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arXiv:2408.06751 · Nature Communications

Polarization entanglement enabled by orthogonally stacked van der Waals NbOCl2 crystals

Qiangbing Guo, Yunkun Wu, Di Zhang, Qiuhong Zhang, Guang‐Can Guo, Andrea Alù, Xi‐Feng Ren, Cheng‐Wei Qiu

Published Dec 2, 2024• 31 citations
arXivHTMLPDF

Abstract

Polarization entanglement holds significant importance for photonic quantum technologies. Recently emerging subwavelength nonlinear quantum light sources, e.g., GaP and LiNbO3 thin films, benefiting from the relaxed phase-matching constraints and volume confinement, have shown intriguing properties, such as high-dimensional hyperentanglement and robust entanglement anti-degradation. Van der Waals (vdW) NbOCl2 crystal, with strong optical nonlinearities, has emerged as a potential candidate for ultrathin quantum light sources. However, polarization entanglement is inaccessible in the NbOCl2 crystal due to its unfavorable nonlinear susceptibility tensor. Here, by leveraging the twist-stacking degree of freedom inherently in vdW systems, we showcase the preparation of polarization entanglement and quantum Bell states. Van der Waals NbOCl2 crystal is a candidate platform for subwavelength thin film photon-pair sources. Here, the authors demonstrate generation of polarization entangled states from a two-layer stack of orthogonally oriented van der Waals crystal.

DOI
10.1038/s41467-024-54876-w

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Polarization entanglement holds significant importance for photonic quantum technologies. Recently emerging subwavelength nonlinear quantum light sources, e.g., GaP and LiNbO3 thin films, benefiting from the relaxed phase-matching constraints and volume confinement, have shown intriguing properties, such as high-dimensional hyperentanglement and robust entanglement anti-degradation. Van der Waals (vdW) NbOCl2 crystal, with strong optical nonlinearities, has emerged as a potential candidate for ultrathin quantum light sources. However, polarization entanglement is inaccessible in the NbOCl2 crystal due to its unfavorable nonlinear susceptibility tensor. Here, by leveraging the twist-stacking degree of freedom inherently in vdW systems, we showcase the preparation of polarization entanglement and quantum Bell states. Van der Waals NbOCl2 crystal is a candidate platform for subwavelength thin film photon-pair sources. Here, the authors demonstrate generation of polarization entangled states from a two-layer stack of orthogonally oriented van der Waals crystal.
Polarization-entangled photon pairs are essential resources for quantum information technologies, yet realizing compact sources with intrinsically controllable entanglement remains challenging. Van der Waals (vdW) nonlinear materials such as NbOCl2 provide atomically thin platforms for quantum light generation, yet their native crystalline anisotropies as natural materials impose limitations on accessible quantum states. Here, we develop a resonant vdW nonlinear metasurface based on NbOCl2 that exploits its intrinsic optical anisotropy to engineer polarization-dependent nonlinear responses. The anisotropic optical dispersion enables selective manipulation of resonant modes, resulting in a three-order-of-magnitude enhancement of the nonlinear response along the c axis. By further tailoring these resonant modes, we redistribute the effective second-order nonlinear susceptibility tensor between orthogonal polarization channels, balancing the spontaneous parametric down-conversion pathways along the b and c axes. This enables polarization-entangled photon generation with a measured fidelity of up to 92%. Our work establishes metasurface-enabled nonlinear optical engineering as a strategy for enhancing and controlling quantum light generation in vdW materials, providing a pathway toward scalable quantum photonic platforms.
Abstract Ultracompact entangled photon sources are pivotal to miniaturized quantum photonic devices. Van der Waals (vdW) nonlinear crystals promise efficient photon-pair generation and on-chip monolithic integration with nanophotonic circuitry. However, it remains challenging to generate maximally entangled Bell states of photon pairs with high purity, generation rate, and fidelity required for practical applications. Here, we realize a polarization-entangled photon-pair source based on spontaneous parametric down conversion in an ultrathin rhombohedral tungsten disulfide (3R-WS 2 ) crystal. This vdW entangled photonic source exhibits a high photon-pair purity with a coincidence-to-accidental ratio of above 800, a generation rate of 31 Hz, and two maximally polarization-entangled Bell states with fidelities exceeding 0.93 and entanglement degree over 0.97. These results stem from scalable optical nonlinearity, enhanced second-order susceptibility by electronic transitions, and a well-defined symmetry-enabled selection rule inherent in 3R-WS 2 . Our polarization entangled photon source can be integrated with photonic structures for generating more complex entangled states, thus paving an avenue for advanced quantum photonic systems toward computation and metrology.
Nanoscale quantum light sources are essential building blocks for integrated quantum photonic systems. Here, we report a wavelength-scale entangled-photon source based on van der Waals-engineered NbOBr2_22​, and benchmark its performance for telecom-wavelength quantum light generation. By exploiting the material's second-order nonlinearity, we generate quantum-correlated photon pairs via spontaneous parametric down-conversion. We then use a 90∘^{\circ}∘ twisted stacking to induce quantum interference in photon-pair generation, yielding polarization-entangled photons. This approach enables tunability of the quantum optical state via control of the excitation laser polarization. We experimentally obtain entanglement fidelities exceeding 95% for Bell states, along with a high coincidence-to-accidental ratio of $\sim$335, and a brightness approximately one order of magnitude higher than recently reported telecom sources based on transition metal dichalcogenide (TMD) 2D materials. These results establish twisted van der Waals engineering as a powerful platform for highly tunable, high-brightness quantum light sources at telecom wavelengths.
Nanoscale quantum light sources are essential building blocks for integrated quantum photonic systems. Here, we report a wavelength-scale entangled-photon source based on van der Waals-engineered NbOBr2 and benchmark its performance for telecom-wavelength quantum light generation. By exploiting the material's second-order nonlinearity, we generate quantum-correlated photon pairs via spontaneous parametric down-conversion. We then use a 90° twisted stacking to induce quantum interference in photon-pair generation, yielding polarization-entangled photons. This approach enables tunability of the quantum optical state via control of the excitation laser polarization. We experimentally obtain entanglement fidelities exceeding 95% for Bell states, along with a high coincidence-to-accidental ratio of ∼335 and a brightness approximately 1 order of magnitude higher than recently reported telecom sources based on transition metal dichalcogenide two-dimensional materials. These results establish twisted van der Waals engineering as a powerful platform for highly tunable, high-brightness quantum light sources at telecom wavelengths.
Bright entangled photon sources with on-demand quantum state control are essential for advancing quantum science and technologies. However, simultaneously achieving high brightness and state tunability remains challenging, as this necessitates a dual-phase control mechanism that facilitates both longitudinal phase matching and transverse polarization modulation. Here, we report a twin-twisted two-dimensional (2D) van der Waals (vdW) crystal architecture that enables spontaneous parametric down-conversion (SPDC) with both high generation efficiency and continuously tunable quantum states. The designed crystal comprises two sections of twisted 2D GaSe vdW flakes with opposite chiral handedness, in which interflake twist angle induces phase matching in SPDC, and intersection twisting provides an additional degree of freedom on tunability. We demonstrate that the twin-twisted GaSe crystals achieve a record-high photon-pair generation rate exceeding 13 200 Hz and a Bell state fidelity above 99% within 2D material family, and enable unprecedented tunability of quantum states from the maximally polarization entangled states to the fully separable states. This study opens a practical avenue toward twist-engineered quantum states, and paves the way for developing compact quantum photonic systems with tailored properties.
Van der Waals (vdW) ferroelectrics are emerging nonlinear photonic materials that combine large second-order susceptibility \c{hi}(2) with heterostructure compatibility, offering an attractive route toward miniaturized spontaneous parametric down-conversion (SPDC) sources. However, vdW SPDC sources operating under continuous irradiation in air remain limited in low brightness and poor operational stability, as oxygen and moisture exposure, together with pump-induced heating, lead to material degradation and permanent damage. Here we demonstrate an air-stable, bright SPDC source based on ferroelectric NbOI2 enabled by graphene encapsulation. Graphene provides robust environmental protection and can effectively supress pump induced degradation by enhancing heat dissipation. We report a record photon-pair generation absolute rate of 258 Hz and a normalized brightness of 19,900 Hz/(mW.mm). Leveraging this stabilized platform, we further generate polarization entangled photon pairs with 94% fidelity with respect to the maximally entangled Bell states from graphene-encapsulated 90° twisted bilayer NbOI2. Our results establish a practical and air-stable vdW ferroelectric SPDC platform that overcomes key limitations of existing vdW quantum light sources and provides a viable pathway toward scalable, integrated entangled photon sources for on chip quantum photonics.