title: Laser-pulse requirements for coherent and mode-selective excitation in the quasicontinuum of polyatomic molecules.
abstract: We show that the theory of nuclear magnetic relaxation applies with equal validity to intramolecular relaxation in the quasicontinuum of polyatomic molecules. This theory permits an analysis of the laser-pulse requirements for vibrational-mode selectivity and coherent multiphoton excitation. The laser Rabi precession frequency, microepsilon/h, should exceed 1/T(1) or 1/T(2), the intramolecular relaxation rates in the quasicontinuum. In practice this requires either an ultra-fast optical-pulse risetime or a slower pulse that is tuned far to the red side of the transition.
authors.forename: E
authors.initials: E
authors.lastname: Yablonovitch