In this thesis, nonlinear periodic structures and their applications in both classical and quantum regime are investigated. New theoretical models are developed, and novel applications of nonlinear periodic structures are proposed and demonstrated. The theoretical studies, both design and simulation, are based on but not limited to InGaAsP material. A new method, namely the time-domain transfer-matrix (TDTM), is presented to simulate optical pulse propagation in layered media with resonant nonlinearity. As there were no satisfactory methods in the literature to model this problem, in order to validate and compare with the TDTM method, the standard FDTD method is generalized to include the rate equation in the analysis of semi-conductors. Also in this work, optical manipulation of absorption in periodic structures is studied for the first time. Thanks to the large accessible nonlinearity that results from the absorption saturation and frequency selectivity of periodic structures, a sensitive and compact optical limiter is designed. The novel design and modeling work developed in this thesis has provided new insights and tools to the utilization of resonant nonlinearities in compact all-optical devices.The experimental studies are based on quasi-phase matched AlGaAs superlattice waveguides. These devices have been previously designed and used for classical optical wavelength conversion such as second harmonic generation and difference frequency generation. In this work, these devices are exploited for spontaneous down conversion, which is a quantum effect, for the first time, through this process, entangled photon pairs are generated. Unprecedented performance, in terms of brightness and purity, of III-V semiconductor-based entangled photon sources has been demonstrated here. Moreover, the quantum properties of these entangled photons are characterized. The experimental studies presented in this thesis open up new application areas for III-V nonlinear optical devices as quantum sources and convincingly demonstrate the promising role of such devices will play in future quantum technologies.
In this thesis, nonlinear periodic structures and their applications in both classical and quantum regime are investigated. New theoretical models are developed, and novel applications of nonlinear periodic structures are proposed and demonstrated. The theoretical studies, both design and simulation, are based on but not limited to InGaAsP material. A new method, namely the time-domain transfer-matrix (TDTM), is presented to simulate optical pulse propagation in layered media with resonant nonlinearity. As there were no satisfactory methods in the literature to model this problem, in order to validate and compare with the TDTM method, the standard FDTD method is generalized to include the rate equation in the analysis of semi-conductors. Also in this work, optical manipulation of absorption in periodic structures is studied for the first time. Thanks to the large accessible nonlinearity that results from the absorption saturation and frequency selectivity of periodic structures, a sensitive and compact optical limiter is designed. The novel design and modeling work developed in this thesis has provided new insights and tools to the utilization of resonant nonlinearities in compact all-optical devices.The experimental studies are based on quasi-phase matched AlGaAs superlattice waveguides. These devices have been previously designed and used for classical optical wavelength conversion such as second harmonic generation and difference frequency generation. In this work, these devices are exploited for spontaneous down conversion, which is a quantum effect, for the first time, through this process, entangled photon pairs are generated. Unprecedented performance, in terms of brightness and purity, of III-V semiconductor-based entangled photon sources has been demonstrated here. Moreover, the quantum properties of these entangled photons are characterized. The experimental studies presented in this thesis open up new application areas for III-V nonlinear optical devices as quantum sources and convincingly demonstrate the promising role of such devices will play in future quantum technologies.
This thesis encompasses a broad area of physics including linear and nonlinear optics, photonics and quantum physics. It combines the phenomena of nonlinearoptical frequency conversion with waveguiding and coupling, taking advantage of new opportunities presented by advances in fabrication technologies of micro- and nano-waveguides. In this dissertation an in-depth analysis of quantum and classical properties of light traveling in nonlinear optical waveguides, directional couplers and waveguide arrays is performed. The concepts of spatial and temporal dispersion, waveguiding in structures with subwavelength dimensions and nonlinear interactions between different frequencies of light are studied both theoretically and experimentally. Some sections of this thesis include development and implementation of novel physical ideas, while other sections are focused on comprehensive experimental and numerical analysis of advanced theoretical concepts. The results presented in this dissertation demonstrate new physical phenomena with potential applications in the areas of telecommunications and quantum information. The research performed in this thesis opens opportunities for frequency conversion with world-leading power efficiency, including operation with ultrashort pulses for a variety of wavelengths to suit a wide range of perspective application requirements. It also shows an approach for simple and energy efficient spatio-temporal optical signal control, which can find applications in next generation telecommunications networks. Furthermore, the results obtained in this dissertation demonstrate the possibility for flexible shaping of quantum statistics of photons generated in photonic waveguiding structures through spontaneous frequency conversion, contributing to the development of integrated quantum circuits. The new methods of frequency conversion in micro- and nano-scale waveguides and optical circuits have potential to advance the performance, energy efficiency, and security of future optical communication networks and computing systems.
One of the main issues in the domain of quantum information and communication is the generation, manipulation and detection of several qubits on a single chip. Several approaches are currently investigated for the implementation of qubits on different types of physical supports and a variety of quantum information technologies are under development: for quantum memories, spectacular advances have been done on trapped atoms and ions, while to transmit information, photons are the ideal support thanks to their high speed of propagation and their almost immunity against decoherence. My thesis work has been focused on the conception, fabrication and characterization of a miniaturized semiconductor source of entangled photons, working at room temperature and telecom wavelengths. First the theoretical concepts relevant to understand the work are described (chapter 1). Then the conception and fabrication procedures are given (chapter 2). Chapter 3 presents the optoelectronics characterization of the device under electrical pumping, and chapter 4 the results on the optical losses measurements and the nonlinear optical characterization (second harmonic generation, spontaneous parametric down conversion and joint spectral intensity reconstruction). Chapters 5 and 6 focus on the characterization of the quantum state generated by a passive sample (demonstration of indistinguishability and energy-time entanglement) and its utilization in a multi- user quantum key distribution protocol (polarization entanglement). Finally the work on the first electrically driven photon pairs source emitting in the telecom range and working at room temperature is presented (chapter 7).
The aim of this thesis is to explore nonlinear nanostructures – photonic systems with one or more dimension with nanoscale feature size – as new platforms for parametric photon-pair generation. This is motivated by the need for photon-pair sources in many technological applications of quantum optics, such as quantum communication, imaging and computing. The initial hypothesis is that nonlinear nanostructures are a promising platform to complement established photon-pair source schemes based on bulk crystals or photonic integrated circuits in terms of quantum state-engineering, footprint, functional density etc. However, nonlinear pair generation, e.g. via spontaneous parametric down-conversion (SPDC), is a new subfield in nanophotonics with a very limited number of studies existing. This constitutes the knowledge-gap addressed in this thesis. Therefore, the objective is to provide first experimental demonstrations of SPDC in subwavelength-scale and nonlinear nanostructures. We investigate the ability of such systems to control the properties of two-photon quantum states such as frequency and angular spectrum or polarization entanglement. To this end we analyze nanostructures with different degrees of complexity, starting with an unstructured thin crystal with one nanoscale dimension, leading up to a 3D nano-scale resonator with subwavelength-sized features in all dimensions. Furthermore, we test different types of nonlinear materials such as lithium niobate, group III-V semiconductors and emerging, highly nonlinear materials such as molybdenum disulfide. Additionally, we also advance the theoretical understanding by developing a comprehensive model of the quantum process of nonlinear parametric pair-generation in photonic nanostructures.
Entanglement is the hallmark of quantum mechanics. Quantum entanglement -- putting two or more identical particles into a non-factorable state -- has been leveraged for applications ranging from quantum computation and encryption to high-precision metrology. Entanglement is a practical engineering resource and a tool for sidestepping certain limitations of classical measurement and communication. Engineered nonlinear optical waveguides are an enabling technology for generating entangled photon pairs and manipulating the state of single photons. This dissertation reports on: i) frequency conversion of single photons from the mid-infrared to 843nm as a tool for incorporating quantum memories in quantum networks, ii) the design, fabrication, and test of a prototype broadband source of polarization and frequency entangled photons; and iii) a roadmap for further investigations of this source, including applications in quantum interferometry and high-precision optical metrology. \n \nThe devices presented herein are quasi-phase-matched lithium niobate waveguides. Lithium niobate is a second-order nonlinear optical material and can mediate optical energy conversion to different wavelengths. This nonlinear effect is the basis of both quantum frequency conversion and entangled photon generation, and is enhanced by i) confining light in waveguides to increase conversion efficiency, and ii) quasi-phase matching, a technique for engineering the second-order nonlinear response by locally altering the direction of a material's polarization vector. Waveguides are formed by diffusing titanium into a lithium niobate wafer. Quasi-phase matching is achieved by electric field poling, with multiple stages of process development and optimization to fabricate the delicate structures necessary for broadband entangled photon generation. \n \nThe results presented herein update and optimize past fabrication techniques, demonstrate novel optical devices, and propose future avenues for device development. Quantum frequency conversion from 1848nm to 843nm is demonstrated for the first time, with >75% single-photon conversion efficiency. A new electric field poling methodology is presented, combining elements from multiple historical techniques with a new fast-feedback control system. This poling technique is used to fabricate the first chirped-and-apodized Type-II quasi-phase-matched structures in titanium-diffused lithium niobate waveguides, culminating in a measured phasematching spectrum that is predominantly Gaussian (R^2 = 0.80), nearly eight times broader than the unchirped spectrum, and agrees well with simulations.
There is a growing belief that we are currently in the midst of a Second Quantum Revolution. More and more quantum technologies, such as communication, computing, and imaging, are moving from academic exploration to practical industrial applications. These technologies often depend on entangled photons, and their increasing use requires the development of novel quantum light sources that are compact, versatile, and integrable into modern photonic systems. Additionally, the trend toward miniaturization and nano-optics is accelerating, driven by rapid advances in nanofabrication. Therefore, there is an urgent need to create new classes of miniaturized and tunable two-photon sources. This thesis is dedicated to the theoretical investigation and experimental demonstration of miniaturized sources of entangled photons based on spontaneous parametric down-conversion in thin nonlinear films. It focuses not only on traditional crystalline materials but also on the emerging platform of liquid crystals, marking the first-ever demonstration of photon-pair generation in a liquid crystal within this thesis. A significant achievement is the ability to relax phase-matching constraints in ultra-thin nonlinear layers, allowing the full utilization of the nonlinear tensor and enhancing the variety of possible entangled two-photon states. Several aspects of two-photon state engineering with relaxed phase-matching are discussed in the thesis. First, this relaxation facilitates the switching between different polarization two-photon states, with a varying degree of polarization entanglement and the ability to generate non-maximally entangled states. In terms of spectral properties, miniaturized two-photon sources generate exceptionally broad two-photon frequency spectra, leading to a high degree of frequency entanglement and an unprecedented number of frequency modes, which also leads to ultra-narrow time correlations. By considering the effects of Fabry-Perot resonances, it becomes possible to engineer the two-photon spectra and even achieve backward emission of photon pairs. Remarkably, the Fabry-Perot effect can be accurately described by a simple modification of the rigorous quantum theory, providing a powerful predictive tool for photon pair generation in advanced nanostructures, metasurfaces, and nonlinear nano-antennas when properly applied. Another central contribution of this work is the introduction of liquid crystals as tunable nonlinear media for photon pair generation. Controlling the molecular orientation through a static twist or applying an external electric field makes it possible to tune the generated two-photon states dynamically. A theoretical model of this process, verified through direct experimental measurements, predicts quasi-phase-matching-like behavior and enhanced conversion efficiency, which can be utilized to develop exceptionally tunable and integrable sources of photon pairs and squeezed light. Finally, a fundamental challenge addressed in this thesis is mitigating a parasitic photoluminescent background. This study demonstrates a two-order-of-magnitude reduction in photoluminescence-induced contamination of photon pairs generated from thin nonlinear films by switching from the commonly used continuous-wave regime to the pulsed regime and performing time-resolved distillation. It also shows a developed theory that relates measured experimental parameters to the intrinsic purity of the two-photon state. Overall, this thesis advances the quantum micro- and nano-photonics field by providing a deeper understanding and enhanced control over photon pair generation in thin nonlinear films. It bridges theoretical insights with experimental realizations and paves the way toward practical, tunable, and highly integrated quantum light sources.
I will discuss our recent results demonstrating exceptional nonlinear optical frequency conversion in transition metal dichalcogenides (TMDs). By fabricating nano-photonic elements such as waveguides, metasurfaces, and periodically poled stacks, we achieve macroscopic frequency conversion efficiencies over microscopic distances, 10 to 100× smaller than current systems with similar performances. Further, we report the broadband generation of entangled photon pairs at telecom wavelength via quasi-phase-matched spontaneous parametric down-conversion, showing the highest coincidence-to-accidental-ratio (CAR) ever demonstrated in a vdW material. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.