The interaction of two narrow band (Δν<100 MHz) UV light pulses of different intensity with a molecular three‐level system is investigated experimentally. The laser frequencies are tuned to an up (pump) and a down (dump) transition sharing a common excited rovibronic S1 level whose population is probed by a transition to the ionization continuum and ion detection. The time sequence of the two pulses results either in a lambda type coherent stimulated Raman adiabatic passage or a stimulated emission pumping (SEP) process. When the first case is realized by a 6.4 ns delay of the low intensity pump laser from the high intensity dump laser pulse, a fourfold increase of the depth of the ion dips compared to the SEP experiment is observed. This is in line with numerical calculations of the level populations using a density matrix formalism including coherent effects. Rotationally resolved ion dip spectra of the 62 state of benzene are presented and demonstrate the high sensitivity of the coherent excitation process of this work for ion dip spectroscopy.
Stimulated Raman adiabatic passage with pulsed lasers: High resolution ion dip spectroscopy of polyatomic molecules
R. Sussmann, R. Neuhauser, H. J. Neusser; Stimulated Raman adiabatic passage with pulsed lasers: High resolution ion dip spectroscopy of polyatomic molecules. J. Chem. Phys. 1 April 1994; 100 (7): 4784–4789. https://doi.org/10.1063/1.466269
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