Self-assembled semiconductor quantum dots have attracted considerable interest recently, ranging from fundamental studies of quantum optics to advanced applications in the field of quantum information science. With their atom-like properties, quantum dot based nanophotonic devices may also substantially contribute to the development of quantum computers. This work presents experimental progress towards the understanding of light-matter interactions that occur beyond well-understood monochromatic resonant light scattering processes in semiconductor quantum dots. First, we report measurements of resonance fluorescence under bichromatic laser excitation. With the inclusion of a second laser, both first-order and second-order correlation functions are substantially altered. Under these conditions, the scattered light exhibits a rich spectrum containing many spectral features that lead to a range of nonlinear multiphoton dynamics. These observations are discussed and compared with a theoretical model. Second, we investigated the light scattered by a quantum dot in the presence of spectral filtering. By scanning the tunable filters placed in front of each detector of a Hanbury-Brown and Twiss setup and recording coincidence measurements, a \two-photon spectrum" has been experimentally reconstructed for the first time. The two-photon spectrum contains a wealth of information about the cascaded emission involved in the scattering process, such as transitions occurring via virtual intermediate states. Our measurements also reveal that the scattered frequency-filtered light from a quantum dot violates the Cauchy-Schwarz inequality. Finally, Franson-interferometry has been performed using spectrally filtered light from quantum dot resonance fluorescence. Visibilities exceeding the classical limit were demonstrated by using a pair of folded Mach-Zehnder interferometers, paving the way for producing single time-energy entangled photon pairs that could violate Bell's inequalities.

Current x-ray technologies provide security personnel with non-invasive sub-surface imaging and contraband detection in various portal screening applications such as checked and carry-on baggage as well as cargo. Computed tomography (CT) scanners generate detailed 3D imagery in checked bags; however, these scanners often require significant power, cost, and space. These tomography machines are impractical for many applications where space and power are often limited such as checkpoint areas. Reducing the amount of data acquired would help reduce the physical demands of these systems. Unfortunately this leads to the formation of artifacts in various applications, thus presenting significant challenges in reconstruction and classification. As a result, the goal is to maintain a certain level of image quality but reduce the amount of data gathered. For the security domain this would allow for faster and cheaper screening in existing systems or allow for previously infeasible screening options due to other operational constraints. While our focus is predominantly on security applications, many of the techniques can be extended to other fields such as the medical domain where a reduction of dose can allow for safer and more frequent examinations. This dissertation aims to advance data reduction algorithms for security motivated x-ray imaging in three main areas: (i) development of a sensing aware dimensionality reduction framework, (ii) creation of linear motion tomographic method of object scanning and associated reconstruction algorithms for carry-on baggage screening, and (iii) the application of coded aperture techniques to improve and extend imaging performance of nuclear resonance fluorescence in cargo screening. The sensing aware dimensionality reduction framework extends existing dimensionality reduction methods to include knowledge of an underlying sensing mechanism of a latent variable. This method provides an improved classification rate over classical methods on both a synthetic case and a popular face classification dataset. The linear tomographic method is based on non-rotational scanning of baggage moved by a conveyor belt, and can thus be simpler, smaller, and more reliable than existing rotational tomography systems at the expense of more challenging image formation problems that require special model-based methods. The reconstructions for this approach are comparable to existing tomographic systems. Finally our coded aperture extension of existing nuclear resonance fluorescence cargo scanning provides improved observation signal-to-noise ratios. We analyze, discuss, and demonstrate the strengths and challenges of using coded aperture techniques in this application and provide guidance on regimes where these methods can yield gains over conventional methods.

京都大学 / 新制・課程博士 / 博士(エネルギー科学) / 甲第24254号 / エネ博第452号 / 新制||エネ||85(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー応用科学専攻 / (主査)教授 大垣 英明, 教授 白井 康之, 教授 宮内 雄平 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

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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.

京都大学 / 0048 / 新制・課程博士 / 博士(エネルギー科学) / 甲第17918号 / エネ博第290号 / 新制||エネ||60(附属図書館) / 30738 / 京都大学大学院エネルギー科学研究科エネルギー応用科学専攻 / (主査)教授 大垣 英明, 教授 白井 康之, 教授 松田 一成 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DGAM

Membrane proteins play a key role in numerous physiological processes such as transport, energy transduction in respiratory and photosynthetic systems, and signal transduction, and are of great pharmaceutical interest, comprising more than 60% of known drug targets. However, crystallisation of membrane proteins, and G protein-coupled receptors (GPCRs) in particular, still relies heavily on the use of protein engineering strategies, which have been shown to hamper protein activity. Here, a range of biophysical methods were used to study the structure and function of two membrane proteins, a prokaryotic peptide transporter, PepT_So and a GPCR, neurotensin receptor 1 (NTS1), using different membrane reconstitution methods to study the proteins in a native-like environment. Firstly, using the pulsed electron paramagnetic resonance (EPR) method of double electron-electron resonance (DEER) the conformation of PepT_So reconstituted into lipid bilayers was assessed and compared to previous structural data obtained from crystallography and modelling. The influence of the membrane potential and the presence of substrate on the conformational heterogeneity of this proton-coupled transporter were investigated. Secondly, NTS1 purification was optimized for biophysical study. Cysteine mutants were created and a labelling protocol was developed and optimized for fluorophore and nitroxide labelling studies. NTS1 was then studied by continuous-wave EPR, to assess the influence of ligand on local protein dynamics, and to assess the structure of a receptor segment known as helix 8, that was proposed to be an α-helix, but was only observed to be helical in one of the NTS1 crystallographic studies. Ensemble and single-molecule Förster resonance energy transfer (FRET), and DEER were combined to study the dimerisation behaviour of NTS1, showing novel dynamics of the interfacial associations. Finally, the signalling mechanism of NTS1 was also investigated using microscale thermophoresis (MST) to assess the affinity of the receptor for G protein in vitro in the absence of ligand, or in the presence of agonist or antagonist. MST measurements were performed in detergent and in nanodiscs of different lipid compositions, to assess the influence of the lipid environment on receptor function. In summary, this thesis demonstrates the potential of biophysical techniques to study various aspects of membrane protein structure and function in native-like lipid systems, complementing e.g. structural data obtained from crystallographic studies with functional data for membrane proteins in more native environments, as well as shedding light on protein dynamics. The work presented here provides novel insights into PepTSo transport, and in particular into NTS1 structure, signalling, and oligomerisation, opening up several avenues for future research.

The problem under consideration in the thesis is a two level atom in a photonic crystal and a pumping laser. The photonic crystal provides an environment for the atom, that modifies the decay of the exited state, especially if the atom frequency is close to the band gap. The population inversion is investigated als well as the emission spectrum. The dynamics is analysed in the context of open quantum systems. Due to the multiple reflections in the photonic crystal, the system has a finite memory that inhibits the Markovian approximation. In the Heisenberg picture the equations of motion for the system variables form a infinite hierarchy of integro-differential equations. To get a closed system, approximations like a weak coupling approximation are needed. The thesis starts with a simple photonic crystal that is amenable to analytic calculations: a one-dimensional photonic crystal, that consists of alternating layers. The Bloch modes inside and the vacuum modes outside a finite crystal are linked with a transformation matrix that is interpreted as a transfer matrix. Formulas for the band structure, the reflection from a semi-infinite crystal, and the local density of states in absorbing crystals are found; defect modes and negative refraction are discussed. The quantum optics section of the work starts with the discussion of three problems, that are related to the full resonance fluorescence problem: a pure dephasing model, the driven atom and resonance fluorescence in free space. In the lowest order of the system-environment coupling, the one-time expectation values for the full problem are calculated analytically and the stationary states are discussed for certain cases. For the calculation of the two time correlation functions and spectra, the additional problem of correlations between the two times appears. In the Markovian case, the quantum regression theorem is valid. In the general case, the fluctuation dissipation theorem can be used instead. The two-time correlation functions are calculated by the two different methods. Within the chosen approximations, both methods deliver the same result. Several plots show the dependence of the spectrum on the parameters. Some examples for squeezing spectra are shown with different approximations. A projection operator method is used to establish two kinds of Markovian expansion with and without time convolution. The lowest order is identical with the lowest order of system environment coupling, but higher orders give different results. / Die Arbeit befasst sich mit der Emission eines 2-Niveau-Atoms in einem photonischen Kristall mit einem treibenden Laser. Der photonische Kristall stellt für das Atom eine Umgebung dar, die seinen Zerfall verändert, insbesondere wenn die Übergangsfrequenz des Atoms nahe an der Bandkante ist. Es werden sowohl die Besetzungen als auch das Emissionsspektrum untersucht. Die Dynamik wird im Kontext offener Quantensysteme analysiert. Durch die vielfachen Reflexionen im photonischen Kristall hat das System ein endliches Gedächtnis, das die Markov-Näherung verhindert. Im Heisenberg-Bild stellen die Bewegungsgleichungen für die Systemvariablen eineunendliche Hierachie von Integro-Differentialgleichungen dar. Um ein geschlossenes System zu erhalten, sind Näherungen wie eine schwache Kopplung nötig. Zunächst wird ein einfacher photonischer Kristall betrachtet.: Der eindimensionale photonische Kristall, der aus wechselnden Lagen besteht. Die Blochmoden innerhalb und die Vakuummoden außerhalb des endlichen photonischen Kristalls sind durch eine Transformationsmatrix, die als Transfermatrix interpretiert werden kann, miteinander verbunden. Einfache Formeln für die Bandstruktur, Reflexion eines halb-unendlichen Kristalls, die lokale Zustandsdichte im absorbierenden Kristall werden gefunden; außerdem werden Defektmoden und negative Brechung diskutiert. Im quantenoptischen Teil der Arbeit werden zu Anfang drei Probleme diskutiert, die im Zusammenhang zum Problem der Resonanzfluoreszenz stehen und die analytisch berechnet werden können: Ein Dephasierungsmodell, das getriebenen Atom und Resonanzfluoreszenz im freien Raum. In der niedrigsten Ordnung der System-Bad-Kopplung werden die Erwartungswerte analytisch berechnet und die stationären Zustände werden für bestimmte Fälle diskutiert. Bei der Berechnung der Zweizeitkorrelationsfunktion und der Spektren taucht das zusätzliche Problem der Korrelationen zwischen den beiden Zeiten auf. Im Markov-Fall gilt das Quantenregressionstheorem. Im allgemeinen Fall kann stattdessen das Fluktuations-Dissipations-Theorem benutzt werden. Die Korrelationsfunktionen werden mit zwei verschiedenen Methoden berechnet. Innerhalb der gewählten Näherungen liefern beide Methoden dasselbe Resultat. Einige Plots zeigen die Abhängigkeit des Spektrums von den verschiedenen Parametern. Mehrere Beispiele für Squeezing-Spektren werden mit den verschiedenen Näherungen gezeigt. Eine Projektions-Operator-Methode wird benutzt, um zwei Arten einer Markov-Entwicklung zu implementieren, mit und ohne Faltungsintegral. Die niedrigste Ordnung ist identisch mit der niedrigsten Ordnung der System-Bad-Kopplung, wohingegen höhere Ordnungen andere Resultate ergeben.