Dual-Frequency Comb Transient Absorption: Broad Dynamic Range Measurement of Femtosecond to Nanosecond Relaxation Processes

Abstract

We experimentally demonstrate a dual-frequency comb-based transient absorption (DFC-TA) technique, which has a 12 fs time resolution and an ultrafast scan rate. Here, the fast scan rate is achieved by employing asynchronous optical sampling (ASOPS), which utilizes two independent mode-locked lasers with a slightly detuned repetition rates. The ASOPS approach is advantageous because photodegradation damage of optical sample during TA measurements can be minimized by a gated sampling. We show that the vibrational and electronic population relaxations of near-IR dye molecules in solution that occur in the time range from femtoseconds to nanoseconds can be resolved even with a single time scan measurement. The phase coherent nature of our dual frequency comb lasers is shown to be the key for successful coherent averaging with femtosecond time resolution preserved over many data acquisitions. We anticipate that the present DFC-TA method without using any pump probe time delay devices could be of use in developing ultrafast TA-based microscopy and time-resolved coherent multidimensional spectroscopy.