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. The 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. The 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.

We develop a robust and realistic mechanism for the generation of indistinguishable single-photon (SP) pulses with identical frequency and polarization. They are produced on demand from a coupled double-Raman atom-cavity system driven by a sequence of laser pump pulses. This scheme features a high efficiency, the ability to produce a sequence of narrow-band SP pulses with a delay determined only by the pump repetition rate, and simplicity of the system free from complications such as repumping process and environmental dephasing. We propose and analyze a simple scheme of parametric frequency conversion for optical quantum information in cold atomic ensembles. Its remarkable properties are minimal losses and distortion of the pulse shape, and the persistence of quantum coherence and entanglement. Efficient conversion of frequency between different spectral regions is shown. A method for the generation of frequency-entangled single photon states is discussed. We suggest a robust and simple mechanism for the coherent excitation of molecules or atoms to a superposition of pre-selected states by a train of femtosecond laser pulses, combined with narrow-band coupling field. The theory of quantum beatings in the generation of ultra-violet radiation via a four wave mixing in pump-probe experiments is developed. The results are in good agreement with experimental data observed in Rb vapor when the laser phase fluctuations are significant.

Nous développons un mécanisme robuste et réaliste pour la génération de photons uniques indiscernables avec des impulsions de fréquence et de polarisation identiques. Ils sont produits à la demande à partir d'un système couplé atome- cavité double-Raman en interaction avec une séquence d'impulsions laser de pompe. Ce processus combine un rendement élevé, la capacité de produire une séquence d'impulsions de photons uniques à bande étroite avec un retard déterminé seulement par le taux de répétition de la pompe, avec la simplicité du système libre de complications comme le repompage et le déphasage de l'environnement.Nous proposons et analysons un schéma simple de conversion paramétrique de fréquence pour l'information quantique optique dans des ensembles atomiques froids. Ses propriétés remarquables sont des pertes réduites, une distorsion de la forme des impulsions minimale, ainsi que la persistance de la cohérence quantique et de l’intrication. Une conversion efficace de fréquence entre les différentes régions spectrales est montrée. Une méthode de génération d’états caractérisant des photons uniques intriqués en fréquence est discutée.Nous proposons un mécanisme robuste et simple d'excitation cohérente de molécules et d’atomes en une superposition d'états pré-sélectionnés par un train d'impulsions laser femtoseconde, combinée avec un champ de couplage à largeur de bande étroite.La théorie des battements quantiques pour la génération du rayonnement ultra-violet par mélange à quatre ondes dans des expériences pompe-sonde est développée. Les résultats sont en bon accord avec les données expérimentales observées dans la vapeur de Rb lorsque les fluctuations de phase laser sont importantes. / We develop a robust and realistic mechanism for the generation of indistinguishable single-photon (SP) pulses with identical frequency and polarization. They are produced on demand from a coupled double-Raman atom-cavity system driven by a sequence of laser pump pulses. This scheme features a high efficiency, the ability to produce a sequence of narrow-band SP pulses with a delay determined only by the pump repetition rate, and simplicity of the system free from complications such as repumping process and environmental dephasing. We propose and analyze a simple scheme of parametric frequency conversion for optical quantum information in cold atomic ensembles. Its remarkable properties are minimal losses and distortion of the pulse shape, and the persistence of quantum coherence and entanglement. Efficient conversion of frequency between different spectral regions is shown. A method for the generation of frequency-entangled single photon states is discussed. We suggest a robust and simple mechanism for the coherent excitation of molecules or atoms to a superposition of pre-selected states by a train of femtosecond laser pulses, combined with narrow-band coupling field. The theory of quantum beatings in the generation of ultra-violet radiation via a four wave mixing in pump-probe experiments is developed. The results are in good agreement with experimental data observed in Rb vapor when the laser phase fluctuations are significant.