A short perspective on long crystals: broadband wave mixing and its application to ultrafast quantum optics
Piotr Wasylczyk, Alfred B. U’Ren, Peter J. Mosley, Jeff S. Lundeen, Matthijs P. A. Branderhorst, S.-P. Gorza, Antoine Monmayrant, Aleksandr S. Radunsky, Ian A. Walmsley
We present an overview of recently developed ideas in ultrafast nonlinear optics, and describe three applications where these ideas have had an impact. A closer look at three wave mixing of broadband electromagnetic fields in birefringent nonlinear crystals shows that not only phase matching, but also group velocity matching is important for understanding the process of up- and down-conversion with ultrashort laser pulses. In fact the higher-order dispersion of nonlinear crystalline materials provides an underused degree of freedom that allows tailoring the interaction so that it is suitable for a number of different applications. We analyse the processes of parametric downconversion for the production of pure single photon states, and upconversion for ultrashort pulse characterization and for quantum state and process tomography in molecules.
We present an overview of recently developed ideas in ultrafast nonlinear optics, and describe three applications where these ideas have had an impact. A closer look at three wave mixing of broadband electromagnetic fields in birefringent nonlinear crystals shows that not only phase matching, but also group velocity matching is important for understanding the process of up- and down-conversion with ultrashort laser pulses. In fact the higher-order dispersion of nonlinear crystalline materials provides an underused degree of freedom that allows tailoring the interaction so that it is suitable for a number of different applications. We analyse the processes of parametric downconversion for the production of pure single photon states, and upconversion for ultrashort pulse characterization and for quantum state and process tomography in molecules.
Nonclassical photon sources are key components in quantum information science and technology. Here, the basic principles and progresses for single photon generation and their further manipulation based on second- or third-order nonlinear processes in various degrees of freedom are briefly reviewed and discussed. Based on spontaneous parametric down-conversion and spontaneous four-wave mixing, various nonlinear materials such as quasi-phase-matching crystals, dispersion-shifted fibers, and silicon-on-insulator waveguides are used for single photon generation. The kinds of entanglement generated include polarization, time-energy, time-bin, and orbital angular momentum. The key ingredient for photon pair generation in nonlinear processes is described and discussed. Besides, we also introduce quantum frequency conversion for converting a single photon from one wavelength to another wavelength, while keeping its quantum properties unchanged. Finally, we give a comprehensive conclusion and discussion about future perspectives for single photon generation and manipulation in nonlinear processes. This chapter will provide an overview about the status, current challenge, and future perspectives about single photon generation and processing in nonlinear processes.
The time-frequency degree of freedom is a powerful resource for implementing high-dimensional quantum information processing. In particular, field-orthogonal pulsed temporal modes offer a flexible framework compatible with both long-distance fibre networks and integrated waveguide devices. In order for this architecture to be fully utilised, techniques to reliably generate diverse quantum states of light and accurately measure complex temporal waveforms must be developed. To this end, nonlinear processes mediated by spectrally shaped pump pulses in group-velocity engineered waveguides and crystals provide a capable toolbox. In this review, we examine how tailoring the phasematching conditions of parametric downconversion and sum-frequency generation allows for highly pure single-photon generation, flexible temporal-mode entanglement, and accurate measurement of time-frequency photon states. We provide an overview of experimental progress towards these goals, and summarise challenges that remain in the field.
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.
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.
Ultrashort light pulses play an important role in the generation, manipulation and characterization of nonclassical light. Nonclassical light is often generated from a classical pump beam using a nonlinear optical process. One might expect that the high peak intensity of ultrashort pulses would provide the necessary driver for such processes, and this is indeed the case. Ultrashort pulses have been used to generate squeezed states, and quadrature entangled states via three and four wave mixing, photon number states, polarization and frequency or directional entangled photon pairs states via three wave mixing.
This thesis presents a study of photon generation and conversion processes in nonlinear optics. Our results extend beyond the first order perturbative regime, in which only pairs of photons are generated in spontaneous parametric down-conversion or four wave mixing. They also allow us to identify the limiting factors for achieving unit efficiency frequency conversion, and to correctly account for the propagation of bright nonclassical photon states generated in the nonlinear material. This is done using the Magnus expansion, which allows us to incorporate corrections due to time-ordering effects in the time evolution of the state, while also respecting the quantum statistics associated with squeezed states (in photon generation) and single photons or coherent states (in photon conversion). We show more generally that this expansion should be the preferred strategy when dealing with any type of time-dependent Hamiltonian that is a quadratic form in the creation and annihilation operators of the fields involved. Using the Magnus expansion, simple figures of merit to estimate the relevance of these time-ordering corrections are obtained. These quantities depend on the group velocities of the modes involved in the nonlinear process and provide a very simple physical picture of the interactions between the photons at different times. These time-ordering effects are shown to be important only when the photons and pump beam overlap within the nonlinear material for a significant amount of time. We also discuss the possibility of preparing Fock states with many photons using parametric down-conversion sources and realistic photon-number-resolving detectors. After discussing photon generation processes, we study photon conversion processes in which a nonlinear material and a classical strong pump field are used modify the frequency of a second incoming low-intensity field. We show that time-ordering effects limit the efficiency of this conversion process, re-examine strategies to get around this problem, and show that it should be possible to have a clear observation of modified upconversion probabilities due to these effects, and thus have an experimental demonstration of time-ordering effects in nonlinear optics.