Development of ultrafast time-resolved dual-comb spectroscopy

Ultrafast time-resolved dual-comb spectroscopy (TR-DCS) has been demonstrated, which enables direct observations of transient responses of complex optical spectra by combining dual-comb spectroscopy with the pump–probe method. TR-DCS achieves two-dimensional spectroscopy with a wide dynamic range for both the temporal and frequency axes. As a demonstration, we investigated the femtosecond relaxation dynamics of a photo-excited InGaAs saturable absorber in the near-infrared frequency region. The transient response of the interferogram was successfully obtained, and both the amplitude and phase spectra of the dynamic complex transmittance were independently deduced without using the Kramers-Kronig relations. A high phase resolution in the order of milliradian was achieved by suppressing the effect from the slow phase drift caused in the experimental system. Our proof-of-principle experiment promotes a pathway to coherent, highly accurate, and multi-dimensional pump–probe spectroscopy using the optical frequency comb technology