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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. 

Mode-locked lasers (MLLs) generate ultrashort pulses with peak powers substantially exceeding their average powers. However, integrated MLLs that drive ultrafast nanophotonic circuits have remained elusive because of their typically low peak powers, lack of controllability, and challenges when integrating with nanophotonic platforms. In this work, we demonstrate an electrically pumped actively MLL in nanophotonic lithium niobate based on its hybrid integration with a III-V semiconductor optical amplifier. Our MLL generates $\sim$4.8-ps optical pulses around 1065 nm at a repetition rate of ∼10 GHz, with energies exceeding 2.6 pJ and peak powers beyond 0.5 W. The repetition rate and the carrier-envelope offset frequency of the output can be controlled in a wide range by using the driving frequency and the pump current, providing a route for fully stabilized on-chip frequency combs. 

Abstract 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. 

Abstract 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. 

We introduce a method for gas sensing without performing direct spectrum measurement using broadband mid-infrared optical parametric oscillators, and experimentally demonstrate proof-of-concept carbon dioxide sensing. 

We utilize the unique formation dynamics of quadratic cavity solitons for enhanced sensing, experimentally show CO₂sensing with high sensitivity and large dynamic range, and present the promising potentials of soliton-enhanced gas sensors. 

We demonstrate broadly-tunable synchronously-pumped optical parametric oscillators in nanophotonic lithium niobate. A picosecond 1-µm pump generates subpicosecond signal/idler frequency combs tunable between 1.5 and 3.3µm with up-conversion to the visible on the same chip. 

We demonstrate mid-infrared frequency combs from synchronously-pumped optical parametric oscillators in nanophotonic lithium niobate at 19 GHz. With a picosecond pump at ~1µm, the output can be tuned between 1.5 and 3.3µm supporting sub-picosecond pulses.