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Optica Publishing Group
  • Quantum Electronics and Laser Science Conference
  • OSA Technical Digest (Optica Publishing Group, 1992),
  • paper QMB2

Time-and frequency-domain studies of ultrafast molecular photodissociation

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Abstract

The analysis of spontaneous resonance rovibrational Raman scattering is a sensitive quantum-specific probe of photodissociation processes that occur on a subrotational-period time scale. The photodissociation of methyl radical and ammonia demonstrate how rotational- and vibrational-specific subpicosecond lifetimes are determined by this frequency-domain analysis and reveal the shape of the excited-potential energy surfaces responsible for the observed photodissociation dynamics. Mode-specific subpicosecond methyl iodide photodissociation rates are determined by the polarization analysis of resonance light-scattering spectra. When pressurized by a “solvent” gas, the character of the resonance emission changes and interference effects between Raman and fluorescence emission pathways are observed. This effect is discussed for the resonance emission of methyl iodide (B-state). The consequences of the interferences are discussed for estimates of electronic dephasing times in solution.

© 1992 Optical Society of America

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