Experimental investigation of the Jahn-Teller effect in the ground and excited electronic states of the tropyl radical. Part II. Vibrational analysis of the A ̃ E 3 ″ 2 -X ̃ E 2 ″ 2 electronic transition Bond-selective photodissociation of partially deuterated ammonia molecules: Photodissociations of vibrationally excited NHD 2 in the 5ν NH state and NH 2 D in the 5ν ND state
We investigated the coherent motion of vibrational wave packets in the |B〉 1Πu state of the potassium dimer applying two color pump/probe spectroscopy with a sub 100 fs time resolution. Special interest was paid to the ionization probe step which was analyzed carefully by varying the probe energy over a wide range. Time-dependent quantum calculations explain the experimental outcomes by introducing a nonconstant transition dipole moment between the |B〉 and the ionic state |X+〉 and by taking into account the excitation of long lived autoionizing Rydberg states.
In a model system, i.e. the K 2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic jB -state and the electronic ground state jX and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment.
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