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.
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.
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.
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. Despite the success in the demonstration of spontaneous parametric down-conversion (SPDC) from such sources, there are almost no works on spontaneous four-wave mixing (SFWM) - an alternative process to generate photon pairs. Meanwhile, SFWM can be implemented in any nanostructures, including ones made of isotropic materials, which are easier to fabricate than crystalline SPDC sources. Here, we investigate photon pair generation through SFWM in subwavelength films of amorphous silicon nitride (SiN) with varying nitrogen content. For all samples, we demonstrate two-photon quantum correlations, indicated by the normalized second-order correlation function g(2)(0): it exceeds 2 and decays as the pump power increases. By observing two-photon interference between SFWM from the SiN films and the fused silica substrate, we find the third-order susceptibilities of films with different nitrogen content.
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. Despite the success in the demonstration of spontaneous parametric downconversion (SPDC) from such sources, there are almost no works on spontaneous four-wave mixing (SFWM)—an alternative process to generate photon pairs. Meanwhile, SFWM can be implemented in any nanostructures, including ones made of isotropic materials, which are easier to fabricate than crystalline SPDC sources. Here, we investigate photon pair generation through SFWM in subwavelength films of amorphous silicon nitride (SiN) with varying nitrogen content. For all samples, we demonstrate two-photon quantum correlations, indicated by the normalized second-order correlation function g (2) (0): it exceeds 2 and decays as the pump power increases. By observing two-photon interference between SFWM from the SiN films and the fused silica (FS) substrate, we find the third-order susceptibilities of films with different nitrogen content.
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.
Miniaturised entangled photon sources are highly demanded for the development of integrated quantum photonics. Since the invention of subwavelength optical metasurfaces and their successes at replacing bulky optical components, the possibility of implementing entangled photon sources on such devices is actively investigated. Here, as a first step towards the development of quantum optical metasurfaces (QOM), we demonstrate photon pair generation via spontaneous parametric down-conversion (SPDC) from subwavelength films. We achieved photon pair generation with a high coincidence-to-accidental ratio in lithium niobate and gallium phosphide nanofilms. In addition, we have measured the SPDC frequency spectrum via fibre spectroscopy, obtaining photon pairs with a spectral bandwidth of 500\;nm, limited only by the overall detection efficiency. Moreover, we have observed the vacuum field enhancement due to a Fabry-Perot resonance inside the nonlinear films. Our experiments lay the groundwork for the future development of flat SPDC sources, including QOM.