Pour des applications technologiques d’enregistrement magnétique de l’information à haute densité et vitesse d’écriture et de lecture ultra-rapide, les chercheurs se sont penchés vers des méthodes de manipulation de l’aimantation sans application de champ magnétique externe. Il a été découvert qu’il était possible de renverser de manière déterministe l’aimantation de plusieurs matériaux ferri- et ferro-magnétiques à l’aide uniquement d’impulsions laser ultracourtes polarisées circulairement. Ce retournement tout-optique s’est avéré être un processus cumulatif nécessitant plusieurs impulsions ultracourtes dans les matériaux ferromagnétiques. Notamment dans les multicouches (Co/Pt), le retournement tout-optique se fait en deux étapes : une désaimantation indépendamment de l’hélicité suivie d’une ré-aimantation dans une direction ou l’autre selon l’hélicité. Pour autant, le mécanisme à l’origine du rétablissement de l’ordre magnétique n’a pas été étudié jusqu’à présent. Dans cette thèse, nous avons étudié le mécanisme de renversement de l’aimantation dans les couches ferromagnétiques résultant de l’excitation par impulsions laser ultracourtes polarisées circulairement. Pour cela, nous étions intéressé par la réponse d’une paroi de domaine dans les couches minces de Pt/Co/Pt à la suite d’une excitation laser et en fonction de la polarisation de la lumière. Nous avons démontré la possibilité d’induire un déplacement tout-optique et déterministe d’une paroi de domaine. Nous montrons que la propagation de la paroi résulte de la compétition entre trois contributions : le gradient de température dû aux effets de chauffage par le laser, l’effet de l’hélicité de la lumière et les effets de piégeages de la paroi. Par ailleurs, par mesures expérimentales du dichroïsme circulaire, nous excluons un mécanisme purement thermique du déplacement de paroi. Ainsi nous confirmons que le retournement tout-optique des couches ferromagnétiques se fait par une nucléation suivie d’une ré-aimantation par propagation déterministe des parois de domaines selon l’hélicité. De plus, nous avons exploré la possibilité d’utiliser le retournement tout-optique dans des dispositifs spintroniques pour l’enregistrement de l’information à haute densité. Pour se faire, il est nécessaire d’étudier les effets de tailles du retournement lorsque le matériau est structuré en îlots à l’échelle du micro- ou nanomètre. Nous avons montré qu’un plus grand nombre d’impulsions laser est nécessaire afin de renverser l’aimantation de micro-disques comparés à la couche continue ferromagnétique. Il en résulte que le champ dipolaire aide le renversement de l’aimantation dans les couches continues rendant ainsi le retournement tout-optique énergétiquement plus favorable / Over the past decade, the demand for an even higher capacity to store data has been gradually increasing. To achieve ultrafast and ultrahigh density magnetic data storage, low-power methods to manipulate the magnetization without applying an external magnetic field has attracted growing attention. The possibility to deterministically reverse the magnetization with only circularly polarized light was evidenced in multiple ferri- and ferro-magnetic materials. This phenomenon was called helicity-dependent all-optical switching (HD-AOS). In ferromagnets, it was demonstrated that HD-AOS was a cumulative and multishot process with a helicity-independent demagnetization followed by a helicity-dependent magnetization recovery. Yet, the microscopic mechanism of this helicity-dependent remagnetization remained highly debated. In this thesis, we investigated the magnetization reversal mechanism of all-optical switching in ferromagnetic materials. To explore a potential switching process through domain nucleation and domain wall (DW) propagation, we studied the response of a DW upon femto- or pico-second laser irradiation in Co/Pt thin films that exhibit HD-AOS. We reported helicity-dependent all-optical domain wall motion. We demonstrated that it results from the balance of three contributions: the temperature gradient due to the laser heating, the helicity effect and the pinning effects. By measuring the magnetic circular dichroism, a purely thermal mechanism of the laser-induced DW motion appears to be excluded. Furthermore, we examined the size effects in AOS in Co/Pt films patterned into microdots with a diameter between 10 and 3 μm. This allowed us to explore the role of the dipolar field in the switching mechanism. We discovered that a larger number of laser pulses was required to reverse the magnetization of a microdot compared to the continuous film. This indicated that the dipolar field actually eases the magnetization reversal in the full film. Thus, AOS is less energy-efficient in patterned films, hence making Pt/Co/Pt multilayers not an ideal candidate for integrating AOS in spintronic devices

Demonstration of ultrafast all-optical signal processing (AOSP) using silicon as the active material has been limited by large two-photon absorption loss and long lifetimes of the resulting free carriers. For AOSP at speeds in the terahertz, an order of magnitude faster than that the fastest current electronic counterpart, a class of π-conjugated organic molecules called polymethines provides a promising alternative to silicon as they possess large third-order nonlinearities, and ultrafast polarization response to an incident field. The challenge in the application of polymethines as active nonlinear optical materials for AOSP is in translating their promising molecular properties into bulk material properties. The large linear polarizability and charged nature of the polymethines molecules strongly promote aggregation and phase-separation in solid blends, offsetting their advantageous molecular optical properties. In this work, polymethines’ resistance to deleterious spontaneous symmetry breaking and aggregation was enhanced by substitutions of metal- and chalcogen- containing terminal groups, and rigid steric groups above and below the π-conjugated plane of polymethine chain. The resulting polymethines/amorphous polycarbonate (APC) blend films demonstrated an unprecedentedly high two-photon figure-of-merit, |Re(χ(3))/Im(χ(3))| and low linear loss. The optical quality of the polymethines/APC films was also improved by replacing the commonly-used alkyl ammonium counterions with more polarizable aryl phosphonium counterions with moderate ground state dipole moment. The resulting dye-polymer blend films showed an enhanced near-infrared transparency while its magnitude of the third-order susceptibility, |χ(3)|, showed a good agreement with that extrapolated from the molecular third-order polarizability, γ. For facile integration of these promising organic materials into SOH, the substrate surface was functionalized using silane coupling chemistry for the reduction of surface energy mismatch between the polymer films and the waveguide containing substrates. The optical and SEM micrographs showed vastly improved coverage and infiltration of the microfeatures. Furthermore, to enable the precise engineering of waveguide cross-sectional dimensions for single-mode propagation in the organic cladding, the dispersion curves of the polymethines/polymer blends were generated using prism coupling and ellipsometry. The combined efforts in the development of molecules and materials discussed in the thesis have culminated into a successful identification and optimization of the polymethines dyes and their polymer blends for imminent demonstrations of on-chip AOSP at terahertz speed.

<p>One of the longstanding goals of photonics research has been to obtain strong optical nonlinearities. A promising method to achieve this goal is to operate in the so-called epsilon near zero (ENZ) spectral regime, where the real part of the dielectric permittivity changes sign. If accompanied by low losses, this region enables a platform to achieve extraordinarily high nonlinear response, along with many other interesting optical phenomena. In this work, some of the common all-optical switching structures employing homogeneous ENZ materials are investigated under varying conditions of frequency, incidence angle, and polarization. The optimum switching conditions have been highlighted to pave the way forward to the best experimental configurations in future studies. Moreover, the properties of some of the emerging novel plasmonic materials such as aluminum-doped zinc oxide (AZO) and titanium nitride (TiN) are investigated, specifically for ENZ applications. Their thickness-dependent crystalline structure and carrier densities are employed as a method to control their optical properties. A near-perfect absorption scheme is demonstrated utilizing the Ferrell-Berreman mode occurring at the ENZ region of ultrathin AZO and TiN film. The ENZ frequency and the associated absorption peak of AZO are engineered through thickness-dependence to cover most of the telecom range. This work covers the theoretical background for ENZ nonlinearities and looks into the materials aspect for better control of nonlinearities in experimental realizations.</p>

This thesis reports an experimental characterization of the ultrafast gain and refractive index dynamics of a novel InAs/InGaAsP/InP quantum-dot (QD) semiconductor optical amplifier (SOA) operating near 1.55-µm wavelengths, assessing its high-speed performance characteristics for the first time. The thesis also studies the influence of the degree of quantum confinement on the dynamics of SOAs by comparing the zero-dimensional (0-D) QD's dynamics to those in 1-D InAs/InAlGaAs/InP quantum-dash (QDash), and 2-D InGaAsP/InGaAsP/InP quantum-well (QW) SOAs, both of which also operate near 1.55-µm wavelengths, and are made with matching or similar materials and structures. The ultrafast (around 1 ps) and long-lived (up to 2 ns) amplitude and phase dynamics of the SOAs are characterized via advanced heterodyne pump-probe measurements with 150-femtosecond resolution. It is found that the QD SOA has an 80-picosecond amplitude, and 110-picosecond phase recovery lifetime in the gain regime, 4-6 times faster than the QDash and QW recovery lifetimes, as well as reduced ultrafast transients, giving it the best properties for high-speed (> 100 Gb/s) all-optical signal processing in the important telecommunications wavelength bands. An impulse response model is developed and used to analyze the dynamics, facilitating a comparison of the gain compression factors, time-resolved linewidth enhancement factors (alpha-factors), and instantaneous dynamic coefficients (two-photon absorption and nonlinear refractive-index coefficients) amongst the three structures. The quantum-dot device is found to have the lowest effective alpha-factor, 2-10, compared to 8-16 in the QW, as well as time-resolved alpha-factors lower than in the QW—promising for reduced-phase-transient operation at high bitrates. Significant differences in the alpha-factors of lasers with the same structure are found, due to the differences between gain changes that are induced optically or through the electrical bias. The relative contributions of stimulated transitions and free-carrier absorption to the total carrier heating dynamics in SOAs of varying dimensionality are also reported for the first time. Examining the QD electroluminescence and linear gain spectra in combination with the carrier dynamics also brings about conclusions on the nature of the quantum confinement, dot energy-level structure, and density of states—aspects of the material that have not been previously well understood.

This thesis reports an experimental characterization of the ultrafast gain and refractive index dynamics of a novel InAs/InGaAsP/InP quantum-dot (QD) semiconductor optical amplifier (SOA) operating near 1.55-µm wavelengths, assessing its high-speed performance characteristics for the first time. The thesis also studies the influence of the degree of quantum confinement on the dynamics of SOAs by comparing the zero-dimensional (0-D) QD's dynamics to those in 1-D InAs/InAlGaAs/InP quantum-dash (QDash), and 2-D InGaAsP/InGaAsP/InP quantum-well (QW) SOAs, both of which also operate near 1.55-µm wavelengths, and are made with matching or similar materials and structures. The ultrafast (around 1 ps) and long-lived (up to 2 ns) amplitude and phase dynamics of the SOAs are characterized via advanced heterodyne pump-probe measurements with 150-femtosecond resolution. It is found that the QD SOA has an 80-picosecond amplitude, and 110-picosecond phase recovery lifetime in the gain regime, 4-6 times faster than the QDash and QW recovery lifetimes, as well as reduced ultrafast transients, giving it the best properties for high-speed (> 100 Gb/s) all-optical signal processing in the important telecommunications wavelength bands. An impulse response model is developed and used to analyze the dynamics, facilitating a comparison of the gain compression factors, time-resolved linewidth enhancement factors (alpha-factors), and instantaneous dynamic coefficients (two-photon absorption and nonlinear refractive-index coefficients) amongst the three structures. The quantum-dot device is found to have the lowest effective alpha-factor, 2-10, compared to 8-16 in the QW, as well as time-resolved alpha-factors lower than in the QW—promising for reduced-phase-transient operation at high bitrates. Significant differences in the alpha-factors of lasers with the same structure are found, due to the differences between gain changes that are induced optically or through the electrical bias. The relative contributions of stimulated transitions and free-carrier absorption to the total carrier heating dynamics in SOAs of varying dimensionality are also reported for the first time. Examining the QD electroluminescence and linear gain spectra in combination with the carrier dynamics also brings about conclusions on the nature of the quantum confinement, dot energy-level structure, and density of states—aspects of the material that have not been previously well understood.