Development of a multiplex fast-scan system for ultrafast time-resolved spectroscopy.

A fast-scan method was developed to obtain time-resolved signals with femtosecond resolution over a picosecond range on the fly and in real time. Traditional fast-scan methods collect data at each probe wavelength one by one, which is time consuming and thus not possible for the study of photofragile materials. In this work, we have developed a system that performs fast scans with multiplex detection. Ultrafast time-resolved spectroscopy was demonstrated using the newly developed system. Femtosecond laser pulses have been used for pump-probe studies of ultrafast processes in various materials, and both electronic relaxation and vibrational dynamics have been studied. However, experiments have been limited in sensitivity and reliability because they are affected by the long-term instability of the ultrashort laser pulses and by the fragility of the samples. The instability of the sources hinders precise determination of electronic decay dynamics and introduces systematic errors. The fragility of the samples reduces their amount or concentration, and can lead to contamination of the materials even if they were pure before the measurement. These effects make it difficult to obtain reproducible and reliable experimental data. In the present work, we have developed a fast-scan pump-probe spectroscopic system that can complete a set of measurements in less than 2 min. Quantitative estimates of the signal reproducibility demonstrate that these measurements provide higher reproducibility and reliability than conventional measurements.