Ultracompact nonlinear optical devices utilizing two-dimensional (2D) materials and nanostructures are emerging as important elements of photonic circuits. Integration of the nonlinear material into a subwavelength cavity or waveguide leads to a strong Purcell enhancement of the nonlinear processes and compensates for a small interaction volume. The generic feature of such devices which makes them especially challenging for analysis is strong dissipation of both the nonlinear polarization and highly confined modes of a subwavelength cavity. Here we solve a quantum-electrodynamic problem of the spontaneous and stimulated parametric down-conversion in a nonlinear quasi-2D waveguide or cavity. We develop a rigorous Heisenberg-Langevin approach which includes dissipation and fluctuations in the electron ensemble and in the electromagnetic field of a cavity on equal footing. Within a relatively simple model, we take into account the nonlinear coupling of the quantized cavity modes, their interaction with a dissipative reservoir and the outside world, amplification of thermal noise and zero-point fluctuations of the electromagnetic field, and other relevant effects. We derive closed-form analytic results for relevant quantities such as the spontaneous parametric signal power and the threshold for parametric instability. We find a strong reduction in the parametric instability threshold for 2D nonlinear materials in a subwavelength cavity and provide a comparison with conventional nonlinear photonic devices.
Ultracompact nonlinear optical devices utilizing two-dimensional (2D) materials and nanostructures are emerging as important elements of photonic circuits. Integration of the nonlinear material into a subwavelength cavity or waveguide leads to a strong Purcell enhancement of the nonlinear processes and compensates for a small interaction volume. The generic feature of such devices which makes them especially challenging for analysis is strong dissipation of both the nonlinear polarization and highly confined modes of a subwavelength cavity. Here we solve a quantum-electrodynamic problem of the spontaneous and stimulated parametric down-conversion in a nonlinear quasi-2D waveguide or cavity. We develop a rigorous Heisenberg-Langevin approach which includes dissipation and fluctuations in the electron ensemble and in the electromagnetic field of a cavity on equal footing. Within a relatively simple model, we take into account the nonlinear coupling of the quantized cavity modes, their interaction with a dissipative reservoir and the outside world, amplification of thermal noise and zero-point fluctuations of the electromagnetic field, and other relevant effects. We derive closed-form analytic results for relevant quantities such as the spontaneous parametric signal power and the threshold for parametric instability. We find a strong reduction in the parametric instability threshold for 2D nonlinear materials in a subwavelength cavity and provide a comparison with conventional nonlinear photonic devices.
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.
Miniaturization of nonlinear optical elements is one of the major trends of modern photonics. In particular, in the ‘flatoptics’ geometry, the sample is ultrathin along the light propagation direction. For nonlinear optical effects in such samples, phase matching is satisfied automatically, which allows for the use of materials with giant nonlinear susceptibilities. The tiny thickness reduces the efficiency but it can be compensated for by using geometric and material resonances. Recently also spontaneous parametric down-conversion (SPDC), leading to the generation of entangled photons, has been implemented in ultrasmall sources: subwavelength layers, metasurfaces, even nanoantennas. The lifted constraint of phase matching gives to SPDC even more freedom than to classical frequency conversion effects. The reason is that SPDC, as a spontaneous effect, is stimulated by quantum vacuum fluctuations, which populate all modes uniformly. SPDC in ultrathin samples demonstrates very broad spectral and angular width, extremely high degrees of continuous-variable entanglement, tunable polarization entanglement, and orders of magnitude enhancement of photon pair production rate due to the geometric resonances of dielectric metasurfaces.
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.
Abstract Among the most prominent effects resulting from nonlinear light–matter interaction is the generation of correlated and entangled photons through various processes, notably via spontaneous parametric down‐conversion or spontaneous four‐wave mixing. Such nonlinear optical processes benefit from the concentration of electromagnetic fields in small volumes. Dielectric nanoresonators and their 2D layouts—metasurfaces—provide efficient ways to control light in subwavelength volumes enabling the enhancement of nonlinear light–matter interaction and the generation of entangled photons. Nanoresonators and metasurfaces offer a radical miniaturization of quantum light sources allowing better scalability, which opens a pathway toward arrangements of photon sources in complex subwavelength configurations for advanced photon state control. In this work, the recent progress in this emergent area of research is reviewed.
Strong light-induced interactions between atoms are known to cause nonlinearities at a few-photon level, which are crucial for applications in quantum information processing. Compared to free space, the scattering and the light-induced dipolar interaction of atoms can be enhanced by a dielectric environment. For this Purcell effect, either a cavity or a waveguide can be used. Here, we combine the high densities achievable in thermal atomic vapors with an efficient coupling to a slot waveguide. In contrast to free-space interactions, atoms aligned within the slot exhibit repulsive interactions that are further enhanced by a factor of 8 due to the Purcell effect. The corresponding blueshift of the transition frequency of atoms arranged in the essentially one-dimensional geometry vanishes above the saturation, providing a controllable nonlinearity at the few-photon level. The experimental results are in good agreement with Monte Carlo simulations that include the dielectric environment, dipolar interactions, and motional effects. The results pave the way towards a robust scalable platform for quantum nonlinear optics and all-optical quantum information processing at room temperature.