Simplified setup for high-resolution spectroscopy that uses ultrashort pulses

Using a broadband femtosecond laser and a simple optical setup, we demonstrate narrow-bandwidth-tunable excitation of vibrational modes in CCl4 and CHBr3 liquids. The resolution obtained is 80 times higher than the laser bandwidth. A pair of time-shifted, linearly chirped pulses is created by use of a high-order dispersion-compensated prism-interferometer setup. We use this pulse pair to selectively excite Raman-active transitions. Our setup represents a significant simplification with improved resolution, of previous approaches to the use of ultrashort pulses for chemically selective spectroscopy. (C) 2003 Optical Society of America.