this thesis lies on the spectral and width manipulation of the front-end amplifiers, trivalent ytterbium-doped calcium fluoride (Yb3+:CaF2) as gain material as well as the pump source for the final two main amplifiers of the PENELOPE laser system. Here, all crucial design parameters were investigated and a further successful scaling of the laser system to its target values was shown. Gain narrowing is the dominant process for spectral bandwidth reduction during the amplification at the high-gain front-end amplifiers. Active or passive spectral gain control filter can be used to counteract this effect. A pulse duration of 121 fs was achieved by using a passive spectral attenuation inside a regenerative amplifier, which corresponds to an improvement by a factor of almost 2 compared to the start of this work. A proof-of-concept experiment showed the capability of the pre-shaping approach. A spectral bandwidth of 20nm was transferred through the first multipass amplifier at a total gain of 300. Finally, the predicted output spectrum calculated by a numerical model of the final amplifier stages was in a good agreement with the experimental results. The spectroscopic properties of Yb3+:CaF2 matches the constraints for ultrashort laser pulse amplification and direct diode pumping. Pumping close to the zero phonon line at 976nm is preferable compared to 940nm as the pump intensity saturation is significantly lower. A broad gain cross section of up to 50nm is achievable for typical inversion levels. Furthermore, moderate cryogenic temperatures (above 200K) can be used to improve the amplification performance of Yb3+:CaF2. The optical quality of the doped crystals currently available on the market is sufficient to build amplifiers in the hundred joule range. The designed pump source for the last two amplifiers is based on two side pumping in a double pass configuration. However, this concept requires the necessity of brightness conservation for the installed laser diodes. Therefore, a fully relay imaging setup (4f optical system) along the optical path from the stacks to the gain material including the global beam homogenization was developed in a novel approach. Beside these major parts the amplifier architecture and relay imaging telescopes as well as temporal intensity contrast (TIC) was investigated. An all reflective concept for the relay imaging amplifiers and telescopes was selected, which results in several advantages especially an achromatic behavior and low B-Integral. The TIC of the front-end was improved, as the pre- and postpulses due to the plane-parallel active-mirror was eliminated by wedging the gain medium.
22

Examination of Surface Morphology and Sub-Surface Crystallographic Changes of Si, Cu, GaP and Ge After Ultrashort Laser Pulse Irradiation

Crawford, Travis H. R. 10 1900 (has links)
This thesis reports the effects of ultrashort laser pulse irradiation of various materials. The morphology after irradiation was examined using several microscopy techniques. Emphasis was placed on the identification of crystallographic changes and the analysis of laser-induced periodic surface structures. Grooves were machined in silicon by translating the target under the focused laser beam. The resulting depths were measured as a function of pulse energy, translation speed, and number of consecutive passes, for 800 and 400nm wavelength irradiation. The wall morphology and a corrugation along the bottom of the grooves were characterized. Various polarization configurations relative to the translation direction were compared. Such characterizations are relevant for the practical application of femtosecond laser micromachining. Silicon and gallium phosphide exhibited periodic structures after irradiation using photon energies less than the bandgap energy, with periods as small as ~20% of the irradiation wavelength. The significantly sub-wavelength periodic structures had a shallow profile on silicon, appearing as fine lines or grids of protrusions and depressions. On gallium phosphide, the surface evolved into planar-like structures with a large aspect ratio, possessing crystalline centers coated with amorphous material. These investigations, along with additional experiments, would help identify the precise physical origins of the short-period structures. On silicon and germanium, the target crystal orientation was shown to affect the formation of certain morphological features. For multiple-pulse irradiation, the (100) and (111) surface orientations exhibited significantly different tendencies for large conical structure formation. A thin layer of defected material coated the conical structures, with some defects present within the periodic structures. The different crystalline orientations did not affect periodic structuring. Cross-sectional transmission electron microscopy of silicon after irradiation by single pulses revealed amorphous material and dislocations in the bulk for sufficiently high pulse fluences. On a sample consisting of a metal layer on thermally-grown oxide on silicon, a range of pulse fluences was found which removed the metal layer without observed thinning of the oxide layer. Within this fluence range, above a particular fluence substantial defects were formed in the underlying silicon. Although ultrashort pulse irradiation of materials is frequently considered to be 'damage-free', attention should be paid to sub-surface modifications not evident from surface imaging. For the drilling of holes in copper foils, the pulse duration did not strongly affect the final morphology for durations under several picoseconds. A photodiode below the foil during drilling recorded transmitted light, indicating the number of pulses required for penetration under a variety of conditions, and characterizing hole evolution during drilling. Periodic surface structuring on the walls of holes depended on the irradiation atmosphere, pulse duration, and laser polarization. These measurements provide insight into the physical processes of material modification, and for the selection of irradiation parameters in practical applications. / Thesis / Doctor of Philosophy (PhD)
23

Study of ultrashort laser-pulse induced ripples formed at the interface of silicon-dioxide on silicon

Liu, Bing 04 1900 (has links)
<p>In this thesis, the ripple formation at the interface of SiO2 and Si were studied in a systematic fashion by irradiating the SiO2-Si samples with ultrashort laser pulses under a broad variety of experimental conditions. They consist of di↵erent irradiating laser wavelengths, incident laser energies, translation speeds, translation directions, spot sizes of the laser beam, as well as oxide thicknesses. The ripples produced by laser irradiation are examined using various microscopy techniques in order to characterize their surface morphology, detailed structures, crystalline properties, and so on. For the experiments carried out at ! = 800 nm, the ripples formed on the SiO2-Si sample with an oxide thickness of 216 nm were first observed under optical microscopy and SEM. After removing the oxide layer with HF solution, the surface features of the ripples on the Si substrate were investigated using SEM and AFM techniques. Subsequently, by means of TEM and EDX analysis, the material composition and crystallinity of the ripples were determined. It is concluded that the ripples are composed of nano-crystalline silicon. In addition to the 216 nm oxide thickness, other oxide samples with di↵erent oxide thicknesses, such as 24, 112, 117, 158 and 1013 nm, were also processed under laser irradiation. The ripple formation as a function of the laser energy, the translation direction and the spot size is discussed in detail. Furthermore, the ripples created at the SiO2-Si interface are compared with</p> <p>the LIPSS created on pure silicon samples that were processed under similar laser irradiation conditions. The spatial periodicities of the ripples were evaluated to be in the range of between 510 nm and 700 nm, which vary with the oxide thickness and other laser parameters. For the experiments using the ! = 400 nm laser pulses, it is found that ripples can also be formed at the SiO2-Si interface, which have spatial periodicities in the range of between 310 nm and 350 nm depending on the oxide thickness. The ripple formation at this 400 nm wavelength as a function of the laser energy, the translation speed, and translation direction is considered as well. For the case of ! = 400 nm irradiation, a comparison is also made between the interface ripples on the SiO2-Si samples and the LIPSS on a pure Si sample. Through FIB-TEM and EDX analysis, it confirmed that the ripples were produced in the substrate while the oxide layer maintained its structural integrity. In addition, the ripples are composed of nano-crystalline silicon whose crystallite sizes are on the order of a few nanometers. Apart from irradiating oxide samples with femtosecond laser pulses, which applies to the two cases of ! = 800 and 400 nm mentioned above, oxide samples with an oxide thickness of 112 nm were irradiated with picosecond laser pulses at ! = 800 nm whose pulse durations are 1 ps and 5 ps, respectively. However, no regular ripples can be produced at the SiO2-Si interface while maintaining the complete integrity of the oxide layer.</p> / Master of Applied Science (MASc)
24

Etude de matériaux solides solgel présentant la proprieté de transmission saturable.

Brunel, Marc 09 January 1996 (has links) (PDF)
Le développement rapide des sources lumineuses intenses, accordables en longueur d'onde, représente une menace croissante pour les différents détecteurs existant, et tout particulièrement l'il. Une méthode de protection envisageable est l'utilisation de composes organiques presentant un comportement d'absorption saturable inverse: leur absorption augmente lorsqu'ils sont eclaires par des faisceaux lumineux tres intenses. En utilisant le procede sol-gel, nous avons pu élaborer des materiaux solides compacts dopes avec des molecules de la famille des phtalocyanines. A la longueur d'onde de 532 nanometres, des echantillons de transmission initiale 0,7, ont permis d'induire une densite optique de 1 sous l'effet d'impulsions de forte densite. Avec des echantillons de transmission lineaire 0,4, la densité optique induite est egale a 1,6. Afin de mieux comprendre le processus de saturation de la transmission, nous avons écrit des programmes informatiques permettant de simuler le comportement observe. Ils se sont averes etre d'excellents outils pour mieux cerner les phenomenes mis en jeu. Pour améliorer les performances obtenues, differents types de synthèses ont ete entrepris, et differentes molecules organiques ont ete introduites dans des matrices sol-gel: des tetrabenzoporphyrines, des molécules de fullerènes et de hitci. Pour déterminer les plages spectrales d'efficacité de ces echantillons, des sources impulsionnelles accordables en longueur d'onde ont ete installees. Apres la synthèse de premiers échantillons efficaces dans la partie bleue du spectre visible, il a ete possible d'en elaborer d'autres efficaces dans la partie rouge du spectre. Disposant de materiaux actifs a la longueur d'onde de 620 nanomètres, nous avons alors pu montrer a cette longueur d'onde qu'il s'agit d'un processus ultrarapide qui intervient en moins de cent femtosecondes. Enfin, en utilisant les programmes de simulation developpes, nous avons étudie les performances que nous sommes en droit d'esperer de composes absorbants saturables inverses qui seraient inseres dans un systeme limiteur optique.
25

Propriétés magnétiques, orbitales et de transport d'hétérostructures basées sur LaMnO3

Galdi, Alice 14 April 2011 (has links) (PDF)
Dans la thèse nous traitons les propriétés magnétiques, orbitales et de transport des super-réseaux (LaMnO3) 2N (SrMnO3) N et des couches minces de LaxMnO3-d déposées par épitaxie à jet moléculaire (MBE) sur des substrats SrTiO3. Ces super-réseaux représentent un nouveau genre d'hétérostructure, récemment très étudié, composée par un nombre entier de mailles, où des effets de reconstruction électronique aux interfaces sont prévus. Dans la première partie du travail de thèse, des techniques de lithographie optique et des différentes techniques de dépôt sont utilisées afin d'effectuer des mesures de transport avec courant perpendiculaire à la surface des échantillons (CPP) et sous l'effet de champ électrique. La technique CPP peut donner de l'information supplémentaire sur les interfaces par rapport aux mesures de transport traditionnelles. L'effet de champ a été largement étudié dans des systèmes de manganite, puisque il représente une méthode pour changer la densité de porteurs, et afin de fabriquer des dispositifs à effet de champ avec des oxydes. On rapporte les résultats de l'optimisation de telles techniques, ainsi que l'optimisation des matériaux utilisés en tant qu'électrode de base, isolateur de flanc ou de barrière et électrode supérieure. Dans la deuxième partie de la thèse, les deux systèmes sont étudiés par des techniques traditionnelles (transport, aimantation par SQUID) et par des techniques d'absorption et d'émission de rayon X par rayonnement de synchrotron. Des informations précieuses sur le ferromagnétisme, l'antiferromagnétisme et l'ordre orbital sont obtenues.
26

Simulations quantiques non-adiabatiques d’un photo-interrupteur moléculaire vers un dialogue expérience-théorie / Quantum non-adiabatic simulations of a molecular photoswitch to a experimental-theoretical collaboration

Gonon, Benjamin 21 November 2017 (has links)
Cette thèse a pour objet l’étude et le contrôle de la photo-réactivité d’interrupteurs moléculaires, en particulier la photo-isomérisation des spiropyranes. Ce travail théorique a été réalisé en collaboration étroite avec l’équipe expérimentale PFL de l’ICB à Dijon. Des simulations de dynamique quantique non-adiabatique ont été réalisées afin de reproduire et rationaliser les résultats expérimentaux de spectroscopie d’absorption transitoire résolue en temps. Ces expériences ont montré une photo-réactivité ultra-rapide (~ 100 fs) suite à une excitation par une pulse LASER ultra-court. Celle-ci est interprétée comme un mécanisme de conversion interne entre le premier état électronique excité singulet et l’état fondamental via une intersection conique. L’étude théorique a utilisé la réaction d’ouverture de cycle du benzopyrane comme modèle. Les développements réalisés ont porté sur : (1) L’exploration du mécanisme réactionnel et le calcul de surfaces d’énergie potentielle via des méthodes de chimie quantique post-CASSCF perturbatives (XMCQDPT2). Cette analyse a montré des résultats variant fortement par rapport à ceux relevés dans la littérature à des niveaux de calcul moins élevés. (2) Le développement d’un modèle de surfaces d’énergie potentielle électronique par la construction d’un hamiltonien diabatique à partir de données ab initio XMCQDPT2. Du fait de l’importante anharmonicité de l’état électronique fondamental, nous avons mis en place une approche effective en rupture avec les études antérieures. (3) La réalisation de simulations de dynamique quantique non-adiabatique par la méthode MCTDH. Les résultats obtenus sont en très bon accord avec les résultats expérimentaux. L’inclusion explicite du pulse LASER a permis de reproduire et de rationaliser l’effet de contrôle par mise en forme d’impulsion observé expérimentalement. Ce travail a ainsi permis la mise en place d’une collaboration et d’un dialogue théorie/expérience effectifs. / This thesis adresses the study and control of the photo-reactivity of molecular switches, here the photo-isomerisation of spiropyrans. This theoretical work has been achieved in close collaboration with the experimental team PFL within the ICB in Dijon. Non-adiabatic quantum dynamics simulations were carried out so as to reproduce and rationalise the experimental results from time-resolved transient absorption spectroscopy. Such experiments have demonstrated ultra-fast photo-reactivity (~ 100 fs) following excitation by an ultra-short LASER pulse. It is interpreted as an internal conversion mechanism between the first singlet excited eletronic state and the ground state via a conical intersection. The theoretical study used the ring-opening reaction of benzopyran as a model. Developments were made regarding: (1) The exploration of the reaction mechanism and the computation of potential energy surfaces with perturbative, post-CASSCF quantum chemistry methods (XMCQDPT2). This investigation showed that results changed significantly compared to those reported in the literature with lower-level calculations. (2) The generation of a diabatic Hamiltonian based on ab initio XMCQDPT2 data. Owing to the significant anharmonicity in the ground electronic state, we designed a new effective approach, quite different from the previous studies. (3) The production of non-adiabatic quantum dynamics simulations using the MCTDH method. The results thus obtained are in excellent agreement with the experimental ones. Including explicitly the LASER pulse allowed us to reproduce and rationalise the action of pulse shaping on control observed in experiments. The present work thus made possible the succesful implementation of a theoretical/experimental collaboration.
27

Diode-Pumped High-Energy Laser Amplifiers for Ultrashort Laser Pulses / Diodengepumpte hochenergetische Laserverstärker für ultrakurze Laserpulse. Das PENELOPE Lasersystem

Loeser, Markus 22 January 2018 (has links) (PDF)
The ultrashort chirped pulse amplification (CPA) laser technology opens the path to high intensities of 10^21 W/cm² and above in the laser focus. Such intensities allow laser-matter interaction in the relativistic intensity regime. Direct diode-pumped ultrashort solid-state lasers combine high-energy, high-power and efficient amplification together, which are the main advantages compared to flashlamp-pumped high-energy laser systems based on titanium-doped sapphire. Development within recent years in the field of laser diodes makes them more and more attractive in terms of total costs, compactness and lifetime. This work is dedicated to the Petawatt, ENergy-Efficient Laser for Optical Plasma Experiments (PENELOPE) project, a fully and directly diode-pumped laser system under development at the Helmholtz–Zentrum Dresden – Rossendorf (HZDR), aiming at 150 fs long pulses with energies of up to 150 J at repetition rates of up to 1 Hz. The focus of this thesis lies on the spectral and width manipulation of the front-end amplifiers, trivalent ytterbium-doped calcium fluoride (Yb3+:CaF2) as gain material as well as the pump source for the final two main amplifiers of the PENELOPE laser system. Here, all crucial design parameters were investigated and a further successful scaling of the laser system to its target values was shown. Gain narrowing is the dominant process for spectral bandwidth reduction during the amplification at the high-gain front-end amplifiers. Active or passive spectral gain control filter can be used to counteract this effect. A pulse duration of 121 fs was achieved by using a passive spectral attenuation inside a regenerative amplifier, which corresponds to an improvement by a factor of almost 2 compared to the start of this work. A proof-of-concept experiment showed the capability of the pre-shaping approach. A spectral bandwidth of 20nm was transferred through the first multipass amplifier at a total gain of 300. Finally, the predicted output spectrum calculated by a numerical model of the final amplifier stages was in a good agreement with the experimental results. The spectroscopic properties of Yb3+:CaF2 matches the constraints for ultrashort laser pulse amplification and direct diode pumping. Pumping close to the zero phonon line at 976nm is preferable compared to 940nm as the pump intensity saturation is significantly lower. A broad gain cross section of up to 50nm is achievable for typical inversion levels. Furthermore, moderate cryogenic temperatures (above 200K) can be used to improve the amplification performance of Yb3+:CaF2. The optical quality of the doped crystals currently available on the market is sufficient to build amplifiers in the hundred joule range. The designed pump source for the last two amplifiers is based on two side pumping in a double pass configuration. However, this concept requires the necessity of brightness conservation for the installed laser diodes. Therefore, a fully relay imaging setup (4f optical system) along the optical path from the stacks to the gain material including the global beam homogenization was developed in a novel approach. Beside these major parts the amplifier architecture and relay imaging telescopes as well as temporal intensity contrast (TIC) was investigated. An all reflective concept for the relay imaging amplifiers and telescopes was selected, which results in several advantages especially an achromatic behavior and low B-Integral. The TIC of the front-end was improved, as the pre- and postpulses due to the plane-parallel active-mirror was eliminated by wedging the gain medium.
28

Diode-Pumped High-Energy Laser Amplifiers for Ultrashort Laser Pulses: The PENELOPE Laser System

Löser, Markus 22 January 2018 (has links)
The ultrashort chirped pulse amplification (CPA) laser technology opens the path to high intensities of 10^21 W/cm² and above in the laser focus. Such intensities allow laser-matter interaction in the relativistic intensity regime. Direct diode-pumped ultrashort solid-state lasers combine high-energy, high-power and efficient amplification together, which are the main advantages compared to flashlamp-pumped high-energy laser systems based on titanium-doped sapphire. Development within recent years in the field of laser diodes makes them more and more attractive in terms of total costs, compactness and lifetime. This work is dedicated to the Petawatt, ENergy-Efficient Laser for Optical Plasma Experiments (PENELOPE) project, a fully and directly diode-pumped laser system under development at the Helmholtz–Zentrum Dresden – Rossendorf (HZDR), aiming at 150 fs long pulses with energies of up to 150 J at repetition rates of up to 1 Hz. The focus of this thesis lies on the spectral and width manipulation of the front-end amplifiers, trivalent ytterbium-doped calcium fluoride (Yb3+:CaF2) as gain material as well as the pump source for the final two main amplifiers of the PENELOPE laser system. Here, all crucial design parameters were investigated and a further successful scaling of the laser system to its target values was shown. Gain narrowing is the dominant process for spectral bandwidth reduction during the amplification at the high-gain front-end amplifiers. Active or passive spectral gain control filter can be used to counteract this effect. A pulse duration of 121 fs was achieved by using a passive spectral attenuation inside a regenerative amplifier, which corresponds to an improvement by a factor of almost 2 compared to the start of this work. A proof-of-concept experiment showed the capability of the pre-shaping approach. A spectral bandwidth of 20nm was transferred through the first multipass amplifier at a total gain of 300. Finally, the predicted output spectrum calculated by a numerical model of the final amplifier stages was in a good agreement with the experimental results. The spectroscopic properties of Yb3+:CaF2 matches the constraints for ultrashort laser pulse amplification and direct diode pumping. Pumping close to the zero phonon line at 976nm is preferable compared to 940nm as the pump intensity saturation is significantly lower. A broad gain cross section of up to 50nm is achievable for typical inversion levels. Furthermore, moderate cryogenic temperatures (above 200K) can be used to improve the amplification performance of Yb3+:CaF2. The optical quality of the doped crystals currently available on the market is sufficient to build amplifiers in the hundred joule range. The designed pump source for the last two amplifiers is based on two side pumping in a double pass configuration. However, this concept requires the necessity of brightness conservation for the installed laser diodes. Therefore, a fully relay imaging setup (4f optical system) along the optical path from the stacks to the gain material including the global beam homogenization was developed in a novel approach. Beside these major parts the amplifier architecture and relay imaging telescopes as well as temporal intensity contrast (TIC) was investigated. An all reflective concept for the relay imaging amplifiers and telescopes was selected, which results in several advantages especially an achromatic behavior and low B-Integral. The TIC of the front-end was improved, as the pre- and postpulses due to the plane-parallel active-mirror was eliminated by wedging the gain medium.
29

Dynamique et contrôle de systèmes quantiques ouverts / Dynamics and control of open quantum systems

Chenel, Aurélie 16 July 2014 (has links)
L'étude des effets quantiques, comme les cohérences quantiques, et leur exploitation en contrôle par impulsion laser constituent encore un défi numérique pour les systèmes de grande taille. Pour réduire la dimensionnalité du problème, la dynamique dissipative se focalise sur un sous-espace quantique dénommé 'système', qui inclut les degrés de liberté les plus importants. Le système est couplé à un bain thermique d'oscillateurs harmoniques. L'outil essentiel de la dynamique dissipative est la densité spectrale du bain, qui contient toutes les informations sur le bain et sur l'interaction entre le système et le bain. Plusieurs stratégies complémentaires existent. Nous adoptons une équation maîtresse quantique non-markovienne pour décrire l'évolution de la matrice densité associée au système. Cette approche, développée par C. Meier et D.J. Tannor, est perturbative en fonction du couplage entre le système et le bain, mais pas en fonction de l'interaction avec un champ laser. Le but est de confronter cette méthodologie à des systèmes réalistes calibrés par des calculs de structure électronique ab initio. Une première étude porte sur la modélisation du transfert d'électron ultrarapide à une hétérojonction oligothiophène-fullerène, présente dans des cellules photovoltaïques organiques. La description du problème en fonction d'une coordonnée brownienne permet de contourner la limitation du régime perturbatif. Le transfert de charge est plus rapide mais moins complet lorsque la distance R entre les fragments oligothiophène et fullerène augmente. La méthode de dynamique quantique décrite ci-dessus est ensuite combinée à la Théorie du Contrôle Optimal (OCT), et appliquée au contrôle d'une isomérisation, le réarrangement de Cope, dans le contexte des réactions de Diels-Alder. La prise en compte de la dissipation dès l'étape d'optimisation du champ permet à l'algorithme de contrôle de contrer la décohérence induite par l'environnement et conduit à un meilleur rendement. La comparaison de modèles à une et deux dimensions montre que le contrôle trouve un mécanisme adapté au modèle utilisé. En deux dimensions, il agit activement sur les deux coordonnées du modèle. En une dimension, le décohérence est minimisée par une accélération du passage par les états délocalisés situés au-dessus de la barrière de potentiel. / The study of quantum effects as quantum coherences and their exploitation for control by laser pulse are still a numerical challenge in big systems. To reduce the dimensionality of the problem, dissipative dynamics focuses on a quantum subspace called 'system', that includes the most important degrees of freedom. The system is coupled to a thermal bath made of harmonic oscillators. The essential tool of dissipative dynamics is the spectral density of the bath, that contains all the information about the bath and the interaction between the system and the bath. Several strategies coexist and complement one another. We adopt a non-Markovian quantum master equation for the evolution of the density matrix associated to the system. This approach, developped by C. Meier and D.J. Tannor, is perturbative in the system-bath coupling, but not in the interaction with a laser field. Our goal is to confront this methodology to realistic systems calibrated by ab initio electronic structure calculations. We first study the ultrafast electron transfer modelling an oligothiophene-fullerene heterojunction, found in organic photovoltaic cells. We present a way of overcoming the limitation of the perturbative regime, using a Brownian oscillator representation to describe the problem. Charge transfer is faster but less complete when the R distance between oligothiophene and fullerene fragments increases. Then we combine the quantum dynamical method described above with the Optimal Control Theory (OCT) method. An application is the control of an isomerization, the Cope rearrangement, in the context of Diels-Alder reactions. Including the dissipation at the design stage of the field enables the control algorithm to react on the environment-induced decoherence and to lead to a better yield. Comparing one and two-dimension models shows that control finds a mechanism adapted to the model. In two dimensions, it actively acts on the two coordinates of the model. In one dimension, decoherence is minimized by accelerating the way through the delocalized states located above the potential energy barrier.
30

Correction de fronts d'onde de faisceaux lasers impulsionnels par mélange d'ondes photoréfractif.

Mager, Loic 10 November 1994 (has links) (PDF)
Nous avons démontré que la correction de fronts d'onde de faisceaux lasers impulsionnels (nanoseconde) pouvait être réalisée par mélange d'ondes dans un cristal photoréfractif. Nous avons commence par déterminer le matériau photoréfractif le mieux adapte pour cette application. Pour des raisons d'efficacité photoréfractive et de tenue en puissance, notre choix s'est porte sur le titanate de baryum. Cela a conditionne le choix de la longueur d'onde utilisée (532 nm) pour cette démonstration. Nous avons étudié un premier dispositif de correction base sur le transfert d'énergie d'un faisceau fort vers un faisceau faible qui, par mélange d'ondes photoréfractif, peut être obtenu sans qu'il y ait de transfert de phase. Dans cette étude nous avons mesure les variations de l'amplification en fonction de différents paramètres (cohérence temporelle, rapport des énergies des faisceaux) et observe les variations de l'effet photorefractif en fonction de la densité de puissance dans le titanate de baryum. Nous avons aussi démontré la correction des déformations introduites par un objet de phase et cela pour différentes densités d'énergie incidente. Une deuxième méthode de correction est basée sur la compensation d'un aberrateur de phase par double passage. On a commence par préciser la notion de conjugaison de phase. Puis, nous avons étudié en particulier un miroir a conjugaison de phase auto pompe, l'oscillateur a boucle de réaction, qui fonctionne sur le principe du mélange a quatre ondes dans un cristal photoréfractif. Nous avons montre expérimentalement que des transformations des faisceaux dans la boucle de réaction améliorent la qualite de la conjugaison de phase et nous avons réalisé la compensation d'objets de phase par double passage en régime impulsionnel. La dernière partie est consacrée a l'étude comparative des deux dispositifs tels qu'ils pourront être mis en oeuvre pour la correction dynamique des lentilles thermiques dans les amplificateurs lasers solides.

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