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Updated: Jun 21, 2026

Measurement of Ultrafast Vibrational Coherences in Polyatomic Radical Cations with Strong-Field Adiabatic Ionization
Published on: August 6, 2018
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.
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