The aim of this thesis is to explore nonlinear nanostructures – photonic systems with one or more dimension with nanoscale feature size – as new platforms for parametric photon-pair generation. This is motivated by the need for photon-pair sources in many technological applications of quantum optics, such as quantum communication, imaging and computing. The initial hypothesis is that nonlinear nanostructures are a promising platform to complement established photon-pair source schemes based on bulk crystals or photonic integrated circuits in terms of quantum state-engineering, footprint, functional density etc. However, nonlinear pair generation, e.g. via spontaneous parametric down-conversion (SPDC), is a new subfield in nanophotonics with a very limited number of studies existing. This constitutes the knowledge-gap addressed in this thesis. Therefore, the objective is to provide first experimental demonstrations of SPDC in subwavelength-scale and nonlinear nanostructures. We investigate the ability of such systems to control the properties of two-photon quantum states such as frequency and angular spectrum or polarization entanglement. To this end we analyze nanostructures with different degrees of complexity, starting with an unstructured thin crystal with one nanoscale dimension, leading up to a 3D nano-scale resonator with subwavelength-sized features in all dimensions. Furthermore, we test different types of nonlinear materials such as lithium niobate, group III-V semiconductors and emerging, highly nonlinear materials such as molybdenum disulfide. Additionally, we also advance the theoretical understanding by developing a comprehensive model of the quantum process of nonlinear parametric pair-generation in photonic nanostructures.
The aim of this thesis is to explore nonlinear nanostructures – photonic systems with one or more dimension with nanoscale feature size – as new platforms for parametric photon-pair generation. This is motivated by the need for photon-pair sources in many technological applications of quantum optics, such as quantum communication, imaging and computing. The initial hypothesis is that nonlinear nanostructures are a promising platform to complement established photon-pair source schemes based on bulk crystals or photonic integrated circuits in terms of quantum state-engineering, footprint, functional density etc. However, nonlinear pair generation, e.g. via spontaneous parametric down-conversion (SPDC), is a new subfield in nanophotonics with a very limited number of studies existing. This constitutes the knowledge-gap addressed in this thesis. Therefore, the objective is to provide first experimental demonstrations of SPDC in subwavelength-scale and nonlinear nanostructures. We investigate the ability of such systems to control the properties of two-photon quantum states such as frequency and angular spectrum or polarization entanglement. To this end we analyze nanostructures with different degrees of complexity, starting with an unstructured thin crystal with one nanoscale dimension, leading up to a 3D nano-scale resonator with subwavelength-sized features in all dimensions. Furthermore, we test different types of nonlinear materials such as lithium niobate, group III-V semiconductors and emerging, highly nonlinear materials such as molybdenum disulfide. Additionally, we also advance the theoretical understanding by developing a comprehensive model of the quantum process of nonlinear parametric pair-generation in photonic nanostructures.
There is a growing belief that we are currently in the midst of a Second Quantum Revolution. More and more quantum technologies, such as communication, computing, and imaging, are moving from academic exploration to practical industrial applications. These technologies often depend on entangled photons, and their increasing use requires the development of novel quantum light sources that are compact, versatile, and integrable into modern photonic systems. Additionally, the trend toward miniaturization and nano-optics is accelerating, driven by rapid advances in nanofabrication. Therefore, there is an urgent need to create new classes of miniaturized and tunable two-photon sources. This thesis is dedicated to the theoretical investigation and experimental demonstration of miniaturized sources of entangled photons based on spontaneous parametric down-conversion in thin nonlinear films. It focuses not only on traditional crystalline materials but also on the emerging platform of liquid crystals, marking the first-ever demonstration of photon-pair generation in a liquid crystal within this thesis. A significant achievement is the ability to relax phase-matching constraints in ultra-thin nonlinear layers, allowing the full utilization of the nonlinear tensor and enhancing the variety of possible entangled two-photon states. Several aspects of two-photon state engineering with relaxed phase-matching are discussed in the thesis. First, this relaxation facilitates the switching between different polarization two-photon states, with a varying degree of polarization entanglement and the ability to generate non-maximally entangled states. In terms of spectral properties, miniaturized two-photon sources generate exceptionally broad two-photon frequency spectra, leading to a high degree of frequency entanglement and an unprecedented number of frequency modes, which also leads to ultra-narrow time correlations. By considering the effects of Fabry-Perot resonances, it becomes possible to engineer the two-photon spectra and even achieve backward emission of photon pairs. Remarkably, the Fabry-Perot effect can be accurately described by a simple modification of the rigorous quantum theory, providing a powerful predictive tool for photon pair generation in advanced nanostructures, metasurfaces, and nonlinear nano-antennas when properly applied. Another central contribution of this work is the introduction of liquid crystals as tunable nonlinear media for photon pair generation. Controlling the molecular orientation through a static twist or applying an external electric field makes it possible to tune the generated two-photon states dynamically. A theoretical model of this process, verified through direct experimental measurements, predicts quasi-phase-matching-like behavior and enhanced conversion efficiency, which can be utilized to develop exceptionally tunable and integrable sources of photon pairs and squeezed light. Finally, a fundamental challenge addressed in this thesis is mitigating a parasitic photoluminescent background. This study demonstrates a two-order-of-magnitude reduction in photoluminescence-induced contamination of photon pairs generated from thin nonlinear films by switching from the commonly used continuous-wave regime to the pulsed regime and performing time-resolved distillation. It also shows a developed theory that relates measured experimental parameters to the intrinsic purity of the two-photon state. Overall, this thesis advances the quantum micro- and nano-photonics field by providing a deeper understanding and enhanced control over photon pair generation in thin nonlinear films. It bridges theoretical insights with experimental realizations and paves the way toward practical, tunable, and highly integrated quantum light sources.
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.
Tunable photonic quantum entanglement promises to advance information processing beyond classical approaches, facilitating applications in quantum communications, imaging and computing. A practical approach to preparing quantum entanglement at room temperature is to engineer photon-pair generation through spontaneous parametric down-conversion (SPDC). Nonlinear flat-optics devices, incorporating subwavelength-thick nonlinear materials, are emerging as new platforms for generating photon pairs at the nanoscale. In particular, nanostructured metasurfaces supporting optical resonances can enhance and tailor SPDC processes, allowing for the generation of spectral, polarization, and spatial entanglement [1]. However, the tunability of polarization entanglement is subject to the symmetry of nonlinear tensors of materials, where the pump photon polarization serves as the only tuning parameter [2].
The recent advent of optical metasurfaces, ultra-thin structures composed of nanoresonators facilitating strong light concentration [1–3], opens the path towards efficient \nfrequency conversion [4–7] in a material thousand times thinner than a human hair [8]. \nThere is a remarkable capacity to individually shape each nanoresonator of the metasurface to spatially and spectrally control the conversion process with unprecedented \nnanoscale resolution, facilitating an ultimate flexibility to selectively convert, focus, \nand image different colours with a single metasurface. The strong enhancement of the \nnonlinear processes in dielectric nanoresonators is largely due to the absence of material \nabsorption and the excitation of Mie-type bulk resonances [2]. The highest conversion \nefficiency to date has been achieved employing III-V semiconductor nanostructures, \nsuch as AlGaAs which is a non-centrosymmetric material with high quadratic nonlinear \nsusceptibility. In particular, second-harmonic generation efficiencies up to 10−4 have \nbeen recently demonstrated [8–12], six orders of magnitude higher than in plasmonics. \nSuch capabilities can make an immense fundamental and practical impact, including \nthe quantum state generation in nonlinear metasurfaces as we discuss in this chapter. \nThe quantum state of correlated photon-pairs is the essential building block for photon entanglement [13, 14], which underpins many quantum applications, including secure networks, enhanced measurement and lithography, and quantum information processing [15]. One of the most versatile techniques for the generation of correlated photons is the process of spontaneous parametric down-conversion (SPDC) [16, 17], see \nFig. 1. It allows for an arbitrary choice of energy and momentum correlations between \nthe generated photons, robust operation at room temperature, as well as for spatial and \ntemporal coherence between simultaneously pumped multiple SPDC sources. Alternative approaches based on atom-like single photon emitters, such as solid-state fluorescent atomic defects [18], quantum dots [19, 20], and 2D host materials [21, 22], have \nreached a high degree of frequency indistinguishability, purity and brightness [19, 20]. \nHowever, this comes with the expense of operation at cryogenic temperatures and lack \nof spatial coherence between multiple quantum emitters. These features might limit \npossible applications and reduce the potential for device scalability. Furthermore, the \nsmall size of the atomic sources often requires complex schemes aimed at coupling to \noptical nanoantennas and improving the photon extraction efficiency [21]. \nThe miniaturization of SPDC quantum-light sources to micro and nanoscale dimensions is a continuing quest, as it enables denser integration of functional quantum \ndevices. Traditionally, bulky cm-sized crystals were utilized for SPDC, entailing the \ndifficulty of aligning multiple optical elements after the SPDC crystal, while offering \nrelatively low photon-pair rates [17]. As a first step of miniaturization, SPDC was \nrealized in low-index-contrast waveguides, which allowed confining light down to several square micrometers transversely to the propagation direction, significantly enhancing the conversion efficiency [23]. However, this approach still requires centimetres \nof propagation length, which makes the on-chip integration with other elements challenging [24]. The introduction of high-index contrast waveguides and ring resonators \nallowed for shrinking the sizes necessary for SPDC to millimetres [25], and to tens \nof micrometers [26]. However, further miniaturisation down to the metasurfaces composed of nanoresonators requires conceptually different approaches.
Spontaneous parametric down-conversion (SPDC) in subwavelength nanostructures is a promising source of quantum light, owing to its multifunctionality and ability to generate complex quantum states. Nevertheless, the mechanisms governing photon-pair generation in such systems remain only partially understood. In particular, experimental investigations of key emission properties in individual resonators, such as directionality and spectral distribution, are still lacking, and predictive theoretical frameworks have not yet been experimentally validated. Here, we report the first measurement of the directional and spectral distributions of photon pairs generated via SPDC in a nanostructured resonator. Both distributions exhibit resonant behaviour, which we describe using an extended quasi-normal-mode theory. This comparison is enabled by photon-pair count rates of up to 0.45 Hz/mW -- to our knowledge, the highest reported for a nanostructured resonator. Our results provide new physical insight into nanoscale SPDC and represent an important step toward designing of efficient miniaturized quantum light sources.
Entangled photon-pairs generated through spontaneous parametric down-conversion (SPDC) have evolved into an indispensable resource for various quantum communication, imaging, sensing and computing schemes. While photon-pair sources are so far mostly based on bulk-optical nonlinear components, resonant nonlinear metasurfaces with sub-wavelength thickness have recently been demonstrated as a new platform for photon-pair generation [1]–[3]. Contrary to bulk and integrated nonlinear structures where phase matching steers the pair generation efficiency in different directions and wavelengths, nanostructures can control these properties via their optical resonances. However, the tunability of spatial photon emission in multiple directions remained an open challenge.