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Photonics offers unique capabilities for quantum information processing (QIP) such as room-temperature operation, the scalability of nanophotonics, and access to ultrabroad bandwidths and consequently ultrafast operation. Ultrashort pulse sources of quantum states in nanophotonics are an important building block for achieving scalable ultrafast QIP; however, their demonstrations so far have been sparse. Here, we demonstrate a femtosecond biphoton source in dispersion-engineered periodically poled lithium niobate nanophotonics. We measure 17 THz of bandwidth for the source centered at 2.09 µm, corresponding to a few optical cycles, with a brightness of 8.8 GHz/mW. Our results open new paths toward realization of ultrafast nanophotonic QIP.

Optical frequency comb is an enabling technology for a multitude of applications from metrology to ranging and communications. The tremendous progress in sources of optical frequency combs has mostly been centered around the near-infrared spectral region, while many applications demand sources in the visible and mid-infrared, which have so far been challenging to achieve, especially in nanophotonics. Here, we report widely tunable frequency comb generation using optical parametric oscillators in lithium niobate nanophotonics. We demonstrate sub-picosecond frequency combs tunable beyond an octave extending from 1.5 up to 3.3 μm with femtojoule-level thresholds on a single chip. We utilize the up-conversion of the infrared combs to generate visible frequency combs reaching 620 nm on the same chip. The ultra-broadband tunability and visible-to-mid-infrared spectral coverage of our source highlight a practical and universal path for the realization of efficient frequency comb sources in nanophotonics, overcoming their spectral sparsity.

Topology is central to phenomena that arise in a variety of fields, ranging from quantum field theory to quantum information science to condensed matter physics. Recently, the study of topology has been extended to open systems, leading to a plethora of intriguing effects such as topological lasing, exceptional surfaces, as well as non-Hermitian bulk-boundary correspondence. Here, we show that Bloch eigenstates associated with lattices with dissipatively coupled elements exhibit geometric properties that cannot be described via scalar Berry phases, in sharp contrast to conservative Hamiltonians with non-degenerate energy levels. This unusual behavior can be attributed to the significant population exchanges among the corresponding dissipation bands of such lattices. Using a one-dimensional example, we show both theoretically and experimentally that such population exchanges can manifest themselves via matrix-valued operators in the corresponding Bloch dynamics. In two-dimensional lattices, such matrix-valued operators can form non-commuting pairs and lead to non-Abelian dynamics, as confirmed by our numerical simulations. Our results point to new ways in which the combined effect of topology and engineered dissipation can lead to non-Abelian topological phenomena.

Dual-comb spectroscopy has been proven beneficial in molecular characterization but remains challenging in the mid-infrared region due to difficulties in sources and efficient photodetection. Here we introduce cross-comb spectroscopy, in which a mid-infrared comb is upconverted via sum-frequency generation with a near-infrared comb of a shifted repetition rate and then interfered with a spectral extension of the near-infrared comb. We measure CO₂absorption around 4.25 µm with a 1-µm photodetector, exhibiting a 233-cm⁻¹instantaneous bandwidth, 28000 comb lines, a single-shot signal-to-noise ratio of 167 and a figure of merit of 2.4 × 10⁶Hz^1/2. We show that cross-comb spectroscopy can have superior signal-to-noise ratio, sensitivity, dynamic range, and detection efficiency compared to other dual-comb-based methods and mitigate the limits of the excitation background and detector saturation. This approach offers an adaptable and powerful spectroscopic method outside the well-developed near-IR region and opens new avenues to high-performance frequency-comb-based sensing with wavelength flexibility.

Driven nonlinear resonators provide a fertile ground for phenomena related to phase transitions far from equilibrium, which can open opportunities unattainable in their linear counterparts. Here, we show that optical parametric oscillators (OPOs) can undergo second-order phase transitions in the spectral domain between degenerate and non-degenerate regimes. This abrupt change in the spectral response follows a square-root dependence around the critical point, exhibiting high sensitivity to parameter variation akin to systems around an exceptional point. We experimentally demonstrate such a phase transition in a quadratic OPO. We show that the divergent susceptibility of the critical point is accompanied by spontaneous symmetry breaking and distinct phase noise properties in the two regimes, indicating the importance of a beyond nonlinear bifurcation interpretation. We also predict the occurrence of first-order spectral phase transitions in coupled OPOs. Our results on non-equilibrium spectral behaviors can be utilized for enhanced sensing, advanced computing, and quantum information processing.

Over the last few decades, nonlinear optics has become significantly more nonlinear, traversing nearly a billionfold improvement in energy efficiency, with ultrafast nonlinear nanophotonics in particular emerging as a frontier for combining both spatial and temporal engineering. At present, cutting-edge experiments in nonlinear nanophotonics place us just above themesoscopicregime, where a few hundred photons suffice to trigger highly nonlinear dynamics. In contrast to classical or deep-quantum optics, the mesoscale is characterized by dynamical interactions between mean-field, Gaussian, and non-Gaussian quantum features, all within a close hierarchy of scales. When combined with the inherent multimode complexity of optical fields, such hybrid quantum-classical dynamics present theoretical, experimental, and engineering challenges to the contemporary framework of quantum optics. In this review, we highlight the unique physics that emerges in multimode nonlinear optics at the mesoscale and outline key principles for exploiting both classical and quantum features to engineer novel functionalities. We briefly survey the experimental landscape and draw attention to outstanding technical challenges in materials, dispersion engineering, and device design for accessing mesoscopic operation. Finally, we speculate on how these capabilities might usher in some new paradigms in quantum photonics, from quantum-augmented information processing to nonclassical-light-driven dynamics and phenomena to all-optical non-Gaussian measurement and sensing. The physics unlocked at the mesoscale present significant challenges and opportunities in theory and experiment alike, and this review is intended to serve as a guide to navigating this new frontier in ultrafast quantum nonlinear optics.

Traditional absorption spectroscopy has a fundamental difficulty in resolving small absorbance from a strong background due to the instability of laser sources. Existing background-free methods in broadband vibrational spectroscopy help to alleviate this problem but face challenges in realizing either low extinction ratios or time-resolved field measurements. Here, we introduce optical-parametric-amplification-enhanced background-free spectroscopy, in which the excitation background is first suppressed by an interferometer, and then the free-induction decay that carries molecular signatures is selectively amplified. We show that this method can improve the limit of detection in linear interferometry by order(s) of magnitude without requiring lower extinction ratios or a time-resolved measurement, which can benefit sensing applications in detecting trace species.

We investigate a resource-efficient distributed quantum sensing (DQS) scheme using phase-sensitive optical parametric amplifiers and linear optics, achieving sensitivity levels close to the optimal limit determined by the quantum Fisher information of the resource state.

We experimentally observe signatures of 475-fs-long sech-squared-shaped solitons in a ps-pumped phase-mismatched parametric oscillator in the normal dispersion regime, purely due to cascaded quadratic nonlinearities. The results are in good agreement with our theoretical predictions.