Dual-comb spectroscopy (DCS) has revolutionized optical spectroscopy by providing broadband spectral measurements with unprecedented resolution and fast response. Photothermal spectroscopy (PTS) with a pump-probe configuration offers a highly sensitive gas sensing method, which is normally performed using a single-wavelength pump laser. The merging of PTS with DCS may enable a spectroscopic method by taking advantage of both technologies, which has never been studied yet. Here, we report dual-comb photothermal spectroscopy (DC-PTS) by passing dual combs and a probe laser through a gas-filled anti-resonant hollow-core fiber, where the generated multi-heterodyne modulation of the refractive index is sensitively detected by an in-line interferometer. As an example, we have measured photothermal spectra of acetylene over 1 THz, showing a good agreement with the spectral database. Our proposed DC-PTS provides opportunities for broadband gas sensing with super-fine resolution and high sensitivity, as well as with a small sample volume and compact configuration.

Photoacoustic dual-comb spectroscopy (DCS), converting spectral information in the optical frequency domain to the audio frequency domain via multi-heterodyne beating, enables background-free spectral measurements with high resolution and broad bandwidth. However, the detection sensitivity remains limited due to the low power of individual comb lines and the lack of broadband acoustic resonators. Here, we develop cavity-enhanced photoacoustic DCS, which overcomes these limitations by using a high-finesse optical cavity for the power amplification of dual-frequency combs and a broadband acoustic resonator with a flat-top frequency response. We demonstrate high-resolution spectroscopic measurements of trace amounts of C₂H₂, NH₃ and CO in the entire telecommunications C-band. The method shows a minimum detection limit of 0.6 ppb C₂H₂ at the measurement time of 100 s, corresponding to the noise equivalent absorption coefficient of 7 × 10⁻¹⁰cm⁻¹. The proposed cavity-enhanced photoacoustic DCS may open new avenues for ultrasensitive, high-resolution, and multi-species gas detection with widespread applications.

Photoacoustic spectroscopy (PAS) based gas sensors with high sensitivity, wide dynamic range, low cost, and small footprint are desirable in energy, environment, safety, and public health. However, most works have focused on either acoustic resonator to enhance acoustic wave or optical resonator to enhance optical wave. Herein, we develop a gas sensor based on doubly resonant PAS in which the acoustic and optical waves are simultaneously enhanced using combined optical and acoustic resonators in a centimeter-long configuration. Not only the lower detection limit is enhanced by the double standing waves, but also the upper detection limit is expanded due to the short resonators. As an example, we developed a sensor by detecting acetylene (C₂H₂), achieving a noise equivalent absorption of 5.7 × 10⁻¹³ cm⁻¹ and a dynamic range of eight orders. Compared to the state-of-the-art PAS gas sensors, the developed sensor achieves a record sensitivity and dynamic range.