Abstract

Femtosecond time-resolved mid-infrared (MIR) spectroscopy based on chirped-pulse upconversion is a promising method for observing molecular structure and vibrational dynamics. By using a polarized narrowband pump pulse in which center frequency is rapidly scanned with an electrically tunable Fabry–Perot filter, we have developed a femtosecond MIR spectrometer that is more sensitive to molecular structure. The pump energy and polarization dependences of transient MIR absorption spectra measured with the spectroscopic system revealed the appearance of a dark (infrared-inactive) mode due to a slight decrease in the molecular symmetry of a metal carbonyl complex, ${\mathrm{Mn}}_2{(\mathrm{CO})}_{10}$, in solution. In addition, the rotational relaxation time of ${\mathrm{Mn}}_2{(\mathrm{CO})}_{10}$ in solution was determined as approximately 20 ps.

© 2018 Optical Society of America

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