Reconstructive comb spectroscopy: A single-pixel detection paradigm beyond dual-comb limitations

Abstract

Frequency comb spectroscopy has revolutionized broadband molecular fingerprinting with mode-defined resolution. While dual-comb spectroscopy stands as a dominant paradigm for high-resolution measurements, it relies on mutually coherent dual combs, and its applicability to non-cooperative sensing is limited by the requirement for phase-sensitive detection and controlled optical returns. Here, we introduce reconstructive comb spectroscopy, a fundamentally different paradigm that eliminates these constraints. By integrating a mode-programmable optical comb with a computational sensing scheme based on single-pixel detection, our method achieves picometer-level spectral resolution over a 10-nm (1.27-THz) instantaneous bandwidth, with single-photon sensitivity down to 10^-4 photons per pulse, and compressed spectral acquisition at 2.5% sampling while maintaining reconstruction errors below 10%. We demonstrate robust performance through scattering media and from non-cooperative targets. These capabilities establish reconstructive comb spectroscopy as a new platform for gas sensing, with broad applicability in remote atmospheric monitoring, industrial leak detection, and standoff chemical-threat identification.