In this work, resonant laser spectroscopy has been utilized in two major projects --resonance fluorescence measurements in solid-state quantum-confined nanostructures and laser-induced fluorescence measurements in gases. The first project focuses on studying resonant light-matter interactions in semiconductor quantum dots "artificial atoms" with potential applications in quantum information science. Of primary interest is the understanding of fundamental processes and how they are affected by the solid-state matrix. Unlike atoms, quantum dots are susceptible to a variety of environmental influences such as phonon scattering and spectral diffusion. These interactions alter the desired properties of the scattered light and hinder uses in certain single photon source applications. One application of current interest is the use of quantum dots in “quantum repeaters” for which two-photon interference is key. Motivated by such an application we have explored the limits imposed by environmental effects on two quantum dots in the same sample, the scattered light from which is being interfered. We find that both one-photon and two-photon interference, although substantial, are affected in a variety of ways, in particular by spectral diffusion. These observations are discussed and compared with a theoretical model. We further investigated correlations in pulsed resonance fluorescence, and found significant unexpected spectral and temporal deviations from those studied under continuous wave excitation. Under these conditions, the scattered light exhibits Rabi oscillations and photon anti-bunching, while maintaining a rich spectrum containing many spectral features. These observations are discussed and compared with a theoretical model. In the second project, the focus is on the investigation of the possibility of detecting N2+ ions in air using laser induced fluorescence, with potential applications in detection of fissile materials at a distance. A photon-counting analysis reveals that the fluorescence decay rate rapidly increases with increasing N2 pressure and thus limits the detection at elevated pressures, in particular at atmospheric pressure. We show that time-gated detection can be used to isolate N2+ fluorescence from delayed N2 emission. Based on the spontaneous Raman signal from N2 simultaneously observed with N2+ fluorescence, we could estimate a limit of detection in air of order 108-1010 cm3.

One of today’s challenges to realise computing based on quantum mechanics is to reliably and scalably encode information in quantum systems. Here, we present a photon source to on-demand deliver photonic quantum bits of information based on a strongly coupled atom-cavity system. The source operates intermittently for periods of up to 100 <i>μ</i>s, with a single-photon repetition rate of 1 MHz, and an intra-cavity production efficiency of up to 85%. Our ability to arbitrarily control the photons’ wavepackets and phase profiles, together with long coherence times of 500 ns, allows to store time-bin encoded quantum information within a single photon. To do so, the spatio-temporal envelope of a single photon is sub-divided in d time bins which allows for the delivery of arbitrary qu-d-its. This is done with a fidelity of > 95% for qubits, and 94% for qutrits verified using a newly developed time-resolved quantum-homodyne measurement technique. Additionally, we combine two separate fields of quantum physics by using our deterministic single-photon source to seed linear optics quantum computing (LOQC) circuits. As a step towards quantum networking, it is shown that this photon source can be combined with quantum gates, namely a chip-integrated beam splitter, a controlled-NOT (CNOT) gate as well as a CNOT4 gate. We use this CNOT4 gate to entangle photons deterministically emitted from our source and observe non-classical correlations between events separated by periods exceeding the travel time across the chip by three orders of magnitude. Additionally, we use time-bin encoded qubits to systematically study the de- and re-phasing of quantum states as well as the the effects of time-varying internal phases in photonic quantum circuits.

No description available.

京都大学 / 0048 / 新制・課程博士 / 博士(薬学) / 甲第18218号 / 薬博第808号 / 新制||薬||238(附属図書館) / 31076 / 京都大学大学院薬学研究科医療薬科学専攻 / (主査)教授 佐治 英郎, 教授 橋田 充, 教授 髙倉 喜信 / 学位規則第4条第1項該当 / Doctor of Pharmaceutical Sciences / Kyoto University / DFAM

We report on the systematic characterization of the optical properties of diamond color centers based on Pb impurities. An ensemble photoluminescence analysis of their spectral emission was performed at different excitation wavelengths in the 405–520 nm range and at different temperatures in the 4–300 K range. The series of observed spectral features consist of different emission lines associated with Pb-related defects. Finally, a room-temperature investigation of single-photon emitters under 490.5 nm laser excitation is reported, revealing different spectral signatures with respect to those already reported under 514 nm excitation. This work represents a substantial progress with respect to previous studies on Pb-related color centers, both in the attribution of an articulated series of spectral features and in the understanding of the formation process of this type of defect, thus clarifying the potential of this system for high-impact applications in quantum technologies.

No description available.

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.

Photonics has consistently played an important role in the investigation of quantum-enhanced technologies and the corresponding study of fundamental quantum phenomena. The majority of these experiments have relied on the free space propagation of light between bulk optical components. This relatively simple and flexible approach often provides the fastest route to small proof-of-principle demonstrations. Unfortunately, such experiments occupy significant space, are not inherently phase stable, and can exhibit significant scattering loss which severely limits their use. Integrated photonics offers a scalable route to building larger quantum states of light by surmounting these barriers. In the first half of this thesis, we describe the operation of on-chip heralded sources of single photons. Loss plays a critical role in determining whether many quantum technologies have any hope of outperforming their classical analogues. Minimizing loss leads us to choose Spontaneous Four-Wave Mixing (SFWM) in a silica waveguide for our source design; silica exhibits extremely low scattering loss and emission can be efficiently coupled to the silica chips and fibers that are widely used in quantum optics experiments. We show there is a straightforward route to maximizing heralded photon purity by minimizing the spectral correlations between emitted photon pairs. Fabrication of identical sources on a large scale is demonstrated by a series of high-visibility interference experiments. This architecture offers a promising route to the construction of nonclassical states of higher photon number by operating many on-chip SFWM sources in parallel. In the second half, we detail one of the first proof-of-principle demonstrations of a new intermediate model of quantum computation called boson sampling. While likely less powerful than a universal quantum computer, boson sampling machines appear significantly easier to build and may allow the first convincing demonstration of a quantum-enhanced computation in the not-distant future. Boson sampling requires a large interferometric network which are challenging to build with bulk optics, we therefore perform our experiment on-chip. We model the effect of loss on our postselected experiment and implement a circuit characterization technique that accounts for this loss. Experimental imperfections, including higher-order emission from our photon pair sources and photon distinguishability, are modeled and found to explain the sampling error observed in our experiment.

In order to improve the sensitivity of an optical receiver, the gain and the collection area of the photo-detectors within the receiver should be increased. Detectors with internal gain such as avalanche photodiodes (APD) are usually used to increase the sensitivity of the receiver. One problem with APDs is the sensitivity of their gain to their bias voltage, which makes them challenging to be fabricated in a standard CMOS process due to variations in their gain. However, when an APD is biased over its breakdown voltage, it is sensitive to a single photon, hence, referred to as a single photon avalanche diodes (SPAD). The SPADs are photon-counting detectors, which are less sensitive to their bias voltage, and can be integrated with rest of the electronic circuitry that form an optical receiver. An avalanche diode requires dedicated circuits to be operated in the SPAD mode. These circuits make the diode insensitive to an incident photon for a duration that is known as deadtime. Unfortunately, The collection area of the PD, APD, and SPADs are limited to their capacitance. Hence, a large photo-detector leads to a larger capacitance, which reduces the bandwidth of the receiver. In this thesis, a photon counting optical receiver based on an array of SPADs is proposed which increases the collection area with a low output capacitance. The avalanche diode and peripheral circuits which operate and readout-out the SPAD array are fabricated in the commercially available UMC 0.18 μm CMOS process. Initially, the avalanche diode is tested and characterised. A high performance circuit is then designed and tested which is able to achieve short deadtimes up to 4 ns. Once the photon counting operation of the SPAD is verified, a numerical model is developed to investigate the influence of several factors, including the deadtime, on the performance of the photon-counting detector in a communication link. Based on the simulation results, which show the advantages of an array over a single detector, a prototype detector array of 64 asynchronous SPADs is designed and tested. This array uses a high-speed readout mechanism which is inspired by the current steering digital-to-analogue converters. Bit error ratio tests (BERT) verify the photon counting capability of the proposed detector, and a bit error rate of 1E-3 has been achieved at data rate of 100 Mbps. In addition, the array of SPAD is compatible with a front-end of conventional optical receiver which uses a photodiode as a photo detector.

Deep brain stimulation (DBS) is a neurosurgical intervention now established for the treatment of movement disorders. For the treatment of chronic pain refractory to medical therapies, several prospective case series have been reported, but few centres worldwide have published findings from patients treated during the last decade using current standards of technology. This thesis seeks to survey the current clinical status of DBS for pain, investigate its mechanisms and their interactions with autonomic function, its clinical limitations and ablative alternatives. Presented first is a review of the current status of analgesic DBS including contemporary clinical studies. The historical background, scientific rationale, patient selection and assessment methods, surgical techniques and results are described. The clinical outcomes of DBS of the sensory thalamus and periventricular / periaqueductal grey (PAVG) matter in two centres are presented including results from several pain and quality of life measures. A series of translational investigations in human subjects receiving DBS for pain elucidating mechanisms of analgesic DBS and its effects upon autonomic function are then presented. Single photon emission tomography comparing PAVG, VP thalamus and dual target stimulation is described. Somatosensory and local field potential (LFP) recordings suggesting PAVG somatotopy are shown. ABPM results demonstrating changes with PAVG DBS are given and Portapres studies into heart rate variability changes with ventral PAVG DBS are detailed. Investigations using naloxone are then shown to hypothesise separate dorsal opioidergic and ventral parasympathetic analgesic streams in the PAVG. Finally, cingulotomy in lung cancer to relieve pain and dyspnoea results are discussed in the context of altering pain and autonomic function by functional neurosurgery. Pain and autonomic interactions and mechanisms in deep brain surgery for pain are then discussed alongside its limitations with proposals made for optimising treatment and improving outcomes.