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Scientific Reports

Generation of broadband ultraviolet frequency-entangled photons using cavity quantum plasmonics

Hisaki Oka

Published Aug 8, 2017• 3 citations
Publisher

Abstract

Application of quantum entangled photons is now extending to various fields in physics, chemistry and biology. In particular, in terms of application to molecular science, broadband ultraviolet frequency-entangled photons are desired because molecules inducing photochemical reactions of interest often have electronic transition energies in the ultraviolet region. Recent standard method for generating such entangled photons is a chirped quasi-phase-matching method, however this method is not suitable for the generation of ultraviolet frequency-entangled photons because it requires down-conversion of a photon with a wavelength shorter than ultraviolet into an entangled photon pair. Here we propose a simple method for generating broadband ultraviolet frequency-entangled photons using cavity quantum plasmonics, in which conventional cavity quantum electrodynamics theory is applied to quantum plasmonics. We introduce a cavity-plasmon system in which localised surface plasmon (LSP) is coupled to the cavity fields of a state-of-the-art microcavity. Using this system, we theoretically show that broadband ultraviolet frequency-entangled photons can be generated simply by utilising the absorption saturation effect of LSP.

DOI
10.1038/s41598-017-08431-x

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Application of quantum entangled photons is now extending to various fields in physics, chemistry and biology. In particular, in terms of application to molecular science, broadband ultraviolet frequency-entangled photons are desired because molecules inducing photochemical reactions of interest often have electronic transition energies in the ultraviolet region. Recent standard method for generating such entangled photons is a chirped quasi-phase-matching method, however this method is not suitable for the generation of ultraviolet frequency-entangled photons because it requires down-conversion of a photon with a wavelength shorter than ultraviolet into an entangled photon pair. Here we propose a simple method for generating broadband ultraviolet frequency-entangled photons using cavity quantum plasmonics, in which conventional cavity quantum electrodynamics theory is applied to quantum plasmonics. We introduce a cavity-plasmon system in which localised surface plasmon (LSP) is coupled to the cavity fields of a state-of-the-art microcavity. Using this system, we theoretically show that broadband ultraviolet frequency-entangled photons can be generated simply by utilising the absorption saturation effect of LSP.
A scheme for the generation of frequency-entangled photons using a plasmon nanoantenna system is proposed. The nanoantenna system consists of two large metallic nanostructures confined in a one-sided microcavity with high spontaneous emission factor. Two input photons are converted into an entangled photon pair via the saturation effect of the nanoantenna. The degree of entanglement of the resultant entangled photons is evaluated using the entropy of entanglement, E. We show that broadband frequency-entangled photons with E up to ≈0.45 are generated owing to rapid plasmon radiative decay.
As some of the most promising quantum applications such as high resolution quantum optical coherence tomography (QOCT) [1] with dispersion cancellation as well as quantum key distribution require frequency entanglement. Therefore, frequency entanglement light sources are an essential importance for implement of many quantum optical applications. So Far, the most prominent method used for the entangled photon pair generation is spontaneous parametric down-conversion (SPDC) in nonlinear crystals. Recently, with adopting chirp quasi-phase matching (QPM) PPSLT (periodically poled stoichiometric lithium tantalate) has been used as source of entangled photons with large bandwidth [2]. However, improving the overall system efficiency is still remain challenging.
Single-photon frequency conversion for quantum interface plays an important role in quantum communications and networks, which is crucial for the realization of quantum memory, faithful entanglement swapping and quantum teleportation. In this talk, I will present our recent experiments about single-photon frequency conversion based on quadratic nonlinear processes. Firstly, we demonstrated spectrum compression of broadband single photons at the telecom wavelength to the near-visible window. A positively chirped single-photon-level laser pulse and a negatively chirped classical one are converted to a narrowband single-photon pulse, with a spectrum compression factor of 58, through sum-frequency generation (SFG), marking a critical step towards coherent photonic interface. Secondly, we demonstrated the nonlinear interaction between two chirped broadband single-photon-level coherent states. A high SFG efficiency of 1.06 × 10−7 is realized, which may be utilized to achieve heralding entanglement at a distance. Finally, we theoretically introduced and experimentally demonstrated single-photon frequency conversion in the telecom band, enabling switching of single photons between dense wavelength-division multiplexing channels. Using cascaded quasi-phase matched sum/difference frequency generation, the signal photon of a photon pair from spontaneous down-conversion is precisely shifted to identically match its counterpart, i.e. idler photon, in frequency to manifest a clear non-classical dip in the Hong-Ou-Mandel interference. Moreover, quantum entanglement between the photon pair is maintained after the frequency conversion. Our researches have realized three significant quantum interfaces via single-photon frequency conversion, which hold great promise for the development of quantum communications and networks.
I will discuss our recent results demonstrating exceptional nonlinear optical frequency conversion in transition metal dichalcogenides (TMDs). By fabricating nano-photonic elements such as waveguides, metasurfaces, and periodically poled stacks, we achieve macroscopic frequency conversion efficiencies over microscopic distances, 10 to 100× smaller than current systems with similar performances. Further, we report the broadband generation of entangled photon pairs at telecom wavelength via quasi-phase-matched spontaneous parametric down-conversion, showing the highest coincidence-to-accidental-ratio (CAR) ever demonstrated in a vdW material. This work opens the new and unexplored field of phase-matched nonlinear optics with microscopic van der Waals crystals, unlocking applications that require simple, ultra-compact technologies such as on-chip entangled photon-pair sources for integrated quantum circuitry and sensing.
Theoretical study on entangled photon generation from a quantum dot (QD) embedded in microcavity is briefly reviewed within a strong coupling regime. In this system, entangled photon pairs can be generated through the cascade photon emission via dressed states in the cavity quantum electrodynamics (CQED). Excitation levels of a QD are modeled by a V-type three-level system and four-level system including a biexciton. In contrast to the entangled-photon generation until now, all four Bell states can be generated from an identical cavity system by simply selecting applied-field polarizations and frequencies as characteristic features of the CQED. The CQED effects play a crucial role in providing a high degree of entanglement: (i) spectral fi ltering can be used to extract entangled photons due to the vacuum Rabi splitting and (ii) non-entangled co-polarized photons are strongly suppressed due to the photon blockade effect.
Energy-time entangled photon pairs (EPPs), which are at the heart of numerous quantum light applications, are commonly generated in nonlinear crystals. Some highly sensitive quantum applications require the use of ultra-broadband entangled photons that cannot be generated in nonlinear crystals due to phase-matching requirements. Here, we investigate the possibility of using metallic nanoparticles (MNPs) as a means for generating entangled photons through spontaneous parametric down-conversion (SPDC). MNPs are known for their strong light-matter coupling at their localized surface plasmon resonance, and since the propagation length through them is negligible relative to optical wavelengths, we consider them as excellent candidates to serve as non-phase matched sources of ultra-broadband entangled photons. To that end, we report experimental results of classical-light second-harmonic generation in silver nanotriangles and nanocubes embedded in polyvinyl alcohol. Based on the results of our experiments, performed using the reference-free hyper-Rayleigh scattering method [A. Ashkenazy et al., J. Phys. B 145401, 2019], we present an estimation of the characteristics of SPDC in MNPs. We show that, despite of the metals' centrosymmetric structure, MNPs exhibit second order nonlinearity that is mainly of an electric dipole nature, and so they are suitable for SPDC. Moreover, we show that localized surface-plasmon resonance can play a significant role in enhancing the generated EPPs flux. Finally, we compare the SPDC capabilities of MNPs to that of commonly used nonlinear crystals and show that the expected EPPs flux from MNPs is weaker but the EPPs have very large bandwidth, which could be helpful for advanced quantum sensing, spectroscopy and communication applications.