Mode-locked laser oscillation with spectral peaks at molecular rovibrational transition lines

We demonstrate spectral peak formation in a mode-locked solid-state laser that contains a gas cell inside the cavity. Symmetric spectral peaks appear in the course of sequential spectral shaping through resonant interaction with molecular rovibrational transitions and nonlinear phase modulation in the gain medium. The spectral peak formation is explained as that narrowband molecular emissions triggered by an impulsive rovibrational excitation are superposed on the broadband spectrum of the soliton pulse by constructive interference. The demonstrated laser, which exhibits comb-like spectral peaks at molecular resonances, potentially provides novel tools for ultrasensitive molecular detection, vibration-mediated chemical reaction control, and infrared frequency standards.