Die hier vorgelegte Dissertation beschäftigt sich mit Untersuchungen an nanoskopischen Emittern und den Möglichkeiten, deren Fluoreszenzverhalten durch kontrollierte Ankopplung an photonische und plasmonische Strukturen zu beeinflussen. Zum einen werden mit Ytterbium- und Erbium-Ionen kodotierte NaYF4 -Nanokristalle untersucht, die hervorragende Eigenschaften bei der Umwandlung von niederenergetischen Photonen in solche höherer Energie besitzen. Das so entstehende Fluoreszenzlicht einer Ansammlung von Nanokristallen wird auf seine Abhängigkeit von der Anregungsintensität untersucht. Mit der Hilfe eines Rasterkraftmikroskops (AFM) wird eine Abhängigkeit der spektralen Zusammensetzung des Fluoreszenzlichts einzelner Nanokristalle von deren Größe im Bereich von wenigen bis 50 nm aufgezeigt. Durch gezielte Manipulation mit dem AFM werden ebenfalls einzelne Nanokristalle an Goldnanokügelchen gekoppelt und die Mechanismen der beobachteten plasmonischen Verstärkung der Emission durch zeitaufgelöste Messungen analysiert. Einzelne Stickstoff-Fehlstellen-Zentren in Nanodiamanten werden in einem zweiten Themenkomplex als Einzelphotonenquellen eigesetzt. Diese werden durch den Einsatz einer Nahfeld-Sonde auf Mikrokugel-Resonatoren aufgebracht, wodurch die Emission aufgrund der Ankopplung an die Flüstergalerie-Moden der Kugeln die typischen, scharfen Überhöhungen im Spektrum aufweist. Diese Methode lässt sich nicht nur verwenden, um zwei oder mehr Emitter an die selben Resonanzen einer Kugel zu koppeln. Es ist auch möglich, die Kugeln in einem Vorbereitungsschritt zu charakterisieren, und so kann insbesondere eine spektrale Übereinstimmung zwischen einer der Resonanzen und dem Emitter erreicht werden. Desweiterne wird demonstriert, wie durch die Kopplung an eine plasmonische Antenne aus Goldnanokugeln mittels AFM auch die Effizienz der Einzelphotonenquelle gesteigert werden kann. / The topic of the dissertation presented here is the investigation of nanoscopic emitters and the possibilities to influence their fluorescence behavior by controlled coupling to photonic and plasmonic structures. NaYF4 nanocrystals codoped with ytterbium and erbium are investigated since they provide excellent properties in upconverting of low-energetic photons to photons with higher energy. The fluorescence light that is generated in this process of a small cluster of nanocrystals is investigated on its dependence on the excitation intensity. With the help of an atomic force microscope (AFM) a dependence of the spectral composition of the fluorescence light from single nanocrystals on their size ranging between a few to 50 nm is demonstrated. By selective manipulation with the AFM, individual nanocrystals are coupled to gold nanospheres and the mechanisms of the observed plasmonic amplification of the emission is analyzed with time-resolved measurements. Single nitrogen–vacancy centers in nanodiamonds are employed as single-photon sources in a second subject area. A near-field probe is employed to attach these single quantum systems to microspherical resonators, by which their emission features the typical peaks in the spectrum due to the coupling to the whispering gallery modes of the spheres. This method can not only be applied to couple two or more single-photon emitters to the very same modes of a microsphere, but the resonators themselves can be pre-characterized to match one of the modes with the emitter. Furthermore, it will be demonstrated how the efficiency of a single-photon source can be enhanced by coupling the nitrogen-vacancy center to a plasmonic antenna made of gold nanospheres.

On demand single-photon and entangled-photon sources are key building-blocks for many proposed photonic quantum technologies. For practical device applications, epitaxially grown quantum dots (QDs) are of increasing importance due to their bright photon emission with sharp line width. Particularly, they are solid-state systems and can be easily embedded within a light-emitting diode (LED) to achieve electrically driven sources. Therefore, one would expect a full-fledged optoelectronic quantum network that is running on macroscopically separated, QD-based single- and entangled-photon devices. An all-electrically operated wavelength-tunable on demand single-photon source (SPS) is demonstrated first. The device consists of a LED in the form of self-assembled InGaAs QDs containing nanomembrane integrated onto a piezoelectric crystal. Triggered single photons are generated via injection of ultra-short electrical pulses into the diode, while their energy can be precisely tuned over a broad range of about 4.8 meV by varying the voltage applied to the piezoelectric crystal. High speed operation of this single-photon emitting diode up to 0.8 GHz is demonstrated. In the second part of this thesis, a fast strain-tunable entangled-light-emitting diode (ELED) is demonstrated. It has been shown that the fine structure splitting of the exciton can be effectively overcome by employing a specific anisotropic strain field. By injecting ultra-fast electrical pulses to the diode, electrically triggered entangled-photon emission with high degree of entanglement is successfully realized. A statistical investigation reveals that more than 30% of the QDs in the strain-tunable quantum LED emit polarization-entangled photon-pairs with entanglement-fidelities up to f+ = 0.83(5). Driven at the highest operation speed ever reported so far (400 MHz), the strain-tunable quantum LED emerges as unique devices for high-data rate entangled-photon applications. In the end of this thesis, on demand and wavelength-tunable LH single-photon emission from strain engineered GaAs QDs is demonstrated. Fourier-transform spectroscopy is performed, from which the coherence time of the LH single-photon emission is studied. It is envisioned that this new type of LH exciton-based SPS can be applied to realize an all-semiconductor based quantum interface in the foreseeable distributed quantum networks.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第22448号 / 工博第4709号 / 新制||工||1735(附属図書館) / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 竹内 繁樹, 教授 白石 誠司, 准教授 浅野 卓 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM

Im Rahmen der vorliegenden Dissertation wurden neuartige integrierte Einzelphotonenquellen (EPQ) und ihre Anwendung für die Quanteninformationsverarbeitung entwickelt und untersucht. Die Erzeugung von Einzelphotonen basiert auf einzelnen Defektzentren in nanometergroßen Diamantkristallen mit einzigartigen optischen Eigenschaften: Stabilität bei Zimmertemperatur ohne optisches Blinken. Diamantkristalle mit Größen bis unter 20nm wurden mit neuartigen „pick-and-place“ Techniken (z.B. mit einem Atomkraftmikroskop) in komplexe photonische Strukturen integriert. Zwei unterschiedliche Ansätze für die Realisierung der neuartigen EPQ wurden verfolgt. Beim ersten werden fluoreszierende Diamantkristalle in nano- und mikrometergroße Faser-basierte oder resonante Strukturen in einem „bottom-up“ Ansatz integriert, dadurch werden zusätzliche optische Komponenten überflüssig und das Gesamtsystem ultra-stabil und wartungsfrei. Der zweite Ansatz beruht auf einem Festkörperimmersionsmikroskop (FIM). Seine Festkörperimmersionslinse wirkt wie eine dielektrische Antenne für die Emission der Defektzentren. Es ermöglicht die höchsten bisher erreichten Photonenzählraten von Stickstoff-Fehlstellen von bis zu 2.4Mcts/s und Einsammeleffizienzen von bis zu 4.2%. Durch Anwendung des FIM bei cryogenen Temperaturen wurden neuartige Anwendungen und fundamentale Untersuchungen möglich, weil Photonenraten signifikant erhöht wurden. Die Bestimmung der spektralen Diffusionszeit eines einzelnen Defektzentrums (2.2µs) gab neue Erkenntnisse über die Ursachen von spektraler Diffusion. Spektrale Diffusion ist eine limitierende Eigenschaft für die Realisierung von Quanteninformationsanwendungen. Das Tisch-basierte FIM wurde außerdem als kompakte mobile EPQ mit Ausmaßen von nur 7x19x23cm^3 realisiert. Es wurde für ein Quantenkryptographie-Experiment implementiert, zum ersten Mal mit Siliziumdefektzentren. Des Weiteren wurde ein neues Konzept für die Erzeugung von infraroten EPQ entwickelt und realisiert. / The presented thesis covers the development and investigation of novel integrated single photon (SP) sources and their application for quantum information schemes. SP generation was based on single defect centers in diamond nanocrystals. Such defect centers offer unique optical properties as they are room temperature stable, non-blinking, and do not photo-bleach over time. The fluorescent nanocrystals are mechanically stable, their size down to 20nm enabled the development of novel nano-manipulation pick-and-place techniques, e.g., with an atomic force microscope, for integration into photonic structures. Two different approaches were pursued to realize novel SP sources. First, fluorescent diamond nanocrystals were integrated into nano- and micrometer scaled fiber devices and resonators, making them ultra-stable and maintenance free. Secondly, a solid immersion microscope (SIM) was developed. Its solid immersion lens acts as a dielectric antenna for the emission of defect centers, enabling the highest photon rates of up to 2.4Mcts/s and collection efficiencies of up to 4.2% from nitrogen vacancy defect centers achieved to date. Implementation of the SIM at cryogenic temperatures enabled novel applications and fundamental investigations due to increased photon rates. The determination of the spectral diffusion time of a single nitrogen vacancy defect center (2.2µs) gave new insights about the mechanisms causing spectral diffusion. Spectral diffusion is a limiting property for quantum information applications. The table-top SIM was integrated into a compact mobile SP system with dimension of only 7x19x23cm^3 while still maintaining record-high stable SP rates. This makes it interesting for various SP applications. First, a quantum key distribution scheme based on the BB84 protocol was implemented, for the first time also with silicon vacancy defect centers. Secondly, a conceptually novel scheme for the generation of infrared SPs was introduced and realized.

Organic semiconductors show promise to yield a novel class of bendable electronic devices, and much research efforts have focused on the optimization of these films for device performance. It is well known that the structure of organic films has a large influence over the electronic properties. In particular, the carrier mobility is often highly anisotropic, and domain boundaries have a detrimental effect on charge transport. Therefore the domain structure and lattice orientation are of particular interest. However, little is known about the domain structure of organic films, and techniques to study these properties have only begun to emerge in recent years. In this thesis, we apply two experimental techniques, Grazing-Incidence X-ray Diffraction (GIXD) and Lateral Force Microscopy (LFM), toward studying the lattice and domain structure of tetracene films grown on the silicon(001)-monohydride surface. We describe the necessary steps toward optimizing the sensitivity of these techniques to the domain structure. Results show that the crystalline tetracene films form a layered morphology in which the a-b plane lies parallel to the substrate surface. The film lattice structure is similar to bulk tetracene, and the lattice is confined to two orthogonal orientations, forming a partially-commensurate relationship with the substrate surface lattice along the film 'a' axis. LFM images reveal two types of polycrystalline domains. The first type ("major domains") are tens of microns in size, and are classified by their lattice orientation. They are subdivided into the second type ("sub-domains"), which range from 0.1 to 5um in size, and are argued to represent regions of uniform molecular tilt direction. The GIXD data show that the single-crystal domains which comprise these two larger domain types are anisotropic in size, being up to two times longer along the film 'b' axis than along 'a'. The single-crystal domains range from 0.05 to 0.2um in size, depending on lattice orientation and film thickness. The mathematical basis for these single-crystal domain size calculations is presented. The single-crystal domain sizes are thickness-dependent, and are two orders of magnitude smaller than a typical surface island observed in atomic-force microscopy (AFM) topographs. Substrate steps can also significantly influence the film structure by inducing boundaries in the single-crystal domains and sub-domains, but not in the major domains. This detailed knowledge of the domain structure of organic thin-films may assist in our understanding of the factors which affect charge transport in thin films, and may help to direct research efforts in optimizing the film structure for device performance. / Natural Sciences and Engineering Research Council (NSERC), Canadian Foundation for Innovation (CFI), Ontario Innovation Trust (OIT).

Ce manuscrit expose le développement de ressources fondamentales pour les communications quantiques à longues distances basées sur les technologies des fibres optiques télécoms et des guides d'onde optiques non linéaires. Après une introduction générale sur les communications quantiques, cette thèse est structurée en trois parties principales. La première partie illustre le développement de deux sources pour la génération de paires de photons intriqués en polarisation et émis à une longueur d'onde télécom via conversion paramétrique spontanée (SPDC) dans des guides d'ondes non linéaires intégrés sur niobate de lithium périodiquement polarisé. Les sources s'appuient respectivement sur un accord de phase de type-II et un accord de phase de type-0 et sur des solutions de filtrage et d'interférométrie mises en place après le cristal non linéaire. Dans la seconde partie, sont discutées les réalisations de deux sources de photons uniques annoncés haut débit. La première s'appuie sur le multiplexage spatial sur puce de photons uniques annoncés. La seconde exploite le multiplexage temporel passif grâce à l'utilisation d'un laser télécom cadencé à 10 GHz. Enfin, nous présentons une approche tout-optique visant la synchronisation de sources distantes de paires de photons intriqués, agencées selon une architecture de type relais quantique distribué. Cette technique innovante repose sur l'utilisation d'un laser télécom impulsionnel en tant qu'horloge optique de référence. Cette horloge autorise la synchronisation de l'émission de paires de photons dans la bande C des télécoms en deux lieux distants. Des résultats préliminaires d'interférence à deux photons sont montrés et discutés. / This manuscript reports the development of fundamental resources for long distance quantum communication based on fibre telecom technology and non-linear optical waveguides. After a general introduction on quantum communication, the thesis is structured along three parts. The first part illustrates the development of two photonic polarization entanglement sources suitable for quantum networking. Both sources generate paired photons at telecom wavelength via spontaneous parametric down conversion (SPDC) in periodically poled lithium niobate waveguides (PPLN/W). They rely on type-II and type 0 phase matching, respectively. In the second part, two high quality heralded single photon sources are highlighted. The first one relies on on-chip generation and spatial multiplexing of heralded single photons towards achieving higher bit rates. The second one takes advantage of passive temporal multiplexing of a single SPDC process. Finally, an all-optical approach towards efficient and accurate synchronization of remote entangled photon pair sources within quantum relay architecture over long distances is presented. This particular synchronization technique highlights the use of ultra-fast picosecond pulsed telecom fiber laser, operating at 2.5 GHz repetition rate, acting as a master optical clock, enabling to accurately synchronize the emission of photon pairs in the telecom C-band of wavelengths at two remote locations. This innovative approach is applied for synchronizing two remote PLLN/W based sources operated at 2.5 GHz, and preliminary results on two-photon interference obtained with single photons coming from each source are shown and discussed.

On demand single-photon and entangled-photon sources are key building-blocks for many proposed photonic quantum technologies. For practical device applications, epitaxially grown quantum dots (QDs) are of increasing importance due to their bright photon emission with sharp line width. Particularly, they are solid-state systems and can be easily embedded within a light-emitting diode (LED) to achieve electrically driven sources. Therefore, one would expect a full-fledged optoelectronic quantum network that is running on macroscopically separated, QD-based single- and entangled-photon devices. An all-electrically operated wavelength-tunable on demand single-photon source (SPS) is demonstrated first. The device consists of a LED in the form of self-assembled InGaAs QDs containing nanomembrane integrated onto a piezoelectric crystal. Triggered single photons are generated via injection of ultra-short electrical pulses into the diode, while their energy can be precisely tuned over a broad range of about 4.8 meV by varying the voltage applied to the piezoelectric crystal. High speed operation of this single-photon emitting diode up to 0.8 GHz is demonstrated. In the second part of this thesis, a fast strain-tunable entangled-light-emitting diode (ELED) is demonstrated. It has been shown that the fine structure splitting of the exciton can be effectively overcome by employing a specific anisotropic strain field. By injecting ultra-fast electrical pulses to the diode, electrically triggered entangled-photon emission with high degree of entanglement is successfully realized. A statistical investigation reveals that more than 30% of the QDs in the strain-tunable quantum LED emit polarization-entangled photon-pairs with entanglement-fidelities up to f+ = 0.83(5). Driven at the highest operation speed ever reported so far (400 MHz), the strain-tunable quantum LED emerges as unique devices for high-data rate entangled-photon applications. In the end of this thesis, on demand and wavelength-tunable LH single-photon emission from strain engineered GaAs QDs is demonstrated. Fourier-transform spectroscopy is performed, from which the coherence time of the LH single-photon emission is studied. It is envisioned that this new type of LH exciton-based SPS can be applied to realize an all-semiconductor based quantum interface in the foreseeable distributed quantum networks.