Abstract
Current models of IR multiphoton excitation of a polyatomic molecule suggest that photon absorption proceeds initially through coherent stepwise excitation of low lying levels of an anharmonic vibrational ladder up to the threshold of the qua sicontinuum.1 The enormous density of states (typically 105/cm-1) and level mixing at this energy provides incoherent excitation and ultimately leads to energy redistribution in the molecule via intramolecular and collisional relaxation processes. Such redistribution creates a broad band of excited vibrational states in spontaneous and anti-Stokes coherent Raman spectra of molecules.2
© 1990 Optical Society of America
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