Sources of single and polarization-entangled photons are an essential component in a variety of potential quantum information applications. Suitable emitters need to generate photons deterministically and at fast repetition rates, with highest degrees of single-photon purity, entanglement and indistinguishability. Semiconductor quantum dots are among the leading candidates for this task, offering entangled-photon pair emission on-demand, challenging current state-of-the-art sources based on the probabilistic spontaneous parametric down-conversion (SPDC). Unfortunately, their susceptibility to perturbations from the solid-state environment significantly affects the photon coherence and entanglement degree. Furthermore, most quantum dot types suffer from poor wavelength control and emitter yield, due to a random growth process. This thesis investigates the emerging family of GaAs/AlGaAs quantum dots obtained by in-situ Al droplet etching and nanohole infilling. Particular focus is laid on the interplay of growth parameters, quantum dot morphology and optical properties. An unprecedented emission wavelength control with distributions as narrow as ± 1 nm is achieved, using four independent growth parameters: The GaAs infilling amount, the deposition sequence, the migration time and the Al concentration in the barrier material. This enables the generation of large emitter ensembles tailored to match the optical transitions of rubidium, a leading quantum memory candidate. The photon coherence is enhanced by an optimized As flux during the growth process using the GaAs surface reconstruction. With these improvements, we demonstrate for the first time two-photon interference from separate, frequency-stabilized quantum dots using a rubidium-based Faraday filter as frequency reference. Two-photon resonant excitation of the biexciton state is employed for the coherent and deterministic generation of photon pairs with negligible multi-photon emission probability. The GaAs/AlGaAs quantum dots exhibit a very small average fine structure of (4.8 ±2.4) µeV and short average radiative lifetimes of 200 ps, enabling entanglement fidelities up to F = 0.94, which are among the highest reported for any entangled-photon source to date. Furthermore, almost all fabricated emitters on a single wafer exhibit fidelities beyond the classical limit - without any post-growth tuning. By embedding the quantum dots into a broadband-optical antenna we enhance the photon collection efficiency significantly without impairing the high degrees of entanglement. Thus, for the first time, quantum dots are able to compete with SPDC sources, paving the way towards the realization of a semiconductor-based quantum repeater - among many other key enabling quantum photonic elements.:Contents List of Figures ix List of Tables xiii 1 Introduction 1 1.1 Researchmotivation ...................1 1.1.1 Structure of this thesis ................. 3 1.2 Applications based on entangled photons ............. 4 1.2.1 Quantum bits ...................4 1.2.2 Quantum key distribution ................ 5 1.2.3 Qubit teleportation .................. 7 1.2.4 Teleportation of entanglement ..............9 1.2.5 The photonic quantumrepeater .............. 10 1.3 Generation of entangled photons ...............12 1.3.1 The ideal entangled-photon source ............. 12 1.3.2 Non-deterministic photon sources ............. 13 1.3.3 Deterministic photon sources ..............14 2 Fundamentals 17 2.1 Semiconductor quantumdots ................17 2.1.1 Introduction to semiconductor quantum dots .......... 17 2.1.2 Formation of confined excitonic states ............ 19 2.1.3 Energy hierarchy of excitonic states ............. 21 2.2 Entangled photons from semiconductor quantumdots ......... 22 2.2.1 The concept of entanglement ............... 22 2.2.2 Polarization-entangled photon pairs fromthe biexciton radiative decay .. 23 2.2.3 Origin and impact of the exciton fine structure splitting ....... 25 2.2.4 Impact of spin-scattering, dephasing and background photons on the degree of entanglement ..................29 2.3 Quantum dot entangled-photon sources - State of the art ........32 2.4 Exciton radiative lifetime .................. 34 2.4.1 The concept of radiative lifetime .............. 34 2.4.2 Measurement of the radiative lifetime ............35 2.5 Single-photon purity ...................37 2.5.1 Photon number distributions ............... 37 2.5.2 Second-order correlation function .............38 2.5.3 Measurement of the second-order correlation function ....... 40 2.6 Measurement of entanglement ................42 2.6.1 Quantum state tomography ...............43 2.7 Photon coherence and spectral linewidth .............46 2.7.1 The concept of coherence ................ 46 2.7.2 First-order coherence ................. 46 2.7.3 Relation between coherence and spectral linewidth ........ 49 2.7.4 homogeneous vs. inhomogeneous broadening in single quantumdots ..50 2.8 Photon indistinguishability .................51 2.8.1 Hong-Ou-Mandel interference ..............51 2.8.2 Hong-Ou-Mandel interference between photons fromseparate sources .. 52 2.8.3 The Bell state measurement with linear optics .......... 53 3 Experimentalmethods 55 3.1 The GaAs and AlAs material system ............... 55 3.2 Molecular beam epitaxy ..................56 3.2.1 The Concept of molecular beam epitaxy ...........56 3.2.2 Layout and components of the III-V Omicron MBE ........58 3.2.3 Growth parameters .................. 59 3.2.4 Reflection high-energy electron diffraction (RHEED) ........ 60 3.2.5 Growth rate determination using RHEED oscillations .......61 3.3 Optical setups .....................63 4 Results 67 4.1 Growth of GaAs/AlGaAs quantum dots by in-situ Al droplet etching .....68 4.1.1 Motivation for the study of GaAs / AlGaAs quantum dots ......68 4.1.2 GaAs / AlGaAs quantum dot growth process ..........69 4.1.3 Interplay between growth parameters, quantumdot morphology and optical properties ................. 71 4.1.4 Nanohole morphology and quantumdot formation ........ 73 4.1.5 Optical characterization ................75 4.1.6 Deterministic wavelength control .............77 4.1.7 Photon coherence and radiative lifetime ...........84 4.1.8 Decoherence processes in semiconductor quantum dots ......86 4.1.9 Chamber conditioning and growth process optimization ......87 4.1.10 Arsenic flux calibration using the GaAs surface reconstruction ..... 88 4.1.11 Enhanced photon coherence after growth process adjustments ....92 4.2 Two-photon interference from frequency-stabilized GaAs/AlGaAs quantum dots .................94 4.2.1 Frequency tuning of semiconductor quantumdots ........95 4.2.2 Experimental setup .................. 95 4.2.3 Optical characterization of the separate GaAs/AlGaAs quantum dots ... 98 4.2.4 Faraday anomalous dispersion optical filter and frequency feedback ... 99 4.2.5 Two-photon interference between remote, frequency-stabilized quantum dots 100 4.3 Solid-state ensemble of highly entangled photon sources at rubidiumatomic transitions ........................102 4.3.1 Fine-structure splitting ................103 4.3.2 Resonant excitation of the biexciton state ...........105 4.3.3 Single photon purity and radiative lifetime ........... 107 4.3.4 Radiative lifetime of GaAs/AlGaAs quantumdots - comparison to other quantumdot types ...................108 4.3.5 Degree of entanglement ................109 4.3.6 Highly-efficient extraction of the obtained entangled photons ..... 116 5 Conclusions 119 5.1 Summary ....................... 119 5.2 Discussion and outlook ..................122 Bibliography 127 Publications and scientific presentations 150 Acknowledgments 154 Selbstständigkeitserklärung 157 Curriculum vitae 157

Mit dem Begriff Wellenleiterquantenelektrodynamik (WQED) wird gemeinhin die Physik des quantisierten und in eindimensionalen Wellenleitern geführten Lichtes in Wechselwirkung mit einzelnen Emittern bezeichnet. In dieser Arbeit untersuche ich Effekte der WQED für einzelne Dreiniveausysteme (3NS) bzw. Paare von Zweiniveausystemen (2NS), die in den Wellenleiter eingebettet sind. Hierzu bediene ich mich hauptsächlich numerischer Methoden und betrachte die Modellsysteme im Rahmen der Drehwellennäherung. Ich untersuche die Dynamik der Streuung einzelner Photonen an einzelnen, in den Wellenleiter eingebetteten 3NS. Dabei analysiere ich den Einfluss dunkler bzw. nahezu dunkler Zustände der 3NS auf die Streuung und zeige, wie sich mit Hilfe stationärer elektrischer Treibfelder gezielt auf die Streuung einwirken lässt. Ich quantifiziere Verschränkung zwischen dem Lichtfeld im Wellenleiter und den Emittern mit Hilfe der Schmidt-Zerlegung und untersuche den Einfluss der Form der Einhüllenden eines Einzelphotonpulses auf die Ausbeute der Verschränkungserzeugung bei der Streuung des Photons an einem einzelnen Lambda-System im Wellenleiter. Hier zeigt sich, dass die Breite der Einhüllenden im k-Raum und die Emissionszeiten der beiden Übergänge des 3NS die maßgeblichen Parameter darstellen. Abschließend ergründe ich die Emissionsdynamik zweier im Abstand L in den Wellenleiter eingebetteter 2NS. Diese Dynamik wird insbesondere durch kavitätsartige und polaritonische Zustände des Systems aus Wellenleiter und Emitter ausschlaggebend beeinflusst. Bei der kollektiven Emission der 2NS treten - abhängig vom Abstand L - Sub- bzw. Superradianz auf. Dabei nimmt die Intensität dieser Effekte mit längerem Abstand L zu. Diese Eigenart lässt sich auf die Eindimensionalität des Wellenleiters zurückführen. / The field of waveguide quantum electrodynamics (WQED) deals with the physics of quantised light in one-dimensional (1D) waveguides coupled to single emitters. In this thesis, I investigate WQED effects for single three-level systems (3LS) and pairs of two-level systems (2LS), respectively, which are embedded in the waveguide. To this end, I utilise numerical techniques and consider all model systems within the rotating wave approximation. I investigate the dynamics of single-photon scattering by single, embedded 3LS. In doing so, I analyse the influence of dark and almost-dark states of the 3LS on the scattering dynamics. I also show, how stationary electrical driving fields can control the outcome of the scattering. I quantify entanglement between the waveguide''s light field and single emitters by utilising the Schmidt decomposition. I apply this formalism to a lambda-system embedded in a 1D waveguide and study the generation of entanglement by scattering single-photon pulses with different envelopes on the emitter. I show that this entanglement generation is mainly determined by the photon''s width in k-space and the 3LS''s emission times. Finally, I explore the emission dynamics of a pair of 2LS embedded by a distance L into the waveguide. These dynamics are primarily governed by bound states in the continuum and by polaritonic atom-photon bound-states. For collective emission processes of the two 2LS, sub- and superradiance appear and depend strongly on the 2LS''s distance: the effects increase for larger L. This is an exclusive property of the 1D nature of the waveguide.

Quasi-particles formed in lithium niobate after pulse exposure were investigated by transient absorption and photoluminescence spectroscopy as well as numerical simulations. This includes the formation process, the transport through the crystal, interim pinning on defects during the relaxation process, and the final recombination with deep centers. It was shown that the charge-transport through the crystal can be described by a hopping transport including different types of hops between regular or defective lattice sites, i.e., the transport includes a mixture of free and bound small polarons. Furthermore, the different types of hops connected with varying activation energies and their distribution are responsible for an altered temporal decay curve when changing the crystal composition or temperature. Additionally, it was shown that the hitherto accepted recombination model is insufficient to describe all transient absorption and luminescence effects in lithium niobate under certain experimental conditions, i.e., long-living absorption dynamics in the blue/UV spectral range do not follow the typical polaron dynamics and cannot be described under the assumption of charge compensation. However, similar decay characteristics between self-trapped excitons known from photoluminescence spectroscopy and the unexpected behavior of the transient absorption were found leading to a revised model. This includes, besides the known polaron relaxation and recombination branch, a significant role of self-trapped excitons and their pinning on defects (pinned STEs). Since the consideration of further absorption centers in the relaxation path after pulse exposure might result in misinterpretations of previously determined polaron absorption cross-sections and shapes, the necessity to perform a review became apparent. Therefore, a supercontinuum pump-probe experiment was designed and all measurements applied under the same experimental conditions (temperature, polarization) so that one can extract the absorption amplitudes of the single quasi-particles in a spectral range of 0.7-3.0eV. The detailed knowledge might be used to deconvolve the absorption spectra and transform them to number densities of the involved centers which enables one to obtain an easier insight into recombination and decay dynamics of small polarons and self-trapped excitons. As the hopping transport of quasi-particles and the concept of pinned STEs might be fundamental processes, a thorough understanding opens up the possibility of their exploitation in various materials. In particular, results presented herein are not only limited to lithium niobate and its applications; an extension to a wide range of further strongly polar crystals in both their microscopic processes and their use in industry can be considered.

This work is dedicated to a comprehensive experimental study on the interaction of femtosecond laser pulses with the nonlinear optical medium lithium niobate. The nonlinear optical response in the nanosecond regime was already studied extensively with a variety of techniques, whereas femtosecond pulses were mainly used in transient absorption or transient grating experiments. Naturally, the temporal resolution of these measurements depends on the pulse duration, however, dynamics during the pulse excitation were barely investigated. The motivation of this work is to widen the limits of femtosecond spectroscopy, not only to temporally resolve faster nonlinear optical processes, but further to show a sensitivity to other coupling mechanisms between the pulses and the material. Especially, the role of transient, dynamic holographic gratings is investigated with a careful determination of the pulse duration, bandwidth and frequency chirp. A basis of this work is established in the first part by studying the material response via light-induced absorption before focusing on the main topic, the pulse interaction with elementary (holographic) gratings, both self-induced and static, in the second part. By this detailed study, several features of femtosecond laser pulses, holographic gratings and the ultrafast material response can be revealed: (i) grating recording is feasible even with pulses of different frequencies, provided that their pulse duration is sufficiently short, (ii) grating based pulse coupling causes a pronounced energy transfer even in a common pump-probe setup for transient absorption measurements with (non-)degenerated frequencies, (iii) beyond expectation, oscillations in the phonon frequency range become apparent in different measurements. The presented results point towards appropriate future experiments to obtain a more consistent, microscopic model for the ultrafast response of the crystal, involving the interplay between photo-generated polarons, self-induced gratings, and phonons.

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.

No description available.

The present work broaches the physics of light-matter interaction, chiefly using nonlinear optical spectroscopy in a newly developed framework termed as Photon Management Concept. This way, existing fragments dealing with specific properties of harmonic and upconversion nanoparticles (HNPs/UCNPs) are consolidated into a full and coherent picture with the primary goal of understanding the underlying physical processes and their impact on the application side, especially in terms of imaging techniques, via suitable experimental and numerical studies. Contemporary optical setups involving contrast-enhancing agents are frequently limited in their excitation and detection configurations owing to a specialization to a select number of markers. As a result, the bandwidth of experimental methods and specimens that may be investigated is severely restricted in a large number of state-of-the-art setups. Here, an alternative approach involving HNPs and UCNPs, respectively, is presented providing an overview from their synthesis to optical characterization and to potential fields of application. Based on their inherent flexibility based on their nonlinear optical response, especially in terms of wavelength and intensity tunability, the PMC alleviates prevalent limitations by dynamically adapting the setup to a sample instead of the preliminary culling to a reduced number of eligible specimens that must not change their optical properties significantly during investigation. The use of HNPs supersedes such concerns due to their nearly instantaneously generated, strongly anti-Stokes shifted, coherent emission capable of producing radiation throughout the visible spectral range, including infrared and ultraviolet wavelengths. This way, HNPs transcend the traditional field of imaging and introduces potential applications in optomanipulation or holographic techniques. Thorough (nonlinear) optical characterization of UCNPs and alkali niobate HNP ensembles is performed to assess the fundamental physical mechanisms interwoven with numerical studies leading to their wide-ranging applicability. Final remarks show that HNPs are ideal candidates for realization of the PMC and yet hold an even further potential beyond current prospects.

In der vorliegenden Arbeit werden die nichtlinearen optischen Eigenschaften der Materialien Lithiumniobat und Di-Zinn-Hexathiohypodiphosphat aufgrund der Suszeptibilität 3. Ordnung und kleiner Polaronen untersucht. Zudem wird gezeigt, dass die Interferenz verschiedenfarbiger Laserpulse die Aufzeichnung von statischen und dynamischen holographischen Gittern ermöglicht. Ein Teil dieser Arbeit ist in den im Anhang angegebenen 6 Publikationen bereits veröffentlicht. Lithiumniobat wird mit einer Erweiterung des Z-Scan Experiments untersucht, welches die Pulslängenabhängige Messung der nichtlinearen Absorption und der nichtlinearen Brechungsindexänderung ermöglicht. Dabei konnte festgestellt werden, dass bei sehr kurzen Pulslängen von 70 fs ein Effekt der Polaronen auf die nichtlineare Absorption vernachlässigbar ist und die Zwei-Photonen-Absorption die nichtlineare Absorption dominiert. Mit größerer Pulslänge gibt es allerdings Abweichungen zwischen der Theorie der Zwei-Photonen-Absorption und den Messergebnissen. Mit der Entwicklung eines Polaronen-Anregungs-Modells, welches eine polaronische Absorption aufgrund wiederholtem optisch induziertem Hopping annimmt, konnte dieser Effekt konsistent erklärt werden. Die Messungen der nichtlinearen Brechungsindexänderung lassen darauf schließen, dass sowohl freie Ladungsträger als auch kleine Polaronen neben der Suszeptibilität 3. Ordnung einen Einfluss auf die Brechungsindexänderung haben, da eine nichtlineare Abhängigkeit von der Intensität auch bei Pulslängen von 70 fs festgestellt werden konnte. Analog dazu konnte in Di-Zinn-Hexathiohypodiphosphat ein großer Zwei-Photonen-Absorptionskoeffizient festgestellt werden, welcher für Photonenenergien nahe der Bandkante Werte zeigt, die größer sind als theoretischen Überlegungen zeigen. Eine transiente Absorption nach optischer Anregung, gemessen durch ein Anreg-Abtast-Experiment, sowie Literatur legen nahe, dass in Di-Zinn-Hexathiohypodiphosphat gebundene Lochpolaronen durch optische Anregung entstehen können. Durch den hohen Zwei-Photonen-Absorptionskoeffizienten konnte das Aufzeichnen eines kontrastreichen, dynamischen Amplitudengitters mittels Femtosekundenpulsen gezeigt und nachgewiesen werden. Die Kürze der Femtosekundenpulse ermöglicht aber nicht nur das Aufzeichnen eines Zwei-Photonen-Absorptionsgitters aufgrund der hohen Intensitäten, sondern erlaubt zudem die Beobachtung von Interferenz zwischen verschiedenfarbigen Pulsen. In der Zeitspanne der Pulslänge beträgt die Bewegung der Interferenzstreifen, welche in der Größenordnung der Lichtgeschwindigkeit liegt, nur ein Bruchteil der Streifendistanz, sodass das Interferenzmuster eingefroren und beobachtbar erscheint. Somit lassen sich statische Hologramme in holographischen Filmen, wie auch dynamische Hologramme aufzeichnen. Über ein dynamisches holographisches Gitter mittels Zwei-Photonen-Absorption konnte so eine Frequenzkonversion durch Dopplerverschiebung in Lithiumniobat gezeigt werden.