Abstract
Vibrational population distributions within the CO-stretching T 1u manifold of W(CO) 6 in room-temperature n-hexane were created by using near-transform limited and linearly chirped picosecond infrared excitation pulses. These pulses were characterized using the second harmonic FROG (frequency-resolved optical gating) algorithm to determine the ∼8 cm −1/ps chirp for both positively- and negatively-chirped 2 ps pulses. FROG and time-resolved transient difference spectra were obtained with an InSb focal plane array detector. While unchirped and positively-chirped excitation leads predominantly to v=1 population, negatively-chirped pulses produce excess population in the v=2 level. These results are compared to predictions from density matrix calculations for a model potential.
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