Spontaneous parametric downconversion (SPDC) has been predicted in atomically thick crystals, though not yet observed. In this work we uncover physical and experimental constraints of photon-pair generation in such planar nonlinear films with a free-space illumination/collection geometry. We measure the material nonlinear response of monolayer tungsten diselenide via second harmonic generation and subsequently calculate the expected SPDC efficiency from appropriate quantum-classical relations. Energy and momentum conservation shape the wavevectors of photon pairs in free-space and allow us to calculate the loss and coincidence-to-accidental ratio in various configurations. This work improves the understanding of the nonlinear quantum optical potential of these crystals, guides their experimental validation, and provides a performance benchmark for these ultrathin materials.
Spontaneous parametric downconversion (SPDC) has been predicted in atomically thick crystals, though not yet observed. In this work we uncover physical and experimental constraints of photon-pair generation in such planar nonlinear films with a free-space illumination/collection geometry. We measure the material nonlinear response of monolayer tungsten diselenide via second harmonic generation and subsequently calculate the expected SPDC efficiency from appropriate quantum-classical relations. Energy and momentum conservation shape the wavevectors of photon pairs in free-space and allow us to calculate the loss and coincidence-to-accidental ratio in various configurations. This work improves the understanding of the nonlinear quantum optical potential of these crystals, guides their experimental validation, and provides a performance benchmark for these ultrathin materials.
The promises of quantum computing is to enable faster and more powerful computation than would ever be possible with a classical processor based on binary logic. Quantum linear optics is one of many promising platforms to build a universal quantum computers by leveraging the interaction between indistinguishable photons. A common technique to prepare such states is photon heralding, where many identical photons can be generated and used to encode and process information. Photon pairs are typically generated from a second-order nonlinear interaction known as spontaneous parametric downconversion (SPDC). In all existing platforms, materials are used as both a source of optical nonlinearity, and a phase-matching medium, often resulting in narrow-band and non-reconfigurable operation. 2D materials promise to change this, thanks to their high nonlinearity, inherent broadband phase-matching, and highly configurable electro-optical properties. To date SPDC has only been reported in structures with many millions of atoms, stimulating experimental efforts to validate its scaling laws in structures only a few atoms thick. In this thesis we investigate SPDC in group IV transition-metal dichalcogenides (TMDCs), and describe efforts towards the experimental observation of non-resonant SPDC from a diffraction-limited area. Because of the intimate connection between the classical second-harmonic generation (SHG) and the quantum SPDC, the efficiency of one process provides insights on the other. This guides the design of single-photon coincidence measurements required to demonstrate the strong temporal correlations of these entangled states. Measurements are hindered by the presence of a broadband, temporally uncorrelated background, attributed to photoluminescence. This work improves the understanding of the nonlinear quantum optical potential of these crystals, and provides a performance benchmark for these ultra-thin materials.
) 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.
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.
Non-phase-matched spontaneous parametric down-conversion (SPDC) in atomically thin materials provides new degrees of freedom and enhanced quantum information capacity compared to conventional phase-matched sources. These systems emerged as promising platforms for quantum computing, communication, and imaging, with the potential to support higher-order nonlinear processes. However, direct observation of photon-pair emission from a monolayer has remained experimentally challenging. In this work, we theoretically modeled SPDC emission across the full angular space from a monolayer GaSe film and experimentally validated the model through measurements of both co- and counter-propagating photon pairs. We demonstrated two-photon quantum correlations in the telecom C-band from the thinnest SPDC source reported to date. The spatially symmetric, broadband emission predicted by theory was confirmed experimentally. Furthermore, we observed high-fidelity Bell states in the counter-propagating configuration, marking the first realization of polarization-entangled photon pairs from a monolayer. Our results revealed the emission characteristics of SPDC in the deeply subwavelength, non-phase-matched regime, and introduced atomically thin, counterpropagating SPDC as a scalable and integrable platform for programmable quantum state generation, extendable via moiré superlattice engineering.
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.