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Applied Physics Reviews

Bulk nonlinear metamaterials for generation of quantum light

Ofir Yesharim, Inbar Hurvitz, Joshua Foley-Comer, Ady Arie

Published Mar 1, 2025• 11 citations
Publisher

Abstract

Quantum states of light, such as fixed photon number (Fock) states, entangled states, and squeezed states, offer important advantages with respect to classical states of light, such as coherent states and thermal states, in different areas: they enable secure communication and distribution of encryption keys, enable realization of sensors with higher sensitivity and resolution, and are considered candidates for quantum computing and simulation applications. To accommodate these applications, suitable methods for generating the quantum states are needed. Today, the quantum states are often produced by a spontaneous nonlinear process in a standard nonlinear material, followed by a series of optical elements necessary for encoding the desired state on the generated photons. In this review, we consider an alternative approach of structuring the nonlinearity of the crystal so that the desired quantum state will be generated directly at the crystal, without the need for additional elements. Our main focus here is on bulk crystals having structured second-order nonlinearity. The rising interest in these nonlinear metamaterials is fueled by advancements in the ability to efficiently simulate and design spontaneous parametric downconversion (SPDC) processes, as well as by new capabilities of structuring the nonlinearity of ferroelectric crystals, either by electric field poling or by laser-induced writing. As a result, nonlinear metamaterials were recently used to directly shape the spatial and spectral correlations of quantum light that is generated in SPDC. The paper covers the theoretical background and the design and fabrication methods of bulk nonlinear metamaterials for generating quantum light, as well as a series of demonstrations of the use of metamaterials in quantum optical applications.

DOI
10.1063/5.0216714

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Quantum states of light, such as fixed photon number (Fock) states, entangled states, and squeezed states, offer important advantages with respect to classical states of light, such as coherent states and thermal states, in different areas: they enable secure communication and distribution of encryption keys, enable realization of sensors with higher sensitivity and resolution, and are considered candidates for quantum computing and simulation applications. To accommodate these applications, suitable methods for generating the quantum states are needed. Today, the quantum states are often produced by a spontaneous nonlinear process in a standard nonlinear material, followed by a series of optical elements necessary for encoding the desired state on the generated photons. In this review, we consider an alternative approach of structuring the nonlinearity of the crystal so that the desired quantum state will be generated directly at the crystal, without the need for additional elements. Our main focus here is on bulk crystals having structured second-order nonlinearity. The rising interest in these nonlinear metamaterials is fueled by advancements in the ability to efficiently simulate and design spontaneous parametric downconversion (SPDC) processes, as well as by new capabilities of structuring the nonlinearity of ferroelectric crystals, either by electric field poling or by laser-induced writing. As a result, nonlinear metamaterials were recently used to directly shape the spatial and spectral correlations of quantum light that is generated in SPDC. The paper covers the theoretical background and the design and fabrication methods of bulk nonlinear metamaterials for generating quantum light, as well as a series of demonstrations of the use of metamaterials in quantum optical applications.
In the process of Spontaneous Parametric Down Conversion (SPDC), a pump photon spontaneously splits inside a quadratic nonlinear crystal to signal and idler photons. By spatially modulating the nonlinear coefficient, we form a bulk nonlinear metamaterial that can shape the first and second order correlations of the down-converted signal and idler photons in either the spatial domain or the spectral domains. These degrees of freedom span a multi-dimensional Hilbert space, which is beneficial for quantum information applications. Recently, we have designed and fabricated, using electric field poling, bulk nonlinear metamaterials in KTiOPO4, for generating spatially entangled signal-idler pairs. This includes a bi-photon Bell state in the Hermite-Gauss basis, or a state with 3 dominant pairs of coincidences, approximating a bi-photon qutrit. As for the spectral domain, we generated a variety of quantum states: high purity frequency uncorrelated states, frequency-bin Bell states and frequency entangled bi-photon qudit states. By increasing the pump power, we reach the regime of bright squeezed vacuum sources, enabling the generation of a square cluster state in the frequency domain.
The recent advent of optical metasurfaces, ultra-thin structures composed of nanoresonators facilitating strong light concentration [1–3], opens the path towards efficient \nfrequency conversion [4–7] in a material thousand times thinner than a human hair [8]. \nThere is a remarkable capacity to individually shape each nanoresonator of the metasurface to spatially and spectrally control the conversion process with unprecedented \nnanoscale resolution, facilitating an ultimate flexibility to selectively convert, focus, \nand image different colours with a single metasurface. The strong enhancement of the \nnonlinear processes in dielectric nanoresonators is largely due to the absence of material \nabsorption and the excitation of Mie-type bulk resonances [2]. The highest conversion \nefficiency to date has been achieved employing III-V semiconductor nanostructures, \nsuch as AlGaAs which is a non-centrosymmetric material with high quadratic nonlinear \nsusceptibility. In particular, second-harmonic generation efficiencies up to 10−4 have \nbeen recently demonstrated [8–12], six orders of magnitude higher than in plasmonics. \nSuch capabilities can make an immense fundamental and practical impact, including \nthe quantum state generation in nonlinear metasurfaces as we discuss in this chapter. \nThe quantum state of correlated photon-pairs is the essential building block for photon entanglement [13, 14], which underpins many quantum applications, including secure networks, enhanced measurement and lithography, and quantum information processing [15]. One of the most versatile techniques for the generation of correlated photons is the process of spontaneous parametric down-conversion (SPDC) [16, 17], see \nFig. 1. It allows for an arbitrary choice of energy and momentum correlations between \nthe generated photons, robust operation at room temperature, as well as for spatial and \ntemporal coherence between simultaneously pumped multiple SPDC sources. Alternative approaches based on atom-like single photon emitters, such as solid-state fluorescent atomic defects [18], quantum dots [19, 20], and 2D host materials [21, 22], have \nreached a high degree of frequency indistinguishability, purity and brightness [19, 20]. \nHowever, this comes with the expense of operation at cryogenic temperatures and lack \nof spatial coherence between multiple quantum emitters. These features might limit \npossible applications and reduce the potential for device scalability. Furthermore, the \nsmall size of the atomic sources often requires complex schemes aimed at coupling to \noptical nanoantennas and improving the photon extraction efficiency [21]. \nThe miniaturization of SPDC quantum-light sources to micro and nanoscale dimensions is a continuing quest, as it enables denser integration of functional quantum \ndevices. Traditionally, bulky cm-sized crystals were utilized for SPDC, entailing the \ndifficulty of aligning multiple optical elements after the SPDC crystal, while offering \nrelatively low photon-pair rates [17]. As a first step of miniaturization, SPDC was \nrealized in low-index-contrast waveguides, which allowed confining light down to several square micrometers transversely to the propagation direction, significantly enhancing the conversion efficiency [23]. However, this approach still requires centimetres \nof propagation length, which makes the on-chip integration with other elements challenging [24]. The introduction of high-index contrast waveguides and ring resonators \nallowed for shrinking the sizes necessary for SPDC to millimetres [25], and to tens \nof micrometers [26]. However, further miniaturisation down to the metasurfaces composed of nanoresonators requires conceptually different approaches.
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.
Single-photon and correlated two-photon sources are important elements for optical information systems. Nonlinear downconversion light sources are robust and stable emitters of single photons and entangled photon pairs. However, the rate of downconverted light emission, dictated by the properties of low-symmetry nonlinear crystals, is typically very small, leading to significant constraints in device design and integration. In this Letter, we study principles of spontaneous emission control (i.e., the Purcell effect) generalized to describe the enhancement of nonlinear generation of quantum light through spontaneous parametric downconversion. We develop a theoretical framework based on eigenmode analysis to study quantum nonlinear emission in a general anisotropic, dispersive, and lossy media. Our theory provides an unprecedented insight into the emission process. We find that spontaneous parametric downconversion in a media with hyperbolic dispersion is broadband and phase-mismatch-free. We further predict a significant enhancement of the downconverted emission rate in experimentally realistic nanostructures. Our theoretical formalism and approach to Purcell enhancement of nonlinear optical processes provides a framework for description of quantum nonlinear optical phenomena in complex nanophotonic structures.
The fields of quantum and nonlinear optics have given rise to a variety of nonclassical states of light that have been proven to surpass certain limitations set by classical physics. Namely, certain squeezed and entangled states have been shown to beat the shot-noise limit when making precision phase measurements in interferometry, as well as write lithographic patterns that are smaller than classically allowed by the Rayleigh diffraction limit. Additionally, single-photon sources and entangled photon pairs have given rise to provably secure quantum key distribution for cryptography. Producing these quantum states of light has proven a difficult task. Nonlinear crystals, when pumped by a laser, produce pairs of single photons via the process of spontaneous parametric down conversion (SPDC). This process is mediated by the second order nonlinear susceptibility of the material. When pumped in a high gain regime, these crystals give rise to optical parametric amplification, which is a viable source of squeezed light. The vast majority of research in this area has focused on crystals that are seeded by vacuum in their two modes. This dissertation concerns the field of quantum nonlinear optics. It is an investigation into the processes that occur when nonlinear materials interact with the electromagnetic field on the single photon level. I have focused on seeding nonlinear crystals with quantum states of light, including single photons and entangled states. This process results in various states directly applicable to interferometry, imaging, and cryptography. Another application investigated is an absolute radiance measurement via stimulated parametric down conversion resulting from non-vacuum seeding of a nonlinear crystal. Additionally, other nonlinear processes, including four-wave mixing, nonlinear magneto-optical effects and coherent population trapping in warm atomic vapor involving quantum states of light are investigated. The process of seeding third-order nonlinear interactions, such as in atomic vapors, gives rise to a variety of interesting, nonclassical phenomena such as entangled image transfer and nonlocal imaging. Strong analogies between SPDC and four-wave mixing are drawn. I also experimentally show an all optical pi-only phase shift of one light beam via another in warm Cesium vapor.
Abstract We discuss the generation of entangled photons using a nonlinear photonic crystal and beam splitter. In our method, the photonic crystal is assumed to be composed of a material with a large second-order nonlinear optical susceptibility χ ( 2 ) . Our proposal relies on two facts: (1) A nonlinear photonic crystal changes coherent incident light into squeezed light. (2) A beam splitter transforms the squeezed light into entangled light beams flying in two different directions. We estimate the yield efficiency of pairs of entangled photons per pulse of the very weak coherent light for our method at 0.0783 for a specific concrete example. Our method is more effective because the conversion efficiency (entangled biphotons per incident pump photons) in the spontaneous parametric downconversion is of the order of 4 × 10 − 6 . The only drawback is that it requires very fine tuning of the frequency of signal photons fed into the photonic crystal; for example, an adjustment is given by Δ ν = 3.11 × 10 8 Hz for the signal light of ν = 3.23 × 10 14 Hz. We investigate the application of entangled photons produced by our method to the BB84 quantum key distribution protocol, and we explore how to detect an eavesdropper. We suggest that our method is promising for decoy-state quantum key distribution using weak coherent light.