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Optica Publishing Group
  • The Thirteenth International Conference on Ultrafast Phenomena
  • 2002 OSA Technical Digest Series (Optica Publishing Group, 2002),
  • paper ME29
  • https://doi.org/10.1364/UP.2002.ME29

Breaking bonds with mid IR pulses: Femtosecond photolysis of gas-phase metal carbonyls

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Abstract

Efficient and selective preparation of highly excited vibrational states in molecules is a challenging objective in physical chemistry. One means of achieving high ground-state vibrational excitation, possibly even leading to bond scission, was infrared multiphoton excitation (IRMPE) by ns lasers [1]. In this approach the resulting distribution over vibrational states always remained uncertain, since the role of intramolecular vibrational relaxation (IVR) as a process competing with or assisting excitation was unclear [2,3]. Femtosecond laser pulses resolve the uncertainty by restricting excitation to timescales faster than IVR. We have therefore applied fs mid IR laser technology toward the dissociation of transition metal carbonyls, which were previously dissociated by nanosecond IR pulses [4]. The fs pulse duration allows detailed modeling of the excitation mechanism. Specifically, analysis of the experimental data affords the number of vibrational modes involved in excitation, which in turn could lead to more efficient schemes for laser-driven dissociation.

© 2002 Optical Society of America

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