archives@tulane.edu / Quantum nonlinear optics has opened up avenues to defy the measurement, sensing, and amplification limits inherent in classical physics. Separately, the use of multimode or spatially structured states in light-based communications allows for remarkable increases in the amount of information that may be transferred by an individual communication or light pulse. In this dissertation, we apply these two boundary-pushing concepts to several experimental projects, with a primary goal to hasten and facilitate the implementation of quantum and classical free-space optical communications schemes into real-life scenarios. We start by applying neural networks to the optimization of spatially-structured and pulsed light communications in Chapter 2, wherein our networks successfully learn to predict distorted optical pulses and classify noisy light patterns carrying non-zero orbital angular momentum. Chapter 3 focuses on four-wave mixing, a nonlinear light-matter interaction in atomic vapor that we use to construct quantum-correlated light beams with nontrivial structures as well as a novel phase-sensitive amplifier. Finally, we continue to take advantage of the complex nonlinear response of atomic vapor in Chapter 4, this time to create "self-regenerating" light beams whose cross-sections resemble Bessel-Gauss functions. / 1 / Erin Knutson

Thulium (Tm) based high repetition rate compact optical frequency comb sources operating in the 2 µm regime with femtosecond pulse durations enable a wide range of applications such as precise micro-machining, spectroscopy and metrology. Applications such as metrology and spectroscopy rely on the stability of mode-locked lasers (MLLs) which provide extreme precision, yet, the complex dynamics of such highly nonlinear systems result in unstable events which could hinder the normal operation of a MLL. MLL as a nonlinear system inherently exists a wide variety of complex attractors, which are sets of states that the system tends to evolve toward, exhibiting unique behaviors. Complex phenomena including pulsating solitons, chaotic solitons, period-doubling, soliton explosion, etc., have been predicted theoretically and observed experimentally in the past decade. However, most experimental observations rely on conventional characterization methods, which are limited to the scanning speed of the spectrometer and the electronic speed of photodetector and digitizer, so that the details of the non-repetitive events can be buried. In recent years, a technique called dispersive Fourier transform (DFT) has been developed and allows consecutive recordings of the pulse-to-pulse spectral evolution of a femtosecond pulse train, opening a whole new world of nonlinear dynamics in MLL. In this dissertation, we first demonstrate the ability of scaling the repetition rate of a Tm MLL to repetition rate as high as 1.25 GHz through miniaturizing the cavity. Our approach of maintaining comparable pulse energies while scaling the repetition rates allows a high-quality femtosecond mode-locking performance with low noise performance in Tm soliton lasers. Then we experimentally study the transition dynamics between consecutive multi-pulsing states through adjusting pump power with a constant rate in an erbium-doped fiber laser, specifically the build-up and annihilation of soliton pulses between a double pulsing and a three-pulse state utilizing DFT. To investigate real-time laser dynamics in Tm based laser systems, we propose and develop a DFT system that up-converts the signal to the 1 µm regime via second harmonics generation (SHG) and stretches the signal in a long spool of single-mode fiber to realize DFT. This approach overcomes the limitation of bandwidth of 2 µm photodetector and high intrinsic absorption of 2 µm light in fused silica fibers. The SHG-DFT system is used to study dynamics of both explosions in a chaotic state between stable single-pulsing and double-pulsing state, and explosions induced by soliton collision in a dual-wavelength vector soliton state. We also study dynamics of transient regimes in a Tm-doped fiber ring laser that can be switched between conventional soliton and dissipative soliton, revealing how spectral filtering plays a role in obtaining stable stationary states. / 2022-11-23T00:00:00Z

Two experimental methods, optical limiting and degenerate four-wave mixing, are employed to study the nonlinear optical properties of various novel fullerenes structures. Optical limiting refers to decreased transmittance of a material with increased incident light intensity. Detailed measurements of the wavelength-dependence of fullerene optical limiters have illustrated several key features of reverse saturable absorption. Most important among these is the requirement of weak but non-negligible ground state absorption. We have shown that the optical limiting performance of C₆₀ can be extended into the near infrared range by appropriate modifications of the structure such as higher cage fullerenes or derivatization of the basic C₆₀ molecule. The higher cage fullerene C₇₆ shows improved optical limiting behavior compared to C₆₀, for wavelengths higher than 650 nm, but becomes a weak limiter in the 800 nm range. C₈₄, even at high concentrations in [alpha]-chloronaphthalene, does not reach the good performance of C₆₀, but instead shows weak optical limiting in the 800 nm range. We also demonstrate that by attaching various groups to the C₆₀ molecule, we can extend the optical limiting performance in the near infrared regime. The C₆₀ derivatives studied, (C₆₀ cyclic ketone, C₆₀ secondary amine, C₆₀CHC₆H₄CO₂H, and C₆₀C₄H₄(CH₃)CH₂O₂C(CH₂)CO₂H), have a similar characteristic: the attached groups cause a symmetry-breaking of the C₆₀ sphere and, therefore, there are new allowed transitions that appear as absorption features up to 750 nm. The optical limiting measurements show that these materials, even for low input energies, have an exceptionally strong optical limiting response in the 640 to 750 nm spectral region. For wavelengths higher than 800 nm, however, they become transparent and no optical limiting is observed. Excited state absorption cross-sections obtained from analysis of the optical limiting data reveal that the C₆₀ derivatives have a maximum triplet-triplet absorption cross-section at 700 nm, which is shifted from the 750 nm value for the C₆₀ molecule. For the first time, optical limiting measurements are performed on five separate C₈₄ isomers. These intriguing results show that the optical limiting behavior is strongly dependent on the cage symmetry. It is also found that the most abundant isomer does not have the strongest optical limiting performance, but is in fact one of the weaker optical limiters of the isomers isolated so far. The endohedral metallofullerenes are a unique class of fullerene materials and consist of one or more metal atoms encapsulated inside the buckyball cage. An important characteristic of these materials is the charge-transfer from the dopant atoms to the fullerene cage, which has a high electron affinity. The charge-transfer is similar to the optical excitation in a material, but although the electrons are placed in the lowest unoccupied molecular orbital (LUMO), there are no holes produced in the highest occupied molecular orbital (HOMO). This is an important analogy, since it has been previously shown that optical excitation enhances the nonlinear optical properties of a material. The nonresonant degenerate four-wave mixing experiments performed on the endohedral metallofullerene Er₂@C₈₂, at 1064 nm, show that the third order nonlinear susceptibility value is increased by orders of magnitude relative to the empty cage fullerenes, thus, confirming the charge-transfer process from the encapsulated atoms to the fullerene cage. We obtain a value [gamma]_xyyx⁽³⁾( &#173 [omega]; [omega], [omega], &#173 [omega])= &#173 8.65 &#215 10⁻³² esu for the molecular second order hyperpolarizability, which is almost three orders of magnitude larger than the values reported in literature for an empty cage fullerene. / Ph. D.

This doctoral dissertation focuses on the nonlinear optical response of water vapour as well as some solids at terahertz (THz) frequencies. In this study, the propagation of broadband single-cycle THz pulses through a medium with the third-order nonlinear optical response is theoretically investigated. Also, a technique to measure the nonlinear response of transparent materials based on the time-domain THz spectroscopy is developed, which provides frequency dispersion curves of the nonlinear Kerr coefficient (n₂). A numerical model is used to simulate the THz pulse propagation. This model takes into account non-paraxial effects, self-focusing, and diffraction, as well as dispersion, in both the linear and nonlinear optical regimes. The contribution of non-instantaneous Kerr-type nonlinearity to the overall instantaneous and delayed Kerr effect at the THz frequencies is investigated. It is shown how increasing the nonlinear relaxation time and its dispersion modifies the THz pulse after the propagation through a transparent medium. The effect of linear dispersion on self-action during pulse propagation is also discussed. Moreover, the nonlinear spectroscopy of water vapour at THz frequencies is reported. Atmospheric water vapour has a rich spectrum with several strong resonances at frequencies below 3 THz, falling within the range of operation of most existing THz sources. An extremely large nonlinear response to THz radiation is observed at the positions of these resonances. Using the optical Kerr model for the nonlinear response, a minimum nonlinear refractive index of the order of 10² m²/W is estimated. The results provide insight into the energy levels of the water molecule and give a more accurate picture of its response to electromagnetic radiation, paving the way to more accurate THz spectroscopy, imaging, and sensing systems, and thereby facilitating future emerging THz technologies. Finally, the nonlinear response of solids at THz frequencies is studied. It has been shown that a phonon-induced THz Kerr effect can result in a larger nonlinear refractive index than the nonlinear refractive index at the visible or near-infrared range (optical Kerr effect). This pronounced nonlinear optical behavior is verified using a time-domain characterization approach. The results indicate a large delay occurred to the THz fields as they transmit through some of the material samples. In the frequency domain, the induced nonlinear phase shift of the intense THz field is shown to be relatively large of the order of 0.1 rad. From the phase information, the nonlinear phase is extracted by which the dispersion profile of n₂ is obtained.

Les sources infrarouges basées sur des effets d'optique du second ordre constituent de très bons outils de spectrométrie des polluants présents dans l'atmosphère, grâce notamment à leur grande accordabilité spectrale. Ils demandent toutefois une forte puissance lumineuse incidente et une grande quantité de matériau non linéaire pour être efficaces. On peut les rendre très compactes en réalisant la conversion de fréquence à l'aide de nanostructures plasmoniques contenant des inclusions diélectriques présentant une susceptibilité du deuxième ordre non nulle. La lumière y est très fortement concentrée à la résonance augmentant fortement la quantité de polarisation non linéaire produite, afin d'y exalter les effets d'optique non linéaire.Ce travail s'attaque d'abord à la conception de nano-résonateurs grâce au développement d'un outil de simulation d’empilements nanostructurés selon une dimension. Trois architectures sont étudiées : les nanorésonateurs de type sillon, les nanorésonateurs de Helmholtz et les guides d'ondes à résonances de modes guidés. Dans chaque cas, le dimensionnement passe par la détermination de géométries bi- voire tri-résonantes pour la réalisation d'accord de modes en génération de second harmonique ou de différence de fréquences.La fabrication en salle blanche des résonateurs sillons et guides d'ondes est ensuite exposée, suite à un important travail de développement technologique, qui a permis l’obtention d’échantillons de très bonne qualité. / Infrared sources based on second order effects are interesting tools for atmospheric pollutants spectrometry thanks to their wide tunability. Such effects nevertheless demand strong incident powers or massive non linear crystals to be efficient. A new way to reduce their size consists in realizing frequency conversion with the help of plasmonic nanostructures containing dielectric inclusions showing a non zero second order susceptibility. Light is greatly harvested and concentrated at resonance leading to the creation of a great quantity of non linear polarization, so as to further enhance non linear optics effects.This work begins with a study of nanoresonators through developing a simulation tool for one dimensional nanostructured multilayered structures. Three architectures are retained : slit nanoresonators, optical Helmholtz nanoresonators and waveguides based on guided mode resonances. In every case, the conception focuses on the finding of bi- and even of tri-resonant geometries to achieve mode matching for second harmonic of difference frequency generation.Clean room fabrication is then detailed step by step following the important works that have permitted the fabrication of samples showing a very good quality.

Le but de cette thèse et de la recherche associée est une démonstration des avantages d’une combinaison de propriétés inhabituelles de nanostructures plasmoniques avec des aspects parmi les plus intéressants de l’optique non-linéaire. Pour cet effet, la modélisation analytique et numérique a été combiné avec le travail expérimental, qui comprenait la production de nanostructures et les mesures effectuées au moyen de la microscopie confocale non-linéaire résolue en polarisations et de la technique Z-scan modifiée (nommée “f-scan”).Il a été montré que l’anisotropie efficace de génération de seconde-harmonique dans les cristaux plasmoniques (formés par des réseaux rectangulaires de cavités tétraédriques sur une surface d’argent) peut être contrôlée par un choix approprié des paramètres de maille. Il a aussi été montré que cette anisotropie provient principalement d’une structure de bande photonique elle-même anisotrope, présentant une bande interdite plasmonique avec des états plasmoniques en bord de bande, permettant de renforcer le champ électrique local. Les arrangements chiraux bidimensionnels de nanoparticules triangulaires d’or, forment des “meta-molécules” plasmoniques énantiomériques, ont été analysés par microscopie non-linéaire à la lumière polarisée circulairement et par modélisation numérique, révélant un fort effet chiroptique par génération de seconde harmonique en rétro-réflexion. La petite taille des énantiomères uniques permet de créer “des filigranes” (“watermarks”) codés par la chiralité des meta-molécules, qui peuvent être lu par imagerie de la génération de seconde harmonique excitée par un rayon polarisé circulairement. Les caractéristiques quantitatives de la non-linéarité optique du troisième ordre et de l’efficacité d’absorption saturable des solutions aqueuses de fragments de graphène et de graphène dopé par des nanoparticules d’or a été effectuée par une nouvelle technique “f-scan”, qui a été créée et développée par incorporation d’une lentille à distance focale accordable dans une technique de Z-scan traditionnelle. Ces études ont montrées que le graphène présente une absorption saturable ultra-rapide très efficace, qui est parfois convertie en absorption saturable inverse. Il apparaît alors qu’une décoration du graphène par des nanoparticules d’or peut causer une légère amélioration du paramètre d’efficacité d’absorption saturable dans la plage spectrale de leurs résonances plasmoniques. En résumé, cette thèse présente une variété de propriétés optiques non-linéaires apparaissant dans les nanostructures plasmoniques. Différentes possibilités de contrôle de ces propriétés au moyen d’une démarche de nano-ingénierie, soutenue par des modélisations à la fois analytique et numérique ont été démontrées et analysées. Ces travaux ouvrent la voie à la fabrication et à l‘optimisation sur mesure de nouveaux nano-matériaux et nano-dispositifs photoniques reposant sur des effets de nano-plasmonique non-linéaire. / The aim of this thesis and the underlying research work is to demonstrate the benefits emerging from combination of the peculiar properties of plasmonic nanostructures with the most interesting aspects of nonlinear optics. For this purpose, analytical and numerical modeling was combined with experimental work, which included nanofabrication and measurements performed by means of polarization-resolved nonlinear confocal microscopy and by modified Z-scan technique (called "f-scan").It has been shown that the effective anisotropy of the second-harmonic generation in plasmonic crystals (formed by rectangular arrays of tetrahedral recesses in silver surface) can be controlled by proper choice of lattice constants. It also has been shown that this anisotropy arises mainly from the anisotropic photonic band structure, exhibiting plasmonic band gap with plasmonic band edge states, enabling enhancement of the local electric field.Two-dimensional chiral arrangements of triangular gold nanoparticles, forming plasmonic enantiomeric "meta-molecules", have been studied by nonlinear microscopy operating with circularly polarized light and by numerical modeling, revealing strong chiroptical effect in backscattered second-harmonic radiation. Small size of individual enantiomers allows to create "watermarks", encoded by the chirality of meta-molecules, which can be readout by imaging of second-harmonic generation excited by circularly polarized laser beam.Quantitative characterization of the third-order optical nonlinearity and saturable absorption efficiency of aqueous solutions of graphene and gold-nanoparticle decorated graphene has been performed by novel "f-scan" technique, which has been created and developed by incorporation of a focus-tunable lens into traditional Z-scan. These studies have shown that the graphene exhibits very efficient ultrafast saturable absorption, which is occasionally suppressed by reverse saturable absorption. Moreover, it turns out that decoration of graphene by gold nanoparticles may cause a slight improvement of the saturable absorption efficiency parameter within spectral range of their plasmon resonances.In summary, the following thesis presents various nonlinear optical properties of plasmonic nanostructures. Different possibilities of controlling these properties by means of nano-engineering, supported by analytical and numerical modeling, is also analyzed and demonstrated. This work opens up new perspectives for fabrication and rational design of novel photonic nano-materials and nano-devices based on nonlinear nanoplasmonic phenomena.

This thesis will explore the ultrafast modulation and optical tunability of plasmonic filters in the terahertz (THz) spectral region. First, the principles and functional design of THz metasurfaces are explored through plasmonic surface lattice resonance interactions and lumped-element circuit models. We will then describe the methodology of generating and detecting THz radiation through the nonlinear processes of optical rectification and electrooptic sampling, respectively. Next, the implementation of a THz time-domain spectroscopy technique is discussed in the context of pump-probe measurements and time-domain resonance analysis. We then show how THz probed materials can be characterized in terms of a temporal and spectral analysis. We will demonstrate how this time-domain technique can allow us to characterize the interaction of plasmonic resonators with optically active substrates and 2D nanomaterials. A completely tunable THz plasmonic notch resonance is modulated utilizing a static and dynamic method of optical tunability in silicon. Active tunability is also demonstrated in a graphene-based plasmonic resonator through the hot carrier multiplication effect. The significance of this work lies in the application of designing controllable devices for future THz communication technologies.

京都大学 / 0048 / 新制・論文博士 / 博士(工学) / 乙第12984号 / 論工博第4131号 / 新制||工||1637(附属図書館) / 32454 / 京都大学大学院工学研究科電子物性工学専攻 / (主査)教授 北野 正雄, 教授 竹内 繁樹, 准教授 久門 尚史 / 学位規則第4条第2項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

The continued development of integrated photonic devices requires low-power, small volume all-optical modulators. The weak nonlinear optical response of conventional optical materials requires the use of high intensities and large interaction volumes in order to achieve significant light modulation, hindering the miniaturization of all-optical switches and the development of lightweight transmission optics with nonlinear optical response. These challenges may be addressed using plasmonic nanostructures due to their unique ability to confine and enhance electric fields in sub-wavelength volumes. The ultrafast nonlinear response of free electrons in such plasmonic structures and the fast thermal nonlinear optical response of metal nanoparticles, as well as the plasmon enhanced nonlinear Kerr-type response of the host material surrounding the nanostructures could allow ultrafast all-optical modulation with low modulation energy. In this thesis, we investigate the linear and nonlinear optical response of engineered effective media containing coupled metallic nanoparticles. The fundamental interactions in systems containing coupled nanoparticles with size, shape, and composition dissimilarity, are evaluated analytically and numerically, and it is demonstrated that under certain conditions the achieved field enhancement factors can exceed the single-particle result by orders of magnitude in a process called cascaded plasmon resonance. It is demonstrated that these conditions can be met in systems containing coupled nanospheres, and in systems containing non-spherical metal nanoparticles that are compatible with common top-down nanofabrication methods such as electron beam lithography and nano-imprint lithography. We show that metamaterials based on such cascaded plasmon resonance structures can produce enhanced nonlinear optical refraction and absorption compared to that of conventional plasmonic nanostructures. Finally, it is demonstrated that the thermal nonlinear optical response of metal nanoparticles can be enhanced in carefully engineered heterogeneous nanoparticle clusters, potentially enabling strong and fast thermal nonlinear optical response in system that can be produced in bulk through chemical synthesis.

Silicon photonics is nowadays a mature technology and is on the verge of becoming a blossoming industry. Silicon photonics has also been pursued as a platform for integrated nonlinear optics based on Raman and Kerr effects. In recent years, more futuristic directions have been pursued by various groups. For instance, the realm of silicon photonics has been expanded beyond the well-established near-infrared wavelengths and into the mid-infrared (3 - 5 µm). In this wavelength range, the omnipresent hurdle of nonlinear silicon photonics in the telecommunication band, i.e., nonlinear losses due to two-photon absorption, is inherently nonexistent. With the lack of efficient light-emission capability and second-order optical nonlinearity in silicon, heterogeneous integration with other material systems has been another direction pursued. Finally, several approaches have been proposed and demonstrated to address the energy efficiency of silicon photonic devices in the near-infrared wavelength range. In this dissertation, theoretical and experimental works are conducted to extend applications of integrated photonics into mid-infrared wavelengths based on silicon, demonstrate heterogeneous integration of tantalum pentoxide and lithium niobate photonics on silicon substrates, and study two-photon photovoltaic effect in gallium arsenide and plasmonic-enhanced structures. Specifically, performance and noise properties of nonlinear silicon photonic devices, such as Raman lasers and optical parametric amplifiers, based on novel and reliable waveguide technologies are studied. Both near-infrared and mid-infrared nonlinear silicon devices have been studied for comparison. Novel tantalum-pentoxide- and lithium-niobate-on-silicon platforms are developed for compact microring resonators and Mach-Zehnder modulators. Third- and second-harmonic generations are theoretical studied based on these two platforms, respectively. Also, the two-photon photovoltaic effect is studied in gallium arsenide waveguides for the first time. The effect, which was first demonstrated in silicon, is the nonlinear equivalent of the photovoltaic effect of solar cells and offers a viable solution for achieving energy-efficient photonic devices. The measured power efficiency achieved in gallium arsenide is higher than that in silicon and even higher efficiency is theoretically predicted with optimized designs. Finally, plasmonic-enhanced photovoltaic power converters, based on the two-photon photovoltaic effect in silicon using subwavelength apertures in metallic films, are proposed and theoretically studied.