Dual-comb spectroscopy from the ultraviolet to mid-infrared region based on high-order harmonic generation

Abstract

Dual-comb spectroscopy (DCS) has revolutionized numerous spectroscopic applications due to its high spectral resolution and fast measurement speed. Substantial efforts have been made to obtain a coherent dual-comb source at various spectral regions through nonlinear frequency conversion, where the preservation of coherence has become a problem of great importance. In this study, we report the generation of coherent dual-comb sources covering from the ultraviolet to mid-infrared region based on high-order harmonic generation. Driven by high-repetition-rate femtosecond mid-infrared dual-comb pump pulses, up to ninth-order harmonic was generated from the ultraviolet to mid-infrared region using an aperiodically poled lithium niobate waveguide. To investigate the coherence property of the high-order harmonic generation, DCS was performed at every generated spectral region from 450 to 3600 nm. The measured dual-comb spectra with distinctive tooth-resolved structures show the well-preserved coherence without apparent degradation after the cascaded quadratic nonlinear processes. The subsequent methane absorption spectroscopy at multiple spectral regions of different harmonics was carried out to characterize the spectroscopic capability of the system. These results demonstrate the potential of our scheme to generate compact and coherent broadband optical frequency combs for simultaneous multi-target detections.