The generation of engineered quantum states of light via nonlinear processes is fundamental for quantum technologies based on photons. Although embedding nonlinear materials within resonant structures allows for the enhancement and tailoring of photon properties, accurately modeling these quantum interactions remains a challenge. In this work, we apply the asymptotic-fields formalism, an approach based on scattering theory, to describe nonlinear optical processes within a Fabry-Pérot cavity. Unlike previous applications of this formalism, we explicitly account for reflections in the system. We derive the interaction Hamiltonian and calculate photon-pair generation rates using perturbation theory. The versatility of this model is illustrated through three examples: (i) spontaneous parametric down-conversion in an idealized cavity with flat-response mirrors; (ii) the generation of counter-propagating photon pairs in a periodically-poled material; and (iii) spontaneous four-wave mixing in a cavity built with Bragg reflectors.
The generation of engineered quantum states of light via nonlinear processes is fundamental for quantum technologies based on photons. Although embedding nonlinear materials within resonant structures allows for the enhancement and tailoring of photon properties, accurately modeling these quantum interactions remains a challenge. In this work, we apply the asymptotic-fields formalism, an approach based on scattering theory, to describe nonlinear optical processes within a Fabry-Pérot cavity. Unlike previous applications of this formalism, we explicitly account for reflections in the system. We derive the interaction Hamiltonian and calculate photon-pair generation rates using perturbation theory. The versatility of this model is illustrated through three examples: (i) spontaneous parametric down-conversion in an idealized cavity with flat-response mirrors; (ii) the generation of counter-propagating photon pairs in a periodically-poled material; and (iii) spontaneous four-wave mixing in a cavity built with Bragg reflectors.
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 underpins quantum photonics by enabling the generation and control of quantum states of light. We present new applications of optical resonators as mode selectors in nonlinear processes. First, we show that cavity-enhanced spontaneous parametric down-conversion can generate spectrally uncorrelated photon pairs with improved decorrelation and wavelength flexibility. Second, we demonstrate that a cavity-assisted sum-frequency generation process realizes a quantum pulse gate with high-resolution temporal-mode selectivity and precise spectral control. Our theoretical framework provides a general methodology for analyzing cavity-enhanced nonlinear processes and highlights the versatility of optical resonators as powerful tools for engineering quantum light.
The ability to generate quantum entangled photon pairs through spontaneous parametric down conversion (SPDC) is playing a pivotal role in many applications in quantum technologies, including quantum communications, quantum computation, and quantum imaging. Metasurfaces, two-dimensional arrays of nanostructures with subwavelength thickness, have recently shown extraordinary capability in manipulating classical and quantum states of light and realizing miniaturized SPDC sources. Whereas previous studies have primarily focused on periodic metasurfaces, we uncover the potential of spatially modulated nanopatterns for further SPDC enhancement and state engineering. Specifically, we propose a nonlinear metasurface featuring a lateral guided-mode cavity formed by two distributed Bragg reflectors. With the quasi-normal mode theory, we predict an SPDC rate up to 157 Hz/mW, which represents about 30 times rate enhancement when compared to the metasurface without a cavity. Furthermore, the cavity supports a continuous set of high-Q resonances across a broad bandwidth, allowing the all-optical tuning of the photon-pair emission directions transverse to the cavity by controlling the pump wavelength, which can find applications in quantum imaging.
Entangled photons have acted as a workhorse in many quantum technologies, including cryptography, imaging, sensing, and computation. With the growing demands of quantum technology, the entangled photon pair sources are required to be compact and integrable. For the last few years, the field of quantum optics in the nanoscale has demonstrated photon pair generation in ’flat’ optics such as thin layers, Van der Waals crystals, micro-, nano-antennas, and metasurfaces. The word ’flat’ is used because such optical platforms have sub-wavelength thicknesses. Due to the short travel length inside the sources, they can possess multiple functions that their bulky counterparts cannot have. This doctoral thesis addresses photon pair generation in ’flat’ optics via second- and third-order nonlinear processes, which are spontaneous parametric down-conversion (SPDC) and spontaneous four-wave mixing (SFWM). The main aims of the thesis are to understand how the photon pair generation is realized via SPDC and SFWM on subwavelength-scale platforms, and to make a bridge between photon pair generation via two nonlinear processes under the presence of optical resonances. The thesis covers two experimental parts related to SPDC and SFWM, and one future expectation of the SFWM in metamaterials. The first part of the thesis addresses one of the multi-functionalities that has recently been reported: the emission direction control of the photon pairs. A 150 nm-thick gallium phosphide (GaP) metasurface is used as a source. The metasurface supports a quasi-bound state in the continuum (quasi-BIC) resonance, enhancing the electric field inside the material. I generate the entangled photons through the SPDC process. The generated photons are in two different wavelengths under the given pump wavelength: signal photon at the resonance, and idler photon out of the resonance. The photon pair generation rate is enhanced by 66 times compared to the unpatterned GaP slab since the vacuum field in the signal mode is enhanced by the resonance. The generated photons obey the transmission spectrum of the metasurface. As a result, the signal photons at resonance are mostly reflected, and the idler photons are transmitted after generation. This result is the first work of photon demultiplexing by a metasurface. The second part of the thesis covers the photon pair generation through SFWM in thin nonlinear films. Silicon-rich silicon nitride (SiN) layers are selected as the sources. The layers have an intriguing characteristic that the third-order nonlinear susceptibility (chi-3) differs with the nitrogen doping rate. I generate the photon pairs through chi-3 variant SiN layers. The thicknesses of the samples are all sub-wavelength level, having a few hundred nanometers. Time-energy correlation measurements are conducted for all samples, and the second-order correlation functions (g(2)(0)) are calculated. The maximum g(2)(0) of the samples exceeds 2. Interestingly, I observed two-photon interference effects between photon pairs generated in the layers and the fused-silica substrate, which allows me to estimate the chi-3 values of the samples by knowing the reference: chi-3 value of the substrate. The last part of the thesis introduces designs of metasurfaces and possible experimental schemes for photon pair generation through SFWM. Yet, due to its weak light-matter interaction in third-order nonlinear processes, the photon pair generation through SFWM has not been observed in metasurfaces. However, it is fairly possible to enhance the vacuum fields at the output photon modes and generate photon pairs because preliminary work in unpatterned slabs has already been observed in this thesis. Finally, I introduce a fabricated metasurface. It needs improvements, but it is quite promising for the ongoing project.
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.
We present a simple quantum-field model for photon frequency conversion processes in dispersive dielectric microcavities, allowing practical calculations of conversion rates and efficiency optimization. The model incorporates the effect of dispersion into the structure of spatial cavity eigenmodes, while the material nonlinear properties enter the calculations through the coupling coefficients. Similar to the radiative atomic transitions, cavity photon-to-photon decay rates are derived for stimulated and spontaneous photon conversion. The phase matching requirement for a nonlinear process in a cavity is shown to be translated into a nonlinear mode overlap, manifesting the momentum conservation in a k space spanned by the cavity eigenmodes. We illustrate the efficiency of the model by calculating degenerate two-photon and three-photon parametric down-conversion rates and analyze the photon lifetime dependence on various cavity and material parameters.