Qudit entanglement is an indispensable resource for quantum information processing since increasing dimensionality provides a pathway to higher capacity and increased noise resilience in quantum communications, and cluster-state quantum computations. In continuous-variable time–frequency entanglement, encoding multiple qubits per photon is only limited by the frequency correlation bandwidth and detection timing jitter. Here, we focus on the discrete-variable time–frequency entanglement in a biphoton frequency comb (BFC), generating by filtering the signal and idler outputs with a fiber Fabry–Pérot cavity with 45.32 GHz free-spectral range (FSR) and 1.56 GHz full-width-at-half-maximum (FWHM) from a continuous-wave (cw)-pumped type-II spontaneous parametric downconverter (SPDC). We generate a BFC whose time-binned/frequency-binned Hilbert space dimensionality is at least 324, based on the assumption of a pure state. Such BFC’s dimensionality doubles up to 648, after combining with its post-selected polarization entanglement, indicating a potential 6.28 bits/photon classical-information capacity. The BFC exhibits recurring Hong–Ou–Mandel (HOM) dips over 61 time bins with a maximum visibility of 98.4% without correction for accidental coincidences. In a post-selected measurement, it violates the Clauser–Horne–Shimony–Holt (CHSH) inequality for polarization entanglement by up to 18.5 standard deviations with an S-parameter of up to 2.771. It has Franson interference recurrences in 16 time bins with a maximum visibility of 96.1% without correction for accidental coincidences. From the zeroth- to the third-order Franson interference, we infer an entanglement of formation (E_of) up to 1.89 ± 0.03 ebits—where 2 ebits is the maximal entanglement for a 4 × 4 dimensional biphoton—as a lower bound on the 61 time-bin BFC’s high-dimensional entanglement. To further characterize time-binned/frequency-binned BFCs we obtain Schmidt mode decompositions of BFCs generated using cavities with 45.32, 15.15, and 5.03 GHz FSRs. These decompositions confirm the time–frequency scaling from Fourier-transform duality. Moreover, we present the theory of conjugate Franson interferometry—because it is characterized by the state’s joint-temporal intensity (JTI)—which can further help to distinguish between pure-state BFC and mixed state entangled frequency pairs, although the experimental implementation is challenging and not yet available. In summary, our BFC serves as a platform for high-dimensional quantum information processing and high-dimensional quantum key distribution (QKD).

Quantum key distribution (QKD) has established itself as a groundbreaking technology, showcasing inherent security features that are fundamentally proven. Qubit-based QKD protocols that rely on binary encoding encounter an inherent constraint related to the secret key capacity. This limitation restricts the maximum secret key capacity to one bit per photon. On the other hand, qudit-based QKD protocols have their advantages in scenarios where photons are scarce and noise is present, as they enable the transmission of more than one secret bit per photon. While proof-of-principle entangled-based qudit QKD systems have been successfully demonstrated over the years, the current limitation lies in the maximum distribution distance, which remains at 20 km fiber distance. Moreover, in these entangled high-dimensional QKD systems, the witness and distribution of quantum steering have not been shown before. Here we present a high-dimensional time-bin QKD protocol based on energy-time entanglement that generates a secure finite-length key capacity of 2.39 bit/coincidences and secure cryptographic finite-length keys at 0.24 Mbits s⁻¹ in a 50 km optical fiber link. Our system is built entirely using readily available commercial off-the-shelf components, and secured by nonlocal dispersion cancellation technique against collective Gaussian attacks. Furthermore, we set new records for witnessing both energy-time entanglement and quantum steering over different fiber distances. When operating with a quantum channel loss of 39 dB, our system retains its inherent characteristic of utilizing large-alphabet. This enables us to achieve a secure key rate of 0.30 kbits s⁻¹ and a secure key capacity of 1.10 bit/coincidences, considering finite-key effects. Our experimental results closely match the theoretical upper bound limit of secure cryptographic keys in high-dimensional time-bin QKD protocols (Mower et al 2013 Phys. Rev. A 87 062322; Zhang et al 2014 Phys. Rev. Lett. 112 120506), and outperform recent state-of-the-art qubit-based QKD protocols in terms of secure key throughput using commercial single-photon detectors (Wengerowsky et al 2019 Proc. Natl Acad. Sci. 116 6684; Wengerowsky et al 2020 npj Quantum Inf. 6 5; Zhang et al 2014 Phys. Rev. Lett. 112 120506; Zhang et al 2019 Nat. Photon. 13 839; Liu et al 2019 Phys. Rev. Lett. 122 160501; Zhang et al 2020 Phys. Rev. Lett. 125 010502; Wei et al 2020 Phys. Rev. X 10 031030). The simple and robust entanglement-based high-dimensional time-bin protocol presented here provides potential for practical long-distance quantum steering and QKD with multiple secure bits-per-coincidence, and higher secure cryptographic keys compared to mature qubit-based QKD protocols.

High-dimensional quantum entanglement is a cornerstone for advanced technology enabling large-scale noise-tolerant quantum systems, fault-tolerant quantum computing, and distributed quantum networks. The recently developed biphoton frequency comb (BFC) provides a powerful platform for high-dimensional quantum information processing in its spectral and temporal quantum modes. Here we propose and generate a singly-filtered high-dimensional BFC via spontaneous parametric down-conversion by spectrally shaping only the signal photons with a Fabry-Pérot cavity. High-dimensional energy-time entanglement is verified through Franson-interference recurrences and temporal correlation with low-jitter detectors. Frequency- and temporal- entanglement of our singly-filtered BFC is then quantified by Schmidt mode decomposition. Subsequently, we distribute the high-dimensional singly-filtered BFC state over a 10 km fiber link with a post-distribution time-bin dimension lower bounded to be at least 168. Our demonstrations of high-dimensional entanglement and entanglement distribution show the singly-filtered quantum frequency comb’s capability for high-efficiency quantum information processing and high-capacity quantum networks.

High-efficient and high-purity photon sources are highly desired for quantum information processing. We report the design of a chip-scale hybrid Si_xN_y and thin film periodically-poled lithium niobate waveguide for generating high-purity type-II spontaneous parametric down-conversion (SPDC) photons in the telecommunication band. The modeled second harmonic generation efficiency of 225% W⁻¹ • cm⁻² is obtained at 1560nm. Joint spectral analysis is performed to estimate the frequency correlation of SPDC photons, yielding intrinsic purity with up to 95.17%. The generation rate of these high-purity photon pairs is estimated to be 2.87 × 10⁷ pairs/s/mW within the bandwidth of SPDC. Our chip-scale hybrid waveguide design has the potential for large-scale on-chip quantum information processing and integrated photon-efficient quantum key distribution through high-dimensional time-energy encoding.