The Temperature Dependence of Homogeneous and Inhomogeneous Vibrational Linewidth Broadening Studies Using Coherent Picosecond Stokes Scattering

  • S. M. George
  • A. L. Harris
  • M. Berg
  • C. B. Harris
Conference paper
Part of the Springer Series in Chemical Physics book series (CHEMICAL, volume 23)


The theoretical interpretation of vibrational dephasing experiments has been dependent on several simplifying assumptions [1]. One important assumption has been low depletion (≤5%) of the laser pump in the stimulated Raman excitation process. We have observed that, given exponential stimulated Stokes gain and pulse intensity fluctuations from passively mode-locked Nd:glass laser systems, maintaining stimulated Stokes conversions between 1–5% is a nearly impossible task. Figure 1 shows that immediately after the stimulated Raman scattering threshold is reached, the laser can be depleted ≥10% and depletion approaches ≈50% as the laser energy increases. Other studies measuring both laser and Stokes pulses after the Raman cell reveal coincident sharp thresholds for stimulated Stokes scattering and laser depletion [2]. Consequently, we believe that most vibrational dephasing experiments [3–6] have been performed in the high Stokes conversion regime.


Stimulate Raman Scattering Dephasing Time Raman Cell Lawrence Livermore Laboratory Homogeneous Linewidth 
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Copyright information

© Springer-Verlag Berlin Heidelberg 1982

Authors and Affiliations

  • S. M. George
    • 1
  • A. L. Harris
    • 1
  • M. Berg
    • 1
  • C. B. Harris
    • 1
  1. 1.Department of ChemistryUniversity of California and Materials and Molecular Research Division, Lawrence Berkeley LaboratoryBerkeleyUSA

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