We consider the common situation of strong vibronic coupling of an optically bright (in absorption from the ground state) excited electronic state to a lower-lying dark electronic state in a polyatomic molecule. It is shown that for sufficiently short pump and probe laser pulses a time-resolved expe
The direct overtone pumping of polyatomic molecules
β Scribed by Karen L. Bintz; Donald L. Thompson; K.L. Kompa; R.D. Levine
- Publisher
- Elsevier Science
- Year
- 1993
- Tongue
- English
- Weight
- 482 KB
- Volume
- 215
- Category
- Article
- ISSN
- 0009-2614
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β¦ Synopsis
The fs solid state tunable lasers that are becoming available operate at peak power in the near infrared (say, 700-l 100 run). We present a computation of the classical power spectrum of CHsONO at this frequency range in order to elucidate the factors that determine the absorption cross section. Fast pumping and an initially already excited molecule are two factors that significantly enhance the probability of a direct (CH) overtone transition. For a molecule in its ground state using continuous wave pumping the cross section for overtone transitions is significantly smaller as compared to the isolated CH chromophore. We attribute this to a dilution, by IVR, of the optically bright mode. The time constant for this is such that fs pumping can access the de facto isolated CHr group.
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