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.
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.
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.
This PhD thesis treats applications of nonlinear optical effects for quantum information processing. The two main applications are four-wave mixing in the form of Bragg scattering (BS) for quantum-state-preserving frequency conversion, and sum-frequency generation (SFG) in second-order nonlinear materials for heralded entanglement. BS is shown to be separable in the input and output modes in the low-conversion regime, the regime of small pump powers or short interaction times. The selective frequency conversion of a signal is found to only depend on one of the pumps, while the temporal output of the converted idler depends on the other pump. This allows for temporal-mode-multiplexing. When the effects of nonlinear phase modulation (NPM) are included, the phases of the natural input and output modes are changed, reducing the separability. These effects are to some degree mediated by pre-chirping the pumps. In the high-conversion regime without the effects of NPM, exact Green functions for BS are derived. In this limit, separability is possible for conversion efficiencies up to 60 %. However, the system still allows for selective frequency conversion as well as re-shaping of the output. One way to obtain a 100 % conversion efficiency is to use multiple stages of frequency conversion, but this setup suffers from the combined effects of NPM. This problem is circumvented by using asymmetrically pumped BS, where one pump is continuous wave. For this setup, NPM is found to only lead to linear phase shifts of the input and output modes, corresponding to shifts of the central frequencies of the fields. The trade-off is that one is only able to select which signals are converted, or change the shape of the output idler. Finally, entanglement swapping using SFG was investigated. Considering two pairs of entangled photons, the process of up-converting one photon from each pair leads to heralded entangled pairs by successful detection of the up-converted photon. It was seen that this was indeed possible in the case of anti-correlated phasematching in the up-conversion crystal. Possible ways of increasing the probability of an up-conversion event were investigated briefly.
We study time-ordering corrections to the description of spontaneous parametric down-conversion (SPDC), four-wave mixing (SFWM), and frequency conversion using the Magnus expansion. Analytic approximations to the evolution operator that are unitary are obtained. They are Gaussian preserving, and allow us to understand order-by-order the effects of time ordering. We show that the corrections due to time ordering vanish exactly if the phase-matching function is sufficiently broad. The calculation of the effects of time ordering on the joint spectral amplitude of the photons generated in SPDC and SFWM are reduced to quadrature.
We study the effects of time ordering in photon generation processes such as spontaneous parametric down-conversion (SPDC) and four wave mixing (SFWM). The results presented here are used to construct an intuitive picture that allows us to predict when time-ordering effects significantly modify the joint spectral amplitude (JSA) of the photons generated in SPDC and SFWM. These effects become important only when the photons being generated lie with the pump beam that travels through the nonlinear material for a significant amount of time. Thus sources of spectrally separable photons are ideal candidates for the observation of modifications of the JSA due to time ordering.
In this thesis I study in detail the quantum dynamics of several nonlinear optical processes in microresonator systems. A Heisenberg-picture input-output formalism is developed from first principles that includes the effects of scattering losses and independent quality factors and coupling ratios for different resonances. The task of calculating the device output is then reduced to solving a set of driven, damped, ordinary differential equations for the resonator mode operators alone. This theoretical framework is used to study photon pair generation via spontaneous four-wave mixing in the weakly pumped regime, on which the effects of scattering losses are appraised. A more strongly driven regime is studied for continuous wave pumps, demonstrating when self- and cross-phase modulation and multi-photon pair generation become important, and their effects on the spectral and power scaling properties of the system are examined; A detuning strategy is presented that compensates for some of these effects. The results of the weak-pump regime are applied to study microresonator-based her- alded single photon sources. The impact of scattering losses is studied, revealing that typical systems suffer from low heralding efficiency due to these losses. A technique to improve heralding efficiency is presented through over-coupling the resonator-channel system, and a resultant trade-off between heralding rate and heralding efficiency is un- covered. Limitations to the spectral purity of the heralded single photon output for conventional microresonator systems are also analysed, and a more sophisticated cou- pling scheme presented to overcome the upper bound for spectral purity of 93% that exists in typical systems, permitting the generation of single photons with spectral pu- rity arbitrarily close to 100% without spectral filtering or sophisticated phase-matching techniques. The theory of quantum frequency conversion in microresonators using four-wave mix- ing is then developed in detail, and the spectral conversion probability and conversion efficiency studied. Efficiencies exceeding 90% using less than 100 mW of pump power are predicted to be achievable with current technology. A dressed mode picture is developed to better understand the conversion dynamics. Rabi-like spectral splitting and temporal oscillations of the intraresonator mean photon number are predicted, exhibiting a novel regime of strongly coupled photonic modes.
Optical quantum computing, quantum information and quantum communication protocols rely on the generation of qubits encoded in optical systems, many of which can be generate via the process of spontaneous parametric down-conversion. In this thesis, we investigate down-converted states, in the context of quantum computing and quantum information. In the high gain regime, a type I down-converted state can be described as a single-mode squeezed vacuum state. We present an analysis of photon-subtracted squeezed vacuum states as a resource for teleportation of coherent state qubits and propose proof-of-principle experiments for the demonstration of coherent-state teleportation and entanglement swapping. In the low gain regime, the output state of a type II parametric down-converter can be approximated as containing pairs of single photons, which can be used to herald the presence of one- or two- photon Fock states in one mode, conditional on the detection of the same number of photons in the other mode. We explore the effects of spectral filtering and inefficient detection, of the heralding mode, on the count rate, g(2) and purity of the heralded state, as well as the fidelity between the resulting state and an ideal Fock state. We also develop a technique for controlling the joint spectral profile of the down-converted photons. By exploiting the dependence of the effective nonlinearity of a periodically poled crystal on its poling order, we tailor the nonlinearity profile and therefore the phase matching function of the down-converted photons. Finally, we consider the validity of the Taylor series expansion of the unitary operator which governs the evolution of the fields within the crystal, in comparison to the strictly correct time-ordered Dyson series expansion.