Ultrafast quantum light pulses with durations of 1ps and below show great promise as information carriers in quantum communication and computation. In future they may also be used to probe physical processes at ultrashort timescales with a resolution beyond the limits of Heisenberg uncertainty. This thesis focuses on the creation and manipulation of quantum light pulses with second order nonlinear optical processes in optical waveguides. In chapter 1. Introduction, we lead the reader towards this work's topic by giving a brief qualitative overview over the EPR paradox, quantum entanglement, three-wave-mixing and quantum light pulses. Chapter 2. Basic concepts familiarizes the reader with the physical concepts and mathematical tools underlying this thesis. In chapter 3. Spectral engineering, we discuss the requirements to produce separable photon pair states with group velocity matching and examine several nonlinear materials widely used for optical waveguide inscription for their suitability to group velocity matching in the telecom wavelength regime. In chapter 4. A PP-KTP waveguide as parametric downconversion source, we give the basic spontaneous parametric downconversion source setup, as well as some initial measurements to characterize the single photon detectors, to demonstrate the production of correlated photons, and to determine the phasematching properties of the PP-KTP source. In the following chapter, 5. Fiber spectrometer, we present the single-photon fiber spectrometer. We discuss the experimental setup and calibration of the device, and measure the joint spectrum of photon pairs from our PP-KTP source. Finally, we investigate the behavior of a joint spectrum measurement of a high mean photon number source with binary detectors. In 6. Two-mode squeezed vacuum source, we characterize spectral correlations of an ultrafast SPDC source with the second order correlation function g². We present the g² measurement results and show that we can control the spectral correlations to produce a two-mode squeezed vacuum state of light. We then determine the mean photon number and gain of the source. 7. Quantum pulse gate: While the previous chapters focus on the creation and characterization of ultrafast quantum pulses of light, we now propose a way to manipulate the mode structure of a given quantum light state. We discuss the concept of an active optical filter sensitive to spectral/temporal pulse shape: The quantum pulse gate. In the final chapter 8. Conclusion and outlook, we recapitulate the main results of this thesis and provide a few pointers towards possibilities for future research building on it.
Ultrafast quantum light pulses with durations of 1ps and below show great promise as information carriers in quantum communication and computation. In future they may also be used to probe physical processes at ultrashort timescales with a resolution beyond the limits of Heisenberg uncertainty. This thesis focuses on the creation and manipulation of quantum light pulses with second order nonlinear optical processes in optical waveguides. In chapter 1. Introduction, we lead the reader towards this work's topic by giving a brief qualitative overview over the EPR paradox, quantum entanglement, three-wave-mixing and quantum light pulses. Chapter 2. Basic concepts familiarizes the reader with the physical concepts and mathematical tools underlying this thesis. In chapter 3. Spectral engineering, we discuss the requirements to produce separable photon pair states with group velocity matching and examine several nonlinear materials widely used for optical waveguide inscription for their suitability to group velocity matching in the telecom wavelength regime. In chapter 4. A PP-KTP waveguide as parametric downconversion source, we give the basic spontaneous parametric downconversion source setup, as well as some initial measurements to characterize the single photon detectors, to demonstrate the production of correlated photons, and to determine the phasematching properties of the PP-KTP source. In the following chapter, 5. Fiber spectrometer, we present the single-photon fiber spectrometer. We discuss the experimental setup and calibration of the device, and measure the joint spectrum of photon pairs from our PP-KTP source. Finally, we investigate the behavior of a joint spectrum measurement of a high mean photon number source with binary detectors. In 6. Two-mode squeezed vacuum source, we characterize spectral correlations of an ultrafast SPDC source with the second order correlation function g². We present the g² measurement results and show that we can control the spectral correlations to produce a two-mode squeezed vacuum state of light. We then determine the mean photon number and gain of the source. 7. Quantum pulse gate: While the previous chapters focus on the creation and characterization of ultrafast quantum pulses of light, we now propose a way to manipulate the mode structure of a given quantum light state. We discuss the concept of an active optical filter sensitive to spectral/temporal pulse shape: The quantum pulse gate. In the final chapter 8. Conclusion and outlook, we recapitulate the main results of this thesis and provide a few pointers towards possibilities for future research building on it.
Squeezed light is expected to enable new quantum metrology and quantum computation applications, but the very high degree of experimental control required in practice places severe demands on the physical devices used to generate it. As ultrafast squeezed light sources are reaching an unprecedented degree of brightness and modal control, there is a strong interest in developing methods for their experimental characterization and theoretical understanding. In this thesis, we demonstrate both a new application and a new characterization technique for pulsed squeezed light. In the first part of the thesis, we present a new metrological application of pulsed squeezed light: quantum-enhanced label-free nonlinear microscopy. Stimulated emission microscopy (SEM) is a state-of-the-art pump-probe microscopy technique whose sensitivity is ultimately limited by shot noise in the probe beam. We propose to overcome this fundamental limitation by using a sub-Poissonian probe generated via optical parametric amplification. We demonstrate an intensity-squeezed sub-picosecond pulsed probe, and a simple stimulated emission microscope. Using this squeezed probe, sub-Poissonian statistics are observed in the SEM signal. After this proof-of-principle experiment, we aim to provide an improved design for a source of intensity-squeezed light. First, we develop a theoretical framework to simulate the photon statistics of a general sub-Poissonian source, considering pulsed and focused pump and seed fields in a unified spatio-temporal description. Next, we use this framework to suggest possible improvements to our previous squeezed probe. In the second part of this thesis, we provide new theoretical and experimental tools to analyze the high gain regime of pulsed spontaneous parametric down-conversion (SPDC). We study a waveguided source capable of generating twin-beams with tens of photons in a single spatio-temporal mode. We develop a framework to efficiently simulate SPDC for an arbitrary nonlinear gain, including the effect of parasitic nonlinearities such as self-phase modulation (SPM) of the pump and cross-phase modulation (XPM) between pump and twin-beams. We experimentally characterize our source using a new technique based on stimulated difference-frequency generation (DFG). In a type-II down-conversion process, we measure the frequency generation produced not only in the orthogonal polarization to the seeding beam, but also in its same polarization, which we interpret as cascaded difference-frequency generation. We argue that the additional information obtained in this measurement allows for a self-referenced estimation of the squeezing gain. Using these measurements, we accurately fit our theoretical model, revealing that, in the high gain regime, parasitic nonlinearities strongly affect the spectral structure of the twin-beams. We propose a simple strategy to reduce the impact of these nonlinearities on the modal structure of SPDC.
Full control over the spatiotemporal structure of quantum states of light is an important goal in quantum optics, to generate, for instance, single-mode quantum pulses or to encode information on multiple modes, enhancing channel capacities. Quantum light pulses feature an inherent, rich spectral broadband-mode structure. In recent years, exploring the use of integrated optics as well as source engineering has led to a deep understanding of the pulse-mode structure of guided quantum states of light. In addition, several groups have started to investigate the manipulation of quantum states by means of single-photon frequency conversion. In this paper, we explore new routes towards complete control of the inherent pulse-modes of ultrafast pulsed quantum states by employing specifically designed nonlinear waveguides with adapted dispersion properties. Starting from our recently proposed quantum pulse gate (QPG), we further generalize the concept of spatiospectral engineering for arbitrary χ (2) -based quantum processes. We analyse the sum-frequency generation-based QPG and introduce the difference-frequency generation-based quantum pulse shaper (QPS). Together, these versatile and robust integrated optical devices allow for arbitrary manipulations of the pulse-mode structure of ultrafast pulsed quantum states. The QPG can be utilized to select an arbitrary pulse mode from a multimode input state, whereas the QPS enables the generation of specific pulse modes from an input wavepacket with a Gaussian-shaped spectrum.
The field of quantum optics offers the intriguing possibility of developing new, potentially ground-breaking technologies based on the laws of quantum physics. Single quanta of light, called photons, are at the heart of many such quantum optical technologies. They can serve, for example, as information carriers in quantum cryptography and in quantum-information processing. If such applications are to fulfill their enormous potential, it is essential to have sources available that provide photons in the required quantum states. An established way of generating states of single photons is based on photon-pair sources. In this approach, the detection of one photon of a pair heralds the presence of the partner photon, which can then be further processed. However, to generate heralded photons in pure quantum states, specific conditions have to be met, making the design and implementation of such sources challenging. This thesis presents two new photon-pair sources that allow the heralded generation of single photons with high purity. Both sources are based on optical fiber, which allows high collection efficiencies for the generated states and opens the possibility of easy integration into modern-day fiber networks. Chapter 1 provides an introduction to quantum optical technologies and gives a short overview of current approaches to generate pure single photons. Chapter 2 presents the basic theory on which the experimental work presented in Chapters 3 and 4 is based. It explains the concept of a spectrally broad single photon and how photon purity can be tested using Hong-Ou-Mandel (HOM) interference. Subsequently, the properties of photon-pair states and the heralded generation of single photons from such states are discussed. It is shown that for a heralded photon to be pure, the original photon pair has to be in a factorable state, that is, free of any correlations. The introduced theory is then applied to spontaneous four-wave mixing (SFWM) in optical fibers, a nonlinear process that allows the generation of photon pairs. It is shown how the factorability of the created pairs depends on the fiber's dispersion properties, and the necessary conditions for the generation of factorable states are derived. The chapter concludes with an analysis of the photon statistics of the four-wave mixing process, explaining how statistics and the g(2) correlation function can be used to evaluate the factorability of the SFWM output state. Chapters 3 and 4 contain the main results of this thesis. Chapter 3 presents the first spectrally decorrelated photon-pair source bridging the visible and telecommunication wavelength ranges. The photon pairs are generated by SFWM in a photonic crystal fiber (PCF). The chapter documents the procedure of how the PCF source was designed and fabricated, as well as its characterization based on spectral measurements and photon statistics. One photon of the pair state is generated in the visible at 513.5 nm, where it can be efficiently detected with silicon-based single-photon detectors. It serves as a herald for its broadband partner photon, which is emitted in the telecom wavelength range at 1547 nm. A spectral coincidence measurement shows that the heralded photon exhibits a purity of up to 0.82. At increased pump powers, even the heralded generation of higher photon-number states in the telecom band becomes feasible. In Chapter 4, we use commercial birefringent fiber to herald high-purity photons of picosecond duration at 848 nm. The presented two-source HOM interference experiment shows that the heralded unfiltered state has a purity of at least 0.73. This value is increased to 0.84 with the application of wavelength filters suppressing low-intensity side peaks in the spectrum. The heralded photons are coupled into a single-mode fiber with an efficiency of 85%, the highest reported value to date for factorable sources. It is also shown that a commercial polarization controller can be used to fine-tune the generated wavelengths. This facilitates matching photons from multiple sources, as required for optical quantum computing schemes. Chapter 5 summarizes all results and provides an outlook toward potential future projects.
Single photons provide a natural platform for quantum communication and quantum networking, as they can be entangled in many degrees of freedom and maintain coherence over long-distance links. However, while their minimal interactions with the environment isolate them from detrimental noise, it can make them difficult to measure and manipulate. In particular, manipulation on the ultrafast timescale is necessary to fully exploit the energy-time (or spectral) photonic degree of freedom. Full control over the spectral properties of single photons is key to many quantum technologies and opens the door to natural high-dimensional quantum encodings. \n \nIn this thesis, we theoretically and experimentally examine the use of nonlinear optical processes mediated by strong laser pulses as a method to control the spectral properties of ultrafast single photons. By mixing single-photon pulses with strong escort pulses that have been shaped through dispersion in a nonlinear crystal, the shape of the escort is imprinted on the photon, resulting in a custom-tailored upconverted pulse. We theoretically examine this process for quadratic spectral phases and show that it has the potential to be simultaneously effective and efficient for the customization of single-photon spectral waveforms, and can be performed in an entanglement-conserving manner. \n \nWe then experimentally demonstrate the range of this technique through three applications. First, we show that sum-frequency generation with shaped pulses can be used to coherently measure time-bin encoded photons with bin separations on the order of picoseconds, well below the timing resolution of our detectors. Secondly, we show that this technique can be adapted to convert a train of pulses to a frequency comb, which can be read out in a straightforward manner using diffraction-based spectrometry. We also show here that this process can be performed in a polarization-maintaining fashion, and demonstrate that entanglement with a partner photon is conserved with high fidelity. Finally, we show that this process can be viewed as a time lens, which modulates a temporal waveform in an analogous fashion to a lens focusing a beam of light. We apply the time lens to a photon from an energy-time entangled pair, and show negative magnification of the joint spectrum through a reversal of the spectral correlations. Such processes could find application in quantum state engineering and high-speed single-photon measurement.
The fields of quantum and nonlinear optics have given rise to a variety of nonclassical states of light that have been proven to surpass certain limitations set by classical physics. Namely, certain squeezed and entangled states have been shown to beat the shot-noise limit when making precision phase measurements in interferometry, as well as write lithographic patterns that are smaller than classically allowed by the Rayleigh diffraction limit. Additionally, single-photon sources and entangled photon pairs have given rise to provably secure quantum key distribution for cryptography. Producing these quantum states of light has proven a difficult task. Nonlinear crystals, when pumped by a laser, produce pairs of single photons via the process of spontaneous parametric down conversion (SPDC). This process is mediated by the second order nonlinear susceptibility of the material. When pumped in a high gain regime, these crystals give rise to optical parametric amplification, which is a viable source of squeezed light. The vast majority of research in this area has focused on crystals that are seeded by vacuum in their two modes. This dissertation concerns the field of quantum nonlinear optics. It is an investigation into the processes that occur when nonlinear materials interact with the electromagnetic field on the single photon level. I have focused on seeding nonlinear crystals with quantum states of light, including single photons and entangled states. This process results in various states directly applicable to interferometry, imaging, and cryptography. Another application investigated is an absolute radiance measurement via stimulated parametric down conversion resulting from non-vacuum seeding of a nonlinear crystal. Additionally, other nonlinear processes, including four-wave mixing, nonlinear magneto-optical effects and coherent population trapping in warm atomic vapor involving quantum states of light are investigated. The process of seeding third-order nonlinear interactions, such as in atomic vapors, gives rise to a variety of interesting, nonclassical phenomena such as entangled image transfer and nonlocal imaging. Strong analogies between SPDC and four-wave mixing are drawn. I also experimentally show an all optical pi-only phase shift of one light beam via another in warm Cesium vapor.
The creation and manipulation of biphotons is important for many applications in quantum optics and quantum information. Topics that benefit from efficient biphoton sources range from the most fundamental quantum science experiments to the highly applied fields of quantum communication and quantum computation. Biphoton sources have long been hailed as one of the leading methods for creating entangled photon pairs for tests of Bell's inequality, creating heralded photon pairs that are used in on-demand single-photon sources and heralded measurement techniques, and for quantum communication protocols to name a few. Specifically for quantum communication, biphoton sources are commonly used for cutting edge quantum key distribution (QKD) protocols. In the first part of the thesis, I focus on realizing an efficient biphoton source that produces high yield photon pairs. More specifically, I develop an optimized biphoton source using the nonlinear optical process of spontaneous parametric down-conversion in a second-order nonlinear crystal. I develop a formalism for predicting the two important metrics of a biphoton source: the heralding efficiency and joint count rate. I show how, from a large parameter space, one can tailor the phase matching of the nonlinear interaction to create a high quality biphoton source that produces both high heralding efficiency and high joint count rate. I achieve heralding efficiencies of 86$\\pm5\\%$ and joint count rates of 2.58$\\pm0.6kHzpermWpumppower.Ishowthatusingacollinearnondegenerategeometryallowsforheraldingefficienciesofupto99.7\\%$ assuming no loss in the system. I verify the theoretical model with experimental results and find good agreement. In the second part of the thesis I turn to manipulating the single photons born from the biphoton source for applications in creating single-photon spectrometers and time-frequency QKD systems. The security of QKD is only guaranteed if the two parties have access to a set of states called mutually unbiased states. I create a set of these states in time and their conjugate states in the frequency basis and show that I can manipulate single photon correlations in time and frequency so that an eavesdropper can be detected if she localizes a photon to a 1 ns time interval. Additionally, in these experiments, I stretch a single photon wavepacket of 5-ps-width to a wavepacket of 8.3-ns-width and subsequently recompress it to at least the resolution of the detectors (sim 300 ps). This demonstrates a stretch factor of >1600 for a single-photon pulse using a group velocity dispersive material. To my knowledge, this is the largest reported stretch factor for a single-photon wavepacket produced by a biphoton source. The ability to stretch and recompress a single photon by this amount has applications in creating high-resolution, high-efficiency, single-photon spectrometers as well as advancing time-frequency QKD systems and other temporal pulse shaping applications.