Physics and potential applications of femtosecond laser pulses interacting with matter have captured interest in various fields, such as nonlinear optics, laser micromachining, integrated optics, and solar cell technologies. On the one hand, such ultrashort intense pulses make them practical elegant tools to be utilized for direct structuring of materials with high accuracy and numerous potential applications. On the other hand, studying the fundamental aspects and nonlinear nature of such interactions opens new remarkable venues for various unique investigations. In recent years, the emerging topic of structured light (also known as twisted or optical vortex light), i.e., a beam of light with a twisted wave-front that can carry orbital angular momentum (OAM), has attracted the attention of many researchers working in the field of light-matter interaction. Such beams offer various applications from classical and quantum communication to imaging, micro/nano-manipulation, and modification of fundamental processes involved in light-matter interactions, e.g., absorption and emission. Nevertheless, the fabrication of complex structures, controlled modification, and achieving a high spatial resolution in material processing still remain in the spotlight. Moreover, the fundamental role of orbital angular momentum in the nonlinear absorption of materials, particularly in solids, has yet remained a subject of debate. Addressing these points was the main motive behind this dissertation. To accomplish this objective and investigate new aspects of structured light-matter interaction, I conducted various experiments, the results of which are presented in this work. The general idea was to study the interaction of femtosecond laser radiation, having a structured phase and polarization, with the matter in two aspects: (i) surface morphology modification and (ii) nonlinear absorption of solids. In this regard, I studied surface processing of crystalline silicon and CVD diamond with femtosecond laser vortex pulses generated by a birefringent phase-plate, known as q-plate, in single and multiple pulse irradiation regimes, respectively. The characterization of the modified region was performed using optical microscopy, scanning electron microscopy (SEM), and atomic force microscopy (AFM). I demonstrated that upon irradiation of a single vortex pulse on silicon, a nano-cone structure is formed within the ablated crater, whose height was independent of the helicity of the twisted light. However, for a linearly polarized vortex pulse, the height of the nano-cone decreases at higher pulse energies. The dynamics of nano-cone formation and the role of polarization were also investigated by simulating the mass transport function in this process. Moreover, using superimposed vortex beams, we fabricated complex patterns containing several nano-cones, by single-shot irradiation on the silicon surface. My experimental results offer an ability to actively control and manipulate material, in terms of the nanocones position, in two dimensions with an ultra-high resolution. I further proceeded with our experiments in the multiple pulse regime on a diamond target. By irradiation of a high number of superimposed vortex pulses, I was able to imprint complex polarization states of structured light on the target surface in the form of periodic nano-ripples. This procedure enabled us to not only generate spatially varying nano-gratings but also directly visualize and study very complex states of polarization. Besides these surface structuring, I carried out experimental studies to investigate the response of bulk material to an incident circularly polarized vortex beam that carries orbital angular momentum. The experimental results reveal, for the first time, that such an interaction can produce a differential absorption that gives rise to helical dichroism. We demonstrate that this response is sensitive to the handedness and degree of the twist in the incident vortex beam. Such a dichroism effect may be attributed to the excitation of dipole-forbidden atomic transitions, e.g., electric quadrupole transitions. However, this explanation is not absolute and remains open to further research and investigations.

Within this thesis, photo-induced mechanisms of the light-matter interaction are investigated in tailored and photofunctional materials that differ significantly in their optical and structural properties. The individual coupling mechanisms in congruently melted, nominally undoped or iron doped lithium niobate crystals as well as in structurally disordered photoswitchable molecules embedded into a solid state polymer are examined in particular by the principle of holographic grating recording and transient absorption spectroscopy which provide new insight into a variety of material response properties. In case of photoswitchable ruthenium sulfoxide compounds, the underlying mechanism can be unambiguously assigned to a photochromic material response evoked by a photochemical reaction, i.e., a non-instantaneous, local ligand isomerisation. Comparable results are obtained for iron-doped, oxidized lithium niobate where holographic grating recording is related to the photophysical generation of transient excitonic states whose photochromic properties are characterized by targeted ns-pump, supercontinuum probe spectroscopy. In the event of nominally undoped lithium niobate, the holographic amplification of two sub-picosecond pulses is attached to the phenomenon of two-beam coupling on a self-induced dynamic grating. By correlating the individually obtained mechanisms of the light-matter interaction and the light-induced material response, generally accepted conclusions on a microscopic level can be achieved. A major influence of the internal structure and orientation of the excited states, i.e., an appropriate threedimensional structural arrangement, is deduced as a prerequisite for the formation of light-induced, macroscopic refractive index changes while absorption and microscopic refractive index alterations linked via the Kramers-Kronig relation are unaffected. In systems featuring a random distribution of excited states, an orientational order might be achieved as a consequence of linear polarized light, i.e., by polarization structuring. Moreover, if the photorefractive effect can be ruled out, the material response in lithium niobate can be solely assigned to a local alteration of the transient electronic states, i.e., to the photochromic properties of polarons and/or excitonic states, which is in particular comparable to the linkage isomerism of molecular photoswitchable molecules. In addition, the influence of structural parameters on the light-matter/surface interaction is studied on the μm-scale by analyzing the diffraction phenomenon arising from a relief grating. A considerable impact on the surface grating assisted coupling is determined by the transition from cw-lasers to ultrashort laser pulses which enables interference quenching. However, this phenomenon is of no consequence in case of selfinduced holographic gratings.

We report on the investigation and observation of Bloch surface wave polaritons, resulting from the interaction between excitons in ZnO and a Bloch surface wave supported by a distributed Bragg reflector (DBR), for temperatures up to 430 K. The samples were fabricated using pulsed laser deposition and consist of a DBR made of 6.5 layer pairs of yttrica-stabilized zirconia and Al2O3 with a ZnO surface layer. We measured the reflectivity of transverse electric modes using a SiO2 prism in Kretschmann–Raether configuration, giving access to high in-plane momenta. Whereas the lower polariton branch was clearly observable, the upper polariton branch was not visible, due to the strong absorption in ZnO above the excitonic resonance. By employing a coupled oscillator model for the interaction between the bare surface mode and exciton, we derived a corresponding Rabi splitting between 100–192 meV at 294 K, which decreases with increasing temperature.

In this thesis we study light-matter coherence phenomena related to the interaction of a coherent laser field and the so-called Λ-system, a three-level quantum system (e.g., an atom). We observe electromagnetically induced transparency (EIT), slow and stored light in hot rubidium vapor. For example, a 6 μs Gaussian pulse propagate at a velocity of ~1 km/s (to be compared with the normal velocity of 300 000 km/s). Dynamic changes of the control parameter allows us to slow down a pulse to a complete stop, store it for ~100 μs, and then release it. During the storage time, and also during the release process, some properties of the light pulse can be changed, e.g., frequency chirping of the pulse is obtained by means of Zeeman shifting the energy levels of the Λ-system. If, bichromatic continuous light fields are applied we observe overtone generation in the beating signal, and a narrow `dip' in overtone generation efficiency on two-photon resonance, narrower than the `coherent population trapping' transparency. The observed light-matter coherence phenomena are explained theoretically from first principles, using the Lindblad master equation, in conjunction with the Maxwell's equations. Furthermore, we analyze an optical delay-line based on EIT and show that there is in principle (besides decoherence) no fundamental limitation, but the usefulness today is scant. The combination of EIT and a photonic crystal cavity is inquired into, and we show that the quality value of a small resonator (area of 2.5λ×2.5λ with a missing central rod) can be enhanced by a factor of 500 due to the increased modal density close to two-photon resonance. Open system effects (decoherence effects) are thoroughly investigated using a coherence vector formalism, furthermore, a vector form of the Lindblad equation is derived. Specifically we find an open system channel that lead to slow light and gain. / QC 20100812

Cette thèse présente une étude exploratoire de plusieurs aspects du couplage fort lumière-matière dans des matériaux moléculaires. Différentes propriétés héritées d’un tel couplage sont démontrées, ouvrant de nombreuses possibilités d’applications, allant du transfert d’énergie à la génération de signaux optiques non-linéaires et à l’élaboration de réseaux polaritoniques chiraux. Au travers des thématiques abordées, l’idée d’un couplage lumière-matière entrant en compétition avec les différentes fréquences de dissipation des molécules se révèle être cruciale. Ainsi, la prédominance du couplage cohérent au champ électromagnétique apparaît comme un moyen de modifier les propriétés quantiques des états moléculaires, ouvrant la voie à une nouvelle chimie des matériaux en cavité. / This thesis presents an exploratory study of several aspects of strong light-matter coupling in molecular materials. Different properties inherited from such a coupling are demonstrated, opening the way to numerous applications, ranging from energy transfer to the generation of non-linear optical signals and to the development of chiral polaritonic networks. Through the topics covered, the idea of a light-matter coupling strength competing with the different frequencies of relaxation of the molecules proves to be crucial. Thus, the predominance of the coherent coupling to the electromagnetic field appears as a new mean of modifying the quantum properties of molecular systems, opening the way to a new chemistry of materials in optical cavities.

This work derives a nonlinear optical spatio-temporal instability. It is a perturbative analysis that begins from Maxwell’s equations and its constituent relations to derive a vectorial nonlinear wave equation. In fact, it is a new theoretical method that has been developed that builds on previous aspects of nonlinear optics in a more general way. The perturbation in the wave equation derived is coupled with its complex conjugate which has been taken for granted so far. Once decoupled it gives rise to a second-order equation and thus a true instability regime because the wavevector can become complex. The solution obtained for the perturbation that co-propagates with the driving laser is a generalization to modulation and filamentation instability, extending beyond the nonlinear Schrodinger and nonlinear transverse diffusion equations[1][2]. As a result of this new mechanism, new phenomena can be explored. For example, the Kerr Nonlinear Instability can lead to exponential growth, and hence amplification. This can occur even at wavelengths that are typically hard to operate at, such as into far infrared wave- lengths. This provides a mechanism for obtaining amplification in the far infrared from a small seed pulse without the need for population inversion. The analysis provides the basic framework that can be extended to many different avenues. This will be the subject of future work, as outlined in the conclusion of this thesis.

Aujourd'hui les outils permettant de moduler la phase d'une onde lumineuse sont nombreux etpour certains disponibles commercialement, seulement ces éléments ne fonctionnentgénéralement que pour une seule longueur d'onde de travail simultanément. Nous développonsplusieurs approches expérimentales pour la mise en forme de la phase de faisceaux à largebande spectrales. Après un état de l'art sur les principales techniques, nous focalisons notreétude sur la mise en forme de vortex optiques large-bande par l'intermédiaire d'élémentspermettant de moduler la phase géométrique, dont nous abordons quatre approches. Lapremière est basée sur la réflexion de Fresnel anisotrope sur les dioptres mettant en jeu aumoins un matériau biréfringent uniaxe, un choix optimal de leurs indices de réfraction et de leursdispersions permet de réfléchir un faisceau dont la phase dépend de l'orientation de l'axe optiquedes milieux. Dans la seconde, également réflective, nous exploitons le phénomène de réflexionde Bragg circulaire qui se produit au sein des cristaux liquides cholestériques, dont la particularitéest de réfléchir efficacement toute une bande spectrale avec acquisition d'une phase de naturegéométrique. Nous appliquons cette propriété en particulier pour la conception d'élémentsinhomogènes pour la mise en forme, à une bonne approximation, de modes de Laguerre-Gauss.Les deux dernières approches sont basées sur la mise en forme de vortex optiques par desmilieux biréfringents inhomogènes en transmission, en particulier les défauts se formantspontanément dans les films de cristaux liquides nématiques à anisotropie diélectrique négative.L'une consiste à mettre deux éléments en série permettant de traiter successivement différentescomposantes spectrales. L'autre consiste à paralléliser ce procédé en séparant le faisceau initialen différents canaux spectraux, adressés sur des défauts topologiques localisés en réseau etindividuellement contrôlables électriquement. Cette dernière solution peut être vue comme unmodulateur spatial de lumière dont les pixels sont inhomogènes et nous a amené à proposer desapplications potentielles en imagerie optique super-résolue et pour la mise en forme spatiotemporelled'impulsions ultracourtes. / Today, several beam shaping tools are available, some of them commercially, but most of themare designed for only one working wavelength. This thesis aims to develop several experimentalapproaches for broadband topological beam shaping of light. After the presentation of the state ofthe art, our work focuses on vortex shaping of polychromatic beam exploiting the spin-orbitinteraction of light. Concretely, we report the development of four techniques to modulate the socalledgeometric phase of polychromatic light fields. First, we describe anisotropic reflection frominterfaces that involves at least one uniaxial crystal. We identify a refractive index matchingcriterion enabling highly pure broadband phase control. Then we discuss the use of circularBragg reflection phenomenon inherent to the optics of cholesteric liquid crystals. This propertyallows the selective reflection of circularly polarized light over a bandgap while the reflected fieldacquires a geometric phase. These properties are exploited to design, fabricate and characterizestructured mirrors reflecting Laguerre-Gauss optical modes to a good approximation. The last twosolutions consist of vortex beam shaping using inhomogeneous anisotropic planar opticalelements, namely, topological defects that spontaneously appear in homeotropic nematic liquidcrystal films characterized by negative dielectric anisotropy. The first option is based on using twodefects in series while the other is based of parallel processing using an array of independentlycontrolled topological defects, each of them being dedicated to process distinct spectralchannels. The latter approach can be viewed as a spatial light modulator whose pixels areinhomogeneous and potential applications are proposed in the field of super-resolution opticalimaging and spatio-temporal beam shaping of ultrashort pulses.

The performance of electrical and optical devices based on two-dimensional semiconductors (2D) such as molybdenum disulfide is critically influenced due to very poor light absorption in the atomically thin layers. In this study, the phonon mediated optical absorption and emission properties in single atomic layers of MoS2 have been investigated. The electronic transitions in MoS2 due to near-field optical interaction and the influence of interface phonons due to the dielectric substrate GaN on the relaxation of optically generated carriers will be described. The near-field interaction can be induced in the presence of metal plasmons deposited on the surface of MoS2 monolayers. A hybrid metal-semiconductor system was realized by the deposition of silver (Ag) NPs on MoS2 layer and the localized plasmon modes were selectively chosen to interact with quasiparticles such as excitons and phonons. These quasiparticles are confined within the single atomic layer of MoS2 and are stable at room temperatures due to high binding energy. The lattice vibrational modes in MoS2 can be optically excited with the pulses from a femtosecond laser. These phonon modes can be optically dressed due to near-field interaction in the hybrid Ag-MoS2 system under an optical excitation resonant to localized plasmon modes. The coherent dynamics of the carriers in MoS2 were manipulated by the generation of dressed phonons. The driving field creates a coherence between the ground levels in the presence of optical near-field. A strong coupling between the exciton and plasmon modes forming a plexciton band is observed at room temperature within the coherence lifetime of the system. A significant enhancement of photoluminescent (PL) emission from MoS2 monolayer occurs due to carrier density modulation in the presence near-field interactions. The absorption and emission properties of MoS2 are influenced due to the interactions with the semiconducting substrate. The coupling of carriers in MoS2 with the interfacial phonons, and the charge and energy transfer across the interface in 2D MoS2-GaN (0001) significantly change the UF absorption properties and the relaxation of carriers from the excitonic absorption states. An increased light absorption and enhanced PL emission from the single atomic layer of MoS2 was observed. The phonon-assisted processes can activate the dipole forbidden transitions and hence can explain the interaction of incident light in single atomic layer of MoS2. The MoS2-GaN heterostructure provides a platform to exploit strong coupling between the free carriers or excitons, plasmons and phonons. The gold (Au) NPs have a plasmon energy resonant to MoS2 and hence results in the strong exciton-plasmon coupling due to near-field interaction. In the meantime, the localized plasmon energy of platinum (Pt) NPs is selected to be in resonance to GaN bandedge emission and resonant to C excitonic state in MoS2. The localized plasmons in Pt can actively interact with carriers in MoS2 near Γ-point. The non-equilibrium absorption characteristics of MoS2 nanosheets on GaN hybridized with Au and Pt NPs are influenced due to activation of the defect levels of GaN induced due to interband optical excitation.

L’émission spontanée de lumière par un émetteur n’est pas un processus intrinsèque. D’une part, il dépend de l’environnement électromagnétique. D’autre part, il dépend de la présence d’autres émetteurs avec lesquels il peut interagir et générer des interférences.Ces deux effets ont été, dans la plupart des cas, étudiés de manière indépendante. L'objectif de cette thèse est d'explorer comment contrôler l'émission de lumière en utilisant simultanément ces deux types d’effets.La première partie est consacrée à une étude théorique d'un système idéal de deux émetteurs couplés à un résonateur. Les deux émetteurs sont placés à proximité, et l’interaction dipôle-dipôle conduit à la formation de deux états, superradiant et sous-radiant. Le système que l’on obtient agit en tant que source et mémoire quantique de photons uniques, efficace et modulable. On étudie ensuite le cas d’un résonateur plasmonique, à symétrie spatiale antisymétrique, qui permet d’exciter efficacement l’état sous-radiant. On montre qu’on obtient ainsi une forte exaltation de l'effet Purcell, tout en conservant un état spectralement étroit.La deuxième partie explore un système comportant un très grand nombre d’émetteurs couplés à un plasmon de surface se propageant le long d’une interface métal air. Les émetteurs sont des nanoplaquettes, ou puits quantiques colloïdaux. Lorsqu’un film de nanoplaquettes est déposé sur le métal, il est possible d’obtenir un couplage fort. Ce couplage au plasmon de surface permet d'obtenir une émission directive et polarisée. / Spontaneous emission of light is not an intrinsic property of an emitter. On the one hand, it depends on the electromagnetic environment. On the other hand, it depends on the presence of other emitters with whom it may interact and generate interferences. Up to date, very few studies address the question of multiple interacting emitters coupled to a resonator. The goal of this thesis is to combine both collective effects and nanoresonators to control the spontaneous emission and scattering of light emitters.First, we theoretically study an ideal system consisting of two emitters coupled to a resonator. The emitters are in close proximity, and the dipole-dipole interaction generates a superradiant state and a subradiant state. The system that we obtain behaves as an efficient, and tunable, single photon source and quantum memory. We then switch to the case of a plasmonic resonator with an antisymmetric mode, which allows to efficiently excite the subradiant state. We show that this results in an enhancement of the Purcell effect while maintaining a spectrally narrow state.In the second part of this thesis, we explore a system of a large number of emitters coupled to a surface plasmon travelling along a metal-air interface.The emitters are nanoplatelets, also called colloidal quantum wells. Strong coupling is obtained when a layer of nanoplatelets is deposited on top of the metal. The coupling of the nanoplatelets to the surface plasmon allows to obtain directional and polarized light emission.

This thesis is devoted to optical properties of Aharonov-Bohm quantum rings in external electromagnetic fields. It contains two problems. The first problem deals with a single-electron Aharonov-Bohm quantum ring pierced by a magnetic flux and subjected to an in-plane (lateral) electric field. We predict magneto-oscillations of the ring electric dipole moment. These oscillations are accompanied by periodic changes in the selection rules for inter-level optical transitions in the ring allowing control of polarization properties of the associated terahertz radiation. The second problem treats a single-mode microcavity with an embedded Aharonov-Bohm quantum ring, which is pierced by a magnetic flux and subjected to a lateral electric field. We show that external electric and magnetic fields provide additional means of control of the emission spectrum of the system. In particular, when the magnetic flux through the quantum ring is equal to a half-integer number of the magnetic flux quantum, a small change in the lateral electric field allows tuning of the energy levels of the quantum ring into resonance with the microcavity mode, providing an efficient way to control the quantum ring-microcavity coupling strength. Emission spectra of the system are calculated for several combinations of the applied magnetic and electric fields.