Optical-parametric-amplification-enhanced background-free spectroscopy.

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.

Ultrafast mode-locked laser in nanophotonic lithium niobate.

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 [Formula: see text]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.

Visible-to-mid-IR tunable frequency comb in nanophotonics.

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.

Octave-spanning tunable infrared parametric oscillators in nanophotonics.

Widely tunable coherent sources are desirable in nanophotonics for a multitude of applications ranging from communications to sensing. The mid-infrared spectral region (wavelengths beyond 2 µm) is particularly important for applications relying on molecular spectroscopy. Among tunable sources, optical parametric oscillators typically offer some of the broadest tuning ranges; however, their implementations in nanophotonics have been limited to narrow tuning ranges in the infrared or to visible wavelengths. Here, we surpass these limits in dispersion-engineered periodically poled lithium niobate nanophotonics and demonstrate ultrawidely tunable optical parametric oscillators. Using 100 ns pulses near 1 µm, we generate output wavelengths tunable from 1.53 µm to 3.25 µm in a single chip with output powers as high as tens of milliwatts. Our results represent the first octave-spanning tunable source in nanophotonics extending into the mid-infrared, which can be useful for numerous integrated photonic applications.

Mid-infrared cross-comb spectroscopy.

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 CO2 absorption around 4.25 µm with a 1-µm photodetector, exhibiting a 233-cm-1 instantaneous bandwidth, 28000 comb lines, a single-shot signal-to-noise ratio of 167 and a figure of merit of 2.4 × 106 Hz1/2. 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.

Few-cycle vacuum squeezing in nanophotonics.

One of the most fundamental quantum states of light is the squeezed vacuum, in which noise in one of the quadratures is less than the standard quantum noise limit. In nanophotonics, it remains challenging to generate, manipulate, and measure such a quantum state with the performance required for a wide range of scalable quantum information systems. Here, we report the development of a lithium niobate-based nanophotonic platform to demonstrate the generation and all-optical measurement of squeezed states on the same chip. The generated squeezed states span more than 25 terahertz of bandwidth supporting just a few optical cycles. The measured 4.9 decibels of squeezing surpass the requirements for a wide range of quantum information systems, demonstrating a practical path toward scalable ultrafast quantum nanophotonics.

Spectral phase transitions in optical parametric oscillators.

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.