Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constrains in device design and integration. In this paper, we show that the principles for spontaneous emission control (i.e. Purcell effect) of isolated emitters in nanoscale structures, such as metamaterials, can be generalized to describe the enhancement of nonlinear light generation processes such as parametric down conversion. We develop a novel theoretical framework for quantum nonlinear emission in a general anisotropic, dispersive and lossy media. We further find that spontaneous parametric downconversion in media with hyperbolic dispersion is broadband and phase-mismatch-free. We predict a 1000-fold enhancement of the downconverted emission rate with up to 105 photon pairs per second in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes, provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.
Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constrains in device design and integration. In this paper, we show that the principles for spontaneous emission control (i.e. Purcell effect) of isolated emitters in nanoscale structures, such as metamaterials, can be generalized to describe the enhancement of nonlinear light generation processes such as parametric down conversion. We develop a novel theoretical framework for quantum nonlinear emission in a general anisotropic, dispersive and lossy media. We further find that spontaneous parametric downconversion in media with hyperbolic dispersion is broadband and phase-mismatch-free. We predict a 1000-fold enhancement of the downconverted emission rate with up to 105 photon pairs per second in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes, provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.
Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constraints in device design and integration. In this Letter, we study principles of spontaneous emission control (i.e., the Purcell effect) generalized to describe the enhancement of nonlinear generation of quantum light through spontaneous parametric downconversion. We develop a theoretical framework based on eigenmode analysis to study quantum nonlinear emission in a general anisotropic, dispersive, and lossy media. Our theory provides an unprecedented insight into the emission process. We find that spontaneous parametric downconversion in a media with hyperbolic dispersion is broadband and phase-mismatch-free. We further predict a significant enhancement of the downconverted emission rate in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.
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 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.
) crystal to realize a new scalable, ultrathin, and efficient SPDC source. By coinciding fundamental and higher order resonances of the metasurface with the generated signal and idler frequencies, respectively, the electric field in the nonlinear media is significantly boosted. This leads to a substantial enhancement in the SPDC process which, subsequently, by using the quantum-classical correspondence principle, translates to very high photon-pair generation rates. The emitted radiation is highly directional and perpendicular to the metasurface in contrast to relevant dielectric structures. The incorporation of circular polarized excitation further increases the photon-pair generation efficiency. The presented work will lead to the design of new efficient ultrathin SPDC single-photon nanophotonic sources working at room temperature that are expected to be critical components in free-space quantum optical communications. In a more general context, our findings can have various applications in the emerging field of quantum plasmonics.