The generation of entangled photons by spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM) attracted enormous interest in the field of quantum optics. Depending on applications, entangled photon sources prioritize either bandwidth (e.g. for quantum imaging) or brightness (e.g. for quantum key distribution). Layered materials offer unique advantages for both. They have already been used to realize thinnest SPDC sources [1], which, like other layered materials such as transition-metal dichalcogenides (TMDs) [2], offer nearly unlimited bandwidth thanks to relaxed phase-matching constraints. Further, their easy integration on photonic platforms is promising for bright on-chip entangled photon sources. In this context, SPDC-based solutions are limited by phase-matching, whereas SFWM would be an almost phase-matching-free process, as pump, idler, and signal photons can be generated at similar wavelengths, thus propagating at the same group velocity in integrated devices. Moreover, exploiting excitonic resonances could enhance FWM even more. However, to date, experiments with resonant FWM in TMDs have been limited to signals in the visible [3], which is unsuitable for integrated photonics and telecom systems due to reabsorption during propagation in the photonic device.
The generation of entangled photons by spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM) attracted enormous interest in the field of quantum optics. Depending on applications, entangled photon sources prioritize either bandwidth (e.g. for quantum imaging) or brightness (e.g. for quantum key distribution). Layered materials offer unique advantages for both. They have already been used to realize thinnest SPDC sources [1], which, like other layered materials such as transition-metal dichalcogenides (TMDs) [2], offer nearly unlimited bandwidth thanks to relaxed phase-matching constraints. Further, their easy integration on photonic platforms is promising for bright on-chip entangled photon sources. In this context, SPDC-based solutions are limited by phase-matching, whereas SFWM would be an almost phase-matching-free process, as pump, idler, and signal photons can be generated at similar wavelengths, thus propagating at the same group velocity in integrated devices. Moreover, exploiting excitonic resonances could enhance FWM even more. However, to date, experiments with resonant FWM in TMDs have been limited to signals in the visible [3], which is unsuitable for integrated photonics and telecom systems due to reabsorption during propagation in the photonic device.
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.
Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests 'flat' platforms - ultrathin layers and metasurfaces - as sources of photon pairs. With the success in demonstrating spontaneous parametric down-conversion (SPDC) from such sources, an alternative process to generate photon pairs, spontaneous four-wave mixing (SFWM), also starts to attract interest. In materials with nonzero second-order nonlinear susceptibility χ(2), SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ(3), and in a cascaded way, through second harmonic generation (SHG) followed by SPDC. Usually, the cascaded process is more efficient. Here, we show that in a thin layer, direct SFWM dominates, because the wavevector mismatch for SFWM is much smaller than for SHG or SPDC. To demonstrate it, we implement the photon pair generation via SFWM in a second-order nonlinear material - a thin layer of lithium niobate (LN). The existence of both second- and third-order nonlinear processes offers broader opportunities for quantum state engineering.
Transition metal dichalcogenides (TMDCs) thinned-down to the monolayer level allow the realisation of very broad-band, phase-matching free nonlinear devices. A particularly interesting application would be the generation of entangled photon-pairs, which form the backbone of many recent implementations in quantum optics. However, the limited absolute efficiency of monolayers has so far only allowed seeded parametric amplification [1], experimental evidence for the generation of entangled photon-pairs through spontaneous parametric down-conversion (SPDC) remained elusive up to now [2]. A promising route for the realization of broad-band photon-pair sources in van der Waals materials are moderately thicker, yet still phase-matching free layer stacks with preserved noncentrosymmetry [3], [4]. Here, we close the gap of a missing entangled photon-pair source in TMDCs and demonstrate, for the first time to our knowledge, pair generation via SPDC in 3R-MoS2.
Generation of entangled photon pairs at telecom wavelength has been garnering a growing interest in the context of quantum communications and quantum computing. Several generation techniques have been proposed, including spontaneous Four-Wave Mixing in resonators or Spontaneous Parametric Down Conversion (SPDC) in Periodically Polled Lithium Niobate (PPLN) waveguides. Large photon pair efficiencies have been demonstrated in particular in PPLN on insulator [3]. However, polarization entangled photon pair generation (Type II phase matching configuration) suffers from a less favourable non-linear coefficient and optical mode birefringence in PPLN.
The efficient and controllable generation of entangled photon pairs is a cornerstone for advancing quantum technologies, including quantum computing, communication, and sensing. Traditional methods, primarily relying on spontaneous parametric down-conversion (SPDC) or spontaneous four-wave mixing (SFWM) in bulk nonlinear crystals or waveguides, often suffer from low efficiency, bulky form factors, and limited control over the spectral and spatial properties of the generated photons. This paper explores a transformative approach leveraging resonant Bound States in the Continuum (BICs) within nanophotonic structures to overcome these limitations. BICs are extraordinary optical resonances characterized by theoretically infinite quality (Q) factors, enabling extreme light localization and immense field enhancement within subwavelength volumes. By integrating nonlinear optical materials into BIC-supporting structures, such as photonic crystal slabs or metasurfaces, the local electric field strength experienced by the nonlinear medium can be dramatically increased, boosting the efficiency of entangled photon generation. Furthermore, the sharp, tailor-able spectral response of BICs offers unprecedented control over the joint spectral amplitude of the photon pairs, promising high degrees of spectral purity and entanglement fidelity. This work outlines the theoretical underpinnings, potential device architectures, and anticipated advantages of BIC-enhanced entangled photon sources, paving the way for compact, high-brightness, and spectrally engineered quantum light sources critical for next-generation quantum technologies.
Pairs of entangled photons are crucial for photonic quantum technologies. The demand for integrability and multi-functionality suggests “flat” platforms—ultrathin layers and metasurfaces—as sources of photon pairs. With the success in demonstrating spontaneous parametric down-conversion (SPDC) from such sources, an alternative process to generate photon pairs, spontaneous four-wave mixing (SFWM), also attracts interest. In materials with nonzero second-order nonlinear susceptibility χ (2) , SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ (3) , and in a cascaded way, through second harmonic generation (SHG) followed by SPDC. Usually, the cascaded process is more efficient. Here, we show that in a thin layer, direct SFWM is likely to dominate, because the wavevector mismatch for SFWM is much smaller than for SHG or SPDC. To demonstrate this, we implement photon pair generation via SFWM in a second-order nonlinear material—a thin layer of lithium niobate (LN). The existence of both second- and third-order nonlinear processes offers broader opportunities for quantum state engineering.