Time-Resolved Impulsive Stimulated Raman Spectroscopy with Synchronized Triple Mode-Locked Lasers

A complete understanding of a photochemical reaction dynamics begins with real-time measurements of both electronic and vibrational structures of photoexcited molecules. Time-resolved impulsive stimulated Raman spectroscopy (TR-ISRS) with femtosecond actinic pump, Raman pump, and Raman probe pulses is one of the incisive techniques enabling one to investigate the structural changes of photoexcited molecules. Herein, we demonstrate that such femtosecond TR-ISRS is feasible with synchronized triple mode-locked lasers without using any time-delay devices. Taking advantage of precise control of the three repetition rates independently, we could achieve automatic scanning of two delay times between the three pulses, which makes both rapid data acquisition and wide dynamic range measurement of the fifth-order TR-ISRS signal achievable. We thus anticipate that the present triple mode-locked laser-based TR-ISRS technique will be of critical use for long-term monitoring of photochemical reaction dynamics in condensed phases and biological systems.