High quality entangled photon sources are a key requirement for many promising quantum optical technologies. However, the production of multi-photon entangled states with good fidelity is challenging. Current sources of multi-photon entanglement require the use of post-selection, which limits their usefulness for some applications. It has been an open challenge to create a source capable of directly producing three-photon entanglement. An important step in this direction was achieved with the demonstration of photon triplets produced by a new process called cascaded downconversion, but these previous measurements were not sufficient to show whether these photons were in an entangled state and only had detection rates of five triplets per hour. In this thesis, we show the first demonstration of a direct source of three-photon entanglement. Our source is based on cascaded downconversion, and we verify that it produces genuine tripartite entanglement in two degrees of freedom: energy-time and polarization. The energy-time entanglement is similar to a three-particle generalization of an Einstein-Podolski-Rosen state; the three photons are created simultaneously, yet the sum of their energies is well defined, which is an indication of energy-time entanglement. To prove it, we use time-bandwidth inequalities which check for genuine tripartite entanglement. Our measurements show that the state violates the inequalities with what constitute, to the best of our knowledge, the strongest violation of time-bandwidth inequalities in a tripartite continuous-variable system to date. We create polarization entanglement by modifying our experimental setup so that two downconversion processes producing orthogonally polarized triplets interfere to create Greenberger-Horne-Zeilinger states. By using highly efficient superconducting nanowire single photon detectors, we improve the detected triplet rate by 2 orders of magnitude to 660 triplets per hour. We characterize the state using quantum state tomography, and find a fidelity of 86\% with the ideal state, beating the previous best value for a three-photon entangled state fidelity measured by tomography. We also use the state to perform two tests of local realism. We violate the Mermin and Svetlichny inequalities by 10 and 5 standard deviations respectively, the latter being the strongest violation to date. Finally, we show that, unlike previous sources of tree-photon entanglement, our source can be used as a source of heralded Bell pairs. We demonstrate this by measuring a CHSH inequality with the heralded Bell pairs, and by reconstructing their state using quantum state tomography.

Realization of linear quantum computation and establishing secure quantum communication among interacting parties demand for triggered quantum sources delivering genuine single and entangled photons. However, the intrinsic energy level spectrum of nanostructures made by the nature or developed under a random growth process energetically lacks the expected figures of merit to produce such quantized states of photons. Here, I present the semi-empirical modeling and experimental investigation on the spin fine structure of strongly confining quantum dots embedded in III-V nanowires. To this end, the quantum dot is numerically modeled via the Configuration Interaction method at two different levels: 1) single-particle level, where its pure energy level structure is resolved in the presence of strain and spin-orbit interaction. 2) Few-particle level, at which the few-body interactions appear as perturbative energy corrections and orbital correlations. I demonstrate the influence of quantum confinement on the binding energies and spin fine structure of excitons in the absence of hyperfine interaction. Importantly, the high-symmetry character of excitonic orbitals in nanowire quantum dots restore the degeneracy of optically-active ground-state excitons, offering an ideal spectrum for the entangled photon pair generation. To experimentally verify the idea, we design and fabricate defect-free nanowire quantum dots with ultra-clean excitonic spectrum, and construct the time correlation function of emitted photons through performing a series of low-temperature statistical quantum optics measurements. We observe a decent performance in terms of single photon generation under low excitation powers. Moreover, photon pairs emitted from the biexciton-exciton cascade of nanowire quantum dots exhibit color indistinguishability and polarization entanglement owing to the trivial fine structure splitting of the ground-state excitons. We further extend the idea by proposing the hybridized states of a nanowire-based quantum dot molecule as the potential source of higher-order entangled states. Tracing the field-dependent spectrum suggests the appearance of dominant features under the weak localization of electrons and coherent tunneling of holes. In addition to their Coulomb correlation, excitons also remain spatially correlated, opening new transition channels normally forbidden in the ground state of a single dot. The proposed structure can be exploited to create tripartite hybrid, GHZ and W-entangled states.

<p dir="ltr">Some of the simplest molecules that are found in abundance in nature, like oxygen, nitrogen, carbon dioxide and water can be playgrounds for complex quantum mechanical phenomenon. Although we can calculate their static properties, like binding energies, equilibrium geometries and ionization/decay rates with extraordinary precision, their dynamics offer new avenues for exploration. Although analytical techniques have been successfully applied in studying single-particle and many-particle systems, few-particle systems like simple molecules are still best understood through a combination of numerical calculations and experimental work. However, the small size of these molecules endows them with dynamics that occur on timescales of a few picoseconds to a few attoseconds, making their experimental study challenging. The overarching goal of this work is the study of such ‘ultrafast’ dynamics in excited state molecules/atoms, by developing and demonstrating novel optical probes of quantum dynamics.</p><p dir="ltr">One way to probe ultrafast dynamics in molecules is by measuring their nonlinear optical response. Such a measurement can potentially track the evolution of the symmetries of excited molecules, shedding light on their transient dynamics. We start chapter 1 with a brief discussion of the formalism behind nonlinear optical spectroscopy. Direct measurement of ultrafast (and ultraweak) optical pulses is discussed as a useful probe of nonlinear processes. After presenting preliminary results on direct electric field reconstruction, experimental work on measuring emitted nonlinear electric fields from impulsively aligned molecules is discussed. In such an experiment, however, contributions from both aligned and unaligned molecules are present, and new experimental capabilities had to be developed to disentangle and measure the ultraweak signal from aligned molecules. Following a detailed discussion of the developed measurement capabilities, results from experiments done on aligned carbon dioxide and nitrogen molecules are discussed.</p><p dir="ltr">Unlike solids, where electronic states can be excited with visible/UV light, binding energies in isolated atoms/molecules are on the order of electron-volts (eVs), and they need vacuum-ultraviolet (VUV) extreme-ultraviolet (EUV) light to excite electronically. Polyatomic molecules, like ethylene, when excited to an electronic state with VUV light, often relax back to the ground state by redistributing energy to their internal degrees of freedom non-adiabatically. These relaxation pathways are important in many chemical and biological systems, and control the yield of chemical reactions ranging from elementary reactions involving few atoms to large biomolecules such as DNA and proteins. For instance, in the photochemical reaction of the protein Rhodopsin, considered to be the primary event in human vision. In chapter 2 we discuss progress made towards extending nonlinear response measurements to study ultrafast dynamics in electronically excited molecules, using a high-harmonic VUV source. Details about the design of the high-harmonic generation beamline, and preliminary experimental data are presented. In chapter 3 we discuss preliminary theoretical work on the development of an EUV entangled-photon source, using two-photon emission from the metastable 2s state in neutral Helium. Such a source, if demonstrated, can possibly even extended to the zeptosecond regime in the future.</p>

We experimentally demonstrate time-frequency entangled photons with comb-like spectra via both bulk optical crystals and on-chip microring resonators and explore their characterization in both time and frequency domain using quantum state manipulation techniques. Our characterization of these quantum frequency combs involves the use of unbalanced Mach-Zehnder interferometers and electro-optic modulators for manipulation in time- and frequency-domain, respectively. By creating indistinguishable superposition states using these techniques, we are able to interfere states from various time- and frequency-bins, consequently proving time- and frequency-bin en-tanglement. Furthermore, our time-domain manipulations reveal pair-wise continuous time-energy entanglement that spans multiple frequency bins, while our utilization of electro-optic modulators to verify high-dimensional frequency-bin entanglement constitutes the proof of this phenomenon for a spontaneous four-wave mixing pro-cess. By doing so, we show the potential of these quantum frequency combs for high-dimensional quantum computing with frequency-encoded quantum states, as well as fully secure quantum communications via quantum key distribution by per-forming a nonlocal dispersion cancellation experiment. To show the potential of our entangled photons source for encoding quantum information in the frequency domain, we carry out a frequency-domain Hong-Ou-Mandel interference experiment by implementing a frequency beam splitter. Lastly, we use the high-dimensionality of our time-frequency entangled source in both time and frequency domain to implement deterministic high-dimensional controlled quantum gates, with the quantum information encoded in both the time and frequency degrees of freedom of a single photon. This novel demonstration of deterministic high-dimensional quantum gates paves the way for scalable optical quantum computation, as quantum circuits can be implemented with fewer resources and high success probability using this scheme.<div><br></div><div> </div>

Die verlässliche Erzeugung einzelner Photonen mit wohldefinierten Eigenschaften in allen Freiheitsgraden ist entscheidend für die Entwicklung photonischer Quantentechnologien. Derzeit basieren die wichtigsten Einzelphotonenquellen auf dem Prozess der spontanen parameterischen Fluoreszenz (SPF), bei dem ein Pumpphoton in einem nichtlinearen Medium spontan in ein Paar aus Signal und Idlerphotonen zerfällt. Resonator-überhöhte SPF, also das Plazieren des nichtlinearen Mediums in einem optischen Resonator, ist ein weit verbreitetes Verfahren, um Einzelphotonenquellen mit erhöhter Helligkeit und angepassten spektralen Eigenschaften zu konstruieren. Das Anpassen der spektralen Eigenschaften durch gezielte Auswahl der Resonatoreigenschaften ist besonders für hybride Quantentechnologienvon Bedeutung, welche darauf abzielen, unterschiedliche Quntensysteme so zu kombinieren, dass sich deren Vorteile ergänzen. Diese Arbeit stellt eine umfassende theoretische und experimentelle Analyse der dreifach resonanten SPF vor. Das aus der Literatur bekannte theoretische Modell wird diesbezüglich verbessert, dass der Einfluss sämtlicher Eigenschaften des Resonators auf die wichtigen experimentellen Größen (z.B. die Erzeugungsrate) gezielt ausgewertet werden kann. Dieses verbesserte und hoch genaue Modell stellt eine wichtige Grundlage für die Entwicklung und Optimierung neuartiger Photonenpaarquellen dar. Im experimentellen Teil dieser Arbeit wird der Aufbau und die Charakterisierung einer dreifach resonanten Photonenpaarquellen präsentiert. Die neu entwickelte digitale Regelelektronik sowie ein hochstabiler, schmalbandiger Monochromator welcher auf monolitischen, polarisationsunabhängigen Fabry-Pérot Resonatoren basiert, werden vorgestellt. Indem diese temperaturstabilisierten Resonatoren als Spetrumanalysator verwendet werden, wird zum ersten Mal die Frequenzkammstruktur des Spektrums der erzeugten Signal- und Idlerphotonen nachgewiesen. Des Weiteren wird der Einfluss der Pumpresonanz auf die Korrelationsfunktion und die Zweiphotoneninterferenz von Signal- und Idlerphotonen simuliert und vermessen. Abschließend werden Experimente aus dem Bereich der hybriden Quantennetzwerke präsentiert, in welchen Quantenfrequenzkonversion verwendet wird um die erzeugten Signalphotonen in das Telekommunikationsband zu transferieren. Dabei wird nachgewiesen, dass das temporale Wellenpaket durch die Konversion nicht beeinflusst wird und aufgezeigt, wie Quantennetzwerke von kommerziellen Telekommunikationstechnologien profitieren können. / The consistent generation of single photons with well-defined properties in all degrees of freedom is crucial for the development of photonic quantum technologies. Today, the most prominent sources of single photons are based on the process of spontaneous parametric down-conversion (SPDC) where a pump photon spontaneously decays into a pair of signal and idler photons inside a nonlinear medium. Cavity-enhanced SPDC, i.e., placing the nonlinear medium inside an optical cavity, is widely used to build photon-pair sources with increased brightness and tailored spectral properties. This spectral tailoring by selective adjustment of the cavity parameters is of particular importance for hybrid quantum technologies which seek to combine dissimilar quantum systems in a way that their advantages complement each other. This thesis provides a comprehensive theoretical and experimental analysis of triply-resonant cavity-enhanced SPDC. We improve the theoretical model found in the literature such that the influence of all resonator properties on the important experimental parameters (e.g., the generation rate) can be analyzed in detail. This convenient and highly accurate model of cavity-enhanced SPDC represents an important basis for the design and optimization of novel photonpair sources. The experimental part of this thesis presents the setup and characterization of a triply-resonant photon-pair source. We describe the digital control system used to operate this source over days without manual intervention, and we present a highly stable, narrow-linewidth monochromator based on cascaded, polarization-independent monolithic Fabry-Pérot cavities. Utilizing these temperature-stabilized cavities as a spectrum analyzer, we verify, for the first time, the frequency comb spectral structure of photons generated by cavity-enhanced SPDC. We further simulate and measure the impact of the pump resonance on the temporal wave-packets and the two-photon interference of signal and idler photons. Finally, we present a series of experiments in the context of hybrid quantum networks where we employ quantum frequency conversion (QFC) to transfer the generated signal photons into the telecommunication band. We verify the preservation of the temporal wave-packet upon QFC and highlight how quantum networks can benefit from advanced commercial telecommunication technologies.