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arXiv:2409.10845 · Science Advances

Nonlinearity symmetry breaking for generating tunable quantum entanglement in semiconductor metasurfaces

Jinyong Ma, Tongmiao Fan, Tuomas Haggrén, Laura Valencia Molina, Matthew Parry, Saniya Shinde, Caitlin McManus-Barrett, Jihua Zhang, Rocio Camacho‐Morales, Frank Setzpfandt, Hark Hoe Tan, C. Jagadish, Dragomir N. Neshev, Andrey A. Sukhorukov

Published Jul 9, 2025• 30 citations
arXivHTMLPDF

Abstract

Tunable biphoton quantum entanglement generated from nonlinear flat optics is highly desirable for cutting-edge quantum technologies, yet its tunability is substantially constrained by the symmetry of material nonlinear tensors. Here, we overcome this constraint by introducing symmetry breaking in nonlinear polarization via resonant metasurfaces. While asymmetric optical responses have enabled breakthroughs in classical applications like nonreciprocal light transmission, we report the experimental demonstration of asymmetric nonlinear responses for biphoton entanglement. Using a structural-asymmetric semiconductor metasurface incorporating [110] InGaP nanoresonators, we realize continuous tuning of polarization entanglement from partially entangled states to a Bell state by adjusting the pump wavelength. We also observe pronounced spatial anti-correlations and theoretically confirm that this approach can extend to tailor hyperentanglement. Furthermore, our nanoscale entanglement source features an ultrahigh coincidence-to-accidental ratio of ≈7 × 10 4 , outperforming existing semiconductor flat optics by two orders of magnitude. Introducing asymmetric nonlinear response in quantum metasurfaces opens directions for tailoring on-demand quantum states.

DOI
10.1126/sciadv.adu4133

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Tunable biphoton quantum entanglement generated from nonlinear flat optics is highly desirable for cutting-edge quantum technologies, yet its tunability is substantially constrained by the symmetry of material nonlinear tensors. Here, we overcome this constraint by introducing symmetry breaking in nonlinear polarization via resonant metasurfaces. While asymmetric optical responses have enabled breakthroughs in classical applications like nonreciprocal light transmission, we report the experimental demonstration of asymmetric nonlinear responses for biphoton entanglement. Using a structural-asymmetric semiconductor metasurface incorporating [110] InGaP nanoresonators, we realize continuous tuning of polarization entanglement from partially entangled states to a Bell state by adjusting the pump wavelength. We also observe pronounced spatial anti-correlations and theoretically confirm that this approach can extend to tailor hyperentanglement. Furthermore, our nanoscale entanglement source features an ultrahigh coincidence-to-accidental ratio of ≈7 × 10 4 , outperforming existing semiconductor flat optics by two orders of magnitude. Introducing asymmetric nonlinear response in quantum metasurfaces opens directions for tailoring on-demand quantum states.
Tunable photonic quantum entanglement promises to advance information processing beyond classical approaches, facilitating applications in quantum communications, imaging and computing. A practical approach to preparing quantum entanglement at room temperature is to engineer photon-pair generation through spontaneous parametric down-conversion (SPDC). Nonlinear flat-optics devices, incorporating subwavelength-thick nonlinear materials, are emerging as new platforms for generating photon pairs at the nanoscale. In particular, nanostructured metasurfaces supporting optical resonances can enhance and tailor SPDC processes, allowing for the generation of spectral, polarization, and spatial entanglement [1]. However, the tunability of polarization entanglement is subject to the symmetry of nonlinear tensors of materials, where the pump photon polarization serves as the only tuning parameter [2].
Entangled photon states are a fundamental resource for optical quantum technologies and investigating the fundamental predictions of quantum mechanics. Up to now such states are mainly generated in macroscopic nonlinear optical systems with elaborately tailored optical properties. In this theoretical work, we extend the understanding on the generation of entangled photonic states toward the nanoscale regime by investigating the fundamental properties of photon-pair generation in sub-wavelength nonlinear nanoresonators. Taking materials with Zinc-Blende structure as an example, we reveal that such systems can naturally generate various polarization-entangled Bell states over a very broad range of wavelengths and emission directions, with little to no engineering needed. Interestingly, we uncover different regimes of operation, where polarization-entangled photons can be generated with dependence on or complete independence from the pumping wavelength and polarization, and the modal content of the nanoresonator. Our work also shows the potential of nonlinear nanoresonators as miniaturized sources of biphoton states with highly complex and tunable properties.
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.
Polarization-entangled photon pair sources are essential for diverse quantum technologies, such as quantum communication, computation, and imaging. However, the generation of complex polarization-entangled quantum states has long been constrained by the available nonlinear susceptibility tensor of natural nonlinear crystals, necessitating a cumbersome and intricate setup for additional coherent superposition or post-selection. In this study, we introduce and experimentally demonstrate a nanoscale polarization-entangled photon pair source utilizing an artificially-engineered metamaterial platform. This platform is based on a plasmonic metasurface that is strongly coupled to an epsilon-near-zero (ENZ) material. By precisely engineering resonances at both pump and signal/idler wavelengths, and leveraging the field enhancement provided by the ENZ effect, the photon pair generation efficiency of the 68-nm-thick metasurface is significantly boosted. More notably, the ENZ metasurface platform facilitates versatile manipulation of the system's anisotropic second-order nonlinear susceptibility tensor, enabling direct control over the polarization states of the photon pairs, which leads to the generation of a polarization-entangled Bell state without the need for additional components. Our approach opens a new avenue for the simultaneous photon pair generation and quantum state engineering in a compact platform.
Photon-based polarization entanglement in the form of Bell states and qutrits is an essential tool for understanding complex quantum phenomena and implementing various quantum technologies such as free-space quantum communication and quantum imaging. Polarization-entangled photons are conventionally generated in bulky nonlinear crystals through spontaneous parametric down-conversion (SPDC). In this approach, the photon polarization is intrinsically defined by the nonlinear tensor of the material, restricting the versatility of the generated quantum states. The recent developments of dielectric nanostructures with sub-wavelength thickness called metasurfaces [1] enable miniaturization of quantum light sources, while dramatically enhancing the photon-pair generation and allowing the preparation of complex quantum states with spectral [2] and spatial [3] entanglement. However, optically reconfigurable generation of biphoton polarization states with metasurfaces remained unexplored.