This chapter begins by reviewing the semi-classical theory of weakly nonlinear optics, in which the atomic polarization is a power series in the field amplitude. After replacing the classical amplitudes by field operators, the expansion for the classical electromagnetic energy becomes the Hamiltonian. The third- and fourth-order classical terms (respectively representing three- and four-wave mixing) become three- and four-photon interaction terms. The three-photon terms describe sum-frequency generation and spontaneous down conversion. Down conversion is the principal modern source of entangled photons pairs. It has also been applied to yield absolute measurements of the quantum efficiency of detectors and as a source of hyper-entangled photons. The four-photon interaction terms describe frequency tripling, three-photon down conversion, and photon-photon scattering. The description of an experimental demonstration of photon-photon scattering in a rubidium vapor is followed by a discussion of Kerr media.
This chapter begins by reviewing the semi-classical theory of weakly nonlinear optics, in which the atomic polarization is a power series in the field amplitude. After replacing the classical amplitudes by field operators, the expansion for the classical electromagnetic energy becomes the Hamiltonian. The third- and fourth-order classical terms (respectively representing three- and four-wave mixing) become three- and four-photon interaction terms. The three-photon terms describe sum-frequency generation and spontaneous down conversion. Down conversion is the principal modern source of entangled photons pairs. It has also been applied to yield absolute measurements of the quantum efficiency of detectors and as a source of hyper-entangled photons. The four-photon interaction terms describe frequency tripling, three-photon down conversion, and photon-photon scattering. The description of an experimental demonstration of photon-photon scattering in a rubidium vapor is followed by a discussion of Kerr media.
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.
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.
This thesis presents an analysis of photon pairs generated via either spontaneous parametric downconversion or spontaneous four-wave mixing in channel waveguides as well as in microring resonators side-coupled to channel waveguides. The state of photons exiting a particular device is calculated within a general Hamiltonian formalism that simplifies the link between quantum nonlinear optics experiments and classical nonlinear optics experiments. This state contains information regarding photon pair production efficiency as well as modal and spectral correlations between the two photons, characterized by a two-dimensional spectral distribution function called the biphoton wave function.\n\nIn the limit of a low probability of pair production, photon pair production fficiencies are cast into forms resembling corresponding well-known classical nonlinear optical frequency conversion efficiencies, making it easy to see what plays the role of a classical “seed” field in an un-seeded (quantum) process. This also allows photon pair production efficiencies to be calculated based on the results of classical nonlinear optical experiments. It is further calculated that, unless enerated photons are collected over a very narrow frequency range, their generation efficiency does not scale the same way with device length in a channel waveguide, or resonance quality factor in a microring resonator, as might be expected from the corresponding classical frequency conversion efficiency. Although calculations do not include self- or cross-phase modulation, nor two-photon absorption\nor free-carrier absorption, it is calculated that their neglect is justified in the low pair production probability limit. Linear (scattering) loss is also neglected, though partially addressed in the final chapter of this thesis.\n\nBiphoton wave functions are calculated explicitly, such that their shape and orientation, including approximate analytic expressions for their widths, can easily be determined. This further allows estimation of the suitability of their associated photon pairs for various quantum information processing applications. As an alternative to dispersion engineering a channel waveguide photon pair source, it is calculated that microring resonators can very naturally produce nearly spectrally uncorrelated photon pairs, which behave very much like idealized single-mode photons and are thus useful for applications involving the interference of photons from multiple sources.
Nonlinear optics is the study of the response of dielectric media to strong optical fields. The fields are sufficiently strong that the response of the medium is, as its name implies, nonlinear. That is, the polarization, which is the dipole moment per unit volume in the medium, is not a linear function of the applied electric field. In the equation for the polarization, there is a linear term, but, in addition, there are terms containing higher powers of the electric field. This leads to significant new types of behavior, one of the most notable being that frequencies different from that of the incident electromagnetic wave, such as harmonics or subharmonics, can be generated. Linear media do not change the frequency of light incident upon them. The first observation of a nonlinear optical effect was, in fact, second-harmonic generation – a laser beam entering a nonlinear medium produced a second beam at twice the frequency of the original. Another type of behavior that becomes possible in nonlinear media is that the index of refraction, rather than being a constant, is a function of the intensity of the light. For a light beam with a nonuniform intensity profile, this can lead to self-focusing of the beam. Most nonlinear optical effects can be described using classical electromagnetic fields, and, in fact, the initial theory of nonlinear optics was formulated assuming the fields were classical. When the fields are quantized, however, a number of new effects emerge. Quantized fields are necessary if we want to describe fields that originate from spontaneous emission. For example, in a process known as spontaneous parametric down-conversion, a beam of light at one frequency, the pump, produces a beam at half the original frequency, the signal. This second beam is a result of spontaneous emission.
In this chapter, we discuss a purely quantum approach to the interaction between an atom and the electromagnetic field. In this treatment, the atom and electromagnetic field form a single quantum system, whose evolution is handled globally within a unified formalism. This will thus have the merit of being fully consistent from the theoretical standpoint. But the main advantage in an entirely quantum approach is that it can treat the full range of matter–radiation interaction phenomena. In particular, it provides a rigorous description of the spontaneous emission of light by an excited atom , something that falls outside the scope of the semi-classical framework applied in Chapters 2 and 3, where the lifetime of an excited atomic state had to be fed in phenomenologically. It can describe other phenomena of the same type, such as parametric fluorescence by a nonlinear crystal subjected to pumping radiation (see Chapter 7), which underlies many recent developments in quantum optics. The fully quantum approach also has the merit of allowing a simple interpretation in terms of photons for the various matter–radiation interaction processes, such as absorption, stimulated emission, scattering, and also the basic processes of nonlinear optics. Indeed, it provides a unified framework for both stimulated and spontaneous processes. Finally, it can be used to tackle completely new situations where matter and radiation interact, which lie outside the scope of any semi-classical description, such as cavity quantum electrodynamics or the production of single-photon or entangled-photons states .