In this paper, we present a formalism for a generalized linear susceptibility applicable to femtosecond (fs) processes. As an application, we analyze the recent experimental results of the real-time fs transition spectra of the photodissociation of NaI and NaBr reported by Zewail et al. In this connection we also investigate in general the behaviors of decaying and trapping of the molecule in an excited electronic state coupled to a continuum.
A theory of the explosive desorption, observed by Chuang and Domen [Phys. Rev. Lett. 59, 1484 (1987); J. Vac. Sci. Technol. A 5, 473 (1987); J. Chem. Phys. (90, 3318 1989; Chem. Phys. Lett. (with A. Mödl). (154, 187 (1989)] is developed. When adsorbates are subjected to UV laser action, an explosive, molecular nonselective desorption takes place. This phenomenon is explained as follows: adsorbate molecules are excited by an UV laser to the higher electronic states. The electronic energy is delivered to the low energy vibronic states. The energy differences of these states are resonant to the corresponding phonon modes. This leads to the excitation of these phonons. When the energy input to the phonon modes exceeds their decay, phonon numbers start to increase exponentially. The phonon avalanche takes place. This in turn causes molecular nonselective desorption. The main result of the theory is the finding of the fluence and coverage dependent threshold conditions.
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