1 |
Synthesis,structures and reactivities of bis(triarylmethylium) dications and related diboranesWang, Huadong 01 November 2005 (has links)
The primary goal of the research described in this thesis concern the synthesis,
characterization and study of 1,8-bis(diarylmethylium)naphthalenediyl dications. Such
dications have been prepared from the corresponding diols and have been fully
characterized. Single crystals X-ray diffraction studies indicate that the two cationic
centers of these derivatives are separated by 3.0 - 3.1 ??. The enforced proximity of the
cationic centers intensifies the electron deficiency of these derivatives which behave as
strong organic oxidants. As indicated by cyclic voltammetry, these dications undergo a
two-electron reduction to afford the corresponding acenaphthenes. The newly formed
C-C bond which links the former methylium are remarkably long (1.628-1.706 ??.) and
can, in some instances, be oxidatively cleaved in the presence of acids. These dications
can also be reduced chemically by reducing reagent, such as hydride, chloride, bromide
and iodide. Remarkably, the reaction of 1,8-bis(diphenylmethylium)naphthalenediyl
dication with fluoride anion results in the formation of a mono fluorinated cation which
features an unsymmetrical C-F?C bridge between the former methylium centers. As
indicated by 1H NMR spectroscopy, the structure of this cation is fluxional with the fluorine atom oscillating between the former methylium centers. Finally, this thesis also
deals with the synthesis and study of 4,6-bis(dimesitylboryl)dibenzofuran and
isoelectronic dications.
|
2 |
Light-atom interaction: mean-field approach and intensity fluctuations / Interação luz-átomo: abordagem de campo médio e flutuações de intensidadeCottier, Florent André Julien 24 January 2019 (has links)
In this thesis, we investigate the coherent scattering of light propagating in a random medium. We are interested in phenomena like the super- and subradiance and Anderson localization that are related to waves interferences and spatial disorder. However, the fundamental difference between subradiance and Anderson localization still needs to be clarified. This thesis gives new elements for the understanding of these phenomena and we present a new method to observe Anderson localization. A mean-field model that does not contain disorder is developed, and we show that super- and subradiance do not require disorder whereas Anderson localization does. In this theoretical work, the coupling between the light and many atoms is reduced to a coupling matrix between the atoms by tracing over the degrees of freedom of the light, which results in a linear problem for the atomic dipoles. The study of the eigenvalues and eigenmodes of this matrix then allows to determine the super- and subradiant modes, and to probe the Anderson localization phase transition with a scaling analysis. Furthermore, the link to the experiment is realized by showing that the intensity fluctuations present an increase at the localization transition. The system is studied in the steady-state regime when the medium is continuously charged by a laser until reaches a stationary regime, and the decay dynamics, when the laser is switched off, so the cloud releases the energy stored. Finally, we present a preliminary work that shows that the diagonal disorder might be a good strategy to reach Anderson localization. / Nesta tese, investigamos o espalhamento coerente de luz propagando em um meio aleatório. Estamos interessados em fenômenos como superradiância, subradiância e localização de Anderson, os quais estão relacionados com interferências de ondas e desordem espacial. No entanto, as diferenças fundamentais entre subradiância e localização de Anderson ainda precisam ser esclarecidas. Esta tese traz novos elementos na compreensão destes fenômenos e apresentamos um novo método para observar a localização de Anderson. Neste trabalho teórico, estudamos os autovalores e os automodos de uma matriz de acoplamento que permite extrair modos super- e subradiantes, e exibem uma transição de fase de localização de Anderson através de uma análise de escalamento. Além disso, a conexão com o experimento é feita através da intensidade irradiada pela nuvem em todas as direções. Distinguimos dois casos: o regime de estado estacionário, quando o meio é continuamente excitado por um laser e alcança um regime estacionário; e o caso dinâmico, onde o laser é desligado e a nuvem libera a energia armazenada. Desenvolvemos um modelo de campo médio que não inclui desordem, e mostramos que super- e subradiância não precisam da desordem para existir, ao contrário da localização de Anderson. Mostramos também que podemos observar uma transição de fase de localização de Anderson na estatística da intensidade. Finalmente, apresentamos um trabalho preliminar que mostra que a desordem diagonal pode ser uma boa estratégia para alcançar a localização de Anderson.
|
3 |
Cooperative Effects of Inflammatory Mediators on Leukocyte and Cancer Cell Interactions with Vascular EndotheliumJanuary 2013 (has links)
Inflammation is a driving force behind various lethal pathological conditions, including atherosclerosis and cancer metastasis. Inflammatory mediators are keys that unlock the immune response via triggering interactions of leukocytes and vascular endothelial cells. Oxidized low density lipoprotein (OxLDL), lipopolysaccharide (LPS), tumor necrosis factor-alpha (TNF-α), and histamine are all strong activators of the inflammatory response, and they can be simultaneously produced during various inflammatory disorders. This study focuses on investigating the cooperative effect of TNF-α and histamine, as well as OxLDL and histamine on monocyte-endothelium interactions. Furthermore, the roles of LPS-activated monocytes and histamine in interactions of breast cancer cells with vascular endothelium are also explored. The results suggest that: 1) TNF-α and histamine have a synergistic effect on monocyte-endothelium interactions; 2) histamine cooperatively works with OxLDL to induce monocyte recruitment on endothelial cells; 3) OxLDL treated macrophages and mast cells respectively release TNF-α and histamine, which in turn synergistically increase the capture of monocytes by endothelial cells; 4) LPS activated monocytes secret TNF-α to activate endothelial cells and assist in adhesion of carcinoma cells to activated vascular endothelium; 5) exposure of activated endothelial cells to histamine exaggerates the carcinoma cell arrest, especially in the presence of LPS activated monocytes. In summary, this study implies that an increased risk of atherogenesis may be among the population affected by allergy or asthma and having lipid rich diet that leads to the production of TNF-α and OxLDL in body. It also highlights that the mechanism by which Gram-negative bacterial infection increases a risk of breast cancer metastasis through the cardiovascular system, and shows the necessity to develop better approaches for preventing this infection after surgical resection or before histamine combined IL-2 immune therapy in order to reduce a risk of cancer metastasis. / acase@tulane.edu
|
4 |
Interaction lumière-atomes : approche de champ moyen et fluctuations d’intensité / Light-atom interaction : mean-field approach and intensity fluctuationsCottier, Florent 24 January 2019 (has links)
Dans cette thèse, nous étudions la diffusion cohérente de la lumière se propageant dans un milieu désordonné. Nous nous intéressons à des phénomènes tels que la super- et sousradiance et la localisation d’Anderson qui sont liées aux interférences et au désordre spatial. Cependant, la différence fondamentale entre la sousradiance et la localisation d'Anderson doit encore être clarifiée. Cette thèse donne de nouvelles idées pour la compréhension de ces phénomènes et nous présentons une nouvelle méthode pour observer la localisation d'Anderson. On développe un modèle à champ moyen qui ne contient pas de désordre, et nous montrons que super- et sousradiance ne nécessitent pas de désordre contrairement à la localisation d’Anderson. Dans ce travail théorique, le couplage entre la lumière et les atomes est réduit à une matrice de couplage entre les atomes en calculant la trace sur les degrés de liberté de la lumière, ce qui nous amène à un problème linéaire pour les dipôles atomiques. L'étude des valeurs propres et des modes propres de cette matrice permet de déterminer des modes super- et sousradiant, et de sonder la transition de phase de localisation avec une scaling analysis. De plus, le lien avec l'expérience est fait en montrant que les fluctuations de l’intensité augmentent à travers la transition de localisation. Le système est étudié en régime stationnaire, quand le milieu est continûment chargé par un laser et que celui-ci atteint l’équilibre, et en dynamique, quand le laser est éteint et que le milieu se décharge de l’énergie stockée. Enfin, nous présentons un travail préliminaire qui montre que le désordre diagonal peut être une bonne stratégie pour atteindre la localisation d’Anderson. / In this thesis, we investigate the coherent scattering of light propagating in a random medium. We are interested in phenomena like the super- and subradiance and Anderson localization that are related to waves interferences and spatial disorder. However, the fundamental difference between subradiance and Anderson localization still needs to be clarified. This thesis gives new elements for the understanding of these phenomena and we present a new method to observe Anderson localization. A mean-field model that does not contain disorder is developed, and we show that super- and subradiance do not require disorder whereas Anderson localization does. In this theoretical work, the coupling between the light and many atoms is reduced to a coupling matrix between the atoms by tracing over the degrees of freedom of the light, which results in a linear problem for the atomic dipoles. The study of the eigenvalues and eigenmodes of this matrix then allows to determine the super- and subradiant modes, and to probe the Anderson localization phase transition with a scaling analysis. Furthermore, the link to the experiment is realized by showing that the intensity fluctuations present an increase at the localization transition. The system is studied in the steady-state regime when the medium is continuously charged by a laser until reaches a stationary regime, and the decay dynamics, when the laser is switched off, so the cloud releases the energy stored. Finally, we present a preliminary work that shows that the diagonal disorder might be a good strategy to reach Anderson localization.
|
5 |
Localisation de la lumière et effets coopératifs dans des nuages d'atomes froids / Light localization and cooperative effects in cold atom cloudsBellando de Castro, Louis 12 November 2013 (has links)
Ce travail de thèse présente une étude numérique et théorique de l’influence des effets coopératifs sur la localisation de la lumière dans des vapeurs atomiques, suivie d’une étude expérimentale de ces effets coopératifs dans le régime de diffusion multiple dans des nuages d’atomes froids dilués. Le premier chapitre décrit le modèle que nous utilisons, basé sur l’Hamiltonien effectif d’interaction matière rayonnement, afin d’étudier numériquement la localisation de la lumière et les effets coopératifs. Nous discutons également des différences fondamentales existant entre la situation réelle où la lumière est assimilée à une onde vectorielle et l’approximation scalaire plus facile à traiter analytiquement. Le deuxième chapitre se concentre sur la présentation des résultats numériques complétée d’une comparaison systématique entre les cas scalaire et vectoriel. Nous remarquons dans cette partie que l’approximation scalaire, valable dans la limite des milieux spatialement dilués, présente des différences drastiques avec le cas vectoriel lorsque nous considérons des milieux spatialement denses. Nous n’observons pas également d’indications suffisantes nous permettant de discriminer le fait que les effets coopératifs ne soient pas à la base des mécanismes de localisation de la lumière. Dans la dernière partie nous nous intéressons expérimentalement aux signatures des effets coopératifs dans le régime de diffusion multiple en confrontant à nos résultats expérimentaux plusieurs approches théoriques tenant compte ou pas des effets d’interférences. / In this thesis we present a numerical and theoretical study of the interplay between cooperative effects and light localization in atomic vapour, completed by an experimental study of these cooperative effects for dilute cold atom clouds in the multiple scattering regime. The first chapter describes the model we use, based on the light matter effective Hamiltonian, in order to investigate numerically light localization and cooperative effects. We also discuss the fundamental differences existing between the real situation where light is considered as a vector wave and its scalar approximation easier to treat analytically. The second chapter focuses on the numerical results where we compare systematically the scalar and the vector cases. We show that the scalar approximation, valid for spatially dilute systems, leads to drastic differences compared to the vector case when we consider spatially dense clouds. We also do not observe sufficient proofs to establish that cooperative effects are not at the origin of light localization mechanisms. In the last chapter we investigate experimentally the signatures of cooperative effects in the multiple scattering regime, comparing our results to several theoretical approaches taking or not into account interference effects related to the wave nature of light.
|
6 |
Design de réseaux apériodiques et des interactions électromagnétiques coopératives dans des structures plasmoniques : application à la conception d’absorbeurs pour le solaire concentré / Design of aperiodic networks and cooperative electromagnetic interactions in plasmonic structures : application to the design of absorbers for concentrated solar power.Langlais, Mathieu 16 December 2014 (has links)
La situation énergétique actuelle impose le développement de technologies qui utilisent des énergies renouvelables pour limiter la dépendance aux ressources fossiles et diminuer l’impact de l’activité humaine sur le changement climatique. Parmi ces technologies, le solaire thermodynamique utilise l’énergie solaire pour chauffer un absorbeur, l’énergie de cet absorbeur étant alors convertie en électricité à travers un cycle thermodynamique classique. L’amélioration des performances de cette technologie passe par la conception d’absorbeurs capables de fonctionner efficacement à haute température. Dans ce travail de thèse, nous explorons deux voies différentes dans ce but.La première est basée sur la conception de structures multicouches optimisées par algorithme génétique. Nous montrons que ces structures permettent d’obtenir un rendement supérieur à 80 %, valeur très proche des limites fondamentales, démontrant ainsi leur fort potentiel pour le solaire thermodynamique.La seconde voie est basée sur l’optimisation des interactions électromagnétiques dans des structures plasmoniques à base de nanoparticules métalliques. Ces structures sont le siège d’effets coopératifs qui peuvent exalter très fortement les pertes dans la structure. Ces mécanismes sont mis à profit pour concevoir des absorbeurs à base de réseaux binaires de nanoparticules d’or et d’argent dispersées dans une matrice transparente. / The current energy situation requires the development of technologies that use renewable energy sources to reduce the dependence on fossil fuels and the impact of human activity on climate change. Among these technologies, thermodynamic solar power uses solar energy to heat an absorber, whose heat is then converted into electricity through a classical thermodynamic cycle. The improvement of the performances of this technology requires the design of absorbers able to operate strongly at high temperature. In this thesis, we explore two different ways for this purpose.The first is based on the design of multilayer structures optimized by a genetic algorithm.We will see that these structures lead to an efficiency higher than 80 %, very close to the fundamental limits, demonstrating so their strong potential for thermodynamic solar technology. The second way is based on the optimization of electromagnetic interactions inside plasmonic nanostructures composed of metal nanoparticles. These structures are the site of cooperative effects between nanoparticles that can exalt strongly losses inside the structure. These mechanisms are exploited to design absorbers based on binary networks made with nanoparticles of gold and silver dispersed in a transparent matrix.
|
7 |
Organic reactivity and through-space effectsBrown, James John January 2014 (has links)
Chapter 1 presents a mini-review of the prominent theoretical models which are employed in the prediction of the outcome of organic chemical reactions. The chapter covers the most widely used empirical and semi-empirical models, as well as some more recently developed models. Most have a common theme in that they were developed using electrophilic aromatic substitution as a model reaction. Chapter 2 describes the development of a predictive model based on the average local ionisation energy. The model is shown to be of use in predicting both the regioselectivity and relative reactivity of a wide range of molecules in electrophilic aromatic substitution reactions. An attempt is made to expand the model beyond electrophilic aromatic substitution to various other electrophilic reactions. Chapter 3 details the investigation into the predicted enhancement of reactivity of aromatic rings. Calculations of electrostatic surface potential surfaces show that the proximity of an electron rich atom to an aromatic ring increases the electron density of the ring. Analysis of the local ionisation energy surfaces of these molecules suggests that the reactivity of these rings towards electrophiles is also increased. Preliminary studies on model systems using NMR spectroscopy aim to determine whether this effect can be observed experimentally. Chapter 4 introduces a method for applying the average local ionisation energy to nucleophilic reactions. The ability of the model to predict the regiochemical outcome and relative reaction rates of various molecules is examined in a variety of reaction types, including nucleophilic aromatic substitution. Chapter 5 reports studies into the polarisation-induced cooperative effects that exist between hydrogen bonding groups. The cooperative effect has been measured quantitatively in some simple hydroxybenzene derivatives. An improved understanding of this effect, developed using small molecule models, should lead to an improved ability to predict the extent of this effect in larger systems.
|
8 |
N3, N4/(N3S, N3O) and N6 Phenanthroline Bases and their Spin Crossover Iron(II) ComplexesDjomgoue, Paul 05 August 2016 (has links) (PDF)
The present dissertation focuses on the synthesis of iron(II) complexes and the study of their SCO behavior. The equilibrium between the HS and the LS states gives to the SCO systems large potential applications for molecular electronics. However, today there is not a single molecular device from SCO compounds in the market. This is due to the fact that the SCO systems discovered up to now were unable (e.g. TLIESST « 300 K) for these applications. The aim of this thesis is to synthesize new SCO compounds with sustainable properties for applications.
In the beginning of the thesis, [Fe(rac-22a))]2+∙2[BF4]- and [Fe(rac-22b)]2+∙2[BF4]- employing rigid hexadentate ligands were described. In contrast to the expectation, the N-methylation of the amines shifts the equilibrium towards the LS state. [Fe(rac-22b)2+∙2[BF4]- shows a T1/2 higher at 74 K and 52 K than the non methylated [Fe(rac-22a)2+∙2[BF4]- respectively in nitrobenzene and acetonitrile. The T1/2 are solvent-dependent for these complexes. After that, ligand series 9-R2-2-(6-R1-pyridin-2-yl)-1,10-phenanthroline 25b (R2 = Me), 25f (R2 = Ph), 25d (R2 = C(O)H), 25c (R1 = Ph), 25l (R1 = oxylphenyl-4-oxymethylene), 25m (R1 = oxymesitylene) and 25j (R1 = pyrol-1-yl) were synthesized. It was observed that the size of the substituent influences the SCO properties (T1/2). In addition, the influence of the counterion was shown with [Fe(25c)2]2+∙2[BF4]- and [Fe(25c)2]2+∙2[B(Ph)4]-. The B(Ph)4- conterions bring π∙∙∙π interactions in the molecular cell which shift the T1/2 parameter to a high temperature (200 K) compared to the complex with BF4- ions (175 K). Moreover the substituents R1 on the terminal position of the pyridine effect on T1/2 more than the substituents R2 on the terminal position of the phenanthroline. For example, [Fe(25f)]2+∙2[BF4]- (R1 = Ph) is a pure HS complex while the complex [Fe(25c)]2+∙2[BF4]- (R2 = Ph) is a SCO system (T1/2 = 175 K). The expansion of the coordination mode from N6 to N8 was investigated by the synthesis of the tetradentate ligands. This expansion shows an unexpected coordination mode, [Fe(25i)2]2+∙2[BF4]- (R2 = pyrazol-1-yl) forms a distorted square antiprism coordination geometry (HS iron(II)-complex) and does not show any Fe-N bond breaking over the application of the temperature as expected. / Die vorliegende Dissertation behandelt die Synthese von Eisen(II)-Komplexen und ihr spin crossover (SCO)-Verhalten. Das Gleichgewicht zwischen high-spin (HS)- und low-spin (LS)-Zustand verleiht den SCO-Systemen eine großes Anwendungspotential im Bereich der molekularen Elektronik. Dennoch existiert bis heute kein SCO-basiertes molekulares Bauteil auf dem Markt. Hauptgrund hierfür ist, dass die bislang bekannten SCO-Systeme keine hinreichenden Eigenschaften (z.B. TLIESST « 300 K) aufweisen. Das Ziel der vorliegenden Arbeit ist die Synthese neuer SCO-Verbindungen mit geeigneten Eigenschaften für die Anwendung.
Zu Beginn der Arbeit werden die Komplexe [Fe(rac-22a)]2+∙2[BF4]– und [Fe(rac-22b)]2+ ∙2[BF4]– mit starren hexadentaten Liganden beschrieben. Entgegen der Erwartung verschiebt die N-Methylierung der Amine das Gleichgewicht in Richtung des LS-Zustandes. Verglichen mit dem nicht-methylierten Komplex Fe(rac-22b)]2+∙2[BF4]– zeigt Fe(rac-22a)]2+∙2[BF4]– eine höhere Übergangstemperatur T1/2, welche in Nitrobenzen 74 K und in Acetonitril 52 K beträgt. Für die Komplexe ist T1/2 lösungsmittelabhängig. Im Folgenden wurde die Ligandenserie 9-R2-2-(6-R1-pyridin-2-yl)-1,10-phenanthrolin mit den Vertretern 25b (R2= Me), 25f (R2 = Ph), 25d (R2 = C(O)H, 25c (R1 = Ph), 25l (R1 = oxyphenyl-4-oxymethylen), 25m (R1 = oxymesitylen) und 25j (R1 = pyrol-1-yl) hergestellt. Es wurde beobachtet, dass die Größe des Substituenten das SCO-Verhalten (T1/2) beeinflusst. Ergänzend wurde der Einfluss des Gegenions anhand der Komplexe [Fe(25c)]2+∙2[BF4]– und [Fe(25c)]2+∙2[B(Ph)4]– untersucht. Das Gegenion B(Ph)4– ermöglicht intra- und intermolekulare π···π-Wechselwirkungen in der Zelle, welche die Übergangstemperature T1/2 (200 K) gegenüber dem BF4–-Komplex (175 K) erhöhen. Des Weiteren beeinflussen die Substituenten R1 an der Pyridin-Einheit die ubergangskomplexes T1/2 stärker als die Substituenten R2 an der Phenanthrolin-Einheit. So ist [Fe(25f)]2+∙2[BF4]– (R1 = Ph) ein reiner HS-Komplex, während der Komplex [Fe(25c)]2+∙2[BF4]– (R2 = Ph) ein SCO-System ist (T1/2 = 175 K). Die Erhöhung der Koordinationszahl von N6 auf N8 wurde über die Synthese von tetradentaten Liganden untersucht. Diese Erhöhung führt zu einem unerwarteten Koordinationsmodus. So bildet [Fe(25i)]2+∙2[BF4]– (R2 = pyrazol-1-yl) eine quadratisch-antiprismatische Koordinationssphäre (HS Eisen(II)-Komplex) und zeigt, wie erwartet, über den untersuchten Temperaturbereich keine Fe–N-Bindungsspaltung.
|
9 |
Effets de cohérence en diffusion multiple de la lumière et intrication des états cohérents / Coherence effects in multiple scattering of light and entangled coherent statesRouabah, Mohamed Taha 09 April 2015 (has links)
L’interaction entre la lumière et un nuage atomique désordonné et dilué donne lieu à des effets de cohérence collectifs dus à l’interaction des dipôles induits par le biais du champ lumineux. L'influence de tels effets de cohérence en diffusion multiple suscite beaucoup d’intérêt. Nous présentons deux modèles théoriques qui décrivent ces effets de cohérence dans différents régimes de diffusion. Le traitement du processus à travers un développement en ordres successifs de diffusion nous permet de mettre en évidence la contribution du premier et second ordres ainsi que l'interférence entre les champs diffusés qui en résultent. Dans le régime de diffusion multiple, nous montrons que la force de pression de radiation n'est pas une bonne observable pour sonder les effets coopératifs. Par ailleurs, nous mettons en évidence une surprenante cohérence de phase qui suggère une persistance des effets coopératifs en diffusion multiple. Cela pourrait être le résultat d'une synchronisation entre les dipôles atomiques couplés. Dans une deuxième partie, nous étudions l'effet d'une déformation de l'algèbre de Weyl-Heisenberg sur l'intrication des états cohérents. Une telle approche permet de décrire la décohérence dans des systèmes quantiques intriqués soumis à une perturbation extérieure. Nous construisons des états cohérents déformés intriqués et nous calculons leur concurrence. Nous montrons que la déformation de l'algèbre pourrait avoir un impact non négligeable sur la qualité de l'intrication bipartie des états cohérents, si cette dernière n'est pas maximale. / This work is devoted on the one hand to the investigation of coherence effects in multiple scattering of light by an atomic cloud and on the other hand to the entanglement of a deformed coherent state. The interaction between light and a dilute disordered atomic cloud gives rise to collective coherent effects due to the interaction of the induced dipoles via the external field. The behavior of such coherent effects in multiple scattering regime is an important question for various physical systems. We present two theoretical models describing those coherence effects in different scattering regimes. The scattering order expansion treatment of light scattering allows us to highlight the role of the first and second scattering orders as well as the interference between the resulting scattered fields. In the multiple scattering regime we show that the radiation pressure force is not a good observable to probe cooperative effects. Furthermore, we discover a surprising phase coherence that hints that collective effects may survive in multiple scattering regime. That could be due to a synchronization between the induced atomic dipoles. In a second part, we study the effect of an algebra deformation on entangled coherent states. Such an approach allows to describe decoherence in perturbed entangled quantum systems. We construct a deformed coherent state and calculate their concurrence. We show that algebra deformation could have a non negligible impact on bipartite entangled coherent states if those later are not maximally entangled.
|
10 |
Super- et sous-radiance dans un nuage dilué d'atomes froids / Super- and subradiance in a dilute cloud of cold atomsOliveira de Araujo, Michelle 11 December 2018 (has links)
Le problème de l'interaction de N atomes avec un faisceau laser et les modes du vide peut donner lieu à de nombreux phénomènes intéressants concernant l’émission spontanée de la lumière et sa propagation dans l’échantillon. Les effets coopératifs, par exemple, tels que la super- et la sous-radiance, sont des effets liés à la cohérence créée entre les atomes lorsqu'un photon est émis spontanément par un seul atome excité. La super-radiance peut être définie comme le renforcement de l'émission spontanée due à une interférence constructive de la lumière diffusée. Son homologue, la sous-radiance, est le piégeage d'une partie de la lumière restante en raison d'interférences destructives. Dans les atomes froids, certains travaux théoriques antérieurs prédisent et caractérisent ces deux effets coopératifs dans un nuage atomique large et diluée, dans le régime des faibles intensités et à grands désaccords du laser incident. Le modèle théorique est un modèle de dipôles couplés pour atomes à deux niveaux pilotés par un champ de faible intensité et dans l'approche scalaire. L'expérience consiste à mesurer les taux de d’décroissance super- et sous-radiants à partir de l’intensité temporelle émise après la coupure du laser incident en régime stationnaire. Notre schéma expérimental consiste en un piège magneto-optique d’atomes de rubidium 87 à grandes épaisseurs optiques à résonance. Un faisceau sonde excite les atomes proches de la raie D2. L’intensité émise est détectée par un détecteur de photons uniques dépourvu d’afterpulsing et une procédure d’étalonnage nous permet de déterminer l’épaisseur optique résonante du nuage et sa température. Dans ce travail, nous rapportons l’observation expérimentale de la super- et sous-radiance dans un grand nuage d’atomes froids. Pour la sous-radiance, le résultat principal est l’évolution linéaire du temps caractéristique avec l’épaisseur optique résonante du nuage et son indépendance du désaccord. Pour la super-radiance, on observe la super-radiance en dehors de la direction vers l’avant. Nous vérifions la validité de nos interprétations avec les prédictions du modèle de dipôles couplés. Finalement, nous discutons l’interaction entre la sous-radiance et le piégeage de radiation, ainsi que des prévisions théoriques concernant : la configuration d’un nuage phasé, pour contrôler l’émission de l’amplitude sousradiante ; et les effets de température, où la sous-radiance s’avère robuste dans une large gamme de températures. / The problem of the interaction of N atoms with a laser beam and vacuum modes can give rise to many interesting phenomena concerning the spontaneous emission of light and its propagation in the medium. The cooperative effects, for example, such as superadiance and subradiance, are effects related to the coherence created between the atoms when a photon is emitted spontaneously by a single excited atom. Superradiance can be defined as the enhancement of the spontaneous emission due to constructive interference of the scattered light. Its counterpart, subradiance, is the trapping of some remaining light due to destructive interference. In cold atoms, some previous theoretical works predict and characterize these two cooperative effects in a large and diluted atomic cloud, in the regime of low intensities and large detunings of the incident laser. The theoretical model is a coupled-dipole model for two-level atoms driven by a low-intensity field and in the scalar approach. The experiment consists in measuring the super- and subradiant decay rates from the temporal emitted intensity after the switch off of the incident laser in the steady state. Our experimental setup consists in a magneto-optical trap of rubidium 87 atoms at large resonant optical thicknesses. A probe beam excites the atoms close to the D2 line. The intensity emitted is detected by a single photon detector with no afterpulsing and a calibration procedure allows us to determine the resonant optical thickness of the cloud and its temperature. In this work, we report the experimental observation of super- and subradiance in a large cloud of cold atoms. For subradiance, the main result is the linear evolution of the characteristic time with the resonant optical thickness of the cloud and its independence of the detuning. For superradiance, we observe superradiance out of the forward direction. We verify the validity of our interpretations with the predictions of the coupled-dipole model. Finally, we discuss the interplay of subradiance and radiation trapping, as well as theoretical predictions for: a setup of a phased cloud, to control the subradiant amplitude emission; and temperature effects, where subradiance is shown to be robust in a large range of temperatures.
|
Page generated in 0.0934 seconds