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Towards photon pair generation via spontaneous four-wave mixing in nonlinear metasurfaces

Son, Changjin

Published Jan 1, 2026• 0 citations
Publisher

Abstract

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.

DOI
10.25593/open-fau-2901

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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)χ^{(2)}χ(2), SFWM can generate photon pairs both directly, through the third-order nonlinear susceptibility χ(3)χ^{(3)}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.
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.
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.
All-dielectric optical metasurfaces are a workhorse in nano-optics, because of both their ability to manipulate light in different degrees of freedom and their excellent performance at light frequency conversion. Here, we demonstrate first-time generation of photon pairs via spontaneous parametric-down conversion in lithium niobate quantum optical metasurfaces with electric and magnetic Mie-like resonances at various wavelengths. By engineering the quantum optical metasurface, we tailor the photon-pair spectrum in a controlled way. Within a narrow bandwidth around the resonance, the rate of pair production is enhanced up to 2 orders of magnitude, compared to an unpatterned film of the same thickness and material. These results enable flat-optics sources of entangled photons-a new promising platform for quantum optics experiments.
The ability to generate quantum entangled photon pairs through spontaneous parametric down conversion (SPDC) is playing a pivotal role in many applications in quantum technologies, including quantum communications, quantum computation, and quantum imaging. Metasurfaces, two-dimensional arrays of nanostructures with subwavelength thickness, have recently shown extraordinary capability in manipulating classical and quantum states of light and realizing miniaturized SPDC sources. Whereas previous studies have primarily focused on periodic metasurfaces, we uncover the potential of spatially modulated nanopatterns for further SPDC enhancement and state engineering. Specifically, we propose a nonlinear metasurface featuring a lateral guided-mode cavity formed by two distributed Bragg reflectors. With the quasi-normal mode theory, we predict an SPDC rate up to 157 Hz/mW, which represents about 30 times rate enhancement when compared to the metasurface without a cavity. Furthermore, the cavity supports a continuous set of high-Q resonances across a broad bandwidth, allowing the all-optical tuning of the photon-pair emission directions transverse to the cavity by controlling the pump wavelength, which can find applications in quantum imaging.