La nanophotonique non-linéaire offre une opportunité unique pour ouvrir de nouvelles voies vers des applications dans les détecteurs, les ordinateurs et la cryptographie quantique. Cependant, la faiblesse intrinsèque de la réponse non-linéaire des milieux de taille inférieure au micromètres limite fortement l’efficacité des sources optique à cette échelle. Combiner l'exaltation du champ électromagnétique dans les métaux (appelée résonance plasmonique) et l'efficacité non-linéaire de nanocristaux non-centosymétriques apparait extrêmement souhaitable et constitue le cœur de ce projet. Dans ce cadre, le travail présenté dans cette thèse consiste en une approche numérique quantitative des processus linéaires et non-linéaires (génération de second harmonique et de paires de photons) mis en jeu dans les nanostructures hybrides afin de pouvoir « accorder » les résonances plasmoniques et optimiser le couplage lumière-matière. L’étude menée prédit une exaltation par plusieurs ordres de grandeur des processus non linéaires modélisés au sein de particules composites. / Nonlinear nanophotonics offers a unique opportunity to open new path toward a wide range of pratical applications in sensors, quantum computers, cryptography devices. The main challenge is to enhance nonlinear response of nanosized particles in order to integrate them in optical components. On this purpose, we want to combine the electromagnetic field enhancement in metals (due to a phenomenon called plasmonic resonances) with non linear efficiency of non centrosymmetric nanocrystals.In this thesis, we present a numerical approach for simulating linear and non linear optical processes (second harmonic generation and spontaneous numerical down conversion) in hybrid nanostructures in order to “ tune “ plasmonic resonances and optimize light/matter coupling. The study predicts an enhancement by several orders of magnitude of the non linear phenomena modeled in composite nano particles.

Le transfert d'énergie par résonance de type Förster (FRET) permet de mesurer des distances nanométriques grâce à la dépendance critique de l'efficacité du transfert avec la séparation entre un donneur et un accepteur d'énergie. Le phénomène se produit quand le fluorophore donneur dans l'état excité transfère son énergie d'excitation à un accepteur à proximité de façon non-radiative avec une interaction dipôle-dipôle de champ proche. Les structures nanophotoniques sont capables de contrôler cette interaction grâce à la modification de la densité local d'états électromagnétiques (LDOS) d'un émetteur quantique. Nous avons démontré clairement l'exaltation du transfert d'énergie des paires FRET individuelles sous l'influence des nano-ouvertures percées en or et en aluminium et aussi à l'aide des designs plus complexes comme la `` antenna-in-box ". Notamment, nous avons dévoilé l'importance essentielle de l'orientation relative entre les dipôles sur les possibilités d'exaltation du transfert d'énergie par le biais des nanostructures. Également, nous avons utilisé des nanofils en argent pour démontrer un transfert d'énergie de long-distance entre deux nanoparticles séparées de plus d'un micromètre. Nos résultats éclairent le chemin de l'exploration du FRET, qui est largement utilisé dans les sciences du vivant et la biotechnologie. Les nanostructures optiques ouvrent de plus des perspectives d'applications innovantes pour la construction de biocapteurs, de sources de lumière ou dans l'industrie photovoltaïque. / The technique of Förster resonance energy transfer (FRET) determines the separation between two molecules at the nanometer scale, where molecular interactions can take place. The phenomenon requires a donor fluorophore transferring its energy in a non-radiative way, through a near-field dipole-dipole interaction, to an acceptor. Nanophotonics achieves accurate control over these interactions by modifying the local density of optical states (LDOS) of a single quantum emitter. We have clearly demonstrated enhanced energy transfer within single FRET pairs confined in single nanoapertures made of gold and also aluminum or in more complex structures like the antenna-in-box design. In particular, we have revealed the strong influence of the mutual dipole orientation on the FRET enhancement using nanostructures. Also, by means of silver nanowires, we have demonstrated a long-range plasmon-mediated fluorescence energy transfer between two nanoparticles separated by micrometer distance. Our results are clearing a new path to improve the energy transfer process widely used in life sciences and biotechnology. Optical nanostructures open up many potential applications for biosensors, light sources or photovoltaics.

Doctor of Philosophy / Department of Physics / Daniel Rolles / Modern laser sources can produce bursts of light that surpass even the fastest molecular vibrations. With durations this short even moderate pulse energies generate peak powers exceeding the average power output of the entire globe. When focused, this can result in an ultrafast electric field greater than the Coulomb potential that binds electrons to nuclei. This strong electric field strips electrons away from atoms in a process known as strong-field ionization. The first experimental realization of photoionization with intense laser pulses occurred only a few years after the invention of the laser. Yet, despite decades of intensive investigation, open questions remain. At the same time, the knowledge gained has led to the creation of multiple exciting fields such as attoscience, femtochemistry, and ultrafast nano-photonics. In this thesis I present my work to advance the fundamental understanding of intense, ultrafast light-matter interactions as well as efforts to expand the technological capabilities of ultrafast light sources and measurement techniques. This includes the photoionization pro- cess of atoms and nanoparticles subject to intense, mid-infrared laser fields. The resulting photoelectron emission is measured, with high precision, in a velocity map imaging spec- trometer. Other parts of this thesis detail my work on the generation and characterization of non-Gaussian optical pulses. Femtosecond Bessel beams are used to drive and study high harmonic generation with the ultimate goal of creating a compact, high-flux XUV source. Further studies include few-cycle pulses and the carrier-envelope phase, specifically methods of locking and tagging the carrier-envelope phase. A single-shot, all optical tagging method is developed and directly compared to the standard tagging method, the carrier-envelope phase meter. Finally, both experimental and computational studies are presented investigating the ultrafast thermal response cycle of nanowires undergoing femtosecond heating.

Nanostructures have received much attention from the physical and engineering communities in the past few years. The understanding of the behavior of nanostructures in various conditions is warranted since the applications of such materials in optics, electronics, and mechanics is ever expanding. This thesis investigates a specific type of structure, a concentric cylindrical. More specifically, the dispersion relation of radiating and non-radiating plasmon polaritons (quasi-particles resulting from interactions of photons and surface electrons) is studied under varying conditions. We intend to show the influence of changing the thickness of the layers, the number of layers, the curvature of each layer, and the type of material the layers has on the dispersion relation. By first solving Maxwell's equations in cylindrical coordinates and applying boundary conditions, we developed a matrix equation through which we were able to obtain the dispersion relation for an N layered cylindrical system characterized by a specified dielectric function placed into a background. For the non-radiative modes we used the bisection method to obtain the dispersion relation; however, since radiative modes encompass virtual modes, which contain real and imaginary components, a Newton method was used to gather that data. The dielectric functions for silver and carbon dielectric functions were used to describe the material layers within the radiative and non-radiative regimes. The results show that curvature changes influence the surface plasmon polariton dispersion by either red shifting or blue shifting the energetics. Lifetimes and damping are seen to be influenced by the curvature as well. The addition of more layers to the system results in an increase in the complexity of the dispersion energetics. The results obtained would help provide better scanning tips within the optical microscopy field. Also, these results can have direct application to the field of photonics. Finally, these results also help provide the foundations to understanding the fundamentals of long-ranged forces in cylindrical layered structures.

Dans une cellule solaire, il existe un compromis entre l’efficacité d’absorption des photons et le rendement quantique de collection des charges électriques. Dans les semi-conducteurs organiques, la longueur de diffusion des porteurs est limitée à une centaine de nanomètres, si bien qu’il est nécessaire de travailler avec des couches photo-actives ultraminces (< 100 nm). Pour limiter l’épaisseur physique des matériaux utilisés tout en maintenant une absorption élevée, il est possible d’utiliser les propriétés des cristaux photoniques (CP), pour allonger la durée d’interaction des photons avec le milieu absorbant. Cela consiste à former un CP dans la couche active ou à son voisinage et d’exciter des modes résonants de la structure. Ce travail de thèse est divisé en plusieurs parties. Dans un premier temps, à l’aide d’outils numériques, nous nous intéressons aux phénomènes qui régissent le gain d’absorption lors du couplage d’une onde plane avec un mode résonant d’une membrane à CP. Ensuite, nous étudions une cellule à CP, où l’électrode d’ITO est nano-structurée, et nous optimisons le gain d’absorption d’une couche photo-active ultramince (50 nm). Enfin, dans un travail expérimental, nous fabriquons des cristaux colloïdaux bidimensionnels à base de microsphères diélectriques par différentes méthodes d’auto assemblage. / In a solar cell, there is a trade-off between light absorption capacity and internal quantum efficiency. In organic semi conductors, charge carrier diffusion is limited to a few hundred nanometers, which implies to work with very thin active layers (< 100 nm). In order to limit the thickness of the material while keeping high light absorption, it is possible to use the properties of photonic crystals (PC) to enhance light matter interaction duration. It consists in forming a PC in or around the active layer, and to excite a resonant mode of the formed photonic structure. The work of this thesis is divided into several parts. In a first approach, using numerical tools, we investigate the phenomena that give rise to absorption enhancement when a plane wave is coupled to a resonant mode of a PC membrane. We then study a nano-structured cell architecture, in which the ITO electrode is periodically patterned, and we optimize absorption enhancement in the thin active layer (50 nm). Finally, in an experimental work, we fabricate two dimensional colloidal crystals formed by dielectric microsphere self assembly.

Plasmonics is a successful new field of science and technology that exploits the exclusive optical properties of metallic nanostructures to manipulate and concentrate light at nano-meter length scales. When light hits the surface of gold or silver nanoparticles it can excite collective oscillations of the conduction electrons called surface plasmons. This surface plasmon undergoes two damping processes; it can decay into photon and reemit the plasmon energy as scattered energy or decay into electron-hole pair with the excitation energy equal to the energy of the plasmon resonance, known as absorption. This high energy electron subsequently undergoes into the carrier multiplication and eventually scatters into the electrons with lower energy. We used Finite-Difference Time-Domain (FDTD) and Finite-Element Method (Comsol) to design nanoscale structures to act as nanoantenna for light harvesting and consequently manipulating radiative and absorption properties of them for Sensing and Photovoltaic applications. To manipulate near and far field we designed our structures in a way that the bright and dark plasmon modes overlap and couple to each other. This process is called Fano resonance and introduces a transparency window in the far-field spectra. At the same time it increases the near-field enhancement. We applied the changes in near-field and far-field to SERS (Surface Enhanced Raman Spectroscopy) and LSPR (Localized Surface plasmon Resonance) shift for sensing purposes. We modeled Fano resonances with classical harmonic oscillator and reproduced the same feature with a simple equation of motion. We used this model to replicate scattering spectra from different geometries and explain the cathodoluminescence results obtained from nanoscale gold clusters structure. All of these nanoantenna optical properties and applications are due to the reemission ability of the plasmon energy to the vacuum and confining optical field, but the plasmon energy can decay into a high energy carrier rather than radiation. Photons coupled into metallic nanoantenna excite resonant plasmons, which can decay into energetic, hot electrons injected over a potential barrier at the nanoantenna-semiconductor interface, resulting in a photocurrent. We design a device which the range of its potential applications is extremely diverse. As silicon based detector capable of detecting sub-band gap photons, this device could be used in photovoltaic devices to harvest solar energy. Plasmon generated hot electrons can be used in photocatalytic dissociation of H2 molecules at the room temperature as well. The hot electrons in their higher energy states can populate the antibonding orbital of H2 molecules adsorbed on the metal surface and thus trigger the H2 molecule dissociation. The goal is to demonstrate the high efficiency of metallic photocatalytic systems by detecting the formation of HD molecules from the individual dissociation of two isotopes, H2 and D2. At the end we introduce lightning rod effect in metallic nanostructures and investigated the relation between the geometry properties of micrometer rod antennas and the electromagnetic field enhancement induced due to the lightning rod effect. At long wavelength, metals behave like perfect equipotential conductors and all the field enhancement results from the drop of potentials across the junctions between individual nanoparticles. This phenomenon is called lightning rod effect. By designing proper geometry we were able to utilize this effect to obtain enough electromagnetic enhancements in MIR region of spectrum to observe SEIRA signals from few hemoglobin molecules. Our simulation shows that the field enhancement obtained from this antenna does not depend sensitively on wavelength which is another advantage for SEIRA spectroscopy. We offered an analytical model to explore the coupling between the hemoglobin molecules and the Efield. We used this model to study the location effect of the molecule on the reflection signal. This technique allows us to detect the vibrational mode of molecules such as Hemoglobin in the real time and study their changes when the molecules are exposed to different environmental circumstances.

The electronic structure and optical properties of metallic nanoparticles are theoretically investigated front first principles. An efficient implementation of time-dependent density functional theory allows a fully quantum mechanical description of systems large enough to display collective electron oscillations and surface plasmon modes. The results are compared with traditional classical electrodynamical approaches. Different regimes of interest are identified, both where classical electrodynamical models yield accurate descriptions, and where quantum effects are indispensable for understanding plasmonic properties in nanostructures. The limits of validity of classical electrodynamics are clearly established for the study of a variety of relevant geometries.

The Photonic Crystal (PC) is a potential candidate for a compact optical integrated circuit on a solid state platform. The fabrication process of a PC is compatible with CMOS technology; thus, it could be potentially employed in hybrid optical and electrical integrated circuits. One of the main obstacles in the implementation of an integrated optical circuit is the polarization dependence of wave propagation. Our goal is to overcome this obstacle by implementing PC based polarization controlling devices. One of the crucial elements of polarization controlling devices is the polarization rotator. The polarization rotator is utilized to manipulate and rotate the polarization of light. In this thesis, we have proposed, designed and implemented an ultra-compact passive PC based polarization rotator. Passive polarization rotator structures are mostly composed of geometrically asymmetric structures. The polarization rotator structure consists of a single defect line PC slab waveguide. The geometrical asymmetry has been introduced on top of the defect line as an asymmetric loaded layer. The top loaded layer is asymmetric with respect to the z-axis propagation direction. To synchronize the power conversion and avoid power conversion reversal, the top loaded layer is alternated around the z-axis periodically. The structure is called periodic asymmetric loaded PC slab waveguide. Due to the compactness of the proposed structure, a rigorous numerical method, 3D-FDTD can be employed to analyze and simulate the final designed structure. For the quick preliminary design, an analytical method that provides good approximate values of the structural parameters is preferred. Coupled-mode theory is a robust and well-known method for such analyses of perturbed waveguide structures. Thus, a coupled-mode theory based on semi-vectorial modes was developed for propagation modeling on square hole PC structures. In essence, we wish to develop a simple yet closed form method to carry out the initial design of the device of interest. In the next step, we refined the design by using rigorous but numerically expensive 3D-FDTD simulations. We believe this approach leads to optimization of the device parameters easily, if desired. To extend the design to a more general shape PC based polarization rotator, a design methodology based on hybrid modes of asymmetric loaded PC slab waveguide was introduced. The hybrid modes of the structure were calculated utilizing the 3D-FDTD method combined with the Spatial Fourier Transform (SFT). The propagation constants and profile of the slow and fast modes of an asymmetric loaded PC slab waveguide were extracted from the 3D-FDTD simulation results. The half-beat length, which is the length of each loaded layer, and total number of the loaded layers are calculated using the aforementioned data. This method provides the exact values of the polarization rotator structure’s parameter. The square hole PC based polarization rotator was designed employing both coupled-mode theory and normal modal analysis for THz frequency applications. Both design methods led to the same results. The design was verified by the 3D-FDTD simulation of the polarization rotator structure. For a square hole PC polarization rotator, a polarization conversion efficiency higher than 90% over the propagation distance of 12 λ was achieved within the frequency band of 586.4-604.5 GHz corresponding to the normalized frequency of 0.258-0.267. The design was extended to a circular hole PC based polarization rotator. A polarization conversion efficiency higher than 75% was achieved within the frequency band of 600-604.5 GHz. The circular hole PC polarization rotator is more compact than the square-hole PC structure. On the other hand, the circular hole PC polarization rotator is narrow band in comparison with the square hole PC polarization rotator. In a circular hole PC slab structure, the Bloch modes (fast and slow modes) couple energy to the TM-like PC slab modes. In both square and circular hole PC slab structures with finite number of rows, and the TM-like PC slab modes are extended to the lower edge of the bandgap. In bandgap calculation using PWEM, it is assumed that the PC structure is extended to infinity, however in practice the number of rows is limited, which is the source of discrepancy between the bandgap calculation using PWEM and 3D-FDTD. In an asymmetric loaded circular hole PC slab waveguide, the leaky TM-like PC slab modes are extended deep inside the bandgap and overlapped with both the slow and fast Bloch modes; whereas, in an asymmetric loaded square hole PC slab waveguide, the leaky TM-like PC slab modes are below the frequency band of slow and fast modes. Therefore, TM-like PC slab modes have significantly more adverse effect on the performance of the circular-hole based polarization rotator leading to a narrow band structure. SOI based PC membrane technology for THz application was developed. The device layer is made of highly resistive silicon to maintain low loss propagation for THz wave. The PC slab waveguide and polarization rotators were fabricated employing this technology. Finally, an a-SiON PC slab waveguide structures were also fabricated at low temperature for optical applications. This technology has the potential to be implemented on any substrate or CMOS chips.

Nanophotonics, especially plasmonics is a kind of very active research area, which deals with the interaction behavior between electromagnetic radiation and metallic nanostructures. It has attracted enormous attention over recent decades due to its great potential of ripple effects on electronics, energy, environmental, and medical industries as well as scientific interests. In particular, noble metal nanoparticles exhibit localized surface plasmon resonance (LSPR), which is the collective oscillating excitation of the free electrons on the surface of metal nanoparticles when light is incident on the particle. The LSPR extinction peak is very sensitive to the dielectric environment near the particle surface and can be tailored by the particle's sizes and shapes. These properties allow LSPR-active substrate using plasmonic gold nanoparticles to be a great transducer for biosensing with real-time and label-free measurement. In addition, the plasmonic gold nanoparticles such as gold nanorod and bipyramid are prepared by the seed-mediated and surfactant-directed method based on the cetyltrimethylammonium bromide (CTAB), which has a great influence on the synthesis. In the growth mechanism, it is believed that CTAB interacts with different facet and defects on the growing nanoparticles to produce different rate of gold ion reduction onto the nanoparticles to generate anisotropic growth. Therefore, CTAB layer is greatly interesting because the modification of nanoparticles surface chemistry is essential to biological targeting, film formation, and assembly of complex structures. Surface enhanced Raman spectroscopy (SERS) of gold nanorods in CTAB solution has been used to analyze a surfactant structural transition based on the distance dependent electromagnetic enhancement. As the surfactant concentration in the gold nanorod solution was reduced, a structural transition in the surfactant layer between 2 mM and 5 mM CTAB solution was observed through a sudden increase in the signal from the alkane chains. A structural transition in the CTAB layer that stabilizes gold nanorods was identified by comparing the intensities of different bands within the CTAB molecule. Therefore, the surface manipulation and analysis of the nanostructures and their interface with controlled environment provide important insight into their structural function and interpretation, and many opportunities for biomedical applications.

The Photonic Crystal (PC) is a potential candidate for a compact optical integrated circuit on a solid state platform. The fabrication process of a PC is compatible with CMOS technology; thus, it could be potentially employed in hybrid optical and electrical integrated circuits. One of the main obstacles in the implementation of an integrated optical circuit is the polarization dependence of wave propagation. Our goal is to overcome this obstacle by implementing PC based polarization controlling devices. One of the crucial elements of polarization controlling devices is the polarization rotator. The polarization rotator is utilized to manipulate and rotate the polarization of light. In this thesis, we have proposed, designed and implemented an ultra-compact passive PC based polarization rotator. Passive polarization rotator structures are mostly composed of geometrically asymmetric structures. The polarization rotator structure consists of a single defect line PC slab waveguide. The geometrical asymmetry has been introduced on top of the defect line as an asymmetric loaded layer. The top loaded layer is asymmetric with respect to the z-axis propagation direction. To synchronize the power conversion and avoid power conversion reversal, the top loaded layer is alternated around the z-axis periodically. The structure is called periodic asymmetric loaded PC slab waveguide. Due to the compactness of the proposed structure, a rigorous numerical method, 3D-FDTD can be employed to analyze and simulate the final designed structure. For the quick preliminary design, an analytical method that provides good approximate values of the structural parameters is preferred. Coupled-mode theory is a robust and well-known method for such analyses of perturbed waveguide structures. Thus, a coupled-mode theory based on semi-vectorial modes was developed for propagation modeling on square hole PC structures. In essence, we wish to develop a simple yet closed form method to carry out the initial design of the device of interest. In the next step, we refined the design by using rigorous but numerically expensive 3D-FDTD simulations. We believe this approach leads to optimization of the device parameters easily, if desired. To extend the design to a more general shape PC based polarization rotator, a design methodology based on hybrid modes of asymmetric loaded PC slab waveguide was introduced. The hybrid modes of the structure were calculated utilizing the 3D-FDTD method combined with the Spatial Fourier Transform (SFT). The propagation constants and profile of the slow and fast modes of an asymmetric loaded PC slab waveguide were extracted from the 3D-FDTD simulation results. The half-beat length, which is the length of each loaded layer, and total number of the loaded layers are calculated using the aforementioned data. This method provides the exact values of the polarization rotator structure’s parameter. The square hole PC based polarization rotator was designed employing both coupled-mode theory and normal modal analysis for THz frequency applications. Both design methods led to the same results. The design was verified by the 3D-FDTD simulation of the polarization rotator structure. For a square hole PC polarization rotator, a polarization conversion efficiency higher than 90% over the propagation distance of 12 λ was achieved within the frequency band of 586.4-604.5 GHz corresponding to the normalized frequency of 0.258-0.267. The design was extended to a circular hole PC based polarization rotator. A polarization conversion efficiency higher than 75% was achieved within the frequency band of 600-604.5 GHz. The circular hole PC polarization rotator is more compact than the square-hole PC structure. On the other hand, the circular hole PC polarization rotator is narrow band in comparison with the square hole PC polarization rotator. In a circular hole PC slab structure, the Bloch modes (fast and slow modes) couple energy to the TM-like PC slab modes. In both square and circular hole PC slab structures with finite number of rows, and the TM-like PC slab modes are extended to the lower edge of the bandgap. In bandgap calculation using PWEM, it is assumed that the PC structure is extended to infinity, however in practice the number of rows is limited, which is the source of discrepancy between the bandgap calculation using PWEM and 3D-FDTD. In an asymmetric loaded circular hole PC slab waveguide, the leaky TM-like PC slab modes are extended deep inside the bandgap and overlapped with both the slow and fast Bloch modes; whereas, in an asymmetric loaded square hole PC slab waveguide, the leaky TM-like PC slab modes are below the frequency band of slow and fast modes. Therefore, TM-like PC slab modes have significantly more adverse effect on the performance of the circular-hole based polarization rotator leading to a narrow band structure. SOI based PC membrane technology for THz application was developed. The device layer is made of highly resistive silicon to maintain low loss propagation for THz wave. The PC slab waveguide and polarization rotators were fabricated employing this technology. Finally, an a-SiON PC slab waveguide structures were also fabricated at low temperature for optical applications. This technology has the potential to be implemented on any substrate or CMOS chips.