Abstract
A series of experiments on vibrationally excited polyatomic molecules revealed an increase in the molecular absorption at line center with decreasing laser-molecule interaction time.1,2 In these experiments, the interaction time was varied by using variable-duration picosecond CO2 laser pulses. We present a calculational approach based on coherent molecular excitation that agrees with experimental data and provides some interesting insight into intramolecular relaxation times in the vibrational quasicontinuum (QC).
© 1991 Optical Society of America
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