Mode-programmable comb spectroscopy enabling non-cooperative computational sensing with single-photon sensitivity

Frequency comb spectroscopy provides broadband access to molecular fingerprints with mode-defined spectral resolution. However, its deployment in non-cooperative gas sensing remains challenging because conventional implementations require cooperative reflectors or well-controlled optical returns. Here, we overcome this limitation by introducing a computational sensing scheme based on a mode-programmable optical comb and a high-sensitivity single-pixel detector. In our approach, a two-dimensional disperser and a high-speed digital micromirror device encode individual comb modes, enabling broadband, mode-resolved spectral acquisition without relying on coherent detection. This architecture supports measurements through highly scattering media and from non-cooperative targets while retaining the core advantages of frequency-comb spectroscopy. Our method achieves picometer-level spectral resolution, a 10-nm (1.27-THz) instantaneous bandwidth, single-photon sensitivity down to 10^-4 photons per pulse, and compressed spectral acquisition with 2.5% sampling for <10% reconstruction error. These capabilities establish a powerful platform for diverse gas-sensing applications, including remote environmental monitoring, industrial leak localization, and explosive-threat detection.